ABSTRACTWe investigated the third-order nonlinear optical response of a Gay-Berne system at the isotropic, nematic, and smectic phases by molecular dynamics simulation. The components of the optical response were calculated for the three different axes with respect to the director of the system, separately. In the nematic phase, in particular, we observed that the response function does not vanish at long times. This means that the orientation of the director of the system is permanently changed by an instant irradiation of polarized light, as a result of third-order nonlinear optical response. In the smectic phase, however, all the components of the response function decay quickly. Our results give a theoretical background at molecular level on the interpretation of the reported experimental observations of peculiar dynamics of liquid crystalline systems at irradiation of laser lights.