Articles producció científica> Química Física i Inorgànica

Effect of Second-Order Spin-Orbit Coupling on the Interaction between Spin States in Spin-Crossover Systems.

  • Identification data

    Identifier: imarina:3997963
    Authors:
    Sousa C, Domingo A, de Graaf C
    Abstract:
    The second-order spin-orbit coupling is evaluated in two transition-metal complexes to establish the effect on the deactivation mechanism of the excited low-spin state in systems that undergo spin transitions under the influence of light. We compare the standard perturbational approach to calculate the second-order interaction with a variational strategy based on the effective Hamiltonian theory and show that the former one can only be applied in some special cases and even then gives results that largely overestimate the interaction. The combined effect of geometry distortions and second-order spin-orbit coupling leads to sizeable interactions for states that are nearly uncoupled in the symmetric (average) structure of the complex. This opens the possibility of a direct deactivation from the singlet and triplet states of the metal-to-ligand charge-transfer manifold to the final high-spin state as suggested from the interpretation of experimental data but so far not supported by theoretical descriptions of the light-induced spin crossover.© 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.
  • Others:

    Author, as appears in the article.: Sousa C, Domingo A, de Graaf C
    Department: Química Física i Inorgànica
    URV's Author/s: De Graaf, Cornelis / Domingo Palau, Anna Maria
    Keywords: Transition-metal Spin crossover Single-molecule magnets Second-order spin-orbit coupling Opbe Light-induced magnetism Femtochemistry Energetics Electronic-structure Dynamics Complexes Charge Ab initio calculations
    Abstract: The second-order spin-orbit coupling is evaluated in two transition-metal complexes to establish the effect on the deactivation mechanism of the excited low-spin state in systems that undergo spin transitions under the influence of light. We compare the standard perturbational approach to calculate the second-order interaction with a variational strategy based on the effective Hamiltonian theory and show that the former one can only be applied in some special cases and even then gives results that largely overestimate the interaction. The combined effect of geometry distortions and second-order spin-orbit coupling leads to sizeable interactions for states that are nearly uncoupled in the symmetric (average) structure of the complex. This opens the possibility of a direct deactivation from the singlet and triplet states of the metal-to-ligand charge-transfer manifold to the final high-spin state as suggested from the interpretation of experimental data but so far not supported by theoretical descriptions of the light-induced spin crossover.© 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.
    Thematic Areas: Química Organic chemistry Medicina i Materiais Interdisciplinar General medicine General chemistry Farmacia Engenharias iii Engenharias ii Ciências biológicas iii Ciências biológicas ii Ciências biológicas i Ciências agrárias i Chemistry, multidisciplinary Chemistry (miscellaneous) Chemistry (all) Chemistry Catalysis Biotecnología Biodiversidade Astronomia / física
    licence for use: https://creativecommons.org/licenses/by/3.0/es/
    ISSN: 15213765
    Author's mail: coen.degraaf@urv.cat annamaria.domingo@estudiants.urv.cat
    Author identifier: 0000-0001-8114-6658
    Record's date: 2024-09-07
    Papper version: info:eu-repo/semantics/acceptedVersion
    Link to the original source: https://chemistry-europe.onlinelibrary.wiley.com/doi/full/10.1002/chem.201704854
    Licence document URL: https://repositori.urv.cat/ca/proteccio-de-dades/
    Papper original source: Chemistry-A European Journal. 24 (20): 5146-5152
    APA: Sousa C, Domingo A, de Graaf C (2018). Effect of Second-Order Spin-Orbit Coupling on the Interaction between Spin States in Spin-Crossover Systems.. Chemistry-A European Journal, 24(20), 5146-5152. DOI: 10.1002/chem.201704854
    Article's DOI: 10.1002/chem.201704854
    Entity: Universitat Rovira i Virgili
    Journal publication year: 2018
    Publication Type: Journal Publications
  • Keywords:

    Catalysis,Chemistry,Chemistry (Miscellaneous),Chemistry, Multidisciplinary,Organic Chemistry
    Transition-metal
    Spin crossover
    Single-molecule magnets
    Second-order spin-orbit coupling
    Opbe
    Light-induced magnetism
    Femtochemistry
    Energetics
    Electronic-structure
    Dynamics
    Complexes
    Charge
    Ab initio calculations
    Química
    Organic chemistry
    Medicina i
    Materiais
    Interdisciplinar
    General medicine
    General chemistry
    Farmacia
    Engenharias iii
    Engenharias ii
    Ciências biológicas iii
    Ciências biológicas ii
    Ciências biológicas i
    Ciências agrárias i
    Chemistry, multidisciplinary
    Chemistry (miscellaneous)
    Chemistry (all)
    Chemistry
    Catalysis
    Biotecnología
    Biodiversidade
    Astronomia / física
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