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@ARTICLE{Schneider:901822,
author = {Schneider, Julia and Höhler, Kristina and Wagner, Robert
and Saathoff, Harald and Schnaiter, Martin and Schorr,
Tobias and Steinke, Isabelle and Benz, Stefan and
Baumgartner, Manuel and Rolf, Christian and Krämer, Martina
and Leisner, Thomas and Möhler, Ottmar},
title = {{H}igh homogeneous freezing onsets of sulfuric acid aerosol
at cirrus temperatures},
journal = {Atmospheric chemistry and physics},
volume = {21},
number = {18},
issn = {1680-7324},
address = {Katlenburg-Lindau},
publisher = {EGU},
reportid = {FZJ-2021-03845},
pages = {14403 - 14425},
year = {2021},
abstract = {Homogeneous freezing of aqueous solution aerosol particles
is an important process for cloud ice formation in the upper
troposphere. There the air temperature is low, the ice
supersaturation can be high and the concentration of
ice-nucleating particles is too low to initiate and dominate
cirrus cloud formation by heterogeneous ice nucleation
processes. The most common description to quantify
homogeneous freezing processes is based on the water
activity criterion (WAC) as proposed by Koop et al. (2000).
The WAC describes the homogeneous nucleation rate
coefficients only as a function of the water activity, which
makes this approach well applicable in numerical models. In
this study, we investigate the homogeneous freezing behavior
of aqueous sulfuric acid aerosol particles by means of a
comprehensive collection of laboratory-based homogeneous
freezing experiments conducted at the AIDA (Aerosol
Interaction and Dynamics in the Atmosphere) cloud simulation
chamber, which were conducted as part of 17 measurement
campaigns since 2007. The most recent experiments were
conducted during October 2020 with special emphasis on
temperatures below 200 K. Aqueous sulfuric acid aerosol
particles of high purity were generated by particle
nucleation in a gas flow composed of clean synthetic air and
sulfuric acid vapor, which was added to the AIDA chamber.
The resulting chamber aerosol had number concentrations from
30 cm−3 up to several thousand per cubic centimeter with
particle diameters ranging from about 30 nm to 1.1 µm.
Homogeneous freezing of the aerosol particles was measured
at simulated cirrus formation conditions in a wide range of
temperatures between 185 and 230 K with a steady increase
of relative humidity during each experiment. At temperatures
between about 205 K and about 230 K, the AIDA results
agree well with the WAC-based predictions of homogeneous
freezing onsets. At lower temperatures, however, the AIDA
results show an increasing deviation from the WAC-based
predictions towards higher freezing onsets. For temperatures
between 185 and 205 K, the WAC-based ice saturation ratios
for homogeneous freezing onsets increase from about 1.6 to
1.7, whereas the AIDA measurements show an increase from
about 1.7 to 2.0 in the same temperature range. Based on the
experimental results of our direct measurements, we suggest
a new fit line to formulate the onset conditions of
homogeneous freezing of sulfuric acid aerosol particles as
an isoline for nucleation rate coefficients between 5×108
and 1013 cm−3 s−1. The potential significant impacts
of the higher homogeneous freezing thresholds, as directly
observed in the AIDA experiments under simulated cirrus
formation conditions, on the model prediction of cirrus
cloud occurrence and related cloud radiative effects are
discussed.},
cin = {IEK-7},
ddc = {550},
cid = {I:(DE-Juel1)IEK-7-20101013},
pnm = {2112 - Climate Feedbacks (POF4-211) / DFG project 392369854
- Erforschung tropischer Zirruswolken durch die Kombination
von Labor- und Feldexperimenten mit Prozess- und
Zirkulationsmodellen},
pid = {G:(DE-HGF)POF4-2112 / G:(GEPRIS)392369854},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000703046400001},
doi = {10.5194/acp-21-14403-2021},
url = {https://juser.fz-juelich.de/record/901822},
}