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@ARTICLE{Schtze:841709,
author = {Schütze, Katharina and Wilson, James Charles and
Weinbruch, Stephan and Benker, Nathalie and Ebert, Martin
and Günther, Gebhard and Weigel, Ralf and Borrmann,
Stephan},
title = {{S}ub-micrometer refractory carbonaceous particles in the
polar stratosphere},
journal = {Atmospheric chemistry and physics},
volume = {17},
number = {20},
issn = {1680-7324},
address = {Katlenburg-Lindau},
publisher = {EGU},
reportid = {FZJ-2018-00017},
pages = {12475 - 12493},
year = {2017},
abstract = {Eleven particle samples collected in the polar stratosphere
during SOLVE (SAGE III Ozone loss and validation experiment)
from January until March 2000 were characterized in detail
by high-resolution transmission and scanning electron
microscopy (TEM/SEM) combined with energy-dispersive X-ray
microanalysis. A total of 4202 particles
(TEM = 3872; SEM = 330) were analyzed
from these samples, which were collected mostly inside the
polar vortex in the altitude range between 17.3 and
19.9 km. Particles that were volatile in the microscope
beams contained ammonium sulfates and hydrogen sulfates and
dominated the samples. Some particles with diameters ranging
from 20 to 830 nm were refractory in the electron beams.
Carbonaceous particles containing additional elements to C
and O comprised from 72 to $100 \%$ of the refractory
particles. The rest were internal mixtures of these
materials with sulfates. The median number mixing ratio of
the refractory particles, expressed in units of particles
per milligram of air, was 1.1 (mg air)−1 and varied
between 0.65 and 2.3 (mg air)−1.Most of the refractory
carbonaceous particles are completely amorphous, a few of
the particles are partly ordered with a graphene sheet
separation distance of 0.37 ± 0.06 nm (mean
value ± standard deviation). Carbon and oxygen are the
only detected major elements with an atomic O∕C ratio of
0.11 ± 0.07. Minor elements observed include Si, S, Fe,
Cr and Ni with the following atomic ratios relative to C:
Si∕C: 0.010 ± 0.011; S∕C: 0.0007 ± 0.0015;
Fe∕C: 0.0052 ± 0.0074; Cr∕C: 0.0012 ± 0.0017;
Ni∕C: 0.0006 ± 0.0011 (all mean
values ± standard deviation).High-resolution element
distribution images reveal that the minor elements are
distributed within the carbonaceous matrix; i.e.,
heterogeneous inclusions are not observed. No difference in
size, nanostructure and elemental composition was found
between particles collected inside and outside the polar
vortex.Based on chemistry and nanostructure, aircraft
exhaust, volcanic emissions and biomass burning can
certainly be excluded as sources. The same is true for the
less probable but globally important sources: wood burning,
coal burning, diesel engines and ship emissions.Recondensed
organic matter and extraterrestrial particles, potentially
originating from ablation and fragmentation, remain as
possible sources of the refractory carbonaceous particles
studied. However, additional work is required in order to
identify the sources unequivocally.},
cin = {IEK-7},
ddc = {550},
cid = {I:(DE-Juel1)IEK-7-20101013},
pnm = {244 - Composition and dynamics of the upper troposphere and
middle atmosphere (POF3-244)},
pid = {G:(DE-HGF)POF3-244},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000413242700002},
doi = {10.5194/acp-17-12475-2017},
url = {https://juser.fz-juelich.de/record/841709},
}