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Title: Rapid and Sensitive Quantification of Isotopic Mixtures Using a Rapidly-Swept External Cavity Quantum Cascade Laser

A rapidly-swept external-cavity quantum cascade laser with an open-path Herriott cell is used to quantify gas-phase chemical mixtures of D2O and HDO at an update rate of 40 Hz (25 ms measurement time). The chemical mixtures were generated by evaporating D2O liquid near the open-path Herriott cell, allowing the H/D exchange reaction with ambient H2O to produce HDO. Fluctuations in the ratio of D2O and HDO on timescales of < 1 s due to the combined effects of plume transport and the H/D exchange chemical reaction are observed. Noise equivalent concentrations (1σ) (NEC) of 147.0 ppbv and 151.6 ppbv in a 25 ms measurement time are estimated for D2O and HDO respectively with a 127 m optical path. These NECs are reduced to 23.0 and 24.0 ppbv with a 1 s averaging time for D2O and HDO respectively. NECs < 200 ppbv are also estimated for N2O, F134A, CH4, Acetone, and SO2 for a 25 ms measurement time. Based on the NECs obtained for D2O and HDO, the isotopic precision for measurement of the [D2O]/[HDO] concentration ratio was studied. An isotopic precision of 33‰ and 5‰ was calculated for the current experimental conditions for measurement times of 25 ms andmore » 1 s, respectively.« less
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Resource Type:
Journal Article
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Journal Name: Photonics, 3(2):Article No. 33
Research Org:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US)
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Country of Publication:
United States