Articles producció científica> Química Física i Inorgànica

A Nonorthogonal Configuration Interaction Approach to Singlet Fission in Perylenediimide Compounds

  • Datos identificativos

    Identificador: imarina:9332031
    Autores:
    Sousa, CSánchez-Mansilla, ABroer, RStraatsma, TPde Graaf, C
    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.
  • Otros:

    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
  • Palabras clave:

    Chemistry, Physical,Medicine (Miscellaneous),Physical and Theoretical Chemistry,Physics, Atomic, Molecular & Chemical
    Charge-transfer states
    valence
    thin-films
    tetracene
    exciton fission
    exchange-energy
    electronic couplings
    dimers
    design
    approximation
    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
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