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We theoretically investigate structural relaxation and activated diffusion ofglass-forming liquids at different pressures using both the ElasticallyCollective Nonlinear Langevin Equation (ECNLE) theory and molecular dynamics(MD) simulation. An external pressure restricts local motions of a singlemolecule within its cage and triggers the slowing down of cooperative mobility.While the ECNLE theory and simulation generally predict a monotonic increase ofthe glass transition temperature and dynamic fragility with pressure, thesimulation indicates a decrease of fragility as pressure above 1000 bar. Thestructural relaxation time is found to be linearly coupled with the inversediffusion constant. Remarkably, this coupling is independent of compression.Theoretical calculations agree quantitatively well with simulations and arealso consistent with prior works.

Coupling between structural relaxation and diffusion in glass-forming liquids under pressure variation