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Peer-reviewedCC BY 4.0Journal of Physical Chemistry A

Time-Resolved Fourier-Transform Millimeter-wave Spectroscopy of the simplest Criegee Intermediate, CH₂OO, in its ν₇ = 1 state

Abstract

In the present work, we have investigated the rotational spectrum of the ν₇ = 1 vibrational state of CH₂OO in the 250-500 GHz range, produced by photolysis of CH₂I₂ precursor in the presence of O₂. In order to carry out such an investigation, we have developed a new experimental setup that combines UV pulsed laser photolysis and a room-temperature flow cell with a Fourier-transform millimeter-wave emission spectrometer. A multiple-pulse acquisition protocol enables time-resolved detection of transient species over millisecond timescales to improve signal-to-noise ratios through averaging. This system enables in situ observation of transient species and their vibrationally excited states under thermal conditions, demonstrating the capabilities of a new instrument that can record time-resolved rotational spectra. A total of 120 transitions were measured and used to determine accurate spectroscopic parameters for the CH2OO (ν₇ = 1).

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BibTeX
@article{chen2026timeresolved,
  title = {{Time-Resolved Fourier-Transform Millimeter-wave Spectroscopy of the simplest Criegee Intermediate, CH₂OO, in its ν₇ = 1 state}},
  author = {Ning Chen and Eugene Alekseev and Roman Motiyenko and Laurent Margulès and Stéphane Bailleux and Brian M. Hays},
  journal = {Journal of Physical Chemistry A},
  year = {2026},
  month = oct,
  doi = {10.1021/acs.jpca.6c02165},
  url = {https://hal.science/hal-05801391v1},
  note = {CC BY 4.0},
}
RIS
TY  - JOUR
TI  - Time-Resolved Fourier-Transform Millimeter-wave Spectroscopy of the simplest Criegee Intermediate, CH₂OO, in its ν₇ = 1 state
AU  - Ning Chen
AU  - Eugene Alekseev
AU  - Roman Motiyenko
AU  - Laurent Margulès
AU  - Stéphane Bailleux
AU  - Brian M. Hays
PY  - 2026
DA  - 2026/10/15
JO  - Journal of Physical Chemistry A
DO  - 10.1021/acs.jpca.6c02165
UR  - https://hal.science/hal-05801391v1
AB  - In the present work, we have investigated the rotational spectrum of the ν₇ = 1 vibrational state of CH₂OO in the 250-500 GHz range, produced by photolysis of CH₂I₂ precursor in the presence of O₂. In order to carry out such an investigation, we have developed a new experimental setup that combines UV pulsed laser photolysis and a room-temperature flow cell with a Fourier-transform millimeter-wave emission spectrometer. A multiple-pulse acquisition protocol enables time-resolved detection of transient species over millisecond timescales to improve signal-to-noise ratios through averaging. This system enables in situ observation of transient species and their vibrationally excited states under thermal conditions, demonstrating the capabilities of a new instrument that can record time-resolved rotational spectra. A total of 120 transitions were measured and used to determine accurate spectroscopic parameters for the CH2OO (ν₇ = 1).
SN  - 1089-5639
SN  - 1520-5215
ER  -