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Ab Initio Static Exchange–Correlation Kernel across Jacob’s Ladder without Functional Derivatives

[Image: see text] The electronic exchange—correlation (XC) kernel constitutes a fundamental input for the estimation of a gamut of properties such as the dielectric characteristics, the thermal and electrical conductivity, or the response to an external perturbation. In this work, we present a forma...

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Autores principales: Moldabekov, Zhandos, Böhme, Maximilian, Vorberger, Jan, Blaschke, David, Dornheim, Tobias
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2023
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9979610/
https://www.ncbi.nlm.nih.gov/pubmed/36724889
http://dx.doi.org/10.1021/acs.jctc.2c01180
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author Moldabekov, Zhandos
Böhme, Maximilian
Vorberger, Jan
Blaschke, David
Dornheim, Tobias
author_facet Moldabekov, Zhandos
Böhme, Maximilian
Vorberger, Jan
Blaschke, David
Dornheim, Tobias
author_sort Moldabekov, Zhandos
collection PubMed
description [Image: see text] The electronic exchange—correlation (XC) kernel constitutes a fundamental input for the estimation of a gamut of properties such as the dielectric characteristics, the thermal and electrical conductivity, or the response to an external perturbation. In this work, we present a formally exact methodology for the computation of the system specific static XC kernel exclusively within the framework of density functional theory (DFT) and without employing functional derivatives—no external input apart from the usual XC-functional is required. We compare our new results with exact quantum Monte Carlo (QMC) data for the archetypical uniform electron gas model under both ambient and warm dense matter conditions. This gives us unprecedented insights into the performance of different XC functionals, and it has important implications for the development of new functionals that are designed for the application at extreme temperatures. In addition, we obtain new DFT results for the XC kernel of warm dense hydrogen as it occurs in fusion applications and astrophysical objects. The observed excellent agreement to the QMC reference data demonstrates that presented framework is capable to capture nontrivial effects such as XC-induced isotropy breaking in the density response of hydrogen at large wave numbers.
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spelling pubmed-99796102023-03-03 Ab Initio Static Exchange–Correlation Kernel across Jacob’s Ladder without Functional Derivatives Moldabekov, Zhandos Böhme, Maximilian Vorberger, Jan Blaschke, David Dornheim, Tobias J Chem Theory Comput [Image: see text] The electronic exchange—correlation (XC) kernel constitutes a fundamental input for the estimation of a gamut of properties such as the dielectric characteristics, the thermal and electrical conductivity, or the response to an external perturbation. In this work, we present a formally exact methodology for the computation of the system specific static XC kernel exclusively within the framework of density functional theory (DFT) and without employing functional derivatives—no external input apart from the usual XC-functional is required. We compare our new results with exact quantum Monte Carlo (QMC) data for the archetypical uniform electron gas model under both ambient and warm dense matter conditions. This gives us unprecedented insights into the performance of different XC functionals, and it has important implications for the development of new functionals that are designed for the application at extreme temperatures. In addition, we obtain new DFT results for the XC kernel of warm dense hydrogen as it occurs in fusion applications and astrophysical objects. The observed excellent agreement to the QMC reference data demonstrates that presented framework is capable to capture nontrivial effects such as XC-induced isotropy breaking in the density response of hydrogen at large wave numbers. American Chemical Society 2023-02-01 /pmc/articles/PMC9979610/ /pubmed/36724889 http://dx.doi.org/10.1021/acs.jctc.2c01180 Text en © 2023 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Moldabekov, Zhandos
Böhme, Maximilian
Vorberger, Jan
Blaschke, David
Dornheim, Tobias
Ab Initio Static Exchange–Correlation Kernel across Jacob’s Ladder without Functional Derivatives
title Ab Initio Static Exchange–Correlation Kernel across Jacob’s Ladder without Functional Derivatives
title_full Ab Initio Static Exchange–Correlation Kernel across Jacob’s Ladder without Functional Derivatives
title_fullStr Ab Initio Static Exchange–Correlation Kernel across Jacob’s Ladder without Functional Derivatives
title_full_unstemmed Ab Initio Static Exchange–Correlation Kernel across Jacob’s Ladder without Functional Derivatives
title_short Ab Initio Static Exchange–Correlation Kernel across Jacob’s Ladder without Functional Derivatives
title_sort ab initio static exchange–correlation kernel across jacob’s ladder without functional derivatives
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9979610/
https://www.ncbi.nlm.nih.gov/pubmed/36724889
http://dx.doi.org/10.1021/acs.jctc.2c01180
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