Electron donor solvent effects on the (hyper) polarizabilities of a solute presenting singlet diradical character

Hideaki Takahashi, Kazuki Kubota, Hitoshi Fukui, Sean Bonness, Kyohei Yoneda, Ryohei Kishi, Takashi Kubo, Kenji Kamada, Koji Ohta, Benoît Champagne, Edith Botek, Masayoshi Nakano

研究成果: Conference contribution

2 被引用数 (Scopus)

抄録

We study the (hyper)polarizabilities of a singlet diradical molecule (2-borapropane-1,3-diyl) which contains a boron atom. For the purpose to control the (hyper)polarizabilities by tuning the diradical character of the boron compound, we employ water solvent as an electron donor to the boron atom. A series of quantum chemical calculations reveal that the electron donation from the lone pair of electrons in a water molecule to the vacant p orbital of boron atom gives rise to the increase of the diradical character, leading to the large variation of the polarizability of the molecule. We also investigate the solvation effects of the bulk water by utilizing the polarizable continuum model (PCM). It is shown that the PCM environment significantly increases the degree of enhancement of the second hyperpolarizability in the intermediate diradical regime of the compound. These results suggest that a singlet diradical boron compound immersed in an electron donor solvent can exhibit efficient third-order nonlinear optical properties, which can be tuned by designing the solute-solvent interactions. We examine the reliability of the PCM results by performing the additional QM/MM simulations. It is found that the QM/MM solvation effects slightly decrease the polarizability in contrast to the PCM calculation, which implies the possibility that PCM tends to overestimate the polarizability due to the lack of the ability to represent the solvation structures.

本文言語English
ホスト出版物のタイトルInternational Conference of Computational Methods in Sciences and Engineering 2009, ICCMSE 2009
ページ899-902
ページ数4
DOI
出版ステータスPublished - 2012
外部発表はい
イベントInternational Conference of Computational Methods in Sciences and Engineering 2009, ICCMSE 2009 - Rhodes, Greece
継続期間: 2009 9月 292009 10月 4

出版物シリーズ

名前AIP Conference Proceedings
1504
ISSN(印刷版)0094-243X
ISSN(電子版)1551-7616

Other

OtherInternational Conference of Computational Methods in Sciences and Engineering 2009, ICCMSE 2009
国/地域Greece
CityRhodes
Period09/9/2909/10/4

ASJC Scopus subject areas

  • 物理学および天文学(全般)

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