Fundamentals of Highly Non-Degenerate Cascaded Four-Wave Mixing

By crossing two intense ultrashort laser pulses with different colors in a transparent medium, like a simple piece of glass, a fan of multicolored broadband light pulses can be simultaneously generated. These newly generated pulses are emitted in several well-defined directions and can cover a broad spectral range, from the infrared to the ultraviolet and beyond. This beautiful phenomenon, first observed and described 15 years ago, is due to highly-nondegenerate cascaded four-wave mixing (cascaded FWM, or CFWM). Here, we present a review of our work on the generation and measurement of multicolored light pulses based on third-order nonlinearities in transparent solids, from the discovery and first demonstration of highly-nondegenerate CFWM, to the coherent synthesis of single-cycle pulses by superposition of the multicolored light pulses produced by CFWM. We will also present the development and main results of a dedicated 2.5-D nonlinear propagation model, i.e., with propagation occurring along a two-dimensional plane while assuming cylindrically symmetric pump beam profiles, capable of adequately describing noncollinear FWM and CFWM processes. A new method for the generation of femtosecond pulses in the deep-ultraviolet (DUV) based on FWM and CFWM will also be described. These experimental and theoretical results show that highly-nondegenerate third-order nonlinear optical processes are formally well understood and provide broader bandwidths than other nonlinear optical processes for the generation of ultrashort light pulses with wavelengths extending from the near-infrared to the deep-ultraviolet, which have many applications in science and technology. Appl. Sci. 2015, 5 486