Subquadratic wavenumber dependence of the structural relaxation of supercooled liquid in the crossover regime

被引:20
作者
Bhattacharyya, Sarika Maitra [1 ]
Bagchi, Biman [1 ]
Wolynes, Peter G. [2 ]
机构
[1] Indian Inst Sci, Solid State & Struct Chem Unit, Bangalore 560012, Karnataka, India
[2] Univ Calif San Diego, Dept Chem & Biochem, La Jolla, CA 92093 USA
关键词
glass transition; liquids; supercooling; KINETIC GLASS-TRANSITION; DYNAMICS; TRANSPORT; CRYSTALS; WATER;
D O I
10.1063/1.3330911
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
As a liquid is progressively supercooled toward its glass transition temperature, an intriguing weakening of the wavenumber (q) dependence of the structural relaxation time tau(q) in the intermediate-to-large q limit is observed both in experiments and simulation studies. Neither continuous Brownian diffusive dynamics nor discontinuous activated events can alone explain the anomalous wavenumber dependence. Here we use our recently developed theory that unifies the mode coupling theory for continuous dynamics, with the random first order transition theory treatment of activated discontinuous motion as a nucleationlike instanton process to understand the wavenumber dependence of density relaxation. The predicted smooth change in mechanism of relaxation from diffusive to activated, in the crossover regime, is wavevector dependent and appears to be responsible for the observed subquadratic, almost linear, q dependence of the relaxation time.
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页数:6
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共 27 条
[1]   Glassy dynamics of simulated polymer melts: Coherent scattering and van Hove correlation functions: Part II: Dynamics in the α-relaxation regime [J].
Aichele M. ;
Baschnagel J. .
The European Physical Journal E, 2001, 5 (2) :245-256
[2]   Experimental evidence by neutron scattering of a crossover from Gaussian to non-Gaussian behavior in the α relaxation of polyisoprene -: art. no. 051802 [J].
Arbe, A ;
Colmenero, J ;
Alvarez, F ;
Monkenbusch, M ;
Richter, D ;
Farago, B ;
Frick, B .
PHYSICAL REVIEW E, 2003, 67 (05) :16
[3]   Non-Gaussian nature of the α relaxation of glass-forming polyisoprene -: art. no. 245701 [J].
Arbe, A ;
Colmenero, J ;
Alvarez, F ;
Monkenbusch, M ;
Richter, D ;
Farago, B ;
Frick, B .
PHYSICAL REVIEW LETTERS, 2002, 89 (24)
[4]   A MOLECULAR EXPLANATION OF THE TRANSITION FROM VISCOUS TO HOPPING MECHANISM OF MASS-TRANSPORT IN THE SUPERCOOLED LIQUID NEAR THE GLASS-TRANSITION [J].
BAGCHI, B .
JOURNAL OF CHEMICAL PHYSICS, 1994, 101 (11) :9946-9955
[5]   Evolution of particle-scale dynamics in an aging clay suspension [J].
Bandyopadhyay, R ;
Liang, D ;
Yardimci, H ;
Sessoms, DA ;
Borthwick, MA ;
Mochrie, SGJ ;
Harden, JL ;
Leheny, RL .
PHYSICAL REVIEW LETTERS, 2004, 93 (22)
[6]   Correlated orientational and translational motions in supercooled liquids [J].
Bhattacharyya, S ;
Mukherjee, A ;
Bagchi, B .
JOURNAL OF CHEMICAL PHYSICS, 2002, 117 (06) :2741-2746
[7]   Facilitation, complexity growth, mode coupling, and activated dynamics in supercooled liquids [J].
Bhattacharyya, Sarika Maitra ;
Bagchi, Biman ;
Wolynes, Peter G. .
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2008, 105 (42) :16077-16082
[8]   Bridging the gap between the mode coupling and the random first order transition theories of structural relaxation in liquids [J].
Bhattacharyya, SM ;
Bagchi, B ;
Wolynes, PG .
PHYSICAL REVIEW E, 2005, 72 (03)
[9]  
BHATTACHARYYA SM, ARXIVCONDMAT0702435
[10]   Mean-field theory, mode-coupling theory, and the onset temperature in supercooled liquids [J].
Brumer, Y ;
Reichman, DR .
PHYSICAL REVIEW E, 2004, 69 (04) :5