The steady-state absorption of a beam of sodium atoms irradiated by a train of pulses from a mode-locked dye laser has been measured. The sodium atoms were prepared as two-level systems by optical pumping with a two-mode laser. Absorption spectra on the 589.0-nm D2 line were recorded over 20 GHz with a frequency-stabilized, tunable, mode-locked dye laser having a bandwidth of 3.7 GHz and a mode spacing of 82 MHz. The laser-pulse profile was determined from the spectral profile assuming transform-limited pulses and was incorporated in theoretical calculations of excitation spectra obtained by numerical integration of the optical Bloch equations. By comparison of measured absorption spectra and theoretical excitation spectra the validity of the weak-field solution as well as the predicted saturation behavior were fully verified by the experimental results. For the highest level of irradiation applied, the laser pulses were identified as π pulses.
We report the results of an experimental study of the effects of velocity-changing collisions on two-photon and stepwise-absorption line shapes. Excitation spectra for the $3{S}_{\frac{1}{2}}\ensuremath{\rightarrow}3{P}_{\frac{1}{2}}\ensuremath{\rightarrow}4{D}_{\frac{1}{2}}$ transitions of sodium atoms undergoing collisions with foreign gas perturbers are obtained. These spectra are obtained with two cw dye lasers. One laser, the pump laser, is tuned 1.6 GHz below the $3{S}_{\frac{1}{2}}\ensuremath{\rightarrow}3{P}_{\frac{1}{2}}$ transition frequency and excites a nonthermal longitudinal velocity distribution of excited
3P21 atoms in the vapor. Absorption of the second (probe) laser is used to monitor the steady-state excited-state distribution which is a result of collisions with rare gas atoms. The spectra are obtained for various pressures of He, Ne, and Kr gases and are fit to a theoretical model which utilizes either the phenomenological Keilson-St\"orer or the classical hardsphere collision kernel. The theoretical model includes the effects of collisionally aided excitation of the
3P21 state as well as effects due to fine-structure state-changing collisions. Although both kernels are found to predict line shapes which are in reasonable agreement with the experimental results, the hard-sphere kernel is found superior as it gives a better description of the effects of large-angle scattering for heavy perturbers. Neither kernel provides a fully adequate description over the entire line profile. The experimental data is used to extract effective hard-sphere collision cross sections for collisions between sodium
3P21 atoms and helium, neon, and krypton perturbers.