Manipulating Nonlinear Optical Response via Domain Control in Nanocrystal-in-Glass Composites

Nanocrystal-in-glass (NIG) is an exciting class of composites, because it can not only combine the advantages of crystal and glass materials but also potentially generate new physical phenomenon in a cooperative manner. Herein, the nonlinear light-matter interaction processes in a broad range of NIG composites homogeneously embedded with LiNbO₃ are investigated. It is shown that, by rational control of the organization manner of crystal and glass phases, second-harmonic generation (SHG) can be precisely tuned. Importantly, an unusual SHG phenomenon, transverse SHG (TSHG), can be realized in the special region of the microstructure map combined with the features of high loading, nanoscale size, and homogenous distribution of nanocrystals. Furthermore, NIG composites exhibit broadband optical response, allowing TSHG in a wide waveband region to be achieved. Based on the above effects, the applications of the constructed NIG composite for precise measurement of the group velocity and duration of ultrashort optical pulses with femtosecond time scales are demonstrated. Indeed, the findings outline a fundamental principle to design NIG configurations for creating new properties, providing new directions for expanding the scope of NIG functional materials.