Spectral line shape of resonant four-wave mixing induced by broad-bandwidth lasers.

We present a theoretical and experimental study of the line shape of resonant four-wave mixing induced by broad-bandwidth laser radiation that revises the theory of Meacher, Smith, Ewart, and Cooper ~MSEC! @Phys. Rev. A 46, 2718 ~1992!#. We adopt the same method as MSEC but correct for an invalid integral used to average over the distribution of atomic velocities. The revised theory predicts a Voigt line shape composed of a homogeneous, Lorentzian component, defined by the collisional rate G, and an inhomogeneous, Doppler component, which is a squared Gaussian. The width of the inhomogeneous component is reduced by a factor of& compared to the simple Doppler width predicted by MSEC. In the limit of dominant Doppler broadening, the width of the homogeneous component is predicted to be 4G, whereas in the limit of dominant homogeneous broadening, the predicted width is 2G. An experimental measurement is reported of the line shape of the four-wave-mixing signal using a broad-bandwidth, ‘‘modeless,’’ laser resonant with the Q1~6! line of the A S2X P(0,0) system of the hydroxyl radical. The measured widths of the Voigt components were found to be consistent with the predictions of the revised theory. @S1050-2947~96!02308-6#