Abstract

In the early 1980s the influence of the optical Stark effect on vibrational and rotational transitions was investigated with coherent anti-Stokes and inverse Raman spectroscopies.¹ For either an inhomogeneous intensity distribution in space or time, or molecules with several overlapping levels with different Stark coefficients, the Stark effect causes broadening and asymmetry in Raman¹ and two-photon spectroscopies.² However, if the inducing field is spatially uniform and temporally a Fourier-transform-limited pulse and if other broadening mechanisms can be neglected, the resulting spectrum should show a strong modulation due to an induced phase modulation in the molecular oscillation.

© 1988 Optical Society of America