Many-Body Nature of Relaxation Processes in Glass-Forming Systems.

Most glass-forming systems are composed of basic units interacting with each other with a nontrivial anharmonic potential. Naturally, relaxation and diffusion in glass formers is a many-body problem. Results from recent experimental studies are presented to show the effects of many-body relaxation and diffusion manifested on the dynamic properties of glass formers. Considering that the effects are general and critical, the problem of glass transition will not be solved until the many-body nature of the relaxation process has been incorporated fundamentally into any theory.

[1]  S Capaccioli,et al.  Interdependence of primary and Johari-Goldstein secondary relaxations in glass-forming systems. , 2008, The journal of physical chemistry. B.

[2]  Pierangelo Rolla,et al.  Secondary dynamics in glass formers: Relation with the structural dynamics and the glass transition , 2007 .

[3]  R. Kohlrausch.  Theorie des elektrischen Rückstandes in der Leidener Flasche , 1854 .

[4]  W. G. Hoover,et al.  Statistical theories of melting , 1971 .

[5]  K. L. Ngai,et al.  Molecular dynamics and physical stability of amorphous anti-inflammatory drug: celecoxib. , 2010, The journal of physical chemistry. B.

[6]  Madalena Dionísio,et al.  Molecular motions in amorphous ibuprofen as studied by broadband dielectric spectroscopy. , 2008, The journal of physical chemistry. B.

[7]  R Casalini,et al.  Thermodynamical scaling of the glass transition dynamics. , 2004, Physical review. E, Statistical, nonlinear, and soft matter physics.

[8]  Seiichi Sudo,et al.  Relaxation processes of water in the liquid to glassy states of water mixtures studied by broadband dielectric spectroscopy , 2007 .

[9]  Naoki Shinyashiki,et al.  Resolving the ambiguity of the dynamics of water and clarifying its role in hydrated proteins , 2011 .

[10]  S Capaccioli,et al.  Dynamics of supercooled and glassy dipropyleneglycol dibenzoate as functions of temperature and aging: Interpretation within the coupling model framework. , 2004, The Journal of chemical physics.

[11]  Ulf R. Pedersen,et al.  Strong pressure-energy correlations in van der Waals liquids. , 2007, Physical review letters.

[12]  S Capaccioli,et al.  Resolving the controversy on the glass transition temperature of water? , 2011, The Journal of chemical physics.

[13]  H. Bai,et al.  Relating activation of shear transformation zones to β relaxations in metallic glasses , 2010 .

[14]  R Böhmer,et al.  Correlation of primary relaxations and high-frequency modes in supercooled liquids. I. Theoretical background of a nuclear magnetic resonance experiment. , 2006, Physical review. E, Statistical, nonlinear, and soft matter physics.

[15]  K L Ngai,et al.  Similarity of relaxation in supercooled liquids and interacting arrays of oscillators. , 1999, Physical review. E, Statistical physics, plasmas, fluids, and related interdisciplinary topics.

[16]  Tsang,et al.  Relaxation in interacting arrays of oscillators. , 1996, Physical review. E, Statistical physics, plasmas, fluids, and related interdisciplinary topics.

[17]  M Paluch,et al.  Determining the structural relaxation times deep in the glassy state of the pharmaceutical Telmisartan , 2010, Journal of physics. Condensed matter : an Institute of Physics journal.

[18]  M Paluch,et al.  Classification of secondary relaxation in glass-formers based on dynamic properties. , 2004, The Journal of chemical physics.

[19]  C. Roland,et al.  Aging of the secondary relaxation to probe structural relaxation in the glassy state. , 2009, Physical review letters.

[20]  Kwok Yeung Tsang,et al.  Dynamics of relaxing systems subjected to nonlinear interactions , 1997 .

[21]  K. L. Ngai,et al.  An extended coupling model description of the evolution of dynamics with time in supercooled liquids and ionic conductors , 2003 .

[22]  George Floudas,et al.  Molecular Dynamics of Glass-Forming Systems , 2011 .

[23]  Martin Goldstein,et al.  Viscous Liquids and the Glass Transition. II. Secondary Relaxations in Glasses of Rigid Molecules , 1970 .

[24]  Alois Loidl,et al.  Relaxation dynamics in plastic crystals , 2002 .

[25]  D. Coslovich,et al.  Thermodynamic scaling of diffusion in supercooled Lennard-Jones liquids. , 2007, The journal of physical chemistry. B.

[26]  L. Carpentier,et al.  Dynamics of the Amorphous and Crystalline α-, γ-Phases of Indomethacin , 2006 .

[27]  Marc Descamps,et al.  Molecular Mobility in Supercooled Trehalose , 2003 .

[28]  G Tarjus,et al.  Disentangling density and temperature effects in the viscous slowing down of glassforming liquids. , 2004, The Journal of chemical physics.

[29]  Simone Capaccioli,et al.  Effect of thermodynamic history on secondary relaxation in the glassy state , 2007 .

[30]  K. L. Ngai,et al.  Relation between some secondary relaxations and the α relaxations in glass-forming materials according to the coupling model , 1998 .

[31]  Martin Goldstein,et al.  The past, present, and future of the Johari–Goldstein relaxation , 2011 .

[32]  Riccardo Casalini,et al.  Dispersion of the Structural Relaxation and the Vitrification of Liquids , 2006 .

[33]  Albert Toelle.  Neutron scattering studies of the model glass former ortho-terphenyl , 2001 .

[34]  K. L. Ngai,et al.  Correlation between primary and secondary Johari-Goldstein relaxations in supercooled liquids: invariance to changes in thermodynamic conditions. , 2008, The Journal of chemical physics.

[35]  C. M. Roland,et al.  Scaling of the segmental relaxation times of polymers and its relation to the thermal expansivity , 2004 .

[36]  Riccardo Casalini,et al.  Identifying the genuine Johari–Goldstein β-relaxation by cooling, compressing, and aging small molecular glass-formers , 2005 .

[37]  M Paluch,et al.  Identification of the molecular motions responsible for the slower secondary (beta) relaxation in sucrose. , 2008, The journal of physical chemistry. B.

[38]  P. Lunkenheimer,et al.  Indications for an “excess wing” in metallic glasses from the mechanical loss modulus in Zr65Al7.5Cu27.5 , 2004 .

[39]  R. Nath,et al.  2H-NMR studies of supercooled and glassy aspirin , 2007 .

[40]  Sergey Vyazovkin,et al.  Probing Beta Relaxation in Pharmaceutically Relevant Glasses by Using DSC , 2005, Pharmaceutical Research.

[41]  K L Ngai,et al.  Component dynamics in miscible mixtures of water and methanol. , 2011, The journal of physical chemistry. B.

[42]  K L Ngai,et al.  Glass transition dynamics of room-temperature ionic liquid 1-methyl-3-trimethylsilylmethylimidazolium tetrafluoroborate. , 2011, The journal of physical chemistry. B.

[43]  K. Ngai.  Relaxation and Diffusion in Complex Systems , 2011 .

[44]  K. L. Ngai,et al.  Resolution of problems in soft matter dynamics by combining calorimetry and other spectroscopies , 2010 .

[45]  S Capaccioli,et al.  The Johari-Goldstein beta-relaxation of water. , 2007, The journal of physical chemistry. B.

[46]  K. L. Ngai,et al.  Johari–Goldstein relaxation as the origin of the excess wing observed in metallic glasses , 2006 .

[47]  S Capaccioli,et al.  Do theories of the glass transition, in which the structural relaxation time does not define the dispersion of the structural relaxation, need revision? , 2005, The journal of physical chemistry. B.

[48]  Jagdish K. Vij,et al.  Localized relaxation's strength and its mimicry of glass-softening thermodynamics , 2002 .

[49]  R. Böhmer,et al.  Correlation of primary relaxations and high-frequency modes in supercooled liquids. II. Evidence from spin-lattice relaxation weighted stimulated-echo spectroscopy. , 2006, Physical review. E, Statistical, nonlinear, and soft matter physics.

[50]  S Capaccioli,et al.  Relation between the activation energy of the Johari-Goldstein beta relaxation and T(g) of glass formers. , 2004, Physical review. E, Statistical, nonlinear, and soft matter physics.

[51]  M Paluch,et al.  Broadband dielectric relaxation study at ambient and elevated pressure of molecular dynamics of pharmaceutical: indomethacin. , 2009, The journal of physical chemistry. B.

[52]  Jagdish K. Vij,et al.  Relaxation strength of localized motions in D-sorbitol and mimicry of glass-softening thermodynamics , 2003 .

[53]  Pierangelo Rolla,et al.  Does the entropy and volume dependence of the structural α-relaxation originate from the Johari–Goldstein β-relaxation? , 2009 .

[54]  G. P. Johari,et al.  GLASS TRANSITION AND SECONDARY RELAXATIONS IN MOLECULAR LIQUIDS AND CRYSTALS , 1976 .

[55]  H. C. Andersen,et al.  Role of Repulsive Forces in Determining the Equilibrium Structure of Simple Liquids , 1971 .

[56]  Rendell.  Interaction of a relaxing system with a dynamical environment. , 1993, Physical review. E, Statistical physics, plasmas, fluids, and related interdisciplinary topics.

[57]  J. Pelletier,et al.  Viscoelasticity and viscosity of Pd-Ni-Cu-P bulk metallic glasses , 2002 .

[58]  R. Böhmer,et al.  Correlation of primary and secondary relaxations in a supercooled liquid. , 2006, Physical review letters.

[59]  R M Pick,et al.  Temperature and pressure study of Brillouin transverse modes in the organic glass-forming liquid orthoterphenyl. , 2003, Physical review. E, Statistical, nonlinear, and soft matter physics.

[60]  Riccardo Casalini,et al.  Supercooled dynamics of glass-forming liquids and polymers under hydrostatic pressure , 2005 .

[61]  Dmitry Bedrov,et al.  Secondary Johari-Goldstein relaxation in linear polymer melts represented by a simple bead-necklace model , 2011 .