Atomic dynamics in fluids: Normal mode analysis revisited

Jaeyun Moon; Lucas Lindsay; Takeshi Egami

doi:10.1103/physreve.108.014601

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arXiv · 2304.09778

Atomic dynamics in fluids: Normal mode analysis revisited

Jaeyun Moon·Lucas Lindsay·Takeshi Egami

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Abstract

Developing microscopic understanding of the thermal properties of liquids is challenging due to their strong dynamic disorder, which prevents characterization of the atomic degrees of freedom. There have been significant research interests in the past few decades to extend the normal mode analysis for solids to instantaneous structures of liquids. However, the nature of normal modes that arise from these unstable structures is still elusive. In this work, we explore the instantaneous eigenmodes of dynamical matrices of various Lennard-Jones argon liquid/gas systems at high temperatures and show that the normal modes can be interpreted as an interpolation of T \to \infty (gas) and T = 0 (solid) mode descriptions. We find that normal modes become increasingly collisional and translational, recovering atomistic gas-like behavior rather than vibrational with increase in temperature, suggesting that normal modes in liquids may be described by both solid-like and gas-like modes.

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Jaeyun Moon, Lucas Lindsay, Takeshi Egami. 2023-04-19. Atomic dynamics in fluids: Normal mode analysis revisited. https://doi.org/10.1103/physreve.108.014601

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