scholarly journals Nitric acid trihydrate nucleation and denitrification in the Arctic stratosphere

2014 ◽  
Vol 14 (2) ◽  
pp. 1055-1073 ◽  
Author(s):  
J.-U. Grooß ◽  
I. Engel ◽  
S. Borrmann ◽  
W. Frey ◽  
G. Günther ◽  
...  
Keyword(s):  
Nitric Acid ◽  
Nucleation Rate ◽  
Regional Scale ◽  
Lagrangian Model ◽  
The Arctic ◽  
Orthogonal Polarization ◽  
Rate Model ◽  
Formation Pathway ◽  
Improved Model

Abstract. Nitric acid trihydrate (NAT) particles in the polar stratosphere have been shown to be responsible for vertical redistribution of reactive nitrogen (NOy). Recent observations by Cloud–Aerosol Lidar with Orthogonal Polarization (CALIOP) aboard the CALIPSO satellite have been explained in terms of heterogeneous nucleation of NAT on foreign nuclei, revealing this to be an important formation pathway for the NAT particles. In state of the art global- or regional-scale models, heterogeneous NAT nucleation is currently simulated in a very coarse manner using a constant, saturation-independent nucleation rate. Here we present first simulations for the Arctic winter 2009/2010 applying a new saturation-dependent parametrisation of heterogeneous NAT nucleation rates within the Chemical Lagrangian Model of the Stratosphere (CLaMS). The simulation shows good agreement of chemical trace species with in situ and remote sensing observations. The simulated polar stratospheric cloud (PSC) optical properties agree much better with CALIOP observations than those simulated with a constant nucleation rate model. A comparison of the simulated particle size distributions with observations made using the Forward Scattering Spectrometer Probe (FSSP) aboard the high altitude research aircraft Geophysica, shows that the model reproduces the observed size distribution, except for the very largest particles above 15 μm diameter. The vertical NOy redistribution caused by the sedimentation of the NAT particles, in particular the denitrification and nitrification signals observed by the ACE-FTS satellite instrument and the in situ SIOUX instrument aboard the Geophysica, are reproduced by the improved model, and a small improvement with respect to the constant nucleation rate model is found.

scholarly journals NAT nucleation and denitrification in the Arctic stratosphere

2013 ◽  
Vol 13 (8) ◽  
pp. 22107-22150 ◽  
Author(s):  
J.-U. Grooß ◽  
I. Engel ◽  
S. Borrmann ◽  
W. Frey ◽  
G. Günther ◽  
...  
Keyword(s):  
Regional Scale ◽  
Lagrangian Model ◽  
The Arctic ◽  
Orthogonal Polarization ◽  
Rate Model ◽  
Formation Pathway ◽  
Trace Species ◽  
Constant Rate ◽  
Research Aircraft

Abstract. Nitric acid trihydrate (NAT) particles in the polar stratosphere have been shown to be responsible for vertical redistribution of reactive nitrogen (NOy). Recent observations by Cloud–Aerosol Lidar with Orthogonal Polarization (CALIOP) aboard the CALIPSO satellite have been explained in terms of heterogeneous nucleation of NAT on foreign nuclei, revealing it to be an important formation pathway for the NAT particles. In state of the art global or regional scale models, heterogeneous NAT nucleation is currently simulated in a very coarse manner using a constant, saturation-independent nucleation rate. Here we present first simulations for the Arctic winter 2009/2010 applying a new saturation-dependent parametrisation of heterogeneous NAT nucleation rates within the Chemical Lagrangian Model of the Stratosphere (CLaMS). The simulation shows good agreement of chemical trace species with in situ and remote sensing observations. The simulated PSC optical properties agree better with CALIOP observations than those simulated with a constant rate model. A comparison of the simulated particle size distributions with observations made using the Forward Scattering Spectrometer Probe (FSSP) aboard the high altitude research aircraft Geophysica, showed that the model reproduces the observed size distribution, except for the very largest particles above 15 μm diameter. The vertical NOy redistribution caused by the sedimentation of the NAT particles, in particular the denitrification and nitrification signals observed by the ACE-FTS satellite instrument and the in-situ SIOUX instrument aboard the Geophysica, are reproduced by the model, but the improvement of the new parametrisation with respect to the constant rate model remains small.

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 Nitrification of the lowermost stratosphere during the exceptionally cold Arctic winter 2015–2016

2019 ◽  
Vol 19 (21) ◽  
pp. 13681-13699 ◽  
Author(s):  
Marleen Braun ◽  
Jens-Uwe Grooß ◽  
Wolfgang Woiwode ◽  
Sören Johansson ◽  
Michael Höpfner ◽  
...  
Keyword(s):  
Nitric Acid ◽  
Cross Sections ◽  
Large Scale ◽  
Potential Temperature ◽  
Lagrangian Model ◽  
The Arctic ◽  
Small Scale ◽  
Mixing Ratios ◽  
Fine Structures ◽  
The Impact

Abstract. The Arctic winter 2015–2016 was characterized by exceptionally low stratospheric temperatures, favouring the formation of polar stratospheric clouds (PSCs) from mid-December until the end of February down to low stratospheric altitudes. Observations by GLORIA (Gimballed Limb Observer for Radiance Imaging of the Atmosphere) on HALO (High Altitude and LOng range research aircraft) during the PGS (POLSTRACC–GW-LCYCLE II–SALSA) campaign from December 2015 to March 2016 allow the investigation of the influence of denitrification on the lowermost stratosphere (LMS) with a high spatial resolution. Two-dimensional vertical cross sections of nitric acid (HNO3) along the flight track and tracer–tracer correlations derived from the GLORIA observations document detailed pictures of wide-spread nitrification of the Arctic LMS during the course of an entire winter. GLORIA observations show large-scale structures and local fine structures with enhanced absolute HNO3 volume mixing ratios reaching up to 11 ppbv at altitudes of 13 km in January and nitrified filaments persisting until the middle of March. Narrow coherent structures tilted with altitude of enhanced HNO3, observed in mid-January, are interpreted as regions recently nitrified by sublimating HNO3-containing particles. Overall, extensive nitrification of the LMS between 5.0 and 7.0 ppbv at potential temperature levels between 350 and 380 K is estimated. The GLORIA observations are compared with CLaMS (Chemical Lagrangian Model of the Stratosphere) simulations. The fundamental structures observed by GLORIA are well reproduced, but differences in the fine structures are diagnosed. Further, CLaMS predominantly underestimates the spatial extent of HNO3 maxima derived from the GLORIA observations as well as the overall nitrification of the LMS. Sensitivity simulations with CLaMS including (i) enhanced sedimentation rates in case of ice supersaturation (to resemble ice nucleation on nitric acid trihydrate (NAT)), (ii) a global temperature offset, (iii) modified growth rates (to resemble aspherical particles with larger surfaces) and (iv) temperature fluctuations (to resemble the impact of small-scale mountain waves) slightly improved the agreement with the GLORIA observations of individual flights. However, no parameter could be isolated which resulted in a general improvement for all flights. Still, the sensitivity simulations suggest that details of particle microphysics play a significant role for simulated LMS nitrification in January, while air subsidence, transport and mixing become increasingly important for the simulated HNO3 distributions towards the end of the winter.

scholarly journals Denitrification by large NAT particles: the impact of reduced settling velocities and hints on particle characteristics

2014 ◽  
Vol 14 (20) ◽  
pp. 11525-11544 ◽  
Author(s):  
W. Woiwode ◽  
J.-U. Grooß ◽  
H. Oelhaf ◽  
S. Molleker ◽  
S. Borrmann ◽  
...  
Keyword(s):  
Stratospheric Ozone ◽  
Spherical Particles ◽  
Lagrangian Model ◽  
The Arctic ◽  
Reference Scenario ◽  
Climate Interactions ◽  
Stratospheric Clouds ◽  
The Impact ◽  
Good Agreement

Abstract. Vertical redistribution of HNO3 through large HNO3-containing particles associated with polar stratospheric clouds (PSCs) plays an important role in the chemistry of the Arctic winter stratosphere. During the RECONCILE (Reconciliation of essential process parameters for an enhanced predictability of Arctic stratospheric ozone loss and its climate interactions) campaign, apparently very large NAT (nitric acid trihydrate) particles were observed by the airborne in situ probe FSSP-100 (Molleker et al., 2014). Our analysis shows that the FSSP-100 observations associated with the flight on 25 January 2010 cannot easily be explained assuming compact spherical NAT particles due to much too short growing time at temperatures below the existence temperature of NAT (TNAT). State-of-the-art simulations using CLaMS (Chemical Lagrangian Model of the Stratosphere; Grooß et al., 2014) suggest considerably smaller particles. We consider the hypothesis that the simulation reproduces the NAT particle masses in a realistic way, but that real NAT particles may have larger apparent sizes compared to compact spherical particles, e.g. due to non-compact morphology or aspheric shape. Our study focuses on the consequence that such particles would have reduced settling velocities compared to compact spheres, altering the vertical redistribution of HNO3. Utilising CLaMS simulations, we investigate the impact of reduced settling velocities of NAT particles on vertical HNO3 redistribution and compare the results with observations of gas-phase HNO3 by the airborne Fourier transform spectrometer MIPAS-STR associated with two RECONCILE flights. The MIPAS-STR observations confirm conditions consistent with denitrification by NAT particles for the flight on 25 January 2010 and show good agreement with the simulations within the limitations of the comparison. Best agreement is found if settling velocities between 100 and 50% relative to compact spherical particles are considered (slight preference for the 70% scenario). In contrast, relative settling velocities of 30% result in too weak vertical HNO3 redistribution. Sensitivity simulations considering temperature biases of ±1 K and multiplying the simulated nucleation rates by factors of 0.5 and 2.0 affect the comparisons to a similar extent, but result in no effective improvement compared to the reference scenario. Our results show that an accurate knowledge of the settling velocities of NAT particles is important for quantitative simulations of vertical HNO3 redistribution.

scholarly journals Microphysical properties of synoptic-scale polar stratospheric clouds: in situ measurements of unexpectedly large HNO<sub>3</sub>-containing particles in the Arctic vortex

2014 ◽  
Vol 14 (19) ◽  
pp. 10785-10801 ◽  
Author(s):  
S. Molleker ◽  
S. Borrmann ◽  
H. Schlager ◽  
B. Luo ◽  
W. Frey ◽  
...  
Keyword(s):  
Nitric Acid ◽  
Scattered Light ◽  
Stratospheric Ozone ◽  
The Arctic ◽  
Size Distributions ◽  
Synoptic Scale ◽  
Cloud Particle ◽  
Regular Feature ◽  
Particle Composition

Abstract. In January 2010 and December 2011, synoptic-scale polar stratospheric cloud (PSC) fields were probed during seven flights of the high-altitude research aircraft M-55 Geophysica within the RECONCILE (Reconciliation of essential process parameters for an enhanced predictability of Arctic stratospheric ozone loss and its climate interaction) and the ESSenCe (ESSenCe: ESA Sounder Campaign) projects. Particle size distributions in a diameter range between 0.46 and 40μm were recorded by four different optical in situ instruments. Three of these particle instruments are based on the detection of forward-scattered light by single particles. The fourth instrument is a grayscale optical array imaging probe. Optical particle diameters of up to 35μm were detected with particle number densities and total particle volumes exceeding previous Arctic measurements. Also, gas-phase and particle-bound NOy was measured, as well as water vapor concentrations. The optical characteristics of the clouds were measured by the remote sensing lidar MAL (Miniature Aerosol Lidar) and by the in situ backscatter sonde MAS (Multiwavelength Aerosol Scatterometer), showing the synoptic scale of the encountered PSCs. The particle mode below 2μm in size diameter has been identified as supercooled ternary solution (STS) droplets. The PSC particles in the size range above 2μm in diameter are considered to consist of nitric acid hydrates, and the particles' high HNO3 content was confirmed by the NOy instrument. Assuming a particle composition of nitric acid trihydrate (NAT), the optically measured size distributions result in particle-phase HNO3 mixing ratios exceeding available stratospheric values. Therefore the measurement uncertainties concerning probable overestimations of measured particle sizes and volumes are discussed in detail. We hypothesize that either a strong asphericity or an alternate particle composition (e.g., water ice coated with NAT) could explain our observations. In particular, with respect to the denitrification by sedimentation of large HNO3-containing particles, generally considered to be NAT, our new measurements raise questions concerning composition, shape and nucleation pathways. Answering these would improve the numerical simulation of PSC microphysical processes like cloud particle formation, growth and denitrification, which is necessary for better predictions of future polar ozone losses, especially under changing global climate conditions. Generally, it seems that the occurrence of large NAT particles – sometimes termed "NAT rocks" – are a regular feature of synoptic-scale PSCs in the Arctic.

scholarly journals Transport of aerosol to the Arctic: analysis of CALIOP and French aircraft data during the spring 2008 POLARCAT campaign

2014 ◽  
Vol 14 (16) ◽  
pp. 8235-8254 ◽  
Author(s):  
G. Ancellet ◽  
J. Pelon ◽  
Y. Blanchard ◽  
B. Quennehen ◽  
A. Bazureau ◽  
...  
Keyword(s):  
Calibration Procedure ◽  
Airborne Lidar ◽  
The Arctic ◽  
Orthogonal Polarization ◽  
Transport Pathways ◽  
Airborne Measurements ◽  
Surface Measurements ◽  
Regional Analyses ◽  
532 Nm

Abstract. Lidar and in situ observations performed during the Polar Study using Aircraft, Remote Sensing, Surface Measurements and Models, Climate, Chemistry, Aerosols and Transport (POLARCAT) campaign are reported here in terms of statistics to characterize aerosol properties over northern Europe using daily airborne measurements conducted between Svalbard and Scandinavia from 30 March to 11 April 2008. It is shown that during this period a rather large number of aerosol layers was observed in the troposphere, with a backscatter ratio at 532 nm of 1.2 (1.5 below 2 km, 1.2 between 5 and 7 km and a minimum in between). Their sources were identified using multispectral backscatter and depolarization airborne lidar measurements after careful calibration analysis. Transport analysis and comparisons between in situ and airborne lidar observations are also provided to assess the quality of this identification. Comparison with level 1 backscatter observations of the spaceborne Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) were carried out to adjust CALIOP multispectral observations to airborne observations on a statistical basis. Recalibration for CALIOP daytime 1064 nm signals leads to a decrease of their values by about 30%, possibly related to the use of the version 3.0 calibration procedure. No recalibration is made at 532 nm even though 532 nm scattering ratios appear to be biased low (−8%) because there are also significant differences in air mass sampling between airborne and CALIOP observations. Recalibration of the 1064 nm signal or correction of −5% negative bias in the 532 nm signal both could improve the CALIOP aerosol colour ratio expected for this campaign. The first hypothesis was retained in this work. Regional analyses in the European Arctic performed as a test emphasize the potential of the CALIOP spaceborne lidar for further monitoring in-depth properties of the aerosol layers over Arctic using infrared and depolarization observations. The CALIOP April 2008 global distribution of the aerosol backscatter reveal two regions with large backscatter below 2 km: the northern Atlantic between Greenland and Norway, and northern Siberia. The aerosol colour ratio increases between the source regions and the observations at latitudes above 70° N are consistent with a growth of the aerosol size once transported to the Arctic. The distribution of the aerosol optical properties in the mid-troposphere supports the known main transport pathways between the mid-latitudes and the Arctic.

scholarly journals Homogeneous nucleation of NAD and NAT in liquid stratospheric aerosols: insufficient to explain denitrification

2002 ◽  
Vol 2 (3) ◽  
pp. 669-687 ◽  
Author(s):  
D. A. Knopf ◽  
T. Koop ◽  
B. P. Luo ◽  
U. G. Weers ◽  
T Peter
Keyword(s):  
Experimental Data ◽  
Nitric Acid ◽  
Nucleation Rate ◽  
Homogeneous Nucleation ◽  
Particle Production ◽  
Rate Coefficients ◽  
The Arctic ◽  
Linear Extrapolation ◽  
Acid Hydrate ◽  
Stratospheric Clouds

Abstract. The nucleation of NAD and NAT from HNO3/H2O and HNO3/H2O/H2SO4 solution droplets is investigated both theoretically and experimentally with respect to the formation of polar stratospheric clouds (PSCs). Our analysis shows that homogeneous NAD and NAT nucleation from liquid aerosols is insufficient to explain the number densities of large nitric acid containing particles recently observed in the Arctic stratosphere. This conclusion is based on new droplet freezing experiments employing optical microscopy combined with Raman spectroscopy. The homogeneous nucleation rate coefficients of NAD and NAT in liquid aerosols under polar stratospheric conditions derived from the experiments are < 2 x 10-5 cm-3 s-1 and < 8 x 10-2 cm-3 s-1 , respectively. These nucleation rate coefficients are smaller by orders of magnitude than the value of ~ 103 cm-3 s-1 used in a recent denitrification modelling study that is based on a linear extrapolation of laboratory nucleation data to stratospheric conditions (Tabazadeh et al., Science, 291, 2591--2594, 2001). We show that this linear extrapolation is in disagreement with thermodynamics and experimental data and, therefore, must not be used in microphysical models of PSCs. Our analysis of the experimental data yields maximum hourly production rates of nitric acid hydrate particles per cm3 of air of about 3 x 10-10 cm-3 h-1 under polar stratospheric conditions. Assuming PSC particle production to proceed at this rate for two months we arrive at particle number densities of < 5 x 10-7 cm-3, much smaller than the value of ~ 10-4 cm-3 reported in recent field observations. This clearly shows that homogeneous nucleation of NAD and NAT from liquid supercooled ternary solution aerosols cannot explain the observed polar denitrification.

scholarly journals Wildfire smoke in the lower stratosphere identified by in situ CO observations

2020 ◽  
Author(s):  
Joram J. D. Hooghiem ◽  
Maria Elena Popa ◽  
Thomas Röckmann ◽  
Jens-Uwe Grooß ◽  
Ines Tritscher ◽  
...  
Keyword(s):  
Lower Stratosphere ◽  
Atmospheric Composition ◽  
Lagrangian Model ◽  
Trace Gas ◽  
Back Trajectory ◽  
Orthogonal Polarization ◽  
Enhancement Ratio ◽  
Wildfire Smoke ◽  
British Colombia

Abstract. Wildfires emit large quantities of aerosols and trace gases, which occasionally reach the lower stratosphere. In August 2017, several pyro-cumulonimbus events injected a large amount of smoke into the stratosphere, observed by lidar and satellites. Satellite observations are in general the main method of detecting these events since in situ aircraft- or balloon-based measurements of atmospheric composition at higher altitudes are not made frequent enough. This work presents accidental balloon-borne trace gas observations of wildfire smoke in the lower stratosphere, identified by enhanced CO mole fractions at approximately 13.6 km. In addition to CO mole fractions, CO2 mole fractions as well as isotopic composition of CO (δ13C and δ18O) have been measured in air samples collected using an AirCore and a LIghtweight Stratospheric Air sampler (LISA) flown on a weather balloon from Sodankylä (4–7 September 2017, 67.37° N, 26.63° E, 179 m a.s.l.), Finland. The greenhouse gas enhancement ratio (∆CO : ∆CO2) and the isotopic signature based on δ13C(CO) and δ18O(CO) independently identify wildfire emissions as the source of the stratospheric CO enhancement. Back-trajectory analysis, performed with the Chemical Lagrangian Model of the Stratosphere (CLaMS), corrected for vertical displacement, due to heating of the wildfire aerosols, by observations made by the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) instrument, trace the smoke’s origin to wildfires in British Colombia with an injection date of 12 August 2017. Knowledge of the age of the smoke allowed for a correction of the enhancement ratio, ∆CO : ∆CO2, for the chemical removal of CO by OH. The stable isotope observations were used to estimate the amount of tropospheric air in the plume at the time of observation to be about 34 ± 14 %. The in situ observations provide information on the trace gas chemistry of smoke plumes that reach the stratosphere, as well as the vertical extent of 1 km of the 2017 smoke plume.

scholarly journals Detailed modeling of mountain wave PSCs

2003 ◽  
Vol 3 (3) ◽  
pp. 697-712 ◽  
Author(s):  
S. Fueglistaler ◽  
S. Buss ◽  
B. P. Luo ◽  
H. Wernli ◽  
H. Flentje ◽  
...  
Keyword(s):  
Remote Sensing ◽  
Nitric Acid ◽  
Weather Prediction ◽  
Detailed Comparison ◽  
Data Interpretation ◽  
Analysis Data ◽  
The Arctic ◽  
Second Phase ◽  
Mountain Wave

Abstract. Polar stratospheric clouds (PSCs) play a key role in polar ozone depletion. In the Arctic, PSCs can occur on the mesoscale due to orographically induced gravity waves. Here we present a detailed study of a mountain wave PSC event on 25-27 January 2000 over Scandinavia. The mountain wave PSCs were intensively observed by in-situ and remote-sensing techniques during the second phase of the SOLVE/THESEO-2000 Arctic campaign. We use these excellent data of PSC observations on 3 successive days to analyze the PSCs and to perform a detailed comparison with modeled clouds. We simulated the 3-dimensional PSC structure on all 3 days with a mesoscale numerical weather prediction (NWP) model and a microphysical box model (using best available nucleation rates for ice and nitric acid trihydrate particles). We show that the combined mesoscale/microphysical model is capable of reproducing the PSC measurements within the uncertainty of data interpretation with respect to spatial dimensions, temporal development and microphysical properties, without manipulating temperatures or using other tuning parameters. In contrast, microphysical modeling based upon coarser scale global NWP data, e.g. current ECMWF analysis data, cannot reproduce observations, in particular the occurrence of ice and nitric acid trihydrate clouds. Combined mesoscale/microphysical modeling may be used for detailed a posteriori PSC analysis and for future Arctic campaign flight and mission planning. The fact that remote sensing alone cannot further constrain model results due to uncertainities in the interpretation of measurements, underlines the need for synchronous in-situ PSC observations in campaigns.

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.

Sign in / Sign up

Export Citation Format

Share Document