Theoretical Study on the Enhancement of the Second Hyperpolarizabilities of Si-, Ge-Disubstituted Quinodimethanes: Synergy Effects of Open-Shell Nature and Intramolecular Charge Transfer
| Autor: | Takeshi Nozawa, Masayoshi Nakano, Kotaro Fukuda, Masaaki Ichinohe, Akira Sekiguchi, Hiroko Yotsuyanagi |
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| Rok vydání: | 2015 |
| Předmět: |
Chemistry
Model study Charge (physics) Surfaces Coatings and Films Electronic Optical and Magnetic Materials Nonlinear optical Transfer (group theory) General Energy Main group element Chemical physics Computational chemistry Intramolecular force Singlet state Physical and Theoretical Chemistry Open shell |
| Zdroj: | The Journal of Physical Chemistry C. 119:1188-1193 |
| ISSN: | 1932-7455 1932-7447 |
| DOI: | 10.1021/jp511521m |
| Popis: | We have investigated the second hyperpolarizabilities (γ), that is, the third-order nonlinear optical (NLO) properties at the molecular scale, of the realistic Si- and Ge-disubstituted para- and meta-quinodimethanes from the viewpoint of synergy effect of the open-shell singlet nature and the donor (D)−π–donor (D) intramolecular charge transfer (ICT). It has been revealed that the disubstituted para isomers exhibit strong D−π–D nature together with the intermediate open-shell singlet nature, which leads to their significantly enhanced γ values. These results well demonstrate the validity of our recent result of the theoretical model study on para-quinodimethane with point charges, and also present a new design strategy based on the concept of open-shell NLO that the replacement of the radical site of the π-conjugated carbon framework with the heavier main group elements induces both the larger open-shell singlet nature and the D−π–D type strong ICT, both of which synergetically contribute to the further e... |
| Databáze: | OpenAIRE |
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