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CAVITY RINGDOWN SPECTROSCOPY AND HIGH SENSITIVITY ABSORPTION MEASUREMENT

Zhao Hong

Published Jan 1, 2001• 0 citations
OpenAlex

Abstract

Cavity ring\|down spectroscopy is a novel spectroscopic technique used for high\|sensitivity measurement of absorption. It has been widely used in atomic, molecular and cluster spectroscopy, with an absorption sensitivity of 10 -6 —10 -14 cm -1 . The development of the cavity ring\|down technology and its application in absorption measurement are reviewed.

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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.

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Due to the phase-coherent relationship of intra-cavity pulse reflections leading to the narrow frequency-selectivity of the cavity, Cavity Ring-Down Laser Absorption Spectroscopy (CRLAS) is a promising method lo study Doppler-free two-photon absorption at resolutions at least two orders of magnitude better than the pulse bandwidth of even Fourier Transform Limited nsec pulsed lasers. The nonlinear absorption will lead to a nouexponential cavity decay with can be used to discriminate it from both linear absorption and intrinsic cavity loss. In this study, several issues have been examined in order to access the feasibility of obtaining the high-resolution two-photon absorption spectra of the Rydberg states of alkali dimers by this technique. Using atomic transition dipoles as an approximation, the laser intensities needed to elicit reasonable excitation were estimated, and found to be well within presently available levels. The importance of the various linewidth- limiting mechanism was also examined. The relative magnitudes of pressure broadening, AC Stark broadening, cavity stability, and time-of-flight broadening lead us to expect a resolution of $\\sim$1 MHz or better.

•Jan 1, 1997•0 citations
Cavity ring|down spectroscopy is a novel spectroscopic technique used for high|sensitivity measurement of absorption. It has been widely used in atomic, molecular and cluster spectroscopy, with an absorption sensitivity of 10 -6 —10 -14 cm -1 . The development of the cavity ring|down technology and its application in absorption measurement are reviewed.
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.
The number density and orientation of molecules at the surface of a total-internal-reflection-ring minicavity are probed with extremely high sensitivity in a novel realization of the cavity ring-down optical absorption experiment. The modes of the ultralow-loss cavity, which are excited by photon tunneling, have long lifetimes that are sensitive to the presence of absorbing species in the evanescent field near a cavity facet. The total-internal-reflection-ring cavity extends cavity ring-down spectroscopy to surfaces and condensed matter, permitting a wide range of novel fundamental studies and applications. Routine single molecule detection may ultimately be feasible.
Due to the phase-coherent relationship of intra-cavity pulse reflections leading to the narrow frequency-selectivity of the cavity, Cavity Ring-Down Laser Absorption Spectroscopy (CRLAS) is a promising method lo study Doppler-free two-photon absorption at resolutions at least two orders of magnitude better than the pulse bandwidth of even Fourier Transform Limited nsec pulsed lasers. The nonlinear absorption will lead to a nouexponential cavity decay with can be used to discriminate it from both linear absorption and intrinsic cavity loss. In this study, several issues have been examined in order to access the feasibility of obtaining the high-resolution two-photon absorption spectra of the Rydberg states of alkali dimers by this technique. Using atomic transition dipoles as an approximation, the laser intensities needed to elicit reasonable excitation were estimated, and found to be well within presently available levels. The importance of the various linewidth- limiting mechanism was also examined. The relative magnitudes of pressure broadening, AC Stark broadening, cavity stability, and time-of-flight broadening lead us to expect a resolution of $\\sim$1 MHz or better.