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Nature
Feb, 2025;638 (8052): 941-948.

Modulated ringdown comb interferometry for sensing of highly complex gases.

Qizhong Liang, Apoorva Bisht, Andrew Scheck, Peter G Schunemann, Jun Ye
Author Information
  1. Qizhong Liang: JILA, National Institute of Standards and Technology and University of Colorado, Boulder, CO, USA. Qizhong.Liang@colorado.edu. ORCID
  2. Apoorva Bisht: JILA, National Institute of Standards and Technology and University of Colorado, Boulder, CO, USA. ORCID
  3. Andrew Scheck: JILA, National Institute of Standards and Technology and University of Colorado, Boulder, CO, USA. ORCID
  4. Peter G Schunemann: BAE Systems, Nashua, NH, USA.
  5. Jun Ye: JILA, National Institute of Standards and Technology and University of Colorado, Boulder, CO, USA. Ye@jila.colorado.edu. ORCID
PMID: 39972145 DOI: 10.1038/s41586-024-08534-2

Abstract

Gas samples relevant to health and the environment typically contain many molecular species that span a huge concentration dynamic range. Mid-infrared frequency comb spectroscopy with high-finesse cavity enhancement has allowed the most sensitive multispecies trace-gas detections so far. However, the robust performance of this technique depends critically on ensuring absorption-path-length enhancement over a broad spectral coverage, which is severely limited by comb-cavity frequency mismatch if strongly absorbing compounds are present. Here we introduce modulated ringdown comb interferometry, a technique that resolves the vulnerability of comb-cavity enhancement to strong intracavity absorption or dispersion. This technique works by measuring ringdown dynamics carried by massively parallel comb lines transmitted through a length-modulated cavity, making use of both the periodicity of the field dynamics and the Doppler frequency shifts introduced from a Michelson interferometer. As a demonstration, we measure highly dispersive exhaled human breath samples and ambient air in the mid-infrared with finesse improved to 23,000 and coverage to 1,010 cm. Such a product of finesse and spectral coverage is orders of magnitude better than all previous demonstrations, enabling us to simultaneously quantify 20 distinct molecular species at above 1-part-per-trillion sensitivity varying in concentrations by seven orders of magnitude. This technique unlocks next-generation sensing performance for complex and dynamic molecular compositions, with scalable improvement to both finesse and spectral coverage.

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MeSH Term

Interferometry
Humans
Gases
Breath Tests
Exhalation
Spectrophotometry, Infrared
Air

Chemicals

Gases
Journal Article
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