Journal
PHYSICAL REVIEW A
Volume 103, Issue 2, Pages -Publisher
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevA.103.022810
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Funding
- Swedish Research Council [2016-03593, 2015-04374]
- Knut and Alice Wallenberg Foundation [KAW 2015.0159]
- Foundation for Polish Science [POIR.04.04.00-00-434D/17-00]
- Kempe Foundations [JCK 1317.1]
- Swedish Research Council [2015-04374] Funding Source: Swedish Research Council
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Optical-optical double-resonance spectroscopy technique was used to measure sub-Doppler transitions in highly excited molecular states. The study focused on methane molecules, with results showing good agreement with theoretical predictions.
Optical-optical double-resonance spectroscopy with a continuous wave pump and frequency comb probe allows measurement of sub-Doppler transitions to highly excited molecular states over a wide spectral range with high frequency accuracy. We report on assessment and characterization of sub-Doppler double-resonance transitions in methane measured using a 3.3-mu m continuous wave optical parametric oscillator as a pump and a 1.67-mu m frequency comb as a probe. The comb spectra were recorded using a Fourier transform spectrometer with comb-mode-limited resolution. With the pump tuned to nine different transitions in the nu(3) fundamental band, we detected 36 ladder-type transitions to the 3 nu(3) overtone band region, and 18 V-type transitions to the 2 nu(3) overtone band. We describe in detail the experimental approach and the pump stabilization scheme, which currently limits the frequency accuracy of the measurement. We present the data analysis procedure used to extract the frequencies and intensities of the probe transitions for parallel and perpendicular relative pump-probe polarization. We compare the center frequencies and relative intensities of the ladder-type transitions to theoretical predictions from the TheoReTS and ExoMol line lists, demonstrating good agreement with TheoReTS.
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