How Dimerization Through a Spiro Junction Modifies the Nonlinear Optical Properties of a Push–Pull Organic Dye: Insights from Theory and Hyper-Rayleigh Scattering

Frédéric Castet, Timothée Lerychard, Kornelia Pielak, György Szalóki, Clément Dalinot, Philippe Leriche, Lionel Sanguinet, Benoît Champagne, Vincent Rodriguez

Résultats de recherche: Contribution à un journal/une revueArticle

Résumé

The second-order nonlinear optical (NLO) properties of a push–pull monomer, as well as of its dimer composed of two monomeric units connected through a non-conjugated spiro junction, are investigated by means of hyper-Rayleigh scattering (HRS) and quantum chemical calculations. It is shown that dimerization to form a molecule with an orthogonal geometry enhances the first hyperpolarizability by circa 20 % and induces a decrease of the dipolar character of the HRS response. Theoretical calculations correlate well with experimental measurements and allow an in-depth rationalization of the impact of the spiro linkage on the NLO properties through a detailed analysis of the relevant electronic excited states.
langueAnglais
Pages93-101
Nombre de pages9
journalChemPhotoChem
Volume1
Numéro3
Les DOIs
étatPublié - 2017

Empreinte digitale

Rayleigh scattering
Dimerization
Coloring Agents
Optical properties
Excited states
Dimers
Monomers
Molecules
Geometry

mots-clés

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    Castet, Frédéric ; Lerychard, Timothée ; Pielak, Kornelia ; Szalóki, György ; Dalinot, Clément ; Leriche, Philippe ; Sanguinet, Lionel ; Champagne, Benoît ; Rodriguez, Vincent. / How Dimerization Through a Spiro Junction Modifies the Nonlinear Optical Properties of a Push–Pull Organic Dye: Insights from Theory and Hyper-Rayleigh Scattering. Dans: ChemPhotoChem. 2017 ; Vol 1, Numéro 3. p. 93-101
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    abstract = "The second-order nonlinear optical (NLO) properties of a push–pull monomer, as well as of its dimer composed of two monomeric units connected through a non-conjugated spiro junction, are investigated by means of hyper-Rayleigh scattering (HRS) and quantum chemical calculations. It is shown that dimerization to form a molecule with an orthogonal geometry enhances the first hyperpolarizability by circa 20 {\%} and induces a decrease of the dipolar character of the HRS response. Theoretical calculations correlate well with experimental measurements and allow an in-depth rationalization of the impact of the spiro linkage on the NLO properties through a detailed analysis of the relevant electronic excited states.",
    keywords = "hyperpolarizabilities, hyper-Rayleigh scattering, nonlinear optics, quantum chemical calculations, push–pull chromophores",
    author = "Fr{\'e}d{\'e}ric Castet and Timoth{\'e}e Lerychard and Kornelia Pielak and Gy{\"o}rgy Szal{\'o}ki and Cl{\'e}ment Dalinot and Philippe Leriche and Lionel Sanguinet and Beno{\^i}t Champagne and Vincent Rodriguez",
    year = "2017",
    doi = "10.1002/cptc.201600039",
    language = "English",
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    How Dimerization Through a Spiro Junction Modifies the Nonlinear Optical Properties of a Push–Pull Organic Dye: Insights from Theory and Hyper-Rayleigh Scattering. / Castet, Frédéric; Lerychard, Timothée; Pielak, Kornelia; Szalóki, György; Dalinot, Clément; Leriche, Philippe; Sanguinet, Lionel; Champagne, Benoît; Rodriguez, Vincent.

    Dans: ChemPhotoChem, Vol 1, Numéro 3, 2017, p. 93-101.

    Résultats de recherche: Contribution à un journal/une revueArticle

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    T1 - How Dimerization Through a Spiro Junction Modifies the Nonlinear Optical Properties of a Push–Pull Organic Dye: Insights from Theory and Hyper-Rayleigh Scattering

    AU - Castet,Frédéric

    AU - Lerychard,Timothée

    AU - Pielak,Kornelia

    AU - Szalóki,György

    AU - Dalinot,Clément

    AU - Leriche,Philippe

    AU - Sanguinet,Lionel

    AU - Champagne,Benoît

    AU - Rodriguez,Vincent

    PY - 2017

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    AB - The second-order nonlinear optical (NLO) properties of a push–pull monomer, as well as of its dimer composed of two monomeric units connected through a non-conjugated spiro junction, are investigated by means of hyper-Rayleigh scattering (HRS) and quantum chemical calculations. It is shown that dimerization to form a molecule with an orthogonal geometry enhances the first hyperpolarizability by circa 20 % and induces a decrease of the dipolar character of the HRS response. Theoretical calculations correlate well with experimental measurements and allow an in-depth rationalization of the impact of the spiro linkage on the NLO properties through a detailed analysis of the relevant electronic excited states.

    KW - hyperpolarizabilities, hyper-Rayleigh scattering, nonlinear optics, quantum chemical calculations, push–pull chromophores

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