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Optics Letters

Polarization spectroscopy of a velocity-selected molecular sample

James M. R. Kirkbride, Andrew R. Dalton, Grant A. D. Ritchie

Published Apr 19, 2014• 3 citations
Publisher

Abstract

This Letter demonstrates polarization spectroscopy of a velocity selected and vibrationally excited molecular sample. Specifically, the anisotropy induced by a circularly polarized IR pump beam tuned to the R(14.5)(1/2)v=1←v=0 transition of nitric oxide is observed using an IR probe resonant with the R(15.5)(1/2)v=2←v=1 hot band transition. Using two detectors in combination with the rapidly swept probe allows both the absorptive and dispersive components of the excited state polarization to be observed for the first time. The data are well described by simulations based upon a three-level density matrix model.

DOI
10.1364/ol.39.002645

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This Letter demonstrates polarization spectroscopy of a velocity selected and vibrationally excited molecular sample. Specifically, the anisotropy induced by a circularly polarized IR pump beam tuned to the R(14.5)(1/2)v=1←v=0 transition of nitric oxide is observed using an IR probe resonant with the R(15.5)(1/2)v=2←v=1 hot band transition. Using two detectors in combination with the rapidly swept probe allows both the absorptive and dispersive components of the excited state polarization to be observed for the first time. The data are well described by simulations based upon a three-level density matrix model.
We investigate polarization spectroscopy of an excited state transition in room-temperature rubidium vapor. By applying a circularly polarized coupling beam, resonant with the 52S1/2 → 52P3/2 transition, we induce anisotropy in the atomic medium that is then probed by scanning a probe beam across the 52P3/2 → 62S1/2 transition. By performing polarimetry on the probe beam, a dispersive spectral feature is observed. We characterize the excited-state polarization spectrum as a function of coupling intensity for both isotopes and find that at high intensities, Autler-Townes splitting results in a sub-feature, which theoretical modelling shows is enhanced by Doppler averaging. This spectroscopic technique produces a narrow dispersive signal which is ideal for laser frequency stabilization to excited-state transitions.
We demonstrate polarization spectroscopy of an excited state transition in room-temperature cesium vapor. An anisotropy induced by a circularly polarized pump beam on the D2 transition is observed using a weak probe on the 6P(3/2)→7S(1/2) transition. At high pump power, a subfeature due to Autler-Townes splitting is observed that theoretical modeling shows is enhanced by Doppler averaging. Polarization spectroscopy provides a simple modulation-free signal suitable for laser frequency stabilization to excited state transitions.
We demonstrate polarization spectroscopy of an excited state transition in room temperature cesium vapor. An anisotropy induced by a circularly polarized pump beam on the D2 transition is observed using a weak probe on the 6P3/2 to 7S1/2 transition. When the D2 transition is saturated, a sub-natural linewidth feature is observed which theoretical modeling shows is enhanced by Doppler averaging. Polarization spectroscopy provides a simple modulation-free signal suitable for laser frequency stabilization to excited state transitions.
Two 5 µm continuous wave quantum cascade lasers are used to perform a counterpropagating pump and probe experiment on a low pressure sample of nitric oxide. The strong pump field excites a fundamental rovibrational transition and the weaker probe field is tuned to the corresponding rotationally resolved hot band transition. When both light fields are in resonance, rapid passage is observed in the hot band absorption lineshape arising from a minimally damped and velocity-selected sample of molecules in the v=1 state. The measured rapid passage signals are well described by a two-level model based on the optical Bloch equations.
The theory of pulsed polarization spectroscopy in the case of a saturating pump pulse and an optically thick sample is presented, both with and without inhomogeneous broadening. It is found that the molecular anisotropy produced by pumping an R- or P-branch transition is maximized by using a pulse whose flip angle is near 2\ensuremath{\pi} for the M component with the largest Rabi frequency. Calculations with no or extreme inhomogeneous broadening differ insignificantly. Such a pump pulse produces an anisotropy (and thus polarization rotation of the probe beam) of the opposite sign of that produced by weak-field excitation. Pulse-propagation calculations obtained by numerically solving the coupled Maxwell-Bloch equations demonstrate that there exist ``stable-area'' pulses, much like for a two-level system. The lowest such stable pulse produces a flip angle of 2.21\ensuremath{\pi} for the M=0 level and produces close to the maximum polarization anisotropy. This pulse still weakly excites the sample, and thus lengthens as it propagates to conserve area. The effective absorption coefficient, however, is much less than that for weak pulses. It is expected that such pulses should provide an order of magnitude or more sensitivity for polarization spectroscopy than that obtained with nonsaturating pulses.
A theoretical analysis of the relative intensities of the Doppler-free signals in saturation spectroscopy, velocity selective optical pumping (VSOP) spectroscopy, polarization spectroscopy and a mixing of saturation and polarization spectroscopies is presented using the approximation of a single cycle of optical pumping in a four-level system. An optical pumping process in the Zeeman sublevels is taken into account owing to the important role of spontaneous emission even if the sublevels are degenerate. Arbitrary polarization combinations are considered for pump and probe beams. The similarities and differences between three kinds of spectroscopy are made clear. Both circular and linear optical anisotropies induced by the pump beam are considered in this theoretical calculation. The magnitude and sign of Doppler-free resonances in each spectroscopy are quite different owing to the polarizations of the pump and probe beams. The four-level system is important as a three-level approximation. The results obtained from the four-level optical pumping theory are in good agreement with experimental reports.