Exchange–correlation entropy from the generalized thermal adiabatic connection

Harding, Brittany P.; Mauri, Zachary; Xie, Vera W.; Pribram-Jones, Aurora

doi:10.1063/5.0196650

Title: Exchange–correlation entropy from the generalized thermal adiabatic connection

Journal Article · 17 April 2024 · Journal of Chemical Physics

DOI: https://doi.org/10.1063/5.0196650 · OSTI ID:2404880

^[1];

^[2]; Xie, Vera W. ^[3];

^[3]

University of California, Merced, CA (United States); University of California, Merced
Stanford University, CA (United States)
University of California, Merced, CA (United States)

Warm dense matter is a highly energetic phase characterized by strong correlations, thermal effects, and quantum mechanical electrons. Thermal density functional theory is commonly used in simulations of this challenging phase, driving the development of temperature-dependent approximations to the exchange–correlation free energy. Approaches using the adiabatic connection formula are well known at zero temperature and have been recently leveraged at non-zero temperatures as well. In this work, a generalized thermal adiabatic connection (GTAC) formula is proposed, introducing a fictitious temperature parameter. This allows extraction of the exchange–correlation entropy S_XC using simulated interaction strength scaling. Here, this procedure uses a Hellmann–Feynman approach to express the exchange–correlation entropy in terms of a temperature- and interaction strength-dependent exchange–correlation potential energy. In addition, analysis of S_XC as a function of interaction strength suggests new forms for approximations, and GTAC itself offers a new framework for exploring both the exact and approximate interplay of temperature, density, and interaction strength across a wide range of conditions.

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Research Organization:: University of California, Merced, CA (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: NA0003984; NA0003866

OSTI ID:: 2404880

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 15 Vol. 160; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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