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Second Harmonic Generation in an Optically Active Liquid: Experimental Observation of a Fourth-Order Optical Nonlinearity Due to Molecular Chirality

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Abstract

Molecular left-right asymmetry is an origin of non-vanishing even order optical nonlinear susceptibilities of non-racemic solutions of chiral molecules. Though second harmonic generation (SHG) due to quadratic dipolar nonlinearity is still symmetry forbidden in optically active liquids yet we have succeeded in experimental observation, for the first time, of noncolli-near SHG due to five-mixing process according to a scheme 2ω=3ωω, governed by a fourth order susceptibility tensor χ(4)D(2ω;ω,ω,ω,−ω) SH signal is found to be well collimated and quasi phase-matched, it shows theoretically predicted polarization, spectral and temporal properties.

© 1992 Optical Society of America

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