Molecular hyperpolarizabilities strongly depend on the frequency of the excitation light source.  Understanding this frequency dispersion is a prerequisite for interpreting experimental data as well as for designing efficient compounds for NLO applications.  This talk will address several issues related to the description of frequency dispersion by using quantum chemistry methods, namely i) the general analytical forms of the frequency dispersion for both the electronic and vibrational contributions to the hyperpolarizabilities, ii) the range of validity of approximate schemes to describe frequency dispersion (including the so-called multiplicative and additive schemes [1-2]), iii) the reliability of using Kleinman's symmetry conditions [3] when analyzing experimental data to determine first hyperpolarizability tensor components.  Particular emphasis will be put on recent studies on small reference molecules for NLO [4] as well as NLO molecular switches [5]. [1] Sekino, H.; Bartlett, R. J., J. Chem. Phys. 1991,  94, 3665-3669.[2] Rice, J. E.; Handy, N. C., J. Chem. Phys. 1991 , 94, 4959-4971.[3] Kleinman, D. A. Phys. Rev. 1962 , 126, 1977-1979.[4] Castet, F.; Bogdan, E.; Plaquet, A.; Ducasse, L.; Champagne, B.; Rodriguez, V., J. Chem. Phys. 2012 , 136, 024506.[5] Castet, F.; Rodriguez, V., Pozzo, J.L.; Ducasse, L.; Plaquet, A.; Champagne, B.; Acc. Chem. Res. 2013 , 46, 2656-2665.

The "optical" of nonlinear optical properties

248th National Meeting (2014)

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