Year: 2026
Type: article
Abstract: In this work we introduce a generalized flavor, in the sense of generalized Kohn-Sham density functional theory (gKS-DFT), of the recently derived local potential functional embedding theory (LPFET) ( J. Chem. Theory Comput. 2025 21 10293), where the in-principle exact formalism of DFT is combined with that of density matrix embedding theory (DMET). In generalized LPFET (gLPFET), the embedding clusters are designed from a full-size gKS system where the (in-principle non-local) Hartree-Fock exchange potential is combined with a local (in the localized orbital representation) correlation potential. The latter is optimized self-consistently such that gKS and local embedding cluster’s densities match. Unlike in DMET, which uses the same (global) chemical potential value in all clusters, each embedded orbital has its own chemical potential in gLPFET. We show analytically that, when electron correlation is strongly local, the latter potential becomes a simple functional of the correlation potential. Numerical calculations on model systems confirm the high accuracy of gLPFET in this regime, in contrast to DMET. Moreover, we show that gLPFET completely fixes the flaw of LPFET in weaker correlation regimes, through its appropriate description of the Hartree-exchange potential.
Source: Electronic Structure
Language: English
Subfield: Atomic and Molecular Physics, and Optics
Field: Physics and Astronomy
Domain: Physical Sciences
Open Access status: bronze
Awards: G1949054838, Par-delà les frontières, l'Université de Strasbourg, G2255650664, Quantum Algorithms to Reveal Electronic structure, G2659019386, Quantum technologies: Education and training to fulfill the strategic skill needs of research and industry in France, G2694206344, G2729097322, Façonner les talents en formation et en recherche à l'Université de Strasbourg, G3357951378, G4779185514, Quantum Science and Nanomaterials, G6136357505, G6276897512, G6803667113, G8050745384
OpenAlex ID: W7165534058