Remarkable two-photon absorption in open-shell singlet systems

Masayoshi Nakano; Kyohei Yoneda; Ryohei Kishi; Hideaki Takahashi; Takashi Kubo; Kenji Kamada; Koji Ohta; Edith Botek; Benòt Champagne

doi:10.1063/1.3225202

Remarkable two-photon absorption in open-shell singlet systems

Masayoshi Nakano, Kyohei Yoneda, Ryohei Kishi, Hideaki Takahashi, Takashi Kubo, Kenji Kamada, Koji Ohta, Edith Botek, Benòt Champagne

Research output: Contribution to journal › Article

49 Citations (Scopus)

Abstract

Remarkable enhancement of two-photon absorption (TPA) peak is theoretically predicted in symmetric open-shell singlet diradical systems with intermediate diradical character as compared to closed-shell and pure diradical systems. It is revealed that the largest TPA peak intensities occur for open-shell singlet diradicals having a ferromagnetically coupled ground state and strongly depend on the ratio between damping factors of the excited states. This result confirms that open-shell singlet conjugated molecules with intermediate diradical characters have precedence over conventional closed-shell conjugated systems in resonant third-order nonlinear optical properties.

Original language	English
Article number	114316
Journal	Journal of Chemical Physics
Volume	131
Issue number	11
DOIs	https://doi.org/10.1063/1.3225202
Publication status	Published - 2009 Dec 1
Externally published	Yes

ASJC Scopus subject areas

Physics and Astronomy(all)
Physical and Theoretical Chemistry

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abstract = "Remarkable enhancement of two-photon absorption (TPA) peak is theoretically predicted in symmetric open-shell singlet diradical systems with intermediate diradical character as compared to closed-shell and pure diradical systems. It is revealed that the largest TPA peak intensities occur for open-shell singlet diradicals having a ferromagnetically coupled ground state and strongly depend on the ratio between damping factors of the excited states. This result confirms that open-shell singlet conjugated molecules with intermediate diradical characters have precedence over conventional closed-shell conjugated systems in resonant third-order nonlinear optical properties.",

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AU - Nakano, Masayoshi

AU - Yoneda, Kyohei

AU - Kishi, Ryohei

AU - Takahashi, Hideaki

AU - Kubo, Takashi

AU - Kamada, Kenji

AU - Ohta, Koji

AU - Botek, Edith

AU - Champagne, Benòt

PY - 2009/12/1

Y1 - 2009/12/1

N2 - Remarkable enhancement of two-photon absorption (TPA) peak is theoretically predicted in symmetric open-shell singlet diradical systems with intermediate diradical character as compared to closed-shell and pure diradical systems. It is revealed that the largest TPA peak intensities occur for open-shell singlet diradicals having a ferromagnetically coupled ground state and strongly depend on the ratio between damping factors of the excited states. This result confirms that open-shell singlet conjugated molecules with intermediate diradical characters have precedence over conventional closed-shell conjugated systems in resonant third-order nonlinear optical properties.

AB - Remarkable enhancement of two-photon absorption (TPA) peak is theoretically predicted in symmetric open-shell singlet diradical systems with intermediate diradical character as compared to closed-shell and pure diradical systems. It is revealed that the largest TPA peak intensities occur for open-shell singlet diradicals having a ferromagnetically coupled ground state and strongly depend on the ratio between damping factors of the excited states. This result confirms that open-shell singlet conjugated molecules with intermediate diradical characters have precedence over conventional closed-shell conjugated systems in resonant third-order nonlinear optical properties.

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