Versatile supercontinuum generation by using chi((2)) and chi((3)) nonlinearities in PPLN crystal for direct multiplex CARS measurement

In this study, we report on experiments of spatio-temporal nonlinear frequency conversion in a periodically poled Lithium Niobate (PPLN) crystal designed for second-harmonic generation (SHG). We demonstrated a novel supercontinuum source based on the mixing of second and third-order nonlinearities. We could adjust the (chi((2)), chi((3))) nonlinearities by controlling the input laser polarization orientation, the pulse duration and the PPLN crystal temperature. We obtained an ultra-broadband spectrum, ranging from visible to infrared domains, by pumping a 20-mm-long PPLN crystal with a 3 ps pulse at 1030 nm. This broadband pulse was used to achieve direct multiplex Coherent Anti-Stokes Raman Scattering (M-CARS) imaging, without the need for any optical delay line to temporally synchronize the pump and the Stokes waves. Simultaneous vibrational signatures ranging from -3200 cm(-1) to -500 cm(-1) were obtained. Several filters were placed on the broadband supercontinuum path, to shape the output spectrum between 1030 nm and 1650 nm, before sending it into the microscope. The output spectral analysis allows for the demonstration of multimodal imaging, by using SHG, M-CARS and multiphoton fluorescence processes.