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Main Authors: Li, Yunzhi, Li, Chen
Format: Preprint
Published: 2025
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Online Access:https://arxiv.org/abs/2501.02243
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author Li, Yunzhi
Li, Chen
author_facet Li, Yunzhi
Li, Chen
contents We introduce the semiclassical limit to electronic systems by taking the limit $\hbar\rightarrow 0$ in the solution of Schrödinger equations. We show that this limit is closely related to one type of strong correlation that is particularly challenging from conventional multi-configurational perspective but can be readily described through semiclassical analysis. Furthermore, by studying the performance of density functional approximations (DFAs) in the semiclassical limit, we find that mainstream DFAs have erroneous divergent energy behaviors as $\hbar \rightarrow 0$, violating the exact constraint of finite energy. Importantly, by making connection of the significantly underestimated DFA energies of many strongly correlated transition-metal diatomic molecules to their rather small estimated $\hbar_{\text{eff}}$, we demonstrate the usefulness of our semiclassical analysis and its promise for inspiring better DFAs.
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publishDate 2025
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spellingShingle Exact Constraint of Density Functional Approximations at the Semiclassical Limit
Li, Yunzhi
Li, Chen
Computational Physics
We introduce the semiclassical limit to electronic systems by taking the limit $\hbar\rightarrow 0$ in the solution of Schrödinger equations. We show that this limit is closely related to one type of strong correlation that is particularly challenging from conventional multi-configurational perspective but can be readily described through semiclassical analysis. Furthermore, by studying the performance of density functional approximations (DFAs) in the semiclassical limit, we find that mainstream DFAs have erroneous divergent energy behaviors as $\hbar \rightarrow 0$, violating the exact constraint of finite energy. Importantly, by making connection of the significantly underestimated DFA energies of many strongly correlated transition-metal diatomic molecules to their rather small estimated $\hbar_{\text{eff}}$, we demonstrate the usefulness of our semiclassical analysis and its promise for inspiring better DFAs.
title Exact Constraint of Density Functional Approximations at the Semiclassical Limit
topic Computational Physics
url https://arxiv.org/abs/2501.02243