Structural Glasses and Supercooled Liquids: Theory, Experiment, and Applications PDF
Preview Structural Glasses and Supercooled Liquids: Theory, Experiment, and Applications
STRUCTURAL GLASSES AND SUPERCOOLED LIQUIDS STRUCTURAL GLASSES AND SUPERCOOLED LIQUIDS Theory, Experiment, and Applications Editedby PETERG.WOLYNES VASSILIYLUBCHENKO Copyright©2012byJohnWiley&Sons,Inc.Allrightsreserved PublishedbyJohnWiley&Sons,Inc.,Hoboken,NewJersey PublishedsimultaneouslyinCanada Nopartofthispublicationmaybereproduced,storedinaretrievalsystem,ortransmittedinanyformor byanymeans,electronic,mechanical,photocopying,recording,scanning,orotherwise,exceptas permittedunderSection107or108ofthe1976UnitedStatesCopyrightAct,withouteithertheprior writtenpermissionofthePublisher,orauthorizationthroughpaymentoftheappropriateper-copyfeeto theCopyrightClearanceCenter,Inc.,222RosewoodDrive,Danvers,MA01923,(978)750-8400,fax (978)750-4470,oronthewebatwww.copyright.com.RequeststothePublisherforpermissionshould beaddressedtothePermissionsDepartment,JohnWiley&Sons,Inc.,111RiverStreet,Hoboken,NJ 07030,(201)748-6011,fax(201)748-6008,oronlineathttp://www.wiley.com/go/permission. 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TA450.S8862012 620.1’44–dc23 2011045245 PrintedintheUnitedStatesofAmerica ISBN:9780470452233 10 9 8 7 6 5 4 3 2 1 CONTENTS Preface vii Contributors xi 1 SupercooledLiquidDynamics:AdvancesandChallenges 1 RankoRichert 2 TheRandomFirst-OrderTransitionTheoryofGlasses: ACriticalAssessment 31 GiulioBiroliandJean-PhilippeBouchaud 3 DielectricSpectroscopyofGlassyDynamics 115 P.Lunkenheimer,M.Ko¨hler,S.Kastner,andA.Loidl 4 GlassesandReplicas 151 MarcMe´zardandGiorgioParisi 5 GlassinessinUniformlyFrustratedSystems 193 M.Dzero,J.Schmalian,andPeterG.Wolynes 6 RandomFirst-OrderPhaseTransitionTheoryoftheStructural GlassTransition 223 T.R.KirkpatrickandD.Thirumalai 7 FragileGlassFormers:EvidenceforaNewParadigm,andaNew RelationtoStrongLiquids 237 C.AustenAngell v vi CONTENTS 8 DynamicsintheCrossoverRegionofSupercooledLiquids 279 BimanBagchi 9 GlassyDynamicsofProteins 319 GuoChen,P.W.Fenimore,andHansFrauenfelder 10 TheoriesofStructuralGlassDynamics:Mosaics,Jamming, andAllThat 341 VassiliyLubchenkoandPeterG.Wolynes Index 381 PREFACE However,duringthereignofTiberiusCaesar,acertainartisaninventedhowtotemper glasstomakeitflexibleandductile.WhenreceivedbytheCaesar,theartisanhandeda vasetotheCaesarwho,inindignantdisbelief,threwthevaseonthefloor.Theartisan howeverpickedupthevase,whichhaddeformedasthoughmadeofbronze,andthen straighteneditusingasmallhammer.Uponthis,theCaesaraskedtheartisan:“Does anyone else know how this property of glass is achieved?” After a negative answer, theCaesarorderedtheartisanbeheaded,lestthispropertybecameknown,goldwas treatedasdirt,andallmetalsweredevalued.Conversely,ifglassvasesdidnotbreak, theywouldbebetterthangoldandsilver.1 FromSt.IsidoreofSeville(c.560-636)Etymologies,BookXVI,“StonesandMetals.” Glassesarefascinatingbecausetheydefyourintuitiveassociationbetweenstability and uniqueness. While crystals, which possess no structurally distinct low-energy configurations,areeternallystable,agivenstructurethatappearsstableagainstper- turbation neither needs to be periodic nor unique. Often very stable mechanically, glassesareactuallyhighlydegeneratesolidswhosefluidityisacontinuousfunction oftemperature,incontrastwithperiodiccrystalswhichmeltdiscontinuously. 1The Latin original (as can be found at http://www.thelatinlibrary.com/isidore/16.shtml) reads: Ferunt autemsubTiberioCaesarequendamartificemexcogitassevitritemperamentum,utflexibileessetetductile. QuidumadmissusfuissetadCaesarem,porrexitphialamCaesari,quamilleindignatusinpavimentum proiecit.Artifexautemsustulitphialamdepavimento,quaeconplicaveratsetamquamvasaeneum;deinde marculumdesinuprotulitetphialamcorrexit.HocfactoCaesardixitartifici:’Numquidaliusscithanc condituramvitrorum?’Postquamilleiuransnegavitalterumhocscire,iussitillumCaesardecollari,ne dumhoccognitumfieret,aurumprolutohabereturetomniummetallorumpretiaabstraherentur;etrevera, quiasivasavitreanonfrangerentur,meliusessentquamaurumetargentum. vii viii PREFACE The answer to this seeming contradiction is simple: Since stability is usually requirednotoninfinite,butonlyonfinitetimescales,sufficientlystablestatesneednot strictlybeunique,butonlysufficientlyrare.Thisinherent,directconnectionbetween kinetics and thermodynamics of the glass transition was advocated already in the 1950s, preceded by the insightful work of Simon, Kauzmann, and Bernal, among others. Fleshing out these ideas quantitatively has, however, proved to be difficult. One problem is that standard thermodynamics at the macroscopic scale becomes strictly valid only at infinite time, and is thus not rigorously applicable to glasses, which are only metastable. Ergodicity breaking, which haunted the very father of statisticalmechanicsLudwigBoltzmann,isrealizedwithvengeanceinglasses.On the other hand, kinetic treatments at the molecular scale that work well in conven- tionalfluidsbecomequicklyboggeddownbycooperativeeffectsarisingathighliquid densities. Atremendousamountofprogressinmeetingthesechallengeshasbeenmadeover thepastdecades.Experimentaltoolstocharacterizequantitativelyboththekineticand thermodynamicpeculiaritiesinglassformersarewidespread.Microscopicimaging and single-molecule techniques to directly determine the spatial extent of cooper- ativity preceding the glass transition have recently been developed, thus providing stricttestsfortheoreticaldescriptions.Manynovelvitreouscompoundswithunique propertieshavebeenmanufactured.Wehavelearnedthatglassesareindeeddifferent from their periodic counterparts both with regard to their bulk properties and local motions,bothnuclearandelectronic.Forinstance,itisasafebetthatthereaderofthis volume presently uses optical drives that exploit the unique optoelectronic anoma- liesofchalcogenideglasses.Ontheotherhand,manyseeminglydisparatephysical systems,suchasproteinsandtheirassembliesinprotoplasm,showsignaturesofthe glasstransition. Paralleling experimental developments, much progress has been achieved in theoretical understanding of both the thermodynamics and the kinetics of the glass transition. The mathematics behind the mechanism connecting the decrease in the densityofstatesandtheviscousslowdown,whichprecedetheglasstransition,has beenwell-developed.Manybeautifulconnectionshavebeenuncoveredbetweenthe physicsofsupercooledliquidsandoptimizationproblemsincomputerscience,social science, and economics. Theoretical tools to describe ergodicity breaking in glass- formers have been developed. The arsenal from liquid-state theory is continuously growing, suggesting the ability to predict the structure and glassforming ability of specificsubstancesisinnearsight. Theaimofthepresentvolumeistobringthereaderseveralmodernviewsofthe glass transition and relaxations in glassy systems, from leading practitioners in the field,bothfromatheoreticalandexperimentalperspective.Bothancientandrecent attempts to categorize the structural glass transition or create new glassy materials seem to have involved some risk. Nor have these attempts been without irony: Reaching an agreement on what would really constitute a microscopic theory of theglasstransitionappearstobesubjecttoaviscousdragnotunlikethatpreceding the physical glass transition itself. We hope the present volume will help ease this PREFACE ix perception of there being an intellectual logjam and allow more scientists to see throughglassclearly. PeterG.Wolynes VassiliyLubchenko CONTRIBUTORS C. Austen Angell, Department of Chemistry and Biochemistry, Arizona State University,Tempe,AZ,USA Biman Bagchi, Solid State and Structural Chemistry Unit, Indian Institute of Science,Bangalore,India GiulioBiroli, InstitutdePhysiqueThéorique(IPhT),CEA,andCNRSURA2306, Gif-sur-Yvette,France Jean-Philippe Bouchaud, (1) Science and Finance, Capital Fund Management, Paris,Franceand(2)E´colePolytechnique,Palaiseau,France GuoChen, (1)TheoreticalDivision,LosAlamosNationalLaboratory,LosAlamos, NM,USAand(2)DepartmentofAppliedPhysics,ChalmersUniversityofTech- nology,Göteborg,Sweden MaximDzero, DepartmentofPhysics,KentStateUniversity,Kent,OH,USA Paul W. Fenimore, Theoretical Division, Los Alamos National Laboratory, Los Alamos,NM,USA Hans Frauenfelder, Theoretical Division, Los Alamos National Laboratory, LosAlamos,NM,USA Stefan Kastner, Experimental Physics V, Center for Electronic Correlations and Magnetism,UniversityofAugsburg,Augsburg,Germany Theodore R. Kirkpatrick, Institute for Physical Sciences and Technology and DepartmentofPhysics,UniversityofMaryland,CollegePark,MD,USA xi xii CONTRIBUTORS Melanie Köhler, Experimental Physics V, Center for Electronic Correlations and Magnetism,UniversityofAugsburg,Augsburg,Germany AloisLoidl, ExperimentalPhysicsV,CenterforElectronicCorrelationsandMag- netism,UniversityofAugsburg,Augsburg,Germany VassiliyLubchenko, DepartmentsofChemistryandPhysics,UniversityofHouston, Houston,TX,USA PeterLunkenheimer, ExperimentalPhysicsV,CenterforElectronicCorrelations andMagnetism,UniversityofAugsburg,Augsburg,Germany MarcMézard, LaboratoiredePhysiqueThéoriqueetModelesStatistiques,Univer- sitédeParisSud—CNRS,Orsay,France Giorgio Parisi, Dipartimento di Fisica, Università di Roma “La Sapienza” Rome, Italy RankoRichert, DepartmentofChemistryandBiochemistry,ArizonaStateUniver- sity,Tempe,AZ,USA Jörg Schmalian, Institute for Theory of Condensed Matter, Karlsruhe Institute of Technology,Karlsruhe,Germany DevarajanThirumalai, InstituteforPhysicalSciencesandTechnologyandDepart- ment of Chemistry and Biochemistry, University of Maryland, College Park, MD,USA PeterG.Wolynes, DepartmentofChemistryandCenterforTheoreticalBiological Physics,RiceUniversity,Houston,TX,USA
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