The Strontium Optical Lattice Clock: Optical
Spectroscopy with Sub-Hertz Accuracy
byAndrew D. Ludlow
B.S. Physics, Brigham Young University, 2002

A thesis submitted to the
Faculty of the Graduate School of the
University of Colorado in partial fulfillmentof the requirements for the degree ofDoctor of Philosophy
Department of Physics
2008This thesis entitled:
The Strontium Optical Lattice Clock: Optical Spectroscopy with Sub-Hertz Accuracy
written by Andrew D. Ludlow
has been approved for the Department of Physics

Jun YeLeo Hollberg

Date

The final copy of this thesis has been examined by the signatories, and we find thatboth the content and the form meet acceptable presentation standards of scholarly
work in the above mentioned discipline.

Ludlow, Andrew D. (Ph.D., Physics)
The Strontium Optical Lattice Clock: Optical Spectroscopy with Sub-Hertz Accuracy
Thesis directed by Assoc. Prof. Adjoint Jun Ye

One of the most well-developed applications of coherent interaction with atoms
is atomic frequency standards and clocks. Atomic clocks find significant roles in a number of scientific and technological settings. State-of-the-art, laser-cooled, Cs-fountainmicrowave clocks have demonstrated impressive frequency measurement accuracy, withfractional uncertainties below the 10−15 level. On the other hand, frequency standards
based on optical transitions have made substantial steps forward over the last decade,benefiting from their high operational frequencies. An interesting approach to such an
optical standard uses atomic strontium confined in an optical lattice. The tight atomic
confinement allows for nearly complete elimination of Doppler and recoil-related effects
which can otherwise trouble the precise atomic interrogation. At the same time, theoptical lattice is designed to equally perturb the two electronic clock states so that theconfinement introduces a net zero shift of the natural transition frequency. This thesis
describes the design and realization of an optical frequency standard using 87 Sr confinedin a 1-D optical lattice. Techniques for atomic manipulation and control are described,
including two-stage laser cooling, proper design of atomic confinement in a lattice potential, and optical pumping techniques. With the development of an ultra-stable coherent
laser light source, atomic spectral linewidths of the optical clock transition are observed
below 2 Hz. High accuracy spectroscopy of the clock transition is carried out utilizing a femtosecond frequency comb referenced to the NIST-F1 Cs fountain. To explore
the performance of an improved, spin-polarized Sr standard, a coherent optical phasetransfer link is established between JILA and NIST. This enables remote comparisonof the Sr standard against optical standards at NIST, such as the cold Ca standard.

iv
The high frequency stability of a Sr-Ca comparison (3 × 10−16 at 200 s) is used to makemeasurements of Sr transition frequency shifts at the fractional frequency level below
10−16 . These systematic shifts are discussed in detail, resulting in a total uncertainty of
the Sr clock frequency at 1.5 × 10−16 , smaller than that of the best Cs standards of thetime. Considerations relevant for future performance improvements are also discussed.

Dedication

to Sharah,
we did it Together

Acknowledgements

Acknowledging in one written space all of the people who played an important rolein the training and successful completion of my Ph.D. dissertation research is perhaps
the impossible task. My interest in science was cultivated early on by individuals like
Mr. Woodruff, my high school chemistry teacher. At the collegiate level, I had theopportunity to work with Scott Bergeson and Mark Nelson at BYU and here had my firstin-depth exposure to experimental physics in the laboratory. Through the stimulating
research experiences in Scott’s lab and with an interest and fascination in atomic andoptical physics, I began graduate school at the University of Colorado. I benefitted
greatly from my involvement in the Optical Science and Engineering program, whichgave me the opportunity to see up-close different research settings (academia, nationallab, and industry) and to get to know and work with talented scientists like Jun Ye, Chris
Oates, Leo Hollberg, Charles Garvin, Charley Hale, Ross Hartman, Dana Anderson, andVictor Bright.
I settled into Jun’s lab and while working on the strontium project, have had thegreat pleasure of working and developing friendships with many very gifted scientists.
Xinye Xu, Tom Loftus, Tetsuya Ido, Tanya Zelevinsky, and Gretchen Campbell werepostdocs on the strontium project at various times over the years. Each one has madecritical contributions to the evolution of the strontium experiment. Perhaps even moresignificantly to me personally, they have taught, guided, and worked alongside me anda good part of my graduate education has come through interaction with them. Marty

vii
Boyd and I were graduate students working together on the Sr experiment for “theduration”. Our research relationship has proven that two minds focused on a common
goal can surely accomplish more than could be done separately. Sebastian Blatt has
been an invaluable ‘wiz’ on many aspects of the Sr experiment and I look forward
to seeing the strontium team’s continued research in subsequent years. Seth Foremanhas been much more than the frequency comb master and played an important role invarious aspects of the strontium experiment, particularly remote frequency transfer andlaser phase noise measurements across the optical spectrum.
Mike Martin and Marcio de Miranda have done a great job continuing that workand enabling the amazingly precise optical frequency measurements in our laboratory.
Benefitting greatly from his expertise, it was largely through working with Mark Notcutt
that I got my feet wet in very-high-stabilization of lasers. I enjoyed many stimulating
discussions with Thomas Zanon-Willette, who helped open the beauty of three-levelatomic systems to me. I’ve genuinely enjoyed interaction with Jan Thomsen, Xueren
Huang, and Long Sheng Ma during their visits to JILA. Our work has benefitted frommany others in the lab, Kevin Holman, Jason Jones, Eric and Darren Hudson, Matt
Stowe, Kevin Moll, Mike Thorpe, Adela Marian, Brian Sawyer, Avi Pe’er and Dylan
Yost to name a few.
I give much thanks to my advisor, Jun Ye. There are innumerable positive things I
could say of him, his talent as a physicist, and his leadership in the lab. I have benefitted
immensely from the environment he cultivates and the opportunities and experiencesin his lab. I deeply respect him and am a better scientist and person for having worked
under his tutelage. He has continued on the tradition of excellence from the lab’s founder
Jan Hall. It is a special opportunity to interact with Jan, ask a question, and open up
the floodgates of his vast expertise. It was Jan and Alan Gallagher who collaborated on
the original Sr experiment in JILA, and I benefitted greatly from continued interaction
with both of them.

viii
JILA is a special place, and there are many reasons for its success as a research
institute. Among these, the electronics and machine shops play a key role. I makeparticular mention of fruitful interactions I had with Terry Brown in the JILA electronics
shop.
It has been the combined efforts of the strontium team which made possible
the exciting exploration into the strontium atom, a part of which I could play a role.
Furthermore, our collaboration with other scientists outside the strontium team has
made many of our efforts possible, including some of the results described in this thesis.
Among these are: P. Naidon, P. Julienne, and R. Ciurylo (ultracold atomic collisions, including density shifts and photoassociation), J. Stalnaker, S. Diddams, and J. Bergquist(coherent optical carrier transfer), T. Fortier, J. Stalnaker, S. Diddams, Y. le Coq, Z. W.
Barber, N. Poli, N. Lemke, K. Beck, and C. Oates (remote optical clock evaluation with
NIST), T. Parker, S. Jefferts, and T. Heavner (NIST H-maser and Cs fountain measurements), E. Arimondo (three-level interactions in strontium), and C. Greene (theoreticalwork and guidance).
I reserve a very special acknowledgement to my family. Through my parents, Alex
and Clyda Ludlow, I learned the value of education and the work ethic to pursue it.
They taught by example the most important principles and attributes, and I recognize
their enormous role in who I am and what I may become. My parents-in-law, Steveand Judy Smith, provided constant love and support to me and my family during thelaborious years of school. And most importantly, it is together with my dear wife Sharah
and my children Rachael, David, and Evan that I have travelled this road. They havebeen my strongest support, my most meaningful inspiration, and the origin of my mostprecious moments. The effort which has culminated in the pages of this thesis has
been a worthwhile endeavor. But its most important characteristic is that it was done
together with them.

Contents

Chapter
1 Introduction: Atomic Clocks and Strontium

1

1.1

Dimensions and Standards . . . . . . . . . . . . . . . . . . . . . . . . . .

1

1.2

Atomic Frequency Standards . . . . . . . . . . . . . . . . . . . . . . . .

3

1.3

Optical Frequency Standards . . . . . . . . . . . . . . . . . . . . . . . .

6

1.4

Strontium: Electronic Structure . . . . . . . . . . . . . . . . . . . . . . .

9

1.5

The Need for Cold Atoms . . . . . . . . . . . . . . . . . . . . . . . . . .

14

1.6

Precision Timing Applications . . . . . . . . . . . . . . . . . . . . . . . .

15

1.7

Thesis At-a-Glance . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

16

2 Atomic Manipulation and Control

18

2.1

Laser Cooling: Basic Concepts . . . . . . . . . . . . . . . . . . . . . . .

18

2.2

Laser cooling strontium: 1 S0 -1 P1 MOT . . . . . . . . . . . . . . . . . . .

23

2.2.1

Laser cooling properties of 1 S0 -1 P1 MOT . . . . . . . . . . . . .

23

2.2.2

Experimental details of the 1 S0 -1 P1 MOT . . . . . . . . . . . . .

29

Laser cooling strontium: Narrow line laser cooling in the 1 S0 -3 P1 MOT

36

2.3.1

Narrow line laser cooling dynamics . . . . . . . . . . . . . . . . .

36

2.3.2

Experimental details of the 1 S0 -3 P1 MOT . . . . . . . . . . . . .

45

Laser cooling and trapping 87 Sr . . . . . . . . . . . . . . . . . . . . . . .

49

The 1 S0 -1 P1 MOT . . . . . . . . . . . . . . . . . . . . . . . . . .

49

2.3

2.4

2.4.1

x
The 1 S0 -3 P1 MOT . . . . . . . . . . . . . . . . . . . . . . . . . .

52

Interrogation of Tightly Confined Atoms . . . . . . . . . . . . . . . . . .

56

2.5.1

Free Space Atom Interrogation . . . . . . . . . . . . . . . . . . .

56

2.5.2

Confinement in a Harmonic Potential . . . . . . . . . . . . . . .

58

2.5.3

Uniform Confinement Regime . . . . . . . . . . . . . . . . . . . .

66

2.5.4

Well resolved sideband regime . . . . . . . . . . . . . . . . . . . .

67

2.5.5

Lamb-Dicke regime . . . . . . . . . . . . . . . . . . . . . . . . . .

70

2.4.2
2.5

2.6

2.7

Atomic Confinement with a Far-Detuned Optical Wave

. . . . . . . . .

72

2.6.1

Dipole Potential . . . . . . . . . . . . . . . . . . . . . . . . . . .

72

2.6.2

Dipole Polarizability . . . . . . . . . . . . . . . . . . . . . . . . .

74

2.6.3

1-D Lattice Confinement . . . . . . . . . . . . . . . . . . . . . . .

85

2.6.4

Benefits of 1-D Lattice Confinement . . . . . . . . . . . . . . . .

88

2.6.5

Further Details of 1-D Lattice Confinement . . . . . . . . . . . .

90

State Preparation via Optical Pumping: Nuclear spin polarization . . .

96

3 Coherent Light-Matter Interaction: Hz level spectral linewidths in the opticaldomain99

3.1

The Need for Atomic and Optical Coherence . . . . . . . . . . . . . . .

99

3.2

Atomic Coherence . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 100

3.3

Optical Coherence: Laser Frequency and Phase Stabilization . . . . . . 102

3.4

3.3.1

Laser Stabilization Design Considerations . . . . . . . . . . . . . 103

3.3.2

Sub-Hz Sr clock laser. . . . . . . . . . . . . . . . . . . . . . . . 113

Atomic spectra of the optical clock transition with Hz level linewidth . . 121
3.4.1

Experimental Setup . . . . . . . . . . . . . . . . . . . . . . . . . 121

3.4.2

Spectra . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 124

3.4.3

Sideband structure . . . . . . . . . . . . . . . . . . . . . . . . . . 129

xi
4 Development of the Sr Optical Standard: High Accuracy Spectroscopy

133

4.1

Counting optical frequencies: the fs frequency comb . . . . . . . . . . . 133

4.2

Frequency reference
4.2.1. . . . . . . . . . . . . . . . . . . . . . . . . . . . . 137

Microwave fiber transfer . . . . . . . . . . . . . . . . . . . . . . . 138

4.3

Evaluation of the Frequency Shifts and their Uncertainty . . . . . . . . 140

4.4

Absolute frequency measurement of the 1 S0 -3 P0 transition . . . . . . . . 147

5 The Strontium Optical Frequency Standard at 10−16 Uncertainty: Remote Optical Comparison of Optical Clocks
5.1

150

Design Improvements in the Sr Optical Standard . . . . . . . . . . . . . 151
5.1.1

Atomic Polarization . . . . . . . . . . . . . . . . . . . . . . . . . 151

5.1.2

Laser Stabilization to the Atomic Transition

5.1.3

Other System Improvements . . . . . . . . . . . . . . . . . . . . 156. . . . . . . . . . . 153

5.2

Optical Carrier Remote Transfer . . . . . . . . . . . . . . . . . . . . . . 160

5.3

Stability Evaluation of the Sr Optical Frequency Standard . . . . . . . . 165

5.4

Accuracy Evaluation of the Sr Optical Frequency Standard . . . . . . . 176
5.4.1

Measurement Description . . . . . . . . . . . . . . . . . . . . . . 176

5.4.2

Lattice AC Stark shift . . . . . . . . . . . . . . . . . . . . . . . . 178

5.4.3

1st - and 2nd - order Zeeman shifts . . . . . . . . . . . . . . . . . . 186

5.4.4

Density shift . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 188

5.4.5Blackbody radiation induced Stark shift . . . . . . . . . . . . . . 202

5.4.6

Probe laser induced AC Stark shift . . . . . . . . . . . . . . . . . 206

5.4.7

Line-pulling . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 207

5.4.8

Servo Error . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 207

5.4.9

Other residual 1st -order Doppler shifts . . . . . . . . . . . . . . . 208

5.4.10 2nd -order Doppler shift . . . . . . . . . . . . . . . . . . . . . . . . 210
5.4.11 Other effects . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 210

xii
5.4.12 Uncertainty Summary . . . . . . . . . . . . . . . . . . . . . . . . 211
5.5

Absolute Frequency Measurement . . . . . . . . . . . . . . . . . . . . . . 213

5.6

Outlook . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 215

Bibliography

217

xiii

TablesTable
1.1

Sr transition parameters . . . . . . . . . . . . . . . . . . . . . . . . . . .

11

1.2

The natural abundances of strontium isotopes . . . . . . . . . . . . . . .

13

2.1

Transition parameters used to calculate the atomic polarizability of the
Sr clock states. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

80

4.1

Measurement 1 systematic uncertainties . . . . . . . . . . . . . . . . . . 144

4.2

Measurement 2 systematic uncertainties . . . . . . . . . . . . . . . . . . 146

5.1

Dick effect limited instability of the JILA Sr standard for various valuesof experimental cycle time Tc and transition probing time tp . . . . . . . 174

5.2

Experimentally measured values of λmagic . . . . . . . . . . . . . . . . . 184

5.3

Systematic shifts and their uncertainties for the 87 Sr 1 S0 -3 P0 clock transition (2007) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 212

xiv

FiguresFigure1.1

Length measurement precision using different rulers . . . . . . . . . . .

8

1.2

Term diagram for 88 Sr . . . . . . . . . . . . . . . . . . . . . . . . . . . .

10

2.1

Abbreviated term diagram for 1 S0 -1 P1 MOT . . . . . . . . . . . . . . .

24

2.2

Two-level steady state excitation and saturation . . . . . . . . . . . . .

26

2.3

Spatial confinement in a J = 0 - J = 1 MOT . . . . . . . . . . . . . . .

29

2.4

Experimental apparatus . . . . . . . . . . . . . . . . . . . . . . . . . . .

30

2.5

1 S -3 P MOT as a function of detuning
01. . . . . . . . . . . . . . . . . .

39

2.6

1 S -3 P MOT as a function of intensity
10. . . . . . . . . . . . . . . . . .

40

2.7

1 S -3 P MOT temperature
01. . . . . . . . . . . . . . . . . . . . . . . . .

42

2.8

1 S -3 P MOT timing diagram . . . . . . . . . . . . . . . . . . . . . . . .
0
1

48

2.9

87 Sr energy level diagram. . . . . . . . . . . . . . . . . . . . . . . . . .

50

2.10 Laser cooling 87 Sr on the 1 S0 -3 P1 transition . . . . . . . . . . . . . . . .

53

2.11 Absorption spectrum of a confined atom . . . . . . . . . . . . . . . . . .

62

2.12 Absorption spectrum of an atomic ensemble from weak to strong confinement . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

69

2.13 Sr clock transition atomic polarizability . . . . . . . . . . . . . . . . . .

79

2.14 Schematic of the optical layout for the 1-D optical lattice . . . . . . . .

86

2.15 Atomic confinement energy band structure in the optical lattice . . . . .

91

xv
2.16 Rabi frequency for pure electronic excitation from a given motional state94

2.17 Optical pumping used for nuclear spin polarization state preparation . .

98

3.1

Stable laser-cavity system . . . . . . . . . . . . . . . . . . . . . . . . . . 114

3.2

Stable-cavity field ringdown . . . . . . . . . . . . . . . . . . . . . . . . . 116

3.3

Sub-Hz laser linewidth . . . . . . . . . . . . . . . . . . . . . . . . . . . . 118

3.4

Clock laser instability and frequency noise . . . . . . . . . . . . . . . . . 119

3.5

Clock laser distribution . . . . . . . . . . . . . . . . . . . . . . . . . . . 122

3.6

Spectra of the 1 S0 -3 P0 clock transition . . . . . . . . . . . . . . . . . . . 125

3.7

Ultra-narrow spectra of the 1 S0 -3 P0 clock transition . . . . . . . . . . . 127

3.8

Motional sideband spectra . . . . . . . . . . . . . . . . . . . . . . . . . . 130

4.1

The frequency comb . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 134

4.2

Remote microwave frequency transfer schematic . . . . . . . . . . . . . . 139

4.3

Remote microwave frequency transfer results . . . . . . . . . . . . . . . 141

4.4

Measurement 1 clock transition uncertainty evaluation (2005) . . . . . . 142

4.5

Measurement 2 clock transition uncertainty evaluation (2006) . . . . . . 145

4.6

Measurement 1 and 2 absolute frequency measurements . . . . . . . . . 148

5.1

Laser stabilization to the clock transition with a spin-polarized atomic
sample . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 154

5.2

Phase coherent optical carrier transfer schematic . . . . . . . . . . . . . 161

5.3

Phase coherent optical carrier transfer performance . . . . . . . . . . . . 163

5.4

Sr frequency counting with both optical and microwave references. . . 166

5.5

Sr frequency counting with both optical and microwave references. . . 167

5.6

Instability of the Sr frequency standard . . . . . . . . . . . . . . . . . . 173

5.7

Experimental setup for Sr-Ca remote measurements . . . . . . . . . . . 177

5.8

Lattice AC Stark shift sensitivity of the clock transition . . . . . . . . . 183

xvi
5.9

First and second order Zeeman shift sensitivity of the clock transition . 187

5.10 Density shift sensitivity of the clock transition . . . . . . . . . . . . . . . 190
5.11 Atomic excitation as a function of time

. . . . . . . . . . . . . . . . . . 194

5.12 Density shift sensitivity as a function of 1 S0 population . . . . . . . . . 196
5.13 Improving the blackbody shift uncertainty: the blackbody chamber . . . 205
5.14 Absolute frequency measurements of the 87 Sr clock transition . . . . . . 214

Chapter 1

Introduction: Atomic Clocks and Strontium

1.1

Dimensions and Standards
As we model the world around us, we neatly categorize the fundamental propertiesof matter into dimensions. Some dimensions are so common in everyday experiencethat most people are accustomed to intuitively perceiving the outside world using these
dimensional basis sets. Among these are length (in all three spatial directions), time, andmass. Others like electric charge, intrinsic spin, quark flavor, and quark color are lesswell-known to the general public, but are predominantly accepted as basic quantities.
Still others, like additional spacetime dimensions included in string theories attempting
to unify gravity with the other fundamental interactions, have been proposed and are
currently being scrutinized by the scientific community.
To be fully useful, any dimension must be sufficiently characterized or defined.
This is equivalent to having a well-defined unit for each dimension. Many systems ofunits exist, and different fields of study frequently have their own natural system ofunits. The International System of Units (SI) has emerged as the most widely usedsystem of units, both internationally and scientifically. The SI unit system employs
seven fundamental base units from which many other derived units originate. The
seven SI base units are: meter (length), second (time), kilogram (mass), ampere (electric
current), kelvin (thermodynamic temperature), mole (quantity), and candela (luminous
intensity). The quantitative utility of the SI system rests on how well-defined each base

2
unit is. From a practical perspective, the job of providing this definition ultimately
lies with a primary standard. A standard is some type of physical exemplar which
realizes the definition of a dimensional unit. As the name denotes, a primary standard
is usually the highest performance standard to which the secondary standards referback. As an example, the current primary standard for the SI kilogram is given by
the international prototype kilogram (IPK). The IPK is a cylindrically shaped pieceof platinum-iridium alloy which is maintained by the International Bureau of Weights
and Measures (referred to as BIPM, which is abbreviated from its French name, thisinstitution provides uniformity and traceability to the SI system). A piece of material
is designated to have a mass of one kilogram when it has the same measurable mass as
the IPK.
Several basic figures of merit relating to any standard can be highlighted byconsidering the case of the IPK standard of the kilogram. The first such figure of meritis the stability of the standard - does the standard provide a fixed definition of the unit
or does it change. For example, by comparing the IPK mass to similarly constructed andcared-for replicas of the IPK, it has been found that the IPK mass changes over time due
to airborne contamination and cleaning processes [1, 2]. For this reason, a standard bornof nature and unsusceptible to mass fluctuations is preferred over man-made artifacts
such as the IPK. For example, the mass of a single unbound electron could, in principle,
serve as the definition of mass. In this case, the mass definition would be expected to beconstant (highly stable) over time. Technical limitations have impeded the developmentof a natural standard realizing this kind of fundamental mass definition (the kilogram
remains the last unit defined by an artificial prototype). However in 2005, motivated inpart by the potential improvement in stability, the International Committee for Weights
and Measures (abbreviated CIPM, which is the supervisory committee to the BIPM)
recommended that the kilogram be defined in terms of fundamental natural constants.
Another figure of merit is related to how the standard changes under different

3environments. For example, how does temperature and humidity affect the mass of
the IPK, and how well controlled can these environmental parameters be maintained
during storage and usage. Standards which have small and well-understood sensitivity
to their environment can realize the unit definition more uniformly as the environmentchanges through space and time. Furthermore, the standard’s utility is limited by thetechnology and science of the relevant measurement itself. If we find a chunk of steel
which has the same measurable mass as the IPK, to how many digits can we trust
the measurement that they are, in fact, the same mass. It is thus useful to choose astandard for which the related measurement science and technology is well-understood.
Each of these considerations relates to what degree of accuracy the standard realizes
the definition of the unit. (Note that for the unique case of the IPK, one can argue
that because the IPK is both the standard and the actual definition of the SI kilogram,environmental sensitivity is not important for its accuracy, since they change together.)
Finally, two similar standards ideally provide the same definition when comparedto each other. This figure of merit is related to the properties which determine thestandard’s accuracy and is typically referred to as reproducibility. A proper choice ofstandard, therefore, includes consideration of the standard’s stability, accuracy, andreproducibility. With these in mind, we now consider the standard of time, the mostwell-defined unit in the SI system.

1.2

Atomic Frequency Standards
In practice, time is and has been measured in units of periodic events which repeat

themselves. The earth’s rotation around the sun or the earth’s rotation around its own
axis has served as an astronomical standard for which hours, days, and years havebeen measured in many civilizations. The pendulum clock uses gears which effectively
counts the periodic swinging back and forth of a physical pendulum, and in so doing
has provided timekeeping for centuries. Since the frequency of these periodic devices

4is related trivially to the period (frequency is the inverse of the period), the role ofa time (interval) standard is essentially equivalent to that of a frequency standard.
As physics has evolved from the time of Newton, so did our understanding of how
these standards quantitatively operated. Experience and improved physical models
revealed how these standards change over time and under different conditions, dictating
their limited accuracy and stability. This led to the search for other physical processes
that nature provides which would better suit the role of a time/frequency standard.
Early understanding of atomic behavior in the nineteenth century and developmentof quantum mechanics in the twentieth century revealed that atomic systems can bevery well suited for just such a task [3]. Electronic excitation of an atom, acting as
nature’s pendulum, resonates at the same, well-defined frequency and does so largely
insensitive to the environment around it. In addition, the excitation energy required toobserve this process is low enough (microwave and optical frequencies) for the laboratoryenvironment. It did not take long (decades) after quantum mechanic’s advent thatatomic systems emerged as the natural choice for frequency standards and ultimately
as the definition of the SI base unit of the second.
For most of their half-century history, frequency standards based on atomic cesium have provided the performance best suited for a primary frequency standard. For
this reason, since 1967, the SI second has been defined as follows: “The second is theduration of 9 192 631 770 periods of the radiation corresponding to the transition between the two hyperfine levels of the cesium 133 atom” [4]. To illuminate the basic
operation of an atomic frequency standard, I describe the Cs standard in outline detail.
The ground state of Cs has two hyperfine states F = 3 and F = 4 (F denotes thetotal angular momentum of the state, given by the vector sum of the electronic andnuclear angular momentum terms, I and J respectively). When Cs atoms are illuminated by radiation resonant with exactly the energy difference between the two statesF = 3 mF = 0 and F = 4 mF = 0 (mF , the magnetic quantum number, denotes the5projection of F along the quantization axis), a weak electronic transition is excited. As
a consequence, electronic population is moved between the hyperfine states and the radiation is absorbed and then re-emitted by the atomic sample. By detecting electronic
population movement or radiation intensity as a function of radiation frequency, theradiation frequency can be stabilized or locked to the resonant frequency of the atomic
excitation. This is the approach of a passive frequency standard, where the radiation is
generated externally but stabilized through spectroscopy of the atomic sample. The frequency of the atomic resonance is fCs = 9.192631770 GHz (by definition). By counting
9,192,631,770 periods of the radiation, a time interval equal to one second is measured.
One of the critical properties of the Cs hyperfine transition frequency is its small
sensitivity to environmental perturbations which shift its frequency. However, since nostandard is completely insensitive to perturbation by its environment, it is importantto specify under what conditions the Cs standard must operate to properly define the
SI second. A natural choice is to specify a completely ideal environment, free of any
perturbations. By controlling the environment as close to ideal as possible, and by quantitatively evaluating the effect of excursions from the ideal environment, a determination
can be made of the uncertainty with which the Cs standard realizes the unperturbed,
true definition of the SI second. For the operating frequency of the Cs standard fCs ,this uncertainty can be smaller than 10 µHz. Expressed as a fraction of fCs , this impressively small uncertainty, δf , is less than 1 × 10−15 . This is equivalent to saying
that, for state-of-the-art Cs standards, the SI second can be realized with a fractional
inaccuracy of less than 1 part per quadrillion, making it (pragmatically speaking) themost well-defined unit in the present SI system.
Unfortunately, this small inaccuracy is not always experimentally accessible in atime/frequency measurement. Noise processes intrinsic to the Cs standard operation
degrade the stability of the frequency output at short timescales. The frequency output
must be accumulated over long times to average through these noise processes and6reach a measurement instability at the level of the inaccuracy. Depending on the detailsof operation, the required averaging time can exceed 1 day [5, 6, 7, 8]. For some
applications, this long averaging time can be prohibitive. Efforts have been made to
reduce the intrinsic noise processes and subsequently reduce the required averaging time
[9, 10, 11]. However, an altogether different approach could yield a frequency standard
with instability smaller than the fundamental limitation of the Cs standards, as well as
provide further reduction in the system’s inaccuracy. This different approach is to use
a standard operating at much higher frequencies in the optical domain.

1.3

Optical Frequency Standards
A common tool for measurement of length is the ruler. As simple as a longstick of wood with regularly spaced tick marks, the ruler makes length measurement
possible by counting the number of ticks between two points of interest. The knowledge
that the ticks have been placed at calibrated intervals allows one to extract the length
measurement. It is instructive to consider what determines the precision to which a
ruler, such as those in Figure 1.1, can measure length. For a given length, the more tickmarks which are indicated on the ruler, the more precisely the ruler can measure. For
example, we suppose that a cm on ruler A is indicated by 5 tick marks and by 25 tickmarks on ruler B. Measuring a 5 cm long object would give 25 ticks from ruler A and
125 ticks from ruler B. Pressed by an observer as to how precisely these measurements
were made, one could naturally respond that the uncertainty was less than one tick,since the toy clearly measured close to the 25th tick on ruler A and the 125th tick onruler B. By simply having more ticks, the measurement using ruler B has a fractional
uncertainty (< 1/125) smaller than the measurement with ruler A (< 1/25).
Now imagine a scenario where we measure two different objects which are nearly
but not quite the same length. Ruler C is identical to ruler A, only with an additional
set of minor tick marks between each major tick. Using ruler A, both objects measure

7
to approximately the 25th large tick, one a bit short of it and the other reaching nearly
exactly the tick. On ruler C, the second object again falls at nearly exactly the 25th
major tick, and the first falls short of it. In this case, however, it is clear that the object
is two minor ticks away from the large tick, and the distance between major ticks canbe divided down more precisely.
These examples illustrate two important features of the ruler which determine
the measurement precision: the number of tick marks for a given length and how welldefined the distance between (major) tick marks is. The same is true for the measurement of time. A clock operates by counting the time ticks generated by its frequency
standard. More ticks in a second (i. e. higher frequency from the standard) gives higher
measurement resolution for a given time interval. More well-defined ticks from the frequency standard (i.e. a low-phase-noise standard with a narrowband frequency output)
also gives higher resolution. This can be stated more formally by considering an atomic
standard which operates by stabilization to an atomic transition with frequency ν0 andlinewidth δν. Assuming the instability is limited by an unspecified white frequency noise
process (equal noise amplitude at all Fourier frequencies), the fractional instability ofsuch a standard is given by [12]:σ (τ ) =δνη√ν0 (S/N ) τ(1.1)

Here S/N indicates the signal to noise ratio of the atomic transition measurement (rms,
1 Hz BW), τ is the averaging time, and η is a parameter close to unity whose exact value
depend on details of the clock operation, including the type of atomic spectroscopy implemented. As stated previously, one way to reduce the final instability is to average forlonger times (although this averaging occurs only as the inverse square root). Anotherway is to increase the measurement S/N , although fundamental limitations exist on
how large this can be. As illustrated in the ruler analogy, instability can be reducedwith an atomic transition of very narrow linewidth. This will be discussed later in the8Ruler A

Ruler B

Ruler C

Figure 1.1: Three rulers used to make length measurements. The number of major ticks
per length and the discrimination between major ticks (represented by the minor ticksof Ruler C) determine the measurement precision of each ruler.

9context of strontium (Sr). Most notably, a straightforward way to reduce the instability
is to operate the standard at higher frequencies, ν0 . This can be accomplished with an
atomic transition at optical frequencies, which can be five orders of magnitude higher
frequency than the microwave transitions used in Cs standards. In principle, this same
argument holds not just for the instability but also for the inaccuracy of the standard
as well. For a given sensitivity to environmental perturbations, moving to an opticalatomic transition can reduce the uncertainty in realizing the ideal frequency output.
This is easier said than done, as a change to the optical domain requires a substantialchange in the tools and technology required to construct such a standard. However,as we see in the next section, there are atomic systems very well suited to be opticalfrequency standards.

1.4

Strontium: Electronic Structure
Elements are organized in the periodic table according to their electronic con-figuration. Elements in the same group (column) have similar electronic configurationand thus similar atomic and chemical properties. Group 1 atoms, the alkali metals,
have only one valence electron and thus have electronic structure similar to that ofhydrogen. The simplicity associated with having just one valence electron has madealkali atoms a popular choice for experimental and theoretical work in atomic physics.
Their ground states, with orbital angular momentum L = 0, have a variety of allowedtransitions to other electronic states, all spin doublet states. The alkaline earth atoms,
located in Group 2 of the periodic table, have two valence electrons. The presence of asecond valence electron creates a rich mixture of electronic states, neatly divided into
spin singlet (intrinsic electronic spin S = 0) and spin triplet (S = 1) states. Among thealkaline earth atoms are elements such as beryllium, magnesium, calcium, and strontium. Similar to the alkaline earth metals, elements such as the lanthanide ytterbium,
the transition metals zinc, cadmium, and mercury, and the synthetically prepared ac-

10

2
1
0

5s6p
5s5d

16
13

5s6s
15

5s6s
9

5s5p

11

10
8
5

5s4d
7
6

14

12

1
5s5p

4

5s4d

2
1
0

2
1
0

3 2

5s2

1S 1P 1D 3S 3P 3D
1
0
1
J
J
2
Figure 1.2: Term diagram for 88 Sr. The states are organized horizontally by their electronic spin. The dashed line indicates the separation between the singlet and triplet spinstates originating from the dipole selection rule, ∆S = 0. The electronic configurationfor each state is listed next to it. Transitions are numbered, with the correspondingtransition wavelength and decay rate given in Table 1.1. Note that for the case of 87 Sr,further hyperfine structure is present.

11

Table 1.1: Sr transitions and their transition wavelength and Einstein A coefficients.
Transition number corresponds to those shown in Figure 1.2.
Transition
1
2
3
4
5
6
7
8
9
10
11
12
13
14
15
16

λ (nm)
461
698
689
671
6.5 × 103
1.8 × 103
1.9 × 103
679
688
707
490
3 × 103717
293
1.12 × 103
2.85 × 103

A (1/s)
1.9 × 108
7 × 10−3 (87 Sr)
4.7 × 104
2 × 10−3
3.9 × 103
2.2 × 103
1.1 × 103
9 × 106
2.8 × 107
4.6 × 107
6.1 × 108
3.5 × 105
1.6 × 107
1.9 × 106
2 × 107
3 × 106

12
tinide nobelium have two valence L = 0 electrons. The energy level term diagram forstrontium is shown in Figure 1.2. While details of the energy level structure are different for each alkaline earth atom, many major features are shared among them. The
ground state is 1 S0 . Strong dipole allowed transitions exist from the ground state tohigher lying 1 P1 states. For strontium and several other alkaline earth atoms the very
first excited state is a triplet state 3 P , with allowed dipole transitions to a variety of
3 S and 3 D states.

No dipole transitions are allowed between the spin singlet and spin

triplet states due to the dipole selection rule ∆S = 0. As a consequence, these states are
predominantly isolated from each other, except for a set of weaker, multipole couplings
connecting them.
One notable exception to the lack of dipole couplings between the singlet andtriplet states is between the ground 1 S0 and the excited 3 P1 states. As a result of L · S
interaction among the excited states, the 3 P1 state acquires a small admixture of the
1P

1 state, which does have dipole coupling to

1 S . As a result, a weak dipole transition0

1 S -3 P exists [13, 14, 15, 16].
0
1

There are four stable isotopes of strontium:

88 Sr, 87 Sr, 86 Sr,and 84 Sr. The

isotopes and their natural abundance are found in Table 1.2 [17]. As a general rule, due
to spin pairing of the nucleons, isotopes with an even atomic number Z and an evenatomic mass number A have a nuclear spin I = 0 [18]. This is the case for the evenisotopes of Sr, which have Z = 38. The odd isotope 87 Sr has I = 9/2. In this case, thepresence of nuclear spin allows hyperfine interaction to perturb the 3 P states shown in
Figure 1.2. Significantly, the hyperfine interaction weakly mixes 3 P0 with the 1 P1 and3P

1 states. Consequently, like

3 P , 3 P acquires a very weak dipole coupling (although10much weaker than 3 P1 ) to 1 S0 [13, 14, 15, 16, 19].
As shown in Figure 1.2, the ground state 1 S0 has at least three noteworthy transitions each with very different strengths. The diversity in these transitions facilitate theiruse for a variety of atomic manipulations, each useful for application to optical frequency

13
Table 1.2: The natural abundances of strontium isotopes.
Atomic Mass Number
88
87
86
84

Natural Abundance
82.56%
7.02%
9.89%
0.56%

standards. The 1 S0 -1 P1 transition is strong (Einstein A coefficient, A = 2.1 × 108 s−1 )and the lowest 1 P1 state has only very weak decay rates to states other than 1 S0 . As
a result, this transition is well-suited for traditional laser cooling, permitting a thermal
beam of dilute Sr gas to be cooled to mK temperatures and collected in a magnetooptical trap. The 1 S0 -3 P1 transition is weaker (A = 4.7 × 104 s−1 ) and is a closed
transition. This transition complements the 1 S0 -1 P1 nicely, by permitting a secondary
stage of laser cooling to further cool the atomic sample below the fundamental limit forthe 1 S0 -1 P1 transition. In this way, the atomic sample can be cooled and trapped at or
below µK temperatures, where thermal energy is small enough for atomic confinement
in a traditional optical dipole potential.
Finally, the 1 S0 -3 P0 is extremely weak (A = 7 × 10−3 s−1 ). According to the criteria expressed above, a good atomic transition for an optical frequency standard has atleast two important qualities: a narrow linewidth and weak sensitivity to perturbations.
1 S -3 P exhibits a serendipitously narrow (but not too narrow) transition linewidth of00∼ 1 mHz. Furthermore, the sensitivity of this transition to most relevant perturbations,
including magnetic fields and optical radiation, is comparatively small. The effect of
blackbody radiation, although fractionally smaller than that for Cs, is non-negligible
but controllably sized [20]. Together with other properties discussed later in this text,
Sr stands as a very favorable candidate for a high performance optical frequency standard. Many laboratories around the world are actively developing standards based on
Sr [21, 22, 23, 24, 25, 26, 27, 28, 29] or similar atoms like Yb [30, 31] and Hg [32, 33].
Along with other optical frequency standards, these systems hope to reach eventual

14inaccuracies of 1 × 10−18 , or approximately 100 times smaller than the expected limit
to the Cs standard inaccuracy.

1.5

The Need for Cold Atoms
It is already worth mentioning one important detail which needs to be addressed

for a high performance atomic clock: the Doppler effect. Almost anyone has experienced
a car drive by honking its horn. From this everyday experience, it is no surprise that thehorn frequency we hear is chirped as the car approaches or leaves. This Doppler effectis a consequence of the frequency (sound) source and observer originating from two
different reference frames, and can be calculated (to first order) with a simple Galileantransformation between the frames (to second order, a Lorentz transformation including
relativistic effects is required) [34]. The same holds true for an atom in motion: the atom
sees radiation which is frequency shifted from the laboratory frame. This can lead todephasing when probing the atomic transition of a large atom ensemble. Furthermore,it can lead to frequency shifts which depend on the geometry of the probing radiation
relative to the atomic motion. Since the Doppler effect scales with the relative velocity
between the atom and laboratory reference frame, the best way to reduce it is to slow theatom down. Laser cooling techniques have demonstrated their ability to reduce atomic
velocity from thermal sources with hundreds of m/s velocity to cm/s scale velocities [35].
As will be discussed in more detail, some caveats exist with respect to the importance of
the Doppler effect. Tightly trapped atoms can be excited with limited Doppler effects.
Nonetheless, most of the useful traps only have sufficient depth to trap laser cooled
atomic samples with low thermal energy. Furthermore, the recoil shift associated withthe absorption of a photon grows to a larger fraction of the transition frequency forincreasing transition frequency, making this shift more significant for optical transitions
than for microwave ones. For all of these reasons, development of state-of-the-art opticalfrequency standards currently requires the use of cold or ultracold atomic samples.

15

1.6

Precision Timing Applications
With the possibility that optical frequency standards could allow clocks to offer

10−18 timing accuracy and precision, one might naturally ask “Why do we need this?”.
Indeed, on the human timescale, such a clock would not help us arrive to an important
meeting any more promptly than a decent wristwatch. But high performance timekeeping is a powerful tool which finds many applications. Some of these applications
already require state-of-the-art technology and will directly benefit from improved primary frequency standards. Many other applications use more robust, proven clocks that
operate below state-of-the-art. But as the best clocks improve, the technology trickles
down to improve other clocks as well. To help motivate the need for more advanced
optical frequency standards, I list here some areas of application which benefit fromhigh performance timekeeping.
• global positioning system (GPS) [36]• computer network and electrical power grid synchronization• deep space navigation• radio telescopy (very long baseline interferometry)• definition of the SI second• measurement of other fundamental units (volt, ampere, ohm, meter)• tests of fundamental physics (time variation of fundamental constants, symmetry postulates, graininess of space)• geodesy (gravitational red shift)• secure communications [37]• tests of special and general relativity

16• gravitational wave detection and long baseline gravitational interferometry [38]• space clock missions [9, 39]

1.7

Thesis At-a-GlanceWith the basic concepts and motivation described in this introduction, I now

turn to the details. In Chapter 2, I describe the tools which were implemented toprepare and manipulate the Sr atomic sample for use in high accuracy spectroscopy.
This includes a general description of laser cooling techniques and our work on narrowline Doppler cooling. It describes atomic confinement in an optical lattice and resonant
laser interactions with confined atoms. I also describe the optical pumping techniques
we used for nuclear spin state preparation.
In Chapter 3, I describe the development of a highly stable, sub-Hz linewidth laser
source, a critical ingredient for high precision atomic spectroscopy. This leads to therealization of coherent atom-light interactions approaching the one second timescale. In
doing so, we report the observation of optical atomic spectra with 2 Hz linewidths.
Towards the development of an optical frequency standard based on 87 Sr, in
Chapter 4 I describe tools such as the optical frequency comb and precision frequency
references. Using these tools, we performed a spectroscopic evaluation of the Sr clocktransition, including several absolute frequency measurements.
In Chapter 5, I describe the current operation of the 87 Sr optical frequency standard at JILA. This system was carefully characterized via a remote optical comparisonof the Sr optical standard to other optical standards at the National Institute of Standards and Technology (NIST). A detailed description of the systematic shifts of theclock frequency is given, including the total systematic shift uncertainty of 1.5 × 10−16 .
Furthermore, an improved absolute frequency measurement of the Sr clock transition
was made with an uncertainty < 9 × 10−16 . Finally, I conclude by briefly considering

17
the future direction of ultracold strontium, both in the context of optical frequency
standards as well as other physical investigations.

Chapter 2

Atomic Manipulation and Control

As described in the introductory chapter, 87 Sr exhibits strong potential as an
optical frequency standard. As with any atomic system, that potential is not necessarily
achievable under the conditions that nature freely provides. In this chapter, I give a basic
introduction to the tools and techniques used for atomic manipulation, which prepare
Sr for use in a high accuracy optical frequency standard. I discuss Doppler laser coolingand trapping techniques in the broad and narrow line regimes, atomic confinement andinterrogation in optical potentials (such as optical lattices), and atomic state preparation
using optical pumping techniques.

2.1

Laser Cooling: Basic Concepts
Laser cooling has proven to be a rich and flexible tool. Much research has beensuccessfully dedicated to understanding and implementing a wide variety of laser coolingtechniques. The interested reader is referred to a few of the many well-written review
and research articles on the topic [35, 40, 41, 42, 43, 44, 45]. Here, I give a brief
conceptual introduction, after which I discuss how these techniques are implemented in
two different regimes in strontium: (1) a primary stage of traditional Doppler cooling topre-cool and collect an atomic sample at 1 mK from a hot, thermal beam source and (2)a secondary stage of narrow line Doppler cooling using the 1 S0 -3 P1 transition to reachphoton-recoil-limited temperatures below 1 µK. These techniques will be discussed first19
in a generic context, with broad applicability to 88 Sr. Later I will give details relevant
specifically to the 87 Sr case.
Like matter, light has both energy and momentum. The idea that light can beused to reduce the (thermal) kinetic energy of atoms can be broadly termed laser cooling.
The basic ideas behind laser cooling were first proposed independently by Hänsch andSchawlow [46] and Wineland and Dehmelt [47], both in 1975. The description andlanguage used in each proposal were distinct, the former lending itself more naturally
to cooling freely moving atoms and the latter to cooling atoms bound to an externalpotential. Nonetheless, the two proposals shared the same core principles, and thelaser cooling phenomenon they described can be qualitatively motivated by a simple
consideration of momentum and energy.
When an atom absorbs a photon of light, conservation of momentum dictatesthat the photon momentum, p~ph = ~~k, is absorbed by the atom. Here ~ is Planck’s
constant divided by 2π and ~k is the light wave vector, where |~k| = 2π/λ and λ is the
wavelength of the light. We consider the case where light illuminates an atom (forsimplicity, we assume an atom with two coupled internal states and mass, m) whose
velocity ~v is antiparallel to the light k-vector ~k. As the photon is absorbed, exciting theatom from the ground to the excited internal state, the atomic momentum is changed
from p~atom = m~v to p~atom = m~v + ~~k. Since ~k and ~v are antiparallel, this corresponds
to a reduction in the atomic momentum and velocity. When the atom relaxes fromthe excited to the ground internal state via spontaneous decay, a photon is re-emitted
and the atom experiences the corresponding momentum impulse from photon emission.
However, due to the isotropic decay process, the photon is emitted in a random direction,
and averaged over many decay events, the atom experiences a net zero momentum
change due to spontaneous emission (i. e. ~kemis averages to zero). In this way, repeatedphoton absorption-emission cycles reduce the atomic velocity ~v and cool the atom.
Due to the Doppler effect, radiation emerging from a laser in the laboratory-

20
stationary reference frame is seen by an atom in motion to have a frequency shift relative
to the laboratory frame. In the reference frame of the atom, we label the energy spacing
between the internal states of the atom as ~ω0 , where ω0 is the angular frequency of
the transition between the two states. Furthermore, we consider laser light which isessentially resonant with the internal transition of the atom in motion. In this case, thefrequency of the light absorbed (in the laboratory-stationary frame) is given by:2~kωabs = ω0 + ~k · ~v +
2m

(2.1)

The second term on the right hand side accounts for the Doppler shift between the moving atom and the stationary laboratory frames. The third term is the recoil frequency
which originates as a natural consequence of conservation of momentum and energy as
the atom takes up the photon momentum. Similarly, the photon frequency emitted by
the atom after internal relaxation is:2~kωemis = ω0 + k~0 · v~0 −
2m

(2.2)

Again, in the case of emission, averaging over the isotropic, random emission direction
results in the Doppler shift term in Equation 2.2 averaging to zero. Consequently, theaverage change in kinetic energy of the atom (the negative of the energy difference
between absorbed and emitted photons) is:2~k∆E = −~(ωabs − ωemis ) = ~k · ~v + 2
2m

(2.3)

2

With ~k · ~v < 0 (antiparallel) and |~k · ~v | > 2 ~k
2m (generally true for optical transitionsof non ultracold atoms), the kinetic energy of the atom is reduced (the atom is cooled)
and this energy is taken away by the photons.
This simple picture is particularly relevant for laser cooling an atomic beam froma hot thermal source. In practice, the frequency range over which proficient laser cooling
occurs is given by the linewidth of the cooling transition. For most of the transitions

21
used, this is on the order of MHz, corresponding to speeds of m/s. To cool a thermal beam source starting at velocities of hundreds of m/s, some mechanism must be
employed to maintain laser cooling efficacy after the Doppler shift experienced by thecooled atom is reduced by an amount comparable to the transition linewidth (where
photons would no longer be absorbed efficiently). Several approaches can be employed,
the most popular being a tapered magnetic field which generates a spatially dependent
Zeeman shift that compensates the change in Doppler shift as the atoms are slowed.
Once cooled to where the total remaining Doppler shift is close to the transition
linewidth, counterpropagating laser beams in each Cartesian dimension (red-detunedof the natural transition in the lab frame) can be utilized to further cool the atoms
three dimensionally. The atom sees light travelling against (with) its motion with ablue (red) Doppler shift. Since the laser light is red-detuned, the atom preferentiallyabsorbs the blue-Doppler shifted photons (travelling antiparallel to the atom) whichappear on resonance. Thus, whatever direction the atom travels, its motion will be
reduced (cooled). Its trajectory constantly changes as it absorbs photons from the 3pairs of orthogonal laser beams. It is straightforward to show (for the simplified 1-Dcase) that this effect results in a mean velocity-dependent cooling force which drives
the atomic velocity towards zero. However, the random absorption of a photon fromany direction by an atom at rest and the random emission direction of any emitted
photons result in velocity fluctuations which effectively heat the atom. This heatingcompetes with the mean cooling force, and the competition between the two yields thetemperature to which the atomic sample can be cooled [41]. The coldest temperatures
are obtained with laser light red-detuned from the atomic transition by one half thenatural linewidth, γ. This Doppler-cooling temperature limit is:
kB Tmin =

hγ
2

(2.4)

where kB is Boltzmann’s constant. Since the atom’s photon scattering rate is deter-22
mined by the relative size between the laser detuning (δ) and the natural transition
linewidth (γ), it is no surprise that the temperature limit corresponds to a thermalenergy approximately equal to the energy width of the transition.
The laser cooling described above can generate samples of millions or billions
of cold atoms. By providing a viscous force on the atoms, the laser fields have been
dubbed “optical molasses” [41, 35]. As the optical molasses yields only a velocitydependent force to damp atomic motion, the atoms are not truly trapped since no
critical spatially-dependent forces are present. To provide the necessary confinement,a spatially dependent magnetic field is introduced to complement the optical molasses.
In a direct analog to the velocity dependent Doppler shift, the spatially dependent
Zeeman shift pushes atoms toward the trap minimum [48]. Usually, the magnetic field isgenerated by a pair of anti-Helmholtz coils, which gives a zero magnetic field at the trap
center and a nonzero field away from the center which varies linearly with distance fromthe center. Optical molasses combined with this magnetic confinement is referred to asa magneto-optical trap (MOT), and was first demonstrated by Pritchard and Chu [49].
The MOT has emerged as an extremely powerful tool for the study and manipulationof neutral atoms, and is the starting point for a large subset of today’s experimental
studies in atomic physics. Several MOT configurations exist, using different atomic
transition types and different laser polarization. Furthermore, some atomic systems
lend themselves to additional cooling mechanisms which can generate temperatures
below the Doppler limit of a standard MOT. The broad field of laser cooling includes
a variety of cooling techniques such as polarization gradient cooling, Sisyphus cooling,cooling using velocity selective coherent population trapping, and Raman cooling (e. g.
[45, 50, 51, 52]).

23

2.2

Laser cooling strontium: 1 S0 -1 P1 MOT

2.2.1

Laser cooling properties of 1 S0 -1 P1 MOT

Figure 2.1 highlights the energy level structure of Sr relevant to laser coolingusing the 1 S0 -1 P1 dipole transition. The diagram does not show the hyperfine structure
relevant for 87 Sr, as this will be discussed later. Please refer back to Figure 1.2 fora more complete energy level diagram including other electronic states. The 1 S0 -1 P1transition has several characteristics which make it well-suited for cooling and trappingSr from a thermal source.
1. Dipole moment. Since laser cooling and trapping relies on atom-laser interaction, the dipole moment, d, of an atomic transition plays a key role in the laser coolingdynamics. The atom-laser dipole interaction strength is given by the Rabi frequency:Ω=~d~ · E~(2.5)

where E is the amplitude of the laser electric field. Conversely, the coupling between
the dipole moment and the vacuum field yields the spontaneous decay rate for thetransition:
Γ=

4α 3 2
2ω03
ω
|d|
=
|d|2
0
3e2 c26π0 ~c3(2.6)

where α ' 1/137 is the fine structure constant, c is the speed of light in vacuum, eis the electron charge, and 0 is the permittivity of free space. The solution to therate equations for a two level atom indicate that the absorption of near resonant laser
radiation, moving population between the ground and excited states, saturates whenthese two rates are approximately equal. In steady state, the excited state fraction,ρexc , is found to be:ρexc =1s
2 1 + s + 4 ∆22

(2.7)

Γ

Here ∆ = ωL − ω0 is the detuning of excitation laser from the atomic resonance, and s

24

3S
1

5s6s
1P
1

5s5p

1D
2

679
9e6

5s4d
461
1.9e8

707
4.6e7

6.5e3 1.9e3
3.9e3 6.6e2
5s5p
689
4.7e4

2
1
0

3P
J

5s2
1S
0
Figure 2.1: Abbreviated term diagram with states relevant for operation of the 1 S0 -1 P1
MOT. Arrows indicate the transitions, with their associated wavelength (in nm) anddecay rates (Einstein A coefficients in 1/s). Decay loss from the excited 1 P1 state isshown, as well as the transitions used to repump this population loss back to 1 S0 .

25
is the saturation parameter for the laser-atom interaction and is given by:
s=2

Ω2
Γ2

(2.8)

s can also be written in terms of the laser intensity, I, as s = I/Isat . Here, Isat is givenby:Isat =~2 c0 Γ2.
2 |d|2(2.9)

A plot of Equation 2.7 is shown in Figure 2.2 as a function of the saturation
parameter s. Note that when s ' 1 (Ω2 ' Γ2 ), ρexc begins to saturate to the steady state
limit of 1/2. This places a key limitation on laser cooling and trapping performance.
Since laser cooling requires many repeated cycles of photon absorption and spontaneousemission, the fastest rate at which the atomic momentum can be reduced by a photon
recoil ~k is Γρexc (maximizing to Γ/2). This is equivalent to saying that the maximum
deceleration possible from laser cooling using a transition with decay rate Γ is:amax =~kΓ.
2m(2.10)For the 1 S0 -1 P1 transition, amax ' 106 m/s2 . This has important implications for bothslowing the atoms from a thermal source as well as loading them into a MOT. The
temperature of a thermal beam source is primarily constrained by the need for sufficient
atom beam flux (higher temperature = higher vapor pressure = higher flux). Of course,
higher temperatures also yield higher initial velocities, and this initial velocity andamax determine the minimum length over which the atoms must travel to be slowed
to near rest (∆x = v0 t + 1/2at2 and ∆v = at). For a typical atomic velocity of 500
m/s, approximately 12 cm is required to slow the Sr atomic beam using the 1 S0 -1 P1transition. Transitions with weaker dipole moments (and hence smaller decay rates)
would require longer slowing paths, experimentally complicating the process. Note alsothat longer slowing paths typically mean lower atom beam flux, due to loss of atoms
from atomic motion perpendicular to the beam axis.

26

ρexc

0.1

0.01
0.01

0.1

1

10

100

s (saturation parameter)
Figure 2.2: Excitation fraction, ρexc , as a function of saturation parameter, s, for a
two level atom in steady state. The excited state fraction saturates to one half arounds ' 1.

27
For efficient loading of atoms from a slowed beam into a MOT, the capture velocityof the MOT can be estimated as [53]:
vc =

√

arc

(2.11)

where rc is the capture radius of the trap, typically set by the radii of the trapping/cooling lasers. Using the 1 S0 -1 P1 transition and with rc = 1 cm, vc can be as
much as 100 m/s, a healthy capture velocity for robust trapping of large atom number.
It is important to remember that a tradeoff exists in the laser cooling process dueto the transition linewidth. Although a large transition linewidth can experimentally
facilitate the cooling and trapping process as described above, this also results in higher
temperatures (see Equation 2.4). A good deal of experimental work requires ultracold,µK atomic temperatures. Although the 1 S0 -1 P1 Doppler limit is a relatively warm 770µK, this temperature is small enough to conveniently and efficiently load the atoms
into a secondary MOT using the 1 S0 -3 P1 transition where much colder temperatures
are achievable. In this way, the 1 S0 -1 P1 MOT serves as means to collect and pre-coollarge Sr samples, readying them for further cooling.
2. Closed transition. The discussion in Section 2.1 assumed an ideal atom with
only two levels. A realistic many-level atom usually has a rich network of couplings
among its internal states. In some cases, two levels can behave nearly isolated fromthe remainder, approximating a two-level system. This is the case for the 1 S0 -1 P1transition in Sr. Atoms excited from the ground 1 S0 state to the 1 P1 state decay nearlycompletely back to 1 S0 . A weak decay channel exists from 1 P1 to 1 D2 (Γ = 3.9 × 103s−1 ), where decay continues to the 3 P1 and 3 P2 states with a branching ratio of 2/3 and1/3 respectively. Atoms falling to the 3 P1 state further decay back to the ground 1 S0state, and so are able to continue the 1 S0 -1 P1 laser cooling process. 3 P2 is a metastablestate (lifetime, τ = 1/A = 500 s) and so atoms that decay here are lost from the 1 S0 -1 P1
MOT. Fortunately, this loss rate (1/3 × 3.9 × 103 = 1.3 × 103 s−1 ) is much smaller than

28
the 1 P1 spontaneous decay rate to 1 S0 (A = 2.1 × 108 s−1 ). As a consequence, theMOT can operate without the assistance of any extra lasers to “repump” atoms fromthe loss channels back to the laser cooling states. This is in contrast to alkali atom
MOTs, which require a repump laser for operation.
Nonetheless, the Sr MOT atom number is enhanced when introducing extra lasers
to pump 3 P2 population back to 1 S0 . Several repumping schemes are feasible [54].
We accomplish this task with two lasers (refer to Figure 2.1). The first, at 707 nm,
resonantly pumps 3 P2 to 3 S1 . From here, decay occurs to 3 P2 , 3 P1 , and 3 P0 with
branching ratios of 5/9, 3/9, and 1/9, respectively. Population decay to 3 P2 is simply
excited to 3 S1 again via the 707 nm repump laser. Population decay to 3 P1 subsequently
decays further to 1 S0 for more MOT cycling. Decay to 3 P0 remains stuck there (τ =150 s for 87 Sr and thousands of years for 88 Sr) and so requires application of a second
repump laser at 679 nm, which pumps the 3 P0 population back to 3 S1 . In this way, alllost population is eventually returned to 1 S0 via 3 P1 . Experimentally, the presence ofrepump lasers can enhance the MOT atom number by more than an order of magnitude.
3. J to J+1 transition. Pure Doppler cooling (optical molasses) exploits the signof the Doppler shift (blue shift for ~v antiparallel to ~k and red shift for ~v parallel to~k) to favor photon absorption from the counterpropogating direction to slow (rather
than heat) the atoms. The spatial confinement added in a MOT exploits the spatiallydependent Zeeman shift of the atomic states. Consider an atom which is located 1 mm
to the right side of the MOT trap center. Absorption of a photon coming in from theright side will give the atom recoil which will push it to the left towards the trap center.
However, to successfully trap the atoms, the atom must preferentially absorb a photon
from the right rather than from the left, as one from the left would push it further
away from the trap center. This is accomplished by optical polarization and the use of
two magnetic states with equal but opposite Zeeman shifts (mJ = ±1, refer to Figure2.3). Counterpropogating laser beams have opposite polarization with respect to the29

Energy

B
σ+

mJ=+1

σ-

-1

0

+1

mJ=-1
Figure 2.3: The combination of σ + and σ − light with a magnetic field to provide spatialconfinement using a J = 0 - J = 1 laser cooling transition. The Zeeman shift of themF = ±1 states permit preferential absorption of the polarized light field, pushing theatom towards the trap center.

atomic quantization axis. The σ − polarized light coming in from the right side can drive
transitions from 1 S0 mJ = 0 to 1 P1 mJ = −1 and the σ + polarized light coming in fromthe left side can drive transitions from 1 S0 mJ = 0 to 1 P1 mJ = +1. The red-detuned
laser light, however, is only resonant with the mJ = 0 - mJ = −1 transition becauseof the negative Zeeman shift of the mJ = −1 state from the (positive) B-field aligned
along the quantization axis. Thus absorption is preferentially made by the photons
from the right, pushing the atom back towards the trap center. The same is true for an
atom to the left of the trap center absorbing the photon from the left. The J = 0 to
J = 1 transition is the simplest transition in the J to J + 1 family which facilitates thispolarization and Zeeman shift dependent absorption for successful spatial confinement.
With a single magnetic sublevel, the J = 0 ground state is optimal for efficient Doppler
cooling since population does not undesirably decay to unwanted substates.

2.2.2

Experimental details of the 1 S0 -1 P1 MOT

The general schematic of the experimental apparatus used to laser cool and trap
strontium (with emphasis on the 1 S0 -1 P1 MOT) is given in Figure 2.4. We use a30Transverse
Cooling

20 cm

M

Approximate Scale

(b)

λ/4
40 l/sIon Pump

NI

Gate
Valve

Atomic Beam OvenCC
Slower
Cooling
Laser

SlowerTo Roughing
Pumps

ChopperBA

Window
Heater

DBS
NI
TSP

BS
PBS

To Roughing
Pumps

λ/2

SMPM Optical Fiber

Figure 2.4: Schematic of the experimental apparatus for cooling and trapping strontium.
From the oven, the thermal atomic beam traverses a collimator, the transverse coolingstage, a mechanical shutter used to chop the atomic beam, a gave valve, a differential
vacuum tube, and the Zeeman slower region. It then travels to the main vacuum
chamber for collection in the MOT. The laser light for the 1 S0 -1 P1 MOT (461 nm) andthe 1 S0 -3 P1 MOT are combined with a dichroic mirror before entering the chamber. The
repump lasers (679 and 707 nm) are either stabilized to a reference cavity (as shownhere) or strongly frequency modulated. TSP: titanium sublimation pump, BA: BayardAlpert vacuum gauge, DBS: dichroic beam splitter, BS: beam splitter, PBS: polarizing
beam splitter, ECDL: external cavity diode laser, SMPM: single mode polarization
maintaining, M: mirror, NI: nude vacuum gauge, CC: compensation coil

31standard six-beam (3 retroreflected beams) 461 nm 1 S0 -1 P1 MOT that is loaded by a
Zeeman slowed and transversely cooled atomic beam. The atomic beam is generated byan effusion oven (2 mm nozzle diameter) whose output is angularly filtered by a 3.6 mm
diameter aperture located 19.4 cm from the oven nozzle. Separate heaters maintainthe oven body (nozzle) at 575 o C (850 o C). The vapor pressure of Sr as a functionof temperature is given in [55]. We have previously measured the atomic beam flux
(divergence half-angle) to be approximately 3×1011 atoms/s (19 mrad) after the filtering
aperture. The atomic beam is then transversely cooled by 2-dimensional 461 nm opticalmolasses. This laser beam, as well as the trapping and slowing beams described below,
all have active intensity stabilization. Furthermore, the transverse cooling and trapping
beams are mode filtered by transmission through a single mode optical fiber (before theintensity stabilization detector). Using cylindrical lenses, the transverse cooling beamis given an elliptical cross-section. These linearly polarized molasses laser beams havea 1/e2 diameter of ∼ 3 cm (∼ 4 mm) along (normal to) the atomic beam propagation
axis, contain 10 - 20 mW of power, and are detuned from the 1 S0 -1 P1 resonance by -10
to -15 MHz. Stray magnetic fields in the transverse cooling region are less than 1 G.
After the transverse cooling region, the atomic beam passes through a 6.4 mm diameterelectro-mechanical shutter and a gate valve that allows the oven to be isolated from therest of the vacuum system.
The atomic beam then enters a water cooled 20 cm long constant deceleration
σ − Zeeman slower [56] with a peak magnetic field of ∼ 600 G, corresponding to acapture velocity of ∼ 500 m/s. The 461 nm Zeeman slowing laser is detuned from the
1 S -1 P resonance by -1030 MHz, contains roughly 60 mW of power, and is focused0
1

to approximately match the atomic beam divergence (although we have seen similar
performance from a small, collimated beam). The window opposite the atomic beam
is a z-cut Sapphire optical flat that is vacuum sealed via the Kasevich technique [57],broadband anti-reflection coated on the side opposite the chamber, and heated to 200 o C

32
to prevent the formation of Sr coatings. The alternating current (ac) window heater,which produces a small stray magnetic field, is only operated during the 1 S0 - 1 P1
MOT pre-cooling phase. A separate compensation coil reduces the slower magnetic
field magnitude (gradient) to < 100 mG (< 8 mG/cm) at the trapping region, located
15 cm from the slower exit. Stray magnetic fields at the trap can be further nulled bythree sets of orthogonally oriented Helmholtz coil pairs.
The trapping chamber is a cylindrical octagon with six 2 3/4” (two 6”) ports
in the horizontal x-y plane (along gravity z-axis). All windows are broadband antireflection coated. The MOT anti-Helmholtz coils, oriented such that the axial magnetic
field gradient dBz /dz lies along gravity, are mounted on a computer controlled precisionlinear track that allows the coil center to be translated from the trapping chamber to a 1
cm × 1 cm × 4 cm rectangular glass cell. The coils are constructed to provide windowlimited optical access to the geometric center of the trapping chamber and produce
axial gradients of 0.819 G/(cm-A). They are made by winding Kapton-insulated copper
tubing with a square cross section (width ' .41 cm) and a hollow core. The hollow
core enables internal water cooling to remove the heat generated from the current flow
(typically 61 A). The gradient is linear over a spatial range of ± 3 cm in both the axial
and transverse directions. Current in the coils is regulated by a computer controlled
servo and monitored with a Hall probe. For the 1 S0 - 1 P1 MOT, the axial magnetic
field gradient dBz /dz = 50 G/cm.
The trapping and oven chambers are each evacuated by a 40 l/s ion pump and atitanium sublimation pump. The two chambers are separated by a 6.4 mm diameter ×
16 mm long cylindrical differential pumping tube located between the electro-mechanicalshutter and the gate valve. Typical vacuum levels in the oven, trapping, and glass cellchambers during operation of the atomic beam are 2×10−8 Torr, 1.5×10−9 Torr, and3×10−10 Torr, respectively.
461 nm cooling and trapping light is produced by frequency doubling the optical-

33
fiber-filtered-output of a tapered diode MOPA (Master Oscillator Power Amplifier)amplifier (Eagleyard Photonics) at 922 nm (we have previously used a single mode
Ti:Sapphire ring laser with intracavity optical diode, birefringent filter, and dual etalonsinstead of this diode system). This amplifier (which outputs 1.5 W, giving 1 W after
the optical fiber) is seeded by an external cavity diode laser (ECDL) (seeding power ∼45 mW). Although the polarization-maintaining optical fiber acts as a Gaussian mode
filter, the high intensity injected into the fiber seems to induce polarization rotation
which occasionally occurs on relatively short time scales (mrad in minutes or less).
Future design could benefit from the use of large-core single mode fiber which tolerates
higher input powers. The frequency doubling occurs by splitting the 922 nm light(approximately 2/3 and 1/3) and injecting the two beams into two external buildup
cavities with intracavity nonlinear crystals[58]. Together, these cavities produce > 250
mW of single-mode light at 461 nm. We chose these short standing wave buildup
cavities (input coupler R > 95% at 922nm, back side of crystal HR at 922 nm), together
with a temperature phase matched (150 o C) KNbO3 nonlinear crystal (high nonlinear
coefficients), because of the very high second harmonic conversion efficiency that could
be achieved (typical 50%, best 60%). We could not achieve these same efficiencies withlonger running wave bow-tie cavities. The motivation for splitting the light into two
cavities was rooted in thermally-induced instability which developed when the generated
461 nm light exceeded ∼175 mW. This thermal effect led to non-Gaussian transverse
mode features (ring structures) that were temperature and phase-matching dependent,
and which limited the amount of useful 461 nm power.
The resulting 461 nm light is then offset locked to the 1 S0 - 1 P1 resonance by
saturated absorption feedback to the ECDL seed laser at 922 nm (laser piezo-electrictransducer, PZT). The saturated absorption spectrometer utilizes a commercially available “see-through” Sr hollow cathode lamp (Hamamatsu). The probe beam is phasemodulated by an electro-optic modulator (EOM), and the pump beam is amplitude

34
modulated by an acousto-optic modulator (AOM). The probe absorption signal thenundergoes two stages of phase-sensitive demodulation to recover the dispersion shaped
signal used for stabilizing the 922 nm laser. Relative frequencies of the transverse
cooling, Zeeman slower, and trapping laser beams are controlled with acousto-optic
modulators (AOMs) which are also used as shutters. Additional extinction of 461 nm
light is provided by mechanical shutters. The intensity stabilized trapping beams have
1/e2 diameters of ∼ 3 cm, are detuned from the 1 S0 -1 P1 resonance by -40 MHz, andtypically have a combined one way power of 30 mW (all three dimensions are retroreflected). For these settings, we find the 1 S0 -1 P1 MOT population is maximized. Further
increases in, for example, the trapping beam power usually only increase the cloud temperature. 1 S0 -1 P1 MOTs are monitored with a charge-coupled-device (CCD) camera
and a calibrated photodiode. Typical trap lifetimes, populations, and temperatures are
20 ms, 3×107 , and 2.5 mK, respectively (without repumping). The atom population
is determined by collecting 461 nm fluorescence from the MOT. This fluorescence iscollected with a 2” lens located 15 cm from the MOT atoms and focused on a calibrated
photodiode. The photon scattering rate is determined either by empirical measure of
the incident trapping laser intensities or directly by the MOT lifetime in the absence ofrepumping [59].
Operation of the 1 S0 -1 P1 MOT efficiently populates the ground-state-like 3 P2
metastable excited-state (see Figure 2.1, ∼ 500 s radiative lifetime [60, 61]) via 1 P1 →
1D

2 →

3P

2 radiative decay.

Consequently, 1 S0 -1 P1 MOT loading times are typicallylimited to 10 - 50 ms [62, 63, 59]. As described in Section 2.2.1, this is overcome by
applying repumping lasers at 707 nm and 679 nm to optically pump this population
to 3 P1 where atomic decay returns it to 1 S0 . These two ECDLs have been operated
in two modes. In the first mode, typically used for 88 Sr, each laser is locked to a reference cavity that is simultaneously locked to a frequency stabilized helium neon laser
utilizing an intracavity iodine cell for stabilization. Double-passed AOMs are then used35
to tune the absolute laser frequencies to the atomic transitions. In a second scheme,
more recently used with 87 Sr, the lasers not locked to stabilization cavities but are
instead strongly frequency modulated by application of a sawtooth waveform to theirdrive current and intracavity laser piezo transducer (PZT). The center frequency andmodulation depth and frequency are empirically tuned to optimize MOT size. The
modulation approach seems particularly useful for 87 Sr, which possesses a large numberof nondegenerate hyperfine states which can become populated during optical pumping
or re-pumping. After passing through a single-mode polarization-maintaining opticalfiber, the co-propagating 707 nm and 679 nm laser beams are expanded to a 1/e2 intensity diameter of ∼ 1 cm and delivered to the 1 S0 - 1 P1 MOT. An AOM and mechanicalshutter located before the beam expansion optics allows for rapid and complete intensity extinction (< 1 µs transition time with AOM). At the trap, the 707 nm (679 nm)
beam contains ∼ 1 mW (∼ 2.5 mW) of power, resulting in an optical re-pumping timeof < 100 µs. With both lasers operating, the 1 S0 -1 P1 MOT population and lifetime are
typically enhanced by 10× and 15×, respectively.
It should be noted that along with contributing to 1 S0 -1 P1 MOT loss, 1 P1 → 1 D2
→ 3 P2 radiative decay continuously loads mK atoms in the 3 P2 (mJ = 1,2) states into amagnetic trap formed by the 1 S0 - 1 P1 MOT quadrupole magnetic field [59, 64, 65, 66].
Importantly, these samples are expected to display a wealth of binary collision resonances that arise due to an interplay between anisotropic quadrupole interactions andthe local magnetic field [67, 68, 69]. Qualitatively similar processes and hence, collision resonances, are predicted for polar molecules immersed in electrostatic fields [70].
Studies of metastable Sr collision dynamics will thus likely impact the understandingof a diverse range of physical systems. To pursue these studies, the trapping apparatus was designed to first load 3 P2 state atoms into the quadrupole magnetic trap andthen mechanically translate [71] the sample to the glass cell chamber. Subsequently,
a tight Ioffe-Pritchard magnetic trap could be used to perform a variety of collision

36
experiments.

Laser cooling strontium: Narrow line laser cooling in the 1 S0 -3 P1

2.3

MOT
The 1 S0 -1 P1 MOT described above conveniently cools and traps Sr at mK temperatures. Unfortunately, this temperature still corresponds to an rms (root-mean-squared)
velocity of 50 cm/s. The Doppler effect resulting from a gaussian velocity distribution
with vrms = 50 cm/s yields a Doppler broadened, spectroscopic profile of 1 MHz. This
would make observation and precise measurement of the very narrow clock transitiondifficult. Still colder temperatures are required to reduce this effect, which scales withthe square root of the temperature. In addition, ultimately tight atomic confinement
is desired for probing the clock transition. Because this confinement is achieved withthe relatively weak interaction of a laser intensity gradient with the induced atomic
dipole polarizability, colder atoms relax the laser intensities required for trap depths
which exceed the atom thermal energy. Although 88 Sr lacks the ground state substructure for sub-Doppler cooling mechanisms, the relatively weak 1 S0 -3 P1 intercombinationtransition is well-suited to Doppler cooling and has a low Doppler limit of T= 200 nK.
Laser cooling on this transition explores the novel regime where the transition linewidth(γ = 7.6 kHz) is similar to the atomic recoil frequency (ωr /2π = 4.7 kHz), hence thename narrow line cooling.

2.3.1

Narrow line laser cooling dynamics

Fully understanding narrow line laser cooling requires first clarifying the difference between broad and narrow Doppler cooling lines. Broad lines, historically used forthe vast majority of laser cooling experiments [44], are defined by Γ/ωr >> 1. The 461
nm 88 Sr 1 S0 - 1 P1 transition shown in Fig. 1(a), which typifies a broad line, has, for example, Γ/ωr ∼ 3×103 . In this case, Γ, or more generally the power-broadened linewidth37√ΓE , is the natural energy scale. Here, ΓE = Γ 1 + s is defined by the saturation parameter s = I/IS where I (IS ) is the single-beam peak intensity (transition saturation
intensity). Semiclassical physics thus governs the cooling process and the photon recoil, although essential to quantitatively understanding energy dissipation [43], serves
more as a useful conceptual tool than a dominant player in system dynamics. Moreover, gravity is essentially negligible since the ratio of the maximum radiative force tothe gravitational force, R = ~kΓ/2mg, is typically on the order of 105 , where g is thegravitational acceleration.
In contrast, narrow Doppler cooling lines are characterized by Γ/ωr ∼ 1. The 689
nm 88 Sr 1 S0 - 3 P1 transition used in this work, for example, has Γ/ωr = 1.6 where Γ/2π
(ωr /2π = ~k 2 /4πm) is 7.5 kHz (4.7 kHz). In this case, the relevant thermal-mechanicalenergy scale and thus the underlying semiclassical or quantum mechanical nature of
the cooling depends on s. Details of a given cooling process are then set by the laser
detuning 2πδ = ∆ = ωL −ωA where ωL (ωA ) is the laser (atomic resonance) frequency. In
particular, δ < 0 1 S0 -3 P1 MOT cooling and trapping dynamics can be divided into three
qualitatively distinct regimes, hereafter labelled (I - III), defined by the relative size of|∆|, Γ ∼ ωr , and ΓE . In regime (III), corresponding to trapping beam intensities on theorder of IS = 3µW/cm2 or s ∼ 1 (ΓE ∼ ωr ), ωr is the natural energy scale. Here, single
photon recoils and consequently, quantum physics, govern trap dynamics. Temperatures
as low as roughly half the photon recoil limit (Tr = 2~ωr /kB = 460 nK) are possible
despite the incoherent excitation provided by the trapping beams [72, 42, 73].
Conversely, for s  1 the system evolves toward semiclassical physics where ΓE 
ωr and hence ΓE is the dominant energy scale. In this case, cooling and motional dynamics are determined by the relative size of ΓE and ∆. In regime (II), the ∆ < ΓE radiative
force produces damped harmonic motion and, in analogy to standard Doppler cooling,
MOT thermodynamics set entirely by the velocity dependence of the force [41, 74]. For
these conditions, the expected δ- and s-dependent temperature minima are observed,

38
although with values globally smaller than standard Doppler theory predictions. Alternatively, in regime (I) where ∆ > ΓE , the atom-light interaction is dominated bysingle-beam photon scattering and trap thermodynamics become intimately linked toboth the velocity and the spatial dependence of the force. Here, gravity plays an essential role as the ratio R for the 1 S0 - 3 P1 transition is only ∼ 16. Consequently, the atoms
sag to vertical positions where the Zeeman shift balances ∆, leading to ∆-independentequilibrium temperatures.
More insight into regime (I) and (II) thermal-mechanical dynamics is provided
by the semiclassical radiative force equation [41]F~ (~v , ~x) =
−

~~kΓ
s
[
~
2 1 + s0 + 4(∆ − ~k · ~v − µdB/dx· ~x)2 /Γ2
s
]
~
0
~
1 + s + 4(∆ + k · ~v + µdB/dx· ~x)2 /Γ2− m~g .

(2.12)~ = {dBx , dBy , dBz }, and µ = (gJ µB /~) where gJ = 1.5 iswhere ~x = {x, y, z}, dB
the 3 P1 state Lande g-factor and µB is the Bohr magneton. The parameter s0 > saccounts, along a single axis, for saturation induced by the remaining four trapping
beams. Figure 2.5(a) shows the 1 S0 - 3 P1 radiative force at s = s0 = 248 for a rangeof δ values while Figure 2.6(a) shows the force at δ = -520 kHz for a range of s = s0
values. As described earlier, the qualitative nature of the force and hence the resulting
trap mechanical dynamics depends on the relative size of ∆ and ΓE . For regime (I),corresponding to |δ| > 120 kHz in Figure 2.5 or s < 248 in Figure 2.6, ∆ > ΓE and the
3D radiative force acts only along a thin shell volume marking the outer trap boundary.
Here, the trap boundary roughly corresponds to positions where the radiative force ispeaked. This situation, as shown by Figures 2.5 and 2.6, produces a box potential with agravitationally induced z-axis tilt. Hence, in the x-y plane, motion consists of free-flightbetween hard wall boundaries while along the z-axis, mechanical dynamics are set by
the relative size of the radiative force “kicks,” gravity, and the cloud thermal energy.

39vX ( or vY ) (m/s)
0-2δ (kHz)2
10-1-2 (a)
-3

K)

0

3 (b)

2

-23

N)

-120
-800
-1800
-2800

PE (x102

Force (1020x (or y) Position (mm)

3

-1.5

0.0
1.5
z Position (mm)(c)
δ = -120 kHz

δ = -800 kHz

δ = -1800 kHz

δ = -2800 kHzg
5.6 mmFigure 2.5: (a) Semiclassical radiative force versus position (bottom axis, vx = vy =0) and velocity (upper axis, x=y=0) for different detunings. The corresponding trap
potential energy in the z direction (b) and in situ images of the 1 S0 -3 P1 MOT (c).
Dashed lines in (c) are calculated maximum force contours (with s =248).

40vX ( or vY ) (m/s)-101s = 33s = 248s = 1800
s = 9120

2

0

3

0

-2 (a)
-2

(b)

K)

6

PE (x10Force (10

-23

N)

2

0
2
x (or y) Position (mm)-101
z Position (mm)(c)
s = 248s = 33s = 1800

s = 9120g
3.0 mmFigure 2.6: (a) Semiclassical radiative force versus position (bottom axis, vx = vy = 0)
and velocity (upper axis, x = y = 0) for different intensities. The corresponding trap
potential energy in the z direction (b) and in situ images of the 1 S0 -3 P1 MOT (c).
Dashed lines in (c) are calculated maximum force contours. For each, δ = −520 kHz.

41
The thermal energy is small compared to the gravitational potential energy. Moreover,
the ratio of the maximum radiative force to the gravitational force is R ∼ 16. Thus, theatoms sink to the bottom of the trap where they interact, along the z-axis, with only
the upward propagating trapping beam.
As δ decreases in Figure 2.5(a) or s increases in Figure 2.6(a), the trap mechanically evolves to regime (II) where ∆ < ΓE produces a linear restoring force and hence,
damped harmonic motion [41, 74]. Consequently the trap potential energy assumes the
U-shaped form familiar from standard broad line Doppler cooling. As the trap moves
more fully into regime (II), perturbations to the potential energy due to gravity becomeless pronounced. One expects, therefore, that the cloud aspect ratio will evolve towardthe 2:1 value set by the quadrupole magnetic field.
The intuitive descriptions developed above are directly confirmed by Figures2.5(c) and 2.6(c) which show in-situ images of the 1 S0 - 3 P1 MOT along with overlaid maximum force contours calculated from Equation 2.12. For excitation conditions
corresponding to regime (II), the cloud approaches the 2:1 quadrupole magnetic field
aspect ratio. In contrast, for regime (I) the cloud x-y width is determined largely by
the separation between x-y force maxima or alternatively, by the wall separation for thex-y potential energy box. In the vertical direction, the atoms sink to the bottom of thetrap where the lower cloud boundary z0 is defined by the location of the z-axis potential
energy minima which is, in turn, proportional to the position where the Zeeman shift
matches the laser detuning. As δ increases, z0 shifts vertically downward, an effectpredicted in Figure 2.5(b) and clearly revealed in Figure 2.5(c).
MOTs using the 1 S0 - 3 P1 transition display a rich variety of thermodynamic
behaviors that are directly linked to the mechanical dynamics explored in section IV.
Figure 2.7 shows the MOT equilibrium temperature TM versus δ for saturation parameters ranging from s = 7.5 to s = 1800. For large δ and s, corresponding to regime(I) where ∆ > ΓE  Γ, TM is basically δ-independent. Recall that for ∆ > ΓE , the

42

10
8
6
4
2

DT x 0.48

Doppler Theory
10

DT x 0.24

hΓE
2kB
1

0.6

2hωR/kB

0.4

s = 1800
s = 248s = 7.5(a)0

1
2
Detuning (-MHz)

Regime (II)
1.0

(I)

(b)

0.1
2

0

10

(III)

4

10
Intensity (I/IS)

10

(I)

(II)

(c)

0.5

0.0
1
10

3

2
10
10
Intensity (I/IS)

4

10

Figure 2.7: 1 S0 -3 P1 MOT temperature versus (a) detuning (δ) for various intensitiesand (b) intensity (s) at δ = −520 kHz. In (a), DT is standard Doppler theory. In (b),solid circles are experimental data while the solid, dashed, and short dashed lines givestandard Doppler theory, the Doppler limit ~Γ/2kb , and the single-photon recoil limit
2~ωr /kb , respectively. (c) Global scaling factor applied to Doppler theory in order tomatch regime (II) data versus intensity.

43
cloud sags to the bottom of the trap where interactions occur, along the vertical zaxis, with only the upward propagating trapping beam. Moreover, due to polarizationconsiderations and the free-flight motion executed by atoms in the horizontal plane,
horizontal beam absorption rates are more than 4× smaller than the vertical rate. Trap
thermodynamics, therefore, are dominated by a balance between gravity and the radiative force due to the upward propagating beam. Here, it is important to realize thatas δ changes, the z-axis atomic position z0 self adjusts such that the effective detuning, ∆ - µ(dBz /dz)z0 , remains constant. Consequently the trap damping and diffusion
coefficients, and thus the equilibrium temperature, remain constant.
To obtain a quantitative expression for TM under these conditions, we first findthe damping coefficient α by Taylor expanding the semiclassical force expression
F (vz , z) =

~kΓ 

2 


s

2
4(∆
−
kv
−
µ(dB
/dz)z)zz
1 + s0 +Γ2− mg.

(2.13)

where (∂F /∂v) = α is evaluated at vz = 0, z = z0 . Solving F (0, z0 ) = 0 and using R =(~kΓ/2mg), the δ-independent effective detuning is given by√
Rs − s0 − 1∆ − µ(dBz /dz)z=−Γ
2(2.14)

which, in combination with Equation 2.13, states that the scattering rate depends only
on R, s, and Γ. Substituting this expression into (∂F /∂v), we obtain the damping
coefficient√2~k 2 Rs − s0 − 1
α=−
R2 s

(2.15)

Next, the diffusion coefficient Dp is calculated by substituting Equation 2.14 into thesingle-beam scattering rate. Dp is then given byDp =~2 k 2 Γ
2R(2.16)

44
Combining Equations 2.15 and 2.16, the predicted δ-independent equilibrium temperature is
T =where we have used

Dp
|α|

√
R
~Γ s
p
2kB 2 R − s0 /s − 1/s


~ΓE
=
NR
2kB
=

(2.17)√√s ∼ s + 1 for s  1. The numerical factor NR is approximately 2over the entire relevant experimental range. Regime (I) temperatures, therefore, depend
only on ΓE . To test this prediction, Figure 2.7(b) shows TM versus s for a fixed large
detuning δ = -520 kHz. For the central portion of the plot where regime (I) dynamics
are relevant, we find good agreement with Equation 2.17 aside from a global scaling
factor of two.
For small δ in Figure 2.7(a), the system evolves from regime (I) to regime (II)where ∆ < ΓE , ΓE  Γ. As this transition occurs, trap dynamics change from free-flightto damped harmonic motion. Here, one expects thermodynamics similar to ordinary
Doppler cooling including δ- and s-dependent minima with equilibrium values having
the functional form [41, 74]
T (s, ∆) = T0

ΓE 
1 + 4(∆/ΓE )2
4|∆|

T0 = (~ΓE )/(2kB )(2.18)

where T0 , realized at ∆ = ΓE /2, is a generalized version of the s  1 Doppler limit.
As shown by the solid lines in Figure 2.7(a), Equation3 2.18 correctly reproduces thefunctional shape of the data. As shown by Figure 2.7(c), however, matching the absolutedata values requires multiplying Equation 2.18 by a s-dependent global scaling factor(≤ 1) whose value decreases with s, leading to temperatures well below the standard
Doppler limit T0 . In contrast to ordinary Doppler cooling, the cloud thermal energy inregime (II) is thus not limited by half the effective energy width of the cooling transition.
Notably, we find this surprising result cannot be explained either by analytic treatments

45
of Equation 2.12 or semiclassical Monte-Carlo simulations of the cooling process. The
Monte-Carlo simulations, in fact, simply reproduce standard Doppler theory. Finally,as s approaches unity in Figure 2.7, the trap enters regime (III) where Γ ∼ ωr ∼ kB T/~
and thus the cooling becomes fully quantum mechanical. Here, we obtain a minimum
temperature of 250(20) nK, in good agreement with the quantum mechanically predictedvalue of half the photon recoil temperature TR /2 = ~ωr /kB = 230 nK [42]. For more
information on the dynamical approach to equilibrium, as well as novel heating dynamics
for δ > 0, see [75, 76].

2.3.2

Experimental details of the 1 S0 -3 P1 MOT

Exploring 689 nm 1 S0 -3 P1 narrow line cooling dynamics requires a laser system
whose short-term linewidth is small compared to the 7.5 kHz transition natural width.
In addition, the absolute laser frequency must be referenced, with similar stability, tothe 1 S0 -3 P1 transition and be tunable over a range of ∼ 10 MHz. The 689 nm laser stabilization and control system consists of a master ECDL, a temperature stabilized andvibration isolated passive optical reference cavity, a Sr saturated absorption spectrometer, and two slave ECDLs phase locked at an offset frequency from the master laser. For
88 Sr, having two slave ECDLs is unnecessary, and we have previously operated the mas-ter as a seeding laser to injection lock a single second laser. In this approach, the masterwas stabilized to the cavity (at short time scales) and the Sr spectrometer (at longer
time scales) and the injected laser simply acted as an amplifier to give sufficient output
power for the 1 S0 -3 P1 MOT operation. However, as described in the next section, the87 Sr MOT requires two 689 nm lasers. To facilitate fast switching between trapping of
87 Sr and 88 Sr, we implemented the offset frequency locking of the two ECDLs.

The linewidth of the master ECDL is first narrowed by locking the laser to astable optical reference cavity via the Pound-Drever-Hall technique [77]. The cavity
consists of high reflectivity Zerodur substrate mirrors that are optically contacted to46
a Zerodur spacer. The measured cavity finesse (free spectral range) at 689 nm is ∼3800 (488.9 MHz), giving a linewidth for the TEM00 mode of ∼ 130 kHz. To isolate
the cavity from environmental perturbations, the cavity is suspended by two thin wires
inside a temperature stabilized can that is evacuated to < 10−6 Torr and mounted onvibration damping material. The 689 laser light is made resonant with the cavity modeby use of a double-passed 1 GHz AOM. The electronic feedback for laser stabilization
has a bandwidth of ∼ 2 MHz, and is divided between a slow loop that adjusts thepiezo-electric mounted ECDL grating and a fast loop to the diode laser current. With
the cavity lock engaged, in-loop analysis shows that jitter in the cavity-laser lock is <1 Hz.
To further evaluate the performance of the 689 nm laser system, the short-term
laser linewidth is determined by beating the cavity-locked 689 nm light against a fs
comb that is locked to a second optical cavity [78]. Here, we find a short-term linewidthof < 300 Hz, where the measurement is limited by the phase-noise originating from theoptical fiber connecting the 689 nm light to the fs comb. Next, the long-term stability of
the 689 nm laser is evaluated by beating the cavity locked 689 nm light against a fs combthat is locked to a hydrogen maser via a fiber optical link to NIST [79, 80]. From thesemeasurements, the laser-cavity system drifts ∼ ± 400 mHz/s and exhibits a 1 s stabilityof < 4×10−13 (i.e., < 180 Hz) with the former value limited by cavity drift and the lattervalue limited by the short-term maser instability. To eliminate the slow cavity induced
drift, the master ECDL is next locked to the 1 S0 -3 P1 resonance via saturated absorption
feedback to the 1 GHz AOM. For added stability, a DC magnetic field is applied to theSr vapor cell and the spectrometer is set to perform frequency modulation spectroscopyon the 1 S0 (m = 0) - 3 P1 (m = 0) transition. The 1 S0 -3 P1 spectrometer is very similar
to the 1 S0 -1 P1 spectrometer described above. The key difference is the atom source:
rather than a hollow cathode lamp, the 1 S0 -3 P1 spectrometer utilizes a simple Sr heatpipe source (with ∼ 25 mTorr of argon buffer gas). Saturation spectroscopy with dual

47
modulation (high frequency phase modulation of the probe beam and low frequency
amplitude modulation of the saturation pump beam) and demodulation provides the
final error signal for stabilizing the master 689 nm laser to the atomic transition. With
the system fully locked, the 1 s stability is then ∼ 4×10−13 while for time scales < 5min, the drift rate can be as small as ∼ ± 10 mHz/s. On longer time scales, baseline
fluctuations in the error signal cause frequency excursions that are ∼ 1 kHz/day.
A portion of the 689 nm master ECDL output is next used to generate heterodyne
beats with the two frequency offset slave lasers. Each slave laser output, after doublepassing through an AOM used for frequency shifting and intensity chopping, is thencoupled into a single-mode polarization-maintaining optical fiber. Upon exiting eachfiber, the 689 nm light has up to 6 mW of power and is expanded to a 1/e2 diameter of
5.2 mm and divided into three equal intensity trapping beams. Dichroic beamsplitters
are then used to co-align the 689 nm and 461 nm trapping beams. The trapping beam
waveplates are 3λ/4 (λ/4) at 461 nm (689 nm).
1S

0-

3P

1 cooling and trapping dynamics are monitored either by in-situ or time-of-flight (TOF) fluorescence images collected with an intensified CCD camera. The camera
can view the cloud in either the horizontal x-y plane or nearly along gravity. The x-yplane (along gravity) images have a spatial resolution of 21 µm/pixel (37 µm/pixel).
For in-situ images, the 461 nm trapping beams are pulsed on for 10 - 50 µs immediately
after the atoms are released from the trap while for TOF images, the atoms are allowed
to first freely expand for a variable amount of time. We have verified that in-situ
images recorded with 461 nm pulses are identical to direct images of the in-trap 689 nm
fluorescence aside from an improved signal-to-noise ratio. Typical TOF flight times are
20 - 35 ms. To determine cloud temperatures, gaussian fits are performed to both thein-situ and TOF images. The temperature TM is then given by TM = (m/4kB tF 2 )(R2F- r2 ) where tF is the flight time and RF (r) is the TOF (in-situ) 1/e2 radius of the cloud.
Figure 2.8 depicts the 1 S0 - 3 P1 MOT loading procedure [81]. A 1 S0 - 1 P1 MOT

48

N = 2.5 x107
TM = 2.6 mK6
N = 6.6 x106 N = 6.6 x10
TM = 110 µK TM = 12.6 µK

N = 6.3 x106
TM = 1.2 µK

N = 6.3 x106
TM = 1.2 µK

gIn-Situ
4.8 mm

In-Situ

In-Situ

In-Situ

TOF

50
dBz (G/cm)

10
3

ON
461 nm Laser

10 - 50 µs
OFF689 nm LaserOFF
689 nm Laser
Spectrum0

ON

BroadbandSingle Frequency
0

20

40

80
60
Time (ms)100

Figure 2.8: 1 S0 -3 P1 MOT timing diagram. Images at top show the atomic cloud at eachstage of the cooling and spatial compression process. Starting from the right, the first
four frames are in situ images while the last frame shows the cloud after 25 ms of free
expansion from the δ = −520 kHz, s = 75 single-frequency MOT. N (TM ) is the cloud
population (temperature).

49
first pre-cools ∼ 3×107 atoms to ∼ 2.5 mK (lasting several hundred ms). At time t =0, the 461 nm light and the atomic beam shutter are switched off, dBz /dz is rapidly(ms) lowered to 3 G/cm, and red-detuned, broadband frequency modulated 689 nm
trapping beams are turned on. 10 ms later and for the following 50 ms (100 ms for 87 Sr
trapping), the cloud is compressed by linearly increasing dBz /dz to 10 G/cm. Frequency
modulation parameters for the 689 nm trapping beams are set to give complete spectral
coverage of the 1 S0 - 1 P1 MOT Doppler profile and, as shown below, manipulate thecloud size at the end of the magnetic field ramp. Subsequently, at t = 60 ms, thefrequency modulation is turned off and the atoms are held in a single-frequency MOT.
As shown by the Figure 2.8 images, the best transfer into the 689 nm MOT decreases
the sample temperature by more than three orders of magnitude while only reducing thecloud population by a typical factor of 3 - 4, giving final temperatures of ∼ 1 µK andpopulations of ∼ 107 . Typical single frequency trap lifetimes and spatial densities are∼ 1 s and ∼ 5×1011 cm−3 , respectively. With 707 nm and 679 nm optical re-pumpingof the 1 S0 - 1 P1 MOT, the 1 S0 - 3 P1 MOT population (spatial density) can be 4×107(3×1012 cm−3 ).

2.4

Laser cooling and trapping 87 Sr

2.4.1

The 1 S0 -1 P1 MOTHyperfine structure in 87 Sr splits the fine structure states as shown in Figure 2.9[59, 17, 82] for the 1 P1 , 3 P1 , and 3 S1 states . With nuclear spin I = 9/2, the J = 1
1P

1 state splits into three hyperfine states, F= 11/2, 9/2, and 7/2. Note in Figure

2.9 the unique ordering of the energy of these states, due to the strong role of theelectric quadrupole hyperfine interaction. As described in Section 2.2.1, laser coolingand trapping is more straightforwardly achieved in J-J + 1 transitions (or in the caseof hyperfine structure for F -F + 1 transitions). For this reason, the 1 S0 F = 9/2 - 1 P1

50

7/2
2.439 GHz
9/2
2.981 GHz
11/2
12 MHz3S1

7/2

43 MHz11/2
23 MHz7/2

9/2
1.130 GHz

1P
1

222 MHz

9/2

1.241 GHz
11/2
3P
1
1S
0

9/2
Figure 2.9: Energy level diagram relevant for laser cooling 87 Sr with its hyperfine structure. The total angular momentum, F , is denoted on the right side of each level. On
the left, frequency shift from the equivalent 88 Sr transition is given (indicated by thedashed line).

51
F = 11/2 transition is used as the laser cooling cycling transition. Experimentally, thedifference is minor. The cooling 461 nm laser is still locked to the 88 Sr spectrometer,
but employs an extra 52-55 MHz frequency shift to yield trapping light which is 40 MHz
red-detuned from the 9/2 to 11/2 transition.
Perhaps the detail most affected by the 87 Sr hyperfine structure is the repumping
process. The 3 P2 state to which atoms are originally shelved has five hyperfine stateswith individual state splittings on the order of a GHz. All states are populated byatomic decay and require repumping to 3 S1 , which has three hyperfine states with 2-3
GHz state separations. The sheer number of states complicates the repumping process.
The most successful MOT population enhancement was found by strongly frequency
modulating the repump lasers. Modulation is applied to both the laser drive current
and the laser PZT of the repump ECDLs, and the modulation frequency and depth arevaried to optimize MOT number. The repump spectrum is smeared across many GHz.
With this approach, the 87 Sr MOT number could be enhanced by the repumping lasers
by a factor of 15.
Unfortunately the 87 isotope has a much smaller natural abundance (7%) than
the 88 isotope (83%). This means that atomic beam flux of 87 Sr emitted from thethermal oven is reduced to 7/83 ' 9% of the 88 Sr flux. The effect of the reduced flux
on the MOT trapped atom number is straightforward. Assuming the simple case of aconstant MOT loading rate L, and a loss rate β that scales with the atom number N(e. g. no binary collisions), the atom number rate equation is just:dN= L − βN
dt

(2.19)

whose solution is:N=1(L − e−βt ).
β(2.20)The steady state population is simply Nss = L/β. Since the loading rate scales linearlywith the atom beam flux, the resulting 87 Sr MOT atom number is smaller than the 88 Sr

52
MOT number by the ratio of the natural abundances. This is roughly what we observe
experimentally.
One bonus associated with cooling the 87-isotope is that the presence of magnetic
sublevels in 1 S0 permits sub-Doppler cooling. Experimentally, temperatures below 500µK have been observed, more than a factor of 2 below the Doppler limit for the trap
intensities used. Although not directly observed, temperature measurements made atdifferent laser detunings and intensity suggest that temperatures as low as 40 µK could
be achieved by operating with low trapping intensity [59]. We have not actively investigated this possibility, although it is an interesting option. Achieving these temperatureswith the 1 S0 -1 P1 MOT could facilitate direct loading of atomic samples into an opticallattice without use of a free space 1 S0 -3 P1 cooling sequence.

2.4.2

The 1 S0 -3 P1 MOT

The experimental operation of the 1 S0 -1 P1 MOT was minimally affected whentrapping 87 Sr rather than 88 Sr. However, this is not the case for the 1 S0 -3 P1 MOT.
The difference originates because of the differences between the 1 S0 -3 P1 and 1 S0 -1 P1transition linewidths, ∆ν, relative to their recoil frequencies, νr = ωr /2π. These details
were first described in the literature in [84]. To appreciate the difference, consider a
MOT operating on the F to F + 1 transition, which like the 1 S0 -1 P1 MOT, is F = 9/2
to F = 11/2. Of course, the Zeeman shift of this transition depends on the magnetic
quantum number, mF , of the states and is given by (for simplicity in 1-D):h∆ν = [(mF ± 1)µe − mF µg ]B(x)(2.21)

where µg and µe are the Zeeman shift coefficients for the mF ground and mF ± 1 excitedstate respectively, and B(x) is the linearly dependent magnetic field generated by theanti-Helmholtz coils with a zero crossing at the trap center. The complication originateswith the case of µe  µg . To distinguish the cases of µe ' µg and µe  µg , consider

(a)

+2

-1

0

+1
σ- σ+

+2

+1
-1

53

(b)

+2

-1

-1

0

0

0

+1

+2

+1

(c)

(e)

photonscatterings

population (%)

population (%)

(d)

2mF

photonscatterings

2mF

Figure 2.10: Laser cooling 87 Sr on the 1 S0 -3 P1 intercombination transition. (a) when
µg ' µe , atomic population in any ground mF level favors absorption of light fromthe appropriate direction for trapping (encoded with polarization). (b) when µg  µe ,absorption of light from a given direction depends on mF , and some mF states arethus not suited to provide spatial confinement in a MOT. (c) Clebsch-Gordan (CG)coefficients (squared) among the 1 S0 -3 P1 F = 9/2-F 0 = 11/2 transition. Note that for agiven ground mF state, the CG coefficients are larger to excited states with larger |mF |.
This difference in CG coefficients is most dramatic for the 1 S0 |mF | = 9/2 states, andcan be used with the σ + and σ − configuration to yield spatial confinement. (d) Basedupon the CG coefficients, in the 1 S0 -3 P1 MOT, spontaneous decay from the excited
3 P F 0 = 11/2 state favors accumulating population in magnetic substates with small
1
mF where the difference in CG coefficients for absorption from the ground state is
reduced [83]. (e) Using σ + and σ − polarized light slightly red-detuned from the 1 S0 -3 P1
F = 9/2-F 0 = 9/2 transition, spontaneous decay evenly distributes population among
all magnetic sublevels. Such an optical field can thus rapidly stir and randomize thepopulation among mF levels. This allows population to move to the mF states best
suited for spatial confinement at a given spatial location in the MOT and thus improve
trap performance.

54
Figure 2.10. We assume the atom is moving relatively slowly (such that ~k · ~v ≤ ∆ν)and is located at x0 such that mµg B(x0 ) > 0 (right hand side). Laser light is incident
on the atom from both sides, σ − from the right and σ + from the left. Because of
the small Doppler shift, the red-detuned laser light remains red-detuned for both laser
beams. For µe ' µg , it is clear that no matter what ground mF state is occupied,
the atom will always favor absorption of the red-detuned σ − photon, and consequently
will experience a net restoring force back to the trap center. For the case of µe  µg ,the scenario is quite different. Due to the approximate degeneracy of the ground spinstates, some spin states favor absorption of red-detuned σ − photon, while others favor
the red-detuned σ + . Which is favored depends strongly not only on the spin state, butalso on the atomic position, x0 (determining the Zeeman shift), and these dependences
frustrate the existence of a mean trapping force. Fortunately, an additional mechanism
facilitates the trapping process: the relative transition probabilities between σ + and σ −transitions, as given by the Clebsch-Gordan (CG) coefficients. As seen in Figure 2.10,
for negative (positive) mF in the ground state, the CG coefficients are larger (smaller)for σ + transitions than for σ − transitions, thus favoring absorption of a σ + (σ − ) photon.
The asymmetry between σ + and σ − transition probabilities is small for |mF | close to0, and becomes more pronounced as |mF | approaches F. This transition probability
difference, aided by the spatially dependent Zeeman shift, can thus be used to generatea spatially dependent restoring force [85].
In order to work effectively, however, population must be able to move between
the ground spin states so that when located at x = x0 (x = −x0 ), the population resides
in negative (positive) mF to experience the proper restoring force. Furthermore, since
the restoring force from the CG asymmetry is most pronounced in the stretched states,
ideally the population would not only be in the spin state with the proper sign, but also
in the stretched state. Here, the narrow linewidth of the 1 S0 -3 P1 transition complicates
the trap realization. Because the linewidth, ∆ν, is comparable to the recoil frequency,

55
νr , a few photon recoils are enough to induce a large enough change in the Doppler shift
such that the transition is no longer in resonance with the laser field, and the transition
is no longer cycled. This means that population is not moved very easily among the spinstates by optical pumping effects from the trapping lasers. This non-mobile spin state
population then has a high probability to be in the wrong spin state and not experience
the efficient restoring force (e.g. in the worse case scenario, the population could be
mF = +9/2 for x0 > 0). This is in contrast to a broad transition such as 1 S0 -1 P1 ,where many photon recoils yield a change in the Doppler shift equal to a small fractionof the transition linewidth. As a consequence, the atom regularly scatters trap photons
and the population is rapidly pumped through all spin states, such that the probability
to be in a spin state well-suited for trapping is reasonable. The reduced population“randomization” by optical pumping with 1 S0 -3 P1 is further exacerbated by the factthat spontaneous decay favors population accumulation in the states with small |mF |.
As described above, these states have reduced CG asymmetry, and thus less efficient
trapping.
To provide population randomization, a second laser is introduced. Named for its
capacity to evenly stir the population among the different spin states, the stirring laseris slightly red-detuned from the F = 9/2 to F 0 = 9/2 transition. The effect of scattering
this σ + and σ − polarized field is shown in Figure 2.10, where many photon scatterings
result in population evenly distributed among the spin states (for simplicity B = 0
was assumed). This rapid population stirring ensures that the population can evolveto the needed spin state for efficient trapping. Furthermore, because µe for the stirringtransition is more than four times smaller than that for the F = 9/2 to F 0 = 11/2
transition, the atoms remain in resonance over a longer distance and thus the laser canpartly function as an optical molasses cooling laser to complement the trapping laser.
The combination of the stirring and trapping laser allows for operation of a µK
temperature MOT with > 105 87 Sr atoms. Experimentally these lasers are frequency

56
stabilized with offset locks from the master ECDL locked to the 1 S0 -3 P1 88 Sr spectrometer. [84] demonstrated a five-fold improvement in the 1 S0 -3 P1 MOT lifetime by adding
the stirring laser to the trapping laser. Still not as efficient as the simpler 88 Sr 1 S0 -3 P1
cooling, when cooling 87 Sr we typically allow for longer cooling times (50 ms single
frequency cooling compared to 25 ms for 88 Sr).

2.5

Interrogation of Tightly Confined Atoms

2.5.1

Free Space Atom Interrogation

In the introduction, I briefly described the motivation for using laser cooled atoms
in optical frequency standards: reducing the Doppler effect. More explicitly, in Equation
2.1, we considered the frequency of laser radiation in the laboratory frame which wasessentially resonant with a moving atom in its own rest frame:ωabs = ω0 + ~k · ~v +

~k 2
2m

(2.22)

A large atom ensemble can allow for high measurement S/N of the transition. The
ensemble usually has a well-defined temperature, T, indicating that the relative distribution of atoms with (1-D) velocity, v, is Gaussian, given by the Boltzmann factor:−mv 2

P (v) = e 2kb T(2.23)For a large atomic sample with rms Doppler shift, kvrms , larger than the natural transition rate, Γ, of the transition being probed, a Gaussian spectroscopic profile is recovered
with full width at half maxima (FWHM) equal to:r∆νD =8kb T ln(2) 1m
λ0(2.24)

where λ0 = 2πc/ω0 is the transition wavelength and m is the atomic mass. This
inhomogeneous, Doppler broadening originates from the fact that atoms in different velocity groups are resonant at different probe frequencies. The negative effect of Doppler

57
broadening on a frequency standard is seen by direct consideration of Equation 1.1.
Any broadening beyond the natural linewidth degrades the achievable stability of an
atomic standard. For decades, Doppler-free spectroscopic techniques such as saturation spectroscopy have been used to probe atomic transitions nearly free of Doppler
broadening. Unfortunately, such techniques typically take advantage of only a small
fraction of the total atomic sample - those atoms with a small enough atomic velocity
that ~k ·~v < Γ. This corresponds to smaller signal size, eventually affecting S/N in Equation 1.1. More sophisticated techniques, like multiple pulse Ramsey interrogation, canobtain spectroscopic features with a linewidth at or even below the natural transition
linewidth while still including the majority of the atomic sample in the laser interaction. Unfortunately, even though this can reduce Doppler broadening effects, thesetechniques, like all other free space ones, are eventually susceptible to measurement
shifts associated with residual Doppler effects. These measurement shifts compromise
the standard’s realizable accuracy. For example, both saturated absorption and four
pulse Ramsey spectroscopy utilize counter-propagating beams (equal but opposite ~k) torealize Doppler cancellation. However, experimentally, the ability to create equal but
opposite ~k is limited by technical considerations and can subsequently result in residual
Doppler shifts of the atomic transition. This problem extends to non-uniform atomic
motion due to gravitational acceleration of a free space atomic sample. Many of thesesometimes subtle but relevant effects were considered in detail in high precision spectroscopy of free space, laser cooled Ca, developed as an optical frequency standard for
now more than a decade [86, 87, 88, 89, 90]. We also investigated some of these effects ina free space spectroscopic interrogation of the 1 S0 -3 P1 transition in 88 Sr [91]. All of thesestudies carefully considered residual Doppler shifts, and although headway in reducing
and controlling these effects has been made, keeping shift uncertainties well below onepart per thousand (ppt) of the transition linewidth is technically very challenging andseemingly prohibitive.

58
It was a reduction of the Doppler effect which motivated the use of laser coolingto begin with. However, even laser cooled samples at µK temperatures have Doppler
broadened linewidths of tens of kHz [91]. The weak square root dependence of the
Doppler width on temperature ensures that even a Boltzmann-distributed Sr sample ata very cold 1 nK has a Doppler broadened linewidth at the kHz level. It was with this inmind that for many years, some researchers considered large Bose-Einstein condensates(BECs), with all atoms uniformly condensed to the ground state of motion, as an ideal
sample for an atomic frequency standard (it has since become clear that strong interactions among the atomic bosons perturb the clock transition frequency [92]). Insteadof merely lowering the temperature of a free space atomic sample, tightly confining theatoms can dramatically reduce the (first-order) Doppler effect, as we see in the next
section.

2.5.2

Confinement in a Harmonic Potential

We now consider a single atom trapped in a simple harmonic potential. The
initial Hamiltonian is composed of two pieces, one for the internal degrees of freedom of
the two level atom and one for the external degrees of freedom of motional confinementin the 1-D harmonic potential.
Hint = ~ω1 |1ih1| + ~ω2 |2ih2|
Hext =p̂2
1+ mω 2 x̂22m 2(2.25)(2.26)

Here the internal states 1 and 2 have energy of ~ω1 and ~ω2 , m is the atomic mass,ω is the trap frequency of the harmonic oscillator, and x̂ and p̂ are the position andmomentum operators. The position and momentum operators of Hext can be re-written
in terms of the annihilation and destruction operators [93]:
r
x̂ =

~
(â + â† )2mω

(2.27)

59rm~ω
(−â + â† )2(2.28)

1
Hext = ~ω(â† â + )2(2.29)p̂ = iand Hext is given by:

The eigenstates of Hint are just the internal states |1i and |2i, while the eigenstatesof Hext , labelled as |ni, are characterized entirely by the motional quantum number n.
The annihilation and creation operators operate on |ni as follows:√n|n − 1i

(2.30)√
n + 1|n + 1i

(2.31)

â|ni =â† |ni =It can thus be shown that energy eigenstates consist of a ladder of equally spaced
motional states |ni, with n ranging from 0 to ∞. Each individual state has well-defined
harmonic motion, whose wave function in position and momentum space is specified by
the motional quantum number, as is the state energy E = ~ω(n + 1/2). In position
space, the normalized state wave function can be written as:
s
 
1
x
− 1 ( x )2
ψn (x) = √ n
e 2 x0 Hn
x0
π2 n!x0
with characteristic length x0 =(2.32)p~/mω, and Hn (x) the Hermite polynomial of order n.

The expectation value of x2 is found to be:hψn (x)|x2 |ψn (x)i =x20(2n + 1)
2

such that the rms spatial extent of the nth motional state is xrms = x0

(2.33)
pn + 1/2. The

n = 0 ground state wave function is gaussian, with a 1/e probability distribution radiusof x0 .
The combined eigenstates for Hint and Hext are simply product states of the internal states |1i and |2i with the motional states |ni. However, we now add a third term to
the Hamiltonian corresponding to an atom-light field interaction. This term originatesfrom the introduction of a nearly resonant probe laser for spectroscopic investigation

60of the confined two-level atom. This interaction couples internal levels with an electricfield and can be expressed as:~Ω ikx̂ −iωL t~
HI = −d~ · E(x,
t) '
(e e
|2ih1| + e−ikx̂ eiωL t |1ih2|)2(2.34)

Here Ω = −dE/~ is the Rabi frequency, d is the atomic dipole moment, k is the 1-D
wave vector, and ωL is the laser frequency. Note that the rotating wave approximation
has been made, but that the dipole approximation has not been made and for now wekeep all orders of eikx̂ . This is important since the confined atomic wavefunction is
not necessarily much smaller than the probe laser wavelength, indicating the atom cansample different values of the electric field at a given time. We now transform to a frame
rotating at the laser frequency, ωL :HI =~Ω ikx̂(e |2ih1| + e−ikx̂ |1ih2|)2(2.35)

This rotating frame also transforms Hint to:
Hint = −~∆|2ih2|(2.36)

where ∆ = ωL − (ω2 − ω1 ) is the laser detuning from the atomic transition and ~ω1 ischosen to be the reference point of zero atomic energy. Returning to Equation 2.35, we
substitute Equation 2.28 in for x̂ to get:HI =~Ω iη(â+â† )†[e|2ih1| + e−iη(â+â ) |1ih2|]2(2.37)√
where η = kx0 / 2. We now write the total system Hamiltonian together [94, 95, 96]:~Ω iη(â+â† )1†
H = Hint + Hext + HI = −~∆|2ih2| + ~ω(â† â + ) +[e|2ih1| + e−iη(â+â ) |1ih2|]22(2.38)
An eigenstate of this Hamiltonian can be written as a linear superposition of productstates of the internal and external degrees of freedom:ψ=∞X(c1n0 |1i|n0 i + c2n0 |2i|n0 i)

n0 =0(2.39)

61
Plugging Equation 2.39 into the Schrödinger equation i~ dψ
dt = Ĥψ, and then taking theinner product with |1i|ni and |2i|mi gives the coupled equations of motion, for n andm from 0 to ∞:
∞

Ω X
1
†
hn|e−iη(â+â ) |n0 ic2n0ċ1n = −iω(n + )c1n − i2
2 0(2.40)

n =0

∞

1
Ω X
†
ċ2m = i[−ω(m + ) + ∆]c2m − i
hm|eiη(â+â ) |n0 ic1n02
2 0(2.41)

n =0

Now we impose the assumption that we can near resonantly address the individualtransition from |1i|ni to |2i|mi and in so doing ignore far-detuned coherent couplings
from |1i|ni and |2i|mi to other states. This allows us to pick out the mth (nth ) term inthe summation of Equation 2.40 (2.41) and reduce our system to two coupled equations:1Ω†ċ1n = −iω(n + )c1n − i hn|e−iη(â+â ) |mic2m2
2(2.42)Ω
1†ċ2m = i[−ω(m + ) + ∆]c2m − i hm|eiη(â+â ) |nic1n22(2.43)

To illuminate the solution to these equations of motion, we compare Equations 2.42 and2.43 to the equations of motion for the well known Rabi flopping solution of a stationary
atom (in the dipole approximation):Ωċ1n = −i c2n2(2.44)Ω
ċ2n = i∆c2n − i c1n2(2.45)

Comparing the first terms in the right hand side of Equations 2.42, 2.43, and 2.45, whenn = m, the harmonically bound atoms have resonant excitation similar to an atom atrest. When n 6= m, the resonant frequency is not simply ~ω2 , but rather ~ω2 +(m−n)~ω.
In this case, the atom is not only excited internally (electronically), but the atom is also
excited (or de-excited) motionally resulting in a change of the motional state within theladder of harmonic states.
Further comparison indicates that the harmonically trapped atoms experience
Rabi flopping similar to the rest atom, but notably the coherent excitation rate isexcitation signal (arb.)

62

1.0
0.8
0.6
0.4
0.2
0.0
-2

(a)

-1

0

1

frequency (units of trap frequency, ω)

1.0

n=0
n=4
n=8

2

0.6

2

0.8

0.4

Ω nn/Ω

2

0.2
0.0
(b)

0.1

η

1

10

Figure 2.11: (a) Absorption spectrum of a confined atom. Zero detuning frequency
corresponds to the natural atomic resonant frequency ω. The atom is also excited at
ω0 ± lω, where l is an integer. This yields the sideband resonances at ±1, ±2, etc. It has
been assumed that the decoherence rate Γ is less than the trap frequency ω, such thatthe sidebands are well-resolved from each other and from the resonance at the natural
atomic resonance. (b) The effective Rabi frequency (squared) for purely electronictransitions as a function of the Lamb-Dicke parameter η for various ground motional
states with quantum number n. With very strong confinement (η  1), Ω2nn /Ω2 ' 1,
indicating the atom is excited at a rate comparable to an atom at rest. With very weak
confinement (η  1), Ω2nn /Ω2  1 as dipole coupling is spread among excitations toother motional states of the excited electronic state.

63different than for the rest atom case (Ω). Rather the effective Rabi frequency is givenby:†Ωmn = Ωhm|eiη(â+â ) |ni(2.46)

By expanding the exponential term and operating with â and â† to the left and right,Ωmn can be explicitly solved to be [94, 95]:s
η2n< ! |m−n| |m−n| 2Ωmn = Ωe− 2
ηLn< (η )n> !

(2.47)

where n< (n> ) is the lesser (greater) of n and m, and Lαn (x) is the generalized Laguerre
polynomial:Lαn (x) =

n
X
p=0



n + α xp(−1)
n − p p!
p

(2.48)For the cases of electronic and motional excitation (m > n), pure electronic excitation(m = n), and electronic excitation and motional de-excitation (m < n), the effective
Rabi rates are explicitly given by:

2q

− η2
n! m−n m−n 2Ln (η ) if m > n
e

m! η


2
− η2 0 2Ωmn =if m = n
Ln (η )
e


q

2


n−m (η 2 ) if n > m e− η2 m! η n−m Lmn!

(2.49)

This leads to atomic spectra which may appear like the one in Figure 2.11(a). Shown
here is the purely electronic excitation, named the carrier, as well as the red (blue)
sidebands associated with de-excitation (excitation) of the atomic motion. The relative
amplitudes of these transitions are given by the square of the Rabi frequencies given in
Equation 2.49. Also shown is the transition had the atom been at rest. As can be seen,
the excitation rate of the carrier transition is diluted due to the decreased coupling between |1i|ni and |2i|ni as a consequence of the confined atomic motion. Shown in Figure2.11(b) is Ωnn (purely electronic excitation) as a function of η. Further ramifications ofη dependence (known as the Lamb-Dicke parameter) on the atomic interrogation will
be discussed later. However, note here that at large η (weak confinement so that the64atomic wavefunction characteristic length x0 is large compared to the wavelength of the
probing light), Ωnn can become substantially smaller than Ω. The combined atomic andmotional eigenstates constitute a complete and normalized basis set, such that:∞X|Ωmn |2 = |Ω|2

(2.50)

m=0

Correspondingly, when Ωnn shrinks as η grows, the total coupling to other motion states(Ωmn for m 6= n) grows. At very small η (strong confinement), Ωnn ' Ω. This makes
intuitive sense as very strong confinement indicates the atom can not experience large
motional displacement, like an atom at rest. Furthermore, stronger confinement meansthat more of the atoms, Boltzmann distributed in the motional state ladder, occupy theground motional state.
Another important consequence of Equation 2.49 is that atoms in different initialmotional states, n, experience different coherent excitation rates to the excited state.
This inhomogeneous excitation is particularly evident when a large number of motional
states are occupied. Furthermore, the differences in the excitation rate are more pronounced in weaker confinement. Like other sources of inhomogeneity, this can lead todamped Rabi oscillations, exhibiting contrast collapse and revival. More details are
given in Section 5.4.4.
Although the quantum mechanical treatment above gives the most complete analysis of the harmonically bound atomic system, it is worthwhile to consider an alternative
semi-classical picture which can provide further intuition into the physical system. In
the quantum mechanical treatment, it was useful to move to a reference frame rotating
at the laser frequency, ωL . Here, we choose the rest frame of the atom. The atom in agiven motional state |ni is oscillating in the lab framex(t) = A sin(ωt + φ)

(2.51)

where A is total oscillation amplitude of displacement, t is time, and φ is a phase factor.
This means that in the atom rest frame, the atoms sees the incident probe radiation as

65
a frequency modulated field:~ atom = E~ 0 sin(kA sin ωt − ωL t)
E(2.52)

where φ has been chosen to be zero. Equation 2.52 matches the initial expression for
signal modulation theory from phase/frequency modulation [97, 43]. Following thatanalysis, the field in Equation 2.52 can be expanded as a series of Bessel functions:~ atom = E~ 0 {J0 (kA) sin[ωL t] + J1 (kA) sin[(ωL + ω)t] − J1 (kA) sin[(ωL − ω)t] + ...} (2.53)
E
The electric field seen by the atom has a component at the original frequency ωL withamplitude given by J0 (kA), but also has sideband components at ωL ± ω with amplitude J1 (kA). The “. . . ” in Equation 2.53 refers to higher lth order sidebands withamplitudes given by Jl (kA). If ωL = ω0 = ω2 − ω1 , then the atom is excited electronically and the absorption and emission spectrum has an intensity proportional to[J0 (kA)]2 . For an atom in the motional state |ni, the oscillation amplitude A is found√to be x0 2n + 1 which corresponds to the classical turning point of the harmonically√ √bound atom. This means that kA = 2 2n + 1η and the intensity is proportional√ √to [J0 (kA)]2 = [J0 ( 2 2n + 1η)]2 . This can be compared to the quantum mechanicalresult (middle equation in Equation 2.49) by recognizing that:√ √η2
J0 ( 2 2n + 1η) ' e− 2 L0n (η 2 )(2.54)

Equation 2.54 is valid for η < 1, presumably because unlike the quantum mechanicaltreatment, this semi-classical picture does not properly account for photon recoil (seefurther discussion below).
The relative size of the red and blue sideband intensities is slightly more complicated. This is because during the excitation, the motional state changes from |ni
to |mi and thus the expansion coefficient J1 (kA) changes because of a change in themodulation depth kA. This is in contrast to the carrier excitation, where the atomic
motion and hence the modulation seen by the atom are independent of the electronic

66
state. To deal with the case of sideband excitation, as a simple approach [98] we evenly
average the effect of the two motional states on the modulation, i. e. n → (n + m)/2.
For the lth order blue sideband (l = m − n), the line intensity is thus proportional to√ √Jl ( 2 2n + 1 + lη). Again the similarity of these results with the quantum mechanicaltreatment can be seen by recognizing numerically that:√ √η2
Jl ( 2 2n + 1 + lη) ' e− 2rn! m−n m−n 2ηLn (η )
m!

(2.55)

again valid for η < 1. The spectrum is thus seen to resemble Figure 2.11.
Already in our discussion on harmonic confinement of atoms, we have implicitly
touched on different regimes which may or may not be ideal for performing high resolution spectroscopy. Here, I explicitly list several important regimes and why they areuseful for the experimental spectroscopy reported later in this thesis.

2.5.3

Uniform Confinement Regime

We have been implicitly assuming that the harmonic potentials are identical forthe ground and excited electronic states. If this were not the case, the carrier transition
frequency would not be ω0 , but would instead include a frequency shift given by theenergy difference between the confinement of the two electronic states. The electronic
degree of freedom and the motional degree of freedom are not cleanly separated unlessthe motional potential is the same for both electronic states.
The presence of a frequency shift dependent on the confinement details makes
it more difficult to maintain a small measurement inaccuracy of the unperturbed clocktransition. These confinement details would need to be known and controlled better
than in the case that the confinement potentials were uniform for the two clock states.
In general, when accuracy and long-term stability are important, it is almost always
better to make the measurement as close to an unperturbed case as possible.
Along with a frequency shift comes line broadening due to spatial or temporal in-

67homogeneities in the confinement of atomic ensemble. This broadening could ultimately
degrade the measurement stability of the transition frequency (see Equation 1.1).
Achieving uniform confinement for the two clock electronic states depends on thetype of confinement used. For the case of frequency standards based on single trapped
ions, the non-zero charge of the ion is exploited to confine the atoms using a timedependent (RF) electric field. This field interacts strongly with the net charge of theion, but extremely weakly with the clock electronic states. In this way, the confinement
is naturally independent of the electronic state. Neutral atoms, with a net charge of zero,
can not be trapped this way. For the work reported here, atomic confinement is achieved
with an optical lattice, exploiting a very strong optical electric field gradient interactingwith the induced dipole moment of the atom. The optical lattice strongly perturbs thevalence electronic wave functions. However, as described in the next section, the fieldparameters can be chosen so that the dipole polarizabilities of the two clock states areequal. In doing so, the uniform confinement regime is realized, cleanly separating theinternal and external degrees of freedom [27, 99, 100, 101].
In many respects, the optical lattice is an ideal atomic trap, providing nearly uniform confinement through its trap sites. This is in contrast to solid state lattice structures, which typically have imperfections which introduce significant inhomogeneities
between the confinement at different sites. This leads to decoherence which, despite
very strong confinement, prevents the same level of spectroscopy for quantum absorbers
bound to a solid state material. The optical lattice has emerged as such a powerfulexperimental tool because of its defect-free confinement through its various sites.

2.5.4

Well resolved sideband regime

Any real system suffers from relaxation or decoherence. As a consequence, spectroscopic features are broadened in the frequency domain. The relative size of thedecoherence rate, Γ, and the trap frequency, ω, strongly influences the two level dy-

68
namics and the observed spectroscopic features. When Γ > ω, the sideband structurein Figure 2.11 is unresolvable. This means that optical excitation at a given frequency
cannot neatly discriminate between purely electronic excitation (the carrier transition)or mixed electronic and motional excitation (sideband transitions). This makes spectroscopic measurements much more sensitive to the motional effects of Doppler and recoil
shifts. This is in contrast to the case Γ  ω, where the Doppler effects are moved tohigh modulation frequencies around the carrier transition. At these high modulation
frequencies, the motional effects interfere substantially less with measurement of thepurely electronic excitation frequency, which is the frequency that is relevant for highaccuracy optical frequency standards. The ability to discriminate carrier and sidebands
is sometimes called the well-resolved sideband regime (or the strong binding regime)[43, 102, 103].
To understand this effect more clearly, consider the spectra in Figure 2.12. Theseabsorption spectra are given by Equations 2.42, 2.43, and 2.49 for varying confinement
strengths and assume a Boltzmann-distributed population among the motional states.
The individual lines are represented in the well-resolved sideband regime (the details of
the individual lineshapes are not shown, but they are resolved). As the trap frequency
is reduced, the spacing between sidebands is reduced and at the same time additional
higher order sidebands appear (η increases as ω decreases). When the trap frequency is
reduced to the point that Γ ' ω, the sideband and carrier lineshapes eventually overlap.
As the trap frequency approaches 0, we approach the limit of free space interrogationof the untrapped atomic sample. In that limit, the spectrum is given by the Dopplerbroadened profile (whose Gaussian width is given by Equation 2.24) and is shown as theblack envelope function of the first spectrum. In this limit, the spectroscopic resolution
and accuracy are degraded because of the direct influence of the motional effects. In
contrast, in the well-resolved sideband regime, the Doppler effects manifested as fardetuned sideband features, only influence the carrier transition by line-pulling (shift

(a)

69

0.10

(b)
transition amplitudetransition amplitude

0.08

0.018

0.009

0.000

0.06
0.04
0.02
0.00

-60

-40

-20

0

20

40

60

-60

-40

-20

frequency (kHz)

0

20

40

60

40

60

frequency (kHz)

(c)

(d)

0.25

transition amplitudetransition amplitude

0.4
0.20
0.15
0.10
0.05

0.3
0.2
0.1
0.0

0.00
-60

-40

-20

0

20

40

60

-60

-40

-20

frequency (kHz)020frequency (kHz)(e)
transition amplitude

0.8
0.6
0.4
0.2
0.0
-60

-40

-20

0

20

40

60

frequency (kHz)

Figure 2.12: Absorption spectrum of an atomic ensemble in the range of very weak
confinement (a) to very strong confinement (e). The horizontal axis indicates frequency
detuning from the natural transition. The atomic recoil frequency ωr /2π is taken to be
4.68 kHz, approximately that of the strontium 1 S0 -3 P0 clock transition. Furthermore,
we assume negligible decoherence (Γ  omega). In (a), the black solid curve gives theabsorption spectrum of the atomic ensemble in free space, corresponding to the Dopplerbroadened profile. This Doppler-broadened profile serves as an envelope for the weak
confinement spectrum shown with trap frequency ω/2π = 1.376 kHz and Lamb-Dicke
parameter η = 1.84. As the atomic confinement becomes stronger and tighter [(b)ω = ωr and η = 1 and (c) ω/2π = 12 kHz and η = 0.62], the photon recoil shift (where
the spectral amplitude maximum is blue-detuned from the natural transition frequency)
is suppressed and the natural atomic transition emerges with the largest transition
amplitude [as in (c)]. Furthermore, the spectrum becomes more symmetric around thenatural transition frequency and the sideband amplitudes are suppressed relative to thecarrier, purely electronic excitation. This recoil suppression effect becomes dramatic far
into the Lamb-Dicke regime [(d) ω/2π = 20 kHz and η = 0.48 and (e) ω/2π = 60 kHz
and η = 0.28].

70
from the “wings” of the sidebands). For even the slowly decaying Lorentzian lineshape,in the well-resolved sideband limit this line-pulling effect scales to the third power inΓ/∆ where ∆ is the angular detuning of the line responsible for pulling. This effect canthus be made very small.
A remarkable outcome of the quantum mechanical solution to the bound atomis that, despite the photon recoil (recoil frequency ωr = ~k 2 /2m as in Equation 2.22),
in the well-resolved sideband regime, the carrier resonance clearly occurs at ω0 andthe sidebands at ω0 ± lω. With η ≥ 1, the recoil strongly determines the relativeline intensities of the carrier and sidebands. As seen in Figure 2.12, the maximum line
intensity is at the line closest to ω0 +ωr (just as the free space lineshape peaks at ω0 +ωr ).
The blue detuned sidebands have intensities larger than their red counterparts, just as
the free space recoil-shifted line is shifted to the blue. In the well-resolved sideband
regime, this asymmetry in the sideband structure around the carrier causes line-pulling
shifts which can be made small with sufficiently narrow spectral lineshapes.

2.5.5

Lamb-Dicke regime

In Section 2.5.2, we defined the parameter η, called the Lamb-Dicke parameter, which gave the relative size between the atomic spatial confinement of the ground√motional state x0 and the wavelength of the probing laser field (η = kx0 / 2). Thisparameter can be further seen to be equal to:√η = kx0 / 2 = k

r

~
=
2mω

r

ωr
ω

(2.56)

We look again at Figure 2.12 which gives the absorption spectra for various values of η.
As we move further into the Lamb-Dicke regime (η  1), the recoil effect on the line
intensities is reduced: the maximum line intensity moves closer to the carrier transition,
the sideband structure becomes more symmetric, and the sideband intensities become
smaller relative to the carrier. In this regime, the photon recoil energy and momentum

71
is taken up less by the atom and more by the confining potential (via lattice photon
generation in the case of an optical lattice). Therefore, the Lamb-Dicke effect is the
suppression of sideband excitation intensities [104], indicating that the atom does nottake up photon recoil. This phenomenon is analogous to the much studied absorptionof γ-rays on the Mossbauer line [105]. This recoil suppression roughly begins when
η = 1 or when ω = ωr . Here, the atomic recoil momentum from one photon absorption
is roughly equal to the rms momentum change from the atom being excited by one
motional quantum. Thus as η becomes less than 1, presumably the higher energy
and momentum needed to excite the atom motionally results in the recoil being morefavorably taken up by the confining potential.
In the Lamb-Dicke regime, the expression for Ωnm becomes simpler. In particular,
the first order red and blue sidebands are seen to have excitation rates of√Ωn,n+1 = η n + 1(2.57)√Ωn,n−1 = η n(2.58)

respectively. Note that while the recoil is suppressed in the Lamb-Dicke regime, it is
only completely suppressed in the limit of η → 0, as evidenced by the fact that with
nonzero η, the blue sideband excitation (Equation 2.57) remains larger than the redone (Equation 2.58). The sidebands continue to get smaller deeper into the Lamb-Dicke
regime, with their intensities scaling as η 2 . Naturally, as the sidebands get smaller, thecarrier excitation rate approaches Ω. This can be seen in Figure 2.11. No matter what n,the Ωnn approaches Ω. This illustrates that in addition to recoil suppression, the LambDicke regimes helps with another unwanted effect: inhomogeneous atomic excitation
as a function of motional state |ni. As η gets smaller, for all n, the carrier transition
coupling becomes more uniform and the sideband transition couplings become smaller.
Thus a large atomic sample distributed over many motional states can be excited morehomogeneously.

72
To clarify further the role of the atomic recoil, we explicitly consider two extreme
cases and their intermediate regime. In a free space atom (limit ω → 0), it is well known
that the atomic transition experiences a blue-detuned shift given by the recoil frequency,
ωr . In the case of an atom rigidly bound to a potential (limit ω → ∞), the photon recoil
is taken up by the combined atom-potential, and since the potential has an effective
mass much larger than the atom, the recoil shift is tiny and approaches zero. In a very
weakly bound, slowly oscillating atom, the atom absorbs the photon recoil. Since theatom is bound, all of this momentum is eventually transferred to the potential. However,
because of the huge effective mass of the potential, the energy predominantly remains
with the atom (Ekinetic = 1/2M v 2 ) [106, 43]. As the atom becomes more tightly bound,the “recoil energy” is reduced and the recoil momentum is taken up more directly by
the combined atom-potential system.

2.6

Atomic Confinement with a Far-Detuned Optical Wave
In the previous sections, we considered properties of atomic confinement thatwere optimal for high precision spectroscopy. We now consider one method to realize
this confinement for neutral atoms: nonresonant interaction with a strong optical field.

2.6.1

Dipole Potential

In Equation 2.38, I listed the Hamiltonian for a two level atom, harmonicallyconfined, and interacting with a laser field with Rabi frequency Ω and detuning ∆.
Originally, we considered the resonant or near resonant case where the atom was excitedinternally. We now focus on the far detuned case, where the atom is illuminated by alaser field with ∆  Ω. Here, no substantial excitation (electronically or motionally)occurs. Rather, the laser field acts as a perturbation on the atomic energy levels, shifting
their energy. We assume that the laser field is so far detuned that the details of the
motional states are not important (∆  ω). In other words, the far-detuned laser is73essentially equally far-detuned from all motional and electronic transitions, and becauseof the normalized couplings between electronic and motional states (Equation 2.50), we
can neglect the effect of confinement in the total Hamiltonian. In particular, we exclude
Hext as we consider the perturbation induced by the far-detuned laser field. Hence wewrite the Hamiltonian, this time in matrix form in the |1i,|2i basis [44] as:


0
Ω
~

H = Hint + HI = 

2
Ω −2∆

(2.59)

By direct diagonalization, the eigen-energies of the “dressed” states can be found. Compared to the energies of the bare, unperturbed states, the energy shift is:
U = ~∆ω =

1
|d|2
~Ω2
= E02
4∆
4 ~(ωL − ω0 )(2.60)

where ∆  Ω has been assumed, and in the last term, the values Ω = dE0 /~ and∆ = ωL − ω0 have been used. We recall that the Hamiltonian originating from Equation 2.38 exploited the rotating wave approximation. In the near resonant case, thisapproximation is entirely justified. In our far-detuned case here, keeping the other wave
yields a second contribution to the observed frequency shift:
E 2 |d|2∆ω = − 0 2
4 ~



1
1
+
ω0 − ωL ω0 + ωL



E2
=− 0
4~



2|d|2 ω0
~ ω02 − ωL2(2.61)The term in parentheses on the right hand side is labelled α, the dipole polarizability.
We now generalize α for a multi-level atom (with far-detuned transitions). We
label the state being shifted as state |ai. All intermediate states with dipole couplings
which contribute to the shift are labelled with the summation index, |ki.
αa =

ωak
2X
|dak |2 2~
ωak − ωL2

(2.62)k∆ωa = −

1
αa E024~(2.63)

where the transition between states |ai and |ki has angular frequency ωak and dipole
moment matrix element dak . The shift, ∆ωa , is referred to as the dynamic or AC Stark

74
shift, or alternately the light shift. The corresponding energy level shift can be exploited
to confine the atoms. By designing a light field with a spatially dependent intensity,
spatial confinement can be achieved at the energy minimum. Classically, the dipole
moment induced by an electric field is given by [107]:~d~ = αE(2.64)The interaction energy between the induced dipole and the field is simply:~
U = d~ · E(2.65)A dipole feels no overall force, only torque, in a uniform field. However, in a nonuniform
field, a dipole experiences an overall force:~ E~
F = (d~ · ∇)(2.66)

It is clear that the light field plays two roles in trapping the atoms. First, it induces
an atomic dipole moment (1st order in E). Second, the spatially varying light fieldforms a trap for the induced dipole (1st order in E). Together, the resulting trap depth,∆U = ~∆ω, scales with the polarizability, α, and the square of the electric field, E 2 .
Furthermore, the stronger the field gradient, the tighter the confinement that can beachieved.

2.6.2

Dipole Polarizability

To calculate the dipole polarizability in Equation 2.62, we need the dipole matrix
element dak which is related to state transition rates as in Equation 2.6. While thedecay rates from states specified by L and S quantum numbers are commonly reported
as experimental and theoretical results, we are concerned with couplings to a very
specific quantum state (the clock state), not the entire family of substates in the LS
state. Determination of how these couplings are subdivided through fine, hyperfine, andmagnetic substructure has been a long-solved problem in angular momentum theory75[108, 109, 110, 111]. We start with a variant of the reduction formula which, as written
here, relates the reduced dipole moment matrix element of a composite spin system to afurther reduced dipole matrix element which removes one spin dependence. Specifically,
here it is used to relate the dipole matrix element in the J,L,S basis to the reduced L,Sbasis only:

Xab =


2

 La Ja Sa |hJa La Sa kD1 kJb Lb Sb i|2= (2Ja + 1)(2Jb + 1)
|hLa Sa kD1 kLb Sb i|2


Jb

Lb

(2.67)

1 The term in curly brackets is the 6 − j symbol, which can be related to the Racah
W coefficient. Note that the reduced dipole matrix element in the denominator has
no J dependence. This matrix element is more directly related to the LS state decayrate. Equation 2.67 gives the relative dipole branching between the states |Ja La Sa i
and |Jb Lb Sb i. When the lower state, indexed by ‘a’, has fine structure, the dipole
coupling between |La Sa i and |Lb Sb i is divided among those substates. To calculate
the normalized branching ratio between |Ja La Sa i and |Jb Lb Sb i, consider the following
summation:
X(2Ja + 1)(2Jb + 1)

Ja


2

 La Ja Sa 


 J

b

Lb


1 

=

2Jb + 1
2Lb + 1(2.68)

Thus the branching ratio between particular fine structures states, each within finestructure manifolds, is given by:2 La Ja Sa Xabφ Ja Jb = P= (2Ja + 1)(2Lb + 1)Ja Xab

Jb

Lb(2.69)

1 Note that the branching ratio in Equation 2.69 is for the relative transition line strength(dipole moment squared) between fine multiplets.
Because of the frequency dependence of the spontaneous decay rate (see Equation
2.6), the nondegeneracy of fine structure states in a multiplet lead to decay rate branching ratios which are close, but not exactly equal, to those of Equation 2.69. This must

76
be kept in mind when extracting dipole moments, d, from measured decay rates of LS
states. As an example relevant to the 87 Sr clock states, we consider coupling between
an upper 3 S1 state and the 3 P0 clock state. Equation 2.69 gives the branching ratio,
φJa Jb , from 3 S1 to 3 P2 , 3 P1 , and 3 P0 as 5/9, 3/9, and 1/9 respectively. Using Equation
2.6, the combined decay rate from 3 S1 can be written asΓ = Γ3 P0 + Γ3 P1 + Γ3 P2 =

2
1
3
5
2
(ω33P0 |d|2 + ω33P1 |d|2 + ω33P2 |d|2 ) =ω 3 |d|26π0 ~c39996π0 ~c3 cm(2.70)

where ω3 PX is the 3 PX -3 S1 transition frequency. It is clear that the relative decay rates
to the 3 P multiplet states scale as φJa Jb and ωJ3a Jb . Equation 2.70 also shows that thedipole moment d is most easily calculated with ωcm , the average transition frequency
weighted by the branching ratios (“center of mass” frequency). Thus, to generalize
Equation 2.6, the dipole moment between LS states is calculated using
ΓLa Lk =2
ω 3 |dL L |2
6π0 ~c3 cm a k(2.71)

X(2.72)3ωcm=

φJa Jk ωJ3a JkJa

We are also concerned with the dipole coupling between particular magnetic substates. Here we refer to the well known Wigner-Eckart theorem (written here for thecase of dipole coupling only). This theorem indicates how to separate the dipole matrix element between two fully specified quantum states into two terms: one a purely
geometric term and the second a dynamical term with no dependence on the magnetic
quantum number. The quantum state is specified explicitly by J, L, S, m. Other
quantum numbers are assumed but not explicitly shown:2|hJa La Sa ma |Di1 |Jb Lb Sb mb i|2 = 

Ja
−ma

1

Jb 
1
2
 |hJa La Sa kD kJb Lb Sb i|
i mb(2.73)

The first term on the right hand side is the Wigner 3 − j symbol and can be expressed interms of the Clebsch-Gordan coefficients [93]. The second term, known as the reduced

77
dipole matrix element (indicated with double bars ’k’ around the dipole operator), is
independent of magnetic quantum number m and the dipole polarization i. Only the
Wigner 3 − j maintains dependence of the geometrically determined m and i. Hence,
the magnetic substructure coupling is isolated from the coupling between the otherquantum degrees of freedom.
One important property of the Wigner 3 − j is:2
X  Ja1 Jb 
1 =2Jb + 1
ma ,i
−ma i mb

(2.74)

As we consider the appropriate dipole coupling strength between particular magnetic
sublevels, the total decay rate from an upper magnetic state must equal that of its
parent fine structure state. Thus, the magnetic branching term for a lower state withma from upper state with mb is given by [112]:
φma mb = (2Jb + 1) 

2
Ja

−ma

1

Jb 

i mb

(2.75)

What states mb are relevant depend on the experimental details. A well-defined laser
polarization may excite only one polarization, i, coupling to a single upper state mb .
On the other hand, an unpolarized field would need to be summed over all three valuesof i with allowed couplings to more mb upper states.
As a side note, it is worth mentioning that the fully specified dipole matrix elements in a composite spin system can be related to the fully specified matrix elementsin the reduced spin basis. Combining the Wigner-Eckart theorem (Equation 2.73) andthe reduction formula (Equation 2.67), it can be shown that:PP
2
2
Jk ,mk ,ma |hJa La Sa ma |Di |Jk Lk Sk mk i|
mk ,ma |hLa Sa ma |Di |Lk Sk mk i|=
2Ja + 12La + 1(2.76)

Thus the sum of the matrix elements for a given Ja in the J basis equals those fora given La in the L basis (for an upper state with Lk ), each weighted by their statedegeneracy in the denominator.

78
With the appropriate branching parameters determined, we can now specify dak
in Equation 2.62 as:|dak |2 = φJa Jk φma mk |dLa Lk |2(2.77)

for upper state k and lower state a. Here dLa Lk is the dipole moment between the |La Sa i
and |Lb Sb i states. This allows us to now calculate the dipole polarizability of the finestructure states. By a similar application of the reduction formula (Equation 2.67) the
hyperfine state (F ) reduced dipole matrix elements can be rigorously related to thoseof the fine structure (J). However, as mentioned below, calculating the polarizability
while ignoring the 87 Sr hyperfine substructure is an approximation that does not limit
the present calculation.
The relevant energy levels with dipole coupling to the clock states are determinedby the dipole selection rules. The ground clock state, 5s2 1 S0 , couples to all higher
lying 1 P1 states. The excited clock state, 5s5p 3 P0 , couples to the higher lying 3 S1 and3D

1 states, as well as a doubly excited

3P

1 state. The dipole polarizability is calculatedusing Equations 2.62, 2.71, and 2.77. The relevant values of ωak , ΓLa Lk , φJa Jk , and ωcm
are listed in Table 2.1. Note that because both clocks states are J = 0 and thus taken
to be mJ = 0, and since the confining dipole trapping laser is assumed to π-polarized,
the φma mk = 1 for all transitions. Plots of α1 S0 and α3 P0 are shown in Figure 2.13
as a function the radiation wavelength, λ = 2πc/ωL . In the bottom panel of Figure
2.13, the difference in the two polarizabilities is plotted, zoomed in around λ = 800
nm. As can be seen, in this region, the polarizabilities of the two clock states are equal,
such that atomic confinement can be made essentially identical for both clock states.
This achieves the very important uniform confinement regime discussed earlier in thechapter.
Before moving to the next sections where we consider the details of the 87 Sr
dipole trapping, I pause here to note the assumptions and imperfections in the above

-359

500
0

1

0

-500
-1000

359
1000

2000

3000

718

AC Stark shift (kHz)-718

α ( S0) (a.u.)

79(a) 1000

-718

500

-359

α ( P0) (a.u.)(b) 1000

0

3

0

359

-500
-1000

1000

2000

3000

718

AC Stark shift (kHz)lattice wavelength (nm)

20

-14

10

-7

0

0

-10

7

3

1

α ( P0) - α ( S0) (a.u.)

(c)

-20
780

790

800

810

14
820

AC Stark Shift (kHz)lattice wavelength (nm)lattice wavelength (nm)Figure 2.13: Sr atomic polarizability (in atomic units) as a function of wavelength (innm). (a) 1 S0 polarizability (b) 3 P0 polarizability (c) difference between 3 P0 and 1 S0
polarizability, on a magnified wavelength axis around the “magic” zero crossing point
near 805 nm. The right hand side axes of each plot gives the corresponding AC Stark
shift for the atomic states in a 1-D lattice with one way intensity I = 5 kW/cm2 (seeSection 2.6.3).

80

Table 2.1: Transition parameters used to calculate the atomic polarizability of the Srclock states. The transition (radial) frequency values ωak are from [113] (1015 1/s). The
decay rates ΓLa Lk (106 1/s) are from the references indicated. φJa Jk and ωcm are definedin the text.
clock state
5s2 1 S05s5p 3 P0

5s5p 3 P0

5s5p 3 P0intermediate state
5s5p 1 P15s6p 1 P15s7p 1 P14d5p 1 P15s8p 1 P1
5s9p 1 P15s10p 1 P1
5s11p 1 P1
5s6s 3 S1
5s7s 3 S1
5s8s 3 S1
5s9s 3 S1
5s10s 3 S1
5s4d 3 D1
5s5d 3 D1
5s6d 3 D1
5s7d 3 D1
5s8d 3 D1
5s9d 3 D1
5p2 3 P1

ωak
4.087
6.423
7.328
7.755
7.755
7.998
8.161
8.276
2.773
4.353
4.981
5.299
5.483
0.724
3.897
4.778
5.190
5.415
5.555
3.961

ΓLa Lk
190.7(3.0)
1.86
4.3
14.5
16.7
11.7
7.6
4.88
75.4
17.5
8.22
4.53
2.77
.345(.024)
60.9
26.7
14.2
8.51
5.51
127

Reference
avg of [114] and [115] exp[116] exp[116] avg of exp & theor[116] avg of exp & theor[116] avg of exp & theor[116] avg of exp & theor[116] theor[116] theor[116] weighted avg of exp[116] theor[116] theor[116] theor[116] theor[117] exp[116] weighted avg of exp[116] theor[116] theor[116] theor[116] theor[116] weighted avg of exp

φJa Jk
1

1/9

5/9

1/3

ωcm
4.087
6.423
7.328
7.755
7.755
7.998
8.161
8.276
2.701
4.281
4.909
5.227
5.411
0.707
3.879
4.760
5.172
5.397
5.537
3.907

81
dipole polarizability calculation. Firstly, as early as our choice of Hamiltonian, we haveassumed the laser radiation is far-detuned from any dipole transition. In other words,
we are in the dispersive, not absorptive regime. It is the violation of this assumption
which gives infinite resonances in Figure 2.13 as a particular transition is crossed.
As mentioned above, the calculation was made on the fine structure states in
the J basis, more appropriate for the hyperfine-free 88 Sr states than for 87 Sr. Again,
the assumption requires a far-detuned laser field, where the sum of the couplings to
the individual higher lying hyperfine states is approximately the same as for the finestructure states. Similar to Equation 2.67, the hyperfine reduced matrix elements can be
related to the fine structure reduced matrix elements. An equality similar to Equation
2.76 can be found indicating that the hyperfine dipole matrix elements sum to the larger
fine structure dipole matrix elements. In fact, for lower states with J = 0, it can beshown that all ground magnetic sub-levels experience equal total dipole coupling to theupper states. However, the resonant frequency dependence ωak in the polarizability(Equation 2.62) indicates that the magnetic sublevels in different nondegenerate upper
hyperfine states will yield different contributions to the clock state polarizability. The
larger the laser detuning relative to the hyperfine splitting (typically many orders ofmagnitude larger), the smaller this effect will be. Discussed more in Chapter 5, thissmall effect results in a mF dependent polarizability which is included in the dipole
polarizability tensor. Furthermore, because the 3 P0 clock state is not perfectly J =0 (due to hyperfine mixing), the magnetic sublevels of the 3 P0 F = 9/2 clock state
have different polarizabilities. In this same spirit, the weak nondegeneracy of magnetic
sublevels in a bias magnetic field and of motional states of the confined atom yield
differential polarizabilities. These splittings, orders of magnitude smaller than hyperfine
splitting, yield effects which are negligible at the current level.
We have considered only the dipole polarizability interacting with the second
order term in the electric field. Higher order multipole interactions as well as the82
atomic hyperpolarizability interacting with the fourth order electric field term will bebriefly discussed in Chapter 5.
Perhaps one of the biggest weaknesses of the dipole polarizability calculation isthe accuracy of the state decay rates listed in Table 2.1. Unlike the well-known transition
frequencies, few decay rates are known at the percent level. With the linear dependenceof the polarizability contributions on these decay rates, knowledge of the polarizability
better than the percent level is difficult. The lowest lying states typically contribute themost to the polarizability in the near-infrared region we are most concerned with for
confinement. Improved measurements of these state decay rates will further improve
the polarizability calculation.
Finally, as seen clearly from Table 2.1, the calculation above includes dipole polarizability contributions from states with principal quantum number, n, as high as
11. Of course, all higher lying states actually contribute (to a lesser degree), including
Rydberg states and the continuum above ionization. The relative importance of suchcontributions varies, and cannot be overlooked. As a straightforward estimate of thesehigher-lying contributions, we first define the oscillator strength for a given transition,
related to the dipole moment [118]:fak =2 ωak m|dak |2
3 ~e2(2.78)

where e(m) is the electron charge (mass). Closely related to the dipole moment squared,
the oscillator strength (a dimensionless quantity) obeys the Thomas-Reiche-Kuhn sum
rule [119]:X

fak = N

(2.79)kwhere N is the valence electron number (for Sr, N = 2). Here the sum is over all
higher lying states, k, including Rydberg states and the continuum. By summing up
the oscillator strengths for the transitions listed in Table 2.1, we can determine theresidual contribution of the unlisted states to the oscillator strength sum of 2. Using

83
the dipole moments calculated from Table 2.1, the sum of oscillator strengths for theP
1 S clock state from the nsnp 1 P states (up to n = 11) is
f1 S0 ' 1.99. For the0
1
3P

0 clock state, the combined contributions from the listed

gives

P

3 S , 3 D , and 3 P states
1
1
1

f3 P0 ' 1.28. In the 1 S0 case, the sum is ∼ 2 predominantly because of the verystrong dipole coupling to the low lying 5s5p 1 P1 state. As a result, the effect of higher
lying discrete states and the continuum on the 1 S0 polarizability are relatively small.
However, in the 3 P0 case, the total oscillator strength contribution from higher lying
states is non-negligible.
As a simple estimate of the effect on the polarizability, we can assume that all of
the residual oscillator strength for each state is concentrated at the ionization energy,
which corresponds to an angular frequency of ωak = 8.65 × 1015 (rad/s) from the 1 S0clock state and ωak = 5.95 × 1015 from the 3 P0 clock state. We first consider thepolarizability in the limit λ → ∞, where the dynamic polarizability simplifies to thestatic polarizability. Using only the states in Table 2.1, the static polarizability of 1 S0
(3 P0 ) is found to be 191 au (351 au) (1 atomic unit of polarizability is 1.64878 × 10−41
in the SI system). By including the residual oscillator strength contribution at theionization threshold, the 1 S0 (3 P0 ) static polarizability is found to be 192 au (455au). As expected, the 1 S0 static polarizability is barely changed, but the 3 P0 static
polarizability is increased by more than 30%. This change puts the values of the static
polarizability in very good agreement with the currently accepted values of 197.2(2) au
and 458.3(3.6) au [20]. However, the effect at near infrared wavelengths is also dramaticfor 3 P0 . As shown in Figure 2.13, using only the states in Table 2.1, a crossing of the 1 S0
and 3 P0 polarizabilities occurs at 805 nm, close to the experimentally observed valueof 813.4 nm. However, the inclusion of the residual oscillator strength at the ionizationthreshold moves that zero crossing far away from the experimentally observed value,
implying that the higher lying contribution is not accounted for properly by this simple
estimate. Note that the static polarizability would be less sensitive to the details of

84
these higher contributions, because these high frequency resonances are far detuned
from the limit λ → ∞.
A more proper and sophisticated inclusion of these high lying contributions is difficult, mostly due to the lack of knowledge of the oscillator strength spectral distribution
for Rydberg states and the continuum. Some experimental and theoretical investigationin this area has been conducted for Sr [120, 121, 122, 123, 124, 125, 126, 127, 128, 129].
By approximating the oscillator strength spectral distribution for Rydberg states andthe continuum as reported in the experimental work of [120] corresponding to the 5s5p
3 P - 5snd 3 D Rydberg series, further polarizability calculations showed qualitatively

similar results to those described in the previous paragraph. Unfortunately, knowledgeof continuum resonances in the oscillator strength spectral distribution is sparse, which
could play an important role.
One approach to including all relevant contributions is making a full ab-initio
calculation of the electronic wave functions and the corresponding transition energies
and coupling matrix elements. The calculation can include a finite, spatial boundaryaround the atom, so that the eigenstates always remain discrete, rather than blending
into a continuum. A complete basis set can be established so that a properly converging
calculation of a quantity such as the polarizability includes all relevant contributions,comparable to a free space atom calculation including both Rydberg states and thecontinuum [130]. Most of these calculations involve designing the proper system Hamiltonian and finding the wave functions by solving an effective Schrodinger equation, often
utilizing perturbation theory. While these calculations are very sophisticated and canbecome complex, in many cases it is easier to solve ab-initio for the entire polarizability
contribution than trying to solve for just the higher lying contributions and add theseto the contributions from states with sufficient experimental data [131].
One well known example of the importance of continuum contributions is theCs microwave clock transition. Agreement between some theoretical and experimental

85
results on the size of the blackbody radiation (BBR) induced clock shift were in disagreement with other theoretical and experimental results [132, 133, 134, 135, 136, 137, 138].
The disagreement, exceeding the 1×10−15 level, was significant considering the role of Cs
in defining the SI second and the projected inaccuracy of Cs fountain systems at 10−16 .
The discrepancy was illuminated by ab-initio calculations which showed the disagreement among theoretical values originated from the lack of continuum contributions in
the clock state polarizability for several semi-classical calculations [139, 140, 131]. While
it is unclear if technical details caused the discrepancy in experimental values, these calculations helped guide the accepted BBR shift value. For the case of Sr, a complete
basis calculation of the Sr dynamic polarizability has been made [136] yielding a crossing
point of the two clock state polarizabilities at 795 nm. Further ab-initio calculations,perhaps guided by known experimental values, should provide more knowledge about
the Sr polarizability (dynamic and static) and structure details. This information will be
useful for several reasons, perhaps most prominently to aid in reducing the uncertaintyof the BBR-induced shift of the Sr clock transition. As shown later in this thesis, thisuncertainty currently limits the realizable accuracy of the Sr optical frequency standard.

2.6.3

1-D Lattice Confinement

Having considered the atomic dipole polarizability interacting with a generic optical potential, we now look at a specific case of trapping: the 1-D optical lattice. Multiple
flavors of the 1-D lattice exist [141]. Here we consider a linearly polarized optical beam
which is focused to a minimum beam radius. After propagating some distance beyond
the beam waist, the beam is retroreflected without polarization rotation and with theappropriate optics so that the returning beam overlaps and maintains the same beam
parameters as the original incident beam (see Figure 2.14). By summing together theelectric fields of the two counterpropogating beams travelling in the x direction:~ = E~0 cos(kx − ωt) + E~0 cos(−kx − ωt)E(2.80)

86

Figure 2.14: Schematic of the optical layout for the 1-D optical lattice. The lattice laser
at 813 nm is tightly focused with an achromatic lens and retroreflected with a curved
mirror whose radius of curvature matches the optical wavefront curvature. The atoms
are confined at the trap focus. Interference along the trap axis and the Gaussian beamprofile perpendicular to the trap axis give pancake shaped lattice sites. Many atoms
are confined in each site and many sites are occupied. The clock laser propagates along
the trap axis and the lattice retroreflector has high transmission (∼ 99%) of the clock
laser at 698 nm.

87
it is straightforward to show that the time average of the square of the electric field forthe resulting standing wave is:
h|E|2 i = 2|E0 |2 cos2 (kx)(2.81)

Here hi denotes the time average. Referring back to the total trapping energy (~ωa ) in
Equation 2.63, and assuming a Gaussian beam profile with 1/e field radius of w0 , thetime averaged trapping potential energy for an atom in state |ai is found to be:h|Ua |i = −αa4P
0 cπw02(2.82)

where P is the one way optical power of the incident optical beam, 0 is the permittivityof free space, c is the speed of light, and w0 is the 1/e probe beam field radius. This peak
trap depth is modulated by the cos2 (kx) term along the optical axis, and has a Gaussianenvelope perpendicular to the optical axis as given by the beam’s Gaussian profile. We
have assumed that the index of refraction around the atom is unity. Equation 2.82 gives
the total trap depth, expressed as energy, for the lattice confined atoms. By dividing
by Boltzmann’s constant kB , we express this trap depth as a temperature. Obviously,
to confine a substantial fraction of the atomic sample, the sample temperature must be
less than the trap depth temperature.
With cos2 confinement along the trap axis and Gaussian confinement orthogonal
to it, we now approximate confinement in all directions as harmonic. This is done in
the standard way, by setting the trap “spring constant” in the ith direction equal to
the second derivative of the trap depth profile with respect to the ith direction, andevaluating this second derivative at the trap minimum. These trap spring constants canpthen be related to the trap frequencies by the standard relation ωtrap = ktrap /m withm the atomic mass. By doing so, we get the trap frequencies along (orthogonal) to thelattice axis as flong (ftrans ):ωlong
1flong ==2πλr

2hUa im(2.83)

88
ftrans =ωtrans
1
=
2π
πw0

r

hUa i
m

(2.84)

These are the trap frequencies precisely at the trap focus. For a more general expression
giving the trap frequencies away from the center of the focus, see Reference [142]. The
trap frequencies ωlong and ωtrans can be used for the trap frequency ω in Equation 2.28
in their respective directions. Thus, these frequencies give the energy spacing between
motional states of the confined atom in the different spatial dimensions.

2.6.4

Benefits of 1-D Lattice Confinement

In Section 2.5.2, we suggested that atomic confinement in an optical potential
could be made uniform and defect-free for large atom numbers. This is in contrast to
traditional crystal lattices which suffer from lattice defects that create inhomogeneities
in the confining environment. Although the typically weaker confinement in the transverse dimension and atomic confinement away from the trap focus can allow for sometrapping inhomogeneity, these effects are rather small and not particularly prohibitivein the matched potential regime. Overall, the optical standing wave makes for a very
clean, defect-free potential, enabling confinement in the uniform potential regime. Thisis only one of several benefits of using lattice confinement for cold Sr atoms.
In Figure 2.13, we saw that the dipole polarizability of the two clock states havethe same value around 805 nm. Experimentally, we have confirmed that the wavelength
corresponding to the realization of matched potentials for the two clock states (sometimes referred to as the magic wavelength λmagic ) is 813.428 nm [23, 22]. This nearinfrared wavelength is relatively convenient for generating optical powers exceeding 1
W using optically pumped Ti:Sapph lasers or diode lasers followed by tapered diodeamplifiers. Furthermore, we have experimentally observed that the sensitivity of theclock transition to excursions of the lattice laser away from the magic wavelength isapproximately 1 GHz of lattice laser excursion to 1 Hz of clock transition shift (for ourtypical operating power of the lattice laser) [21]. This is in agreement with Figure 2.13,

89
and means that using standard techniques to frequency stabilize the lattice laser at<MHz level, we can ensure that the lattice laser operating at the magic wavelength will
yield AC Stark shifts of the clock transition <1 mHz (1 × 10−18 of the clock transition
frequency). Of course, at this level, we must be careful to consider higher order effects.
Nevertheless, confinement of 87 Sr in an optical lattice is well suited to operating in thematched potential regime. It is also worth noting that because the clock states haveJ = 0 (nearly J = 0 for 3 P0 ), the Clebsch-Gordan coefficients (or Wigner 3−j values) for
all optical polarizations are identical, meaning that the atomic confinement is not very
sensitive to rotations of the lattice polarization, further facilitating the experimental
realization of the matched potential regime.
Experimentally, it is straightforward to provide several hundred mW of latticelaser power focused to a 65 µm beam radius, corresponding to single beam laser intensities of 5 − 10 kW/cm2 . Using Equation 2.82 together with the calculated atomic
polarizability around λmagic , we can straightforwardly achieve trap depths of 10-20 µK.
This depth could be enhanced using an optical power build-up cavity around the atoms[143]. Since our laser cooling provides atomic samples at the µK level, the achievabletrap depth facilitates trapping a large atom number from our laser cooled source. Furthermore, the Stark shift of the 1 S0 -3 P1 cooling transition in the lattice at λmagic issmall enough that proper choice of detuning of the cooling laser can still yield efficientcooling. This means that cooling can occur simultaneously during loading of the opticallattice, which enables atoms which “roll” into the conservative lattice potential to becooled before “rolling” back out.
With this kind of trap depth, we see from Equations 2.83 and 2.84 that longitudinal and transverse trap frequencies exceeding 40 kHz and 150 Hz, respectively, canbe achieved. As shown in the next chapter, coherent interrogation of the 1 S0 -3 P0 clocktransition for lattice trapped atoms has yielded transition linewidths, γ, of a few Hz.
This means that the 1-D lattice confinement realizes the well-resolved sideband regime

90
for all dimensions. Furthermore, with a clock transition recoil frequency of νr = 4.7
kHz, we can operate in the Lamb-Dicke regime in the longitudinal dimension. For thisreason, the clock transition is probed with a laser k-vector aligned parallel to the latticeaxis. In doing so, we achieve both the well-resolved sideband and Lamb-Dicke regime,
critical for high precision spectroscopy.

2.6.5

Further Details of 1-D Lattice Confinement

In Section 2.6.3, we looked at how the 1-D lattice provides harmonic confinementof Sr atoms. This confinement was shown to be approximately harmonic only by Taylor
expanding the real potential around the trap minimum in each dimension. In the longitudinal direction, if we leave the full cos2 (kx) term in the 1-D confinement Hamiltonian,
the Schrodinger equation can be transformed to be written as Mathieu’s equation. The
eigen-energies are found from well-known solutions to this equation. An example of
the resulting energy spectrum is shown in Figure 2.15. The periodic cos2 (kx) potential
results in a band structure, where the quantum states have finite energy bandwidths.
Figure 2.15 corresponds to a trap depth that yields approximate harmonic trap frequencies of 80 kHz. In the matched potential and well resolved sideband regimes, while
the anharmonicity has no appreciable effect on the purely electronic carrier transition,
red and blue sideband transition frequencies depend on the initial quantum state |ni.
As a consequence, a thermal distribution of many motional states leads to first order
sidebands with a range of different frequencies, and their maximum frequency separation from the carrier being ωlong [21]. By enabling spectroscopic discrimination, thisanharmonicity could prove beneficial for studying the dynamics of individual motional
states.
Another consequence of confinement in a finite, periodic potential is the possibility
for quantum tunnelling between lattice sites. Such tunnelling can lead to two pernicious
effects. The first is that atoms escape the potential, spatially lost to spectroscopic

91

E/Erecoil @ 813 nm

160
140

Etrap
~20 µK

120
100
80
60
40
20
0

3
2
1
0

(n)

Figure 2.15: Atomic confinement energy band structure due to the anharmonic andperiodic cos2 (kx) potential. The motional state quantum number, n, of the levels is
indicated. Here the trap depth ∼ 20 µK corresponds to a lattice laser intensity of
I = 10 kW/cm2 .

92
probing. More significantly, the corresponding band structure can shift the carriertransition frequency from the pure atomic transition frequency. Furthermore, the finite
bandwidth of the motional states leads to line broadening. Both of these effects can beconsidered as residual Doppler and recoil effects associated with the delocalization of
the atom due to quantum tunnelling. These effects have been estimated for the case of
Sr in a 1-D optical lattice [144]. It has been determined that to keep them at or below
the 10−17 fractional frequency level, the lattice depth should be at least 50 to 100 Er(where Er = ~ωr for the magic wavelength lattice photon at 813 nm) to suppress thesetunnelling effects. Alternatively, introduction of a term in the system Hamiltonian withlinear spatial dependence can lift the degeneracy between neighboring lattice sites andmore strongly localize the atom. This can be accomplished simply by aligning the 1-D
lattice axis along gravity (as is roughly the case in our experimental setup). In thiscase, the eigenstates are referred to as Wannier-Stark states, typically organized into aladder structure, with each state separated from its neighbor by the gravitational energy
difference. Transition shifts and broadening are strongly suppressed in this case, and it
is estimated that lattice depths of only 5-10 Er are sufficient to keep these effects below
10−17 [144].
As seen in the previous section, confinement in a 1-D lattice can be very spatiallyasymmetric. For our typical operating conditions, flong ' 40 kHz and ftrans ' 150 Hz.
The much weaker confinement in the transverse axis creates some additional complications. First of all, the weaker confinement means that the atomic wavefunction has alarger spatial extent (see characteristic length x0 in Section 2.5.2). Because flong becomes smaller away from the optical axis [142], this larger transverse spatial extent can
result in longitudinal spectroscopic sidebands which are smeared out, with a maximum
frequency flong [21]. The details of the smearing depend on the atomic sample temperature (which determines the population of motional states and thus the spatial extent,
for more details see [16, 145]). This effect and the anharmonicity described above yield

93
broad asymmetric sideband spectra described more fully in Section 3.4.3
Perhaps a more significant consequence of the weak transverse confinement isthat probing along that direction is not in the Lamb-Dicke regime. Although we try toprobe along the strong confinement axis, for both practical and fundamental reasons,
we can never perfectly do this. As a result, some component of excitation occurs in
the transverse dimension. This is perhaps most notably observed through the Rabi
excitation rate of the confined atom, as given in Equation 2.49. As seen in Figure 2.16,
out of the Lamb-Dicke regime, the purely electronic excitation rate Ωnn can become
strongly diluted as a function of the initial motional state |ni. For a Boltzmann thermal
distribution occupying many transverse motional states, significant inhomogeneity in
the Rabi frequency for different motional states can lead to a strongly damped Rabi
excitation for the total atom ensemble [94, 146, 147]. This inhomogeneous excitation
will be discussed more quantitatively in Section 5.4.4. This effect is present for both thetransverse and longitudinal dimensions, but because we are in the Lamb-Dicke regime
longitudinally, this effect is much smaller there.
Finally, we have shown how the atoms can be confined optically by considering
atom-light interactions in the dispersive regime. Of course, even far off resonance, somephoton absorption occurs. This leads to residual heating which transfers thermal energy
to the atomic sample so that it is no longer confined in the lattice. In the far detuned
case, the photon scattering rate (via spontaneous emission) is (see Equations 2.7 and2.8 or see also [148]):
Γscatt =X Γ k Ω2X Γk Uak

k

k

ak
=
4∆2ak

∆ak ~

(2.85)

where Γk is the (total) spontaneous decay rate from upper state k, ∆ak is the (angular)transition detuning, and in the last equality we have used Equation 2.60 for the Stark
energy term Uak . Under current experimental conditions, the atom spends the bulk of
its time in the lattice occupying the ground state. The ground state photon scattering

94(Ωnn/Ω0)

2

0.04
0.03
0.02
0.01
0.00
0

50

100

150

200

motional state quantum number, nFigure 2.16: The diluted Rabi frequency (squared) for purely electronic excitation froma given motional state with quantum number n. The Rabi frequency is normalized tothat of an atom in free space at rest. Here the atoms are not in the Lamb-Dicke regime(η ' 5.3), as is the case for atomic interrogation along the weak transverse axes of the
1-D lattice (as shown here ftrans = 170 Hz).

95
contribution is dominated by the very strong 5s2 1 S0 - 5s5p 1 P1 transition. Assuming
each scattering event yields sufficient gain in thermal energy to heat the atom outof confinement, for typical experimental conditions, the trap lifetime due to photon
scattering from the ground state (τ = 1/Γscatt ) exceeds 5 s. This lifetime is morethan sufficient for spectroscopic probing of Fourier limited spectra with state-of-the-art
resolution (see next chapter). As the probing times evolve to longer times, this lifetime
may become an issue. Furthermore, with longer probing times, the atom spends moretime in the excited clock state. This requires consideration of the photon scattering ratefrom 3 P0 . Using only the dominant contribution from the 5s6s 3 S1 state (and typicaloperating parameters), the trap lifetime of 3 P0 atoms also exceeds 5 s.
Another important contribution to finite trap confinement time comes from collisions between the trapped Sr with the hot vacuum background gas. Higher vacuum
lowers the density of the background particles and thus the trap loss rate. The thermalenergy of these hot gas particles is so large compared to the confinement energy, inmany cases it is assumed that each collision successfully removes a Sr atom from thetrap [149]. This assumption is not always valid, and quantum diffractive background gas
collisions can play a role [150]. Accurate calculations of the loss rate due to backgroundgas collisions require some knowledge of interaction potentials between the trapped andhot background particles (e. g. C5 or C6 coefficient). Here, empirical measurements canplay an important role in determining this loss rate. Some experimental data exists forSr [64, 115, 60]. Assuming a background-gas-limited-lifetime that is independent of thetrap depth, application of the measurement by [64] to our typical vacuum at the trap(∼ 2 × 10−9 torr) yields a loss rate of 1 s−1 . This is in reasonable agreement with ourobserved trap lifetime of 1 s, indicating that background gas collisions could be playing
the limiting role in our trap lifetime. Other physical mechanisms worth consideration
including tunnelling loss and atomic heating due to phase or amplitude noise on the
optical potential.

96

2.7

State Preparation via Optical Pumping: Nuclear spin polarization
In the case of 87 Sr, I = 9/2 meaning that the clock states with F = I have amagnetic state degeneracy of 2I + 1 = 10. Because J = 0, each mF state corresponds
to a unique nuclear spin orientation (mF = mI ). In small or negligible backgroundmagnetic fields, these nuclear spin states are nearly degenerate. After laser cooling on
the narrow 1 S0 -3 P1 transition, we have observed that the ground state 1 S0 population
is approximately evenly distributed among all ten nuclear spin substates. Due to thefact that each magnetic substate has different Zeeman and lattice Stark dependence,
this mixed population is not ideal for high accuracy and high precision spectroscopy.
For this reason, it is desirable to interrogate isolated spin states by applying a magnetic
field to split the nuclear spin state degeneracy. Sequential interrogation of opposite
spin states (±mF ) has the added advantage of measuring two transitions whose averagefrequency is independent of some perturbing fields, like the B-field (to 1st order). Since
the spectroscopic signal scales with atom number, it would be efficient to push all of theatomic population into the nuclear spin state to be probed. This also reduces unwantedline pulling effects due to off-resonant transitions from neighboring spin states in a bias
magnetic field. This state preparation preceding spectroscopy can be accomplished by
optical pumping to one or more nuclear spin states.
Optical pumping has already been discussed in this chapter in different contexts.
In Section 2.2 on laser cooling, we discussed unwanted optical pumping as the 1 S0 1P

1 transition was cycled with a small spontaneous decay from

1P

1 to

1 D , eventually2

populating the 3 P states. In Section 2.4, we discussed the role of the stirring laser for
laser cooling 87 Sr on the 1 S0 -3 P1 transition. One of key roles of the stirring laser wasthat of optically pumping the population, in this case so that the population could be
randomized among the magnetic sublevels. For state preparation, we are interested in

97
optically exciting the atoms where spontaneous decay favors a particular decay route(via the relative sizes of the Clebsch-Gordan coefficient for different decay routes) sothat many pumping cycles move the population to the desired ground nuclear spinstate. Like the stirring laser, we can utilize the 1 S0 -3 P1 transition to accomplish this.
Figure 2.17 shows the results of a Monte-Carlo simulation where the atomic population
is assumed to be initially distributed evenly among all populations [83]. In one case,the 1 S0 F = 9/2 - 3 P1 F 0 = 7/2 transition is driven using π-polarized light. After< 10 photon scattering events, the population has been pumped to an equal mixtureof stretched states mF = ±9/2. In the other case, the 1 S0 F = 9/2 - 3 P1 F 0 = 9/2
transition is driven with pure σ + -polarized light, and the entire population is driven to
mF = 9/2. Switching to pure σ − -polarized light drives population to mF = −9/2. Here,degeneracy among all nuclear spin states has been assumed. In practice, we typically
apply a very small bias magnetic field (< 50 mG) during the optical pumping. We findoptical pumping times of 20-50 ms give sufficient pumping of the population. Detailsof how well this pumping process works experimentally can be seen spectroscopically in
Chapter 5.

98(a) 50population (%)

40
30
20
10
0

-3/2
1/2

m

8
5/2
9/2

4

ph

F

ot
on

-7/2

sc
at
te
r

in

gs

20
16
12

(b) 100

population (%)

80
60

20

-3/2
1/2

m

5/2

4
9/2

ph

F

8

ot
on

-7/2

sc

0

at
te
ri n

20
16
12

gs

40

Figure 2.17: Optical pumping used for nuclear spin polarization state preparation. The
population is assumed to be initially distributed evenly among all spin states. (a) Opticalpumping by scattering π-polarized light on the 1 S0 -3 P1 F = 9/2-F 0 = 7/2 transition.
After ∼ 10 photon scatterings, the population is evenly shared between the mF = ±9/2
states. (b) Optical pumping by scattering σ − -polarized light on the 1 S0 -3 P1 F = 9/2F 0 = 9/2 transition. After ∼ 10 photon scatterings, the population accumulates in the
mF = −9/2 states.

Chapter 3

Coherent Light-Matter Interaction: Hz level spectral linewidths in the
optical domain

3.1

The Need for Atomic and Optical Coherence
As seen in Chapter 2, the spectroscopic probing of an atomic transition is de-~ (e. g. Equation 2.34).
scribed by the interaction term of the Hamiltonian, HI = d~ · E
Coherent excitation of the atomic transition requires the individual coherent evolutionof both the atomic dipole d and the electric field E. The longer that this coherence canbe maintained, the higher the resulting spectral resolution. This is seen in the Rabi
flopping solution for the excitation of a two-level atom (with equations of motion as inEquations 2.44 and 2.45):Ω2
Pe (t, ∆) = 2
sin2Ω + ∆2√Ω2 + ∆ 2 T
2

!
(3.1)

where Ω is given in Equation 2.5, ∆ is the (angular) detuning from the atomic transition,
and T is time. For convenience, we choose ΩT = π (pi pulse). The resulting sinc2 spectral feature has a Fourier-limited full width at half-maximum equal to ∆νRabi ' 0.89/T .
Longer times T give narrower features ∆νRabi . Eventually decoherence limits the achievable coherent interaction time T . Regardless of the type of spectroscopy employed, often
a primary goal of very high precision spectroscopy is to probe the atomic sample fora maximum time. For atomic frequency standards, the enhanced spectral resolution
with long timescale interactions enables very high measurement stability (Equation

1001.1), which subsequently improves the precision of systematic shift measurements andthus the accuracy. In some cases, like line-pulling from nearby transitions, the size ofthe shift itself decreases with narrower linewidths. Also, we saw in Section 2.5.4 that
Doppler and recoil effects are reduced with confinement in the well-resolved sideband
regime. The narrower transition linewidths relax the potential depths needed to operate
in this regime. For all of these reasons, a good deal of effort is made to permit longcoherence times for both the atom and the probing electric field.

3.2

Atomic Coherence
The coherence relevant for an atomic frequency standard focuses on the two clockstates (and their relative eigen-energies). This coherence must be observable in a reference frame where the probing optical wave is coherent. These important criteria can be
frustrated by a multitude of noise processes coupling to the atoms. Among these, motional effects can play a significant role. The recoil and Doppler effects we have alreadyconsidered in previous sections manifest themselves in a variety of shift mechanisms andinhomogeneities across a thermal velocity distribution of atoms. Although some typesof spectroscopy remain less sensitive to these effects, none are completely insensitive.
The reduction of the effect itself, by reducing the velocity distribution and by confining the atoms in the well-resolved sideband and Lamb-Dicke regime, is critical. The
success of single-trapped ions and now lattice-trapped neutral atoms in achieving thehighest resolution optical coherent spectroscopy [151, 152] is made possible through theelimination of motional effects due to the quantum confinement of these cold particles.
A key ingredient is uniform confinement, where the two clock states are differentially
unaffected by the confinement.
Many mechanisms can perturb the relative phase evolution of the clock statesand decohere the atomic sample. One such mechanism is collisions between the cold
Sr atoms, which leads to density dependent frequency shifts of the measured transition

101
frequency. Up until recently, this effect has been unobservable. In Chapter 5, using
the high measurement resolution resulting from a direct optical comparison between
optical standards, we will see non-negligible collisional effects in the dilute Sr gas anddiscuss how these effects can be further minimized. Another perturbing mechanism isspatially or temporally varying fields, which can lead to random phase accumulation
which decoheres the atomic sample as the atoms sample these fields in space and time[153]. We work to minimize such potential perturbations, including: using low magnetic
susceptibility stainless steel vacuum chambers, electrically grounding the chamber, using
electromagnetic trim coils to zero residual bias fields (designed with spatial homogeneity
in mind) driven by low noise current sources, using optically thick enclosure around
vacuum chamber (curtains) to reduce stray optical fields, using mechanical shutters toblock unwanted residual laser fields during probing, etc.
Finally, while ideal lattice confinement removes most motional problems, noisein the trap potential itself can re-introduce these problems. For example, phase noisein the lattice standing wave (e. g. shaking lattice retroreflector) may introduce sizeable
Doppler effects during spectroscopy. We utilize high stability optical mounts for thelattice and probe lasers, and a large fraction of the optical path for these beams isshared, allowing for partial common mode rejection of vibration. We typically float
the optical table on which the spectroscopy takes place, using standard compressed
air legs with an isolation roll-off frequency of a few Hz. Furthermore, we mounted a
PZT on the lattice retroreflector, and using the lattice standing wave as one arm ofa homodyne Michelson interferometer (the other arm serving as a reference arm), we
have actively stabilized the retroreflector position along the lattice axis (by monitoring
optical phase of the interferometer). For measurements described in this chapter, thisactive stabilization did not make noticeable improvements and is typically not used. We
also took care to avoid amplitude noise in the lattice trap by actively stabilizing thelattice optical power incident on the vacuum chamber viewport.

102

3.3

Optical Coherence: Laser Frequency and Phase Stabilization
Generation of coherent, single-frequency electromagnetic radiation has a rich his-

tory in the radio, microwave, and optical domains. The invention of the laser was alandmark step towards this goal for optical frequencies. Lasers, usually consisting ofan excited optical gain medium interior to an optical resonance cavity, can generatehigh intensity radiation with relatively high spatial and temporal coherence. The laser
radiation frequency is given by a resonant frequency of the laser’s optical cavity. This
resonant frequency is susceptible to a variety of noise processes originating from thedriven gain medium, other intracavity optical elements, optical path length changes of
the round trip cavity length, and amplified spontaneous emission. These processes give
finite temporal coherence to the laser output, with a coherence time often insufficient for
the very high resolution desired in precision optical spectroscopy. With the possibility to
reduce all of these noise processes, a much more well-defined resonant frequency can beachieved in a properly designed, purely passive optical cavity. Highly coherent opticalradiation can be obtained by stabilizing the frequency output of a laser to the passive
optical cavity resonance. This stabilization typically exploits electronic feedback to thelaser. Several schemes for deriving the stabilization signal exist, the most popular forhigh performance laser phase and frequency stabilization being the Pound-Drever-Hall(PDH) technique [77]. With the wide use of PDH stabilization in different laboratory
and technical environments, a basic review of this technique will not be given here.
The interested reader is referred to several useful references in the literature, dealing
both with the PDH technique and laser stabilization in general [77, 154, 155, 156, 97].
Rather, I give here a partial list of important design considerations relevant to laser
frequency stabilization at the current state-of-the-art.

103
3.3.1

Laser Stabilization Design Considerations

PDH locking has several advantages over many alternative stabilization schemes.
By utilizing the reflected signal (“composed” of both the cavity reflection and the cavity
leakage field), PDH stabilization accesses optical phase information at Fourier frequencies above the cavity linewidth (δνcavity ) and optical frequency information below it.
Unlike the transmitted signal, the feedback bandwidth is not limited to the inverse of
the cavity storage time [77]. Furthermore, because detection is moved to a high modulation frequency where the laser intensity noise spectral density can approach the shotnoise, PDH locking is typically less sensitive to intensity fluctuations [77]. The PDH
error signal is dispersion shaped, and the region between maximum and minimum canbe approximated by a line whose slope, called the discriminator slope, is given by [154]:√
8 Pc PsD=δνcavity(3.2)

where Pc is the optical power in the carrier, Ps is the optical power in the one sideband,and it has been assumed that the cavity reflection contrast is unity. The fundamental
noise process limiting PDH locking is photon shot noise, with a white spectral density.
The shot noise sets a limit on the laser frequency noise spectrum which is achievableusing PDH locking, and is given by dividing the shot noise by the discriminator slope.
This frequency noise amplitude spectral density of shot noise can be written as [154]:√sf =hc ∆νcavity
√
4
λPc

(3.3)

where λ is the laser wavelength. Note that for true white frequency noise, the resulting
laser spectrum is Lorentzian with a full width at half maximum given by πs2f [157, 97].
From Equation 3.2, it is clear that in PDH locking, a narrower linewidth cavity canyield a more stable laser (less frequency noise and narrower laser linewidth). It is withthis motivation that high reflection, low loss mirrors are used in optical cavities forstate-of-the-art laser stabilization, with cavity finesses approaching 106 (cavity finesse,

104
F = ∆νF SR /∆νcavity , where ∆νF SR = c/2L and L is the cavity length). According toEquation 3.2, lower frequency noise could also be achieved using a stronger laser power(higher shot noise signal to noise ratio - S/N ). Unfortunately, in practice, this is not
generally true for at least two important reasons. It is common that as optical power isturned up, the S/N becomes limited by technical noise which scales with power, limiting
Equation 3.2. Second, optical power buildup in high finesse cavities can result in very
high circulating powers which can be weakly absorbed by the dielectric thin films of thecavity mirrors. This results in heating which causes cavity length drift/noise and thus
degrades the stability of the cavity resonance. How much absorption occurs depends
on individual dielectric coatings and surface contaminants. In one case, a cavity withfinesse F ≥ 150, 000 experienced a cavity resonance shift of 1 Hz per 1 µW of incident
power [158]. To this end, the optical power incident on the cavity (or the reflected ortransmitted power) can be stabilized to limit drift/noise from this effect. It should be
noted that the mirrors used in these high finesse cavities have optical coatings with very
low transmission and absorption/scattering losses. Ideally the absorption/scattering
losses would be zero, but are usually not smaller than a few parts per million (ppm).
With smaller and smaller transmission losses for high reflectivity, the non-negligible
absorption/scattering losses in the cavity mirrors result in less than unity reflection
contrast. This degrades the PDH error signal. In this more general case, the photon
shot noise limited frequency noise amplitude spectral density can be found to be:sπ ∆νcavity 2hc(2Ps + Rimp Pc )sν (f ) = 2(3.4)
8
λPc Psrt1 F
where r is the amplitude reflection coefficient of both mirrors of the passive FabryPerot cavity, t1 is the amplitude transmission coefficient of the input mirror, and Rimp
is the fraction of the resonant carrier power reflected back due to imperfect “impedance
matching” of the cavity.
A very high finesse cavity can sometimes have a linewidth much narrower than

105
the power spectrum of the laser needing to be stabilized. This can lead to several
complications. In some cases, pre-stabilization of a laser to a broader linewidth cavity
is used to spectrally narrow the laser so that the subsequent laser radiation incident
on the high finesse cavity has a spectral linewidth similar to or less than the highfinesse cavity linewidth [158, 159]. Such an approach avoids the error signal distortion
which otherwise occurs, helping to keep detection and feedback operation in the linear
regime. This helps make characterization and optimization of the cavity and cavity
lock more straightforward. Furthermore, it can reduce the probability of saturationin the high gain electronic feedback. However, in many cases, this approach is notessential [160]. Several groups developing stable laser sources for optical frequency
standards have chosen to lock directly to a high finesse cavity and avoid the complexityof a pre-stabilization cavity [161, 162, 163, 164, 165, 166]. Note that these issues areless relevant for intrinsically frequency stable lasers like Nd:YAG MISER (Monolithic
Isolated Single-mode End-pumped Ring) lasers and single mode fiber lasers, whose freerunning linewidth can sometimes be below the 10 kHz level.
A major weakness of PDH locking is that the required laser phase modulation cannever be realized perfectly, but rather there is always some level of residual amplitude
modulation (RAM). Time dependent RAM introduces measurement noise where it isleast wanted: at the detection frequency. This typically limits the locking performance
to worse than the photon detection shot noise, and unfortunately RAM can be quite
large (1% level) [167]. There are many physical origins of RAM. Some of these include
etaloning effects in the phase-modulation crystal, time dependent crystal birefringence(e. g. temperature induced), spatial inhomogeneity of the modulation field in the crystal,piezo-electric response of the modulation crystal causing beam steering, amplitude noisein the RF drive, and vibration of optical components. Fortunately, steps can be taken
to reduce these mechanisms. Active control of amplitude modulation by feedback on abias electric field in the electro-optic (EO) crystal has demonstrated real-time zeroing

106
of RAM to reach shot noise limited detection [168]. Furthermore, two tone modulation
can reduce RAM effects. We have generally taken a passive approach to limiting RAM.
For example, some steps we have taken include: temperature stabilization of the electrooptic phase modulation crystal; anti-reflection (AR) coating on EO crystal faces; use ofa crystal with large cross section and large electrodes with center stripe for uniform field
generation at crystal center [169]; 4 axis kinematic mount for EO crystal to periodicallyalign crystal to minimize RAM; a high quality polarizer before EO crystal; opticalisolator after EO crystal; EO crystal with reduced RAM sensitivity (ADP, reduced
piezoelectricity) [167]; low noise RF drive source; mounting of both the EO crystal,high finesse cavity, detection photodetector, and all intermediate optics on a vibration
isolation platform; and detection of the entire optical beam after the EOM on a large
area photodetector.
With a properly designed feedback system, utilizing high bandwidth components
with minimal temporal delay and phase excursions, the PDH error signal is filtered totightly lock the laser phase/frequency to the resonant optical cavity (error signal analysis
can characterize the locking efficacy) [97]. The generation of frequency-stable laser
radiation now transforms into the task of designing an optical cavity with a very stablecavity length (resonant frequency), and this is where a large fraction of the effort is spent.
As a first effort to maintain length stability, the cavity mirrors are mounted (opticallycontacted) to a rigid spacer. The optical cavity is also typically placed in vacuum,
motivated by several considerations. First, by reducing convective and conductive heatflow through air, the vacuum acts as a thermal insulating layer which aids the effort totemperature stabilize the cavity. Temperature stability is critical due to the coefficientof thermal expansion of the material(s) used to construct the optical cavity. Second,the vacuum acts as an acoustic shield, preventing the optical cavity from being shaken
and deformed by airborne acoustic waves. Third, the vacuum helps reduce index ofrefraction fluctuations which translate into changes in the optical length of the cavity.

107
For example, the index of refraction, n, at standard temperature and pressure (STP)
can be related to n somewhat away from STP by the empirical model:(n − 1)T,P = (n − 1)ST P × 0.0013882

PT orr
1 + 0.003671TCelsius(3.5)

Temperature change of 1 o C or pressure change of 5 Torr (the approximate daily pressurechange over 24 hours) can result in changes of the index of refraction ∆n ' 1 × 10−6 .
Remembering the changes in the index of refraction, the cavity length, and the resulting
laser frequency drift can be related simply by:
∆l
∆f
∆n
=
=
n
l
f

(3.6)

such a large ∆n can be prohibitive in obtaining low drift rates of a sub-Hz stable laser.
To estimate the effect while under vacuum, we treat the residual vacuum gas asan ideal gas. From the ideal gas law, the particle density is given by:
ρ=

N
P
=
V
kB T

(3.7)

Furthermore, we treat the index of refraction with the simple model:
n = 1 + αchem ρ(3.8)

where αchem is the gas particle polarizability in units of volume (αchem = α/4π0 , where
α is the polarizability as given in Chapter 2). For a typical polarizability of several
common vacuum gases (αchem ' 1 × 10−30 ), a pressure change of 5 torr gives a change
in the index of refraction of ∆n ' 1 × 10−11 . Thus by operating in vacuum and keeping
the technical vacuum fluctuations below 10−4 torr, index of refraction contributions may
be kept sufficiently small for sub-Hz laser stability and minimal vacuum induced laser
drifts. Note that this simple model may underestimate the vacuum pressure effect, but
experimentally we have observed that a ∼ 10−6 Torr vacuum level is sufficient to reduce
cavity drift levels below thermal induced drifts described below.

108
Finally, before leaving the topic of vacuum, it should be noted that fundamental vacuum fluctuations can introduce index of refraction noise with a relatively highbandwidth. This noise originates in the Poissonian fluctuations of the number of vacuum gas particles which alter the index of refraction in the volume given by the opticalcavity mode. The effect of these fluctuations, expressed as a frequency noise amplitude
spectral density, is found to be [170]:
5/2 5/4sν (f ) = 2παchem cλ5/4 L3/4rρ −√2πλLf /v̄
e
v̄

(3.9)

where f is the Fourier frequency, L is the cavity length, v̄ is the mean gas particle speed,
c is the speed of light, and λ is the laser radiation wavelength. This noise from residual
gas is regularly considered in the context of large interferometers for gravitational wave
detectors. For laser stabilization used by optical frequency standards, the technicalsources of vacuum-induced laser drift/noise usually put a more stringent constraint on
the required vacuum than this more fundamental effect.
One of the key properties considered in the choice of materials used to makethe optical cavity (spacer and mirror substrates) is the coefficient of thermal expansion (CTE). It is, of course, desirable to have as small a CTE as possible. For thisreason, glass materials such as Corning ultra-low expansion glass (ULE) and Schott
Zerodur are commonly used, with typical CTEs as low as 10 parts per billion (ppb) per
K. The vacuum chamber enclosing the cavity is temperature stabilized, where 24 hourtemperature stability at the mK level can keep laser frequency drifts at or below the 1
Hz/s level. Note that it is principally the CTE of the cavity spacer which is of interest, but when the cavity spacer and mirror substrates are made of different materials
with unmatched CTEs, stress-induced deformation of the mirror substrate can makethe overall cavity CTE significantly depend on the mirror substrate CTE [171]. ULE
has the added advantage that the CTE has a zero crossing temperature, typically above
the freezing point of water. Unfortunately, lack of manufacturing control makes it diffi-

109cult to design this CTE zero crossing around a convenient room temperature, howevergroups have worked to operate around the CTE zero crossing of their particular ULE
sample and have seen laser drifts as small as the several mHz/s level [172, 173]. Somematerials cooled to cryogenically cooled temperatures, like crystalline sapphire, exhibit
remarkably small CTEs or CTE zero crossings [174, 175, 176]. Finally, because ULE and
Zerodur glasses are non-crystalline amorphous solids, they experience long-term settlingchanges referred to as material creep. It seems that the material creep rate reduces as
the glass ages. Furthermore, based on the use of a few samples, it seems that ULE
has a smaller material creep rate than Zerodur. In one case, using a year-old Zerodur
cavity at 698 nm yielded a laser drift rate of ∼ 5 Hz/s, which appeared to be limited
by material creep. Beyond this long term material creep, small discrete jumps in thecavity length also occur and are commonly attributed to the settling of the amorphousglass or the optical contacts between the spacer and mirror substrates.
Although the optical cavity utilizes a rigid spacer to hold the mirror spacing
constant, no material is infinitely rigid, and as such is susceptible to elastic deformation. For the case of optical cavities, acceleration-induced deformation can result incavity length changes which can seriously degrade both the short and long timescalefrequency noise of the spectrum of the laser locked to the cavity. The details dependon the acceleration noise spectrum shaking the cavity. The efforts to reduce this effectare two-fold. First, vibration isolation is implemented to reduce the amplitude of theacceleration noise spectrum affecting the cavity. Different groups have utilized different
isolation systems [158, 159, 161, 164], passive or active, commercial or homemade, andthe gravitation wave detection community has a good deal of experience in this area (e.
g. [177, 178, 179]). For optical frequency standards, particular emphasis must be placedon the very pernicious vibrations at low Fourier frequencies. The second, and somewhat more elegant approach to reducing acceleration-induced cavity noise is making
the cavity length less sensitive to acceleration-induced deformation. With the vacuum

110
limiting airborne noise, acceleration is transferred to the cavity at the points where thecavity is physically held and connected to the vacuum chamber and environment. If
the cavity can be designed and held in such a way that length changes from deformations are either reduced in amplitude or enjoy cancellation along different parts of thecavity, then acceleration-induced cavity noise can be reduced. Many cavity mounting
techniques in the last few years thus try to exploit symmetry in the acceleration-induced
cavity stress to reduce the cavity sensitivity. A number of experimental and theoretical(finite-element-analysis) results have been presented [165, 180, 181, 182]. Cross coupling of deformation must be taken into account with Poisson’s ratio. While a typicalcavity held with relatively standard techniques might have an acceleration sensitivity of> 100 kHz/(m/s2 ) (expressed as a resonance shift for a 1 m/s2 acceleration), some cavity designs and mounting have shown sensitivities reduced by more than 100 times. As
discussed in the next section, the cavity we used exploited a vertical-oriented symmetry
to reduce the acceleration sensitivity.
Perhaps the most fundamental limit to cavity length stability is thermal mechanical noise of the cavity components. Any object not at absolute-zero temperature hasthermal energy which on the microscopic scale corresponds to the motion of its constituent particles. This thermal energy off-resonantly excites mechanical modes of themirror substrates, dielectric thin film mirror coatings, and the cavity spacer. In this way,
the cavity length dynamically changes according to the random, Brownian thermal motion, introducing frequency noise to the laser which is locked to it. Thermal-mechanicalnoise has been studied in different contexts, most notably in gravity wave interferometers [183, 184] and recently in rigid cavities for laser stabilization. Thermal mechanicalnoise in the wires used to hang interferometer mirrors can play a limiting role in the detection sensitivity of gravitational wave detectors. The quantitative relevance of thermal
mechanical noise to state-of-the-art cavity stabilization was illuminated by [185]. Using the fluctuation dissipation theorem [186], the authors of [185] derived approximate

111
formulas for the length noise spectral densities of the cavity spacer, mirror substrates,and dielectric thin films. In most cases, the mirror contributions dominates over the
spacer contribution. Expressed as a frequency noise amplitude spectral density (for thecavity), the mirror and dielectric coating thermal mechanical noise is [185]:sc
4kB T 1 − σ 2√sν (f ) =
φη
Lλ
2πf
πEw0

(3.10)

where E is the Young’s modulus of the mirror material, σ is Poisson’s ratio, w0 is thebeam radius at the mirror, φ is the loss of mirror substrate (φ = 1/Q, where Q is
the mechanical quality factor), and η is a correction factor ≥ 1 including the effectof the mirror coating [185]. State-of-the-art cavities at room temperature made from
ULE glass with cavity lengths typically in the range of 10-20 cm have a frequency noise
spectrum (Equation 3.10) which corresponds to a fractional frequency instability limit
in the range of 4 × 10−16 - 1 × 10−15 . This instability limit is consistent with the bestexperimentally demonstrated instabilities (e. g. [158, 185, 159]), and thermal-mechanicalnoise is seen as the current limitation to frequency stabilization at the state-of-the-art.
Equation 3.10 gives a straightforward description of how the thermal-mechanicalnoise can be reduced from its current magnitude. Reduction can be achieved by (1)improved choice of cavity materials (increased E and Q = 1/φ) (2) increased beam
radius w0 (3) increased cavity length L (4) reduced cavity temperature T . Each one ofthese approaches comes with technical difficulties. Frequently-used ULE has Q = 6×104 ,20 times larger than that of Zerodur. Fused silica looks attractive, with Q = 106 [185]and E ' 70 GPa (E approximately similar to that of ULE and Zerodur). However,
the CTE for fused silica is approximately 50 times larger than that of ULE, implyingthat much more stringent temperature control would need to be employed if using fusedsilica anywhere in the cavity. With a similar motivation, the gravitational wave detection
community is considering at least two other mirror substrate materials: cryogenicallycooled crystalline sapphire and silicon. Both have E several times larger than ULE

112(measured at room temperature). Near room temperature, both have Q similar to fusedsilica. However, with cryogenic cooling, both have demonstrated remarkable Q increases,
with Q ' 108 − 109 (near 4 K) [187, 188]. Furthermore, both materials have been shown
to possess remarkably small CTEs at cryogenic temperatures [174, 175, 176]. It must be
remembered, however, that as thermal noise contributions from the mirrors decrease,the contribution from the dielectric coating (summarized by η) may dominate. The
mechanical Q for high quality dielectric coatings is typically 2 − 3 × 103 , and so far thesevalues are roughly independent of temperature [189]. Again motivated by gravitational
wave detectors, work has investigated whether a particular choice of dielectric coating(including coatings with doping) could result in larger Q. Unfortunately, thus far, only
small gains (TiO2 -doping of Ta2 O5 in Ta2 O5 / SiO2 coatings has twice the mechanicalQ ) have been observed [190, 189].
Increasing the beam radius allows further transverse spatial averaging of the thermal mechanical noise. One approach to increasing the effective beam size is by exciting
higher order transverse modes of the cavity [191]. Otherwise, thermal noise reduction bybeam size is limited by the cavity mode radius for mirrors of available radii of curvature.
Another cavity parameter can yield much more noise reduction: of all the parameters inEquation 3.10, cavity length has the strongest dependence, and could thus most reduce
thermal noise effects. Unfortunately, extending cavity lengths beyond those now used(typically from 5 − 20 cm) introduces increased complexity and cost in manufacturing
and isolation of the cavity. Furthermore, for some mounting schemes, the acceleration
sensitivity scales with the cavity length (e. g. [165]), and longer cavities can prove difficult for keeping acceleration-induced cavity length changes down. Nonetheless, somegains may be available here.
Finally, reducing the thermal energy at lower temperatures reduces the thermalmechanical noise. To be productive, large temperature reductions must be made (cryogenic cooling). As mentioned above, several candidate materials could be used. Other

113
important material properties for cooling include the thermal conductivity and heat
capacity. Cryogenically cooled sapphire cavities have already been used to demonstratelaser frequency stabilization at the 1 Hz instability level [175]. Perhaps the primarydifficulty with cryogenic cooling is the ability to do so without introducing excess vibrational noise, deforming the cavity. Cooling to reduce thermal noise holds promise, andexpertise in quiet cooling is already being developed in other fields, such as gravitational
wave detection.
As we move to the next section describing particular details of the 87 Sr clock laserat 698 nm, I mention in passing one or two other design details. To limit RAM, we
discussed the use of optical isolation after the modulation crystal. Generally speaking,etaloning effects from any optical surface can cause problems to the measurement detection. We always implement an optical isolator between the EO crystal and the highfinesse cavity and have seen gains from doing so. We also utilize optical isolation after
beam pick-offs from the light headed toward the cavity. At times, we have also usedisolation immediately before the photodetection. Time dependent electronic biases originating from ground loops, mixers, or input stages to the loop filter used for feedback
should also be monitored carefully.

3.3.2

Sub-Hz Sr clock laser

The clock laser source is a diode laser (Hitachi HL6738MG, AR-coated) in an
external cavity of the Littman configuration operating at 698 nm (see Figure 3.1).
The laser is first pre-stabilized to a simple optical cavity with finesse of ∼ 10, 000 andlinewidth of several hundred kHz. The PDH stabilization is accomplished via feedback
to the laser diode current and the laser cavity piezoelectric transducer (PZT). The
servo bandwidth is 2-3 MHz. The pre-stabilized laser light is first-order diffracted by an
acousto-optic modulator (AOM) and fiber coupled to a platform on which an ultra-stablecavity resides. This platform is mounted on a commercially available passive vibration

114(a) vibration and acoustic isolation
isol

EOM

1/4

1/2

ultrastablecavityout to fiber
coupling

diodepre-stab.
lasercavity 1/4

pbs

pd
EOM
AOM

lens

(b)

Figure 3.1: (a) Schematic of the laser-cavity system used to probe the 87 Sr clock transition. 1/4: quarter wave plate, 1/2: half wave plate, pd: photodetector, EOM: electrooptic modulator, AOM: acousto-optic modulator. The diode laser, in an external cavity
configuration, is electronically frequency locked by two stages of Pound-Drever-Hallstabilization, first to the pre-stabilization cavity and ultimately to the high finesse,
ultra-stable optical cavity. (b) The tapered, high finesse ultra-stable cavity in the vertical mounting configuration. The mirrors are optically contacted on the spacer. The
midplane mounting ring, monolithically integrated to the spacer, loosely rests on threeteflon rods which themselves are tightly held by a Zerodur ring fastened to the vacuum
chamber.

115
isolation unit (Minus K, resonant frequency of 0.5-1 Hz). Both the platform and theisolation unit are within an enclosure lined with acoustic-damping foam. At times, thisenclosure has been temperature controlled at the 100 mK level. On the platform, thepre-stabilized laser light is phase modulated by an electro-optic modulator operating at
5 MHz. Approximately 10 µW of optical power is incident on the ultra-stable cavity
for PDH locking. Stabilization to this cavity is accomplished via feedback to the AOM
and a PZT controlling the pre-stabilization cavity length. The servo bandwidth for thisfinal locking stage is ∼ 100 kHz, limited in part by the acoustic wave propagation timein the AOM. The useful output of the laser is delivered from a fiber port located near
the ultra-stable cavity on the same platform, and utilizes fiber phase noise cancellation[192, 193]. The entire optical setup occupies less than 1 m3 . Further details can befound in [159].
The ultra-stable cavity has a finesse near 250,000 and is 7 cm long (cavity
linewidth of ∼7 kHz). The high reflectivity mirrors are made from ion beam sputtereddielectric coatings, using alternating quarter wave stacks of SiO2 (silica) and Ta2 O5(tantala). The cavity linewidth is determined by a heterodyne cavity ringdown measurement (Figure 3.2). The cavity reflection contrast was measured to be 50 %. By alsomeasuring the cavity transmission (when locked), each mirror was seen to have transmission losses (power) of 6 ppm and absorption/scattering losses of almost 10 ppm.
The laser is locked to the TEM00 transverse cavity mode, as observed by a CCD camera
image of the cavity transmission. For the results shown below, no stabilization of theincident optical power on the cavity was employed.
Both the spacer and the optically bonded mirror substrates are made of ULE. To
maintain a small sensitivity of the cavity length to acceleration, we implemented thefollowing design features. First, the cavity is held at its midplane to achieve symmetricstretching and compressing of the two halves of the cavity during acceleration to suppress
vibration sensitivity [165]. The cavity is mounted vertically to exploit the intuitivesignal amplitude (arb.)

116

0.04
0.02
0.00
-0.02

τ=46 µs

-0.04
40

60

80

100 120 140

time(µs)
Figure 3.2: Measurement of the cavity field ringdown time from the heterodyne interference of the decaying cavity field and a linearly-frequency-chirped reflected laser field.
For this particular ultra-stable cavity, the measured field decay time is 46 µs.

117symmetry in the vertical direction (see Figure 3.1). This mounting is accomplishedby a monolithically attached midplane ring resting on three Teflon rods. Second, withthis mounting design, because the acceleration sensitivity of fractional cavity lengthscales with the cavity length, we chose a somewhat short cavity spacer [165] (7 cm).
Third, the cavity is wider in the middle and tapered at the ends, allowing more rigid
construction without excess material. This cavity was designed in our laboratory andconstructed in conjunction with a dozen other quantum metrology laboratories aroundthe world. It is now commercially available, facilitating 1 Hz laser stabilization to any
interested research lab [159]. The cavity and supporting rods are held in a vacuum
enclosure (10−6 Torr) pumped by an ion pump (2 l/s); the cavity spacer has symmetricevacuation holes perpendicular to the optical axis. Optical access to the cavity was
made through AR-coated, wedged vacuum windows of BK7 glass. The vacuum canis single point temperature controlled to ∼305 K within 500 µK (typical best results)
over a 24 h period. Since the ion pump is not temperature controlled, we installed ablackbody radiation baffle between the vacuum can and the ion pump.
To evaluate the final laser stability, a second cavity-laser system was constructedwith a separate diode laser and a separate ultra-stable cavity mounted on an independentvibration isolation platform in an independent enclosure. Light was transferred fromone system to the other via optical fiber (employing fiber-phase-noise cancellation [192])
and a heterodyne beat between the two stabilized lasers was detected (Figure 3.3). A
linear drift of ≤1 Hz/s of the heterodyne beat was removed by applying a feedforward
linear correction to reduce the drift to less than 50 mHz/s. At 300 mHz resolution
bandwidth (RBW), the laser linewidth is 400 mHz (full width at half maximum). As
the RBW is reduced to 150 mHz, linewidths of 220 mHz can be observed, while somefraction of the carrier power is moved into low-frequency noise sidebands. The fractional
linewidth is below 1 × 10−15 .
We have already discussed general expressions for frequency instability of ansignal power (arb. units)

(a)

118

1.0
0.8
0.6

FWHM=400 mHz
RBW=300 mHz

0.4
0.2
0.0
-10

-5
0
5
frequency (Hz)10(b)
signal power (arb. units)

-7

2x10

-7

2x10

FWHM=220mHz
RBW= 150mHz

-7

1x10

-8

5x10

0
-10

(c)

-5

0
5
frequency (Hz)10-7signal power (arb. units)

1x10

-7

1x10

-8

8x10

-8

6x10

30 s integration
FWHM=2.1Hz

-8

4x10

-8

2x10

0
-15

-10

-5
0
5
frequency (Hz)10

15

Figure 3.3: After stabilization to the ultra-stable cavity, sub-Hz laser linewidths aremeasured by detecting the RF heterodyne beat between two√ similar but independent
laser-cavity systems (frequency axis has been scaled by 1/ 2 for equal contributions
from both laser systems) are shown in (a) and (b) at 300 mHz and 150 mHz resolution
bandwidth, respectively. Spectra with several hundred mHz linewidths are measured.
In (b), a feature as narrow as 220 mHz is resolved, as the carrier power decreases due
to low frequency noise manifest as enlarged sideband power. In (c), the measurement
is integrated over 30 s (with linear drift nominally cancelled), giving a 2 Hz power
spectrum linewidth.

119

fractional frequency stability

(a)
1E-13

1E-14

1E-15
1E-3

0.01

0.1

signal amplitude(arb. units)(b)

1time (s)

10

100

1.0
0.5
0.0

-0.5
-1.0
-1.0

frequency noise
spectrum (Hz/√Hz)

(c)

-0.5

0.0
time (s)

0.5

1.0

1

0.1

0.01
1
10
Fourier frequency (Hz)100

Figure 3.4: (a) The measured fractional frequency instability of the 698 nm clock laser asgiven by the Allan deviation. The solid, black line indicates the instability limit dictatedby the thermal-mechanical noise of the mirror substrates and dielectric coatings in theultra-stable cavity. Note that except for a noise bump near 100 s, from 100 ms to 100s
the laser instability is given by the thermal-mechanical noise limit. (b) Time domain
measurement of the heterodyne beat between two similar but independent clock laser
systems, mixed down to low frequency. The measurement data is shown by the black
dots, whereas a weakly chirped sinusoidal fit is indicated in red. From t = −1 s to
+1 s, the fit matches the data to better than π radians, whereas for |t| > 1 s, the fit
does not match due to excess accumulation of laser phase noise. This indicates thatthe clock laser can provide a coherent optical wave for times at or somewhat exceeding
1 s. (c) The measured frequency noise amplitude spectral density of the clock laser(black trace). The frequency noise contribution from acceleration√ sensitivity of thecavity length is shown in green. The red solid line shows the 1/ f flicker frequency
noise contribution from the thermal-mechanical noise of the ultra-stable cavity. The
black dashed line gives the white frequency noise originating from a technical source:
electronic noise in the transimpedance amplifier used in photodetection of the cavity
reflection.

120
atomic frequency standard. One important characterization of the frequency instabilityof any frequency source is the two-sample Allan deviation, given by [194, 195]:
"

N −1

X
1
σy (τ ) =(fn+1 − fn )22(N − 1)

#1/2
(3.11)

n=1

for N frequency measurements (y) taken with an averaging (gate) time τ . For moredetails on the Allan deviation, and relationships between the Allan deviation and thefrequency noise spectral density, see [194]. Here we report the Allan deviation as afraction of the laser frequency (4.29 × 1014 Hz). The instability of one of the lasers
as measured by the fractional Allan deviation is also shown in Figure 3.4(a). Thismeasurement was taken directly by counting the heterodyne beat under linear drift
cancellation (relative to a stable microwave source). The theoretical estimate of thethermal-noise-limited instability is indicated as a solid horizontal line in the figure.
This modelled thermal noise limit (see Equation 3.10) has nearly negligible contribution
from the ULE spacer itself, while the contribution from the ULE mirror substrates isapproximately 1.5 times that from the dielectric high-reflective coating [185]. Except
for a small noise bump at 100 s, the laser stability from 0.5 to 300 s coincides precisely
with the modelled thermal noise limit.
Laser phase coherence was also observed via time domain measurements. A 15
Hz heterodyne beat signal between the two lasers and its sine wave fit are shown in
Figure 3.4(b), with a linear chirp to account for the simple residual linear drift between
the two lasers. The fit shows that the lasers remain phase coherent within 1 rad at the
optical frequency of 4.29 × 1014 Hz for a period 2 s.
The sensitivity of the cavity length to accelerations was measured by shaking thecavity and observing the additional frequency noise present on the laser when tightly
locked to the cavity resonance. This was also accomplished via an optical heterodyne
measurement, with the system that was not shaken serving as the reference oscillator.
The vertical acceleration sensitivity was measured to be 30 kHz/(m/s2 ). The horizontal

121
acceleration sensitivity was 20 kHz/(m/s2 ) at 5 Hz and it dropped to 5 kHz/(m/s2 ) at 15
Hz because of mechanical isolation provided by the Teflon cavity mounting posts. The
relatively short cavity used here constitutes a compromise between cavity acceleration
sensitivity and the fractional thermal noise contributions (from the mirrors) to thecavity length stability. This compromise facilitates impressive diode laser stability at
the 10−15 level with relatively straightforward vibration isolation. The difference inperformance between this system and that of the highest recorded stability [158] isconsistent with the difference in cavity length that scales the fractional thermal noise.
To see this compromise more quantitatively, Figure 3.4(c) shows the laser frequency
noise spectrum. Below 5 Hz, the laser noise is dominated by thermal noise. Also shownis the laser noise contribution due to cavity acceleration. This is simply the measured
acceleration noise spectrum on the vibration isolation platform scaled by the empiricallydetermined acceleration sensitivity given above. The thermal noise contributes roughlya factor of 2 to 4 more than the acceleration noise. Consequently, the system could befurther improved by using similar, but longer, mounted optical cavities together withfine tuning of the symmetrical rejection of acceleration sensitivity [165]. In this case,the combined thermal and acceleration noise contributions can be kept small enoughfor laser fractional frequency instability at the low side of the 10−16 decade.

3.4

Atomic spectra of the optical clock transition with Hz level
linewidth
With the atomic and optical coherence described above, we are now ready toconsider the coherent atom-light interaction during the probing of the clock transition.

3.4.1

Experimental Setup

The stable laser light is transferred from the enclosed vibration isolation platformby noise cancelled fiber link to a second isolated breadboard in a plexiglass enclosure,

122

PMT

from
lattice laser
gravity

to fs combfrom stablecavityenclosure

to atoms

AOM3

AOM2

AOM1

distribution center
Figure 3.5: Schematic of the distribution of the cavity-stabilized light. From the stablecavity enclosure, the light reaches the enclosed distribution center (via phase-noisecancelled fiber link) where it is split between two phase-noise-cancelled fiber links: one
to the fs frequency comb for counting, and the other to be co-propagated and copolarized with the lattice laser for interrogation of the clock transition. As describedlater, AOM1 is used for frequency stabilization to the atomic transition, whereas AOM2and AOM3 are utilized in the heterodyne Michelson interferometers (dashed line box)
for phase-noise-cancellation over the fiber links.

123
referred to as the distribution center. The fiber phase noise cancellation utilizes aheterodyne Michelson interferometer, where the round trip fiber phase is locked to thephase of a local reference arm [192]. On the distribution center, the light is split into
two beams, one going by fiber-phase-noise-cancelled link to the fs optical frequency
comb to have its optical frequency counted. The second beam goes through a second
fiber-phase-noise-cancelled link to the Sr vacuum chamber (see Figure 3.5). Here thelight is passed through a polarizer and a liquid crystal shutter and is co-propagatedwith the lattice laser using a dichroic mirror. The combined lattice and probe laser
pass through a Glan-Taylor polarizer, ensuring identical polarization of the two beams.
Furthermore, the optical polarization is oriented for π-polarization (relative to the bias
B-field). The lasers are subsequently focused by an achromatic lens (f = 14 cm) into
the vacuum chamber, with their k-vectors oriented about 15 degrees away from gravity.
The collimated probe and lattice beam waists incident on the lens are chosen to give theprobe beam a 1/e field radius at the trap focus which is five times larger than the lattice
focus radius (assuming diffraction-limited focusing). This is done to prevent probe
inhomogeneity along the transverse trap axis due to the Gaussian intensity envelopeof the probe beam. The vacuum chamber windows are AR-coated for 698 nm. At thelattice laser wavelength, 813 nm, the vacuum windows are not optimally AR-coated(transmission is 85% per window), but the lasers are incident at an angle so that no
etaloning occurs. The 813 nm reflection off the first vacuum window is used for intensity
stabilization. After exiting the vacuum chamber, the lattice light is retroreflected bya concave mirror (radius of curvature R = 15 cm and reflection 99% at 813 nm) tooverlap with the original lattice beam and form the focused lattice standing wave. The
retroreflecting mirror is a poor reflector of the probing laser (1% reflection at 698 nm)
to reduce probe standing wave effects. The focusing lens is mounted on a translation
stage. This translation stage and the lattice/probe beam pointing is walked to optimize
lattice overlap with the 1 S0 -3 P1 MOT. By blocking the back reflection, good overlap is124
determined by a large atom number in the dipole trap, which leaks down the trap axis
because of gravity. The retroreflector alignment is varied to optimize the amount oflattice light retro-coupled to the optical fiber delivering it to the chamber, as well as thetrapped atom number in the focused lattice trap. The retroreflector is also mounted ona translation stage oriented along the trap axis, and this degree of freedom is used to
optimize the observed trap frequency (as described below), consistent with good focus
overlap between the incident and reflected lattice beam. Co-alignment of the probe andlattice is accomplished by looking for spot overlap over several meters of optical path.

3.4.2

SpectraFigure 3.6(a) shows a spectrum of the 1 S0 -3 P0 clock transition (ground state
population) with optical-lattice-confined 87 Sr atoms. The spectrum is of the purely
electronically excited transition carrier, i. e. no motional excitation. The lattice is operated at the magic wavelength, λmagic ' 813.428 nm. Bias coils in all three Cartesiandimensions were used to zero the magnetic field at the atomic sample. This was accomplished by systematically scanning the magnetic field in all dimensions and looking forthe narrowest possible spectrum as a function of the field. Under nonzero field, the magnetic states are made non-degenerate, resulting in Zeeman broadening of the observed,
overlapped transitions. By probing the atomic sample for 80 ms, allowing Fourier limited linewidths of ∼ 10 Hz, this technique could usually determine the field zero within
10 mG. As shown in Figure 3.6(a), narrow resonances with linewidths (FWHM) as small
as 5 Hz were observed for longer probing times.
To further push the coherence limit of the system, a small bias magnetic field
was applied (along the probing polarization axis) in order to separate out distinct πpolarized transitions from the individual mF states. A spectrum as shown in Figure
3.6(b) results, where the relative transition strengths are determined by the ClebschGordan coefficients between particular mF states, and the relative populations of the125photon counts(a) 3000
2500
FWHM:
4.6 Hz

2000
1500
-10

P0 signal (norm.)

10

laser detuning (Hz)

(b)

3

0

0.10 +9/2
0.08

-9/2

+7/2

-7/2
+5/2

-5/2

0.06
0.04

-3/2

+3/2

0.02

+1/2

-1/2

0.00
-400

-200

0
200
laser detuning (Hz)

-400

0
400
laser detuning (Hz)

0.06
0.04
0.02

3

P0 signal (norm.)

(c)

400

0.00
-800

800

Figure 3.6: (a) Narrow, 5 Hz linewidth dip in the ground state population due toexcitation of the clock transition. This is made at near zero B-field with all nuclear spinstates degenerate, so that π transitions from all mF states are excited simultaneously.
(b) Applying a non-zero bias magnetic field to lift the nuclear spin state degeneracy,
the resolved π transitions from individual mF states are observed in the excited state
population. (c) Same as (b), but with the σ + and σ − transitions.

126
mF levels in the ground state (approximately equally distributed). A similar spectrum
in Figure 3.6(c) shows the σ + and σ − transitions. Note that the π and σ spectra canbe used to determine the differential g-factor (∆g = 7.7 × 10−5 ) for the clock states bydetermining the relative shifts between different mF states [151].
If we spectroscopically focus on a particular π-transition (e. g. 5/2 or 7/2) inFigure 3.6(b), a spectrum as shown in Figure 3.7(a) can be revealed. Here, the optical probing time has been extended to 480 ms, corresponding to a Fourier-limited
linewidth of 1.8 Hz (FWHM). The linewidth of the spectrum in Figure 3.7(a) is 2 Hz.
Repeated measurements of these narrow optical transitions yields a histogram of transition linewidths as shown in the inset of Figure 3.7(a). The distribution spreads out over
several Hz due to the residual drift and low Fourier frequency noise of the probing laser.
The bare probe laser drift was mostly compensated by applying a feedforward drift via
an AOM which kept the spectral peak at a constant frequency. This compensation isnever perfect, due to time-dependent changes in the laser drift, and so the directionof the frequency scan across the spectrum was toggled between scans so as to averageout the effect of the drift of the measured linewidths. The mean histogram value corresponds well with the Fourier limited width of 1.8 Hz. This corresponds to a line quality
factor (ratio of transition frequency ν to the transition linewidth ∆ν) of Q ≥ 2.3 × 1014 ,currently the highest observed line Q in coherent spectroscopy. This represents coherent
atom-light interaction at ∼ 0.5 s. Attempts to push probing times to longer time scales(≥ 1 s) did not result in clean, narrower spectra, but rather revealed the low frequency
jitter in the laser frequency as noisy spectra. This is seen from the probe laser coherence
as seen in Figure 3.4(b). Here two lasers were able to maintain phase coherence over 2
s timescale. However, during narrow scans, while individual points on a scan represent
approximately 1 s of probing, they are separated by almost 1 s of dead time during
which time the atoms are cooled in the MOT, loaded into the lattice, etc. Made worse
by imperfect drift compensation, the laser does not have sufficient temporal coherence

127

3

8

Occurences

P0(mF=5/2) Population(a) 0.10

0.08
0.06

4
2
0

0

1

2

3

4

5

6

Transition Linewidth (Hz)

0.04

FWHM:
2.1 Hz

0.02
0.00

3

P0(mF=5/2) Population-6(b)

Fourier
Limit:
1.8 Hz

6

-4

-2

0

2

4

Laser Detuning (Hz)

0.20

0.08

0.16

6

1.7 Hz

0.04

0.12

10 Hz

0.00
-10 -5

0.08

0

5 10

0.04
0.00
-60

-30

0

30

60

90

Laser Detuning (Hz)Figure 3.7: (a) With an applied bias field to separate individual π transitions from thedifferent mF levels, a narrow spectrum of the π transition from the 1 S0 mF = 5/2 state
is observed. The 2 Hz spectral linewidth of this optical transition is close to the Fourier
limit of 1.8 Hz, set by the probing time of 480 ms. The inset shows a histogram of
measured spectral linewidths, consistent with the Fourier limit. (b) Similar to (a), theatoms are now probed with two pulse Ramsey spectroscopy. The inset shows Ramsey
fringes with a full width at half maximum of 1.7 Hz.

128
to enable scans of the atomic transition with < 1 Hz spectral linewidth. Shown alsoin Figure 3.7 is an atomic spectrum taken with two-pulse Ramsey spectroscopy and alinewidth (FWHM) of 1.7 Hz (inset of (b)).
Concerned also with the possibility of noisy Doppler contributions from shaking
optical elements around the optical lattice in Figure 3.5, we also considered introducing
free space active phase noise cancellation while probing the narrow optical transition.
With the optical setup given in Figure 3.5, this is not completely straightforward, sincevibration in different places along the optical path affects the probe and lattice phasedifferently, and it is the relative optical phase at the lattice trapped atom which mattersfor the Doppler contribution. For example, if the lattice retroreflector alone is shaken,
this introduces phase noise in the lattice sites, but does not affect the probe light since(nearly) all probe light is transmitted through the retroreflector. On the other hand,once the probe and lattice beams are combined, shaking elements definitely introducesphase noise on the probe beam. However, the lattice sites are less sensitive to suchnoise. To see this, we describe the lattice by two counterpropogating waves:~ = E~0 [cos(kx + ωt + φ1 ) + cos(−kx + ωt + φ2 )]E(3.12)

where φ1 and φ2 are time dependent phase noise terms. For the particular case where
the second wave is simply the first one retroreflected, the relationship between φ1 andφ2 is determined by applying the boundary condition that the phase of the optical waves
are shifted by π at the retroreflector position, x0 :kx0 + ωt + φ1 = −kx + ωt + φ2 − π(3.13)For simplicity, we set x0 = 0 and have φ1 = φ2 −π. Equation 3.14 becomes E~0 sin(kx) sin(ωt+φ2 ), and the standing wave nodes are unaffected by the phase noise. In the current configuration, phase noise from the probe beam is corrected only up to the optical fiber
tip, before being combined with the lattice beam. Perhaps the ideal scenario for noise

129
cancellation would be to have the lattice standing wave defined by a Fabry-Perot cavity around the atoms, with active stabilization of the cavity by feedback to a PZT on
the retroreflector. Then the probe light could be phase stabilized to the input reflector of the cavity. In our situation, assuming that the bulk of the optical phase noise
would originate from the lattice retroreflector, we mounted this mirror on a PZT andelectronically stabilized its position by using the lattice standing wave as one arm of ahomodyne Michelson interferometer, and stabilizing the relative phase between it anda short, stable reference arm. Introducing this extra stabilization did not improve theobserved narrow spectra.
With optical transition linewidths as narrow as 2 Hz, the 87 Sr frequency standard
has the potential for very low instability. Looking at Equation 1.1, a mere S/N of 10
could yield a 1 s instability below 10−15 . Achieving the narrow optical transition is thus
an important step toward development of an optical frequency standard. Before wemove to consider the other important pieces for this frequency standard, we look at thepart of the atomic spectra far from the carrier clock transition: the sideband structure.

3.4.3

Sideband structure

In Section 2.5, using the Hamiltonian describing harmonically trapped atoms
interacting with a resonant light field, we saw that the atom could be excited bothelectronically and motionally. In the appropriate regimes, this resulted in a spectrum of
carrier and sideband transitions. In Section 2.6.5, we discussed how trap anharmonicity
resulted in non-degenerate sideband structure for atoms with different initial motional
states. This anharmonicity is particularly relevant for the strong confinement axis, sincehere there are only several discrete motional states present. We also discussed (Section
2.6.5) how the transverse atomic spread (along the weak confinement axes) resulted inasymmetric broadening of the longitudinal sideband structure. These effects combine
to yield a spectrum as shown in Figure 3.8(a). With π-polarized interrogation, the

130

3

P0 population fraction

0.20
0.15

3

P0 population fraction

(a)

0.10

0.5
0.4
0.3
0.2
0.1
0.0
-200

-100

0

100

200

laser detuning (Hz)

0.05
0.00
-60

-40

-20

0

20

40

60

laser detuning (kHz)

(b)
3P

0

1S
0

hω
Figure 3.8: Measurement of the motional sideband structure. (a) The first order red
and blue longitudinal motional sidebands around the purely electronic carrier transition. The broad asymmetric lineshape of the sidebands originate from the longitudinalanharmonic confinement as well as the transverse spatial extent of the atomic wave
function where (off-axis) the trap confinement is weaker. The inset shows observationof the transverse motional sidebands with a strongly saturated carrier. (b) The sideband structure corresponds to motional excitation and de-excitation while the atom isbeing excited electronically. In the harmonic approximation, the motional states are
separated by the trap frequency ω.

131carrier and the ±1st order red and blue sidebands are shown. In order to accentuate
the sideband details, the carrier transition is saturated. This sideband structure is notdirectly useful for the generation of a well-defined optical frequency, but rather must be
considered as a line-pulling mechanism for frequency shift. Furthermore, the structure
manifests useful information about the confinement details of the atomic sample.
From Figure 3.8(a), we can directly read off the trap frequency along the longitudinal axis (approximately from the peak of the sideband to the carrier). A finer
resolution scan of the carrier may also reveal motional excitation along the transverse
axis (see Figure 3.8(a) inset, where the transition is being power broadened with strong
saturation). Because of the careful co-alignment of the probe and lattice k-vectors, thetransverse sidebands are difficult to excite and hence observe without introducing somerelative misalignment. Using Equations 2.83 and 2.84, the measured longitudinal andtransverse trap frequencies can be used to determine the trap depth and the latticebeam waist (in the harmonic approximation).
Atoms in the ground motional state of 1 S0 cannot contribute to the red sideband(because the motion cannot be de-excited below the ground state, see Figure 3.8(b)).
However, these atoms do contribute to the blue sideband. The largest contribution to
the red sideband comes from those atoms occupying the first motional state of 1 S0 . The
second biggest contributions to the blue and red sidebands are from the first and second
excited motional state of 1 S0 , respectively. And so on. Typically following a thermal
distribution, the atomic population among the different motional states is given by the
Boltzmann factor. Thus, the relative size of the blue and red first order sidebands,
whose amplitudes are weighted by the population distribution, gives the atomic sample
temperature.
~ω
Pred
N1
− long'= e kb T
Pblue
N0(3.14)

where Pred (Pblue ) is the peak amplitude of the first-order red (blue) sidebands, N0 (N1 )132
is the atomic population in the ground (first excited) 1 S0 motional states, and ωlong is 2π
times the longitudinal trap frequency. In principal, Equation 3.14 holds approximately
for the transverse axes (ωtrans ) as well. For our confinement, however, the transverse
trap frequencies are small enough that the difference in the first-order blue and red
sideband amplitudes is quite small (∼ 1%) and typically below the measurement S/N .
Note that for the particular case of strong trap anharmonicity (similar to ourcase), the blue and red sidebands for each motional state are non-degenerate, and thesum of the individual transitions can be fit to the observed spectra. The relative amplitude weighting for the red or blue sideband of each motional state is given by theappropriate Boltzmann factor, and can be alternatively used to determine the sample
temperature. The two measures of temperature typically agree [21]. For such fits, wehave previously assumed that all transitions from one motional state to the next have a
Lorentzian lineshape with a common broadened linewidth. While the previous measurements yield the sample temperature along the longitudinal axis, the shared linewidthof each transition (determined by fit) gives a crude estimate of the sample temperature
along the transverse axis. Without dedicated sideband cooling along a particular axis,
the measured longitudinal and transverse temperatures typically agree within the fit
uncertainties. Efforts are being made to properly account for the asymmetric lineshapeof each transition due to the transverse spatial extent and temperature, using a modelsuitable for fitting the many degrees-of-freedom [145, 16, 196]. Note also that while theLamb-Dicke parameter can be directly calculated with the known trap frequencies andrecoil frequency, the sideband amplitudes can provide further quantitative verification(as in Section 2.5).

Chapter 4

Development of the Sr Optical Standard: High Accuracy Spectroscopy

In Chapter 3, we motivated 87 Sr as an optical frequency standard with the observation of Hz-level-linewidth optical spectra. We now discuss the tools and measurements
which developed this system as an optical frequency standard.

4.1

Counting optical frequencies: the fs frequency comb
In Section 1.3, the benefits of optical frequency standards were highlighted. For

years, these benefits were heavily outweighed by the difficulty of measuring optical frequencies. Except for measurements between optical standards operating at similar frequencies (difference of operational frequencies in microwave regime), comparison among
different optical standards was extremely difficult, and thus the utility of optical standards was limited. The behemoth optical frequency chains developed in a few national
laboratories laboriously enabled optical frequency measurements referenced to the Csdefined SI second [197, 198]. Within the last ten years, a revolutionary approach to
optical frequency measurement has made the process relatively straightforward. With
the pioneers of this technique rewarded by the 2005 Nobel Prize in Physics, these opticalmeasurements are now made regularly with amazing precision in laboratories aroundthe world.
Somewhat paradoxical, the heart of the apparatus used to measure well-defined
CW optical frequency sources is a femtosecond (fs) pulsed laser. Consider the optical

134

Time Domain(a) E(t)t=1/frep2∆φtFrequency Domain
fbeat(b) I(f)2π fCEO = ∆φ frep

fCEO
frep
νn

ν2n
control
fCEO

SHG

νopt

νopt=Mfrep+fCEO+fbeat

Figure 4.1: Emission from a mode-locked femtosecond (fs) pulsed laser (a) In the time
domain, the laser output generates fs pulse-width envelopes separated in time by 1/frep .
Another important degree of freedom is the phase difference between the envelope maximum and the underlying electric field oscillating at the carrier optical frequency. (b)By Fourier transformation to the frequency domain, the corresponding frequency comb
spectrum is revealed. Each tooth in the comb, a particular single frequency mode, isseparated from its neighbor by frep . The relative carrier-envelope phase in the time
domain is related to the offset frequency fCEO in the frequency domain. fCEO is givenby the frequency of one mode of the comb (e. g. νn ) modulo frep , and can be measured
and stabilized with a f-2f interferometer. In this interferometer, one comb mode, νn ,is frequency doubled and heterodyne beat with the comb mode at twice the frequency,
ν2n . Thus, by stabilizing fCEO and frep to a well known frequency reference, each comb
mode frequency is well known. Measurement of the frequency of a poorly known opticalfrequency source (e. g. previously measured at the resolution of a wavemeter) can be
determined by measuring the heterodyne beat between the frequency source and thefrequency comb. The previously determined coarse frequency knowledge of the opticalsource can be used to determine which comb mode is adjacent the optical source in thefrequency domain.

135
output of such a laser, as illustrated in Figure 4.1. Pulses with temporal widths ofseveral to tens of fs are generated in a pulse train. The repetition rate of the pulse train(frep ) is given by the inverse of the round trip cavity travel time inside the mode-locked
laser. The frequency and phase properties of this pulse train can be fully constrained bycontrol of two degrees of freedom: the relative phase between the carrier wave and theenvelope packet (known as the carrier envelope offset), and the repetition rate. Now weapply a Fourier transform to describe the laser output in the frequency domain. The
pulse train transforms to a comb of many single frequency modes. The spacing between
each mode is given by the laser repetition rate, and the spectral range covered by thefrequency comb is related to the temporal width of each pulse. With the repetition rate
known, the frequency of the individual modes (comb teeth) could be extrapolated tothe mode closest to zero frequency (DC). The extrapolated mode closest to DC has afrequency offset known as fCEO (note that fCEO < frep ). It can be shown that fCEO
determines the carrier envelope phase offset [199]. Thus the frequency properties can beconstrained, in the frequency domain, by control of frep and fCEO . This is equivalent
to saying that each comb mode has a frequency given by ν = N frep + fCEO , where N
is an integer representing the mode number, counting from the first mode at frequency
fCEO .
With an appropriately large spectral bandwidth, determining the value of fCEO
is straightforward. Consider the N th comb mode in the low frequency spectrum of thecomb, whose frequency is given by νN = N frep + fCEO . We frequency double thiscomb mode (using the appropriate nonlinear crystal for second harmonic generation) tocompare its frequency with that of ν2N = 2N frep + fCEO . The difference between thetwo frequencies, 2νN −ν2N is seen to equal fCEO . The same holds true for the Mth comb
component. Thus, if the comb spectrum covers an entire octave, fCEO can be measured
by comparing the comb output to the frequency doubled output of the comb. Some
mode-locked lasers, exploiting Kerr nonlinearity in the laser gain medium to generate

136strong phase modulation, intrinsically produce a full octave output of an optical comb.
We use such an octave-spanning frequency comb. In other cases, the fs laser output
can be injected into a microstructure optical fiber, where strong nonlinearities broaden
the comb spectrum to cover an entire octave. The other comb degree of freedom, frep
(which is typically a value between 100 MHz and a few GHz), can be measured directlywith a properly designed photodetector. Thus, both comb degrees of freedom can bemeasured. By appropriate actuation on the laser cavity [200, 201], it has been shownthat the measured values fCEO and frep can be controlled and stabilized at impressive
levels of precision and accuracy [202].
The utility of the comb is now evident. After stabilizing frep and fCEO to a
microwave frequency reference, an unknown laser frequency can be determined by measuring the heterodyne beat between the unknown laser and the stabilized comb (assuming the comb has sufficient spectral overlap with the unknown laser). A coarse, independent measurement of the unknown laser frequency using a commercially available
wavelength meter allows one to determine which comb mode, N , makes the heterodyne beat with the laser. The laser frequency is then determined straightforwardly byνlaser = N frep + fCEO ± fbeat , where fbeat is the measured heterodyne beat frequency
and the ± is determined by whether the comb mode or the unknown laser is at higher
frequency (straightforward to constrain). Such a measurement can be currently madeat the stability level of the best microwave frequency references.
The situation above can also be inverted. If the heterodyne beat is formed witha well-defined optical frequency standard, fbeat can be locked by actuating on the fs
comb. The repetition rate of the comb can then be measured, which is stabilized to theoptical frequency standard. In this way, the comb enables the phase information of an
optical frequency standard to be used in the microwave domain. Furthermore, whenstabilized to one optical frequency standard, the comb can be compared to a second
optical standard at a different frequency and thus enable easy comparison of different

137
optical standards. The ability of the comb to inherit the accuracy and stability of the
optical standard to which it is locked and then transfer this across large spectral gaps formeasurement with a second standard has been shown to far exceed the current accuracy
and stability of the standards themselves [202].
The fs comb, using relatively standard laboratory techniques, thus enables microwaveto-optical, optical-to-microwave, and optical-to-optical phase-coherent measurements.
For this reason, the comb is considered the vital “gear system” which allows an opticalfrequency standard to be counted. Together, the optical standard and fs comb constitute the heart of an optical atomic clock. Using a stabilized fs comb, we measure
and characterize our Sr standard against other well established frequency references, as
discussed in the next sections.

4.2

Frequency reference
Experimental characterization of 87 Sr as an optical frequency standard includes

determination of systematic shifts of the atomic transition frequency and its absolutemeasurement. Both of these require measuring the Sr transition frequency relative to awell-accepted frequency standard, the later ultimately requiring a Cs standard to linkto the SI second. In our laboratory, one reference option was an in-house commercial
Cs clock (HP 5071A). These robust clocks have 1 s fractional instabilities of ≤ 5 ×
10−12 and average down to ≤ 1 × 10−14 over 5 days. The factory specified inaccuracy
is 2 × 10−13 , although Dr. Judah Levine provides GPS-based steering to the UTCNIST timebase with an inaccuracy of 1 × 10−14 . This microwave frequency reference
would have been usable for our first characterization of the Sr system. However, asuperior reference was available from NIST: one hydrogen maser from an ensemble ofmultiple masers which is periodically calibrated to the NIST-F1 cesium fountain clock(calibration services provided by Dr. Tom Parker and the Cs fountain team at NIST).
The H-maser typically exhibits a 1 s instability of 2 × 10−13 and averages down to as

138√
low as 10−16 roughly as 1/ τ (averaging time τ ). Depending on the behavior of themaser and the details of the Cs-calibration, during the measurements described below,
the maser frequency was determined accurately to anywhere from the several 10−15level to 5 × 10−16 . Besides the higher accuracy, the H-maser/Cs reference provides morethan an order of magnitude reduced instability beyond our in-lab Cs clock, strongly
relaxing the required measurement time for a given measurement precision. The only
complication originates from the need to remotely transfer this standard from the NIST
Boulder campus to our laboratory in JILA.

4.2.1

Microwave fiber transfer

A schematic of the frequency transfer scheme that we used is shown in Figure
4.2. The H-maser reference signal (typically using H-maser ST-4 or ST-5) at 5 MHz
is sent from the H-maser ensemble room at NIST to the lab of Drs. Leo Hollberg andScott Diddams over a low-temperature-coefficient coaxial cable. This 5 MHz reference
signal is frequency doubled and used as the reference for a tunable analog synthesizer(e. g. Agilent E4428C-503). This synthesizer, operating at approximately 950 MHz, isused to amplitude modulate a Nd:YAG laser operating at 1320 nm. This amplitude
modulation is realized using a telecom Mach-Zehnder interferometer with an internal
electro-optic modulator. The amplitude modulated light is transferred by optical fiber
link (part of the Boulder Research Area Network, BRAN) approximately 3.5 km oneway. The amplitude modulation is detected at JILA by illuminating a photodetector(EOT ET-3000A-FC) with the transferred light. This RF signal at fmaser ' 950 MHz
serves as the comb frequency reference by counting the difference frequency between
fmaser and the tenth harmonic of the repetition rate (fcount = 10frep − fmaser ' 40
kHz) on a frequency counter referenced to the HP Cs standard. More details on the
microwave fiber transfer can be found in reference [79, 203, 201, 21, 22]. At shorttimescales, extra phase noise accumulated by the synthesizer phase lock and dispersion

139

mixer
f=5 MHzPD
f=950 MHz

H-maserensemblefrequency
synthesizer

YAG with fiber
fiber
EO MZI
circulator stretcher

count frepPDpartialreflector

Figure 4.2: The microwave reference frequency transfer from NIST to JILA over opticalfiber link. A synthesizer at 950 MHz is phase locked to the hydrogen maser reference
at 5 MHz. This synthesizer drives amplitude modulation of a YAG laser at 1320 nm
utilizing a commercially available Mach-Zehnder interferometer with an internal electrooptic modulator. This amplitude modulated light is transferred to JILA and detected
on a photodetector. This signal is then used as a frequency reference to count therepetition rate, frep , of the frequency comb which is stabilized to the Sr clock laser. For
frequency measurements with an accuracy at or better than the fractional 10−14 level,
long term phase noise accumulated in the fiber transfer must be compensated. This isdone by detecting the round trip microwave phase along the fiber path and stabilizing
it to the synthesizer phase reference using a fiber stretcher.

140
in the optical fiber is relatively small, permitting the use of a passive, uncompensatedsignal transfer. At 1 s, the H-maser reference transferred to JILA gave instabilities of√
2 − 3 × 10−13 , averaging down like 1/ τ to 100 s. Excess phase noise, presumably
originating from thermal drifts, could degrade the instability at many hundred seconds,
but never worse than several 10−14 . This effect is shown is Figure 4.3(a), where thetransferred microwave phase is measured as a function of time. The largest phase drift
observed corresponds to a frequency shift of 10−14 . For our first measurement of the
87 Sr 1 S -3 P transition frequency, the passive microwave transfer gave sufficient stability00

and accuracy. For our second, improved measurement, our measurement uncertainty
was on the 10−15 level, requiring more accurate control of the fiber phase noise. This
was accomplished by adding a fiber stretcher at the NIST fiber end (see Figure 4.2).
The modulated light was sent to JILA, with a fraction of it reflected back to NIST for
homodyne phase detection with the local microwave copy using a mixer. The detectedroundtrip microwave phase was stabilized by actuating on the fiber stretcher with low
bandwidth feedback (unity gain bandwidth just below the Hz level). By doing so,
the fiber group delay could be compensated and the long timescale phase noise in the
microwave signal cancelled, reducing potential frequency shifts well below the 10−15 level[22, 203, 201]. This is demonstrated in Figure 4.3(b). Shown here is the stability of thestrontium standard measured against the H-maser. At longer timescales, the instability√
continues to average down as 1/ τ , demonstrating control of the group delay noise thatwould otherwise result from the fiber transfer.

4.3

Evaluation of the Frequency Shifts and their Uncertainty
A very long list of physical mechanisms can systematically shift the measurementof atomic transition frequencies. An atomic system well suited as a frequency standard
has very weak sensitivity to most of these mechanisms. Many shift mechanisms are very
well understood, and together with excellent knowledge of the environmental conditions,141

Phase [mrad](a)

RF freq.: 950 MHz
100
0
-100

Changing phase yields-14
1 x 10 frac. freq. offset

(a)
0

2

4

]

8

10-13

Total Deviation(b)

6

Time [hours]

2

10-14

2

10-15
101

102

103

104

105

Averaging Time (s)Figure 4.3: (a) Long-term phase noise present in the microwave reference transfer acrossthe optical fiber link when no microwave phase stabilization is utilized. Thermal andother effects can result in phase chirps producing fractional frequency offsets as large as
10−14 . Although these effects can be averaged over with measurement durations at orexceeding 24 hours, measurement below the 10−14 accuracy level benefits from control ofthis microwave phase to eliminate any possible offset in the delivered frequency reference.
(b) Using the microwave phase noise cancellation (with a fiber stretcher) over the opticalfiber link, the relative instability between the Sr clock at JILA and the Cs-fountaincalibrated H-maser at NIST is shown. The instability averages down to 10−15 roughly
as white frequency noise. If no feedback control of the fiber-link induced microwave
phase noise were implemented, large instability bumps beyond the 100s timescale would
be observed.

142

Signal Amplitude (Arb. Units)(a) 4600(b)
νsr - 429228004229900 [Hz]

4400
4200
4000
3800
3600 177 Hz
3400

400

200
100
0

-100

Linewidth

-200

3200
-1.0 -0.5 0.0

Magnetic Shift-32(7) Hz / G

300

0.5

-4 -3 -2 -1 0

1

2

3

4

axial magnetic field [G]1.0

698 nm probe frequency [kHz](d)
Lattice Stark shift:17(8) Hz/I0

0

-10
-20
-30

0.0

0.2

0.4

0.6

0.8

1.0

1.2

100
50
0
-50
-100
4x10

νsr - 429228004229952 [Hz]

10

10

11

10

12

4x10

12

3

Lattice Intensity [I/I0](e)

Density shift12-3
1.0(6.4) Hz / (10
cm )

150

sr

-40

ν - 429228004229900 [Hz]

νsr - 429228004229900 [Hz](c)

A tom ic D ensity [atom s/cm ]

300
200
100
0
-100
-200
-300
-400

884(15) Hz/nm

-0.3

-0.2

-0.1

0.0

0.1

0.2

0.3

0.4

0.5

Lattice wavelength - 813.4718 [nm]Figure 4.4: Measurement 1 uncertainty evaluation (2005) (a) Clock transition linewidth
below 200 Hz. Sensitivity of the clock transition frequency to (b) magnetic field (along
the axial direction) (c) AC Stark shift induced by the lattice laser and (d) density shift
from interatomic collisions. (e) at a one way lattice laser intensity of 10 kW/cm2 , theclock transition frequency shift as a function of lattice laser wavelength.

143
the size of these shifts can be estimated computationally. Nonetheless, a rigorous determination of the transition frequency requires experimental investigation of the key
systematic shifts. As a first measurement (2005) [21], we investigated critical shifts byspectroscopically scanning the clock transition while systematically varying the environmental parameters. The scans, whose absolute frequency axis was determined using the
H-maser reference, were fit to determine the transition line center. Figure 4.4(a) shows
one particular scan, with a linewidth of < 200 Hz. Note that at this time a different
probe laser system was being used than the one described in Chapter 3. Although thislaser had been previously characterized with a linewidth of several Hz [159], it was later
determined that during the following weeks of atomic spectroscopy, etaloning near thehigh finesse cavity had developed, compromising the laser stabilization to the cavity.
This led to laser linewidth broadening which limited the atomic spectra to 200 Hz.
Despite this limitation, the uncertainties in the fit of the center of the atomic spectra
were typically smaller than the uncertainty in the absolute frequency axis, determinedby the stability of the H-maser on the timescale of the scan (50-100 s). Many suchline centers were averaged together for a particular parameter value (averaging scans inboth the positive and negative frequency direction) and the parameter values were varied to determine dependence on a particular effect. Figure 4.4(b-d) shows the observed
dependence on the magnetic field, the atomic density, and the lattice intensity (for thiswork λlattice = 813.437 nm). Figure 4.4(e) shows the dependence of the clock transition
frequency for a fixed intensity as λlattice was varied. Table 4.1 summarizes the measured
systematic shifts and their uncertainties.
Further details on this measurement can be found in [21]. A detailed descriptionof individual systematic effects will be reserved for the next chapter. I mention here a
few of many differences between the system operation for the results here and that in
Chapter 5. First, in the measurement discussed here, the atomic sample was probed atnearly zero B-field, with transitions from all spin states essentially degenerate. Second,144
Table 4.1: Measurement 1 (2005): Systematic corrections and their associated uncertainties for the absolute frequency of the 1 S0 - 3 P0 clock transition.
Contributor
AC Stark shift (lattice)
AC Stark shift (probe)
Blackbody shift
Zeeman shift
Recoil/Doppler shift
Density shift
Systematic total

Correction (Hz)
-17
7.0
2.2
0
0
-2.0
-9.8

Uncertainty (Hz)
8.3
0.9
0.05
12
1.9
12
19

the probe laser illuminating the atoms was intentionally phase-modulated so that a weak
first order sideband could probe the transition, while a far-detuned (∼ 10 MHz) but
stronger carrier could be used for optical path phase noise cancellation. During this firstmeasurement, the fiber delivering the probe laser was angle-cleaved at the fiber output
to reduce back reflections into the fiber. The reflected signal for noise cancellation was
taken from the lattice retroreflector, which at that time had a 698 nm reflection of 70%.
The benefit of this approach was that phase noise in the optical path after the fiber could
be compensated for. However, as our measurement accuracy improved, the drawbacks ofhaving probe standing wave effects and a strong, RF-detuned optical beam outweighed
the benefit, and this was changed. Also during the earlier measurements, the probe
beam and lattice beam were also focused to the same beam waist, w0 = 65 µm. This
resulted in stronger transverse spatial inhomogeneity of the Rabi excitation frequency,
reducing the observed excitation fraction. To counteract this effect and enhance thespectroscopic signal (measuring the ground state population), after spectral probing on
the clock transition for 10-40 ms, we illuminated the atoms with 2 ms of 679 nm light,
pumping the excited 3 P0 population to the 3 S1 state for shelving to 3 P2 . See Figure
1.2 in Chapter 1. This process of probing and pumping was repeated multiple times toenhance the ground state population dip on resonance.
In a second measurement (2006), we had implemented the improved stable laseratom number (norm.)

1.0
0.8
0.6
0.4
0.2
0.0
-60

-40

-20

0

20

40

laser detuning (Hz)60

atom number (norm.)

atom number (norm.)

145

1.0
0.8
0.6
0.4
0.2
0.0
-60

-40

-20

0

20

40

60

-20

0

20

40

60

laser detuning (Hz)

1.0
0.8
0.6
0.4
0.2
0.0
-60

-40

laser detuning (Hz)Figure 4.5: Measurement 2 uncertainty evaluation (2006). In order to measure shiftsensitivities using the clock laser as a stable optical frequency reference, measurementsof the clock transition were made interleaving different environmental parameters at
the second timescale. As shown, we traced out the clock transition spectrum, alternating each point (approximately 1 s per point) with different atomic conditions. Here,the atomic number was varied as a handle on the density shift sensitivity. The collective spectrum is separated into the underlying spectrum for each condition and a fit
determines the line center of each. A frequency difference is measured for the conditions. Collection of hundreds of spectra like these allowed determination of the relevant
frequency shifts below the 10−15 level.

146
Table 4.2: Measurement 2 (2006): Systematic corrections and their associated uncertainties for the absolute frequency of the 1 S0 - 3 P0 clock transition.
Contributor
AC Stark (Lattice)
AC Stark (Probe)
AC Stark (BBR)
Zeeman EffectDensity Shift
Total

Correction (10−15 )
0.25
-0.02
5.44
0
-0.01
5.66

Uncertainty (10−15 )
0.60
0.12
0.16
0.53
0.33
0.88

system described in Chapter 3. Well aware from our first measurement of the painful
averaging time required to characterize the systematic shifts with the limited stability of
the H-maser, we were anxious to use an improved frequency reference. The evaluationof systematic shifts does not require an accurate reference, but typically only a stableone. The stability of the reference must be suitable on the timescale that is required todetermine possible frequency shifts for different environmental parameter values. Knowing the impressive stability of the 698 nm probe laser itself (1 × 10−15 for timescalesof 1-100 s with proper drift cancellation), we decided to characterize systematic shiftmechanisms using the probe laser as the reference oscillator. To make this possible, agiven environmental condition (density, probe intensity, magnetic field strength, etc. )was switched during each loading and spectroscopy cycle (∼ 1 s) among different parameter values. The spectrum was scanned out as these parameters were varied. During
data analysis, the spectrum consisting of multiple parameter values was separated into
multiple spectra, one for each parameter value (see Figure 4.5). These spectra were fit,
and the line center difference was determined as a function of the parameter. Manysuch spectra, scanning in both frequency directions, were averaged to determine theclock transition sensitivity to a given parameter. The results are summarized in Table
4.2. More details are found in [22]. As in the first measurement, spectroscopy wasdone by scanning the transition at near zero magnetic field, with all nuclear spin states
degenerate.

147

4.4

Absolute frequency measurement of the 1 S0 -3 P0 transition
With the systematic shifts and uncertainties determined in the two measurementsof Section 4.3, absolute frequency measurements of the 87 Sr 1 S0 -3 P0 transition frequency
could be made using the Cs-calibrated H-maser reference. The absolute frequency measurement accompanying Measurement 1 (2005) is shown in Figure 4.6(a). In addition
to the shifts and uncertainties in Table 4.1, measurement related shifts and their uncertainties for the H-maser calibration to Cs and the gravitational red shift between Sr andCs were included. The 1 S0 -3 P0 transition frequency was measured to be 429 228 004 229
869 ±19 (sys) ±2.8 (stat) Hz, with the systematic and statistical uncertainties also inunits of Hz. This was the highest precision measurement of the 87 Sr clock transition at
the time, but disagreed with a different measurement published several months earlier[28]. The disagreement between the measurements was ∼ 80 Hz, corresponding to threetimes the combined uncertainty (see Figure 4.6(a)). This disagreement was later resolved by an independent measurement by the Paris group [24] as well as with a second
measurement [29] by the authors of [28] which corrected a previous measurement error.
Measurement 1 thus played an important role as the first high accuracy measurementof the lattice-trapped Sr 1 S0 -3 P0 transition, improving on the first direct excitation ofthis transition ([204], 20 kHz uncertainty) and the erroneous measurement of [28].
The improved systematic uncertainty evaluation of measurement 2 was also accompanied by an absolute frequency measurement of the clock transition. The resultsof almost 900 consecutive measurements (taken over a 24 hour period) of the transition
frequency are shown in Figure 4.6(b). With the goal of measurement inaccuracy near the
1 × 10−15 level, we more carefully characterized measurement errors resulting from the
H-maser transfer (such as that shown in Figure 4.3(a)). As discussed above, phase noise
cancellation was implemented to compensate for group delay drift in the optical fiber
link (see Figure 4.2). The fiber link was characterized to quantify additional frequency

148νsr - 429228004229900 [Hz](a)80Tokyo 2005
60
40
20
0
JILA 2005
-20
-40
-60
5/3 5/17 5/31 6/14 6/28 7/12 7/26
Date (2005)

(b)

(c)
160
140

νSR-ν0 (Hz)Occurances

60

40

20

120
100
80
60

0
0

20

40

60

80 100 120 140

νSr - ν0 (Hz)

1

2

3

4

5

Measurement

Figure 4.6: (a) Measurement 1 absolute frequency (2005). Our measurements are indicated by circles on the dates indicated on horizontal axis. The final weighted mean andstatistical (systematic) error bars for the measurement are given by the filled (unfilled)blue bars. The final 2005 measurement by the University of Tokyo group is shown, again
with the statistical and systematic error bars. The discrepancy is ∼ 80 Hz. (b) Measurement 2 absolute frequency (2006). Histogram of frequency measurements binned in
30 s intervals over a 24 hour period. The data shown is not yet corrected for all systematic shifts. (c) Absolute frequency measurements of the Sr clock transition performed
by JILA (circles), Tokyo (squares), and Paris (triangle). The first circle corresponds
to Measurement 1 (2005) and the second to Measurement 2 (2006). Measurement by
Paris, Tokyo, and JILA after 2005 confirmed the Measurement 1 result.

149
shifts and uncertainties of the remotely delivered Cs/H-maser reference. One criticalshift mechanism was the temperature dependence of the synthesizer used for amplitude
modulation in the H-maser link. This was determined by measuring the frequency shiftof the synthesizer output (compared to a stable reference) while applying a known temperature ramp (K/hr) to the synthesizer [measured to be 4 × 10−14 1/(K/hr)]. Then,
during the absolute frequency measurement, the synthesizer was kept in a temperaturestabilized enclosure and the ambient temperature was monitored. The measured shift
and uncertainty was the measured time rate of temperature change scaled by the measured sensitivity coefficient, yielding a shift value of −1.7(0.7) × 10−15 during the 24
hour measurement run. Another shift uncertainty was imperfect fiber noise cancellation
over the microwave link. An in-loop estimate of residual frequency shift from this effectwas below the 10−17 level. A conservative estimate of 1 × 10−16 was assigned to thiseffect, and we later made a more rigorous out-of-loop evaluation confirming the absenceof systematic shift at the 10−16 level. Microwave transfer from the H-maser lab to the
Optical Frequency Measurements lab was estimated to be negligible on the 1 × 10−16level (by comparing a high quality, low temperature dependent link with a separate linkusing standard RG-58 cable with a different path between the labs). Counter error andother synthesizer error was also determined to be negligible. As a final precaution, theabsolute frequency measurement was made over a 24 hour period to average over diurnal
environmental fluctuations. The 1 S0 -3 P0 transition frequency was measured to be 429
228 004 229 874.0 (1.1) Hz, with the uncertainty dominated by the H-maser calibration
to the Cs-fountain. Figure 4.6(c) shows this result together with the first measurement,
as well as comparable measurements made by the Tokyo and Paris groups. The final
fractional uncertainty of 2.5 × 10−15 made this the highest accuracy optical frequency
measurement for neutral atoms (at the time), at the time falling short of the Hg+ ion
measurement as the most accurate optical measurement of any system.

Chapter 5
The Strontium Optical Frequency Standard at 10−16 Uncertainty:
Remote Optical Comparison of Optical Clocks

In the previous chapter, we saw high precision and high accuracy spectroscopyof the clock transition of 87 Sr atoms confined in a 1-D optical lattice. These results
demonstrated the potential of Sr as an optical frequency standard and illuminated how
refinement of the Sr system could yield improved performance. Aided by the agreement
among the independent high-accuracy measurements of different groups (JILA, Paris,
and Tokyo), the lattice trapped 87 Sr 1 S0 -3 P0 transition was recommended by the CIPM
as a standard frequency “for applications including the practical realization of the metre and secondary representations of the (SI) second” [205]. Further improvements in
the Sr standard could rival or surpass the uncertainties in the best Cs standards, theprimary standard. Characterizing an improved Sr standard would benefit greatly fromcomparison with other optical standards, since the averaging time required to makehigh accuracy measurements against microwave standards was sometimes prohibitively
long. For this reason, we developed a direct optical frequency link between JILA and
NIST to enable a Sr clock comparison with other optical clocks at NIST (e. g. Ca, Yb,
Hg+ , and Al+ ). This chapter details the characterization of the improved Sr standard
by remote optical comparison and an improved absolute frequency measurement of theclock transition, culminating in the evaluation of the overall uncertainty at the 10−16level.

151

5.1

Design Improvements in the Sr Optical Standard

5.1.1

Atomic Polarization

As seen in the systematic shift and uncertainty evaluation in 2005 and 2006 (seeSection 4.3), the first order Zeeman shift played a significant role in the final total
systematic uncertainty. Between Measurement 1 (2005) and Measurement 2 (2006),
the Zeeman shift uncertainty was reduced because of the improved capacity to maintain the magnetic field at or near zero value. The enhanced field determination wasderived from the narrower spectra observed in Measurement 2, which more sensitively
revealed B-field induced broadening of the nearly-degenerate, overlapping transitions
from all magnetic sublevels. This yielded a factor of 50 improvement in the Zeeman
shift uncertainty (similar to the ratio of the spectral linewidths observed in the two
measurements). Besides continuing to improve the B-field characterization, reducing
the clock transition sensitivity to the B-field would ideally reduce the uncertainty fromthis effect. As mentioned in Chapter 1, hyperfine interaction mixes the pure 3 P0 witha small admixture of 1 P1 and 3 P1 . This accounts for the fact that 1 S0 and 3 P0 , which
would otherwise have identical g-factors, have relatively small but unequal energy dependence on B-field (∆g = 7.7 × 10−5 ) [151]. The first order shift for a π-transition isδν = µB ∆gmF B/h, where µB is the Bohr magneton, and the magnetic field strength(along the quantization axis) is given by B. The first order Zeeman shift for magnetic
sublevels with equal but opposite mF is thus equal but opposite. Taking the averageof two such transitions (±mF ) gives an effective transition frequency which is (1) equal
to the zero field transition frequency and (2) has no first-order Zeeman dependence.
Thus, the first-order Zeeman sensitivity can be greatly reduced. Techniques using different magnetic states to measure or cancel mF -dependent shifts have been applied ina variety of different contexts (e. g. [206]).
The most straightforward way to average the Zeeman components would be to152sequentially interrogate the resolved transitions under a bias B-field, and average theindividual measurement results. To avoid wasting atomic population, ideally all of the
population would reside in the mF state being interrogated. However, after latticeloading, the atomic population is approximately evenly distributed among the magnetic
sublevels. For this reason, optical pumping may be employed to drive population to
one or two sublevels for interrogation (as discussed in Section 2.7). Utilizing the 1 S0
F = 9/2 - 3 P1 F 0 = 7/2 transition with π-polarized light (with the light propagation
along the lattice axis), the atomic population is pumped to two sublevels mF = ±9/2
with experimental ease. A primary disadvantage to this dual spin state approach is thatafter one of the two spin states is interrogated, the population is read off using 1 S0 -1 P1
fluorescence. This broad transition does not discriminate the spin states, consequently
heating away all spin states. Thus one half of the lattice trapped atoms are wasted in ameasurement cycle (which remains much better than the 90% wasted in the unpolarized
case, but still not ideal). Nonetheless, as seen from experimental data later in thischapter, this approach easily facilitates a Sr frequency standard with nominally no firstorder Zeeman shift. As will be further detailed in Section 5.4.2, the effect of the latticeinduced AC Stark shift includes a component depending linearly on mF through thevector polarizability. This interaction can be thought of as between the atomic magnetic
dipole and an effective magnetic field along the lattice k-vector [207]. Because of its mF
dependence, the ±mF interrogation also enjoys cancellation of the vector Stark shift.
Another optical pumping approach is to use the 1 S0 F = 9/2 - 3 P1 F 0 = 9/2
transition with pure σ + -polarized light (with light propagation along the quantization
axis, which we set with a bias magnetic field along the lattice polarization axis). Thisdrives all of the population to mF = +9/2. These atoms are then interrogated and theclock state populations are read off. Then in the next experimental cycle (after loadinga new group of atoms into the MOT and lattice) the optical pumping light is switched toσ − -polarized, driving all the population into mF = −9/2 for interrogation. In this case,153
100% of the atoms may contribute to spectroscopy. Experimentally, there are one or
two additional details to this approach. We utilized a liquid crystal variable wave plate(Meadowlark Optics) to switch between σ + and σ − polarization between experimental
cycles. When stabilizing the clock laser to the atomic transition (discussed below) propersynchronization must be maintained between the clock laser feedback from the atoms
and the σ + and σ − experimental cycles. Figure 5.1(a-b) shows atomic polarization
for both schemes and we have operated the clock with both schemes. Most of theuncertainty evaluation in this chapter uses the first scheme, the doubly-spin-polarizedcase of mF = ±9/2. The spin state will also be relevant as we investigate collisional
effects between the ultracold Sr atoms.

5.1.2

Laser Stabilization to the Atomic Transition

To operate as a standard, the clock laser frequency must reflect the atomic standard transition frequency. The clock laser derives its short-term frequency stability
from locking to the high-finesse optical cavity. The longer-term frequency stability isderived by locking the laser frequency to the atomic transition. Methods to do thishave been developed for various frequency standards over the decades. We implement a
modulation based lock to the clock transition, which is largely insensitive to long term
fluctuations in the atom excitation signal. Since we want to stabilize the laser to theaverage of the two mF = ±9/2 transitions, we operate two independent locks which
are time multiplexed and whose average frequency is calculated digitally. The basic
approach for this two peak lock is illustrated in Figure 5.1(c). At first, for lock acquisition, the laser is frequency scanned across the doubly-polarized atomic sample. For
efficiency, this scan typically skips a large range of frequencies known to be between thetwo peaks. This spectrum is fit to two peak-functions (usually Lorentzian). The laser
frequency is then set to the low frequency half maximum of the first peak and spectroscopy is performed, detecting the population excitation, and recording it digitally.

8 (b)(a)3
2

P0 population (norm.)

4

6

1

2

3

4

4
2

1

0

0

3

3

P0 population (norm.)154

0
100 200
laser detuning (Hz)

-100
0
100
laser detuning (Hz)

(c)
m1-m2

PID

m3-m4

PID

A/D

DDS1

AOM1

PMT
avg

PID

DDS2

manual drift
feedforward

DDS3

+

Figure 5.1: (a) Spectra of the π clock transitions under a bias magnetic field with(blue) and without (green) state preparation to the doubly spin-polarized mF = ±9/2
states. The vertical axis gives the excited 3 P0 population and is normalized to themF = 9/2 peak height in the unpolarized case. (b) Spectra with spin polarization toa single spin state, mF = 9/2. As in (a), other spin states contain < 5% residual
population. Although negative detuning is not shown, no observable population resides
in the negative mF states. (c) Schematic for stabilization of the clock laser to the atomic
transition. The ground and excited states are measured by fluorescence collected by thephotomultiplier tube, PMT. After amplification and filtering, this signal is digitized by
the A/D analog-to-digital converter. To stabilize to the average of the mF = ±9/2transitions, the four points are measured as shown in (a) over four experimental cycles(at the half maxima). The difference of the measurements on the first peak, m1 − m2,
gives the error signal to lock to that peak, and likewise for the second peak (m3 − m4).
These measurements are time multiplexed. The error signal for each peak has its own
PID loop filter (proportional, integral, differential gain) to stabilize the clock laser toeach peak in a time-multiplexed fashion. The average of the two correction frequencies
for locking to each of the two peaks is calculated in software. A second PID loop filter
is fed to DDS2 and is used to keep the original correction frequency drift near zero.
A user operated manual drift feedforward (DDS3) is also implemented to compensate
laser drifts.

155
In the next measurement cycle, the laser frequency is set to the other half maximum of
the first peak. The difference in the excitation between these two peaks is computed
and represents the first error signal. When the excitations are equal (difference = 0),then the laser is properly centered on the symmetric transition lineshape. A positive or
negative difference indicates that the frequency must be adjusted to remain centered on
the line. This error signal is filter by a PID (proportional, integral, derivative) filter tofeedback on the AOM shifting the laser light into resonance with the atoms. In the thirdand fourth measurement cycles, the half maxima of the second peak are interrogated,
the second error signal is calculated, and a second PID filter provides feedback to theAOM (over the time interval synchronized with interrogation of the second peak).
After the excitation signal is digitized using a fast, hardware re-triggerable 16-bit
A/D converter, all of the error signal calculation, filtering, and transfer to the frequency
transducer (DDS1, a GPIB controlled DDS synthesizer driving AOM1) is handled insoftware (LabVIEW). No analog biases are present in these digital operations. The
output of the two PID filters is averaged together and fed in-series to a third PID filter.
The output of this third filter actuates on a separate DDS synthesizer, DDS2. Rather
than actuating on the frequency output of DDS2, DDS2 is set to have a linear frequency
drift with controllable amplitude (Hz/s). This drift amplitude is feedback controlled,
and has a primary function of compensating for any residual drift of the clock laser
relative to the atoms. When operating properly, DDS2 keeps the drift of the control
frequency in DDS1 below 1 mHz/s. Furthermore, DDS2 is summed with a third DDS
synthesizer, DDS3, which is reserved for manual feedforward compensation of the laser
drift relative to the atomic transition. During lock operation, we periodically update
this feedforward value so that DDS2 does not accumulate too much drift amplitude as
the clock laser drift changes over the course of a day (varies between ±1 Hz/s). In thisway, each DDS handles laser drift/noise on different timescales and the frequency sumof DDS1, DDS2, and DDS3 (using a frequency mixer) is applied to the AOM1. Note

156
that all critical frequency sources in the experiment are phase locked to the 10 MHz
output of the HP Cs atomic frequency standard.
To tightly lock the clock laser to the atomic transition, the PID filters must be
properly tuned. As a first effort at tuning the PID values, we implemented the ZieglerNichols tuning algorithm. We then optimized the filter by observing the error signal inboth the time and frequency (FFT) domains, and varied the PID values to minimize
the error signal, particulary at low frequencies. The primary lock (with feedback toAOM1) typically used an integrator with a PI corner at 20 s. The secondary lock (withfeedback to AOM2) typically used an integrator corner at 200 s. After the two peaks
were measured over four experimental cycles, the process is repeated. When operatingwith experimental cycles of approximately 1 s, this sets the Nyquist detection frequency
as ∼ 1/(8 s), limiting the servo bandwidth. Under these conditions we typically operated
with a unity gain bandwidth of ∼ 1/(20 s). We sometimes required faster servo response,
trimming the experimental cycle down to a total of 600 ms. We were still limited by
the extra time needed to measure both peaks, and in some cases, operated the lockon a single peak, for the fastest servo attack time. Since the benefit of the two peakis predominantly to cancel very slowly drifting magnetic-field induced Zeeman shifts,
another way to achieve faster attack time is to simply make the multiplexing time
between the two peaks much longer (lock on one peak for a given amount of time, andthen switch to the next peak for the same amount of time).

5.1.3

Other System Improvements

In Section 3.3.1, we saw that laser stabilization to the high finesse cavity is limited by the measurement S/N ratio. The same holds true for laser stabilization to theatomic resonance (the S/N limitation in the atomic case is more severe). This is reflected in the stability of the frequency standard as given in Equation 1.1. A number oftechnical mechanisms exist which limit the achievable S/N ratio of the atom excitation

157
measurement, but which can be overcome or avoided with proper design. We determine
the atomic excitation by measuring the remaining 1 S0 population after clock interrogation by collecting 1 S0 -1 P1 fluorescence. This transition is driven with an intense, nearlyresonant 461 nm probing beam (10 MHz red-detuned, s ' 3) with a beam radius muchlarger than the lattice-trapped atom cloud radius, to avoid inhomogeneities, or noisefrom pointing instability. This 461 nm probing laser is intensity stabilized using an
AOM, and then pulsed on with a second AOM (and a shutter). To ensure high T EM00
mode quality, before illuminating the atoms, the 461 probing beam is sent through asingle mode fiber. The intensity stabilization does not correct for fluctuations due tothe second pulsing AOM or the fiber coupling, so before entering the vacuum chamber, a fraction of the 461 nm probing light is split off with a pellicle beam splitter andmonitored on a photodetector. We use this signal to ensure minimal intensity drift
over many experimental cycles. Over the course of a day, intensity drifts are kept to∼ ±10%. After illuminating the atoms to drive the 1 S0 -1 P1 transition, a fraction of
the total 4π steradians of emitted photons (∼ 1%) is collected by a large aperture (2inch) lens and imaged onto a photo-multiplier tube (PMT, Hamamatsu R7400U-20).
Here we enjoy the fact that a large number of photons are scattered because of thelarge spontaneous decay rate of 1 S0 -1 P1 . Nevertheless, to ensure that we collect morethan sufficient photon numbers so that we are not limited by the Poissonian photon
shot noise, we typically collect photons for a full 5 ms. This is also sufficient time toresonantly heat the 1 S0 atoms out of the lattice.
Despite our efforts to reduce technical noise from the 461 nm probing, our excitation measurement remains limited by a technical source: atom number fluctuationsin the lattice. After loading a lattice with X number of atoms, we make a 1 S0 population measurement proportional to X. Our locking procedure requires a measurement
on each side of the peak to determine the line center. We start a new experimental
cycle, loading a new group of atoms into the lattice. Unfortunately, shot-to-shot load-

158
ing fluctuation can give a new atom number X + ∆X, where ∆X/X is typically near
10%. The next 1 S0 measurement is proportional to X +∆X, and the difference between
the two, used for locking, has excess noise proportional to ∆X. To overcome this, we
implement normalized excitation detection. After measuring the 1 S0 population andheating these atoms out of the trap, we illuminate the atoms with the 679 nm and707 nm repumping laser, driving the 3 P0 population to decay to 1 S0 . Now what waspreviously 3 P0 population can be measured identically as the original 1 S0 population- by scattering 461 nm photons on the 1 S0 -1 P1 transition. The excitation fraction is
simply the 3 P0 signal divided by the sum of the 3 P0 and the 1 S0 signals. Fluctuationsin the lattice-loaded atom number scale both measurements the same, and thus divide
out. Furthermore, because the method for measuring the 1 S0 and 3 P0 is identical, othertechnical noises enjoy common mode rejection (for example, the 461 nm probing laser
typically only fluctuates in power at the 1% level over the timescale between the 1 S0 and
3P

0 measurements).

Using this normalization technique, excitation could be detectedwith a S/N ratio (∼ 50) nearly that of the fundamental limit, the quantum projection
noise (see next section).
In addition to the Zeeman shift uncertainties in Section 4.3, another dominant
contributor to the final achievable frequency uncertainty originated from the AC Stark
shift induced by the lattice confinement. We saw that for typical lattice trap depths,
a lattice laser frequency 1 GHz from the “magic” operating point resulted in a ∼ 1 Hzclock transition shift. For a frequency shift uncertainty at the 10−16 level, this requires
stabilizing the laser frequency at or better than the 100 MHz level. We had previously
used a CW, single mode Ti:Sapphire laser as the lattice laser source. With naturallaser drift on a timescale of tens of minutes typically at or below the 100 MHz level, we
previously provided this laser stabilization by simply monitoring the output frequency
on a high accuracy (50 MHz) commercial wavemeter, and periodically adjusting thelaser cavity to keep the output near the magic wavelength. To improve the lattice

159
laser stability, the laser frequency is now locked to the optical frequency comb, whichitself is stabilized to the clock transition. In doing so, the lattice laser frequency iscontrolled more carefully than is needed for even 10−18 clock operation. To facilitatestabilization to the fs comb, we changed the lattice laser source from a CW Ti:Sapphire
to a diode laser injection locking a Ti:Sapphire system. With feedback to the diodedriving current and laser PZT, the diode laser was locked to the Ti:Sapphire cavity.
With single-mode operation from the laser seeding, the Ti:Sapphire laser required no
additional intracavity elements, such as a birefringent filter, optical diode, or thickand thin etalons [208]. The removal of these optical elements eliminated cavity loss,
facilitating higher output power from the Ti:Sapphire system (as much as 1.5×). The
heterodyne beat between the frequency comb and the lattice laser was stabilized to a 70
MHz RF frequency reference, by feeding back on the Ti:Sapphire intracavity PZT. By
using the wavemeter as a course guide, and by operating the comb at the same repetition
rate each day (made possible by adjusting a New Focus picomotor that translated oneof the fs comb cavity mirrors), the lattice laser frequency could be controlled as close
to the magic wavelength (frequency) as the Stark shift measurements could determine.
Finally, the other major contributor to previous frequency shift uncertainty was
atomic collisions resulting in a density-dependent frequency shift. While no observable
shift had been measured, the uncertainty was dictated by the measurement precision.
Lacking the immediate means to magnify the potential density-related shift by simply
increasing the atomic density one or two orders of magnitude beyond our normal operating density (e. g. as done in [91]), the brute-force use of higher measurement precision
could better characterize these density related effects. This was made possible by theall optical comparison of two high stability optical atomic clocks, motivating the opticalcarrier remote transfer described in the next section.

160

5.2

Optical Carrier Remote Transfer
In Section 4.2.1, amplitude modulation of an optical carrier was used to transmit astable microwave frequency over several km. This could be done with a stability level atshort timescales comparable to the H-maser [79]. Excess noise at longer time scales could
be avoided by implementing a low bandwidth fiber-stretcher to compensate for timevarying group delay of the fiber link. These techniques have been refined and improved
upon, where transfer over an 86 km link has now achieved instability of 5 × 10−15 at 1 s
and 2×10−18 after one day [209, 210]. Just as the high operating frequency of an opticalfrequency standard offers an advantage over a microwave standard, frequency transfer
using a coherent optical carrier can outperform its microwave counterparts. Combinedwith the broad spectral coverage of a fs frequency comb, optical transfer techniques are
the best solution for comparing optical frequency standards. To this end, we developed
a coherent optical phase transfer system for use over the BRAN fiber network, designed
particularly for comparison of the Sr standard to other optical standards at NIST.
Figure 5.2 shows the experimental setup for phase coherent optical transfer. A
CW 1064 nm Nd:YAG is phase-locked to the JILA frequency comb, which itself isphase-locked to the Sr clock. The 1064 nm light is transferred to NIST for measurement with the NIST frequency comb. To actively cancel the accumulated fiber phasenoise, the transfer laser coherence time must exceed the fiber network round-trip travel
time. Our transfer laser has an intrinsic linewidth of 1 kHz in 1 ms, sufficient for fiber
noise cancellation over the (round trip) 7-km link. On the JILA end, ∼ 1 mW fromthe transfer laser is picked off by a polarizing beam splitter (PBS) and detected on a
photodiode (PD), while up to ∼ 40 mW is coupled into the fiber (below threshold forstimulated Brillouin scattering) after being frequency shifted by an AOM. On the NIST
end, the final length of fiber has a gold-coated, flat-polished tip which reflects 90%of the 1064 nm light back to JILA, and transmits 10% for heterodyne measurement

161

stable cavitySr

fs combtransfer
laser

fiber noise
cancellation
λ/4

photodiodeRF frequency
reference (to Cs)

dig phase
detector
w/ pre-scaling

Ca, Yb,stable cavity Hg+, Al+

fs combpol. paddle

AOM

polarizer

loop
filter4 km
fiber link

gold tip

Figure 5.2: Schematic of the phase coherent optical carrier transfer system implemented
to remotely compare the Sr standard at JILA to other optical standards at NIST. The
clock laser, pre-stabilized to the high finesse ultra-stable cavity, is locked to the atomic
transition. A self-referenced fs frequency comb is phase-locked to the Sr clock laser andsubsequently a transfer laser, a Nd:YAG at 1064 nm, is phase-locked to the frequency
comb. In this way, the comb serves as a “gear” linking the lasers in different parts of
the optical spectrum. The Nd:YAG is injected into the fiber link eventually arriving
at NIST ∼ 4 km later. To cancel carrier phase noise accumulated over the fiber link,
phase noise cancellation is implemented using a heterodyne Michelson interferometer.

162
with the NIST fs frequency comb. Light returning from the remote end accumulatesa round-trip phase, again passes through the AOM, and is heterodyned with the local
1064 nm light on the PD. Similar to the fiber phase noise cancellation used elsewhere
for the clock laser (Chapter 3), the beat frequency is used for fiber noise cancellationby phase locking it to an RF reference (fN EN IST ) via feedback to the AOM driving
frequency [193, 192]. In this way, noise processes that are stationary during the roundtrip time are pre-compensated by the AOM. This is not the case for noise at Fourier
frequencies corresponding to times shorter than the round trip time. A pre-scaling of
the detected heterodyne beat frequency by a division factor of 50 is utilized to givethe phase lock a large enough dynamic range to avoid cycle slips under burst noise.
Furthermore, a set of birefringent fiber paddles is used on the input end of the fiber
link to adjust the polarization state of the round-trip light to maximize the power ofheterodyne beat signal. The beat signal power still fluctuates by 1 dB at frequencies
of a few Hz, and slowly degrades by as much as 5 to 10 dB over the course of 1 day
due to time-changing birefringence of the fiber link. Every few hours the fiber paddles
are adjusted to maximize the beat signal strength. To help control polarization mode
dispersion [211] on a fast timescale, a linear polarizer is placed just before the local fiber
input.
To quantify the optical carrier transfer performance, rather than utilizing the gold
fiber tip at the NIST end to terminate the fiber, the gold tip was removed and the fiber
was spliced to a second fiber making the return trip to JILA. The gold tip was installedat the JILA end, so that the transfer scheme could operate with the local and remoteends co-located for out-of-loop comparison. This link has twice the fiber phase noiseof the original JILA-NIST only link. Figure 5.3(a) shows the Allan deviation of theheterodyne beat (mixed down to 10 kHz) between the local and remote 1064 nm light.
Also shown is the frequency stability with the noise cancellation inactive (i. e. freerunning fiber noise) and the measured in-loop instability of the locked heterodyne beat

163

10

Allan Deviation

10
10
10
10
10
10

-14

-15

-17

-18

-19

-20

-21

(a)
10

0

10

1

10

2

10

3

10

4

10

5

Power (dB)

0
-20
-40
-60

(b)

1 mHz
RBW

Power (arb. linear)

Averaging Time (s)
1.0
0.8

(e)
(c)
1 Hz

0.6
0.4
0.2
0.0

0
-0.2
0.0
0.2
Fourier Frequency (Hz) y (Hz)

-10
0
10
frequency (Hz)Figure 5.3: Measurements of the phase coherent optical carrier transfer. (a) Instability
versus time of the remotely transferred optical carrier versus the original, local opticalcarrier. Open circles: No phase noise cancellation over 32 km fiber, Open diamonds:
No phase noise cancellation over 7 km fiber, Closed diamonds: Phase-noise cancellation
over 32 km fiber, Closed circles: Phase-noise cancellation over 7 km fiber, Closed triangles: In-loop estimate of phase noise cancellation. (b) Heterodyne beat between 7 km
remotely transferred 1064 nm light and the frequency comb to which the local 1064 nm
is phase-locked. (c) Heterodyne beat between the Hg+ ion clock laser and the Sr clock
laser remotely transferred from JILA to NIST with the phase coherent optical carriertransfer.

164(divided by two for the one way instability). An impressive 1 s instability of < 10−17
demonstrates that the transfer scheme can be used to compare optical standards withtransfer noise well below the intrinsic noise of the current optical standards. The phaselock loop for the fiber transfer itself has demonstrated locking durations of 70 hours.
Furthermore, the transferred frequency accuracy is 1 × 10−19 , consistent with the best
measured instability.
The effectiveness of the fiber transfer scheme is also shown in Figure 5.3(b),which gives the measured power spectrum for the heterodyne beat between the remote1064 nm light and the comb mode to which the local 1064 nm light is locked. The
uncancelled transfer broadens the relative linewidth to ∼ 1 kHz, whereas the lockedcase reveals a resolution-bandwidth-limited linewidth of 1 mHz. For more details on thecoherent optical carrier transfer, including the resulting phase spectral noise density andextending the transfer scheme to longer distances using a coherent repeater station, see[212, 201]. The choice of optical transfer at 1064 nm was convenient for the spectrum of
the fs frequency combs at JILA and NIST. For longer distance comparisons, the opticalpower attenuation through the fiber link (< 4 dB for 7 km roundtrip path) can begreatly reduced using telecom friendly wavelengths.
As an exhaustive out-of-loop evaluation of the optical carrier transfer scheme,
Figure 5.3(c) shows the linewidth of the optical heterodyne beat between the 1064 nm
light phase-locked to the Sr clock laser via the comb and transferred to NIST and the
NIST fs frequency comb which is locked to the Hg+ ion clock laser [212]. The recovered 1
Hz linewidth demonstrates the exquisite generation and transfer of optical phase control
across the optical spectrum and across km-scale distances, despite the accumulated noiseof more than a dozen phase-lock-loops.
Figures 5.4 and 5.5 give a summary schematic of frequency counting of the Srstandard using both the optical and microwave transfer with NIST. As is clear from
Figure 5.4, the comb plays a critical, centralized role of allowing lasers at different parts

165
of the spectrum to be phase stabilized relative to each other, and does so with dramatic
fidelity [202]. Note that the comb is phase-locked to the cavity-stabilized 698 nm light
before AOM1 used to lock the cavity-stabilized light to the atomic transition. The
synthesizer used as the phase/frequency reference for the comb lock to the 698 laser has
a computer-controlled frequency output (fSRSlock ). The locking program (Section 5.1.2)
updates fSRSlock (see frequency 8 in Figure 5.5) to keep the comb locked to the atomic
transition, counteracting the cavity-stabilized laser frequency drift. This approach wastaken to minimize the number of AOMs used to transfer the atomic transition lock to thefs comb (and the remote optical standard), but not transfer the lock modulation. Using
the formulas in Figure 5.5, for absolute frequency measurements using the Cs-calibrated
H-maser reference link, the Sr transition is found to be:



N
νSr =
(fmaser + fcount ) + fCEO + (fN Ecomb + fN ESr ) − (fof f set + fARP )
10

(5.1)

For a frequency measurement using the optical transfer to NIST, the Sr frequency isgiven by:



N
νSr =
(Y fY AGlock + νY AG − fCEO ) + fCEO +(fN Ecomb +fN ESr )−(fof f set +fARP )M(5.2)
where NIST measures νY AG − fN EN IST using their frequency comb stabilized to an
optical (or microwave) standard. Note that as described in Section 4.1, the integer
mode numbers N and M are determined using wavemeter readings for the clock laser
and YAG transfer laser, respectively.

5.3

Stability Evaluation of the Sr Optical Frequency Standard
In Chapter 1, we looked at a generic expression for the fractional instability of an

atomic frequency standard, which we repeat here for convenience:σy (τ ) =δνη√
ν0 S/N τ

(5.3)

166

stable cavity
enclosure1

distribution
center

2
AOM1

3
AOM2

5 AOM3YAG

4

12

optical transfer
to NIST
AOM

14

11

fs
comb

13

counter

Sr

9
15

PZT

6

16
Y*fYAGlockZ*fSRSlockfDDS2+ fDDS3
8

10

microwave
transferfrom NIST

7

Figure 5.4: Summary schematic of Sr frequency counting with both optical and microwave references. Figure 5.5 gives the relevant frequency relationships at the numbered locations.

167

1: νcavity
2: AOM1 = fDDS1+fDDS2+fDDS3+fARP
fDDS2+fDDS3 ≈ 75 MHz, fARP = 22.3 MHz
3: AOM2 = fNESr = ½ x 155.46464 MHz
4: νSr = νcavity-(fDDS1+fDDS2+fDDS3+fARP)+fNESr
5: AOM3 = fNEcomb = ½ x 155.46464 MHz
6: comb-698 beat = (Nfrep+fCEO)-(νcavity-fNEcomb)
fCEO = 70 MHz
7: (Nfrep+fCEO)-(νcavity-fNEcomb)+(fDDS1+fDDS2)
8: comb lock: (Nfrep+fCEO)-(νcavity-fNEcomb)+(fDDS1+fDDS2) = Z fSRSlock ≈ 100 MHz
for lock to Sr: fSRSlock = (foffset – fDDS1)/Z, Z=80
9: tenth harmonic of rep rate = 10 frep ≈ 950 MHz
10: modulation from NIST H-maser: fmaser ≈ 950 MHz
11: fcount = 10frep-fmaser ≈ 40 kHz
12: transfer YAG = νYAG
13: AOM = fNENIST
14: νYAG ± fNENIST
15: comb-YAG beat = (Mfrep+fCEO) ± νYAG
16: YAG lock: (Mfrep+fCEO) ± νYAG = Y fYAGlock = 60 MHz
Figure 5.5: Frequency relationships for Figure 5.4. For more details on fDDS1 , fDDS2 ,and fDDS3 , see Figure 5.1(c). fARP is an arbitrary offset. fN ESr , fN Ecomb , and fN EN IST
are the phase/frequency references used in the fiber noise cancellation for optical transfer from the distribution center to Sr apparatus, from the distribution center to thefrequency comb, and from the frequency comb at JILA to NIST, respectively. fSRSlockis the reference for the phase lock of the frequency comb to the Sr clock laser andfY AGlock is the reference for the phase lock of the YAG transfer laser to the frequency
comb. fmaser is the modulation frequency referenced to the NIST H-maser, as shownin Figure 4.2. The comb parameters fCEO and frep are illustrated in Figure 4.1. For
more details on the complete system details, see the main text.

168
We have assumed that the noise process dominating the instability is white. The parameter η is approximately unity and depends on the details of the spectroscopic lineshape. We saw that enhancing the signal-to-noise ratio S/N allows us to improve upon
the measurement resolution (stability) provided by the transition line quality factor(Q = ν0 /δν). The standard’s instability can be expressed as the Allan deviation, as
defined in Equation 3.11. A number of different noise processes work to limit the achievable instability, some of them eluded to in Section 5.1. As a starting point to consider
the most relevant noise processes, we write the fractional instability as a sum of several
effects [39]:1σy (τ ) =
πQ

r

Tc
τ



2σ 2
1
1
+
+ N
+γ
N
N nph
N2

 12
(5.4)

Two pulse Ramsey spectroscopy is assumed here (similar but not identical to the caseof Rabi spectroscopy given below). By comparison to Equation 1.1, it is clear thateach term in parentheses is related to the signal to noise ratio (S/N ) for different noise
processes. The first term originates from quantum projection noise, the second fromphoton shot noise, the third from technical atom number fluctuations, and the fourthfrom frequency noise of the interrogation laser. Tc is the experimental cycle time (ofwhich some fraction is spent interrogating the clock transition), N is the atom number,
nph is the number of signal photons detected for each atom, σN is the uncorrelated rms(root mean squared) fluctuations of the atom number, and γ is the frequency noise of
the probe laser.
Using the fluorescence-based measurement described in Section 5.1.3, typicallynph  1 so that photon shot noise (2nd term) is below the quantum projection noise(1st term). Atom loading fluctuations in the lattice limited the detection S/N to avalue typically in the range of 10-15. However, the normalization procedure permitted
measurement S/N up to ∼ 50. This was estimated by exciting the atoms using ashort, strong Rabi pulse which power and Fourier broadened the excitation (reducing

169
the effect of laser frequency noise). We then measured the normalized, shot-to-shot
excitation fluctuations as we re-loaded the optical lattice with new samples.
The most fundamental limit to the atomic frequency standard instability is thequantum projection noise (also referred to as atom shot noise). It is a well known postulate of quantum mechanics that any physical measurement of a quantum system canbe modelled by a Hermitian operator acting on the wave function of the system being
measured, and that the result of that measurement is an eigenvalue of the operator.
Thus a measurement on an atomic state which is a superposition of eigenstates yields astatistical result: one eigenvalue with a measurement probability given by the superposition weighting of its eigenstate. This implies fluctuation (noise) in the measurement
as the wavefunction collapses and is projected onto a particular eigen-basis. For thetwo level system of an atomic frequency standard, this quantum projection noise for thepmeasurement of the ground or excited state is equal to ∆exc = ∆gnd = N p(1 − p),where N is the number of atoms interrogated and p is the excitation fraction [213].
The S/N for the excitation fraction, equivalent to the S/N of the excited state populaption, becomes N p/(1 − p). For comparison to the experimentally measured S/N after
normalization, N ' 2000 − 4000 and p ' 0.4 − 0.5, yielding an S/N ' 50, indicatingthat the observed S/N is consistent with that limited by quantum projection noise.
The quantum projection noise limited instability for the case of Rabi spectroscopy of aLorentzian lineshape with FWHM given by γ can be found to be:sγ
2(1 − p) Ttc
σy (τ ) =
2ν0
pN
τ

(5.5)

where the transition frequency is ν0 and the total cycle time is Ttc (for probing both half
maxima of the Lorentzian). Using typical values for the operation of our Sr standard(γ = 10 Hz, ν0 = 4.29 × 1014 Hz, p ' 0.4, N ' 4000/2, Ttc ' 2 × 1 s), the fundamental
fractional instability limit is approximately 7 × 10−16 .
We have not yet considered measurement instability induced by the clock laser

170
frequency noise. We do not treat here the integrated laser frequency noise over the probe
pulse time (typically tp = 80 ms for the Sr standard) which is relevant for the instability
at that timescale. Rather we focus on spectroscopic probing repeated every experimental
cycle time Tc and separated by nonzero dead time, which contributes to long-term
instability. The atomic excitation measurement corresponds to a temporally-binned,“digital” sampling with sampling rate of fc = 1/Tc . With no means to low pass filter theexcitation measurement resulting from the atom-laser interaction, excitation resulting
from high frequency laser noise is aliased into the detection bandwidth, indistinguishable
from excitation originating from laser noise in the detection bandwidth. The lock to theatomic transition, unable to distinguish the two, improperly compensates for the aliased
noise and introduces extra instability into the frequency standard. All sequentiallyoperated cold atom standards suffer from this effect as do any atomic standards withmodulated interrogation around the line center. Larger dead time in the experimental
cycle makes this effect more pronounced. Sequential cold atom samples have a minimum
dead time associated with cooling and loading the atomic sample. The dead time of
the Sr standard (typically from 0.5 to 1 s) also includes loading the optical lattice,polarizing the atomic sample, and reading off the populations after interrogation. The
aliasing effect depends upon the particular spectroscopy implemented, which influences
how sensitive the population excitation is to frequency fluctuations (in the general case,this is a time-dependent sensitivity). This effect, which can be viewed as resulting fromtime-dependent gain in the atom-laser feedback loop, was first illuminated by G. John
Dick at the NASA Jet Propulsion Laboratory and is now referred to as the Dick effect.
The fractional instability resulting from this effect can be shown to be [214, 215]:v
u ∞  2 
2 
X gc,m gs,m1u
1mt
σy (τ ) =+ 2 Sf
(5.6)
2
µ0 τ
Tc
g0
g0
m=1

Here Sf (m/Tc ) is the one-sided power spectral density of the free running probe laser(local oscillator) at the Fourier frequency m/Tc . The factors gc,m and gs,m correspond

171
to the Fourier sine and cosine series coefficients giving the sensitivity spectral content
at f = m/Tc and are given by:
1
gs,m =
Tc

Z Tc

1
gc,m =Tc

Z Tc

g() sin0g()cos

0

2πm
Tc



2πm
Tc



d

(5.7)

d

(5.8)

and the normalization factor g0 is:
1
g0 =
Tc

Z Tc
g()d

(5.9)

0

The physics of the atom laser interaction is hidden in the time-dependent sensitivity
function g(t). This function can be found for the particular spectroscopic details bysolving for the population evolution as a function of probing time and detuning fromthe atomic transition. For the special case of coherent excitation from a Rabi π-pulse,
the sensitivity function is:∆HM[sin Ω1 (t)(1 − cos Ω2 (t)) + sin Ω2 (t)(1 − cos Ω1 (t))](5.10)(1 + ∆2HM )3/2
q
where Ω1 (t) = βt/tp , Ω2 (t) = β − Ω1 (t), β = π 1 + ∆2HM and the half maximum
g(t) =

detuning is ∆HM ' .799. Figure 5.6(a) shows this Rabi π-pulse g(t) for tp = 80 ms and
Tc = 1 s. Using this g(t) and the known probe laser frequency noise spectrum (Figure
3.4(c)), Equation 5.6 can be solved for the Dick-effect-limited instability, found to be∼ 2 × 10−15 τ −1/2 , larger than the quantum projection noise instability. This sets a
Dick effect limit on the Sr instability.
Looking at Equations 5.6-5.10, there are several ways to reduce the Dick noise
instability limit. The first is to reduce the clock laser frequency noise. Some considerations for improving the laser frequency noise were discussed in Chapter 3. Interestingly,
as the laser frequency noise is reduced, narrower transition linewidths will be observed
for the atomic systems with this potential. This means that the quantum projection
noise instability will also decrease. As a result, although reduced laser noise will reduce the instability, in some cases the Dick effect may continue to play a limiting role.

172
Fortunately, a quieter laser means that the probing time can be increased to a larger
fraction of the total cycle time. A reduction in dead time results in further reduction of
the Dick effect. Thus, whether the standard ends up being stability-limited by quantum
projection noise or the Dick effect depends on the details.
Without improving the laser frequency noise, increasing the probing time can stilldecrease the Dick effect. In the Sr case, a typical probing time of 80 ms is chosen to
give a very reliable ∼ 10 Hz wide line. As seen in Chapter 3, we have probed for longer
intervals. However, a tradeoff does seem to exist: going to too long probing times results
in noisier, less well-defined spectra (becoming more sensitive to clock laser noise). This
creates extra problems for the lock to the atomic transition. Note also that even in thelimit when tp = Tc , the Dick effect is nonzero because of the time dependence of thesensitivity function g(t).
Another way to reduce the Dick effect is by reducing the cycle time Tc for a
fixed probe time tp . In the case of pure white frequency noise from the clock laser,
the reduction is similar to that seen from increasing tp for a fixed Tc . In other words,
tp /Tc or the fraction of dead time (1 − tp /Tc ) is the important parameter. However,in the case of frequency noise which falls off at higher frequency, going to shorter cycle
times has the extra advantage that the aliased laser noise originates from higher Fourier
frequencies where the noise spectral density is reduced. This is partially the case for
the Sr clock laser, which at the lowest frequencies has noise set by the thermal noiseof the cavity, resulting in a frequency noise power spectral density that falls off as 1/f(see Figure 3.4(c)). Table 5.1 gives the Dick-limited instability of the Sr clock laser forseveral values of Tc and tp .
Decreasing the dead time reduces the Dick effect by making the sensitivity function g(t) more homogeneous over the cycle time Tc . This idea could be taken further
by designing a pulse shape which has a more even g(t) over the probe duration. This is
the case for two-pulse Ramsey spectroscopy (as one might expect the sensitivity must

g(t) sensitivity

173

(a)

1.0
0.8
0.6
0.4
0.2
0.0
0.0

0.1

1.0

1.1

1.2

Allan deviation

time (s)

-15

10

-16

10

total deviation

(b)

1

10

-15

10

-16

10

time (s)

100

1000

-17

10
1
(c)

10

100
time (s)

1000

10000

Figure 5.6: (a) The sensitivity function, g(t), with an atomic probe time of tp = 80
ms and an experimental cycle time of Tc = 1 s. During the probe time, the sensitivity
function is given by the Rabi interrogation of the atoms. All other times are deadtime, with g(t) = 0. The Dick effect results from time-dependence of the sensitivity
function, introducing atom-laser interaction sensitivity at frequencies equal to fc = 1/Tc
and its harmonics. This measurement noise is then aliased to DC where the servo tothe atomic transition, unable to recognize its aliased origin, compensates for it. (b)Stability figures for the Sr atomic clock. Black dashed line: quantum projection noise
limit. Solid red line: estimate for the Sr clock instability. At short times, this is thefree-running instability of the Sr clock laser. At τ = 20 s, the atom servo crosses unity
gain with a single integrator, allowing the clock laser instability to average down withthe atomic transition at nearly 1/τ . After 100 s, the Dick effect limit is reached, where√
the instability then averages down as 1/ τ . Green open circles: In-loop measure of the
Sr clock instability based on the error signal. Blue filled circles: Measured instability
between the JILA Sr system and the NIST Ca system, linked by the remote carriertransfer. (c) Instability between remotely transferred JILA Sr system and the NIST Yb
system. Here, Sr is operated with a single peak lock to maximize the atom servo attack
time.

174
Table 5.1: Dick effect limited instability of the JILA Sr standard for various values ofexperimental cycle time Tc and transition probing time tp
tp
80 ms
80 ms
80 ms
80 ms
160 ms
320 ms
1s
1s
80 ms

Tc
1s
500 ms
160 ms
1s
1s
1s
1s
1s
80 ms

σ(τ = 1s)
2 × 10−15
1.2 × 10−15
5 × 10−16
2 × 10−15
1.6 × 10−15
1.2 × 10−15
4 × 10−16
4 × 10−16
2 × 10−16

be constant during the Ramsey dark time). In the limit of a Ramsey dark time much
longer than the pulse time of the two Ramsey pulses, g(t) approaches a box function. As
we considered the relative advantages of Rabi or Ramsey spectroscopy on our latticetrapped Sr atoms, the atomic confinement puts the two methods on similar footing.
One possible advantage of Ramsey spectroscopy (particularly when the Ramsey darktime is much longer than the pulse time) is a reduction in the Dick effect. However, thebenefits of the shape of g(t) during the spectroscopic interrogation are only substantial
when the interrogation accounts for a large fraction of Tc , i. e. when the dead time issmall. For our normal operating conditions, the smallest dead time is ∼ 85% of Tc , andthe corresponding Dick instability reduction for Ramsey spectroscopy is only at the 10%
level [216]. However, as the experimental cycle is refined, decreases in Tc and especially
increases in tp may eventually merit worthwhile instability reduction from the use ofRamsey interrogation.
Finally, another approach to reducing the Dick effect is to have multiple atomic
samples, so that the local oscillator can sequentially interrogate the different atomic
samples and effectively reduce or eliminate the dead time. This solution is conceptually straightforward, however increases experimental complexity. For Cs fountains, thistechnique may be compatible with the multi-atomic-cloud juggling fountains proposed

175
to circumvent density related shifts [217]. The use of multiple traps to reduce the Dickeffect has recently been demonstrated for a Cs microwave standard [218].
With insight into the relevant instability limitations, we now consider the performance of the Sr standard. Figure 5.6(b) shows different stability estimates for the Srstandard. The dashed black line indicates the fundamental limit given by the quantum
projection noise. The solid red line gives the best known estimate of the current operational instability for the Sr standard. At short time scales, the instability is governedby the free-running instability of the clock laser (see Chapter 3). At approximately
20 s, the servo to the atomic transition crosses unity gain with a single integrator (20dB/decade) with the instability improving almost as 1/τ as the laser tracks the atoms.
This continues until ∼ 100 s, where the white-frequency Dick noise limit is reached,√at which point the instability averages down as 1/ τ . To reduce long timescale oscillations, we have at times operated the atom-laser servo aggressively, yielding a servo
bump in the instability at 10-20 s. The green open circles (in Figure 5.6(b)) indicate
an in-loop measure of the Sr instability, taken from the error signal of the lock to theatomic transition. Finally, the blue dots indicate an independent, out-of-loop evaluation
made by comparing the Sr JILA standard to the NIST Ca standard, using the opticalcarrier fiber link described in Section 5.2.
To better characterize the potential stability, Figure 5.6(c) shows the measured
fractional instability between the Sr JILA standard and the NIST Yb standard, again
utilizing the optical fiber link. For the measurement shown, the Sr standard was operated by locking to just one of the mF = ±9/2 transitions, helping to facilitate faster
servo time. The instability of 1 × 10−16 near 1000 s and crossing into the 10−17 decadeshows strong potential of both the Yb and Sr standards. At the current time, thisrepresents the best stability for a neutral atom system and is comparable to the best
stability observed in a single-trapped ion system. With the large atom number enjoyedby the neutral atom samples, the stability of the neutral atom system has the potential

176
to substantially exceed that of the single ion standards. As seen by the analysis of thissection, doing so will foremost require a more stable clock laser, to reduce the Dickeffect and allow narrower atomic transitions. Afterwards, enhancing the lattice-trapped
atom number will bring the quantum projection noise further down.

5.4

Accuracy Evaluation of the Sr Optical Frequency Standard

5.4.1

Measurement Description

In Section 4.3, I described our systematic uncertainty evaluation of the Sr clocktransition frequency utilizing an atomic microwave reference and later a stable laserreference. As seen in the last section, the measurement precision made possible bydirectly comparing two optical atomic standards gives an even higher resolution probe of
the physics governing the Sr clock transition shifts. This enables a significantly improved
characterization of the Sr clock frequency uncertainty. We make this characterization byremote comparison of the Sr standard to the NIST Ca standard (measurement schemesummarized in Figure 5.7). The Ca clock is a simple and robust system that uses freely
expanding cold atoms. Like a hydrogen maser, it serves as a highly stable frequency
reference, but with 100 times better stability at short times. As we just saw, the stabilityof the Sr-Ca comparison can reach below 3 × 10−16 after 200 s. However, the Ca clock
is susceptible to long-term (> 1000 s) drifts due to residual Doppler effects associatedwith the free space Ca. As we evaluate frequency shifts from individual mechanisms, inorder to optimize the shift uncertainties, frequency measurements are thus made in 100s time windows. To remove sensitivity to long-term Ca drifts, these 100-s windows areinterleaved as a particular parameter of the Sr clock is systematically varied. Typically,
the parameter is toggled between two settings for two consecutive 100-s windows, anda Sr clock frequency shift is measured between them. Many such pairs are accumulated
to average to a measurement precision below 1 × 10−16 , enabling rigorous evaluations of177

Figure 5.7: Summary of the experimental setup used for evaluation of systematic shiftsof the Sr system by remote comparison with the NIST Ca optical frequency standard.
The Sr atomic reference is counted and distributed in direct analogy to traditional clocks
using mechanical gears, albeit at optical frequencies. The Sr atomic clock at JILA (1,consisting of lattice trapped Sr system and the cavity-stabilized clock laser) serves as
the atomic standard to which an optical frequency comb (2) is phase-locked. A CW
Nd:YAG laser at 1064 nm (3, a non-planar ring oscillator as shown in the figure) isphase-locked to the same frequency comb and transferred to NIST via a phase-noisecancelled fiber link (4). The 1064 light emerges from the fiber at NIST and is phasecoherent with the light originating from JILA, as symbolized by the syntonized clocks
on either fiber end. The Ca optical clock at NIST (5, consisting of free space Ca system
and a cavity-stabilized laser at 657 nm) is the atomic reference to which another opticalfrequency comb (6) operating at NIST is phase locked. The clock comparison (7) is
made by a heterodyne measurement between the NIST frequency comb and the 1064
nm transmitted light.

178
key Sr clock frequency shifts at this level. This measurement approach is facilitated by
the robustness of these optical clocks, as both systems are regularly operated on-demand
for timescales of a day.
For the Sr clock operation reported here, approximately 4000 87 Sr atoms are laser
cooled to 2.5 µK and confined in the one-dimensional optical lattice with a longitudinal(transverse) trap frequency of 42 kHz (120 Hz), a lattice depth U ' 35Er , and asingle beam lattice intensity of I0 = 3 kW/cm2 . With the optical pumping techniques
previously described, the atoms are (doubly) spin polarized and occupy only the twostates mF = ±9/2 . Under a weak bias field of B = 200 mG, we interrogate the isolated
mF = ±9/2 clock transitions for 80 ms, allowing Fourier-limited spectral linewidths of
10 Hz. The average atomic density is ρ0 ' 1 × 1011 cm−3 .
We now consider systematic shifts and their uncertainties from a variety of physical origins:

5.4.2

Lattice AC Stark shift

In Section 2.6, we derived an expression for the dipole polarizability of an atomic
state, which provided the means to confine the atoms in the lattice dipole potential. We
implicitly made a simplifying assumption that the perturbing electric field was polarizedalong a particular axis. This enabled us to neglect anisotropic terms of the polarizability,
which accounts for an induced dipole moment along an axis orthogonal to the electricfield. Analogous to the classical picture, in a more general case the induced dipole mustaccount for all contributions including anisotropic ones [219]:



 
 dx   αxx αxy αxz   Ex 



 



 
 dy  =  αyx αyy αyz   Ey 



 


 

Ez
αzx αzy αzz
dz(5.11)

179
The stark shift can be written as:
1~ ↔ ~11
α E = − Ei αij Ej = − Ei di
U =− E222(5.12)

where the double arrow denotes the tensor nature of α, and the last two lines use theEinstein summation convention where summation over repeated indices is presumed. In
an atomic system, the polarizability operator can be derived from perturbation theory
for a state a. When the fine structure splitting is much larger than the magnetic sublevel
splitting (due to m dependent Stark effect), then this operator can be represented as amatrix in the subspace of the ground magnetic sublevels of Ja :hJa ma |αˆij |Ja m0a i =1 X hJa ma |di |Jk mk ihJk mk |dj |Ja m0a i hJa ma |dj |Jk mk ihJk mk |di |Ja m0a i+~
ωak − ωL
ωak + ωL
k6=a(5.13)
where k denotes the summation index over the intermediate states, and the other quantum numbers besides J and m are not explicitly shown. Furthermore, we have assumed
large detuning from any atomic transition. Note also that while we are considering only
total electronic spin J and fine structure here, under the appropriate conditions theformalism trivially extends to other angular momentum quantum numbers (e. g. total
angular momentum F if the hyperfine structure splitting dominates the magnetic state
splitting).
It is common to transform the Cartesian operator α̂ij into a sum of polarizability
terms, known as the scalar (αs ), vector (αv ), and tensor (αt ) polarizabilities [219]. Thisis a transformation to the spherical tensor basis:3(Ĵi Jˆj + Jˆj Ĵi ) − Ja (Ja + 1)δˆij
αˆij = αs δˆij − αv (Ĵi Jˆj − Jˆj Ĵi ) + αt 2
Ja (2Ja − 1)

(5.14)

2 X |hJa kdkJk i|2 ωak(δJk ,Ja −1 + δJk ,Ja + δJk ,Ja +1 )2 − ω23~gJ
ωak
L(5.15)αs =k6=a

1 X |hJa kdkJk i|2 ωLαv =2 − ω2
~gJ
ωak
L
k6=a



−1
1
1
δJk ,Ja −1 −δJk ,Ja +δJ ,J +1
Ja
Ja (Ja + 1)
Ja + 1 k a(5.16)

180
2Ja − 1
2 X |hJa kdkJk i|2 ωak
Ja (2Ja − 1)−δJk ,Ja −1 +αt =δJ ,J −
δJ ,J +1
2 − ω2
3~gJ
Ja + 1 k a (Ja + 1)(2Ja + 3) k a
ωak
L
k6=a

(5.17)
Here gJ = 2Ja + 1 is the ground state degeneracy, and δij is the Kronecker delta
function. The Wigner-Eckart theorem has been applied, so that the scalar, vector, andtensor polarizabilities are functions of the reduced dipole matrix elements only. All of
the geometrical details remain in Equation 5.14. Note also that αt = 0 for Ja = 0, 1/2,
and while it is not obvious from Equation 5.16, αv = 0 for Ja = 0. To find the AC stark
shift for a state with Ja , the scalar, vector, and tensor polarizabilities can be calculatedusing Equations 5.15 - 5.17. The polarizability operator matrix for the relevant ij
dimensions (determined by the electric field) can then be calculated with Equation 5.14
in the ma subspace of Ja . In general, this matrix is not diagonal. Diagonalization yields
the total polarizability for each ma state in Ja and a given direction ij. By choosing~ the AC-stark shift
the particular sub-level of interest together with the electric field E,
is determined by Equation 5.12.
In some cases, the polarizability matrix is already diagonal in the m basis forthe important dimensions, leading to a straightforward AC stark shift calculation. For
example, for light which is linearly polarized along the quantization axis, the AC stark
shift is found to be (e. g. [220]):
E02
3m2a − Ja (Ja + 1)
U =−αs (ωL ) + αt (ωL )4
Ja (2Ja − 1)

(5.18)On the other hand, circularly polarized light with the k-vector along the quantization
axis has an AC stark shift given by (e. g. [221]):ma
3m2a − Ja (Ja + 1)
E02
U =−αs (ωL ) +ξαv (ωL ) −αt (ωL )4
2JaJa (2Ja − 1)

(5.19)

where ξ = 2γ/(1 + γ 2 ) = ±1 (circular polarization) and γ is the ellipticity parameter.
References [220, 207] points out additional geometrical factors for the more general casewhere the linear polarization is at an angle to the quantization axis or the circularlypolarized k-vector is at angle relative the quantization axis [207]. Note that in Equations

181
5.13, 5.14, 5.18, and 5.19, F can replace J when the hyperfine structure energy also
dominates the Stark shift. Equations relating α(J) to α(F ) can be found in multiplereferences (e. g. [219, 220]).
For J = 0, the vector and tensor polarizabilities are zero. It can be seen that
Equation 2.62 corresponds to the scalar polarizability. However, we remember that
the Sr clock states are not perfectly J = 0 because of hyperfine interaction. This
makes the calculation of the vector and tensor polarizability terms more complex. To
be done properly, rather than using the polarizability operator (Equation 5.13) which
originates from perturbation theory to second order in the electric field, the atom-lightand hyperfine interaction can be treated simultaneously as a perturbation. A solution
to third order (two orders in the electric field, and one order of hyperfine interaction)
can yield the vector and tensor polarizabilities for 3 P0 [222]. This was done for the caseof Yb. The magnetic dipole hyperfine interaction was seen to introduce only a non-zero
vector polarizability, with the vector Stark shift given by:U=

E02 mFξαv (ωL )4 2F(5.20)

It has been further seen that the electric quadrupole hyperfine interaction introduces
at least a non-zero tensor polarizability [220]. Another approach to calculation of theseeffects may include the effective operator formalism [223].
To estimate the size of the vector and tensor polarizabilities, one may consider
the effects of the hyperfine interaction on the polarizability. The first is that the higherlying intermediate states coupling to the clock states exhibit hyperfine splitting. As
the different clock state sublevels couple to these higher lying hyperfine split states, thepolarizability of the individual sublevels differs by an amount scaling with the hyperfine
splitting. A Taylor expansion of Equation 2.62 with the hyperfine splitting included
leads to a correction term of order ∆hf s /(ωak − ωL ). Dominated by the 3 S1 effect on
3 P , this correction term is on the order of 10−4 [100].
0

The authors of [100] used the

182
hyperfine splitting to estimate the vector AC stark shift, finding it to be < 10−4 of thescalar shift (< 10 Hz). The hyperfine interaction also mixes a small fraction of 3 P1 into
3 P , which with J = 1 is much more sensitive to vector and Stark shifts. This admixture0

can also be used to approximate a further contribution to the vector and tensor shifts[222, 16].
For Sr clock operation using ±mF spin-polarized samples, the vector and tensor
shifts do not play a major limitation. This is partly because of their small estimatedmagnitude, but further because of the design of the interrogation. Optical confinementof the Sr atoms occurs at the “magic” wavelength where the polarizabilities of thetwo clock states are equal [100]. As seen above, the scalar Stark shift exhibits no mF
dependence, the vector shift exhibits linear mF dependence, and the tensor shift exhibits
quadratic mF dependence. The opposite symmetries of the vector and tensor shifts
facilitate orthogonalization of their effects experimentally. Because of the antisymmetricmF -dependence of the vector shift, clock stabilization to the average of the mF = ±9/2transitions eliminates dependence of the clock frequency on the vector light shift, just
as for the 1st order Zeeman shift. Its effect would instead be observed as a change in thefrequency separation between the two ±9/2 transitions added to the Zeeman splittingfrom the bias magnetic field. The averaged clock transition retains dependence on
the symmetric tensor shift. However, the tensor shift simply adds a |mF |-dependent
offset to the much more dominant scalar term. Thus, for a given lattice polarization,
each spin state has a well-defined magic wavelength for insensitive confinement. By
experimentally ensuring that we operate at λmagic for our given pair of nuclear spinstates, we can safely eliminate the scalar, vector, and tensor shifts.
The lattice laser providing the atomic confinement is frequency stabilized to theoptical frequency comb which itself is locked to the Sr clock laser. At a lattice peak intensity of I0 = 3 kW/cm2 and at the typical operating lattice laser frequency (368554.324
GHz), we observe a 6.5(5) × 10−16 shift in the clock frequency compared to zero in-183

occurrences

20
15
10
5
0

-0.3

0.0
0.3
0.6
frequency shift (Hz/I0)

0.9

Figure 5.8: Histogram of the experimentally measured frequency shift sensitivity of the
Sr clock transition due to the AC Stark shift from the lattice laser intensity. I0 = 3
kW/cm2 .

184
Table 5.2: Experimentally measured values of λmagic .
λ (nm)
813.420(7)813.418(10)813.428(1)813.4283(12)813.4274(4)Reference
[29]
[21]
[143]
[22]
[23]

tensity (see Figure 5.10). Note that because of a non-zero density shift (see below),
it is difficult to completely separate density related effects from measurement of thelattice Stark effects as the lattice intensity is changed. For example, as the lattice
depth and thus trap frequency is reduced, the spatial extent of a given motional stateincreases (see Equation 2.33 and the surrounding equations). Assuming all other things
remaining constant, this results in a density reduction (as the effective trap volume
increases). However, a reduced lattice trap typically traps less atoms, and in manycases the trapped sample is colder. The reduced temperature corresponds to a smaller
spatial extent of the wavefunction, partially counteracting a density reduction. We havetypically observed a constant blue and red longitudinal sideband amplitude ratio whilechanging the lattice depth. In this case, the mean density scales with the square root of
each trap frequency. With the added complexity that the electronic excitation depends
on the confinement, a non-zero density shift can muddy the measurement waters of thelattice Stark shift. For this reason, it was useful to measure the lattice Stark shift below
the highest achievable densities (reduced atom number). Nonetheless, a correction tothe observed lattice Stark shift was included to account for the density change induced
shift.
Combining this lattice Stark shift measurement with our previous measurement of
the weak clock sensitivity to the lattice frequency (Figure 4.4), we extrapolate the magic
lattice frequency to be 368,554.68(18) GHz, corresponding to a vacuum wavelengthof 813.4274(4) nm. Table 5.2 shows the measured λmagic values since high precision

185
interrogation of the 1 S0 -3 P0 transition in an optical lattice was begun. Although tensor
shifts are estimated to be small, it should be remembered that the magic frequency wereport here is specified for the π-transitions from the mF = ±9/2 nuclear spin states.
Even though the total electric dipole polarizability contribution to the transition
shift is cancelled to zero, the shift of each clock state is large (100 kHz). This large
state shift motivates the question of how large the next order contribution is: thedipole hyperpolarizability (fourth order in E). The hyperpolarizability is somewhat
complicated, with dependence on both one and two photon atomic resonances [222, 224].
For 87 Sr, one worrisome contributor to the hyperpolarizability is a two-photon transition
3 P -3 F which is 5 nm detuned from the λ02magic at 818.6 nm. This contribution has been

experimentally investigated [143]. Furthermore, by probing the clock transition undervery high lattice intensity, the authors of [143] made a measurement of the fourth-order
Stark shift, finding a coefficient of < 10(10) µHz/Er2 . This experimental measurement
is approximately an order of magnitude larger than theoretical calculations based on
the calculated magic wavelength at 795 nm [136, 100]. For our operating conditions andbased upon the experimentally determined shift coefficient, the shift is 2 × 10−17 , withthe same uncertainty.
The Stark effect from higher order multipoles can provide additional shifts to theclock transition. The magnetic dipole (M1) and electric quadrupole (E2) polarizabilities
are suppressed by at least the fine structure constant squared compared to the electric
dipole polarizability [222, 100]. Numerical estimates put αM 1 ' αE2 ' 10−7 αE1 . Thesehigher multipole contributions are particularly important in the standing wave of an
optical lattice: the Stark shift spatial dependence from the higher-order multipole polarizability differs from that of the larger electric dipole polarizability and frustrates theexistence of perfectly well-defined magic frequency for all multipoles [225].
Before leaving the lattice-induced Stark shift, it is worth mentioning that during
the experimental measurement of the shift of the mF = ±9/2 averaged clock transi-

186tion, while varying the lattice intensity, we also observed a small (10−15 ) change in thefrequency separation between the mF = ±9/2 transitions. As mentioned above, one
possible explanation for this is the vector Stark shift. Unfortunately we have not yet
had the opportunity to further investigate this observation. Other possible explanations
include an inhomogeneous magnetic field which, as a varied lattice intensity changes thespatial confinement of the interrogated atoms, the atoms sample this field differently
yielding a lattice-dependent 1st order Zeeman shift. Furthermore, an mF antisymmetricdensity shift could also play a role, due to unwanted density change as the lattice isvaried. If the observed shift was assumed to be the vector Stark shift, knowledge of thestress-induced birefringence of the vacuum window would be important. This observation merits further investigation, particularly with well-controlled circularly polarized
lattice light.

5.4.3

1st - and 2nd - order Zeeman shifts

As with the lattice vector Stark shift on the clock transition, the 1st order Zeeman shift on the clock transition (−108.4(4) × mF Hz/G [151]) is cancelled due to theantisymmetric linear dependence of the ±9/2 states on the magnetic field. To individually address spin states, we choose a bias field (B0 = 20 µT = 200 mG) large enoughto resolve π-transitions and reduce line pulling from residual populations of other spinstates, but small enough to keep the spin-symmetric 2nd order Zeeman shift small. The
B-field is calibrated by measuring the frequency spacing between the two spin statetransitions. To determine the 2nd -order sensitivity and the 1st -order insensitivity, wemeasure clock frequency shifts as a function of B. An example of one such measurement is shown in Figure 5.9(a). Each set of data is fit to a second-order polynomial.
To extract the 2nd order coefficient, we constrain the linear term to zero and performthe fit. To extract the 1st order coefficient, we constrain the quadratic term to thewell-established theoretical estimate. The fit parameters of many such sets of data are

187

(b)

-2.0
-1.5

B for clock
operation

-1.0

6.0
occurrences

frequency shift (Hz)

(a)

3.5

-0.5
0.0

1.0

0.5
0
100 200
bias B-field (µT)

-90 0
90
lin. shift (mHz)

Figure 5.9: Experimentally measured frequency shift sensitivity of the Sr clock transition
due to the Zeeman shift. (a) Measurement of the shift at three magnetic field values.
The data is fit to a 2nd order polynomial to extract the 1st and 2nd order Zeeman
shift coefficient. (b) Histogram of the linear (1st order) Zeeman shift coefficients. The
mean, consistent with zero, indicates that the two-peak lock to the mF = ±9/2 stateseffectively eliminates sensitivity to the linear Zeeman effect. A similar histogram forthe quadratic term gives the 2nd order Zeeman sensitivity.

188
averaged (see Figure 5.9(b)) and the 1st -order shift is found to be 2(2) × 10−17 (for
B0 ), consistent with zero. The second order shift is 2.3(2) × 10−17 and the measured
shift coefficient is 5.8(8) × 10−8 T−2 , consistent with other measurements [26]. This
number also agrees with previous theoretical calculations (e. g. [226, 151]). Note that
this 2nd order Zeeman shift is significantly smaller than that observed in Cs and othermicrowave standards [227]. This is in part because the Sr clock states, with J = 0, haveno hyperfine structure and so the intermediate states contributing to this second ordershift (principally 3 P1 ) have much larger atomic detuning (fine structure splitting) than
the nearby hyperfine states in microwave standards. While the B-field was a dominant
contributor in previous shift evaluations near zero field, note that the averaging technique of the mF = ±9/2 transitions under a small bias field makes this shift uncertainty
quite small, with room for further improvement.

5.4.4

Density shift

While an ensemble of neutral atoms enables large signal-to-noise measurements forhigh precision and stability, interactions among colliding atoms can result in frequency
shifts that degrade the system accuracy. Density dependent collisional shifts play animportant role in the operation of the highest accuracy Cs fountain standards (e. g.
[7, 228, 229]). The reduced collisional interaction of cold Rb atoms is the principal
motivation for the development of Rb fountain standards [230, 231]. For the case oflattice clocks, unity (or less)-filled sites in a 3-D lattice can keep atomic spacing to atleast half an optical wavelength and thus reduce interatomic interactions [100, 232],keeping the expected density shift small. For the 1-D lattice, use of identical 87 Sr
fermions at ultracold temperature can exploit the Pauli-exclusion principle to reduce
interactions by eliminating even-wave collisions [233, 234]. If the atomic sample issufficiently cold, the lowest odd-wave (p-wave) collisions are frozen out. With the s-wave
collisions remaining forbidden by the Pauli exclusion principle, the density shift could189
be very small even at high ultracold densities. Because of this property, fermions havebeen anticipated as good candidates for atomic frequency standards. Pauli-blocking
resulting in the absence of collisional frequency shifts has been observed experimentallyat high densities for RF transitions [234, 235].
In the experimental situation described for our normal clock operation, although
only one nuclear spin state is interrogated at a given time, the presence of a second
spin state in the ground electronic state means that the atomic sample is not composedof identical fermions. Collisions between identical spin states would presumably be
suppressed, while collisions with the secondary spectator spin state would not be. Withor without Pauli-suppression and the presence of a second spin state, the details of
the resulting density shifts require knowledge of the interatomic potentials. Ground(1 S0 -1 S0 ) and excited (3 P0 -3 P0 ) state inter-atomic potentials have been theoreticallycalculated [236, 237], but the only experimental measurements exist in photoassociation
spectroscopy of the even isotopes of Sr [238] pertaining to ground state interactions.
Our previous investigations of unpolarized, nuclear-spin-degenerate 87 Sr revealed
no indication of collision related frequency shifts. Using the high measurement precision afforded by the optical-optical comparison, we now observe a non-zero densitydependent frequency shift in our doubly-spin-polarized sample. This measurement wasmade using a fixed lattice environment, and observing clock transition shifts as thenumber of trapped atoms was varied. Typically, low atom numbers were achieved byremoving a loading mechanism on the 1 S0 -1 P1 MOT, either the Zeeman slower or theatomic beam transverse cooling. As discussed below, the measured frequency shift value
depends on a number of details including the excitation fraction and the nuclear spinstate. By proper control of these parameters (ρ0 = 1 × 1011 cm−3 , mF = ±9/2, excitation fraction ∼ 16%), we are able to measure and control this shift to 8.9(8) × 10−16(see Figure 5.10).
As a result of the shift dependence on several experimental details, further control

190

occurrences

40
30
20
10
0

-0.9 -0.6 -0.3 0.0 0.3
frequency shift (Hz/ρ0)

Figure 5.10: Experimentally measured frequency sensitivity of the Sr clock transition
to the atomic density. ρ0 = 1 × 1011 cm−3 . These measurements were made by varying
the atom number loaded into a fixed lattice environment.

191
or characterization of the density shift requires a quantitative understanding of therelevant collision mechanisms yielding the shift. Study of these ultracold collisions [239]
can yield important interaction details relevant both to Sr and more broadly to othersystems, and are worthwhile in their own right. Furthermore, understanding theseeffects can be useful for quantum information applications such as quantum simulation
or multi-particle entanglement for universal quantum logic gates (e. g. [240, 241, 242,
243, 244, 245]), which try to exploit atomic collisions. To this end, we utilized the 87 Sr
frequency standard as a sensitive tool for studying interatomic collisions by measuring
their corresponding density-dependent shifts under different conditions.
At sufficiently cold temperatures, where higher-order partial waves are frozen out
due to their centrifugal barrier, the collision process of two particles can be describedby their dominant s-wave interaction. Here we consider only two body collisions. In
this case, the interaction strength, which depends upon the internal state of each atom,
can be characterized by a single parameter, the s-wave scattering length. For two-levelatoms, the transition frequency shift due to cold collisions can be derived by applicationof the quantum Boltzmann equation [246, 247] or by consideration of the mean fieldinteraction [248, 249, 250], and is found to be:∆ν12 =

2~n[g22 a22 ρ22 − g11 a11 ρ11 + (ρ11 − ρ22 )g12 a12 ]m(5.21)

Here m is the atomic mass, axy is the scattering length describing collisions between
particles in the x and the y internal states, ρ11 (ρ22 ) is the ground (excited) state
population fraction, and n is the atomic density. gxy is the two particle correlation
function at zero separation and is given by the wavefunction overlap integrals:
gxy =hΨ†x Ψ†y Ψx Ψy ihΨ†x Ψx ihΨ†y Ψy i

(5.22)The value of the gxx correlation function can be neatly divided into four cases: (1) for
two identical bosons in a thermal gas, gxx = 2 (2) for two atoms in a Bose-Einstein

192
Condensate (BEC), gxx = 1 (3) for two distinguishable particles, gxx = 1 (4) for two
identical fermions, gxx = 0. In the case of excited state population originating fromcoherent excitation from the ground state (or vice versa), then the spatial correlations
are transferred between the atomic states and g11 = g22 = g12 = g [249, 248]. In thiscase, the density shift can be simplified to:∆ν12 =

2~ng [a22 ρ22 − a11 ρ11 + (ρ11 − ρ22 )a12 ]m(5.23)

In general, the scattering lengths a can be positive (attractive) or negative (repulsive),and the density shift depends on the excitation fraction. We have assumed sufficiently
cold temperature that s-waves dominate. Sometimes referred to as the Wigner threshold regime, s-waves dominate with the condition a/λT  1, where a is the largest relevant scattering length, and λT = h(2πmkb T )−1/2 is the thermal deBroglie wavelength[239, 250]. Note that when the deBroglie wavelength exceeds the scattering length,
the quantum statistics of the particles influence the scattering properties (through g,
the two-particle correlation function). For this reason, a/λT  1 is also the condition
for quantum scattering effects [251, 239, 250]. In general, this condition is easier met
than the quantum degeneracy condition requiring the “average” particle spacing to besmaller than the deBroglie wavelength [251, 250].
From Equation 5.23, the benefit of identical fermions is clear - they do not interact
and no collisional shift is present. If we take the s-wave collisions of identical fermions
to be identically zero, then we must consider the residual effects from the next higher
order wave, the p-wave. The shift resulting from p-wave interactions takes on a form
similar to Equation 5.23 and is given by [252]:∆ν12 =

π~n 2
hk i [v22 ρ22 − v11 ρ11 + (ρ11 − ρ22 )v12 ]m T(5.24)

Here vxy is the p-wave scattering volume given by vxy = (ap−wave)3 and ~2 hkT2 i/m is thexyaverage collision energy.

193With these basic models in place, to better clarify the role of dual spin statesin our observed density-dependent clock shift, we operate the clock with a single spinstate. This was done by replacing the dual-spin-state preparation by optical pumping
yielding a single spin state only (see Sections 2.7 and 5.1). The remaining operational
conditions were left the same. Before giving the results of these shift measurements,
I first describe two important experimental details. Unlike Ramsey spectroscopy withlong dark times and short π/2-pulses, typically used in microwave standards, during theSr Rabi spectroscopy, the ground and excited state populations are changing during thecollision process. This is an extra complication beyond the measurements demonstrated
in Cs [229], where the density shift is measured as a function of the excited state fraction
during the Ramsey dark time. In our case, the population evolution during collisions
make the resulting density shift a non-linear function of the excitation after the Rabi
pulse. In other words, in a simple picture, the density shift in Equation 5.23 or 5.24
should include time dependent populations ρ11 (t) and ρ22 (t) which must be integrated
over the Rabi pulse to determine the resulting shift.
Furthermore, as eluded to in Section 2.6.5, the population does not evolve as
simple Rabi flopping. Instead, weak transverse confinement outside of the Lamb-Dicke
regime results in motional-state-dependent dipole couplings. Unfortunately, the probe
laser has a small k-vector component along the transverse direction, exciting the atomalong this weak confinement axis. This is due not only to technical limitations (imperfectoverlap of the lattice and probe beams and their foci), but a fundamental reason as well.
At the probe and lattice foci, the Heisenberg uncertainty principle dictates that thefinite beam waist yields a spread in k-vectors (at the waist). This has been observed ina variety of Bragg scattering measurements (e. g. [253]). Although our probe beam focus
is designed to be relatively large (∼ 100 µm) to homogeneously probe the transverse
spatial extent of the trapped atoms, the lattice focus is much tighter (original diffraction
limited design radius of 20 µm, measurement of the trap frequencies typically indicated a

194

0.8
0.6
0.4
0.2

3

P0 population fraction(a) 1.0

0.0

100

1.0

200

300

400

500

400

500

time (ms)

0.8
0.6
0.4
0.2

3

P0 population fraction

(b)

0

0.0

0

100

200

300

time (ms)Figure 5.11: Atomic excitation as a function of time with Rabi frequencies similar to
those used for clock operation. (a) Excitation of a single spin state (mF = 9/2) startingin the ground state 1 S0 (b) De-excitation of a single spin state starting in 3 P0 , asdescribed in the text. In both cases, the measured excitation is shown by black circles,
and the theoretical fits based on Rabi inhomogeneity from dephasing among different
motional states are shown as solid curves. The model matches the data very well for atleast one full Rabi cycle, but is less reliable on the second. When these measurements
are made with much higher Rabi frequencies, the fit matches over many more cycles.

195
65 µm radius, although recent improvements indicate a radius of 35 µm). The relative kvector alignment of the lattice and probe determine the transverse excitation component.
The k-vector uncertainty due to small lattice beam focus leads to an rms probe-lattice
misalignment as large as a several mrad. This inhomogeneous excitation of the atomic
sample among transverse motional states (in dramatic case, see Figure 2.16) leads todephasing of the Rabi flopping process, exhibiting an excitation damping. Experimental
measurement of the excitation (3 P0 ) as a function of time as well a theoretical estimatebased upon this Rabi inhomogeneity from misalignment is shown in Figure 5.11(a).
Here, I have assumed a Rabi inhomogeneity taking into account a residual k-vector
component along one transverse dimension (here a generous 8 mrad). A more realistic
3-D treatment increases the Rabi dephasing, so that less misalignment is required toachieve the same damping. Note that at long enough times, t, the Rabi contrast revives
in the calculation.
With these details in mind, Figure 5.12 shows the observed density shift as afunction of the final excitation fraction (after the Rabi pulse) for the single spin state(red squares) described above. These measurements were taken using the typical lockto the atomic transition and looking for shifts relative to Ca. In order to change thefinal excitation fraction, the modulation depth of the lock to the atomic transition waschanged, i. e. the symmetrically-probed detuning on either side of transition center waschanged (small detuning for higher excitation). Because of the Rabi contrast reduction,
as well as the need to lock at a detuning large enough from the line center so thatthe laser sampled a monotonic discriminator, the density shift at high final excitation
could not be probed. For this reason, we took a second set of data under different initialconditions. After double spin polarization to the mF = ±9/2 states, a strong clock pulse
was applied under bias B-field with the purpose of pumping a single spin state of 1 S0
into 3 P0 (the pulse was strong to excite the atoms with less frequency sensitivity). At
this point, the 461 nm laser was applied to cycle the 1 S0 -1 P1 transition and heat away

196

density shift (Hz/ρ0)

2.0
Single Spin Polarization
Inverted Spin
Two Spin Operation

1.5
1.0
0.5

-3.40(.29)

0.0

-0.5
-1.0
-1.5
0.0

density shift (Hz/ρ0)

2.0
1.5
1.0

-0.13(0.48)
0.2
0.4
0.6
0.8
1
S0 population fraction

1.0

Single Spin Polarization
Inverted Spin
Two Spin Operatin
Inhomogenous Theor
Homogeneous Theor x 6

0.5
0.0

-0.5
-1.0
-1.5
0.0

0.2
0.4
0.6
0.8
1
S0 population fraction

1.0

Figure 5.12: Measured density shift sensitivity as a function of ground state 1 S0 population. Probing time tp = 80 ms. Red squares: A single nuclear spin state startingfrom 1 S0 . Blue circles: A single nuclear spin state starting from 3 P0 , as described in the
text. Green triangle: Normal clock operational conditions with double spin polarization(mF = ±9/2). (a) includes linear fits to the data, with slope and uncertainty indicated,while (b) includes theoretical models of the density shift, for the cases of homogeneousand inhomogeneous Rabi excitation.

197
the remaining 1 S0 population, including all of the other nuclear spin states originallypresent. Done directly before spectroscopy, this gave a sample of 3 P0 atoms with a single
spin state and somewhat different motional state distribution than prior to the opticalpumping (due to Rabi inhomogeneity). Standard spectroscopy was then performed on
this inverted population. This was alternatively done for one spin state and then theother, so that the atomic lock operated on the average of the ±mF transition. The timedependent excitation is shown in Figure 5.11(b), along with the theoretical fit basedon Rabi inhomogeneity. The measured density shift for this case, again as a functionof final excitation fraction, is shown in Figure 5.12 as blue circles, along with a linear
fit to guide the eye. Also shown is the measurement corresponding to traditional clock
operation with both spin states present (green triangle).
The first item to note from Figure 5.12 is that a density shift remains for the caseof only one spin state during spectroscopy (either red squares or blue circles). The originof this shift seems likely to be from one or both of two mechanisms. The first is p-wave
interactions. As stated above, p-wave collisions freeze out at cold temperatures due tothe centrifugal barrier. Based on the theoretical ground and excited state potentials,
the threshold for freezing out p-wave interactions is ∼ 30 µK, substantially warmer than
2 − 3 µK sample temperature. Below the p-wave threshold, the p-wave collision crosssection scales as σp /σs ∝ (kT a)4 where kT = 2π/λT is the wavenumber corresponding
to the relative thermal collision energy [251]. This yields more than 100 fold reductionin p-wave collision cross section. Based upon the experimentally determined scattering
lengths for 88 Sr and 86 Sr [238], an isotope mass scaling gives an s-wave scattering length
estimate of a11 ' 4.3 nm [252] for 87 Sr. This implies that the ultracold Sr collides in
the Wigner-threshold regime. The size of the observed shift, if accounted for by p-wave
interactions, would require a p-wave scattering length of many nanometers.
Another possible explanation is that the single spin state 87 Sr atoms are not
identical fermions and that s-wave collisions occur. Indistinguishability originates from

198
the internal wavefunction of the atom (identical set of quantum numbers for the internal
degrees of freedom). Because of the motional state dependent Rabi excitation, atoms
within one lattice site evolve as different superpositions of clock electronic states, and are
therefore not identical. Neither are they perfectly distinguishable, as the superpositionof each atom is not orthogonal to the others. In this sense, collisions between the 87 Sr
atoms could be described by the time dependent Equation 5.23 with a time-dependent,
effective correlation function g(t)ef f with a value between 0 (perfectly indistinguishable)
and 1 (perfectly distinguishable). This would result in partial, but not complete, swave collision suppression. This is in dramatic contrast to the experimental results of[234, 235], where atoms were excited uniformly as the interrogation was made far in theLamb-Dicke regime for the RF transition being probed.
Another interesting result seen in Figure 5.12 is the remarkable difference between
the two single spin cases in the slope of the density shift as a function of excitation
fraction. The first case, with an initial 1 S0 ground state population, has much weakerdependence than the atoms starting from 3 P0 . I mentioned one difference in this lattercase is that “pumping” the population to 3 P0 before spectroscopy favors some motional
states as a consequence of the Rabi inhomogeneity. This can lead to a decrease in
the inhomogeneity and thus reduced dephasing of the excitation in time. While notdramatic, comparison of Figures 5.11(a) and 5.11(b) show that, in fact, the latter caseshows higher Rabi contrast. This was coarsely estimated in the theoretical fit with aslightly colder sample temperature of 2 µK. Note that to rule out effects from differencesin the atomic samples from the two-spin an one-spin polarization techniques (using
optical pumping along different lattice axes), a single spin state was prepared and thenpumped to 3 P0 . Spectroscopy was then performed on this inverted population. One of
the blue circles in Figure 5.11 is actually this case, indicating that the difference between
blue circles and red squares was not the spin-state polarization prior to spectroscopy.
Assuming p-wave interactions, to model these effects we use the time dependent

199
version of Equation 5.24 and calculate the density shift as a function of final excitation
fraction. To match the experimental conditions, the different excitation fractions correspond to different detunings from the line center. Different degrees of dephasing due
to Rabi inhomogeneity are allowed for the two single spin state cases. For simplicity,
we assume v12 = 0. Unfortunately, because of the huge difference in slopes for the twocases plotted in Figure 5.12(a), no ratio of v22 /v11 was found that can fit the two data
curves, despite the difference in population evolution between the two cases (as shown in
Figure 5.11). Instead, a good fit was found by taking v22 /v11 ' .55 and allowing v11 tobe six times larger for the inverted population case than for the case of excitation fromthe ground state. Furthermore, while single ground spin state excitation was assumed
to have a Rabi inhomogeneity as seen in Figure 5.11(a), for the inverted population caseit was necessary to assume a homogeneous Rabi evolution (more homogenous than thatshown in Figure 5.11(b)). Results of this calculation are shown in Figure 5.12(b). For
the inverted population case, the data indicates ap−wave' 20 nm, and six times smaller
11
for the other case.
It is necessary to consider the qualitative motivations for the above described fit
model. For the inverted population case, it is seems from Figure 5.11(b) that the population evolution implies a more homogeneous Rabi excitation than other case. However,
it is not obvious to justify more dramatic homogeneity than that implied in Figure5.11(b), other than to say that the optical pumping which creates the inverted population does not necessarily preserve a simple Boltzmann distribution among motional
states (which is assumed in the theoretical fit of Figure 5.11(b)). With the resulting
shift coming from an integrated population, a more careful analysis of the actual timedependent population for the motional states occupied in the inverted population casewould be useful.
Another possible effect of the Rabi inhomogeneity is particle distinguishability
allowing s-wave collisions. One would expect that in the more homogenous case, the200
distinguishability would be smaller, reducing the s-wave collision. We see a much larger
effect for the inverted case, thought to be more homogeneous. One possible explanation
for this is that the s and p-wave interactions have opposite sign, so that the addition of swaves in the case of evolution from the ground state partly cancels the purer p-wave effectobserved in the inverted population case. If this were the case, however, it would imply
that the mass-scaled approximation of the s-wave scattering length for 87 Sr, a11 ' 4 nm,
is underestimated. Note also that it is sometimes difficult to experimentally determine
the absolute density of a cold atomic sample, which scales the scattering lengths. While
several methods were used here and yielded similar results, it would be worthwhile to
make a direct optical absorption measurement to confirm the absolute density. With therather complex experimental conditions during the density shift measurement (motional
state inhomogeneity, time dependent populations), many details remain unanswered.
However the data shown in Figure 5.11 gives many hints at the underlying physics.
We are currently considering the quantitative effect of distinguishability. Furthermore,
we are exploring sideband cooling of the atomic sample to observe the temperaturedependence of the density shift (e. g. Equation 5.24). Unfortunately, temperature also
influences the Rabi inhomogeneity among motional states. Two changes to the current
experiment which would simplify analysis include two pulse Rabi spectroscopy (withshort pulses, population is fixed during collisions) and cooling to a single motional state(eliminate inhomogeneity) in the longitudinal and transverse directions.
One very important result shown in Figure 5.12 is the existence of a zero crossingin the density shift [229, 233], for the inverted population case. While it is highlyinteresting to use the remarkable precision of the Sr standard as a tool to explore
the atomic interaction physics, for clock operation we prefer as small a density shift
as possible. The presence of a zero crossing implies that the current density shiftuncertainties may be substantially reduced with further investigation. For the case of a
3-D lattice with unity or less filled sites, collisions are suppressed by atomic confinement.

201
The density shift in the 1-D lattice case gives insight into requirements for the 3-D latticecase. The 3-D lattice also enjoys much more uniform atomic excitation, since all three
dimensions are strongly confined in the Lamb-Dicke regime.
Before leaving the topic of density related effects, we also considered the dependence of the collision interaction strength on spin state mF (e. g. [247]). As a simple
probe of the mF dependence, we measured the frequency shift as the density of an
unpolarized 87 Sr sample was varied (with roughly equal population in the ten mF levels). We first did this under a bias magnetic field (B = 470 mG). In this scenario,
we still addressed individual mF = ±9/2 nuclear spin states spectroscopically, so that
only one nuclear spin state was excited at a time (mF = 9/2 or −9/2) to 3 P0 . This
constrained 3 P0 -3 P0 interactions to a single spin state, but allowed all spin combinationsof 1 S0 -1 S0 interactions as well as many possible 1 S0 -3 P0 interactions. This yielded a
density-dependent shift similar to, but slightly smaller, than the polarized case. Even
more dramatic, we probed an unpolarized sample around zero B-field, so that transitions from all spin transitions were degenerate. This was similar to the experimental
conditions during our previous evaluations of the density shift (see Section 4.3 [22, 21]),
except that we the lock the clock laser to the atomic transition rather than tracing acrossthe line and fitting the center. In this case, all combinations of allowed 1 S0 -1 S0 , 1 S0 -3 P0 ,and 3 P0 -3 P0 collisions from the different spin states were present, as all spin states experienced some excitation. In this case, we observed a density shift 2-3 times smaller (forthe same total density) than the polarized case (also smaller than the polarized case atzero B-field). Although the large number of spin states and possible interactions makes
this measurement difficult to interpret quantitatively, the reduced shift indicated that
smaller interaction strengths may exist for spin states besides mF = ±9/2. Further
investigation of individual spin state interactions is another avenue worthy of consideration in an effort to reduce the observed density dependent shift.

202
5.4.5

Blackbody radiation induced Stark shift

The room temperature black body radiation (BBR) field induces a Stark shift
on the clock states. This can be found from Equations 2.62 and 2.63, except one must
integrate over the BBR spectral density (e. g. [254]):1∆ωa = − 2
6π 0 ~c3



kT
~

3 X

2

Z ∞

|hb|di |ai|

b,i

0

x3
dx x
e −1



1
1
+
yb + x yb − x

(5.25)

where x = ~ωBBR /kT and yb = ~ωab /kT , T is the temperature of the blackbody
environment, and ωBBR is the blackbody radiation frequency being integrated over. In
Section 2.6.2, we calculated the dipole polarizability and discussed the importance ofcontinuum contributions for the 3 P0 state, particularly near long wavelengths where
the BBR distribution is peaked. The highest accuracy calculation of the BBR shiftconsiders both bound- and continuum-state contributions, dynamical corrections to thestatic polarizability, and higher-order multipole contributions [20]. With higher ordermultipole contributions found to be smaller than the present uncertainty in the dipole
contributions, the BBR shift was expressed as:∆ωa = −

2
(αf s π)3 T 4 αaE1 (0) (1 + η)
15

(5.26)

where αf s is the fine structure constant, αaE1 (0) is the static dipole polarizability, andη is a dynamic correction term accounting for the fact that the BBR Stark interaction
is not exactly static. Using an ab initio, many body perturbation calculation (with alink to experimental data) the static polarizabilities were found to be α1 S0 = 197.2(2)au and α3 P0 = 458.3(3.6) au [20]. At T = 23o C, the BBR shift for our Sr clockis 2.24 Hz, a fractional frequency of 5.21 × 10−15 . The uncertainty of this shift is
7 × 10−17 , originating from uncertainty in the differential polarizability for the clockstates (1%). Further experimental uncertainty in the BBR shift originates from lack ofcontrol and homogeneity of the blackbody environment (at room temperature, T). By
monitoring the temperature of many positions on the Sr vacuum chamber, we determine

203
the blackbody environment to T ' 1 K (rms), leading to a shift uncertainty of 7.5 ×
10−17 . Combining the two effects yields a 1 × 10−16 total BBR uncertainty. Notethat although the atomic oven nozzle is kept at 850 o C, it is far removed from theatoms and mostly shielded by the atomic collimator at all times. Furthermore, during
spectroscopy, a mechanical shutter blocks the atomic beam altogether, also blocking the
BBR line of sight from the oven. The long vacuum tube for the atomic beam contacts
several different water cooling blocks to maintain cool temperature. Also, approximately
15 cm from the atoms is a heated sapphire window (200 o C, to prevent Sr corrosion
from the incident atomic beam) which contributes at total BBR shift of < 2 × 10−17 .
To further improve the Sr accuracy, the differential static polarizability of theclock states must be known to better than 1% (with the dynamical correction η contributing < 5% to the total shift). Such a measurement could be approached fromseveral angles. One technique is to measure the static polarizability directly by observing a clock shift as a well-controlled DC electric field is applied to the atoms [134].
Another is to constrain the static polarizability value with knowledge of the dynamic
polarizability. From Equation 5.25, it is found that more than five dipole couplings
contribute to the 3 P0 BBR shift above the 1% level (5s4d 3 D1 , 5p2 3 P1 , 5s5d 3 D1 ,5s6s 3 S1 , 5s6d 3 D1 , and the sum of the higher-lying/continuum contributions). The
influence of so many levels complicates an accurate extrapolation of the dynamic polarizability to DC, and would require improved experimental data for the dipole couplingstrengths. Measuring the dynamic polarizability with lasers at longer, BBR-like wavelengths could be more effective (particulary at several different λ), as the uncertainties
needed for extrapolation are more reasonable. A polarizability measurement at a longwavelength combined with an improved lifetime measurement from the dominant shiftstate 5s4d3 D1 (currently known at the 10% level experimentally) could also further
constrain the polarizability important for BBR. Such measurements might benefit fromnearby well-known atomic transitions that could be used to self-calibrate the optical

204
field strength (e. g. using the measured Stark shift), or from other methods [255]. To
improve upon the 1% uncertainty, any measurement will require careful design.
Another measurement approach is to measure the BBR shift directly by enclosing
the atoms in a well-characterized blackbody environment and recording the clock shift
as the environment temperature is systematically varied (such an approach would simultaneously decrease the shift uncertainty due to the BBR environment). The technicalchallenge lies in the control of temperature homogeneity over various functional areasof the vacuum chamber while accommodating sufficient optical access for a variety ofatomic manipulations. Without active temperature control, we measure temperature
differences between different areas of the vacuum chamber surrounding the Sr of ∼ 1 K(rms). Furthermore, at the highest clock accuracy level, it is important to account for
the effect of the transmissivity of glass viewports for visible and infrared wavelengths
on the blackbody environment. For example, as a rough estimate, if we model the BBR
environment for wavelengths above λ = 4 µm to be for T = 300 K (the chamber temperature), whereas for below λ = 4 µm, the transmissivity of the vacuum windows allow theatoms to sample the room BBR field (let’s say at 293 K), then the BBR induced shift is∼ 1 part per thousand (ppt) different than for the pure T = 300 K environment. This
represents a substantial difference in the BBR shift relative to a goal of 10−18 clock
operation. Ray-tracing Monte-Carlo algorithms can be used to accurately determine
the effective emissivity of a particular cavity geometry and material at different λ (e. g.
[256]), and may become important for these measurements.
Perhaps a much cleaner and workable solution is to cool and trap atoms in a standard chamber, and then transport them in a moving lattice [257, 258] to a secondary
BBR chamber, where an ideal, well-defined blackbody environment is established (seeFigure 5.13). The small chamber needs accurate temperature control at the 10 mK
level and would require the use of only small, far-removed optical access to introduce
the optical lattice and probe beams. With the appropriate geometry, the effective black-205

trapping
and cooling

BBR
chamber

Figure 5.13: One approach to measuring and controlling the BBR shift in Sr at an
improved level. The atoms are cooled and trapped in the traditional vacuum chamberwith sufficient optical access for atomic manipulation. Once loaded into the lattice, theatoms are transported by the lattice to a secondary chamber, a BBR cavity. This small
BBR chamber has excellent and accurate temperature control. Furthermore, there islimited optical access, so that viewport transmission of the room blackbody field (inthe NIR and optical region) has limited effect on the internal blackbody environment.
In other words, the geometry is well-suited for maintaining an effective emissivity extremely close to unity. Here the atoms are probed spectroscopically and measured.
The BBR induced AC Stark shift is directly measured by systematically changed thewell-controlled chamber temperature.

206
body emissivity of the interior can reach nearly unity and the total BBR environment
can be known at the 1 × 10−4 level, necessary for 10−18 clock uncertainty. The accurately controlled temperature of this BBR chamber could then be systematically varied
to measure the induced BBR shift, and determine the polarizability with reduced uncertainty. Such an approach avoids the complexity of cryogenic operation and can begeneralized to other lattice clock species. These improvements can potentially reducethe BBR-related uncertainty to far below 10−16 . Note that sizeable BBR shifts in many
atomic standards has motivated pursuing atomic species with a reduced BBR sensitivity,
including lattice trapped neutral Hg [32, 33] and the single trapped Al+ ion [255, 259].

5.4.6

Probe laser induced AC Stark shift

The two clock states have different polarizabilities at the clock transition frequency (see Figure 2.13). Consequently, the clock probe laser introduces a minute AC
Stark shift. In other words, the atom is only approximately a two-level system, andcoupling of the clock levels to outside levels allows for a probe induced Stark shift. The
small detuning of the probe laser from couplings to other motional states can lead tosuch shifts, but this effect is much smaller than coupling to other electronic states. As
discussed previously, imperfect alignment between the probe and the lattice axes leads
to degradation in the transverse Lamb-Dicke condition and necessitates an increased
probe power to excite the clock transition. By strongly saturating the transition withexcess probe intensity, we measure a non-zero shift. Determining the laser intensity
using the measured power and beam waist, the measured shift is consistent with the
dynamic polarizabilities at 698 nm. By scaling to the intensity value typically used forclock operation, the shift is found to be 2(1) × 10−17 . More careful probe alignment,interrogation in a 3-D lattice (stronger confinement along all axes), and longer probe
times can further decrease the required probe power and the resulting shift.

207
5.4.7

Line-pulling

Quantum confinement in the well-resolved-sideband limit means that Doppler
effects are manifested in the sideband structure which can be isolated from the clocktransition. These effects are further reduced in the Lamb-Dicke regime where photon
recoil is transferred to the optical potential and the sidebands are suppressed. However,off-resonant, weakly excited motional transitions can pull the center frequency of theclock transition. More relevant is line-pulling originating from transitions of other spinstates with residual populations after imperfect atomic polarization (typically < 5%).
Fortunately, many such effects largely occur in a (mF ) symmetric fashion such that theline-pulling, already small, is reduced. Furthermore, the 20 µT bias B-field separates
excitation of neighboring spin states by more than two linewidths. The overall linepulling effect is conservatively estimated to be < 2 × 10−17 .

5.4.8

Servo Error

Servo errors in steering the clock laser to the atomic transition can also resultin frequency offsets. Our digital servo operates via standard modulation techniquesby probing the half maxima of the resonance. Noise processes around the modulation
frequency, round-off error, and an asymmetric probe laser power spectrum are potential
contributors to the servo error (e. g. [260, 261]). In our system, we are mostly concernedwith residual laser drifts and finite loop gain. As described in Section 5.1.2, we typically
implement a linear feed-forward frequency compensation for drift of the stable cavity
to which the clock laser is locked. This feed-forward value is estimated by measuring
the laser drift relative to the NIST H-maser via the frequency comb. To overcome
imperfect feed-forward compensation, we utilize two integration stages in the laser-atom
feedback loop. Operating properly, this approach keeps residual drifts compensated by
the primary servo integrator (actuating on AOM1) to a measured value of < 1 mHz/s.

208
For a single integrator servo loop, the average drift-induced servo error can be estimatedas tservo df /dt where tservo is the servo time constant and df /dt is the constant linear
drift [262]. From our measured drift, as well as from analysis of the overall servo signal
record for residual offsets, we conservatively estimate the servo error to be < 5 × 10−17 .

5.4.9

Other residual 1st -order Doppler shifts

Line-pulling is one way that residual 1st -order Doppler (and recoil) effects could
introduce a systematic shift of the clock transition. Other mechanisms can also play arole. The first, as discussed in Section 2.6.5, is the residual Doppler and recoil effectdue to tunnelling in the lattice potential. Exploiting gravity to lift degeneracy among
different lattice sites and suppress tunnelling, for our lattice parameters this effect isestimated to be below the 10−17 shift level. As we consider interrogation of atoms in
a 3-D optical lattice, it remains beneficial to probe the atoms along the gravitational
axis.
Another residual 1st -order Doppler effect, as discussed in Section 3.4.2, originatesfrom relative shaking between the lattice potential and the clock laser. With the possibility to give a frequency offset, we are concerned with relative motion during probing
synchronized with the experimental cycle at the frequency f = 1/Tc (Tc being the experimental cycle time) and its harmonics. For example, the NIST Ca clock has observed
problematic frequency shifts associated with turning on and off the quadrupole MOT
field which systematically shakes the optical table. They have circumvented this problem by isolating the vacuum chamber from the table [86]. The NIST ion group wasrecently concerned with a Doppler shift synchronized to their atomic probing inducedby photo-electron buildup on their trap electrodes due to illumination by the UV clock
laser. To average out this effect, they alternated probing from opposite directions [259].
This leaves residual Doppler sensitivity at the frequency f = 1/2Tc , where any motional noise is presumably much smaller. In the case of lattice trapped neutral atoms,

209
the neutral atom is not strongly pushed by charged particles (which, except for vacuum particles, are neither present) and the relative lattice-probe motion is set by large,
heavy optical components which can be designed to be very stable and placed on an
isolated optical table. We investigated some of these effects as we probed narrow linesand did not observe any influence at the Hz level. Beyond this, our experience withphase noise cancellation for free space optical paths in our laboratory indicates that laboratory seismic noise and airborne fluctuations degrade laser instability from Doppler
noise in the free space optical path well-below the 10−16 level at 1 s (approximately Tc ).
However, while mechanically switching optical shutters are typically isolated from theoptics table, we do use switching magnetic fields like the Ca experiment. Fortunately,with our long Tc , this field switching is temporally far removed from the atomic interrogation time. Also, vacuum chamber motion is much less critical than for the lattice andprobe laser optical components, which are further distanced from any switching fields.
As discussed in Section 3.4.2, future interrogation will exploit active noise cancellation,
where the lattice retroreflector is stabilized to make a weak lattice cavity resonant withthe lattice laser, and fiber noise cancellation of the clock laser can be implemented all
the way to the first lattice cavity mirror. In this way, the clock laser phase is locked tothe atomic confinement reference frame.
A related Doppler effect involves switching the RF power in an AOM to pulse
the clock laser for spectroscopy. This pulsing is known to induce phase chirps of thespectroscopic pulses, both from RF ringing and thermal effects [263]. The AOM we
use for switching the clock pulse is the same used for the fiber-noise-cancellation pathbringing the clock laser to the atoms. This means that with the fiber noise cancellation
servo engaged, the optical phase is stabilized and Doppler frequency excursions arecancelled to < 10 mHz. After turning the RF power on, the fiber noise cancellation
servo takes ∼ 100 µs to properly engage, a small fraction of the pulse length time
tp = 80 ms. Additionally, we also use a liquid-crystal shutter to give time for this

210
servo to engage before illuminating the atoms. Interferometric techniques can be used
to further characterize this effect.

5.4.10

2nd -order Doppler shift

The 2nd -order Doppler shift originates from expansion of the relativistic Doppler
shift, accounting for time dilation. It is simply:
1∆ω = β 2 ωL
2(5.27)

where β = v/c is proportional to the atomic velocity and ωL is the laser (angular)
frequency. The atomic velocity of our ultracold lattice-trapped strontium is characteristically given by the sample temperature, T = 2.5 µK, corresponding to a velocity of∼ 15 cm/s. This results in a 2nd -order Doppler shift below 100 µHz (< 10−18 ). Shakingof the trap results in much smaller velocities and thus an even more negligible 2nd -order
Doppler shift.

5.4.11Other effects

Although gravitational fields are not known to change the local operation of an
atomic clock [264], general relativity dictates that comparison of clocks in different
gravitational potentials is subject to the gravitational red shift:
∆ω =

gL
ωL
c2

(5.28)

where g is the local gravitational acceleration, L is the distance (component along gravity) between the standards, ωL is the laser radiation frequency, and radiation travelling
towards a weaker gravitational field is red-shifted. In Equation 5.28, we have assumed
that g is constant at and between both clocks in the comparison. At the earth’s surface the fractional gravitational red shift is ∼ 1 × 10−18 /cm. Because of their amazingstability and accuracy, optical clocks in the future may exploit this effect to perform
geodesy.

211
The presence of a DC electric field induces a static Stark shift. The groundedvacuum chamber acts as a Faraday cage around the atoms as well as keeps charged
objects far removed from the atoms. However, charge can build up on the dielectriccoated glass viewports. If charge is collected on the large viewports closest to the atoms(top and bottom of chamber) sufficient to yield even a large 1 V potential difference,
based on the DC polarizability (Section 5.4.5), the resulting clock transition shift wouldbe < 10−18 .
No significant AC magnetic fields are present, the largest probably at the 60 Hz
electrical line frequency. With the small 2nd -order Zeeman shift for the clock transition(Section 5.4.3), AC Zeeman shifts are negligible. This effect is sometimes considered forthe trapped ion case, due to the RF trapping potential (e. g. [265]).
To prevent AC Stark shifts from the unwanted presence of other laser beams used
for the strontium experiment (laser cooling, optical pumping, etc.), mechanical shuttersand acousto-optic shutters are typically used together to impede this laser radiationfrom reaching the atoms. Furthermore, the vacuum chamber is covered by an opticallyopaque curtain.
Finally, the clock states possess no permanent electric quadrupole moment, sothat field-gradient induced shifts are negligible.

5.4.12

Uncertainty Summary

Table 5.3 summarizes the systematic shifts and uncertainties in realizing the natural Sr atomic transition frequency [23]. The total uncertainty of 1.5 × 10−16 represents
the smallest frequency uncertainty for any neutral atom system to-date, including theCs primary standard. It falls short of impressive Hg+ and Al+ trapped ion results as
the smallest uncertainty for any type of frequency standard. The largest Sr uncertainty
originates from the blackbody Stark shift, with the next largest being the density shift.
Progress towards more fully characterizing and controlling these shift mechanisms will

212

Table 5.3: Systematic shifts and their uncertainties for the 87 Sr 1 S0 -3 P0 clock transition(2007)
Contributor
Lattice Stark (scalar/tensor)
Hyperpolarizability (lattice)BBR Stark
AC Stark (probe)
1st order Zeeman
2nd order Zeeman
DensityLine pulling
Servo error
2nd order Doppler
Systematic total

Correction (10−16 )
-6.5
-0.2
52.1
0.2
0.2
0.2
8.9
0
0
0
54.9

Uncertainty (10−16 )
0.5
0.2
1.0
0.1
0.2
0.02
0.8
0.2
0.5
0.01
1.5

213
facilitate determination of the Sr standard in the 10−17 range. The 10−16 uncertainty
demonstrated here is an important milestone towards the 10−18 accuracy goal sharedby many optical standards.

5.5

Absolute Frequency Measurement
With the reduced uncertainty of the Sr optical standard, we performed a new

absolute frequency measurement of the Sr clock transition using the H-maser based fiber
link to the NIST-F1 Cs fountain. With the anticipated uncertainty at or below the 10−15
fractional frequency level, we re-characterized the microwave link from JILA to the Hmaser ensemble. This included a full out-of-loop evaluation of the microwave electronics
used for the microwave phase-stabilized, fiber-based transfer scheme from the laboratoryof Drs. Leo Hollberg and Scott Diddams to JILA (this evaluation used a short piece oftest fiber). This revealed a transfer instability of 10−14 at 1 s which averaged down to10−17 for > 104 s, with no observable offset. In addition to the temperature sensitivityof the H-maser-referenced synthesizer used for amplitude modulation of the transfer
laser, temperature sensitivity for a variety of microwave components (mixers, frequency
doublers, cable, amplifiers) was found to be at the several 10−16 /(K/hr) level, and we
could thus apply a small but complete temperature based correction to the frequency
measurement.
The Sr system was run under conditions similar to, but not exactly the same as,
those of the uncertainty evaluation described in the previous section. The measurement
was made over 50 consecutive hours. Accounting for small breaks during which themicrowave transfer link or a Sr laser was un-locked and then re-locked, the final measurement data set included ∼ 184, 000 s. The measurement instability averaged down
predominantly characteristic of the H-maser. The NIST-F1 fountain was operated witha total fractional frequency uncertainty (systematic and statistical) of 6 × 10−16 . An additional 6 × 10−16 uncertainty originated from dead time in the strontium measurement

214

Tokyo
JILA
Paris

νSr-ν0 (Hz)

80
70
78
76

60

74
72

50

4

2

5

4

6

6

7

8

Measurement
Figure 5.14: Plot of high accuracy absolute frequency measurements of the Sr clocktransition. 1: JILA 2005, 2: Paris 2006, 3: Tokyo 2006, 4: JILA 2006, 5: Paris 2007, 6:
JILA 2007, based on 48 hour measurement with the NIST F1 Cs fountain. The inset isa magnification of the last four points.

215
during which the Cs continued to average down with the H-maser. The measurement
yielded a Sr transition frequency of 429 228 004 229 873.8 (4) Hz, with a fractional frequency uncertainty < 10−15 , making it one of the most accurately determined opticaltransitions (similar to measurement level of the Hg+ optical clock transition [6]) [266].
This measurement, combined with other recent measurements of the Sr clock transition,is shown in Figure 5.14. The excellent agreement among groups makes strontium thebest-agreed upon optical standard. In fact, this excellent agreement allows for analysis of the combined international Sr frequency data set for time dependent frequencychanges that could be put additional constraints on possible variation of the fundamental constants [264].

5.6

OutlookIn 2003, the 87 Sr 5s2 1 S0 - 5s5p 3 P0 clock transition was directly excited for the

first time and its frequency was determined with a 20 kHz uncertainty (∼ 5 × 10−11 )[204]. Less than five years later, its absolute frequency has been measured to < 10−15
and its frequency uncertainty has been characterized at the 10−16 level, representing
five orders of magnitude improvement. This rapid progress has been facilitated by anatomic system well-suited for high precision and high accuracy spectroscopy. Anotherkey ingredient was the ability to manipulate and control the strontium to generatelarge atomic samples uniformly confined in the well-resolved sideband and Lamb-Dicke
regimes. The neutral lattice-trapped strontium system demonstrates many qualities
which are well-suited for its continued development towards the 10−18 accuracy level.
Paramount to this goal, near-future steps for the strontium system must include better
control and characterization of the BBR and density shifts. Operation in a 3-D lattice has immediate implications for the collisional interactions as well as the benefit ofstrong confinement in all axes. An important enabling step will be the development ofa clock laser system with coherence times exceeding 10 s. This will not only make ultra-

216
narrow resonance atomic interrogation possible, but will allow neutral atom systems
to emerge as ultra-stable optical frequency standards. No major clock limitations haveso far originated from the added complexity of the hyperfine interaction in the oddisotope alkaline earth standards. Nevertheless even isotopes (with no hyperfine interaction) using external magnetic field state mixing [226] or electromagnetically-induced
transparency [267, 268] may be an interesting exploration. Already recommended asa secondary representation of the SI second, strontium will surely continue to play animportant role in high accuracy time and frequency standards. Together with interesting possible applications in ultracold molecular association and spectroscopy [269, 270],
cold collisions [23, 269, 68], measurement of fundamental constants [264, 270], quantum non-demolition measurements [271], quantum simulations, quantum computation,
quantum degeneracy [84, 68, 269], ultracold plasmas [272], coherent population trapping [268, 267], and more, strontium will continue to help both better define and better
understand the world around us.

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