Subquadratic wavenumber dependence of the structural relaxation of supercooled liquid in the crossover regime.
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.
Bhattacharyya
Sarika Maitra
SM
Solid State and Structural Chemistry Unit, Indian Institute of Science, 560012 Bangalore, India.
Bagchi
Biman
B
Wolynes
Peter G
PG