Reversible suppression of second harmonic generation in dye-doped liquid crystal by light-induced thermal phase transition on sub-micrometer scale

Optically controllable signals are fundamental to various applications from communication to super-resolution imaging. However, literature on non-fluorescent, nonlinear optical signals that can be reversibly turned on/off on a sub-micrometer scale is scant. In this work, we experimentally demonstrate a scheme for the reversible suppression of second harmonic generation (SHG) based on dye-doped nematic liquid crystal molecules. Under a pump (suppressing SHG) and probe (generating SHG) setup with a tightly focusing microscope and a time-gated detection, outstanding modulation depth (>80%) has been realized. Surprisingly, the mechanism of liquid crystal SHG switch on a sub-micrometer scale was found to be light-induced thermal phase transition as against optical Frederick's transition. Quantitative analysis of the optical nonlinearity χ(2) versus local heating shows an excellent agreement of SHG signal suppression as well as its dependence on the liquid crystal molecular order and phase change. Our work provides an innovative example of applying nonlinear optical properties of soft materials, and can be further optimized for all-optical modulation applications.