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Springer Theses Recognizing Outstanding Ph.D. Research James Keaveney Collective Atom–Light Interactions in Dense Atomic Vapours Springer Theses Recognizing Outstanding Ph.D. Research For furthervolumes: http://www.springer.com/series/8790 Aims and Scope The series ‘‘Springer Theses’’ brings together a selection of the very best Ph.D. theses from around the world and across the physical sciences. Nominated and endorsed by two recognized specialists, each published volume has been selected for its scientific excellence and the high impact of its contents for the pertinent fieldofresearch.Forgreateraccessibilitytonon-specialists,thepublishedversions includeanextendedintroduction,aswellasaforewordbythestudent’ssupervisor explaining the special relevance of the work for the field. As a whole, the series will provide a valuable resource both for newcomers to the research fields described, and for other scientists seeking detailed background information on specialquestions.Finally,itprovidesanaccrediteddocumentationofthevaluable contributions made by today’s younger generation of scientists. Theses are accepted into the series by invited nomination only and must fulfill all of the following criteria • They must be written in good English. • ThetopicshouldfallwithintheconfinesofChemistry,Physics,EarthSciences, Engineering andrelatedinterdisciplinaryfieldssuchasMaterials, Nanoscience, Chemical Engineering, Complex Systems and Biophysics. • The work reported in the thesis must represent a significant scientific advance. • Ifthethesisincludespreviouslypublishedmaterial,permissiontoreproducethis must be gained from the respective copyright holder. • They must have been examined and passed during the 12 months prior to nomination. • Each thesis should include a foreword by the supervisor outlining the signifi- cance of its content. • The theses should have a clearly defined structure including an introduction accessible to scientists not expert in that particular field. James Keaveney Collective Atom–Light Interactions in Dense Atomic Vapours Doctoral Thesis accepted by Durham University, UK 123 Author Supervisor Dr. JamesKeaveney Prof.Charles Adams Department of Physics Department of Physics Durham University Durham University Durham Durham UK UK ISSN 2190-5053 ISSN 2190-5061 (electronic) ISBN 978-3-319-07099-5 ISBN 978-3-319-07100-8 (eBook) DOI 10.1007/978-3-319-07100-8 Springer ChamHeidelberg New YorkDordrecht London LibraryofCongressControlNumber:2014939383 (cid:2)SpringerInternationalPublishingSwitzerland2014 Thisworkissubjecttocopyright.AllrightsarereservedbythePublisher,whetherthewholeorpartof the material is concerned, specifically the rights of translation, reprinting, reuse of illustrations, recitation,broadcasting,reproductiononmicrofilmsorinanyotherphysicalway,andtransmissionor informationstorageandretrieval,electronicadaptation,computersoftware,orbysimilarordissimilar methodology now known or hereafter developed. Exempted from this legal reservation are brief excerpts in connection with reviews or scholarly analysis or material supplied specifically for the purposeofbeingenteredandexecutedonacomputersystem,forexclusiveusebythepurchaserofthe work. Duplication of this publication or parts thereof is permitted only under the provisions of theCopyright Law of the Publisher’s location, in its current version, and permission for use must always be obtained from Springer. Permissions for use may be obtained through RightsLink at the CopyrightClearanceCenter.ViolationsareliabletoprosecutionundertherespectiveCopyrightLaw. The use of general descriptive names, registered names, trademarks, service marks, etc. in this publicationdoesnotimply,evenintheabsenceofaspecificstatement,thatsuchnamesareexempt fromtherelevantprotectivelawsandregulationsandthereforefreeforgeneraluse. While the advice and information in this book are believed to be true and accurate at the date of publication,neithertheauthorsnortheeditorsnorthepublishercanacceptanylegalresponsibilityfor anyerrorsoromissionsthatmaybemade.Thepublishermakesnowarranty,expressorimplied,with respecttothematerialcontainedherein. Printedonacid-freepaper SpringerispartofSpringerScience+BusinessMedia(www.springer.com) Supervisor’s Foreword Theinteractionoflightandmatterunderliesmanyareasofscience.Eventhoughour understandinghasadvancedenormouslythereremainsomefundamentalquestions thatareverydifficulttoanswer.Forexample,ifonetakesthesimplestconceivable systemoflight-induceddipolesandthenallowsthesedipolestointeract,thetheo- retical description quickly becomes unmanageable as we have N interacting par- ticles,whereN maybelarge,inanopenquantumsystem.Theinteractingdipoles establish correlations that invalidate the mean field description of Maxwell’s equations in a medium. However, if there is strong dephasing of the interacting dipolesthecorrelationsaredestroyedandamean-fielddescriptionisre-established. To understand these ideas requires detailed simple model systems where experi- mentaldatacanbecomparedtotheoreticalsimulations. This thesis presents one approach to address such questions. The main results concern an experimental study of interacting atomic dipoles in a thin almost two-dimensional gaseous layer with a thickness in the range of 100 nm–1 lm. Thelayerconsists ofalkaliatoms (withasingleactivevalence electron) confined betweentwosuperpolishedsapphirewindows.Theatomsareprobedusingaweak laser beam tuned through the main atomic resonance. The ability to compare the measuredspectrawithamodelthatprovidesanaccuratedescriptionintheweakly interacting regime makes it possible to extract the interesting physics of strongly interacting dipoles. Due to the thermal motion of the atoms there is strong dephasing of the dipoles but, remarkably, it is still possible to observe coherent features of the dipole–dipole interaction. For example, as the length of the cell is varied one sees that the dipole–dipole-induced shift of the atomic resonance line oscillates with a period equal to one half the wavelength of the incident light. Historically, this propagation dependence of the mean-field shift is referred to as the collective or cooperative Lamb shift. This term arose because the dipole–dipole interactions within an ensemble may be modelled in terms of the exchange of virtual photons, similar to the self-interaction of an electron with a field of virtual photons. Despite the fact that these ideas have a long history, this thesis reports the first experimental measurement of the length dependence of the collective Lamb shift. v vi Supervisor’sForeword The experiment reported here has stimulated new theoretical work and further experiments that have enhanced our understanding of light–matter interactions in simple systems where the full many-body description is still challenging. Thisknowledgecannowbeexploitedtodesignopticalsystemswiththepotential for new applications in quantum optics. Durham, April 2014 Prof. Charles Adams Abstract This thesis presents an investigation of the fundamental interaction between light andmatter,realisedwitharubidiumvapourconfinedinacellwhosethickness(in the propagation direction) is less than the optical wavelength. This confinement allows observation of spectroscopic features not found in longer cells, such as Dicke narrowing. These effects are measured experimentally and a theoretical model is developed, which allows the characterisation of the medium in terms of the atomic electric susceptibility. Interactions between the atoms and their surroundings, whether this be the walls of the cell or other nearby atoms, are explored. In the frequency domain we observe broadening and shifts of the spectral features due to these interactions. The atom–surface interaction shifts the spectral lines, following the expected 1/r3 van-der-Waals behaviour. The interatomic dipole–dipole interactions are more complex, and we find collective effects play an important role. We present an experimental verification of the full spatial dependence of the cooperative Lamb shift, which follows the theoretical predictionmade40yearsago,animportantdemonstrationofcoherentinteractions in a thermal ensemble. The interactions also play a role in determining the refractive index of the medium,limitingthemaximumnear-resonantindexton=1.31.Usingheterodyne interferometry, we experimentally measure an index of n = 1.26 ± 0.02. This index enhancement leads to large bandwidth regions where a significant slow- or fast-light effect is present. We verify the fast-light effect in the time domain by observing the superluminal propagation of a sub-nanosecond optical pulse, and measurethegroupindexofthemediumtoben = -1.0 ± 0.1 9 105,thelargest g negative group index measured to date. Weinvestigatetheradiativedecayrateusingtime-domainfluorescence,andwe observe radiation trapping effects in a millimetre-thickness vapour. Finally, we present results on sub-nanosecond coherent dynamics in the system which are achieved by pumping the medium with a strong optical pulse. vii Acknowledgments This thesis would not have been possible without the help and support of many people. First and foremost I would like to thank my supervisor, Charles Adams, without whom this thesis would not have been possible. His passion and enthu- siasm for science is second to none, and his guidance and insight have been invaluable over the past few years. My thanks also go to Ifan Hughes for his valuable contributions to the project, innumerable enlightening conversations about physics and proof-reading of this thesis, as well as many ‘fruitful discus- sions’ about all things football.Aspecial mention must goto ourcollaborators in Armenia, Armen and David, who make the finest, thinnest vapour cells in the world. Certainly without these cells this thesis would not be what it is today. Thanks go to my office mates Lee (cheers, mush), Dan and Tim. Their friendship and banter has made the days spent in the office more enjoyable, par- ticularlyinthelastfewmonthswhilstwritingup.ItisagreatrelieftoknowthatI will never again be forced to listen to Radio 1 Xtra, courtesy of Chris. Questionable taste in music aside, it has been a pleasure to share a lab with him andIamfortunatetohavebenefittedfromhisexpertise(andoftenhisequipment) overtheyears.IamalsogratefultoUlrichforteachingmetheexperimentalskills andsettingmeoffontherighttrackinthelabatthebeginningofmyPh.D.andto Christophe and Rob for many discussions about dipole–dipole interactions. Kate joinedtheprojectinOctober2012,andItakethisopportunitytowishherluckfor the future, as well as thank her for proof-reading a large part of this thesis. I would like to extend my thanks to the rest of AtMol. I am sure that the friendly atmosphere and real camaraderie that exists in the group has a direct influence on its success, whether that be through stimulating discussions in the tea room or the willingness of every member to share their time and expertise to help someone else out. My acknowledgments would not be complete without thanking the most important people in my life. To mam, dad, Veronica and Joseph—thank you for helping me achieve as much as I have done, for your constant encouragement in everythingthatIdo.Andfinally,toZara—thelastthreeandahalfyearshavehad their ups and downs, and you’ve been there with me through all of it. Thank you for all of your love and support, I couldn’t have done it without you. ix Contents 1 Introduction. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1 1.1 Strong Interactions and Collective Effects. . . . . . . . . . . . . . . . 1 1.2 Thermal Vapours . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3 1.3 Nano-Cells . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4 1.4 Structure of this Thesis. . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5 References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6 2 Atom–Light Interactions for Independent Atoms. . . . . . . . . . . . . 9 2.1 The Two-Level Atom. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9 2.1.1 Hamiltonian. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11 2.1.2 Time Evolution . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12 2.2 Electric Susceptibility. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13 2.3 Motion and the Doppler Effect . . . . . . . . . . . . . . . . . . . . . . . 15 2.4 Lineshapes: Lorentzians, Gaussians and the Voigt Profile. . . . . 16 2.5 Atomic Structure . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 18 2.6 Summary. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 18 References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 19 3 Thin Cell Spectroscopy. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 21 3.1 Dicke Narrowing . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 21 3.1.1 Modelling Dicke Narrowing . . . . . . . . . . . . . . . . . . . . 24 3.2 Mixing of Reflection and Transmission. . . . . . . . . . . . . . . . . . 26 3.2.1 Thin Film Theory. . . . . . . . . . . . . . . . . . . . . . . . . . . . 27 3.3 The Weak-Probe Limit. . . . . . . . . . . . . . . . . . . . . . . . . . . . . 31 3.4 Summary. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 33 References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 34 4 Atom–Surface Interactions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 35 4.1 The van der Waals Atom–Surface Interaction . . . . . . . . . . . . . 35 4.1.1 Atom–Surface Potential in the Nano-Cell . . . . . . . . . . . 36 4.2 Monte-Carlo Simulation of Interaction Time Distribution . . . . . 37 4.3 Experiment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38 4.4 Outlook. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 41 References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 41 xi

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