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@ARTICLE{Woiwode:820664,
author = {Woiwode, Wolfgang and Höpfner, Michael and Bi, Lei and
Pitts, Michael C. and Poole, Lamont R. and Oelhaf, Hermann
and Molleker, Sergej and Borrmann, Stephan and Klingebiel,
Marcus and Belyaev, Gennady and Ebersoldt, Andreas and
Griessbach, Sabine and Grooß, Jens-Uwe and Gulde, Thomas
and Krämer, Martina and Maucher, Guido and Piesch, Christof
and Rolf, Christian and Sartorius, Christian and Spang,
Reinhold and Orphal, Johannes},
title = {{S}pectroscopic evidence of large aspherical β-{NAT}
particles involved in denitrification in the {D}ecember 2011
{A}rctic stratosphere},
journal = {Atmospheric chemistry and physics},
volume = {16},
number = {14},
issn = {1680-7324},
address = {Katlenburg-Lindau},
publisher = {EGU},
reportid = {FZJ-2016-05933},
pages = {9505 - 9532},
year = {2016},
abstract = {We analyze polar stratospheric cloud (PSC) signatures in
airborne MIPAS-STR (Michelson Interferometer for Passive
Atmospheric Sounding – STRatospheric aircraft)
observations in the spectral regions from 725 to 990 and
1150 to 1350 cm−1 under conditions suitable for the
existence of nitric acid trihydrate (NAT) above northern
Scandinavia on 11 December 2011. The high-resolution
infrared limb emission spectra of MIPAS-STR show a
characteristic “shoulder-like” signature in the spectral
region around 820 cm−1, which is attributed to the ν2
symmetric deformation mode of NO3− in β-NAT. Using
radiative transfer calculations involving Mie and T-Matrix
methods, the spectral signatures of spherical and aspherical
particles are simulated. The simulations are constrained
using collocated in situ particle measurements. Simulations
assuming highly aspherical spheroids with aspect ratios (AR)
of 0.1 or 10.0 and a lognormal particle mode with a mode
radius of 4.8 µm reproduce the observed spectra to a high
degree. A smaller lognormal mode with a mode radius of
2.0 µm, which is also taken into account, plays only a
minor role. Within the scenarios analyzed, the best overall
agreement is found for elongated spheroids with
AR = 0.1. Simulations of spherical particles and
spheroids with AR = 0.5 and 2.0 return results
very similar to each other and do not allow us to reproduce
the signature around 820 cm−1. The observed
“shoulder-like” signature is explained by the
combination of the absorption/emission and scattering
characteristics of large highly aspherical β-NAT particles.
The size distribution supported by our results corresponds
to ∼ 9 ppbv of gas-phase equivalent HNO3 at the flight
altitude of ∼ 18.5 km. The results are compared with
the size distributions derived from the in situ
observations, a corresponding Chemical Lagrangian Model of
the Stratosphere (CLaMS) simulation, and excess gas-phase
HNO3 observed in a nitrification layer directly below the
observed PSC. The presented results suggest that large
highly aspherical β-NAT particles involved in
denitrification of the polar stratosphere can be identified
by means of passive infrared limb emission measurements.},
cin = {IEK-7 / JSC},
ddc = {550},
cid = {I:(DE-Juel1)IEK-7-20101013 / I:(DE-Juel1)JSC-20090406},
pnm = {244 - Composition and dynamics of the upper troposphere and
middle atmosphere (POF3-244) / 511 - Computational Science
and Mathematical Methods (POF3-511)},
pid = {G:(DE-HGF)POF3-244 / G:(DE-HGF)POF3-511},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000381213300040},
doi = {10.5194/acp-16-9505-2016},
url = {https://juser.fz-juelich.de/record/820664},
}