Spectroscopic evidence of large aspherical <i>β</i>-NAT particles involved in denitrification in the December 2011 Arctic stratosphere
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<sup>−1</sup> under conditions suitable for the exis...
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Copernicus Publications
2016-07-01
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| Series: | Atmospheric Chemistry and Physics |
| Online Access: | https://www.atmos-chem-phys.net/16/9505/2016/acp-16-9505-2016.pdf |
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| author | W. Woiwode M. Höpfner L. Bi L. Bi M. C. Pitts L. R. Poole H. Oelhaf S. Molleker S. Borrmann S. Borrmann M. Klingebiel M. Klingebiel G. Belyaev A. Ebersoldt S. Griessbach J.-U. Grooß T. Gulde M. Krämer G. Maucher C. Piesch C. Rolf C. Sartorius R. Spang J. Orphal |
| author_facet | W. Woiwode M. Höpfner L. Bi L. Bi M. C. Pitts L. R. Poole H. Oelhaf S. Molleker S. Borrmann S. Borrmann M. Klingebiel M. Klingebiel G. Belyaev A. Ebersoldt S. Griessbach J.-U. Grooß T. Gulde M. Krämer G. Maucher C. Piesch C. Rolf C. Sartorius R. Spang J. Orphal |
| author_sort | W. Woiwode |
| collection | DOAJ |
| description | 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<sup>−1</sup> 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<sup>−1</sup>, which is attributed to the <i>ν</i><sub>2</sub> symmetric deformation
mode of NO<sub>3</sub><sup>−</sup> in <i>β</i>-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<sup>−1</sup>. The
observed “shoulder-like” signature is explained by the combination of the
absorption/emission and scattering characteristics of large highly aspherical
<i>β</i>-NAT particles. The size distribution supported by our results
corresponds to ∼ 9 ppbv of gas-phase equivalent HNO<sub>3</sub> 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
HNO<sub>3</sub> observed in a nitrification layer directly below the observed PSC.
The presented results suggest that large highly aspherical <i>β</i>-NAT
particles involved in denitrification of the polar stratosphere can be
identified by means of passive infrared limb emission measurements. |
| first_indexed | 2024-12-23T11:28:01Z |
| format | Article |
| id | doaj.art-b2ed00821f27472e911d8fc68d233ce9 |
| institution | Directory Open Access Journal |
| issn | 1680-7316 1680-7324 |
| language | English |
| last_indexed | 2024-12-23T11:28:01Z |
| publishDate | 2016-07-01 |
| publisher | Copernicus Publications |
| record_format | Article |
| series | Atmospheric Chemistry and Physics |
| spelling | doaj.art-b2ed00821f27472e911d8fc68d233ce92022-12-21T17:48:53ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242016-07-01169505953210.5194/acp-16-9505-2016Spectroscopic evidence of large aspherical <i>β</i>-NAT particles involved in denitrification in the December 2011 Arctic stratosphereW. Woiwode0M. Höpfner1L. Bi2L. Bi3M. C. Pitts4L. R. Poole5H. Oelhaf6S. Molleker7S. Borrmann8S. Borrmann9M. Klingebiel10M. Klingebiel11G. Belyaev12A. Ebersoldt13S. Griessbach14J.-U. Grooß15T. Gulde16M. Krämer17G. Maucher18C. Piesch19C. Rolf20C. Sartorius21R. Spang22J. Orphal23Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, Karlsruhe, GermanyInstitute of Meteorology and Climate Research, Karlsruhe Institute of Technology, Karlsruhe, GermanyDepartment of Atmospheric Sciences, Texas A&M University, College Station, TX 77843, USAnow at: School of Earth Sciences, Zhejiang University, Hangzhou, China, 310027NASA Langley Research Center, Hampton, VA 23681, USAScience Systems and Applications, Incorporated, Hampton, VA 23666, USAInstitute of Meteorology and Climate Research, Karlsruhe Institute of Technology, Karlsruhe, GermanyParticle Chemistry Department, Max Planck Institute for Chemistry, Mainz, GermanyParticle Chemistry Department, Max Planck Institute for Chemistry, Mainz, GermanyInstitute for Physics of the Atmosphere (IPA), University of Mainz, Mainz, GermanyInstitute for Physics of the Atmosphere (IPA), University of Mainz, Mainz, Germanynow at: Atmosphere in the Earth System Department, Max Planck Institute for Meteorology, Hamburg, GermanyMyasishchev Design Bureau, Zhukovsky-5, Moscow Region, RussiaInstitute for Data Processing and Electronics, Karlsruhe Institute of Technology, Karlsruhe, GermanyJülich Supercomputing Centre (JSC), Forschungszentrum Jülich GmbH, 52425 Jülich, GermanyInstitute of Energy and Climate Research (IEK-7), Forschungszentrum Jülich GmbH, 52425 Jülich, GermanyInstitute of Meteorology and Climate Research, Karlsruhe Institute of Technology, Karlsruhe, GermanyInstitute of Energy and Climate Research (IEK-7), Forschungszentrum Jülich GmbH, 52425 Jülich, GermanyInstitute of Meteorology and Climate Research, Karlsruhe Institute of Technology, Karlsruhe, GermanyInstitute of Meteorology and Climate Research, Karlsruhe Institute of Technology, Karlsruhe, GermanyInstitute of Energy and Climate Research (IEK-7), Forschungszentrum Jülich GmbH, 52425 Jülich, GermanyInstitute of Meteorology and Climate Research, Karlsruhe Institute of Technology, Karlsruhe, GermanyInstitute of Energy and Climate Research (IEK-7), Forschungszentrum Jülich GmbH, 52425 Jülich, GermanyInstitute of Meteorology and Climate Research, Karlsruhe Institute of Technology, Karlsruhe, GermanyWe 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<sup>−1</sup> 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<sup>−1</sup>, which is attributed to the <i>ν</i><sub>2</sub> symmetric deformation mode of NO<sub>3</sub><sup>−</sup> in <i>β</i>-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<sup>−1</sup>. The observed “shoulder-like” signature is explained by the combination of the absorption/emission and scattering characteristics of large highly aspherical <i>β</i>-NAT particles. The size distribution supported by our results corresponds to ∼ 9 ppbv of gas-phase equivalent HNO<sub>3</sub> 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 HNO<sub>3</sub> observed in a nitrification layer directly below the observed PSC. The presented results suggest that large highly aspherical <i>β</i>-NAT particles involved in denitrification of the polar stratosphere can be identified by means of passive infrared limb emission measurements.https://www.atmos-chem-phys.net/16/9505/2016/acp-16-9505-2016.pdf |
| spellingShingle | W. Woiwode M. Höpfner L. Bi L. Bi M. C. Pitts L. R. Poole H. Oelhaf S. Molleker S. Borrmann S. Borrmann M. Klingebiel M. Klingebiel G. Belyaev A. Ebersoldt S. Griessbach J.-U. Grooß T. Gulde M. Krämer G. Maucher C. Piesch C. Rolf C. Sartorius R. Spang J. Orphal Spectroscopic evidence of large aspherical <i>β</i>-NAT particles involved in denitrification in the December 2011 Arctic stratosphere Atmospheric Chemistry and Physics |
| title | Spectroscopic evidence of large aspherical <i>β</i>-NAT
particles involved in denitrification in the December 2011 Arctic
stratosphere |
| title_full | Spectroscopic evidence of large aspherical <i>β</i>-NAT
particles involved in denitrification in the December 2011 Arctic
stratosphere |
| title_fullStr | Spectroscopic evidence of large aspherical <i>β</i>-NAT
particles involved in denitrification in the December 2011 Arctic
stratosphere |
| title_full_unstemmed | Spectroscopic evidence of large aspherical <i>β</i>-NAT
particles involved in denitrification in the December 2011 Arctic
stratosphere |
| title_short | Spectroscopic evidence of large aspherical <i>β</i>-NAT
particles involved in denitrification in the December 2011 Arctic
stratosphere |
| title_sort | spectroscopic evidence of large aspherical i β i nat particles involved in denitrification in the december 2011 arctic stratosphere |
| url | https://www.atmos-chem-phys.net/16/9505/2016/acp-16-9505-2016.pdf |
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