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Detection sensitivity is one of the most important attributes to considerduring selection of spectroscopic techniques. However, high sensitivity aloneis insufficient for spectroscopic measurements in spectrally congested regions.Two-color cavity ringdown spectroscopy (2C-CRDS), based on intra-cavitypump-probe detection, simultaneously achieves high detection sensitivity andselectivity. The technique enables mid-infrared detection of radiocarbondioxide ($^{14}$CO$_2$) molecules in room-temperature CO$_2$ samples, withbetter than 10 parts-per-quadrillion (ppq, 10$^{15}$) quantitation accuracy (4ppq on average). These $highly$-$reproducible$ measurements, which are the most$\it{sensitive}$ and $\it{quantitatively}$ $\it{accurate}$ in the mid-infrared,are accomplished despite the presence of$\it{orders}$-$\it{of}$-$\it{magnitude}$ stronger, one-photon signals fromother CO$_2$ isotopologues. This is a major achievement in laser spectroscopy.A room-temperature-operated, compact, and low-cost 2C-CRDS sensor for$^{14}$CO$_2$ benefits a wide range of scientific fields that utilize $^{14}$Cfor dating and isotope tracing, most notably atmospheric $^{14}$CO$_2$monitoring to track CO$_2$ emissions from fossil fuels. The 2C-CRDS techniquesignificantly enhances the general utility of high-resolution mid-infrareddetection for analytical measurements and fundamental chemical dynamicsstudies.

Mid-infrared trace detection with parts-per-quadrillion quantitation accuracy: Expanding frontiers of radiocarbon sensing