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Title: Imaging a multidimensional multichannel potential energy surface: Photodetachment of H (NH 3) and NH 4

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 NH 4 and the double Rydberg anion NH 4 represent a polyatomic system for benchmarking electronic structure and nine-dimensional quantum dynamics calculations. Photodetachment of the H (NH 3) ion-dipole complex and the NH 4 DRA probes different regions on the neutral NH 4 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 NH 4 In conclusion, Rydberg radical occurs to H + NH 3 with a peak kinetic energy of 0.13 eV, showing the ground state of NH 4 to be unstable, decaying by tunneling-induced dissociation on a time scale beyond the present scope of multidimensional quantum dynamics.
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [5] ; ORCiD logo [6]
  1. Univ. of California San Diego, La Jolla, CA (United States); Anasys Instruments Corp., Santa Barbara, CA (United States)
  2. Univ. of New Mexico, Albuquerque, NM (United States); Chinese Academy of Sciences, Wuhan (China)
  3. Univ. of California San Diego, La Jolla, CA (United States); Stony Brook Univ., Stony Brook, NY (United States)
  4. Chongqing Univ., Chongqing (China)
  5. Univ. of New Mexico, Albuquerque, NM (United States)
  6. Univ. of California San Diego, La Jolla, CA (United States)
Publication Date:
Grant/Contract Number:
FG02-05ER15694
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)
Research Org:
Univ. of California, San Diego, CA (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1467571
Alternate Identifier(s):
OSTI ID: 1259738

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., Web. doi:10.1063/1.4954187.
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. doi:10.1063/1.4954187.
Hu, Qichi, Song, Hongwei, Johnson, Christopher J., Li, Jun, Guo, Hua, and Continetti, Robert E.. 2016. "Imaging a multidimensional multichannel potential energy surface: Photodetachment of H–(NH3) and NH4–". United States. doi:10.1063/1.4954187. https://www.osti.gov/servlets/purl/1467571.
@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 = {2016},
month = {6}
}