title: NLO properties of metallabenzene-based chromophores: a time-dependent density functional study.
abstract: The static and dynamic first hyperpolarizabilities for a series of substituted metallabenzene-based nonlinear optical (NLO) chromophores were determined by time-dependent density functional theory (TDDFT). The electronic excitation contributions to the first hyperpolarizability are rationalized in terms of the two-level model. The effects on the hyperpolarizabilities of (a) the metal center (Os, Ir, Pt); (b) the ligand environment (PH3, CO, Cl); (c) various donor and acceptor substituents (NH2, OH, Me, H, Cl, Br, I, COOMe, COOH, CN, NO2); and (d) the length of pi-conjugation were studied. Our calculations predict that metallabenzenes have significant second-order NLO susceptibilities, ranging from = 1.0 x 10(-29) to 5.6 x 10(-28) esu and from mu = 3.0 x 10(-47) to 1.1 x 10(-44) esu, that can be tuned by changing the metal center and/or ligand environment.
authors.affiliation: Department of Organic Chemistry, Weizmann Institute of Science, 76100 Rehovot, Israel.
authors.forename: Amir
authors.initials: A
authors.lastname: Karton
authors.forename: Mark A
authors.initials: MA
authors.lastname: Iron
authors.forename: Milko E
authors.initials: ME
authors.lastname: van der Boom
authors.forename: Jan M L
authors.initials: JM
authors.lastname: Martin