Charge delocalization dynamics of ammonia in different hydrogen bonding environments: free clusters and in liquid water solution
(2009) In Physical Chemistry Chemical Physics 11(11). p.1758-1764- Abstract
- Valence and core level photoelectron spectra and Auger electron spectra of ammonia in pure clusters have been measured. The Auger electron spectra of gas-phase ammonia, pure ammonia clusters and ammonia in aqueous solution are compared and interpreted via ab initio calculations of the Auger spectrum of the ammonia monomer and dimer. The calculations reveal that the final two-hole valence states can be delocalized over both ammonia molecules. Features at energies pertaining to delocalized states involving one, or more, hydrogen bonding orbitals can be found in both the ammonia cluster Auger electron spectrum and in that of the liquid solvated molecule. The lower Coulombic repulsion between two delocalized valence final state holes gives... (More)
- Valence and core level photoelectron spectra and Auger electron spectra of ammonia in pure clusters have been measured. The Auger electron spectra of gas-phase ammonia, pure ammonia clusters and ammonia in aqueous solution are compared and interpreted via ab initio calculations of the Auger spectrum of the ammonia monomer and dimer. The calculations reveal that the final two-hole valence states can be delocalized over both ammonia molecules. Features at energies pertaining to delocalized states involving one, or more, hydrogen bonding orbitals can be found in both the ammonia cluster Auger electron spectrum and in that of the liquid solvated molecule. The lower Coulombic repulsion between two delocalized valence final state holes gives higher kinetic energy of the Auger electrons which is also observed in the spectra. This decay path-specific to the condensed phase-is responsible for more than 5% of the total cluster Auger intensity. Moreover, this interpretation is also applicable to the solid phase since the same features have been observed, but not assigned, in the Auger spectrum of solid ammonia. (Less)
Please use this url to cite or link to this publication:
https://lup.lub.lu.se/record/1370938
- author
- Lindblad, A. ; Bergersen, H. ; Pokapanich, W. ; Tchaplyguine, Maxim LU ; Ohrwall, G. and Bjorneholm, O.
- organization
- publishing date
- 2009
- type
- Contribution to journal
- publication status
- published
- subject
- in
- Physical Chemistry Chemical Physics
- volume
- 11
- issue
- 11
- pages
- 1758 - 1764
- publisher
- Royal Society of Chemistry
- external identifiers
-
- wos:000263838200012
- scopus:61649127608
- pmid:19290347
- ISSN
- 1463-9084
- DOI
- 10.1039/b815657c
- language
- English
- LU publication?
- yes
- id
- dc827b4c-8e67-4234-b6f3-388c0b41e4ce (old id 1370938)
- date added to LUP
- 2016-04-01 13:55:43
- date last changed
- 2022-03-21 21:21:14
@article{dc827b4c-8e67-4234-b6f3-388c0b41e4ce,
abstract = {{Valence and core level photoelectron spectra and Auger electron spectra of ammonia in pure clusters have been measured. The Auger electron spectra of gas-phase ammonia, pure ammonia clusters and ammonia in aqueous solution are compared and interpreted via ab initio calculations of the Auger spectrum of the ammonia monomer and dimer. The calculations reveal that the final two-hole valence states can be delocalized over both ammonia molecules. Features at energies pertaining to delocalized states involving one, or more, hydrogen bonding orbitals can be found in both the ammonia cluster Auger electron spectrum and in that of the liquid solvated molecule. The lower Coulombic repulsion between two delocalized valence final state holes gives higher kinetic energy of the Auger electrons which is also observed in the spectra. This decay path-specific to the condensed phase-is responsible for more than 5% of the total cluster Auger intensity. Moreover, this interpretation is also applicable to the solid phase since the same features have been observed, but not assigned, in the Auger spectrum of solid ammonia.}},
author = {{Lindblad, A. and Bergersen, H. and Pokapanich, W. and Tchaplyguine, Maxim and Ohrwall, G. and Bjorneholm, O.}},
issn = {{1463-9084}},
language = {{eng}},
number = {{11}},
pages = {{1758--1764}},
publisher = {{Royal Society of Chemistry}},
series = {{Physical Chemistry Chemical Physics}},
title = {{Charge delocalization dynamics of ammonia in different hydrogen bonding environments: free clusters and in liquid water solution}},
url = {{http://dx.doi.org/10.1039/b815657c}},
doi = {{10.1039/b815657c}},
volume = {{11}},
year = {{2009}},
}