Heterogeneous formation of polar stratospheric clouds-nucleation of nitric acid trihydrate (NAT) in the arctic stratosphere

2013 ◽  
Author(s):  
C. R. Hoyle ◽  
I. Engel ◽  
B. P. Luo ◽  
M. C. Pitts ◽  
L. R. Poole ◽  
...  
Keyword(s):  
Nitric Acid ◽  
The Arctic ◽  
Polar Stratospheric Clouds ◽  
Heterogeneous Formation ◽  
Stratospheric Clouds

scholarly journals Heterogeneous formation of polar stratospheric clouds – Part 1: Nucleation of nitric acid trihydrate (NAT)

2013 ◽  
Vol 13 (18) ◽  
pp. 9577-9595 ◽  
Author(s):  
C. R. Hoyle ◽  
I. Engel ◽  
B. P. Luo ◽  
M. C. Pitts ◽  
L. R. Poole ◽  
...  
Keyword(s):  
Nitric Acid ◽  
Companion Paper ◽  
Solid Particles ◽  
The Arctic ◽  
Orthogonal Polarization ◽  
Polar Stratospheric Clouds ◽  
Formation Pathway ◽  
Immersion Freezing ◽  
Heterogeneous Formation ◽  
Stratospheric Clouds

Abstract. Satellite-based observations during the Arctic winter of 2009/2010 provide firm evidence that, in contrast to the current understanding, the nucleation of nitric acid trihydrate (NAT) in the polar stratosphere does not only occur on preexisting ice particles. In order to explain the NAT clouds observed over the Arctic in mid-December 2009, a heterogeneous nucleation mechanism is required, occurring via immersion freezing on the surface of solid particles, likely of meteoritic origin. For the first time, a detailed microphysical modelling of this NAT formation pathway has been carried out. Heterogeneous NAT formation was calculated along more than sixty thousand trajectories, ending at Cloud Aerosol Lidar with Orthogonal Polarization (CALIOP) observation points. Comparing the optical properties of the modelled NAT with these observations enabled a thorough validation of a newly developed NAT nucleation parameterisation, which has been built into the Zurich Optical and Microphysical box Model (ZOMM). The parameterisation is based on active site theory, is simple to implement in models and provides substantial advantages over previous approaches which involved a constant rate of NAT nucleation in a given volume of air. It is shown that the new method is capable of reproducing observed polar stratospheric clouds (PSCs) very well, despite the varied conditions experienced by air parcels travelling along the different trajectories. In a companion paper, ZOMM is applied to a later period of the winter, when ice PSCs are also present, and it is shown that the observed PSCs are also represented extremely well under these conditions.

scholarly journals Nitric Acid Trihydrate (NAT) formation at low NAT supersaturation in Polar Stratospheric Clouds (PSCs)

2005 ◽  
Vol 5 (5) ◽  
pp. 1371-1380 ◽  
Author(s):  
C. Voigt ◽  
H. Schlager ◽  
B. P. Luo ◽  
A. Dörnbrack ◽  
A. Roiger ◽  
...  
Keyword(s):  
Nitric Acid ◽  
High Altitude ◽  
Equilibrium Temperature ◽  
In Situ Measurements ◽  
The Arctic ◽  
Polar Stratospheric Clouds ◽  
Research Aircraft ◽  
Stratospheric Clouds ◽  
Polar Ozone

Abstract. A PSC was detected on 6 February 2003 in the Arctic stratosphere by in-situ measurements onboard the high-altitude research aircraft Geophysica. Low number densities (~10-4cm-3) of small nitric acid (HNO3) containing particles (d<6µm) were observed at altitudes between 18 and 20km. Provided the temperatures remain below the NAT equilibrium temperature TNAT, these NAT particles have the potential to grow further and to remove HNO3 from the stratosphere, thereby enhancing polar ozone loss. Interestingly, the NAT particles formed in less than a day at temperatures just slightly below TNAT (T>TNAT-3.1K). This unique measurement of PSC formation at extremely low NAT saturation ratios (SNAT≤10) constrains current NAT nucleation theories. We suggest, that the NAT particles have formed heterogeneously, but for certain not on ice. Conversely, meteoritic particles may be favorable candidates for triggering NAT nucleation at the observed low number densities.

scholarly journals Heterogeneous formation of polar stratospheric clouds – Part 1: Nucleation of nitric acid trihydrate (NAT)

2013 ◽  
Vol 13 (3) ◽  
pp. 7979-8021 ◽  
Author(s):  
C. R. Hoyle ◽  
I. Engel ◽  
B. P. Luo ◽  
M. C. Pitts ◽  
L. R. Poole ◽  
...  
Keyword(s):  
Nitric Acid ◽  
Companion Paper ◽  
Solid Particles ◽  
The Arctic ◽  
Formation Pathway ◽  
Constant Rate ◽  
Immersion Freezing ◽  
Heterogeneous Formation ◽  
Stratospheric Clouds ◽  
First Time

Abstract. Satellite based observations during the Arctic winter of 2009/2010 provide firm evidence that, in contrast to the current understanding, the nucleation of nitric acid trihydrate (NAT) in the polar stratosphere does not only occur on preexisting ice particles. In order to explain the NAT clouds observed over the Arctic in mid December 2009, a heterogeneous nucleation mechanism is required, occurring via immersion freezing on the surface of solid particles, likely of meteoritic origin. For the first time, a detailed microphysical modelling of this NAT formation pathway has been carried out. Heterogeneous NAT formation was calculated along more than sixty thousand trajectories, ending at Cloud Aerosol Lidar with Orthogonal Polarisation (CALIOP) observation points. Comparing the optical properties of the modelled NAT with these observations enabled the thorough validation of a newly developed NAT nucleation parameterisation, which has been built into the Zurich Optical and Microphysical box Model (ZOMM). The parameterisation is based on active site theory, is simple to implement in models and provides substantial advantages over previous approaches which involved a constant rate of NAT nucleation in a given volume of air. It is shown that the new method is capable of reproducing observed PSCs very well, despite the varied conditions experienced by air parcels travelling along the different trajectories. In a companion paper, ZOMM is applied to a later period of the winter, when ice PSCs are also present, and it is shown that the observed PSCs are also represented extremely well under these conditions.

Record springtime stratospheric ozone depletion at 80°N in 2020

2021 ◽  
Author(s):  
Ramina Alwarda ◽  
Kristof Bognar ◽  
Kimberly Strong ◽  
Martyn Chipperfield ◽  
Sandip Dhomse ◽  
...  
Keyword(s):  
Ozone Depletion ◽  
Transport Model ◽  
Stratospheric Ozone ◽  
Polar Vortex ◽  
The Arctic ◽  
Optical Absorption Spectroscopy ◽  
Chemical Transport Model ◽  
Polar Stratospheric Clouds ◽  
Ozone Loss ◽  
Stratospheric Clouds

&lt;p&gt;The Arctic winter of 2019-2020 was characterized by an unusually persistent polar vortex and temperatures in the lower stratosphere that were consistently below the threshold for the formation of polar stratospheric clouds (PSCs). These conditions led to ozone loss that is comparable to the Antarctic ozone hole. Ground-based measurements from a suite of instruments at the Polar Environment Atmospheric Research Laboratory (PEARL) in Eureka, Canada (80.05&amp;#176;N, 86.42&amp;#176;W) were used to investigate chemical ozone depletion. The vortex was located above Eureka longer than in any previous year in the 20-year dataset and lidar measurements provided evidence of polar stratospheric clouds (PSCs) above Eureka. Additionally, UV-visible zenith-sky Differential Optical Absorption Spectroscopy (DOAS) measurements showed record ozone loss in the 20-year dataset, evidence of denitrification along with the slowest increase of NO&lt;sub&gt;2&lt;/sub&gt; during spring, as well as enhanced reactive halogen species (OClO and BrO). Complementary measurements of HCl and ClONO&lt;sub&gt;2&lt;/sub&gt; (chlorine reservoir species) from a Fourier transform infrared (FTIR) spectrometer showed unusually low columns that were comparable to 2011, the previous year with significant chemical ozone depletion. Record low values of HNO&lt;sub&gt;3&lt;/sub&gt; in the FTIR dataset are in accordance with the evidence of PSCs and a denitrified atmosphere. Estimates of chemical ozone loss were derived using passive ozone from the SLIMCAT offline chemical transport model to account for dynamical contributions to the stratospheric ozone budget.&lt;/p&gt;

scholarly journals Effects of polar stratospheric clouds in the Nimbus 7 LIMS Version 6 data set

2016 ◽  
Vol 9 (7) ◽  
pp. 2927-2946 ◽  
Author(s):  
Ellis Remsberg ◽  
V. Lynn Harvey
Keyword(s):  
Stratospheric Aerosol ◽  
Transport Processes ◽  
The Arctic ◽  
Additional Parameter ◽  
Polar Stratospheric Clouds ◽  
Data Set ◽  
Screening Criteria ◽  
Temperature Thresholds ◽  
Level 3 ◽  
Stratospheric Clouds

Abstract. The historic Limb Infrared Monitor of the Stratosphere (LIMS) measurements of 1978–1979 from the Nimbus 7 satellite were re-processed with Version 6 (V6) algorithms and archived in 2002. The V6 data set employs updated radiance registration methods, improved spectroscopic line parameters, and a common vertical resolution for all retrieved parameters. Retrieved profiles are spaced about every 1.6° of latitude along orbits and include the additional parameter of geopotential height. Profiles of O3 are sensitive to perturbations from emissions of polar stratospheric clouds (PSCs). This work presents results of implementing a first-order screening for effects of PSCs using simple algorithms based on vertical gradients of the O3 mixing ratio. Their occurrences are compared with the co-located, retrieved temperatures and related to the temperature thresholds needed for saturation of H2O and/or HNO3 vapor onto PSC particles. Observed daily locations where the major PSC screening criteria are satisfied are validated against PSCs observed with the Stratospheric Aerosol Monitor (SAM) II experiment also on Nimbus 7. Remnants of emissions from PSCs are characterized for O3 and HNO3 following the screening. PSCs may also impart a warm bias in the co-located LIMS temperatures, but by no more than 1–2 K at the altitudes of where effects of PSCs are a maximum in the ozone; thus, no PSC screening was applied to the V6 temperatures. Minimum temperatures vary between 187 and 194 K and often occur 1 to 2 km above where PSC effects are first identified in the ozone (most often between about 21 and 28 hPa). Those temperature–pressure values are consistent with conditions for the existence of nitric acid trihydrate (NAT) mixtures and to a lesser extent of super-cooled ternary solution (STS) droplets. A local, temporary uptake of HNO3 vapor of order 1–3 ppbv is indicated during mid-January for the 550 K surface. Seven-month time series of the distributions of LIMS O3 and HNO3 are shown based on their gridded Level 3 data following the PSC screening. Zonal coefficients of both species are essentially free of effects from PSCs on the 550 K surface, based on their average values along PV contours and in terms of equivalent latitude. Remnants of PSCs are still present in O3 on the 450 K surface during mid-January. It is judged that the LIMS Level 3 data are of good quality for analyzing the larger-scale, stratospheric chemistry and transport processes during the Arctic winter of 1978–1979.

scholarly journals Denitrification, dehydration and ozone loss during the Arctic winter 2015/2016

2017 ◽  
Author(s):  
Farahnaz Khosrawi ◽  
Oliver Kirner ◽  
Björn-Martin Sinnhuber ◽  
Sören Johansson ◽  
Michael Höpfner ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Stratospheric Ozone ◽  
Satellite Observations ◽  
The Arctic ◽  
Cold Pool ◽  
Polar Stratospheric Clouds ◽  
Airborne Measurements ◽  
Ozone Loss ◽  
Polar Stratosphere ◽  
Stratospheric Clouds

Abstract. The Arctic winter 2015/2016 was one of the coldest stratospheric winters in recent years. A stable vortex formed by early December and the early winter was exceptionally cold. Cold pool temperatures dropped below the Nitric Acid Trihydrate (NAT) existence temperature of about 195 K, thus allowing Polar Stratospheric Clouds (PSCs) to form. The low temperatures in the polar stratosphere persisted until early March allowing chlorine activation and catalytic ozone destruction. Satellite observations indicate that sedimentation of PSC particles led to denitrification as well as dehydration of stratospheric layers. Model simulations of the Arctic winter 2015/2016 nudged toward European Center for Medium-Range Weather Forecasts (ECMWF) analyses data were performed with the atmospheric chemistry–climate model ECHAM5/MESSy Atmospheric Chemistry (EMAC) for the Polar Stratosphere in a Changing Climate (POLSTRACC) campaign. POLSTRACC is a High Altitude and LOng Range Research Aircraft (HALO) mission aimed at the investigation of the structure, composition and evolution of the Arctic Upper Troposphere and Lower Stratosphere (UTLS). The chemical and physical processes involved in Arctic stratospheric ozone depletion, transport and mixing processes in the UTLS at high latitudes, polar stratospheric clouds as well as cirrus clouds are investigated. In this study an overview of the chemistry and dynamics of the Arctic winter 2015/2016 as simulated with EMAC is given. Further, chemical-dynamical processes such as denitrification, dehydration and ozone loss during the Arctic winter 2015/2016 are investigated. Comparisons to satellite observations by the Aura Microwave Limb Sounder (Aura/MLS) as well as to airborne measurements with the Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) performed on board of HALO during the POLSTRACC campaign show that the EMAC simulations are in fairly good agreement with observations. We derive a maximum polar stratospheric O3 loss of ~ 2 ppmv or 100 DU in terms of column in mid March. The stratosphere was denitrified by about 8 ppbv HNO3 and dehydrated by about 1 ppmv H2O in mid to end of February. While ozone loss was quite strong, but not as strong as in 2010/2011, denitrification and dehydration were so far the strongest observed in the Arctic stratosphere in the at least past 10 years.

scholarly journals Nucleation of nitric acid hydrates in Polar Stratospheric Clouds by meteoric material

2017 ◽  
Author(s):  
Alexander D. James ◽  
James S. A. Brooke ◽  
Thomas P. Mangan ◽  
Thomas F. Whale ◽  
John M. C. Plane ◽  
...  
Keyword(s):  
Nitric Acid ◽  
Heterogeneous Nucleation ◽  
Ozone Depletion ◽  
Mode Of Action ◽  
Polar Stratospheric Clouds ◽  
Water Ice ◽  
Meteoric Smoke ◽  
Polar Stratosphere ◽  
Stratospheric Clouds ◽  
Meteoric Material

Abstract. Heterogeneous nucleation of crystalline nitric acid hydrates in Polar Stratospheric Clouds (PSCs) enhances ozone depletion. However, the identity and mode of action of the particles responsible for nucleation remains unknown. It has been suggested that meteoric material may trigger nucleation of nitric acid trihydrate (NAT), but this has never been directly demonstrated in the laboratory. Meteoric material is present in two forms in the stratosphere, smoke which results from the ablation and re-condensation of vapours, and fragments which result from the disruption of meteoroids entering the atmosphere. Here we show that analogues of both materials have a capacity to nucleate nitric acid hydrates. In combination with estimates from a global model of the amount of meteoric smoke and fragments in the polar stratosphere we show that meteoric material probably accounts for NAT observations in early season polar stratospheric clouds in the absence of water ice.

scholarly journals A closer look at Arctic ozone loss and polar stratospheric clouds

2010 ◽  
Vol 10 (17) ◽  
pp. 8499-8510 ◽  
Author(s):  
N. R. P. Harris ◽  
R. Lehmann ◽  
M. Rex ◽  
P. von der Gathen
Keyword(s):  
Nitric Acid ◽  
Climate Models ◽  
Empirical Relationship ◽  
Early Spring ◽  
Aerosol Formation ◽  
Polar Stratospheric Clouds ◽  
Ozone Loss ◽  
Relationship Analysis ◽  
Near Ultraviolet ◽  
Stratospheric Clouds

Abstract. The empirical relationship found between column-integrated Arctic ozone loss and the potential volume of polar stratospheric clouds inferred from meteorological analyses is recalculated in a self-consistent manner using the ERA Interim reanalyses. The relationship is found to hold at different altitudes as well as in the column. The use of a PSC formation threshold based on temperature dependent cold aerosol formation makes little difference to the original, empirical relationship. Analysis of the photochemistry leading to the ozone loss shows that activation is limited by the photolysis of nitric acid. This step produces nitrogen dioxide which is converted to chlorine nitrate which in turn reacts with hydrogen chloride on any polar stratospheric clouds to form active chlorine. The rate-limiting step is the photolysis of nitric acid: this occurs at the same rate every year and so the interannual variation in the ozone loss is caused by the extent and persistence of the polar stratospheric clouds. In early spring the ozone loss rate increases as the solar insolation increases the photolysis of the chlorine monoxide dimer in the near ultraviolet. However the length of the ozone loss period is determined by the photolysis of nitric acid which also occurs in the near ultraviolet. As a result of these compensating effects, the amount of the ozone loss is principally limited by the extent of original activation rather than its timing. In addition a number of factors, including the vertical changes in pressure and total inorganic chlorine as well as denitrification and renitrification, offset each other. As a result the extent of original activation is the most important factor influencing ozone loss. These results indicate that relatively simple parameterisations of Arctic ozone loss could be developed for use in coupled chemistry climate models.

scholarly journals Chemical analysis of refractory stratospheric aerosol particles collected within the arctic vortex and inside polar stratospheric clouds

2016 ◽  
Author(s):  
Martin Ebert ◽  
Ralf Weigel ◽  
Konrad Kandler ◽  
Gebhard Günther ◽  
Sergej Molleker ◽  
...  
Keyword(s):  
Aerosol Particles ◽  
Stratospheric Aerosol ◽  
The Arctic ◽  
Late Winter ◽  
General Tendency ◽  
Polar Stratospheric Clouds ◽  
Metal Mixtures ◽  
Air Masses ◽  
Size And Morphology ◽  
Stratospheric Clouds

Abstract. Stratospheric aerosol particles with diameters larger than about 10 nm were collected within the arctic vortex during two polar flight campaigns: RECONCILE in winter 2010 and ESSenCe in winter 2011. Impactors were installed on board of the aircraft M-55 Geophysica, which was operated from Kiruna, Sweden. Flights were performed in a height of up to 21 km and some of the particle samples were taken within distinct polar stratospheric clouds (PSC). The chemical composition, size and morphology of refractory particles were analyzed by scanning electron microscopy and energy-dispersive X-ray microanalysis. During ESSenCe no refractory particles with diameters above 500 nm were sampled. In total 116 small silicate-, Fe-rich-, Pb-rich and aluminum oxide spheres were found. In contrast to ESSenCe early winter, during the late winter RECONCILE mission the air masses were subsiding inside the Arctic winter vortex from upper stratosphere and mesosphere, thus initializing a transport of refractory aerosol particles into the lower stratosphere. During RECONCILE 759 refractory particles with diameters above 500 nm were found consisting of silicates, silicate/carbon mixtures, Fe-rich particles, Ca-rich particles and complex metal mixtures. In the size range below 500 nm additionally the presence of soot was proven. While the data base is still sparse, the general tendency of a lower abundance of refractory particles during PSC events compared to non-PSC situations was observed. The detection of such large refractory particles in the stratosphere, and the fact that these particles were not observed in the particle samples (upper size limit about 5 µm) taken during PSC events, strengthen the hypothesis that such particles are present in the polar stratosphere in late winter and that they can provide a surface for heterogeneous condensation during PSC formation.

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