Phase Matching and Coherence of High-Order
Harmonic Generation in Hollow Waveguides
byAmy Louise Lytle
B.A., The College of Wooster, 2001

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:
Phase Matching and Coherence of High-Order Harmonic Generation in Hollow
Waveguides
written by Amy Louise Lytle
has been approved for the Department of Physics

Margaret Murnane

Prof. Henry Kapteyn

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.

iii
Lytle, Amy Louise (Ph.D., Physics)
Phase Matching and Coherence of High-Order Harmonic Generation in Hollow Waveguides
Thesis directed by Prof. Margaret Murnane

Over the last twenty years, high-order harmonic generation has emerged as ascientifically useful, temporally and spatially coherent source of extreme ultraviolet light.
Because of the nature of the generation process, the harmonics are emitted in a seriesof attosecond bursts, creating a spectroscopic and imaging tool with high temporal andspatial resolving power. The coherence and short time-duration, in combination withthe accessibility of this table-top source, have made high harmonic generation a truly
unique light source, opening possibilities for new science.
The current limitation to this source is its brightness, limited mainly throughpoor phase matching of the nonlinear conversion process. This thesis presents work
performed toward better understanding of the physics and the engineering of high harmonic generation, specifically in a waveguide geometry. First is a survey of the relevant
theory and review of previous work on high harmonic generation and phase matching
techniques. Presented next are selected experimental results related to optimizing theharmonic photon yield in hollow waveguides, including a measurement of the photon
yield at 45 eV, measurements of the density-dependent energy loss in the driving laser
beam, and a study of the effects of modulation depth in the technique of quasi-phasematching using hollow waveguides with a modulated inner diameter.
Counterpropagating light is used for the first time as a tool for measuring the insitu coherence length of the harmonic generation process. Through this measurementof the coherence length, several other quantities can be inferred. The ionization level atwhich different harmonic orders are generated can be determined, giving insight into theiv
temporal dynamics of high harmonic generation. Intensity variations caused by energy
loss in the driving laser beam due to ionization or refraction, or by interference between
coupled modes of the waveguide, are measured. The dynamic nature of the coherence
length of high harmonic generation makes an in-situ measurement of this kind crucial
for any implementation of quasi-phase matching.
Finally, all-optical quasi-phase matching of high harmonic generation is demonstrated by using trains of counterpropagating pulses for periodic correction of the phasemismatch. Enhancements of more than two orders of magnitude are demonstrated athigh photon energies, where conventional phase matching techniques are currently notpossible. All-optical quasi-phase matching is also shown to be selective in terms ofenhanced bandwidth, and can even isolate one of the two electronic trajectories contributing to harmonic emission. These advances have the potential for improving theharmonic flux at high photon energies that cannot currently be phase matched, andfor permitting manipulation of the temporal and spectral structure of the harmonic
emission.

Dedication

For Etienne.

vi

Acknowledgements

A body of work the magnitude of a PhD career cannot be completed alone. In
the case of my own, there were many extraordinary people who supported and assisted
me through the last several years. I may have been the common thread in the work
presented here, but friends, family, and colleagues contributed in ways that are impossible to quantify. A partial list includes: Margaret Murnane and Henry Kapteyn, mytireless advisors, who shared their support and considerable expertise, helping me tolearn and achieve more than I thought possible; The Kapteyn-Murnane research groupmembers, many of whom contributed significantly to this work, and all of whom weregood friends and colleagues: Dave Gaudiosi, Ra’anan Tobey, Luis Miaja-Avila, Mark
Siemens, Xiaoshi Zhang, Daisy Raymondson, Richard Sandberg, Tenio Popmintchev,
Mike Grisham, Paul Arpin, Nick Wagner, Ariel Paul, Arvinder Sandhu, Oren Cohen,
and Sterling Backus; Barry Walker, for help with the modulated waveguide measurements; Don Jacobs, Shila Garg, and John Lindner, still my models for great scientists
and educators; The JILA staff, particularly Rachael Tearle; The National Science Foundation, for a greatly appreciated fellowship; My family, for the love they express in somany ways; Most of all my appreciation goes to Etienne Gagnon, for more reasons than
I can fit into a PhD thesis.

viiContents

Chapter
1 Introduction
1.1

1.2

1

High-Order Harmonic Generation as a Source of Coherent EUV/ SoftX-Ray Light . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

1Contents . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

42 Background and Theory6

2.1

Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

6

2.2

High-Order Harmonic Generation: Single-Atom Response . . . . . . . .

7

2.3

Macroscopic Phase Effects . . . . . . . . . . . . . . . . . . . . . . . . . .

19

2.4

Phase Matching . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

27

2.5

Quasi-Phase Matching . . . . . . . . . . . . . . . . . . . . . . . . . . . .

42

2.6

Hollow Waveguides . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

47

2.7

Counterpropagating Light . . . . . . . . . . . . . . . . . . . . . . . . . .

57

3 Characterization of Waveguide High Harmonic Generation

67

3.1

Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

67

3.2

Experimental Setup . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

67

3.3

Absolute Harmonic Photon Yield . . . . . . . . . . . . . . . . . . . . . .

75

3.4

Ionization Loss . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

83

3.5

Modulated Waveguides . . . . . . . . . . . . . . . . . . . . . . . . . . . .

90

viii
4 Probing and Quasi-Phase Matching of High-Order Harmonic Generation Using
Counterpropagating Light

97

4.1

Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

97

4.2

Experimental Setup . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

98

4.3

Single Pulse Probing . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 105

4.4

Double Pulse Probing . . . . . . . . . . . . . . . . . . . . . . . . . . . . 118

4.5

Quasi-Phase Matching . . . . . . . . . . . . . . . . . . . . . . . . . . . . 126

4.6

Quantum Electronic Trajectories . . . . . . . . . . . . . . . . . . . . . . 135

5 Summary and Future Work

142

5.1

Summary . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 142

5.2

Future Work . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 144

Bibliography

149

Appendix
A Variable Repetition-Rate Ti:Sapphire Oscillators

162

A.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 162
A.2 Theory . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 164
A.3 Low Repetition Rate Laser . . . . . . . . . . . . . . . . . . . . . . . . . 166
A.4 High Repetition Rate Laser . . . . . . . . . . . . . . . . . . . . . . . . . 169
A.5 Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 172
B High Harmonic/ Fundamental Beamsplitter

174

B.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 174
B.2 Design . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 175
B.3 Beam Splitter Performance . . . . . . . . . . . . . . . . . . . . . . . . . 179

ix
B.4 Analysis and Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . 182
C Alignment Procedure for a Ti:Sapphire Oscillator

184

C.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 184
C.2 Components . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 184
C.3 Alignment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 187
C.4 Diagnostics and Common Instabilities . . . . . . . . . . . . . . . . . . . 192

x

TablesTable
2.1

Critical ionization values for the noble gases, as well as the highest harmonic order that can be phase matched, generated at the peak of a 25
f s pulse of center wavelength 0.8 µm. . . . . . . . . . . . . . . . . . . .

2.2

39

Attenuation constants, phase velocities, and group velocities for severalof the low-order hybrid modes, for λ = 0.8 µm and a = 75 µm. . . . . .

49

A.1 Cavity parameters for ABCD matrices . . . . . . . . . . . . . . . . . . . 165
A.2 Astigmatism compensation angles . . . . . . . . . . . . . . . . . . . . . . 166
B.1 Layer thicknesses for broadband, grazing incidence, antireflection coating
at 800 nm. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 177
C.1 Abbreviations for cavity elements (shown in Figure C.1) used throughout
the appendix. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 186

xi

FiguresFigure2.1

Atomic Coulomb potential when distorted by an intense laser field, in thetunneling regime. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

2.2

Fraction of ionization of neutral argon as a function of time within a 25
f s pulse of peak intensity 5 1015 W/cm2 . . . . . . . . . . . . . . . . . .

2.3

9

11

Possible paths for the electron during rescattering as a function of laser
phase (time), and several selected values of the phase of the laser at
ionization (or, equivalently, time at ionization). Intersection with thex-axis indicates a possible opportunity for recombination. . . . . . . . .

2.4

Kinetic energy at the return of the electron to the parent ion, as a functionof phase of the laser at ionization.

2.5

13

. . . . . . . . . . . . . . . . . . . . .

13

Possible paths for the electron during rescattering, indicating the origin of
the “cutoff” photon energy, as well as the “long” and “short” trajectories
contributing to a photon energy below cutoff.

. . . . . . . . . . . . . .

15

2.6

Values of K as a function of release phase. . . . . . . . . . . . . . . . . .

17

2.7

Harmonic phase of the 31st harmonic generated in argon, as a functionof the intensity. Ith,31 indicates the threshold intensity for generating
the 31st harmonic. The curves show a stronger dependence on intensityof the phase of the emission from the long trajectory. Reproduced from
Ref. [55]. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

18

xii
2.8

Harmonic spectra generated in argon with driving laser pulses of varying
chirp. Reproduced from Ref. [56]. . . . . . . . . . . . . . . . . . . . . . .

2.9

18

Calculated spectral (a) and temporal (b) structure of the 55th harmonicorder generated by a 150 f s pulse with a peak intensity of 1015 W/cm2 .
Different electron trajectories appear with different frequencies, due tothe intensity-dependent phase of harmonic emission. Reproduced from
Ref. [60]. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

24

2.10 Harmonic spectra generated in 5 torr argon, with a 27 f s pulse with apeak intensity of ∼ 5 1014 W/cm2 , showing peak splitting due to nonadiabatic blue-shifting. The two peaks correspond to emission from thelong and short electron trajectories.

. . . . . . . . . . . . . . . . . . . .

25

2.11 Phase fronts for the different trajectories that contribute to plateau harmonic orders. The stronger dependence of the harmonic phase on intensity leads to a greater curvature for the long (τ2 , dashed curve) comparedto the short (τ1 , solid curve) trajectories. Reproduced from Ref. [65]. . .

27

2.12 Harmonic intensity as a function of the phase mismatch. . . . . . . . . .

29

2.13 Harmonic intensity as a function of propagation distance, in the case ofphase matching and a nonzero phase mismatch. . . . . . . . . . . . . . .

30

2.14 Dipole phase as a function of propagation distance. The long-dashed line
shows the phase evolution of the fundamental through the focus due tothe Guoy phase shift. The short-dashed line shows the evolution of theharmonic phase due to the intensity-dependent phase. The solid curve isthe sum of the two contributions. Reproduced from Ref. [73]. . . . . . .

35

xiii
2.15 Conversion efficiency of HHG for the 45th harmonic order as a function of
the distance of the focus from the gas jet (z). The 3D plots illustrate theharmonic field at z = −1 and z = 3mm, as a function of the propagation
distance and the transverse direction (azimuthal symmetry is assumed).
Reproduced from Ref. [73]. . . . . . . . . . . . . . . . . . . . . . . . . .

36

2.16 a) Measured and b) calculated pressure dependence of the harmonic yieldfor several gases. In order of increasing optimum pressure, the curves
correspond to xenon, krypton, argon, and hydrogen. Reproduced from
Ref. [74]. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

38

2.17 Phase matched HHG photon emission as a function of the propagation
distance (in units of the absorption length, Labs ) in the presence of absorption. Reproduced from Ref. [75]. . . . . . . . . . . . . . . . . . . . .

42

2.18 Measured (squares) and predicted (solid curve) brightness of the 61st
harmonic order generated in neon, as a function of propagation distance.
Reproduced from Ref. [88]. . . . . . . . . . . . . . . . . . . . . . . . . .

43

2.19 Harmonic intensity as a function of propagation distance, in the case offull phase matching (blue curve), traditional quasi-phase matching withperiodically poled nonlinear crystal (black curve), quasi-phase matching
through periodic suppression of the harmonic signal (red curve), and nophase matching (green curve). . . . . . . . . . . . . . . . . . . . . . . . .

44

2.20 Energy of the 95th harmonic order for a large phase mismatch in the caseof a) a straight, unmodified waveguide, and b) a modulated waveguide.
Reproduced from Ref. [29]. . . . . . . . . . . . . . . . . . . . . . . . . .

45

2.21 Measured harmonic emission from neon generated in straight (black curve)
and modulated (red curve) waveguides. Reproduced from Ref. [35]. . . .

46

xiv
2.22 Analytically calculated intensity profile of a beam (λ0 = 0.8 µm) propagating through a hollow waveguide (a = 75 µm), including the first threelowest order modes.

. . . . . . . . . . . . . . . . . . . . . . . . . . . . .

51

2.23 Numerical simulation of the intensity profile of a Gaussian beam, λ =0.8 µm, coupled into and propagating in a hollow waveguide with innerdiameter 150 µm. Coupling parameter: R = w0 /a = 0.6. . . . . . . . . .

52

2.24 Numerical simulation of the intensity profile of a Gaussian beam, λ =0.8 µm, coupled into and propagating in a hollow waveguide with innerdiameter 150 µm. Coupling parameter: R = w0 /a = 0.6435 (optimal
coupling into the EH11 mode). . . . . . . . . . . . . . . . . . . . . . . .

53

2.25 Numerical simulation of the intensity profile of a Gaussian beam, λ =0.8 µm, coupled into and propagating in a hollow waveguide with innerdiameter 150 µm. Coupling parameter: R = w0 /a = 0.7. . . . . . . . . .

53

2.26 Influence of a weak counterpropagating field on the phase of HHG. a)
Example of the intensity-dependent phase modulation, with a different
amplitude for the two trajectories. Amplitude of the phase modulations
calculated as a function of the field ratio, r. c) Amplitude of the phaseoscillations for a particular contribution as a function of emission time.
d) Bessel dependence of the microscopic effective emission factor on theamplitude of the phase modulation. Reproduced from Ref. [106]. . . . .

61

2.27 Scan of the collision point of the driving laser pulse with a counterpropagating pulse through a narrow gas jet. The well-phase matched harmonic
signal is suppressed strongly in the presence of the counterpropagating
light. Reproduced from Ref. [33]. . . . . . . . . . . . . . . . . . . . . . .

63

xv
2.28 Scan of the collision point of the driving laser pulse with a counterpropagating pulse through a wider gas jet. The poorly-phase matching harmonic signal is restored through suppression of destructively interfering
harmonic emission. Reproduced from Ref. [33]. . . . . . . . . . . . . . .

64

2.29 QPM efficiency factor for a) hyperbolic secant and b) square counterpropagating pulses as a function of pulse width and peak phase modulation
amplitude. Reproduced from Ref. [106]. . . . . . . . . . . . . . . . . . .
3.1

3D rendering of the components of a v-groove vacuum fixture for mounting the hollow waveguides. Reproduced from [1]. . . . . . . . . . . . . .

3.2

70

Image of a laser-drilled hole in the side of a hollow waveguide, used forgas delivery. Reproduced from [1]. . . . . . . . . . . . . . . . . . . . . .

3.3

66

71

Comparison of the absolute first order diffraction efficiencies of the survey
gratings, measured from replicas of the gratings used in the spectrometer.
Incidence angle for these measurements was 88.75◦ . . . . . . . . . . . . .

3.4

74

Experimental setup for generation, propagation, and detection of HHG
under vacuum. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

75

3.5

Schematic of the detection circuit of the Al2 O3 NIST vacuum photodiode. 76

3.6

Quantum efficiency of the Al2 O3 NIST vacuum photodiode, serial no.
397. Measured June 2005. . . . . . . . . . . . . . . . . . . . . . . . . . .

77

3.7

Experimental setup for photon yield measurement. . . . . . . . . . . . .

78

3.8

Current measured from a vacuum photodiode as a function of pressure,for several different input pulse energies. . . . . . . . . . . . . . . . . . .

79

xvi
3.9

e) Current measured from a vacuum photodiode and counts from a CCD
camera measured at the peak of the 27th harmonic, as a function ofpressure. For several of the pressures, indicated by arrows, the spectra
are plotted (a)-d)), along with the transmission of the gas and filters
used. These data were generated at a high pulse energy of 990 µJ. . . .

81

3.10 Measured output power from a 3.5 cm length waveguide, inner radius 150µm, as a function of gas pressure, for three different gases (open circles)
and three different input powers (individual plots). Repetition rate of thepulses was 1 kHz. Gas pressure was constant at the value indicated overa distance of 2.5 cm in the waveguide, with 5 mm differential pumping
sections on either side. Solid curves show the results of a simulation ofionization loss. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

85

3.11 Measured output power from a 11 cm length waveguide, inner radius 150µm, as a function of gas pressure, for three different gases (open circles)
and three different input powers (individual plots). Repetition rate of thepulses was 1 kHz. Gas pressure was constant at the value indicated overa distance of 10 cm in the waveguide, with 5 mm differential pumping
sections on either side. Solid curves show the results of a simulation ofionization loss. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

86

3.12 Correlation between loss and harmonic photon yield. a) Measured transmission from 3.5 cm and 11 cm total length (2.5 cm and 10 cm constantpressure regions) as a function of argon pressure. b) Corresponding measured diode current. Input power was ∼ 300 mW , corresponding to an
ionization low enough to allow pressure-tuned phase matching. . . . . .

89

3.13 Schematic of a hollow waveguide with a modulated inner diameter, including typical physical parameters. . . . . . . . . . . . . . . . . . . . .

90

xvii
3.14 Data showing enhancement of HHG in helium through QPM using modulated waveguides. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

91

3.15 Data showing enhancement of HHG in neon through QPM using modulated waveguides. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

92

3.16 Data showing HHG emission from helium extending into the “water window” up to the Ti L edge.

. . . . . . . . . . . . . . . . . . . . . . . . .

93

3.17 HHG yield from neon as a function of wavelength, generated in modulated
waveguides with varying modulation depth, for a pulse energy of 0.7 mJ
and a pressure of 3 torr. . . . . . . . . . . . . . . . . . . . . . . . . . . .
4.1

96

Experimental setup for generation and coupling of a single counterpropagating pulse, using bulk material for stretching the pulse. Delay lines
are not to scale. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

4.2

99

Experimental setup for the generation and coupling of one or more counterpropagating pulses, using phase masks within a grating pulse compressor.101

4.3

Photograph of the air plasma filament created in the free focus of thecounterpropagating beams. The bright point of plasma emission occurs
at the collision point of the two pulses. . . . . . . . . . . . . . . . . . . . 105

4.4

The effect of a single counterpropagating pulse on the high harmonic
emission from orders q = 37-45 in low pressure argon. . . . . . . . . . . 106

4.5

Measuring the coherence length of HHG in a hollow waveguide. A schematicof the coherence zones present within a waveguide when the phase mismatch is nonzero. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 108

4.6

Intensity modulations of the 41st harmonic order generated in argon. Achanging periodicity of the intensity modulation with propagation distance indicates a reduction in the intensity of the driving laser toward
the exit of the waveguide. . . . . . . . . . . . . . . . . . . . . . . . . . . 110

xviii
4.7

Variation of the harmonic emission generated in argon as function of
the overlap region of the forward and counterpropagating pulses, for two
harmonic orders, q = 25 and 39. . . . . . . . . . . . . . . . . . . . . . . 111

4.8

Calculated intensity of the driving laser as a function of propagation distance and inner radius of the waveguide, including interference of coupledmodes as well as ionization loss. . . . . . . . . . . . . . . . . . . . . . . . 112

4.9

On-axis intensity modulations due to modebeating between the first two
coupled modes of a hollow waveguide, both for the forward- (red) andcounterpropagating (blue) modes. Intensity peaks of the modulations
do not coincide well for a 6 cm waveguide (a), but do for an 11 cm
waveguide (b). c) The on-axis intensity ratio of the counterpropagating
to the forward propagating beams. In the 6 cm waveguide (solid curve),
this ratio fluctuates more strongly with position in the waveguide thanin the 11 cm waveguide (dashed curve), and is lower at the regions ofhighest intensity of the driving laser (indicated by vertical lines).

. . . 113

4.10 Probing temporal dynamics of HHG. a) Coherence length vs. harmonicorder. b)Time of harmonic generation within the ultrafast pulse. . . . . 114
4.11 a) Enhancement factor (I/Iavg ) of the 27th harmonic as a function of gas
pressure and position of the pulse collision point in the waveguide. The
coherence length increases as expected near the phase matching pressureof 45 torr, leading to a disappearance of the modulations. The position
within the waveguide at which the harmonic is strongly generated alsochanges with pressure. b) Average harmonic output (Iavg ) as a functionof pressure, demonstrating phase matching at ∼ 45 torr. . . . . . . . . . 117
4.12 Simulation of a scan of a single counterpropagating pulse when the singleatom strength of the harmonic emission and the coherence length do notvary with propagation distance. . . . . . . . . . . . . . . . . . . . . . . . 121

xix
4.13 Simulation of a scan of one and two counterpropagating pulses when the
single-atom strength of the harmonic emission varies with propagation
distance due to modebeating. . . . . . . . . . . . . . . . . . . . . . . . . 122
4.14 Harmonic spectra as a function of the collision region of one and two
counterpropagating pulses. . . . . . . . . . . . . . . . . . . . . . . . . . . 124
4.15 Simulation of a scan of two counterpropagating pulses when the singleatom strength of the harmonic emission varies with propagation distancedue to modebeating. For each of the curves, the suppression region (Ls )is constant, while the coherence length (Lc ) varies. The simulation reproduces features visible in Fig. 4.14b. . . . . . . . . . . . . . . . . . . . 125
4.16 Data demonstrating all-optical QPM at 65 eV in argon. . . . . . . . . . 127
4.17 A schematic illustrating the selectivity and tunability of all-optical QPM
using two counterpropagating pulses, by varying their separation. . . . . 130
4.18 Selectivity and tunability of all-optical QPM using two counterpropagating pulses with variable separation. Enhancement occurs when the pulse
separation is 2N Lc . Selectivity improves when N > 1. HHG spectrain argon show the shift of the enhancement with harmonic order as theseparation between the pulses is varied. . . . . . . . . . . . . . . . . . . 131
4.19 Selectivity and tunability of all-optical QPM using two counterpropagating pulses with variable separation. The spectrum enhanced by one pulse(solid gray) is plotted along with spectra enhanced by two pulses, for two
different pulse separations: 1.3 mm (red) and 1.0 mm (blue). . . . . . . 132
4.20 Data demonstrating all-optical QPM at 140 eV in helium. . . . . . . . . 133

xx
4.21 HHG spectra from argon in the presence of one counterpropagating pulse
held fixed in position at z ≈ 9 mm, while a second counterpropagating
pulse is scanned through a 2 cm region of the waveguide. Variation of
the periodicity of the oscillations with harmonic order (photon energy)
reveal dependences of the phase on the time the electron spends in thecontinuum before recombination. . . . . . . . . . . . . . . . . . . . . . . 137
4.22 Harmonic spectra in argon as a function of the collision position of thedriving laser pulse and a single counterpropagating pulse, revealing thepresence of several quantum trajectories with different coherence properties.138
4.23 Selective enhancement of either the long or short quantum trajectories
using all-optical QPM in helium. . . . . . . . . . . . . . . . . . . . . . . 140
A.1 Diagram of the standard Ti:sapphire cavity. . . . . . . . . . . . . . . . . 164
A.2 Diagram of the low repetition rate cavity. . . . . . . . . . . . . . . . . . 167
A.3 Low repetition rate laser data. . . . . . . . . . . . . . . . . . . . . . . . 168
A.4 Diagram of the high repetition rate cavity. . . . . . . . . . . . . . . . . . 170
A.5 High repetition rate laser data. . . . . . . . . . . . . . . . . . . . . . . . 172
B.1 Calculated transmission of the beamsplitter at 85◦ (a) and normal (b)incidence, including the original coating design, and the fits corresponding
to spectrophotometer and ellipsometer measurement.

. . . . . . . . . . 178

B.2 Ellipsometer measurements (black curves) and fitted model calculations(red curves) for Ψ (a) and ∆ (b). . . . . . . . . . . . . . . . . . . . . . . 178
B.3 Predicted (red) and measured (blue) reflectivities of the beam splitter at
EUV wavelengths. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 180
B.4 Measured spectral reflectance of a typical broadband spectrum from a
Ti:sapphire oscillator, for a variety of incidence angles. . . . . . . . . . . 181

xxi
C.1 Parameters of a standard Ti:sapphire laser cavity. . . . . . . . . . . . . . 186
C.2 Positions of optics on rail.

. . . . . . . . . . . . . . . . . . . . . . . . . 188

C.3 Appearance of fluorescence at P1 (a) and P2 (b). . . . . . . . . . . . . . 189
C.4 Appearance of the green and red beams at either of the curved mirrors
for maximum coupling between the pump beam and the red beam.

. . 191

C.5 Appearance of the (cw) output mode when the laser is aligned to favormodelocked operation. . . . . . . . . . . . . . . . . . . . . . . . . . . . . 192

Chapter 1
Introduction

1.1

High-Order Harmonic Generation as a Source of Coherent
EUV/ Soft X-Ray Light
The ability of the laser to produce intense and coherent light has precipitated a

revolution in science and technology. From spectroscopy to data storage, from communications to laser cooling, the laser has infiltrated not only our laboratories, but
our society. With the invention of the laser came the advent of nonlinear optics, andtogether they quickly expanded the range of frequencies over which it is possible to generate coherent light. The motivation to generate coherent light at short wavelengths andhigh photon energies has grown stronger. However, the production of coherent light at
VUV, EUV, and soft x-ray frequencies becomes difficult for a number of reasons. Thesefrequencies are strongly absorbed by any material, making the construction of optics
challenging, and the choice of gain or nonlinear media is quite limited. In addition, thepower requirement for obtaining laser action follows a λ−4 scaling with wavelength [2],placing high demands on pump sources. Lasers in the EUV, with wavelengths as shortas 10 nm, have been demonstrated with useful pulse energies [3], but are limited in
the available frequencies to a few electronic excitation transitions, and have yet to be
developed into commercially available products. Alternative sources of EUV and soft
x-ray light include synchrotron light sources [4] and free-electron laser (FEL) accelerator
facilities [5]. However, these large scale facilities are quite expensive and have limited

2
accessibility to researchers.
High-order harmonic generation (HHG) is a nonlinear optical process for upconverting coherent light from visible frequencies up to EUV and soft x-ray frequencies.
This technique for producing short wavelength light was made possible by the development of ultrafast, high intensity laser sources [6, 7] that can routinely produce visible
light pulse with peak intensities of 1015 to 1018 W/cm2 . Sources based on HHG have aconvergence of several attractive qualities in comparison with sources mentioned above.
HHG is fully temporally and spatially coherent [8, 9] and it can be used to produce
coherent radiation ranging from the UV up to photon energies > 1 keV [10]. It is anultrafast pulse source, with pulse durations from femtoseconds to attoseconds [11–13],
and it is accessible, since it is produced with a tabletop laser system. Demonstrated applications of HHG include studies surface dynamics [14], high-resolution imaging [15,16],
molecular dynamics [17–19], as well as static molecular structure [20], and attosecond
dynamics [21, 22].
As with any harmonic generation process, the main technical obstacle to a highconversion efficiency for HHG is the difference in the phase velocities between the fundamental and harmonic fields due to dispersion of the nonlinear material. Because ofthis phase mismatch, the phase of the fundamental field will shift by π rad relative tothe harmonic field as it propagates. This means that harmonic light generated earlyin the nonlinear medium will be exactly out of phase with harmonic light generated
a certain propagation distance later. This dephasing distance is called the coherence
length. This destructive interference limits the total achievable coherent buildup of theharmonic field. Balancing of the major dispersion terms to minimize the phase mismatch of HHG has led to bright HHG sources up to ∼ 100 eV , or λ ≈ 12 nm. Photon
yields here are on the order of 1011 photons/sec [23–25], allowing studies of the kindlisted above.
In high harmonic generation, the situation becomes complicated for generation

3
at high photon energies (200 eV and above). Because the laser generating the harmoniclight also ionizes the medium, a large dispersion results from the free electrons. Once thefraction of ionization increases above about 5%, conventional phase matching techniques
are no longer possible. Typical coherence lengths range from a few millimeters at
lower photon energies to a few microns at the highest observed photon energies. New
techniques for raising the conversion efficiency for HHG are crucial to extending thissource to high photon energies.
The density of free electrons can also change rapidly, both in time and in space. Intime, the ionization fraction can ramp up rapidly during the ultrafast pulse. In space,
the intensity can vary strongly due to refraction of the plasma and other nonlinear
effects. The dynamic nature of the phase mismatch is difficult to model accurately, andeven more difficult to compensate accurately. Phase matching is transient at best underconditions where the phase mismatch changes rapidly. The absence of experimental
techniques for measuring the local phase mismatch also limits further progress.
Quasi-phase matching (QPM) is an alternative method for compensating for thephase mismatch to improve conversion efficiency. In this technique, the phase of thedriving laser is corrected at a periodicity equal to twice the coherence length, so thatthe destructive interference is eliminated. Several proposals [26–32] and demonstrations[33–36] of QPM of HHG have been published to date. However, many of these havetechnical limitations, or limited scaling to higher conversion efficiency. One of thereasons for this is that there has not been an easy, in-situ technique for measuring the
dynamically changing coherence length of HHG.
In this thesis, I present new work using counterpropagating light for accurate
measurements of the local coherence length. This information provides previously unknown information about the dynamics of HHG. Measurement of the coherence length
is then used for a demonstration of efficient QPM using multiple counterpropagating
pulses. This technique is found to be flexible, customizable to the measured conditions,4and scalable both in terms of the enhancement factor and the phase mismatch it maycompensate.

1.2

Contents
The structure of this thesis is as follows: Chapter 2 contains a survey of the manydifferent physical processes involved in HHG, including the physics of electron rescattering, and nonlinear optical effects that influence HHG. Coupling and propagation oflight in hollow waveguides is reviewed, since this is the geometry used for the nonlinear interaction region. The mechanisms for phase matching and quasi-phase matchingof HHG are reviewed, along with proposals and previous demonstrations. Finally, theeffect of counterpropagating light on high harmonic generation is discussed, along withthe basic process for all-optical QPM.
The general experimental setup for generation and detection of harmonic lightis outlined in Chapter 3, and selected results are presented from exploratory work on
generating bright HHG from hollow waveguides. One of the main advantages of using
a hollow waveguide over a free-focus for HHG is its ability to maintain a high intensity
over a longer propagation distance. In order to characterize this, the density-dependent
energy loss of the driving laser beam is measured and simulated under a range of conditions. An estimate of the absolute photon yield at 45 eV is presented along with ashort discussion of optimization of the yield. Finally, quasi-phase matching using hollow waveguides with a modulated inner diameter is characterized. The enhancement of
HHG at high photon energies (200− 300 eV ) is reproduced, and the optimal modulation
depth is investigated.
Chapter 4 includes experimental results related to the use of counterpropagating
light both to probe and to quasi-phase match the process of HHG. Counterpropagating
pulses are used to probe the coherence of HHG, and provide a previously inaccessible
measurement of the local coherence length of the generation process. They are also used5
to study the spatial and temporal dynamics of the harmonic generation process. Since
the local phase mismatch is sensitive to the local intensity, measurement of the coherence
length provides information about intensity fluctuations present in the waveguide. Thesevariations are shown to be caused both by energy loss and the interference of propagating
modes of the waveguide. A two-pulse probing technique overcomes difficulties discoveredin the measurement of coherence with only one pulse. Counterpropagating pulses arealso used to implement an all-optical quasi-phase matching technique. Enhancement
is shown for emission from two different noble gases, helium and argon, for photon
energies that cannot be conventionally phase matched for the driving laser wavelength
used. Studies of the effect of this technique on the spectral and temporal structure of
the harmonic emission are also presented.
The final chapter includes a summary of the major experimental results, and a
discussion of possible avenues for future research on high harmonic generation using
counterpropagating light.
Three appendices describe work done in areas indirectly related to HHG. The firstis a demonstration and analysis of a cavity geometry change in a Ti:sapphire femtosecond laser that allows a variation of the repetition rate and pulse energy obtainable. The
second contains specifications and an analysis of a grazing-incidence, dichroic beamsplitter, designed to transmit the HHG driving laser wavelength, 800 nm, and to reflectharmonic photon energies in the range ∼35-100 eV . The third appendix is an alignment procedure for a Ti:sapphire oscillator of the kind used in our research group. It is
intended as an introduction to alignment and the characteristic behavior of these lasers
for those unfamiliar with their operation.

Chapter 2
Background and Theory

2.1

Introduction
This chapter reviews the theoretical models and previous work relevant to themeasurements described in Chapters 3 and 4. An understanding of high-order harmonic generation as an extreme nonlinear optical process, requires a description at
both the atomic and macroscopic levels. First, the origin of the microscopic nonlinear
polarization of the medium that leads to harmonic emission must be considered. Second,
it is necessary to understand how the macroscopic polarization evolves with propagation through an extended medium. Other important considerations are effects due tononlinear optical processes, inescapable at the intensities involved, including plasma
defocusing and blue-shifting of harmonic fields. To understand the propagation effects,
the major sources of dispersion in the present regime of HHG are described, and experimental background on previous efforts to phase match and quasi-phase match HHG aresummarized. Harmonic generation is found to depend sensitively on the coupling into
hollow waveguides and propagation of the intense laser beam that drives the process. A
discussion of propagation in hollow waveguides provides some insight into these effects.
Finally, the effects of counterpropagating light on HHG are described, particularly those
relevant to the probing and quasi-phase matching techniques discussed in Chapter 4.

7

2.2

High-Order Harmonic Generation: Single-Atom Response
The discovery of the processes of above-threshold ionization [37] and high-orderharmonic generation [38, 39] required a new description for the response of atoms tostrong fields. In particular, experimental studies of HHG showed a spectrum of harmonic emission peaks at odd multiples of the driving frequency. The strength of thepeaks decreased rapidly for the first few harmonic orders, then leveled out for several orders in a plateau region, then sharply decreased at specific cutoff photon energy.
Empirical and numerical [40] studies agreed on the shape of the plateau and locationof cutoff, but a cohesive physical picture was still lacking. A quantum and then semiclassical analytical theory was developed by Kulander et al. [41] and Corkum [42], which
accurately describes the main observable characteristics of high-order harmonic generation. It is also an intuitive and useful description of the physical processes involved.
This theory outlines three basic steps in the generation of high harmonic radiation:(1) Tunneling ionization of an atom by an intense laser field.
(2) The electron, now free of the atom, is driven by the electrical force of the sinusoidal
laser field.
(3) The electron may recombine with the ion to its ground state, the system emitting aphoton with energy equal to the ionization potential of the atom and the kinetic energyof the electron at recombination.
This model was subsequently expanded into a semi-analytical, quantum mechanical model by Lewenstein et al. [43]. This model quite accurately describes characteristics
of HHG seen experimentally, as well as providing a rigorous description of the picureof the semi-classical theory. In this theory, the emission of harmonic radiation from an
oscillating dipole is given as a product of three probability amplitudes, corresponding
to the three steps described above.

8
Step 1: Ionization
In a theoretical sense, high-order harmonic generation is fundamentally different
from low-order harmonic generation because of the process of optical ionization. Oncethe electric field of the laser has a strength comparable to the Coulomb field of the atom(∼ 1011 V /m), the laser field is no longer a small perturbation to the polarization of
the nonlinear material, and the atom can be ionized. While the induced polarizationof low-order nonlinear processes can be developed using perturbation theory [44], thisapproximation breaks down with increasing field strength.
Depending on the strength of the electric field, there are three basic models forphotoionization: multiphoton ionization, tunneling ionization, and above-barrier ionization [45]. A parameter defined by Keldysh [46] classifies which of these three mechanisms
is dominant. The Keldysh parameter is defined as:
s
Ip
,
γ=
2Up

(2.1)

where Ip is the ionization potential of the atom and Up is the ponderomotive energy.
The ponderomotive energy is the time-average of the kinetic energy obtained by anelectron in an oscillating electric field:
Up =e2 E02
e2 I
=
,
4mω 2
2mǫ0 cω 2(2.2)

where e is the electron charge, E0 is the amplitude of the laser field, m is the electron
mass, ω is the frequency of the laser field, ǫ0 is the permittivity of free space, and c isthe speed of light. Up is proportional to the laser intensity and the square of the laser
wavelength: Up [eV ] ≈ 9.3 10−14 I0 [W/cm2 ] λ2 [µm2 ].
Multiphoton ionization is the dominant mechanism for laser intensities at whichγ ≫ 1. In this case, the ionization can be modeled as the absorption of enough photons
by the atom for the electron to reach an energy level higher than the ionization potential.
For γ ≤ 1/2, the appropriate model becomes tunneling ionization. In this case, the laser

9electric field distorts the Coulomb potential strongly enough to form a potential barrier
through which part of the electron wavefunction may leak into the continuum (see Fig.
2.1). This process can occur when the laser frequency is small enough that the field isapproximately constant during the tunneling process. Another, more intuitive way toexpress the Keldysh parameter is γ = Tl /τt , where Tl is the period of the oscillating
laser field, and τt is the tunneling time. Tunneling ionization can only occur when
the laser period is shorter than the tunneling time. This is the regime in which HHG
takes place. The intensity at which tunneling ionization becomes dominant, for a laser
wavelength of 0.8 µm, in neutral argon gas (Ip = 15.78 eV ), is 5 1014 W/cm2 . In thethird regime, above-barrier ionization, the intensity is strong enough that the Coulomb
potential is suppressed below the ionization threshold, and the electron is essentially nolonger bound.

Coulomb Potential
Laser Potential

Potential

Quasistatic Sum Potential

Ionization Threshold

Distance from nucleus
Figure 2.1: Atomic Coulomb potential when distorted by an intense laser field, in thetunneling regime.

10
The probability for tunneling photoionization of an atom is the first step of thethree-step model outlined above. Ionization rates for the tunneling regime were developed by Ammosov, Delone, and Krainov [47], and later generalized to arbitrarily complex atoms and ions by including the effect of the Coulomb potential of the ion [48, 49].
The rate of ionization from the ground state can be expressed as:
ω (t) = ωp |C |
n∗

2



4ωp
ωt

2n∗ −1



4ωp
exp −
3ωt



,

(2.3)

where
ωp = Ip /h̄ωt = (eE(t)) / (2mIp )1/2n∗ = Z (IH /Ip )1/2
|Cn∗ |2 = 22n [n∗ Γ (n∗ + 1) Γ (n∗ )]−1∗

For Eqn. 2.3 and the definitions following it, Ip is the ionization potential of the atom,h̄ is Planck’s constant divided by 2π, E(t) is the electric field of the laser, m is theelectron mass, Z is the ion charge after ionization, IH is the ionization potential ofatomic hydrogen, and Γ(x) is the Gamma function.
The fraction of atoms ionized (or alternatively, the density of free electrons) is
given by:
 Z t

′
′
ω(t )dt .
η(t) = exp −

(2.4)

−∞

This value is important particularly for estimates of phase mismatch, since, as will beshown in more detail below, the phase mismatch is sensitively dependent on the relative
proportions of neutral atoms and free electrons. Figure 2.2 shows a sample calculationof the fraction of singly ionized argon as a function of time during a 25 f s pulse withpeak intensity 5 1014 W/cm2 . The stepwise nature of the curve results from the factthat ionization occurs strongly at the peak of field amplitude, which occurs at every
half cycle. It is important to note that the fraction of ionization is quite sensitive to11
the intensity at the time of ionization. Figure 2.2 shows the variation in time within
an ultrafast pulse. The ionization fraction will also depend on spatial variations in theintensity, making models of laser beam propagation important to modeling free electron

Fraction of ionization (η)

density.

1.0
0.8
0.6
0.4

Ioniz. Fraction: ηPulse profile

0.2
0.0
-20

-10

0
Time [fs]10

20

Figure 2.2: Fraction of ionization of argon as a function of time within a 25 f s pulse ofpeak intensity 5 1015 W/cm2 .

Steps 2 & 3: Rescattering and Recombination
Once the atom is ionized, the semi-classical three step model assumes the electron
starts with zero velocity, then is driven purely by the oscillating electric field of the laser.
The kinetics are calculated using the classical equations of motion. Under the influenceof a sinusoidal laser field E(t) = E0 cos(ωt), the velocity of the electron is−eE0(sin(ωt) − sin(ωt0 )) ,
mw

(2.5)

eE0
(cos(ωt0 ) − cos(ωt) − sin(ωt0 ) (ωt − ωt0 )) .
mw2

(2.6)

v(t, t0 ) =and its position isx(t, t0 ) =The electron’s specific path in the continuum depends on the phase of the driving
laser at the time of ionization, φ0 = ωt0 . Figure 2.3 shows the path of the electron for12several different values of the laser phase at the time of ionization. In this plot, the phasevalue of 0 rad represents the peak of the laser field. For phase values 0 < φ0 < π/2, alinearly polarized laser field will first carry the electron away from the ion, then, when
the field changes direction, drive it back toward the vicinity of the ion, then recombine.
A few of these trajectories are shown as the colored curves in Fig. 2.3. These paths
recross the x axis with a nonzero slope, indicating that the electron encounters the ion
with a nonzero kinetic energy. At φ0 = 0, the electron has exactly zero kinetic energy
when it reaches the ion (black curve, labeled 0 rad). For phase values π/2 ≤ φ0 ≤ π,
the electron will never reencounter the ion, but be driven away by the laser. A few
of these trajectories are shown in black on Fig. 2.3. This cycle repeats itself for the
next half-cycle of the electric field: phase values π < φ0 ≤ 2π. Again, recombinationis possible only for π < φ0 < 3π/2. Since the field reverse direction, the electrons are
driven in the opposite direction.
Harmonic emission, then, is most likely to occur twice within a single optical cycle.
The electron can reencounter the parent ion multiple times (see, e.g., the blue curve in
Fig. 2.3), providing multiple opportunities for recombination at varying times within
the optical cycle. However, the quantum nature of the electron makes recombination
increasingly unlikely. The electron wavepacket spreads transversely with respect to thedirection of its motion, at a rate of ∼ 1.5 Å/f s [42]. The probability of recombination
increases for a larger parent ion or a shorter laser wavelength. Higher collision crosssections [50] of nonlinear gaseous media increase the probability of recombination, sothat larger rare gas atoms have a higher nonlinear susceptibility. Only linear polarizationof the laser field is used for HHG. Even a slight ellipticity will steer the electron awayfrom the parent ion, reducing the chances of recombination.
The velocity of the electron at the time it reencounters the parent ion determines
the energy imparted to the high harmonic photon. Figure 2.4 shows the kinetic energy ofthe electron at recollision as a function of the phase value at which it was ionized. Again,

13

Distance of Electron from Ion
2
0 rad

1

0.07 rad−1

2

x/ (eE/mw )00.31 rad−2−3

0.72 rad−4
2.36 rad−5

2.09 rad−6

1.57 rad

−7
−8
0

0.5

1

1.5

2

2.5

3

3.5

4

Laser phase (rad/pi)
Figure 2.3: Possible paths for the electron during rescattering as a function of laser phase(time), and several selected values of the phase of the laser at ionization (or, equivalently,
time at ionization). Intersection with the x-axis indicates a possible opportunity forrecombination.

Kinetic Energy at Return
3.5
3

KE/ Up

2.5
2
1.5
1
0.5
0
0

0.1

0.2

0.3

0.4

0.5

Laser phase at release (rad/pi)
Figure 2.4: Kinetic energy at the return of the electron to the parent ion, as a functionof phase of the laser at ionization.

14phase values are plotted only for 0 < φ0 < π/2, for which the electron path reencounters
the ion. Kinetic energy values are given in terms of Up , the ponderomotive energy. The
graph shows that for each value of the return kinetic energy, there are two values ofthe phase at which the electron was originally released. At the peak of the curve is thehighest return kinetic energy, KE ≈ 3.17Up , at φ0 ≈ 0.09π. These features are further
illustrated in a plot of the electron trajectories, Fig. 2.5. This plot shows trajectories
for the singular path of the highest kinetic energy, as well as the two paths that returnto the ion with KE = 1.5Up . The middle green curve represents the trajectory that
contributes to the highest photon energy that can be generated with a sinusoidal driver
field. This is known as the “cutoff” photon energy. The red and blue curves represent
what are called the “short” and “long” trajectories, respectively, for generating photon
energies that are smaller than the cutoff. The short and long trajectories are mostdistinct at low harmonic orders and throughout the plateau region, and converge at thecutoff.
If the electron recombines with the ion into its ground state, the system will
emit a photon with energy equal to the ionization potential of the atom plus the return
kinetic energy of the electron. Using the largest possible return kinetic energy from Fig.
2.4, the cutoff photon energy is given by:hνmax = Ip + 3.17Up .

(2.7)

This equation describes the highest observable photon energy, assuming a perfectly
sinusoidal field (a less than accurate assumption for ultrafast pulses < 30 f s [51]), andemission from the first encounter with the ion. The cutoff rule has, however, been wellborne out as a general rule both by experiment and theory [40–43,52]. Since Up ∝ Iλ2 , ahigher cutoff may be obtained by increasing either the intensity or the wavelength. Eachof these changes, however, reduces the brightness of harmonic emission, albeit in very
different ways. A higher intensity increases the dephasing of the coherent buildup of the15

Distance of Electron from Ion
2
Maximum slope (KE)02x/ (eE/mw )1

Equal slopes (KE)−1−2"Long" trajectory at 1.5 Up"Cutoff" trajectory at 3.17 Up"Short" trajectory at 1.5 Up

−3

−4
0

0.5

1

1.5

2

Laser phase (rad/pi)
Figure 2.5: Possible paths for the electron during rescattering, indicating the origin of
the “cutoff” photon energy, as well as the “long” and “short” trajectories contributing
to a photon energy below cutoff.

harmonic field, which will be described in greater detail below. A larger wavelength,
on the other hand, will cause the electron to spend a longer time in the continuum,
reducing the probability of recombination due to the spread of the electron wavepacket.
Intensity-Dependent Phase
Since high-harmonic generation is a coherent process, the phase of the emitted
harmonic light depends in part on the phase of the laser field. However, there is asecond, significant component to the phase of the harmonic emission that depends on
the intensity. The dipole phase, also called the intrinsic phase, is the phase accumulatedby the electron wavefunction as it propagates in the continuum. The total phase of theharmonic field, the sum of these two components, is given by
φq = qωtr −1
S(t0 , tr ),
h̄

(2.8)

in which t0 and tr are the ionization and recombination times, respectively, q is the

16harmonic order, ω is the angular frequency of the laser field, and S(t0 , tr ) is the quasiclassical action [53], which can be approximated as:
S(t0 , tr ) =

Z tr

dt

t0




p(t0 , tr )2+ Ip .
2m(2.9)

In Eqn. 2.9, p(t0 , tr ) is the momentum of the electron at ionization, m is the mass ofthe electron, and Ip is the ionization potential of the atom. The two components of thephase described by Eqn. 2.8 correspond to: 1) the phase of the laser field at the timeof recombination, tr , and 2) the intrinsic phase.
A direct implication of Eqn. 2.8 is that each of the two trajectories that contributes to a given harmonic order q acquires a different phase, since each corresponds
to a different time of recombination, tr . Also, the dependence of the phase on the actionmeans that the intrinsic phase is intensity dependent. Combining Eqns. 2.5 and 2.8
makes this intensity dependence explicit:
2Up
φq =
h̄ω

Z φr
φ0

dφ (sin(φ) − sin(φ0 ))2 +Ip(φr − φ0 ),h̄ω(2.10)

where φ0 = ωt0 , φr = ωtr , and Up ∝ I (Eqn. 2.2). The dependence of the harmonic
phase on the intensity is given by the derivative:∂φq
2K ∂UpKe2==,∂Ih̄ω ∂Ih̄mǫ0 cω 3

(2.11)

using the definition for Up , Eqn. 2.2. K is the solution of the integral in Eqn. 2.10,
a dimensionless constant whose value depends on the trajectory of the electron [54].
Figure 2.6 shows the dependence of K on φ0 , the phase at the time of ionization. The
black vertical line at φ0 = 0.09π rad indicates the phase at cutoff (cf. Fig. 2.4). Long
trajectories originate with φ0 < 0.09π rad, and short trajectories for φ0 > 0.09π rad. In
general, for a given kinetic energy contribution to the harmonic photon energy, the long
trajectory has a much larger value of K than does the short trajectory. For example,
for the plateau harmonic which is generated with a kinetic energy component of 1.5Up ,

17
3.5
3
2.5

K

2
Long

1.5 Trajectories

Short
Trajectories

1
0.5
0
0

0.1

0.2

0.3

0.4

0.5

Laser phase at release (rad/pi)
Figure 2.6: Values of K as a function of release phase.

Klong = 2.89, while Kshort = 0.323. The phase of the long trajectories are thus much
more sensitive to the intensity than are the short.
Figure 2.7 shows the intensity dependent phase for the short and long trajectories
as a function of intensity for q = 31, using a full analytical model. The slopes of thethe two curves are determined by the value of the dimensionless constant K. This
plot illustrates the rapid accumulation of phase with increasing intensity of the long
trajectory compared to the short.
The intrinsic phase can have a significant effect on the temporal and spectral
structure of HHG. One of these effects occurs with a short driving laser pulse, in which
the intensity changes significantly between half-cycle peaks. On the leading edge of thepulse, a changing intensity from peak to peak results in both a higher generated photon
energy and intrinsic phase shift with time. This causes an inherent negative chirp in theharmonic emission, particularly for the photon energies near cutoff, where the emission

18

Figure 2.7: Harmonic phase of the 31st harmonic generated in argon, as a function of
the intensity. Ith,31 indicates the threshold intensity for generating the 31st harmonic.
The curves show a stronger dependence on intensity of the phase of the emission fromthe long trajectory. Reproduced from Ref. [55].

Figure 2.8: Harmonic spectra generated in argon with driving laser pulses of varying
chirp. Reproduced from Ref. [56].

19
is limited to a few trajectories. The temporal structure of the HHG may be controlled
by varying the chirp of the driving laser pulse, as shown in Ref. [56]. Figure 2.8 shows
several harmonic spectra generated using driving laser pulses of varying chirp. The
appearance of strong harmonic peaks indicates the role of intrinsic phase in the spectral
structure of HHG.

2.3

Macroscopic Phase Effects
Equally important to the microscopic, or single-atom, effects on the properties ofhigh-order harmonic generation are the macroscopic, or propagation effects. There areseveral physical processes which affect the spectral, spatial, and temporal properties of
HHG, and below are descriptions of a few that are most relevant to the data presented
in Chapters 3 and 4. Emitted harmonics are frequently blue-shifted in frequency undercertain experimental conditions, either due to self-phase modulation caused by ionization, or non-adiabatic effects of the ultrafast laser pulse. The propagating laser beam isalso greatly affected by the process of ionization through energy loss and a tendency todefocus in the presence of the generated plasma. Finally, the spatial profile and coherence properties of HHG are largely determined by propagation effects. One of the mostsignificant processes affecting the conversion efficiency of HHG, dephasing between thefundamental and harmonic fields, will be addressed in the following section.
Self-Phase Modulation
Self-phase modulation (SPM) is a common occurrence whenever ultrafast pulses
interact with matter. The ultrafast pulse induces a time-varying index of refraction in
the material it propagates through, due to a nonlinear interaction, which in turn varies
the instantaneous frequency of the laser pulse. For a pulse with a high and rapidly
varying intensity, this frequency variation can significantly change the laser spectrum.
Two main nonlinear processes vary the index of refraction in the case of the ultrafast
pulses used to drive high harmonic generation.

20
The intensity-dependent index of refraction is a third order nonlinear process,also called the optical Kerr effect, which easily becomes significant at the intensities
used for HHG. The nonlinear index is expressed asn(t) = n0 + n2 I(t),(2.12)

in which n2 is referred to as the nonlinear index coefficient and I(t) is the time evolutionof the intensity of the ultrafast pulse. Since the index of refraction of the material
depends on intensity, the index of the material rapidly changes in time as the pulse
propagates through. The instantaneous phase of the laser pulse is given by
φ(t) = ω0 t −2πn(t)L,
λ0(2.13)

where ω0 and λ0 are the center frequency and wavelength of the pulse, respectively, and
L is the length propagated in the medium. This phase shift, which is time-dependent,
causes a shift in the instantaneous frequency of the pulse:ω(t) =

2πLn2 dI(t)dφ= ω0 −.
dt
λ0
dt(2.14)For a typical ultrafast pulse, the temporal shape is similar to a Gaussian or hyberbolic
secant squared. On the rising edge of the pulse, dI(t)dt > 0, causing a shift toward lower
frequencies, while the falling edge ( dI(t)dt < 0) is shifted toward higher frequencies.
At modest intensities, HHG occurs only near the peak of the pulse, so that harmonic light is emitted symmetrically toward the rising and falling edges of the pulse.
In this case, the frequency shift will be translated symmetrically to the spectrum ofeach harmonic peak. When the intensity is higher, however, harmonic generation canbe limited to only the rising edge of the pulse. The main reason for this is that thegas medium can become almost completely ionized by the peak of the pulse (see, e.g.,
Fig. 2.2). In this case, the harmonic light should be red-shifted, since the frequencies ofthe laser pulse are also red-shifted. However, the ionization itself causes a time-varying

21
refractive index which tends to dominate the third-order effect, and causes a blue-shiftof the harmonic peaks.
Ionization-Induced Blue-Shifting
Blue-shifting of the harmonic frequencies has been extensively studied throughexperimental observation [55–58] and modeling [55, 59, 60]. The rapid ionization of thegas medium is one of the main causes of this phenomenon, called ionization-induced blueshifting. The time-dependent index of refraction of a plasma depends on the density,and is given by
np (t) =s1−ωp2 (t)ωp2 (t)
≈
1
−
,
ω2
2ω 2

(2.15)

where ω is the angular frequency of the laser field,s
Ne (t)e2
ωp (t) =ǫ0 m(2.16)

is the plasma frequency, and Ne (t) is the free electron density. (For a derivation of
the plasma index, see Ref. [61] or [62].) The approximate value of Eqn. 2.15 holds forω 2 ≫ ωp2 . As the free electron density, Ne (t), increases with time during ionization by theultrafast pulse, the plasma index decreases. Since the plasma dispersion is anomalous,a decreasing index results in a greater phase shift. At the same time, the number ofneutral atoms is proportionately decreased, and so this normal dispersion contribution
to the index is decreased. The time-dependent index due to the free electron plasma interms of the fraction of ionization, η(t), is
np (t) = 1 − η(t)Natm P e2,
2ω 2 Patm ǫ0 m

(2.17)

since Ne (t) = η(t)Natm P/Patm , where Natm is the number density at 1 atm, and P/Patmis the fractional pressure with respect to atmospheric pressure. The instantaneous
frequency shift of the laser field due to the increasing plasma is:
2πL dnp (t)2πL dη(t)ω(t) = ω0 −= ω0 +
λ0
dt
λ0 dt



Natm P e2
2ω 2 Patm ǫ0 m

.

(2.18)

22
Note in this case that the increasing free electron density causes a shift to higher frequencies throughout the duration of the pulse. Figure 2.2 shows that the ionization level
increases throughout the pulse, since the plasma lifetime (∼ ns) is significantly longer
than the typical ultrafast pulse (∼ f s). This causes an overall blue-shift of the laser
frequencies that is proportional to the ionization rate. For low intensities, when the
final ionization fraction is significantly smaller than 1, the strongest blue-shifting will
occur, symmetrically, near the peak of the pulse where the ionization rate is high. On
the other hand, when the gas is fully ionized by the peak of the pulse, for very intense
pulses like the one shown in Fig. 2.2, the strongest blueshifting will occur on the risingedge of the pulse.
While ionization-induced blue-shifting can also directly shift the harmonic frequencies, the dominant effect is indirect, by shifting the fundamental laser frequency.
The reason for this can be seen in Eqn. 2.18: the time-dependent frequency is proportional to λ, thus the indirect shift is a factor of q stronger.
Non-Adiabatic Blue-Shifting
The rapidly changing intensity of the ultrafast pulse contributes to a second significant blue-shifting process. However, in this case there is a direct shift in the harmonicfrequencies. This blue-shifting results from the intensity-dependent phase of the harmonic light, and is referred to as non-adiabatic blue-shifting [55]. For this process, thedegree of blue-shifting varies with the harmonic order and contributions from different
trajectories. This contrasts with ionization induced blue-shifting, which affected theharmonics indirectly through a frequency shift of the laser field, and is independent ofboth harmonic order and trajectory contribution. In non-adiabatic blue-shifting, there
is a significant difference in the degree of frequency shift with harmonic order, particularly for harmonic orders well below cutoff. For mid-plateau harmonics, there is a large
difference in the intensity-dependent phase accumulated by the long and short trajectories that contribute to them. This difference decreases toward the cutoff, where the23phase variation between the long and short trajectories disappears.
Non-adiabatic blue-shifting can be described starting with Eqn. 2.8, for the phaseof the harmonic emission. The time derivative of the phase is the instantaneous frequency:
ω(t) =dφq
Ke2 dI(t)= qω0 −,dth̄mǫ0 cω 3 dt

(2.19)

using Eqn. 2.11 for the intensity dependence of the harmonic phase. Like self-phasemodulation, and unlike ionization-induced blue-shifting, the frequency shifting will besymmetric about the peak of the pulse, especially for pulses of modest intensity. However, this effect is strongest for very intense pulses, when harmonics are generated on
the rising edge of the pulse, where the intensity varies most rapidly.
This blue-shifting can be detected in the spectral content of the harmonic emission. Since the value of K is larger for long trajectories, the long trajectories will beblue-shifted more strongly than the short trajectories. This can lead to a splitting of
the harmonic peaks within the plateau. Figure 2.9 shows the result of a calculation performed by Kan et al. [60] using the Lewenstein model for HHG. Figure 2.9a) shows the
harmonic spectrum for a 150 f s pulse with a peak intensity of 1015 W/cm2 , displaying
two main separated peaks corresponding to the long and short trajectories, in which thelong trajectory appears at a higher frequency than the short. The temporal structureof the emission of the 55th harmonic order is shown in Fig. 2.9b), clearly showing theemission in the rising edge of the pulse.
Figure 2.10 shows an harmonic spectrum generated in 5 torr argon, using a 27
f s pulse with a peak intensity of ∼ 5 1014 W/cm2 . The harmonics shown are within
the plateau region; for the peak intensity used, the cutoff is around the 61st order.
A clear double peak structure is visible for each of the harmonic orders shown. The
capability to distinguish emission from the different trajectories in the spectral data
provides information about the temporal structure of the emission, and can be used

24

Figure 2.9: Calculated spectral (a) and temporal (b) structure of the 55th harmonicorder generated by a 150 f s pulse with a peak intensity of 1015 W/cm2 . Different
electron trajectories appear with different frequencies, due to the intensity-dependent
phase of harmonic emission. Reproduced from Ref. [60].

as an indicator for the use of counterpropagating pulses to manipulate HHG, discussed
further in Chapter 4.
The properties of HHG are not only affected strongly by the temporally varying
intensity of the ultrafast laser pulse, but they are also affected by the spatially varying
intensity of the laser beam. Two of the spatial effects are ionization-induced defocusingof the laser beam, and a different divergence in the harmonic emission from each of the25

Intensity [a.u.]

2500
2000
Long

1500

Short

1000
500
0
21

23

25

27

31

35

39

43

Harmonic Order

Figure 2.10: Harmonic spectra generated in 5 torr argon, with a 27 f s pulse with a peakintensity of ∼ 5 1014 W/cm2 , showing peak splitting due to non-adiabatic blue-shifting.
The two peaks correspond to emission from the long and short electron trajectories.

two main trajectories which contribute to harmonic emission.
Ionization-Induced Defocusing
Ionization-induced defocusing is a mechanism that can change the propagation of
the intense laser beam used to generate high harmonics [63,64]. Because of the refractionof the free electrons that are generated during ionization, the beam can diverge more
quickly and lose the high intensity needed for HHG. In a free-focusing geometry, thelaser beam is loosely focused through the gas medium. For a Gaussian laser mode, theintensity will be highest at the axis of propagation and fall off radially. The ionization
rate is directly related to the intensity, meaning that the free electron density will behighest at the central axis of the propagating beam, and will fall off radially. From Eqns.
2.15 and 2.16, it can be seen that the plasma index is directly proportional to the freeelectron density. A significant radial change in the index will produce a lensing effect.
However, since the dispersion of a plasma is anomalous, the high free electron density at
the center will have a comparatively low index that increases radially outward, creating

26
a diverging lens. The strength of this effect can be quantified by what is called thedefocusing length [63], given by
lD =

λ Ncr
,
2 Ne

(2.20)

where Ncr = ǫ0 mω 2 /e2 is the critical free electron density, at which ω = ωp . The
defocusing length, lD , is the propagation length in the presence of the plasma at which
the divergence of the beam doubles. This effect becomes more prominent at higher
intensities, as well as higher gas pressures, both of which increase the free electron
density. This effect is counteracted by the use of hollow waveguides, which can partiallyrefocus the light to maintain the intensity over a longer propagation distance.
Trajectory-Dependent Divergence
The second effect involving spatial phase variation is a different divergence between the long and short trajectories. For a Gaussian radial distribution of the intensity,
there will be a corresponding radial difference in the accumulation of the intensity dependent phase (Eqn. 2.10). The long trajectories are more more sensitive to the intensity,and so the phase fronts for contributions from the long trajectories will be more strongly
curved. Figure 2.11 shows the different phase fronts for the long, denoted as “τ2 contribution,” and short, denoted as “τ1 contribution,” trajectories. With a strongly curved
phase front, the contribution from the long trajectories will be much more divergent,
which has been confirmed both by calculation [65] and experiment [8].
These phase differences between emission from the two trajectories ultimately
determine the coherence of the HHG beam. Studies of the temporal [8, 65] and spatial [9, 66–68] coherence of HHG sources show that interference between emission fromthe two trajectories tends to degrade both the temporal and spatial coherence of theemission. Coherence tends to improve when the conversion efficiency of one of the two
trajectories is selectively enhanced through phase matching of the nonlinear conversion
process. For free-focusing geometries, this is accomplished by placing the gas inter-

27

Figure 2.11: Phase fronts for the different trajectories that contribute to plateau harmonic orders. The stronger dependence of the harmonic phase on intensity leads to agreater curvature for the long (τ2 , dashed curve) compared to the short (τ1 , solid curve)
trajectories. Reproduced from Ref. [65].

action region after the focus of the laser beam to avoid the Guoy phase shift at thefocus [65, 67]. For HHG in a waveguide geometry, dispersion from the waveguide isindependent of propagation distance and importantly, pressure, so that tuning of thepressure creates phase matching conditions for a single trajectory. Finally, all-opticalquasi-phase matching with counterpropagating light in a hollow waveguide also canselectively enhance a single trajectory [69].

2.4

Phase Matching
The most significant macroscopic effect on the conversion efficiency and bright-

ness of high harmonic generation is the phase mismatch between propagation of thefundamental and harmonic frequencies. Phase mismatch describes the degree to which
dispersion causes the fundamental and harmonic frequencies to propagate at different

28phase velocities through the nonlinear medium. Without compensation for this phasemismatch, the propagation length over which the harmonic field may sum coherently islimited, and so the total brightness of the harmonic source is likewise limited. Essentially, if the fundamental field propagates at a different phase velocity than the aggregate
harmonic field, after a certain propagation distance the fundamental field will be exactly out of phase with the co-propagating harmonic field. At this point, subsequently
generated harmonic light will begin to destructively interfere. The phase mismatch isexpressed as the difference between the propagation vectors of the fundamental and q th
harmonic fields:∆k = qk0 − kq ,(2.21)

in which k0 is the propagation vector of the fundamental and kq is that of the q th
harmonic order. A simple description of the harmonic field at the end of a nonlinear
medium of length L is:
EHHG (L) =

Z L
0

0
EHHG
(z) exp (i∆kz) dz,(2.22)

0in which EHHG(z) is the microscopic amplitude of the generated harmonic field as afunction of propagation distance, z. Classical derivations of the nonlinear response
adapted for high harmonic generation can be found in [54, 70]. The harmonic field will
be maximal when ∆k = 0, otherwise the strength of the field will oscillate sinusoidallywith propagation distance. The periodicity of this oscillation is twice a characteristic
length known as the coherence length:
Lc =

π
.
∆k

(2.23)

Lc describes the propagation distance between two locations of harmonic emission thatare exactly out of phase. In other words, at the end of the coherence length, there is a
π phase slip between the fundamental field and the harmonic field that was generated
at the beginning of the coherence length. The intensity of the harmonic light detected29
at the end of nonlinear medium of length L depends sensitively on the phase mismatch:
Iq = Iqmax

sin2 (∆kL/2),(∆kL/2)2(2.24)

which is plotted in Fig. 2.12, showing the sharp decrease in the obtainable harmonic
intensity with increasing phase mismatch.

Normalized Intensity (I/Imax)

1

0.8

0.6

0.4

0.2

0
0

0.5

1

1.5

∆ kL/2/ π

2

2.5

3

Figure 2.12: Harmonic intensity as a function of the phase mismatch.

When the phase mismatch is zero, the fundamental and harmonic fields are inphase throughout the medium, and the harmonic field grows linearly with distance.
The harmonic intensity, then, grows quadratically with distance. Figure 2.13 illustrates
the growth of harmonic intensity in two cases: for phase matching, and for a non-zerophase mismatch. Note than even after a single coherence length, the non-phase matchedintensity is only 40% of the phase matched intensity.
In general, material dispersion of the nonlinear medium precludes phase matching,since different frequencies propagate with different phase velocities. In low-order nonlinear optical harmonic generation, such as second harmonic generation (SHG), phaseOutput Harmonic Signal

30

Phase
Matched∆ k=0

Not Phase Matched
∆ k≠0
0

1

2

3

4

5

6

7

8

L/Lc
Figure 2.13: Harmonic intensity as a function of propagation distance, in the case ofphase matching and a non-zero phase mismatch.

matching is most often achieved through the use of a birefringent crystal. The anglesof the polarizations of the fundamental and harmonic fields with respect to the optic
axis are tuned carefully so that the two fields propagate with the same phase velocity.
Unfortunately this technique cannot be transferred to HHG. The nonlinear medium for
HHG is most often a dilute, isotropic noble gas, for a couple of reasons. First, the highionization potential of the noble gas atoms allows generation of higher photon energies(Eqn. 2.7), since the atoms can persist to a high instantaneous laser intensity before
ionization. Second, high order harmonics are at frequencies which are strongly absorbed
by any material, making a low pressure gas necessary to prevent excessive reabsorptionof the harmonic photons.
Minimization of the phase mismatch in HHG has been studied extensively inthe pursuit of maximizing the conversion efficiency [23, 71–76]. Two often-used tech-

31
niques for minimizing phase mismatch involve a balance of the main dispersion terms in
HHG, in particular taking advantage of phase mismatch terms originating from the laser
propagation geometry. In initial studies by L’Huillier and coworkers [71–73], high-orderharmonics were generated by placing a gas jet at or near the focus of the laser beam.
These studies were restricted to very low pressures and low intensities, and the dispersion from the neutral gas and free electrons were neglected. Instead, transient phasematching was achieved through a balance of the geometrical Guoy phase shift across thefocus and the intrinsic phase shift through the variation of the intensity at the focus.
Hollow waveguides were subsequently used for HHG by Murnane and Kapteyn [23, 74].
Guiding of the laser light extends the region of high intensity and may partially counteract the ionization-induced defocusing, while providing a new mechanism for minimizing
the phase mismatch. In this case, the range of phase matching was extended to higher
pressures, as the contributions from the neutral gas and free electron dispersion weretaken into account. In fact, the hollow waveguide provides a mechanism for true phasematching over a long interaction distance by removing the transient nature of the Guoyphase shift and instead, providing a “plane wave” propagation geometry. Below are
discussed three of the main contributions the phase mismatch: neutral gas and plasma
dispersion, and geometrical corrections to the propagation vector.
Neutral gas dispersion
For the noble gas atoms used as the nonlinear medium for HHG, the resonancefrequency is most often present somewhere between the fundamental and harmonic frequencies. Thus the index for the fundamental frequency is positive and for the harmonicfrequency is negative. The phase mismatch contribution due to material dispersion, forharmonic order q, is simply
∆k =

2πq
(n(λ0 /q) − n(λ0 )).
λ0(2.25)The index of refraction of noble gases, being very close to unity, are often reported

32
in the form δ(λ) = n(λ) − 1, at STP (1 atm and 298 K) [77, 78], using the Sellmeierequation to express frequency dependence. The index scales linearly with pressure,so the index can be scaled by P/Patm , or the ratio of the gas pressure relative toatmospheric pressure. For the fundamental wavelength of λ0 = 0.8 µm, δ(λ0 ) ∼ 10−5 ,and for harmonics q > 21, δ(λ0 /q) ∼ −10−4 to −10−6 . Because of ionization, thedensity of neutral atoms is also scaled by the fraction of ionization, η, giving a phasemismatch between the fundamental and harmonic fields of:
∆kN =

2πq P
δn (1 − η),
λ0 Patm(2.26)

in which δn = δ(λ0 /q) − δ(λ0 ) is the difference in the index of refraction between thefundamental and harmonic wavelengths. The dispersion of the resultant ions are often
neglected for a couple of reasons: first, the resonance frequency is higher than that ofneutral atoms, and second, by the time there is a significant population of ions, whenη > 0.1, the free electron contribution to the phase mismatch is much greater than any
other term.
Plasma dispersion
For the dispersion of the plasma, Eqn. 2.25 also applies, using Eqn. 2.17 for theplasma index. The electron number density, Ne , can be rewritten as ηNatm P/Patm , inwhich Natm is the atomic number density at STP. A substitution can also be made for21ethe classical electron radius, re = 4πǫ
2 . Substituting and simplifying Eqn. 2.25 gives
0 mc∆kP l = ηNatm re λ0

P q2 − 1.
Patm q(2.27)

Since (q 2 − 1)/q ≈ q when q ≫ 1, this factor is often approximated for high orders.
Geometrical phase mismatch
Propagation of the driving laser mode also contributes to the phase mismatch
through effects on the propagation vector. Two geometrical situations are common in
HHG: a free Gaussian focus, and guiding through a hollow dielectric waveguide. A free33
focus through a gas jet or a gas cell is commonly used in HHG experiments, and suffersfrom a phase shift across the focal region of π radians, called the Guoy phase shift. This
phase shift is in the form of the arctangent near the focus:
φGuoy = arctan(z/b),(2.28)

where b = ωwo2 /2c is the Rayleigh range and w0 is the 1/e2 intensity beam radius of thefundamental beam. The Guoy term for the harmonic light is smaller than that for the2o (λ0 )
fundamental by a factor of ≈ q12 wwo (λ2 , and is therefore neglected for high harmonic
0 /q)orders. Thus the phase mismatch resulting from the Guoy phase is that from the effecton the fundamental field:
∆kG =

qλ0
.
πwo2

(2.29)

This large phase shift is often avoided by placing the interaction medium either before
or after the focus.
The propagation of guided modes within a hollow waveguide will be discussed
in more detail in Section 1.7. The correction to the propagation vector by guiding isconstant through the interaction distance. Since high harmonic generation typicallyoccurs only close to the central axis of the waveguide, where the intensity is highest,
the harmonic light does not encounter the walls of the waveguide. The phase mismatchis therefore also given only in terms of the effect on the fundamental beam:∆kW =qu2nm λ0,4πa2(2.30)

where a is the inner radius of the waveguide, and unm is the mth root of the (n − 1)thBessel function of the first kind, specifying the coupled mode. Given a linearly polarized
fundamental beam, n = 1 for the most strongly excited modes.
Although far from rigorous, these formulae are useful in practice for estimation of
the phase mismatch and coherence length. However, several parameters are neglected,
including the intensity-dependent phase of the harmonic field, which has been shown34
to significantly affect the phase mismatch (e.g. see the results of Chapter 4 as well as
Refs. [53, 73]). In addition, it is worth noting that although the phase mismatch canbe expressed relatively simply in terms of the experimental parameters involved, theseparameters themselves are often far from constant. For example, two of the terms are
dependent on the ionization fraction, η, which can change drastically in time as well as
both the propagation and radial directions. The phase mismatch is thus a dynamicallychanging quantity, and the phase matching techniques described below often can only
correct for the phase mismatch within a limited temporal or spatial window. In the caseof a free focus geometry in particular, the geometrical Guoy phase shift, as well as thegas density in a typical gas jet, also change with propagation and radial dimensions,allowing minimization of the phase mismatch over a limited volume.
Balancing Phase Mismatch: Free Focus and Hollow Waveguide
Phase matching of HHG can be achieved by balancing the various dispersion terms
for a zero net phase mismatch. In the case of free focusing, the total phase mismatch is
given by :∆k = ∆kN + ∆kP l + ∆kG = −

P
qλ0
2πq P
δn (1 − η) + qηNatm re λ0−
λ0 Patm
Patm
πwo2(2.31)

Recall that the geometrical term is valid only near the focus. Note that the neutral atoms
and the geometrical phase mismatch are negative terms, while the free electron term is
positive. These terms may be balanced by adjusting either the level of ionization throughthe peak intensity, or the gas pressure. In practice, this technique is only applicablefor very low levels of ionization, at most a few percent (as will be shown below). At
the intensities used in this situation, the variation of the intensity dependent phaseof the harmonic emission with propagation is stronger than the dispersion of the freeelectrons. Thus the brightest emission from a free focus geometry is often achieved
through balancing the Guoy phase and the intensity dependent phase.
The effect of the intensity dependent phase was investigated by L’Huillier and35
coworkers [71, 73]. In particular, they showed that observed improvement in conversion
efficiency as well as changes in the harmonic beam’s divergence, through adjusting thelocation of the gas jet relative to the focus of the driving laser beam, can be explained
through the effect of the intensity dependent phase. Figure 2.14 shows the on-axis
dependence of the harmonic phase as a function of propagation distance relative tothe focus. The long-dashed line shows the Guoy phase shift of the fundamental laser
beam, the short-dashed line shows the calculated dipole phase, which varies with theon-axis intensity through the focus, and the solid line is the sum of the two. The phasemismatch will be minimal where the variation of the phase with propagation is minimal,
i.e., at ∼ 3 mm in the figure. Note that neither of these effects are dependent on thegas density.

Figure 2.14: Dipole phase as a function of propagation distance. The long-dashedline shows the phase evolution of the fundamental through the focus due to the Guoyphase shift. The short-dashed line shows the evolution of the harmonic phase due tothe intensity-dependent phase. The solid curve is the sum of the two contributions.
Reproduced from Ref. [73].

36

Figure 2.15: Conversion efficiency of HHG for the 45th harmonic order as a function of
the distance of the focus from the gas jet (z). The 3D plots illustrate the harmonic fieldat z = −1 and z = 3mm, as a function of the propagation distance and the transverse
direction (azimuthal symmetry is assumed). Reproduced from Ref. [73].

A calculation of the conversion efficiency as a function of the distance, denotedby z, between the focus and a gas jet of width 0.8 mm FWHM is shown in Fig. 2.15.
There are two local maxima in the conversion efficiency, one of which is in fact locatednear z = 3 mm, with another at z = −1 mm. Inset in the figure are 3D plots of theharmonic buildup at each of these two maxima as a function of both the propagation
distance and the dimension perpendicular to the propagation axis. These insets reveal
one of the realities of phase matching techniques in HHG, especially in the case of a freefocus: its transient nature. The maximum in conversion efficiency at z = 3 mm occurs
on-axis, as Fig. 2.14 predicts. The second maximum, however, at z = −1 mm, resultsfrom off-axis phase matching. This strong, off-axis emission results in an annular beam.
In either case, the minimization of phase mismatch occurs only over a limited region,
both in the propagation and radial directions. Predictions for the far-field harmonic

37
beam proflies have been verified closely through experiment [73].
In any case, maximization of the conversion efficiency of HHG using a free focusing
geometry consists of making the coherence length of the process only at least as longas the width of the interaction region. For a free focus geometry, this width is limited,either due to the width of the gas jet used, the Rayleigh length, or the defocusing lengthof the driving laser beam.
In the case of hollow waveguides, the total phase mismatch caused by the threeterms described above: neutral atoms, free electron plasma, and the guiding in thehollow waveguide, is given by the sum of these terms:∆k = ∆kN + ∆kP l + ∆kW = −P
qu2 λ0
2πq P
δn (1 − η) + qηNatm re λ0+ nm2 , (2.32)
λ0 Patm
Patm
4πa

For a hollow waveguide, the phase correction of the waveguide is the same sign as thefree electron dispersion, in contrast with the Guoy phase.
There are three main advantages to using hollow waveguides over a free focus: thegeometrical phase correction term is constant with propagation distance, the intensity
can be maintained at a high level over a long propagation distance, and the gas may becontained conveniently at a well-defined pressure. The fact that two of the terms of Eqn.
2.32, for the neutral atoms and free electrons, depend on the pressure of the gas, while
the waveguide term does not, indicates the experimental mechanism for phase matching. Pressured-tuned waveguide phase matching of HHG was reported in Rundquist etal., [23] and Durfee et al. [74]. These were the first publications to account for the dispersion of the neutral atoms and free electrons, both of which become significant at even
low pressure and low ionization fraction. Also, this is the first demonstration of truephase matching of HHG, since the geometrical phase shift is constant with propagation
distance. Phase matching could be achieved over a longer propagation distance due tothe “plane wave” nature of the propagation geometry, in contrast with the transientphase matching of Figs. 2.14 and 2.15. Figure 2.16 shows the pressure tuning curves

38
for four different gases along with the predicted behavior. As the pressure is increased,
there is a local maximum in the HHG signal when the phase mismatch is minimized.

Figure 2.16: a) Measured and b) calculated pressure dependence of the harmonic yieldfor several gases. In order of increasing optimum pressure, the curves correspond to
xenon, krypton, argon, and hydrogen. Reproduced from Ref. [74].

The dependence of the harmonic signal on pressure when phase matched is asinc2 , since the phase mismatch is proportional to the pressure (Eqn. 2.24 and Fig.
2.12). However, the measured pressure-tuning curves are broadened in comparison withthe prediction of a sinc2 profile [70]. This is due to absorption of the gas, as well as thebroadening effect of the rapidly changing phase mismatch.
Limits to Phase Matching
There are two major limitations to pressure-tuned phase matching: ionization andabsorption. The above technique of pressure tuned phase matching works by balancing
the contributions to the phase mismatch. The dispersion of the neutral atoms present
cancels that from the free electrons and the waveguide. However, at a critical value

39of the ionization fraction, ηcr , the dispersion from the remaining neutral atoms is notenough to balance the dispersion from the free electrons. This value may be estimatedby equating Eqns. 2.26 and 2.27, and solving for the ionization fraction, η:
−1
λ2 re Natm1
ηcr = 1 + 0
1− 2
2πδn
q

(2.33)

Since both phase mismatch terms are proportional to pressure, the critical ionization is
independent of the pressure. Without the inclusion of the waveguide phase mismatch,
Eqn. 2.33 gives an upper limit for the ionization fraction, since the sign of the waveguideterm is the same as the free electron term. Table 2.1 shows the values of the critical
ionization for the noble gases. The harmonic order quoted is the highest harmonic orderwhich may be phase matched, assuming that the critical ionization is reached at thepeak of a 25 f s pulse of center wavelength 0.8 µm. Ionization fractions were calculated
used the ADK ionization rates (Eqn. 2.3).
Gas Species
He
Ne
Ar

ηcr
0.005
0.011
0.048

Harmonic order
91
69
35

Table 2.1: Critical ionization values for the noble gases, as well as the highest harmonicorder that can be phase matched, generated at the peak of a 25 f s pulse of center
wavelength 0.8 µm.

Once the ionization fraction is higher than critical, the dispersion from the freeelectron density will be the dominant component in the phase mismatch. This leadsin general to a decreasing coherence length with harmonic order, since ever higher
intensities are required to produce higher photon energies, and higher intensities resultin a higher free electron density. The photon energy that can be generated before theionization level reaches critical may be maximized in a couple of different ways. First,
the shorter the driving laser pulse, the greater the probability that the electron will
not be driven from the atom before the peak electric field within the pulse. Since40
ionization occurs discretely at every half cycle, the fewer half cycles there are with
sufficient amplitude for ionization before the peak of the pulse, the less the degree ofionization. This is why “few-cycle” laser pulses are useful for the generation of thehighest photon energies [45, 79]. It is worth noting also that the ADK ionization rates
overestimate the degree of ionization for few-cycle laser pulses, because the field envelopechanges significantly between half-cycle peaks of the field within the pulse. Numericalestimates of this “non-adiabatic” effect can be found in Refs. [11] and [80].
The second method for phase matching higher photon energies works in essentially the same way as the first, by reducing the number of half-cycle peaks within apulse. In this case, the technique is to use a longer wavelength in the driving laser
pulse. Recall that the cutoff photon energy is proportional to the square of the driving
laser wavelength (Eqn. 2.7), making this an advantageous scaling factor [81, 82]. Significant extension of the cutoff energy through the use of long driving wavelength wasdemonstrated in several experiments [81, 83, 84]. The disadvantage is that the electron
spends more time in the continuum during rescattering, lowering the recombination
cross-section. It was recently found both theoretically and experimentally that thesingle-atom yield scales as λ−5.5±0.5 , which greatly reduces the efficiency of HHG driven
by longer wavelengths [85]. Recent experimental and theoretical work has shown that
it is possible to extend true phase matching of the high harmonic generation process
to significantly higher photon energies (in theory up to 1 keV ) using long wavelength
driving lasers [86]. However, the unfavorable single atom yield may limit applicationsof harmonics driven by long wavelength drivers to photon energies around 300 eV , evenwhen perfectly phase matched.
The drawbacks to each of these techniques is the higher degree of technical difficulty in generating the driving laser pulse. Pulse compression techniques for generating
few-cycle laser pulses are improving due to interest in the multiple applications of such
short pulses, but still reduce the overall efficiency. Similarly, generation of intense laser

41
pulses at near- to mid-IR wavelengths require the use of nonlinear optical conversion
techniques that also reduce overall efficiency. Each of these things places higher demandson the base laser system in terms of energy and beam quality.
The high intensities needed for the generation of very high harmonic orders leadto other limits on generating bright emission at high photon energies. Defocusing limits
the interaction length, for a free focus geometry, and can lead to extra loss or theexcitation of higher order modes in a hollow waveguide geometry. Strong ionization
depletes the energy in the driving laser beam, reducing the intensity. Nonlinear opticaleffects, such as the optical Kerr effect, can become quite significant at high intensities,
leading to a reshaping of the ultrashort pulse [87]. Even subtle changes in the phasefront or the local intensity can alter the local phase matching conditions in ways difficult
to predict. The major difficulty with improving conversion efficiency of HHG at highphoton energies is this rapidly varying phase mismatch.
Finally, absorption plays a major role in the maximum obtainable conversion
efficiency. Especially for VUV and EUV frequencies, strong absorption of the harmoniclight becomes the ultimate limitation of the achievable flux. The strong absorption
originates for the same reason that these photon energies are of particular interest: thevalence electrons of many materials are bound with energies of ∼ 10− 100 eV . Constant
et al. [75] calculated that the maximum harmonic yield saturates once the interaction
length is longer than a few absorption lengths, even for perfect implementation of phasematching. The result of their calculation is shown in Fig. 2.17. The overall optimization
conditions predicted by this analysis are:
Lint < 3Labs , Lc > 5Labs(2.34)

This description of absorption-limited harmonic generation has been confirmed experimentally [75, 88]. Figure 2.18 shows the results of such a measurement. Because of
the relationship expressed in Eqn. 2.34, in the case of strong absorption, the phase42matching condition may be relaxed so that Lc is simply much longer than Labs . It isalso worth noting in designing the region of gas density, whether this is a gas jet, or thepressure profile in a hollow waveguide. The absorption length places an upper limit on
the length of the interaction region that will be practical for phase matching.

Figure 2.17: Phase matched HHG photon emission as a function of the propagation distance (in units of the absorption length, Labs ) in the presence of absorption. Reproduced
from Ref. [75].

2.5

Quasi-Phase Matching
When full phase matching is impossible or inconvenient, a reasonable and efficient

alternative is quasi-phase matching (QPM). Originally proposed [89, 90] soon after thedemonstration of nonlinear optical harmonic generation, QPM can drastically improvethe conversion efficiency of harmonic generation through a periodic correction to thephase mismatch. This periodic correction can take multiple forms, but among the mostsuccessful techniques is the use of periodically-poled ferromagnetic crystalline structures [91–93]. In this method, the spontaneous polarization of the crystal is reversed
periodically, inverting the relative phase between the fundamental and harmonic fields.
Ideally, this reversal happens at every coherence length, so that, on average, the phasesof the two fields remain within π radians, the condition for continued coherent addition

43

Figure 2.18: Measured (squares) and predicted (solid curve) brightness of the 61st
harmonic order generated in neon, as a function of propagation distance, showing theeffect of absorption on the conversion efficiency. Reproduced from Ref. [88].

of the harmonic field. Reversal of the polarization at a periodicity of any odd numberof coherence lengths will also improve the conversion efficiency, but scales down with anincreasing number of coherence lengths per period. Figure 2.19 illustrates the harmonic
growth as a function of propagation distance with the application of QPM. The black
curve corresponds to the growth of harmonic signal in a periodically-poled nonlinear
material. The dashed curve illustrates that this signal growth is essentially quadraticwith distance, as in full-phase matching, except scaled by a factor of approximately
π 2 /4 [91].
The red curve describes a slightly different version of QPM. Instead of reversing
the phase relationship at every coherence length, the harmonic emission is suppressed inevery other coherence length. Essentially, the destructive interference which occurs at
every other coherence length is suppressed, and only constructive interference between
zones of similar phase occurs. It may be seen from the figure that the harmonic intensity
achieved after a propagation distance L is the same as that achieved with QPM usingOutput Harmonic Signal

44

Full Phase
Matching

QPM: Periodically
Polarized Crystal

QPM: Periodic Suppressionof Harmonic Buildup
No Phase
Matching

0

1

2

3

4

5

6

7

8

L/Lc
Figure 2.19: Harmonic intensity as a function of propagation distance, in the case of fullphase matching (blue curve), traditional quasi-phase matching with periodically poled
nonlinear crystal (black curve), quasi-phase matching through periodic suppression of
the harmonic signal (red curve), and no phase matching (green curve).

periodic polarization after a propagation distance of L/2.
QPM using a periodically poled nonlinear crystalline structure is not applicableto high-order harmonic generation for the same reason that phase matching using birefringent materials is not applicable: the strong absorption of high harmonic frequencies
by dense media. Several proposals and a few experimental demonstrations of techniquesfor QPM of HHG have appeared since the demonstration of HHG itself. These QPM
techniques involve periodic modulation of either the gas density [26, 30, 36] or the driving laser intensity [27–29, 31, 32, 34, 35]. However, nearly all of these proposals neglect
an important problem specific to QPM of HHG. Quasi-phase matching techniques areneeded mainly for high photon energies that are generated at ionization levels that preclude true phase matching techniques. However, the high degree of ionization leads also
to a rapidly varying phase mismatch that can be difficult to predict. In addition to theionization, propagation effects in the waveguide, such as modebeating, ionization andguiding loss, refraction, and group velocity dispersion lead to a dynamically changing

45
laser intensity in both space and time along the propagation direction of the driving
laser. These changes in turn result in a longitudinally-varying phase mismatch (coherence length). Most of the proposals simplistically assume a constant phase mismatch,which is often not realistic.
Three techniques for QPM of HHG have been successfully demonstrated experimentally to date. In the first approach, the driving laser intensity is varied by modulating the inner diameter of a hollow waveguide, while the gas pressure and laser
intensity are tuned to match the coherence length to the waveguide modulation period [1, 29, 34, 35, 94]. When the intensity is modulated above and below the thresholdfor generating a given harmonic, and the periodicity is matched to the coherence lengthof the process, the process can be phase matched. Figure 2.20 shows a calculation by
Ivan Christov of the harmonic signal as a function of propagation distance. Because of

Figure 2.20: Energy of the 95th harmonic order for a large phase mismatch in the caseof a) a straight, unmodified waveguide, and b) a modulated waveguide. Reproduced
from Ref. [29].

the variation of the phase mismatch with propagation distance, QPM using a modulated

46
waveguide structure only partially compensates for the phase mismatch. As a result,significant enhancements of 1-2 orders of magnitude were demonstrated. Figure 2.21
shows an enhancement of the harmonic signal from neon using modulated waveguides,
at photon energies up to ∼ 284 eV . As can be seen in the figure, the enhancement

Figure 2.21: Measured harmonic emission from neon generated in straight (black curve)
and modulated (red curve) waveguides. Reproduced from Ref. [35].

is broadband, rather than applying only to the cutoff harmonics. It is possible that
QPM is partially achieved for plateau harmonics through modulation of the intensitydependent phase. However, all these improvements are much less than is in principle
possible under full phase matching conditions that coherently combine the emission overextended distances and many coherence lengths.
In analogy to periodic polarization of the nonlinear medium, multiple researchers
have proposed modulation of the gas density as a method for quasi-phase matching of
HHG [26, 30, 36]. Numerical simulations predict large enhancements of the conversion
efficiency, but without a mechanisms for appropriate modulation of the density, experimental demonstrations were not possible. Recently, Seres, et al., [36] demonstrated
this type of QPM by periodic modulation of the gas pressure in a free focus geometry.

47
Enhancement factors of ∼ 4 were achieved at very short wavelengths of ∼ 2 − 5 nm by
optimizing the distance between two regions of high gas density along the axis of laser
propagation. However, the scalability to higher enhancements appears to be limited inthis geometry. The width of the gas jets were comparable to the Rayleigh range of thelaser focus, limiting the number of gas jets that could be efficiently used.

2.6

Hollow Waveguides
Hollow waveguides were the geometry used for all the HHG data presented in

Chapters 3 and 4. This geometry has several advantages over free focusing through a gas
jet or gas cell. First, despite the relative lossiness of hollow waveguides in comparison toother types of waveguides, the guiding mechanism maintains a high laser intensity overa long distance, often several times the typical Rayleigh range of a free focus geometry.
It also counteracts the decrease in intensity due to ionization-induced defocusing. These
two consequences of the guiding maximize the interaction region between the laser field
and the nonlinear medium. As shown above, the waveguide alters the propagation vectorof the fundamental field so that there is effectively a slightly different index of refraction
for a given excited mode of the waveguide. This phase effect contributes to the phasemismatch of the nonlinear generation process which allows a phase matching techniquebased on pressure tuning. As shown in the previous section, quasi-phase matching
can be achieved through modulation of the inner diameter to influence the intensityand phase profile of the fundamental field. Hollow waveguides provide a convenientmechanism for gas management. Since HHG frequencies are readily absorbed by evena low pressure gas, it is imperative to limit the gas density to the region of high laser
intensity, and reduce the density to a moderate vacuum (10−6 torr) elsewhere to allow
propagation of the harmonic beam. Current designs for the hollow waveguide feature
either long (∼ cm) regions of constant gas density, with short (∼ 5 mm) differential
pumping sections at the entrance and exit, or long pressure ramp regions. The small

48
inner bore (∼ 150 µm) diameter of the waveguide guarantees a small conductance into
the larger vacuum system. For a summary of pressure profiles in hollow waveguides, see
Ref. [70]. Finally, the extended interaction region and the plane wave propagation of
the fundamental light in a hollow waveguide facilitate phase matching techniques.
Hollow waveguides differ from the more common optical fiber used in communications in their index profile. Telecom fiber guides light using total internal reflection,in which the inner core of the fiber has a higher index (ni ) than the outer cladding material (no ). Hollow waveguides have the reverse index profile, but when the wavelengthof the light guided is much smaller than the diameter of the inner bore (2a, where a is
the radius), then the light is guided through glancing-incidence reflection from the innerboundary. The following summarizes the description of low-loss mode propagation indielectric waveguides by Marcatili and Schmeltzer [95]. In general, there are three maintypes of modes supported by hollow waveguides:
Circular electric modes: T E0m , in which the field components are restricted
to Eθ , Hr , and Hz .
Circular magnetic modes: T M0m , in which the field components are restrictedto Hθ , Er , and Ez .
Hybrid modes: EHnm , in which all field components may be present.
A linearly polarized, T EM00 Gaussian beam, when coupled into a hollow waveguide, will preferentially excite modes of the hybrid type, specifically the EH1m modes.
Linear polarization is maintained when n = 1. Modes with a linear polarization are also
possible as a linear combination of T E0m and EHnm modes, but are attenuated more
rapidly given the cladding index used in the present work. Inside the waveguide, theamplitude of the field will vary radially as
E1m (r) =

r


r
µ0
.
H1m = J0 u1m
ǫ0a(2.35)

Again assuming that λ ≪ a, as well as that the index of the cladding is real at the

49
propagating wavelength, the propagation constant can be written as:
γ1m = β1m + iα1m ,(2.36)"
 #2π
1 u1m λ 2
β1m =
1−
λ
2 2πa

(2.37)

whereis the phase constant, from which Eqn. 2.30 originates, and!
 u 2 λ2(n2o + 1)
1m
p
α1m =
2π
a3 2 n2o − 1(2.38)

is the attenuation constant. Since the value of u1m increases with m, the mode withthe smallest loss will be the “lowest-order” mode, EH11 , and attenuation will increase
with higher order. Table 2.2 shows the attenuation parameters and phase velocities ofseveral of the hybrid modes. Group velocities are calculated using Eqn. 2.42, defined
below.
Mode
EH11
EH12
EH13
EH14
EH15

1/e Attenuation
313 cm
59 cm
24 cm
13 cm
8.7 cmPhase Velocity
1.00001c
1.00004c
1.00011c
1.0002c1.0003cGroup Velocity
0.999983c
0.999912c
0.999784c
0.999601c
0.999403c

Table 2.2: Attenuation constants, phase velocities, and group velocities for several of
the low-order hybrid modes, for λ = 0.8 µm and a = 75 µm.

Hollow Waveguide Coupling
The coupling of a free space propagating laser beam into a hollow waveguide canbe described by the projection of the incident field profile onto the eigenmodes of thehollow waveguide. For a linearly polarized incident beam, the incident field distribution
can be expressed as:
Ei (r) =∞X

m=1

Cm E1m (r)(2.39)

50
where E1m (r) is given by Eqn. 2.35 and Cm is the coupling coefficient for the mth mode,
given by [96]:
Cm =

r

2 1
π w0

Z a
0

E1m (r)Lm−1



2r 2
w02



exp



−r 2
w02



2πrdr,(2.40)

where Lm−1 is the Laguerre polynomial of the (m − 1)th degree.
In practice, a free-space propagating laser beam is coupled into a hollow waveguideby placing the entrance to the waveguide at the focus of the beam, and choosing theappropriate beam waist in relation to the inner diameter of the waveguide. For mostefficient coupling and lowest-loss propagation in the waveguide, the ideal coupling ofa Gaussian T EM00 mode into a EH11 mode occurs for the beam waist w0 at which∂C1∂w0 = 0. When this condition is satisfied, w0 /a = 0.6435, for which 98% of the energy

is coupled into the EH11 mode.
Modebeating
The excitation of multiple modes in the waveguide is common, either throughcoupling parameters or laser-plasma interactions within the waveguide. Because eachmode has a different phase velocity, the modes present will interfere, resulting in avariation of the intensity with propagation distance. In general, the on-axis intensity
can be expressed as:2

ǫ0 c X
I(z) =Am exp(iγ1m z) ,2 m

(2.41)

where Am is the amplitude of excitation. Figure 2.22 displays the results of a twodimensional analytical model that includes contributions from the first three lowest
order modes, EH11 , EH12 , and EH13 . The energy of the beam is divided among thethree modes: 70%, 20%, and 10%, respectively. Although a higher proportion of theenergy can be coupled into the lowest order mode in practice, this plot illustrates thebasic behavior of the slowly varying intensity modulations that result. The inclusionof only the first few modes shows oscillations of the largest periodicity. The periodicity
from the interference between the EH11 and EH12 modes, at λ = 0.8 µm, in a waveguide51
of inner diameter 150 µm, is approximately 2.2 cm. The periodicity decreases as thedifference in the values of m for the interfering modes increases. In other words, thefastest modulations appear for the interference between the lowest order mode with thehighest order excited mode.

Figure 2.22: Analytically calculated intensity profile of a beam (λ0 = 0.8 µm) propagating through a hollow waveguide (a = 75 µm), including the first three lowest ordermodes.

A numerical simulation, written by David Gaudiosi, of the coupling of a Gaussian beam into a hollow waveguide and its subsequent propagation illustrates the twodimensional intensity profile in the waveguide. Figures 2.23 - 2.25 show the results ofthis simulation for three different coupling parameters: R = 0.6, 0.6435, and 0.7, where
R = w0 /a describes the size of the Gaussian beam relative to the inner radius of the
waveguide. For a waveguide with a = 75 µm, these correspond to w0 = 45, 48.25, and52.5 µm, which were within the typical range of beam waists used for the experimental
work described in later chapters. A beam that is slightly smaller than optimal couples

52
more energy into the EH12 mode, resulting in the strong modulation with periodicity
2.2 cm. Optimal coupling, with 98% of the energy in the EH11 mode, still shows significant modulations in the intensity. The standard deviation of the on-axis intensity,
for a Gaussian beam of peak intensity 9.57 x 1014 W/cm2 , is 26%. A beam slightly
larger than optimal further reduces the appearance of long range modulations, but thestandard deviation of the on-axis intensity fluctuation increases to 38%. This amplitudeof intensity modulations can affect the local phase mismatch significantly.
2

Intensity [W/cm ] x 1014

18
16

−100
14

Radius [um]

−50

12
10

0
8
50

6
4

100
2
0

1

2
3
Propagation distance [cm]4

5

Figure 2.23: Numerical simulation of the intensity profile of a Gaussian beam, λ = 0.8µm, coupled into and propagating in a hollow waveguide with inner diameter 150 µm.
Coupling parameter: R = w0 /a = 0.6.

The above simulations simplistically assume vacuum within the waveguide. This
assumption may be valid for low pressures and small degrees of ionization, but a significant increase in either the neutral density or the free electron density will alter
the intensity profile. Nonlinear effects, such as SPM, will result in a radially varying
phase for the propagating field. Several recent publications deal with the propagationof an intense, ultrashort pulse through an ionizing medium [97], and in a hollow waveguide [87, 98–101]. As discussed above, the free electrons are strongly dispersive and can
defocus the propagating field.

53

2

Intensity [W/cm ] x 1015

2

1.8
−100

1.6
1.4

Radius [um]

−50

1.2
0

1
0.8

50

0.6
0.4

100

0.2
0

1

2
3
Propagation distance [cm]

4

0

5

Figure 2.24: Numerical simulation of the intensity profile of a Gaussian beam, λ = 0.8µm, coupled into and propagating in a hollow waveguide with inner diameter 150 µm.
Coupling parameter: R = w0 /a = 0.6435 (optimal coupling into the EH11 mode).

2

Intensity [W/cm ] x 1015

2

−100

Radius [um]

−50

1.5

0
1
50
0.5
100

0

1

2
3
Propagation distance [cm]

4

5

0

Figure 2.25: Numerical simulation of the intensity profile of a Gaussian beam, λ = 0.8µm, coupled into and propagating in a hollow waveguide with inner diameter 150 µm.
Coupling parameter: R = w0 /a = 0.7.

54
Experimentally, modulations in the intensity of the propagating laser beam translate to modulations in the brightness of the plasma emission, such as those shown in
Ref. [32]. For the waveguide radius used, 150 µm, modulations are commonly observedin the plasma emission with propagation distance with a periodicity of roughly 2 cm.
This is only a qualitative correspondence, since there is a complicated relationship between ionization and intensity, as well as between ionization and brightness of the plasma
emission. However, this modulation is a good indication of the presence of modebeating,even when care is taken to select the correct waist size for optimal coupling. One reason
for this could be the defocusing effect of the free electrons. Long range modulations
occur for a slightly smaller than optimal focal spot size. In this case, the beam is able
to diverge to a greater degree, resulting in a periodic focusing and defocusing. Thiseffect may be mimicked by the presence of defocusing free electrons. The refraction of
the free electrons will also result in a greater coupling of the field into the cladding of
the waveguide, and an increased attenuation of the intensity with propagation.
Another limiting assumption of the above simulations is that they assume a CW
propagation field. In HHG, the propagating field has a limited spatial extent along the
propagation direction due to the short duration of the pulses. Because of the differencein group velocities between the modes, the original pulse will split into multiple pulses,
each traveling at a slightly different group velocity. The group velocity for the hybrid
modes is given by:
vg =



∂β1m
∂ω

−1

"

1
=c 1+
2



u1m .λ2πa

2 #−1(2.42)

Group velocities for the first several modes are listed in Table 2.2. Once the separationof the pulses grows larger than the width of the pulse, the modes will no longer interact.
For example, one can calculate the propagation distance over which the delay between
the EH11 and higher order modes grows larger than the width of the pulse. The modes
EH12 , EH13 , EH14 , and EH15 have a separation of 25 f s from the EH11 mode after a

55
propagation distance of 10.5 cm, 3.8 cm, 2.0 cm, and 1.3 cm, respectively. This effectmay be a partial reason that the spatial coherence of HHG improves with waveguidelength [68]. The EH11 mode has the largest group velocity and will be the first to
encounter the atoms toward the end of the waveguide. In addition to acting as a spatial
filter due to the loss of high order modes, the waveguide’s isolation of the lowest ordermode from other propagating modes may allow a more well-defined spatial phase profile.
These intensity variations can strongly affect the brightness of the harmonic generation process in multiple ways. The local field strength determines the ionization rate,or the single atom strength of the emission. When the amplitude of intensity variationis strong enough, the regions of strong emission will be limited to that where the intensity is sufficient for a significant ionization rate. In the case of strong modebeating, theharmonic emission may be limited to regions of ∼ 1 cm length where the intensity ishigh (see e.g., Fig. 2.22). The intensity variation will also have a strong effect on thephase mismatch. The free electron density is strongly and nonlinearly dependent on thelocal intensity, both in space and in time. The phase of the harmonic emission is alsoquite sensitive to the local intensity, through the intrinsic phase, as described above in
Section 2.2.
Quasi-Phase Matching with Modebeating
Recently, there has been some interest in the use of modebeating intensity variations as a method of quasi-phase matching HHG [31,32,102]. In contrast with modulated
waveguides, the intensity modulations can be established by selection of the appropriate
coupling conditions for excited multiple interfering modes. Pfeifer and Downer [32] show
experimental measurements, as well as numerical models, of the modulation of plasmabrightness due to modebeating between the first two lowest order modes. For the experiment, they use a waveguide of inner radius a = 25.5 µm, and observe a periodicity of∼ 2.6 mm. However, this publication does not examine how the phase mismatch evolves
with the variation of the on-axis free electron density. With such strong modulation of

56
the intensity, the harmonic generation would be limited to the regions of high intensity,and the intrinsic phase would also be modulated. Although not specified, presumably
the mechanism for phase matching would be to choose the periodicity such that thephase of the fundamental was the same for each generation region.
There are several limitations to this type of quasi-phase matching. Like withmodulated waveguides, the intensity profile is fixed by the structure of the waveguide.
For a given inner diameter, the periodicity established by interaction between the twolowest order modes is fixed. Thus tuning of the periodicity to maximize conversion
efficiency is not possible. Shaping of the spatial profile of the incident beam might beused, however, to create a more complex, tunable beating pattern through excitation ofhigher order modes. Such shaping has already been shown to control HHG in waveguides[103]. Second, it is limited in how short a coherence length it may compensate efficiently.
Shorter periodicity may be achieved with a smaller inner radius, but this limits thetotal gas density and thus the absolute photon number achievable. The attenuation
constant, temporal separation of pulses, and phase mismatch also increase with a smaller
waveguide radius.
Hooker and coworkers [31] consider, instead of interference from only the twolowest order modes, a more complex and realistic intensity modulation resulting fromthe interaction of several modes. In this case the intensity modulations of highest frequency are also of much smaller amplitude. They numerically simulate the coherent
growth of the harmonic field, comparing the case of optimal coupling into the lowest
order mode with an incident Gaussian beam with an incident beam of an Airy profile
for which w0 /a = 0.2, coupling more of the laser energy into higher orders. In a subsequent publication [102], an experimental demonstration of bright emission from argon
ions is attributed to quasi-phase matching of the nonlinear process through multimodemodulation of the intensity. However, in neither publication do the authors include theeffect of the presence of gas on the propagation of the laser in the waveguide. This

57
is especially important considering the intensities used, and the fact that they claim
harmonic emission from singly ionized argon. The resulting, substantial free electron
density is considered in relation to contributing to the bulk of the phase mismatch, but
not in relation to how it would affect the on-axis intensity profile. Their own calculations
predict that the ultimate conversion efficiency is quite sensitive to subtle differences in
the intensity profile. Also, no measurements support the claim that multimode beatingis the cause of the increase in conversion efficiency other than the measurement of flux
itself. Considering the complex dynamics which result in a changing phase mismatchin both space and time, the assumption of a constant coherence length is dubious. Recent work [104] suggests that the mechanism for the generation of bright emission, andextension of the observed cutoff to the water window, from argon ions in waveguides isdue to pulse compression [87].

2.7Counterpropagating LightCounterpropagating light can have a substantial effect on HHG in any geometry,

and control of harmonic generation may be achieved through control of the counterpropagating field. The influence of counterpropagating light on HHG was first theoreticallystudied by Peatross and coworkers [27,28], and later developed further by Landreman etal., [105] and Cohen et al., [106]. The principal effect of a counterpropagating field is tosuppress the coherent buildup of the harmonic field by establishing a rapid, stationary
phase modulation. As will be shown in Chapter 4, this process can be exploited to
study coherence properties of HHG in hollow waveguides, as well as to achieve a newquasi-phase matching technique. QPM using counterpropagating light turns out to bea flexible and highly selective tool for enhancement of the conversion efficiency.
Parallel Polarizations
To understand how counterpropagating pulses may suppress harmonic generation,
consider two plane waves of the same frequency and parallel polarization that travel in58
opposite directions. The electric field of the light may be written as:
ET (z, t) = EF exp[i(kz − ωt)] + EC exp[i(−kz − ωt)] = E0T (z) exp[i(kz − ωt + φ(z))],(2.43)
in which EF and EC are the amplitudes of the forward and counterpropagating fields,
respectively, andE0T (z) = EFandp

1 + r 2 + 2r cos(2kz)(2.44)

(2.45)

φ(z) = − arctan

r sin(2kz)
1 + r cos(2kz),r = EC /EF being the field amplitude ratio. Both the field and the phase have atime-independent, sinusoidal variation in the propagation direction, with a periodicityof half the wavelength of the forward or counterpropagating fields. The peak-to-peakamplitude of the phase modulation is given by:∆φ = 2 arctanr√
1 − r2≈ 2r,(2.46)

where the approximation is true for r ≪ 1. Coherent buildup of the harmonic field
will be suppressed when the phase modulation translated to the harmonic field has anamplitude of π or greater. This condition is met when
r=

π
.
2q

(2.47)For large q, it can be seen that the approximation r ≪ 1 is valid, meaning that a counterpropagating field with an amplitude much smaller than that of the forward propagating
field is sufficient to suppress coherent buildup of the harmonic signal. In fact, the higher
the order of the harmonic, the smaller a counterpropagating field required to suppress
its coherent buildup.
In addition to the direct phase modulation of the harmonic driving laser field,
there is an indirect phase modulation through the intrinsic, or intensity-dependent

59
phase. This component arises through Eqn. 2.44, or the stationary modulation of
the intensity. The peak-to-peak variation of the intensity is∆I =p

4IF IC ,(2.48)

with IF and IC as the instantaneous forward and counterpropagating intensities. Combination with Eqn. 2.11 gives the peak-to-peak variation in the intensity-dependent
phase:
2Ke2 IF r.
h̄mǫ0 cω 3

∆φp =(2.49)

While Eqn. 2.47 describes a phase variation of the fundamental field, which then istransferred to the harmonic phase, Eqn. 2.50 describes a direct variation of the harmonic
phase. The dependence on harmonic order enters through the parameter K, which
varies with the release phase as shown in Fig. 2.6. The effect on a given harmonic orderthus also depends on which trajectory contributes. Since the value of K is generally
significantly higher for the long trajectories in comparison with the short, the harmonic
emission from the long trajectories will be suppressed for a smaller value of r, or in otherwords, a lower counterpropagating intensity. An example of such a phase modulationis shown in Fig. 2.26a), displaying the difference in the modulation amplitude between
the two trajectories. The condition for suppressing emission due to modulation of theintensity is when ∆φp = π, or when
KIF r =h̄mǫ0 cω 3.
2πe2(2.50)To show how the harmonic emission may be suppressed by the phase modulations,the microscopic effective emission may be modeled [28, 106]. This is the ratio between
the generated harmonic fields without and with the presence of the counterpropagating
light, for one period of the standing wave, Λ = λ0 /2:
1
ξ=
Λ

Z Λ
0

1
exp[i∆φ(z)]dz =
Λ

Z Λ
0



exp iA cos



2π
z
Λ



dz = J0 (A),

(2.51)

60
in which A is the amplitude of the phase variation and J0 (A) is the zero-order Bessel
function of the first kind. This phase amplitude A is directly proportional to r, the field
amplitude ratio, as can be seen in Eqns. 2.47 and 2.50. Figure 2.26, reproduced from
Ref. [106], shows the effect of a weak counterpropagating pulse on HHG emission, froma calculation using the generalized Lewenstein model [43]. For these calculations, themedium was helium, and the driving laser pulse had a peak intensity of 1015 W/cm2
and a FWHM pulse duration of 20 f s. Figures 2.26a) and b) confirm that the phasemodulation is stronger for the long trajectories compared to the short, and that thephase amplitude A is directly proportional to the field amplitude ratio r. Figure 2.26d)shows the form of the microscopic effective emission factor ξ, illustrating that for thepresence of even a small counterpropagating field, the harmonic emission is effectively
suppressed. Notably, for some values of A, ξ is negative, corresponding to a phase shiftof π in the harmonic phase. This is important for the implementation of QPM using
counterpropagating light, which will be discussed further below.
Perpendicular Polarizations
Harmonic emission may also be suppressed under the influence of counterpropagating light with a polarization that is linear and perpendicular to the forward propagating driving field. In this case, the physical mechanism is different. Rather than creating
a longitudinally varying phase that suppresses the coherent buildup of harmonic signal,
the counterpropagating light lowers the probability of emission itself by creating a sinusoidally varying ellipticity in the driving laser field. As has been described in several
studies of HHG (e.g. Refs. [107–109]), even a slight ellipticity in the fundamental field
will reduce the probability of recombination due to the transverse spread of the electron
wavefunction during rescattering. The advantage of using a perpendicular polarization
for suppression of HHG with counterpropagating light is that it may be attenuated usinga polarizer before it feeds back into the laser system.
The ellipticity induced by counterpropagating light was derived by Landreman et

61

Figure 2.26: Influence of a weak counterpropagating field on the phase of HHG. a)
Example of the intensity-dependent phase modulation, with a different amplitude forthe two trajectories. Amplitude of the phase modulations calculated as a function of
the field ratio, r. c) Amplitude of the phase oscillations for a particular contribution as
a function of emission time. d) Bessel dependence of the microscopic effective emission
factor on the amplitude of the phase modulation. Reproduced from Ref. [106].

al., [105]. In this case, the sum of the electric fields of the forward and counterpropagating beams can be written as:








 1 
 0 
ET (z, t) = EF exp[i(kz − ωt)]   + rEF exp[i(−kz − ωt)]   ,0
1(2.52)

where the vectors represent possible polarization orientations in the 2D transverse plane.
Any two-component complex vector can be expressed in form:
 
 


a
u
v
 
 


  = exp(iφ)   + iǫ 
 ,
b
v
−u

(2.53)

where u, v, φ, and ǫ are real quantities, so that the total electric field can be rewritten

62
as








 u(z)  v(z) ET (z, t) = EF exp[−iωt] exp(iφ(z))  + iǫ(z) 
 .
v(z)
−u(z)

(2.54)The ellipticity of the electric field will evolve with propagation distance, the major andminor axes of the ellipse given by the two-component vectors in Eqn. 2.54, and theellipticity given by ǫ(z). The ellipticity is defined as the ratio of the peak field in the
direction of the minor axis and the peak field in the direction of the major axis, and isgiven byǫ(z) =

1 + r2 +p

1 + r 4 + 2r 2 cos(4kz)
2r sin(2kz)(2.55)

The authors show both theoretically and experimentally that the suppression of HHG
emission generally requires a larger field ratio, r, when using a counterpropagating
field of perpendicular polarization compared to parallel polarization. Their calculations
indicate that the ratio of intensities, IF /IC , needed to reduce the harmonic signal by
50% is roughly 10x greater for the perpendicular polarization when compared to thephase modulation of the fundamental field with a parallel polarization (of the typedescribed by Eqn. 2.47).
Quasi-Phase Matching with Counterpropagating Pulses
Quasi-phase matching of HHG may be achieved by using counterpropagating
pulses to suppress harmonic emission from the out-of-phase coherence lengths createdby the phase mismatch between the fundamental and harmonic fields. As described in
Section 2.5, when the phase mismatch is nonzero, the harmonic signal oscillates witha period of twice the coherence length. The harmonic field increases until the phaseslip between the driving laser and harmonic fields reaches π radians, at which point thesubsequently emitted harmonic field begins to interfere destructively. All-optical QPM
using counterpropagating pulses is implemented by arranging for the overlap region of
the colliding pulses to suppress emission from one or more coherence zones that would
otherwise cause destructive interference (see Fig. 2.19).

63
Peatross and coworkers have shown that counterpropagating light can effectively
suppress the coherent buildup of HHG in free-focus geometries through a gas jet [33,110]
or a gas cell [111,112]. In Voronov et al. [33], efficient suppression of the harmonic signal
was observed over well phase matched conditions. The interaction region consisted ofa ∼ 300 µm wide jet of argon gas, and the experimental conditions were adjusted forhighest harmonic signal near the 23rd harmonic order. The collision region (effective
width ∼ 300 µm) of the driving laser pulse and a counterpropagating pulse of duration
1 ps was scanned through the interaction region by adjusting a delay stage in the
counterpropagating beam line. The results are shown in Fig. 2.27. The harmonic signal
is strongly suppressed.

Figure 2.27: Scan of the collision point of the driving laser pulse with a counterpropagating pulse through a narrow gas jet. The harmonic signal is suppressed strongly inthe presence of the counterpropagating light. Reproduced from Ref. [33].

The authors also demonstrate an enhancement of the harmonic signal for poor
phase matching conditions. The focus was moved away from the gas nozzle to a region
where the gas region is approximately 1 mm wide, drastically reducing the harmonic

64
signal through dephasing. For the given experimental conditions, the authors estimate
the presence of approximately three coherence zones. The scan of the collision region
now results in a restoration of the harmonic signal (see Fig. 2.28) as the destructively
interfering emission is now suppressed.

Figure 2.28: Scan of the collision point of the driving laser pulse with a counterpropagating pulse through a wider gas jet. The poorly-phase matching harmonic signal
is restored through suppression of destructively interfering harmonic emission. Reproduced from Ref. [33].

Similar plots of suppression and restoration of the harmonic signal from neon are
shown in Ref. [112]. In that experiment, the harmonics were generated in a gas cellof several cm, and the counterpropagating pulse had a duration of ∼ 10 ps, (effective
width ∼ 3 mm). Measurements provided a rough estimate of the coherence length overa distance of 1 to 2Lc . However, in all cases, the interaction medium was limited, either
due to the width of the gas jet, the absorption depth of the gas, or the region of sufficientlaser intensity. This ultimately limits the potential enhancement using counterpropagating pulses. While an enhancement of the harmonic signal was observed due to the65presence of counterpropagating light, this enhancement was not an improvement above
other phase matching techniques. Moreover, they were unable to match the width ofthe counterpropagating pulse to the coherence length without the ability to measure
the coherence length.
To implement all-optical QPM efficiently, a train of counterpropagating pulses isneeded to suppress harmonic generation in several selected out-of-phase regions of themedium. Hollow waveguides provide an ideal medium for this technique, since the guiding provides an extended interaction region. A sequence of counterpropagating pulses
can allow significant enhancement of the HHG signal if constructed appropriately. Eachpulse must have the correct width for suppressing the out-of-phase harmonic emission
from one coherence zone, and the sequence of pulses must have the correct spacing forsuppressing consecutive out-of-phase coherence zones, while allowing in-phase zones tocoherently add. Assuming a constant single-atom efficiency and a constant phase mismatch with propagation, the expected enhancement of harmonic intensity for a sequenceof N pulses is (N + 1)2 . However, as will be described in Chapter 4, a varying harmonic
emission efficiency or phase mismatch can lead to significantly higher enhancements. In
addition, it is predicted that for a correct ratio of the forward and counterpropagating
fields, the counterpropagating light can cause an overall phase shift in the harmonic
emission of π radians [106]. In this case, the out-of-phase coherence zone is partiallyconverted to an in-phase coherence zone, further increasing the overall conversion efficiency.
The optimal shape of the counterpropagating pulses for QPM is that which mosteffectively suppresses destructive interference from out-of-phase zones. The overlap region between the counterpropagating and driving laser pulses corresponds to half thewidth of the longer counterpropagating pulse, since the pulses move in opposite directions. In other words, although the counterpropagating pulse may be, for example, 2
ps in duration, with a physical extent of ∼ 600 µm, its overlap region with the forward

66
propagating pulse will be only ∼ 300 µm. This resulting overlap region is referred toas the “effective” width of the counterpropagating pulse. Thus, the optimal counterpropagating pulses will have a square temporal profile with effective width equal to asingle coherence length. The enhancement due to a sequence of counterpropagating
pulses was calculated in Ref. [106] for both a square pulse and a sech2 pulse. This
calculation is shown in Fig. 2.29, which plots the QPM efficiency factor: the generated total harmonic signal with the counterpropagating pulses, normalized to the signal
generated under perfect phase matching. Two parameters were varied in order to findthe optimal pulse shapes: the peak amplitude of the phase modulation, A0 , and theeffective suppression width of the pulse, z0 . From the calculation, it was found thatthe optimal effective FWHM of a sech2 pulse is 0.26Lc , which, along with the optimalphase modulation amplitude, gives a harmonic efficiency factor of 0.14. Because of theextra phase shift of π radians induced by the counterpropagating field at the appropriate
phase modulation amplitude, part of the emission in the out-of-phase zone is shifted to
be in-phase, and adds to the total signal. This gives an efficiency that is 40% larger
than simply completely suppressing the out-of-phase emission.

Figure 2.29: QPM efficiency factor for a) hyperbolic secant and b) square counterpropagating pulses as a function of pulse width and peak phase modulation amplitude.
Reproduced from Ref. [106].

Chapter 3
Characterization of Waveguide High Harmonic Generation

3.1

Introduction
This chapter contains a general description of the laser system, the HHG waveg-

uide setup, and the detection of EUV light. Also included are some selected experimental
results from exploratory work on optimizing the conversion efficiency of HHG in waveguides. Specifically, the measurement and estimation of the photon yield of HHG fromhollow waveguides at 45 eV is presented. Measurements are presented of the energy loss
in the interaction medium within the hollow waveguide, and are compared with a simple
numerical model of energy loss due to ionization. This model appears to account for amajority of the loss of energy in the driving laser beam. Finally, a brief characterizationof the enhancement of the HHG signal from modulated hollow waveguides is presented.

3.2

Experimental Setup
Laser System
The laser source used was a Ti:sapphire amplifier system (KMLabs Red Dragon).

This is a two-stage, multipass, chirped pulse amplification (CPA) system, operatingat 1 kHz, capable of generating pulses as short as 20 f s, and pulse energies as large
as 6 mJ. Although this system is more technically advanced than those described inRef. [7], this reference is a very useful and detailed review, especially for a review of thecomponents and overall design of this type of CPA laser system. The first stage pump

68
laser was an arclamp-pumped, frequency-doubled Nd:YLF laser (Quantronix Falcon)
with a pulse energy of ∼ 20 mJ and a pulse duration of ∼ 150 ns at a wavelength of 527
nm. The first stage of amplification had a multipass (∼ 10 passes) ring configurationof the folded type described in Ref. [113], used to minimized astigmatism. The second
stage was pumped by either a Photonics Industries DM-40 or DM-50: both diodepumped, frequency-doubled Nd:YLF lasers at 527 nm, with a pulse duration of ∼ 150
ns and maximum pulse energies of 40 and 50 mJ, respectively. The second stage of
amplification was a simple two pass configuration.
The front end of the laser system was a Ti:sapphire, Kerr-lens passively modelocked oscillator operating at a repetition frequency of ∼ 90 M Hz.

The prism-

dispersion-compensated laser generated a bandwidth of typically ∼ 150 nm tail-to-tailat a center wavelength of 780 nm, supporting a transform-limited pulse of about 10 f s.
The repetition frequency of the oscillator was reduced to 1 kHz using a Pockels cell.
A second Pockels cell pulse selector, placed before the entrance to the second stage,
limited crosstalk of optical noise between the two stages due to amplified spontaneousemission.
The pulse duration at the output of the amplifier was typically 25 − 30 f s. The
amplifier could be operated with no amplification in the second stage, in which casethe amplified bandwidth typically supported a transform-limited pulse of 20 f s. However, uncompensated high-order dispersion prevented full compression. When the pulse
was amplified further in the second stage, gain-narrowing of the spectrum tended tobroaden the pulse duration as more energy was extracted. At an output of 4 mJ,
the pulse duration was at least 30 f s. The pulse durations quoted were measured using SHG-FROG [114]. The output mode of the amplifier was characterized througha measurement of M 2 , using a Spiricon M2 Beam Propagation Analyzer. Typical M 2
values were ∼ 1.1 without amplification in the second stage, at about 1 W total power,
increasing to ∼ 1.3 at 4 W total power.

69
The laser beam was coupled into the vacuum system through a thin (250 µm),
anti-reflection coated sapphire window, with a clear aperture diameter of approximately
1 cm. The window was located between the focusing optics of the beam and the entrance to the waveguide, as far from the focus of the beam as possible without clipping
the beam. This configuration minimized the accumulation of nonlinear phase, or “Bintegral” [7], which would distort the phase front of the beam. The beam was focusedwith a curved mirror at near normal incidence, mounted on a translation stage for optimization of the coupling into the waveguide. A curved mirror was used, rather than alens, to avoid further dispersion that would lengthen the duration of the ultrafast pulse.
Capillary Waveguide Setup
The guided-wave geometry for HHG has been shown in previous work [23, 74] toprovide certain advantages over the gas jet or gas cell geometries. Since EUV and soft
x-ray frequencies are strongly absorbed by bulk material, HHG beams must propagate
in a vacuum of ∼ 10−4 torr or lower for a typical beam path of a few meters. Hollow
core waveguides are a convenient vehicle for maintaining a constant pressure of dilutegas within a limited region, with short differential pumping regions that prevent reabsorption of the HHG photons. Although a hollow waveguide is more lossy than the
more familiar step-index telecom fiber, the guiding properties of the capillary waveguide
maintain the high intensity necessary for HHG over an interaction distance longer thanis possible in a free-focus geometry. Finally, as described in Chapter 2, the guiding properties of the capillary result in a constant phase correction of the driving laser beam,
which may be exploited to phase match the nonlinear HHG process.
Two suppliers were used for the hollow waveguide, or capillary, employed in thework here: Wilmad Glass Co., Inc. or Polymicro Technologies, LLC. The cladding
material is fused silica, with an outer diameter of 1.2 mm and an inner diameter (ID)ranging from 100 − 400 µm. For the majority of data presented (and unless indicatedotherwise), 150 µm ID capillary was used. Until around April of 2005, the hollow

70
waveguides were mounted using an outer capillary to hold three separate sections ofcapillary. Variations in the inner bore of the outer capillary, as well as the relativeorientations of the three segments of waveguide, resulted in significant variations in the
coupling conditions and loss. In 2005, a modular, custom-designed, vacuum fixture wasdevised that holds the waveguide very straight using a v-groove design to minimize
bending. The v-groove setup is designed to hold a single section of capillary, into which
gas is injected through laser-drilled holes. This has resulted in much better coupling
efficiencies and much more reproducible results. For more details on the v-groove andquantitative comparisons of the two designs, please see Ariel Paul’s PhD Thesis [1].

Figure 3.1: 3D rendering of the components of a v-groove vacuum fixture for mounting
the hollow waveguides. Reproduced from [1].

Depending on the length of the central v-groove section, the waveguide mount
can accommodate total waveguide lengths from 1.5 − 20 cm. Waveguide lengths for71data presented in this thesis include 3.5, 6, and 11 cm total length, sometimes referred
to as 2.5, 5, and 10 cm waveguides, respectively. The latter refers to the length ofthe constant-pressure section. Each waveguide also has two 5 mm sections used for
differential pumping. With the development of the new v-groove apparatus and theability to drill holes into the capillary for introducing gas, waveguides have since been
produced as one piece, leading to the extra 1 cm of length. Gas is delivered into thehollow bore of the waveguide through small holes drilled into one side of the capillaryusing a focused CO2 laser beam. Gas input blocks attach to the v-groove block, sealingover the hole in the waveguide to prevent contamination of the gas.

Figure 3.2: Image of a laser-drilled hole in the side of a hollow waveguide, used for gas
delivery. The apparent tapering of the inner bore of the waveguide is a refraction effectdue to the deformation of the outer surface of the waveguide. Reproduced from [1].

Modulated waveguides were constructed using a finely-tuned glassblowing lathe
apparatus, in conjunction with a CO2 laser. Details of this apparatus as well as examples

72
of its capabilities can be found in Ref. [1]. Smooth modulations are introduced to theinner diameter of the waveguide by focusing the CO2 laser beam, at wavelength 10 µm,
onto the capillary spinning in the lathe. The hollow core of the waveguide is kept at agauge pressure of 50 − 100 torr, so that as the fused silica softens, it is pushed outward
slightly. This technique can create smoothly varying modulations in the waveguide up
to a few % of the inner diameter. The same apparatus is used, under slightly different
focusing conditions and while the waveguide is stationary, to ablate the fused silica tocreate the gas delivery and pumping holes. Figure 3.2 shows a magnified image of alaser-drilled hole in the side of a waveguide. The hole is roughly the same diameter as
the inner diameter of the waveguide, 150 µm. The apparent tapering of the inner boreof the waveguide is simply a refraction effect due to the deformation of the outer surfaceof the waveguide. In fact, the inner bore of the waveguide is minimally altered, as was
confirmed by examination under a microscope.
For the HHG described below, the nonlinear media were the noble gases: helium,
neon, and argon, with 99.995% purity. The pressure of the gas introduced to the waveguide was controlled using either an electronic MKS Instruments Model 640A pressure
controller – for ranges of pressure 1 − 110 torr, or a Siemens sub-atmospheric pressure
regulator (Model 43-20L) and constant differential relay (Model 63A) – for pressures
ranging from 2 torr up to several hundred torr. Backing pressures for the exhaust weretypically 10−2 - 10−3 torr, provided by roughing pumps of either oil or scroll pumpdesign. Swagelok or Swagelok Ultratorr fittings were used for the vacuum connections
for the gas lines, roughing pump lines, and between the tubing in the vacuum system.
The noble gas was injected into the waveguide through laser-drilled holes at varying
locations in the waveguide. Typically, the pressure profile was constant through the
majority of the waveguide, with a ramp down in the 5 mm on either end of the waveguide. However, in several cases, the pressure was injected only at the entrance, only atthe exit, or even only at some location in between, creating a pressure ramp profile in

73
the waveguide. The gas profile that was used will be indicated for data in this and thefollowing chapter.
Coupling of the laser beam into the fiber was accomplished by adjustment of theorientation of the fiber, rather than the laser beam. This ensured that the alignment of
the laser into the EUV spectrometer, and hence the co-propagating HHG beam, was notaltered. The waveguide vacuum setup is supported on either side between clamps rigidly
attached to two x-z translation stages, allowing horizontal and vertical adjustment ofeach end (see Fig. 3.4).
Detection of EUV
For nearly all measurements presented in this thesis, with the exception of thephoton yield measurements, the EUV and soft x-ray light was characterized using a
Kirkpatrick-Baez imaging, flat-field spectrometer (Hettrick Scientific) with an EUV and
x-ray sensitive CCD camera (Andor Technology, model D0420-BN). The spectrometerconsisted of two grazing incidence (∼ 2 − 3◦ ), first surface gold coated, cylindricallycurved mirrors, and a grazing incidence gratings. Two spectrometers were used: theolder model spectrometer used contained both constant linespace and varied linespace,or survey, gratings, to allow efficient diffraction of wavelengths ranging from ∼ 10 − 300
Å. The newer model spectrometer used only survey gratings. The survey gratings were
designed to have efficient (∼ 0.1) first-order diffraction over a large range of wavelengths.
The gratings were labeled A, B, and C, or SA, SB, and SC (survey gratings) corresponding to rough wavelength ranges of 10 − 30, 30 − 90, and 90 − 270 Å, respectively. Figure
3.3 shows the first order diffraction efficiency for replicas of the newer spectrometer’ssurvey gratings, supplied by Hettrick Scientific. The spectrometer included the capability for adjusting the angle of incidence of the gratings, so that the camera could
remain stationary while the grating could be tilted for detection of zero-order reflection
vs. first-order diffraction, etc. Alignment of the spectrometer was accomplished while
vented (at atmospheric pressure) using the IR laser light. The laser beam was aligned

74First Order Diffraction Efficiency

0.25

SA1
SB1
SB2
SC1

0.20

0.15

0.10

0.05

0.00
7

8 9

2

3

4

5

6

1

7

8 9

2

10
Wavelength [nm]Figure 3.3: Comparison of the absolute first order diffraction efficiencies of the survey
gratings, measured from replicas of the gratings used in the spectrometer. Incidence
angle for these measurements was 88.75◦ .

to the grid of the optical table for repeatability, and the orientation of the spectrometer
was adjusted manually to the laser beam and clamped into place. The CCD camera wasmounted on an x-y translation stage so that the plane of the CCD could be adjusted
to the image plane of the spectrometer. The CCD chip had a resolution of 256 x 1024,
pixel size 26 µm, with the long side oriented vertically, along the diffraction axis.
The vacuum was maintained at a level of 10−6 torr (with no gas load present)
using one 50 L/s (near the exit of the fiber) and one 17 L/s (at the spectrometerchamber) turbomolecular pump (Leybold and Pfeiffer), backed using scroll roughing
pumps (Varian). The total propagation length of the vacuum line was determined by
the imaging parameters of the spectrometer. The space between the waveguide setup
and the spectrometer chamber was frequently used for plunger feedthroughs, which
could accommodate anything from metal foil filters to mirrors to apertures. A series ofPlunger
FeedthroughTurbo.
Pump

75
Spectrometer

Metal Foil
Filter Wheels

Valve

CCD Camera

Waveguide
Setup
Mirrors
Gratings

Waveguide

Turbo.
Pump

X-Z Translation Stages

Figure 3.4: Experimental setup for generation, propagation, and detection of HHG
under vacuum.

filter wheels [1] were located between the spectrometer chamber and the CCD camera
for attenuation of all but the EUV and soft x-ray light incident on the camera. Figure
3.4 shows a schematic of the vacuum propagation and detection line, as well as an inset
showing detail of the waveguide setup.
Thin metal foils were used as bandpass filters to allow detection of the harmonic
signal while attenuating the co-propagating, intense driving laser beam. These were
mounted either in a plunger vacuum feedthrough, or a vacuum filter wheel that could
accomodate up to three different filters. Two filters were used for full attenuation of thedriving laser, since often there were small holes in the filters. Attenuation of the laser
was especially important when using either the CCD camera or the vacuum photodiodefor detecting harmonic intensities. At the extreme laser intensities, saturation of thedetectors or even optical damage is possible.

3.3

Absolute Harmonic Photon Yield
As a basis of comparison for the available photon yield from HHG by other re-searchers, the absolute photon yield at 45 eV was estimated using the laser systemand hollow waveguide setup described above. For relatively high photon rates (> 109
photons/sec), the measurement was accomplished using a NIST Al2 O3 vacuum pho-

76
todiode (serial no. 397) [115]. A basic schematic of the diode is shown in Fig. 3.5.
Incident radiation generates photoelectrons from the aluminum oxide surface, that are

Figure 3.5: Schematic of the detection circuit of the Al2 O3 NIST vacuum photodiode.

then accelerated to an anode ring held at a bias relative to ground. The resulting current
is proportional to the rate of incident photons for a given photon energy. The quantum
efficiency of the diode was measured in 2005, and the calibration is shown in Fig. 3.6.
Because both the quantum efficiency and the expected photon rates are so low, theexpected currents are on the order of pA to nA. Such a small current can be measured
using an electrometer (Keithley, Model 6517), with care taken to eliminate noise sources.
The experimental setup for measuring absolute photon yield is shown in Fig. 3.7. The
triaxial cable connecting the terminals of the diode to the electrometer was shielded
within the chassis for the bias circuit and a braided shielding cable. Careful attention
was paid to grounding the shielding as well as the appropriate places in the circuit toprevent a floating ground. A bias of 65.5 V was supplied using batteries to introduce
minimal electrical noise. While measurements were conducted, all cables were held
stationary to reduce triboelectric effects, caused by friction between the conducting
wire and the surrounding insulator [116]. Noise measurements conducted using these77
Quantum Efficiency [electrons/photon]

0.18
0.16
0.14
0.12
0.10
0.08
0.06
0.04
0.02
2

3

4

5

6

7

8

10

9

2

100
Photon Energy [eV]

Figure 3.6: Quantum efficiency of the Al2 O3 NIST vacuum photodiode, serial no. 397.
Measured June 2005.

shielding precautions indicated that the electronic noise was reduced to approximately±0.05 pA when sampled at a frequency of ∼ 1 Hz, however, longer scale drifts occurredon the order of 30 min., causing a variation in the current of 0.5 pA. Even this drift
amplitude was smaller than the standard deviation of the measured data, typicallyseveral pA. As an indication of the lower limit of the photon yield measurement, ameasured current of 1 pA corresponds to a photon yield of 108 photons/sec at a photon
energy near 45 eV .
Thin metal foils were used as a bandpass filter in order to limit the region ofemission measured, especially to attenuate the intense driving laser beam. Although
the vacuum photodiode is normally non-responsive to visible radiation, at the highintensities used here, multiphoton ionization or optical damage could result.
The combined transmission of argon and the Al filter permitted a bandwidth near
45 eV including about 5 bright harmonic orders. A rough calibration of the transmission

78

Bias Circuit
Plunger
Feedthrough(Filters)

To Electrometer
Diode
FeedthroughWaveguide
Setup
Valve

Figure 3.7: Experimental setup for photon yield measurement.

of the 150 nm aluminum filter indicated that it transmitted about 10% of the harmonicenergy. The total harmonic yield was measured as a function of pressure for several input
intensities, shown in Fig. 3.8. The energies listed in the graph indicate the transmitted
pulse energy through the waveguide when under vacuum. Error bars in the plots show
the standard deviation of the data averaged for each pressure. Each of these curves isbroad, especially compared to the phase matching curve for argon from Ref. [74] (Fig.
2.16). The diode will detect the entire bandwidth transmitted by the aluminum filter.
Since different harmonic orders are phase matched at different pressures, the maximum
photon yield curve will be broadened with pressure.
The highest photon yield occurs for a higher pulse energy than expected. For a
23 f s pulse, the critical ionization for phase matching of argon occurs at the peak of
the pulse with an energy of 250 µJ. In this situation, the waveguide and free electron
dispersion are balanced with the neutral gas dispersion, allowing pressure tuned phasematching. However, the highest photon yield, more than twice the yield under phasematching conditions, was found for an input energy of 1.07 mJ. Here, phase matching
happens on the rising edge of the pulse. The higher flux in this case may be due

791640 µJ
1070 µJ
510 µJ
298 µJ
192 µJ
125 µJ

1000

Current [pA]

800

600

400

200

0
20

40
60
Pressure [torr]

80

100

Figure 3.8: Current measured from a vacuum photodiode as a function of pressure, forseveral different input pulse energies.

to a larger spatial volume of emission, since there is more energy in the pulse. Pulse
compression was also observed at higher pulse energies [87,117], which could allow phasematching at a higher ionization rate.
The fact that the peak current for every pulse energy, except the highest (1640µJ), occurs at roughly the same pressure could indicate one or both of the following
mechanisms. First, phase matching could occur always at the ionization just below
critical. For this ionization fraction, phase matching will be observed at the same peakpressure that minimizes the phase mismatch. As the pulse energy increases, phasematching will occur earlier and earlier in the pulse, before the ionization fraction israised above critical. Second, the decrease at high pressures occurs due to reabsorption
by the argon gas medium. For the highest energy, the falloff occurs at a lower pressure.
This could indicate that the limiting mechanism is energy loss, described in further

80
detail in the following section.
Estimation of the harmonic yield at 45 eV was relatively straightforward. The
current was scaled by three factors: the Al filter transmission (0.1 ± 0.05), the quantum
efficiency of the diode at 45 eV (0.050 ± 0.003), and since five harmonic orders werevisible with similar brightness, another factor of 5 ± 1. The photon yield is given by:yield =

current≈ 2 ± 1 x 1011 photons/sec
eQEtAl 5(3.1)

where e is the electron charge, QE is the quantum efficiency of the diode at 45 eV,
and tAl is the transmission of the Al filter at 45 eV. This corresponds to an energyof ∼ 2 nJ/harmonic/pulse. Given a driving pulse energy of ∼ 1 mJ, the conversion
efficiency is approximately 2 x 10−6 . In comparison, phase matching at the peak of thepulse occurs for a pulse energy of 298 µJ. In this case, given the peak diode currentof ∼ 450 pA, the photon yield is 1.1 ± 0.5 photons/sec, and the conversion efficiency isapproximately 3 x 10−6 . A more accurate estimate of the photon yield would require
the use of energy-selective EUV optics.
In the past, phase matching was investigated only at low pulse energies, for which
the ionization level remained low throughout the duration of the pulse. In this case,
phase matching could occur near the peak of the pulse. When harmonics are generated using high pulse energies, the gas may be fully ionized. In this situation, thecharacteristic harmonic spectra are quite different. To further illustrate the behaviorof the harmonic emission generated at such a high pulse energy (∼ 1 mJ), harmonic
spectra were recorded concurrently with a measurement of the photon yield. The diodecurrent as a function of pressure is shown in Fig. 3.9e) along with selected spectra(Figs. 3.9a)-d)) recorded at corresponding experimental conditions. For these data, thepower recorded exiting the waveguide when under vacuum was 990 mW , and the pulse
duration was ∼ 20 f s.
One of the features of the diode current data in Fig. 3.8 noted above is the

81

0.10
2500

0.08

2000

0.06

1500

0.04

1000

0.02
0.00

500

30

40 50 60 70 80
Photon energy [eV]

55 torr
Ar + AlCounts

3000

0.10
2500

0.08

2000

0.06

1500

0.04

1000

0.02
0.00

500

30

40 50 60 70 80
Photon energy [eV]

3000

0.10
2500

0.08

2000

0.06

1500

0.04

1000

0.02
0.00

500

30

40 50 60 70 80
Photon energy [eV]

d)
0.14

3500

65 torr
Ar + Al

3000

0.12
0.10

2500

0.08

2000

0.06

1500

0.04

1000

0.02
0.00

500

30

40 50 60 70 80
Photon energy [eV]

600
3500

Diode
Spectrometer

500

3000

400
2500

300
2000

200

th

Current [pA]

0.12Counts at peak of 27 harmonic order

e)

0.12

35 torr
Ar + AlGas and Filter Transmission

0.14

3500

Gas and Filter Transmission

c)

0.14

3500

Counts0.12b)CountsCounts3000

0.14

Gas and Filter Transmission

15 torr
Ar + Al3500

Gas and Filter Transmission

a)

1500

100
1000

0
20

40

60

Pressure [torr]

80

100

Figure 3.9: e) Current measured from a vacuum photodiode and counts from a CCD
camera measured at the peak of the 27th harmonic, as a function of pressure. For
several of the pressures, indicated by arrows, the spectra are plotted (a)-d)), along withthe transmission of the gas and filters used.These data were generated at a high pulse
energy of 990 µJ, for which argon is fully ionized.

82
fact that the pressure tuning curves are quite broad. Plotted in Fig. 3.9e) along withthe diode current is the number of counts recorded at the peak of the 27th harmonicorder as a function of pressure. This provides a comparison of the photon yield for all
harmonics detected with the photon yield for a single harmonic. Figure 3.9e) showsthat the pressure tuning curve for a single harmonic order is narrower than that for all
the harmonics together. While the diode current peaks at a pressure of 35 torr, the27th harmonic, as detected by the CCD camera, peaks at 55 torr.
The harmonic spectra generated using a high pulse energy are also qualitatively
different than the spectra generated with a low energy, such as those presented inprevious work (i.e., Ref. [70]). The red curves in Figs. 3.9a)-d) show the transmissionof the Al filter used in addition to the transmission of argon at the pressure used. For
lower pressures, photon energies are generated over the entire observable bandwidth of∼ 35 eV up to the Al absorption edge at 72 eV . The absorption depth at low pressures
is long enough to transmit a significant amount of energy. Pulse compression has also
been observed at high pulse energy combined with low pressure [87, 117], which canallow the generation of high photon energies. At higher pressures, however, the strong
emission is limited to photon energies below 55 eV . In this case, energy loss may preventthe generation of high photon energies. The pressure of the brightest emission from the27th harmonic order is higher than the predicted phase matching pressure. However,neglecting phase matching effects, the brightness of the harmonic emission depends on
the square of the pressure. This, in combination with the smoothing effects of higher
absorption could result in an optimal pressure higher than that predicted by the phasematching equation.
The spectra also appear to cover a continuum, rather than exhibit well-separated
peaks. This could be due to self-phase modulation from the generation of a plasma,
which broadens the driving laser spectrum and hence the harmonic spectrum as well.
Also easily possible is the presence of non-adiabatic blue-shifting. Since the argon is

83
fully ionized by the peak of the pulse, the emission is likely from the leading edge of thepulse, where the intensity is changing rapidly.

3.4

Ionization Loss
Loss of intensity in the driving laser beam is one of several effects that limit

the total harmonic intensity achievable. One of the loss mechanisms, common to bothfree-focus and hollow waveguide geometries, is ionization loss. Because of the necessary process of photoionization that occurs during HHG, some of the laser energy istransferred in creating a plasma. Since this mechanism should depend on gas species,
density, and intensity, the transmission of several waveguides were measured as a function of pressure and for a few intensities and gases. Ionization loss was also simulatedusing a simple numerical propagation code, the results of which are compared to thedata.
Figure 3.10 shows the measured output of a 3.5 cm total length waveguide as afunction of pressure for three different gases and three different input powers. The gaspressure was constant at the value indicated for the central 2.5 cm of the waveguide,
and the 5 mm segments on either end were used for differential pumping. The input
power is indicated for each graph. (Figure 3.11 shows the same for a 11 cm total
length waveguide.) The input power was measured before the vacuum window, and theoutput power was measured after reflection from a silver mirror mounted in a vacuum
feedthrough, and transmission through a second, uncoated glass window. A densityindependent loss originates from these reflective and transmissive optics.
The ionization loss simulation models the amount of energy lost to ionization
using the ADK ionization rates (Eqns. ??). The code was a 2D propagation code, inwhich the energy was assumed to be distributed radially in the EH11 mode. The intensity was calculated for an array of annular segments. For each radial intensity value,
the ionization fraction was calculated. The number of atoms was determined from the

84density and the volume of the annular segment for a small propagation increment. For
each atom, an energy equivalent to the ionization potential plus the ponderomotive potential (Ip + Up ) was subtracted from the pulse energy. A new intensity was calculated
and then applied to the next propagation segment, etc., for the full length of the waveguide. Because the initial intensity was highest on-axis, the highest ionization rate andtherefore the highest loss was also on-axis. The final output power was determined bysumming the energy over the radial direction after propagation.
The ionization loss simulation does capture some of the significant elements of
the loss as a function of pressure. The density-independent loss was neglected by fixing
the incident power to that measured at the exit of the waveguide under vacuum. Higher
loss was measured for the gas species with a smaller ionization potential, as expected.
For helium and neon, the loss is relatively constant with pressure, however, with argon,
the loss is very sharp at first, then levels out at higher pressure. This is reproduced
and explained well by the simulation. What happens is that at low pressures, the gas
is fully ionized throughout the waveguide. In this case, an increase in pressure simply
results in more atoms to ionize, leading to a sharp loss with propagation distance. At
some pressure, the rate of loss will be high enough that the intensity is reduced to apoint where the ionization is less than 100% before the pulse reaches the end of the
waveguide. After this point in the waveguide, the loss with further propagation is lessrapid. The loss then levels out and changes only slowly with pressure. For example, inthe data of the center plot of Fig. 3.10, at the beginning of the waveguide, with a powerof 1.05 W and a pulse duration of 25 fs, the total ionization fractions are: helium: 4.5%,
neon: 35%, and argon: 100%.
Although it appears to account for a large fraction of the density-dependent loss,
the ionization loss simulation decidedly underestimates the loss in each case. One of
the mechanisms for the loss of energy is due to coupling of the light into the cladding
material of the waveguide. The attenuation of energy from the excited modes of the

85
1.4

Power [W]

1.2
1.0
0.8
0.6
0.4

HeliumNeon

0.2

2.50 W in

0.0
0

20

40
60
Pressure [torr]

80

100

80

100

80

100

1.0

Power [W]

0.8
0.6
0.4

Helium
Neon
Argon

0.2
0.0
0

20

1.75 W in

40
60
Pressure [torr]

0.30

Power [W]

0.25
0.20
0.15
0.10

Helium
Neon
Argon

0.05

0.52 W in

0.00
0

20

40
60
Pressure [torr]

Figure 3.10: Measured output power from a 3.5 cm length waveguide, inner radius 150µm, as a function of gas pressure, for three different gases (open circles) and threedifferent input powers (individual plots). Repetition rate of the pulses was 1 kHz. Gas
pressure was constant at the value indicated over a distance of 2.5 cm in the waveguide,with 5 mm differential pumping sections on either side. Solid curves show the resultsof a simulation of ionization loss.

86

Power [W]

1.0
0.8
0.6
0.4

HeliumNeon

0.2

2.53 W in

0.0
0

20

40
60
Pressure [torr]

80

100

80

100

80

100

Power [W]

0.8

0.6

0.4

0.2

Helium
Neon
Argon

0.0
0

1.70 W in
20

40
60
Pressure [torr]

0.30

Power [W]

0.25
0.20
0.15
0.10

Helium
Neon
Argon

0.05

0.51 W in

0.00
0

20

40
60
Pressure [torr]

Figure 3.11: Measured output power from a 11 cm length waveguide, inner radius 150µm, as a function of gas pressure, for three different gases (open circles) and threedifferent input powers (individual plots). Repetition rate of the pulses was 1 kHz. Gas
pressure was constant at the value indicated over a distance of 10 cm in the waveguide,with 5 mm differential pumping sections on either side. Solid curves show the resultsof a simulation of ionization loss.

87
waveguide depends on specific mode. This attenuation is described in Chapter 2, andthe attenuation distances for several modes are listed in Table 2.2. Another unavoidable
mechanism is coupling loss at the entrance to the waveguide. These two mechanisms
cannot account, however, for the discrepancy between the ionization loss model and theloss measurement. Neither is dependent on the pressure of the gas within the waveguide,and so they instead account for the reduction of energy present when the waveguide is
at vacuum.
Ionization-induced defocusing is likely the density-dependent loss mechanism nottaken into account by the simulation. First, at high pressures, residual gas may bepresent in the region just in front of the entrance to the waveguide, due to inefficientpumping. Ionization in this region will reduce the coupling efficiency into the waveguide.
Inside the waveguide, ionization-induced defocusing causes the driving laser light either
to refract strongly into the cladding material, or to couple into higher order modes
which are attenuated more quickly. In fact, especially for high pressures, ionizationinduced blueshifting is clearly evident in the shifting of the laser beam to higher, visible
frequencies. Coupling of light into the cladding is visible under these conditions, anda portion of the beam exiting the waveguide is highly divergent. In the experimental
setup used for measuring loss, the steering optics aperture the exit beam, so that someof the energy does not reach the power meter detector. This also explains why thesimulations appear to agree more closely with the data for the shorter waveguide.
Some of the assumptions inherent to the code will result in an underestimateof the ionization loss. First, the code calculates free electron density only from single
ionization. When the singly ionized population is high early in the pulse, there is apossibility for multiple ionization, which will reduce the beam energy further. This will
only reasonably effect situations where the ionization fraction is very high. The codealso assumes the propagation of only the lowest order mode. The intensity fluctuations
that result from mode beating can also alter the rate of ionization loss.

88
The maximum possible harmonic yield will depend strongly both on the transmission of the waveguides and the absorption depth of the gas. For the first case, Fig.
3.12 shows an interesting correlation between the density-dependent loss of the waveguide and the measured flux. For these data, a low pulse energy of ∼ 300 µJ was used,
so that phase matching will occur near the peak of the pulse, and so that ionization
loss is not too rapid. Figure 3.12a) shows the measured transmission as a function ofpressure in 3.5 cm and 11 cm waveguides. Figure 3.12b) shows the diode current measured through a 200 nm thickness aluminum filter under corresponding experimental
conditions. A pressure tuning curve is evident for both waveguides. However, for the
11 cm waveguide the peak of the curve is at a very low pressure, while for the 3.5 cm
waveguide, the peak is at the expected phase matching pressure. It is interesting tonote that the beginning of the decrease in photon yield is located at the pressure that
results in the same fractional transmission (∼ 32%) for both waveguides. This suggeststhat energy loss with increased pressure in the longer waveguide overcomes the increasein brightness due to phase matching effects.
Absorption, of course, also plays a major role, especially for photon energies
around 50 eV , which are strongly absorbed by argon. The data in Fig. 3.12b) areconsistent with the predictions of Constant et al. [75], as outlined in Eqn. 2.34. Recall
that maximum conversion efficiency occurs when the interaction region is > 3Labs . Near
the phase matching pressure of 45 torr, the absorption depth of argon at 50 eV is Labs ≈0.9 cm. This corresponds well to a waveguide with a 2.5 cm constant pressure region.
The peak in photon yield for the 11 cm waveguide occurs at 20 torr. Here, the absorption
depth of argon at 50 eV is Labs ≈ 2 cm. However, energy loss in the waveguides, evenat the low level of ionization present for these data, will establish an upper limit to thelength of the waveguide that will produce bright, phase matched HHG. The analysis byConstant assumes that the generation of harmonics has a constant strength throughout
the interaction region. However, in practice, it is clear that in the presence of loss, the89harmonic production is shut down after a given propagation distance. This could explain
why high pulse energies produce a higher flux, since sufficient energy is maintained overa longer propagation distance.

Transmission [Pout/Pin]a)
2.5 cm
10 cm

0.50

0.40

0.30

0.20
0

20

40
60
Pressure [torr]

80

100

Current [pA]b) 5002.5 cm
10 cm

400
300
200
100
0
0

20

40
60
Pressure [torr]

80

100

Figure 3.12: Correlation between loss and harmonic photon yield. a) Measured transmission from 3.5 cm and 11 cm total length (2.5 cm and 10 cm constant pressure regions)as a function of argon pressure. b) Corresponding measured diode current. Input power
was ∼ 300 mW , corresponding to an ionization low enough to allow pressure-tuned
phase matching.]

90

3.5

Modulated Waveguides
As discussed in Chapter 2, quasi-phase matching using a hollow waveguide with amodulated inner diameter is achieved through a periodic modulation of the intensity [29].
In this scheme, the cutoff photon energies are generated only in the regions of highest
intensity. When this periodicity is matched to the coherence length, the conversion
process can be quasi-phase matched. Figure 3.13 shows a schematic of the modulated
waveguide design used in the experimental demonstration of QPM.

Figure 3.13: Schematic of a hollow waveguide with a modulated inner diameter, including typical physical parameters.

Among the first measurements made using the new and more reproducible vgroove mounting design were a measurement of HHG yield using modulated waveguides.
In previous work [34, 35], enhancements of around 1 to 2 orders of magnitude of thephoton yield, over a broad range of photon energies were demonstrated. However,while these initial measurements showed great potential for enhancement of HHG athigh photon energies, it was unclear how the enhancement depended on the specificwaveguide characteristics. Systematic measurements were impossible until the use of

91
the v-groove mount, since there was a large variation between individual waveguides.
Using the v-groove setup, previous results were subsequently reproduced. Figures 3.14
and 3.15 show typical enhancements seen for HHG in helium and neon, respectively.
2500

HeliumCounts [a.u.]

2000

Modulated
fiber
1500

1000

C edge500
Straight fiber

0
2

4

6
Wavelength [nm]810Figure 3.14: Data showing enhancement of HHG in helium through QPM using modulated waveguides.

The experimental parameters for the data in Figs. 3.14 and 3.15 were as follows.
For data collected in helium, a 6 cm waveguide was used, with a constant pressure of 10
torr throughout the waveguide. Modulations of depth ∼ 1.5% of the inner diameter andperiodicity 0.5 mm extended through the final 1 cm before the exit of the waveguide.
The input pulse energy was ∼ 1 mJ. The harmonic emission was detected using the
SB grating, and was transmitted through 400 nm thickness Ti and 150 nm thickness
Ag filters. For data collected in neon, all parameters were the same as in helium except
for the following. In this case, a 3.5 cm waveguide was used, with a constant pressureof 10 or 12 torr throughout the waveguide. Also, the modulations extended throughout
the waveguide.

92
QPM 10 torr
QPM 12 torr
Straight 10 torr
Straight 12 torr

Counts [a.u.]

6000

4000
Modulated
20000Straight
4

5

6
7
8
Wavelength [nm]910

Figure 3.15: Data showing enhancement of HHG in neon through QPM using modulated
waveguides.

The main effect of the modulated waveguides, in each case, is to enhance thephoton yield by a factor of 2-20x higher than that produced from a waveguide with nomodulations. The enhancement occurs, again, over the entire observed bandwidth. In
the case of neon, the highest observable photon energy was also dramatically extended,from ∼ 7 nm down to ∼ 5 nm. This type of enhancement was reproducible for moderate
pulse energies of ∼ 1 mJ. At this pulse energy, the ionization level reaches ∼ 30% by theend of the pulse in neon, and only ∼ 4% in helium. At such low ionization levels, energy
loss and refraction effects from the plasma are kept to a minimum, and the intensity
modulation is expected to be dominated by the guiding effects of the modulated innerwall of the waveguide.
However, with the implementation of the v-groove mounting, an extension of
the cutoff was observed for unmodulated waveguides as well. Figure 3.16 shows aspectrum generated in 15 torr helium that extends into the “water window” region

93of the spectrum, in an unmodulated waveguide. For this spectrum, the pulse energy
used was ∼ 4 mJ. At this pulse energy, the gas is fully ionized, and the plasma would
be expected to have a significant effect on the propagation of the driving laser beam.
Under these conditions, higher order modes may be excited in the waveguide, producing
short regions of higher-than-expected intensity. This boost in intensity could explain
the very high cutoff photon energies observed. Pulse compression may also play a role:pulse compression in argon was observed under similar ionization conditions [87, 117].
Although it was not measured in this case, it is possible that self-pulse compression

Intensity [a.u.]

contributed to the generation of very high photon energies seen in Fig. 3.16.

1000

C edge100

10

Ti edge
3

4
5
6
7
8
Wavelength [nm]9

Figure 3.16: Data showing HHG emission from helium extending into the “water window” up to the Ti L edge.

Without the ability to measure intensity fluctuations in the waveguides, however,
it is difficult to make further claims, either about the nature of QPM using modulated
waveguides, or the generation of high photon energies in unmodulated waveguides. The
need to understand the dynamics of the intensity was, in part, the motivation to develop

94
the probing technique described in Chapter 4. A better understanding of the spatiotemporal dynamics of the driving laser beam is essential to further progress in quasiphase matching techniques.
Modulation Depth Dependence
Another measurement performed using the v-groove mounting was a study of
how the modulation depth affects the enhancement. The goal of the modulation depth
study was to determine the optimal modulation depth for QPM enhancement. In paststudies, it had been found that modulation depths estimated to be a few percent of theinner diameter of the waveguide had produced the highest enhancements. However, acareful measurement and correlation had never been performed.
Modulated waveguides were manufactured using the glassblowing lathe setup described above (and in more detail in Ref. [1]). In order to characterize the waveguides,
the modulation depth was measured by placing the waveguide in an index-matching
fluid to eliminate lensing effects by the curved outer surface of the waveguide. The
waveguides were placed in the fluid in a such a way that the inner bore remained filledwith air, to provide a good contrast for measurement. Images of each waveguide wererecorded using a digital camera equipped microscope. With the magnification used, thepixel size was estimated to be roughly 1 µm. For each waveguide used, a consistent modulation depth was confirmed. The transmission efficiency of each waveguide was also
tested using a HeNe laser to ensure consistency. Waveguides with a transmission of lessthan 90% of the energy, or with a mode that did not appear symmetrically round, were
rejected. The only exception to this was the largest modulation depth tested, for whichmode degredation and reduced transmission was consistent. Six different modulation
depths were tested: 0%, or the “straight,” control waveguides, 0.8 ± 0.7%, 1.6 ± 0.3%,
2.4 ± 0.6%, 4.2 ± 1.6%, 6.5 ± 2.5%, where the uncertainties are the standard devationsof the measured modulations.
The measurements were performed in very low pressure neon (0.7 − 3 torr), for95
several pulse energies (in the range 0.85 − 1.70 mJ). Low pressures and pulse energies
were chosen in order to minimize detrimental effects due to ionization. The waveguides
each had a total length of 3.5 cm, with a central constant pressure region 2.5 cm long,
and a 5 mm pumping section on either end. The modulations had a periodicity of 0.5mm and were present throughout the 2.5 cm central section. For the data collection, thewavelength scale was calibrated using boron and carbon filters, and for each data set,
an identical background scan was taken in which the harmonic emission was suppressedby rotating a quarter-waveplate in the driving laser beam path. The integration timeon the camera was 240 s, and 6 pixels were binned in the direction of the diffraction, inorder to increase signal-to-noise. The grating used was the SB survey grating, and thedriving laser wavelengths were attenuated using a 400 nm Ti and a 150 nm Ag filter.
For each modulation depth, five individual waveguides were tested. The plots in
Fig. 3.17 include the averaged spectra from each of the five modulation depths. Typicalstandard devation error bars are included on the spectrum average for the modulation
depth of 4.2%. Five “straight,” or unmodulated, waveguides were also measured. The
shaded region on the graph represents the range included in one standard deviation
above and below the average straight fiber spectrum.
Figure 3.17 shows the results for the lowest pulse energy tested, which is representative of the general trends of the data. Enhancements were observed only for thesmallest modulation depths of 0.8 and 1.6% of the inner diameter. The enhancement istypically broadband, extending from ∼ 8 nm to the cutoff at ∼ 8 nm. The signal tends
to exhibit a general decrease with increasing modulation depth, however. The only
exception to this was the modulation depth of 2.4%, which consistently produced theweakest HHG signal. For the largest depths, the HHG signal drops dramatically, whichis consistent with their reduced transmission of the driving laser beam. It seems that ingeneral, however, the optimal modulation depth is <2%, since for greater depths, theloss appears to counteract any gains from a quasi-phase matching effect.

96

Figure 3.17: HHG yield from neon as a function of wavelength, generated in modulated
waveguides with varying modulation depth, for a pulse energy of 0.7 mJ and a pressureof 3 torr.

Chapter 4
Probing and Quasi-Phase Matching of High-Order Harmonic
Generation Using Counterpropagating Light

4.1

Introduction
In this chapter, I describe the use of counterpropagating pulses for probing andmanipulating HHG. Counterpropagating light is used to selectively suppress the coherent buildup of HHG, leading to several new types of measurements. In particular,
information about the coherence of HHG and evolution of the phase of the generated
harmonic field with propagation is revealed. Accurate measurements are shown of thein-situ coherence length of the nonlinear conversion process. From the direct measurement of the coherence of HHG, new information may be indirectly obtained about
several different aspects of this process. First, the evolution of the coherence, or phasemismatch, is sensitively dependent on the local and instantaneous driving laser intensity.
Fluctuations of the intensity due to loss or interference mechanisms are thus directly
mapped onto the coherence, and can hence be inferred from a measurement of coherence length. Until now, the precise location of harmonic emission within the waveguidewas not known. By probing with a counterpropagating pulse, the location of brightest
generation of a given harmonic order may be mapped within the waveguide, and it has
been found to be more complex than previously thought. Even temporal dynamics canbe inferred from measurements of coherence with sub-cycle resolution.
Careful measurements of the coherence length are then used to implement a

98
new, all-optical technique for quasi-phase matching. Using trains of counterpropagating pulses, enhancement of HHG is demonstrated for high photon energies, for whichconventional phase matching techniques are not possible. In two different cases, the
HHG signal is enhanced by more than two orders of magnitude. The photon yields
obtained with all-optical QPM are shown to be comparable to those obtained with conventional phase matching techniques at lower photon energies. Further enhancements
should be straightforward with with implementation of longer pulse trains. This technique is shown to be flexible, applying to range of photon energies and ionization levels,and customizable for compensating a wide range of phase mismatch. All-optical QPM
is also shown to provide a mechanism for controlled enhancement of HHG. Selectivity
and tunability of the enhanced photon energy is shown, along with selectivity of eitherof the two quantum paths that contribute to HHG emission. This selectivity could, inthe future, allow temporal and spatial manipulation of high harmonic generation, as
well as provide a mechanism for improved temporal and spatial coherence.
This importance of this work is in gaining insight and information on previously
unknown and inaccessible physics of the HHG process in hollow waveguides. This
information will be invaluable in overcoming the present limitations on HHG to makeit possible to implement a useful, tabletop source of ultrafast, coherent, soft x-ray light.

4.2

Experimental Setup
The laser source, HHG waveguide setup, vacuum setup, and EUV detection used

for the studies described in this chapter are the same as were described in Chapter 3.
The parts of the setup relevant to the counterpropagating pulse scheme are outlined
here.
The initial setup for creating counterpropagating pulses is shown in Fig. 4.1.
The output of a Ti:sapphire CPA system is split after compression; part of the energy,
compressed to 25 − 30 f s, is coupled into a hollow waveguide to drive the harmonic

99

SF18 glass
Ti:sapphire
amplifier
5 mJ, 1 kHz
25-30 fs

Delay
stage
Gratingcompressor

Gas input

X-ray generating
pulseCounterpropagating
pulsesFigure 4.1: Experimental setup for generation and coupling of a single counterpropagating pulse, using bulk material for stretching the pulse. Delay lines are not to scale.

generation. The other part of the beam propagates through 10 cm of SF18 glass,stretching the pulse through normal material dispersion to around 1.6 ps. This pulse
then propagates through a delay line, which allows relative adjustment of the timingof the forward and counterpropagating pulses. A polarizer in the delay line is adjusted
to assure a close match in the polarizations of the forward and counterpropagating
beams. Finally the beam is coupled into the opposite end of the waveguide using alens. Since the orientation of the waveguide is fixed for optimal alignment of the HHG
beam into the spectrometer, fine adjustments to the coupling of the counterpropagating
beam were accomplished by adjusting the X-Y position of the lens. The forward andcounterpropagating pulses have the same propagation distance between the splitting of
the beam and the coupling into the waveguide, so that they overlap in space and timein a small region the waveguide.
To allow propagation of the harmonic light to the detection system, a 3 mm holeis drilled into a mirror at a 45◦ angle past the exit of the waveguide. This mirror thendirects most of the energy of the counterpropagating beam into the waveguide. The

100
mirror is located between the focusing lens and the end of the waveguide. The annularshape of the counterpropagating beam focuses to a nearly Gaussian beam, as shown in
Ref. [118]. However, diffraction at the sharp edges degrades the quality of the beamat the focal spot, leading to poor coupling. At high intensities, imperfect coupling
also results in ablation of glass at the entrance to the waveguide, further degrading thecoupling efficiency. The counterpropagating beam, when focused with a 50 cm focal
length lens, positioned about 15 cm before the mirror, loses about 30% of its totalenergy due to this hole.
This setup was used for initial measurements of coherence length, but was eventually changed for several reasons. First, the ultimate pulse duration was determinedby the length of the material and was not continuously adjustable. Adjustment of
the pulse duration by using different lengths of material was prohibitively expensive.
Second, since the pulse was compressed in time before propagating through the SF18
glass, nonlinear phase accumulated while the intensity remained high in the first several millimeters of propagation. This distorted the beam, making coupling of the lightinto the waveguide more difficult. Finally, there was no simple method for creating
multiple pulses for all-optical QPM. The use of a thin sapphire substrate to create aseries of pulses was briefly explored. By exploiting the birefringence of sapphire, a beam
passed through the plate with its polarization at 45◦ relative to the optic axis. This
produced two slightly delayed pulses. generating a sinusoidally modulation of the intensity. However, this configuration did not yield significant enhancements, mostly due
to the inflexibility of the design.
Figure 4.2 shows a revised design for the creation of a counterpropagating pulse
train. Instead of splitting the beam after the compressor, the beam was split before
compression. Each beam propagated through separate, grating pulse compressors, sothat the pulse durations could be adjusted separately and continuously. The advantageof splitting the beam before compression is that each beam propagates only once through101
the grating pulse compressors, each having a throughput efficiency of about 60%. This
allows the new design the same overall efficiency as the material stretcher design.
Glass delay
platesa)

Ti:sapphire
amplifier
5 mJ, 1 kHz
25-30 fs

b)

Delay
stage

Gratingcompressor 2
Delay
stage
Gratingcompressor 1

Gas input

X-ray generating
pulseCounterpropagating
pulsesFigure 4.2: Experimental setup for the generation and coupling of one or more counterpropagating pulses, using phase masks within a grating pulse compressor.

Insets a) and b) in Figure 4.2 illustrate diagrammatically how multiple counterpropagating pulses, separated by a small time delay, were created using the grating pulse
compressor. In a), glass plates are inserted in the beam path at the frequency-dispersed
plane of the compressor (see Ref. [7] for details on grating-based stretcher/ compressor
designs). By propagating different frequency components through different amounts ofmaterial, a series of pulses with differing center wavelength were created. The frequency
range was typically chosen so that each delayed component had approximately the same
total energy. The separation is static and depends on the thickness and index of theglass used. For data presented in this chapter, the counterpropagating beam was lin-

102
early chirped by the compressor, so that the low frequency light preceded the higher
frequency light. Third order dispersion was minimized. Combinations of 2 mm and 5mm thickness, uncoated BK7 plates, were used to create 3 pulses in sequence at various
delays.
In principle, the setup of Fig. 4.2 could serve as an almost lossless technique.
However, efficient implementation requires some care. First, the windows must havesufficiently parallel surfaces, so that one part of the beam is not deflected relative tothe other. Even a very small wedge can severely affect coupling into a 150 µm innerdiameter waveguide several meters away. Second, with about 4% loss at each surface,multiple windows can add up to significant loss without proper antireflection coatings.
For the data presented here, the windows used were not coated, however, they wereselected for minimum deflection of the beam.
Inset b) of Fig. 4.2 shows a second iteration of this setup. In this case, a mirror
directs half the beam’s energy to a second retroreflector which is mounted on a motorized
delay stage. The advantage of setup b) relative to setup a) is that the time delay between
the two pulses can be adjusted continuously. However, this is a more complex setup andrequires additional care in alignment. First, the two retroreflectors in the compressor
are ideally identical, and have very little deviation of the beam with vertical tilt. The
mirror reflecting light to the moveable retroreflector must be large enough in area toreflect both the incoming and vertically displaced outgoing beams. It is oriented asindicated in inset b) of Fig. 4.2 so that the depth of the substrate and mount do
not clip the beam on either side. The static retroreflector may be moved farther fromgratings to accommodate this mirror. However, minimal propagation of the beam in thefrequency-dispersed region reduces instability due to air currents. Properly recombining
the two time-delayed beams requires two additional alignment considerations. First, thebeam must encounter both retroreflectors at the same height so that the outgoing beams
return at the same height. Second, the delay stage must translate smoothly and parallel

103
to the direction of the beam, so that the coupling into the fiber (again, several metersaway) is not altered significantly.
In order for the two pulses to interfere within the waveguide, the path lengths of
the forward propagating beam line and the counterpropagating beam line must be equal(Figs. 4.1, 4.2 are hence not drawn to scale). For the present work, this was accomplished by careful, manual measurement of the two path lengths from the beamsplitterthat separates the beams combined with adjustment of the path lengths through static,
optical delay lines. The path length of each beam was ∼10 m. For stability, thesebeam lines were enclosed by custom acrylic boxes and beam tubing constructed to minimize air currents. Maintaining efficient and consistent coupling into the waveguide is aparticular challenge when using this setup. However, especially in the initial stages ofsetup and testing, a long path length was preferable, for flexibility. Furthermore, it islikely that the long path length partially prevented feedback into the amplifier from thecounterpropagating beams. Upon exiting the waveguide, the counterpropagating light
was refracted strongly by the plasma, and this strong divergence limited the energy
propagating back through the delay lines.
Information about the coherence of HHG was inferred by observing the HHG
output while scanning the suppression region where the two pulses collide along thecommon axis of propagation. This scan was performed using a motorized delay stage
in the counterpropagating beam line (see Figs. 4.1 and 4.2). A hollow corner cube
retroreflector was mounted on the delay stage. Adjustment of the delay stage positionchanges the relative path lengths of the forward and counterpropagating pulses, so thatthe position of the collision point can be adjusted. One of two microstepper motors wasused: a Melles Griot Nanomover, with a range of approximately 1 in, and a Thorlabs
NRT motor, with a range of 10 cm. Typical step sizes used for data collection were50 − 200 µm. For the experimental setup used, the step size of the motor corresponded
directly to the change in position of the collision region. For example, when the motor

104
moves a distance 1 mm, the change in path length for the counterpropagating pulse is
2 mm due to the retroreflection. However, since the two pulses propagate in opposite
directions, each pulse makes up half this distance before colliding, so that the positionof the collision point moves 1 mm.
Identification of the collision point of the two pulses was accomplished as follows.
The pulse for each beam was fully compressed through optimization of the grating pulse
compressor. The two beam lines were propagated to the interaction region, but withthe waveguide removed, and the delay was adjusted so that the pulses were focusedat the same location in space. Both the forward and counterpropagating pulses werecapable of generating a visible filament of plasma (∼ 2 − 3 cm in length). Astigmatism
was minimized by slight tilting of the lenses to minimize the length of the filament.
Once the two counterpropagating plasma filaments were overlapped well in space, thecollision point could readily be observed as a brighter spot in the plasma that moved
when the relative path lengths of the two pulses were adjusted. A photograph of thefilament with a bright collision point, along with a schematic of the beams, is shown in
Fig. 4.3.
If the collision point could not be located this way, it was possible that thecollision point occurred on either side of the filament, where the beam was not focusedstrongly enough to ionize the air. The bright collision point will be visible only when
the two pulses are overlapped well in space and in time. However, the collision point
could be located indirectly. When the air is ionized, self-phase modulation generates
new frequencies which lie outside the reflectivity bandwidth of the steering mirrors foreach beam. This means that there is visible light that can easily be observed leaking
through the steering optics. Consider the following example. If the forward pulse collides
with the counterpropagating pulse before it reaches the plasma region at the focus, itwill propagate through the counterpropagating pulse’s plasma wake and be spatiallydistorted by refraction of the plasma. The plasma will diffract away the central part of

105

Figure 4.3: Photograph of the air plasma filament created in the free focus of thecounterpropagating beams. The bright point of plasma emission occurs at the collision
point of the two pulses.

the forward beam. However, the counterpropagating pulse will not propagate throughthe forward pulse’s plasma, since it collides after the focus region, and hence the beam
will not be distorted. By identifying which beam is distorted, it can be deduced on
which side of the filament the collision point is located.

4.3

Single Pulse Probing
One of the more revealing and useful measurements that can be accomplished withcounterpropagating light is that of the local coherence length of high-order harmonic
generation. In fact, this technique is capable of measuring coherence lengths in-situ, over
several harmonic orders simultaneously, and over an extended length. The coherence
length is shown to evolve with propagation distance in the waveguide. This measurement
provides previously unknown detail in the evolution of the phase of harmonic light, andindirectly, the evolution of the intensity and phase of the driving laser light.
The coherence length can be measured by using the counterpropagating pulse to106
suppress the harmonic field buildup in the overlap region of the forward and counterpropagating pulses. This overlap region is then scanned along the propagation directionof the waveguide by adjusting the time delay between the forward and counterpropagating pulses. Figure 4.4 shows the result of such a scan. Harmonic spectra, generated
in argon, are shown as a function of the position of the collision point of the two pulses.

Figure 4.4: The effect of a single counterpropagating pulse on the high harmonic emission from orders q = 37-45 in low pressure argon. The local coherence length can bedirectly measured in-situ from the coherence fringes which appear as a function of theintersection point, z, of the forward and counterpropagating pulses [119].

For these data, a 3.5 cm waveguide was used, with 5 torr of argon introduced
approximately 5 mm from each end of the waveguide, producing a constant pressure
throughout most of the waveguide, and a rapid pressure drop at either end. In Fig. 4.4,
the exit of the waveguide is located at z = 0 mm, the differential pressure region at z = 0
to 5 mm, and the gas inlet at z = 5 mm. The forward pulse duration and energy were 27
f s and 0.65 mJ, respectively, while the counterpropagating pulse duration and energy
were 1.6 ps and 0.155 mJ, respectively. The fundamental light is suppressed with two

107
200 nm thickness aluminum filters. The integration time of the CCD camera was 0.2 s,
and the spectrometer grating used was SC (see Chapter 3 for grating information).
When the overlap region is approximately the same width as the coherence length
for the generation of a particular harmonic order, the counterpropagating light canhave a significant effect on the overall output harmonic intensity. In the absence ofphase matching, the observed harmonic signal originates from a single coherence length.
Suppression of the harmonic light originating from a similar strength coherence zone
will thus have a large effect on the observed signal. Consider a simple picture of thenonlinear conversion process in which the phase slip (coherence length) and harmonic
emission strength are constant with propagation distance (see Fig. 4.5). The final, Nthcoherence length is the one detected, while the zones preceding it will have alternating
overall phase values. If the harmonic field from zone N-1 is suppressed, then it will
no longer be destructively interfering with the harmonic light immediately precedingit, from the zone N-2. Now zone N-2 interferes constructively with zone N, doubling
the overall detected field strength (the intensity increasing by 4x). This will be referred
to as suppression from an “out-of-phase” coherence zone. Conversely, suppression ofharmonic buildup from an “in-phase” coherence zone will cause an overall decrease in
the detected harmonic signal.
As can be seen in Fig. 4.4, distinct modulations are observed in the intensity ofeach harmonic order, as the overlap region that suppresses harmonic buildup is scanned
through the interaction region. The periodicity of these modulations is twice the coherence length, 2Lc , allowing the local coherence length of the process to be directly
measured from these data. The contrast of the modulations can be seen to vary withboth location and harmonic order. This is due to the fact that the coherence lengthand harmonic emission strength vary with both position and harmonic order. Thesevariations are described in more detail below. The greatest contrast will occur when
the overlap region precisely matches that of the coherence length, and when the signal

108
Driving laser
WaveguideCounter beam

HHG beam

27 fs~1.6 ps-+-+-+-+-+
Coherencezones

N-4 N-2...
...

N-3 N-1

N In phase (+)
Out of phase (-)

Figure 4.5: Measuring the coherence length of HHG in a hollow waveguide. A schematicof the coherence zones present within a waveguide when the phase mismatch is nonzero.
For N total coherence zones, the total harmonic signal detected is only from the final,
Nth , zone, since all other “in-phase” zones can be paired with a destructively interfering,“out-of-phase” zone.

strength of the two constructively interfering zones is the same. When the counterpropagating light permits transmission from a coherence zone that has a smaller fieldstrength than the final zone, either due to absorption by the gas medium, or a weakerharmonic emission, the contrast of the fringes will decrease. In these cases, however,weak contrast of the modulations is not an indication of poor relative coherence.
Strong contrast in the measured interference fringes, over an extended interaction
distance is then not a necessary, but is a sufficient, indication of strong relative coherence
between harmonic emission from different locations in the waveguide. The longer the
distance over which the harmonic emission maintains a good relative coherence, thegreater the potential for enhancing HHG using QPM. Strong contrast of the modulations
have been observed for distances over 1 cm in hollow waveguides (see, e.g., Fig. 4.6).
This shows that the waveguide geometry provides the long range coherence necessary for
implementing all-optical QPM. Especially when the coherence length is very short, in thecase of high photon energies, substantial enhancements could be made by correction of

109
the phase mismatch over a long propagation distance. Ultimately, the absorption depthof the gas medium for the photon energy of interest is what will limit the obtainable
flux [75]. For certain photon energies, such as the “water window” region at ∼ 2 − 4nm, helium has a very long absorption length at typical useful gas pressures (∼10’s ofcm), much longer than the typical coherence length there (∼10’s of µm). In this typeof situation, all-optical QPM in a hollow waveguide is an ideal solution for improving
the conversion efficiency. For example, if Lc was approximately constant at 10 µm, andall-optical QPM can be implemented over a distance of 1 cm, the total enhancement of
the conversion efficiency would be nearly six orders of magnitude.
Spatial Dynamics
While the hollow waveguide geometry provides a long interaction distance by
maintaining a high intensity through guiding of the driving laser, the HHG process issensitive even to small variations in the peak intensity and pulse shape of the driving
field. Probing with a single counterpropagating pulse can provide information about
the variation of the intensity of the driving laser. As described in Chapters 2 and 3, theenergy of the driving laser pulse will vary with propagation distance. In particular, theintensity decreases with propagation due to various loss mechanisms: from the imperfect
guiding of the hollow waveguide, from the energy lost to the ionization process, andfrom defocusing of the light by the plasma. The effect of this decreasing intensity on
the coherence length is through the level of ionization. The free electrons are strongly
dispersive, and even a slight change in their density will affect the phase mismatch. As
the intensity decreases, the ionization level follows, reducing the phase mismatch. The
expected effect is an increase in the coherence length toward the exit of the waveguide.
This effect is shown in Fig. 4.6: the periodicity of the modulations increases toward theexit, indicating a lower density of free electrons, and hence a decreasing intensity.
Another source of variation in the driving laser intensity is the interference of
propagating modes of the waveguide. When there is a significant amount of energy

Enhancement Factor

110

1.6

0.7 mm

1.1 mm1.4
1.2
1.0
Propagation direction

0.8
0.6
8

12

16
z [mm]

20

Figure 4.6: Intensity modulations of the 41st harmonic order generated in argon. Achanging periodicity of the intensity modulation with propagation distance indicates a
reduction in the intensity of the driving laser toward the exit of the waveguide [120].

propagating in both of the two lowest-order modes, EH11 and EH12 , of a waveguidewith inner diameter 150 µm, an on-axis intensity modulation forms with a period of∼ 2.2 cm. (See Chapter 2 for details on mode propagation.) In fact, a modulation of
the brightness of the plasma emission with roughly this periodicity is typically observed,
similar to those shown in Ref. [32]. For a sufficiently strong modulation of the intensity,
the harmonic generation will be limited to the regions of highest on-axis intensity. Thiseffect is shown in Fig. 4.7, which shows modulations in the intensity of harmonics 25
and 39, generated in a 6 cm waveguide filled with argon.
The periodicity in the data of Fig. 4.7 agrees well with that observed in a simulation of the modebeating effect, shown in Fig. 4.8. For this calculation, the energy ofthe driving laser beam was divided between two modes, with 67% of the laser energy
in the EH11 mode and 33% of the energy in the EH12 mode. Decreasing energy withpropagation distance can been seen in the simulation, as a result of guiding loss andsimulation of ionization loss as described in Chapter 3. The intensity profile is plotted
as a function of both propagation distance and waveguide radius.

111
Another aspect worth noting about the data of Fig. 4.7 is where within the
waveguide the different harmonic orders are generated. At z ≈ 5 cm, there is detectableemission from the 25th , but not the 39th harmonic order. This makes sense from thestandpoint that, due to loss, the driving field does not maintain sufficient intensity
to generate the higher photon energies further in the waveguide. Additionally, theabsorption depth of the 25th harmonic is ∼ 0.5 cm at the pressure used here, while
the absorption depth of the 39th harmonic is ∼ 4 cm. This explains why there is no
detectable response at the 25th harmonic order to the counterpropagating light near theentrance of the waveguide, at z ≈ 0.8 cm.

Intensity [au]

500

25th
39th

400
300
200
100
0
0

1

2

3
4
z [cm]

5

6

Figure 4.7: Variation of the harmonic emission generated in argon as function of theoverlap region of the forward and counterpropagating pulses, for two harmonic orders, q= 25 and 39. In the figure, the harmonic light propagates toward increasing z. Modulations appear only in limited locations within the 6 cm length waveguide (circled), witha periodicity corresponding to the periodicity of intensity modulations due to modebeating [120].

Modulations were often observed only in limited regions within the waveguide.
Two possible reasons for this observation are absorption of harmonic light by the gas
medium and a restricted region of high intensity due to modebeating. Another possible
reason is that modebeating can occur for the counterpropagating as well as the for-

112

Figure 4.8: Calculated intensity of the driving laser as a function of propagation distanceand inner radius of the waveguide. Simulation includes interference of the two lowest
order modes (beam energy: 67% EH11 and 33% EH12 ) of a waveguide with 150 µm
inner diameter, as well as numerically calculated ionization loss [120].

ward propagating beam. The ability of the counterpropagating light to suppress HHG
depends on the ratio of intensities of the counter- and forward propagating pulses.
Modebeating in each of the beams can result in a periodic variation of the intensity
ratio. Figure 4.9 shows a model of on-axis intensity modulations due to modebeatingpresent for both the forward and counterpropagating beams for two different length
waveguides. For the 6 cm waveguide (Fig. 4.9a)), the oscillations of the intensity do
not coincide, meaning that in the regions of high intensity for the driving laser beam,
where harmonics are expected to be strongly generated, the counterpropagating beam
has a low intensity, and therefore may not suppress the HHG strongly enough to disrupt the detected signal. In contrast, the intensity modulations do coincide in an 11 cm
waveguide (Fig. 4.9b)). The intensity ratios for each of these waveguides as a functionof propagation distance are shown in Fig. 4.9c). For the 6 cm waveguide, the intensity
ratio varies greatly with propagation distance, and may prevent efficient suppression of1.5

Intensity [a.u.]

1.0

6 cm waveguide
ForwardCounter

0.5

0.0

b)

1.5

Intensity [a.u.]

a)

1.0

113
11 cm waveguide
ForwardCounter

0.5

0.0
0

1

2

3
4
Position [cm]

5

6

0

2

4
6
Position [cm]8

10

Intensity Ratio (Ic/If)

c)
6 cm waveguide
11 cm waveguide

10

1

0.1

0

2

4
6
Position [cm]8

10

Figure 4.9: On-axis intensity modulations due to modebeating between the first two
coupled modes of a hollow waveguide, both for the forward- (red) and counterpropagating (blue) modes. Intensity peaks of the modulations do not coincide well for a 6 cm
waveguide (a), but do for an 11 cm waveguide (b). c) The on-axis intensity ratio of thecounterpropagating to the forward propagating beams. In the 6 cm waveguide (solid
curve), this ratio fluctuates more strongly with position in the waveguide than in the
11 cm waveguide (dashed curve), and is lower at the regions of highest intensity of thedriving laser (indicated by vertical lines).

HHG. An insufficient intensity ratio could also account for less-than-complete suppression of the HHG signal, causing weak modulations in the HHG signal as the collision
region is scanned.
Temporal Dynamics
The counterpropagating pulse probing technique has also been used to gather
information about the temporal dynamics of HHG. Under constant experimental conditions (i.e., gas pressure, laser intensity, ionization fraction, waveguide diameter, etc.),
the coherence length is expected to vary inversely with the harmonic order, due to theplasma-induced frequency dependence of the dispersion. This inverse relationship can

114
be seen in the calculated (solid and dashed) curves of Fig. 4.10a, which are based on
the phase mismatch equation (Eqn. 2.32) including the major dispersion source termsof the neutral atoms, free electrons, and the waveguide.
b)

LC [mm]

1.0

0.5

20

25

30
35
40
Harmonic Order

45

43rd
33rd
23rd

70
60

0.4

50

0.3

40

0.2

30

0.1

20

Ionization Fraction

Experimental data
Calculated, η = 0.18
Calculated, η = 0.22
Calculated, η = 0.26

1.5

Threshold Photon Energy [eV]

a)

0.0
-10

0
Time [fs]10

Figure 4.10: Probing temporal dynamics of HHG. a) Coherence length vs. harmonicorder at a single location in the hollow waveguide (black diamonds), as well as calculated
dependences at different levels of ionization (solid and dashed curves). Measured Lc
decreases faster than 1/q due to increasing ionization levels with harmonic order. b)
Time of harmonic generation within the generating ultrafast pulse for three harmonicorders, based on the measured coherence length, and the inferred ionization level using
ADK ionization rates. Dotted lines indicate the energetically allowed ranges for thesame harmonics, based on the cutoff rule [121].

For the data in Fig. 4.10a) (black diamonds), the coherence length for several
harmonics, generated in 5 torr argon, was measured at the same location, near the exitof the waveguide. The driving laser pulse had a duration of ∼ 24 f s and an energyof 375 µJ, while the counterpropagating pulse had a duration of ∼ 2.5 ps, and an
energy of 210 µJ. Error bars indicate standard devation of measurements of coherence
length from several scans. When the data are compared to the calculated curves of
the coherence length, however, it seems that higher harmonic orders are generated atincreasing levels of ionization. Thus, such a measurement of coherence length can beused to infer the ionization level at which each harmonic order was generated in thisregion of the waveguide, using Eqn. 2.32. Knowledge of the ionization level thenallows us to determine at what time within the laser pulse a particular harmonic order

115
was generated. Fig. 4.10b) shows the result of such a calculation, using the ADK
tunneling ionization rates [47], for three of the harmonic orders: q = 23, 33, and 43.
The range of ionization levels corresponding to the uncertainty in the coherence lengthis superimposed on a plot of ionization level vs. time within the ultrafast pulse. The
different levels of ionization indicate that the brightest signal for each harmonic is not
generated simultaneously. Instead, the lower photon energies are generated earlier in thepulse, at a lower ionization level, compared with the higher photon energies. This leads
to a stronger variation in the coherence length with harmonic order, since the higher
harmonic orders are generated in a more highly ionized, and hence more dispersive,
medium.
Another time domain phenomenon is indicated by the data in Fig. 4.10b). According to the cutoff rule (Eqn. 2.7), a given energy harmonic may only be generated
within a limited time range of the pulse, during which the intensity is high enough.
Thus, lower harmonic orders may be generated over a longer range than higher harmonic orders. The horizontal dashed lines in the plot indicate this range for each of
the three harmonic orders. The data in Fig. 4.10b) indicate that harmonics are generated, not necessarily at the peak of the pulse, where the ionization rate is expected
to be highest, nor even throughout the energetically allowed region, but closer to thetime when the intensity reaches threshold. The ability to probe these sub-optical cycle
dynamics of harmonic generation may lead to further characterization and temporalcontrol of the HHG process using all-optical QPM.
Limitations to Single Pulse Probing
There are, of course, several limitations to this single-pulse probing technique formeasuring coherence length. First, the counterpropagating pulse will have a significant
effect on the harmonic signal only when its width is similar to the local coherence
length of the process. Simulations indicate that modulations should be clearly visible
when the overlap region of the pulses is within the range of ∼0.1-2Lc . An overlap

116
region of 2Lc would be expected to have no effect, since it would suppress emission
from both an in-phase and an out-of-phase zone. An overlap region much smaller thanthe coherence length would not suppress enough of the emission to interfere strongly
enough. In practice, signal-to-noise ratio in the detection of the harmonic spectrum
is what will ultimately limit resolution of the coherent oscillations when using a pulse
shorter than the coherence length. Unless the duration of the counterpropagating pulse
used is similar to the local coherence length, modulations will not be observed, eventhough there may be HHG emission from the probed region.
Second, there is a limit to what size coherence length may be conveniently measured. For nearly all the data presented in this thesis, the coherence lengths were on
the order of ∼ 100 µm. The larger the coherence length, the greater the strength of
the harmonic signal. However, coherence lengths much larger than a few millimeters
are problematic since there is an energy limit to how long the counterpropagating pulse
can be made while still having enough intensity to efficiently suppress the HHG. For
small coherence lengths (less than about 50 µm) noise in the detection will limit theresolution, regardless of how well matched the overlap region is to the coherence length.
Also, smaller step sizes in the time delay scan increase the data collection time. Since
all-optical QPM is expected to be most useful for compensating phase mismatch in thecase of very small coherence lengths, the signal-to-noise must be improved. The two
major sources of noise in the current setup are the inherent intensity fluctuations of thelaser system, and pointing stability associated with large propagation distances.
An experimental example demonstrating the limitation in probing long coherence
lengths involves the idea of waveguide phase matching [23]. When the ionization levelis below critical (i.e., 5% for argon), phase matching may be achieved through tuning
the pressure of the gas within a waveguide to minimize the phase mismatch. Until now,the evidence for this process was a measurement of the harmonic signal as a functionof pressure, which peaked at the expected phase matching pressure of 30 − 40 torr, in117
the case of argon gas and in a 150 µm waveguide [23].
Probing with a counterpropagating pulse confirms phase matching of HHG underthese conditions. A counterpropagating pulse was used to probe the coherence lengthof the 27th harmonic generated in argon over a range of gas pressures from far below to
far above the optimal phase matching pressure. The normalized harmonic intensity as
a function of pulse collision point and pressure is shown in Fig. 4.11a. In this case thecounterpropagating pulse had a duration of about 2.5 ps, resulting in an overlap region
with the driving laser pulse of ∼ 375 µm. Modulations are clear at low pressures (5torr) and high pressures (> 60 torr), but disappear near the phase matching pressure(25 and 45 torr). Figure 4.11b shows the average (unnormalized) harmonic intensity
vs. pressure, showing the distinct rise in intensity at these mid-range pressures.

a)

b)

1

s ur
e[

80
60

0

40
0

5
z [mm]

10

20
15

tor
r]

100

2

Pre
s

I/Iavg [A.U.]

120
3

Iavg [A.U]

6
4
2
0
20

40

60

80

100

Pressure [torr]

0

Figure 4.11: a) Enhancement factor (I/Iavg ) of the 27th harmonic as a function ofgas pressure and position of the pulse collision point in the waveguide. The coherence
length increases as expected near the phase matching pressure of 45 torr, leading toa disappearance of the modulations. The position within the waveguide at which theharmonic is strongly generated also changes with pressure. b) Average harmonic output(Iavg ) as a function of pressure, demonstrating phase matching at ∼ 45 torr.

It can also be seen in Fig. 4.11a that the modulations appear at different locationsin the waveguide for different pressures. These data were collected by scanning the pulse

118
collision point from the exit of the waveguide toward the front. The horizontal axis
indicates distance from the exit of the waveguide. Strong modulations appear closer
to the exit of the waveguide at high pressure. There are two different reasons for this.
First, the absorption depth of the gas decreases from ∼ 18 cm at 5 torr to ∼ 2 mm
at 105 torr. The strongest modulations at high pressure are therefore visible in the 5mm differential pumping end section of the waveguide. At low pressures, the strongest
modulations are visible in the center, constant pressure section. Second, the phasemismatch will be lowest where the pressure is closest to the correct pressure (∼ 30 − 40torr), and therefore the strongest contributions at high pressure are in the differential
pumping region since the pressure ramps down through the phase matching pressure inthis section of the waveguide. For the low pressure case, the modulations occur where
the pressure is highest, near the gas input in the central section.

4.4

Double Pulse Probing
As shown in the previous section, the local phase mismatch is sensitive to changes

in the intensity of the driving laser pulse, leading to spatial variations of the measured
coherence length with propagation distance. In hollow waveguides, one of the effects
examined was the interference of excited propagation modes, which depend sensitively
on the coupling of the laser beams into the waveguide (see Section 2.6). This effect influences harmonic generation in several ways. As shown in Fig. 4.7, emission of the highest
harmonics may be confined longitudinally to regions corresponding to maximum laser
intensity. In addition, since the ionization rate of the gas medium is proportional to theintensity, there will also be a variation in the single-atom efficiency of harmonic emission. This variation in efficiency significantly influences the harmonic signal detected at
the exit of the waveguide.
A scan of the collision region of the driving laser pulse and a single counterpropagating pulse through several coherence zones can result in coherent oscillations in the119detected HHG signal, such as that shown in Fig. 4.4. In this case, the length andharmonic emission efficiency of the zones are approximately constant with propagation
distance. As discussed above, the size of the coherence lengths, as well as the spatial dynamics of the HHG, can be obtained from the periodicity of these oscillations.
This information is essential for understanding how harmonics are generated and how
the phase mismatch evolves. However, when the harmonic emission varies significantly
along the propagation direction (e.g., due to mode interference and nonlinear laserplasma interactions), a scan of a single counterpropagating pulse will not give rise toclear oscillations in the HHG signal. Instead, regions of large enhancement in the HHG
signal are typically observed. Thus, a new technique is necessary for probing HHG
coherence under these conditions.
It is possible to demonstrate strong coherence and probe the coherence lengths,
even in the presence of intensity oscillations, by using two counterpropagating pulses.
When the scan of a single counterpropagating pulse does not show coherent oscillations,the relative phase between emission from different locations in the waveguide may bemeasured using two counterpropagating pulses whose separation is continuously varied.
The following analysis illustrates the case where the collision region of one of the pulses
is fixed in space, while the other is scanned through the region of interest, to determine
the mutual phase of the HHG emission from the two regions.
A simple model of HHG emission under the influence of counterpropagating pulses
reproduces many of the qualitative and quantitative features of a counterpropagating
pulse scan. The harmonic field at the output of the nonlinear medium, of length L, canbe expressed as
EHHG (L) =

Z L
0

o
EHHG
(z) expπi
Lc (z)



dz

(4.1)

o
where EHHG(z) is the strength of the generated harmonic field as a function of the

propagation distance, z, and Lc (z) is the z-dependent coherence length. Two represen-

120
tative regimes may be considered which correspond to the experimental observations
described above.
ooRegime 1: Constant Emission Strength (CES). EHHG(z) ≈ EHHG
and Lc (z) ≈ Lc

This regime is characterized by oscillation of the detected HHG signal as thecollision region of a counterpropagating pulse and the driving laser pulse is scanned
through the interaction region (as seen in Fig. 4.4). In this regime, the strength of
the harmonic emission and the coherence length are both approximately constant withpropagation distance. Except for the final, Nth , coherence zone, all the preceding zones
are paired with an identical zone of opposite overall phase that destructively interferes(see Fig. 4.5). Without a counterpropagating pulse, the only emission detected is thatfrom the Nth zone. When a counterpropagating pulse suppresses the emission from oneof the preceding zones, the emission from its “partner” zone will interfere with the Nthzone. If all zones are constant in length and emission strength, the suppression of any
zone will either double the total field exiting the waveguide, or completely suppress it.
Thus, as the collision region is scanned through the nonlinear medium, high contrast
fringes appear in the detected HHG signal.
A simple calculation of this effect is shown in Fig. 4.12. For this calculation,o
EHHG
is assumed to be constant with propagation distance and proportional to theionization rate, calculated for typical parameters for HHG in argon. Fig. 4.12a) shows
the constant ionization rate profile as a function of propagation distance. The simulationof the counterpropagating pulse scan is performed by calculating Eqn. 4.1 as a functionof the collision region of the pulses, from which the HHG emission is subtracted. The
counterpropagating pulse is approximated as square in time, with an effective width
equal to the coherence length, and with the optimal laser intensity needed to suppress
HHG emission completely. Figure 4.12b) shows the coherent oscillations which appear
for such a scan in this regime.
oRegime 2: Varying Emission Strength (VES). EHHG(z) and/or Lc (z) vary signif-

8
7

0.8

0.6

0.4

121

Single pulse scanb)

1

HHG signal [au]Ionization rate (x 1015) s−1

a)6

Regime 1:
EHHGo constant

5
4
3
2

0.2

1
0
0

5

10

15

z/Lc

20

25

30

0
0

5

10

15

20

25

30

z/Lc

Figure 4.12: Simulation of a scan of a single counterpropagating pulse when the singleatom strength of the harmonic emission and the coherence length do not vary with propagation distance. a) A constant ionization rate with propagation and b) the variation in
the intensity of the detected harmonic signal for the scan of a single counterpropagating
pulse, showing coherent oscillations [120].

icantly with z.
This regime is characterized by a significant change of the detected HHG signal
when the collision region of a single counterpropagating pulse and the driving laseropulse is scanned through the interaction region. A significant variation in EHHG
(z)

and/or Lc (z) means that the emitted harmonic signal is varying significantly along its
propagation. As an example, we consider the case where Lc is constant with propagation
distance and the harmonic emission strength oscillates with propagation distance (Fig.
4.13a)). (This is the case almost always observed experimentally. However, future study
could elaborate on what happens when Lc (z) varies with z.) Now the final coherencezone is weak relative to the preceding zones. If the collision point suppresses harmonic
emission from a zone that has a much stronger emission, then its “partner” zone will
dominate the spectrum, exhibiting only a small modulation due to interference from themuch weaker Nth zone. Figure 4.13 shows the results of the propagation simulation inthis case. Figure 4.13a) shows the profile of the ionization rate as a function of distancein the medium for a changing laser intensity. This profile was generated taking into

122
account the interaction of the two lowest order coupled modes of a hollow waveguidewith inner diameter 150 µm. For this calculation, the intensity variation used was thesame shown in Fig. 4.8. The 1D ionization rate was calculated from the intensity
variation at the central axis of the waveguide. For the simulation of a single pulse scan,
the same calculation was performed as for Fig. 4.12b), but now with a longitudinallyvarying ionization rate. The coherent oscillations disappear, and the HHG signal canbe greatly enhanced using a single counterpropagating pulse (Fig. 4.13b)).
a)

8
7Regime 2:
EHHGo varies with z

0.8

HHG signal [au]Ionization rate (x 1015) s−1

Single pulse scan

b)

1

0.6

0.4

6
5
4
3
2

0.2

1
0
0

5

10

15

20

25

0
0

30

5

10

15

20

25

30

z/Lc

z/Lc
Second pulse scanc)8

HHG signal [au]

7
6
5
4
3
2
1
0
0

5

10

15

20

25

30

z/Lc

Figure 4.13: Simulation of a scan of one and two counterpropagating pulses when the
single-atom strength of the harmonic emission varies with propagation distance due tomodebeating. a) A varying intensity due to modebeating leads to a varying ionization
rate. b) A single counterpropagating pulse does not reveal coherent oscillations, since
the harmonic emission is much stronger at z/Lc = 15 than at 5 or 25. c) A second
counterpropagating pulse, scanned while the first is held fixed at z/Lc = 15 gives rise
to clear oscillations [120].

123
In order to measure the coherence length in this second regime, a second counterpropagating pulse is required so that clear coherent oscillations can be observed. For
these experiments, the first counterpropagating pulse is held at a fixed position where
the emission strength is high, while the second counterpropagating pulses is scanned
through the nonlinear medium. The second scan probes the relative coherence between
the bright emission now detected due to the presence of the first pulse, and the HHG
emission throughout the rest of the region. In this case, the harmonic emission fromthe zone detected due to the second pulse is of similar or lesser strength, resulting instrong contrast fringes. A simulation of this effect is shown in Fig. 4.13c), where thefirst pulse is held fixed near z/Lc = 15. When the two pulses are exactly overlapped,
the signal remains as though only one pulse was present. However, when the pulses are
separated by a distance 2Lc , the signal further increases by about a factor of four, whichis the increase in intensity expected when the harmonic field is doubled. The ability tocontinuously change the distance between the two counterpropagating pulses pinpoints
the exact separation of the pulses required for the greatest enhancement of the HHG
signal. Additionally, the periodicity of the fringes provides a measurement of the local
coherence length in this second regime, which was previously inaccessible.
Experimentally, both of the above regimes have been observed by scanning asingle counterpropagating pulse through the interaction region. Figure 4.4 shows anexample of the Constant Emission Strength (CES) regime, in which strong modulations
are resolved using a single counterpropagating pulse scan. Figure 4.14a) shows a typical
data set showing the Varying Emission Strength (VES) regime, obtained by scanninga single counterpropagating pulse through a region of strong intensity variation. For
these data, the interaction region consists of 8 torr argon in a 6 cm long waveguide.
The driving laser pulse had a duration of 27 f s and an energy of 470 µJ, while thecounterpropagating pulse had a duration of ∼ 1 ps, and an energy of 80 µJ. The
integration time of the CCD camera was 0.5 s, the grating used was SC, and two 200

124

Figure 4.14: Harmonic spectra as a function of the collision region of one and two
counterpropagating pulses. a) A single counterpropagating pulse is scanned throughthe interaction region, showing no coherent oscillation. b) A second counterpropagating
pulse is scanned through the interaction region while the first remains stationary at z
≈ 6 mm [120].

nm thickness aluminum filters attenuated the driving laser.
The effect of the single counterpropagating pulse is to strongly enhance the harmonic flux over a distance of 4 mm or more. The result of scanning a second counterpropagating pulse, while holding the first fixed in position, is shown in Fig. 4.14b).
This plot reveals the relative coherence of the harmonic emission in this region. The
first counterpropagating pulse is held stationary at position z ≈ 6 mm, while the second
pulse is scanned through the same region. Modulations appear with strong visibility,
demonstrating the strong relative coherence and also providing a measurement of thecoherence length. The signal is weak at the position where the two counterpropagating pulses are exactly overlapped, since they suppress coherent addition in the same
region of emission. However, when the pulses are separated by 2Lc , the signal is enhanced dramatically, because two coherence zones from a region of strong emission are
permitted to add coherently. Further enhancement could be achieved by adding morecounterpropagating pulses, while optimizing the width and separation of each pulse.

125
The ratio of the coherence length compared with the region suppressed by each of
the counterpropagating pulses can also be inferred from the data. Figure 4.15 shows theresults of the two pulse scan simulation for parameters mimicking the experimental conditions. The length of the region suppressed by each of the counterpropagating pulses,
Ls , is held constant, while the coherence length is varied. It is clear that the periodicityof the modulations matches the coherence length, regardless of the counterpropagating
pulse length. Also the appearance of a double peak near the first, stationary pulse, whenLs < Lc , matches the behavior seen in Fig. 4.14. This is a good indicator of the widthof the effective suppression region, which could be used to select the appropriate widthof the counterpropagating pulse for maximum enhancement. The agreement with theexperimental data also supports the validity of the simple model used in the simulation.

1.64
1.41

20

1.23

10

1.13

0
0

1.05
4

8

12

16

20

24

Lc/Ls

Intensity [a.u.]

1.36

1
28

Position [z/Ls]

Figure 4.15: Simulation of a scan of two counterpropagating pulses when the single-atomstrength of the harmonic emission varies with propagation distance due to modebeating.
For each of the curves, the suppression region (Ls ) is constant, while the coherence length(Lc ) varies. The simulation reproduces features visible in Fig. 4.14b.

This measurement constitutes a new technique for probing the local phase mismatch as well as the spatial and temporal emission of HHG in hollow waveguides.
The simulations of the counterpropagating pulse scans presented show clear qualitative

126
agreement with the observed data, providing evidence for the validity of the simple
model presented. Because the largest enhancements due to all-optical QPM have been
observed in this second regime, where the harmonic emission varies strongly with propagation distance, this approach yields the necessary information required to achieve
further enhancement.
One future application of this two-pulse probing technique is to determine therelative coherence of HHG at greater separations (> 1 cm) within the hollow waveguide.
Because HHG is most strongly generated in regions of strong laser intensity on-axis,
nonlinear reshaping and modebeating can limit strong emission to a several millimeter
length region separated by cm-scale distances. For a 6 cm length, 150 µm hollow
waveguide, there are three regions of high laser intensity, assuming most of the energy
is propagating in the two lowest order modes. The coherent addition of light from eachof these three intense regions could lead to significant further enhancements of HHG.

4.5

Quasi-Phase Matching
Once the coherence length has been measured, a train of counterpropagating

pulses with the correct width and separation can be designed that suppresses emission
from multiple, out-of-phase coherence zones [119,122]. This enables buildup of the x-ray
signal from in-phase zones only, leading to enhancement of the HHG signal. The firstattempts to implement all-optical QPM of HHG with counterpropagating pulses were
performed by the Peatross group. In their work, they used a free focus geometry. As
described in Chapter 2, they were not able to increase the harmonic signal above what
could be obtained by optimizing phase matching conditions. This work, in contrast,
deals with regimes where the photon energies cannot be truly phase matched, becauseof the high level of ionization. In further contrast with previous work, hollow waveguides
are shown to be an ideal medium for all-optical QPM due to the long-range coherence
described in the previous section.

127
Here, all-optical QPM of HHG is demonstrated in two different cases. An enhancement of ∼300 was obtained using three counterpropagating pulses in argon at
65 eV , and an enhancement of ∼150 was obtained using only two counterpropagating pulses in helium at 140 eV . In both cases, the photon yield increased to a levelcomparable to or higher than that which could be obtained for either photon energy
by optimizing the pressure and intensity level. In particular, HHG at 65 eV may bephase matched in helium. At 140 eV , however, HHG cannot be conventionally phasematched in any gas for the driving laser wavelength used. These preliminary results
showcase the great potential of all-optical QPM for further substantial enhancements of
HHG when longer trains of counterpropagating pulses are employed. All-optical QPM
is particularly promising, as will be described below, for enhancing emission at very
high, soft and hard x-ray photon energies, where the photon yield is currently severely
limited by a large phase mismatch.
All-Optical QPM at 65 eV
a)

b)

10

10

10

Enhancement Factor

Intensity [au]

10

3

2

1

3 Counter Pulses
1 Counter Pulse
0 Counter Pulses

10

10

10

3 Counter Pulses
1 Counter Pulse

2

1

0

0

27

31

33

35

37 39 41 43 45

Harmonic Order

27

31

33

35

37 39 41 43 45

Harmonic Order

Figure 4.16: Data demonstrating all-optical QPM at 65 eV in argon. a) Observed
harmonic emission from argon with no (gray), one (blue), and three (red) counterpropagating pulses present. b) Enhancement factor as a function of harmonic order, for one(blue) and three (red) counterpropagating pulses [119].

Figure 4.16 shows the enhancement of HHG at 65 eV in argon using three counterpropagating pulses. The gas was introduced at a pressure of 10 torr at about 7 cm
from the entrance of an 11 cm long, 150 µm inner diameter waveguide. Thus, instead128
of having a long constant pressure region, this waveguide had a long pressure ramp
region that increased with the direction of propagation of the driving laser pulse. The
collision point of the forward and counterpropagating pulses was scanned over a 2 cm
region around 4 cm from the entrance, in the center of this pressure ramp. In this experiment, the separation of the counterpropagating pulses was set using a static phasemask (shown in inset a) of Fig. 4.2). The integration time for the CCD camera was
0.5 s, the grating used was SC, and the fundamental light was attenuated using two
200 nm thickness aluminum filters. The approximate effective pulse separation was 1.1
mm and each counterpropagating pulse had a FWHM effective extent of about 340 µm.
The HHG spectra detected in the presence of zero, one, and three counterpropagating
pulses are shown in Fig. 4.16a).
For this experiment, the harmonic emission varied significantly along the propagation direction due to strong modebeating modulation of the laser intensity, corresponding to the VES regime described in the previous section. In this regime, a single
counterpropagating pulse can significantly enhance the total output of the HHG signal
without producing coherent oscillations of the signal. Indeed, in this experiment, any
one of the three counterpropagating pulses enhances the 41st harmonic order by approximately two orders of magnitude, which can be seen in Fig. 4.16b. The first pulseintersects with the driving laser pulse within the region where the harmonic emission isstrongest. As a result, bright harmonic generation from that region is now detected at
the output of the waveguide. The second and third pulses enhance the signal further,but by a much smaller factor, corresponding to the addition of similar strength coherence zones. The enhancement in this case is likely limited by imperfect delay between
the counterpropagating pulses, since the pulse train is created using a static, nonadjustable, phase mask. The thickness of the plates was selected to match the observed
coherence length, and the gas pressure and driving laser intensity were optimized forthe greatest enhancement. However, it is possible that further enhancement could be129
obtained through finer adjustment of the counterpropagating pulses.
The enhancement factor was calculated for each harmonic order and is shown in
Fig. 4.16b). Enhancement factor is defined as the ratio of integrated counts from thespectrum with quasi-phase matching compared to the spectrum without quasi-phasematching. Specifically, an enhancement factor was calculated for each harmonic order
within a narrow bandwidth around the harmonic peak. Uncertainty originates with thedetection noise of the CCD camera. Error bars indicate the standard deviation of the
CCD signal for the average pixel.
Even though this photon energy range may be phase matched in helium, alloptical QPM is found to enhance the photon yield to a level comparable to true phasematching. The photon yield of the 41st harmonic order was estimated to be ∼ 101 0
photons/sec, based on roughly calibrated estimates of the detection efficiency. The
CCD count rates for phase matched emission at the 27th harmonic order, which have acorresponding measured photon yield using a vacuum photodiode (described in Chapter 3) are compared to the CCD count rates for the 41st harmonic order enhanced by
all-optical QPM. Corrections were made for differences in efficiency of the filter transmission, the optical components of the spectrometer, and the quantum efficiency of the
CCD camera. This photon yield is comparable to that of phase matched emission fromhelium at these wavelengths, which is mostly limited by the absorption depth of heliumat the high pressures required for phase matching. At 65 eV , the absorption depths ofhelium and argon are ∼ 3 mm and ∼ 3 cm, respectively. Hence further enhancements
are possible in argon by the addition of more counterpropagating pulses, since the absorption depth is still much longer than the region over which QPM was implemented,∼ 3 mm.
Selectivity of Photon Energy
A consequence of the strong coherence of HHG generated in hollow waveguides
is that all-optical QPM will be selective, enhancing a narrow bandwidth. For example,

130
the enhancement in Fig. 4.16 is selective, enhancing the the 41st harmonic order morestrongly than the adjacent orders. Because the coherence length of the harmonics
varies by at least 1/q, as described earlier in the chapter, a pulse train with a given
delay between the individual pulses will selectively enhance a single harmonic order.
The addition of more counterpropagating pulses will not only enhance the HHG signal
further, but will become more selective of a narrower bandwidth. This feature of alloptical QPM is particularly attractive for applications of HHG that require a narrow
bandwidth, e.g., for coherent imaging [15] or selective energetic excitation of chemical
or electronic processes [19].
The selectivity of all-optical QPM can be improved further if the counterpropagating pulses suppress out-of-phase coherence zones that are not adjacent, but are
farther apart. Figure 4.17 illustrates this effect: the size of the coherence zones for two
different harmonic orders will be slightly different due to the frequency dependence ofthe dispersion. A given pair of counterpropagating pulses can be adjusted to match thespacing of out-of-phase coherence zones for one harmonic order, but will not match thespacing of another harmonic order. This effect becomes more prominent the greater the
spacing between the pulses, or the more counterpropagating pulses that are used.
X-ray generating
pulse
25 fs
Coherencezones

Counterpropagating
pulses~1 ps+-+-+-+-+-+-+-+-+-+-

pulse
separation
= 4Lc
>4Lc

Figure 4.17: A schematic illustrating the selectivity and tunability of all-optical QPM
using two counterpropagating pulses, by varying their separation [120].

An example of this selectivity of photon energy is shown in Fig. 4.18. This
plot shows enhanced spectra of HHG from argon, at different pulse separations. The

131
width of each counterpropagating pulse was kept constant at ∼ 300 µm, but the delay
between them was varied around a pulse separation of approximately 4Lc . As the pulse
separation is changed, the harmonic order that is most strongly enhanced is shifted.
Essentially, the pulse separation will precisely match a distance of 4Lc for different
harmonic orders as the separation is varied.

1.4

1.2
1.1

Pulse Separation [mm]

1.3

1.0
0.9
57 55 53 51 49 47

45

43

41

Harmonic Order

Figure 4.18: Selectivity and tunability of all-optical QPM using two counterpropagating
pulses with variable separation. Enhancement occurs when the pulse separation is
2N Lc . Selectivity improves when N > 1. HHG spectra in argon show the shift of theenhancement with harmonic order as the separation between the pulses is varied [120].

Figure 4.19 includes the same data, and further illustrates both the selectivity
and tunability capabilities of all-optical QPM. Two of the spectra from Fig. 4.18 areplotted along with the spectrum observed when only one of the two counterpropagating
pulses is present. Without all-optical QPM, no harmonic peaks are visible. The blue
curve, for which the pulses were separated by 1.0 mm, shows in particular the selectivityof all-optical QPM. Only three of the harmonic orders, q = 49, 51, and 53, are enhanced

132
250
1 pulseIntensity [a.u.]200

2 pulses
1.3 mm sep.
1.0 mm sep.

150
100
50
0
57 55 53 51 49 47 45

43

Harmonic Order

Figure 4.19: Selectivity and tunability of all-optical QPM using two counterpropagating
pulses with variable separation. The spectrum enhanced by one pulse (solid gray) is
plotted along with spectra enhanced by two pulses, for two different pulse separations:
1.3 mm (red) and 1.0 mm (blue).

further by the addition of the second pulse. In fact, for orders 45 and 47, the second
counterpropagating pulse actually reduces the degree of enhancement to below that withthe first counterpropagating pulse. The red spectrum illustrates the tunability. For aslightly different pulse separation, 1.3 mm, the harmonic orders enhanced shift to lower
photon energy.
All-Optical QPM at 140 eV
All-optical QPM has also been used to demonstrate enhancement of HHG athigh photon energies in helium [122]. Helium has the highest ionization potential of
the noble gases, at 24 eV , and thus offers the highest possible photon energies that canbe phase matched. The upper limit of the phase matching region for helium is ∼ 130
eV , when using a driving laser wavelength of 800 nm. Higher photon energies can only
be produced at higher laser intensities, which necessarily results in a higher degree ofionization of the gas medium. Above the critical fraction of ionization, ηcr (Eqn. 2.33),
the dispersion from the free electrons is too strong to be compensated by that from the133
neutral atoms. Therefore, QPM techniques are required for enhancing HHG at highphoton energies.
10

b)

4

Enhancement Factora)Intensity [au]500 torr
10
10
10
10

3

2

1

0

110 torr
2 Counter Pulses
1 Counter Pulse
0 Counter Pulses

100

QPM enh.
at 110 torr

10

1

QPM enh. (110 torr)
vs max. signal w/o
QPM (500 torr)

0.1
67

71

75

79

83

Harmonic Order

87

91 95

79

83

87

91

95

Harmonic Order

Figure 4.20: Data demonstrating all-optical QPM at 140 eV in helium. a) Observed
harmonic emission from helium for no (gray), one (blue), and two (red) counterpropagating pulses. The dotted curve shows harmonic emission under similar laser conditions,but at a pressure of 500 torr, which is optimal for conventionally phase matching lower
harmonic orders, below q = 77. b) Enhancement factors for harmonic orders 79-95. Red
circles show the ratio of the QPM emission obtained using a two counterpropagating
pulses to that without counterpropagating light at a pressure of 110 torr. Black triangles show the ratio of QPM emission at 110 torr to that without counterpropagating
light at a pressure of 500 torr.

Figure 4.20 shows the enhancement of HHG in helium using two counterpropagating pulses. The gas was introduced at a pressure of 110 torr at 5 mm from theexit of a 6 cm, 150 µm inner diameter waveguide. The forward propagating pulse had aduration of 27 f s and an energy of ∼ 1 mJ. The collision point of the forward and counterpropagating pulses was scanned over a 2 cm region near the exit of the waveguide.
Since the gas was introduced only at the exit of the waveguide, there was a long sectionof the waveguide with a pressure ramp increasing with propagation distance. The separation between the two counterpropagating pulses was adjusted using the setup shownin inset b) of Fig. 4.2. The coherence length was measured using the two pulse method,since these data were observed in VES regime. This also allowed careful tuning of both
the width of each pulse and their separation to produce the maximum enhancement.
The width of each pulse was approximately 750 f s FWHM, and the approximate pulse

134
separation at highest enhancement was 3 ps, making the effective separation about 1.5
ps. The energy in each counterpropagating pulse was ∼ 200 µJ. The integration time
for the CCD camera was 1 s, the grating used was SC, and the fundamental light was
attenuated using one 200 nm thickness silver filter, and one 200 nm thickness zirconium
filter. The HHG spectra with zero, one, and two counterpropagating pulses are shownin Fig. 4.20a).
Without the counterpropagating pulses present, harmonics are observed from helium at a pressure of 110 torr up to the 87th order at 134 eV . The presence of evenone counterpropagating pulse increases the brightness of several harmonic orders. At
the laser intensity used, the cutoff is well above the highest photon energies observed,
indicating that the falloff of the 87th harmonic is due to phase mismatch. As in thedata presented in Fig. 4.16 in argon, the enhancement is selective, occurring only
over a limited range of photon energies whose coherence length matches that of thecounterpropagating pulse train used. The enhancement factor obtained using two counterpropagating pulses is shown in Fig. 4.20b, reaching factors of 150 and 120 of the87th and 89th harmonic orders, respectively. The highest observable harmonic is also
extended from the 87th to the 95th , due to partial suppression of out-of-phase zones.
Error bars are calculated in a similar way to those of Fig. 4.16b.
The efficiency of all-optical QPM was maximized through fine-tuning of the widthand separation of the counterpropagating pulses. The coherence length, for q = 89, forexample, was measured to be 217 ± 25 µm near the region of highest harmonic emission,
through the observed oscillations of the harmonic signal. This was used to determine
the optimal separation of the two pulses, which was independently measured as ∼3 ps,
appropriate for enhancing a coherence length of 225 ± 25 µm. The measured single pulse
FWHM of 225 ± 15 µm approximately matches the prediction [106] that the largest
QPM enhancement occurs when the Sech2 pulse width corresponds to ∼ 0.92Lc ≈ 203
µm.

135
This measured coherence length can be used to calculate the ionization level atwhich the harmonics were generated, using the phase mismatch equation: Eqn. 2.32.
Solving this equation gives an ionization level of η ≈ 1.7%, for the above experimental
conditions. This number is also consistent with the ionization level predicted at thetime when the cutoff intensity reaches 140 eV , as calculated using the ADK tunnelingionization rates [47]. The critical ionization for helium may be determined using Eqn.
2.33, giving 0.5% for a driving laser wavelength of 800 nm. The measured harmonics,
then, are generated at a level of ionization three times that which can be conventionallyphase matched.
For these data, the pressure of the gas at the input to the waveguide was kept
constant at 110 torr. To get a sense of the absolute enhancement obtained using alloptical QPM, a comparison was made between the emission with all-optical QPM at
a pressure of 110 torr, and the emission for which the pressure was optimized for thebrightness of the highest harmonic orders. All other experimental parameters weresimilar to those described above. Overlaid in Fig. 4.20a) is a spectrum taken at apressure of 500 torr, which is near the phase matching pressure for q = 79 and below.
Fig. 4.20b) shows the enhancement factor obtained by the two-pulse all-optical QPM at
110 torr compared to the maximum emission without QPM at 500 torr (black triangles).
The 89th harmonic order in particular is enhanced by a factor of 40, and all harmonicorders > q = 83 are enhanced using all-optical QPM above that which can be obtained
simply by optimizing the pressure.

4.6

Quantum Electronic Trajectories
As described in Chapter 2, in the semi-classical picture of HHG, there are two

distinct paths an electron may travel in the continuum and return to the parent ion withthe same kinetic energy, hence producing the same harmonic order. These paths are
the so-called “long” and “short” trajectories, referring to the relative time the electron

136
spends as a “free” electron in the time interval between field-ionization and recombination with the parent ion. These different quantum trajectories can often be distinguishedin spectral measurements. Non-adiabatic blueshifting of the harmonics is stronger forthe long trajectories than the short trajectories, leading to a splitting of the harmonicpeaks. When driven with a high pulse energy, HHG spectra in argon often show strong
peak splitting between the two trajectories in Fig. 2.10. In some cases, even more
complicated structures can be seen due to multiple trajectory peaks. This differential blueshifting of the different quantum trajectories allows distinction of the effects ofcounterpropagating pulses in the spectral data, allowing insight into, and even controlof, sub-cycle time scale processes.
The phase modulations induced by the counterpropagating pulse affect the long
trajectories more strongly than the short, as described in Chapter 2 and Ref. [119].
Emission originating from the long trajectory may in fact be suppressed at a lower
counterpropagating intensity than that from the short, due to the greater contribution
from the intensity-dependent phase. In Figs. 4.14 and 4.4, for example, it is emission from the long trajectory that exhibits modulations, while emission from the short
trajectory is unaffected. For Fig. 4.4, the cutoff photon energy for the driving laser
intensity used is about 100 eV . Thus, the harmonic orders shown are well within theplateau region, where the intensity-dependent phase accumulation is significantly different for the long and short trajectories. For these data, the ratio of the counter- to
the forward propagating intensities, IC /IF , is about 0.25%. Calculations have shownthat for such a small intensity ratio, there is a significant difference in the degree ofsuppression between the two trajectories, mostly owing to intensity-dependent phasefluctuations [119].
Information may be also be extracted that relates to the difference in the macroscopic phase evolution with propagation between the two different quantum paths. The
data set shown in Fig. 4.21 was taken in argon using the two-pulse probing technique.

137
For some of the harmonic orders, the two distinct long and short peaks are readily apparent, as for orders 35-39. At the higher orders, modulations extend through the spectral
region between the bright, long trajectory peaks. The probing of coherence reveals

Figure 4.21: HHG spectra from argon in the presence of one counterpropagating pulse
held fixed in position at z ≈ 9 mm, while a second counterpropagating pulse is scanned
through a 2 cm region of the waveguide. Variation of the periodicity of the oscillations
with harmonic order (photon energy) reveal dependences of the phase on the time theelectron spends in the continuum before recombination.

several interesting features. First, the enhancement peaks, which correspond to suppression of out-of-phase regions, appear to fan out in the direction of longer wavelength(lower photon energy). This means that the less blue-shifted, short trajectories have
longer coherence lengths than do the long trajectories. In fact, it is apparent that thecoherence lengths change more rapidly among different trajectories which correspondto the same harmonic order than do coherence lengths from harmonic peak to peak.
One possible explanation for this is that the electron wavefunction acquires more phasethe longer it is present in the continuum. Therefore the long trajectories will have agreater phase mismatch, and hence shorter coherence length than the short trajectories.

138
Another thing revealed by the probing is simply the existence of emission from the short
trajectories. Because of the ringdown of harmonic signal due to intensity fluctuations,the emission from the short trajectories is not detectable without counterpropagating
light, especially for the 43rd and 45th harmonic orders. In other words, the harmonic
emission from the short trajectories is of the VES regime described in Section 4.4.

Figure 4.22: Harmonic spectra in argon as a function of the collision position of thedriving laser pulse and a single counterpropagating pulse, revealing the presence ofseveral quantum trajectories with different coherence properties.

Probing with counterpropagating pulses has revealed even more complex trajectory phase information which is not easily explainable. Figure 4.22 shows a plot of
harmonic spectra from argon as a function of the collision point of a single counterpropagating pulse, showing a more complex structure than in Fig. 4.21. In particular, thisplot shows the difference in the brightness of emission from different trajectories as afunction of position within the waveguide. This plot was again acquired in the centerof a high intensity region of modebeating. Short trajectories (toward the low photon

139
energy or low harmonic order) appear to be strongly generated in two general regions
along the axis of propagation, while the long trajectories are located in one. Numericalsimulations may be required to describe the coherence properties of different trajectories, as well as the relative emission strength of trajectories as a function of driving laser
intensity.
A direct consequence of the fact that different trajectories have different coherence
lengths is that all-optical QPM may be used to selectively enhance a single trajectory. In
fact, since the coherence length changes more rapidly with time of recombination thanwith harmonic order, the distinction between trajectories is expected to be even stronger
than between harmonic orders. The harmonic spectra in Fig. 4.23 illustrate this ability
to preferentially enhance one electronic trajectory over the other using all-optical QPM
with two counterpropagating pulses.
The experimental parameters for the data in Fig. 4.23 were as follows. The
harmonics were generated in 200 torr helium. The gas was introduced into an 11 cm
waveguide at about 7 cm from the entrance. The pulse collision point was scanned
through a 2 cm region just ahead of the gas input. The driving laser pulse had aduration of 27 f s, and an energy of 1.3 mJ, while each counterpropagating pulse had aduration of ∼ 750 f s and an energy of ∼ 0.2 mJ. The driving laser light was attenuatedby a 200 nm silver and a 200 nm zirconium filter, and the spectrometer grating used
was SB. Integration time of the CCD camera was 1 s, and each point shows the sum of
three pixels, binned in order to reduce integration time. Two counterpropagating pulses
were generated using the static delay method shown in inset a) of Fig. 4.2.
In the figure, the gray curve shows a typical spectrum detected in 200 torr helium
without the use of counterpropagating pulses. In this case the spectrum is dominatedby the short trajectory. As shown by the red spectrum, all-optical QPM enhances theseshort trajectory peaks when two counterpropagating pulses with a pulse separation of∼ 840 µm are used. Dashed lines show that the peaks of the gray and red spectra occur

140

Intensity [a.u.]

600
Long Traj.
Short Traj.
No CP Pulses
400

200

0
79

83

87
91
Harmonic Order95

Figure 4.23: Selective enhancement of either the long or short quantum trajectories
using all-optical QPM in helium. The dashed lines indicate the position of the harmonicpeaks for the short trajectories. Harmonic spectra are show for no counterpropagating
pulses (gray) or two counterpropagating pulses present at pulse separations of ∼ 350µm (blue) or ∼ 840 µm (red). (These data were obtained from the same data set as
Figure 3 in [69]at the same approximate photon energy. In neither of these two spectra are double
peaks, indicating the absence of strong emission from the long trajectory; only theshort trajectory is enhanced. The blue spectrum, on the other hand, shows a two-pulse
enhancement with a pulse separation of ∼ 350 µm. The enhanced peaks are clearlyblue-shifted relative to the short trajectory peaks, especially for harmonic orders 81-91,
indicating that it is the long trajectory which has been enhanced. Furthermore, theshort trajectory peaks are clearly not enhanced as well as in the red spectrum.
The only difference between these two enhanced spectra is the separation between
the counterpropagating pulses. Further analysis reveals that for the blue spectra, thepulse separation corresponds to adjacent out-of-phase coherence zones, separated by
2Lc , while for the red spectra, the pulse separation corresponds to 4Lc . The distinction

141
between the two trajectories diminishes closer to the higher orders, q > 91. These
harmonic orders are close to the cutoff photon energy for the laser parameters used,
and the two trajectories merge near cutoff.
This ability to selectively enhance a single trajectory has great implications for
spatio-temporal control of HHG. In particular, selection of a single quantum trajectory
improves both the temporal and spatial coherence of HHG. These coherence properties are especially important for applications of HHG such as coherent imaging techniques [15,123]. Emission from long trajectories is strongly divergent compared to short
trajectories for a couple of different reasons. First, the long trajectories have stronger
coupling to the intensity dependent phase, and hence have a stronger modulation of
the wavefront from a Gaussian or Bessel-shaped laser mode [65]. Second, better phasematching conditions off-axis will result in a more divergent harmonic spatial mode forthe long trajectories, as described in Refs. [73] and [74].
Spatial and temporal coherence can be degraded due to interference of emission from different quantum trajectories. Previously, coherence properties have been
improved through aperturing of the harmonic beam in the far field [8], or the use oflong waveguides [68]. All-optical QPM not only isolates a single trajectory with good
coherence properties, but also enhances its conversion efficiency, without the need forprevious techniques which tend to be lossy. These qualities will become especially important as imaging and measurements requiring strong coherence move toward eversmaller wavelengths. Additionally, preferential selection of emission from a single trajectory has great implications for temporal shaping of HHG. The ability to control thegeneration of harmonic on a sub-cycle time scale can lead to the shaping of attosecond
pulse trains, or even isolated attosecond pulses. Attosecond sources based on HHG havealready been shown to be quite powerful in time-resolved measurements of electronic
processes [21, 124], and as attosecond sources become more accessible and tunable, newdiscoveries are sure to follow.

Chapter 5
Summary and Future Work

5.1

Summary
The work presented in this thesis includes several advances in the understanding

and ability to control high-order harmonic generation. Energy loss in the driving laser
beam obviously limits both the observable cutoff energy and the total harmonic intensity, and is documented here, illustrating its dependence on pressure. Simulations ofionization loss show that this is one of the major mechanisms for loss, but consistently
accounts for only a portion of the total loss, regardless of the degree of ionization or freeelectron density. The use of a new experimental waveguide setup allowed two updated
measurements: a higher harmonic photon yield estimate at 45 eV, and a systematic
study of QPM with modulated waveguides. Concerning the modulated waveguides, enhancements at high photon energies (150 − 250 eV ) were shown to be reproducible in
the new waveguide setup. A study of modulation depth showed that the optimal modulation is < 2% of the inner diameter. It is possible that the use of counterpropagating
pulses to probe the generation process in modulated waveguides would further illustrate
this QPM technique.
Probing the harmonic generation process with counterpropagating pulses has
proven invaluable in providing previously unknown information about the coherence
and the dephasing of HHG in hollow waveguides. Knowledge of the local, dynamicallyvarying phase mismatch will be crucial in any quasi-phase matching scheme for HHG,

143
regardless of the geometry used or the QPM mechanism. Counterpropagating light has
also shown some of the limitations, as well as advantages, of the use of hollow waveguides
for HHG that could not have been easily predicted. Modebeating limits the longitudinal
regions of high intensity, and therefore strong harmonic emission. However, the mutual
coherence of harmonic emission from hollow waveguides was shown to be strong overextended interaction distances of at least 1 cm and possibly more. This fact makes
the possibility for enhancing conversion efficiency through quasi-phase matching very
promising.
Probing of the local coherence length also showed that the brightest emission ofseveral harmonic orders occurs at different times within the femtosecond driving laser
pulse. Temporal information such as this will provide information about the temporal
structure of harmonic emission and how best to control it. Evidence for pressure-tuned
phase matching in a hollow waveguide was also observed as an evident divergence of thecoherence length when close to the optimal pressure. Intensity modulations from energy
loss and modebeating were also unambiguously observed through variation of the local
phase mismatch. Until now, the location of harmonic emission within the waveguidewas not known. This type of characterization may be important in demonstrating theeffect of plasma dynamics on HHG.
Two different regimes of coherent buildup of HHG were identified through probing, one where the harmonic emission strength is constant with propagation, and theother varying with propagation. In the first regime, strong coherent modulations areobserved with the scan of a single counterpropagating pulse. In the second regime, asingle counterpropagating pulse can lead to strong enhancement, but coherent modulations are not observed. The coherence in this region, as well as a measurement of
the coherence length, can be demonstrated using a two-pulse probing technique. The
ability to measure coherence length in both of these regimes is crucial to implementing
QPM.

144
Counterpropagating pulses suppress the coherent buildup of the harmonic fieldby modulating the phase of the driving laser pulse over a small region. When destructive interference is suppressed using a series of counterpropagating pulses, the HHG
process can be quasi-phase matched. All-optical quasi-phase matching using multiple
counterpropagating pulses was demonstrated, producing enhancements of more than
two orders of magnitude, both for emission from argon and helium. In each of these
media, QPM was shown for photon energies that could not be phase matched using
conventional techniques. The main advantages of this QPM technique are its flexibility,
scalability, and efficiency. The coherence length was similar for both of the experimental demonstrations, however, the degree of ionization was quite different, demonstrating
the applicability of all-optical QPM to varying plasma conditions. Since the coherence
length can be measured carefully, the destructive interference can be suppressed efficiently. A larger enhancement simply requires a greater number of pulses. All-optical
QPM is easily scaled to the shorter coherence lengths expected at higher photon energies.
Finally, all-optical QPM of HHG is selective, enhancing a narrow bandwidth ofharmonic frequencies. This feature is especially attractive for applications requiring
monochromaticity. Contributions to the harmonic emission from either of the electronic trajectories can also be selectively enhanced. This has important implications for
improving the spatial coherence and transverse mode profile of harmonic emission, as
well as manipulation of the temporal structure of the emission.

5.2

Future Work
Enhancements from all-optical QPM could certainly be improved beyond theresults presented here. The enhancement is expected to increase with the addition ofmultiple counterpropagating pulses. For the shorter coherence lengths present at highharmonic orders, less energy is required in each counterpropagating pulse. The phase of

145
a higher harmonic order can be sufficiently modulated by a lower counterpropagating
intensity. Also, for a short coherence length, the counterpropagating pulse duration is
also shorter, lowering the total required energy. This will permit the generation of a
train of many pulses for all-optical QPM for high harmonic orders. This is particularly
beneficial, since the highest orders are currently the least efficiently generated.
To date, all-optical QPM has only been demonstrated for relatively long coherence
lengths of ∼ 100’s of µm. In this situation, the harmonic signal can be increased substantially even with a few pulses, since each coherence length summed adds a relatively
large amount to the total intensity. All-optical QPM using shorter counterpropagating
pulses is technically more difficult. The detection noise can mask the effect of a single,
probing pulse, and necessarily longer integration times makes the data collection timeconsuming. One way of extending efficient phase matching to higher photon energies
is to use a longer driving laser wavelength [81, 83, 84]. However, the longer wavelengths
reduce the recombination probability [85]. All-optical QPM used in combination witha longer driving laser wavelength could be a good compromise.
The addition of shaping techniques could allow more precise control over both
HHG and all-optical QPM. In previous work, temporal [125] and spatial [103] shapingof the driving laser beam have led to greater conversion efficiency and manipulation of
the harmonic beam. In our work, temporal pulse shaping was not used, but could beapplied to generating a shorter driving laser pulse, or to carefully shaping the counterpropagating pulse train. As a first step, the optimal counterpropagating pulse shape
could be determined using a pulse shaper to obtain the highest enhancement from asingle pulse. More sophisticated shaping could be used to generate custom sequences ofcounterpropagating pulses. Genetic algorithms for pulse optimization may even provide
new information on the QPM mechanism. Spatial shaping of either beam could be used
to produce more optimal coupling conditions. Intensity fluctuations from modebeating
may be reduced or selected for advantageous conditions.

146
Pulse trains could also be extended to different regions of the waveguide for
substantially higher enhancements. As shown in Fig. 4.7, the harmonic generation issometimes limited to local regions of the waveguide by guided mode interactions. So
far, pulse trains used for QPM have been limited to only one of these regions at a time.
By adding more pulses, delayed to interact in other regions of high intensity, more inphase harmonic emission could be coherently summed. As a first step, it should bedetermined, through two-pulse probing, whether the emission from different regions ismutually coherent. This technique would be also be limited by the absorption depth of
the gas used.
It is likely that in the regimes used for pressure-tuned phase matching in waveguides, low ionization and moderate pressure, the conversion efficiency is not maximized.
The ionization loss and modebeating simulations and measurements presented aboveshow that the intensity is likely not contained to the lowest-order, EH11 , propagation
mode. Varying intensities and localized regions of harmonic generation can lead to an
inefficient compensation of the phase mismatch, or unavoidable ringdown in the harmonic signal. Counterpropagating pulses may be useful for improving the obtainableharmonic signal. A long counterpropagating pulse could suppress out-of-phase emission
from a long coherence length or a region of coherent ringdown of the signal in a region ofstrong intensity fluctuation. Another option is to use a compressed counterpropagating
pulse to pre-ionize the gas. This is a potential way of suppressing the harmonic generation over an extended longitudinal region. At the low intensities used for pressure-tuned
phase matching, insufficient for generating harmonics from ions, the harmonic generation will be essentially shut down in the region after the collision of the two pulses. The
plasma will also tend to refract the driving laser beam. This technique was exploredbriefly, but without definitive results.
Several proposals [26,30] and one experimental demonstration [36] have dealt withthe manipulation of the gas density as a means of quasi-phase matching. Certainly, the147
gas density has a significant effect on HHG in many different ways. In the demonstrations of all-optical QPM and exploratory studies not presented here, it has been foundthat pressure ramps rather than constant pressure regions inside the waveguide produce
higher harmonic orders, or a brighter harmonic signal. One possible area of future study
is modeling of how pressure ramps affect both the local phase matching conditions andhow different pressure profiles could be used to facilitate pressure-tuned phase matching,minimization of the detriments of ionization loss, or to facilitate all-optical QPM.
Absolute harmonic photon yield, however, can sometimes be secondary to thequality of the harmonic beam. For certain applications of HHG, such as coherent imaging, the spatial coherence and mode quality of the harmonic beam is just as crucial as
the number of photons. Also important to imaging as well as molecular dynamics studies is the monochromaticity of the harmonic beam. Often multilayer mirrors and metal
filters are used to select a narrow bandwidth, but these techniques often have a poortransmission efficiency. All-optical QPM has been shown to be effective in selecting asingle harmonic, and selectivity is predicted to improve with both number of pulses andthe order of QPM. It is also effective in selectively enhancing a single trajectory. Interference between multiple trajectories can lead to a degredation of the spatial coherence,and so a strong selection of a single trajectory should improve the spatial coherence,
although this effect has yet to be shown experimentally. It is also likely that the selectivity of all-optical QPM will affect the spatial mode profile of the harmonic beam, sincedifferent trajectories have different phase fronts due to the intensity-dependent phaseaccumulation. This is also an effect that has not yet been measured and compared withpredictions. Finally, all-optical QPM should have an effect on the temporal structureof the attosecond pulse train, and further studies could show if proper implementation
of QPM with counterpropagating pulses would give more desirable temporal structures.
Pulse and beam shaping would be powerful tools in manipulating the properties of theharmonic beam in combination with all-optical QPM.

148
Lastly, in a proposal by Oren Cohen, QPM with counterpropagating light could
be extended to very short coherence lengths, on the order of a few microns, through atechnique called grating-assisted phase matching (GAPM) [126]. In this technique, aquasi-cw counterpropagating beam, rather than a series of pulses, is used to modulated
the phase of the driving laser. However, instead of using the counterpropagating lightto suppress harmonic generation, in GAPM the counterpropagating field periodicallycorrects for the phase mismatch. When the wavelength of the counterpropagating lightis matched to twice the coherence length, the phase of the driving laser is shifted at every
coherence length in order to allow coherent buildup throughout the interaction medium.
Optical parametric amplifiers (OPA’s) are likely necessary to generate enough energy inthe counterpropagating beam at the correct wavelength, on the order of microns. This
technique is promising in combination with plasma waveguiding for generating very highphoton energies. In plasma waveguides, harmonics can be generated in a pre-ionizedgas medium, giving higher photon energies due to the higher ionization potential of theions [127]. However, due to the high free electron density, the phase mismatch is very
high, creating ideal conditions for GAPM. Variations in the local phase mismatch could
be compensated through the use of pulse shaping to create the ideal counterpropagating
field.

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Appendix A
Variable Repetition-Rate Ti:Sapphire Oscillators

A.1

Introduction
Since the first demonstration of self-modelocking [128], ultrafast Ti:sapphire lasers

have become the workhorse devices for generating ultrafast pulses in the near infrared.
Typical modelocked oscillators operate at a repetition rate between 70 and 100 MHz,
with an output power of about 500 mW when pumped with 5 W of CW green laser
radiation. This corresponds to a pulse energy of about 6 nJ. Since the gain bandwidth of
Ti:sapphire is so large, pulse durations of 10 fs and shorter are routinely achievable [129].
Thus the typical peak output power of the standard oscillator is about 0.6 MW.
Several techniques have been demonstrated for increasing the peak power directly from an oscillator without the use of extracavity amplification. Cavity dumping
has been shown to generate peak powers of up to 5 MW [130, 131]. However, cavity
dumped lasers are complex, expensive, and generally more difficult to operate than asimple laser oscillator. Recently, alternative approaches to increasing the peak powerfrom oscillator have been developed by increasing the cavity length [132–134]. The
lower repetition rate allows for more energy in a single pulse for a given average power.
However, simply increasing the length of a Ti:sapphire laser cavity quickly results inan unstable geometry. By inserting a telescope, or multiple telescopes, into the cavity,
the overall physical length of the cavity can be increased without changing the roundtrip “ABCD” matrix [135] that determines the stability of the laser. This procedure162
has been demonstrated for repetition rates as low as 5.85 MHz with pulse durations
as short as 43 fs [133]. In some of these designs, the use of saturable Bragg mirror
reflectors (SBR) to prevent multiple pulsing limits the pulse duration obtainable fromthe laser. Alternatively, there has also been interest in the development of compact,high repetition rate lasers, which have applications in frequency metrology, high speed
communications, and biological imaging [136]. Several examples of high repetition rateoscillators have been demonstrated [137–141], some of which have repetition rates of
1 GHz or more. However, these designs are also more specialized and expensive, requiring custom coatings and optics, and are not tunable. Most are forced to sacrifice
bandwidth, average output power, or experimental robustness. The Kerr lens modelocking (KLM) mechanism that results in ultrashort pulse generation is simple in principle,
but is complex and incompletely understood in practice. Extensive work has been donein modeling KLM laser resonators using ABCD formalisms [142–144], and also using
more rigorous approaches including full space-time propagation models [145]. However,dynamics such as space-time focusing and self- phase modulation in the Ti:sapphire
crystal [146] are complex enough that modeling gives limited guidance on real world
usability and stability issues. As a consequence, experimentation is necessary for eachnew cavity design, and few variations have a robustness comparable to the “standard”
modelocked Ti:sapphire cavity design [129].
In this Appendix, I describe a very simple approach that can be applied to both
extending and shortening the length of a Ti:sapphire cavity. We use a simple asymmetric focusing geometry that alters the cavity length while preserving the overall cavity
propagation, and that provides the exceptional stability and ease of use inherent to thestandard cavity configuration.

163

A.2

TheoryThe basic cavity configuration of the modelocked Ti:sapphire laser is shown in

Fig. A.1, along with definitions of various cavity parameters.
Fused silica prisms

R 1 = 10 cm

L
dO.C. 12%R 2 = 10 cm

Figure A.1: Diagram of the standard Ti:sapphire cavity.

Calculations were performed to determine how the stability could be maintained
as the cavity length was altered. The dynamics of modelocking are neglected in thecalculation. As in previous research [133], the goal of these calculations is to constructa round-trip ABCD matrix that is effectively the same as the standard cavity, evenas the overall cavity length is altered. We can do this by changing the length L andthe radius of curvature R, of one or both “arms” of the cavity, as referenced to theTi:sapphire crystal. If the q-parameter is the same for the asymmetric cavity as for astandard cavity in cw operation, the idea is that the modelocking initiation procedureand behavior will be the same as well. Ignoring the astigmatism in the cavity introducedby the off-axis reflection, the round trip ABCD matrix for one arm of the cavity, startingfrom the edge of the crystal, reflecting from the curved mirror and to the plane mirror
and back, is given by





1
R

R − 4 (L + d) + 8Ld
R
4
R

2L
R −1





2
R


 
4Ld2
2
R (L + d) − 4Ld − 2d + R



1
8Ld
R
−
4
(L
+
d)
+
R
R

(A.1)

164
where L is the distance from the curved mirror to the output coupler, d is the distancefrom the curved mirror to the crystal, and R is the radius of curvature (ROC) of themirror. Generally in the cw Ti:sapphire cavity, R ≈ 2d. Setting R = 2d simplifies thematrix considerably to





0 


2L
−
1
−1
R
−1

4
R

(A.2)

By equating the value of the “C” element of the matrix for two different cavities,
we determine cavity parameters (Lb , Rb ), that give an overall ray matrix similar to thestandard cavity (La , Ra ). Lb corresponds to

1
Lb =
2

"

Rb
Ra

2

(2La − Ra ) + Rb

#

(A.3)

Using the parameters from the standard cavity, Table A.1 lists the corresponding values
for two possible asymmetric cavities, having altered the output coupling arm, whichgive the same ABCD matrix in this approximation.
Standard cavity
L = 60 cm
d = 5 cm
R1 = 10 cm

Low rep rate cavity
L = 230 cm
d = 10 cm
R1 = 20 cm

High rep rate cavity
L = 16.25 cm
d = 2.5 cm
R1 = 5 cm

Table A.1: Cavity parameters for ABCD matrices

Without changing the q parameter of the Gaussian beam, and therefore withoutchanging the laser stability, the distance to the output coupler may be nearly quadrupledby using a 20 cm ROC as one of the focusing optics, and it may be nearly quartered byusing a 5 cm ROC optic. The length of the prism arm of the cavity could be altered ina similar way.
The radii of curvature of the two focusing mirrors are different, and therefore theincidence angles must also be different in order to compensate for astigmatism. The

165
incidence angles for this laser were calculated using ABCD matrices [147, 148].

lc
cos θ =
2nL R



s


 
1
lc 2
1
1 2
−1 ∓
+ R2
1− 2
R
2nL
n2L
nL

(A.4)

Here lc is the length and nL is the refractive index of the Brewster angled crystal, R1
and R2 are the radii of curvature of the mirrors as indicated in Fig. A.1, and θ is theincidence angle. The angles of incidence for each of the curved mirrors were calculatedusing Eqn. A.4 and are listed in Table A.2. In all cases, nL = 1.75.
Standard cavity
lc = 4.75 mm
R1,2 = 10 cm

Low rep rate cavity
lc = 4.75 mm
R2 = 100 mm, θ = 7.5◦
R1 = 200 mm, θ =5.3◦

High rep rate cavity
lc = 3.00 mm
R2 = 50 mm, θ = 8.7◦
R1 = 75 mm, θ = 7.1◦

Table A.2: Astigmatism compensation angles

A.3

Low Repetition Rate Laser
DesignOur design for extending the cavity length of the Ti:sapphire laser requires chang-

ing only two optics in a standard Ti:sapphire laser: the output coupler and one of thecurved mirrors. Instead of using two identical mirrors with the same radius of curvature
to focus the beam into the Ti:sapphire crystal, this laser uses one mirror with twice theROC (20 cm) of the other (10 cm). This is the first time to our knowledge that suchan asymmetric cavity has been employed for the purpose of changing the repetition
rate of a modelocked Ti:sapphire laser, although past ABCD analyses for modelocked
Ti:sapphire lasers have included the possibility of an asymmetric cavity [143]. Asymmetric cavities have been demonstrated [149, 150] in modelocked Cr:LiSAF systems sothat they may be directly pumped by a single diode laser and have a small footprint. In
this case, the larger ROC optic allows the distance to the output coupler to be increased

166
significantly, while maintaining cavity stability as discussed above. The length of theprism arm remains unchanged. This results in a laser with approximately twice thecavity length and therefore half the repetition rate of the standard Ti:sapphire laser.
Fused silica prisms

Fold mirrors
R 1 = 20 cm

dO.C. 20%R 2 = 10 cm

Figure A.2: Diagram of the low repetition rate cavity.

The setup, shown in Fig. A.2, is quite similar to that of a standard Ti:sapphirelaser. The laser has two flat end mirrors, three flat fold mirrors, two curved mirrors
focusing into a Ti:sapphire crystal, and two prisms for intracavity dispersion compensation. The Ti:sapphire crystal is 4.75 mm long, doped at 0.15%. The three fold mirrors
and one of the end mirrors are dielectric and > 99% reflective at center wavelength 800
nm. A larger output coupler of 20% is used to suppress multiple pulsing and to increase
the output power. The curved mirrors, with radii of curvature 10 cm and 20 cm, arealigned in an astigmatism compensated X configuration about the crystal. The 10 cm
mirror was set to an astigmatism compensation angle of 7.5 ± 1.0◦ , and the 20 cm was
set to an angle of 5.3 ± 1.0◦ . The Ti:sapphire crystal is pumped by 4.75 W from afrequency doubled Nd:Vanadate laser (Coherent Verdi) at 532 nm. The pump beam is
focused into the cavity with a lens of focal length 10.5 cm through the R = 10 cm optic.
The flat side of the mirror was AR coated for 532 nm to minimize loss. The prisms are
Brewster cut fused silica, at a separation of ∼63 cm. The total length of the single passcavity is ∼333 cm, resulting in a pulse repetition rate of 45 ± 1 MHz, as measured by afast photodiode.

167
Performance
An extracavity prism pair compensated for the dispersion of the output coupler,
crystal, and pulse measurement optics. Calculations indicated that the equilateral,
fused silica prisms should be separated by about 100 cm in order to correct for GVD.
The compressed pulse was measured using SHG FROG [114]. The FROG trace wasdeconvolved using Femtosoft FROG3 software to yield a FWHM pulse duration of 15±2
fs, shown in Fig. ??(a). The pulse duration was limited by uncompensated third orderdispersion, as can be seen as a “ringing” effect at the leading edge of the pulse. Thisand the 1 fs resolution of the FROG setup were the main sources of uncertainty in themeasurement of the pulse duration. The transform limited pulse duration, determinedby an inverse Fourier transform of the experimental spectrum shown in Fig. A.3(b), isa) 1.0b)

2000

Intensity [au]∼13 fs.

1500

Intensity [au]

0.8
0.6
0.4

1000
500

0.2
0.0
-40

-20

0
20
Time [fs]

40

720

760
800
Wavelength [nm]840

Figure A.3: (a) The deconvolved pulse width and (b) experimental spectrum for the
low repetition rate laser.

When modelocked in the standard negative dispersion regime, stable, ∼15 fs
pulses were obtained at an average output power of 400 mW, with a typical power discrimination of 50 mW. At a repetition rate of 45 MHz, this corresponds to a pulse energyof 10 nJ, or twice that usually obtained from a standard Ti:sapphire laser operating at
such short pulse widths.

168
In order to initiate modelocking, we decrease the length d until the intracavity power reaches a value that favors stably modelocked operation, then introduce a
brief disturbance to initiate a pulse. This is the same procedure used for a standard
Ti:sapphire laser. However, for a similar bandwidth, the extended cavity laser operates
at a slightly lower average output power of ∼400 mW, likely the result of a somewhat lower than optimum output coupling. Modelocking is achieved as a result ofgain-aperturing, as in the standard Kerr lens modelocked Ti:sapphire laser. Stability islimited mainly by environmental factors- in our case from air currents and significant
temperature fluctuations. The laser would persist in modelocked operation for several
hours uncovered in the lab. The absence of multiple pulse instabilities, self Q-switching,and double pulsing was confirmed by observation of the pulse train by a fast photodiodeand a spectrometer.

A.4

High Repetition Rate Laser
DesignTo shorten the cavity length, we incorporated asymmetric focusing mirrors alongwith other techniques. Since the main limit on the length of the cavity is determined by
the prism pair, two steps were taken to minimize the prism separation. First, a shorter
Ti:sapphire crystal was used, introducing less dispersion. Second, chirped mirrors wereadded to the cavity, adding negative chirp and thereby reducing the prism separation.
This allowed us to shrink both cavity arm lengths. We also further shortened the cavity
by shrinking the arm lengths while maintaining the same arm-length ratio, until thelaser operation became noticeably less stable. The output coupling was also reduced to
3.5%, to compensate for a lower intracavity peak intensity.
The optimal length for the output coupling arm (L in Fig. A.1) is smaller thanthat predicted by Eqn. A.2. The value of this distance in the cavity demonstrated
was 11.5 cm, compared with the predicted 16.5 cm. According to ray-propagation

169
simulations, the astigmatism is quite large (a factor of 1.5 difference between the twodimensions of the beam waist) at stable resonator values of the ABCD matrix when
L = 16.5 cm. This astigmatism caused the unstable modelocking observed with thisconfiguration. Another reason for this discrepancy is that the dispersive arm of thecavity was also altered. Had the dispersive arm of the cavity remained similar to thatof the standard cavity, the prediction of Eqn. A.2 results in a stable, non-astigmatic
beam in the cavity, according to the ray-propagation calculations.

Chirped mirrors

Fused silica prisms

O.C. 3.5%

R1 = 5 cm
3 mm crystal
R2 = 7.5 cm

Figure A.4: Diagram of the high repetition rate cavity.

The setup for the high repetition rate laser is shown in Fig. A.4. The laser has twoflat end mirrors, two flat chirped mirrors, two curved mirrors focusing into a Ti:sapphire
crystal, and two prisms for intracavity dispersion compensation. The Ti:sapphire crystal
is 3 mm long, doped at 0.25%. One of the end mirrors is dielectric and > 99% reflectiveat center wavelength 800 nm. The chirped mirrors are a dispersion compensated pairwith a GVD of ∼ −60f s2 each, introducing a total of ∼ −480f s2 GVD with eightbounces round-trip. The OC is 3.5% transmissive. The curved mirrors, with ROC 7.5
cm and 5 cm, are aligned in an astigmatism compensated X configuration about the
crystal. The 7.5 cm mirror was set to an astigmatism compensation angle of 7.1 ± 1.0◦ ,and the 5 cm was set to an angle of 8.7 ± 1.0◦ . The Ti:sapphire crystal is pumped by 4.0
W from a frequency doubled Nd:Vanadate laser (Spectra-Physics Millennia) at 532 nm.

170
The pump beam is focused into the cavity with a lens of focal length 10.5 cm throughthe R = 7.5 cm optic. The flat side of the mirror was AR coated for 532 nm to minimize
loss. The prisms are Brewster cut fused silica, at a separation of about 25 cm. The
total length of the single pass cavity is ∼54.5 cm, resulting in a pulse repetition rate of
275 ± 1 MHz.
Performance
The pulse was compressed as described for the low repetition rate cavity, and thepulse duration was again measured by SHG FROG. The FROG trace was deconvolved
to yield a FWHM pulse duration of 14 ± 2 fs, shown in Fig. A.5(a), limited by uncompensated third order dispersion. The transform limited pulse duration, determinedby a Fourier transform of the experimental spectrum shown in Fig. A.5(b), is ∼10.3 fs.
When modelocked in the standard negative dispersion regime, stable, ∼14 fs pulses wereobtained at an average output power of 400 mW, with a typical power discriminationof 50 mW. At a repetition rate of 275 MHz, this corresponds to a pulse energy of about
1.5 nJ.
Modelocking is again achieved as a result of gain-aperturing. The procedure for
initiating and maintaining modelocking is also nearly identical to that of a standard
laser, except that the spatial mode of the output is not TEM00 at bandwidths greaterthan ∼40nm. These larger bandwidths are likely caused by single-pass self-phase modulation, which is not governed by the spatial modes of the cavity. However, stability isagain limited mainly by environmental factors. The laser would persist in modelocked
operation for several hours uncovered in the lab. The group of spectral peaks around875 nm is due to unidentified cavity dynamics, but contributes only a small amount tothe spectrum and does not affect the cavity perfomance. Although the spectra in Figs.
A.3(b) and A.5(b) have different structure, Fourier analysis shows that they will eachsupport a short pulse (13 fs and 10.3 fs respectively). The fact that the pulses shown in
the time domain, Figs. A.3(a) and A.5(a), appear similar, is a result of the fact that the171same compression scheme, with limiting third order dispersion, was used. The shape of
the pulses presented is dominated by the spectral phase rather than the shape of thespectrum. The particular shapes of the spectra are likely determined by the dispersionof the respective optics, particularly the chirped mirrors in the high repetition rate cavity, and the coating of the output couplers. The absence of multiple pulse instabilities,
self Q-switching and double pulsing, was confirmed by observation of the pulse train bya fast photodiode and a spectrometer.

0.8

400
Intensity [au]b) 500Intensity [au]a) 1.0

0.6
0.4

300
200
100

0.2
0.0
-40

-20

0
20
Time [fs]

40

0
700

750
800
850
Wavelength [nm]900

Figure A.5: (a) The deconvolved pulse width and (b) experimental spectrum for thehigh repetition rate laser.

We also investigated a symmetric cavity of comparable repetition rate which
employs two R = 5 cm curved mirrors in place of the asymmetric pair. This cavity
was observed experimentally to be unstable in modelocked operation and overall quitesensitive to alignment. ABCD matrix models confirmed this alignment sensitivity. The
asymmetric cavity did not have these stability issues, and operated with generally thesame stability observed in a standard 100 MHz laser.

A.5

Conclusions
In conclusion, we have demonstrated the operation of Ti:sapphire oscillators withnovel geometries. By constructing cavities with asymmetric pairs of curved mirrors,

172
we have demonstrated a simple method of altering the repetition rate of a Ti:sapphireoscillator while maintaining the simplicity of the standard cavity.
This technique is useful especially for applications in which a repetition rate withina factor of 2-3 of the standard 80-100 MHz is needed. Only slight changes to a standard
Ti:sapphire oscillator are needed to effect this result. For repetition rates outside thisrange, other techniques, such as cavity-dumping or chirped mirror based cavities, may
be appropriate. However, the cavities described above maintain characteristics similar
to a standard 100 MHz oscillator. Our results indicate that for low- and high-repetition
rate asymmetric cavities, both laser geometries are stable, easy to construct and to use,and can support the generation of sub-20 fs pulses, limited only by dispersion and theonset of multiple pulse instabilities.

Appendix B
High Harmonic/ Fundamental Beamsplitter

B.1

Introduction
High-order harmonic generation (HHG) has the potential to be a unique sourceof coherent, ultrafast light at high photon energies. One of the technical challenges
to the development of this source is the attenuation of the high-power fundamental
laser beam that typically propagates colinearly with the harmonic beam. In current
systems for generating high harmonics, either in guided [23, 35] or free space [10, 24]
propagation, the fundamental laser beam has a necessarily high fluence, which provides
the intensities required for driving the extreme nonlinear process. Pulse energies for thehighest demonstrated fluxes of HHG to date [24, 151] can reach up to tens of millijoules
within a duration of tens of femtoseconds. This level of power can optically damage
EUV optics or samples under study, saturate sensitive detectors, or indeed interferewith a physical process due to the strength of the optical field.
Thin metal filters [152] are commonly used as a way of separating the two beams.
The fundamental light is reflected, since its frequency is below that of the plasma frequency. Harmonic frequencies, on the other hand, are above the plasma frequency,
allowing passbands which depend on the absorption characteristics of the given metal.
However, metal filters are certainly a less than ideal solution. Filters with thicknessesof hundreds of nanometers are quite delicate, and are often not robust enough to withstand handling or the high fluence of the fundamental beam. Heat dissipation can be174a significant problem at the high vacuum (∼ 10− 5 torr) needed for EUV propagation.
Oxidation of the metals over time leads to degradation of the transmission of harmoniclight. Multiple filters, in combination with apertures, are required if the fundamental
transmission is to be kept at a minimum, and combinations of materials can be required
to achieve the necessary robustness and desired passband of photon energies. Hencethin filters can become an expensive, consumable solution for this problem. Other
techniques have also been proposed and in some cases implemented successfully, including the use of an annular fundamental beam [118] which can be apertured after some
propagation distance from the HHG interaction region, a dichroic beam splitter [153] for
separating narrowband fundamental and lower order harmonic frequencies, and recently,
a beamsplitter of Si, SiC, or Mo oriented at the Brewster angle of the fundamental frequency [154]. The major advantage of each of these techniques is their high damage
threshold or lack of consumables, reducing the costs of operation.
In this appendix, I describe a new dielectric beam splitter for separating the fundamental and high-order harmonic beams. The design involves a multilayer coating which
is antireflective for the broadband and powerful fundamental beam at a grazing angle
of incidence, allowing the much shorter wavelength harmonic light to be reflected fromthe top surface. An estimate of the performance was made for 45 eV light. Comparedto the transmission of two aluminum foil filters, the combination of the beamsplitterwith one aluminum filter improves the efficiency by about 5x and reduces the risk ofburning filters and/or samples.

B.2

DesignThe particular design for this beam splitter exploits the large difference between

the wavelengths of the light to be separated. The thin film structure is constructedentirely for interaction with the long wavelength light, near 800 nm, while the shortwavelengths (10-40 nm) interact only with the surface layer of SiO2 . Since EUV is175strongly absorbed by bulk material, the reflectivity is not achieved through a quarterwave or other thin film structure but through reflectivity at a grazing incidence angle
from the top surface. One great advantage of this strategy is the broad nature of thereflectivity, allowing this design to be useful for a very broad range of harmonic wavelengths, limited ultimately by the absorption characteristics of the surface material.
Unfortunately, since light near 800 nm is not absorbed by the materials used for thisdesign, it is also strongly reflected at grazing incidence. Furthermore, since the fundamental light is ultrafast, its bandwidth can be very broad, exceeding 50 nm FWHM.
Hence the multilayer structure must achieve the difficult combination of antireflection(AR) both for grazing incidence, and for a broad bandwidth [155]. The tradeoff then,involves minimizing the total reflected energy of the fundamental beam, made easierat low angles of incidence, while maximizing the total reflected energy of the harmonic
beam, which is easier at high angles of incidence.
Under these conditions, a good balance between reasonable reflection of EUV
and transmission of 800 nm was achieved at an incidence angle of 82-85◦ (8-5◦ grazing
incidence). The coating was an alternating material, 10-layer design, using SiO2 andHfO2 . Table B.1 lists the layer thicknesses for the original AR coating design. (Thisoriginal design was based on previously developed broadband antireflection coatings
found in Ref. [156].) The transmission curve at 85◦ incidence is shown in Figure B.1ain the red curve, showing a peak in transmission of ∼ 0.9 near 800 nm.
A sample coating was produced by collaborators at Colorado State University
using reactive ion beam sputtering with a Veeco SPECTOR IBS deposition system.
Ref. [157] describes some of the capabilities of this system. Characterization of thesample’s layer thicknesses was done in two ways: using a spectrophotometer and an
ellipsometer. The layer thicknesses obtained from these measurements are also listed inTable B.1, along with estimated uncertainties, described in more detail below.
Characterization was essential to calibration of the deposition source as well asMaterial

Design

HfO2
SiO2
HfO2
SiO2
HfO2
SiO2
HfO2
SiO2
HfO2
SiO2

448.16 nm
181.49 nm
112.05 nm
181.73 nm
111.46 nm
545.87 nm
111.36 nm
545.95 nm
111.94 nm
363.48 nm

Measured(Spectrophotometer)
472 (± 5) nm
188 nm117 nm
186 nm
115 nm
547 nm
115 nm
547 nm
120 nm
358 nmMeasured(Ellipsometer)
464 (± 3) nm
189 nm
115 nm
185 nm
120 nm
535 nm117 nm
540 nm
118 nm354 nm176

Table B.1: Layer thicknesses for broadband, grazing incidence, antireflection coating at
800 nm.

the efficiency of the AR coating. Several iterations led to the production of the sample described in this appendix. The optical properties are quite sensitive to variationsin the thicknesses at such a large angle of incidence, requiring a significant degree ofprecision in the deposition. The measurement of the layer thicknesses using the spectrophotometer was performed as follows. A spectrophotometer was used to measure
the transmission of the sample over a large range of wavelengths at normal incidence.
This data is plotted in Figure B.1b as the violet curve. Although the design for antireflection was for a grazing incidence angle, the spectrophotometer alignment was much
simpler for normal incidence, and this measurement could be easily compared with thepredicted behavior of the design at normal incidence. In addition, small differencesin the layer thicknesses may have a small effect at grazing incidence, but are more
distinguishable at normal incidence (as can be seen above in Figure B.1). Data fromthe spectrophotometer measurement were used as fit criteria for determining the actual
layer thicknesses using an optimization routine in TFCalc (an optical thin film design
software). Once layer thicknesses were determined which matched the behavior at normal incidence (listed in Table B.1), a prediction of the transmission at 85◦ incidence was
generated and is shown in Figure B.1a. This method of determining the sample’s actual

100
DesignEllipsometer fit
Spectrophotometer fit

80
60
40
20

b)

100

Transmittance [%]Transmittance [%]

a)

80

0

177

60
40
DesignEllipsometer fit
Spectophotometer
Measurement

20
0

500

600 700 800 900 1000
Wavelength [nm]500

600 700 800 900 1000
Wavelength [nm]Figure B.1: Calculated transmission of the beamsplitter at 85◦ (a) and normal (b)incidence, including the original coating design, and the fits corresponding to spectrophotometer and ellipsometer measurement.

layer thicknesses involved uncertainty in both the fit, but also the spectrophotometermeasurement, which is difficult to calibrate, since it is normally used to determine relative, rather than absolute absorption. However, the spectrophotometer measurement
was less sensitive to the smoothness of the surface. This uncertainty is reflected in theestimated error for the layer thicknesses listed in Table B.1.

b)
70 degPsi in degrees

80

75 deg60

65 degExperimental Data
Fitted Model

60 deg40
20

Delta in degrees

a)

200

Experimental Data
Fitted Model

60 deg65 deg150
100
70 deg50

75 deg

0

0
500

600

700
800
900
Wavelength [nm]

1000

500

600

700
800
900
Wavelength [nm]1000

Figure B.2: Ellipsometer measurements (black curves) and fitted model calculations(red curves) for Ψ (a) and ∆ (b).

A more reliable measurement of the layer thicknesses was made using a J.A.

178
Woollam ellipsometer. This measurement characterizes thin film coatings by comparing
the reflectivities at various incidence angles of s and p polarizations. Specifically, given
the quantity
Rp= tan Ψei∆ ,
Rs

(B.1)

where Rp and Rs are the Fresnel reflection coefficients for s and p polarizations, respectively, the ellipsometer measures the values of Ψ and ∆ as a function of both specified
wavelength and incidence angle. From this information, it can fit the measured data to agiven coating structure to determine the specific layer thicknesses. The raw data, alongwith the fits produced by the accompanying software, are shown in Figure B.2. Data
was collected at 60◦ , 65◦ , 70◦ , and 75◦ incidence, over the wavelength range 500-1000
nm. One aspect which proved to be significant in the correspondence of the fits and themeasured layer thicknesses was the particular indices of refraction. Measurements of
the indices of SiO2 and HfO2 , provided by researchers at CSU, allowed much closer fits
than those obtained with the default data provided with the software. The measured
layer thicknesses and corresponding transmission curves are also presented in Table B.1
and Figure B.1, respectively. Uncertainty estimates include both the error in the fit, as
well as measurement error. These error values are smaller due to the careful calibration
routines performed and the closeness of the fits.

B.3

Beam Splitter Performance
The beam splitter sample was found to allow significant reflection of the EUV

wavelengths from the top surface of SiO2 at grazing incidence. Figure B.3 shows thepredicted [78] reflectivity calculated assuming a thick (>100 nm), perfectly flat top layerof SiO2 . The blue curve shows the reflectivity, at 8◦ grazing incidence of the the sample
described above in Section B.2. This measurement was performed at the Advanced Light
Source by collaborators at the Lawrence Berkeley Laboratory. The measured reflectivity

179

1.0
82deg incidence

Reflectivity

0.8
0.6
0.4

Measured
Calculated

0.2
0.0
15

20
25
30
Wavelength [nm]35

Figure B.3: Predicted (red) and measured (blue) reflectivities of the beam splitter at
EUV wavelengths.

is significantly smaller than that predicted. This discrepancy is most likely due either
to variations in the flatness of the surface, caused by variations in the deposition of
the AR coating, or absorptive surface contamination. The surface smoothness andflatness are mostly likely the limiting factors in the ultimately achievable reflectivityof the harmonic (EUV) wavelengths. Especially at such large incidence angles, even a
relatively small beam of ∼ 1-2 mm in diameter will reflect from a much larger area on
the substrate. Further improvements could include the use of superpolished substrates,and development of the coating capabilities and performance.
After the characterization of the EUV reflectance, a study was made of the transmission of typical spectra present in the fundamental beam. In particular, since theantireflection efficiency of the coating is highly dependent on the incidence angle, it was
important to determine at which angle the beam splitter should be oriented for efficientand broadband transmission of the NIR light. Because of the slight differences between
the design and the produced sample coating, measurements were needed to determine

180
whether the AR coating was efficient at an incidence angle high enough for significant
reflection of the EUV. This was also a secondary evaluation of the accuracy of the prepared AR coating sample. Figure B.4 shows the typical spectrum from a broadband

Intensity [a.u.]

3500

Incident Spectrum
Reflected Spectra
80 deg 84 deg
82 deg 86 deg

3000
2500
2000
1500
1000
500
700

750
800
850
Wavelength [nm]900

Figure B.4: Measured spectral reflectance of a typical broadband spectrum from a
Ti:sapphire oscillator, for a variety of incidence angles.

Ti:sapphire oscillator along with the spectra reflected from the beam splitter sample
at various angles of incidence. It is clear that the reflectance of the beam splitter far
from the transmission peak increases with increasing angle of incidence, as expected.
However, at the transmission peak of the AR coating, the reflectance remains low up
to an angle of 84◦ . In fact, the integrated reflectance of the beamsplitter over 700-900
nm is ∼45% of the incident spectrum. If the spectrum is truncated to 750-830 nm, as a
mimic of the bandwidth of a typical amplified spectrum, this efficiency is improved toa reflectance of ∼30% of the spectral energy.

181

B.4

Analysis and Conclusions
The beam splitter design presented here is a robust and useful way of reducing

the transmission of high fluence 800 nm light which propagates colinearly with highharmonic generation. However, the design has certain limitations which must be considered before using the beam splitter as a replacement for the more costly method ofthin metal filters. Ultimately, this design’s utility will be determined by its ease of use
and efficiency compared to other techniques. As an example, consider the harmonic
wavelength of 30 nm (45 eV), which can be well phase matched, and is therefore used
often in HHG applications. The fundamental light may be effectively rejected by two
200 nm thickness aluminum filters in series. The typical transmission of a single filter,
taking into account the transmission of aluminum and aluminum oxide, is about 0.1,
making the total transmission 0.01. Using a single beam splitter with an efficiency of
0.5-0.6 in combination with a single aluminum filter should also eliminate the fundamental light and increase the total efficiency by a factor of 5-6, while reducing the riskof burning the filter.
One consideration unmentioned so far is scattering of the fundamental light. Samples produced so far were coated on round substrates of 1 inch diameter, which was
determined to be large enough to reflect the entire HHG beam at a reasonable distance(∼50cm) from the nonlinear generation region for the optics to be mounted under vacuum. However, this aperture is significantly smaller than the width of the fundamental
beam at this distance (∼ 2-3 cm). Thus precautions must be taken against the scatter of light, either which does not encounter the surface of the beam splitter, or thatwhich transmits through the beam splitter. It is likely that an optic coated on bothsides, allowing transmission of the beam completely through the optic would allow easier
management of the scattered light than a wedged optic.
Related to the reduction of scattered light is the engineering consideration of the

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beam splitter’s mounting in the vacuum line which allows propagation of the harmoniclight. Takahashi et al. [154] use two Brewster-angled Si beam splitters in series, sothat the harmonic light has only a lateral offset, but propagates parallel to its original
direction. An advantage of this setup is that it could be aligned at atmosphere witha visible light source. However, two reflections, while reducing the fundamental light
power, would not eliminate it below a factor of ∼ 10−2 , and for some applications may
require an additional thin metal filter. If such strong attenuation of the fundamental
light is required, the transmission of the EUV may not ultimately be improved over theuse of metal filters alone.
Another limitation to the beam splitter described above is the limited reflection
bandwidth in the EUV. In this design, the surface layer used was SiO2 , which has anabsorption resonance at 99 eV, limiting the range of efficient reflection of harmonic light.
Since HHG photon energies extend well above 99 eV, variations in this design will be
required to extend the reflection bandwidth. The use of this material was determinedby availability of deposition materials, but other low index materials, such as ZrO2 , orother low/high index combinations of dielectrics may be considered.

Appendix C
Alignment Procedure for a Ti:Sapphire Oscillator

C.1

Introduction
This appendix contains an informal manual for alignment and operation of a

Ti:sapphire oscillator of the type described in Ref. [129]: a prism-based dispersion compensation, soft-apertured, Kerr-lens modelocked (KLM) oscillator. This is the type ofoscillator commonly used in our labs, and the following manual was written with theuninitiated in mind. In that spirit, the origin of different mechanisms and physicalprinciples are not cited within. For the interested reader, there is a vast amount ofliterature on the operation and nonlinear optical dynamics in such lasers. As a starting
point, there are the original report of KLM in Ti:sapphire [128], a review on femtosecond
solid-state lasers [158], and theory of KLM [159].

C.2

Components
The efficiency and stability of a Ti:sapphire femtosecond laser are only as goodas its components. It pays to use very stable optomechanics. In particular, the mounts
used in the cavity are most preferably Lees, Newport Ultima, or similar quality mountson 1” diameter posts for stability. Posts of 1/2” diameter in combination with post
holders will noticeably affect the stability of modelocking and the output power of thelaser, as well as beam steering. Also, stability counts in preventing misalignment fromexternal vibrations and bumps.

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The cw pump laser should have a Gaussian, TEM00 mode, and a wavelength
near the peak of the absorption bandwidth of Ti:sapphire. Often used are frequencydoubled, diode pumped Nd:Vanadate lasers at 532 nm or flashlamp-pumped argon ion
lasers operated at the 514 nm line. For pump beam steering, broadband or green
dielectric mirrors are necessary. Silver coated mirrors are less efficient, and will also
distort or even burn with the intensity from a 4-5 W pump laser. This affects not only
the efficiency of the oscillator, but the stability of the modelocking, since this is very
sensitive to the mode of the pump beam focus at the crystal.
The fused silica, Brewster angle prisms must be mounted so that they are flaton the translation stages, and that the base of the prism is parallel to the side of thetranslator. If this is not carefully done, the translation of the prisms will cause unwanted
deflection of the beam. For a typical, “standard” cavity, the titanium-doped sapphire
crystal has 0.33% doping, figure of merit (FOM) >150, and a path length of 4 mm.
The amount of doping influences the intracavity power, and hence the amount of pump
power needed for a given output coupling. The length of the crystal will affect the total
intracavity dispersion, and hence the separation of the prisms.
All mirrors except the output coupler should have a highly reflective (>0.99),
broadband coating. The reflection bandwidth and dispersion of the output coupler areoften limiting factors in the achievable output bandwidth. The curved mirrors should
be antireflection (AR) coated for the pump laser’s wavelength on the planar side, andhave a curvature of R = 10 cm on the concave side. The output coupling should be∼12%, for a pump power of ∼4.5 - 5 W. Different amounts of output coupling will
determine the appropriate pump power, and will affect the amount of average output
power. In order to work stably in the “standard” configuration, the oscillator needs anapproximately constant intracavity power.
Figure C.1 shows relevant parameters in the cavity, as well as the beam path ofthe linear resonant cavity. The light has, in a single round trip of the cavity, one bounce

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each on the end mirror (EM) and output coupler (OC), and two bounces each on thetwo curved mirrors and the fold mirror (FM), and passes through the crystal and eachof the prisms twice. These must all be considered when determining the round trip
dispersion or loss.

EM
P1
d

e

f
P2

c
FM
a

CM

OC

b

θ

Figure C.1: Parameters of a standard Ti:sapphire laser cavity. a∼62 cm, b∼10.4 cm,
θ ∼16◦ , c∼22 cm, total prism separation (d+e)∼62 cm, f∼5 cm Abbreviations aredefined in Table C.1.

OC
FM
CM
EM
P1
P2

Output Coupler
Fold Mirror
Curved Mirror
End Mirror
First Prism
Second Prism

Table C.1: Abbreviations for cavity elements (shown in Figure C.1) used throughout
the appendix.

The path lengths within the cavity are important for correct dispersion compensation and modelocking, and the reflection angles from the curved mirrors compensate
the astigmatism caused by the crystal. The crystal should be mounted at Brewster
angle, and this can be adjusted by eye (at low pump power) by adjusting the angle until
the reflected pump beam is at minimum intensity. Incidentally, the polarization of the186pump beam must be parallel to the table for the Brewster angle of the crystal as shownin Figure C.1.

C.3

Alignment
Step 1: Align the pump beam along the rail, at low power (∼ 10 mW or less).

For consistency, the pump beam should be parallel to both the rail (in the horizontal
plane) and the table (in the vertical plane) when there are no optics present. This may
be done by removing all optics and aligning with two mirrors and two pinholes. The
height of the beam may be established, if necessary, by the height of the crystal. Next,
replace the green focusing lens so that the beam passes through the center of the lens,and translating the lens does not deflect the beam from the second pinhole (this is moreaccurately done by propagating the beam farther, if possible). Then the curved mirrors
and crystal may be replaced. The beam should pass through the crystal at the focus of
the lens, and roughly through the centers of the curved mirrors. There may be defects
in the crystal which scatter the pump beam and therefore must be avoided. The two
curved mirrors should be symmetric about the crystal, roughly 10.4 cm apart. The
laser is easier to align when the curved mirror, through which the pump beam passes,
is stationary and all translational adjustments are made with the other curved mirror,
denoted CM in Figure C.1. For detail of the crystal and both curved mirrors, see Fig.
C.2.
Step 2: The KMLabs commercial rail is designed so that the beam which propagates toward the OC should line up with the tapped-hole grid of the table. In otherwords, the central translational axis of the rail rests at an angle of 16◦ to the grid ofbreadboard or table. The reflection of the CM to the OC should be parallel to the grid.
Use the green light to retroreflect from the OC to the CM.
Step 3: Now the pump power should be increased, with care, to 4.5 5.0 W. At
this pump power, there will be a bright, reddish fluorescence propagating through thef=11 cmlens

stationary
mirror187

10.4 cm

crystalmoveable
mirrorFigure C.2: Positions of optics on rail.

cavity to allow alignment for lasing. Low room lights will improve the visibility of thefluorescence. For convenience, set the prism translation stages at the middle of theirscale when the maximum amount of visible fluorescence passes through. (Eventually,
the prisms will be adjusted so that the beams propagate through the minimum amountof glass, to reduce total dispersion. However, this does not affect cw operation, andalignment is easiest with the greatest amount of fluorescent light propagating throughthe cavity.) Set P1 at minimum deviation, adjust the FM so that the incidence angle
is small, then set P2 at minimum deviation. Finally, retroreflect the fluorescence spotwith the EM.
Note: Minimum deviation describes the angle at which the beam both entersand leaves the prism at Brewster angle, and so passes through the material of theprism parallel to its base. Of course, this is precisely true for only one wavelength, sowith a broad band of fluorescence, the spot will be slightly dispersed horizontally by
the prisms. To find the proper angle, rotate the prism on its mount (preferably withthe prism centered on the rotation axis) to change the propagation direction of thefluorescence through it. Rotate in one direction until the deflection of the fluorescencespot reaches a point where it stops and begins to reverse direction. This point where themovement of the propagating light changes direction is the minimum deviation angle.

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Greater accuracy can be achieved by propagating the beam over a long distance (∼ 1
m or more).
Step 4: If the OC is retroreflecting well, and the rail optics are close to theiroptimal positions, there should be a characteristic shape to the fluorescence at P1, asshown in Fig. C.3a. The diameter of the larger, diffuse red spot should be roughly thesize of the prism. This is the light reflected directly from the crystal, and its size may be
adjusted by the position of the crystal. The smaller, focused spot is the light reflectedfrom the OC. It may not be in focus at P1, but this can be achieved by adjusting thetranslational position of the CM reflecting to the output coupler. Once this shape isseen at P1, the spatially dispersed shape to the fluorescence should be seen at P2, seenin Fig. C.3b. If this is not what the fluorescence looks like, small adjustments can bemade in the translational positions of the CM and crystal.

a)b)

Figure C.3: Appearance of fluorescence at P1 (a) and P2 (b).

Step 5: At this point, the retroreflected beam from the EM must be aligned
to overlap with that of the OC. The two beams can be viewed with an index card
at the FM between the prisms. The retroreflected beams can be viewed often only
one at a time, since the index card blocks the propagating fluorescent light. If thecrystal and CM can be adjusted so that the two spots of fluorescence are focused at
the FM, this is much easier to do. When the beams are aligned, lasing can be initiatedby small adjustments to the OC, EM, and the position of the CM. (In fact, optimumalignment for lasing often occurs for a different position of the CM than was convenientfor viewing and aligning the fluorescence.) The oscillator will lase only when the mirrors

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are aligned fairly accurately, and the curved optics and crystal are in approximately thecorrect positions. The distances between the curved mirrors and the endmirrors (a andc-f in Fig. C.1) are not as crucial for cw operation; these become more important formodelocking stability. It is helpful to make sure that the fluorescence is passing throughthe centers of the prisms (keep in mind that some of the fluorescence is infrared, andtherefore invisible). When modelocking later, the prism insertion will likely require
adjustment for optimal dispersion compensation.
Step 6: Once the laser lases, the peak power can be increased by careful alignment.
One method which seems to work well for this is iterative adjustment of: the horizontal
and vertical tilt of the EM and OC, then small tweaks on the CM, crystal, and lenstranslational positions. At 4.5 - 5.0 W of pump power, the laser should easily have an
output power of about 600-700 mW, and with a very careful alignment and depending on
the exact output coupling, up to 1 W. If it is difficult to achieve these output powers, it
may be that the optics are backwards in their mounts, there is clipping of the intracavity
beam, or that the relative distances of the rail optics are incorrect. Using a tape measure
to set the positions of the rail optics should be sufficient to correct the latter problem.
Another diagnostic strategy for tweaking up the cw power is to align the green
and red beams in the crystal so that there is efficient coupling between the pump beamand the red beam. To do this, look at the scatter of both beams (this works best withamber goggles intended to block 514 nm) on the surface of either of the curved mirrors.
The red beam may be made more visible by adding more prism glass until the laser
lases at shorter, visible wavelengths. The red beam should appear very slightly to theright of the green beam (see fig. C.4). This is because the two different wavelengths
will be refracted at slightly different angles by the crystal. The exact positions of thetwo beams is not as important as getting the best coupling between the two modes.
Alignment for highest power should correlate with this configuration, unless the red
beam is clipped somewhere within the cavity. High power with significant separation

190
between the red and green beams, or with the red to the left of the green beam suggestthat the red beam may be clipped.

Figure C.4: Appearance of the green and red beams at either of the curved mirrors for
maximum coupling between the pump beam and the red beam.

For modelocking, one of the critical parameters is the distance between the CM
and the crystal. In the “standard” configuration, the oscillator will lase for a rangeof values for this distance. When the oscillator is running well for cw operation, as
described above, there will be two “stability regions” in which lasing will occur. Startingwith the largest distance between the CM and the crystal at which the cavity is stilllasing, and moving the CM inward, the laser will at one point stop lasing, start again
as the mirror is moved further, then stop a second time. Modelocking will occur moststably when the CM has been moved to the “inside” of the “outer” stability region, orin other words, just before the first cease of lasing as the CM is moved inward toward
the crystal. When the laser is aligned well in cw operation, it should have highest power
when the CM is farthest from the crystal.
Step 7: Running at high output powers and aligned well for cw operation, the laser
may now be slightly misaligned in a specific way to favor pulsed operation. This effectis commonly known as Kerr-Lens Modelocking (KLM), and is a passive modelocking
mechanism. First, pull the prisms back so that the beam passes through their tips,
taking care that the beam is no clipped, especially at the first prism. Move the CM
toward the crystal until the output power is reduced to about 350 mW, or until the
shape of the mode beyond the OC is elongated slightly to an oval shape (see Fig. C.5).
Use only the OC and EM to tweak up the power as high as it will go. Then repeat
these two steps until the power no longer increases with adjustment of the OC and EM.

191
Give the translation stage of one of the prisms a quick, slight push to introduce a brief
fluctuation in the intensity of the beam. Sometimes a tap on one of the mirror mounts
is also sufficient. Because the cavity is aligned to favor modelocked operation, a small
peak in the intensity of the beam will be amplified into a pulse train by the Kerr lenseffect of the crystal.

Figure C.5: Appearance of the (cw) output mode when the laser is aligned to favormodelocked operation. When in a stable modelocking configuration, the modelocked
mode should collapse to a more circular shape.

Once the oscillator is modelocked, the beam should collapse into a more circularshape and will lose its characteristic cw speckle. The power may be be tweaked up
by very slight adjustments to the EM and OC. Typical average powers from a “standard” modelocked oscillator are 400-500 mW. The modelocking is most stable when
there is “positive discrimination” in the average output power, meaning that the powerincreases when the laser switches from cw to modelocked operation. For stability, thediscrimination should fall within the range of 50-100 mW difference in the power. The
second prism may be translated to adjust the dispersion characteristics of the cavity
to facilitate modelocking. The laser will modelock stably when there is a small, net
negative, linear dispersion. This is because the self-phase modulation in the Ti:sapphire
crystal gives a slight positive dispersion.

C.4

Diagnostics and Common Instabilities
Intracavity Power
Stable, long-term operation of a modelocked Ti:sapphire oscillator depends on

192mechanical and temperature stability. However, there are certain common problems
associated with drift of the cavity alignment that can be readily diagnosed and addressed. One easy way to tell if the oscillator is close to modelocking is to look at theoutput with a fast photodiode and an oscilloscope, or a spectrometer. When it is close
to modelocking, the oscilloscope signal should show a pulse train briefly when you tap
the prism. Among the common reasons that the oscillator does not modelock is thatthe intracavity power is too high or too low, or that the total intracavity dispersion isincorrect. Intracavity power may be adjusted by the amount of pump power. For a
10% output coupler, 4-5 W is appropriate, for 20%, 6-7 W. Also, the peak power at the
crystal increases with the amount of bandwidth, as the pulse duration is assumed to betransform-limited at the crystal.
Intracavity Dispersion
The intracavity dispersion may be adjusted by the amount of prism glass. The
separation of the prisms determines the amount of negative second order dispersion; inserting more prism glass adds more positive second order dispersion. Stable, broadband
operation is optimal in the so-called “negative dispersion” regime. This refers to the
net amount of dispersion from the prism separation (anomalous) and prism glass andsapphire material dispersion (normal). When there is slightly more anomalous dispersion from the prisms, it can partially compress the extra frequencies generated in the
crystal due to self-phase modulation. In this regime, the spectrum may be broadened byadding more prism glass into the beam path. When there is a net normal, or “positive
dispersion,” the output spectrum will appear truncated, and narrow with added glass.
Second order is the only adjustment with the prisms. Third order dispersion may
be minimized by setting the prisms at a separation such that there is the minimum
amount of prism glass in the beam path. The third order dispersion of fused silica has
the opposite sign of that of sapphire, making it a good choice for the prism material. For
cavities which use fused silica prisms as the sole dispersion compensation mechanism,

193
third order dispersion will always be the limiting factor in the number of modes which
can propagate with the same round-trip time.
Despite third order dispersion, very broad bandwidths can be achievable directlyfrom Ti:sapphire oscillators. This is often due to spectral broadening in the sapphire
crystal due to the third order nonlinear effect known as self-phase modulation. For verybroad spectra (≥200 nm tail-to-tail), often this broadening is achieved in the final passthrough the crystal, and has a characteristically poor mode quality. This is because theoptical coatings are often not reflective over such a large bandwidth, and leakthrough ofthe visible wavelengths can be observed in this situation. Thus, there is often a tradeoff
between bandwidth and mode quality. For a poorly shaped mode which is not due tothis effect, corrections can often be made through adjustment of the crystal position.
Double Pulsing
Double pulsing is a common instability which occurs when there is too much
intracavity power for the Kerr lensing mechanism to passively modelock the cavity
stably. Symptoms of double pulsing are a large output power, a periodically modulated
spectrum, or a pulse train at double the expected repetition rate of the cavity. Thismay most often be remedied by reducing the pump power. However, double pulsing
may occur when the CM has not been moved close enough to the crystal (see step 7 onmodelocking the oscillator) or is otherwise in the wrong stability region.
Spontaneous Q-switching
Self-Q switching is another common instability. This is an unstable periodic
modulation on the pulse train with a period on the order of picoseconds, and is easily
seen with a fast photodiode. It often appears when the prism is inserted in order toincrease the bandwidth. The beam intensity may also appear to flicker. This problem
may be fixed by turning the pump power up or adjusting the EM or OC. It can also be
eliminated by changing the position of the CM or crystal.

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CW-BreakthroughAnother power-related instability is referred to as cw-breakthrough. This occurs
when the intracavity power is too high for purely modelocked operation, and an extra
cw mode propagates simultaneously. This can be corrected by reduction of the pump
power, or moving the CM toward the crystal slightly.