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Optics Letters

Frequency-switched heterodyne cavity ringdown spectroscopy

M. D. Levenson, Barbara A. Paldus, Thomas G. Spence, C. C. Harb, Richard N. Zare, M. J. Lawrence, Robert L. Byer

Published Jun 15, 2000• 23 citations
Publisher

Abstract

When the frequency of light coupled into a cavity is suddenly shifted, the radiation emanating from the input port of the previously excited cavity can beat with the reflection of the frequency-shifted input on the surface of a photodetector. When the beat frequency is stable, the time decay of the resulting optical heterodyne signal can be used to measure intracavity absorption spectra with near quantum-limited sensitivity.

DOI
10.1364/ol.25.000920

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When the frequency of light coupled into a cavity is suddenly shifted, the radiation emanating from the input port of the previously excited cavity can beat with the reflection of the frequency-shifted input on the surface of a photodetector. When the beat frequency is stable, the time decay of the resulting optical heterodyne signal can be used to measure intracavity absorption spectra with near quantum-limited sensitivity.
We present an ac heterodyne technique in cavity ringdown spectroscopy that permits $1\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}10}$ absorption sensitivity with microwatt-level light power. Two cavity modes, one probing the empty cavity and the other probing intracavity absorption, are excited simultaneously but with their intensities temporally out of phase, with one mode decaying and the other rising. Heterodyne detection between the two modes reveals the dynamic time constants associated with the empty cavity and the additional intracavity gas absorption. The method offers a quick comparison between the on- and off-resonance information, a prerequisite to reaching the fundamental shot-noise limit. This simple and yet important improvement of cavity ringdown spectroscopy should lead to the enhanced performance of a wide range of applications.
We introduce optical feedback frequency stabilized cavity ring-down spectroscopy (OFFS-CRDS), a near-shot-noise-limited technique that combines kilohertz resolution with an absorption detection sensitivity of 5×10(-13) cm(-1) Hz(-1/2). Its distributed feedback laser source is stabilized to a highly stable V-shaped reference cavity by optical feedback and fine-tuned by means of single-sideband modulation. The stability of this narrow laser is transferred to a ring-down (RD) cavity using a new fibered Pound-Drever-Hall (PDH) locking scheme without a dedicated electro-optic phase modulator, yielding several hundred RD events per second. We demonstrate continuous coverage of more than 7 nm with a baseline noise of 5×10(-12) cm(-1) and a dynamic range spanning six decades. With its resonant intracavity light intensity on the order of 1 kW/cm2, the spectrometer was used for observing a Lamb dip in a transition of carbon dioxide involving four vibrational quanta. Saturating such a weak transition at 160 μW input power, OFFS-CRDS paves the way to Doppler-free molecular overtone spectroscopy for precision measurements of hyperfine structures and pressure shifts.
Cavity Ring Down Spectroscopy has become an important method in gas phase spectroscopy and its uses promise to expand. While previous investigators have considered the decay of the stored energy in the cavity ring down cell following short pulsed excitation, this paper considers the effects of pulse reshaping during cavity ring down. It is found that in order to properly model these effects, one must consider not only the mode dependent loss of the ring down cavity, but also dispersion that shifts the resonant modes of the cavity. Only by considering the latter effect does one get a "causal" result where the free induction decay signal of the absorber occurs after the excitation pulse. It is demonstrated that in the limit that the cavity round trip time is long compared to both the T 2 time of the intracavity absorber and the temporal width of the excitation pulse, the reshaping of the n'th pulse out of the ring down cavity is the same as the reshaping produced by free space propagation over a distance of (2 n + 1) L where L is the separation of the mirrors in the cell. However, when the absorber T 2 becomes comparable to or longer than the cavity round trip time, then discrete modes of the ring down cavity become important. A general expression for the output is given for the important case of a weak absorber, and changes in the output are computed for a single absorption line as a function of the ratio of T 2 to the cavity round trip time for several values of the optical thickness of the sample. Lastly, it is suggested that monitoring changes in the pulse shape of the cavity ring down signal provides a way to characterize an absorption spectrum on a frequency scale of the laser bandwidth down to the cavity free spectral range.
Theoretical quantitative considerations as well as experimental data are presented based on absorption population depletion coupled with cavity ringdown spectroscopy. The absorbing number densities inside the cavity are determined by numerical integration of the coupled rate equations. The number of photons involved in absorption, cavity losses due to mirror reflectivity and stimulated emission are taken into account. The principle is to monitor a first transition by cavity ringdown spectroscopy while a second transition, with a state in common, is resonantly excited by the decaying radiation of different frequency also trapped inside the optical cavity. A numerical example is given for atomic lines of neon and the measurements carried out in a supersonic slit-jet expansion discharge demonstrate the feasibility of the technique. The technique is also proven to work with two resonant transitions of C2. Translational velocity of the jet modifying the rate equations is included in the model.