Four-wave mixing of picosecond pulses in hollow fibers: expanding the possibilities of gas-phase analysis

Third-harmonic, difference-frequency, and sum-frequency generation processes in hollow fibers are experimentally studied with 30-ps pulses having an energy of several millijoules. The experimental dependence of the difference-frequency signal on the pressure of the gas filling the fiber agrees well with the results of calculations when the contribution of higher order waveguide modes is taken into consideration, thus indicating the importance of nonlinear-optical processes involving higher order waveguide modes of a hollow fiber. Hollow fibers are also shown to expand the possibilities of nonlinear-optical analysis of gases by allowing the generation of third-harmonic and sum-frequency signals, which vanish in the regime of tight focusing in a medium with normal dispersion.