title: Finite-field method with unbiased polarizable continuum model for evaluation of the second hyperpolarizability of an open-shell singlet molecule in solvents.
abstract: The static second hyperpolarizability γ of the complexes composed of open-shell singlet 1,3-dipole molecule involving a boron atom and a water molecule in aqueous phase are investigated by the finite-field (FF) method combined with a standard polarized continuum model (PCM) and with a newly proposed unbiased PCM (UBPCM). On the basis of the comparison with the results calculated by the FF method using the full quantum and the quantum-mechanical/molecular-mechanical and molecular-dynamics (QM/MM-MD) treatments, the present FF-UBPCM method is demonstrated to remedy the artificial overestimation of the γ caused by standard FF-PCM calculations and to well reproduce the FF-QM/MM-MD and FF-full-QM results with much lower costs.
authors.affiliation: Department of Materials Engineering Science, Graduate School of Engineering Science, Osaka University, Toyonaka, Osaka, 560-8531, Japan.
authors.forename: Tomoya
authors.initials: T
authors.lastname: Inui
authors.forename: Yasuteru
authors.initials: Y
authors.lastname: Shigeta
authors.forename: Katsuki
authors.initials: K
authors.lastname: Okuno
authors.forename: Takeshi
authors.initials: T
authors.lastname: Baba
authors.forename: Ryohei
authors.initials: R
authors.lastname: Kishi
authors.forename: Masayoshi
authors.initials: M
authors.lastname: Nakano
keywords: finite field method; hyperpolarizability; nonlinear optical properties; polarizable continuum model; quantum-mechanical/MM; solvent effects