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@ARTICLE{Kaur:626043,
author = {Kaur, Harmanjot and Thuermer, Stephan and Gholami, Shirin
and Credidio, Bruno and Trinter, Florian and Vasconcelos,
Debora and Marinho, Ricardo and Pinheiro, Joel and Bluhm,
Hendrik and Naves de Brito, Arnaldo and Oehrwall, Gunnar and
Winter, Bernd and Bjoerneholm, Olle},
title = {{B}oosting aerosol surface effects: strongly enhanced
cooperative surface propensity of atmospherically relevant
organic molecular ions in aqueous solution},
journal = {Atmospheric chemistry and physics},
volume = {25},
number = {6},
issn = {1680-7316},
address = {Katlenburg-Lindau},
publisher = {EGU},
reportid = {PUBDB-2025-01267},
pages = {3503 - 3518},
year = {2025},
note = {Open Access},
abstract = {The effects of atmospheric aerosols are key uncertainties
in climate models. One reason is the complex aerosol
composition which includes a relatively large fraction of
organics. Another reason is the small size of aerosols,
which makes surface effects and processes important. These
two factors make surface-active organics relevant for
atmospheric aerosols, as they can affect crucial processes,
such as chemical aging and water accommodation, as well as
properties such as the surface tension, which drives droplet
formation. Two exemplary types of atmospherically relevant
organics are carboxylic acids and alkyl amines, and often
both are found together within aerosols. In the most
atmospherically significant pH range, these exist as
alkyl-carboxylate ions and alkyl-ammonium ions. Using
liquid-jet photoelectron spectroscopy, tuned to high surface
sensitivity, we measured the alkyl-carboxylate anions and
the alkyl-ammonium cations of alkyl chain lengths of 1 to 6
carbon atoms, both as single-component and mixed-component
aqueous solutions. This enabled us to systematically study
how their surface propensity is affected by the length of
the alkyl chains and how cooperative ion–ion interactions
result in strongly increased surface propensity. An
exponential increase in surface propensity is found for the
single-species solutions, with cooperative solute–solute
effects in mixed solutions of 1 : 1 molar ratio
drastically increasing the number of molecules present at
the solutions' surfaces up to a factor of several hundred.
This cooperative surface propensity is shown to strongly
affect the amounts of organics at the surface. These changes
can significantly influence radiative forcing via aerosol
growth, cloud condensation nuclei activity, and aerosol
chemical aging. Our results demonstrate the principal
feasibility of a more advanced input of molecular details
for creating parameterized descriptions of aerosol surface
composition needed to properly account for their impacts in
climate models.},
cin = {DOOR ; HAS-User},
ddc = {550},
cid = {I:(DE-H253)HAS-User-20120731},
pnm = {6G3 - PETRA III (DESY) (POF4-6G3) / FS-Proposal: I-20220937
EC (I-20220937-EC) / AQUACHIRAL - Chiral aqueous-phase
chemistry (883759) / DFG project G:(GEPRIS)509471550 -
Dynamik photoionisations-induzierter Prozesse in
laser-präparierten Molekülen in der Gasphase und der
wässrigen Phase (509471550) / SWEDEN-DESY - SWEDEN-DESY
Collaboration $(2020_Join2-SWEDEN-DESY)$},
pid = {G:(DE-HGF)POF4-6G3 / G:(DE-H253)I-20220937-EC /
G:(EU-Grant)883759 / G:(GEPRIS)509471550 /
$G:(DE-HGF)2020_Join2-SWEDEN-DESY$},
experiment = {EXP:(DE-H253)P-P04-20150101},
typ = {PUB:(DE-HGF)16},
UT = {WOS:001451152800001},
doi = {10.5194/acp-25-3503-2025},
url = {https://bib-pubdb1.desy.de/record/626043},
}