Origin of the enhancement of the second hyperpolarizability of singlet diradical systems with intermediate diradical character

Masayoshi Nakano, Ryohei Kishi, Suguru Ohta, Akihito Takebe, Hideaki Takahashi, Shin Ichi Furukawa, Takashi Kubo, Yasushi Morita, Kazuhiro Nakasuji, Kizashi Yamaguchi, Kenji Kamada, Koji Ohta, Benoît Champagne, Edith Botek

Résultats de recherche: Contribution à un journal/une revueArticle

Résumé

The origin of the diradical character dependence of the second hyperpolarizability (γ) of neutral singlet diradical systems is clarified based on the perturbation formula of γ using the simplest diradical molecular model with different diradical characters, i.e., H2 under bond dissociation. The enhancement of γ in the intermediate diradical character region turns out to originate from the increasing magnitude of the transition moment between the first and second excited states and the decrease of that between the ground and first excited states, respectively, with the increase in diradical character. This feature confirms that open-shell singlet conjugated molecules with intermediate diradical characters constitute a new class of third-order nonlinear optical systems, whose γ values can be controlled by the diradical character in addition to the conjugation length.

langue originaleAnglais
Numéro d'article074113
journalThe journal of chemical physics
Volume125
Numéro de publication7
Les DOIs
étatPublié - 28 août 2006

Empreinte digitale

Excited states
augmentation
Electron transitions
conjugation
Optical systems
excitation
dissociation
moments
perturbation
Molecules
molecules

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Nakano, Masayoshi ; Kishi, Ryohei ; Ohta, Suguru ; Takebe, Akihito ; Takahashi, Hideaki ; Furukawa, Shin Ichi ; Kubo, Takashi ; Morita, Yasushi ; Nakasuji, Kazuhiro ; Yamaguchi, Kizashi ; Kamada, Kenji ; Ohta, Koji ; Champagne, Benoît ; Botek, Edith. / Origin of the enhancement of the second hyperpolarizability of singlet diradical systems with intermediate diradical character. Dans: The journal of chemical physics. 2006 ; Vol 125, Numéro 7.
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title = "Origin of the enhancement of the second hyperpolarizability of singlet diradical systems with intermediate diradical character",
abstract = "The origin of the diradical character dependence of the second hyperpolarizability (γ) of neutral singlet diradical systems is clarified based on the perturbation formula of γ using the simplest diradical molecular model with different diradical characters, i.e., H2 under bond dissociation. The enhancement of γ in the intermediate diradical character region turns out to originate from the increasing magnitude of the transition moment between the first and second excited states and the decrease of that between the ground and first excited states, respectively, with the increase in diradical character. This feature confirms that open-shell singlet conjugated molecules with intermediate diradical characters constitute a new class of third-order nonlinear optical systems, whose γ values can be controlled by the diradical character in addition to the conjugation length.",
author = "Masayoshi Nakano and Ryohei Kishi and Suguru Ohta and Akihito Takebe and Hideaki Takahashi and Furukawa, {Shin Ichi} and Takashi Kubo and Yasushi Morita and Kazuhiro Nakasuji and Kizashi Yamaguchi and Kenji Kamada and Koji Ohta and Beno{\^i}t Champagne and Edith Botek",
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Nakano, M, Kishi, R, Ohta, S, Takebe, A, Takahashi, H, Furukawa, SI, Kubo, T, Morita, Y, Nakasuji, K, Yamaguchi, K, Kamada, K, Ohta, K, Champagne, B & Botek, E 2006, 'Origin of the enhancement of the second hyperpolarizability of singlet diradical systems with intermediate diradical character', The journal of chemical physics, VOL. 125, Numéro 7, 074113. https://doi.org/10.1063/1.2213974

Origin of the enhancement of the second hyperpolarizability of singlet diradical systems with intermediate diradical character. / Nakano, Masayoshi; Kishi, Ryohei; Ohta, Suguru; Takebe, Akihito; Takahashi, Hideaki; Furukawa, Shin Ichi; Kubo, Takashi; Morita, Yasushi; Nakasuji, Kazuhiro; Yamaguchi, Kizashi; Kamada, Kenji; Ohta, Koji; Champagne, Benoît; Botek, Edith.

Dans: The journal of chemical physics, Vol 125, Numéro 7, 074113, 28.08.2006.

Résultats de recherche: Contribution à un journal/une revueArticle

TY - JOUR

T1 - Origin of the enhancement of the second hyperpolarizability of singlet diradical systems with intermediate diradical character

AU - Nakano, Masayoshi

AU - Kishi, Ryohei

AU - Ohta, Suguru

AU - Takebe, Akihito

AU - Takahashi, Hideaki

AU - Furukawa, Shin Ichi

AU - Kubo, Takashi

AU - Morita, Yasushi

AU - Nakasuji, Kazuhiro

AU - Yamaguchi, Kizashi

AU - Kamada, Kenji

AU - Ohta, Koji

AU - Champagne, Benoît

AU - Botek, Edith

PY - 2006/8/28

Y1 - 2006/8/28

N2 - The origin of the diradical character dependence of the second hyperpolarizability (γ) of neutral singlet diradical systems is clarified based on the perturbation formula of γ using the simplest diradical molecular model with different diradical characters, i.e., H2 under bond dissociation. The enhancement of γ in the intermediate diradical character region turns out to originate from the increasing magnitude of the transition moment between the first and second excited states and the decrease of that between the ground and first excited states, respectively, with the increase in diradical character. This feature confirms that open-shell singlet conjugated molecules with intermediate diradical characters constitute a new class of third-order nonlinear optical systems, whose γ values can be controlled by the diradical character in addition to the conjugation length.

AB - The origin of the diradical character dependence of the second hyperpolarizability (γ) of neutral singlet diradical systems is clarified based on the perturbation formula of γ using the simplest diradical molecular model with different diradical characters, i.e., H2 under bond dissociation. The enhancement of γ in the intermediate diradical character region turns out to originate from the increasing magnitude of the transition moment between the first and second excited states and the decrease of that between the ground and first excited states, respectively, with the increase in diradical character. This feature confirms that open-shell singlet conjugated molecules with intermediate diradical characters constitute a new class of third-order nonlinear optical systems, whose γ values can be controlled by the diradical character in addition to the conjugation length.

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