2014
DOI: 10.1021/jz5008559
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Mid-Infrared Time-Resolved Frequency Comb Spectroscopy of Transient Free Radicals

Abstract: We demonstrate time-resolved frequency comb spectroscopy (TRFCS), a new broadband absorption spectroscopy technique for the study of trace free radicals on the microsecond timescale. We apply TRFCS to study the time-resolved, mid-infrared absorption of the deuterated hydroxyformyl radical trans-DOCO, an important short-lived intermediate along the OD + CO reaction path. Directly after photolysis of the chemical precursor acrylic acid-d 1 , we measure absolute trans-DOCO product concentrations with a sensitivit… Show more

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Cited by 137 publications
(106 citation statements)
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“…VIPA-based systems allow fast measurements (on the order of ms), but the simultaneous spectral coverage is limited by the detector size, so recording of the entire comb bandwidth requires sequential measurement and changing the positions of the grating [5]. Moreover, retrieving absorption spectra from the camera images requires rather complex signal analysis [5,15,23] and MIR VIPAs and cameras are quite expensive. However, VIPA-based systems can rather easily be combined with enhancement cavities using a low-bandwidth dither lock, and the high sensitivity and short acquisition time have made possible, e.g., time-resolved measurements of transient radicals [23] and reaction kinetics [24].…”
mentioning
confidence: 99%
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“…VIPA-based systems allow fast measurements (on the order of ms), but the simultaneous spectral coverage is limited by the detector size, so recording of the entire comb bandwidth requires sequential measurement and changing the positions of the grating [5]. Moreover, retrieving absorption spectra from the camera images requires rather complex signal analysis [5,15,23] and MIR VIPAs and cameras are quite expensive. However, VIPA-based systems can rather easily be combined with enhancement cavities using a low-bandwidth dither lock, and the high sensitivity and short acquisition time have made possible, e.g., time-resolved measurements of transient radicals [23] and reaction kinetics [24].…”
mentioning
confidence: 99%
“…Moreover, retrieving absorption spectra from the camera images requires rather complex signal analysis [5,15,23] and MIR VIPAs and cameras are quite expensive. However, VIPA-based systems can rather easily be combined with enhancement cavities using a low-bandwidth dither lock, and the high sensitivity and short acquisition time have made possible, e.g., time-resolved measurements of transient radicals [23] and reaction kinetics [24]. Open-air broadband trace gas sensing using a VIPA-based spectrometer has also been demonstrated [5].…”
mentioning
confidence: 99%
“…For example, Fleisher et al studied the microsecond dynamic chemical reaction using comb spectroscopy with a virtually imaged phased array. 14 As with other examples, such as observing picosecond phenomena with DCS, a short-time Fourier transform (STFT) was applied to the free induction decay signal from a molecular sample. 4 However, in the STFT scheme, the temporal resolution is restricted due to the Fourier limit.…”
Section: © 2017 Author(s) All Article Content Except Where Otherwismentioning
confidence: 99%
“…For example, individual comb components can be tuned to scan over the frequency gap. [16][17][18][19][20][21] Other methods include spatially separating the comb lines using gratings, 21 Fourier transform spectroscopy of a single OFC 22 and dual-mode spectroscopy using two OFCs. 23,24 Nevertheless, few efforts have been made to decrease the comb spacing to improve the spectral resolution.…”
Section: Introductionmentioning
confidence: 99%