A Mode-Coupling Theory of Vibrational Line Broadening in Near-Critical Fluids † (original) (raw)

The Journal of Physical Chemistry B, 2005

Abstract

We present a fully microscopic mode-coupling theory of near-critical line broadening. All the structural and dynamical input required by the theory is calculated directly from intermolecular potentials. We compute vibrational frequency time-correlation functions and line shapes as the critical point is approached along both the critical isochore and the liquid-gas coexistence curve. Theory is shown to be in good agreement with simulation.

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