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We study nearly degenerate four-wave mixing using a two-photon-allowedvibrational transition of parahydrogen. A signal photon is generated by atrigger photon and coherence among parahydrogen, which is prepared by twocounterpropagating pump pulses. The dependence of the signal pulse energy onthe trigger frequency are investigated. The measured spectra vary depending onthe geometry. They shift depending on the direction of the signal pulse and onthe small angle formed by the counterpropagating pump pulses. Furthermore, thedependence of signal pulse energy on the incident time of the trigger pulse isinvestigated. The measured signal pulse energy is high if the trigger pulse isslightly delayed with respect to the pump pulses. We demonstrate that thesegeometry-dependent spectra and coherent-transient response can be explained byusing simple models.

Geometry-dependent spectra and coherent-transient measurement of nearly degenerate four-wave mixing using two-photon resonance