Fission of charged nano-hydrated ammonia clusters-microscopic insights into the nucleation processes
(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.
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- author
- 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
- organization
- publishing date
- 2019-12-14
- 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}}, }