Minimal-active-space multistate density functional theory for excitation energy involving local and charge transfer states

Abstract Multistate density functional theory (MSDFT) employing a minimum active space (MAS) is presented to determine charge transfer (CT) and local excited states of bimolecular complexes. MSDFT is a hybrid wave function theory (WFT) and density functional theory, in which dynamic correlation is f...

Descripción completa

Guardado en:

Detalles Bibliográficos
Autores principales:	Ruoqi Zhao, Christian P. Hettich, Xin Chen, Jiali Gao
Formato:	article
Lenguaje:	EN
Publicado:	Nature Portfolio 2021
Materias:	Materials of engineering and construction. Mechanics of materials TA401-492 Computer software QA76.75-76.765
Acceso en línea:	https://doaj.org/article/9bc5d925cc3d45eaa81326f7f84d3c12
Etiquetas:	Agregar Etiqueta Sin Etiquetas, Sea el primero en etiquetar este registro!

id	oai:doaj.org-article:9bc5d925cc3d45eaa81326f7f84d3c12
record_format	dspace
spelling	oai:doaj.org-article:9bc5d925cc3d45eaa81326f7f84d3c122021-12-02T18:02:06ZMinimal-active-space multistate density functional theory for excitation energy involving local and charge transfer states10.1038/s41524-021-00624-32057-3960https://doaj.org/article/9bc5d925cc3d45eaa81326f7f84d3c122021-09-01T00:00:00Zhttps://doi.org/10.1038/s41524-021-00624-3https://doaj.org/toc/2057-3960Abstract Multistate density functional theory (MSDFT) employing a minimum active space (MAS) is presented to determine charge transfer (CT) and local excited states of bimolecular complexes. MSDFT is a hybrid wave function theory (WFT) and density functional theory, in which dynamic correlation is first incorporated in individual determinant configurations using a Kohn–Sham exchange-correlation functional. Then, nonorthogonal configuration-state interaction is performed to treat static correlation. Because molecular orbitals are optimized separately for each determinant by including Kohn–Sham dynamic correlation, a minimal number of configurations in the active space, essential to representing low-lying excited and CT states of interest, is sufficient to yield the adiabatic states. We found that the present MAS-MSDFT method provides a good description of covalent and CT excited states in comparison with experiments and high-level computational results. Because of the simplicity and interpretive capability through diabatic configuration weights, the method may be useful in dynamic simulations of CT and nonadiabatic processes.Ruoqi ZhaoChristian P. HettichXin ChenJiali GaoNature PortfolioarticleMaterials of engineering and construction. Mechanics of materialsTA401-492Computer softwareQA76.75-76.765ENnpj Computational Materials, Vol 7, Iss 1, Pp 1-10 (2021)
institution	DOAJ
collection	DOAJ
language	EN
topic	Materials of engineering and construction. Mechanics of materials TA401-492 Computer software QA76.75-76.765
spellingShingle	Materials of engineering and construction. Mechanics of materials TA401-492 Computer software QA76.75-76.765 Ruoqi Zhao Christian P. Hettich Xin Chen Jiali Gao Minimal-active-space multistate density functional theory for excitation energy involving local and charge transfer states
description	Abstract Multistate density functional theory (MSDFT) employing a minimum active space (MAS) is presented to determine charge transfer (CT) and local excited states of bimolecular complexes. MSDFT is a hybrid wave function theory (WFT) and density functional theory, in which dynamic correlation is first incorporated in individual determinant configurations using a Kohn–Sham exchange-correlation functional. Then, nonorthogonal configuration-state interaction is performed to treat static correlation. Because molecular orbitals are optimized separately for each determinant by including Kohn–Sham dynamic correlation, a minimal number of configurations in the active space, essential to representing low-lying excited and CT states of interest, is sufficient to yield the adiabatic states. We found that the present MAS-MSDFT method provides a good description of covalent and CT excited states in comparison with experiments and high-level computational results. Because of the simplicity and interpretive capability through diabatic configuration weights, the method may be useful in dynamic simulations of CT and nonadiabatic processes.
format	article
author	Ruoqi Zhao Christian P. Hettich Xin Chen Jiali Gao
author_facet	Ruoqi Zhao Christian P. Hettich Xin Chen Jiali Gao
author_sort	Ruoqi Zhao
title	Minimal-active-space multistate density functional theory for excitation energy involving local and charge transfer states
title_short	Minimal-active-space multistate density functional theory for excitation energy involving local and charge transfer states
title_full	Minimal-active-space multistate density functional theory for excitation energy involving local and charge transfer states
title_fullStr	Minimal-active-space multistate density functional theory for excitation energy involving local and charge transfer states
title_full_unstemmed	Minimal-active-space multistate density functional theory for excitation energy involving local and charge transfer states
title_sort	minimal-active-space multistate density functional theory for excitation energy involving local and charge transfer states
publisher	Nature Portfolio
publishDate	2021
url	https://doaj.org/article/9bc5d925cc3d45eaa81326f7f84d3c12
work_keys_str_mv	AT ruoqizhao minimalactivespacemultistatedensityfunctionaltheoryforexcitationenergyinvolvinglocalandchargetransferstates AT christianphettich minimalactivespacemultistatedensityfunctionaltheoryforexcitationenergyinvolvinglocalandchargetransferstates AT xinchen minimalactivespacemultistatedensityfunctionaltheoryforexcitationenergyinvolvinglocalandchargetransferstates AT jialigao minimalactivespacemultistatedensityfunctionaltheoryforexcitationenergyinvolvinglocalandchargetransferstates
_version_	1718378944024018944

Minimal-active-space multistate density functional theory for excitation energy involving local and charge transfer states

Ejemplares similares