Second hyperpolarizabilities (gamma) of bisimidazole and bistriazole benzenes: diradical character, charged state, and spin state dependences.
The second hyperpolarizabilities of bisimidazole- and bistriazole-benzene compounds have been calculated at different levels of approximation to unravel the effects of diradical character as well as of charge and spin multiplicity. The largest second hyperpolarizabilities are associated with intermediate diradical character, provided positive charging does not compensate for this effect. For the neutral diradical bisimidazole compound, the singlet diradical species possesses a second hyperpolarizability two to three times larger than the corresponding triplet, demonstrating the possibility of spin state control of the third-order NLO responses for diradical species.
Nakano
Masayoshi
M
Department of Materials Engineering Science, Graduate School of Engineering Science, Osaka University, Toyonaka, Osaka 560-8531, Japan. mnaka@cheng.es.osaka-u.ac.jp
Kishi
Ryohei
R
Nakagawa
Nozomi
N
Ohta
Suguru
S
Takahashi
Hideaki
H
Furukawa
Shin-Ichi
S
Kamada
Kenji
K
Ohta
Koji
K
Champagne
Benoît
B
Botek
Edith
E
Yamada
Satoru
S
Yamaguchi
Kizashi
K
D001555:Benzene Derivatives / Q000737:chemistry*; D003198:Computer Simulation; D005609:Free Radicals / Q000737:chemistry; D007093:Imidazoles / Q000737:chemistry*; D008956:Models, Chemical; D015394:Molecular Structure; D011789:Quantum Theory; D014230:Triazoles / Q000737:chemistry*
D001555:Benzene Derivatives; D005609:Free Radicals; D007093:Imidazoles; D014230:Triazoles