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Anthony O’Keefe

Bio: Anthony O’Keefe is an academic researcher. The author has contributed to research in topics: Absorption spectroscopy & Cavity ring-down spectroscopy. The author has an hindex of 2, co-authored 2 publications receiving 1468 citations.

Papers
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Journal ArticleDOI
TL;DR: In this paper, the authors have developed a technique which allows optical absorption measurements to be made using a pulsed light source and offers a sensitivity significantly greater than that attained using stabilized continuous light sources.
Abstract: We have developed a technique which allows optical absorption measurements to be made using a pulsed light source and offers a sensitivity significantly greater than that attained using stabilized continuous light sources. The technique is based upon the measurement of the rate of absorption rather than the magnitude of absorption of a light pulse confined within a closed optical cavity. The decay of the light intensity within the cavity is a simple exponential with loss components due to mirror loss, broadband scatter (Rayleigh, Mie), and molecular absorption. Narrowband absorption spectra are recorded by scanning the output of a pulsed laser (which is injected into the optical cavity) through an absorption resonance. We have demonstrated the sensitivity of this technique by measuring several bands in the very weak forbidden b1Σg−X3Σg transition in gaseous molecular oxygen. Absorption signals of less than 1 part in 106 can be detected.

1,540 citations

Journal ArticleDOI
TL;DR: A method of repeatedly re-injecting light reflected off the front mirror of the optical cavity to boost the cavity's circulating power and deliver more light to the photodetector and thus increase the signal-to-noise ratio of the absorption measurement, demonstrating the improved ability to resolve weakly absorbing spectroscopic features.
Abstract: Non-mode-matched cavity-enhanced absorption spectrometry (e.g., cavity ringdown spectroscopy and integrated cavity output spectroscopy) is commonly used for the ultrasensitive detection of trace gases. These techniques are attractive for their simplicity and robustness, but their performance may be limited by the reflection of light from the front mirror and the resulting low optical transmission. Although this low transmitted power can sometimes be overcome with higher power lasers and lower noise detectors (e.g., in the near-infrared), many regimes exist where the available light intensity or photodetector sensitivity limits instrument performance (e.g., in the mid-infrared). In this article, we describe a method of repeatedly re-injecting light reflected off the front mirror of the optical cavity to boost the cavity's circulating power and deliver more light to the photodetector and thus increase the signal-to-noise ratio of the absorption measurement. We model and experimentally demonstrate the method's performance using off-axis cavity ringdown spectroscopy (OA-CRDS) with a broadly tunable external cavity quantum cascade laser. The power coupled through the cavity to the detector is increased by a factor of 22.5. The cavity loss is measured with a precision of 2 × 10−10 cm−1/ Hz ; an increase of 12 times over the standard off-axis configuration without reinjection and comparable to the best reported sensitivities in the mid-infrared. Finally, the re-injected CRDS system is used to measure the spectrum of several volatile organic compounds, demonstrating the improved ability to resolve weakly absorbing spectroscopic features.

9 citations


Cited by
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Journal ArticleDOI
TL;DR: In this article, the authors present the basis for each technique, recent developments in methods and performance limitations, and present a performance comparison of different techniques, taking data reported over the preceding decade, and draw conclusions from this benchmarking.
Abstract: The detection and measurement of gas concentrations using the characteristic optical absorption of the gas species is important for both understanding and monitoring a variety of phenomena from industrial processes to environmental change. This study reviews the field, covering several individual gas detection techniques including non-dispersive infrared, spectrophotometry, tunable diode laser spectroscopy and photoacoustic spectroscopy. We present the basis for each technique, recent developments in methods and performance limitations. The technology available to support this field, in terms of key components such as light sources and gas cells, has advanced rapidly in recent years and we discuss these new developments. Finally, we present a performance comparison of different techniques, taking data reported over the preceding decade, and draw conclusions from this benchmarking.

1,293 citations

Journal ArticleDOI
TL;DR: In this paper, the authors present diagnostic techniques based on optical emission spectroscopy and cavity ring-down Spectroscopy for atmospheric pressure plasmas under conditions ranging from thermal and chemical equilibrium to thermochemical nonequilibrium.
Abstract: Atmospheric pressure air plasmas are often thought to be in local thermodynamic equilibrium owing to fast interspecies collisional exchange at high pressure. This assumption cannot be relied upon, particularly with respect to optical diagnostics. Velocity gradients in flowing plasmas and/or elevated electron temperatures created by electrical discharges can result in large departures from chemical and thermal equilibrium. This paper reviews diagnostic techniques based on optical emission spectroscopy and cavity ring-down spectroscopy that we have found useful for making temperature and concentration measurements in atmospheric pressure plasmas under conditions ranging from thermal and chemical equilibrium to thermochemical nonequilibrium.

915 citations

Journal ArticleDOI
TL;DR: A comprehensive overview of sensor technology exploiting optical whispering gallery mode (WGM) resonances by detailing the fundamental principles and theory of WGMs in optical microcavities and the transduction mechanisms frequently employed for sensing purposes.
Abstract: We present a comprehensive overview of sensor technology exploiting optical whispering gallery mode (WGM) resonances. After a short introduction we begin by detailing the fundamental principles and theory of WGMs in optical microcavities and the transduction mechanisms frequently employed for sensing purposes. Key recent theoretical contributions to the modeling and analysis of WGM systems are highlighted. Subsequently we review the state of the art of WGM sensors by outlining efforts made to date to improve current detection limits. Proposals in this vein are numerous and range, for example, from plasmonic enhancements and active cavities to hybrid optomechanical sensors, which are already working in the shot noise limited regime. In parallel to furthering WGM sensitivity, efforts to improve the time resolution are beginning to emerge. We therefore summarize the techniques being pursued in this vein. Ultimately WGM sensors aim for real-world applications, such as measurements of force and temperature, or alternatively gas and biosensing. Each such application is thus reviewed in turn, and important achievements are discussed. Finally, we adopt a more forward-looking perspective and discuss the outlook of WGM sensors within both a physical and biological context and consider how they may yet push the detection envelope further.

715 citations

Journal ArticleDOI
TL;DR: In this paper, the authors demonstrate that a commercial single-frequency cavity ring down spectroscopy (CRDS) can also be conveniently employed, allowing to gain in spectral resolution, signal intensity and data acquisition rate.

512 citations

Journal ArticleDOI
TL;DR: In the short space of 15 years since their first demonstration, quantum cascade lasers have become the most useful sources of tunable mid-infrared laser radiation as discussed by the authors, and the potential application of quantum cascade laser in other areas of chemical physics such as research on helium droplets, in population pumping and in matrix isolation infrared photochemistry.

510 citations