FREQUENCY-DEPENDENT HYPERPOLARIZABILITIES OF POLYYNES

被引:31
作者
JASZUNSKI, M
JORGENSEN, P
KOCH, H
AGREN, H
HELGAKER, T
机构
[1] LINKOPING UNIV,INST PHYS & MEASUREMENT TECHNOL,S-58183 LINKOPING,SWEDEN
[2] UNIV OSLO,DEPT CHEM,N-0315 OSLO,NORWAY
[3] POLISH ACAD SCI,INST ORGAN CHEM,PL-01224 WARSAW,POLAND
关键词
D O I
10.1063/1.464714
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Ab initio calculations have been performed for the static and dynamic polarizability and hyperpolarizability for a series of polyynes C2nH2 using self-consistent field (SCF) (n = 1-6) and multiconfiguration self-consistent field (MCSCF) (n = 1-4) wave functions. We have considered the longitudinal component of the static hyperpolarizability and the same component of the dynamic hyperpolarizability measured in electric-field induced second harmonic generation gamma(ESHG) = gamma(-2omega;omega,omega,0). The frequency dependence of the polarizability and hyperpolarizability has been rationalized in terms of the coefficients in expansions in omega2. The static hyperpolarizabilities vary smoothly with the chain length and satisfy gamma (C2nH2) = gamma(C2H2) X n(X), where X almost-equal-to 3.0. The dynamic hyperpolarizability satisfies a similar relation where X in creases slowly with omega.
引用
收藏
页码:7229 / 7235
页数:7
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