Graduate Texts in Physics Forfurthervolumes: www.springer.com/series/8431 Graduate Texts in Physics Graduate Texts in Physics publishes core learning/teaching material for graduate- and ad- vanced-levelundergraduatecoursesontopicsofcurrentandemergingfieldswithinphysics, both pure and applied. These textbooks serve students at the MS- or PhD-level and their instructorsascomprehensivesourcesofprinciples,definitions,derivations,experimentsand applications(asrelevant)fortheirmasteryandteaching,respectively.Internationalinscope and relevance, the textbooks correspond to course syllabi sufficiently to serve as required reading.Theirdidacticstyle,comprehensivenessandcoverageoffundamentalmaterialalso makethemsuitableasintroductionsorreferencesforscientistsentering,orrequiringtimely knowledgeof,aresearchfield. SeriesEditors ProfessorRichardNeeds CavendishLaboratory JJThomsonAvenue CambridgeCB30HE,UK [email protected] ProfessorWilliamT.Rhodes DepartmentofComputerandElectricalEngineeringandComputerScience ImagingScienceandTechnologyCenter FloridaAtlanticUniversity 777GladesRoadSE,Room456 BocaRaton,FL33431,USA [email protected] ProfessorSusanScott DepartmentofQuantumScience AustralianNationalUniversity ScienceRoad Acton0200,Australia [email protected] ProfessorH.EugeneStanley CenterforPolymerStudiesDepartmentofPhysics BostonUniversity 590CommonwealthAvenue,Room204B Boston,MA02215,USA [email protected] ProfessorMartinStutzmann WalterSchottkyInstitut TUMünchen 85748Garching,Germany [email protected] Frank Grossmann Theoretical Femtosecond Physics Atoms and Molecules in Strong Laser Fields Second Edition FrankGrossmann InstitutfürTheoretischePhysik TechnischeUniversitätDresden Dresden,Sachsen,Germany ISSN1868-4513 ISSN1868-4521(electronic) GraduateTextsinPhysics ISBN978-3-319-00605-5 ISBN978-3-319-00606-2(eBook) DOI10.1007/978-3-319-00606-2 SpringerChamHeidelbergNewYorkDordrechtLondon LibraryofCongressControlNumber:2013944233 ©SpringerInternationalPublishingSwitzerland2008,2013 Thisworkissubjecttocopyright.AllrightsarereservedbythePublisher,whetherthewholeorpartof thematerialisconcerned,specificallytherightsoftranslation,reprinting,reuseofillustrations,recitation, broadcasting,reproductiononmicrofilmsorinanyotherphysicalway,andtransmissionorinformation storageandretrieval,electronicadaptation,computersoftware,orbysimilarordissimilarmethodology nowknownorhereafterdeveloped.Exemptedfromthislegalreservationarebriefexcerptsinconnection with reviews or scholarly analysis or material supplied specifically for the purpose of being entered and executed on a computer system, for exclusive use by the purchaser of the work. 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Printedonacid-freepaper SpringerispartofSpringerScience+BusinessMedia(www.springer.com) To thememoryofmyfather HansGrossmann Preface to the Second Edition Themainmotivationforthissecondeditionofthebookwastheinclusionofmore exercisesand,mostimportantly,alsoacollectionofsolutionsoftheseexercisesat theendofthebook.Sometypeerrorsandmoresevereflawsofthefirsteditionthat havecometomyattentionhavebeencorrected.Thebookis,however,intendedas a comprehensive introduction to a topic of current interest and not as a complete review of the field. I have therefore not added more (advanced) material into the maintext.Furthermore,Ihavereservedlyupdatedtheliteraturelistbyincludinga fewmoreresearchpapers,althoughalotmoreworkhasbeendoneinthelastfive years and a related new field, the field of attosecond physics, has emerged. Some moretextbookreferencesandreviewshavealsobeenaddedwhereappropriate. Again, I would like to express my thanks for enlightening discussions on the topics touched herein to more generations of students that attended my related lectures at TU Dresden and also to Larry Schulman, Jan Handt, Werner Koch, Christoph-MarianGoletz,AlexanderKästner,MichaelFischer,CarlosZagoya,Se- bastianKrause,NiklasRohling,MaxBuchholz,andTobiasFiedelschusterfor on- goingexchangeofideasandtoAlexanderKästnerforprovidingnumericalresults. Formakingthebookavailableaspartoftheseries“GraduateTextsinPhysics”, and for support during the production stage I would like to thank Claus Ascheron andhisteamfromSpringerVerlag. Dresden,Germany FrankGrossmann March2013 vii Preface to the First Edition The development of modern pulsed lasers with power densities larger than 1016 W/cm2 andwithveryshortpulsedurationinthefemtosecondregimeenables experimentaliststostudyelementaryprocessessuchaschemicalreactionsandex- citation mechanisms in different areas in physics in the time domain. In parallel totheexperimentalinvestigations,analyticalandnumericalstudiesoflaserdriven atomsandmoleculeswitha limitednumberofdegreesoffreedomareperformed. Thesetheoreticalinvestigationshaveledtothepredictionand/ortheexplanationof a large variety of partly counter-intuitive phenomena. Among those are the gener- ation of high harmonics using laser excited atoms or molecules, the ionization of atomsabovethecontinuumthreshold,thestabilizationofatomsagainstionization inverystrongfields,counter-intuitivepulsesequencestoselectivelypopulatevibra- tional states in molecules and, last but not least, the control of chemical reactions byspeciallytailoredlaserpulses. This book originated out of a course, that I have given on a regular basis since 2000 for advanced undergraduate and graduate students at Technische Universität Dresden.Itoffersatheoreticallyorientedapproachtothefieldoflaserdrivenatomic and molecular systems and requires some knowledge of basic classical and quan- tum mechanics courses as well as of classical electrodynamics. The book has two introductorychaptersinPartIthatpavethewayfortheapplicationsinPartII.PartI andalsoChap.3ofPartIIcontainaselectionoftextbookmaterialthatisneededto understand the rest of the book. The material presented in the last two chapters is closetotherecentliterature.Ihavechosenonlysuchworks,however,thatdealwith fundamentalconceptsandarebasedonsimplemodelcalculations.Abiasedandin- completelistareferencesisgivenattheendofthechapters,precededbysomenotes andhintsforfurtherreading.Forthosereaderswhoareinterestedinsomecomputa- tionaldetails,thesearegivenintheappendicesattheendofthecorrespondingchap- ters.Furthermore,atseveralplacesthroughoutthetext,exercisesareplaced,whose independentsolutionallowsadeeperunderstandingofthematerialpresented. InChap.1,westartwithashortintroductionintothefoundationsofthelaser.We willespeciallyconcentrateonthoseaspectsofpulsedlasersthatwillbeimportant forthetheoreticalinvestigationsinPartIIofthebook. ix x PrefacetotheFirstEdition The next fundamental chapter is devoted to the non-relativistic time-dependent Schrödinger equation. In the case of lasers of up to atomic field strengths, this equation allows the theoretical description of the phenomena we want to investi- gateinPartII.Analyticalaswellasnumericalmethodstosolvethetime-dependent Schrödinger equation are thus in the focus of Chap.2. Throughout the whole pre- sentation,inordertokeeptheapproachassimpleaspossible,wetouchthetopicof correlatedmanyparticledynamicsonlywherenecessaryandconcentrateonthede- scriptionofelectronicaswellasnucleardynamicswiththehelpofmodelswithas fewdegreesoffreedomaspossible.ThecontentsandthepresentationofChap.2are inspiredbytheexcellentnewtextbookbyDavidTannor,IntroductiontoQuantum Mechanics: A Time-Dependent Perspective, which hopefully will start a “revolu- tion”inthewayquantummechanicsistaughtinthefuture. Thesecondpartofthebook,startingwithChap.3,containsacollectionofequiv- alentwaystocouplea chargedparticletoaclassicalelectromagneticfield.As the basic postulate we use the principle of minimal coupling. By using unitary trans- formations,onecantheneitherderivethelengthformortheKramers-Henneberger form of the coupling. As first examples of laser-matter interaction, we study the dynamicsof(structure-less)two-levelsystemsinlaserfields.PhenomenalikeRabi oscillations of the occupation probability, occurring there, will be encountered off an on in the remainder of the book. Furthermore, also the fundamental so-called rotatingwaveapproximationwillbediscussedforthefirsttimeinthiscontext. Selectedexamplesoflaser-matterinteractioninatomicphysicsarereviewedin Chap.4.Here,weconcentrateonthephenomenaofionizationandhighharmonic generationofasingleelectroninaCoulombpotentialofpossiblyreduceddimen- sionality.Itturnsoutthataperturbationtheoreticapproachwouldnotbesuitedto understand most of the phenomena presented in this chapter. Thus the numerical wavepacketmethodsthatwereinthefocusof Chap.2willfindtheirfirstapplica- tion. The next step in the direction of higher complexity of the dynamics will be takeninChap.5.Herewedealwithlaser-drivensystemsinmolecularandchemical + physics. The simplest molecule, the hydrogen molecular ion, H , will serve as a 2 vehicletounderstandsomeofthebasicconceptsofmolecularphysicssuchaselec- tronicpotentialsurfaces.Inthefollowing,thefullnumericalsolutionofthecoupled + electron nuclear problem of H in a monochromatic laser field will be reviewed. 2 AfterdiscussingthefundamentalBorn-Oppenheimerapproximation,fortherestof thechapter,wethenassumethatthesolutionoftheelectronicmanybodyproblem isatourdisposalintheformofanalyticallyornumericallygivenpotentialenergy surfaces.Afterashortdigressiononnuclearmotiononasingleelectronicsurface, andthediscussionofasimpletwocoupledsurfacesproblem,wethenreviewsome modernapplicationsinthefieldsoffemtosecondspectroscopy,optimalcontrolthe- ory,andquantuminformationprocessingundertheforegoingassumption. AtthispointIthankthestudentsatTUDresdenwhohaveattendedmylectures. Theyhaveinspiredmeenormously,throughtheirintensecollaboration,duringthe lectures, as well as during the exercise classes. This has motivated me to rethink PrefacetotheFirstEdition xi thematerialpresentedagainandagainandthestudentshavethuscontributedsub- stantially to the improvement of the manuscript. Also the hospitality of the Max- Planck-InstituteforthePhysicsofComplexSystems,thatofferedmetheopportu- nitytoattendandrunseveralconferencesinthefieldwasveryimportanttoshape myunderstandingpresentedhere.Furthermore,IexpressmydeepgratitudetoJan- MichaelRostandRüdigerSchmidtfortheircontinuousavailabilityfordiscussions andforlong-termcollaboration.Moreover,IamgratefultoPeterHänggiforthein- troductiontothefieldofdrivenquantumsystemsduringmyPh.D.workwithhim, andtoEricHellerforopeningtheworldoftime-dependentsemiclassicstome.In addition,I have benefittedfrom uncountablediscussions with and valuable advice offormermembersoftheTheoreticalQuantumDynamicsGroupinFreiburg,espe- ciallyGernotAlber,RichardDehnen,VolkerEngel,ChristophMeier,Gerdvande Sand, and Gerhard Stock. Furthermore, former and present members of the Theo- reticalAtomicandMolecularPhysicsGroupattheInstituteofTheoreticalPhysics ofTUDresdenandtheFiniteSystemsDepartmentattheMPIPKSinDresdenhave helped shape my understanding. Among many others these are Andreas Becker, AgapiEmmanouilidou,CelalHarabati,AnatoleKenfack,ThomasKunert,UlfSaal- mann, and Mathias Uhlmann. For helping me by answering specific questions or supplyinginformationandvaluablegraphs,IwouldliketothankWolfgangSchle- ich,JanWerschnik,MatthiasWollenhauptandShuheiYoshida.Foradviceandhelp withrespecttographicsissues,IthankArndBäckerandWernerKoch.Finally,Iam indebtedtoDavidTannor,whosuppliedmewithpreliminaryversionsofhisbook ataveryearlystageandthushelpedshapethepresentationheretoasubstantialde- gree.ThefocusofDavid’sbookonatime-dependentviewofquantumphenomena isanabsolutenecessityifonewantstostudylaser-drivensystems. Dresden,Germany FrankGrossmann May2008