Abstract

Abstract Lithium niobate thin film (LNTF) is a promising platform for ultra‐low loss nonlinear integrated photonics. Here, the simultaneous generation of second harmonic wave (SHW) and dispersive wave (DW) are demonstrated in a single LNTF under the pump of a femtosecond pulse laser, with a conversion efficiency exceeding 25%. The second harmonic generation (SHG) uses the modal phase matching mechanism based on the second‐order nonlinear effect, while the DW generation is based on the perturbations of soliton dynamics caused by self‐phase modulation and higher‐order dispersion. Notably, significant and symmetrical SHW and DW patterns are observed, which exhibit strong spatial dispersion properties. A comprehensive analysis of the phase‐matching conditions are conducted for SHG and DW generation and provide a clear elucidation of the spectral properties of different regions of the emitted light patterns. Additionally, the evolution of the pump light in LNTF is thoroughly investigated, and the solutions of the generalized Schrödinger equation are in good agreement with these experimental results. This work sheds new light on the rich physics of nonlinear optical interactions on LNTF, and by utilizing the synergistic effect of second‐order and third‐order nonlinear effects, this study anticipates achieving efficient and high energy on‐chip broadband frequency conversion and supercontinuum generation across octaves.