Engineering nonlinear optical phenomena by arbitrarily manipulating the phase relationships among the relevant optical fields

Abstract

Nonlinear optical processes are intrinsically dominated by the phase relationships among the relevant electromagnetic fields, including the phase of nonlinear polarization produced in them. If one can arbitrarily manipulate these phase relationships at a variety of desired interaction lengths, direct and highly designable manipulations for the nonlinear optical phenomenon could be achieved. Here, we report a proof-of-principle experiment in which a high-order Raman-resonant four-wave-mixing process is used as a representative nonlinear optical process and is tailored to a variety of targets by implementing such arbitrary manipulations of the phase relationships in the nonlinear optical process. We show that the output energy is accumulated to a specific, intentionally selected Raman mode on demand; and at the opposite extreme, we can also distribute the output energy equally over broad high-order Raman modes in the form of a frequency comb. This concept in nonlinear optical processes enables an attractive optical technology: a single-frequency tunable laser broadly covering the vacuum ultraviolet region, which will pave the way to frontiers in atomic-molecular-optical physics in the vacuum ultraviolet region.