Thermodynamic signature of growing amorphous order in glass-forming liquids

被引:288
作者
Biroli, G. [3 ]
Bouchaud, J. -P. [4 ]
Cavagna, A. [5 ]
Grigera, T. S. [1 ,2 ,6 ]
Verrocchio, P. [7 ]
机构
[1] Natl Univ La Plata, Fac Ciencias Exactas, Inst Invest Fisicoquim Teor & Aplicadas, CCT La Plata, RA-1900 La Plata, Argentina
[2] Natl Univ La Plata, Fac Ciencias Exactas, Dept Fis, RA-1900 La Plata, Argentina
[3] MPPU, CEA, CNRS,URA2306, DSM,Inst Phys Theor, F-91191 Gif Sur Yvette, France
[4] Capital Fund Management, Sci & Finance, F-75009 Paris, France
[5] CNR INFM, Ctr Stat Mech & Complex SMC, I-00185 Rome, Italy
[6] Consejo Nacl Invest Cient & Tecn, RA-1900 La Plata, Argentina
[7] Univ Trent, Dipartimento Fis, I-38050 Trento, Italy
关键词
D O I
10.1038/nphys1050
中图分类号
O4 [物理学];
学科分类号
0702 ;
摘要
Supercooled liquids exhibit a pronounced slowdown of their dynamics on cooling(1) without showing any obvious structural or thermodynamic changes(2). Several theories relate this slowdown to increasing spatial correlations(3-6). However, no sign of this is seen in standard static correlation functions, despite indirect evidence from considering specific heat(7) and linear dielectric susceptibility(8). Whereas the dynamic correlation function progressively becomes more non-exponential as the temperature is reduced, so far no similar signature has been found in static correlations that can distinguish qualitatively between a high-temperature and a deeply supercooled glass-forming liquid in equilibrium. Here, we show evidence of a qualitative thermodynamic signature that differentiates between the two. We show by numerical simulations with fixed boundary conditions that the influence of the boundary propagates into the bulk over increasing length scales on cooling. With the increase of this static correlation length, the influence of the boundary decays non-exponentially. Such long-range susceptibility to boundary conditions is expected within the random first-order theory(4,9,10) (RFOT) of the glass transition. However, a quantitative account of our numerical results requires a generalization of RFOT, taking into account surface tension fluctuations between states.
引用
收藏
页码:771 / 775
页数:5
相关论文
共 32 条
[1]   ON TEMPERATURE DEPENDENCE OF COOPERATIVE RELAXATION PROPERTIES IN GLASS-FORMING LIQUIDS [J].
ADAM, G ;
GIBBS, JH .
JOURNAL OF CHEMICAL PHYSICS, 1965, 43 (01) :139-&
[2]   SOFT-SPHERE MODEL FOR THE GLASS-TRANSITION IN BINARY-ALLOYS - PAIR STRUCTURE AND SELF-DIFFUSION [J].
BERNU, B ;
HANSEN, JP ;
HIWATARI, Y ;
PASTORE, G .
PHYSICAL REVIEW A, 1987, 36 (10) :4891-4903
[3]   Direct experimental evidence of a growing length scale accompanying the glass transition [J].
Berthier, L ;
Biroli, G ;
Bouchaud, JP ;
Cipelletti, L ;
El Masri, D ;
L'Hôte, D ;
Ladieu, F ;
Pierno, M .
SCIENCE, 2005, 310 (5755) :1797-1800
[4]   Nonlinear susceptibility in glassy systems: A probe for cooperative dynamical length scales [J].
Bouchaud, JP ;
Biroli, G .
PHYSICAL REVIEW B, 2005, 72 (06)
[5]   On the Adam-Gibbs-Kirkpatrick-Thirumalai-Wolynes scenario for the viscosity increase in glasses [J].
Bouchaud, JP ;
Biroli, G .
JOURNAL OF CHEMICAL PHYSICS, 2004, 121 (15) :7347-7354
[6]   A novel method for evaluating the critical nucleus and the surface tension in systems with first order phase transition [J].
Cammarota, Chiara ;
Cavagna, Andrea .
JOURNAL OF CHEMICAL PHYSICS, 2007, 127 (21)
[7]   Mosaic multistate scenario versus one-state description of supercooled liquids [J].
Cavagna, Andrea ;
Grigera, Tomas S. ;
Verrocchio, Paolo .
PHYSICAL REVIEW LETTERS, 2007, 98 (18)
[8]   Thermodynamics of binary mixture glasses [J].
Coluzzi, B ;
Mézard, M ;
Parisi, G ;
Verrocchio, P .
JOURNAL OF CHEMICAL PHYSICS, 1999, 111 (19) :9039-9052
[9]   Activated events in glasses: The structure of entropic droplets [J].
Dzero, M ;
Schmalian, J ;
Wolynes, PG .
PHYSICAL REVIEW B, 2005, 72 (10)
[10]   Supercooled liquids and glasses [J].
Ediger, MD ;
Angell, CA ;
Nagel, SR .
JOURNAL OF PHYSICAL CHEMISTRY, 1996, 100 (31) :13200-13212