Normal mode description of phases of matter: Application to heat capacity

Jaeyun Moon; Simon Thébaud; Lucas Lindsay; Takeshi Egami

doi:10.1103/PhysRevResearch.6.013206

Normal mode description of phases of matter: Application to heat capacity

Jaeyun Moon, Simon Thébaud, Lucas Lindsay, Takeshi Egami

Materials Theory

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2 Scopus citations

Abstract

Understanding thermodynamics in liquids at the atomic level is challenging because of strong atomic interactions and lack of spatial symmetry. Recent prior theoretical works have focused on describing heat capacity of liquids in terms of phonon-like excitations but often rely on fitting factors and ad hoc assumptions. In this work, we propose characterizing various phases in terms of instantaneous normal modes (INMs) of structural snapshots from molecular dynamics simulations of single-element systems over wide ranges of temperature and pressure. We use the INMs to build a mode-level microscopic description of heat capacity and demonstrate that heat capacity of liquids can be described by a combination of both solidlike and gaslike degrees of freedom, leading to a more unified framework to fundamentally describe heat capacity of all three phases of matter: solid, liquid, and gas.

Original language	English
Article number	013206
Journal	Physical Review Research
Volume	6
Issue number	1
DOIs	https://doi.org/10.1103/PhysRevResearch.6.013206
State	Published - Jan 2024

Funding

This research was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. This work used the Extreme Science and Engineering Discovery Environment (XSEDE) Expanse under Allocation No. TG-MAT200012. This research used resources of the National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility located at Lawrence Berkeley National Laboratory, operated under Contract No. DE-AC02-05CH11231 using NERSC Award No. BES-ERCAP0023621. We are grateful for discussions with Alan McGaughey. This research was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. This work used the Extreme Science and Engineering Discovery Environment (XSEDE) Expanse under Allocation No. TG-MAT200012. This research used resources of the National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility located at Lawrence Berkeley National Laboratory, operated under Contract No. DE-AC02-05CH11231 using NERSC Award No. BES-ERCAP0023621.

Funders	Funder number
U.S. Department of Energy
Office of Science
Basic Energy Sciences
Lawrence Berkeley National Laboratory	DE-AC02-05CH11231, BES-ERCAP0023621
Division of Materials Sciences and Engineering	TG-MAT200012

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Normal mode description of phases of matter: Application to heat capacity

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