期刊
CHEMPHYSCHEM
卷 15, 期 12, 页码 2575-2581出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cphc.201402083
关键词
dyes/pigments; hyperpolarizability; merocyanines; nonlinear optics; quantum chemistry
资金
- CNRS (Chemistry Department)
- Region Aquitaine
- Conseil Regional d'Aquitaine
- French Ministry of Research and Technology
Hyper-Rayleigh scattering experiments and quantum chemical calculations are combined to investigate the second-order nonlinear optical responses of a series of three-arm merocyanine derivatives. They exhibit an octupolar hyperpolarizability response with lower amplitude than crystal violet due to a lower extent of the photoinduced charge transfer and reduced bond length alternation. Strong effects on the second-order optical response measured close to the two-photon absorption level are clearly evidenced; for example, the effective measured polarization ratio deviates below the ideal octupolar value of 3/2 even at very low excitation power. These effects are attributed to two-photon absorption resonance, which we believe modifies dynamically the population of the ground state versus that of the excited state.
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