Importance of Many Particle Correlations to the Collective Debye-Waller Factor in a Single-Particle Activated Dynamic Theory of the Glass Transition

Abstract

We theoretically study the importance of many body correlations on the collective Debye Waller (DW) factor in the context of the Nonlinear Langevin Equation (NLE) single particle activated dynamics theory of glass transition and its extension to include collective elasticity (ECNLE theory). This microscopic force-based approach envisions structural alpha relaxation as a coupled local-nonlocal process involving correlated local cage and longer range collective barriers. The crucial question addressed here is the importance of the deGennes narrowing contribution versus a literal Vineyard approximation for the collective DW factor that enters the construction of the dynamic free energy in NLE theory. While the Vineyard-deGennes approach-based NLE theory and its ECNLE theory extension yields predictions that agree well with experimental and simulation results, use of a literal Vineyard approximation for the collective DW factor massively overpredicts the activated relaxation time. The current study suggests many particle correlations are crucial for a reliable description of activated dynamics theory of model hard sphere fluids.