Articles producció científica> Química Física i Inorgànica

Non-orthogonal Configuration Interaction Study on the Effect of Thermal Distortions on the Singlet Fission Process in Photoexcited Pure and B,N-Doped Pentacene Crystals

  • Identification data

    Identifier: imarina:9327605
  • Authors:

    López, X
    Straatsma, TP
    Sánchez-Mansilla, A
    de Graaf, C
  • Others:

    Author, as appears in the article.: López, X; Straatsma, TP; Sánchez-Mansilla, A; de Graaf, C
    Department: Química Física i Inorgànica
    URV's Author/s: De Graaf, Cornelis / López Fernández, Javier / Sánchez Mansilla, Aitor María
    Keywords: Transition Total-energy calculations States Initio molecular-dynamics Efficiency
    Abstract: The present computational work analyzes singlet fission(SF) asa pathway for multiplication of photogenerated excitons in crystallinepolyacenes. Our study explores the well-known crystalline pentacene(C22H14) and the prospective and potentiallyinteresting doped B,N-pentacene (BC20NH14).At the molecular level, the singlet fission process involves a pairof neighboring molecules and is based on the coupling between an excitedsinglet state (S1S0) and two singlet-coupledtriplets ((T1T1)-T-1), which, typically,is influenced by an intermolecular charge transfer state. Taking datafrom periodic density functional theory and ab initio wave functioncalculations, we applied the non-orthogonal configuration interactionmethod to determine electronic coupling parameters. The comparisonof the results for both equilibrium structures reveal smaller SF couplingfor pentacene than for B,N-pentacene by a factor of & SIM;5. Introductionof the dynamic behavior to the crystals (vibrations, thermal motion)provides a more realistic picture of the effect of the disorder atthe molecular level on the SF efficiency. The coupling values associatedto out-of-equilibrium structures show that most of the S1S0/(T1T1)-T-1 couplings remainvirtually constant or slightly increase for pentacene when moleculardisorder is introduced. Homologous calculations on B,N-pentacene showa generalized decrease in the coupling values, notably if large phonondisplacements are considered. A few of the structures analyzed featuremuch larger SF coupling if some distortion results in (nearly) degeneratecharge transfer and excited singlet and triplet states. For theseparticular situations, an acceleration of the SF process could occuralthough in competition with electron-hole separation as analternative pathway.
    Thematic Areas: Surfaces, coatings and films Química Physical and theoretical chemistry Nanoscience and nanotechnology Nanoscience & nanotechnology Medicina ii Medicina i Materials science, multidisciplinary Materiais Interdisciplinar General energy Farmacia Ensino Engenharias iv Engenharias iii Engenharias ii Engenharias i Energy (miscellaneous) Energy (all) Electronic, optical and magnetic materials Ciências biológicas iii Ciências biológicas ii Ciências biológicas i Ciências ambientais Ciências agrárias i Chemistry, physical Biotecnología Biodiversidade Astronomia / física
    licence for use: https://creativecommons.org/licenses/by/3.0/es/
    Author's mail: coen.degraaf@urv.cat aitor.sanchezm@estudiants.urv.cat javier.lopez@urv.cat
    Author identifier: 0000-0001-8114-6658 0000-0003-0322-6796
    Record's date: 2024-07-20
    Papper version: info:eu-repo/semantics/publishedVersion
    Link to the original source: https://pubs.acs.org/doi/10.1021/acs.jpcc.3c02083
    Licence document URL: http://repositori.urv.cat/ca/proteccio-de-dades/
    Papper original source: Journal Of Physical Chemistry c.
    APA: López, X; Straatsma, TP; Sánchez-Mansilla, A; de Graaf, C (2023). Non-orthogonal Configuration Interaction Study on the Effect of Thermal Distortions on the Singlet Fission Process in Photoexcited Pure and B,N-Doped Pentacene Crystals. Journal Of Physical Chemistry c, (), -. DOI: 10.1021/acs.jpcc.3c02083
    Article's DOI: 10.1021/acs.jpcc.3c02083
    Entity: Universitat Rovira i Virgili
    Journal publication year: 2023
    Publication Type: Journal Publications
  • Keywords:

    Chemistry, Physical,Electronic, Optical and Magnetic Materials,Energy (Miscellaneous),Materials Science, Multidisciplinary,Nanoscience & Nanotechnology,Nanoscience and Nanotechnology,Physical and Theoretical Chemistry,Surfaces, Coatings and Films
    Transition
    Total-energy calculations
    States
    Initio molecular-dynamics
    Efficiency
    Surfaces, coatings and films
    Química
    Physical and theoretical chemistry
    Nanoscience and nanotechnology
    Nanoscience & nanotechnology
    Medicina ii
    Medicina i
    Materials science, multidisciplinary
    Materiais
    Interdisciplinar
    General energy
    Farmacia
    Ensino
    Engenharias iv
    Engenharias iii
    Engenharias ii
    Engenharias i
    Energy (miscellaneous)
    Energy (all)
    Electronic, optical and magnetic materials
    Ciências biológicas iii
    Ciências biológicas ii
    Ciências biológicas i
    Ciências ambientais
    Ciências agrárias i
    Chemistry, physical
    Biotecnología
    Biodiversidade
    Astronomia / física
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