Autor según el artículo: Sousa, C; Sánchez-Mansilla, A; Broer, R; Straatsma, TP; de Graaf, C
Departamento: Química Física i Inorgànica
Autor/es de la URV: De Graaf, Cornelis / Sánchez Mansilla, Aitor María
Palabras clave: Charge-transfer states valence thin-films tetracene exciton fission exchange-energy electronic couplings dimers design approximation
Resumen: 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.
Áreas temáticas: Química Physics, atomic, molecular & chemical Physical and theoretical chemistry Odontología Medicine (miscellaneous) Medicina ii Medicina i Materiais Interdisciplinar Geociências General medicine Farmacia Ensino Engenharias iv Engenharias iii Engenharias ii Ciências biológicas ii Ciências biológicas i Ciências ambientais Ciências agrárias i Chemistry, physical Biotecnología Biodiversidade Astronomia / física
Acceso a la licencia de uso: https://creativecommons.org/licenses/by/3.0/es/
Direcció de correo del autor: coen.degraaf@urv.cat aitor.sanchezm@estudiants.urv.cat
Identificador del autor: 0000-0001-8114-6658
Fecha de alta del registro: 2024-08-03
Versión del articulo depositado: info:eu-repo/semantics/publishedVersion
Enlace a la fuente original: https://pubs.acs.org/doi/full/10.1021/acs.jpca.3c04975
URL Documento de licencia: https://repositori.urv.cat/ca/proteccio-de-dades/
Referencia al articulo segun fuente origial: Journal Of Physical Chemistry a. 127 (47): 9944-9958
Referencia de l'ítem segons les normes APA: Sousa, C; Sánchez-Mansilla, A; Broer, R; Straatsma, TP; de Graaf, C (2023). A Nonorthogonal Configuration Interaction Approach to Singlet Fission in Perylenediimide Compounds. Journal Of Physical Chemistry a, 127(47), 9944-9958. DOI: 10.1021/acs.jpca.3c04975
DOI del artículo: 10.1021/acs.jpca.3c04975
Entidad: Universitat Rovira i Virgili
Año de publicación de la revista: 2023
Tipo de publicación: Journal Publications