Sub-Doppler slit jet infrared spectroscopy of astrochemically relevant cations: The NH stretching mode in ND3H+
Abstract
High-resolution rotationally resolved spectra of the N–H stretch vibrational mode (ν1) of jet-cooled ND3H+ ions are collected and analyzed in a sub-Doppler slit-jet infrared spectrometer. The isotopomeric ammonium ions are generated by proton transfer from H3+ to ND3 in a discharge of an ND3/H2 gas mixture, whereby the slit jet expansion cools the nascent ND3H+ ions into lower rotational states. Rotational assignments are confirmed by four-line combination differences that agree to within the spectrometer precision (9 MHz). Based on precision two-line ground-state combination differences and a symmetric top Hamiltonian, the B, DJ, and DJK rotational constants for the ground vibrational state of ND3H+ are determined with high precision for the first time. Approximate rotational constants for the ν1 excited state are also determined, with a band origin at 3316.8425(19) cm-1 and in remarkable (~0.1 cm-1) agreement with high level anharmonic theoretical predictions by Guo and co-workers [J. Phys. Chem. A, 120, 2185 (2016)]. Our results allow us to predict several low-J pure rotational transitions of ND3H+, which we hope will support future studies of this important ion in laboratory and astronomical rotational spectroscopy.
- Authors:
-
- Spectra Sensors, Houston, TX (United States)
- Univ. of Colorado, Boulder, CO (United States)
- Publication Date:
- Research Org.:
- Univ. of Colorado, Boulder, CO (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1610626
- Alternate Identifier(s):
- OSTI ID: 1476693; OSTI ID: 1924533
- Grant/Contract Number:
- SC0002123; FG02-09ER16021
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 149; Journal Issue: 14; Journal ID: ISSN 0021-9606
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Chemistry; Physics; Vibrational spectroscopy; Infrared spectroscopy; Interstellar medium; Isotopes; Ab initio coupled-cluster calculations; Rotational spectroscopy
Citation Formats
Chang, Chih-Hsuan, Scrape, Preston G., and Nesbitt, David J. Sub-Doppler slit jet infrared spectroscopy of astrochemically relevant cations: The NH stretching mode in ND3H+. United States: N. p., 2018.
Web. doi:10.1063/1.5049603.
Chang, Chih-Hsuan, Scrape, Preston G., & Nesbitt, David J. Sub-Doppler slit jet infrared spectroscopy of astrochemically relevant cations: The NH stretching mode in ND3H+. United States. https://doi.org/10.1063/1.5049603
Chang, Chih-Hsuan, Scrape, Preston G., and Nesbitt, David J. Mon .
"Sub-Doppler slit jet infrared spectroscopy of astrochemically relevant cations: The NH stretching mode in ND3H+". United States. https://doi.org/10.1063/1.5049603. https://www.osti.gov/servlets/purl/1610626.
@article{osti_1610626,
title = {Sub-Doppler slit jet infrared spectroscopy of astrochemically relevant cations: The NH stretching mode in ND3H+},
author = {Chang, Chih-Hsuan and Scrape, Preston G. and Nesbitt, David J.},
abstractNote = {High-resolution rotationally resolved spectra of the N–H stretch vibrational mode (ν1) of jet-cooled ND3H+ ions are collected and analyzed in a sub-Doppler slit-jet infrared spectrometer. The isotopomeric ammonium ions are generated by proton transfer from H3+ to ND3 in a discharge of an ND3/H2 gas mixture, whereby the slit jet expansion cools the nascent ND3H+ ions into lower rotational states. Rotational assignments are confirmed by four-line combination differences that agree to within the spectrometer precision (9 MHz). Based on precision two-line ground-state combination differences and a symmetric top Hamiltonian, the B, DJ, and DJK rotational constants for the ground vibrational state of ND3H+ are determined with high precision for the first time. Approximate rotational constants for the ν1 excited state are also determined, with a band origin at 3316.8425(19) cm-1 and in remarkable (~0.1 cm-1) agreement with high level anharmonic theoretical predictions by Guo and co-workers [J. Phys. Chem. A, 120, 2185 (2016)]. Our results allow us to predict several low-J pure rotational transitions of ND3H+, which we hope will support future studies of this important ion in laboratory and astronomical rotational spectroscopy.},
doi = {10.1063/1.5049603},
journal = {Journal of Chemical Physics},
number = 14,
volume = 149,
place = {United States},
year = {Mon Oct 08 00:00:00 EDT 2018},
month = {Mon Oct 08 00:00:00 EDT 2018}
}
Web of Science
Works referenced in this record:
Concentration modulation spectroscopy with a pulsed slit supersonic discharge expansion source
journal, August 2001
- Davis, Scott; Fárnı́k, Michal; Uy, Dairene
- Chemical Physics Letters, Vol. 344, Issue 1-2
Slit Discharge IR Spectroscopy of a Jet-Cooled Cyclopropyl Radical: Structure and Intramolecular Tunneling Dynamics †
journal, March 2006
- Dong, Feng; Davis, Scott; Nesbitt, David J.
- The Journal of Physical Chemistry A, Vol. 110, Issue 9
Vibrations of the ammonium-d ion in ammonium tetrafluoroborate crystals at low temperatures
journal, July 1987
- Roberts, Malcolm P.; Strauss, Herbert L.
- The Journal of Physical Chemistry, Vol. 91, Issue 16
Accurate ab initio quartic force field and vibrational frequencies of the NH4+ ion and its deuterated forms
journal, August 1996
- Martin, Jan M. L.; Lee, Timothy J.
- Chemical Physics Letters, Vol. 258, Issue 1-2
The abundances of nitrogen-containing molecules during pre-protostellar collapse
journal, August 2006
- Flower, D. R.; Pineau des Forêts, G.; Walmsley, C. M.
- Astronomy & Astrophysics, Vol. 456, Issue 1
Sub-Doppler slit jet infrared spectroscopy of astrochemically relevant cations: Symmetric (ν1) and antisymmetric (ν6) NH stretching modes in ND 2 H 2 +
journal, January 2018
- Chang, Chih-Hsuan; Nesbitt, David J.
- The Journal of Chemical Physics, Vol. 148, Issue 1
An intense slit discharge source of jet-cooled molecular ions and radicals (Trot < 30 K
journal, August 1996
- Anderson, David T.; Davis, Scott; Zwier, Timothy S.
- Chemical Physics Letters, Vol. 258, Issue 1-2
Does metallic ammonium exist? (From old and new literature)
journal, August 1978
- Stishov, Sergei M.
- Soviet Physics Uspekhi, Vol. 21, Issue 8
Rotation and Solvation of Ammonium Ion
journal, December 1987
- Perrin, C. L.; Gipe, R. K.
- Science, Vol. 238, Issue 4832
IMPROVED DETERMINATION OF THE 1 0 -0 0 ROTATIONAL FREQUENCY OF NH 3 D + FROM THE HIGH-RESOLUTION SPECTRUM OF THE ν 4 INFRARED BAND
journal, June 2013
- Doménech, J. L.; Cueto, M.; Herrero, V. J.
- The Astrophysical Journal, Vol. 771, Issue 1
Detection of the Ammonium ion in Space
journal, June 2013
- Cernicharo, J.; Tercero, B.; Fuente, A.
- The Astrophysical Journal, Vol. 771, Issue 1
Structure of the ammonium radical from a rotationally resolved photoelectron spectrum
journal, April 1997
- Signorell, R.; Palm, H.; Merkt, F.
- The Journal of Chemical Physics, Vol. 106, Issue 16
Observation of forbidden transitions of ammonium ion (NH + 4 ) ν 3 band and determination of ground state rotational constants. Observation of ν 3 band allowed transitions of ND + 4
journal, June 1987
- Crofton, Mark W.; Oka, Takeshi
- The Journal of Chemical Physics, Vol. 86, Issue 11
Observations of NH \documentclass{aastex} \usepackage{amsbsy} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{bm} \usepackage{mathrsfs} \usepackage{pifont} \usepackage{stmaryrd} \usepackage{textcomp} \usepackage{portland,xspace} \usepackage{amsmath,amsxtra} \usepackage[OT2,OT1]{fontenc} \newcommand\cyr{ \renewcommand\rmdefault{wncyr} \renewcommand\sfdefault{wncyss} \renewcommand\encodingdefault{OT2} \normalfont \selectfont} \DeclareTextFontCommand{\textcyr}{\cyr} \pagestyle{empty} \DeclareMathSizes{10}{9}{7}{6} \begin{document} \landscape $_{2}$ \end{document} D toward Dark Molecular Clouds
journal, May 2000
- Saito, Shuji; Ozeki, Hiroyuki; Ohishi, Masatoshi
- The Astrophysical Journal, Vol. 535, Issue 1
Rotation, solvation, and hydrogen bonding of aqueous ammonium ion
journal, March 1986
- Perrin, Charles L.; Gipe, Robert K.
- Journal of the American Chemical Society, Vol. 108, Issue 5
Electron-Driven Acid-Base Chemistry: Proton Transfer from Hydrogen Chloride to Ammonia
journal, February 2008
- Eustis, Soren N.; Radisic, Dunja; Bowen, Kit H.
- Science, Vol. 319, Issue 5865
Mechanism of Ammonia Transport by Amt/MEP/Rh: Structure of AmtB at 1.35 A
journal, September 2004
- Khademi, S.
- Science, Vol. 305, Issue 5690
Infrared spectrum of the NH4-dn+ cation trapped in solid neon
journal, January 2005
- Jacox, Marilyn E.; ThompsonGuest researcher, National, Warren E.
- Physical Chemistry Chemical Physics, Vol. 7, Issue 5
Jet cooled spectroscopy of H2DO+: Barrier heights and isotope-dependent tunneling dynamics from H3O+ to D3O+
journal, October 2006
- Dong, Feng; Nesbitt, David J.
- The Journal of Chemical Physics, Vol. 125, Issue 14
Orientational order-disorder of ND4+/NH4+ in synthetic ND4/NH4-phlogopite: a low-temperature infrared study [Orientational order-disorder of ND4+/NH4+ in synthetic ND4/NH4-phlogopite: a low-temperature infrared study]
journal, November 2002
- Mookherjee, Mainak; Redfern, Simon A. T.; Zhang, Ming
- European Journal of Mineralogy, Vol. 14, Issue 6
PGOPHER: A program for simulating rotational, vibrational and electronic spectra
journal, January 2017
- Western, Colin M.
- Journal of Quantitative Spectroscopy and Radiative Transfer, Vol. 186
Characterization of an Ammonium Transport Protein from the Peribacteroid Membrane of Soybean Nodules
journal, August 1998
- Kaiser, B. N.
- Science, Vol. 281, Issue 5380
The ν4Band of Ammonium, NH+4
journal, September 1996
- Park, Joonbum; Xia, Changhong; Selby, Stan
- Journal of Molecular Spectroscopy, Vol. 179, Issue 1
Detection of Triply Deuterated Ammonia in the Barnard 1 Cloud
journal, May 2002
- Lis, D. C.; Roueff, E.; Gerin, M.
- The Astrophysical Journal, Vol. 571, Issue 1
A channel-like transporter for NH4+ on the symbiotic interface of N2-fixing plants
journal, December 1995
- Tyerman, Stephen D.; Whitehead, Lynne F.; Day, David A.
- Nature, Vol. 378, Issue 6557
Ultrasensitive laser measurements without tears
journal, January 1997
- Hobbs, Philip C. D.
- Applied Optics, Vol. 36, Issue 4
Full-Dimensional Quantum Calculations of Vibrational Levels of NH 4 + and Isotopomers on An Accurate Ab Initio Potential Energy Surface
journal, April 2016
- Yu, Hua-Gen; Han, Huixian; Guo, Hua
- The Journal of Physical Chemistry A, Vol. 120, Issue 14
Interstellar deuterated ammonia: from NH 3 to ND 3
journal, July 2005
- Roueff, E.; Lis, D. C.; van der Tak, F. F. S.
- Astronomy & Astrophysics, Vol. 438, Issue 2
Difference-frequency laser spectroscopy of the ν 4 fundamental band of NH 3 D +
journal, October 1986
- Nakanaga, T.; Amano, T.
- Canadian Journal of Physics, Vol. 64, Issue 10
The ν3 Fundamental in C2H2
journal, February 1993
- Vanderauwera, J.; Hurtmans, D.; Carleer, M.
- Journal of Molecular Spectroscopy, Vol. 157, Issue 2
Ground State Rotational Lines of Doubly Deuterated Ammonia as Tracers of the Physical Conditions and Chemistry of Cold Interstellar Medium
journal, January 2006
- Lis, D. C.; Gerin, M.; Roueff, E.
- The Astrophysical Journal, Vol. 636, Issue 2
Origin of the 6.85 $\mathsf{\mu}$m band near young stellar objects: The ammonium ion (NH 4^+ ) revisited
journal, January 2003
- Schutte, W. A.; Khanna, R. K.
- Astronomy & Astrophysics, Vol. 398, Issue 3
Does metallic ammonium exist? (From old and new literature) [Существует ли металлический аммоний? (Из старой и новой литературы)]
journal, January 1978
- Stishov, Sergei M.
- Uspekhi Fizicheskih Nauk, Vol. 125, Issue 8
Gaseous ammonia and ammonium ions in the free troposphere
journal, May 1986
- Ziereis, H.; Arnold, F.
- Nature, Vol. 321, Issue 6069
Gas‐Phase Production of NHD 2 in L134N
journal, June 2001
- Rodgers, S. D.; Charnley, S. B.
- The Astrophysical Journal, Vol. 553, Issue 2
Spin-state chemistry of deuterated ammonia
journal, September 2015
- Sipilä, O.; Harju, J.; Caselli, P.
- Astronomy & Astrophysics, Vol. 581
A high resolution study of the ν 3 band of the ammonium ion (NH + 4 ) by velocity modulation laser absorption spectroscopy
journal, May 1984
- Schäfer, Eckhard; Saykally, Richard J.; Robiette, Alan G.
- The Journal of Chemical Physics, Vol. 80, Issue 9
Infrared studies of molecular ions. I. The ν 3 band of NH 4 +
journal, September 1983
- Crofton, Mark W.; Oka, Takeshi
- The Journal of Chemical Physics, Vol. 79, Issue 6
The ν 3 vibrational spectrum of the free ammonium ion (NH 4 + )
journal, September 1983
- Schäfer, Eckhard; Begemann, Marianne H.; Gudeman, Christopher S.
- The Journal of Chemical Physics, Vol. 79, Issue 6
Velocity modulation infrared laser spectroscopy of molecular ions: The
journal, April 1989
- Polak, Mark; Gruebele, Martin; DeKock, Bruce W.
- Molecular Physics, Vol. 66, Issue 6
Triply deuterated ammonia in NGC 1333
journal, June 2002
- van der Tak, F. F. S.; Schilke, P.; Müller, H. S. P.
- Astronomy & Astrophysics, Vol. 388, Issue 3
Laser spectroscopy of jet-cooled ethyl radical: Infrared studies in the CH2 stretch manifold
journal, January 2000
- Davis, Scott; Uy, Dairene; Nesbitt, David J.
- The Journal of Chemical Physics, Vol. 112, Issue 4
Laboratory rotational ground state transitions of NH 3 D + and CF +
journal, September 2016
- Stoffels, A.; Kluge, L.; Schlemmer, S.
- Astronomy & Astrophysics, Vol. 593
Observing the gas temperature drop in the high-density nucleus of L 1544
journal, May 2007
- Crapsi, A.; Caselli, P.; Walmsley, M. C.
- Astronomy & Astrophysics, Vol. 470, Issue 1
Works referencing / citing this record:
Suppressed-Doppler slit jet infrared spectroscopy of astrochemically relevant cations: ν1 and ν4 NH stretching modes in NH 3 D +
journal, August 2019
- Scrape, Preston G.; Chang, Chih-Hsuan; Nesbitt, David J.
- The Journal of Chemical Physics, Vol. 151, Issue 8
Accurate Rotational Rest Frequencies for Ammonium Ion Isotopologues
journal, October 2018
- Doménech, José L.; Schlemmer, Stephan; Asvany, Oskar
- The Astrophysical Journal, Vol. 866, Issue 2