Novel Ground States of Bose-Condensed Gases
by
Jamil R. Abo-Shaeer
Submitted to the Department of Physics
on October 1, 2004, in partial fulfillment of therequirements for the degree ofDoctor of Philosophy

Abstract
Bose-Einstein condensates (BEC) provide a novel tool for the study of macroscopic
quantum phenomena and condensed matter systems. Two of the recent frontiers,
quantized vortices and ultracold molecules, are the subject of this thesis.
The formation of highly-ordered vortex lattices in a Bose-condensed gas has been
observed. These triangular lattices contain more than 150 vortices with lifetimesof several seconds. The vortices were generated by rotating the condensate with ascanning blue-detuned laser beam. Depending on the stirrer size, vortices were either nucleated at discrete surface-mode resonances (large beams) or over a broad
range of stirring frequencies (small beams). Additionally, the dynamics of the lattices have been studied at finite temperature by varying the condensed fraction of
atoms in the system. The decay of angular momentum is observed to be strongly
temperature-dependant, while the crystallization of the lattice appears to be insensitive to temperature change.
Recently, the field of BEC has been extended to include cold molecules. Hereultra-cold sodium molecules were produced from an atomic BEC by ramping anapplied magnetic field across a Feshbach resonance. These molecules were used todemonstrate coherent molecular optics. In particular, we have extended KapitzaDirac and Bragg diffraction to cold molecules. By measuring the Bragg spectrum of
the molecules immediately after their creation, the conversion from atoms to molecules
was shown to be coherent - the matter wave analog to frequency doubling in optics.
In addition, the more general process of sum-frequency generation was demonstrated.
Atoms prepared in two momentum states, prior to creating molecules, were observed
to cross-pair, generating a third momentum state. Finally, molecular matter-wave
interference was realized using an autocorrelation technique.
Thesis Supervisor: Wolfgang Ketterle
Title: John D. MacAurthur Professor of Physics

For my family,
Nadya, Amir, Anita and Muhsin.

Acknowledgments
In my time in the Ketterle lab I have witnessed the group grow by leaps and bounds.
When I arrived at MIT there were only two sodium experiments. Now we have arubidium and lithium machine as well. Because of this, I have had the pleasure ofworking with many great people over the last five years and my acknowledgements
are numerous. It’s impossible to do each person justice in one or two sentences, but
in the interest of brevity I must try. For the purposes of bookkeeping, I will try to
go through lab by lab, although this will not be the rule.
First, I would like to thank Wolfgang Ketterle for giving me the opportunity towork in his lab. I only hope that I have been able to repay him in my time here.
Wolfgang’s cleverness is well-documented, so I needn’t restate this fact. Rather, I’dlike to thank him for his kindness and skill for inspiring excitement about physics.
In addition, Wolfgang’s ability to keep us feeling good about our work when we mostneeded it will always be appreciated.
When I arrived at MIT I was assigned to the “New Lab”, the newly christened,
2nd generation BEC machine. In the beginning I had the benefit of working with three
wonderful postdocs: Roberto Onofrio, Johnny Vogels, and Chandra Raman. Each
had his own unique set of talents that contributed to my development. The four of us
worked together on the second critical velocity experiment. Despite playing a smallrole in the experiment, I had more fun with this project than any other I’ve been apart of, and our off-key sing-a-longs are now a late-night standard in the New Lab.
Roberto Onofrio was the first to take me under his wing, showing me how to run
the machine. Roberto’s easy-going nature was a calming force in a lab known for
its “strong personalities”. His sense of humor kept us going during many frustratingnights. In particular, his impressions of members of the greater atomic physics community are second to none. Additionally, I thank him for his continued support andadvice throughout my career.
Johnny Vogels and I had differing styles to say the least. This led to many
“disagreements”, but just like family we always resolved our differences quickly. Onesimilarity that Johnny and I did share was our eagerness in lab. Johnny’s spirit was
contagious, and he always kept things lively and fun. His free thinking led him topursue many crazy ideas that didn’t work and even crazier ones that did. It’s taken
me years of experience in the lab to fully appreciate Johnny’s brilliance.
My time working with Chandra Raman was unforgettable. For my development
as an experimental physicist I owe the greatest debt of gratitude to him. Chandrataught me most everything I know about BEC experiment and almost every good
habit I have in lab is due to him. I greatly appreciate that he would step back andgive me time in lab to work things out until I got them right. It was comfortingto know that he was always there to put me back on track when I was confused or
frustrated. His grad students are lucky to have him.
I’d like to thank Chris Kuklewicz for “showing me the ropes” in lab, and at MIT,when I first arrived. Special thanks also go to Dallin Durfee, and Michael Köhl.
I didn’t have the opportunity to work with either of them substantially, but I am
grateful for their help in leaving such a wonderful experiment for me to work on.
Kaiwen Xu arrived in lab a year after me. At first I wasn’t sure that we had muchin common. But our mutual love of basketball quickly brought us together. Kaiwen
and I endured much frustration working together on optical lattices, but we also had
a lot of fun. Kaiwen’s talent in both experiment and theory have made him an ideal
coworker (and voice of reason). It’s been a pleasure to work with him and I will sorely
miss his fall-away jump shot and vastly underrated sense of humor.
Towards the end of my stay I had the pleasure of working with two wonderful,
but vastly different individuals: Takashi Mukaiyama and Dan Miller. As a postdoc
in the New Lab, Takashi established himself as a quiet leader. He was fun to workwith and his intricate electronic inventions always amazed me. I learned a lot fromTakashi, and I’m very sorry for what he learned from me. On one frustrating day I
was horrified to find Takashi transcribing some of my particularly strong language inorder to help himself learn English.
I can leave MIT confident that the quirky tradition and often erratic behavior of
the New Lab is left in the buzz-saw hands of Dan Miller. Hollywood’s eagerness andsense of humor provided a much needed shot in the arm at a time when work in lab
was particularly frustrating. Despite the obvious embarrassment it would cause him,
Goose’s gift of “Song 3” to the Ketterle Lab proved that he is the ultimate teamplayer. I only hope that Soldier Boy’s pain was worth the joy it brought to the restof us. So C.O.G.S., I thank you for being a great labmate and friend.
Any discussion of the New Lab would not be complete without mentioning its
forgotten member. My first memories of MIT are the times I spent talking to Zoran
Hadzibabic. Zoran’s “strange” sense of humor always kept me entertained. I will
always regret not having the opportunity to continue working with him. However,
we did have our fare share of communication outside of lab. Zoran and I had many
profound discussions. The shortest being a knowing glance to me as he passed by myoffice, and the longest going from lab to the Miracle to the cold streets of Cambridge
for another 4 hours.
I had the honor of entering MIT alongside Aaron Leanhardt. I could not havepicked a better person to go through this experience with. Although I’m sure that
it was an easy choice, I will always be indebted to Wolfgang and Dave Pritchard
for choosing him. I could write several pages about Aaron, but I’ll try to keep it
brief. Aaron has been a great labmate, roommate, and friend to me. Over the past
5 years we’ve done problem sets, played and watched about every sport, worked, ateand lived together. Most of my favorite memories at MIT involve him. Cooking
Thanksgiving dinner for the lab, watching him make the opposition look silly in IM
football, filling our apartment up with a half ton of sand, and going with him to theemergency room after he shattered the lab obstacle course record (and the glass in
Bldg. 36), are just a few. Inside and outside of lab Aaron never ceases to amaze me.
His skills as a physicist are unquestionable. But besides being able to answer any
question you throw at him, experimental or theoretical, Aaron also makes a better
Christmas wreath, runs faster, and consistently eats the same meal better than any
graduate student I’ve ever seen. I’ve got high expectations for him and I hope that
our work allows us to continue our friendship for many more years.
As the grad students one rung above me, Ananth Chikkatur and Deep Gupta

were great role models both inside and outside of lab. They helped Aaron and me
get our first apartment at 4 Marion (right below theirs). My discussions with Ananth(which invariably ended with him telling me I was crazy) were a constant source ofamusement. Deep’s level-headiness when those around him were going crazy and his
ability to strike very thoughtful poses always impressed me. I will always cherish
their sendoffs from lab: Ananth drumming on his back in a pile of sand in my livingroom and Deep’s emergenece as the undisputed oil-wrestling champion of the lab.
The Old Lab/Science Chamber has had a revolving door of great students andpostdocs. I always enjoyed discussing physics, politics, and basketball with Axel
Görlitz. More recently Yong-Il Shin, Tom Pasquini, André Schirotzek, and Michele
Saba have joined the effort. Besides being a great physicist, Yong’s skills as a midfielder have provided our soccer team some much-needed credibility. Tom has gone
above and beyond the call of duty in his short time at MIT. He spearheaded a successful effort to provide free healthcare for MIT graduate students. As a true Berkeleyan,
he fought the good fight and I eagerly await his return to the East Bay. In addition to
being a great guy, Andre provided solid blocking for our IM football and I thank him
for never taking me up on my numerous offers to box/wrestle/fight him. Michele’s
cheeriness and good humor have been a great addition to the lab and he has also
provided the soccer team with some much-needed ball control.
Now, on to the Lithium Lab. What’s always impressed me about Claudiu Stanis his deep sense of electronics aesthetics. Claudiu’s boxes appear as though they’rebuilt by the hands of God. Christian Schunck and Sebastian Raupauch are without
a doubt the two nicest members of lab. Christian always has a bright smile andSebastian’s character and thoughtfulness are second to none.
I had the pleasure of knowing Martin Zwierlein first as an officemate and later asa labmate. My short partnership with Martin was very memorable, especially our $17
breakfasts at Fresco’s (if you’re familiar with Fresco’s prices you know this is no smallfeat). I’ll never forget Martin’s deafening laugh and use of Rubik’s cube imagery todescribe social encounters. In addition, I’ll miss our 4 a.m. coffee breaks, watching
him chase a double espresso with a Red Bull and Snickers, and his pregame Bürger

König.
Every lab has to have a straight man, and Dominik Schneble has fulfilled this role
for the Rubidium Lab. Dominik’s easy-going nature and subtle humor will make him
a great advisor for future grad students.
It’s important to know that when a bad idea is too good to pass up, you always
have someone there to encourage you to follow through. Which brings me to MicahBoyd. Micah and I have had many “memorable” moments (I’ll leave it at that). He’s
been a great friend and partner in crime. I hope to continue our long and fruitfulrelationship of poor judgement at future conferences.
Gretchen Campbell is the little sister I never had. She does a lot for everyone
and has brought some much need sweetness to the lab. I only hope that the restof us don’t rub off too much on her. Gretchen’s dedication to work is incredible(and somewhat disturbing). Along with Aaron, those two make an unholy pair. Her
cleverness and honesty will lead her to many great things and I eagerly anticipate
reading of her future successes. I’ll certainly be trying to convince her to join me out
west when she’s done at MIT. Finally, I must thank Gretchen for all the help she’s
given me while I finished up at MIT (including turning in this thesis).
The Ketterle lab has had a number of fine diploma students and undergraduates who deserve mention. The first of these is Robert Loew, with whom I spent
many wonderful nights building our first AOM drivers together. Edem Tsikata wasa hard worker and a great guy. I wish him much success at Harvard. Mimi Xue andWidagdo Setiawan both built a number of important boxes for the New Lab and also
contributed a lot of youthful exuberance. Finally, Till Rosenband is in this group only
by title. Till was a super-UROP and at one time the senior member of the Ketterlelab. His electronic skills are legendary. I wish I could have convinced him to stay atMIT, but I realize he needed to go off to the greener pastures of Boulder. I had a lotof fun working with him he gets some extra credit in Chapter 5.
Dave Pritchard deserves a lot of credit for graciously allowing us to take out ourfrustration as grad students on him. Despite agreeing with us, he still played itcool when Tom and I held sit-ins in his office or berated him for the actions of theadministration. Because of this, I forgive him for his incessant cheating in the labpools.
There are a few other people from lab that also deserve mention: Dan StamperKurn, Timan Pfau, Shin Inouye, Todd Gustavson, Christian Sanner, Eric Streed,
Yoshio Torii, Jongchul Mun, Kai Dieckmann, Jamie Kerman, and Ellenor Emery.
Carol Costa was the surrogate mother to countless graduate students, postdocs,
and professors. Carol always made sure that her family was happy and well-fed. She
is deeply missed, but her legacy lives on in the sense of community that she helped
to foster. As a hometown girl and diehard fan, I wish that Carol could have sharedin the joy of our beloved Sox finally reversing the curse.
As the theorist of the hall, James Anglin was an invaluable source of information.
James was always there to explain physics to me, and then re-explain it several times
when I got confused. I particularly loved our discussions when James would partner
up with Michael Crescimanno to play good cop/bad cop.
I arrived at MIT at the same time as Hydrogen group members Lia Matos andKendra Vant. Much has changed in our time here, including the two of them becoming
mothers. However, I will never forget the first semester we spent together doing latenight problem sets. I was always pleased to pass Julia Steinberger in the corridor
because she was quick to deliver some politically charged statement (of which I always
agreed). The contributions of these three, and Cort Johnson, to the MIT community
are commendable.
Unfortunately, the Vuletic group only recently joined our CUA family. I enjoyedgetting to know Igor Teper, Adam Black, and Yu-ju Lin. Despite having been at
MIT for my entire stay, I only recently got to know James Thompson. I had a greattime playing IM sports with him and the excitement on his face when we successfully
executed his hook-and-lateral play was priceless.
Finally, I would like to thank some people outside of lab who have helped in mydevelopment (not always in a positive way).
My high school friends are always there to simultaneously support and mock myefforts in physics. I am forever grateful to: Jeff Riley for phoning in live play-by-playwhen I was missing important games because I had to be in lab. Dave Andreasen for
keeping me grounded by sharply reminding me how uncool physics is. Lian Ramesonfor sarcastically opining on the sexiness of physics whenever I got too excited about
it. Teresa Mendez for a providing me a link to the world outside MIT and briefing
me before her book club events so I could pretend I had read the book. Jeff Shelton
for reminding me that I better figure out a use for this stuff if I want to be employed.
Dave Mayer for reliving the glory days with me, one old grad student to another.
Brett Bezsylko for the time we spent together in college learning how to be good
students. Better late than never.
At UCSB I had the good-fortune of sharing the college experience with Omer
Ansari, Run Dul and Joe Gonzalez. I had a wonderful time with each of these guys.
In addition, I’d like to thank Hau Hwang for preventing me from failing out during
my second quarter and teaching me good study habits (i.e. read the book and do thehomework). My first physics TA, Seth Rosenberg, showed me that physics was fun
and really got me excited about the field. The courses I took from Roger Freedman
were among the best I’ve had. I am greatly indebted to Phil Lubin and Jeff Childers
for giving me my first lab experience. Jeff Childers took me under his wing, teaching
me to leave all places better than I found them and that nice-looking electronics work
better.
Shortly after arriving at Berkeley I met two other transfer students, Kelly Campbell and Eric Jones. I could not have met to better guys. I had a great time learning
physics with them and sharing in disbelief as one of our professors destroyed a trash
can during class. Stuart Freedman gave me my first shot at cold atom physics. I
hope to repay him for this during my postdoctoral work. Paul Vetter taught me agreat deal about cooling and trapping sodium. Because of him, I was able to make aquick transition to work at MIT.
My first year at MIT I lucked out by getting placed with three great roommates:
Anton Thomas, Johann Chan, and Peter McNamara. It was a pleasure living withthem and I wish them all the success. In particular, Anton is without a doubt thenicest guy I’ve ever met and now a great father too.

Despite the bitter cold, my last winter in Boston was made warm by Royce Brooks.
God only knows why she would ever get mixed up with a boy from the wrong sideof town, but I’m certainly glad she did. Royce’s sense of humor and quick wits werealways dazzling. I hope that she can one day forgive me for putting carrots in her
sweet potato pie to make it extra sport-healthy.
It’s fitting that Aaron and I shared an apartment with the fortuitously named
Kate DuBose. In addition to providing me with sorely needed background vocals,
Kate also had the unenviable job of taste-tester for all my culinary inventions. More
importantly, she taught Aaron and me that there was nothing funny about physics.
Besides all these things, our shared love for the worst in reality tv always made me
eager to rush home. On a final note - Kate and Aaron were the greatest roommates
ever. The night we got vortices and I called home at 4:00 a.m. to tell Aaron and her.
When I got home at 6:00 a.m. they both jumped out of bed to congratulate me andshare in my excitement. (Kate fondly remembers this moment because I made hercelebratory pancakes for breakfast.)
Jamila Wignot has been a very important part of my life throughout the last 12
years. She’s seen me at my best, but mostly at my worst, yet she has been a constantthroughout. Her friendship means a tremendous amount to me and I was very lucky
to have her share in this experience with me. Jamila’s wit/charm/talent delight me
to no end. She’s always challenged me to be a better person, and hopefully after thisexperience I will be. I’ll let her be the judge.
Finally, I would like to thank my family, for whom this work is dedicated. I owe
everything to them. To my sister Nadya, who always seems to think what I do isgreat, no matter how stupid it actually is. She also deserves extra credit for providing
some wonderful artwork for my thesis. My brother Amir, who always reminds methat physics is useless if you can’t convey your message to others. My mother Anita,
who has always been caring and nurturing, as evident by the 7 meals a day she fed me
while I wrote this thesis from her kitchen table. And to my Father, Muhsin, who has
been my greatest mentor, spending countless hours teaching me the right approachto physics and to life.

Contents
1 Introduction

17

1.1

Identical Particles . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

17

1.2

Bosons and Fermions . . . . . . . . . . . . . . . . . . . . . . . . . . .

20

1.3

Quantum Statistical Mechanics . . . . . . . . . . . . . . . . . . . . .

20

1.4

Bose-Einstein Condensation . . . . . . . . . . . . . . . . . . . . . . .

22

1.4.1

The Effect of Interactions . . . . . . . . . . . . . . . . . . . .

23

1.4.2

The Gross-Pitaevskii Equation . . . . . . . . . . . . . . . . . .

23

Outline of the Thesis . . . . . . . . . . . . . . . . . . . . . . . . . . .

24

1.5

2 Vortices in Bose-Einstein Condensates

26

2.1

Vortices - Simple Theory . . . . . . . . . . . . . . . . . . . . . . . . .

27

2.2

Vortex Lattice Tutorial . . . . . . . . . . . . . . . . . . . . . . . . . .

31

2.2.1

The Rotating Bucket . . . . . . . . . . . . . . . . . . . . . . .

32

2.2.2

The Swizzle Stick . . . . . . . . . . . . . . . . . . . . . . . . .

32

2.2.3

Stirring it Up . . . . . . . . . . . . . . . . . . . . . . . . . . .

34

2.2.4

The Golden Parameters . . . . . . . . . . . . . . . . . . . . .

35

3 Vortex Lattices

37

3.1

Perspective . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

37

3.2

Observation of Vortex Lattices . . . . . . . . . . . . . . . . . . . . . .

40

3.3

Formation and Decay of a Vortex Lattice . . . . . . . . . . . . . . . .

43

4 Vortex Nucleation

45

12

4.1

Perspective . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

45

4.1.1

A Brief Aside... . . . . . . . . . . . . . . . . . . . . . . . . . .

48

4.2

Vortex Structure . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

49

4.3

Effects of Rotation . . . . . . . . . . . . . . . . . . . . . . . . . . . .

50

5 Formation and Decay of Vortex Lattices

52

5.1

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

52

5.2

Decay of Vortex Lattices . . . . . . . . . . . . . . . . . . . . . . . . .

53

5.3

Formation of Vortex Lattices . . . . . . . . . . . . . . . . . . . . . . .

54

5.3.1

Damping Mechanism . . . . . . . . . . . . . . . . . . . . . . .

57“Visible” Vortices Revisited . . . . . . . . . . . . . . . . . . . . . . .

57

5.4.1

58

5.4

Vortex Counting Algorithm . . . . . . . . . . . . . . . . . . .

6 Formation of Ultracold Sodium Molecules

60

6.1

Why Cold Molecules? . . . . . . . . . . . . . . . . . . . . . . . . . . .

61

6.2

Feshbach Resonances . . . . . . . . . . . . . . . . . . . . . . . . . . .

63

6.2.1

Model of Feshbach Resonance . . . . . . . . . . . . . . . . . .

64

6.2.2

Experimental Notes . . . . . . . . . . . . . . . . . . . . . . . .

65

6.3

Production of Molecules . . . . . . . . . . . . . . . . . . . . . . . . .

66

6.4

Molecular Properties . . . . . . . . . . . . . . . . . . . . . . . . . . .

70

6.4.1

Phase-Space Density . . . . . . . . . . . . . . . . . . . . . . .

70

6.4.2

Molecular Lifetimes . . . . . . . . . . . . . . . . . . . . . . . .

71

What Makes a BEC a BEC? . . . . . . . . . . . . . . . . . . . . . . .

76

6.5.1

77

6.5

A Final Note . . . . . . . . . . . . . . . . . . . . . . . . . . .

7 Bragg Scattering
7.1

7.2

78

Bragg Scattering: A Practical Guide . . . . . . . . . . . . . . . . . .

78

7.1.1

Grating Picture . . . . . . . . . . . . . . . . . . . . . . . . . .

79

7.1.2

Raman Picture . . . . . . . . . . . . . . . . . . . . . . . . . .

81

7.1.3

Coherent Population Transfer . . . . . . . . . . . . . . . . . .

82

Bragg Spectroscopy . . . . . . . . . . . . . . . . . . . . . . . . . . . .

84

13

7.2.1

Width of a Thermal Distribution . . . . . . . . . . . . . . . .

84

Broadening Mechanisms . . . . . . . . . . . . . . . . . . . . . . . . .

85

7.3.1

Finite-Size Broadening . . . . . . . . . . . . . . . . . . . . . .

85

7.3.2

Mean-Field Broadening . . . . . . . . . . . . . . . . . . . . . .

86

7.3.3

Pulse Broadening . . . . . . . . . . . . . . . . . . . . . . . . .

87

7.3.4

Motional Broadening . . . . . . . . . . . . . . . . . . . . . . .

89

7.4

Summary of Results . . . . . . . . . . . . . . . . . . . . . . . . . . .

90

7.5

Discussion of Results . . . . . . . . . . . . . . . . . . . . . . . . . . .

91

7.6

Putting it all Together: A Real Example . . . . . . . . . . . . . . . .

91

7.7

Noise Rejection . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

93

7.3

8 Coherent Molecular Optics
8.1

95

Optics . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

95

8.1.1

Conventional Optics . . . . . . . . . . . . . . . . . . . . . . .

96

8.1.2

Atom Optics. . . . . . . . . . . . . . . . . . . . . . . . . . .

97

8.2

Molecular Optics . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

98

8.3

Bragg Diffraction of Molecules . . . . . . . . . . . . . . . . . . . . . . 100

8.4

Characterization of the “Source” . . . . . . . . . . . . . . . . . . . . 100

8.5

Sum-Frequency Generation . . . . . . . . . . . . . . . . . . . . . . . . 102

8.6

Molecular Interferometery . . . . . . . . . . . . . . . . . . . . . . . . 104

8.7

Conclusions and Outlook . . . . . . . . . . . . . . . . . . . . . . . . . 104

A Observation of Vortex Lattices in Bose-Einstein Condensates106

B Vortex Nucleation in a Stirred Bose-Einstein Condensate

111

C Formation and Decay of Vortex Lattices

116

D Dissociation and Decay of Ultracold Sodium Molecules

121

E Coherent Molecular Optics using Sodium Dimers

126

Bibliography

131

14

List of Figures
1-1 The “social nature” of Fermions and Bosons. . . . . . . . . . . . . . .

21

2-1 Uroboros dining on his tail. . . . . . . . . . . . . . . . . . . . . . . .

27

2-2 Bulk lattice flow fields. . . . . . . . . . . . . . . . . . . . . . . . . . .

31

2-3 Bullseye . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

33

2-4 Optical “Swizzle” Stick. . . . . . . . . . . . . . . . . . . . . . . . . .

34

2-5 Stirring up a Bose-Einstein Condensate. . . . . . . . . . . . . . . . .

35

2-6 “Fool-proof” vortex lattice. . . . . . . . . . . . . . . . . . . . . . . . .

36

3-1 First signal of vortices. . . . . . . . . . . . . . . . . . . . . . . . . . .

39

3-2 Observation of vortex lattices. . . . . . . . . . . . . . . . . . . . . . .

41

3-3 Density profile through a vortex lattice. . . . . . . . . . . . . . . . . .

42

3-4 Structure of a vortex lattice. . . . . . . . . . . . . . . . . . . . . . . .

43

3-5 Vortex lattices with defects. . . . . . . . . . . . . . . . . . . . . . . .

44

3-6 Formation and decay of a vortex lattice. . . . . . . . . . . . . . . . .

44

4-1 Discrete resonances in vortex nucleation. . . . . . . . . . . . . . . . .

47

4-2 Nonresonant nucleation using a small stirrer. . . . . . . . . . . . . . .

48

4-3 Surface instabilities nucleate vortices. . . . . . . . . . . . . . . . . . .

49

4-4 Three-dimensional structure of vortices. . . . . . . . . . . . . . . . . .

50

4-5 Centrifugal effects on a rotating condensate. . . . . . . . . . . . . . .

51

5-1 Spin down of a rotating condensate in a static magnetic trap.

. . . .

53

5-2 Decay of a vortex lattice at finite temperatures. . . . . . . . . . . . .

54

5-3 Decay rates for vortex lattices at several temperatures. . . . . . . . .

55

15

5-4 Crystallization of the vortex lattice. . . . . . . . . . . . . . . . . . . .

56

5-5 Vortex counting algorithm. . . . . . . . . . . . . . . . . . . . . . . . .

59

6-1 Methods for producing ultracold molecules. . . . . . . . . . . . . . . .

62

6-2 Resonant enhancement of the scattering length. . . . . . . . . . . . .

64

6-3 Toy potential to illustrate resonant scattering. . . . . . . . . . . . . .

65

6-4 Loss mechanism in the vicinity of a Feshbach resonance. . . . . . . .

66

6-5 Experimental method for producing and detecting ultracold molecules.

67

6-6 “Blast” pulse for removing unpaired atoms.

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

68

6-7 Ballistic expansion of a pure molecular sample. . . . . . . . . . . . . .

69

6-8 Temperature of the molecular cloud. . . . . . . . . . . . . . . . . . .

71

6-9 Collapse of a molecular cloud. . . . . . . . . . . . . . . . . . . . . . .

72

6-10 Decay mechanism for molecules. . . . . . . . . . . . . . . . . . . . . .

73

6-11 Decay of ultracold molecules. . . . . . . . . . . . . . . . . . . . . . .

74

6-12 Conversion of atoms to molecules for various ramp times. . . . . . . .

75

7-1 Bragg scattering of x-rays from a crystal . . . . . . . . . . . . . . . .

79

7-2 Bragg Scattering viewed as a stimulated Raman transition. . . . . . .

81

7-3 Bragg diffraction of a BEC. . . . . . . . . . . . . . . . . . . . . . . .

82

7-4 Bragg spectrum of a trapped condensate. . . . . . . . . . . . . . . . .

83

7-5 Broadening mechanisms for Bragg transitions. . . . . . . . . . . . . .

86

7-6 Kapitza-Dirac scattering of a BEC. . . . . . . . . . . . . . . . . . . .

88

7-7 Frequency resolution of a finite pulse . . . . . . . . . . . . . . . . . .

89

7-8 Doppler broadening caused by random motion. . . . . . . . . . . . . .

93

8-1 Key Features of conventional optics. . . . . . . . . . . . . . . . . . . .

97

8-2 Key Features of atom/molecular optics. . . . . . . . . . . . . . . . . .

99

8-3 Bragg Diffraction of Atoms and Molecules . . . . . . . . . . . . . . . 101
8-4 Bragg spectra for atoms and molecules. . . . . . . . . . . . . . . . . . 102
8-5 Sum frequency generation of atomic matter waves. . . . . . . . . . . . 103
8-6 Matter wave interference of molecules. . . . . . . . . . . . . . . . . . 105

16

Chapter 1
Introduction
By convention color, by convention bitter, by convention sweet, in reality atoms andvoid.
-Democritus
The birth of atomic theory can be traced back to the 5th century B.C. when Greek
philosophers Democritus and Leucippus postulated that matter and space were notinfinitely divisible. Human perception leads to gross classifications based primarily
on senses, such as ’hot’ or ’cold’. The revolutionary postulate of the Greek atomists
was that such outward qualities of matter are reducible and should be fundamentally
determined by the species of atom and the amount of void that it is composed of. Many
however, including Aristotle, rejected this idea, and so it lay dormant for centuries.
In the early 1800’s atomic theory reemerged with John Dalton’s observation that
aggregate matter is reducible to elements, and that all atoms of a certain element
have the same size and weight. Thus, it is with these two notions, classification andsameness, that I begin this work.

1.1

Identical Particles

The strange behavior of matter at low temperatures stems from Nature’s desire tocreate like particles identically to one another. That is to say, there is no discernable difference between any two electrons, protons, atoms, etc. Indistinguishability
17profoundly affects the behavior of quantum systems, leading to such phenomena as
Bose-Einstein Condensation and superfluidity.
To see how this is manifest, consider two (non-interacting) identical particles occupying the single-particle states ψa and ψb . Suppose now we are charged with thetask of constructing a composite wavefunction Ψ(~
r1 , r~2 ) to describe this system. Ournaive choice might be to simply take the product of the two states.
Ψ(~
r1 , r~2 ) = ψa (~r1 )ψb (~
r2 )

(1.1)

This would certainly be the correct choice if the two particles were distinguishable.
However, it is a bit more complicated for identical particles. Remember, we cannot
distinguish between the two, so how can we say with certainty that particle 1 is inψa and particle 2 is in ψb ? We only really know that one particle resides in ψa andthe other in ψb . To solve this dilemma, we look for eigenstates of the Hamiltonian
describing the two-particle system.
Let us define an exchange operator O that, when applied to Ψ(~
r1 , r~2 ), swaps thetwo particlesOΨ(~
r1 , r~2 ) = Ψ(~r2 , r~1 )(1.2)

Since these two particles are identical we know that the potential energy term V (~r1 , r~2 )in the Hamiltonian H must treat the two particles equally e.g. V (~r1 , r~2 )=V (~r2 , r~1 ).
Therefore, the exchange operator O and H are compatible observables ([H, O] = 0),
and so eigenstates of O are also eigenstates of H. If we apply O twice to Ψ(~
r1 , r~2 ) wemust return to the original stateO2 Ψ(~
r1 , r~2 ) = Ψ(~r2 , r~1 )(1.3)

Therefore, the eigenvalues of O are ±1, which means our composite wavefunctionΨ(~r1 , r~2 ) is either symmetric (+1) or antisymmetric (-1) under exchange.
Ψ(~
r1 , r~2 ) = ±Ψ(~
r1 , r~2 )
18

(1.4)

Our naive guess (Eq(1.1)) fails to meet this criteriaΨ(~
r1 , r~2 ) = ψa (~r1 )ψb (~r2 ) 6= ±ψa (~r2 )ψb (~
r1 )

(1.5)

Because our particles are identical, our intuition tells us that they must each be
represented equally in both states. With this in mind we construct the following
1r1 )ψb (~r2 ) + ψa (~r2 )ψb (~
r2 )]
Ψ+ (~
r1 , r~2 ) = √ [ψa (~
2
1
Ψ− (~
r1 , r~2 ) = √ [ψa (~r1 )ψb (~r2 ) − ψa (~r2 )ψb (~
r1 )]
2

(1.6)
(1.7)

Both of these states clearly obey the (anti-)symmetry condition of Eq(1.4). As was
the case with our naive guess ψa (~r1 )ψb (~r2 ), superpositions of these two eigenstates
are forbidden by Eq(1.4). Hence, we see that identical particles come in two distinct
classes. Those symmetric under exchange, Ψ+ (~r1 , r~2 ), we call “Bosons” and thoseantisymmetric under exchange, Ψ− (~r1 , r~2 ), we dub “Fermions”.
All particles in nature must fall into one of these two categories (Democritus isredeemed!). The actual mechanism that makes them one or the other relates to their
spin. The proof of this is beyond the scope of this simple treatment so I simply state
the result:1
All Particles with integer spin (0, 1, 2 ...) are Bosons.
All particles with half-integer spin (1/2, 3/2, 5/2 ...) are Fermions.
Although implicitly stated above, I must stress that even composite particles suchas atoms fall into one of these two classes. Since atoms are composed of Fermions(electrons, protons, neutrons), those with an odd number of constituent particles are
Fermions and those with even number are Bosons.
1

The spin-statistics theorem is a well-documented result of relativistic quantum mechanics.

19

1.2

Bosons and Fermions

The subtle distinction in symmetry leads to profoundly different behavior between
the two species. To see this, consider the case of ψa = ψb . For Bosons we find that√1r1 )ψa (~r2 ) + ψa (~r2 )ψa (~r1 )] = 2[ψa (~r1 )ψa (~r2 )]Ψ(~r1 , r~2 )+ = √ [ψa (~
2

(1.8)

However, for Fermions1r1 )ψa (~r2 ) − ψa (~r2 )ψa (~r2 )] = 0Ψ(~r1 , r~2 )+ = √ [ψa (~
2

(1.9)

which is to say that Bosons may occupy the same quantum state, while Fermionscannot (the Pauli Exclusion principle). Because of this we sometimes attribute “social” characteristics to Bosons and Fermions. Fermions are introverts, avoiding theirneighbors at all costs (see Figure 1-1). Bosons, on the other hand, are quite jovial
and enjoy each other’s company (bosonic enhancement).

1.3

Quantum Statistical Mechanics

The observation that Fermions obey Pauli exclusion, while any number of Bosons
can occupy a single quantum state, leads to profound differences in their many-bodystates. However, we shall see that these differences are only manifest at very low
temperatures. Without invoking the full machinery of quantum statistical mechanics,
we can still get a general sense for this behavior by examining the ground states ofboth systems. At zero temperature, Bosons will fully accumulate in the lowest energy
level, while Fermions “stack up”, each occupying a distinct energy level (see Figure1-1). The fact that every boson occupies the same quantum mechanical state hints atthe strange nature of Bose-Einstein Condensates (BEC). More surprisingly though,we’ll see that the macroscopic occupation of the ground state persists even as we raise
the temperature.
Taking into account the quantum statistics for Bosons and Fermions, it is a20

Figure 1-1: The “social nature” of Fermions and Bosons. Fermions are individualists,and refuse to mingle with one another (Pauli exclusion). Bosons are quite the opposite, enjoying each others company (Bosonic enhancement). Illustration by Nadya
Abo-Shaeer.

straightforward affair to calculate the occupancy of a state of energy ǫ [48]:< N (ǫ) >m−b = e−(ǫ−µ)/kT , M axwell − Boltzmann Distribution
1, Bose − Einstein Distribution< N (ǫ) >b−e = (ǫ−µ)/kTe−1
1, F ermi − Dirac Distribution< N (ǫ) >f −d = (ǫ−µ)/kTe+1(1.10)(1.11)(1.12)

where µ is the chemical potential. We note that at high temperatures ((ǫ − µ) ≫kT ) both distributions approach the classical limit given by the Maxwell-Boltzmann
distribution. The differences between Bosons and Fermions are only manifest for21

occupations < N (ǫ) > on the order of unity.

1.4

Bose-Einstein Condensation

At this point we leave Fermions behind and turn our full attention to Bosons.2 Because it is well-known derivation, I will forego calculating the BEC transition temperature Tc , and simply state the result [48]3
For free particles
h2
kB Tc =2πmÃN
ζ(3/2)V!2/3,(1.13)

where V is the size of the system and ζ(3/2) ≈ 2.612 is the Riemann Zeta function.
For harmonically confined atoms (as is the case for typical atom traps)ÃN
kB Tc = h̄ω̄
ζ(3)

!1/3

,

(1.14)

where ζ(3) ≈ 1.202 and ω̄ = (ωx ωy ωz )1/3 .
A more intuitive picture for the onset of condensation relies on wave-function
overlap. Only then will the particles’ indistinguishability come into play. This occurs
when the thermal de Broglie wavelength λT is roughly equal to the interparticle
spacing n−1/3 , where n is the particle density, such thatnλ3T ∼ 1(1.15)Aside from a numerical constant, this reproduces the results of Eq(1.13) andEq(1.14)2This is not due to a lack of interesting phenomena. One need only go two doors down from ourlab to prove this.
3
One integrates over the Bose-Einstein distribution to find the total number of thermally excited
particles. This result is then subtracted from the total number of particles in the system, yielding
the occupation of the ground state.

221.4.1The Effect of Interactions

In the ultracold regime (∼ 1 µK) atomic interactions are dominated by s-wave scattering. Here, the two-body Hamiltonian V (~r1 , ~r2 ) can be approximated by the local
Hamiltonian [81]4πh̄2 aV (~r1 , ~r2 ) =δ(~r1 − ~r2 )m(1.16)

where m is the atomic mass and a is the s-wave scattering length. The precise value ofa depends on details of the interatomic potential, and very small changes can produce
dramatic variation. The fact that the interaction strength depends critically on thissingle parameter a has very important consequences (see Chapter 6).
Interactions play an essential role in evaporative cooling and thermalization. As weshall see, they also also define the ground state characteristics of a BEC. Furthermore
interactions lead to such phenomena as superfluidity, molecule creation, and nonlinear
atom optics. (The subjects of this thesis.)

1.4.2

The Gross-Pitaevskii Equation

To construct a Schrödinger equation for a zero-temperature BEC we need to include
the effect of the binary interactions discussed above. From Eq(1.16) we see that atest particle moving through a system with density n will have mean-field energy
4πh̄2 anm

(1.17)

Therefore, the wave equation takes on a nonlinear form given by
4πh̄2 ah̄2 2
∇ + Vext (~r) +|ψ(~r)|2 ψ(~r) = µψ(~r),
−
2m
m
!

Ã

(1.18)

where Vext (~r) is the external trapping potential, and n = |ψ(~r)|2 . Thus, the manybody ground state is described by the macroscopic order parameter (wavefunction)
Ψ(~r, t) = ψ(~r)e−i(µ/h̄)t23(1.19)

Because the interaction energy of a condensate typically dominates its kinetic
energy (the Thomas-Fermi regime), we may omit the kinetic energy from Eq(1.18),
yieldingÃ

4πh̄2 a|ψ(~r)|2 ψ(~r) = µψ(~r)
Vext (~r) +m!

T homas − F ermi Limit(1.20)

From here it is trivial to see that the density is given byn(~r) = |ψ(~r)|2 =m[µ − V (~r)]
4πh̄2 a(1.21)

and we arrive at the well-known result that the condensate density takes on the inverse
profile of its trap (typically a parabola).

1.5

Outline of the Thesis

I had the benefit of arriving to the New Lab just six months after their first BEC.
Although our machine has undergone many changes in the past five years, the basics
remain the same. Because our apparatus has been well-documented previously [27,62], I will omit this discussion in favor of more unique material. In particular, I
include two tutorial chapters on vortex production and Bragg diffraction, which I
hope will prove useful to my successors.
A major portion of my work at MIT has been devoted to the study of quantizedvortices. Chapter 2 is intended as a primer for the basic theory and experimental
techniques underlying vortex physics. Chapters 3-5 detail our studies of nucleationand dynamics of vortex lattices. More recently, I have worked on cold molecules
created via Feshbach resonance. Chapter 6 explains the motivation for creating cold
molecules, along with our initial experimental results. Chapter 7 is devoted to techniques of Bragg spectroscopy, which were important for our demonstration of coherent
molecular optics (Chapter 8).
Finally, having spent the last five years of my life working on the 2nd floor of
Building 26, I have had the pleasure of sharing in many triumphs and an equal
24number of defeats. With this in mind, I will to try to convey some of the excitement
we’ve felt, whether it be over something meaningful or something mundane.
This thesis is by no means a complete survey of Bose-Einstein Condensation.
Indeed, the field has grown so rapidly in my time at MIT that I cannot even do
justice to my particular areas of expertise. Fortunately, a large body of work alreadyexists. In particular, I refer readers to the following useful references:• Bose-Einstein Condensation in Atomic Gases
Proceedings of the International School of Physics Enrico Fermi, Course CXL
Edited by M. Inguscio, S. Stringari and C.E. Wieman (1999) Ref [49]• Bose-Einstein Condensation in Dilute Gases
C.J. Pethick and H. Smith (2002) Ref [81]• Laser Cooling and Trapping
H. Metcalf and P. van der Straten (1999) Ref [71]In addition, a wealth of practical knowledge lies in the theses of my predecessors.

25

Chapter 2
Vortices in Bose-Einstein
Condensates...the well-known invariant called the hydrodynamic circulation is quantized; the quantum of circulation is h/m.
-Lars Onsager, on the behavior of a Bose gas at zero temperature. (1949)
As we shall see, this statement has very profound implications. The fact that
Bose-condensed systems can be described by a macroscopic order parameter Ψ puts
important restrictions on the way these fluids flow. The requirement that Ψ be singlevalued (Figure 2-1) leads directly to Onsager’s conclusion. When these “superfluids”
are rotated, angular momentum can only enter the system in the form of discrete line
defects.
I begin this chapter with a brief (and humble) explanation of the basic principles
of vortices in BEC. As an obligation to my successors, I finish with a discussion of
the “nuts and bolts” of vortex lattice generation. Chapters 3-5 are dedicated to theexperimental study of vortices in superfluid systems.

26

λ

R

Figure 2-1: Uroboros dining on his tail. The Bohr-Sommerfeld Quantization condition
requires that an integer number of wavelengths fit within any closed loop. This insuresthat the wavefunction is single-valued. Illustration by Nadya Abo-Shaeer.

2.1

Vortices - Simple Theory

The theory of vortex nucleation, dynamics, interactions etc. has been the subject of
exhaustive study, first in liquid helium systems [26] and later for BEC [33]. Whileatomic BEC is in some ways fundamentally different from liquid helium (inhomogeneous density, weaker interactions), the similarities between the two systems has
facilitated rapid theoretical development. One unifying feature of these two fields isthat most of the theory is beyond my comprehension. With this in mind, I leave
the details to the theorists, and present a phenomenological description of superfluid
vortices.
In Chapter 1 we saw that the static properties of a zero-temperature dilute
Bose gas are characterized by the time-independent Gross-Pitaevskii (G-P) equation (Eq(1.18)). To study the dynamic properties of the system, we must invoke the27time-dependent G-P equation∂h̄2 2ih̄ Ψ = −∇ + Vext + U0 |Ψ|2 Ψ
∂t
2m
!

Ã

(2.1)

where U0 = 4πh̄2 /a. To better represent the flow characteristics it is instructive torecast this equation in an equivalent quantum-hydrodynamical form. Multiplying
through by Ψ∗ yields
ih̄Ψ∗h̄2 ∗ 2∂Ψ=−
Ψ ∇ Ψ + Vext |Ψ|2 + U0 |Ψ|4
∂t
2m

(2.2)

Subtracting Eq(2.2) from its complex conjugate yields
Ã

∗ ∂

ih̄ Ψ

∂t

∗ ∂

Ψ+Ψ

∂t

!

Ψ =

´
h̄2 ³
Ψ∇2 Ψ − Ψ∗ ∇2 Ψ∗
2m

(2.3)

or more succinctly∂h̄|Ψ|2 =∇ · (Ψ∗ ∇Ψ − Ψ∇Ψ∗ )
∂t
2mi

(2.4)

∂
n + ∇ · (n~v ) = 0
∂t

(2.5)

Re-expressing Eq(2.4) ashelps to identify this as a continuity equation for compressible flow, where n = |Ψ|2
is the fluid density and the fluid velocity is given by~v =h̄(Ψ∗ ∇Ψ − Ψ∇Ψ∗ )
2mni

(2.6)

Without loss of generality, the order parameter can be expressed in terms of an√amplitude and phase Ψ = neiφ such that
~v =

h
∇φ
m

(2.7)

Thus, we identify the velocity of the condensate with the gradient of the phase. The
fact that the velocity is field conservative (known as potential flow) places restrictions

28

on the fluid motion. Provided that φ is not singular∇ × ~v = 0(2.8)

and the flow is irrotational. More generally, for the wavefunction to be single-valued,
the phase accumulated around a closed loop must be an integer multiple of 2π.
∆φ =I∇φ · d~l = 2π

(2.9)

This is just a restatement of the Bohr-Sommerfeld quantization condition (Figure2-1). The circulation C around a closed loop is thusC=Ih~v · d~l = ℓm(2.10)

and we arrive at Onsager’s statement that circulation is quantized in units of κ = h/m.
In general,∇ × ~v = ℓhδ(~r)ẑm(2.11)

To demonstrate the implications of quantized circulation, we recognize from Eq(2.10)
that the radial velocity profile isvr = ℓκ2πr(2.12)

Because the energy diverges at the origin, the density must go to zero there. Fluid
is expelled, and a hole appears in the liquid. The size of this hole is determinedby the balance of two competing processes. Mean-field repulsion seeks to fill in thehole, but the requirement of zero density at the core places a hard wall at the center.
Therefore, we must balance the mean-field’s desire to fill the hole with the kinetic“cost” of bending the wavefunction (recall that kinetic energy is given by the curvatureof the wavefunction). For a feature of size ξ, the kinetic energy per particle is roughlyh̄2 /2mξ 2 . The size of the core is then determined by
h̄2
= nU0
2mξ 2
29

(2.13)

Thus, the characteristic size of the vortex is,
ξ=√

1
8πna

(2.14)

which is typically called the “healing length”. In passing, we note that the flow
velocity (Eq(2.12)) at the core (r=ξ) is equal to the local speed of sound c

c=

s

2nU0
m

(2.15)

We conclude with a few remarks on the bulk properties of systems containing
many vortices. In the limit of very high angular momentum, the quantum system
will mimic the behavior of a classical fluid. That is, the “course-grained” flow fieldof the quantum fluid is identical to the rigid-body rotation of a classical fluid (Figure2-2). Intuitively we know this must be true, because at some point the quantum
and classical pictures must match up (Bohr correspondence principle). Now, using awell-known result from classical fluid dynamics for the kinetic energy per unit lengthof a hollow vortex of radius a and circulation C [26]
E=

Z r0
a

1 2 2 ρC 2 r0
ρv dr =ln24πa(2.16)

we find that for a superfluid E = (ρℓ2 κ2 /4π)ln(r0 /ξ). Because this energy is quadratic
in the vortex winding ℓ, multiply charged vortices are unstable and will decay into
vortices of unit circulation.1 Due to this repulsive vortex-vortex interaction, we might
expect vortices will distribute themselves in some sort of array to minimize energy.
Indeed, numerical simulations [4, 98], followed by experiment [109, 67, 2] have proventhis to be the case, with the lattice taking on a triangular configuration.
Lastly, we note that the angular momentum per particle a distance r from theorigin is mvr = ℓh̄. For rigid-body rotation v = Ωr, where Ω is the (angular) rotation
frequency. Now, a closed loop around the origin will encircle N vortices. Therefore,
1

This result is also evident from Eq(2.12). The flow velocity is linear in vortex winding ℓ, therefore
the kinetic energy is proportional to ℓ2 .

30

a)

b)

Figure 2-2: Bulk lattice flow fields. a) A system containing many vortices will arrange
itself in a triangular lattice to minimize energy. b) The coarse-grained flow field of
the lattice mimics rigid-body rotation.

the vortex density N/2πr2 in the bulk is
nv =

2.2

2Ω
.
κ

(2.17)

Vortex Lattice Tutorial

When the New Lab began its effort to produce vortices the nucleation process was still
somewhat mysterious (see Chapter 4). Indeed, we tried for 3-4 months before obtaining our first signal. Later, I witnessed Aaron Leanhardt go through similar struggles
in his effort to imprint vortices topologically [65]. In both cases the difficulty was notin setting-up the experiment, but rather finding the proper parameter space to workin. In retrospect, we both agree that once you know where to look, making vortices
is actually quite easy. Thus, the impetus for this section is to provide the reader witha “fool-proof recipe” for making vortices.2 Many of the past techniques used by ourgroup and others are needlessly complicated, and in some cases misleading. I will try
to pare down the process to only its most essential elements.
The courage to write this section stems from my work with Martin Zwierlein
during my final few months in lab. I made a promise to the Lithium Lab that I would“bring over the vortices” before I left. In my bravado, I also made strong claims
2

Disclaimer: The information contained herein is provided as a public service with the understanding that the author makes no warranties, either expressed or implied, concerning the accuracy,completeness, reliability, or suitability of the information.

31

about the ease with which it would be done. Finally, I was forced to deliver on myclaims, and as luck would have it, it was much easier than I had anticipated. The
entire process took less than a day and it gave me confidence in the transferability ofthe techniques outlined below.

2.2.1

The Rotating Bucket

Vortices are created by rotating the condensate about its symmetric axis. We havemade vortices in a variety of different “buckets”, with aspect ratios varying from 2 to
30. However, it is wise to choose a smaller aspect ratio for two reasons:
1) Vortices are 3-dimensional objects. They can twist and bend. This behavior
reduces imaging contrast. In addition, if the imaging axis is tilted with respect
the condensate axis, the reduction in contrast is more severe for longer clouds.
In our first two papers we used a “slicing” technique to image only the centerof the condensate [2, 83]. However, the necessity of this technique is probably
overstated a bit. It is only essential for imaging small numbers of vortices orvortices created in very long traps.
2) Smaller aspect ratios correspond to a larger radial size. Larger objects are lesssensitive to stirrer alignment and therefore much easier to get rotating.
I prefer an aspect ratio of ∼ 4, mostly because our Ioffe-Prtichard-type magnetic
traps tend to be less round below these values (due to trap imperfections and gravitational sag). One should try to work in a regime where the trap is as round as possible.
However, my definition of round is somewhat arbitrary. For instance, JILA’s top trap
is round to 1 part in 2000, while most of our work was done in a trap with asymmetryǫr = (ωx2 − ωy2 )/(ωx2 + ωy2 ) = 6.4%.

2.2.2

The Swizzle Stick

The condensate is stirred using the optical dipole force created by a detuned laser
beam.
32

Figure 2-3: Bullseye. Alignment of the stirrer using in situ phase contrast imaging.
The beam power exceeds the chemical potential of the condensate so atoms are fully
expelled from the center.

The size of the stirring beam should be small compared to the size of thecondensate!
Much of the mystery that surrounded early work on vortex nucleation stemmed
from inefficient coupling of angular momentum to the condensate. The big beam
“Rotating Bucket” approach only works well near the surface mode resonance. As
demonstrated in Chapter 4, a small stirrer is efficient at coupling angular momentum
to the condensate at all frequencies. If you are wedded to the rotating bucket analogy,
think of the small beams as roughness on the surface of an otherwise smooth bucket(magnetic trap).
Because we are using small beams, a blue-detuned beam is necessary because it
creates a repulsive potential. A red-detuned beam will act as an optical trap. The
stirrer should be made as small as possible for the greatest flexibility. Gaussian beam
waists (1/e2 ) of 5 µm should be relatively easy to attain. Beam profile is not critical.
The intensity of the stirrer should be enough to overcome the chemical potential µ of
the condensate, such that the beam fully pierces the condensate (Figure 2-3).
The technical question that most often arises relates to how the stirring beam is
actually rotated. The method is quite simple. The beam becomes a “swizzle stick”
by passing it through a two-axis acousto-optic deflector. By frequency modulating
the two channels 90◦ out-of-phase, the (1,1) order will rotate. The method is outlinedin Figure 2-4. It is preferable to use two spots rather than one because symmetricstirring will induce less dipole oscillation. A lens must be placed a focal length

33

a)

b)
ω

ωx = 0ωy = 0Ω

0Θ(ωf) =−Ω

c)

ωx = Ω0ωy = 0d)ωx = Θ(ωf)ωy = 0cos(Ωrot) =ωx = Θ(ωf)cos(Ωrot)ωy = Θ(ωf)sin(Ωrot)sin(Ωrot) =00 order

θ = f(ω)e)
Quartz Crystal+1 orderFigure 2-4: Optical “Swizzle” Stick. a) Light traveling through a quartz crystal canbe deflected from its path by an acoustic wave. The acoustic wave creates a density
modulation in the crystal off which the beam can Bragg scatter. The angle at which
the beam is scattered is proportional to the acoustic wave drive frequency ω. b)
For (ωx , ωy )=(0,0) the beam is undeflected. c) When (ωx , ωy )=(Ω0 , 0) the beam isdeflected by a fixed amount. d) A fast square pulse will split the beam in two. Thisfrequency should be much faster than the trap frequencies so that the condensate
sees a time-averaged potential. e) By driving the channels 90◦ out-of-phase, the two
beams rotate in space. The amplitude and frequency of rotation are Ω0 and Ωrot ,respectively.

away from the deflector in order to image the separated beams onto condensate.3
Course alignment of the beam can be done using mirrors after the deflector. Fine
adjustments can then be made by changing the center frequency of each deflector.
The final alignment should be made using the condensate as a guide. It is preferable
here to use in situ phase-contrast imaging [57] to center the beam (see Figure 2-3).
However, the alignment can also be done using absorption imaging by leaving thebeam on in short time-of-flight (∼2 ms). This is necessary to reduce the opticaldensity.

2.2.3

Stirring it Up

Now that the machinery is in place, we turn our attention to stirring the condensate.
Again, phase-contrast imaging is a valuable technique because the stirring can bemonitored directly. Figure 2-5 shows a “movie” of the stirring process. As the stirrer
3

These defelectors are large objects so this is a somewhat ambiguous statement. Getting it close
is good enough. As the lens moves out of focus, the deflection sensitivity (beam separation per unit
frequency) is degraded.

34

Stirring

Equilibration

Figure 2-5: Stirring up a Bose-Einstein Condensate. Axial phase contrast images
showing the condensate at 4.4 ms intervals. The “smoking gun” for vorticity is thebuild-up of fluid in front of the stirrer. These images demonstrate both the violent
nature of the stirring and the resilience of the condensate. Representative absorption
images are also included.

is turned on we see fluid begin to build-up in front of it. The beam is clearly exertinga torque on the condensate. The process may seem too violent, but this is exactly
what you would like to see. From Figure 2-5 we see that the condensate is quite
able to “heal” itself. One need not ramp up the power or rotation frequency of thestirrer. Simply “slam” on the beams, get angular momentum into the system, getout, and leave it to the condensate to do the rest. There is one caveat: In order forthe condensate to heal itself it must have a sink for all the excess energy.
Keep the rf-knife on during equilibration!
In fact, we simply leave the rf-knife on at its final value during the entire process,stirring included.

2.2.4

The Golden Parameters

In my time working on vortices I have noticed that there seem to be universal parameters for making vortices. That is, parameters that work regardless of trap geometry.
35

Figure 2-6: “Fool-proof” vortex lattice. Using the techniques outlined in this section,
the Lithium lab had over 120 sodium vortices in less than a day. Shown here is thefirst shot.

As mentioned earlier, a lot of the difficulty in making vortices is finding the properparameter space to work in. These values should provide a good starting point:4
Stir Power:
Stirring Time:
Stirring Frequency:
Stirring Radius:
Equilibration Time

1.5µ200 ms0.85ωr
0.5RT F
500 msTable 2.1: Golden parameters for vortex creation.
In fact, Martin and I used these parameters in our first attempt at vortices andvoila! (Figure 2-6).5

4

These parameters are not pulled from thin air. Their origin can be found in the following 3
chapters.
5
I will never forget Martin’s reaction when this image appeared on the screen. He was so excitedthat he temporarily could only speak in German. It was a wonderful reminder of how Chandra andI felt the first time we made vortices.

36

Chapter 3
Vortex Lattices
Properties of vortex lattices are of broad interest in superfluids, superconductors andeven astrophysics. Fluctuations in the rotation rate of pulsars are attributed to the
dynamics of the vortex lattice in a superfluid neutron liquid [31, 26]. Here we showthat vortex formation, and the subsequent self-assembly into a regular lattice, are robust features of rotating BECs. Gaseous condensates may serve as a model system tostudy the dynamics of vortex matter.

This chapter supplements work reported in the following publication:
J.R. Abo-Shaeer, C. Raman, J.M. Vogels, and W. Ketterle“Observation of Vortex Lattices in a Bose-Einstein Condensate,”
Science 292 p.476-479 (2001).
(Included in Appendix A) Ref [2]3.1

Perspective

When I began my work at MIT in the summer of 1999, one of the major efforts inthe field was to demonstrate that BEC was a superfluid. There was not much doubtthat this was the case, however the proof was still very important. At the time,
two papers simultaneously provided the first evidence for superfluidity. One, from
E. Cornell’s group at JILA, used a phase-engineering technique to observe quantized37

circulation (a vortex) in a two-component condensate [70]. The second, from the
New Lab, used a “stirring” beam to demonstrate a critical velocity for the onsetof dissipation. A more dramatic demonstration of superfluidity came half a year
later from J. Dalibard’s group at ENS. Uniting the work of JILA and MIT, the ENS
group used a rotating stirrer to generate up to 4 vortices in their condensate [67].
The results were quite stunning. As a consequence of vortex-vortex interactions, thevortices arranged themselves into symmetric arrays. In addition, the vortices weremore robust than had been expected, with lifetimes over 1 s.
While our critical velocity results indicated that the dissipative mechanism wasindeed vortex creation, our direct entry into vortices did not begin until the summerof 2000. At this time Wolfgang suggested we attempt to image the vortices created
via our stirring technique. The prospects were exciting because our experiment had
25 times more atoms than the ENS experiment. My rough calculation predicted we
could see as many as 136 vortices.1 However, we were hoping for around 30, whichstill seemed very ambitious.
The road leading to the actual observation of vortex lattices was very rocky.
Chandra and I spent 3-4 months trying to make vortices. We spent many long nights
wondering where the vortices were. Finally, Chandra decided we needed put an end
to the experiment. I was disappointed, but I begrudgingly agreed on the condition
that we give it one last shot.2 Methodically, we went through the process of aligning
the stirring beams to the condensate. The beam size was tailored to what we believed
was the ideal size. The final, and most crucial, step was to verify that the condensate
was actually rotating.
The mistake we made from the outset was to assume that a larger set of stirring
beams (similar to ENS’s set-up) would be superior to a small stirrer (similar to our
critical velocity set-up) for making vortices. We thought that it was probably betterto gently rotate the entire fluid, rather than to simply tear through a section of1

My methods for arriving at this value were primitive and lacked any physical understanding ofvortices. I was clever enough to recognize that this number was too high. Under the calculation I
noted “This is Ridiculous!” Ironically, for quite awhile our record number of vortices stood at 134.
2
I agreed recognizing that Chandra was soft-hearted and would probably have continued withthe experiment so as not crush me.

38

Figure 3-1: First signal of vortices. The best image from the night we observed
vortices.

it. As we will see in Chapter 4, large beams are only effective at stirring over anarrow frequency range, corresponding to the surface mode resonance [78]. In ourpast attempts to stir we chose our frequency arbitrarily. This time we set our stirring
frequency to the surface mode frequency and observed in situ that our condensate
was rotating (See ref.[78] for an explanation of how this is done.). When we released
the condensate from the trap, we noticed a marked difference from our past attempts
to stir. The surface of the condensate was very rough, possibly due to vortices. After
another few shots we had convinced ourselves that they were indeed vortices. Our
best image that night was no thing of beauty (see Figure 3-1). Nonetheless, I wasable to count around 30 vortices in the image. Chandra and I were overjoyed.3 The
next day we were surprised to find that by varying the stirring parameters a bit andallowing 500 ms of equilibration time after the stir, a beautiful lattice of (85) vortices
formed. Our next two weeks in lab are the subject of the present chapter.
As a side note, prior to the work at ENS, vortex physics (in BEC) was driven
mainly by theory. Indeed, JILA’s method for observing the first vortex came from a3

I regret that were unable to share in this excitement with our former colleague Roberto Onofrio,
who had completed his tour in the lab 6 months earlier. His work in the the New Lab helped tomotivate this study.

39theoretical proposal by Williams and Holland [105]. Most theory at this time focusedon systems of one or two vortices. (Because vortices had proven so difficult to create, it
might have seemed too ambitious to consider systems with many.) The experimental
results of ENS and our lab surpassed expectation. Theorists were forced to playcatch up, developing new tools to model the bulk properties of vortices. However,
the theorists fought back,4 proposing new experiments requiring as many vortices
as particles [47]. Our current experiment is still 99,999,828 vortices away from thisregime, which should give theorists plenty of time to catch their breath.

3.2

Observation of Vortex Lattices

A detailed description of our observation of vortex lattices can be found in Appendix
A. Here I will only highlight important results that set the foundation for futurestudies.
The main result (Figure 3-2) shows highly-ordered triangular lattices of variable
vortex density containing up to 130 vortices. Such “Abrikosov” lattices were firstpredicted for quantized magnetic flux lines in type-II superconductors [4]. A slice
through images shows the visibility of the vortex cores (Fig. 3-3), which was as high as
80%. The lattice had a lifetime of several seconds, with individual vortices persisting
up to 40 s. We can estimate from Eq(2.15) that during its lifetime, the superfluid
flow field near the central vortex core had completed more than 500,000 revolutions
and the lattice itself had rotated approximately 100 times.
At the time, this represented a marked improvement for superfluid vortices. Prior
to this work, the direct observation of vortices had been limited to small arrays(up to 11 vortices), both in liquid 4 He [108] and in rotating gaseous Bose-Einsteincondensates (BEC) [67, 68]. This new regime enabled us to explore the propertiesof bulk “vortex matter”, including dynamics, local structure, defects, and long rangeorder.
A remarkable feature of these lattices is their extreme regularity, free of any major
4

An alternate view is that the dramatic strides made them overly optimistic.

40

A)

B)

C)

D)

Figure 3-2: Observation of vortex lattices. The examples shown contain (A) 16 (B) 32(C) 80 and (D) 130 vortices. The vortices have ”crystallized” in a triangular pattern.
The diameter of the cloud in (D) was 1 mm after ballistic expansion which represents
a magnification of 20.

41

Column Density (arb. units)

1.0

0.5

0.0
0

600
Position ( µm)

1200

Figure 3-3: Density profile through a vortex lattice. The curve represents a 5 µm
wide cut through a 2D image similar to those in Fig. 3-2 and shows the high contrast
in the observation of the vortex cores.

distortions, even near the boundary. This was a very surprising result for threereasons:
1) The condensate density is inhomogeneous. Why then should this not distort theradial symmetry?
2) The condensate has a hard boundary. Why are no edge effects manifest?
3) Numerical simulations under more ideal conditions (uniform density, infinite system) show distortion. Campbell and Ziff [13] tell us that in an infinite systemof uniform density, a configuration with perfect triangular symmetry can lower
its energy by rearranging the outermost rings of vortices into circles (see Figure
3-4).
This third reason only added to our bewilderment. Was nature really conspiringwith us?5 In a way it was comforting to see images like that in Figure 3-4c. Indeed,
we did observe more complex lattice configurations in a fraction of the images. Someshow patterns characteristic of dislocations (Fig. 3-5a), grain boundaries (Fig. 3-5b),
and partial crystallization (Fig. 3-6b).
5

I didn’t want to look a gift horse in the mouth, but times like this made me question whether
Chandra had made a deal with the Devil. Only time will tell.

42

a)

b)

c)

Figure 3-4: Structure of a vortex lattice. a) Numerical Simulation of the lattice structure in an infinite system with uniform density (taken from Ref[13]). The outermost
vortices lower the energy of the system by shifting slightly off-site. b) The real-world
situation is typically free of distortion. c) However, not every lattice is perfectly triangular. (We now recognize these types of features as collective modes of the lattice.
More on this in Chapter 5.)

3.3

Formation and Decay of a Vortex Lattice

The feature of our work that most fascinated me was the crystallization process(Figure 3-6). It is quite remarkable that such a turbulent system can relax into a
perfect lattice. The mechanism that “freezes out” the vortices was quite mysterious
then, and is still somewhat today. An in-depth analysis of this process is the subjectof Chapter 5.

43

a

b

Figure 3-5: Vortex lattices with defects. In (A) the lattice has a dislocation near thecenter of the condensate. In (B) there is a defect reminiscent of a grain boundary.

a

b

c

d

e

f

g

h

Figure 3-6: Formation and decay of a vortex lattice. The condensate was rotated for
400 ms and then equilibrated in the stationary magnetic trap for various hold times.
(A) 25 ms (B) 100 ms (C) 200 ms (D) 500 ms (E) 1 s (F) 5 s (G) 10 s (H) 40 s.
The decreasing size of the cloud in (E)-(H) reflects a decrease in atom number due
to inelastic collisions. The field of view is approximately 1 mm × 1.15 mm.

44

Chapter 4
Vortex Nucleation
Since the realization of BEC in 1995, the nature of quantized vortices has been the subject of much debate within the community. The first questions centered on creationand detection of vortices. How does one put angular momentum into the system?
How would vorticity manifest itself ? Initial difficulties in creating vortices led many
to question whether they were even stable. While work at JILA showed promise [70],all doubts were laid to rest by the pioneering work of the ENS group [67]. However,their work did raise new questions, specifically about the anomalously high criticalfrequency for nucleation. It is at this point that this chapter picks up.

This chapter supplements work reported in the following publication:
C. Raman, J.R. Abo-Shaeer, J.M. Vogels, K.Xu, and W. Ketterle“Vortex Nucleation in a Stirred Bose-Einstein Condensate,”
Phys. Rev. Lett. 87 210402 (2001).
(Included in Appendix B) Ref [83]4.1

Perspective

Work in this chapter was borne out from the desire to reconcile the results of ourstudies of critical velocity [84, 79] with our work on quantized vortices [2]. Even
before we had actually observed vortices, we were confident that the critical velocity
45

we measured could be attributed to the creation of vortices. Indeed, numerical simulations of our system predicted the appearance of vortex pairs at a critical velocity
very close to what we had observed [52]. These simulations relied on an energetic
argument given by the Landau criterion, which states that above a certain stirring
velocity excitations are energetically possible. The Landau critical velocity is given
by [48]vc = minp (ǫp /p).

(4.1)

where ǫp is the energy of the excitation with momentum p. However, initial results by
the ENS group [67] seemed to indicate that vortices were nucleated only at rotationalfrequencies much higher than those expected from the Landau criterion. At the time
this was a confusing result, and several ideas were proposed to explain it [30, 35],
including tunnelling barriers that required a higher rotation frequency to stabilize
the vortex. However, the ENS group correctly recognized that this discrepancy was
actually due to the stirring process itself. Their idea was that vortices were formed via
a dynamic instability (breakdown) of a surface wave. Surface mode resonances occur√
at ωr / ℓ, where ωr is the radial trap frequency, and ℓ is the polarity of the mode.
Therefore, because their two-point stirrer could only efficiently drive the ℓ = 2 surface
mode, this is the only region where they could produce vortices. However, stirrers ofhigher polarity should generate vortices at lower frequencies until the Landau criterion
is met.

√Ωs = minl (ωr / l).

(4.2)

Expressed here in terms of critical rotation frequency, but formally equivalent toEq(4.1).
In our first paper we observed this same resonant production, however we also√
showed that vortices could be generated at much lower frequencies than ωr / 2, simply by driving the surface mode off resonance (essentially power broadening it) [2].
However, the number of vortices we observed was always much smaller than theequilibrium value corresponding to rigid-body rotation.
In the present work we demonstrate that increasing the polarity of the stirrer does46

Number of Vortices

80
2-Points
3-Points
4-Points
60

40

20

0
20

30

40
50
60
Stirring Frequency [Hz]70

80

Figure 4-1: Discrete resonances in vortex nucleation. The number of vortices createdby multi-point patterns is shown.√The arrows below the graph show the positions of
the surface mode resonances ωr / l. Inset shows 2-,3-, and 4-point dipole potentials
produced by a 25 µm waist laser beam imaged onto the CCD camera.

indeed lower the frequency at which the maximum number of vortices are produced(Figure 4-1). More importantly, we demonstrate that the “global” surface wave resonances are not a necessity for creating vortices. Rather, they only act as an efficientmeans for coupling angular momentum into the system. The proof of this comeswhen we reduce the size of the stirring beams. In this case we no longer address
the condensate globally. Rather, vortices are generated via local instabilities. As
expected from our work on critical velocity, the number of vortices produced in thisregime simply increases linearly with rotation frequency (velocity).
As is often the case, what was once very confusing, is obvious in retrospect.
Vortices can be generated both locally, and globally, but the two mechanisms arefundamentally the same. At the time, this work went a long way in demystifying
the vortex making process. Indeed, we found that not only was it not necessary todrive the surface modes, it was actually an inferior scheme to creating the vortices
locally. Our findings can be summed up succinctly by two statements, one attributed
to James Anglin, and the other to Wolfgang Ketterle.1
1

These statements must be qualified. They only relate to vortices generated via stirring. Vortices
created using phase-engineering techniques [70, 65] need not meet these requirements.

47

a)
120

Rotation Frequency [Hz]100
Number of Vorticesb)

25 ms stir
80 ms stir
300 ms stir
600 ms stir

80
60
40

60

40

20

20
0

0
0

20

40
Stirring Frequency [Hz]

60

80

0

20

40
60
Stirring Frequency [Hz]80

Figure 4-2: Nonresonant nucleation using a small stirrer. a) Average number ofvortices created using a 2-point pattern positioned at the edge of the condensate. b)
Effective lattice rotation frequency. The lines in both graphs indicate the rigid-bodylimit (shifted to account for the critical velocity for nucleation.)• Vortices are generated at surfaces! Whenever questions arose about thedifference between local and global vortex excitation, James would emphaticallymake this statement. At the time it seemed a bit reductionist to me. Now I
cannot decide whether it is profound or trivial. In essence the statement is this:
There is no a priori reason to believe that vortices can only be generated at theThomas-Fermi surface of the condensate. The surface created by a small stirrer
passing through the condensate is just as good.
• Vortices are generated by surface instabilities. Wolfgang was fond of
making this statement in talks while showing the slide in Figure 4-3. It is essentially a restatement of the Landau criterion: above a certain critical velocity,
the flow at the surface becomes turbulent and breaks apart into vortices.

4.1.1

A Brief Aside...

The resonances in Figure 4-1 were close to the frequencies of excitation of l =2, 3√
and 4 surface modes (ωl /l = ωr / l) [19]. A second, higher resonance appeared inthe 3- and 4-point data. We originally postulated that this structure “could be due
to additional coupling to the quadrupole (l = 2) mode caused by misalignment of thelaser beams [16]. The extra peaks and the shift of the resonances from the frequencies
48

a)

b)

Figure 4-3: Surface instabilities nucleate vortices. a) As the fluid is excited, surface
instabilities begin to appear. b) At some critical excitation amplitude a vortex stateis energetically favored. The field of view is 20” × 15”. Experimental data courtesyof W. Ketterle.

ωl /l may be due to the presence of vortices and the stirrer, both of which make anunperturbed surface mode analysis inadequate.”
I would like to add an additional note that again seems obvious in retrospect. The
most likely explanation for the the structure in the 3- and 4-point data is that thesystem was overdriven. (The 2-point data was taken at much lower stirring powerand hence does not exhibit this same behavior.) The coupling was so strong on
resonance that vortices were ejected from the system. Thus, the number of vortices
dips sharply on resonance. We see similar behavior when we stir the condensate near
the trap frequency. This simple explanation did not occur to any of us at the time.
It actually came about three years later when I showed the data to Martin Zwierlein,
who upon glancing at the curves said something to the effect of “Aaahhh, this is where
you super power-broadened the resonances.” to which I responded with an ”Oohh —(expletive)!”

4.2

Vortex Structure

At low rotational velocities, vortices should not be rectilinear as assumed in many
theoretical calculations but bent [36, 5]. Such bent vortices should have lower visibility

49

Figure 4-4: Three-dimensional structure of vortices. Shown are several examples oftime-of-flight pictures of condensates at low rotational frequencies, where “smearedout” vortex cores and elongated features were observed. The condensate radius was
510 µm.

due to the line of sight integration across the optically pumped condensate slice.
Figure 4-4 shows several examples. Some appear as vortex lattices with tilted vortex
cores. Other images show structures reminiscent of half rings and coiled vortices.
However, it is not obvious how some of the observed time-of-flight features are related
to spatial structures in the trapped condensate.

4.3

Effects of Rotation

In our earlier work we observed that the size of a condensate with vortices exceeded
the size of the non-rotating condensate [2]. Figure 4-5 shows an enhancement of
the cloud size R in time-of-flight by up to 25% due to additional rotational kinetic
energy. Rotation adds a centrifugal potential − 21 M Ω2 r2 , leading to an effective radialtrapping frequency ofnext chapter.

qωr2 − Ω2 .2 Let us keep this effect in mind as we move to the2This, of course, sets the trap frequency ωr as the limit to how fast we can rotate the condensate
before losing confinement.

50

a)

Radial Size [Rstir /Rtof ]

1.20

1.10

1.00

0
b)

20

40
60
80
Number of Vortices
c)

100

120
d)

e)

Figure 4-5: Centrifugal effects on a rotating condensate. a) Observed radial size ofthe condensate, as determined from a parabolic fit to the time-of-flight distribution
after 41.5 ms. (b,c) Comparison of a non-rotating condensate (Rtof = 570 µm) and
one with 160 vortices. Radial in-situ phase contrast imaging of d) a condensate atrest, and e) in rotation at a frequency of 75 Hz, showing the modified aspect ratio.
The length of the condensate in d) was 200 µm.

51Chapter 5
Formation and Decay of Vortex
Lattices
The striking regularity of vortex lattices may be viewed as a rather auspicious featureof nature. While Abrikosov and Tkachenko showed that these triangular lattices areenergetically favored, it was unclear whether the dynamics of the system would allow adisordered state to “crystallize”. Here we investigate the time scales and mechanisms
for this crystallization. In contrast to the decay of the vortex lattice, temperature appears not to play a critical role in its formation.

This chapter supplements work reported in the following publication:
J.R. Abo-Shaeer, C. Raman, and W. Ketterle“Formation and Decay of Vortex Lattices in Bose-Einstein
Condensates at Finite Temperatures,”Phys. Rev. Lett. 91 070409 (2002).
(Included in Appendix C) Ref [1]5.1

Introduction

Here we report the first quantitative investigation of vortex dynamics at finite temperature. The crystallization and decay of a vortex lattice have been studied and52

Figure 5-1: a) Spin down of a rotating condensate in a static magnetic trap. The firstphase contrast image is taken 200 ms after turning off the drive, with each subsequent
image spaced by 200 ms. The rotating vortex lattice caused a radial swelling of thecondensate, reducing the aspect ratio. As vortices leave the system the aspect ratio
approaches its static value of 4.2. The field of view is 25 µm by 75 µm.

a striking difference is found between the two processes: while the crystallization
is essentially temperature independent, the decay rate increases dramatically withtemperature.
As mentioned in Chapter 4, the condensate’s rotation rate can be inferred fromits centrifugal “bulge”. Because of this, the decay rate can be determined by taking
a series of in situ images of a single condensate.
In studying the formation process an interesting experimental challenge arises:
How exactly can we quantify formation? A clever method devised by my colleague T.
Rosenband will be introduced, and then revisited in more depth later. Results fromthe formation analysis will allow us to draw some surprising conclusions about themechanism driving formation.1

5.2

Decay of Vortex Lattices

The decay of the vortex lattice can be observed by monitoring the centrifugal distortion of the cloud due to the presence of vorticity. This is a quantitative measure forthe rotation frequency, Ω, of the lattice, and therefore the number of vortices [77].
Such distorted shapes have been observed previously for rotating clouds[2, 41, 83].
The shape of a rotating condensate is determined by the magnetic trapping po1

As is often the case in physics, what seems surprising to some is obvious to others. However, tothe best of my knowledge, this formation mechanism is still an open-ended question.

53

Aspect Ratio

4.0
3.5
3.0

Nc / N
0.78
0.75
0.71
0.62

2.5
2.0
0

2

4

6
Time (s)8Lattice Rotation Frequency (Hz)

b)

a)

60
50
40
30
20
0

10

2

4

6
Time (s)810Figure 5-2: Decay of a vortex lattice at finite temperatures. a) The aspect ratio of
the condensate approaching its static value. b) The decay of the rotation rate of thelattice for the same data using Eq. (5.1). The decay of the rotation depends strongly
on the thermal component.

tential and the centrifugal potential − 12 M Ω2 r2 , where M is the atomic mass. Fromthe effective radial trapping frequency ωr → ωr′ =ratio of the rotating cloud, A′ = ωr′ /ωz , asqωr2 − Ω2 , one obtains the aspectqA′ = A 1 − (Ω/ωr )2 .

(5.1)

The damping rate of the vortex lattice, obtained from exponential fits to the data,
was studied at different temperatures by varying the condensed fraction of atoms in
the trap.
Figure 5-2a shows how the aspect ratio of the condensate approaches its static
value as the vortex lattice decays. The decrease of the angular speed appears to
be exponential (Figure 5-2b) and strongly depends on temperature (Figure 5-3). It
should be noted that the exponential nature of the decay is related to the co-rotationof the thermal cloud with the condensate. When the thermal cloud is fixed, theoretical[112] and experimental [67] studies show nonexponetial behavior.

5.3

Formation of Vortex Lattices

In addition to the decay process, the formation of the vortex lattice has also been
examined. After rotating the condensate it typically took hundreds of ms for the54

Decay Rate (1/s)

Decay Rate (1/s)

2.5
2.0
1.5

3.0
1.5
0.0
0.0

1.0

0.3
T / Tc

0.6

0.5
0.60

0.65
0.70
0.75
Condensate Fraction

0.80

Figure 5-3: Decay rates for vortex lattices at several temperatures. The rates are
determined from data taken during the 1st second of equilibration.

lattice to form (see Figure 4 in ref. [2]). One may expect the lattice to form in therotating frame during the stirring because the lattice is the lowest energy state fora given angular momentum. The absence of equilibration in the rotating frame ispresumably due to heating and excitation of collective lattice modes by the stirring
beams. The crystallization of the vortex lattice was studied by determining thecontrast or visibility of the vortex cores as a function of equilibration time. To avoid
any bias, we used an automated vortex recognition algorithm. First, each image wasnormalized by dividing it by a blurred duplicate of itself. A binary image was thencreated, with a threshold set to the value at which the algorithm reliably detected
almost all vortices that were identified by visual inspection of equilibrated images(there was less than 5% discrepancy). Clusters of contiguous bright pixels withina circular area were counted as “visible” vortices. Figure 5-4a shows three vortex
lattices after different equilibration times with the visible vortices identified.
Figure 5-4b,c show that the formation of the lattice depends very weakly, if at all,on temperature over the range studied. The larger number of vortices crystallized atlower temperatures (Figure 5-4b) is due to the strong temperature dependence of thelattice decay rates, which differed by more than a factor of 5. We can correct for thisby estimating the number of vortices Nv (t) as a function of time from the centrifugal
distortion measurements described above as Nv (t) = 2Ω(t)/κ·πR(t)2 , where κ = h/M

55

a)

b)
Number of Visible Vortices

140
120
100
80
60
Nc / N
0.78
0.75
0.71
0.62

40
20
0

c)

100

200
300
Time (ms)

400

500

100

200
300
Time (ms)

400

500

Visibility of Vortices

1.0
0.8
0.6
0.4
0.2
0.0

Figure 5-4: Crystallization of the vortex lattice. a) The top row shows three condensates that have equilibrated for 50, 150 and 300 ms, respectively, and have 48, 86
and 140 vortices recognized as “visible” by our algorithm. The bottom row shows
the same condensates with the “visible” vortices circled. The field of view was 1.4
mm by 1.6 mm. b) Growth of the number of visible vortices for several temperatures
expressed by the condensate fraction (Nc /N ). c) Visibility of vortices derived fromthe data in figure b, normalized by the number of vortices inferred from centrifugal
distortion measurements.
56

is the quantum of circulation, M the sodium mass and R the radial Thomas-Fermi
radius. By normalizing the number of visible vortices by this estimate, we deduce thevortex visibility as a function of time. These lattice formation curves overlap almost
perfectly for different temperatures (Figure 5-4c).

5.3.1

Damping Mechanism

In contrast to the decay, the crystallization process of the vortex lattice was essentiallyindependent of temperature. This was unexpected because all dissipative processes
observed thus far in BECs, including the decay of the vortex lattice, have shown astrong temperature dependence [53, 92]. D. Feder has numerically simulated a stirredcondensate using only the Gross-Pitaevskii equation. The results show that the absence of dissipation leads to rapid, irregular motion of the vortices. The addition of aphenomenological dissipative term in ref. [99] resulted in the formation of triangularvortex lattices. However, the origin of the dissipation was not identified. Our results
suggest that the time-limiting step for the evolution of a vortex tangle into a regularlattice does not depend strongly on temperature. One possibility is that the thermal
cloud is not directly involved. This may be similar to the reconnection of vortices orthe damping of Kelvin modes, where the spontaneous creation of excitations act as adissipative mechanism [63]. Another possibility is that the rearrangement of the vortices into a rectilinear lattice is slow and not limited by dissipation. Our quantitative
analysis of the formation process seems to contradict qualitative observations madein Paris [67], in which the lattice ordering appeared to have temperature dependence.
This indicates that further study may be necessary to fully characterize the role ofthe thermal cloud in the formation process.

5.4“Visible” Vortices Revisited

The algorithm for defining a “visible” vortex was touched upon earlier. I revisit ithere because it was not only crucial to the experiment, but because it made such a
qualitative difference in our lives. Vortex lattices were both a blessing and a curse57

for Chandra Raman and me. This algorithm grew out of our desire to automate thevortex counting. For the previous paper on vortex nucleation [83], the two of us spentendless hours methodically counting the vortices as they appeared on our monitor.
For that paper alone we counted over 50,000 vortices by hand. By my estimate,
Chandra and I counted over 1 million total! Throughout this time Till Rosenband,
UROP extraordinaire, kept telling me he could write a program to do the counting
for us. Finally one night I demanded that he deliver. By the time I came to work thenext morning Till had a working program.

5.4.1

Vortex Counting Algorithm

How can we quantify the formation process? The answer is relatively simple: countthe number of vortices that become “visible” over time. The obvious question thenbecomes: What defines a “visible” vortex? This answer is again simple. It does notmatter how you define a visible vortex as long as the following criteria are met:
• There should be some time dependence on the number of “visible” vortices. We
know that as the lattice crystallizes, the visibility increases. Thus, our program
should detect this qualitative behavior• Under identical conditions, the visibilty should be consistent from shot-to-shot.
• The number of vortices that the program counts after crystallization should beconsistent with hand counts.
Any algorithm that meets these three criteria works. Figure 5-5 details our approach.

58

a)

b)

c)

Smoothf)e)d)ThresholdEnhance

Count
g)

h)

FinishFigure 5-5: Vortex counting algorithm. The raw image in (a) is divided by the imagein (b), a blurred duplicate of itself, resulting in the image in (c). This removes thedensity profile of the condensate and normalizes the brightness of each vortex. This
image is then smoothed to remove noise, resulting in image (d). Bright features(vortices) are enhanced by taking the exponential of image (d). A binary thresholdis then applied to image (e) such that all pixels below a certain value are set to zero
(white), while those above are set to 1 (black). (f) Clusters of contiguous bright
pixels above a certain area are counted as “visible” vortices. (g) The location ofeach “visible” vortex is marked on the original image. In this example the computer
counted 133 vortices, while a hand count yielded 134.

59

Chapter 6
Formation of Ultracold Sodium
Molecules
Extending the ultralow temperature regime from atoms to molecules has been a primary
goal for atomic physicists. Ultracold molecules offer promise for tests of fundamental symmetry and coherent quantum chemistry. Here I discuss experiments in whichquantum-degenerate molecules are created from cold atomic samples.

This chapter describes work reported in the following publications:K.Xu, T. Mukaiyama, J.R. Abo-Shaeer, J.K. Chin, D.M. Miller, and W.
Ketterle “Formation of Quantum-Degenerate Sodium Molecules,”Phys. Rev. Lett. 91 210402 (2003).
T. Mukaiyama, J.R. Abo-Shaeer, K. Xu, J.K. Chin, and W. Ketterle“Dissociation and Decay of Ultracold Sodium Molecules,”Phys. Rev. Lett. 92 180402 (2004).
(Included in Appendix D) Ref [76]

60

6.1

Why Cold Molecules?

The motivation for producing ultracold molecules is many-fold. Atomic Bose-Einsteincondensates are an ideal system for studies of macroscopic quantum phenomena, including tests of coherence, superfluidity, and collective excitations. The production ofmolecular condensates could facilitate an entirely new class of experiments. Promisingareas include quantum gases with anisotropic dipolar interactions, tests of fundamental symmetries, and “Superchemistry”, where chemical reactions are stimulated via
macroscopic occupation of a quantum state [44].
Despite substantial effort, the creation of molecular condensates has proven difficult. Unfortunately, some techniques that are successful for atom cooling are noteasily applied to molecules. Laser cooling is one example of this. Because molecules
lack closed (cycling) transitions, it is difficult to coax them into repeatedly scatteringresonant light [8]. Until recently, efforts to cool molecules focused mainly on buffer gas
loading [104] and Stark deceleration [9]. However, these techniques are still several
orders of magnitude from a phase-space density of unity.
Recently, the difficulty in cooling molecules directly has been circumvented by
preparing molecules from quantum-degenerate atomic samples. This, of course, requires that the molecules are formed without release of energy. Two methods have
proven successful for doing this: photoassociation [106, 87] and magneto-association[28, 45, 107, 85, 55, 113, 18, 96] (Figure 6-1). Photoassociation is a process whereby
two colliding atoms collectively absorb a pair of photons, forming a bound molecule.1
Magneto-association occurs when the energy of two colliding atoms is magneticallyshifted into resonance with a molecular state. While the translational temperatureof these molecules is commensurate with their source atoms, both methods create
molecules in highly-vibrational states. In the case of photoassociation, poor wavefunction overlap limits coupling to the last few levels of the ground state potential(The Franck-Condon principle). For magneto-association, the vibrational levels arelimited to those that are (magnetically) accessible. The closest states to threshold
1

This is a specific case of photoassociation. Single photon transitions are also possible, howevermolecules can only be formed in an excited molecular state (due to selection rules).

61

a)

b)
V(r)

V(r)

EnergyEnergyB-Field

ν1

ν2

Atomic Separationr

Atomic Separationr

Figure 6-1: Methods for producing ultracold molecules. a) Photoassociation: By
choosing ν1 , ν2 properly, one can induce Raman transitions between free-atom andbound molecular states. b) Magnetoassociation: An applied magnetic field shifts aclosely-lying molecular state into resonance with a free-atom state. As the molecularstate passes below the free-atom state, atoms are converted to molecules. As discussed in the text, both processes create molecules in translationally cold, but highvibrational states.

are typically the highest vibrational states of an excited molecule (on the order of thehyperfine splitting). Because the vibrational ground state of the excited molecule is∼ 50 GHz below these states, a field of ∼ 5 T is required bring it into resonance.
It is important to note that these ultracold samples are not molecular condensates(at least not directly after creation). For Fermionic molecules2 the reason is simple,
they were not a condensate to begin with. Indeed, these molecules simply inherit
the momentum distribution of their source (a degenerate Fermi gas). For Bosonicmolecules the reasons are more subtle and may even depend on how one defines a
BEC.
I begin this chapter with a discussion of basic principles underlying Feshbach resonances. Feshbach resonances are currently the most popular method for generating
ultracold molecules. Next, I describe the experimental realization of quantum degenerate sodium molecules. Some important (and unfortunate) properties are covered,such as initial phase-space density and lifetime. Finally, I conclude with a discus2

To clarify, I use the terms “Fermionic molecules” to describe molecules composed of Fermionic
atoms and “Bosonic molecules” to describe molecules composed of Bosonic atoms. Of course, bothclasses of molecules are Bosonic. The terminology is a bit sloppy, but it greatly simplifies the text.

62

sion of the characteristics that define a Bose-Einstein Condensate, and why Bosonicmolecules have (thus far) failed to meet these criteria.

6.2

Feshbach Resonances

The analysis of atom-atom interactions is fairly simple in the ultracold regime (∼1 µK). At these temperatures the de Broglie wavelengths (∼ 104 a0 ) of colliding atoms
extend much further than their atomic diameters (∼ 102 a0 ). Because waves impinging
on small objects (compared to their wavelength) produce primarily isotropic scattering, it is appropriate to limit our treatment of ultracold interactions to the s-wave
regime. In this case the two-body Hamiltonian V (~r1 , ~r2 ) can be approximated by the
local Hamiltonian [81]V (~r1 , ~r2 ) =4πh̄2 aδ(~r1 − ~r2 )
m

(6.1)

where m is the atomic mass and a is the s-wave scattering length. The precise valueof a depends on details of the interatomic potential, and very small variations can
produce dramatic variation. Recall from Chapter 1 that the magnitude and sign ofa dictate the macroscopic properties of the condensate, including the density profileand stability. When the scattering length is positive, atoms bounce off one anotherlike hard spheres of radius a. When the scattering length is negative, atoms tend to
attract, and the condensate is stable only for small numbers of atoms [86].
The fact that the interaction strength depends critically on this single parametera has very important consequences. As we shall see, both the magnitude and sign ofa can be externally controlled, providing experimentalists with unprecedented control
over the properties of the system. The feature that allows us to “tune” a is known
as a Feshbach Resonance [32]. In the vicinity of these resonances a diverges to ±∞(Fig. 6-2). Feshbach resonances occur when the total energy of two colliding atoms
equals the energy of a molecular state. Therefore, if the magnetic moment of themolecular state differs from the atomic state, one can use a magnetic field to Zeeman
shift the two states into resonance. The use of Feshbach resonances to tune atomic
interactions was first suggested in 1992 by B. Verhaar and colleagues [97].
63

a

a0
∆B

B

B

0

Figure 6-2: Resonant enhancement of the scattering length in the vicinity of a Feshbach resonance. Resonances of this type occur when a new bound state is introduced
to the system. The lineshape has functional form a = a0 [1 − ∆B/(B − B0 )], wherea0 is the background scattering length, ∆B is the width of the resonance, and B0 is
the resonance center.

6.2.1

Model of Feshbach ResonanceTo understand why scattering is enhanced in the vicinity of a Feshbach resonance weturn our attention to a simple model for colliding atoms at threshold (Figure 6-3)[20]. The van der Waal potential, typical of interatomic interactions, is replaced bya spherical box of depth V0 and extent b. Since we are considering only s-waves welook for solutions to the Schrodinger equation with ℓ = 0.
ψ ′′ (r) −2µV (r)ψ(r) = 0h̄2where µ is the reduced mass of the system. Defining k =

(6.2)
√

2µV0 /h̄, the solutions toEq(6.2) are A(r − a)ψ(r) =  Bsin(kr)

r≥b

(6.3)

r<b

Therefore, the scattering length has form

a=b−tan(kb)k

A plot of this function is given in Figure 6-3c. From this we note the following:
64

(6.4)

a)

b)

V(r)

c)
V(r)

a/b 4

EnergyEnergy

3
2
1
2

r

b

r

4

6

8

10

kb

-1
-2

-V0
Atomic Separation-3

Atomic Separation

Figure 6-3: Toy potential to illustrate resonant scattering. a) The van der Waal
potential is typical of interatomic interactions. This potential is modelled by b) an
exactly-solvable toy potential. c) As the potential depth V0 is increased, the scattering
length diverges each time a new bound state is introduced to the system.

1) As the depth of the well V0 is increased, the scattering length diverges wheneverkb = (2n + 1)π/2. This is equivalent to the condition that the spherical wellpossesses a zero-energy bound state. Thus, we see that resonances occur upon
the appearance of a new bound state.
2) Away from the resonances the scattering length approaches the background valueb, the same behavior we observed in Figure 6-2.
3) Slightly below the threshold for the appearance of a bound state, a becomes large
and negative. Above threshold a switches sign. Therefore, in order to makemolecules we should sweep the atoms from the negative side of the resonanceto the positive side.
To be clear, the model used here is that of a single-channel resonance. Feshbachresonances are inherently two-channel features. However, the characteristic behavior
is identical.

6.2.2

Experimental Notes

The first observations of Feshbach resonances were not made by observing molecule
creation directly, rather by measuring enhanced losses and a dispersive variation of
the scattering length in the vicinity of the resonance[50, 93]. Typically, the main loss65a) V(r)
b)

c)

Pow!
m = +10-1r

Figure 6-4: Loss mechanism in the vicinity of a Feshbach resonance. a) In three-bodyrecombination two atoms form a deeply bound molecule, with the third carrying away
the excess energy. When the scattering length is increased, the probability that threeatoms will come in contact also increases. b) The three hyperfine states just below
the 907 G resonance of |1, 1 > state. c) Passing through the resonance, atoms in them = +1 are preferentially lost.

mechanism for a condensate is three-body recombination (Figure 6-4). In this process
three atoms come together to form binary molecule, with one atom carrying away thebinding energy. Because this process requires three atoms to come in contact, its
occurrence is rare.3 However, at the Feshbach resonance |a| is greatly enhanced, andthus, so to is the likelihood of contact. Therefore, the primary signature of Feshbachresonances in bosonic systems is strong inelastic decay.

6.3

Production of Molecules

To generate the molecules, sodium condensates in the |F = 1, mF = −1i state wereprepared in an optical dipole trap. The radial and axial trap frequencies of ωr =2π×290 Hz and ωz = 2π×2.2 Hz, respectively, gave Thomas-Fermi radii of Rr = 5 µm
and Rz = 650 µm, and a peak density of 1.7 × 1014 cm−3 for 5 million atoms. An
adiabatic radio frequency sweep was used to transfer the atoms into the |1, 1i state,
which has a 1 G wide Feshbach resonance at 907 G [50, 100].
After 1 second equilibration in the optical trap, the molecules were generated
3

At least this is the case for typical peak densities of ∼2 1020 m−3 .

66

a)
B
a<0

(ii)

(iii)

a>0 (i)

c)

Blast

(iv)

Optical Trap On
b)

(vi)

d)

(v)

TOF

(vii)

913 G
907 G
903 G

ImagingTimee)Figure 6-5: (a) Experimental method for producing and detecting ultracold molecules.
(i) Bose condensed atoms in an optical dipole trap are exposed to a magnetic field justbelow a Feshbach resonance. (ii) The field is quickly stepped through the resonanceto minimize atom loss. (iii) The field is then swept back through the resonance,
creating an atom-molecule mixture. (iv) Unpaired atoms are removed from the trapwith resonant light, yielding a pure molecular sample. (v) The trap is switched off,
allowing the molecules to expand ballistically. (vi) Finally, the magnetic field is swept
back across the resonance to reconvert the molecules to atoms for imaging (vii). (b)Image of the atomic sample after ramping the field to produce molecules; (c) after
the resonant light pulse has removed all unpaired atoms; (d) after the molecules(∼ 105 ) have been reconverted to atoms. (b-c) were taken along the weak axis of thetrap after 17 ms ballistic (time-of-flight – TOF) expansion. (e) An image showing
both atomic (top) and molecular (bottom) clouds after 14 ms ballistic expansion,
spatially separated by a magnetic field gradient. With 4 ms field ramp-down time,some molecules survived even without the blast pulse, but are much more heated.
The field of view of each image is 1.8 mm × 1.3 mm.

67

a)

b)

V(r)

Blast

x

Blast

δ

r

Figure 6-6: “Blast” pulse for removing unpaired atoms. a) To remove unpaired
atoms from the trap, the sample was irradiated with a 10 µs pulse of resonant light.
b) Because the blast was done at a field far from the Feshbach resonance, the mixing between atomic and molecular states was small, and therefore molecules weretransparent to pulse.

using the field ramping scheme illustrated in Figure 6-5a. An applied magnetic field
was ramped in ∼100 ms to 4 G below the 907 G Feshbach resonance. The field was
generated using a pair of large bias and small anti-bias coils. Because molecules are
only created when sweeping across the resonance from negative to positive scattering
length, the field was stepped up to 913 G as quickly as possible (∼1 µs) to jumpover the resonance with minimal atom loss. After allowing 2.5 ms for transient field
fluctuation to damp out, the field was ramped down in time τDown . Due to atommolecule coupling, part of the atomic population was transferred into the molecularstate following the Landau-Zener avoided crossing. With the given width of theresonance and the atomic density, we use a simple Landau-Zener model to calculatea ramp speed of ∼104 G/s to transfer roughly half the atoms to the molecular state[72, 101, 110]. However, inelastic collisions led to fast decay for both the atoms andthe molecules near the resonance. We found that a faster ramp speed of ∼105 G/s(corresponding to τDown = 50 µs) gave optimal results. The conversion efficiency ofatoms to molecules was ∼4%. Slower ramp speeds resulted in a similar number ofmolecules, but at higher temperature (see Figure 6-5e).
The blast pulse was applied along the radial axis of the trap to minimize collisions68

4 ms 6 ms 8 ms 10 ms 12 ms 14 ms 16 ms 18 ms 20 ms
Figure 6-7: Ballistic expansion of a pure molecular sample. Absorption images ofmolecular clouds (after reconversion to atoms) are shown for increasing expansion
time after switching off the optical trap. The small expansion velocity corresponds
to a temperature of ∼30 nK, characteristic of high phase-space density. The images
are taken along the weak axis of the trap. The field of view of each image is 3.0 mm
× 0.7 mm.
between the escaping atoms and the molecules at rest (see Figure 6-6a). A 20 µs
pulse of resonant light removed all atoms from the optical trap, leaving behind a puremolecular sample (see Fig. 6-5). At only 4 G below the Feshbach resonance, the light
was still close to resonance with molecular photodissociation to low-velocity atoms,
but the overlap matrix element was sufficiently diminished to leave the molecules
unaffected (see Figure 6-6b). After a variable hold time, the optical trap was switched
off and the molecules expanded ballistically for between 4 to 20 ms. The molecules
were detected by converting them back to atoms with field ramp-up in τU p = 100 µs
at the end of expansion. Varying τU p between 50 µs and 4 ms did not affect therecovered atom number, though shorter τU p ’s recovered atoms with larger kinetic
energy [76]. Thus we assume all molecules are converted back to atoms. A resonant
absorption image was taken after an additional 500 µs, which allowed the imaging
field to settle. The rapid conversion of molecules to atoms after a long expansion timeensured that the absorption images accurately depicted the momentum distributionof the molecular cloud.
69

Atoms and molecules were separated during the ballistic expansion by a SternGerlach technique (Figure 6-5e). Due to trap imperfections, the large bias coils
provided an additional radial gradient of the axial field of ∼2.8 G/cm in the vicinityof the condensate. This value was determined from the trajectory of the falling atoms.
Since the molecules have a different magnetic moment, they separate from the atoms
during the ballistic expansion (Figure 6-5e). From the separation of the atomic andmolecular clouds at different times, we determined the difference between atomic
and molecular magnetic moments to be 3.2µB (µB is the Bohr magneton), in good
agreement with theory [110].

6.4

Molecular Properties

6.4.1

Phase-Space Density

For different ramp down times τDown , the time-of-flight images of the molecular cloudexhibit drastically different momentum distribution. The coldest cloud was obtainedwith the fastest ramp down time possible, τDown = 50 µs (Fig. 6.3). A gaussian fit
was used to determine the molecular temperature Tm and the phase-space density.
Due to the rapid ramp down, the molecules had no time to adjust to the externaltrapping potential or any mean-field interactions. Therefore, we assume the molecules
were uniformly created with the Thomas-Fermi profile of the original atomic BEC.
The peak phase-space density is then given by
P SDpeak =Ãh√2πkB Tm Mm

!3

Nm
8π 2
R R
15 r z(6.5)

where h is the Planck constant, kB is the Boltzmann constant, Mm is the molecularmass, Nm is the number of molecules. The second factor in the equation is the peakdensity for a Thomas-Fermi profile.
Phase-space densities in excess of 20 were observed, much larger than the criticalvalue of 2.6. This demonstrates that a quantum-degenerate cloud of atoms can betransformed into a quantum-degenerate molecular gas.
70

150
100

Temperature (nK)

300

50
0

2

4

6

200

100

0

10

Hold Time (ms)20

30

Figure 6-8: Temperature of the molecular cloud. After 15 ms, the temperature saturates at ∼ 250 nK. Error bars represent the statistical error (standard deviation).
The inset shows finer resolution data for holding times up to 6 ms. The solid line isa guide to the eye.

6.4.2

Molecular Lifetimes

Further experiments with ultracold sodium molecules will critically depend on theircollision properties. Therefore we studied heating and inelastic collision processes.
As shown in Figure 6-8, we observed monotonic heating of the pure molecular sample
over ∼ 30 ms. In addition, we observed short timescale oscillations (6 ms) in the fitted
temperature (inset of Figure 6-8). Such breathing oscillations were excited because
the molecules were formed over the volume of the atomic condensate and started
oscillation around their equilibrium volume (see Figure 6-9). The equilibrium volume
deduced from the observed released energy is much smaller than the initial volume.
The absence of damping implies a collision time of at least 6 ms, or a molecular
scattering length smaller than 17 nm (obtained using the expression for the collision
rate 8πa2 vth nm where vth is the thermal velocity). It is unclear whether the oscillation
disappeared due to collisions or limited signal-to-noise ratio.
The temperature of the molecular cloud saturated at ∼ 250 nK after 15 ms. A
possible explanation is the balance between heating due to inelastic molecular decay
and the evaporative cooling caused by the finite trap depth (1.7 µK). This would imply
71

a)

b)

c)

Pair

Blast

d)

Collapse

Figure 6-9: Collapse of a molecular cloud. a) The size of the atomic condensate is set
by its mean-field energy. b) After passing through the Feshbach resonance a small
fraction of the sample is converted to molecules. c) When unpaired atoms are blasted
away the molecules no longer have sufficient mean-field energy to sustain their size.
d) The molecules collapse and undergo breathing oscillations for a short period oftime (see the inset of Figure 6-8) before reaching their new equilibrium size.

a collision time of 15 ms. However, we have no clear evidence that thermalization has
occurred. Clearly, further studies of elastic collisions between ultracold molecules arenecessary.
Molecules formed via an s-wave Feshbach resonance are created in the rotational
ground state, but in high vibrational states. Therefore, one expects vibrational relaxation to be a strong, inelastic decay mechanism (Figure 6-10).
Figure 6-11(a) shows the decay of a pure molecular sample. The decay was analyzed with the rate equationṄm= −Kmm nm .
Nm

(6.6)

Here Nm , nm is the number and the density of the molecules respectively, and Kmm
is the molecule-molecule collision rate coefficient. Because of the changing size andtemperature of the molecular cloud during the first ∼ 15 ms (Fig. 6-8), we only fit
data points at later times, assuming a thermal equilibrium volume for the molecules.
The decay at earlier times is slower, consistent with a larger molecular cloud. The fit
yields a molecule-molecule collision coefficient of Kmm ∼ 5.1 × 10−11 cm3 /s, about 2
orders of magnitude larger than the typical values reported for fermions [54, 18].
Inelastic collisions between molecules and atoms were also observed by keeping
atoms in the trap (Figure 6-11(b)). The decay was analyzed assuming that the lossof molecules occurred mainly due to collisions with atoms, resulting in an exponential

72

V(r)

Smack!

r

Figure 6-10: Decay mechanism for molecules. In the presence of atoms, molecules
quickly decay due to inelastic collisions. A molecule colliding with an atom will decay
into a lower vibrational state, with the excess energy converted to kinetic energy.
For bosonic molecules, these collisions limit the conversion efficiency and prevent
molecular condensation. In Fermi systems these collisions are suppressed by to Pauliblocking.

decay:Ṅm= −Kam na .
Nm

(6.7)

Here na is the density of atoms, and Kam is the atom-molecule collision rate coefficient.
From the fit, we extract a lifetime of 106 µs and a rate coefficient Kam ∼ 5.5 ×
10−11 cm3 /s, which agrees well with theoretical predictions [111, 110].

The inelastic losses determine the maximum conversion efficiency from atoms tomolecules. For an adiabatic ramp, one expects close to 100% conversion efficiency.
Indeed, in experiments with fermionic atoms, efficiencies up to 85% have been observed [18]. Figure 6-12 shows the results for magnetic field ramps of different durations. The two sets of images show that applying the blast pulse dramatically
improved the molecular number and temperature. Without it, a slower ramp time
(4 ms) appeared to be more favorable for molecule formation (open circles in Fig. 612(c)). No molecules were observed for a 50 µs ramp time. However, with the blast
pulse, a similar number of molecules was obtained for all ramp times between 50 µs
to 4 ms (closed circles in Fig. 6-12(c)).

73

(a)

blast

B
τhold
Time

(b)
+

τhold

blast

B

Time

Figure 6-11: Decay of ultracold molecules trapped alone (a) or together with atoms(b). The solid lines in (a) and (b) are fits of eq.(6.6) and (6.7) to data, which assume
vibrational relaxation in the collision of molecules (a) or collisions between molecules
and atoms (b). The insets illustrate the experimental sequences.

74

(a)

(b)

50 µs

(c)

Molecule Number

150x10200 µs

3

1 ms

4 ms

100
50
0
5

6 7 8 9

100

2

3

4

5

6 7 8 9Ramp Time (µs)

2

3

4

1000

Figure 6-12: Conversion of atoms to molecules for various ramp times. During a given
time, the magnetic field was swept by 10 G. Figures (a) and (b) show absorption images taken after 14 ms TOF. The molecules (bottom) were radially separated fromthe atoms (top) by a field gradient of 2.8 G/cm. The molecules were converted backto atoms only 0.5 ms before imaging by ramping the magnetic field back across the
Feshbach resonance. This time was chosen to be long enough for any transient field
fluctuations to damp out, but short enough such that the size of the imaged cloudreflected the molecular temperature, not the dissociation energy. (a) The atoms
remained in the trap. (b) The atoms were removed by a resonant laser pulse immediately after the magnetic field ramp. (c) Number of molecules as a function of ramp
time for (a) (open circles) and (b) (closed circles).

75

We assume that these results reflect the interplay of two competing processes.
The adiabatic condition requires a relatively slow field ramp for efficient conversion.
However, this means that the atoms and molecules spend more time near or at the
Feshbach resonance, where inelastic collision rates are enhanced. In contrast to Fig.612(b), the absence of molecular signal in Fig. 6-12(a) for 50 µs ramp time reflectsthat the atomic density reduction due to the mean-field expansion is too slow for themolecules to survive the inelastic collisions with the atoms.

6.5

What Makes a BEC a BEC?

Now that we have seen how bosonic molecules behave we are ready to make statements
about what they are (and what they are not). The translational temperature of themolecules is indeed (instantaneously) commensurate with their source (a BEC), and30 nK is well below the transition temperature Tc for this number of molecules.
Unfortunately, we also see that these molecules undergo fast vibrational relaxation.
Whether our molecular sample is a condensate depends on one’s definition of BEC.
If phase-space density in excess of 2.6 (corresponding to a diagonal matrix element of
the single-particle density matrix larger than one) is sufficient, then one may regarda short-lived atom-molecule superposition state [25] as a molecular BEC. However,following this definition, a small excited state admixture in an optically trapped BEC
would qualify as BEC of electronically excited atoms. If one asks for the additional
requirement of a pure molecular sample, we have achieved that in this work. Anotherdefinition would require phase coherence, which could again be observed even in shortlived samples. Should one also require a lifetime of the degenerate sample exceeding
the collision time (to achieve local equilibrium), the trap period (to achieve global
equilibrium), or the inverse mean-field energy (the typical dynamic timescale)? In our
opinion, BEC requires thermal equilibrium. High phase-space density is necessary,
but not sufficient.

76

6.5.1A Final Note

As we have seen, vibrational relaxation not only prevents Bosonic molecules fromcondensing, it also severely limits their conversion efficiency [28, 45, 107]. The creation of molecules in highly vibrational states is not a problem if there is no decay
mechanism to lower states. Indeed, this is the case for Fermionic molecules. Although
Pauli blocking starts them off at a disadvantage temperature-wise (compared to their
Bosonic counterparts), it also prevents three-body losses. Molecular condensation
then proceeds via simple evaporative cooling [85, 55, 113].

77

Chapter 7
Bragg Scattering
In recent years Bragg scattering has become an increasingly important tool in cold
atom physics. Its popularity can be attributed to its dual role as both an atom-opticaland spectroscopic instrument. This dual role was established early on by two papers:
In M. Kozuma et al. [60] Bragg scattering was used to coherently manipulate matterwaves. Their rudimentary use of Bragg scattering for coherent beam splitting advanced
the field of coherent atom optics and led to the development of nonlinear atom optics.
J. Stenger et al.[94] established Bragg diffraction as a tool for condensate diagnostics.
Here a measurement of the Bragg spectrum confirmed that the coherence length ofthe condensate is equal to its physical size [94]. Oftentimes experiments employ bothaspects of Bragg, first using it to prepare the condensate in some initial state and thenusing it to “readout” the response of the system. An example is found in ref [102],
where phonons were first imprinted with Bragg diffraction, and then their excitation
spectrum was measured using another set of Bragg beams.

7.1

Bragg Scattering: A Practical Guide

This chapter is intended to give the basics of Bragg1 for those interested in simple
theory and experimental techniques. The results are general and, therefore, appli1

Here I begin to use the colloquialism “Bragg” to encompass both Bragg processes (i.e. scatteringand spectroscopy), which are fundamentally the same.

78

Incident
Beamθ

Reflected
Beam

D

Figure 7-1: Bragg scattering of x-rays from a crystal. Due to superposition, x-raysreflected from the crystal planes constructively interfere only at certain angles. Thissame effect was demonstrated by Davisson and Germer (1927) using an electron beam,offering definitive proof of the wave nature of matter.

cable to atoms and molecules alike. The use of Bragg diffraction as a spectroscopic
tool is discussed in detail. Included are discussions of line shifts and broadenings,
both fundamental and technical. In addition, experimental techniques to limit noiseare covered. This section is by no means a complete discussion of Bragg scattering.
Rather, it is a summary of important results and technical issues that I found useful in our study of coherent molecular optics (see Chapter 8). For a review of thebasic theory of Bragg scattering, I refer readers to ref [38]. A discussion of Bragg
spectroscopy in the phonon regime can be found in ref [91].
In the most general sense, Bragg scattering arises from the diffraction of waves
from a grating. Because waves superpose, there are only certain scattering angles atwhich they interfere constructively. This is true for both light and matter. However,
because the Bragg diffraction of condensates employs gratings created by standing
light waves, a second picture arises to describe the system: Bragg scattering as a
stimulated Raman process. Both pictures are equally valid and rely on the same
basic principles of energy and momentum conservation. However, for clarity, I will
focus on the latter picture because coherent atom optics follows more naturally.

7.1.1

Grating Picture

Bragg scattering of matter waves is by no means a new technique. It has its rootsin two important experiments from the early 20th century. In 1912 M. von Laue
79

and later W.L. Bragg demonstrated that the wavelength of x-rays could be measured
by studying their diffraction from a crystal. Due to the wave nature of light, xrays were observed to scatter only at certain angles given by the Bragg condition for
constructive interferencenλ = Dsinθ(7.1)

where n is an integer and D is the atomic spacing (see Fig. 7-1). In 1927 C.J. Davisson and L.H. Germer used this same method to test de Broglie’s hypothesis thatmatter also possesses wave-like properties. Using a monoenergetic electron beam,
they observed the same directional scattering effect as had been demonstrated withlight. In the words of Davisson and Germer [21]:Because of these similarities between the scattering of electrons by the crystal andthe scattering of waves by three- and two-dimensional gratings a description of theoccurrence and behavior of the electron diffraction beams in terms of the scattering ofan equivalent wave radiation by the atoms of the crystal, and its subsequent interference, is not only possible, but most simple and natural.

In essence, the result is explainable if one attributes a wavelength to the electrons.
Furthermore, by changing the energy of their source, Davisson and Germer also confirmed the de Broglie wavelength relationship λdB = h/p, where p is the particle’s
momentum.
Bragg diffraction of atoms was demonstrated shortly thereafter (1930) [29]. However, only recently (1987) has it become a practical atom optical tool, with scatteringfrom optical gratings demonstrated first with thermal atoms [69] and subsequently
BEC [60]. In their simplest form, these optical gratings consist of two laser beams ofwavelength λL , which form a standing wave of periodicity λL /2sin(θ/2), where θ isthe angle between the beams. However, because condensates are produced in static
traps, it is more straightforward to move the grating rather than the BEC. This isaccomplished by applying a small, relative detuning, δ, between the beams. As a

80

a)

b)

θ
ν

1

κ

k1

ν

Energy

c)

k2

|e>

p2
2m

2

ν1

|g>

ν

2

-1
0
+1
Momentum (precoil)Figure 7-2: Bragg Scattering viewed as a stimulated Raman transition. a) Two beams
with frequencies ν1 , ν2 illuminate the condensate. b) The momentum imparted to thecondensate is equal to the difference in momenta, h̄~κ, between photons in the two
beams. c) Transitions to higher momentum states occur only if ~k1 , ~k2 are chosen suchthat energy and momentum are conserved.

consequence of energy conservation, scattering only occurs if the atoms’ speed in thegrating frame is conserved in the process (The condition for specular reflection).

7.1.2

Raman Picture

As stated earlier, Bragg scattering from an optical grating can also be viewed as a
stimulated Raman transition between momentum states (see Figure 7-2). One canthink of this process as an atom absorbing a photon from one beam and then being
stimulated to emit into the other.2 The difference in momenta between these two
photons h̄~κ, is transferred to the recoiling atom.
From Figure 7-2b we see that the recoil momentum and energy are given by3h̄~κ = h̄(~k1 − ~k2 ) = 2h̄ksin(θ/2)κ̂2h̄2 k 2
sin2 (θ/2)
hδ = h(ν1 − ν2 ) =
2m

(7.2)
(7.3)

where k = 2π/λL is the photon wavenumber. Thus, the condition for Bragg scattering
2

Strictly speaking, the correct view of this process is one of paired stimulated absorption andemission, resulting in the redistribution of a photon between the two beams.
3
Here we approximate |~k1 | = |~k2 | = k, which is justified because δ ∼ 100 kHz, compared to theoptical frequency of ∼ 500 THz.

81

a)

b)

0

c)

0
hκ
Momentum

hκ

0

hκ

Figure 7-3: Bragg diffraction of a BEC. Time-of-flight images represent a momentum
analysis of the condensate. Because the kinetic energy of the scattered atoms is muchlarger than the mean-field energy of the condensate, the momentum states are wellresolved in time-of-flight. a) The Bragg pulse scatters a fraction of the condensate
into h̄~κ momentum state. (The image is taken in the plane of the Bragg beams.)b) By choosing the pulse duration correctly one can make a “50/50 beamsplitter”
for matter waves. c) Out-of-plane view of the “50/50 beamsplitter”. The halos arecaused by collisions between the two momentum states [17]. From (c) it is evident
that atoms on the inner edges undergo more collisions. This is to be expected because
the two regions interact with one another longer.

is
ν0 =

2h
sin2 (θ/2)
2
mλ

(7.4)

Of course, this derivation assumes that the atoms were at rest. For atoms moving
with velocity ~vi , the resonance condition ishν = hν0 + h̄~κ · ~vi(7.5)

where the second term represents the Doppler shift (δνm = κ̂/λL ·~vi ) of the resonancedue to motion. The inclusion of this term illustrates the velocity selectivity of atomic
Bragg diffraction and foreshadows its use as a spectroscopic tool.

7.1.3

Coherent Population Transfer

Based on the stimulated Raman picture, coherent population transfer between momentum states is expected. Assuming coupling only between the |0i and |h̄~κi momentum states, the system behaves like a two-level system. Thus, for a given pulse

82

b)

1

Outcoupled Fraction [A.U.]a)Left Box
Right Box
0.5

0
-50

0

50

Relative Detuning (δ) [kHz]Figure 7-4: Bragg spectrum of a trapped condensate. (a) The spectrum is obtainedby varying the relative detuning δ of the Bragg beams. The sign of δ determines the
direction of scattering. For each image the number of particles in all three boxes arecounted. The outcoupled fractions are determined by taking the ratio of particles in
the left and right boxes to the center. (b) The locations and widths of the resonances
result from a combination of mean-field interactions and finite size effects.

duration τ , the population of the excited state |h̄~κi is2
ωr(2)Ωr(2) τPe (τ ) = 2 sin2
Ωr(2)
2

!

where ωr(2) is the two-photon Rabi rate and Ωr(2) =

q

Ã

(7.6)

2
ωr(2)
+ [2π(δ − ν0 )]2 . Thus,

the population will undergo coherent oscillations between the two momentum states
at frequency Ωr(2) . By varying τ arbitrary populations can be produced in eachstate. On resonance (δ − ν0 = 0) the Bragg beams act as a “50/50 beamsplitter” forτ = π/2Ωr(2) (see Figure 7-3b,c).
The treatment above must be qualified. As we shall see, atoms in a condensate
have a distribution of energies and velocities. Thus, the Bragg beams do not address
the entire condensate uniformly. Because of this, atoms in different regions of thecondensate oscillate at slightly different Rabi frequencies. After many cycles, one
expects equal populations in both states. In addition, collisions between the twostates (see Figure 7-3) cause further decoherence.

83

7.2

Bragg Spectroscopy

Figure 7-4b shows a typical Bragg spectrum. The spectrum is taken by varying therelative detuning δ, and then measuring the fraction of outcoupled atoms. The signof δ dictates the direction in which atoms are diffracted. By using both positive andnegative detunings two resonances are observed.
Evident from Figure 7-4b, Bragg transitions have a finite width. Eq(7.5) hints
that this width may result from a distribution of velocities in the condensate (seeFigure 7-5a). As we shall see, mean-field interactions also contribute to the width.
Therefore, to characterize the system accurately, it is important to understand how
these effects, and others, can both broaden and shift the spectrum.

7.2.1

Width of a Thermal Distribution

The onset of Bose-Einstein condensation is characterized by a sudden narrowing of theatomic momentum distribution. For later comparison, it is useful to find the frequency
width ∆νT of a thermal distribution at temperature T . From kinetic theory
2
kB T = mvrms(7.7)

where vrms is the RMS velocity. From Eq(7.5) we see that atoms moving at vrms are
Doppler shifted by the width of the resonance ∆νTh̄~κ · ~vrms = h∆νT

(7.8)

Thus, for a given temperature, the width of the distribution is
∆νT =

s

2kB T sin(θB /2)
m
λL

84

(7.9)

7.3

Broadening Mechanisms

Broadening mechanisms can be separated into two categories: fundamental and technical. Fundamental broadening is inherent to the system. For condensates, there
are two contributors to the fundamental width ∆νF : the finite sample size and themean-field. Both factors are related to the inhomogeneous density distribution of thetrapped condensate. Technical broadening is caused primarily by random motion of
the condensate and, in some cases, the finite duration of the Bragg pulses. With care,
contributions from technical noise can be made insignificant.
To understand how each mechanism contributes to the total width, we must firstconsider how broadening mechanisms combine with one another. For simplicity welimit the discussion to gaussian distributions.4 Consider the case of a transition ofwidth γ and a probe beam of width δ. The measured lineshape I(ν) is the convolutionof the two,I(ν) ∝

Z ∞

−∞

−ν

2

e γ 2 e−(ν+ε)2δ2−ν2dε ∝ e γ 2 +δ2(7.10)

Thus, we expect that contributions from unrelated mechanisms to add to width inquadrature.

7.3.1

Finite-Size Broadening

Heisenberg’s uncertainty relation requires that a sample with coherence length χc
has a momentum spread given by ∆p · χc ∼ h̄. Therefore, even if the coherence
length is the size of the sample (as is the case for a condensate), the Bragg transition
will still be Doppler broadened. To determine a precise value for the momentum
width, we must account for the particular density distribution. For a condensate, themomentum distribution is given byg(px ) ∝
4

Z

¯Z
¯2
¯
¯
i~
p·~
r 3 ¯
¯
dpy dpz ¯ Ψ(~r)e d ~r¯(7.11)For our purposes this will be sufficient because the lineshapes of interest are well approximatedby gaussian distributions.

85

a)

b)
EnergyEnergy
|e>

|e>

p2
2m

ν2

ν1

p2
2m

|g>

ν1

ν

2

|g>
d
|g>
i

µ{
-1
0
+1
Momentum (precoil)-10+1Momentum (precoil)Figure 7-5: Broadening mechanisms for Bragg transitions. a) Atoms moving withdifferent velocities require different frequencies ν2 to complete the transition. The
width of the Bragg transition, therefore, depends on the velocity distribution. b)
Mean-Field Broadening. Because distinguishable particles experience twice the meanfield repulsion, the frequency at which the transition occurs is shifted. The transitionis broadened as well because mean-field interactions are not uniform throughout thecondensate (possibly show lines?).

Fitting a gaussian to this lineshape yields an rms width5 of [95]∆νp = 3.16h̄ sin(θB /2)
mλL x0(7.12)

where x0 is the Thomas-Fermi radius in the direction κ̂.

7.3.2

Mean-Field Broadening

The dispersion relation for a weakly interacting uniform condensate is [48]ν=q

ν02 + 2ν0 nU/h

(7.13)

where n is the particle density, U=4πh̄2 a/m, m is the atomic mass, and a the scattering length. For energies hν ≫ nU , the excitation spectrum is particle-like (quadratic
in momentum)ν = ν0 + nU/h5

(7.14)In all cases we use the rms width σ as the figure of merit, defined by the normalized distribution
ν21e− 2σ2f (ν) = √2πσ
286The mean-field shift nU/h results from the repulsion of excitations by the condensate. Distinguishable atoms experience twice the mean-field of condensed atoms [57].
Therefore, scattered atoms originating in the condensate (indistinguishable) groundstate |gii end up in a distinguishable ground state |gid , resulting in an overall shiftof the Bragg spectrum. This effect is illustrated in Figure 7-5b.
In order to determine the shift for a nonuniform condensate, the inhomogeneousdensity distribution must be accounted for. This effect is easy to model using a local
density approximation. The observed shift is simply an average of each individual
particle’s shift. Recall from Chapter 1 that the (normalized) density distribution of
the condensate is given by
s

15n
n
1−
I(n) =
4n0
n0(7.15)

where n0 is the peak density. Using Eq(7.14), we replace the density n with the local
density h(ν − ν0 )/U ,sh(ν − ν0 )15h(ν − ν0 )1−
I(ν) =
4n0 U
n0 U(7.16)The line shift is then given by the first momentδνn =< ν >=Z

νI(ν)dν =Zsh(ν − ν0 )4n0 U
15hν(ν − ν0 )
1−
dν =
4n0 U
n0 U
7h

(7.17)In addition to the mean-field shift, the resonance is also broadened. This resultsfrom a smearing of the individual particle shifts caused by inhomogeneous mean-fieldinteractions. The rms width is given by the second moment
∆νn =

7.3.3

√

< ν 2 > − < ν >2 =s

8 n0 U147 h(7.18)

Pulse Broadening

As demonstrated in 7.3, the probe itself contributes to the measured linewidth. The
instrumental resolution is limited by the fourier spectrum of the pulse. The shorter
the pulse duration, the broader the frequency distribution. Indeed, for short enough
87

-2

-1

0

1

2

Recoil Frequency (ν0)
Figure 7-6: Kapitza-Dirac scattering of a BEC. Multiple momentum states are populated due to the broad frequency distribution of a short Bragg pulse (2 µs). The
recoil frequency is νr ≃ 45 kHz, while the pulse has frequency width ∆νpulse ≃ 175
kHz.

pulses, Bragg processes populate multiple momentum states (see Figure 7-6). This is
known as the Kapitza-Dirac regime. For high resolution spectroscopy, it is importantto quantify the probe resolution so that a suitable pulse duration can be chosen.
Figure 7-7 illustrates the instrumental resolution of Bragg. The beams are typically flashed on at fixed intensity for time τ , such that the average electric field isĒ(t) = E0 f (t), wheref (t) =


 f0

−τ /2 ≤ t ≤ τ /2


 0

(7.19)

Otherwise

The fourier transform of f (t) gives the field amplitude in frequency space, Ē(ν) =E0 g(ν), whereg(ν) ∝sin(πντ )ν

(7.20)The intensity I(ν) in frequency space is proportional to |g(ν)|2 . A gaussian fit to I(ν)
yields rms width1∆νpulse = √8τ(7.21)

Thus, the instrumental resolution is given by Eq(7.21). As an example, the 2 µs

88

f(τ)

|g(ν)|2g(ν)

Fourier
Transform

-0.5

0.5

-3

-2

-1

1

2

3

Frequency (τ-1)

time (τ)

-3

-2

-1

1

2

3

Frequency (τ-1)

Figure 7-7: Frequency resolution of a finite pulse. For a square pulse of duration τ ,the frequency distribution g(ν) is obtained by taking the Fourier transform of f (t).
The resolution of the pulse is obtained by fitting a Gaussian (dashed line) to g(ν)2pulse used in Figure 7-6 has a frequency distribution of ≃ 175 kHz, which is broad
enough to populate momentum states separated by ≃ 180 kHz. It should be notedthat the pulse duration for in-trap Bragg spectroscopy should be less than a quarter
trap period because initially scattered atoms will come to rest in this time. When
this is the case, scattered atoms do not separate from the condensate during ballistic
expansion.

7.3.4

Motional Broadening

Random center-of-mass motion from shot-to-shot will broaden the measured Bragg
spectrum. The extent to which this motion contributes, ∆νm , depends on its amplitude Xrms (= vrms /ω). Following the derivation of 7.1.2 the Doppler shifted width
is
∆νm =

2ωx sin(θB /2)
Xrms
λL

89

(7.22)

7.4

Summary of Results

The important results of this chapter are given below:
The resonance condition for Bragg scattering isν0 =2hsin2 (θ/2)
mλ2(7.23)For a thermal distribution at temperature T the width of the Bragg resonance is
∆νT =

s

2kB T sin(θB /2)m
λL(7.24)For a condensate the factors that contribute to the width of the Bragg spectrum are


B /2)

∆νp = 3.16 h̄ sin(θmλL x0q
8 n0 U ∆νn =

F inite Sample Size

147 hBroadening M echanisms ∆νpulse = √18τ





 ∆ν = 2ωx sin(θB /2) X
m

λL

rms

M ean − F ield Interactions
F inite P ulse Duration
Random M otion(7.25)

In principle the overall width should be the quadrature sum of these values.
Factors that lead to a shift of the Bragg spectrum are

Shif ting M echanisms δνn = 4n0 U
7hv
m = λL δν

a : Scattering Lengthn0 : P eak Density
T : T emperatureωx : Radial T rap F requency

M ean − F ield Interactions

λL : Laser W avelengthθB : Beam Angle
U : Interaction P arameter (4πh̄2 a/m)
Xrms : Oscillation Amplitude
Table 7.1: Notation
90(7.26)

Reproducible M otion

m : M ass
τ : P ulse Durationv : V elocity
x0 : T − F Radius

7.5

Discussion of Results

Typically, condensate parameters such as atom number N and peak density n0 are
determined by measuring the size of the sample in time-of-flight Xtof . The ThomasFermi radius is then given by [14]6x0 = qXtof
1 + (ωx t)2(7.27)

where t is the time-of-flight. x0 and ωx provide us with everything we need to characterize the condensate.7
An interesting result from 7.3.2 is that the mean-field shift δνn depends explicitly
only on the peak density. Therefore, measurements of δνn provide an alternate means
for measuring condensate parameters.8 Recasting the the peak density and size interms of the shift yields
7h
δνn
4U
s
7h
=
δνn
2mωx2

n0 =

(7.28)

x0(7.29)

Of course, it is much easier to measure the size of the cloud than to take an entire
Bragg spectrum. The real value in determining δνn is that it provides a useful checkfor the validity of the Bragg spectrum.

7.6

Putting it all Together: A Real Example

With the features of the spectrum now well-characterized, we turn our attention toa real example. From fits to the spectrum in Figure 7-4b, the following experimental
6

This assumes a purely 2-D expansion, characteristic of the cigar-shaped condensates we typicallyuse.
7

The trap frequency is typically measured by inducing dipole motion of the condensate and thenmeasuring the ensuing oscillation frequency. Of all the parameters we measure, this is usually thebest known.
8
This requires that both ±δ’s are used so that any shift due to reproducible motion of thecondensate is removed by using the average shift.

91values were extracted for the shift and width, respectively:
δνExp = 3.75 kHz∆νExp = 2.5 kHz

As discussed above, we first check that the condensate parameters found via theshift δνExp agree with those found in time-of-flight. Table 7.2 shows that these two
methods compare favorably, giving us confidence in the spectrum.
Parameterx0 (µm)n0 (1014 cm−3 )N (106 )δνn (kHz)∆νn (kHz)∆νp (kHz)∆νF (kHz)

TOF
14.4
4.04
22.5
3.5
1.4
0.62
1.5

M-F Shift
16.2
4.32
27.8
3.7
1.5
0.60
1.6

Table 7.2: Comparison of condensate parameters using time-of-flight (TOF) analysis and the mean-field (M-F) shift. Bold values represent the measured parameter.
(Strictly speaking x0 is not directly measured, rather, it is found using Xtof = 580µm,
t = 40 ms and ωx = 2π×146 Hz.)
Next, we compare the measured width ∆νExp to that of a thermal distribution
near the critical temperature Tc . For a typical value of Tc ∼ 1 µK, the width of athermal sample is ∆νT = 30 kHz, much larger than our measured width. As we shallsee (in direct analogy to a laser), the narrow linewidth of the condensate is indicativeof high spatial coherence.
For a perfect condensate the coherence length χc should equal the size of thesample x0 . χc is experimentally determined by subtracting out contributions to ∆νExp
from mean-field interactions and pulse broadening. Ideally, the remaining width isaccounted for by the finite-size broadening. In practice this may not be the case.
Thus, the remaining width sets a lower bound on the coherence lengthχc ≥ q

∆νp
2
2
∆νExp
− ∆νn2 − ∆νpulse

92x0(7.30)

a)b)

Figure 7-8: Doppler broadening caused by random motion. In these images each
Bragg beam has both frequencies mixed in. (a) The ratio of out-coupled atoms should
be unity. (b) Some shots, however, show asymmetric out-coupling due to motion of
the condensate. Unless shots like this are discarded, the measured Bragg spectrum
will be broadened.

The pulse duration used in this example was τ = 200 µs. Using Eq(7.21) andthe values from Table 7.2 we find that χc ≃ 0.66x0 or ∼ 10 µm.9 This measurement
demonstrates high spatial coherence over the sample and the existence of a macroscopic de Broglie wave. However, if we assume that the coherence length is indeed
the sample size, then there is 700 Hz of width unaccounted for.

7.7

Noise Rejection

The unaccounted for width in our Bragg spectrum is most likely due to Doppler
broadening caused by random center-of-mass motion and other collective excitations.
A line broadening of 700 Hz corresponds to a vibrational amplitude of only ≃ 0.35 µm(compared to x0 = 14 µm). Therefore, it seems likely that this width is attributableto random motion. This possibility was investigated by mixing both frequencies ν1 ,
ν2 into each Bragg beam to out-couple particles in both ±x directions. For particles
at rest, the out-coupling should be symmetric. However, we observed the ratio ofout-coupled particles to fluctuate (see Figure 7-8).
Doppler broadening caused by random motion can, in principle, be eliminatedusing the two-frequency technique described above. Discarding data in which theout-coupled ratio falls outside a certain bandwidth should improve spectroscopic resolution. The bandwidth should be narrow enough such that ∆νm is small compared
9

J. Stenger et al. [94] measure a coherence length of 0.8x0 .

93

to the finite size width ∆νp , but not so small as to require Herculean data collection. Finally, it must be noted that this method fails if the spectrum is shifted byreproducible motion δνm . Because of this shift, one cannot expect symmetric outcoupling. This effect plagued our measurement of the molecular Bragg spectrum (seeChapter 8) [3]. In this case a stray magnetic field provided a reproducible kick to themolecules upon their creation. This effect can be compensated for with some extra
effort. This requires providing frequencies ν1 ,ν2 to one beam and ν1 ,ν2 + δνm to theother to compensate for the shift.

94

Chapter 8
Coherent Molecular Optics
The unprecedented intensity and coherence properties of lasers have led directly to theobservation of effects such as wave-mixing and parametric down-conversion. Similarly, atom and molecular optics have benefitted greatly from the realization of BoseEinstein condensates (BEC). High phase-space density (particles per mode) and uniform spatial phase give the condensate laser-like qualities, opening the door for studies
of nonlinear and quantum particle optics.

This chapter supplements work reported in the following publication:
J.R. Abo-Shaeer, D.M. Miller, J.K. Chin, K. Xu, T. Mukaiyama, and W.
Ketterle “Coherent Molecular Optics using Sodium Dimers,”
cond-mat/0409327 (2004).
(Included in Appendix E) Ref [3]8.1

OpticsRecent developments in atom/molecular optics parallel the revolution that took placein conventional optics after the invention of the laser. Indeed, many useful analogies
between the two fields can be drawn. With this in mind, I begin the chapter with a
discussion of the key features of conventional optics, before turning my attention toatom optics and finally molecular optics.
958.1.1

Conventional Optics

The field of optics underwent a dramatic shift midway through the twentieth century.
Prior to the invention of the laser (1960), optics consisted mainly of two subfields:
ray and wave optics. Ray optics has, in some sense, been understood since the dawnof man, evident in phenomena such as the bending and reflection of light by water.1
In ray optics coherence plays no role. Rather, light behaves as small particles (photons) that move in straight-line trajectories. This picture is sufficient for describing
reflection and refraction, the basis of geometric optics.
Wave optics describes phenomena in which photons travel in “lockstep” with one
another. Unlike particles, waves overlap, adding constructively and destructively.
Similar to ray optics, the wave nature of light is manifest in everyday life such as
thin-film interference on a soap bubble. However, effects such as this are more subtle.
It was not until 1803 that T. Young’s double slit experiment gave conclusive evidence
for the wave-nature of light.
The key differences between a laser and thermal source are its intensity and coherence. These features produce remarkable effects that have led to the developmentof two new subfields of optics: nonlinear2 and quantum optics. Nonlinear opticalphenomena such as wave-mixing, result from the interaction of light with matter. In
free space photons do not interact with one another. However, in materials there
can be an effective photon interaction, caused by an intensity dependent index ofrefraction. Frequency doubling was the first qualitatively new nonlinear optical effectobserved using lasers (1961) [34]. Here a crystal irradiated with an intense pulse of
red laser light produced a small amount blue light at twice the input frequency. Frequency doubling is a specific example of the more general process of sum-frequency
generation, where two light waves mix to create a third wave at the sum frequency.
Quantum optics deals partly with study of nonclassical light fields. Nonclassi1

Primitive fishermen, for example, realized that they had to aim their spears at a sharper angle
than they perceived to make their catch.
2
Strictly speaking, some nonlinear phenomena such as the D.C. Kerr effect (1875) were observed
before the advent of the laser. However, the full potential of nonlinear optics was not realized until
the invention of the laser.

96

Subfield:

Ray

Wave

Nonlinear

Quantum

Photons are:Particles

Waves

Interacting

Correlated

Verification:

Phenomena:

Requirements:

Fish

Two-Slit

DC Kerr

Parametric

Spearing

Interference

EffectDown-Conversion(Dawn of Man)

(1802)(1875)(1970)

Reflection

Interference

Wave-Mixing"Squeezed" Light

Refraction

Diffraction

Induced Birefringence

Anti-Bunching---

Coherent Light

Intense Fields

Intense Fields/
Coherent Light

Source:ThermalThermal

Laser

Laser

Tools:

Lenses

Gratings

Nonlinear Media

Nonlinear Media

Figure 8-1: Key Features of conventional optics.

cal light can be generated via parametric down-conversion [12], the inverse processof sum-frequency generation. In this case, photons travelling through a material
are split in two. This splitting is, however, fundamentally different from that of abeamsplitter. Beamsplitters are governed by poissonian statistics, which requires aminimum uncertainty in the number of photons in each arm. In parametric downconversion energy and momentum conservation make the resultant photons emerge
strongly correlated, with complementary direction and frequency. This “squeezing”
of number fluctuations can produce measurements below the shot-noise limit.
The key features of each subfield of conventional optics are summarized in Figure
8-1.

8.1.2

Atom Optics

Ray atom optics concerns itself only with the particle nature of atoms. Although theseproperties are well-understood, considerable effort is still devoted to the field, partly
for its applications to cold atom physics. Recent experiments have demonstrated novel
tools for the manipulation of atoms, including atomic mirrors, waveguides, conveyor
belts, and BEC Chip experiments [46, 24, 74, 59, 43, 42, 64].
Wave atom optics has its roots in the pioneering work on crystal diffraction from97

the early 20th century. Davisson and Germer used this technique to demonstratematter-wave interference of electrons (1927)[22]. Shortly thereafter, J. Estermann and
O. Stern used crystal diffraction to prove that more massive objects (He atoms) also
propagate as waves (1930)[29]. Unfortunately, most atoms tend to stick to surfaces
rather than reflecting off or passing through them. Therefore, Bragg diffraction did
not become a useful atom-optical tool until much later (1987) [82], when atoms were
demonstrated to diffract from standing light waves [69] and nanofabricated gratings[56] .
Until recently, atom optics experiments were limited to single-particle phenomena where interactions between particles could be neglected. However, in 1993 a
new regime was considered in which interactions play a crucial [66]. For sufficiently
dense samples atomic mean-field interactions can play the role of a nonlinear medium.
Indeed, the Gross-Pitaevskii equation (the nonlinear Schrodinger equation used to describe condensates) is similar in form to a certain class of wave equations governing
nonlinear optics [6]. Nonlinear atom optics has benefitted greatly from the realization of Bose-Einstein condensates (BEC). High phase-space density (atoms per mode)
and a uniform phase [94, 40] give the condensate laser-like qualities. Although notfundamentally required [75, 58], BEC has led to the observation of such nonlinear
phenomena as four-wave mixing [23] and matter wave amplification [51, 61]. In addition, quantum atom optic effects such as atom number squeezing have also been
observed [80, 37].
The key features of atom optics are summarized in Figure 8-2. Note the similarities
to Figure 8-1.

8.2

Molecular Optics

The current state of molecular optics is similar to atom optics prior to the realization of BEC. Diffraction and interferometry of thermal molecular beams has been
demonstrated [11, 15, 39, 88], yet monoenergetic beams lack the density necessary
to observe nonlinear effects. However, recent experiments using Feshbach resonances98Subfield:

Ray

Wave

Nonlinear

Quantum

Atoms are:Particles

Waves

Interacting

Correlated

Verification:

Phenomena:

Requirements:

Democritus'

He

4-WaveAtom Number

Atom & Void

Diffraction

MixingSqueezing(500 BC)(1930)(1999)(2001)

Reflection

Interference

Wave-Mixing"Squeezed" Atoms

Refraction

Diffraction

Solitons

Entanglement---

Coherent Atoms

High Density

High Density/
Coherent Atoms

Source:ThermalThermal

BEC

BEC

Tools:

E-M Fields

Gratings

Mean-Field

Mean-Field

Interactions

Interactions

Figure 8-2: Key Features of atom/molecular optics.

have demonstrated the conversion of degenerate atomic bosons [28, 45, 107] andfermions [85, 55, 113, 18, 96] into ultracold molecules. These sources have the potential to greatly advance molecular optics. Furthermore, atom-molecule coupling can
be studied as the first steps towards “superchemistry”, where chemical reactions arestimulated via macroscopic occupation of a quantum state [44].
Here we demonstrate the ability to apply Kapitza-Dirac and Bragg diffraction[60] to cold molecules. Using optical standing waves of suitably chosen frequencies,
sodium dimers were coherently manipulated with negligible heating or other incoherent processes. First, we characterized the coherence of our “source” molecules,
created via Feshbach resonance. By measuring the Bragg spectrum of the molecules
immediately after their creation, the conversion from atoms to molecules was shown tobe coherent - the matter wave analog to frequency doubling in optics. The quadratic
spatial dependence of the phase of the expanding molecules was observed using an autocorrelation interference technique. By creating a duplicate sample of molecules andoverlapping it with the original, matter wave interference was observed. Finally, thematter wave analog to sum-frequency generation was demonstrated. Atoms preparedin two momentum states, prior to creating molecules, were observed to cross-pair,generating a third momentum state.

99

8.3

Bragg Diffraction of Molecules

The theory and experimental techniques underlying Bragg diffraction are discussed
in detail in Chapter 7. The following touches upon the main points of the Appended
text.
Figure 8-3 shows time-of-flight images of Bragg scattering for atoms and molecules.
Because the kinetic energy of the scattered particles was much larger than theirmean-field energy, individual momentum states were well-resolved in ballistic expansion. Both atoms and molecules receive equal two-photon recoil momentum,
pr = 2h sin(θB /2)/λL , where λL is is the wavelength of the Bragg beams. However, scattered molecules move away from the central peak with half the velocity ofatoms, owing to their doubled mass. Figure 8-3c,d show Kapitza-Dirac scattering,where multiple atomic and molecular momentum states were populated due to thebroad frequency distribution of the short pulse (5 µs).

8.4Characterization of the “Source”

Furthering the analogy between conventional optics and atom optics, the conversion of
atoms to molecules may be viewed as the atom optic equivalent of frequency doubling[89]. Indeed, the relevant Hamiltonian for atom-molecule coupling has the same form
as that for the optical frequency doubling process:a†2m am am(8.1)

where am is the annihilation operator for the atomic field and a†2m is the creation
operator for the molecular field.
Here we apply the technique of Bragg spectroscopy to measure the linewidth of amolecular sample. The goal is to gain insight into the process of molecule creation.
Does the Feshbach process preserve the coherence of the sample? Or, to put it anotherway, does a frequency doubled atom laser inherit the linewidth of the source?
The linewidth of a coherent light source is typically measured by scattering it from100

Atomic Momentum (pr)
-2

-1

0

1

2

a)

b)
c)

d)

-2

-1

0

1

2

Molecular Momentum (pr)Figure 8-3: Bragg diffraction of (a) atoms and (b) molecules. Scattered particles
recoil with identical momenta, pr . However, during ballistic expansion diffracted
molecules expand with half the velocity of atoms, due to their doubled mass. The
pulse duration in each image was 200 µs. A shorter pulse (5 µs) populated multiple(c) atomic and (d) molecular momentum states. The halos in (c) are due to collisions
between different momentum states [17]. The time-of-flight in each image is 17 ms.

a grating. It is easy to show that monochromatic light will only be diffracted at certain
angles given by the Bragg condition nλ = Dsinθ, where D is the grating spacing andn is an integer. However, because the source is not perfectly monochromatic, theBragg condition is actually satisfied over some range of angles δθ. The linewidth isthen δλ = Dδθ/n. In the same way, the linewidth of an “atom laser” (condensate)can be measured by diffracting it from a light grating. The technique, known as Bragg
spectoscopy, has been used to demonstrate that the coherence length of a condensate
is equal to its physical size [94].
To study the coherence properties of the sample, Bragg spectra [94] were taken.
Figure 8-4 shows three spectra for (a) atoms above the Feshbach resonance, as wellas (b) atoms and (c) molecules after sweeping through the resonance. Atoms below
the resonance coexisted with a small fraction of molecules (2%). As expected from
101

a)

c)

Outcoupled Fraction (a.u.)

b)

1

0

1

0

1

0
-100

-50

0

50

100

Detuning (kHz)

Figure 8-4: Bragg spectra for atoms and molecules. In (a) the spectrum is taken
for a pure atomic sample above the Feshbach resonance. (b) and (c) are spectra ofatoms and molecules, respectively, below the resonance. In (c) atoms were removed
from the trap with resonant light to limit losses due to atom-molecule collisions. The
Bragg resonance condition for molecules occurs at half the frequency of the atomic
resonance.

the resonance condition, molecular resonances occur at half the frequency of atomic
resonances.
Detailed analysis can be found in Appendix E. Suffice it to say, the width of the
Bragg spectrum corresponds to a molecular temperature of 20 nK, comparable to aprevious value obtained using a time-of-flight technique [107]. The BEC transition
temperature for our trap parameters and 5 × 104 molecules is much higher (115 nK).
This demonstrates a deeply degenerate, purely molecular sample, where as previous
experiments have demonstrated coherent admixture of molecular character into an
atomic BEC [25].

8.5Sum-Frequency Generation

The measurement of the Bragg spectrum shows that the sharp “linewidth” of theseed (atom) laser is inherited by the molecular laser. In nonlinear optics, photon
interactions are typically mediated by a refractive medium. Here, the nonlinearity
arises from the atoms themselves, in the form of s-wave interactions. The high density,

102

Atomic Momentum (pr)
0
1

a)

b)

0
1
2
Molecular Momentum (pr)Figure 8-5: Sum frequency generation of atomic matter waves. (a) Atoms were
initially prepared in momentum states 0, 1. (b) By sweeping through the Feshbachresonance, atoms combine to form molecules with momenta 0, 1, and 2. Momentum
state 1 is the sum frequency of the two atomic matter waves. The “nonlinear medium”
is provided by the atomic interactions. The time-of-flight in each image is 17 ms.

or “brightness”, of the source, together with the enhanced interactions at the Feshbachresonance provide the means to combine two matter waves.
By combining two disparate matter waves, rather than identical ones, we extend
the analogy of frequency doubling to the more general process of sum frequency
generation. To do this, atoms were initially prepared in momentum states 0, 1 (inunits of pr ). By sweeping through the resonance, molecules were produced in threemomentum states: 0, 1, and 2 (see Figure 8-5). States 0 and 2 are simply thefrequency doubled components of the two initial matter waves. State 1 however,results from cross pairing between the initial momentum states, and is thus their sum
frequency. This is the first time that a Feshbach resonance was observed between
atoms colliding with a controlled non-vanishing momentum. The Feshbach resonanceshould be slightly shifted compared to the resonance for atoms at rest, which reflects
the same physics encountered in the temperature dependence of the position of theresonance [103].

103

8.6

Molecular Interferometery

The spatial phase of the expanding molecular cloud was directly imaged using an autocorrelation method [90], which gives rise to self-interference of the molecular sample(see Figure 8-6). To accomplish this, two identical copies of the sample were madeusing a short Kapitza-Dirac pulse (10 µs), applied after 2 ms of ballistic expansion.
The copies, with momentum ±pr , moved away from the zero momentum peak fortime ∆t before an identical pulse recombined them with the original. This type ofinterferometer has three readout ports, with momenta 0, ±pr . The straight-line interference fringes are characteristic of a quadratic spatial phase. The fringe spacing
we measure is consistent with λf = ht/md [7], where d = pr ∆t/m is the distancethe copies moved between pulses.3 Interference fringes can only be resolved for smalld. Therefore, this method cannot be used to observe coherence lengths longer thanthose inferred from Bragg spectroscopy. It should be noted that the appearance ofinterference fringes does not imply that the sample is condensed. Rather, it demonstrates only that the coherence length in time-of-flight is longer than the separationd. Therefore, similar interference can also be observed for a cloud of thermal atoms[10, 73].

8.7

Conclusions and Outlook

We have demonstrated coherent molecular optics using standing light waves. The
ability to coherently convert atoms into molecules makes molecular optics even richer
than atom optics. These experiments demonstrate the scalable nature of atom optics
and offer the promise of coherently manipulating more complex structures. In the longrun this could prove useful for atom lithography and holography. In the short term
the techniques demonstrated here could prove useful for probing molecules formed inquantum-degenerate fermi systems, and possibly even Cooper pairs.

3

Strictly speaking, this analysis only applies to the outcoupled ports. The center port is comprisedof three copies.

104

a)

b)

c)

-1
0
1
Momentum (pr)Figure 8-6: Matter wave interference of molecules. (a) The molecular sample issplit with a short Kapitza-Dirac pulse, creating two identical copies with momenta±pr . (b)-(c) After the copies have separated for time ∆t = 100 µs, a second pulse
recombines them, giving rise to interference in each momentum component. The
time-of-flight in each image is 12 ms.

105

Appendix A
Observation of Vortex Lattices in
Bose-Einstein Condensates
J.R. Abo-Shaeer, C. Raman, J.M. Vogels, and W. Ketterle“Observation of Vortex Lattices in a Bose-Einstein Condensate,”
Science 292 p.476-479 (2001).

106

REPORTS
7. S. Kirkpatrick, B. Selman, Science 264, 1297 (1994).
8. E. Farhi et al., unpublished data.
9. L. K. Grover, Phys. Rev. Lett. 78, 325 (1997).
10. E. Farhi, S. Gutmann, Phys. Rev. A 57, 2403 (1998);
C. H. Bennett, E. Bernstein, G. Brassard, U. V. Vazirani,
SIAM J. Comput. 26, 1510 (1997) (available at http://xxx.lanl.gov/abs/quant-ph/9701001).

11. A. M. Childs, E. Farhi, J. Goldstone, S. Gutmann,
http://xxx.lanl.gov/abs/quant-ph/0012104.
12. Supported in part by the U.S. Department of Energy
under cooperative agreement DE-FC02-94ER40818 andalso by MIT’s Undergraduate Research Opportunities
Program. We thank the Computer Facility of the MIT
Laboratory for Nuclear Science for extensive use of the

Observation of Vortex Lattices
in Bose-Einstein Condensates
J. R. Abo-Shaeer, C. Raman, J. M. Vogels, W. Ketterle
Quantized vortices play a key role in superfluidity and superconductivity. We
have observed the formation of highly ordered vortex lattices in a rotating
Bose-condensed gas. These triangular lattices contained over 100 vortices withlifetimes of several seconds. Individual vortices persisted up to 40 seconds. The
lattices could be generated over a wide range of rotation frequencies and trap
geometries, shedding light on the formation process. Our observation of dislocations, irregular structure, and dynamics indicates that gaseous Bose-Einstein condensates may be a model system for the study of vortex matter.
The quantization of circulation has a profoundeffect on the behavior of macroscopic quantum
systems. Magnetic fields can penetrate type-II
superconductors only as quantized flux lines.
Vorticity can enter rotating superfluids only inthe form of discrete line defects with quantizedcirculation. These phenomena are direct consequences of the existence of a macroscopic
wavefunction, the phase of which must change
by integer multiples of 2p around magnetic
flux or vortex lines. In superconductors, magnetic flux lines arrange themselves in regularlattices that have been directly imaged (1). In
superfluids, direct observation of vortices has
been limited to small arrays (up to 11 vortices),
both in liquid 4He (2) and, more recently, inrotating gaseous Bose-Einstein condensates(BECs) (3, 4).
We report the observation of vortex lattices in a BEC. We are now able to explore
the properties of bulk vortex matter, which
includes local structure, defects, and longrange order. In contrast, the properties ofsmall arrays are strongly affected by surface
and finite size effects. The vortex lattices arehighly excited collective states of BECs withan angular momentum of up to 60 \ perparticle. Our experiments show that suchstates can be prepared and are much morestable than predicted (5).
Vortices in BECs have been the subjectof extensive theoretical study (6 ). Experimental progress began only recently withthe observation of quantized circulation in
Department of Physics, Center for Ultracold Atoms at
Massachusetts Institute of Technology (MIT) and Harvard University, and Research Laboratory of Electronics, MIT, Cambridge, MA 02139, USA.
*To whom correspondence should be addressed. Email: jamil@mit.edu

476

a two-component condensate by a phaseengineering technique (7 ) and of vortex
arrays in a single-component BEC (3). A
condensate can be subjected to a rotating
perturbation by revolving laser beams
around it. This technique was used to study
surface waves in a trapped BEC (8), andsubsequently for the creation of vortices(3). In 1997, we tried unsuccessfully todetect quantized circulation as a “centrifugal hole” in ballistic expansion of the gas(9, 10). Theoretical calculations (11–13)
and ultimately the pioneering experimental
work (3) showed that vortices can indeed
be detected through ballistic expansion,
which magnifies the spatial structure of thetrapped condensate.
BECs of up to 5 3 107 Na atoms with anegligible thermal component (condensate fraction $ 90%) were produced by a combination of laser and evaporative cooling techniques (8, 10, 14). A radio-frequency “shield”
limited the magnetic trap depth to 50 kHz (2.3mK), preventing high-energy atoms from heating the condensate. Experiments were performed in cylindrical traps with widely varying
aspect ratios. Most of the results and all of theimages were obtained in a weak trap, withradial and axial frequencies of nr 5 84 Hz andnz 5 20 Hz (aspect ratio 4.2), respectively. In
this weak trap inelastic losses were suppressed,
resulting in larger condensates of typically 5 3
107 atoms. Such clouds had a chemical potential (m) of 310 nK (determined from time-offlight imaging), a peak density of 4.3 3 1014
cm23, a Thomas-Fermi radius along the radial
direction (Rr) of 29 mm, and a healing length (j)of about 0.2 mm.
Vortex lattices were produced by rotating
the condensate around its long axis with theoptical dipole force exerted by blue-detuned

computer Abacus. We benefited greatly from conversations with A. Childs, B. Selman, and L. Valiant. We also
thank D. Fisher, B. Halperin, M. Kardar, and P. Lee for
useful discussions about the connection of our work tostatistical mechanics systems.
27 November 2000; accepted 19 March 2001

laser beams at a wavelength of 532 nm. A
two-axis acousto-optic deflector generated apattern of two laser beams rotating symmetrically around the condensate at variable
drive frequency V (8). The two beams wereseparated by one Gaussian beam waist (w 5
25 mm). The laser power of 0.7 mW in eachbeam corresponded to an optical dipole potential of 115 nK. This yielded a strong,anharmonic deformation of the condensate.
After the condensate was produced, thestirring beam power was ramped up over 20
ms, held constant for a variable stirring time,
and then ramped down to zero over 20 ms.
The condensate equilibrated in the magnetic
trap for a variable hold time (typically 500ms). The trap was then suddenly switched
off, and the gas expanded for 35 ms to radial
and axial sizes of lr > 1000 mm and lz > 600
mm, respectively. We probed the vortex cores
using resonant absorption imaging. To avoid
blurring of the images due to bending of thecores near the edges of the condensate, we
pumped a thin, 50- to 100-mm slice of atoms
in the center of the cloud from the F 5 1 to
the F 5 2 hyperfine state (15). This section
was then imaged along the axis of rotation
with a probe pulse resonant with the cycling
F 5 2 3 3 transition. The duration of thepump and probe pulses was chosen to be
sufficiently short (50 and 5 ms, respectively)
to avoid blurring due to the recoil-induced
motion and free fall of the condensate.
We observed highly ordered triangularlattices of variable vortex density containing
up to 130 vortices (Fig. 1). A striking featureis the extreme regularity of these lattices, freeof any major distortions, even near theboundary. Such “Abrikosov” lattices werefirst predicted for quantized magnetic flux
lines in type-II superconductors (16).
Tkachenko showed that their lowest energy
structure should be triangular for an infinite
system (17). A slice through images shows
the high visibility of the vortex cores (Fig. 2),
which was as high as 80%. For a trapped
condensate with maximum vortex density,
we infer that the distance between the vortices was > 5 mm. The radial size of thecondensate in the time-of-flight images wasover 10% larger when it was filled with the
maximum number of vortices, probably due
to centrifugal forces.
When a quantum fluid is rotated at afrequency V, it attempts to distribute thevorticity as uniformly as possible. This issimilar to a rigid body, for which the vorticity

20 APRIL 2001 VOL 292 SCIENCE www.sciencemag.org

REPORTS
Fig. 1. Observation ofvortex lattices. The
examples shown containapproximately(A) 16, (B) 32, (C) 80,
and (D) 130 vortices.
The vortices have“crystallized” in a triangular pattern. The
diameter of the cloudin (D) was 1 mm after
ballistic
expansion,
which represents amagnification of 20.
Slight asymmetries in the density distribution were due to absorption of the optical pumping light.

W . For a superfluid,
is constant … 3 v¢ 5 2V
the circulation of the velocity field, v¢ , isquantized in units of k 5 h/M, where M is theatomic mass and h is Planck’s constant. The
quantized vortex lines are distributed in thefluid with a uniform area density (18)n v 5 2V/k

Fig. 2. Density profile through avortex lattice. The curve represents a 5-mm-wide cut through a
two-dimensional image similar to
those in Fig. 1 and shows the highcontrast in the observation of thevortex cores. The peak absorption
in this image is 90%.

(1)

In this way the quantum fluid achieves thesame average vorticity as a rigidly rotating
body, when “coarse-grained” over several
vortex lines. For a uniform density of vortices, the angular momentum per particle isNv\/2, where Nv is the number of vortices inthe system.
The number of observed vortices is plotted
as a function of stirring frequency V for two
different stirring times (Fig. 3). The peak near
60 Hz corresponds to the frequency V/2p 5
vr/=2, where the asymmetry in the trapping
potential induced a quadrupolar surface excitation, with angular momentum l 5 2, about theaxial direction of the condensate (the actual
excitation frequency of the surface mode v 5=2vr is two times larger due to the twofold
symmetry of the quadrupole pattern). The same
resonant enhancement in the vortex production
was observed for a stiff trap, with nr 5 298 Hz
and nz 5 26 Hz (aspect ratio 11.5), and has
recently been studied in great detail for small
vortex arrays (19).
Far from the resonance, the number of vortices produced increased with the stirring time.
By increasing the stir time up to 1 s, vortices
were observed for frequencies as low as 23 Hz(>0.27nr). Similarly, in a stiff trap we observed
vortices down to 85 Hz (>0.29 nr). From Eq. 1
one can estimate the equilibrium number ofvortices at a given rotation frequency to be
Nv 5 2pR2V/k. The observed number wasalways smaller than this estimate, except nearresonance. Therefore, the condensate did notreceive sufficient angular momentum to reachthe ground state in the rotating frame. In addition, because the drive increased the moment ofinertia of the condensate (by weakening thetrapping potential), we expect the lattice to rotate faster after the drive is turned off.
Looking at time evolution of a vortex lattice(Fig. 4), the condensate was driven near the

Fig. 3. Average number of vortices as a function of the stirring
frequency V for two different
stirring times, (F) 100 ms and(h) 500 ms. Each point represents the average of three measurements with the error bars
given by the standard deviation.
The solid line indicates the equilibrium number of vortices in aradially symmetric condensateof radius Rr 5 29 mm, rotating at
the stirring frequency. The arrow
indicates the radial trapping
frequency.

quadrupole resonance for 400 ms and thenprobed after different periods of equilibration in
the magnetic trap. A blurry structure was already visible at early times. Regions of low
column density are probably vortex filamentsthat were misaligned with the axis of rotationand showed no ordering (Fig. 4A). As the dwell
time increased, the filaments began to disentangle and align with the axis of the trap (Fig. 4, B
and C), and finally formed a completely ordered Abrikosov lattice after 500 ms (Fig. 4D).
Lattices with fewer vortices could be generated
by rotating the condensate off resonance. In
these cases, it took longer for regular lattices toform. Possible explanations for this observation
are the weaker interaction between vortices atlower vortex density and the larger distancethey must travel to reach their lattice sites. In
principle, vortex lattices should have alreadyformed in the rotating, anisotropic trap. We
suspect that intensity fluctuations of the stirrer
or improper beam alignment prevented this.
The vortex lattice had lifetimes of several
seconds (Fig. 4, E to G). The observed stability of vortex arrays in such large condensates is surprising because in previous work
the lifetime of vortices markedly decreased
with the number of condensed atoms (3).
Theoretical calculations predict a lifetime inversely proportional to the number of vortices(5). Assuming a temperature kBT > m, where
kB is the Boltzmann constant, the predicteddecay time of > 100 ms is much shorter thanobserved. After 10 s, the number of vortices

www.sciencemag.org SCIENCE VOL 292 20 APRIL 2001

477

REPORTS
Fig. 4. Formation anddecay of a vortex lattice. The condensate
was rotated for 400 ms
and then equilibrated
in the stationary magnetic trap for various
hold times. (A) 25 ms,(B) 100 ms, (C) 200 ms,(D) 500 ms, (E) 1 s, (F)5 s, (G) 10 s, and (H)
40 s. The decreasing
size of the cloud in (E)to (H) reflects a decrease in atom number
due to inelastic collisions. The field of viewis ;1 mm by 1.15 mm.

478

Fig. 5. Vortex lattices with defects. In (A), the lattice has adislocation near the center ofthe condensate. In (B), there is a
defect reminiscent of a grainboundary.

pers have discussed the barrier for the entry
of a vortex from the edge (6, 25, 26 ). The
condensate becomes unstable against surface deformations when the stirring frequency exceeds

had diminished considerably. In several cases
we observed a single vortex near the condensate center after 30 to 40 s (Fig. 4H). This
dwell time is much longer than that observedfor elongated clouds (1 to 2 s) (3) and fornearly spherical condensates (15 s) (20). We
estimate that during its lifetime, the superfluid flow field near the central vortex core
had completed more than 500,000 revolutions and the lattice itself had rotated ;100
times.
A feature of the lattices is their almost perfect triangular shape. Deformations are less pronounced than in theoretical calculations thatpredicted circular distortions (13, 21). It was
shown (21) that a configuration with perfect
triangular symmetry can lower its energy byrearranging the outermost ring of vortices into a
circle. This distortion is caused by the cylindrical symmetry of rotation and not by boundary
effects (which were neglected in the calculations). In condensates of finite size and inhomogeneous density, one may expect even larger
distortions. However, in images containing
large numbers of vortices (Fig. 1, C and D), thelattice is triangular throughout the condensate
even up to the edge. We have observed more
complex lattice configurations in a fraction of(3)
V s 5 minl ~v l /l !
where vl is the frequency of a surface excitation with angular momentum l in the axisymmetric trap (27, 28). For our condensates,
the instability is predicted to occur at l > 18,
yielding Vs > 0.3vr, which is in fair agreement with our observations (29). The instabilities occur on a practical time scale only
when the cloud is sufficiently deformed toexcite high-l modes. In other experiments (3,19), a sizable deformation was achieved only
by resonantly driving the l 5 2 mode near
0.7vr. In contrast, we strongly deformed thecondensate over a broad range of frequencies.
For such deformations, l is no longer a goodquantum number, allowing for coupling intohigher-order modes. Our technique is therefore well suited to studying the threshold forvortex formation.
The surface instability criterion of Eq. 3
applies to rotational excitation. In the spirit of
our earlier stirring experiments on critical velocities (14, 30), we also explored linear motionof the stirrer. When we moved a small laser
beam (>10 mm in diameter) at a velocity of 2
mm/s once through the condensate along theradial direction, we observed large lattices containing > 50 vortices after an equilibration timeof 1 s, indistinguishable from those generated
with the rotating anisotropy. We assume thatimperfect alignment of the stirring beam imparted a torque on the condensate. However,
the mechanism of vortex formation warrants
further study.

the images. Some show patterns characteristicof partial crystallization (Fig. 4B), dislocations(Fig. 5A), and grain boundaries (Fig. 5B).
Our experiments may shed light on theongoing discussion of vortex formation (6).
A single vortex is expected to be thermodynamically stable when the rotation frequency
exceeds (22)VC 5

0.671R r
5 \ln
2 MR 2r
z

F

G

(2)

For our trap this yields a critical angularfrequency of > 2p 3 6 Hz, or 0.08vr. Vortices were only observed at rotation frequencies much higher than VC. Some have suggested that the critical frequency of > 0.7 vr
observed in other experiments was related tothe suppression of unstable excitations (socalled anomalous modes) of rectilinear vortices (6, 23, 24). These anomalous modes depend strongly on the aspect ratio of the trap.
Our observation of vortices at ;0.25vr intraps where the aspect ratio varied by a factorof 2.7 seems to rule out a crucial role of theanomalous modes, possibly because their frequencies are lower for dense condensates.
Apart from stability conditions, vortices
must be nucleated. Several theoretical pa-

20 APRIL 2001 VOL 292 SCIENCE www.sciencemag.org

REPORTS
Properties of vortex lattices are of broadinterest in superfluids, superconductors, andeven astrophysics. Fluctuations in the rotation
rate of pulsars are attributed to the dynamics ofthe vortex lattice in a superfluid neutron liquid(5, 31). Our experiments show that vortex formation and self-assembly into a regular lattice
is a robust feature of rotating BECs. Gaseouscondensates may serve as a model system tostudy the dynamics of vortex matter, in analogy
to work in type-II superconductors (32). Of
particular interest are collective modes of thelattice. In liquid helium, transverse oscillations
in a vortex lattice (Tkachenko oscillations)have already been investigated (33, 34). Further
studies may address the nucleation, ordering,and decay of lattices, in particular to delineate
the role of the thermal component (5), andpossible phase transition associated with melting and crystallization.
References and Notes
1. H. Träuble, U. Essmann, Phys. Lett. 24A, 526 (1967).
2. E. J. Yarmchuk, M. J. V. Gordon, R. E. Packard, Phys.
Rev. Lett. 43, 214 (1979).
3. K. W. Madison, F. Chevy, W. Wohlleben, J. Dalibard,
Phys. Rev. Lett. 84, 806 (2000).
4.
, J. Mod. Opt. 47, 2715 (2000).
5. P. O. Fedichev, A. E. Muryshev, preprint available at
http://arXiv.org/abs/cond-mat/0004264.
6. Reviewed in A. L. Fetter, A. A. Svidzinsky, J. Phys.
Condens. Matter 13, R135 (2001).
7. M. R. Matthews et al., Phys. Rev. Lett. 83, 2498
(1999).
8. R. Onofrio et al., Phys. Rev. Lett. 84, 810 (2000).
9. M. R. Andrews, thesis, Massachusetts Institute ofTechnology (1998).
10. Reviewed in W. Ketterle, D. S. Durfee, D. M. Stamper-Kurn, in Bose-Einstein Condensation in Atomic
Gases, Proceedings of the International School ofPhysics Enrico Fermi, Course CXL, M. Inguscio, S.
Stringari, C. Wieman, Eds. (International Organisations Services B.V, Amsterdam, 1999), pp. 67–176.
11. E. Lundh, C. J. Pethick, H. Smith, Phys. Rev. A 58, 4816
(1998).
12. F. Dalfovo, M. Modugno, Phys. Rev. A 61, 023605(2000).
13. Y. Castin, R. Dum, Eur. Phys. J. D 7, 399 (1999).
14. R. Onofrio et al., Phys. Rev. Lett. 85, 2228 (2000).
15. M. R. Andrews et al., Science 275, 637 (1997).
16. A. A. Abrikosov, J. Exp. Theor. Phys. 5, 1174 (1957)[Zh. Eksp. Teor. Fiz. 32, 1442 (1957)].
17. V. K. Tkachenko, J. Exp. Theor. Phys. 22, 1282 (1966)[Zh. Eksp. Teor. Fiz. 49, 1875 (1965)].
18. P. Nozières, D. Pines, The Theory of Quantum Liquids(Addison-Wesley, Redwood City, CA, 1990).
19. K. W. Madison, F. Chevy, V. Bretin, J. Dalibard, preprint available at http://arXiv.org/abs/cond-mat/?0101051.
20. P. C. Haljan, B. P. Anderson, I. Coddington, E. A.
Cornell, preprint available at http://arXiv.org/abs/
cond-mat/0012320.
21. L. J. Campbell, R. M. Ziff, Phys. Rev. B 20, 1886 (1979).
22. E. Lundh, C. J. Pethick, H. Smith, Phys. Rev. A 55, 2126
(1997).
23. D. L. Feder, A. A. Svidzinsky, A. L. Fetter, C. W. Clark,
Phys. Rev. Lett. 86, 564 (2001).
24. J. J. Garcı́a-Ripoll, V. M. Pérez-Garcı́a, preprint available at http://arXiv.org/abs/cond-mat/0012071;, preprint available at http://arXiv.org/abs/
con-mat/0101219.
25. T. Isoshima, K. Machida, Phys. Rev. A 60, 3313 (1999).
26. A. A. Svidzinsky, A. L. Fetter, Phys. Rev. Lett. 84, 5919
(2000).
27. F. Dalfovo, S. Giorgini, M. Guilleumas, L. P. Pitaevskii,
S. Stringari, Phys. Rev. A 56, 3840 (1997).
28. F. Dalfovo, S. Stringari, Phys. Rev. A 63, 011601(2001).

iiii

iiii

29. J. R. Anglin, personal communication.
30. C. Raman et al., Phys. Rev. Lett. 83, 2502 (1999).
31. R. J. Donnelly, Quantized Vortices in Helium II (Cambridge Univ. Press, Cambridge, 1991).
32. G. Blatter, M. V. Feigel’man, V. B. Geshkenbein, A. I.
Larkin, V. M. Vinokur, Rev. Mod. Phys. 66, 1125
(1994).
33. V. K. Tkachenko, J. Exp. Theor. Phys. 23, 1049 (1966)[Zh. Eksp. Teor. Fiz. 50, 1573 (1966)].
34. S. J. Tsakadze, Fiz. Nizk. Temp. 4, 148 (1978) [Sov. J.
Low Temp. Phys. 4, 72 (1978)].

35. We thank J. R. Anglin, A. Görlitz, R. Onofrio, and L.
Levitov for useful discussions and critical readings ofthe manuscript and T. Rosenband for assistance withthe two-axis deflector. Supported by NSF, Office ofNaval Research, Army Research Office, NASA, andthe David and Lucile Packard Foundation.
26 February 2001; accepted 14 March 2001
Published online 22 March 2001;
10.1126/science.1060182
Include this information when citing this paper.

Self-Assembly of
Subnanometer-Diameter
Single-Wall MoS2 Nanotubes
Maja Remskar,1* Ales Mrzel,1 Zora Skraba,1 Adolf Jesih,1Miran Ceh,1 Jure Demšar,1 Pierre Stadelmann,2 Francis Lévy,3Dragan Mihailovic1
We report on the synthesis, structure, and self-assembly of single-wall subnanometer-diameter molybdenum disulfide tubes. The nanotubes are up to
hundreds of micrometers long and display diverse self-assembly properties on
different length scales, ranging from twisted bundles to regularly shaped “furry”
forms. The bundles, which contain interstitial iodine, can be readily disassembled into individual molybdenum disulfide nanotubes. The synthesis was performed using a novel type of catalyzed transport reaction including C60 as a
growth promoter.
The discovery of free-standing microscopic
one-dimensional molecular structures, such as
nanotubes of carbon, has attracted a great dealof attention in the last decade because of various interesting properties associated with theirsmall dimensions, high anisotropy, and intriguing tube-like structures. These range from avariety of quantum effects (1, 2) to potentially
useful properties such as efficient field emission(3) and exceptional mechanical strength (4).
Finding that curled-up dichalcogenide sheets
can also form tube-like objects and fullerenelike nanoparticles (5–8) suggested that synthesis of nanotubes made of atoms other thancarbon may be possible, and relatively small,
15-nm-diameter tubes made of tungsten andmolybdenum disulfide have since been reported(9–11). The ultralow friction and wear properties of MoS2 fullerene-like particles (12, 13)
make inorganic fullerenes important tribological materials. Other layered materials synthesized as nanotubes, tube-like forms, oronion-like structures have been reported, suchas boron nitride nanotubes with diameters of afew nanometers (14, 15), W18O49 hollow micro1
Jozef Stefan Institute, Jamova 39, SI-1000 Ljubljana,
Slovenia. 2Centre de Microscopie Électronique-CIME,
Ecole Polytechnique Fédérale de Lausanne, CH-1015
Lausanne, Switzerland. 3Institute of Applied Physics,
Ecole Polytechnique Fédérale de Lausanne, CH-1015
Lausanne, Switzerland.

*To whom correspondence should be addressed. Email: maja.remskar@ijs.si

fibers (16), and NiCl2 multiwall nanotubes(17). Other layered compounds, such as NbS2(18) and GaSe (19), have been the subject ofextensive theoretical calculations, which havepredicted conditions for their stability in cylindrical form and some interesting electronic
properties.
We report on the synthesis and basic
structural properties of subnanometer-diameter monomolecular MoS2 single-wall nanotubes (SWNTs) produced by a catalyzed
transport reaction involving C60, and showthat the MoS2 nanotubes grow in twistedchiral bundles of identically structured molecules stuck together with interstitial iodine.
The tubes vary only in length, but not indiameter.
The single-wall MoS2 nanotubes weregrown by a catalyzed transport method using
C60 as a growth promoter in the reaction. The
C60 (5 weight %) was added to MoS2 powder inthe transport tube as catalyst, and the reaction
was run typically for 22 days at 1010 K in an
evacuated silica ampoule at a pressure of 1023
Pa with a temperature gradient of 6 K/cm.
Iodine was used as a transport agent. Approximately 15% (by weight) of the starting material
was transported by the reaction to form
SWNTs, with the rest remaining in the form oflayered material. The transported material was
subsequently thoroughly washed with toluene
to remove the C60.
The transported material grows in the formof bundles oriented perpendicular to the sub-www.sciencemag.org SCIENCE VOL 292 20 APRIL 2001

479

Appendix B
Vortex Nucleation in a Stirred
Bose-Einstein Condensate
C. Raman, J.R. Abo-Shaeer, J.M. Vogels, K.Xu, and W. Ketterle“Vortex Nucleation in a Stirred Bose-Einstein Condensate,”
Phys. Rev. Lett. 87 210402 (2001).

111

VOLUME 87, NUMBER 21

PHYSICAL REVIEW LETTERS

19 NOVEMBER 2001

Vortex Nucleation in a Stirred Bose-Einstein Condensate
C. Raman,* J. R. Abo-Shaeer, J. M. Vogels, K. Xu, and W. Ketterle
Department of Physics, MIT– Harvard Center for Ultracold Atoms, and Research Laboratory of Electronics,
MIT, Cambridge, Massachusetts 02139(Received 12 June 2001; published 1 November 2001)
We studied the nucleation of vortices in a Bose-Einstein condensate stirred by a laser beam. The
vortex cores were observed using time-of-flight absorption imaging. Depending on the stirrer size, either
discrete resonances or a broad response was visible as the stir frequency was varied. Stirring beams
small compared to the condensate size generated vortices below the critical rotation frequency for the
nucleation of surface modes, suggesting a local mechanism of generation. In addition, we observed thecentrifugal distortion of the condensate due to the rotating vortex lattice and found evidence for bent
vortices.
DOI: 10.1103/PhysRevLett.87.210402

PACS numbers: 03.75.Fi, 32.80.Pj, 67.40.Vs

This corresponds to a Landau critical velocity for surface waves yc 苷 Vs RTF , where RTF is the Thomas-Fermi
radius [15].
Recent experiments [9,19] observed vortices only atmuch higher frequencies, giving rise to a variety of theoretical models [17,20]. One explanation is that those experiments excited only the l 苷 2 mode, requiring a higher
drive frequency than Eq. (1) [16,19,21,22]. We tested thisprediction by stirring the condensate with anisotropies ofdifferent symmetries 共l 苷 2, 3, 4兲 and observing distinct
resonance frequencies for vortex formation.
Our central observation is that a small, localized stirring
beam can generate vortices below Vs . This indicates thatthe current surface mode analysis of vortex nucleation isincomplete. One might expect such a stirrer to couple tomany modes l. Surprisingly, the small beam did not excite
resonances but could generate vortices as effectively as aresonant drive.
Our method of vortex generation has been outlined inprevious work [10]. We start with nearly pure BECs(.90% condensate fraction) of up to 5 3 107 sodium
atoms in a cylindrically shaped Ioffe-Pritchard magnetic
trap with a mean radial frequency of vr 苷 2p 3 86 Hz
and axial frequency vz 苷 2p 3 20 Hz. A radio frequency “shield” limited the magnetic trap depth to 50 kHz
共2.3 mK兲. The condensate chemical potential, peak density, and healing length j were 300 nK, 4 3 1014 cm23 ,and 0.2 mm, respectively.
Vortices were generated by rotating the condensate
about its long axis with a scanning blue-detuned laser
beam (532 nm) whose beam waist varied between 5 and25 mm [23]. For the tightest focus, the peak optical dipole
potential was 620 nK. We used multiple beam patterns(formed by rapidly scanning the laser beam from 1.5 to
10 kHz) with scan radii as large as the Thomas-Fermi
radius RTF , which varied from 27 30 mm. The laser
beam was left on during evaporation to damp out dipole
motion. Immediately after producing a condensate webegan the rotation for times of up to 500 ms, generating
a vortex tangle. The laser beams were then instantly shutoff and the cloud equilibrated for 500 ms, during whichtime the vortices crystallized into an Abrikosov lattice asshown in Fig. 4c and detailed in previous work [10]. For
small numbers of vortices the gas did not fully settle intoa regular lattice before imaging.
The vortex cores were observed using resonant absorption imaging after 41 ms of ballistic expansion,
which magnified them by 20 from their size j in the
trap. As in our previous work we imaged a 50 150 mm

210402-1© 2001 The American Physical Society

Dissipation and turbulence in superfluid flow often involve the creation and subsequent motion of quantized vortices [1]. Since vortices are topological defects they may
be created only in pairs or can enter a system individuallyfrom its boundary. The nucleation process has been thesubject of much theoretical interest [2]. Experiments with
Bose-Einstein condensates (BEC) confined in atom traps
are well suited to test theories of nucleation because theboundary of the condensate is well controlled, and vortices can be directly imaged.
Vortex nucleation usually involves dynamical instabilities and superfluid turbulence [1,2]. Exceptions are thedirect coupling between ground and vortex states for small
condensates [3] and the engineering of states of quantizedcirculation by manipulating the phase of the wave function [4–6]. Turbulent flow can be created by perturbing
the system with a time-dependent boundary, for example,
by a small laser beam [7,8] or by a rotating trap anisotropy[9 –11]. The resulting vortices have been directly imaged[8 –10].
In a rotating frame, vortices are energetically favored
above a critical rotational frequency Vc [2,12]. Current
theories suggest that vortices must be nucleated by surface
waves which “collapse” into a vortex state [13–17]. This
corresponds to the disappearance of the energy barrier fora vortex to enter the cloud [2,14,18]. For surface excitations with angular momentum l h̄ and frequency vl , theminimum rotational frequency is
Vs 苷 minl 共vl 兾l兲 .

(1)0031-9007兾01兾 87(21)兾210402(4)$15.00

210402-1

PHYSICAL REVIEW LETTERS

slice of atoms in the center of the cloud using spatiallyselective optical pumping on the F 苷 2 to F 苷 3 cyclingtransition [10].
By varying the stirring parameters we explored different mechanisms for vortex nucleation. A large stirrer,
with a beam waist comparable to the Thomas-Fermi radius showed enhanced vortex generation at discrete frequencies. Figure 1 shows the number of vortices versus
the stirring frequency of the laser beam using 2-, 3-, and4-point patterns. The total laser beam power corresponded
to an optical dipole potential between 60 and 240 nK.
The resonances were close to the frequencies of excitap
tion of l 苷 2, 3, and 4 surface modes 共vl 兾l 苷 vr 兾 l兲[13]. A second, higher resonance appeared in the 3- and4-point data. This could be due to additional coupling to
the quadrupole 共l 苷 2兲 mode caused by misalignment of
the laser beams [22]. The extra peaks and the shift of theresonances from the frequencies vl 兾l may be due to thepresence of vortices and the stirrer, both of which make anunperturbed surface mode analysis inadequate.
Our results clearly show discrete resonances in the nucleation rate of vortices that depend on the geometry of
the rotating perturbation. This confirms the role of discretesurface modes in vortex formation. A dependence on thesymmetry of the stirrer (1-point versus 2-point) has also
been explored in Paris [22]. For longer stirring times andhigher laser powers the condensate accommodated more
vortices at all frequencies, and the resonances became lesspronounced.
A stirrer much smaller than the condensate size could
generate vortices very rapidly — more than 100 vortices
were created in 100 ms of rotation. Figure 2a shows thenumber of vortices produced using a 2-point pattern with ascan radius close to RTF for various stirring times. Above

19 NOVEMBER 2001

300 ms the angular momentum of the cloud appeared tosaturate and even decreased, accompanied by visible heating of the cloud.
The maximum number of vortices was roughly proportional to the stirring frequency. For a lattice rotating at frequency V, the quantized vortex lines are distributed witha uniform area density ny 苷 2V兾k, where k 苷 h兾M is
the quantum of circulation and M is the atomic mass [12].
Therefore, the number of vortices at a given rotation frequency should be
Ny 苷 2pR 2 V兾k(2)

in a condensate of radius R. The straight line in Fig. 2aassumes R 苷 RTF and that the lattice has equilibrated withthe drive. In contrast to the large stirrer no resonanceswere visible even when the number of vortices had not yet
saturated. This suggests a different mechanism of vortex
nucleation for which further evidence was obtained fromthe frequency and spatial dependences.
For our experimental conditions, a numerical calculation
by Feder yields Vs ⯝ 0.25vr 苷 21 Hz [24]. With thesmall stirrer, we observed vortices at frequencies as low
as 7 Hz. Below this frequency the velocity of the stirrer
was not much larger than the residual dipole oscillation of
the condensate. The rotational frequency below which aa)120

Number of Vortices

VOLUME 87, NUMBER 21

25 ms stir
80 ms stir
300 ms stir
600 ms stir

100
80
60
40
20
0
0

20

40

60

80

0

20

40

60

80

FIG. 1. Discrete resonances in vortex nucleation. The numberof vortices created by multipoint patterns is shown. The condensate radius was RTF 苷 28 mm. Each data point is the averageof three measurements. The arrows below thepgraph show thepositions of the surface mode resonances vr 兾 l. The stirring
times were 100 ms for the 2- and 3-point data, and 300 ms forthe 4-point data. The inset shows 2-, 3-, and 4-point dipole
potentials produced by a 25 mm waist laser beam imaged onto
the charge-coupled device camera. The separation of the beams
from the center is 25 mm for the 2-point pattern and 55 mm forthe 3- and 4-point patterns. The laser power per spot was 0.35,
0.18, and 0.15 mW for the 2-, 3-, and 4-point data, respectively.

210402-2

Rotation Frequency [Hz]b)

Stirring Frequency [Hz]

60

40

20

0

Stirring Frequency [Hz]FIG. 2. Nonresonant nucleation using a small stirrer. (a) Average number of vortices created using a 2-point pattern positioned
at the edge of the condensate. The beam waist, total power, andseparation were 5.3 mm, 0.16 mW, and 54 mm, respectively.
(b) Effective lattice rotation frequency. The lines in both graphs
indicate the predictions of different models described in the text.
The fewer vortices observed near half the trapping frequency(42 Hz) are probably due to parametric heating.

210402-2

VOLUME 87, NUMBER 21

PHYSICAL REVIEW LETTERS

19 NOVEMBER 2001

rectilinear vortex in the condensate center is energeticallyfavored is 7 Hz [2].
In Fig. 3 we varied the radius of the 2-point scan. The
stirring frequency was chosen to keep the linear velocity of
the laser beam constant. Vortices could be generated overa broad range of radii. The maximum number was obtained at intermediate radii rather than the Thomas-Fermi
surface, providing further evidence that surface excitationsof the unperturbed condensate are not the dominant nucleation mechanism. The observed radial dependence makes
it unlikely that the thermal cloud plays a crucial role inthe vortex nucleation, since at very low temperatures its
maximum density occurs at the surface of the condensate.
Indeed, we observed fewer vortices at higher temperatures.
The nucleation mechanism for small stirrers may be related to our earlier experiments on the onset of dissipationin stirred condensates. There we observed a drag force atvelocities above ⬃0.1c, where c is the speed of sound at
the condensate center [7,25]. The friction with the moving
stirrer causes an asymmetry in the density profile in frontof and behind the laser beam. This has been directly imaged for linear motion [25]. Similar flow field effects canbe observed in Fig. 3b, where they are clearly linked to theformation of vortices. Vortex pairs are predicted to arise
from linear stirring [26,27]. When the laser beam moves ina circle, corotating vortices will be favored, whereas counterrotating vortices will be expelled from the system.
For an object smaller than the healing length j, thecritical velocity for vortex formation occurs at the Landau
value given by Eq. (1). For larger objects such as ourlaser beam, the flow field around the stirrer can reduce thecritical velocity relative to Eq. (1) [26], which may explain
our observation of vortices below 21 Hz.
In our earlier work we observed that the size of a condensate with vortices exceeded the size of the nonrotatingcondensate [10]. Here we study these centrifugal distortions quantitatively (also note [11]). Figure 4 shows theenhancement of the cloud size R in time of flight by up to
25% due to additional rotational kinetic energy. Rotation2
adds a centrifugal potential 2共1兾2兲M共Vr兲
p , leading to an
2
effective radial trapping frequency of vr 2 V 2 . For aconstant number of atoms N, this increases the ThomasFermi radius

FIG. 3. Spatial dependence of vortex nucleation. (a) The number of vortices produced at a constant stirring velocity 共0.2c兲.
At the Thomas-Fermi radius, the angular frequency of the stirrer was 17.5 Hz. The error bars are the standard deviation of
three measurements at the same radius. (b) Axial phase contrast
images showing the pure condensate with the aligned stirrer (1),and at 4.4 ms intervals, the condensate during (2–7) and after(8 –10) stirring. Each frame is 120 mm wide.

FIG. 4. Centrifugal effects on a rotating condensate. (a) Observed radial size of the condensate, as determined from a parabolic fit to the time-of-flight distribution after 41.5 ms. (b),(c)Comparison of a nonrotating condensate 共Rtof 苷 570 mm兲 and
one with 160 vortices. Radial in situ phase contrast imagingof (d) a condensate at rest, and (e) in rotation at a frequencyof 75 Hz, showing the modified aspect ratio. The length of thecondensate in (d) was 200 mm.

210402-3

RTF 苷 R0 兾关1 2 共V兾vr 兲2 兴3兾10(3)

and reduces the mean-field interaction energy Eint .
The total release energy of the gas is then E 苷
1Eint 1 2 Ieff V 2 1 Ey0Ny . The second term accounts
for the rigid rotation of the lattice while the third term is aquantum correction due to the kinetic energy of the cores,
which is negligible for large Ny . The effective moment
2
N . Theof inertia of the condensate is Ieff 苷 2兾7MRTF
energy per unit length of a single vortex Ey0 must be
averaged over the Thomas-Fermi distribution [28]. We
predict a 30% increase in E for 120 vortices, whereas theobserved increase in R 2 is about 50%. This discrepancy
is probably due to our selection of the central slice of thecigar, where the rotational energy is the highest, and due

210402-3

VOLUME 87, NUMBER 21

PHYSICAL REVIEW LETTERS

to the unobserved axial expansion, which may depend on
the angular momentum of the cloud.
If we account for centrifugal effects and combine
Eqs. (2) and (3), we expect a divergence of the number ofvortices near the trap frequency (dashed line in Fig. 2a).
The deviation of the data from this line suggests thatthe condensate did not fully equilibrate with the rotating
drive. Taking into account the critical velocity for vortex
nucleation, yc ⯝ 0.1c [25], we expect the maximum
rotation frequency of the lattice to be VS 2 yc 兾RTF ,where VS is the frequency of the stirrer moving at
radius RTF . Using the measured number of vortices, we
can invert Eqs. (2) and (3) to derive the lattice rotation
frequency, which is shown in Fig. 2b, along with the
expected value VS 2 2p 3 6 Hz assuming a constant
N . The discrepancy can be partly attributed to loss of
atom number due to heating by the stirrer, which was
up to 30%. We can also derive from these equations theflow velocity at the edge of the condensate. For a latticewith 144 vortices, this velocity exceeded the speed ofsound at the condensate center by 40%, in contrast toa recent suggestion that supersonic rotation speeds areunattainable [29].
At low rotational velocities, vortices should not be rectilinear as assumed in many theoretical calculations but bent
[30,31]. Such bent vortices should have lower visibility in
our images due to the line of sight integration across the
optically pumped condensate slice. Figure 5 shows several examples. Some appear as vortex lattices with tilted
vortex cores. Other images show structures reminiscent ofhalf rings and coiled vortices. However, it is not obvious
how some of the observed time-of-flight features are related to spatial structures in the trapped condensate.
In conclusion, we have identified two distinct mechanisms for vortex nucleation in rotating condensates —FIG. 5. Three-dimensional structure of vortices. Shown areseveral examples of time-of-flight pictures of condensates at low
rotational frequencies, where “smeared-out” vortex cores andelongated features were observed. The condensate radius was
510 mm.

210402-4

19 NOVEMBER 2001

surface modes and local turbulence. It would be intriguing
to study the vortex phase diagram [32,33] and the role ofthe thermal cloud in vortex decay [29].
We thank J. R. Anglin, D. Feder, A. E. Leanhardt, and
A. P. Chikkatur for useful discussions. This research is
supported by NSF, ONR, ARO, NASA, and the David andLucile Packard Foundation.

*Present address: School of Physics, Georgia Institute ofTechnology, Atlanta, GA 30332-0430.
Email address: craman@gatech.edu[1] R. J. Donnelly, Quantized Vortices in Helium II (Cambridge
University Press, Cambridge, 1991).
[2] A. L. Fetter and A. A. Svidzinsky, J. Phys. Condens. Matter
13, R135 (2001).
[3] B. M. Caradoc-Davies, R. J. Ballagh, and K. Burnett, Phys.
Rev. Lett. 83, 895 (1999).
[4] M. R. Matthews et al., Phys. Rev. Lett. 83, 2498 (1999).
[5] Ł. Dobrek et al., Phys. Rev. A 60, R3381 (1999).
[6] K.-P. Marzlin and W. Zhang, Phys. Rev. A 57, 4761 (1998).
[7] C. Raman et al., Phys. Rev. Lett. 83, 2502 (1999).
[8] S. Inouye et al., e-print cond-mat/0104444.
[9] K. W. Madison et al., Phys. Rev. Lett. 84, 806 (2000).
[10] J. R. Abo-Shaeer, C. Raman, J. M. Vogels, and W. Ketterle,
Science 292, 476 (2001).
[11] P. Haljan et al., e-print cond-mat/0106362.
[12] P. Nozières and D. Pines, The Theory of Quantum Liquids(Addison-Wesley, Redwood City, CA, 1990).
[13] F. Dalfovo et al., Phys. Rev. A 56, 3840 (1997).
[14] T. Isoshima and K. Machida, Phys. Rev. A 60, 3313 (1999).
[15] U. A. Al Khawaja et al., Phys. Rev. A 60, 1507 (1999).
[16] F. Dalfovo and S. Stringari, Phys. Rev. A 63, 011601(2001); M. Tsubota et al., e-print cond-mat/0104523.
[17] D. L. Feder et al., Phys. Rev. Lett. 86, 564 (2001).
[18] D. L. Feder et al., Phys. Rev. A 61, 011601(R) (2000).
[19] K. W. Madison et al., Phys. Rev. Lett. 86, 4443 (2001).
[20] J. J García-Ripoll and V. M. Pérez-García, e-print condmat/0006368.
[21] S. Sinha and Y. Castin, e-print cond-mat/0101292.
[22] F. Chevy et al., e-print cond-mat/0104218.
[23] R. Onofrio et al., Phys. Rev. Lett. 84, 810 (2000).
[24] D. Feder (private communication).
[25] R. Onofrio et al., Phys. Rev. Lett. 85, 2228 (2000).
[26] T. Frisch et al., Phys. Rev. Lett. 69, 1644 (1992).
[27] B. Jackson et al., Phys. Rev. Lett. 80, 3903 (1998).
[28] D. Stauffer and A. Fetter, Phys. Rev. 168, 156 (1968).
[29] P. O. Fedichev and A. E. Muryshev, e-print cond-mat/
0004264.
[30] J. J. García-Ripoll and V. M. Pérez-García, e-print condmat/01021297.
[31] A. Aftalion and T. Riviere, e-print cond-mat/0105208.
[32] S. Stringari, Phys. Rev. Lett. 82, 4371 (1999).
[33] T. Mizushima et al., e-print cond-mat/0104358.

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Appendix C
Formation and Decay of Vortex
Lattices
J.R. Abo-Shaeer, C. Raman, and W. Ketterle“Formation and Decay of Vortex Lattices in Bose-Einstein
Condensates at Finite Temperatures,”Phys. Rev. Lett. 91 070409 (2002).
(Included in Appendix C)

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VOLUME 88, NUMBER 7

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Formation and Decay of Vortex Lattices in Bose-Einstein Condensates at Finite Temperatures
J. R. Abo-Shaeer,* C. Raman,† and W. Ketterle
Department of Physics, MIT-Harvard Center for Ultracold Atoms, and Research Laboratory of Electronics,
Massachusetts Institute of Technology, Cambridge, Massachusetts 02139(Received 13 August 2001; published 1 February 2002)
The dynamics of vortex lattices in stirred Bose-Einstein condensates have been studied at finite temperatures. The decay of the vortex lattice was observed nondestructively by monitoring the centrifugal
distortions of the rotating condensate. The formation of the vortex lattice could be deduced from theincreasing contrast of the vortex cores observed in ballistic expansion. In contrast to the decay, theformation of the vortex lattice is insensitive to temperature change.
DOI: 10.1103/PhysRevLett.88.070409

PACS numbers: 03.75.Fi, 32.80.Pj, 67.40.Vs

symmetric stirring beams were used (Gaussian waist
w 苷 5.3 mm, stirring radius 24 mm). The laser power of
0.16 mW per beam corresponded to an optical dipole potential of 310 nK. After the stirring beams were switched
off, the rotating condensate was left to equilibrate in thestatic magnetic trap for various hold times. As in ourprevious work, the vortex cores were observed using
optical pumping to the F 苷 2 state and resonant absorption imaging on the F 苷 2 to F 苷 3 cycling transition[9]. After 42.5 ms of ballistic expansion the cores weremagnified to 20 times their size, j, in the trap.
The decay of the vortex lattice can be observed by allowing the condensate to spin down in the trap for variable
times before the ballistic expansion and subsequent observation of the vortex cores. However, this method requires
destructive imaging and suffers from shot-to-shot variations. In situ phase-contrast imaging is nondestructive, but
the vortex cores are too small to be resolved. Instead, wemonitored the centrifugal distortion of the cloud due to thepresence of vorticity. This is a quantitative measure forthe rotation frequency, V, of the lattice, and therefore thenumber of vortices [15]. Such distorted shapes have been
observed previously for rotating clouds [9,11,13].
The shape of a rotating condensate is determined by themagnetic trapping potential and the centrifugal potential
1
2 2 MV 2 r 2 , where M is the atomic mass. Fromp the effective radial trapping frequency vr ! vr0 苷 vr2 2 V 2 ,one obtains the aspect ratio of the rotating cloud, A0 苷
vr0 兾vz , asGaseous Bose-Einstein condensates (BEC) have becomea test bed for many-body theory. The properties of a condensate at zero temperature are accurately described by anonlinear Schrödinger equation. More recently, theoreticalwork on the ground state properties of condensates [1] hasbeen extended to rotating condensates containing one orseveral vortices [2] and their dynamics. These include vortex nucleation [3,4], crystallization of the vortex lattice [5],and decay [6,7]. Experimental study has focused mainlyon the nucleation of vortices, either by stirring condensates
directly with a rotating anisotropy [8–10] or creating condensates out of a rotating thermal cloud [11]. In addition,
the decay of vortices in nearly pure condensates has also
been analyzed [8,11,12]. Here we report the first quantitative investigation of vortex dynamics at finite temperature. The crystallization and decay of a vortex lattice havebeen studied and a striking difference is found between
the two processes: while the crystallization is essentiallytemperature independent, the decay rate increases dramatically with temperature.
The method used to generate vortices has been outlined
in previous work [9,13]. Condensates of up to 75 million
sodium atoms (.80% condensate fraction) were preparedin a cigar-shaped Ioffe-Pritchard magnetic trap using
evaporative cooling. The radial and axial trap frequencies of vx 苷 2p 3 共88.8 6 1.4兲 Hz, vy 苷 2p 3
共83.3 6 0.8兲 Hz, and vz 苷 2p 3 共21.1 6 0.5兲 Hz, corresponded to a radial trap asymmetry of er 苷 共vx2 2 vy2 兲兾
共vx2 1 vy2 兲 苷 共6.4 6 0.2兲% and an aspect ratio of A 苷vx 兾vz 苷 共4.20 6 0.04兲. The relatively large value ofthe radial trap asymmetry is due to gravitational sag andthe use of highly elongated pinch coils (both estimatedto contribute equally). The radio frequency (rf) used forevaporation was held at its final value to keep the temperature of the condensate roughly constant throughout
the experiment. The condensate’s Thomas-Fermi radii,
chemical potential, and peak density were Rr 苷 28 mm,
Rz 苷 115 mm, 300 nK, and 4 3 1014 cm23 , corresponding to a healing length j ⯝ 0.2 mm.
Vortices were produced by spinning the condensate for
200 ms along its long axis with a scanning, blue-detuned
laser beam (532 nm) [8,14]. For this experiment two

For the decay measurements, the condensate was stirred
for 200 ms, producing ⬃130 vortices on average at thecoldest temperature (determined using time-of-flight imaging). After the drive was stopped the cloud equilibrated in
the stationary magnetic trap. Ten in situ images of eachcondensate were taken at equal time intervals using nondestructive phase-contrast imaging detuned 1.7 GHz fromresonance (see Fig. 1a). We verified that the decay rate
was not affected due to repeated imaging by varying the070409-1© 2002 The American Physical Society

0031-9007兾02兾 88(7)兾070409(4)$20.00

q
A0 苷 A 1 2 共V兾vr 兲2 .

(1)

070409-1

PHYSICAL REVIEW LETTERSb)c)FIG. 1. (a) Spin down of a rotating condensate in a static magnetic trap. The first phase contrast image is taken 100 ms after
turning off the drive, with each subsequent image spaced by
100 ms. The rotating vortex lattice caused a radial swelling of
the condensate, reducing the aspect ratio. As vortices leave thesystem the aspect ratio approaches its static value of 4.2. The
field of view is 25 by 75 mm. (b) Observation of a rotating
thermal cloud. The parameters are identical to (a), but the probe
light detuning is closer to resonance, enhancing the sensitivity
to the more dilute thermal cloud. The phase shift of the dense
condensate exceeds 2p and is displayed as saturated (black) in
the image. The apparent loss in atom number is due to Rayleighscattering of the probe light. (c) The inner and outer contours
represent the aspect ratio of the condensate and thermal cloud,respectively, as obtained from two-dimensional fits to phase-contrast images.

time between exposures. The theoretical treatment of the
decay has two limiting cases, one where the thermal cloudis nearly stationary and the other where the thermal cloudis closely following the rotating condensate [6]. Because
the thermal cloud could not easily be discerned in images taken with 1.7 GHz detuning, we used light closer toresonance (400 MHz detuning) to determine the shape ofthe thermal cloud (Fig. 1b).
The aspect ratio of the condensate was obtained by fitting a 2D Thomas-Fermi profile to the 1.7 GHz images.
The aspect ratio of the thermal cloud was determined fromthe 400 MHz images by masking off the condensate in the
inner region of the cloud and then fitting a 2D Gaussian
to the image. The comparison of the contours of the condensate and thermal cloud (condensate fraction of Nc 兾N 苷0.62) shows that the thermal cloud is also rotating. The images for the thermal cloud show that the aspect ratio decays
from 3.0 to 4.2 on the same time scale as the condensate.
This corresponds to an initial rotation rate of ⬃2兾3 that of
the condensate.
The damping rate of the vortex lattice, obtained fromexponential fits to the data, was studied at different temperatures by varying the condensed fraction of atoms in the
trap. The condensate fractions were obtained from fits totime-of-flight images of the condensate before the stirring.
The temperature was derived from these values using thescaling theory for an interacting Bose gas [16]. At a fixed
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18 FEBRUARY 2002

rf frequency for evaporation, the centrifugal potential lowers the trap depth by a factor 1 2 共V兾vr 兲2 for a thermal
cloud rotating at frequency V. Evaporation should lower
the temperature of the rotating cloud by the same factor.
Figure 2a shows how the aspect ratio of the condensate
approaches its static value as the vortex lattice decays. The
decrease of the angular speed appears to be exponential(Fig. 2b) and strongly depends on temperature (Fig. 3).
The crystallization of the lattice occurs during the first
500 ms of hold time. Examination of Fig. 2 during thistime frame indicates that this process has no effect on
the decay. It should be noted that the exponential natureof the decay is related to the corotation of the thermal
cloud with the condensate. When the thermal cloud isfixed, theoretical [6] and experimental [8] studies show
nonexponetial behavior.
In addition to the decay process, the formation of thevortex lattice has also been examined. After rotating thecondensate it typically took hundreds of ms for the lattice
to form (see Fig. 4 in Ref. [9]). One may expect the lattice
to already form in the rotating frame during the stirring
because the lattice is the lowest energy state for a given
angular momentum. This absence of equilibration in therotating frame is presumably due to heating and excitationa)4.0

Aspect Ratio

a)

3.5
3.0

Nc / N
0.78
0.75
0.71
0.62

2.5
2.0

b)

Lattice Rotation Frequency (Hz)VOLUME 88, NUMBER 7

0

2

4

6
Time (s)

8

10

0

2

4

6
Time (s)

8

10

60
50
40
30
20

FIG. 2. Decay of a vortex lattice at finite temperatures. (a) The
aspect ratio of the condensate approaching its static value. Eachpoint represents the average of ten measurements. Error bars
given for 共≤兲 are statistical and are typical of all four data sets.
(b) The decay of the rotation rate of the lattice for the same datausing Eq. (1). The decay of the rotation depends strongly on thethermal component.

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Decay Rate (1/s)

PHYSICAL REVIEW LETTERS
Decay Rate (1/s)

VOLUME 88, NUMBER 7

2.0
1.5

18 FEBRUARY 2002

a)

3.0
1.5
0.0
0.0

1.0

0.3
T / Tc

0.6

0.5
0.80

FIG. 3. Decay rates for vortex lattices at several temperatures.
The rates are determined from data taken during the first secondof equilibration. Each point represents the average of five measurements. The inset figure emphasizes the strong dependenceof the decay rate on temperature, T. The transition temperature
was Tc 苷 790 nK and varied by less than 7% for the data shown.

of collective lattice modes by the stirring beams. The crystallization of the vortex lattice was studied by determining
the contrast or visibility of the vortex cores as a functionof equilibration time. To avoid any bias, we used an automated vortex recognition algorithm. Each image was normalized by dividing it by a blurred duplicate of itself. A
binary image was then created with a threshold set to thevalue at which the algorithm reliably detected almost all
vortices that were identified by visual inspection of equilibrated images (there was less than 5% discrepancy). Clusters of contiguous bright pixels within a circular area werecounted as “visible” vortices. Figure 4a shows three vortex
lattices after different equilibration times with the visible
vortices identified.
The lowest temperature (337 nK, corresponding to acondensate fraction of 艐80%) was close to the chemical
potential. Further cooling would have resulted in smaller
condensates. The highest temperature (442 nK) was
limited by the rapid decay of the vortex lattice.
Figure 4b and 4c show that the formation of the lattice depends very weakly on temperature, if at all, over therange studied. The larger number of vortices crystallized atlower temperatures (Fig. 4b) is due to the strong temperature dependence of the lattice decay rates, which differedby more than a factor of 5. We can correct for this by estimating the number of vortices Ny 共t兲 as a function of timefrom the centrifugal distortion measurements describedabove as Ny 共t兲 苷 关2V共t兲兾k兴pR共t兲 2 , where k 苷 h兾M is
the quantum of circulation, M is the sodium mass, and R is
the radial Thomas-Fermi radius. By normalizing the number of visible vortices by this estimate, we deduce the vortex visibility as a function of time. These lattice formation
curves overlap almost perfectly for different temperatures(Fig. 4c).
The decay of a vortex lattice is discussed in Refs. [6,7].
The process is modeled as a two-step transfer of angular momentum. The rotation of the condensate is damped
due to friction with the thermal cloud (mc2th ), which is in
070409-3b)140
Number of Visible Vortices

0.65
0.70
0.75
Condensate Fraction

120
100
80
60
Nc / N
0.78
0.75
0.71
0.62

40
20
0

c)

100

200
300
Time (ms)

400

500

100

200
300
Time (ms)

400

500

1.0
Visibility of Vortices

0.60

0.8
0.6
0.4
0.2
0.0

FIG. 4. Crystallization of the vortex lattice. (a) The top row
shows three condensates that have equilibrated for 50, 150, and
300 ms, respectively, and have 48, 86, and 140 vortices recognized as visible by our algorithm. The bottom row shows thesame condensates with the visible vortices circled. The field ofview was 1.4 by 1.6 mm. (b) Growth of the number of visible
vortices for several temperatures expressed by the condensate
fraction (Nc 兾N). (c) Visibility of vortices derived from the datain (b), normalized by the number of vortices inferred from centrifugal distortion measurements.

turn damped via friction with the trap anisotropy (mth2er ).
Even at our highest temperatures, mc2th is sufficiently
larger than mth2er as to allow the thermal cloud to spin
up to ⬃2兾3 of the lattice rotation rate. mth2er is calculated in Ref. [17] for a classical Boltzmann gas. For ourparameters the relaxation time trot for the thermal cloudrotation is trot 苷 4t, where t is the relaxation time forquadrupolar deformations. t is approximately 5兾4 of thetime between elastic collisions tel 苷 2兾nyth s [18], where
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PHYSICAL REVIEW LETTERS

n is the atomic density, yth is the thermal velocity, and s isthe elastic cross section. For a quantum-saturated thermal
cloud, this gives a relaxation time proportional to T 22 .
The presence of the condensate adds an additional
moment of inertia, extending the rotational relaxation
time by a factor finertia 苷 共Ith 1 Ic 兲兾Ith , where Ith and Ic
are the moments of inertia of the thermal cloud andthe condensate, respectively. At high temperatures thisfactor approaches 1, because the moment of inertia of thethermal cloud is dominant. For very low temperatures
finertia ⬃ 共Ic 兾Ith 兲. This ratio is [6]Ic
15z 共3兲 Nc m,苷Ith
16z 共4兲 Nth kB T

In conclusion, we have studied the crystallization anddecay of vortex lattices. Both processes are dissipativeand require physics beyond the Gross-Pitaevskii equation.
The dynamics of vortices nicely illustrates the interplay ofexperiment and theory in the field of BEC.
The authors acknowledge T. Rosenband for the development of the vortex recognition algorithm. We also thankJ. M. Vogels and K. Xu for their experimental assistanceand J. R. Anglin, Z. Hadzibabic, A. E. Leanhardt, and
R. Onofrio for insightful discussions. This research is supported by NSF, ONR, ARO, NASA, and the David andLucile Packard Foundation.

(2)

where the numerical prefactor is 1.04. Thus, for a noninteracting Bose gas in the low temperature limit, finertia
scales as T 24 and the relaxation time of the vortex lattice
should scale as T 26 . (For very round traps a weaker T 22
temperature dependence is expected, due to the t 21 scalingof the thermal cloud relaxation time.) The observed temperature dependence of the relaxation time, decreasing bya factor of 17 for a 60% increase in the temperature, agrees
fortuitously well given the approximations made in the theory. The absolute relaxation rates predicted by Refs. [6,17]
are on the order of 1 s21 , in reasonable agreement with our
results. However, for a quantitative comparison to theory it
will be necessary to further characterize the rotating thermal cloud, which may not be in full equilibrium.
In contrast to the decay, the crystallization process ofthe vortex lattice was essentially independent of temperature. This was unexpected because all dissipative processes
observed thus far in BECs, including the decay of the vortex lattice, have shown a strong temperature dependence[19,20]. Feder [21] has numerically simulated a stirredcondensate using only the Gross-Pitaevskii equation. The
results show that the absence of dissipation leads to a rapid,
irregular motion of the vortices. The addition of a phenomenological dissipative term in Ref. [5] resulted in theformation of triangular vortex lattices. However, the originof the dissipation was not identified. Our results suggestthat the time-limiting step for the evolution of a vortex
tangle into a regular lattice does not strongly depend on
temperature. One possibility is that the thermal cloud is
not directly involved. This may be similar to the reconnection of vortices or the damping of Kelvin modes, where
the spontaneous creation of excitations acts as a dissipative
mechanism [22]. Another possibility is that the rearrangement of the vortices into a rectilinear lattice is slow andnot limited by dissipation. Our quantitative analysis of
the formation process seems to contradict qualitative observations made in Paris [8], in which the lattice ordering
appeared to have temperature dependence. This indicatesthat further study may be necessary to fully characterize
the role of the thermal cloud in the formation process.
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*Electronic address: jamil@mit.edu†
Present address: School of Physics, Georgia Institute ofTechnology, Atlanta, Georgia 30332-0430.
[1] F. Dalfovo, S. Giorgini, L. P. Pitaevskii, and S. Stringari,Rev. Mod. Phys. 71, 463 (1999).
[2] A. L. Fetter and A. A. Svidzinsky, J. Phys. Condens. Matter
13, R135 (2001).
[3] F. Dalfovo and S. Stringari, Phys. Rev. A 63, 011601(2001).
[4] J. R. Anglin, cond-mat/0106619.
[5] M. Tsubota, K. Kasamatsu, and M. Ueda, cond-mat/
0104523.
[6] O. N. Zhuravlev, A. E. Muryshev, and P. O. Fedichev,
cond-mat/0007246.
[7] P. O. Fedichev and A. E. Muryshev, cond-mat/0004264.
[8] K. W. Madison, F. Chevy, W. Wohlleben, and J. Dalibard,
Phys. Rev. Lett. 84, 806 (2000).
[9] J. R. Abo-Shaeer, C. Raman, J. M. Vogels, and W. Ketterle,
Science 292, 476 (2001).
[10] E. Hodby, G. Hechenblaikner, S. A. Hopkins, andO. M. Maragò, and C. J. Foot, cond-mat/0106262.
[11] P. C. Haljan, I. Coddington, P. Engels, and E. A. Cornell,
cond-mat/0106362.
[12] P. C. Haljan, B. P. Anderson, I. Coddington, and E. A.
Cornell, Phys. Rev. Lett. 86, 2922 (2000).
[13] C. Raman, J. R. Abo-Shaeer, J. M. Vogels, K. Xu, and
W. Ketterle, Phys. Rev. Lett. 87, 210402 (2001).
[14] R. Onofrio, D. S. Durfee, C. Raman, M. Köhl, C. E.
Kuklewicz, and W. Ketterle, Phys. Rev. Lett. 84, 810(2000).
[15] P. Nozières and D. Pines, The Theory of Quantum Liquids(Addison-Wesley, Redwood City, CA, 1990).
[16] S. Giorgini, L. P. Pitaevskii, and S. Stringari, J. Low Temp.
Phys. 109, 309 (1997).
[17] D. Guéry-Odelin, Phys. Rev. A 62, 033607 (2000).
[18] D. Guéry-Odelin, F. Zambelli, J. Dalibard, and S. Stringari,Phys. Rev. A 60, 4851 (1999).
[19] D. S. Jin, M. R. Matthews, J. R. Ensher, C. E. Wieman, andE. A. Cornell, Phys. Rev. Lett. 78, 764 (1997).
[20] D. M. Stamper-Kurn, H.-J. Miesner, S. Inouye, M. R.
Andrews, and W. Ketterle, Phys. Rev. Lett. 81, 500(1998).
[21] D. L. Feder, MIT-Harvard Center for Ultracold Atoms
Seminar, 2001.
[22] M. Leadbeater, T. Winiecki, D. C. Samuels, C. F. Barenghi,
and C. S. Adams, Phys. Rev. Lett. 86, 1410 (2001).

070409-4

Appendix D
Dissociation and Decay of
Ultracold Sodium Molecules
T. Mukaiyama, J.R. Abo-Shaeer, K. Xu, J.K. Chin, and W. Ketterle“Dissociation and Decay of Ultracold Sodium Molecules,”Phys. Rev. Lett. 92 180402 (2004).

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Dissociation and Decay of Ultracold Sodium Molecules
T. Mukaiyama, J. R. Abo-Shaeer, K. Xu, J. K. Chin, and W. Ketterle
Department of Physics, MIT-Harvard Center for Ultracold Atoms,
and Research Laboratory of Electronics, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA(Received 24 November 2003; published 4 May 2004)
The dissociation of ultracold molecules was studied by ramping an external magnetic field through a
Feshbach resonance. The observed dissociation energies directly yielded the strength of the atommolecule coupling. They showed nonlinear dependence on the ramp speed. This was explained by aWigner threshold law which predicts that the decay rate of the molecules above threshold increases
with the density of states. In addition, inelastic molecule-molecule and molecule-atom collisions werecharacterized.
DOI: 10.1103/PhysRevLett.92.180402

PACS numbers: 03.75.Nt, 32.80.Pj, 33.80.Ps, 34.20.Cf

Recently, it has become possible to create ultracold
molecular gases from precooled atomic samples [1–11].
Extending the ultralow temperature regime from atoms tomolecules is an important step towards controlling the
motion of more complicated objects. The complex structure of molecules may lead to new scientific opportunities,
including the search for a permanent electric dipole moment, with sensitivity much higher than for heavy atoms[12], and the realization of quantum fluids of bosons andfermions with anisotropic interactions [13]. Furthermore,stable mixtures of atomic and molecular condensates are
predicted to show coherent stimulation of atom-molecule
or molecule-atom conversion, constituting quantumcoherent chemistry [14].
To date, all realizations of ultracold molecules( < 1 mK) have bypassed the need for direct cooling of
the molecules, which is difficult due to the complicatedrovibrational structure. Rather, molecules were formed
from ultracold atoms using Feshbach resonances [2–11],
where a highly vibrational excited molecular stateis magnetically tuned into resonance with a pair of colliding atoms.
In this Letter, we study the dissociation and decay ofsuch highly excited molecules. Figure 1 shows a schematic of the dissociation process. For magnetic fields
above the Feshbach resonance, the molecular state crosses
the free atomic states, shown here as discrete states in a
finite quantization volume. The interaction between
atoms and molecules turns these crossing into anticrossings. When the magnetic field is swept very slowly
through the resonance, the molecules follow the adiabatic
curve and end up in the lowest energy state of the atoms.
For faster ramps, the molecular populations will partiallycross some of the low-lying states, and the dissociation
products will populate several atomic states. The stronger
the coupling between the molecular state and the atomic
states, the faster the molecules dissociate and the smaller
the energy release in the dissociation. Observing theatom-molecule coupling in one-body decay (dissociation)
is a new method to experimentally determine the strengthof a Feshbach resonance. Previous measurements
used two- or three-body processes to characterize the
Feshbach resonance and therefore required accurate
knowledge of the atomic density distribution.
Collisional properties of the molecules were alsostudied. Inelastic collisions limit both the production ofmolecules and their lifetime. We observed loss of molecules by collisions both with atoms and other molecules.
These two processes were studied by separating atoms
and molecules with a short pulse of laser light [9].
To generate molecules, sodium condensates in the
jF; mF i  j1; 1i state were prepared in an optical dipole
trap. The trap frequencies of 290 Hz in the radial directionand 2.2 Hz in the axial direction yielded typical densitiesof 1:7  1014 cm3 for 5  106 atoms. Atoms were thenspin-flipped using an adiabatic radio frequency sweep tothe j1; 1i state, where a 1 G wide Feshbach resonanceexists at 907 G [15].

180402-1

 2004 The American Physical Society

0031-9007=04=92(18)=180402(4)$22.50

a<0Energy

a>0

δE

atoms

molecule
B0

Magnetic Field

FIG. 1. Schematic diagram of energy levels for molecules andatoms. The diabatic energy levels are shown as dashed lines.
The adiabatic curves (solid lines) include the atom-molecule
coupling. When the magnetic field is swept from positive tonegative scattering length, dissociated molecules end up in one
or several atomic states, depending on the ramp rate of themagnetic field. The spheres represent the distribution of the
population before and after the ramp.

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The magnetic field sequence used to create and detect
Na2 molecules was identical to our previous work [9].
Briefly, the axial magnetic field was ramped to 903 G in
100 ms using two pairs of bias coils. In order to prepare
the condensate on the negative scattering length side of
the resonance, the field was stepped up to 913 G as quickly
as possible (  1 s) to jump through the resonance withminimal atom loss. The field was then ramped back down
to 903 G in 50 s to form molecules. In order to remove
nonpaired atoms from the trap, the sample was irradiatedwith a 20 s pulse of resonant light. Because 903 G is far
from the Feshbach resonance, the mixing between atomic
and molecular states was small and therefore molecules
were transparent to this ‘‘blast’’ pulse. By ramping thefield back to 913 G molecules were converted back to
atoms. Absorption images were taken at high fields (either
at 903 or 913 G) after 10 to 17 ms ballistic expansion, with
the imaging light incident along the axial direction of thecondensate.
To study the momentum distribution of the backconverted atoms, the magnetic field was ramped up immediately after turning off the optical trap, or for areference, at the end of the ballistic expansion. The difference between the energies of ballistic expansion is thereleased dissociation energy. Energies were obtained
from the rms width of the cloud hx2 i as E 
3mhx2 i=2t2 , where t is the ballistic expansion time andm is the atomic mass. Figure 2 shows that faster fieldramps created hotter atoms.
An earlier theoretical treatment assumes a constantpredissociation lifetime of the molecules and predicts a
linear relation between dissociation energy and field ramp
rate [16]. This theory predicts a much faster dissociation(and therefore smaller dissociation energy) than was observed. Furthermore, our data show a nonlinear dependence. Linear behavior would be expected if the lifetimeof the molecules was independent of the energy fromthe dissociation threshold. The fact that the slope be-comes smaller for increasing ramp rate indicates thatthe lifetime of molecules decreases with the ramp rate.
As we show, this can be explained by pan increase of thedensity of atomic states, leading to adependence ofthe molecular decay rate (Wigner threshold law [17]).
The decay rate follows from Fermi’s golden ruleas h
 2 jVma j2 D [18], where Vma is the matrix
element between atomic and molecular states, which toleading order is independent of . The density of states
D is given by 3=2
V
m
1=2
D 
;
(1)
2
2
h 2
where V is the quantization volume for free atomic states.
An expression for the matrix element Vma is obtainedby comparing the energy shift near a Feshbach resonancewith second-order perturbation theory. Assuming two
atoms in a volume V, the energy shift of the low-lying
continuum states due to the coupling with a bound molecular state is

jVma j2



jVma j2;
 B  B0(2)

where  is the difference between atomic and molecular magnetic moments, B is the applied magnetic field,
and B0 is the position of the Feshbach resonance.
The energy shift can also be expressed in terms of themean field energy 4 h 2 a=mV, where a  abg B= B 
B0 is the scattering length near the Feshbach resonance(abg is the background scattering length and B is theresonance width [19]):

4 h 2 abg B:
mV B  B0(3)

Comparing Eqs. (2) and (3) yields
jVma j2 

4 h 2a B:mV bg(4)

If the entire population is initially in the molecularstate, the fraction of molecules, m , at energy follows
the rate equation,
 1
 1
dm
d
d
dm

 m
(5)
dt
dt
dt
d


FIG. 2. Dissociation energy of molecules as a function ofmagnetic field ramp rate. The dashed line represents the linear
relation described in Ref. [16], the solid line shows the result ofour model using a theoretical value for B  0:98 G and abg 
3:4 nm, and the dotted line shows a curve with the productabg B as a fitting parameter.

180402-2

2 jVma j2 D
hj

B_ j

m

:

(6)

Using Eqs. (1) and (4), we solve the differential equation for m ,s
2B ma2bg
3=2m  e 2=3 C ;
C
:
(7)
h 2
h B_
In the laboratory frame, the atoms have kinetic energy=2, and therefore the average energy of an atom after
dissociation is180402-2

VOLUME 92, N UMBER 18
E 

Z1
0

2

dm

PHYSICA L R EVIEW LET T ERS

10v
u 2
_ 2=3
u h
h

B
A : (8)
 0:591@t 2
mabg 2B

Using theoretical values abg  3:4 nm, =h 
3:65  1:4 MHz=G, and B  0:98 G [20,21], the data
show good agreement with our model. A fit of the productabg B to our data results in abg B  3:64 G nm  2%
(dotted line in Fig. 2). The discrepancy between thetheoretical and fitted values is 4 times bigger than thestatistical error, but within the systematic error of themeasurement of the release energy.
Further experiments with ultracold sodium molecules
will critically depend on their collision properties.
Therefore we also studied heating and inelastic collision
processes. As shown in Fig. 3, we observed monotonic
heating of the pure molecular sample over 30 ms. In
addition, we observed short time scale oscillations (6 ms)
in the fitted temperature (inset of Fig. 3). Such breathing
oscillations were excited because the molecules wereformed over the volume of the atomic condensate andstarted oscillations around their equilibrium volume. The
equilibrium volume deduced from the observed released
energy is much smaller than the initial volume. The
absence of damping implies a collision time of at least
6 ms, or a molecular scattering length smaller than 17 nm(obtained using the expression for the collision rate
8 a2 vth nm , where vth is the thermal velocity). It is unclear whether the oscillation disappeared due to collisions or limited signal-to-noise ratio.
The temperature of the molecular cloud saturated at
250 nK after 15 ms. A possible explanation is thebalance between heating due to inelastic molecular decay
and the evaporative cooling caused by the finite trap depth(1:7 K). This would imply a collision time of 15 ms.
However, we have no clear evidence that thermalization
has occurred. Clearly, further studies of elastic collisions
between ultracold molecules are necessary.

FIG. 3. Temperature of the molecular cloud. After 15 ms, thetemperature saturates at 250 nK. Error bars represent thestatistical error (standard deviation). The inset shows finer
resolution data for holding times up to 6 ms. The solid line isa guide to the eye.

180402-3

week ending
7 MAY 2004

Molecules formed via an s-wave Feshbach resonanceare created in the rotational ground state, but in highvibrational states. Therefore, one expects vibrational relaxation to be a strong, inelastic decay mechanism.
Figure 4(a) shows the decay of a pure molecularsample. The decay was analyzed with the rate equation
N_ m Kmm nm :Nm

(9)Here Nm ; nm is the number and the density of themolecules, respectively, and Kmm is the moleculemolecule collision rate coefficient. Because of the changing size and temperature of the molecular cloud during
the first 15 ms (Fig. 3), we fit data points only atlater times, assuming a thermal equilibrium volume forthe molecules. The decay at earlier times is slower, consistent with a larger molecular cloud. The fit yields amolecule-molecule collision coefficient of Kmm  5:1 
1011 cm3 =s, about 2 orders of magnitude larger than the
typical values reported for fermions [4,5].
Inelastic collisions between molecules and atoms werealso observed by keeping atoms in the trap [Fig. 4(b)].
The decay was analyzed assuming that the loss of

FIG. 4. Decay of ultracold molecules trapped alone (a) or
together with atoms (b). The solid lines in (a) and (b) are fits ofEqs. (9) and (10) to data, which assume vibrational relaxationin the collision of m olecules (a) or collisions between molecules and atoms (b). The insets illustrate the experimental
sequences.

180402-3

PHYSICA L R EVIEW LET T ERSVOLUME 92, N UMBER 18

(a)

(b)

50 ms

(c)

Molecule Number

150x10200 ms

1 ms

4 ms

3

100
50
0
5

6 7 8 9

100

2

3

4

5

6 7 8 9Ramp Time (µs)

1000

2

3

4

FIG. 5. Conversion of atoms to molecules for various ramp
times. During a given time, the magnetic field was swept by
10 G. (a) and (b) show absorption images taken after 14 ms timeof flight. The molecules (bottom) were radially separated fromthe atoms (top) by a field gradient of 2:8 G=cm. The molecules
were converted back to atoms only 0.5 ms before imaging by
ramping the magnetic field back across the Feshbach resonance.
This time was chosen to be long enough for any transient field
fluctuations to damp out, but short enough such that the size ofthe imaged cloud reflected the molecular temperature, not the
dissociation energy. (a) The atoms remained in the trap. (b) The
atoms were removed by a resonant laser pulse immediately
after the magnetic field ramp. (c) Number of molecules as afunction of ramp time for (a) (open circles) and (b) (closed
circles).

molecules occurred mainly due to collisions with atoms,
resulting in an exponential decay:
N_ m Kam na :
Nm

(10)

Here na is the density of atoms, and Kam is the atommolecule collision rate coefficient. From the fit, we extract a lifetime of 106 s and a rate coefficient Kam 
5:5  1011 cm3 =s, which agrees well with theoreticalpredictions [21,22].
The inelastic losses determine the maximum conversion efficiency from atoms to molecules. For an adiabatic
ramp, one expects close to 100% conversion efficiency.
Indeed, in experiments with fermionic atoms, efficiencies
up to 85% have been observed [5]. Figure 5 shows theresults for magnetic field ramps of different durations.
The two sets of images show that applying the blast pulse
dramatically improved the molecular number and temperature. Without it, a slower ramp time (4 ms) appeared
to be more favorable for molecule formation [open circles
180402-4

week ending
7 MAY 2004

in Fig. 5(c)]. No molecules were observed for a 50 sramp time. However, with the blast pulse, a similar number of molecules was obtained for all ramp times between
50 s to 4 ms [closed circles in Fig. 5(c)].
We assume that these results reflect the interplay of twocompeting processes. The adiabatic condition requires a
relatively slow field ramp for efficient conversion.
However, this means that the atoms and molecules spend
more time near or at the Feshbach resonance, whereinelastic collision rates are enhanced. In contrast to
Fig. 5(b), the absence of a molecular signal in Fig. 5(a)for 50 s ramp time reflects that the atomic density
reduction due to the ballistic expansion is too slow for
the molecules to survive the inelastic collisions withthe atoms.
In conclusion, we observed a Wigner threshold behavior in the dissociation of ultracold molecules. We wereable to characterize a Feshbach resonance using a onebody decay (dissociation) process. The rapid decay of themolecules due to collisions with atoms and other molecules imposes a severe limit to further evaporative cooling for bosons. This also explains the low conversion
efficiency (  4%), in contrast to recent experimentswith fermions.
The authors thank D. E. Miller for experimental assistance and A. E. Leanhardt, M. Saba, and D. Schneble for
their critical reading of the manuscript. We also thank P. S.
Julienne, B. J. Verhaar, and V. A. Yurovsky for useful discussion. This research is supported by NSF, ONR, ARO,
and NASA.

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[5] J. Cubizolles et al., Phys. Rev. Lett. 91, 240401 (2003).
[6] K. E. Strecker et al., Phys. Rev. Lett. 91, 080406 (2003).
[7] S. Dürr et al., Phys. Rev. Lett. 92, 020406 (2003).
[8] C. Chin et al., Phys. Rev. Lett. 90, 033201 (2003).
[9] K. Xu et al., Phys. Rev. Lett. 91, 210402 (2003).
[10] M. Greiner et al., Nature (London) 426, 537 (2003).
[11] S. Jochim et al., Science 302, 2101 (2003).
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[13] M. Baranov et al., Phys. Scr. T102, 74 (2002).
[14] D. J. Heinzen et al., Phys. Rev. Lett. 84, 5029 (2000).
[15] S. Inouye et al., Nature (London) 392, 151 (1998).
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1550 (1999).
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[18] F. H. Mies et al., Phys. Rev. A 61, 022721 (2000).
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[21] V. A. Yurovsky et al., Phys. Rev. A 62, 043605 (2000).
[22] V. A. Yurovsky and A. Ben-Reuven, Phys. Rev. A 67,
043611 (2003).

180402-4

Appendix E
Coherent Molecular Optics using
Sodium Dimers
J.R. Abo-Shaeer, D.M. Miller, J.K. Chin, K. Xu, T. Mukaiyama, and W.
Ketterle “Coherent Molecular Optics using Sodium Dimers,”
cond-mat/0409327 (2004).

126

Coherent Molecular Optics using Sodium Dimers
J.R. Abo-Shaeer∗ , D.E. Miller, J.K. Chin, K. Xu, T. Mukaiyama, and W. Ketterle†arXiv:cond-mat/0409327 v1 13 Sep 2004

Department of Physics, MIT-Harvard Center for Ultracold Atoms,
and Research Laboratory of Electronics, MIT, Cambridge, MA 02139(Dated: September 13, 2004)
Coherent molecular optics is performed using two-photon Bragg scattering. Molecules were produced by sweeping an atomic Bose-Einstein condensate through a Feshbach resonance. The spectral
width of the molecular Bragg resonance corresponded to an instantaneous temperature of 20 nK,
indicating that atomic coherence was transferred directly to the molecules. An autocorrelating interference technique was used to observe the quadratic spatial dependence of the phase of an expanding
molecular cloud. Finally, atoms initially prepared in two momentum states were observed to crosspair with one another, forming molecules in a third momentum state. This process is analogous tosum-frequency generation in optics.
PACS numbers: PACS 03.75.Fi, 34.20.Cf, 32.80.Pj, 33.80.Ps

Similar to the field of optics, where the high intensity
and coherence of lasers allowed for the observation of effects such as frequency doubling and wave-mixing, atom
optics has benefited greatly from the realization of BoseEinstein condensates (BEC). High phase-space density(atoms per mode) and a uniform phase [1, 2] give thecondensate its laser-like qualities. Although not fundamentally required [3, 4], BEC has led to the observationof such phenomena as four-wave mixing [5], matter wave
amplification [6, 7], and atom number squeezing [8].
The current state of molecular optics is similar toatom optics prior to the realization of BEC. Diffraction
and interferometry of thermal molecular beams has been
demonstrated [9, 10, 11, 12], yet monoenergetic beams
lack the density necessary to observe nonlinear effects.
However, recent experiments using Feshbach resonances
have demonstrated the conversion of degenerate atomic
bosons [13, 14, 15] and fermions [16, 17, 18, 19, 20] into
ultracold molecules. These sources have the potential togreatly advance molecular optics. Furthermore, atommolecule coupling can be studied as the first steps towards “superchemistry”, where chemical reactions arestimulated via macroscopic occupation of a quantum
state [21].
The coherent manipulation of atomic matter waves via
stimulated light scattering has been crucial in the development of nonlinear atom optics (for a review see [23]).
Here we demonstrate the ability to apply Kapitza-Dirac
and Bragg diffraction [24] to cold molecules. Using optical standing waves of suitably chosen frequencies, sodium
dimers were coherently manipulated with negligible heating or other incoherent processes. First, we characterized
the coherence of our “source” molecules, created via Feshbach resonance. By measuring the Bragg spectrum of
the molecules immediately after their creation, the con-∗ Contact Info: jamil@mit.edu† Website: cua.mit.edu/ketterle group

Atomic Momentum (pr)
-2

-1

0

1

2

a)

b)
c)

d)

-2

-1

0

1

2

Molecular Momentum (pr)FIG. 1: Bragg diffraction of (a) atoms and (b) molecules.
Scattered particles recoil with identical momenta, pr . However, during ballistic expansion diffracted molecules expand
with half the velocity of atoms, due to their doubled mass.
The pulse duration in each image was 200 µs. A shorter
pulse (5 µs) populated multiple (c) atomic and (d) molecular
momentum states. The halos in (c) are due to collisions between different momentum states [22]. The time-of-flight ineach image is 17 ms.

version from atoms to molecules was shown to be coherent - the matter wave analog to frequency doubling in
optics. The quadratic spatial dependence of the phaseof the expanding molecules was observed using an autocorrelation interference technique. By creating a duplicate sample of molecules and overlapping it with theoriginal, matter wave interference was observed. Finally,

2
a)

b)

c)

1

Outcoupled Fraction (a.u.)

the matter wave analog to sum-frequency generation wasdemonstrated. Atoms prepared in two momentum states,
prior to creating molecules, were observed to cross-pair,generating a third momentum state.
To produce molecules, sodium condensates were prepared in a crossed optical dipole trap in the |F, mF i =|1, −1i state. Trap frequencies of (ωx , ωy , ωz ) = 2π×(146,
105, 23) Hz yielded a typical peak density of n0 ≃4.3 × 1014 cm−3 for 25 million atoms. Atoms were thenspin-flipped to the |1, 1i state, in which a 1 G wide Feshbach resonance exists at 907 G [25].
The magnetic field sequence used to create and detect
Na2 molecules was identical to our previous work [15, 26].
Briefly, the axial (z-axis) magnetic field was ramped to903 G in 100 ms. In order to prepare the condensate
on the negative scattering length side of the resonance,
the field was stepped up to 913 G as quickly as possible(∼ 1 µs) to jump through the resonance with minimal
atom loss. After waiting 1200 µs for the transient field
to die down, the field was ramped back down to 903 G in
50 µs to form molecules. In order to remove non-paired
atoms from the trap, the sample was irradiated with a
10 µs pulse of resonant light. Because 903 G is far fromthe Feshbach resonance, the mixing between atomic andmolecular states was small, and therefore molecules weretransparent to this “blast” pulse. By ramping the fieldback to 913 G, molecules were converted back to atoms.
Absorption images were taken at high fields (either at
903 G or 913 G), with the imaging light incident along
the axial direction of the condensate. Bragg scatteringof atoms and molecules was carried out using two nearly
orthogonal beams (θB = 84◦ ), aligned such that particles
were scattered along the x-axis of the trap. The beams
were far-detuned from atomic/molecular transitions tolimit spontaneous scattering. For atoms the detuningwas ≃ 4 nm from the sodium D lines. To find a suitable transition for the molecules, we scanned the laser
wavelength and measured the Rabi frequency for Bragg
transitions. Several narrow transitions were observed,
but not carefully characterized. For this work the laser
was set to 590.159 nm, yielding a Rabi frequency of 2
kHz and corresponding to an effective detuning of ∼ 50
MHz from the resonance.
Fig 1 shows time-of-flight images of Bragg scattering for atoms and molecules. Because the kinetic energy of the scattered particles was much larger thantheir mean-field energy, individual momentum states
were well-resolved in ballistic expansion. Both atoms
and molecules receive equal two-photon recoil momentum, pr = 2h sin(θB /2)/λL , where λL is is the wavelength of the Bragg beams. However, scattered molecules
move away from the central peak with half the velocity of atoms, owing to their doubled mass. Fig 1c,dshow Kapitza-Dirac scattering, where multiple atomic
and molecular momentum states were populated due tothe broad frequency distribution of the short pulse (5 µs).

0

1

0

1

0
-100

-50

0

50

100

Detuning (kHz)FIG. 2: Bragg spectra for atoms and molecules. In (a)the spectrum is taken for a pure atomic sample above the
Feshbach resonance. (b) and (c) are spectra of atoms andmolecules, respectively, below the resonance. In (c) atoms
were removed from the trap with resonant light to limit losses
due to atom-molecule collisions. The Bragg resonance condition for molecules occurs at half the frequency of the atomic
resonance.

In order to study the coherence properties of the sample, Bragg spectra [1] were taken by pulsing on the twolaser beams for 250 µs (∼ 1 kHz resolution), before releasing the particles from the trap. For noninteracting
particles, the Bragg resonance occurs at a relative detuning of ν0 = ±p2r /2mh between the beams, where thesign of ν0 dictates the direction of out-coupling. Interactions in a condensate give rise to a mean-field shift of
the resonance δν = 4n0 U/7h, where U=4π~2 a/m and ais the scattering length. Fig 2 shows three spectra for(a) atoms above the Feshbach resonance, as well as (b)atoms and (c) molecules after sweeping through the resonance. The reduced mean-field shift for atoms below theresonance (Fig 1b) can be attributed to inelastic losses
caused by passing through the resonance. Atoms below
the resonance coexisted with a small fraction of molecules(2%). The peak output for each set of data is normalized
to 1. The actual peak out-coupled fractions were 0.06 forthe atoms and 0.5 for the molecules. The atomic signal
was kept intentionally low to minimize collisions, whichmake the data analysis difficult (see halos in Fig 1c). As
expected from the resonance condition, molecular resonances occur at half the frequency of atomic resonances.
Two mechanisms contribute to the fundamental widthof the Bragg resonance [1, 27]. For a parabolic density
distribution, the finite size of the sample yields a momentum spread∆νp = 1.58

pr
,
2πmx0

(1)

where x0 is the Thomas-Fermi radius. In addition, theinhomogeneous density distribution of the sample pro-

3
duces a spread in mean-field energyr
8 n0 U
∆νn =
.
147 h

a)
(2)

b)

The fundamental width is approximately given by thequadraturesum of these two broadening mechanismsq2∆ν = ∆νn + ∆νp2 .
The fundamental width, ∆ν, and measured rms width,σ, are compared for each case in Table I. n0 and x0 were
determined from the size of the condensate in time-offlight. The measured widths cannot be accounted for by
fundamental broadening mechanisms alone. For atoms
above resonance, the fundamental width is ∆ν=1.39 kHz,
compared to the measured value of 4.46 kHz. Therefore,
another broadening mechanism must contribute ∼ 4 kHz
to the width. Most likely this is due to Doppler broadening caused by random center-of-mass motion and othercollective excitations of the condensate. This was investigated by mixing two frequencies into each Bragg beam toout-couple particles in both ±x directions. For particles
at rest, the out-coupling should always be symmetric.
However, we observe the ratio of out-coupled particles ineither direction to fluctuate. In addition we measure asmall, consistent shift in the Bragg spectrum, indicatinga drift velocity. A line broadening of 4 kHz corresponds
to a velocity of ≃ 2 mm/s, or a vibrational amplitude of≃ 2 µm (compared to x0 = 13µm). This is not unreasonable, because the field ramping scheme used to bring theatoms to high field is violent and may induce collective
excitations such as breathing modes.
Spectrum∆ν (kHz) σ (kHz) T (nK)
Atoms (Above) 1.39
4.46(17)
10
Atoms (Below)
1.03
4.50(60)
10
Molecules
0.36 ‡ 4.53(14)20TABLE I: Fundamental width (∆ν), measured rms width (σ),
and the corresponding temperature (T), assuming a thermal
distribution.
‡ This lower bound assumes that the molecules have the same spatial profile as the atoms, which our results indicate is not the case.

Despite vibrational noise making the dominant contribution to the width of the spectra, the measured values
are still narrow enough to indicate quantum degeneracy.
For a given σ, the corresponding temperature for a thermal distribution of particles isT =m h2 σ 2
kB p2r(3)

Thus, for an rms width of 4.5 kHz, the temperature for athermal distribution of molecules would be 20 nK, comparable to a previous value obtained using a time-of-flighttechnique [15]. The BEC transition temperature for our
trap parameters and 5 × 104 molecules is much higher

c)

-1
0
1
Momentum (pr)FIG. 3: Matter wave interference of molecules. (a) The molecular sample is split with a short Kapitza-Dirac pulse, creating two identical copies with momenta ±pr . (b)-(c) After the
copies have separated for time ∆t = 100 µs, a second pulse recombines them, giving rise to interference in each momentum
component. The time-of-flight in each image is 12 ms.

(115 nK). This demonstrates a deeply degenerate, purely
molecular sample, where as previous experiments havedemonstrated coherent admixture of molecular character
into an atomic BEC [28].
The molecular Bragg Spectrum showed a surprisingly
large shift of δν = 625 Hz. If interpreted as a meanfield shift, this would imply either a very high density(possible due to a spatial collapse) or an anomalously
large molecular scattering length outside the Feshbachresonance. Further study is necessary.
The spatial phase of the expanding molecular cloud
was directly imaged using an autocorrelation method[29], which gives rise to the self-interference of the molecular sample (see Fig. 3). To accomplish this, two identical copies of the sample were made using a short KapitzaDirac pulse (10 µs), applied after 2 ms of ballistic expansion. The copies, with momentum ±pr , moved away fromthe zero momentum peak for time ∆t before an identical pulse recombined them with the original. This typeof interferometer has three readout ports, with momenta
0, ±pr . The straight-line interference fringes are characteristic of a quadratic spatial phase. The fringe spacing
we measure is consistent with λf = ht/md [30], whered = pr ∆t/m is the distance the copies moved between
pulses [31]. Interference fringes can only be resolved forsmall d. Therefore, this method cannot be used to observe coherence lengths longer than those inferred from
Bragg spectroscopy. It should be noted that the appearance of interference fringes does not imply that the sample is condensed. Rather, it demonstrates only that thecoherence length in time-of-flight is longer than the separation d. Therefore, similar interference can also be observed for a cloud of thermal atoms [32, 33].
The conversion of atoms to molecules may be viewed as
the atom optic equivalent of frequency doubling [34]. The

4relevant Hamiltonian for the atom-molecule coupling has
the same form as that for the optical frequency doublingprocess:a†2m am am

Atomic Momentum (pr)
0
1

a)

(4)

where am is the annihilation operator for the atomic field
and a†2m is the creation operator for the molecular field.
The measurement of the Bragg spectrum shows that the
sharp “linewidth” of the seed (atom) laser is inheritedby the molecular laser. In nonlinear optics, photon interactions are typically mediated by a refractive medium.
Here, the nonlinearity arises from the atoms themselves,in the form of s-wave interactions. The high density, or“brightness”, of the source, together with the enhanced
interactions at the Feshbach resonance provide the means
to combine two matter waves. By combining two disparate matter waves, rather than identical ones, we extend the analogy of frequency doubling to the more general process of sum frequency generation. To do this,atoms were initially prepared in momentum states 0, 1
(in units of pr ). By sweeping through the resonance,molecules were produced in three momentum states: 0,
1, and 2 (see Fig. 4). States 0 and 2 are simply thefrequency doubled components of the two initial matter waves. State 1 however, results from cross pairing
between the initial momentum states, and is thus theirsum frequency. This is the first time that a Feshbachresonance was observed between atoms colliding with acontrolled non-vanishing momentum. The Feshbach resonance should be slightly shifted compared to the resonance for atoms at rest, which reflects the same physics
encountered in the temperature dependence of the position of the resonance [35].
In conclusion, we have demonstrated coherent molecular optics using standing light waves. The ability tocoherently convert atoms into molecules makes molecular optics even richer than atom optics. In addition, thetechniques demonstrated in this paper could prove useful for probing molecules formed in quantum-degeneratefermi systems, and possibly even Cooper pairs.
The authors would like to acknowledge M. Boyd and
W. Setiawan for experimental contributions and thankA.E. Leanhardt and M. W. Zwierlein for critical readingsof the manuscript. This research is supported by NSF,
ONR, ARO, and NASA.

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b)

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1
2
Molecular Momentum (pr)FIG. 4: Sum frequency generation of atomic matter waves.
(a) Atoms were initially prepared in momentum states 0, 1.
(b) By sweeping through the Feshbach resonance, atoms combine to form molecules with momenta 0, 1, and 2. Momentum
state 1 is the sum frequency of the two atomic matter waves.
The “nonlinear medium” is provided by the atomic interactions. The time-of-flight in each image is 17 ms.

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Coherent Molecular Optics using Sodium Dimers.

2004.

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