Adaptive pumping for spectral control of broadband second-harmonic generation.

Second-harmonic generation (SHG) is always a significant frequency conversion process in nonlinear optics for many great applications but can be limited when broadband spectral laser sources are involved, e.g., femtosecond pulses. The conversion efficiency can be high, but the spectral control is hard because of the phase-matching (PM) limitation. Recently, a random quasi-phase-matching (QPM) scheme was proposed to make use of highly nonlinear materials that are difficult to be phase matched under traditional configurations. The spectral control is even harder in anisotropic random materials, and the coherence is completely lost. Here, we proposed an approach to solve this problem by coherent light control via feedback-based wavefront shaping. We utilized this method for spectral control of broadband SHG, which can be efficient even in strongly scattering media. Randomly selected wavelengths in the broadband spectra were enhanced with a good selectivity, and the direction was also controlled in a three-dimensional (3D) configuration. This technique paves the way for convenient spatial and spectral control of both linear and nonlinear emissions and a local enhancement of their conversion efficiency, indicating great progress in both random and ultrafast nonlinear optics.