Imaging a multidimensional multichannel potential energy surface: Photodetachment of H–(NH3) and NH4–

Hu, Qichi; Song, Hongwei; Johnson, Christopher J.; Li, Jun; Guo, Hua; Continetti, Robert E.

doi:10.1063/1.4954187

Title: Imaging a multidimensional multichannel potential energy surface: Photodetachment of H^–(NH₃) and NH₄^–

Abstract

Probes of the Born-Oppenheimer potential energy surfaces governing polyatomic molecules often rely on spectroscopy for the bound regions or collision experiments in the continuum. A combined spectroscopic and half-collision approach to image nuclear dynamics in a multidimensional and multichannel system is reported here. The Rydberg radical NH₄ and the double Rydberg anion NH₄^– represent a polyatomic system for benchmarking electronic structure and nine-dimensional quantum dynamics calculations. Photodetachment of the H^–(NH₃) ion-dipole complex and the NH₄^– DRA probes different regions on the neutral NH₄ PES. Photoelectron energy and angular distributions at photon energies of 1.17, 1.60, and 2.33 eV compare well with quantum dynamics. Photoelectron-photofragment coincidence experiments indicate dissociation of the nascent NH₄ In conclusion, Rydberg radical occurs to H + NH₃ with a peak kinetic energy of 0.13 eV, showing the ground state of NH₄ to be unstable, decaying by tunneling-induced dissociation on a time scale beyond the present scope of multidimensional quantum dynamics.

Authors:

Hu, Qichi ^[1]; Song, Hongwei ^[2]; Johnson, Christopher J. ^[3]; Li, Jun ^[4]; Guo, Hua ^[5];

^[6]

Univ. of California San Diego, La Jolla, CA (United States); Anasys Instruments Corp., Santa Barbara, CA (United States)
Univ. of New Mexico, Albuquerque, NM (United States); Chinese Academy of Sciences, Wuhan (China)
Univ. of California San Diego, La Jolla, CA (United States); Stony Brook Univ., Stony Brook, NY (United States)
Chongqing Univ., Chongqing (China)
Univ. of New Mexico, Albuquerque, NM (United States)
Univ. of California San Diego, La Jolla, CA (United States)

Publication Date:: Tue Jun 28 00:00:00 EDT 2016

Research Org.:: Univ. of California, San Diego, CA (United States)

Sponsoring Org.:: USDOE

OSTI Identifier:: 1467571

Alternate Identifier(s):: OSTI ID: 1259738

Grant/Contract Number:: FG02-05ER15694

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Chemical Physics

Additional Journal Information:: Journal Volume: 144; Journal Issue: 24; 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

Citation Formats


                    Hu, Qichi, Song, Hongwei, Johnson, Christopher J., Li, Jun, Guo, Hua, and Continetti, Robert E. Imaging a multidimensional multichannel potential energy surface: Photodetachment of H–(NH3) and NH4–.  United States: N. p., 2016. 
Web.  doi:10.1063/1.4954187.

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                    Hu, Qichi, Song, Hongwei, Johnson, Christopher J., Li, Jun, Guo, Hua, & Continetti, Robert E. Imaging a multidimensional multichannel potential energy surface: Photodetachment of H–(NH3) and NH4–.  United States.  https://doi.org/10.1063/1.4954187

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                    Hu, Qichi, Song, Hongwei, Johnson, Christopher J., Li, Jun, Guo, Hua, and Continetti, Robert E. Tue .  
"Imaging a multidimensional multichannel potential energy surface: Photodetachment of H–(NH3) and NH4–".  United States.  https://doi.org/10.1063/1.4954187.  https://www.osti.gov/servlets/purl/1467571.

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@article{osti_1467571,

  title        = {Imaging a multidimensional multichannel potential energy surface: Photodetachment of H–(NH3) and NH4–},

  author       = {Hu, Qichi and Song, Hongwei and Johnson, Christopher J. and Li, Jun and Guo, Hua and Continetti, Robert E.},

  abstractNote = {Probes of the Born-Oppenheimer potential energy surfaces governing polyatomic molecules often rely on spectroscopy for the bound regions or collision experiments in the continuum. A combined spectroscopic and half-collision approach to image nuclear dynamics in a multidimensional and multichannel system is reported here. The Rydberg radical NH4 and the double Rydberg anion NH4– represent a polyatomic system for benchmarking electronic structure and nine-dimensional quantum dynamics calculations. Photodetachment of the H–(NH3) ion-dipole complex and the NH4– DRA probes different regions on the neutral NH4 PES. Photoelectron energy and angular distributions at photon energies of 1.17, 1.60, and 2.33 eV compare well with quantum dynamics. Photoelectron-photofragment coincidence experiments indicate dissociation of the nascent NH4 In conclusion, Rydberg radical occurs to H + NH3 with a peak kinetic energy of 0.13 eV, showing the ground state of NH4 to be unstable, decaying by tunneling-induced dissociation on a time scale beyond the present scope of multidimensional quantum dynamics.},

  doi          = {10.1063/1.4954187},

  journal      = {Journal of Chemical Physics},

  number       = 24,

  volume       = 144,

  place        = {United States},

  year         = {Tue Jun 28 00:00:00 EDT 2016},

  month        = {Tue Jun 28 00:00:00 EDT 2016}

}

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Works referencing / citing this record:

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Title: Imaging a multidimensional multichannel potential energy surface: Photodetachment of H–(NH3) and NH4–

Abstract

Citation Formats

Cross Sections for Electron Collisions with Nitrogen Molecules journal, March 2006

Vertical and adiabatic ionization energies of NH − 4 isomers via electron propagator theory and many body perturbation theory calculations with large basis sets journal, September 1987

Double‐Rydberg anions: Ground‐state electronic and geometric stabilities journal, September 1990

Solvation effects on angular distributions in H − (NH 3 ) n and NH 2 − (NH 3 ) n photodetachment: Role of solute electronic structure journal, October 2011

Photodetachment spectroscopy of cluster anions. Photoelectron spectroscopy of H – (NH 3 ) 1 , H – (NH 3 ) 2 and the tetrahedral isomer of NH–4 journal, January 1988

Photoelectron–multiple-photofragment coincidence spectrometer journal, May 1999

Stability of the ammonium and methylammonium radicals from neutralized ion‐beam spectroscopy journal, October 1982

Angular Distribution of Photoelectrons journal, January 1968

Negative ion photoelectron spectroscopy of the negative cluster ion H − (NH 3 ) 1 journal, September 1985

Spectra of the ammonium radical: the schüler bands journal, June 1984

ARPACK Users' Guide book, January 1998

A simple and efficient CCSD(T)-F12 approximation journal, December 2007

ND 4 Schüler band absorption observed by laser FM spectroscopy in a photochemical reaction journal, January 1984

The absorption spectrum of NH 2 between 6250 and 9500 Å journal, September 1976

Slow photoelectron velocity-map imaging spectroscopy of cold negative ions journal, December 2012

Structure of the ammonium radical from a rotationally resolved photoelectron spectrum journal, April 1997

Nine-dimensional quantum dynamics study of the H 2 + NH 2 → H + NH 3 reaction: a rigorous test of the sudden vector projection model journal, January 2014

Full-dimensional quantum calculations of the vibrational states of H5+ journal, March 2013

On the H − migration in the ion journal, December 1984

Interpolated potential energy surface for abstraction and exchange reactions of NH3 + H and deuterated analogues journal, March 2005

Structures and properties of double-Rydberg anions journal, June 1990

Stability of the Ground and Low-Lying Vibrational States of the Ammonium Radical journal, October 2013

"Dougle-Rydberg" molecular anions journal, November 1988

Full dimensional time-dependent quantum dynamics study of the H+NH3→H2+NH2 reaction journal, August 2008

Double Rydberg anions: Photoelectron spectroscopy of NH4−, N2H7−, N3H10−, N4H13−, and N5H16− journal, September 2002

A time-independent theory of photodissociation based on polynomial propagation journal, February 1998

Theoretical prediction of the structure and infrared spectrum of the molecule–ion complexes NH 3 –H − , NH 3 –D − , and ND 3 –H − journal, September 1995

A double Rydberg anion with a hydrogen bond and a solvated double Rydberg anion: Interpretation of the photoelectron spectrum of N2H7− journal, September 2002

Threshold photodetachment of H − journal, June 1991

Absorption spectrum and analysis of the ND4 Schüler band journal, September 1984

Dynamics on the HOCO potential energy surface studied by dissociative photodetachment of HOCO− and DOCO− journal, May 2007

Simplified CCSD(T)-F12 methods: Theory and benchmarks journal, February 2009

Dynamics of dissociative electron attachment to ammonia journal, May 2016

Photoelectron-photofragment coincidence studies of dissociation dynamics journal, April 1998

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

Analytical potential energy surface for the NH 3 +H↔NH 2 +H 2 reaction: Application of variational transition-state theory and analysis of the equilibrium constants and kinetic isotope effects using curvilinear and rectilinear coordinates journal, March 1997

A nine-dimensional global potential energy surface for NH 4 (X 2 A 1 ) and kinetics studies on the H + NH 3 ↔ H 2 + NH 2 reaction journal, January 2014

Transition state spectroscopy of the OH + H2 .fwdarw. H2O + H reaction via photodetachment of H3O- and D3O- journal, September 1995

Dissociative recombination of NH4+ and ND4+ ions: Storage ring experiments and ab initio molecular dynamics journal, April 2004

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

Effects of reactant rotational excitations on H2 + NH2 → H + NH3 reactivity journal, December 2014

Imaging Dynamics on the F + H2O -> HF + OH Potential Energy Surfaces from Wells to Barriers journal, January 2014

Double-Rydberg molecular anions journal, July 1991

Delay line anodes for microchannel‐plate spectrometers journal, December 1987

Rydberg spectra of triatomic hydrogen and of the ammonium radical journal, January 1981

Formation of the NH4- ion in the gas phase journal, April 1983

Velocity map imaging of ions and electrons using electrostatic lenses: Application in photoelectron and photofragment ion imaging of molecular oxygen journal, September 1997

Observation of the ND4 Sch�ler band in a neutralized ion beam experiment journal, December 1988

OH3− and O2H5− double Rydberg anions: Predictions and comparisons with NH4− and N2H7− journal, July 2007

Spectroscopy and dynamics of the HOCO radical: insights into the OH + CO → H + CO 2 reaction journal, January 2014

An Ab initio study of the tetrahedral NH4− ion journal, November 1986

A Theoretical Study of NH4- and PH4- journal, August 1995

Communication: New insight into the barrier governing CO2 formation from OH + CO journal, May 2011

OH3- and O2H5- double Rydberg anions: Predictions and comparisons with NH4- and N2H7- text, January 2021

Photoelectron-photofragment coincidence studies of I 3 − using an electrospray ionization source and a linear accelerator journal, January 2019

Double Rydberg anions with solvated ammonium kernels: Electron binding energies and Dyson orbitals journal, August 2019

Title: Imaging a multidimensional multichannel potential energy surface: Photodetachment of H^–(NH₃) and NH₄^–

Cross Sections for Electron Collisions with Nitrogen Molecules
journal, March 2006

Vertical and adiabatic ionization energies of NH ⁻ ₄ isomers via electron propagator theory and many body perturbation theory calculations with large basis sets
journal, September 1987

Double‐Rydberg anions: Ground‐state electronic and geometric stabilities
journal, September 1990

Solvation effects on angular distributions in H ⁻ (NH ₃ ) _n and NH ₂ ⁻ (NH ₃ ) _n photodetachment: Role of solute electronic structure
journal, October 2011

Photodetachment spectroscopy of cluster anions. Photoelectron spectroscopy of H ^– (NH ₃ ) ₁ , H ^– (NH ₃ ) ₂ and the tetrahedral isomer of NH–4
journal, January 1988

Photoelectron–multiple-photofragment coincidence spectrometer
journal, May 1999

Stability of the ammonium and methylammonium radicals from neutralized ion‐beam spectroscopy
journal, October 1982

Angular Distribution of Photoelectrons
journal, January 1968

Negative ion photoelectron spectroscopy of the negative cluster ion H ⁻ (NH ₃ ) ₁
journal, September 1985

Spectra of the ammonium radical: the schüler bands
journal, June 1984

ARPACK Users' Guide
book, January 1998

A simple and efficient CCSD(T)-F12 approximation
journal, December 2007

ND ₄ Schüler band absorption observed by laser FM spectroscopy in a photochemical reaction
journal, January 1984

The absorption spectrum of NH ₂ between 6250 and 9500 Å
journal, September 1976

Slow photoelectron velocity-map imaging spectroscopy of cold negative ions
journal, December 2012

Structure of the ammonium radical from a rotationally resolved photoelectron spectrum
journal, April 1997

Nine-dimensional quantum dynamics study of the H ₂ + NH ₂ → H + NH ₃ reaction: a rigorous test of the sudden vector projection model
journal, January 2014

Full-dimensional quantum calculations of the vibrational states of H5+
journal, March 2013

On the H ⁻ migration in the ion
journal, December 1984

Interpolated potential energy surface for abstraction and exchange reactions of NH3 + H and deuterated analogues
journal, March 2005

Structures and properties of double-Rydberg anions
journal, June 1990

Stability of the Ground and Low-Lying Vibrational States of the Ammonium Radical
journal, October 2013

"Dougle-Rydberg" molecular anions
journal, November 1988

Full dimensional time-dependent quantum dynamics study of the H+NH3→H2+NH2 reaction
journal, August 2008

Double Rydberg anions: Photoelectron spectroscopy of NH4−, N2H7−, N3H10−, N4H13−, and N5H16−
journal, September 2002

A time-independent theory of photodissociation based on polynomial propagation
journal, February 1998

Theoretical prediction of the structure and infrared spectrum of the molecule–ion complexes NH ₃ –H ⁻ , NH ₃ –D ⁻ , and ND ₃ –H ⁻
journal, September 1995

A double Rydberg anion with a hydrogen bond and a solvated double Rydberg anion: Interpretation of the photoelectron spectrum of N2H7−
journal, September 2002

Threshold photodetachment of $H^{-}$
journal, June 1991

Absorption spectrum and analysis of the ND4 Schüler band
journal, September 1984

Dynamics on the HOCO potential energy surface studied by dissociative photodetachment of HOCO− and DOCO−
journal, May 2007

Simplified CCSD(T)-F12 methods: Theory and benchmarks
journal, February 2009

Dynamics of dissociative electron attachment to ammonia
journal, May 2016

Photoelectron-photofragment coincidence studies of dissociation dynamics
journal, April 1998

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

Analytical potential energy surface for the NH ₃ +H↔NH ₂ +H ₂ reaction: Application of variational transition-state theory and analysis of the equilibrium constants and kinetic isotope effects using curvilinear and rectilinear coordinates
journal, March 1997

A nine-dimensional global potential energy surface for NH ₄ (X ² A ₁ ) and kinetics studies on the H + NH ₃ ↔ H ₂ + NH ₂ reaction
journal, January 2014

Transition state spectroscopy of the OH + H2 .fwdarw. H2O + H reaction via photodetachment of H3O- and D3O-
journal, September 1995

Dissociative recombination of NH4+ and ND4+ ions: Storage ring experiments and ab initio molecular dynamics
journal, April 2004

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

Effects of reactant rotational excitations on H2 + NH2 → H + NH3 reactivity
journal, December 2014

Imaging Dynamics on the F + H2O -> HF + OH Potential Energy Surfaces from Wells to Barriers
journal, January 2014

Double-Rydberg molecular anions
journal, July 1991

Delay line anodes for microchannel‐plate spectrometers
journal, December 1987

Rydberg spectra of triatomic hydrogen and of the ammonium radical
journal, January 1981

Formation of the NH4- ion in the gas phase
journal, April 1983

Velocity map imaging of ions and electrons using electrostatic lenses: Application in photoelectron and photofragment ion imaging of molecular oxygen
journal, September 1997

Observation of the ND4 Sch�ler band in a neutralized ion beam experiment
journal, December 1988

OH3− and O2H5− double Rydberg anions: Predictions and comparisons with NH4− and N2H7−
journal, July 2007

Spectroscopy and dynamics of the HOCO radical: insights into the OH + CO → H + CO ₂ reaction
journal, January 2014

An Ab initio study of the tetrahedral NH4− ion
journal, November 1986

A Theoretical Study of NH4- and PH4-
journal, August 1995

Communication: New insight into the barrier governing CO2 formation from OH + CO
journal, May 2011

OH3- and O2H5- double Rydberg anions: Predictions and comparisons with NH4- and N2H7-
text, January 2021

Photoelectron-photofragment coincidence studies of I ₃ ⁻ using an electrospray ionization source and a linear accelerator
journal, January 2019

Double Rydberg anions with solvated ammonium kernels: Electron binding energies and Dyson orbitals
journal, August 2019