Mountain-wave-induced polar stratospheric clouds and their representation in the global chemistry model ICON-ART

Polar stratospheric clouds (PSCs) are a driver for ozone depletion in the lower polar stratosphere. They provide surface for heterogeneous reactions activating chlorine and bromine reservoir species during the polar night. The large-scale effects of PSCs are represented by means of parameterisations in current global chemistry–climate models, but one process is still a challenge: the representation of PSCs formed locally in conjunction with unresolved mountain waves. In this study, we investigate direct simulations of PSCs formed by mountain waves with the ICOsahedral Nonhydrostatic modelling framework (ICON) with its extension for Aerosols and Reactive Trace gases (ART) including local grid refinements (nesting) with two-way interaction. Here, the nesting is set up around the Antarctic Peninsula, which is a well-known hot spot for the generation of mountain waves in the Southern Hemisphere. We compare our model results with satellite measurements of PSCs from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) and gravity wave observations of the Atmospheric Infrared Sounder (AIRS). For a mountain wave event from 19 to 29 July 2008 we find similar structures of PSCs as well as a fairly realistic development of the mountain wave between the satellite data and the ICON-ART simulations in the Antarctic Peninsula nest. We compare a global simulation without nesting with the nested configuration to show the benefits of adding the nesting. Although the mountain waves cannot be resolved explicitly at the global resolution used (about 160 km), their effect from the nested regions (about 80 and 40 km) on the global domain is represented. Thus, we show in this study that the ICON-ART model has the potential to bridge the gap between directly resolved mountain-wave-induced PSCs and their representation and effect on chemistry at coarse global resolutions

A climatology of polar stratospheric cloud composition between 2002 and 2012 based on MIPAS/Envisat observations

The Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument aboard the European Space Agency (ESA) Envisat satellite operated from July 2002 to April 2012. The infrared limb emission measurements provide a unique dataset of day and night observations of polar stratospheric clouds (PSCs) up to both poles. A recent classification method for PSC types in infrared (IR) limb spectra using spectral measurements in different atmospheric window regions has been applied to the complete mission period of MIPAS. The method uses a simple probabilistic classifier based on Bayes' theorem with a strong independence assumption on a combination of a well-established two-colour ratio method and multiple 2-D probability density functions of brightness temperature differences. The Bayesian classifier distinguishes between solid particles of ice, nitric acid trihydrate (NAT), and liquid droplets of supercooled ternary solution (STS), as well as mixed types. A climatology of MIPAS PSC occurrence and specific PSC classes has been compiled. Comparisons with results from the classification scheme of the spaceborne lidar Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) on the Cloud-Aerosol-Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) satellite show excellent correspondence in the spatial and temporal evolution for the area of PSC coverage (APSC) even for each PSC class. Probability density functions of the PSC temperature, retrieved for each class with respect to equilibrium temperature of ice and based on coincident temperatures from meteorological reanalyses, are in accordance with the microphysical knowledge of the formation processes with respect to temperature for all three PSC types. This paper represents unprecedented pole-covering day- and nighttime climatology of the PSC distributions and their composition of different particle types. The dataset allows analyses on the temporal and spatial development of the PSC formation process over multiple winters. At first view, a more general comparison of APSC and AICE retrieved from the observations and from the existence temperature for NAT and ice particles based on the European Centre for Medium-Range Weather Forecasts (ECMWF) reanalysis temperature data shows the high potential of the climatology for the validation and improvement of PSC schemes in chemical transport and chemistry–climate models

Unusual chlorine partitioning in the 2015/16 Arctic winter lowermost stratosphere: Observations and simulations

The Arctic winter 2015/16 was characterized by cold stratospheric temperatures. Here we present a comprehensive view of the temporal evolution of chlorine in the lowermost stratosphere over the course of the studied winter. We utilize two-dimensional vertical cross sections of ozone (\chem{O_3}) and chlorine nitrate (\chem{ClONO_2}), measured by the airborne limb imager GLORIA (Gimballed Limb Observer for Radiance Imaging of the Atmosphere) during the POLSTRACC/GW-LCYCLE~II/GWEX/SALSA campaigns, to investigate the tropopause region in detail. Observations from three long-distance flights in January, February, and March~2016 are discussed. \chem{ClONO_2} volume mixing ratios up to 1100\,pptv were measured at 380\,K potential temperature in mesoscale structures. Similar mesoscale structures are also visible in \chem{O_3} measurements. Both trace gas measurements are applied to evaluate simulation results from the chemistry transport model CLaMS (Chemical Lagrangian Model of the Stratosphere) and the chemistry--climate model EMAC (ECHAM5/MESSy Atmospheric Chemistry). These comparisons show agreement within the expected performance of these models. Satellite measurements from Aura/MLS (Microwave Limb Sounder) and SCISAT/ACE-FTS (Atmospheric Chemistry Experiment -- Fourier Transform Spectrometer) provide an overview over the whole winter and information about the stratospheric situation above the flight altitude. Time series of these satellite measurements reveal unusually low hydrochloric acid (HCl) and \chem{ClONO_2} at 380\,K from the beginning of January to the end of February~2016, while chlorine monoxide (ClO) is strongly enhanced. In March~2016, unusually rapid chlorine deactivation into HCl is observed instead of deactivation into \chem{ClONO_2}, the more typical pathway for deactivation in the Arctic. Chlorine deactivation observed in the satellite time series is well reproduced by CLaMS. Sensitivity simulations with CLaMS demonstrate the influence of low abundances of \chem{O_3} and reactive nitrogen (\chem{NO_\mathit{y}}) due to ozone depletion and sedimentation of \chem{NO_\mathit{y}}-containing particles, respectively. On the basis of the different altitude and time ranges of these effects, we conclude that the substantial chlorine deactivation into HCl at 380\,K arose as a result of very low ozone abundances together with low temperatures. Additionally, CLaMS estimates ozone depletion of at least 0.4\,ppmv at 380\,K and 1.75\,ppmv at 490\,K, which is comparable to other extremely cold Arctic winters. We have used CLaMS trajectories to analyze the history of enhanced \chem{ClONO_2} measured by GLORIA. In February, most of the enhanced \chem{ClONO_2} is traced back to chlorine deactivation that had occurred within the past few days prior to the GLORIA measurement. In March, after the final warming, air masses in which chlorine has previously been deactivated into \chem{ClONO_2} have been transported in the remnants of the polar vortex towards the location of measurement for at least~11\,d

CLaMS simulations of aerosol transport from the Asian monsoon anticyclone into the extratropical UTLS

The Asian Tropopause Aerosol Layer (ATAL) in the Northern Hemisphere during summer was first discovered in satellite observation of aerosol particles in the Upper Troposphere / Lower Stratosphere (UTLS) by Vernier et al. (2011; 2015). It is related to the Asian monsoon anticyclonic circulation at UTLS altitudes. Motivated by the current lack of detailed understanding of the origin of ATAL particles and the transport of aerosols from the Asian monsoon anticyclone into the extratropical UTLS, we propose a model study based on simulations with the three-dimensional chemical transport model CLaMS. Simulations will be performed for the Asian summer monsoon 2017. In the framework of the StratoClim project, an aircraft measurement campaign was conducted in Kathmandu (Nepal) in summer 2017. A variety of trace gases and aerosol characteristics have been measured for the first time in the Asian monsoon anticyclone up to 20 km altitude. By using artificial tracers of air mass origin (Vogel et al., 2015; 2016; 2019), we plan to analyze the transport of aerosol particles into the extratropical UTLS with the help of the new ERA-5 reanalysis data from ECMWF

Aerosol Transport from the Asian Summer Monsoon into the Arctic Lower Stratosphere

The Asian summer monsoon is linked to deep convection over the Indian subcontinent and to an anticyclonic flow that extends from the upper troposphere into the lower stratosphere region. This allows both gas-phase aerosol precursors and aerosol particles from surface sources to reach the stratosphere. The horizontal transport out of the Asian monsoon anticyclone towards the extratropical lower stratosphere of the Northern Hemisphere is the focus of this study. We present an annual record of Lidar observations at AWIPEV in Ny-Ålesund. The data record is free from obvious layers like polar stratospheric clouds, volcanic eruptions or forest fires. Nevertheless, the lower stratosphere reveals an annual cycle with lower backscatter values in winter and spring and higher backscatter values in summer and autumn. The Lidar measurements have been linked to backward trajectory calculations and simulations of artificial surface origin tracers with the three-dimensional Chemical Lagrangian Model of the Stratosphere (CLaMS). The simulations show that air masses observed above Ny-Ålesund have been transported from surface sources in Asia into the Arctic lower stratosphere. Thus, the increased backscatter values during summer and autumn can be explained by transport of aerosol particles from the Asian summer monsoon into the Arctic lower stratosphere

Vortex-wide chlorine activation by a mesosclae PSC event in the Arctic winter of 2009/10

In the Arctic polar vortex of the 2009/10 winter temperatures were low enough to allow widespread formation of Polar Stratospheric Clouds (PSC). These clouds occurred during the initial chlorine activation phase which provided the opportunity to investigate the impact of PSCs on chlorine activation. Satellite observations of gas-phase species and PSCs are used in combination with trajectory modeling to assess this initial activation. The initial activation occurred in association with the formation of PSCs over the east coast of Greenland at the beginning of January 2010. Although this area of PSCs covered only a small portion of the vortex, it was responsible for almost the entire initial activation of chlorine vortex wide. Observations show HCl mixing ratios decreased rapidly in and downstream of this region. Trajectory calculations and simplified heterogeneous chemistry modeling confirmed that the initial chlorine activation continued until ClONO2 was completely depleted and the activated air masses were advected throughout the polar vortex. For the calculation of heterogeneous reaction rates, surface area density is estimated from backscatter observations. Modeled heterogeneous reaction rates along trajectories intersecting with the PSC indicate that the initial phase of chlorine activation occurred in just a few hours. These calculations also indicate that chlorine activation on the binary background aerosol is significantly slower than on the PSCs and the observed chlorine activation can only be explained by an increase in surface area density due to PSCs. Furthermore, there is a strong correlation between the magnitude of the observed HCl depletion and PSC surface area

Polar Stratospheric Clouds: Satellite Observations, Processes, and Role in Ozone Depletion

The important role of polar stratospheric clouds (PSCs) in stratospheric ozone depletion during winter and spring at high latitudes has been known since the 1980s. However, contemporary observations by the spaceborne instruments MIPAS (Michelson Interferometer for Passive Atmospheric Sounding), MLS (Microwave Limb Sounder), and CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) have brought about a comprehensive and clearer understanding of PSC spatial and temporal distributions, their conditions of existence, and the processes through which they impact polar ozone. Within the SPARC (Stratosphere-troposphere Processes And their Role in Climate) PSC initiative (PSCi), those datasets have been synthesized and discussed in depth with the result of a new vortex-wide climatology of PSC occurrence and composition. We will present our results within this vPICO together with a review of the significant progress that has been made in our understanding of PSC nucleation, related dynamical processes, and heterogeneous chlorine activation. Moreover, we have compiled different techniques for parameterizing PSCs and we will show their effects in global models.</p

Polar Stratospheric Clouds: Satellite Observations, Processes, and Role in Ozone Depletion

The important role of polar stratospheric clouds (PSCs) in stratospheric ozone depletion during winter and spring at high latitudes has been known since the 1980s. However, contemporary observations by the spaceborne instruments MIPAS (Michelson Interferometer for Passive Atmospheric Sounding), MLS (Microwave Limb Sounder), and CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) have brought about a comprehensive and clearer understanding of PSC spatial and temporal distributions, their conditions of existence, and the processes through which they impact polar ozone. Within the SPARC (Stratosphere-troposphere Processes And their Role in Climate) PSC initiative (PSCi), those datasets have been synthesized and discussed in depth with the result of a new vortex-wide climatology of PSC occurrence and composition. We will present our results within this vPICO together with a review of the significant progress that has been made in our understanding of PSC nucleation, related dynamical processes, and heterogeneous chlorine activation. Moreover, we have compiled different techniques for parameterizing PSCs and we will show their effects in global models.</p