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@ARTICLE{Evoy:866828,
author = {Evoy, Erin and Maclean, Adrian M. and Rovelli, Grazia and
Li, Ying and Tsimpidi, Alexandra P. and Karydis, Vlassis A.
and Kamal, Saeid and Lelieveld, Jos and Shiraiwa, Manabu and
Reid, Jonathan P. and Bertram, Allan K.},
title = {{P}redictions of diffusion rates of large organic molecules
in secondary organic aerosols using the
{S}tokes–{E}instein and fractional {S}tokes–{E}instein
relations},
journal = {Atmospheric chemistry and physics},
volume = {19},
number = {15},
issn = {1680-7324},
address = {Katlenburg-Lindau},
publisher = {EGU},
reportid = {FZJ-2019-05891},
pages = {10073 - 10085},
year = {2019},
abstract = {Information on the rate of diffusion of organic molecules
within secondary organic aerosol (SOA) is needed to
accurately predict the effects of SOA on climate and air
quality. Diffusion can be important for predicting the
growth, evaporation, and reaction rates of SOA under certain
atmospheric conditions. Often, researchers have predicted
diffusion rates of organic molecules within SOA using
measurements of viscosity and the Stokes–Einstein relation
(D∝1/η, where D is the diffusion coefficient and η is
viscosity). However, the accuracy of this relation for
predicting diffusion in SOA remains uncertain. Using
rectangular area fluorescence recovery after photobleaching
(rFRAP), we determined diffusion coefficients of fluorescent
organic molecules over 8 orders in magnitude in proxies of
SOA including citric acid, sorbitol, and a sucrose–citric
acid mixture. These results were combined with literature
data to evaluate the Stokes–Einstein relation for
predicting the diffusion of organic molecules in SOA.
Although almost all the data agree with the
Stokes–Einstein relation within a factor of 10, a
fractional Stokes–Einstein relation (D∝1/ηξ) with
ξ=0.93 is a better model for predicting the diffusion of
organic molecules in the SOA proxies studied. In addition,
based on the output from a chemical transport model, the
Stokes–Einstein relation can overpredict mixing times of
organic molecules within SOA by as much as 1 order of
magnitude at an altitude of ∼3 km compared to the
fractional Stokes–Einstein relation with ξ=0.93. These
results also have implications for other areas such as in
food sciences and the preservation of biomolecules.},
cin = {IEK-8},
ddc = {550},
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},
UT = {WOS:000480315800006},
doi = {10.5194/acp-19-10073-2019},
url = {https://juser.fz-juelich.de/record/866828},
}