Probing Stark-induced nonlinear phase variation with opto-optical modulation

We extend the recently developed technique of opto-optical modulation (OOM) to probe state-resolved ac-Stark-induced phase variations of a coherently excited ensemble of helium atoms. In a joint experimental and theoretical study, we find that the spatial redirection of the resonant emission from the OOM process is different for the low-lying 1s2p state as compared with the higher-lying Rydberg states, and that this redirection can be controlled through the spatial characteristics of the infrared (IR) probe beam. In particular, we observe that the intensity dependence of the IR-induced Stark phase on the 1s2p emission is nonlinear, and that the phase accumulation changes sign for moderate intensities. Our results suggest that OOM, combined with precise experimental shaping of the probe beam, could allow future measurements of Stark-induced phase shifts of excited states.