Detection of trace gases, such as radioactive carbon dioxide, clumped isotopes, and reactive radicals, is of great interest and poses significant challenges in various fields. Achieving both high selectivity and high sensitivity is essential in this context. We present a highly selective molecular spectroscopy method based on comb-locked, mid-infrared, cavity-enhanced, two-photon absorption. The Doppler-free nature of two-photon transitions considerably reduces the width of the resonance, which improves the selectivity and avoids interference due to nearby transitions from other molecules. The high-finesse optical cavity increases the laser power by thousands of times and compensates for the small cross-section of the two-photon transition. The quantitative capability of the method is demonstrated by measuring CO abundances in CO samples. The method is promising for the quantitative measurement of extremely trace molecules or isotopologues in gas samples.
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http://dx.doi.org/10.1021/acs.analchem.4c05414 | DOI Listing |
Anal Chem
January 2025
Hefei National Laboratory, University of Science and Technology of China, Hefei 230088, China.
Detection of trace gases, such as radioactive carbon dioxide, clumped isotopes, and reactive radicals, is of great interest and poses significant challenges in various fields. Achieving both high selectivity and high sensitivity is essential in this context. We present a highly selective molecular spectroscopy method based on comb-locked, mid-infrared, cavity-enhanced, two-photon absorption.
View Article and Find Full Text PDFWe present a novel technique for in-vacuum cavity-enhanced UV spectroscopy that allows nearly continuous measurements over several days, minimizing mirror degradation caused by high-power UV radiation. Our method relies on pulsing of the cavity's internal power, which increases the UV intensity to maximum only for short periods when the studied atom is within the cavity mode volume while keeping the average power low to prevent mirror degradation. Additionally, this method significantly decreases laser-induced background on charged particle detectors.
View Article and Find Full Text PDFNat Nanotechnol
May 2022
State Key Laboratory of Optoelectronic Materials and Technologies, School of Physics, School of Electronics and Information Technology, Sun Yat-sen University, Guangzhou, China.
The coherent interaction of electromagnetic fields with solid-state two-level systems can yield deterministic quantum light sources for photonic quantum technologies. To date, the performance of semiconductor single-photon sources based on three-level systems is limited mainly due to a lack of high photon indistinguishability. Here we tailor the cavity-enhanced spontaneous emission from a ladder-type three-level system in a single epitaxial quantum dot through stimulated emission.
View Article and Find Full Text PDFFrequency-stabilized mid-infrared lasers are valuable tools for precision molecular spectroscopy. However, their implementation remains limited by complicated stabilization schemes. Here we achieve optical self-locking of a quantum cascade laser to the resonant leak-out field of a highly mode-matched two-mirror cavity.
View Article and Find Full Text PDFNano Lett
December 2019
Center for Integrated Nanotechnologies, Materials Physics and Applications Division , Los Alamos National Laboratory , Los Alamos , New Mexico 87545 , United States.
Indistinguishable single photon generation at telecom wavelengths from solid-state quantum emitters remains a significant challenge to scalable quantum information processing. Here we demonstrate efficient generation of "indistinguishable" single photons directly in the telecom O-band from aryl-functionalized carbon nanotubes by overcoming the emitter quantum decoherence with plasmonic nanocavities. With an unprecedented single-photon spontaneous emission time down to 10 ps (from initially 0.
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