A Thermodynamic Perspective on Polymer Glass Formation

Wen-Sheng Xu; Zhao-Yan Sun

doi:10.1007/s10118-023-2951-1

Your Location：

Home >

Browse articles >

A Thermodynamic Perspective on Polymer Glass Formation

PERSPECTIVE | Updated：2023-08-24

- A Thermodynamic Perspective on Polymer Glass Formation
- Chinese Journal of Polymer Science Vol. 41, Issue 9, Pages: 1329-1341(2023)
- Affiliations：
  
  1.State Key Laboratory of Polymer Physics and Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China
- Author bio：
  
  [ "Wen-Sheng Xu received his Ph.D. degree from Changchun Institute of Applied Chemistry, Chinese Academy of Sciences in 2012. From 2013 to 2018, he was a postdoctoral scholar first with Professor Karl F. Freed at the University of Chicago and then with Dr. Yangyang Wang at Oak Ridge National Laboratory. He is currently a professor in the State Key Laboratory of Polymer Physics and Chemistry at Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, where he has been a faculty member since 2019. His research group utilizes theoretical methods and computer simulations to investigate the dynamics of noncrystalline polymer materials\t\t\t\t\t\t" ]
  [ "Zhao-Yan Sun received her Ph.D. degree from Jilin University in 2001. She was a postdoctoral fellow at University of Dortmund from 2001 to 2002. Since 2003, she has been a faculty member in the State Key Laboratory of Polymer Physics and Chemistry at Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, initially as an assistant professor and then an associate professor, before becoming a full professor in 2010. She was awarded the Young Chemistry Award of the Chinese Chemical Society in 2005. Her research group focuses on the structure and dynamics of polymers and nanocomposites and the development of computer simulation methods\t\t\t\t\t\t" ]
- Funds：
- DOI：10.1007/s10118-023-2951-1
  CLC：
Scan for full text
Wen-Sheng Xu, Zhao-Yan Sun. A Thermodynamic Perspective on Polymer Glass Formation. [J]. Chinese Journal of Polymer Science 41(9):1329-1341(2023)
DOI：

Wen-Sheng Xu, Zhao-Yan Sun. A Thermodynamic Perspective on Polymer Glass Formation. [J]. Chinese Journal of Polymer Science 41(9):1329-1341(2023) DOI： 10.1007/s10118-023-2951-1.

摘要

The present paper provides an overview of the thermodynamic models of glass formation, with an emphasis on the advances that attempt to bring together some of the seemingly disparate thermodynamic viewpoints on glass formation.

Abstract

The dynamics of polymeric and other glass-forming liquids dramatically slows down upon cooling toward the glass transition temperature without any obvious significant change in their static structure. A quantitative understanding of this extraordinary dynamic slowdown remains one of the most significant challenges in condensed matter physics. Historically, extensive efforts have been devoted to explaining the dynamics of glass-forming liquids in terms of thermodynamic properties, leading to a number of semi-empirical models emphasizing distinct thermodynamic properties. Here, a thermodynamic perspective is provided on the glass formation of polymeric and other materials. We begin with an overview of the thermodynamic models of glass formation, including the intuitively appealing “free volume” models, enthalpy models originally emphasized by Goldstein and later by others, and the highly influential configurational entropy-based models. The review of these models is followed by a discussion of the advances that attempt to bring together some of the seemingly disparate thermodynamic viewpoints on glass formation by revealing a close interrelation between thermodynamic properties. We conclude this review with remarks on several key topics in this field, along with our viewpoint for future work.

关键词

Keywords

Glass formationEntropyFree volumeEnthalpy

references

Debenedetti,P.G.;Stillinger,F.H.Supercooledliquidsandtheglasstransition.Nature2001,410,259−267..

Ediger,M.D.;Angell,C.A.;Nagel,S.R.Supercooledliquidsandglasses.J. Phys. Chem.1996,100,13200−13212..

Berthier,L.;Biroli,G.Theoreticalperspectiveontheglasstransitionandamorphousmaterials.Rev. Mod. Phys.2011,83,587−645..

Ediger,M.D.;Harrowell,P.Perspective:supercooledliquidsandglasses.J. Chem. Phys.2012,137,080901..

Biroli,G.;Garrahan,J.P.Perspective:theglasstransition.J. Chem. Phys.2013,138,12A301..

Debenedetti,P.G.;Stillinger,F.H.Glasstransitionthermodynamicsandkinetics.Annu. Rev. Condens. Matter Phys.2013,4,263−285..

Parry,B.;Surovtsev,I.;Cabeen,M.;O’Hern,C.;Dufresne,E.;Jacobs-Wagner,C.Thebacterialcytoplasmhasglass-likepropertiesandisfluidizedbymetabolicactivity.Cell2014,156,183−194..

Roos,Y.H.Glasstransitiontemperatureanditsrelevanceinfoodprocessing.Annu. Rev. Food Sci. Technol.2010,1,469−496..

Xu,Z.;Dai,X.;Bu,X.;Yang,Y.;Zhang,X.;Man,X.;Zhang,X.;Doi,M.;Yan,L.T.Enhancedheterogeneousdiffusionofnanoparticlesinsemiflexiblenetworks.ACS Nano2021,15,4608−4616..

Dai,X.;Zhang,X.;Gao,L.;Xu,Z.;Yan,L.T.Topologymediatestransportofnanoparticlesinmacromolecularnetworks.Nat. Commun.2022,13,4094..

Dai,X.;Zhu,Z.;Li,Y.;Yang,B.;Xu,J.F.;Dong,Y.;Zhou,X.;Yan,L.-T.;Liu,D.“Shutter”effectsenhanceproteindiffusionindynamicandrigidmolecularnetworks.J. Am. Chem. Soc.2022,144,19017−19025..

DiMarzio,E.A.Equilibriumtheoryofglasses.Ann. N. Y. Acad. Sci.1981,371,1−20..

Smallenburg,F.;Sciortino,F.Liquidsmorestablethancrystalsinparticleswithlimitedvalenceandflexiblebonds.Nat. Phys.2013,9,554−558..

Zhang,G.;Stillinger,F.H.;Torquato,S.Theperfectglassparadigm:disorderedhyperuniformglassesdowntoabsoluteZero.Sci. Rep.2016,6,36963..

Ingebrigtsen,T.S.;Dyre,J.C.;Schrøder,T.B.;Royall,C.P.Crystallizationinstabilityinglass-formingmixtures.Phys. Rev. X2019,9,031016..

Roland,C.M.;Hensel-Bielowka,S.;Paluch,M.;Casalini,R.Supercooleddynamicsofglass-formingliquidsandpolymersunderhydrostaticpressure.Rep. Prog. Phys.2005,68,1405−1478..

Roland,C.M.Relaxationphenomenainvitrifyingpolymersandmolecularliquids.Macromolecules2010,43,7875−7890..

Cangialosi,D.Dynamicsandthermodynamicsofpolymerglasses.J. Phys.: Condens. Matter2014,26,153101..

Napolitano,S.;Glynos,E.;Tito,N.B.Glasstransitionofpolymersinbulk,confinedgeometries,andnearinterfaces.Rep. Prog. Phys.2017,80,036602..

McKenna,G.B.;Simon,S.L.50thAnniversaryperspective:challengesinthedynamicsandkineticsofglass-formingPolymers.Macromolecules2017,50,6333−6361..

Dudowicz,J.;Freed,K.F.;Douglas,J.F.Generalizedentropytheoryofpolymerglassformation.Adv. Chem. Phys.2008,137,125−222..

Xu,W.-S.;Douglas,J.F.;Sun,Z.Y.Polymerglassformation:roleofactivationfreeenergy,configurationalentropy,andcollectivemotion.Macromolecules2021,54,3001−3033..

Götze,W.inComplex Dynamics of Glass-Forming Liquids: A Mode-Coupling Theory.OxfordUniversityPress,Oxford,2008..

PazmiñoBetancourt,B.A.;Hanakata,P.Z.;Starr,F.W.;Douglas,J.F.Quantitativerelationsbetweencooperativemotion,emergentelasticity,andfreevolumeinmodelglass-formingpolymermaterials.Proc. Natl. Acad. Sci. U. S. A.2015,112,2966−2971..

Goldstein,M.Somethermodynamicaspectsoftheglasstransition:freevolume,entropy,andenthalpytheories.J. Chem. Phys.1963,39,3369−3374..

Caruthers,J.M.;Medvedev,G.A.Quantitativemodelofsuper-Arrhenianbehavioringlassformingmaterials.Phys. Rev. Materials2018,2,055604..

Medvedev,G.A.;Caruthers,J.M.Aquantitativemodelofsuper-Arrhenianbehavioringlass-formingpolymers.Macromolecules2019,52,1424−1439..

Zhao,X.;Simon,S.L.Amodel-freeanalysisofconfigurationalpropertiestoreducethetemperature-andpressure-dependentsegmentalrelaxationtimesofpolymers.J. Chem. Phys.2020,152,044901..

Kauzmann,W.Thenatureoftheglassystateandthebehaviorofliquidsatlowtemperatures.Chem. Rev.1948,43,219−256..

Xu,X.;Douglas,J.F.;Xu,W.S.Thermodynamic–dynamicinterrelationsinglass-formingpolymerfluids.Macromolecules2022,55,8699−8722..

Lucretius,InGreat Books of the Western World.Hutchins,R.M.,Ed.;EncyclopaediaBritannica,Inc.:Chicago,1952;BookI..

Robertson,R.E.Theoryfortheplasticityofglassypolymers.J. Chem. Phys.1966,44,3950−3956..

Batschinski,A.J.UntersuchungenüberdieinnereReibungderFlüssigkeiten.Z. Phys. Chem.1913,84U,643−706..

Hildebrand,J.H.inViscosity and Diffusivity: A Predictive Treatment.Wiley,NewYork,1977..

Hildebrand,J.H.;Lamoreaux,R.H.Fluidity:ageneraltheory.Proc. Natl. Acad. Sci. U. S. A.1972,69,3428−3431..

Doolittle,A.K.StudiesinNewtonianflow.I.Thedependenceoftheviscosityofliquidsontemperature.J. Appl. Phys.1951,22,1031−1035..

FoxJr.,T.G.;Flory,P.J.Second-ordertransitiontemperaturesandrelatedpropertiesofpolystyrene.I.Influenceofmolecularweight.J. Appl. Phys.1950,21,581−591..

Vogel,H.Thelawoftherelationshipbetweenviscosityofliquidsandthetemperature.Phys. Z.1921,22,645−646..

Fulcher,G.S.Analysisofrecentmeasurementsoftheviscosityofglasses.J. Am. Ceram. Soc.1925,8,339−355..

Tammann,G.;Hesse,W.DieAbhängigkeitderviscositätvondertemperaturbieunterkühltenflüssigkeiten.Z. Anorg. Allg. Chem.1926,156,245−257..

Ferry,J.D.inViscoelastic Properties of Polymers.Wiley,NewYork,1980..

Williams,M.L.;Landel,R.F.;Ferry,J.D.Thetemperaturedependenceofrelaxationmechanismsinamorphouspolymersandotherglass-formingliquids.J. Am. Chem. Soc.1955,77,3701−3707..

White,R.P.;Lipson,J.E.G.Polymerfreevolumeanditsconnectiontotheglasstransition.Macromolecules2016,49,3987−4007..

White,R.P.;Lipson,J.E.G.ExplainingtheT,V-dependentdynamicsofglassformingliquids:Thecooperativefreevolumemodeltestedagainstnewsimulationresults.J. Chem. Phys.2017,147,184503..

White,R.P.;Lipson,J.E.G.Pressure-dependentdynamicsofpolymermeltsfromArrheniustonon-Arrhenius:thecooperativefreevolumerateequationtestedagainstsimulationdata.Macromolecules2018,51,4896−4909..

White,R.P.;Lipson,J.E.G.Connectingpressure-dependentdynamicstodynamicsunderconfinement:thecooperativefreevolumemodelappliedtopoly(4-chlorostyrene)bulkandthinfilms.Macromolecules2018,51,7924−7941..

Debot,A.;White,R.P.;Lipson,J.E.G.;Napolitano,S.Experimentaltestofthecooperativefreevolumeratemodelunder1Dconfinement:theinterplayoffreevolume,temperature,andpolymerfilmthicknessindrivingsegmentalmobility.ACS Macro Lett.2019,8,41−45..

Xu,W.S.;Douglas,J.F.;Xia,W.;Xu,X.Understandingactivationvolumeinglass-formingpolymermeltsviageneralizedentropytheory.Macromolecules2020,53,7239−7252..

Xu,W.S.;Douglas,J.F.;Freed,K.F.Entropytheoryofpolymerglass-formationinvariablespatialdimension.Adv. Chem. Phys.2016,161,443−497..

Xu,W.-S.;Douglas,J.F.;Xu,X.Roleofcohesiveenergyinglassformationofpolymerswithandwithoutbendingconstraints.Macromolecules2020,53,9678−9697..

Floudas,G.;Paluch,M.;Grzybowski,A.;Ngai,K.L.inMolecular Dynamics of Glass-Forming Systems: Effects of Pressure.1stEd.;Springer-Verlag:Berlin,2010..

Sanchez,I.C.Dimensionlessthermodynamics:anewparadigmforliquidstateproperties.J. Phys. Chem. B2014,118,9386−9397..

Simha,R.;Boyer,R.F.Onageneralrelationinvolvingtheglasstemperatureandcoefficientsofexpansionofpolymers.J. Chem. Phys.1962,37,1003−1007..

Foreman,K.W.;Freed,K.F.Latticeclustertheoryofmulticomponentpolymersystems:chainsemiflexibilityandspecificinteractions.Adv. Chem. Phys.1998,103,335−390..

Xu,W.S.;Freed,K.F.Latticeclustertheoryforpolymermeltswithspecificinteractions.J. Chem. Phys.2014,141,044909..

Adam,G.;Gibbs,J.H.OnthetemperaturedependenceofcooperativerelaxationPropertiesinglass-formingLiquids.J. Chem. Phys.1965,43,139−146..

Stukalin,E.B.;Douglas,J.F.;Freed,K.F.Applicationoftheentropytheoryofglassformationtopoly(α-olefins).J. Chem. Phys.2009,131,114905..

Yang,Z.;Xu,X.;Xu,W.S.Influenceofionicinteractionstrengthonglassformationofanion-containingpolymermelt.Macromolecules2021,54,9587−9601..

Starr,F.W.;Sastry,S.;Douglas,J.F.;Glotzer,S.C.Whatdowelearnfromthelocalgeometryofglass-formingliquids?Phys. Rev. Lett.2002,89,125501..

Hanakata,P.Z.;Douglas,J.F.;Starr,F.W.Localvariationoffragilityandglasstransitiontemperatureofultra-thinsupportedpolymerfilms.J. Chem. Phys.2012,137,244901..

Zhang,W.;Starr,F.W.;Douglas,J.F.Reconcilingcomputationalandexperimentaltrendsinthetemperaturedependenceoftheinterfacialmobilityofpolymerfilms.J. Chem. Phys.2020,152,124703..

Douglas,J.F.;PazminoBetancourt,B.A.;Tong,X.;Zhang,H.Localizationmodeldescriptionofdiffusionandstructuralrelaxationinglass-formingCu-Zralloys.J. Stat. Mech.: Theory Exp.2016,054048,.

Zhang,H.;Wang,X.;Douglas,J.F.LocalizationmodeldescriptionofdiffusionandstructuralrelaxationinsuperioniccrystallineUO2.J. Chem. Phys.2019,151,071101..

Simmons,D.S.;Cicerone,M.T.;Zhong,Q.;Tyagi,M.;Douglas,J.F.Generalizedlocalizationmodelofrelaxationinglass-formingliquids.Soft Matter2012,8,11455−11461..

Sutherland,W.XXXVI.Anewperiodicpropertyoftheelements.London, Edinburgh Dublin Philos. Mag. J. Sci.1890,30,318−323..

Sutherland,W.V.Akinetictheoryofsolids,withanExperimentalIntroduction.London, Edinburgh Dublin Philos. Mag. J. Sci.1891,32,31−43..

Sutherland,W.XXIX.Akinetictheoryofsolids,withanexperimentalintroduction.London, Edinburgh Dublin Philos. Mag. J. Sci.1891,32,215−225..

Sutherland,W.LXIII.Akinetictheoryofsolids,withanexperimentalintroduction.London, Edinburgh Dublin Philos. Mag. J. Sci.1891,32,524−553..

Larini,L.;Ottochian,A.;DeMichele,C.;Leporini,D.Universalscalingbetweenstructuralrelaxationandvibrationaldynamicsinglass-formingliquidsandpolymers.Nat. Phys.2008,4,42−45..

Davies,R.O.;Jones,G.O.Theirreversibleapproachtoequilibriuminglasses.Proc. R. Soc. A1953,217,26−42..

Goldstein,M.Onthetemperaturedependenceofcooperativerelaxationpropertiesinglass-formingliquids—commentonapaperbyAdamandGibbs.J. Chem. Phys.1965,43,1852−1853..

Simon,F.ÜberdenZustandderunterkühltenFlüssigkeitenundGläser.Z. Anorg. Allg. Chem.1931,203,219−227..

Berthier,L.;Ozawa,M.;Scalliet,C.Configurationalentropyofglass-formingliquids.J. Chem. Phys.2019,150,160902..

Gibbs,J.H.;DiMarzio,E.A.Natureoftheglasstransitionandtheglassystate.J. Chem. Phys.1958,28,373−383..

Flory,P.J.Statisticalthermodynamicsofsemi-flexiblechainmolecules.Proc. R. Soc. Lond. A1956,234,60−73..

DiMarzio,E.A.;Yang,A.J.M.Configurationalentropyapproachtothekineticsofglasses.J. Res. Natl. Inst. Stand. Technol.1997,102,135−157..

Bestul,A.B.;Chang,S.S.Excessentropyatglasstransformation.J. Chem. Phys.1964,40,3731−3733..

Glasstone,S.;Laidler,K.J.;Eyring,H.inThe Theory of Rate Processes: The Kinetics of Chemical Reactions, Viscosity, Diffusion and Electrochemical Phenomena.InternationalChemicalSeries;McGraw-HillBookCompany:Incorporated,1941..

Kauzmann,W.;Eyring,H.TheViscousflowoflargemolecules.J. Am. Chem. Soc.1940,62,3113−3125..

Kincaid,J.F.;Eyring,H.;Stearn,A.E.Thetheoryofabsolutereactionratesanditsapplicationtoviscosityanddiffusionintheliquidstate.Chem. Rev.1941,28,301−365..

Goldstein,M.Viscousliquidsandtheglasstransition:apotentialenergybarrierpicture.J. Chem. Phys.1969,51,3728−3739..

Stillinger,F.H.;Weber,T.A.Hiddenstructureinliquids.Phys. Rev. A1982,25,978−989..

Stillinger,F.H.;Weber,T.A.Packingstructuresandtransitionsinliquidsandsolids.Science1984,225,983−989..

Xu,X.;Douglas,J.F.;Xu,W.S.Influenceofside-chainlengthandrelativerigiditiesofbackboneandsidechainsonglassformationofbranchedpolymers.Macromolecules2021,54,6327−6341..

Xu,X.;Xu,W.S.Meltpropertiesandstringmodeldescriptionofglassformationingraftpolymersofdifferentside-chainlengths.Macromolecules2022,55,3221−3235..

Xu,W.-S.;Douglas,J.F.;Freed,K.F.Generalizedentropytheoryofglass-formationinfullyflexiblepolymermelts.J Chem. Phys.2016,145,234509..

Chen,D.;McKenna,G.B.Deepglassystatedynamicdatachallengeglassmodels:configurationalentropymodels.J. Non-Cryst. Solids2021,566,120871..

Kirkpatrick,T.R.;Wolynes,P.G.Stableandmetastablestatesinmean-fieldPottsandstructuralglasses.Phys. Rev. B1987,36,8552−8564..

Kirkpatrick,T.R.;Thirumalai,D.;Wolynes,P.G.Scalingconceptsforthedynamicsofviscousliquidsnearanidealglassystate.Phys. Rev. A1989,40,1045−1054..

Bouchaud,J.P.;Biroli,G.OntheAdam-Gibbs-Kirkpatrick-Thirumalai-Wolynesscenariofortheviscosityincreaseinglasses.J. Chem. Phys.2004,121,7347−7354..

Lubchenko,V.;Wolynes,P.G.Theoryofstructuralglassesandsupercooledliquids.Annu. Rev. Phys. Chem.2007,58,235−266..

Rosenfeld,Y.Relationbetweenthetransportcoefficientsandtheinternalentropyofsimplesystems.Phys. Rev. A1977,15,2545−2549..

Rosenfeld,Y.Aquasi-universalscalinglawforatomictransportinsimplefluids.J. Phys.: Condens. Matter1999,11,5415−5427..

Dyre,J.C.Perspective:excess-entropyscaling.J. Chem. Phys.2018,149,210901..

Weeks,J.D.;Chandler,D.;Andersen,H.C.Roleofrepulsiveforcesindeterminingtheequilibriumstructureofsimpleliquids.J. Chem. Phys.1971,54,5237−5247..

Schweizer,K.S.;Saltzman,E.J.Theoryofdynamicbarriers,activatedhopping,andtheglasstransitioninpolymermelts.J. Chem. Phys.2004,121,1984−2000..

Saltzman,E.J.;Schweizer,K.S.Universalscaling,dynamicfragility,segmentalrelaxation,andvitrificationinpolymermelts.J. Chem. Phys.2004,121,2001−2009..

Chen,K.;Saltzman,E.J.;Schweizer,K.S.Moleculartheoriesofsegmentaldynamicsandmechanicalresponseindeeplysupercooledpolymermeltsandglasses.Annu. Rev. Condens. Matter Phys.2010,1,277−300..

Mirigian,S.;Schweizer,K.S.Elasticallycooperativeactivatedbarrierhoppingtheoryofrelaxationinviscousfluids.I.Generalformulationandapplicationtohardspherefluids.J. Chem. Phys.2014,140,194506..

Mirigian,S.;Schweizer,K.S.Elasticallycooperativeactivatedbarrierhoppingtheoryofrelaxationinviscousfluids.II.Thermalliquids.J. Chem. Phys.2014,140,194507..

Mirigian,S.;Schweizer,K.S.Dynamicaltheoryofsegmentalrelaxationandemergentelasticityinsupercooledpolymermelts.Macromolecules2015,48,1901−1913..

Xie,S.J.;Schweizer,K.S.NonuniversalcouplingofcagescaleHoppingandcollectiveelasticdistortionastheoriginofdynamicfragilitydiversityinglass-formingpolymerliquids.Macromolecules2016,49,9655−9664..

Varotsos,P.;Alexopoulos,K.Decisiveimportanceofthebulkmodulusandtheanharmonicityinthecalculationofmigrationandformationvolumes.Phys. Rev. B1981,24,904−910..

Varotsos,P.;Alexopoulos,K.Calculationofdiffusioncoefficientsatanytemperatureandpressurefromasinglemeasurement.I.Selfdiffusion.Phys. Rev. B1980,22,3130−3134..

Khonik,V.A.;Mitrofanov,Y.P.;Lyakhov,S.A.;Vasiliev,A.N.;Khonik,S.V.;Khoviv,D.A.RelationshipbetweentheshearmodulusG,activationenergy,andshearviscosityηinmetallicglassesbelowandaboveTg:directin situmeasurementsofGandη.Phys. Rev. B2009,79,132204..

Sjögren,L.Temperaturedependenceofviscosityneartheglasstransition.Z. Phys. B-Condensed Matter1990,79,5−13..

Dyre,J.C.Colloquium:Theglasstransitionandelasticmodelsofglass-formingliquids.Rev. Mod. Phys.2006,78,953−972..

Douglas,J.F.;Xu,W.S.Equationofstateandentropytheoryapproachtothermodynamicscalinginpolymericglass-formingliquids.Macromolecules2021,54,3247−3269..

Novikov,V.N.;Sokolov,A.P.Qualitativechangeinstructuraldynamicsofsomeglass-formingsystems.Phys. Rev. E2015,92,062304..

Angell,C.A.Relaxationinliquids,polymersandplasticcrystals-strong/fragilepatternsandproblems.J. Non-Cryst. Solids1991,131-133,13−31..

Angell,C.A.Formationofglassesfromliquidsandbiopolymers.Science1995,267,1924−1935..

Tanaka,H.Anewscenariooftheapparentfragile-to-strongtransitionintetrahedralliquids:waterasanexample.J. Phys.: Condens. Matter2003,15,L703..

Tanaka,H.Bondorientationalorderinliquids:towardsaunifieddescriptionofwater-likeanomalies,liquid-liquidtransition,glasstransition,andcrystallization.Eur. Phys. J. E2012,35,113..

Shi,R.;Russo,J.;Tanaka,H.Originoftheemergentfragile-to-strongtransitioninsupercooledwater.Proc. Natl. Acad. Sci. U. S. A.2018,115,9444−9449..

Zhang,C.;Hu,L.;Yue,Y.;Mauro,J.C.Fragile-to-strongtransitioninmetallicglass-formingliquids.J. Chem. Phys.2010,133,014508..

Zhang,H.;Wang,X.;Yu,H.B.;Douglas,J.F.Fastdynamicsinamodelmetallicglass-formingmaterial.J. Chem. Phys.2021,154,084505..

Zhang,H.;Wang,X.;Yu,H.B.;Douglas,J.F.Dynamicheterogeneity,cooperativemotion,andJohari-Goldsteinβ-relaxationinametallicglass-formingmaterialexhibitingafragile-to-strongtransition.Eur. Phys. J. E2021,44,56..

Schmidtke,B.;Petzold,N.;Kahlau,R.;Hofmann,M.;Rössler,E.A.Fromboilingpointtoglasstransitiontemperature:transportcoefficientsinmolecularliquidsfollowthree-parameterscaling.Phys. Rev. E2012,86,041507..

Schmidtke,B.;Petzold,N.;Kahlau,R.;;Rössler,E.A.Reorientationaldynamicsinmolecularliquidsasrevealedbydynamiclightscattering:fromboilingpointtoglasstransitiontemperature.J. Chem. Phys.2013,139,084504..

Schmidtke,B.;Hofmann,M.;Lichtinger,A.;Rössler,E.A.Temperaturedependenceofthesegmentalrelaxationtimeofpolymersrevisited.Macromolecules2015,48,3005−3013..

Johari,G.P.;Goldstein,M.Viscousliquidsandtheglasstransition.II.Secondaryrelaxationsinglassesofrigidmolecules.J. Chem. Phys.1970,53,2372−2388..

Johari,G.P.;Goldstein,M.Viscousliquidsandtheglasstransition.III.Secondaryrelaxationsinaliphaticalcoholsandothernonrigidmolecules.J. Chem. Phys.1971,55,4245−4252..

Johari,G.P.Intrinsicmobilityofmolecularglasses.J. Chem. Phys.1973,58,1766−1770..

Xu,W.S.;Douglas,J.F.;Freed,K.F.Influenceofcohesiveenergyonrelaxationinamodelglass-formingpolymermelt.Macromolecules2016,49,8355−8370..

Xu,W.S.;Douglas,J.F.;Freed,K.F.Influenceofpressureonglassformationinasimulatedpolymermelt.Macromolecules2017,50,2585−2598..

Xu,W.S.;Douglas,J.F.;Xu,X.Moleculardynamicsstudyofglassformationinpolymermeltswithvaryingchainstiffness.Macromolecules2020,53,4796−4809..

Wang,X.;Xu,W.-S.;Zhang,H.;Douglas,J.F.Universalnatureofdynamicheterogeneityinglass-formingliquids:acomparativestudyofmetallicandpolymericglass-formingliquids.J. Chem. Phys.2019,151,184503..

Singh,M.;Agarwal,M.;Dhabal,D.;Chakravarty,C.Structuralcorrelationsandcooperativedynamicsinsupercooledliquids.J. Chem. Phys.2012,137,024508..

Banerjee,A.;Sengupta,S.;Sastry,S.;Bhattacharyya,S.M.Roleofstructureandentropyindeterminingdifferencesindynamicsforglassformerswithdifferentinteractionpotentials.Phys. Rev. Lett.2014,113,225701..

Yang,Z.Y.;Nie,W.J.;Liu,L.Y.;Xu,X.L.;Xia,W.J.;Xu,W.S.Applicationsofmachinelearningmethodsinthestudiesofpolymerglassformation.Acta Polymerica Sinica(inChinese)2023,54,432−450..

Cubuk,E.D.;Schoenholz,S.S.;Rieser,J.M.;Malone,B.D.;Rottler,J.;Durian,D.J.;Kaxiras,E.;Liu,A.J.Identifyingstructuralflowdefectsindisorderedsolidsusingmachine-learningmethods.Phys. Rev. Lett.2015,114,108001..

Schoenholz,S.S.;Cubuk,E.D.;Sussman,D.M.;Kaxiras,E.;Liu,A.J.Astructuralapproachtorelaxationinglassyliquids.Nat. Phys.2016,12,469−471..

Cubuk,E.D.;Schoenholz,S.S.;Kaxiras,E.;Liu,A.J.Structuralpropertiesofdefectsinglassyliquids.J. Phys. Chem. B2016,120,6139−6146..

Cubuk,E.D.;Ivancic,R.J.S.;Schoenholz,S.S.;Strickland,D.J.;Basu,A.;Davidson,Z.S.;Fontaine,J.;Hor,J.L.;Huang,Y.R.;Jiang,Y.;Keim,N.C.;Koshigan,K.D.;Lefever,J.A.;Liu,T.;Ma,X.G.;Magagnosc,D.J.;Morrow,E.;Ortiz,C.P.;Rieser,J.M.;Shavit,A.;Still,T.;Xu,Y.;Zhang,Y.;Nordstrom,K.N.;Arratia,P.E.;Carpick,R.W.;Durian,D.J.;Fakhraai,Z.;Jerolmack,D.J.;Lee,D.;Li,J.;Riggleman,R.;Turner,K.T.;Yodh,A.G.;Gianola,D.S.;Liu,A.J.Structure-propertyrelationshipsfromuniversalsignaturesofplasticityindisorderedsolids.Science2017,358,1033−1037..

Boattini,E.;Marín-Aguilar,S.;Mitra,S.;Foffi,G.;Smallenburg,F.;Filion,L.Autonomouslyrevealinghiddenlocalstructuresinsupercooledliquids.Nat. Commun.2020,11,5479..

Boattini,E.;Smallenburg,F.;Filion,L.Averaginglocalstructuretopredictthedynamicpropensityinsupercooledliquids.Phys. Rev. Lett.2021,127,088007..

Alkemade,R.M.;Boattini,E.;Filion,L.;Smallenburg,F.Comparingmachinelearningtechniquesforpredictingglassydynamics.J. Chem. Phys.2022,156,204503..

Bapst,V.;Keck,T.;Grabska-Barwińska,A.;Donner,C.;Cubuk,E.D.;Schoenholz,S.S.;Obika,A.;Nelson,A.W.R.;Back,T.;Hassabis,D.;Kohli,P.Unveilingthepredictivepowerofstaticstructureinglassysystems.Nat. Phys.2020,16,448−454..

Li,H.;Jin,Y.;Jiang,Y.;Chen,J.Z.Y.DeterminingthenonequilibriumcriticalityofaGardnertransitionviaahybridstudyofmolecularsimulationsandmachinelearning.Proc. Natl. Acad. Sci. U. S. A.2021,118,e2017392118..

Zhang,K.;Li,X.;Jin,Y.;Jiang,Y.Machinelearningglasscagingorderparameterswithanartificialnestedneuralnetwork.Soft Matter2022,18,6270−6277..

Views

Downloads

CSCD

Alert me when the article has been cited

Submit

Tools

Publicity Resources

Understanding Mass Dependence of Glass Formation in Ring Polymers

A Facile Strategy for Non-fluorinated Intrinsic Low-k and Low-loss Dielectric Polymers: Valid Exploitation of Secondary Relaxation Behaviors

Positron Spectroscopy of Free Volume in Poly(vinylidene fluoride) after Helium Ions Irradiation

Related Author

No data

Related Institution

School of Applied Chemistry and Engineering, University of Science and Technology of China

School of Materials Science and Engineering, Tianjin University

PCFM Lab, GD HPPC Lab, Guangdong Engineering Technology Research Centre for High-performance Organic and Polymer Photoelectric Functional Films, State Key Laboratory of Optoelectronic Materials and Technologies, School of Chemistry, Sun Yat-sen University

Division for Experimental Physics, School of Nuclear Science & Engineering, National Research Tomsk Polytechnic University, Lenina Ave. 43

Physics Department, Faculty of Education, Ain Shams University

⁰