Articles producció científica> Química Física i Inorgànica

Influence of the crystal packing in singlet fission: one step beyond the gas phase approximation

  • Datos identificativos

    Identificador: imarina:9216301
    Autores:
    Aguilar Suarez, Luis Enriquede Graaf, CoenFaraji, Shirin
    Resumen:
    Singlet fission (SF), a multiexciton generation process, has been proposed as an alternative to enhance the performance of solar cells. The gas phase dimer model has shown its utility to study this process, but it does not always cover all the physics and the effect of the surrounding atoms has to be included in such cases. In this contribution, we explore the influence of crystal packing on the electronic couplings, and on the so-called exciton descriptors and electron-hole correlation plots. We have studied three tetracene dimers extracted from the crystal structure, as well as several dimers and trimers of the alpha and beta polymorphs of 1,3-diphenylisobenzofuran (DPBF). These polymorphs show different SF yields. Our results highlight that the character of the excited states of tetracene depends on both the mutual disposition of molecules and inclusion of the environment. The latter does however not change significantly the interpretation of the SF mechanism in the studied systems. For DPBF, we establish how the excited state analysis is able to pinpoint differences between the polymorphs. We observe strongly bound correlated excitons in the beta polymorph which might hinder the formation of the (TT)-T-1 state and, consequently, explain its low SF yield.
  • Otros:

    Autor según el artículo: Aguilar Suarez, Luis Enrique; de Graaf, Coen; Faraji, Shirin;
    Departamento: Química Física i Inorgànica
    Autor/es de la URV: De Graaf, Cornelis
    Palabras clave: Thin-film Tetracene State analysis State Singlet fission Pentacene Nonorthogonal configuration-interaction Multiexciton generation Molecules Model Mechanism Gases Excitons Exciton fission Excited states Electronic coupling Electron-hole correlation Dimers Dimer model Descriptors Crystal structure Crystal packings Charge-transfer
    Resumen: Singlet fission (SF), a multiexciton generation process, has been proposed as an alternative to enhance the performance of solar cells. The gas phase dimer model has shown its utility to study this process, but it does not always cover all the physics and the effect of the surrounding atoms has to be included in such cases. In this contribution, we explore the influence of crystal packing on the electronic couplings, and on the so-called exciton descriptors and electron-hole correlation plots. We have studied three tetracene dimers extracted from the crystal structure, as well as several dimers and trimers of the alpha and beta polymorphs of 1,3-diphenylisobenzofuran (DPBF). These polymorphs show different SF yields. Our results highlight that the character of the excited states of tetracene depends on both the mutual disposition of molecules and inclusion of the environment. The latter does however not change significantly the interpretation of the SF mechanism in the studied systems. For DPBF, we establish how the excited state analysis is able to pinpoint differences between the polymorphs. We observe strongly bound correlated excitons in the beta polymorph which might hinder the formation of the (TT)-T-1 state and, consequently, explain its low SF yield.
    Áreas temáticas: Química Physics, atomic, molecular & chemical Physics and astronomy (miscellaneous) Physics and astronomy (all) Physical and theoretical chemistry Odontología Medicina ii Medicina i Materiais Matemática / probabilidade e estatística Interdisciplinar Geociências General physics and astronomy General medicine Farmacia Ensino Engenharias iv Engenharias iii Engenharias ii Ciências biológicas ii Ciências biológicas i Ciências ambientais Ciências agrárias i Ciência de alimentos Ciência da computação 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
    Identificador del autor: 0000-0001-8114-6658
    Página final: 14177
    Fecha de alta del registro: 2024-07-27
    Volumen de revista: 23
    Versión del articulo depositado: info:eu-repo/semantics/publishedVersion
    Enlace a la fuente original: https://pubs.rsc.org/en/content/articlelanding/2021/CP/D1CP00298H#!divAbstract
    URL Documento de licencia: https://repositori.urv.cat/ca/proteccio-de-dades/
    Referencia al articulo segun fuente origial: Physical Chemistry Chemical Physics. 23 (26): 14164-14177
    Referencia de l'ítem segons les normes APA: Aguilar Suarez, Luis Enrique; de Graaf, Coen; Faraji, Shirin; (2021). Influence of the crystal packing in singlet fission: one step beyond the gas phase approximation. Physical Chemistry Chemical Physics, 23(26), 14164-14177. DOI: 10.1039/d1cp00298h
    DOI del artículo: 10.1039/d1cp00298h
    Entidad: Universitat Rovira i Virgili
    Año de publicación de la revista: 2021
    Página inicial: 14164
    Tipo de publicación: Journal Publications
  • Palabras clave:

    Chemistry, Physical,Physical and Theoretical Chemistry,Physics and Astronomy (Miscellaneous),Physics, Atomic, Molecular & Chemical
    Thin-film
    Tetracene
    State analysis
    State
    Singlet fission
    Pentacene
    Nonorthogonal configuration-interaction
    Multiexciton generation
    Molecules
    Model
    Mechanism
    Gases
    Excitons
    Exciton fission
    Excited states
    Electronic coupling
    Electron-hole correlation
    Dimers
    Dimer model
    Descriptors
    Crystal structure
    Crystal packings
    Charge-transfer
    Química
    Physics, atomic, molecular & chemical
    Physics and astronomy (miscellaneous)
    Physics and astronomy (all)
    Physical and theoretical chemistry
    Odontología
    Medicina ii
    Medicina i
    Materiais
    Matemática / probabilidade e estatística
    Interdisciplinar
    Geociências
    General physics and astronomy
    General medicine
    Farmacia
    Ensino
    Engenharias iv
    Engenharias iii
    Engenharias ii
    Ciências biológicas ii
    Ciências biológicas i
    Ciências ambientais
    Ciências agrárias i
    Ciência de alimentos
    Ciência da computação
    Chemistry, physical
    Biotecnología
    Biodiversidade
    Astronomia / física
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