Universal law for the vibrational density of states of liquids

Abstract

An analytical derivation of the vibrational density of states (DOS) of liquids, and in particular of its characteristic linear in frequency low-energy regime, has always been elusive because of the presence of an infinite set of purely imaginary modes -- the instantaneous normal modes (INMs). By combining an analytic continuation of the Plemelj identity to the complex plane with the purely overdamped dynamics of the INMs, we derive a closed-form analytic expression for the low-frequency DOS of liquids. The obtained result explains from first principles the widely observed linear in frequency term of the DOS in liquids, whose slope appears to increase with the average lifetime of the INMs. The analytic results are robustly confirmed by fitting simulations data for Lennard-Jones liquids, and they also recover the Arrhenius law for the average relaxation time of the INMs, as expected.

Accepted for publication in PNAS

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• To the Theory of Unstable States
• Universal Character of Atomic Motions at the Liquid-Solid Transition

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