We have measured the tensor components c1111 and c1221 of third‐order nonlinear optical susceptibility of two nematic liquid crystals, MBBA (p‐methoxy‐benzylidene p‐n‐butylaniline) and EBBA (p‐ethoxy‐benzylidene p‐n‐butylaniline), in the picosecond regime. We observed that the molecule with ethoxy group (EBBA) has a larger third‐order nonlinearity than the one with methoxy group (MBBA) and present a model to explain this effect.
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