A Non-orthogonal Configuration Interaction approach to Singlet Fission in Perylenediimide compounds

Perylenediimide molecules constitute a family of chromophores that undergo singlet fission, a process in which an excited singlet state converts into lower energy triplets on two neighboring molecules, potentially increasing the efficiency of organic solar cells. Here, the nonorthogonal configuratio...

Descripción completa

Detalles Bibliográficos
Autores: Sousa Romero, Carmen, Sanchez-Mansilla, Aitor, Broer, Ria, Straatsma, T. P., de Graaf, Coen
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2023
País:España
Institución:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
Repositorio:Recercat. Dipósit de la Recerca de Catalunya
OAI Identifier:oai:recercat.cat:2445/219447
Acceso en línea:https://hdl.handle.net/2445/219447
Access Level:acceso abierto
Palabra clave:Monòmers
Oligòmers
Fissió nuclear
Monomers
Oligomers
Nuclear fission
id ES_6cfb2c44f3776e961a7f452c00a3e0b0
oai_identifier_str oai:recercat.cat:2445/219447
network_acronym_str ES
network_name_str España
repository_id_str
spelling A Non-orthogonal Configuration Interaction approach to Singlet Fission in Perylenediimide compoundsSousa Romero, CarmenSanchez-Mansilla, AitorBroer, RiaStraatsma, T. P.de Graaf, CoenMonòmersOligòmersFissió nuclearMonomersOligomersNuclear fissionPerylenediimide molecules constitute a family of chromophores that undergo singlet fission, a process in which an excited singlet state converts into lower energy triplets on two neighboring molecules, potentially increasing the efficiency of organic solar cells. Here, the nonorthogonal configuration interaction method is applied to study the effect of the different crystal packing of various perylenediimide derivatives on the relative energies of the singlet and triplet states, the intermolecular electronic couplings, and the relative rates for singlet fission. The analysis of the wave functions and electronic couplings reveals that charge transfer states play an important role in the singlet fission mechanism. Dimer conformations where the PDI molecules are at large displacements along the long axis and short on the short axis are posed as the most favorable for singlet fission. The role of the substituent at the imide group has been inspected concluding that, although it has no effect in the energies, for some conformations it significantly influences the electronic couplings, and therefore, replacing this substituent with hydrogen may introduce artifacts in the computational modeling of the PDI molecules.American Chemical Society2025202520232025info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersion15 p.application/pdfapplication/pdfhttps://hdl.handle.net/2445/219447Articles publicats en revistes (Ciència dels Materials i Química Física)reponame:Recercat. Dipósit de la Recerca de Catalunyainstname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)InglésReproducció del document publicat a: https://doi.org/10.1021/acs.jpca.3c04975Journal of Physical Chemistry A, 2023, vol. 127, p. 9944-9958https://doi.org/10.1021/acs.jpca.3c04975cc-by (c) Sousa Romero, Carmen et al., 2023http://creativecommons.org/licenses/by/3.0/es/info:eu-repo/semantics/openAccessoai:recercat.cat:2445/2194472026-05-29T05:05:01Z
dc.title.none.fl_str_mv A Non-orthogonal Configuration Interaction approach to Singlet Fission in Perylenediimide compounds
title A Non-orthogonal Configuration Interaction approach to Singlet Fission in Perylenediimide compounds
spellingShingle A Non-orthogonal Configuration Interaction approach to Singlet Fission in Perylenediimide compounds
Sousa Romero, Carmen
Monòmers
Oligòmers
Fissió nuclear
Monomers
Oligomers
Nuclear fission
title_short A Non-orthogonal Configuration Interaction approach to Singlet Fission in Perylenediimide compounds
title_full A Non-orthogonal Configuration Interaction approach to Singlet Fission in Perylenediimide compounds
title_fullStr A Non-orthogonal Configuration Interaction approach to Singlet Fission in Perylenediimide compounds
title_full_unstemmed A Non-orthogonal Configuration Interaction approach to Singlet Fission in Perylenediimide compounds
title_sort A Non-orthogonal Configuration Interaction approach to Singlet Fission in Perylenediimide compounds
dc.creator.none.fl_str_mv Sousa Romero, Carmen
Sanchez-Mansilla, Aitor
Broer, Ria
Straatsma, T. P.
de Graaf, Coen
author Sousa Romero, Carmen
author_facet Sousa Romero, Carmen
Sanchez-Mansilla, Aitor
Broer, Ria
Straatsma, T. P.
de Graaf, Coen
author_role author
author2 Sanchez-Mansilla, Aitor
Broer, Ria
Straatsma, T. P.
de Graaf, Coen
author2_role author
author
author
author
dc.subject.none.fl_str_mv Monòmers
Oligòmers
Fissió nuclear
Monomers
Oligomers
Nuclear fission
topic Monòmers
Oligòmers
Fissió nuclear
Monomers
Oligomers
Nuclear fission
description Perylenediimide molecules constitute a family of chromophores that undergo singlet fission, a process in which an excited singlet state converts into lower energy triplets on two neighboring molecules, potentially increasing the efficiency of organic solar cells. Here, the nonorthogonal configuration interaction method is applied to study the effect of the different crystal packing of various perylenediimide derivatives on the relative energies of the singlet and triplet states, the intermolecular electronic couplings, and the relative rates for singlet fission. The analysis of the wave functions and electronic couplings reveals that charge transfer states play an important role in the singlet fission mechanism. Dimer conformations where the PDI molecules are at large displacements along the long axis and short on the short axis are posed as the most favorable for singlet fission. The role of the substituent at the imide group has been inspected concluding that, although it has no effect in the energies, for some conformations it significantly influences the electronic couplings, and therefore, replacing this substituent with hydrogen may introduce artifacts in the computational modeling of the PDI molecules.
publishDate 2023
dc.date.none.fl_str_mv 2023
2025
2025
2025
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv https://hdl.handle.net/2445/219447
url https://hdl.handle.net/2445/219447
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv Reproducció del document publicat a: https://doi.org/10.1021/acs.jpca.3c04975
Journal of Physical Chemistry A, 2023, vol. 127, p. 9944-9958
https://doi.org/10.1021/acs.jpca.3c04975
dc.rights.none.fl_str_mv cc-by (c) Sousa Romero, Carmen et al., 2023
http://creativecommons.org/licenses/by/3.0/es/
info:eu-repo/semantics/openAccess
rights_invalid_str_mv cc-by (c) Sousa Romero, Carmen et al., 2023
http://creativecommons.org/licenses/by/3.0/es/
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv 15 p.
application/pdf
application/pdf
dc.publisher.none.fl_str_mv American Chemical Society
publisher.none.fl_str_mv American Chemical Society
dc.source.none.fl_str_mv Articles publicats en revistes (Ciència dels Materials i Química Física)
reponame:Recercat. Dipósit de la Recerca de Catalunya
instname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
instname_str Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
reponame_str Recercat. Dipósit de la Recerca de Catalunya
collection Recercat. Dipósit de la Recerca de Catalunya
repository.name.fl_str_mv
repository.mail.fl_str_mv
_version_ 1869410307241148416
score 15,811543

Similares en LA Referencia