Femtosecond nonresonant degenerate four-wave mixing at atmospheric pressure and in a free jet

2 , N₂, and CO₂. For CO₂ additional experiments have been performed at reduced pressure and in a molecular beam. By delaying the probe pulse a periodic recovery of the DFWM signal is observed. The period of these transients can be assigned unambiguously to rotational Raman transitions of the ground state within the laser bandwidth. The decay of the transients yields the collisional dephasing of the Raman-induced polarization. At zero delay also optical-field-induced birefringence of electronic nature contributes to the signal. The different time scales of the Raman and electronic effects allow us to estimate their relative strength. Received: 3 August 1998 / Revised version: 21 October 1998 / Published online: 24 February 1999