Observation of an Optical Stark Effect on Vibrational and Rotational Transitions

Vibrational and rotational Raman transitions are shown to be shifted to lower frequencies in the presence of a nonresonant, high-intensity optical field. Experimental results using coherent anti-Stokes Raman spectroscopy for hydrogen and nitrogen are presented. The magnitude of the observed shift is in agreement with a calculation which considers the coupling of the optical field to the internuclear separation via the molecular electronic polarizability. The magnitude of the shift is predicted to be proportional to the optical field intensity.