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

Oostenrijk, Bart (author)
Lund University,Lunds universitet,Synkrotronljusfysik,Fysiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Synchrotron Radiation Research,Department of Physics,Departments at LTH,Faculty of Engineering, LTH
Barreiro, Dario (author)
Univ Autonoma Madrid, Dept Quim, Modulo 13, E-28049 Madrid, Spain.,Autonomous University of Madrid
Walsh, Noelle (author)
Lund University,Lunds universitet,Fysiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Department of Physics,Departments at LTH,Faculty of Engineering, LTH
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Sankari, Anna (author)
Lund University,Lunds universitet,Synkrotronljusfysik,Fysiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Synchrotron Radiation Research,Department of Physics,Departments at LTH,Faculty of Engineering, LTH
Månsson, Erik P. (author)
DESY, Attosecond Sci Grp, Photon Sci Div, Schenefeld, Germany.,German Electron Synchrotron (DESY)
Maclot, Sylvain (author)
KTH Royal Institute of Technology,Lund University,Lunds universitet,KTH,Biomedicinsk fysik och röntgenfysik,Department of Physics, Lund University, Box 118, Lund, 22100, Sweden,Atomfysik,Fysiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Atomic Physics,Departments at LTH,Faculty of Engineering, LTH
Sorensen, Stacey L. (author)
Lund University,Lunds universitet,Synkrotronljusfysik,Fysiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Synchrotron Radiation Research,Department of Physics,Departments at LTH,Faculty of Engineering, LTH
Diaz-Tendero, Sergio (author)
Univ Autonoma Madrid, Dept Quim, Modulo 13, E-28049 Madrid, Spain.;Univ Autonoma Madrid, IFIMAC, E-28049 Madrid, Spain.;Univ Autonoma Madrid, IAdChem, E-28049 Madrid, Spain.,Autonomous University of Madrid
Gisselbrecht, Mathieu (author)
Lund University,Lunds universitet,Synkrotronljusfysik,Fysiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Synchrotron Radiation Research,Department of Physics,Departments at LTH,Faculty of Engineering, LTH
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 (creator_code:org_t)
2019
2019
English.
In: Physical Chemistry, Chemical Physics - PCCP. - : Royal Society of Chemistry. - 1463-9076 .- 1463-9084. ; 21:46, s. 25749-25762
Related links:
https://arxiv.org/ab... (free)
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http://dx.doi.org/10...
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  • Journal article (peer-reviewed)
Abstract Subject headings
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  • 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 similar to 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.

Subject headings

NATURVETENSKAP  -- Kemi (hsv//swe)
NATURAL SCIENCES  -- Chemical Sciences (hsv//eng)
NATURVETENSKAP  -- Kemi -- Fysikalisk kemi (hsv//swe)
NATURAL SCIENCES  -- Chemical Sciences -- Physical Chemistry (hsv//eng)
NATURVETENSKAP  -- Fysik -- Atom- och molekylfysik och optik (hsv//swe)
NATURAL SCIENCES  -- Physical Sciences -- Atom and Molecular Physics and Optics (hsv//eng)

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