Abstract
We carry out infrared-infrared double-resonance spectroscopy of the $2{\ensuremath{\nu}}_{3}{A}_{1}\text{\ensuremath{-}}{\ensuremath{\nu}}_{3}$ band of methane. Ten transitions of Q(1) to Q(4) are observed with an 88.5-THz difference-frequency-generation (DFG) source, while the lower levels are pumped through the ${\ensuremath{\nu}}_{3}$ band transition by another 90.5-THz DFG source phase-locked to an optical frequency comb (OFC). The transition frequencies are determined using the OFC with an uncertainty of 10 kHz, which is an improvement of 4 orders of magnitude compared with the previous studies.
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