Effect of Doppler broadening on Autler-Townes splitting in the molecular cascade excitation scheme

Theoretical analysis of the Autler-Townes splitting pattern in a three-level cascade excitation of a Doppler-broadened sample reveals that the observed Autler-Townes splitting is not only a function of the coupling-laser Rabi frequency, as in the homogeneously broadened case, but can also strongly depend on the wavenumber ratio of the coupling and probe lasers. Utilizing a steady-state density matrix formalism, we derive exact expressions for the populations of the intermediate and upper levels for a homogeneously broadened system. In the limit of a weak probe field, analytical expressions for Doppler-broadened excitation spectra from the intermediate and upper levels are derived. Using these expressions, we investigate the critical role of Doppler broadening on the observation of Autler-Townes splitting and its asymptotic behavior as a function of the coupling Rabi frequency for counterpropagating and copropagating configurations for different wavenumber ratios of the lasers