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-μm continuous wave optical parametric oscillator as a pump and a 1.67-μm 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 ν 3 fundamental band, we detected 36 ladder-type transitions to the 3ν 3 overtone band region, and 18 V-type transitions to the 2ν 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.
We report the first measurement of sub-Doppler molecular response using a frequency comb by employing the comb as a probe in optical-optical double-resonance spectroscopy. We use a 3.3 μm continuous wave pump and a 1.67 μm comb probe to detect sub-Doppler transitions to the 2ν 3 and 3ν 3 bands of methane with ∼1.7 MHz center frequency accuracy. These measurements provide the first verification of the accuracy of theoretical predictions from highly vibrationally excited states, needed to model the high-temperature spectra of exoplanets. Transition frequencies to the 3ν 3 band show good agreement with the TheoReTS line list.
We experimentally demonstrate in a difference-frequency generation mid-infrared frequency comb source the effect of temporal overlap between pump-and signal-pulse to the relative intensity noise (RIN) of the idler pulse. When scanning the temporal delay between our 130 fs long signal-and pump pulses, we observe a RIN minimum with a 3 dB width of 20 fs delay and an RIN increase of 20 dB in 40 fs delay at the edges of this minimum. We also demonstrate active long-term stabilization of the mid-infrared frequency comb source to the temporal overlap setting corresponding to the lowest RIN operation point by an on-line RIN-detector and active feedback control of the pump-signal-pulse delay. This active stabilization set-up allowed us to dramatically increase the signal-to-noise ratio of mid-infrared absorption spectra.
We use a 3.3 μm continuous wave optical parametric oscillator as a pump and a 1.67 μm frequency comb as a probe to record 36 sub-Doppler double-resonance transitions in the 3v3 band of methane (including 26 previously unreported) with ~1.5 MHz center frequency accuracy
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