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 ◽  
...  

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.

2013 ◽  
Vol 13 (22) ◽  
pp. 11503-11517 ◽  
Author(s):  
S. M. Khaykin ◽  
I. Engel ◽  
H. Vömel ◽  
I. M. Formanyuk ◽  
R. Kivi ◽  
...  

Abstract. We present high-resolution measurements of water vapour, aerosols and clouds in the Arctic stratosphere in January and February 2010 carried out by in situ instrumentation on balloon sondes and high-altitude aircraft combined with satellite observations. The measurements provide unparalleled evidence of dehydration and rehydration due to gravitational settling of ice particles. An extreme cooling of the Arctic stratospheric vortex during the second half of January 2010 resulted in a rare synoptic-scale outbreak of ice polar stratospheric clouds (PSCs) remotely detected by the lidar aboard the CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation) satellite. The widespread occurrence of ice clouds was followed by sedimentation and consequent sublimation of ice particles, leading to vertical redistribution of water inside the vortex. A sequence of balloon and aircraft soundings with chilled mirror and Lyman- α hygrometers (Cryogenic Frostpoint Hygrometer, CFH; Fast In Situ Stratospheric Hygrometer, FISH; Fluorescent Airborne Stratospheric Hygrometer, FLASH) and backscatter sondes (Compact Optical Backscatter Aerosol Detector, COBALD) conducted in January 2010 within the LAPBIAT (Lapland Atmosphere-Biosphere Facility) and RECONCILE (Reconciliation of Essential Process Parameters for an Enhanced Predictability of Arctic Stratospheric Ozone Loss and its Climate Interactions) campaigns captured various phases of this phenomenon: ice formation, irreversible dehydration and rehydration. Consistent observations of water vapour by these independent measurement techniques show clear signatures of irreversible dehydration of the vortex air by up to 1.6 ppmv in the 20–24 km altitude range and rehydration by up to 0.9 ppmv in a 1 km thick layer below. Comparison with space-borne Aura MLS (Microwave Limb Sounder) water vapour observations allow the spatiotemporal evolution of dehydrated air masses within the Arctic vortex to be derived and upscaled.


2005 ◽  
Vol 5 (1) ◽  
pp. 875-909
Author(s):  
B. Vogel ◽  
R. Müller ◽  
A. Engel ◽  
J.-U. Grooß ◽  
D. Toohey ◽  
...  

Abstract. Chlorine monoxide (ClO) plays a key role in stratospheric ozone loss processes at midlatitudes. We present two balloonborne in situ measurements of ClO conducted in northern hemisphere midlatitudes during the period of the maximum of total inorganic chlorine loading in the atmosphere. Both ClO measurements were conducted on board the TRIPLE balloon payload, launched in November 1996 in León, Spain, and in May 1999 in Aire sur l'Adour, France. For both flights a ClO daylight and night time vertical profile could be derived over an altitude range of approximately 15–31 km. ClO mixing ratios are compared to model simulations performed with the photochemical box model version of the Chemical Lagrangian Model of the Stratosphere (CLaMS). Simulations along 24-h backward trajectories were performed to study the diurnal variation of ClO in the midlatitude lower stratosphere. Model simulations for the flight launched in Aire sur l'Adour 1999 show a good agreement with the ClO measurements. For the flight launched in León 1996, a similar good agreement is found, except at around ≈650 K potential temperature (≈26 km altitude). However, a tendency is found that for solar zenith angles greater than 86°–87° the simulated ClO mixing ratios substantially overestimate measured ClO by approximately a factor of 2.5 or more for both flights. Therefore we conclude that no indication can be deduced from the presented ClO measurements that substantial uncertainties exist in midlatitude chlorine chemistry of the stratosphere. An exception is the situation at solar zenith angles greater than 86°–87° where model simulations substantial overestimate ClO observations.


2005 ◽  
Vol 5 (6) ◽  
pp. 1623-1638 ◽  
Author(s):  
B. Vogel ◽  
R. Müller ◽  
A. Engel ◽  
J.-U. Grooß ◽  
D. Toohey ◽  
...  

Abstract. Chlorine monoxide (ClO) plays a key role in stratospheric ozone loss processes at midlatitudes. We present two balloon-borne in situ measurements of ClO conducted in northern hemisphere midlatitudes during the period of the maximum of total inorganic chlorine loading in the atmosphere. Both ClO measurements were conducted on board the TRIPLE balloon payload, launched in November 1996 in León, Spain, and in May 1999 in Aire sur l'Adour, France. For both flights a ClO daylight and night-time vertical profile was derived over an altitude range of approximately 15-35 km. ClO mixing ratios are compared to model simulations performed with the photochemical box model version of the Chemical Lagrangian Model of the Stratosphere (CLaMS). Simulations along 24-hour backward trajectories were performed to study the diurnal variation of ClO in the midlatitude lower stratosphere. Model simulations for the flight launched in Aire sur l'Adour 1999 show an excellent agreement with the ClO measurements. For the flight launched in León 1996, an overall good agreement is found, whereas the flight is characterized by a more complex dynamical situation due to a possible mixture of vortex and non-vortex air. We note that for both flights at solar zenith angles greater than 86°-87° simulated ClO mixing ratios are higher than observed ClO mixing ratios. However, the present findings indicate that no substantial uncertainties exist in midlatitude chlorine chemistry of the stratosphere.


2012 ◽  
Vol 12 (10) ◽  
pp. 26245-26295 ◽  
Author(s):  
I. Wohltmann ◽  
T. Wegner ◽  
R. Müller ◽  
R. Lehmann ◽  
M. Rex ◽  
...  

Abstract. Stratospheric chemistry and denitrification are simulated for the Arctic winter 2009/2010 with the Lagrangian Chemistry and Transport Model ATLAS. A number of sensitivity runs is used to explore the impact of uncertainties in chlorine activation and denitrification on the model results. In particular, the efficiency of chlorine activation on different types of liquid aerosol versus activation on nitric acid trihydrate clouds is examined. Additionally, the impact of changes in reaction rate coefficients, in the particle number density of polar stratospheric clouds, in supersaturation, temperature or the extent of denitrification is investigated. Results are compared to satellite measurements of MLS and ACE-FTS and to in-situ measurements onboard the Geophysica aircraft during the RECONCILE measurement campaign. It is shown that even large changes in the underlying assumptions have only a small impact on the modeled ozone loss, even though they can cause considerable differences in chemical evolution and denitrification. In addition, it is shown that chlorine activation on liquid aerosols alone is able to explain the observed magnitude and morphology of the mixing ratios of active chlorine, reservoir gases and ozone.


2014 ◽  
Vol 14 (5) ◽  
pp. 5893-5927 ◽  
Author(s):  
W. Woiwode ◽  
J.-U. Grooß ◽  
H. Oelhaf ◽  
S. Molleker ◽  
S. Borrmann ◽  
...  

Abstract. Vertical redistribution of HNO3 through condensation, sedimentation and evaporation of large HNO3-containing particles inside polar stratospheric clouds (PSCs) plays an important role in the chemistry of the Arctic winter stratosphere. In situ observations by the particle probe FSSP-100 during the RECONCILE campaign indicate unexpected large potential NAT (nitric acid trihydrate) particles inside PSCs. The observations can hardly be explained assuming particles with compact morphology and spherical shape due to limited growing time at temperatures below the existence temperature of NAT (TNAT). Utilizing simulations by the CLaMS and measurements by the airborne Fourier transform infrared spectrometer MIPAS-STR we study the impact of reduced settling velocities of NAT particles on vertical HNO3 redistribution. Reduced settling velocities are expected for spherical NAT particles with low mass density or aspheric NAT particles that might explain the maximum sizes of the particles observed in situ. The results of our study support the hypothesis that denitrification is produced by significantly aspheric (i.e. columnar) compact NAT particles which are characterised by reduced settling velocities.


2021 ◽  
Author(s):  
Ramina Alwarda ◽  
Kristof Bognar ◽  
Kimberly Strong ◽  
Martyn Chipperfield ◽  
Sandip Dhomse ◽  
...  

<p>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°N, 86.42°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<sub>2</sub> during spring, as well as enhanced reactive halogen species (OClO and BrO). Complementary measurements of HCl and ClONO<sub>2</sub> (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<sub>3</sub> 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.</p>


2017 ◽  
Author(s):  
Farahnaz Khosrawi ◽  
Oliver Kirner ◽  
Björn-Martin Sinnhuber ◽  
Sören Johansson ◽  
Michael Höpfner ◽  
...  

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.


2014 ◽  
Vol 7 (4) ◽  
pp. 5087-5139 ◽  
Author(s):  
R. Pommrich ◽  
R. Müller ◽  
J.-U. Grooß ◽  
P. Konopka ◽  
F. Ploeger ◽  
...  

Abstract. Variations in the mixing ratio of trace gases of tropospheric origin entering the stratosphere in the tropics are of interest for assessing both troposphere to stratosphere transport fluxes in the tropics and the impact of these transport fluxes on the composition of the tropical lower stratosphere. Anomaly patterns of carbon monoxide (CO) and long-lived tracers in the lower tropical stratosphere allow conclusions about the rate and the variability of tropical upwelling to be drawn. Here, we present a simplified chemistry scheme for the Chemical Lagrangian Model of the Stratosphere (CLaMS) for the simulation, at comparatively low numerical cost, of CO, ozone, and long-lived trace substances (CH4, N2O, CCl3F (CFC-11), CCl2F2 (CFC-12), and CO2) in the lower tropical stratosphere. For the long-lived trace substances, the boundary conditions at the surface are prescribed based on ground-based measurements in the lowest model level. The boundary condition for CO in the free troposphere is deduced from MOPITT measurements (at ≈ 700–200 hPa). Due to the lack of a specific representation of mixing and convective uplift in the troposphere in this model version, enhanced CO values, in particular those resulting from convective outflow are underestimated. However, in the tropical tropopause layer and the lower tropical stratosphere, there is relatively good agreement of simulated CO with in-situ measurements (with the exception of the TROCCINOX campaign, where CO in the simulation is biased low ≈ 10–20 ppbv). Further, the model results are of sufficient quality to describe large scale anomaly patterns of CO in the lower stratosphere. In particular, the zonally averaged tropical CO anomaly patterns (the so called "tape recorder" patterns) simulated by this model version of CLaMS are in good agreement with observations. The simulations show a too rapid upwelling compared to observations as a consequence of the overestimated vertical velocities in the ERA-interim reanalysis data set. Moreover, the simulated tropical anomaly patterns of N2O are in good agreement with observations. In the simulations, anomaly patterns for CH4 and CFC-11 were found to be consistent with those of N2O; for all long-lived tracers, positive anomalies are simulated because of the enhanced tropical upwelling in the easterly phase of the quasi-biennial oscillation.


2018 ◽  
Vol 12 (6) ◽  
pp. 1921-1937 ◽  
Author(s):  
Aleksey Malinka ◽  
Eleonora Zege ◽  
Larysa Istomina ◽  
Georg Heygster ◽  
Gunnar Spreen ◽  
...  

Abstract. Melt ponds occupy a large part of the Arctic sea ice in summer and strongly affect the radiative budget of the atmosphere–ice–ocean system. In this study, the melt pond reflectance is considered in the framework of radiative transfer theory. The melt pond is modeled as a plane-parallel layer of pure water upon a layer of sea ice (the pond bottom). We consider pond reflection as comprising Fresnel reflection by the water surface and multiple reflections between the pond surface and its bottom, which is assumed to be Lambertian. In order to give a description of how to find the pond bottom albedo, we investigate the inherent optical properties of sea ice. Using the Wentzel–Kramers–Brillouin approximation approach to light scattering by non-spherical particles (brine inclusions) and Mie solution for spherical particles (air bubbles), we conclude that the transport scattering coefficient in sea ice is a spectrally independent value. Then, within the two-stream approximation of the radiative transfer theory, we show that the under-pond ice spectral albedo is determined by two independent scalar values: the transport scattering coefficient and ice layer thickness. Given the pond depth and bottom albedo values, the bidirectional reflectance factor (BRF) and albedo of a pond can be calculated with analytical formulas. Thus, the main reflective properties of the melt pond, including their spectral dependence, are determined by only three independent parameters: pond depth z, ice layer thickness H, and transport scattering coefficient of ice σt.The effects of the incident conditions and the atmosphere state are examined. It is clearly shown that atmospheric correction is necessary even for in situ measurements. The atmospheric correction procedure has been used in the model verification. The optical model developed is verified with data from in situ measurements made during three field campaigns performed on landfast and pack ice in the Arctic. The measured pond albedo spectra were fitted with the modeled spectra by varying the pond parameters (z, H, and σt). The coincidence of the measured and fitted spectra demonstrates good performance of the model: it is able to reproduce the albedo spectrum in the visible range with RMSD that does not exceed 1.5 % for a wide variety of melt pond types observed in the Arctic.


2019 ◽  
Vol 19 (21) ◽  
pp. 13681-13699 ◽  
Author(s):  
Marleen Braun ◽  
Jens-Uwe Grooß ◽  
Wolfgang Woiwode ◽  
Sören Johansson ◽  
Michael Höpfner ◽  
...  

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.


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