Time-domain polarization coherent anti-Stokes Raman spectroscopy of Tl atoms: dephasing measurements of separate multipole moments.

Polarization nondegenerate nonstationary coherent anti-Stokes Raman spectroscopy was used in measurements of pulse responses for separate electronic multipole moments. The 6P(1/2)-6P(3/2) transition of Tl atoms was investigated. Doppler dephasing conditions, quantum beats of the hyperfine components of this transition are clearly seen when pure anisotropic scattering is registered, but they are small in the case of purely antisymmetric scattering. Under collisional dephasing conditions the relaxation rates of anisotropic and antisymmetric scattering agree with existing theory within +/-5%.