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Accurately Measuring Molecular Rotational Spectra in Excited Vibrational Modes.

Publication ,  Journal Article
Chevalier, P; Piccardo, M; Amirzhan, A; Capasso, F; Everitt, HO
Published in: Applied Spectroscopy
December 2022

Although gas phase rotational spectroscopy is a mature field for which millions of rotational spectral lines have been measured in hundreds of molecules with sub-MHz accuracy, it remains a challenge to measure these rotational spectra in excited vibrational modes with the same accuracy. Recently, it was demonstrated that virtually any rotational transition in excited vibrational modes of most molecules may be made to lase when pumped by a continuously tunable quantum cascade laser (QCL). Here, we demonstrate how an infrared QCL may be used to enhance absorption strength or induce lasing of terahertz rotational transitions in highly excited vibrational modes in order to measure their frequencies more accurately. To illustrate the concepts, we used a tunable QCL to excite v3 R-branch transitions in N2O and either enhanced absorption or induced lasing on 20 v3 rotational transitions, whose frequencies between 299 and 772 GHz were then measured using either heterodyne or modulation spectroscopy. The spectra were fitted to obtain the rotational constants B3 and D3, which reproduce the measured spectra to within the experimental uncertainty of ± 5 kHz. We then show how this technique may be generalized by estimating the threshold power to make any rotational transition lase in any N2O vibrational mode.

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Published In

Applied Spectroscopy

DOI

EISSN

1943-3530

ISSN

0003-7028

Publication Date

December 2022

Volume

76

Issue

12

Start / End Page

1494 / 1503

Related Subject Headings

  • Vibration
  • Spectrum Analysis
  • Lasers, Semiconductor
  • Analytical Chemistry
  • 0913 Mechanical Engineering
  • 0306 Physical Chemistry (incl. Structural)
  • 0301 Analytical Chemistry
 

Citation

APA
Chicago
ICMJE
MLA
NLM
Chevalier, P., Piccardo, M., Amirzhan, A., Capasso, F., & Everitt, H. O. (2022). Accurately Measuring Molecular Rotational Spectra in Excited Vibrational Modes. Applied Spectroscopy, 76(12), 1494–1503. https://doi.org/10.1177/00037028221111174
Chevalier, Paul, Marco Piccardo, Arman Amirzhan, Federico Capasso, and Henry O. Everitt. “Accurately Measuring Molecular Rotational Spectra in Excited Vibrational Modes.Applied Spectroscopy 76, no. 12 (December 2022): 1494–1503. https://doi.org/10.1177/00037028221111174.
Chevalier P, Piccardo M, Amirzhan A, Capasso F, Everitt HO. Accurately Measuring Molecular Rotational Spectra in Excited Vibrational Modes. Applied Spectroscopy. 2022 Dec;76(12):1494–503.
Chevalier, Paul, et al. “Accurately Measuring Molecular Rotational Spectra in Excited Vibrational Modes.Applied Spectroscopy, vol. 76, no. 12, Dec. 2022, pp. 1494–503. Epmc, doi:10.1177/00037028221111174.
Chevalier P, Piccardo M, Amirzhan A, Capasso F, Everitt HO. Accurately Measuring Molecular Rotational Spectra in Excited Vibrational Modes. Applied Spectroscopy. 2022 Dec;76(12):1494–1503.
Journal cover image

Published In

Applied Spectroscopy

DOI

EISSN

1943-3530

ISSN

0003-7028

Publication Date

December 2022

Volume

76

Issue

12

Start / End Page

1494 / 1503

Related Subject Headings

  • Vibration
  • Spectrum Analysis
  • Lasers, Semiconductor
  • Analytical Chemistry
  • 0913 Mechanical Engineering
  • 0306 Physical Chemistry (incl. Structural)
  • 0301 Analytical Chemistry