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@ARTICLE{Carlsson:889800,
author = {Carlsson, Philip and Celik, Steven and Becker, Daniel and
Olenius, Tinja and Elm, Jonas and Zeuch, Thomas},
title = {{N}eutral {S}ulfuric {A}cid–{W}ater {C}lustering {R}ates:
{B}ridging the {G}ap between {M}olecular {S}imulation and
{E}xperiment},
journal = {The journal of physical chemistry letters},
volume = {11},
number = {10},
issn = {1948-7185},
address = {Washington, DC},
publisher = {ACS},
reportid = {FZJ-2021-00413},
pages = {4239 - 4244},
year = {2020},
abstract = {The role of sulfuric acid during atmospheric new particle
formation is an ongoing topic of discussion. In this work,
we provide quantitative experimental constraints for quantum
chemically calculated evaporation rates for the smallest
H2SO4–H2O clusters, characterizing the mechanism governing
nucleation on a kinetic, single-molecule level. We compare
experimental particle size distributions resulting from a
highly supersaturated homogeneous H2SO4 gas phase with the
results from kinetic simulations employing quantum
chemically derived decomposition rates of electrically
neutral H2SO4 molecular clusters up to the pentamer at a
large range of relative humidities. By using high H2SO4
concentrations, we circumvent the uncertainties concerning
contaminants and competing reactions present in studies at
atmospheric conditions. We show good agreement between
molecular simulation and experimental measurements and
provide the first evaluation of theoretical predictions of
the stabilization provided by water molecules.},
cin = {IEK-8},
ddc = {530},
cid = {I:(DE-Juel1)IEK-8-20101013},
pnm = {243 - Tropospheric trace substances and their
transformation processes (POF3-243)},
pid = {G:(DE-HGF)POF3-243},
typ = {PUB:(DE-HGF)16},
pubmed = {32357300},
UT = {WOS:000537432500069},
doi = {10.1021/acs.jpclett.0c01045},
url = {https://juser.fz-juelich.de/record/889800},
}