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Applied Optics

Raman spectroscopy in the presence of stray resonant light

Jon P. Davis, Frank A. Narducci

Published Oct 20, 2016• 2 citations
Publisher

Abstract

In this paper, we explore and quantify the effects of stray light on stimulated Raman transitions. The stray light causes decoherence in the measurement of Rabi cycling and also causes increased differential AC Stark shift. These results are quantified as a function of the power of the stray light.
DOI
10.1364/ao.55.000c39

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We have measured the ac Stark effect in a two-zone stimulated Raman interaction in a sodium atomic beam. In addition, we have derived simple theoretical expressions for the ac Stark shift, based on a closed three-level system, in the Λ configuration, and have achieved qualitative agreement with the data. In particular, the magnitude and sense of the ac Stark shifts are found to depend on laser intensities as well as on the initial populations of the two low-lying levels of the Λ configuration. Specifically, the observed ac Stark shifts are smaller for larger laser intensities and also for smaller initial population differences between the two low-lying levels. The ac Stark effect must be considered for many potential applications of the Raman effect, such as a Raman clock. In this connection, we have identified conditions for the reduction of the ac Stark shift in our sodium Raman clock.
We demonstrate that when laser light is circularly polarized and properly detuned, the ac Stark shift of an alkali-metal atom in its ground state takes the form of a pure Zeeman shift. The condition is satisfied when the laser frequency is between the D1D1D1 and D2D2D2 transition frequencies, with the size of the detuning from the D2D2D2 resonance twice that from the D1D1D1 resonance. The direction of the effective magnetic field is along the laser propagation axis, and its magnitude is proportional to the vector polarizability of the atom and to the laser intensity. We use stimulated Raman spectroscopy on an optically pumped slow atomic beam from a magneto-optical trap to measure the vector polarizability and saturated absorption spectroscopy to show that the scalar polarizability vanishes at the particular detuning.
In the presence of coherent saturated near-resonant two-photon excitation, the ordinary Raman scattering line is replaced by a dynamic Stark shifted or Stark split doublet, and Rabi nutations appear in the time-resolved ordinary Raman spectrum. The relative intensity of the peaks of the doublet depends on the shape and on the average frequency of the exciting pulse. Striking new features arise from the interfering contributions of the upper and lower states of the two-photon transition to the Raman scattering process. The theory is applied to Raman scattering in atomic Na in the presence of the 3 2 S 1 2/(F=1, M F =1) to 4 2 D 3 2,5/2/(F=3,M F =3) two-photon resonances.
The energy shift of an atom due to its interaction with the oscillating electric field of an electromagnetic wave, or a laser light, is called the ac Stark shift. It has been studied both in the field of precision spectroscopy and atom optics. When the laser intensity is not constant spatially, its gradient gives rise to a dipole force. The force was used either to trap atoms in an optical trap or to reflect or guide atoms. We studied the ac Stark effect taking into account the fine structure of an alkali atom. We found that when the laser light is circularly polarized and properly detuned between the D1 and D2 transitions, the ac Stark shift can take the form of a pure Zeeman shift, hence the name analogous Zeeman shift.