Suppressed-Doppler slit jet infrared spectroscopy of astrochemically relevant cations: $$ν_1$$ and $$ν_4$$ NH stretching modes in NH3D+
Abstract
A suppressed-Doppler (Δν = 180 MHz) infrared spectrum of monodeuterated ammonium ions (NH3D+) has been obtained for the ν1 (symmetric) and ν4 (degenerate) N–H stretch bands via direct absorption high resolution IR laser spectroscopy in a planar slit jet discharge expansion. The ion is efficiently generated by H3+ protonation of NH2D in a discharge mixture of H2/NH2D, with the resulting expansion rapidly cooling the molecular ions into low rotational states. The first high-resolution infrared spectrum of ν1 is reported, as well as many previously unobserved transitions in the ν4 rovibrational manifold. Simultaneous observation of both ν1 and ν4 permits elucidation of both the vibrational ground and excited state properties of the ion, including rigorous benchmarking of band origins against high-level anharmonic ab initio theory as well as determination of the ν1:ν4 intensity ratio for comparison with bond-dipole model predictions. Ground-state combination differences from this work and earlier studies permit the rotational constants of NH3D+ to be determined to unprecedented accuracy, the results of which support previous laboratory and astronomical assignment of the 10–00 pure rotational transition and should aid future searches for other rotational transitions as well.
- Authors:
-
[2];
[1]
- National Inst. of Standards and Technology (NIST), Boulder, CO (United States); Univ. of Colorado, Boulder, CO (United States)
- SpectraSensors, Houston, TX (United States)
- Publication Date:
- Research Org.:
- Univ. of Colorado, Boulder, CO (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC); National Science Foundation (NSF)
- OSTI Identifier:
- 1610628
- Alternate Identifier(s):
- OSTI ID: 1558705; OSTI ID: 1924531
- Grant/Contract Number:
- SC0002123; FG02-09ER16021; CHE 1665271; PHY 1734006
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 151; Journal Issue: 8; Journal ID: ISSN 0021-9606
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 47 OTHER INSTRUMENTATION; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; chemistry; physics
Citation Formats
Scrape, Preston G., Chang, Chih-Hsuan, and Nesbitt, David J. Suppressed-Doppler slit jet infrared spectroscopy of astrochemically relevant cations: $ν_1$ and $ν_4$ NH stretching modes in NH3D+. United States: N. p., 2019.
Web. doi:10.1063/1.5113962.
Scrape, Preston G., Chang, Chih-Hsuan, & Nesbitt, David J. Suppressed-Doppler slit jet infrared spectroscopy of astrochemically relevant cations: $ν_1$ and $ν_4$ NH stretching modes in NH3D+. United States. https://doi.org/10.1063/1.5113962
Scrape, Preston G., Chang, Chih-Hsuan, and Nesbitt, David J. Fri .
"Suppressed-Doppler slit jet infrared spectroscopy of astrochemically relevant cations: $ν_1$ and $ν_4$ NH stretching modes in NH3D+". United States. https://doi.org/10.1063/1.5113962. https://www.osti.gov/servlets/purl/1610628.
@article{osti_1610628,
title = {Suppressed-Doppler slit jet infrared spectroscopy of astrochemically relevant cations: $ν_1$ and $ν_4$ NH stretching modes in NH3D+},
author = {Scrape, Preston G. and Chang, Chih-Hsuan and Nesbitt, David J.},
abstractNote = {A suppressed-Doppler (Δν = 180 MHz) infrared spectrum of monodeuterated ammonium ions (NH3D+) has been obtained for the ν1 (symmetric) and ν4 (degenerate) N–H stretch bands via direct absorption high resolution IR laser spectroscopy in a planar slit jet discharge expansion. The ion is efficiently generated by H3+ protonation of NH2D in a discharge mixture of H2/NH2D, with the resulting expansion rapidly cooling the molecular ions into low rotational states. The first high-resolution infrared spectrum of ν1 is reported, as well as many previously unobserved transitions in the ν4 rovibrational manifold. Simultaneous observation of both ν1 and ν4 permits elucidation of both the vibrational ground and excited state properties of the ion, including rigorous benchmarking of band origins against high-level anharmonic ab initio theory as well as determination of the ν1:ν4 intensity ratio for comparison with bond-dipole model predictions. Ground-state combination differences from this work and earlier studies permit the rotational constants of NH3D+ to be determined to unprecedented accuracy, the results of which support previous laboratory and astronomical assignment of the 10–00 pure rotational transition and should aid future searches for other rotational transitions as well.},
doi = {10.1063/1.5113962},
journal = {Journal of Chemical Physics},
number = 8,
volume = 151,
place = {United States},
year = {2019},
month = {8}
}
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