Coupling between structural relaxation and diffusion in glass-forming liquids under pressure variation
文献信息
Katsunori Wakabayashi
We theoretically investigate structural relaxation and activated diffusion of glass-forming liquids at different pressures using both Elastically Collective Nonlinear Langevin Equation (ECNLE) theory and molecular dynamics (MD) simulations. An external pressure restricts local motions of a single molecule within its cage and triggers slowing down of cooperative mobility. While the ECNLE theory and simulations generally predict a monotonic increase of the glass transition temperature and dynamic fragility with pressure, the simulations indicate a decrease of fragility as pressures above 1000 bar. The structural relaxation time is found to be linearly coupled with the inverse diffusion constant. Remarkably, this coupling is independent of compression. The theoretical calculations quantitatively agree well with the simulations and are also consistent with prior work.
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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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