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

Title: Mechanisms and dynamics of the NH+2 + H+ and NH+ + H+ + H fragmentation channels upon single-photon double ionization of NH3

Journal Article · · Journal of Physics. B, Atomic, Molecular and Optical Physics
ORCiD logo [1];  [2];  [3];  [2];  [4];  [5];  [1];  [6];  [7]; ORCiD logo [6];  [8];  [8];  [9];  [10];  [7];  [8];  [3]; ORCiD logo [2];  [6]; ORCiD logo [2] more »; ORCiD logo [2] « less
  1. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Davis, CA (United States)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Max Planck Inst. fur Kernphysik, Heidelberg (Germany); J.W. Goethe Univ., Frankfurt (Germany)
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Auburn Univ., AL (United States)
  6. Kansas State Univ., Manhattan, KS (United States)
  7. Auburn Univ., AL (United States)
  8. Univ. of Nevada, Reno, NV (United States)
  9. Max Planck Inst. fur Kernphysik, Heidelberg (Germany)
  10. J.W. Goethe Univ., Frankfurt (Germany)

We present state-selective measurements on the NH$$_2^{+}$$ + H$$^{+}$$ and NH$$^{+}$$ + H$$^{+}$$ + H dissociation channels following single-photon double ionization at 61.5 eV of neutral NH$$_{3}$$, where the two photoelectrons and two cations are measured in coincidence using 3-D momentum imaging. Three dication electronic states are identified to contribute to the NH$$_2^{+}$$ + H$$^{+}$$ dissociation channel, where the excitation in one of the three states undergoes intersystem crossing prior to dissociation, producing a cold NH$$_2^+$$ fragment. In contrast, the other two states directly dissociate, producing a ro-vibrationally excited NH$$_2^+$$ fragment with roughly 1 eV of internal energy. The NH$$^{+}$$ + H$$^{+}$$ + H channel is fed by direct dissociation from three intermediate dication states, one of which is shared with the NH$$_2^{+}$$ + H$$^{+}$$ channel. We find evidence of autoionization contributing to each of the double ionization channels. Finally, the distributions of the relative emission angle between the two photoelectrons, as well as the relative angle between the recoil axis of the molecular breakup and the polarization vector of the ionizing field, are also presented to provide insight on the ionization mechanisms for the different dication states.

Research Organization:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Kansas State Univ., Manhattan, KS (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; National Science Foundation (NSF)
Grant/Contract Number:
AC02-05CH11231; FG02-86ER13491; PHY-1807017
OSTI ID:
1658358
Alternate ID(s):
OSTI ID: 1840508
Journal Information:
Journal of Physics. B, Atomic, Molecular and Optical Physics, Vol. 53, Issue 24; ISSN 0953-4075
Publisher:
IOP PublishingCopyright Statement
Country of Publication:
United States
Language:
English

References (25)

Molecular-frame photoelectron and electron-frame photoion angular distributions and their interrelation journal January 2007
The Simplest Double Slit: Interference and Entanglement in Double Photoionization of H2 journal November 2007
Complete photo-fragmentation of the deuterium molecule journal September 2004
Diabolical conical intersections journal October 1996
Photofragment Alignment and Orientation journal October 1982
Calculated Auger emission spectrum of ammonia journal June 1976
The double ionization of ammonia. Its dissociation into the doubly ionized fragment N2+ journal July 1987
Double photoionisation spectra of methane, ammonia and water journal April 2006
Photofragment angular momentum distributions in the molecular frame: Determination and interpretation journal February 1999
Absorption and dissociative photoionization cross sections of NH 3 from 80 to 1120 Å journal December 1987
On the doubly ionized states of ammonia journal July 1985
Ionization of ammonia and deuterated ammonia by electron impact from threshold up to 180 eV journal October 1977
Electron-impact excitation of the b 3 Σ u + state of H 2 using the complex Kohn method: R dependence of the cross section journal November 1988
Electronic states of doubly ionized ammonia journal May 1974
Photo-double-ionization of ethylene and acetylene near threshold journal January 2014
Delayed predissociation and collision-induced processes of the ammonia di-cation NH32+ journal December 1985
Recoil-ion and electron momentum spectroscopy: reaction-microscopes journal August 2003
An experimental determination of the energy of the first triplet doubly-ionized state of ammonia journal October 1990
The measured auger electron spectrum of ammonia vapour journal September 1977
Absolute triple differential cross sections for photo-double ionization of helium - experiment and theory journal December 1998
Photoelectron and fragmentation dynamics of the H + + H + dissociative channel in NH 3 following direct single-photon double ionization journal October 2020
Photo double ionization of helium 100 eV and 450 eV above threshold: III. Gerade and ungerade amplitudes and their relative phases journal March 2005
About the double ionization of ammonia and carbon dioxide. A comparison between photoionization and electron impact journal November 1989
The double photoionisation of NH 3 using the triple coincidence (PEPIPICO) technique journal January 1989
The dissociative electroionization of ammonia and ammonia-d3. I. The NH+ and NH2+ dissociation channels journal July 1988