Room-temperature quantification of 14^{14}CO2_{2} below the natural abundance with two-color cavity ring-down spectroscopy

Abstract

Radiocarbon's natural production, radiative decay, and isotopic rarity make it a unique tool to probe carbonaceous systems in the life and earth sciences. However, the difficulty of current radiocarbon (14^{14}C) detection methods limits scientific adoption. Here, two-color cavity ring-down spectroscopy detects 14^{14}CO2_{2} in room-temperature samples with an accuracy of 8% of the natural abundance in 3 minutes. The intra-cavity pump-probe measurement uses two cavity-enhanced lasers to cancel out cavity ring-down rate fluctuations and strong one-photon absorption interference (>10,000 1/s) from hot-band transitions of CO2_{2} isotopologues. Selective, room-temperature detection of small 14^{14}CO2_{2} absorption signals (<1 1/s) reduces the technical and operational burdens for cavity-enhanced measurements of radiocarbon, which can benefit a wide range of applications like biomedical research and field-detection of combusted fossil fuels.Comment: 4 main figures, 2 supplementary figure

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