skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Full-dimensional quantum calculations of vibrational levels of NH4+ and isotopomers on an accurate ab initio potential energy surface

Abstract

Vibrational energy levels of the ammonium cation (NH4+) and its deuterated isotopomers are calculated using a numerically exact kinetic energy operator on a recently developed nine-dimensional permutation invariant semiglobal potential energy surface fitted to a large number of high-level ab initio points. Like CH4, the vibrational levels of NH4+ and ND4+ exhibit a polyad structure, characterized by a collective quantum number P = 2(v1 + v3) + v2 + v4. As a result, the low-lying vibrational levels of all isotopomers are assigned and the agreement with available experimental data is better than 1 cm–1.

Authors:
;  [1];  [2]
  1. Univ. of New Mexico, Albuquerque, NM (United States); Northwestern Univ., Shaanxi (China)
  2. Univ. of New Mexico, Albuquerque, NM (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1245399
Report Number(s):
BNL-111996-2016-JA
Journal ID: ISSN 1089-5639; R&D Project: CO006; KC0301020
Grant/Contract Number:  
SC00112704
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory
Additional Journal Information:
Journal Volume: 67; Journal Issue: 10; Journal ID: ISSN 1089-5639
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Hua -Gen Yu, Han, Huixian, and Guo, Hua. Full-dimensional quantum calculations of vibrational levels of NH4+ and isotopomers on an accurate ab initio potential energy surface. United States: N. p., 2016. Web. https://doi.org/10.1021/acs.jpca.6b01946.
Hua -Gen Yu, Han, Huixian, & Guo, Hua. Full-dimensional quantum calculations of vibrational levels of NH4+ and isotopomers on an accurate ab initio potential energy surface. United States. https://doi.org/10.1021/acs.jpca.6b01946
Hua -Gen Yu, Han, Huixian, and Guo, Hua. Tue . "Full-dimensional quantum calculations of vibrational levels of NH4+ and isotopomers on an accurate ab initio potential energy surface". United States. https://doi.org/10.1021/acs.jpca.6b01946. https://www.osti.gov/servlets/purl/1245399.
@article{osti_1245399,
title = {Full-dimensional quantum calculations of vibrational levels of NH4+ and isotopomers on an accurate ab initio potential energy surface},
author = {Hua -Gen Yu and Han, Huixian and Guo, Hua},
abstractNote = {Vibrational energy levels of the ammonium cation (NH4+) and its deuterated isotopomers are calculated using a numerically exact kinetic energy operator on a recently developed nine-dimensional permutation invariant semiglobal potential energy surface fitted to a large number of high-level ab initio points. Like CH4, the vibrational levels of NH4+ and ND4+ exhibit a polyad structure, characterized by a collective quantum number P = 2(v1 + v3) + v2 + v4. As a result, the low-lying vibrational levels of all isotopomers are assigned and the agreement with available experimental data is better than 1 cm–1.},
doi = {10.1021/acs.jpca.6b01946},
journal = {Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory},
number = 10,
volume = 67,
place = {United States},
year = {2016},
month = {3}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 2 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Theoretical Methods for Rovibrational States of Floppy Molecules
journal, October 1989


Methods for calculating vibrational energy levels
journal, June 2004

  • Carrington, Tucker
  • Canadian Journal of Chemistry, Vol. 82, Issue 6
  • DOI: 10.1139/v04-014

Variational quantum approaches for computing vibrational energies of polyatomic molecules
journal, August 2008

  • Bowman, Joel M.; Carrington, Tucker; Meyer, Hans-Dieter
  • Molecular Physics, Vol. 106, Issue 16-18
  • DOI: 10.1080/00268970802258609

Two-layer Lanczos iteration approach to molecular spectroscopic calculation
journal, November 2002

  • Yu, Hua-Gen
  • The Journal of Chemical Physics, Vol. 117, Issue 18
  • DOI: 10.1063/1.1511721

An exact variational method to calculate vibrational energies of five atom molecules beyond the normal mode approach
journal, August 2002

  • Yu, Hua-Gen
  • The Journal of Chemical Physics, Vol. 117, Issue 5
  • DOI: 10.1063/1.1488575

New ideas for using contracted basis functions with a Lanczos eigensolver for computing vibrational spectra of molecules with four or more atoms
journal, October 2002

  • Wang, Xiao-Gang; Carrington, Tucker
  • The Journal of Chemical Physics, Vol. 117, Issue 15
  • DOI: 10.1063/1.1506911

A contracted basis-Lanczos calculation of vibrational levels of methane: Solving the Schrödinger equation in nine dimensions
journal, July 2003

  • Wang, Xiao-Gang; Carrington, Tucker
  • The Journal of Chemical Physics, Vol. 119, Issue 1
  • DOI: 10.1063/1.1574016

A general rigorous quantum dynamics algorithm to calculate vibrational energy levels of pentaatomic molecules
journal, August 2009


On the variational computation of a large number of vibrational energy levels and wave functions for medium-sized molecules
journal, August 2009

  • Mátyus, Edit; Šimunek, Ján; Császár, Attila G.
  • The Journal of Chemical Physics, Vol. 131, Issue 7
  • DOI: 10.1063/1.3187528

Rotational and vibrational energy levels of methane calculated from a new potential energy surface
journal, January 2011


Computing rovibrational levels of methane with curvilinear internal vibrational coordinates and an Eckart frame
journal, March 2013

  • Wang, Xiao-Gang; Carrington, Tucker
  • The Journal of Chemical Physics, Vol. 138, Issue 10
  • DOI: 10.1063/1.4793474

High resolution spectroscopy and the first global analysis of the Tetradecad region of methane 12CH4
journal, January 2013

  • Nikitin, A. V.; Boudon, V.; Wenger, Ch.
  • Physical Chemistry Chemical Physics, Vol. 15, Issue 25
  • DOI: 10.1039/c3cp50799h

Vibrational transition moments of CH4 from first principles
journal, September 2013

  • Yurchenko, Sergei N.; Tennyson, Jonathan; Barber, Robert J.
  • Journal of Molecular Spectroscopy, Vol. 291
  • DOI: 10.1016/j.jms.2013.05.014

Spectrum of hot methane in astronomical objects using a comprehensive computed line list
journal, June 2014

  • Yurchenko, Sergei N.; Tennyson, Jonathan; Bailey, Jeremy
  • Proceedings of the National Academy of Sciences, Vol. 111, Issue 26
  • DOI: 10.1073/pnas.1324219111

An efficient method for energy levels calculation using full symmetry and exact kinetic energy operator: Tetrahedral molecules
journal, March 2015

  • Nikitin, A. V.; Rey, M.; Tyuterev, Vl. G.
  • The Journal of Chemical Physics, Vol. 142, Issue 9
  • DOI: 10.1063/1.4913520

Vibrational energy levels of the simplest Criegee intermediate (CH 2 OO) from full-dimensional Lanczos, MCTDH, and MULTIMODE calculations
journal, August 2015

  • Yu, Hua-Gen; Ndengue, Steve; Li, Jun
  • The Journal of Chemical Physics, Vol. 143, Issue 8
  • DOI: 10.1063/1.4929707

Vibrational energy levels for CH4 from an ab initio potential
journal, March 2001

  • Schwenke, David W.; Partridge, Harry
  • Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy, Vol. 57, Issue 4
  • DOI: 10.1016/S1386-1425(00)00451-0

Nitrous oxide dimer: A new potential energy surface and rovibrational spectrum of the nonpolar isomer
journal, October 2010

  • Dawes, Richard; Wang, Xiao-Gang; Jasper, Ahren W.
  • The Journal of Chemical Physics, Vol. 133, Issue 13
  • DOI: 10.1063/1.3494542

Communication: An accurate global potential energy surface for the ground electronic state of ozone
journal, November 2013

  • Dawes, Richard; Lolur, Phalgun; Li, Anyang
  • The Journal of Chemical Physics, Vol. 139, Issue 20
  • DOI: 10.1063/1.4837175

ExoMol line lists – IV. The rotation–vibration spectrum of methane up to 1500 K
journal, March 2014

  • Yurchenko, Sergei N.; Tennyson, Jonathan
  • Monthly Notices of the Royal Astronomical Society, Vol. 440, Issue 2
  • DOI: 10.1093/mnras/stu326

High-Level, First-Principles, Full-Dimensional Quantum Calculation of the Ro-vibrational Spectrum of the Simplest Criegee Intermediate (CH 2 OO)
journal, June 2014

  • Li, Jun; Carter, Stuart; Bowman, Joel M.
  • The Journal of Physical Chemistry Letters, Vol. 5, Issue 13
  • DOI: 10.1021/jz501059m

Toward spectroscopically accurate global ab initio potential energy surface for the acetylene-vinylidene isomerization
journal, December 2014

  • Han, Huixian; Li, Anyang; Guo, Hua
  • The Journal of Chemical Physics, Vol. 141, Issue 24
  • DOI: 10.1063/1.4904859

Near Spectroscopically Accurate Ab Initio Potential Energy Surface for NH 4 + and Variational Calculations of Low-Lying Vibrational Levels
journal, March 2015

  • Han, Huixian; Song, Hongwei; Li, Jun
  • The Journal of Physical Chemistry A, Vol. 119, Issue 14
  • DOI: 10.1021/acs.jpca.5b01835

Nitrogen hydrides and the H 2 ortho-to-para ratio in dark clouds
journal, December 2011


Neutral and ion chemistry in low pressure dc plasmas of H2/N2 mixtures: routes for the efficient production of NH3 and NH4+
journal, January 2011

  • Carrasco, Esther; Jiménez-Redondo, Miguel; Tanarro, Isabel
  • Physical Chemistry Chemical Physics, Vol. 13, Issue 43
  • DOI: 10.1039/c1cp22284h

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
  • DOI: 10.1063/1.446147

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
  • DOI: 10.1063/1.446148

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
  • DOI: 10.1063/1.447279

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
  • DOI: 10.1139/p86-240

Velocity modulation infrared laser spectroscopy of molecular ions: The
journal, April 1989


The ν4Band of Ammonium, NH+4
journal, September 1996

  • Park, Joonbum; Xia, Changhong; Selby, Stan
  • Journal of Molecular Spectroscopy, Vol. 179, Issue 1
  • DOI: 10.1006/jmsp.1996.0193

Predicting the Proton Affinities of H 2 O and NH 3
journal, April 1998

  • Peterson, Kirk A.; Xantheas, Sotiris S.; Dixon, David A.
  • The Journal of Physical Chemistry A, Vol. 102, Issue 14
  • DOI: 10.1021/jp971510r

The equilibrium N–H bond length
journal, October 2000


Breaking a tetrahedral molecular ion with electrons: study of NH + 4
journal, February 2012

  • Douguet, N.; Kokoouline, V.; Orel, A. E.
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 45, Issue 5
  • DOI: 10.1088/0953-4075/45/5/051001

Accurate ab initio quartic force field and vibrational frequencies of the NH4+ ion and its deuterated forms
journal, August 1996


Permutation invariant polynomial neural network approach to fitting potential energy surfaces
journal, August 2013

  • Jiang, Bin; Guo, Hua
  • The Journal of Chemical Physics, Vol. 139, Issue 5
  • DOI: 10.1063/1.4817187

Permutation invariant polynomial neural network approach to fitting potential energy surfaces. II. Four-atom systems
journal, November 2013

  • Li, Jun; Jiang, Bin; Guo, Hua
  • The Journal of Chemical Physics, Vol. 139, Issue 20
  • DOI: 10.1063/1.4832697

Sur une transformation des équations différentielles de la dynamique
journal, January 1868

  • Radau, R.
  • Annales scientifiques de l'École normale supérieure, Vol. 5
  • DOI: 10.24033/asens.48

Modified Heliocentric Coordinates for Particle Dynamics
journal, October 1980


Quantum approaches to polyatomic reaction dynamics
journal, March 2013


Potential optimized discrete variable representation
journal, March 1992


The discrete variable representation of a triatomic Hamiltonian in bond length–bond angle coordinates
journal, September 1992

  • Wei, Hua; Carrington, Tucker
  • The Journal of Chemical Physics, Vol. 97, Issue 5
  • DOI: 10.1063/1.463044

A four dimensional quantum scattering study of the Cl+CH4⇌HCl+CH3 reaction via spectral transform iteration
journal, April 1999

  • Yu, Hua-Gen; Nyman, Gunnar
  • The Journal of Chemical Physics, Vol. 110, Issue 15
  • DOI: 10.1063/1.478627

An iteration method for the solution of the eigenvalue problem of linear differential and integral operators
journal, October 1950

  • Lanczos, C.
  • Journal of Research of the National Bureau of Standards, Vol. 45, Issue 4
  • DOI: 10.6028/jres.045.026

Global analysis of the high resolution infrared spectrum of methane 12CH4 in the region from 0 to 4800cm−1
journal, February 2009


Using experimental data and a contracted basis Lanczos method to determine an accurate methane potential energy surface from a least squares optimization
journal, October 2014

  • Wang, Xiao-Gang; Carrington, Tucker
  • The Journal of Chemical Physics, Vol. 141, Issue 15
  • DOI: 10.1063/1.4896569

High-Resolution Near Infrared Spectroscopy and Vibrational Dynamics of Dideuteromethane (CH 2 D 2 )
journal, March 2009

  • Ulenikov, O. N.; Bekhtereva, E. S.; Albert, S.
  • The Journal of Physical Chemistry A, Vol. 113, Issue 10
  • DOI: 10.1021/jp809839t

High resolution infrared spectroscopy and global vibrational analysis for the CH 3 D and CHD 3 isotopomers of methane
journal, April 2010


Accurate quantum dynamics calculations of vibrational spectrum of dideuteromethane CH2D2
journal, May 2015

  • Yu, Hua-Gen
  • The Journal of Chemical Physics, Vol. 142, Issue 19
  • DOI: 10.1063/1.4921411

    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
    • DOI: 10.1063/1.5113962

    Potential energy surfaces from high fidelity fitting of ab initio points: the permutation invariant polynomial - neural network approach
    journal, July 2016


    Sub-Doppler slit jet infrared spectroscopy of astrochemically relevant cations: The NH stretching mode in ND 3 H +
    journal, October 2018

    • Chang, Chih-Hsuan; Scrape, Preston G.; Nesbitt, David J.
    • The Journal of Chemical Physics, Vol. 149, Issue 14
    • DOI: 10.1063/1.5049603