Skip to main content

Lund University Publications

LUND UNIVERSITY LIBRARIES

Fission of charged nano-hydrated ammonia clusters-microscopic insights into the nucleation processes

Oostenrijk, Bart LU ; Barreiro, Darío ; Walsh, Noelle LU ; Sankari, Anna LU ; Månsson, Erik P. LU ; Maclot, Sylvain LU ; Sorensen, Stacey L. LU ; Díaz-Tendero, Sergio and Gisselbrecht, Mathieu LU orcid (2019) In Physical Chemistry Chemical Physics 21(46). p.25749-25762
Abstract

While largely studied on the macroscopic scale, the dynamics leading to nucleation and fission processes in atmospheric aerosols are still poorly understood at the molecular level. Here, we present a joint experimental-theoretical study of a model system consisting of hydrogen-bonded ammonia and water molecules. Experimentally, the clusters were produced via adiabatic co-expansion. Double ionization ionic products were prepared using synchrotron radiation and analyzed with coincidence mass- and 3D momentum spectroscopy. Calculations were carried out using ab initio molecular dynamics to understand the fragmentation within the first ∼500 fs. Further exploration of the potential energy surfaces was performed at a DFT level of theory to... (More)

While largely studied on the macroscopic scale, the dynamics leading to nucleation and fission processes in atmospheric aerosols are still poorly understood at the molecular level. Here, we present a joint experimental-theoretical study of a model system consisting of hydrogen-bonded ammonia and water molecules. Experimentally, the clusters were produced via adiabatic co-expansion. Double ionization ionic products were prepared using synchrotron radiation and analyzed with coincidence mass- and 3D momentum spectroscopy. Calculations were carried out using ab initio molecular dynamics to understand the fragmentation within the first ∼500 fs. Further exploration of the potential energy surfaces was performed at a DFT level of theory to gain information on the energetics of the processes. Water was identified as an efficient nano-droplet stabilizer, and is found to have a significant effect even at low water content. On the molecular level, the stabilizing role of water can be related to an increase in the dissociation energy between ammonia molecules and the water enriched environment at the cluster surface. Furthermore, our results support the role of ammonium as a charge carrier in the solution, preferentially bound to surrounding ammonia molecules, which can influence the atmospheric nucleation process.

(Less)
Please use this url to cite or link to this publication:
author
; ; ; ; ; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Physical Chemistry Chemical Physics
volume
21
issue
46
pages
14 pages
publisher
Royal Society of Chemistry
external identifiers
  • scopus:85075813588
  • pmid:31720608
ISSN
1463-9076
DOI
10.1039/c9cp04221k
language
English
LU publication?
yes
id
c0890fd8-9636-4bfe-83e5-e5950af4969c
alternative location
https://arxiv.org/abs/2106.11201v1
date added to LUP
2019-12-16 13:00:05
date last changed
2024-02-16 06:43:14
@article{c0890fd8-9636-4bfe-83e5-e5950af4969c,
  abstract     = {{<p>While largely studied on the macroscopic scale, the dynamics leading to nucleation and fission processes in atmospheric aerosols are still poorly understood at the molecular level. Here, we present a joint experimental-theoretical study of a model system consisting of hydrogen-bonded ammonia and water molecules. Experimentally, the clusters were produced via adiabatic co-expansion. Double ionization ionic products were prepared using synchrotron radiation and analyzed with coincidence mass- and 3D momentum spectroscopy. Calculations were carried out using ab initio molecular dynamics to understand the fragmentation within the first ∼500 fs. Further exploration of the potential energy surfaces was performed at a DFT level of theory to gain information on the energetics of the processes. Water was identified as an efficient nano-droplet stabilizer, and is found to have a significant effect even at low water content. On the molecular level, the stabilizing role of water can be related to an increase in the dissociation energy between ammonia molecules and the water enriched environment at the cluster surface. Furthermore, our results support the role of ammonium as a charge carrier in the solution, preferentially bound to surrounding ammonia molecules, which can influence the atmospheric nucleation process.</p>}},
  author       = {{Oostenrijk, Bart and Barreiro, Darío and Walsh, Noelle and Sankari, Anna and Månsson, Erik P. and Maclot, Sylvain and Sorensen, Stacey L. and Díaz-Tendero, Sergio and Gisselbrecht, Mathieu}},
  issn         = {{1463-9076}},
  language     = {{eng}},
  month        = {{12}},
  number       = {{46}},
  pages        = {{25749--25762}},
  publisher    = {{Royal Society of Chemistry}},
  series       = {{Physical Chemistry Chemical Physics}},
  title        = {{Fission of charged nano-hydrated ammonia clusters-microscopic insights into the nucleation processes}},
  url          = {{http://dx.doi.org/10.1039/c9cp04221k}},
  doi          = {{10.1039/c9cp04221k}},
  volume       = {{21}},
  year         = {{2019}},
}