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Long-wave mid-infrared time-resolved dual-comb spectroscopy of short-lived intermediates

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Abstract

In this Letter, an electro-optic dual-comb spectrometer with a central tunable range of 7.77–8.22 µm is demonstrated to perform transient absorption spectroscopy of the simplest Criegee intermediate (${{\rm{CH}}_2}{\rm{OO}}$), a short-lived species involved in many key atmospheric reactions, and its self-reaction product via comb-mode-resolved spectral sampling at microsecond temporal resolution. By combining with a Herriott-type flash photolysis cell, ${{\rm{CH}}_2}{\rm{OO}}$ can be probed with a detection limit down to ${\sim}{{1}} \times {{10}^{11}}\; {\rm molecules }\,{{\rm{cm}}^{- 3}}$. Moreover, pressure broadening of ${{\rm{CH}}_2}{\rm{OO}}$ absorption lines can be studied with spectrally interleaved dual-comb spectroscopy. This Letter holds promise for high-resolution precision measurements of transient molecules, especially for the study of large molecules in complex systems.

© 2020 Optical Society of America

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