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Physical Review A

Cavity ringdown heterodyne spectroscopy: High sensitivity with microwatt light power

Jun Ye, J. L. Hall

Published May 17, 2000• 52 citations
Publisher

Abstract

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.

DOI
10.1103/physreva.61.061802

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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.

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We present a cavity-enhanced optical absorption measurement technique based on high-bandwidth Pound-Drever-Hall (PDH) sideband locking, which naturally provides a real-time, resonant amplitude quadrature readout that can be mapped onto the cavity’s internal loss rate. Cavity-enhancement is widely used in the detection of small signals -- an optical cavity traps photons between two highly reflective mirrors, thereby enhancing the effective path length through the absorber [Romanini et al., 2014]. Most of the available techniques, however, probe transmission signals and/or do not provide the stability required for the detection of fast signals.To ensure optimal enhancement of absorption sensitivity, probe light must be locked on resonance with the cavity. PDH locking relies on phase modulation of a laser beam, creating two sidebands on the original carrier frequency [Black, 2001]. Upon reflection from a cavity, this modulated light produces a heterodyne signal (beat note) that can be detected and demodulated. We use the phase quadrature of the beat note to lock the cavity on resonance with one of the sidebands, achieving a locking bandwidth in the MHz range that keeps cavity and probe light resonant for hours [Reinhardt et al., 2017]. Simultaneously, we monitor the amplitude quadrature, which provides a continuous, real-time, heterodyne-amplified readout of the cavity’s internal absorption. Our PDH sideband cavity-enhanced absorption readout technique (SideCAR) ensures high sensitivity without reaching saturation limits in the intracavity medium by keeping a relatively low intracavity power, since only one of the sidebands is allowed to enter the cavity, but the signal is boosted above the detector noise by heterodyne detection (using the carrier as a local oscillator).This thesis presents the theoretical formulation of the sensing technique together with the expressions for the sensitivity limit (ultimately given by the laser quantum noise), and the experimental results from a test cavity setup. Probing a proof-of-concept 5-cm-long Fabry-Perot cavity with a coupled power of 160 uW, we measure an absorption sensitivity of 7*10^(-11) cm^(-1)/sqrt(Hz) at 100 kHz (roughly the cavity bandwidth), a factor of 11 from the shot-noise limit. This technique allows the detection of small, transient signals against absorptive backgrounds with sensitivity close to the shot noise limit using a reflection-based measurement in a fairly simple setup, opening the possibility of developing new microscopic single-port real-world sensors for transients, for example using micron-scale optical fiber cavities

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Dispersion and Cavity-Ringdown Spectroscopy

Kevin K. Lehmann

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.

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Kevin K. Lehmann, D. Romanini

Cavity ring-down is becoming a widely used technique in gas phase spectroscopy. It holds promise for further important extensions, which will lead to even more frequent use. However, we have found widespread confusion in the literature about the nature of coherence effects, especially when the optical cavity constituting the ring-down cell is excited with a short coherence length laser source. In this paper we use the superposition principle of optics to present a general and natural framework for describing the excitation of a ring-down cavity regardless of the relative values of the cavity ring-down time, the input pulse coherence time, or the dephasing time of absorption species inside the cavity. This analysis demonstrates that even in the impulsive limit the radiation inside a high finesse cavity can have frequency components only at the natural resonance frequencies of the cavity modes. As an immediate consequence, a sample absorption line can be detected only if it overlaps at least one of the cavity resonances. Since this point is of particular importance for high resolution applications of the technique, we have derived the same conclusion also in the time domain representation. Finally, we have predicted that it is possible to use this effect to do spectroscopy with a resolution much higher than that of the bandwidth of the excitation laser. In order to aid in the design of such experiments, expressions are derived for the temporal and spatial overlap of a Fourier transform limited input Gaussian beam with the TEMmn modes of the cavity. The expressions we derive for the spatial mode overlap coefficients are of general interest in applications where accurate mode matching to an optical cavity is required.

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Johannes Burkart, D. Romanini, S. Kassi

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.

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CAVITY RINGDOWN SPECTROSCOPY AND HIGH SENSITIVITY ABSORPTION MEASUREMENT

Zhao Hong

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.

•Jan 1, 2001•0 citations
We present an ac heterodyne technique in cavity ringdown spectroscopy that permits 1\ifmmode×\else\texttimes\fi10\ensuremath−101\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}10}1\ifmmode×\else\texttimes\fi10\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 present a cavity-enhanced optical absorption measurement technique based on high-bandwidth Pound-Drever-Hall (PDH) sideband locking, which naturally provides a real-time, resonant amplitude quadrature readout that can be mapped onto the cavity’s internal loss rate. Cavity-enhancement is widely used in the detection of small signals -- an optical cavity traps photons between two highly reflective mirrors, thereby enhancing the effective path length through the absorber [Romanini et al., 2014]. Most of the available techniques, however, probe transmission signals and/or do not provide the stability required for the detection of fast signals.To ensure optimal enhancement of absorption sensitivity, probe light must be locked on resonance with the cavity. PDH locking relies on phase modulation of a laser beam, creating two sidebands on the original carrier frequency [Black, 2001]. Upon reflection from a cavity, this modulated light produces a heterodyne signal (beat note) that can be detected and demodulated. We use the phase quadrature of the beat note to lock the cavity on resonance with one of the sidebands, achieving a locking bandwidth in the MHz range that keeps cavity and probe light resonant for hours [Reinhardt et al., 2017]. Simultaneously, we monitor the amplitude quadrature, which provides a continuous, real-time, heterodyne-amplified readout of the cavity’s internal absorption. Our PDH sideband cavity-enhanced absorption readout technique (SideCAR) ensures high sensitivity without reaching saturation limits in the intracavity medium by keeping a relatively low intracavity power, since only one of the sidebands is allowed to enter the cavity, but the signal is boosted above the detector noise by heterodyne detection (using the carrier as a local oscillator).This thesis presents the theoretical formulation of the sensing technique together with the expressions for the sensitivity limit (ultimately given by the laser quantum noise), and the experimental results from a test cavity setup. Probing a proof-of-concept 5-cm-long Fabry-Perot cavity with a coupled power of 160 uW, we measure an absorption sensitivity of 7*10^(-11) cm^(-1)/sqrt(Hz) at 100 kHz (roughly the cavity bandwidth), a factor of 11 from the shot-noise limit. This technique allows the detection of small, transient signals against absorptive backgrounds with sensitivity close to the shot noise limit using a reflection-based measurement in a fairly simple setup, opening the possibility of developing new microscopic single-port real-world sensors for transients, for example using micron-scale optical fiber cavities
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.
Cavity ring-down is becoming a widely used technique in gas phase spectroscopy. It holds promise for further important extensions, which will lead to even more frequent use. However, we have found widespread confusion in the literature about the nature of coherence effects, especially when the optical cavity constituting the ring-down cell is excited with a short coherence length laser source. In this paper we use the superposition principle of optics to present a general and natural framework for describing the excitation of a ring-down cavity regardless of the relative values of the cavity ring-down time, the input pulse coherence time, or the dephasing time of absorption species inside the cavity. This analysis demonstrates that even in the impulsive limit the radiation inside a high finesse cavity can have frequency components only at the natural resonance frequencies of the cavity modes. As an immediate consequence, a sample absorption line can be detected only if it overlaps at least one of the cavity resonances. Since this point is of particular importance for high resolution applications of the technique, we have derived the same conclusion also in the time domain representation. Finally, we have predicted that it is possible to use this effect to do spectroscopy with a resolution much higher than that of the bandwidth of the excitation laser. In order to aid in the design of such experiments, expressions are derived for the temporal and spatial overlap of a Fourier transform limited input Gaussian beam with the TEMmn modes of the cavity. The expressions we derive for the spatial mode overlap coefficients are of general interest in applications where accurate mode matching to an optical cavity is required.
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.