Nonlinear, ground-state, pump-probe spectroscopy

A theory of pump-probe spectroscopy is developed in which optical fields drive two-quantum, Raman-like transitions between ground state sublevels. Three fields are incident on an ensemble of atoms. Two of the fields act as the pump field for the two-quantum transitions. The absorption or gain of an additional probe field is monitored as a function of its detuning from one of the fields which constitutes the pump field. Although the probe absorption spectrum displays features common to those found in pump-probe spectroscopy of single-quantum transitions, new interference effects are found to modify the spectrum. Many of these features can be explained within the context of a dressed atom picture.