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The tropopause layer plays a key role in manifold processes in atmospheric chemistry and physics. Here we compare the representation and characteristics of the lapse rate tropopause according to the definition of the World Meteorological Organization (WMO) as estimated from European Centre for Medium-Range Weather Forecasts (ECMWF) reanalysis data. Our study is based on 10-year records (2009 to 2018) of ECMWF's state-of-the-art reanalysis ERA5 and its predecessor ERA-Interim. The intercomparison reveals notable differences between ERA5 and ERA-Interim tropopause data, in particular on small spatiotemporal scales. The monthly mean differences of ERA5 minus ERA-Interim tropopause heights vary between −300 m at the transition from the tropics to the extratropics (near 30∘ S and 30∘ N) to 150 m around the Equator. Mean tropopause temperatures are mostly lower in ERA5 than in ERA-Interim, with a maximum difference of up to −1.5 K in the tropics. Monthly standard deviations of tropopause heights of ERA5 are up to 350 m or 60 % larger than for ERA-Interim. Monthly standard deviations of tropopause temperatures of ERA5 exceed those of ERA-Interim by up to 1.5 K or 30 %. The occurrence frequencies of double-tropopause events in ERA5 exceed those of ERA-Interim by up to 25 percentage points at middle latitudes. We attribute the differences between the ERA5 and ERA-Interim tropopause data and the larger, more realistic variability of ERA5 to improved spatiotemporal resolution and better representation of geophysical processes in the forecast model as well as improvements in the data assimilation scheme and the utilization of additional observations in ERA5. The improved spatiotemporal resolution of ERA5 allows for a better representation of mesoscale features, in particular of gravity waves, which affect the temperature profiles in the upper troposphere and lower stratosphere (UTLS) and thus the tropopause height estimates. We evaluated the quality of the ERA5 and ERA-Interim reanalysis tropopause data by comparisons with COSMIC and MetOp Global Positioning System (GPS) satellite observations as well as high-resolution radiosonde profiles. The comparison indicates an uncertainty of the first tropopause for ERA5 (ERA-Interim) of about ±150 to ±200 m (±250 m) based on radiosonde data and ±120 to ±150 m (±170 to ±200 m) based on the coarser-resolution GPS data at different latitudes. Consequently, ERA5 will provide more accurate information than ERA-Interim for future tropopause-related studies.

Atmospheric gravity waves yield substantial small-scale temperature fluctuations that can trigger the formation of polar stratospheric clouds (PSCs). This paper introduces a new satellite record of gravity wave activity in the polar lower stratosphere to investigate this process. The record is comprised of observations of the Atmospheric Infrared Sounder (AIRS) aboard NASA's Aqua satellite from January 2003 to December 2012. Gravity wave activity is measured in terms of detrended and noise-corrected 15 µm brightness temperature variances, which are calculated from AIRS channels that are the most sensitive to temperature fluctuations at about 17–32 km of altitude. The analysis of temporal patterns in the data set revealed a strong seasonal cycle in wave activity with wintertime maxima at mid- and high latitudes. The analysis of spatial patterns indicated that orography as well as jet and storm sources are the main causes of the observed waves. Wave activity is closely correlated with 30 hPa zonal winds, which is attributed to the AIRS observational filter. We used the new data set to evaluate explicitly resolved temperature fluctuations due to gravity waves in the European Centre for Medium-Range Weather Forecasts (ECMWF) operational analysis. It was found that the analysis reproduces orographic and non-orographic wave patterns in the right places, but that wave amplitudes are typically underestimated by a factor of 2–3. Furthermore, in a first survey of joint AIRS and Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) satellite observations, nearly 50 gravity-wave-induced PSC formation events were identified. The survey shows that the new AIRS data set can help to better identify such events and more generally highlights the importance of the process for polar ozone chemistry.

More than 3 decades after the discovery of the ozone hole, the processes involved in its formation are believed to be understood in great detail. Current state-of-the-art models can reproduce the observed chemical composition in the springtime polar stratosphere, especially regarding the quantification of halogen-catalysed ozone loss. However, we report here on a discrepancy between simulations and observations during the less-well-studied period of the onset of chlorine activation. During this period, which in the Antarctic is between May and July, model simulations significantly overestimate HCl, one of the key chemical species, inside the polar vortex during polar night. This HCl discrepancy is also observed in the Arctic. The discrepancy exists in different models to varying extents; here, we discuss three independent ones, the Chemical Lagrangian Model of the Stratosphere (CLaMS) as well as the Eulerian models SD-WACCM (the specified dynamics version of the Whole Atmosphere Community Climate Model) and TOMCAT/SLIMCAT. The HCl discrepancy points to some unknown process in the formulation of stratospheric chemistry that is currently not represented in the models. We characterise the HCl discrepancy in space and time for the Lagrangian chemistry–transport model CLaMS, in which HCl in the polar vortex core stays about constant from June to August in the Antarctic, while the observations indicate a continuous HCl decrease over this period. The somewhat smaller discrepancies in the Eulerian models SD-WACCM and TOMCAT/SLIMCAT are also presented. Numerical diffusion in the transport scheme of the Eulerian models is identified to be a likely cause for the inter-model differences. Although the missing process has not yet been identified, we investigate different hypotheses on the basis of the characteristics of the discrepancy. An underestimated HCl uptake into the polar stratospheric cloud (PSC) particles that consist mainly of H2O and HNO3 cannot explain it due to the temperature correlation of the discrepancy. Also, a direct photolysis of particulate HNO3 does not resolve the discrepancy since it would also cause changes in chlorine chemistry in late winter which are not observed. The ionisation caused by galactic cosmic rays provides an additional NOx and HOx source that can explain only about 20 % of the discrepancy. However, the model simulations show that a hypothetical decomposition of particulate HNO3 by some other process not dependent on the solar elevation, e.g. involving galactic cosmic rays, may be a possible mechanism to resolve the HCl discrepancy. Since the discrepancy reported here occurs during the beginning of the chlorine activation period, where the ozone loss rates are small, there is only a minor impact of about 2 % on the overall ozone column loss over the course of Antarctic winter and spring.

Cirrus clouds play an important role in the radiation budget of the Earth; nonetheless, the radiative effect of ultra-thin cirrus clouds in the tropopause region and in the lowermost stratosphere remains poorly constrained. These clouds have a small vertical extent and optical depth and are frequently neither observed even by sensitive sensors nor considered in climate model simulations. In addition, their short-wave (cooling) and long-wave (warming) radiative effects are often in approximate balance, and their net effect strongly depends on the shape and size of the cirrus particles. However, the CRyogenic Infrared Spectrometers and Telescopes for the Atmosphere instrument (CRISTA-2) allows ultra-thin cirrus clouds to be detected. Here we use CRISTA-2 observations in summer 1997 in the Northern Hemisphere midlatitudes together with the Suite Of Community RAdiative Transfer codes based on Edwards and Slingo (SOCRATES) radiative transfer model to calculate the radiative effect of observed ultra-thin cirrus. Using sensitivity simulations with different ice effective particle size and shape, we provide an estimate of the uncertainty in the radiative effect of ultra-thin cirrus in the extratropical lowermost stratosphere and tropopause region during summer and – by extrapolation of the summer results – for winter. Cloud top height and ice water content are based on CRISTA-2 measurements, while the cloud vertical thickness was predefined to be 0.5 or 2 km. Our results indicate that if the ice crystals of these thin cirrus clouds are assumed to be spherical, their net cloud radiative effect is generally positive (warming). In contrast, assuming aggregates or a hexagonal shape, their net radiative effect is generally negative (cooling) during summer months and very likely positive (warming) during winter. The radiative effect is in the order of ±(0.1–0.01) W m−2 for a realistic global cloud coverage of 10 %, similar to the magnitude of the contrail cirrus radiative forcing (of ∼ 0.1 W m−2). The radiative effect is also dependent on the cloud vertical extent and consequently the optically thickness and effective radius of the particle size distribution (e.g. effective radius increase from 5 to 30 µm results in a factor ∼ 6 smaller long- and short-wave effects, respectively). The properties of ultra-thin cirrus clouds in the lowermost stratosphere and tropopause region need to be better observed, and ultra-thin cirrus clouds need to be evaluated in climate model simulations.

Cloud particle size distributions (PSDs) are crucial in determining the clouds physical and optical properties and hence their radiative feedback to the climate. Here we present unprecedented occurrence patterns of cloud particles derived from 270 h of cloud measurements (≈ 975 000 PSDs). The focus of the analysis is on cirrus clouds, but liquid and mixed-phase clouds are also shown. In particular, cirrus PSDs for cold to warm cirrus temperatures and microphysically thin to thick cirrus clouds are provided in a novel presentation as heat maps. The observations are accompanied by simulations of ice crystal growth in in situ-origin cirrus, showing that the maximum size to which the cirrus ice crystals can grow increases from approx. 60 µm@T < 200 K to 230 µm@T > 220 K. Crystals larger than this size are most likely of liquid-origin. The combined evaluation of observations and simulations allows the attribution of processes shaping the PSDs. Important results are that, with increasing temperature and cirrus thickness, the most frequent ice particles change from smaller and fewer crystals of in situ-origin to larger and more crystals of both in situ and liquid-origin i.e. the cirrus type changes from in situ- to liquid-origin. In addition, three characteristic ice crystal size ranges are identified. The nucleation/evaporation size interval (∼ 3–20 µm), most frequent in the coldest, thinnest in situ-origin cirrus; the – most common – overlap size interval (∼ 20–230 µm), where both in situ-origin liquid-origin cirrus occur and the uplift/sedimenation size interval (>∼ 230 µm), which consists mostly of liquid-origin ice crystals.

Ice clouds play an important role in regulating water vapor and influencing the radiative budget in the atmosphere. This study investigates stratospheric ice clouds (SICs) in the latitude range between ±60∘ based on the Cloud–Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO). As polar stratospheric clouds include other particles, they are not discussed in this work. Tropopause temperature, double tropopauses, clouds in the upper troposphere and lower stratosphere (UTLS), gravity waves, and stratospheric aerosols are analyzed to investigate their relationships with the occurrence of and variability in SICs in the tropics and at midlatitudes. We found that SICs with cloud-top heights of 250 m above the first lapse rate tropopause are mainly detected in the tropics. Monthly time series of SICs from 2007 to 2019 show that high occurrence frequencies of SICs follow the Intertropical Convergence Zone (ITCZ) over time in the tropics and that SICs vary interannually at different latitudes. Results show that SICs associated with double tropopauses, which are related to poleward isentropic transport, are mostly found at midlatitudes. More than 80 % of the SICs around 30∘ N/S are associated with double tropopauses. Correlation coefficients of SICs and all the other abovementioned processes confirm that the occurrence of and variability in SICs are mainly associated with the tropopause temperature in the tropics and at midlatitudes. UTLS clouds, which are retrieved from the Atmospheric Infrared Sounder (AIRS) and used as a proxy for deep convection in the tropics and high-altitude ice cloud sources at midlatitudes, have the highest correlations with SICs in the monsoon regions and the central United States. Gravity waves are mostly related to SICs at midlatitudes, especially over Patagonia and the Drake Passage. However, the second-highest correlation coefficients show that the cold tropopause temperature, the occurrence of double tropopauses, high stratospheric aerosol loading, frequent UTLS clouds, and gravity waves are highly correlated with the SICs locally. The long-term anomaly analyses show that interannual anomalies of SICs are correlated with the tropopause temperature and stratospheric aerosols instead of the UTLS clouds and gravity waves. The overlapping and similar correlation coefficients between SICs and all processes mentioned above indicate strong associations between those processes themselves. Due to their high inherent correlations, it is challenging to disentangle and evaluate their contributions to the occurrence of SICs on a global scale. However, the correlation coefficient analyses between SICs and all abovementioned processes (tropopause temperature, double tropopauses, clouds in the upper troposphere and lower stratosphere (UTLS), gravity waves, and stratospheric aerosols) in this study help us better understand the sources of SICs on a global scale.

Ice clouds in the lowermost stratosphere affect stratospheric water vapour and the Earth's radiation budget. The knowledge of its occurrence and driving forces is limited. To assess the distribution and possible formation mechanisms of stratospheric ice clouds (SICs) over North America, we analysed SIC occurrence frequencies observed by the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) instrument during the years 2006 to 2018. Possible driving forces such as deep convection are assessed based on Atmospheric Infrared Sounder (AIRS) observations during the same time. Results show that at nighttime, SICs are most frequently observed during the thunderstorm season over the Great Plains from May to August (MJJA) with a maximum occurrence frequency of 6.2 %. During the months from November to February (NDJF), the highest SICs occurrence frequencies are 5.5 % over the north-eastern Pacific and western Canada and 4.4 % over the western North Atlantic. Occurrence frequencies of deep convection from AIRS, which includes storm systems, fronts, mesoscale convective systems, and mesoscale convective complexes at midlatitude and high latitude, show similar hotspots like the SICs, with highest occurrence frequencies being observed over the Great Plains in MJJA (4.4 %) and over the north-eastern Pacific, western Canada, and the western North Atlantic in NDJF (∼ 2.5 %). Both, seasonal patterns and daily time series of SICs and deep convection show a high degree of spatial and temporal relation. Further analysis indicates that the maximum fraction of SICs related to deep convection is 74 % over the Great Plains in MJJA and about 50 % over the western North Atlantic, the north-eastern Pacific, and western Canada in NDJF. We conclude that, locally and regionally, deep convection is the leading factor related to the occurrence of SICs over North America. In this study, we also analysed the impact of gravity waves as another important factor related to the occurrence of SICs, as the Great Plains is a well-known hotspot for stratospheric gravity waves. In the cases where SICs are not directly linked to deep convection, we found that stratospheric gravity wave observations correlate with SICs with as much as 30 % of the cases over the Great Plains in MJJA, about 50 % over the north-eastern Pacific and western Canada, and up to 90 % over eastern Canada and the north-west Atlantic in NDJF. Our results provide a better understanding of the physical processes and climate variability related to SICs and will be of interest for modellers as SIC sources such as deep convection and gravity waves are small-scale processes that are difficult to represent in global general circulation models.

We have performed backward trajectory calculations and simulations with the three-dimensional Chemical Lagrangian Model of the Stratosphere (CLaMS) for two succeeding monsoon seasons using artificial tracers of air mass origin. With these tracers we trace back the origin of young air masses (age <6 months) at the top of the Asian monsoon anticyclone and of air masses within the tropical pipe (6 months < age <18 months) during summer 2008. The occurrence of young air masses (<6 months) at the top of the Asian monsoon anticyclone up to ∼460 K is in agreement with satellite measurements of chlorodifluoromethane (HCFC-22) by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument. HCFC-22 can be considered as a regional tracer for continental eastern Asia and the Middle East as it is mainly emitted in this region. Our findings show that the transport of air masses from boundary layer sources in the region of the Asian monsoon into the tropical pipe occurs in three distinct steps. First, very fast uplift in “a convective range” transports air masses up to 360 K potential temperature within a few days. Second, air masses are uplifted from about 360 K up to 460 K within “an upward spiralling range” within a few months. The large-scale upward spiral extends from northern Africa to the western Pacific. The air masses are transported upwards by diabatic heating with a rate of up to 1–1.5 K per day, implying strong vertical transport above the Asian monsoon anticyclone. Third, transport of air masses occurs within the tropical pipe up to 550 K associated with the large-scale Brewer–Dobson circulation within ∼1 year. In the upward spiralling range, air masses are uplifted by diabatic heating across the (lapse rate) tropopause, which does not act as a transport barrier, in contrast to the extratropical tropopause. Further, in the upward spiralling range air masses from inside the Asian monsoon anticyclone are mixed with air masses convectively uplifted outside the core of the Asian monsoon anticyclone in the tropical adjacent regions. Moreover, the vertical transport of air masses from the Asian monsoon anticyclone into the tropical pipe is weak in terms of transported air masses compared to the transport from the monsoon anticyclone into the northern extratropical lower stratosphere. Air masses from the Asian monsoon anticyclone (India/China) contribute a minor fraction to the composition of air within the tropical pipe at 550 K (6 %), and the major fractions are from Southeast Asia (16 %) and the tropical Pacific (15 %).

The rise of ammonia emissions in Asia is predicted to increase radiative cooling and air pollution by forming ammonium nitrate particles in the lower troposphere. There is, however, a severe lack of knowledge about ammonia and ammoniated aerosol particles in the upper troposphere and their possible effects on the formation of clouds. Here we employ satellite observations and high-altitude aircraft measurements, combined with atmospheric trajectory simulations and cloud-chamber experiments, to demonstrate the presence of ammonium nitrate particles and also track the source of the ammonia that forms into the particles. We found that during the Asian monsoon period, solid ammonium nitrate particles are surprisingly ubiquitous in the upper troposphere from the Eastern Mediterranean to the Western Pacific—even as early as in 1997. We show that this ammonium nitrate aerosol layer is fed by convection that transports large amounts of ammonia from surface sources into the upper troposphere. Impurities of ammonium sulfate allow the crystallization of ammonium nitrate even in the conditions, such as a high relative humidity, that prevail in the upper troposphere. Solid ammonium nitrate particles in the upper troposphere play a hitherto neglected role in ice cloud formation and aerosol indirect radiative forcing.

Temperature fluctuations induced by mountain waves can play a crucial role in the formation of polar stratospheric clouds (PSCs). In particular, the cold phase of the waves can lower local temperatures sufficiently to trigger PSC formation, even when large-scale background temperatures are too high. To provide new quantitative constraints on the relevance of this effect, this study analyzes a decade (2002–2012) of ice PSC detections obtained from Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) measurements and ERA5 data in the polar winter lower stratosphere. In the MIPAS observations, we find that approximately 52 % of the Arctic ice PSCs and 26 % of the Antarctic ice PSCs are detected at temperatures above the local Tice. Ice PSCs above Tice are concentrated around mountainous regions and their downwind directions. A backward-trajectory analysis is performed to investigate the temperature history of each ice PSC observation. The cumulative fraction of ice PSCs above Tice increases as the trajectory gets closer to the observation point. The most significant change in the fraction of ice PSCs above Tice occurs within the 6 h preceding the observations. At the observation point, the mean fractions of ice PSCs above Tice, taking into account temperature fluctuations along the backward trajectory, are 33 % in the Arctic and 9 % in the Antarctic. The results provide a quantitative assessment of the occurrence of ice PSCs above Tice in connection with orographic waves. Additionally, the observational statistics presented can be utilized for comparison with chemistry climate simulations.