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Simulations of Antarctic chlorine and ozone chemistry in previous work show that in the core of the Antarctic vortex (16–18 km, 85–55 hPa, 390–430 K) HCl null cycles (initiated by reactions of Cl with CH4 and CH2O) are effective. These HCl null cycles cause both HCl molar mixing ratios to remain very low throughout Antarctic winter and spring. They cause ozone-destroying chlorine (ClOx) to remain enhanced so that rapid ozone depletion proceeds. Here we investigate the impact of the observed dehydration in Antarctica, which strongly reduces ice formation and the uptake of HNO3 from the gas phase; however the efficacy of HCl null cycles is not affected. Moreover, also when using the observed very low HCl molar mixing ratios in Antarctic winter as an initial value, HCl null cycles are efficient in maintaining low HCl (and high ClOx) throughout winter and spring. Further, the reaction CH3O2+ClO is important for the efficacy of the HCl null cycle initiated by the reaction CH4+Cl. Using the current kinetic recommendations instead of earlier ones has very little impact on the simulations. All simulations presented here for the core of the Antarctic vortex show extremely low minimum ozone values (below 50 ppb) in late September to early October in agreement with observations.

The Asian summer monsoon has a strong convectional component with which aerosols are able to be lifted up into the lower stratosphere. Due to usually long lifetimes and long-range transport aerosols remain there much longer than in the troposphere and are also able to be advected around the globe. Our aim of this study is a synergy between simulations by Chemical Lagrangian Model of the Stratosphere (CLaMS) and KARL (Koldewey Aerosol Raman Lidar) at AWIPEV, Ny-Ålesund in the Arctic, by comparing CLaMS results with exemplary days of lidar measurements as well as analyzing the stratospheric aerosol background. We use global three-dimensional Lagrangian transport simulations including surface origin tracers as well as back trajectories to identify source regions of the aerosol particles measured over Ny-Ålesund. We analyzed lidar data for the year 2021 and found the stratosphere generally clear, without obvious aerosol layers from volcanic eruptions or biomass burnings. Still an obvious annual cycle of the backscatter coefficient with higher values in late summer to autumn and lower values in late winter has been found. Results from CLaMS model simulations indicate that from late summer to early autumn filaments with high fractions of air which originate in South Asia – one of the most polluted regions in the world – reach the Arctic at altitudes between 360 and 380 K potential temperature. We found a coinciding measurement between the overpass of such a filament and lidar observations, and we estimated that backscatter and depolarization increased by roughly 15 % during this event compared to the background aerosol concentration. Hence we demonstrate that the Asian summer monsoon is a weak but measurable source for Arctic stratospheric aerosol in late summer to early autumn.

Diabatic transport schemes with hybrid zeta coordinates, which follow isentropes in the stratosphere, are known to greatly improve Lagrangian transport calculations compared to the kinematic approach. However, some Lagrangian transport calculations with a diabatic approach, such as the Chemical Lagrangian Transport Model of the Stratosphere (CLaMS), are not well prepared to run on modern high-performance computing (HPC) architectures. Here, we implemented and evaluated a new diabatic transport scheme in the Massive-Parallel Trajectory Calculations (MPTRAC) model. While MPTRAC can be used either with shared-memory multiprocessing on CPUs or with GPUs to offload computationally intensive calculations, making it flexible for many HPC applications, it has been limited to kinematic trajectories in pressure coordinates. The extended modelling approach now enables the use of either kinematic or diabatic vertical velocities and the coupling of different MPTRAC modules based on pressure or hybrid zeta coordinates. This study focus on the accuracy of the implementation in comparison to the CLaMS model. The evaluation of the new transport scheme in MPTRAC shows that, after 90 d of forward calculations, distributions of air parcels in the upper troposphere and lower stratosphere (UTLS) are almost identical for MPTRAC and CLaMS. No significant bias between the two Lagrangian models was found. Furthermore, after 1 d, internal uncertainties (e.g. due to interpolation or the numerical integration method) in the Lagrangian transport calculations are at least 1 order of magnitude smaller than external uncertainties (e.g. from reanalysis selection or downsampling of ERA5). Differences between trajectories using either CLaMS or MPTRAC are on the order of the combined internal uncertainties within MPTRAC. Since the largest systematic differences are caused by the reanalysis and the vertical velocity (diabatic vs. kinematic), the results support the development efforts for trajectory codes that can access the full resolution of ERA5 in combination with diabatic vertical velocities. This work is part of a larger effort to adapt Lagrangian transport in state-of-the-art models such as CLaMS and MPTRAC to current and future HPC architectures and exascale applications.

Aerosol particles with diameters larger than 40 nm were collected during the flight campaign StratoClim 2017 within the Asian tropopause aerosol layer (ATAL) of the 2017 monsoon anticyclone above the Indian subcontinent. A multi-impactor system was installed on board the aircraft M-55 Geophysica, which was operated from Kathmandu, Nepal. The size and chemical composition of more than 5000 refractory particles/inclusions of 17 selected particle samples from seven different flights were analyzed by use of scanning electron microscopy (SEM) and transmission electron microscopy (TEM) combined with energy dispersive X-ray (EDX) microanalysis. Based on chemical composition and morphology, the refractory particles were assigned to the following particle groups: extraterrestrial, silicates, Fe-rich, Al-rich, Hg-rich, other metals, C-rich, soot, Cl-rich, and Ca-rich. Most abundant particle groups within the refractory particles are silicates and C-rich (non-volatile organics). In samples taken above the tropopause, extraterrestrial particles are becoming increasingly important with rising altitude. The most frequent particle sources for the small (maximum in size distribution DP-max=120 nm) refractory particles carried into the ATAL are combustion processes at the ground (burning of fossil fuels/biomass burning) and the agitation of soil material. The refractory particles in the ATAL represent only a very small fraction (< 2 % by number for particles > 40 nm) of the total aerosol particles, which are dominated by species like ammonium, sulfate, nitrate, and volatile organics. During one flight, a large number of very small (DP-max=25 nm) cinnabar particles (HgS) were detected, which are supposed to originate from a ground source such as coal combustion or underground coal fires.

During the Asian monsoon season, greenhouse gases and pollution emitted near the ground are rapidly uplifted by convection up to an altitude of ∼ 13 km, with slower ascent and mixing with the stratospheric background above. Here, we address the robustness of the representation of these transport processes in different reanalysis data sets using ERA5, ERA-Interim and ERA5 1∘×1∘. This transport assessment includes the mean age of air from global three-dimensional simulations by the Lagrangian transport model CLaMS (Chemical Lagrangian Model of the Stratosphere), as well as different trajectory-based transport times and associated ascent rates compared with observation-based age of air and ascent rates of long-lived trace gases from airborne measurements during the Asian summer monsoon 2017 in Nepal. Our findings confirm that the ERA5 reanalysis yields a better representation of convection than ERA-Interim, resulting in different transport times and air mass origins at the Earth's surface. In the Asian monsoon region above 430 K, the mean age of air driven by ERA-Interim is too young, whereas the mean age of air from ERA5 1∘×1∘ is too old but somewhat closer to the observations. The mean effective ascent rates derived from ERA5 and ERA5 1∘×1∘ back trajectories are in good agreement with the observation-based mean ascent rates, unlike ERA-Interim, which is much faster above 430 K. Although a reliable CO2 reconstruction is a challenge for model simulations, we show that, up to 410 K, the CO2 reconstruction using ERA5 agrees best with high-resolution in situ aircraft CO2 measurements, indicating a better representation of Asian monsoon transport in the newest ECMWF reanalysis product, ERA5.

The Asian tropopause aerosol layer (ATAL) is present during the Asian summer monsoon season affecting the radiative balance of the atmosphere. However, the source regions and transport pathways of ATAL particles are still uncertain. Here, we investigate transport pathways from different regions at the model boundary layer (MBL) to the ATAL by combining two Lagrangian transport models (CLaMS, Chemical Lagrangian Model of the Stratosphere; MPTRAC, Massive-Parallel Trajectory Calculations) with balloon-borne measurements of the ATAL performed by the Compact Optical Backscatter Aerosol Detector (COBALD) above Nainital (India) in August 2016. Trajectories are initialised at the measured location of the ATAL and calculated 90 d backwards in time to investigate the relation between the measured, daily averaged, aerosol backscatter ratio and source regions at the MBL. Different simulation scenarios are performed to find differences and robust patterns when the reanalysis data (ERA5 or ERA-Interim), the trajectory model, the vertical coordinate (kinematic and diabatic approach) or the convective parameterisation are varied. The robust finding among all scenarios is that the largest continental air mass contributions originate from the Tibetan Plateau and the Indian subcontinent (mostly the Indo-Gangetic Plain), and the largest maritime air mass contributions in Asia come from the western Pacific (e.g. related to tropical cyclones). Additionally, all simulation scenarios indicate that the transport of maritime air from the tropical western Pacific to the region of the ATAL lowers the backscatter ratio (BSR) of the ATAL, while most scenarios indicate that the transport of polluted air from the Indo-Gangetic Plain increases the BSR. While the results corroborate key findings from previous ERA-Interim-based studies, they also highlight the variability in the contributions of different MBL regions to the ATAL depending on different simulation scenarios.

Atmospheric convection plays a key role in tracer transport from the planetary boundary layer to the free troposphere. Lagrangian transport simulations driven by meteorological fields from global models or reanalysis products, such as the European Centre for Medium-Range Weather Forecasts' (ECMWF's) ERA5 and ERA-Interim reanalysis, typically lack proper explicit representations of convective updrafts and downdrafts because of the limited spatiotemporal resolution of the meteorology. Lagrangian transport simulations for the troposphere can be improved by applying parameterizations to better represent the effects of unresolved convective transport in the global meteorological reanalyses. Here, we implemented and assessed the effects of the extreme convection parameterization (ECP) in the Massive-Parallel Trajectory Calculations (MPTRAC) model. The ECP is conceptually simple. It requires the convective available potential energy (CAPE) and the height of the equilibrium level (EL) as input parameters. Assuming that unresolved convective events yield well-mixed vertical columns of air, the ECP randomly redistributes the air parcels vertically between the surface and the EL if CAPE is present. We analyzed statistics of explicitly resolved and parameterized convective updrafts and found that the frequencies of strong updrafts due to the ECP, i.e., 20 K potential temperature increase over 6 h or more, increase by 2 to 3 orders of magnitude for ERA5 and 3 to 5 orders of magnitude for ERA-Interim compared to the explicitly resolved updrafts. To assess the effects of the ECP on tropospheric tracer transport, we conducted transport simulations for the artificial tracer e90, which is released globally near the surface and which has a constant e-folding lifetime of 90 d throughout the atmosphere. The e90 simulations were conducted for the year 2017 with both ERA5 and ERA-Interim. Next to sensitivity tests on the choice of the CAPE threshold, an important tuning parameter of the ECP, we suggest a modification of the ECP method, i.e., to take into account the convective inhibition (CIN) indicating the presence of warm, stable layers that prevent convective updrafts in the real atmosphere. While ERA5 has higher spatiotemporal resolution and explicitly resolves more convective updrafts than ERA-Interim, we found there is still a need for both reanalyses to apply a convection parameterization such as the ECP to better represent tracer transport from the planetary boundary layer into the free troposphere on the global scale.

Dusty cirrus clouds are extended optically thick cirrocumulus decks that occur during strong mineral dust events. So far they have mostly been documented over Europe associated with dust-infused baroclinic storms. Since today's global numerical weather prediction models neither predict mineral dust distributions nor consider the interaction of dust with cloud microphysics, they cannot simulate this phenomenon. We postulate that the dusty cirrus forms through a mixing instability of moist clean air with drier dusty air. A corresponding sub-grid parameterization is suggested and tested in the ICOsahedral Nonhydrostatic model with Aerosol and Reactive Trace gases (ICON-ART). Only with the help of this parameterization is ICON-ART able to simulate the formation of the dusty cirrus, which leads to substantial improvements in cloud cover and radiative fluxes compared to simulations without this parameterization. A statistical evaluation over six Saharan dust events with and without observed dusty cirrus shows robust improvements in cloud and radiation scores. The ability to simulate dusty cirrus formation removes the linear dependency on mineral dust aerosol optical depth from the bias of the radiative fluxes. For the six Saharan dust episodes investigated in this study, the formation of dusty cirrus clouds is the dominant aerosol–cloud–radiation effect of mineral dust over Europe.

Aircraft-borne in situ measurements of the chemical aerosol composition were conducted in the Asian tropopause aerosol layer (ATAL) over the Indian subcontinent in the summer of 2017, covering particle sizes below ∼3 µm. We have implemented a recently developed aerosol mass spectrometer, which adopts the laser desorption technique as well as the thermal desorption method for quantitative bulk information (i.e., a modified Aerodyne AMS), aboard the high-altitude research aircraft M-55 Geophysica. The instrument was deployed in July and August 2017 during the StratoClim EU campaign (Stratospheric and upper tropospheric processes for better Climate predictions) over Nepal, India, Bangladesh, and the Bay of Bengal, covering altitudes up to 20 kma.s.l. For particles with diameters between 10 nm and ∼3 µm, the vertical profiles of aerosol number densities from the eight research flights show significant enhancements in the altitude range of the ATAL. We observed enhancements in the mass concentrations of particulate nitrate, ammonium, and organics in a similar altitude range between approximately 13 and 18 km (corresponding to 360 and 410 K potential temperature). By means of the two aerosol mass spectrometry techniques, we show that the particles in the ATAL mainly consist of ammonium nitrate (AN) and organics. The single-particle analysis from laser desorption and ionization mass spectrometry revealed that a significant particle fraction (up to 70 % of all analyzed particles by number) within the ATAL results from the conversion of inorganic and organic gas-phase precursors, rather than from the uplift of primary particles from below. This can be inferred from the fact that the majority of the particles encountered in the ATAL consisted solely of secondary substances, namely an internal mixture of nitrate, ammonium, sulfate, and organic matter. These particles are externally mixed with particles containing primary components as well. The single-particle analysis suggests that the organic matter within the ATAL and in the lower stratosphere (even above 420 K) can partly be identified as organosulfates (OS), in particular glycolic acid sulfate, which are known as components indicative for secondary organic aerosol (SOA) formation. Additionally, the secondary particles are smaller in size compared to those containing primary components (mainly potassium, metals, and elemental carbon). The analysis of particulate organics with the thermal desorption method shows that the degree of oxidation for particles observed in the ATAL is consistent with expectations about secondary organics that were subject to photochemical processing and aging. We found that organic aerosol was less oxidized in lower regions of the ATAL ( K) compared to higher altitudes (here 390–420 K). These results suggest that particles formed in the lower ATAL are uplifted by prevailing diabatic heating processes and thereby subject to extensive oxidative aging. Thus, our observations are consistent with the concept of precursor gases being emitted from regional ground sources, subjected to rapid convective uplift, and followed by secondary particle formation and growth in the upper troposphere within the confinement of the Asian monsoon anticyclone (AMA). As a consequence, the chemical composition of these particles largely differs from the aerosol in the lower stratospheric background and the Junge layer.

Urban aerosol pollution was analyzed over the Moscow megacity region using the COSMO-ART (COSMO – COnsortium for Small-scale MOdelling, ART – Aerosols and Reactive Trace gases) online coupled mesoscale model system and intensive measurement campaigns at the Moscow State University Meteorological Observatory (MSU MO, 55.707∘ N, 37.522∘ E) during the April–May period in 2018 and 2019. We analyzed mass concentrations of particulate matter with diameters smaller than 10 µm (PM10), black carbon (BC) and aerosol gas precursors (NOx, SO2, CHx) as well as columnar aerosol parameters for fine and coarse modes together with different meteorological parameters, including an index characterizing the intensity of particle dispersion (IPD). Both model and experimental datasets have shown a statistically significant linear correlation of BC with NO2 and PM10 mass concentrations, which indicates mostly common sources of emissions of these substances. There was a pronounced increase in the BC/PM10 ratio from 0.7 % to 5.9 %, with the decrease in the IPD index related to the amplification of the atmospheric stratification. We also found an inverse dependence between the BC/PM10 ratio and columnar single-scattering albedo (SSA) for the intense air mixing conditions. This dependence together with the obtained negative correlation between wind speed and BC/PM10 may serve as an indicator of changes in the absorbing properties of the atmosphere due to meteorological factors. On average, the relatively low BC / PM10 ratio (for urban regions) of 4.7 % is the cause of the observed relatively high SSA = 0.94 in Moscow. Using long-term parallel aerosol optical depth (AOD) measurements over the 2006–2020 period at the MSU MO and under upwind clean background conditions at Zvenigorod Scientific Station (ZSS) of the IAP RAS (55.7∘ N, 36.8∘ E), we estimated the urban component of AOD (AODurb) and some other parameters as the differences at these sites. The annual mean AODurb at 550 nm was about 0.021 with more than 85 % of the fine aerosol mode. The comparisons between AODurb obtained from the model and measurements during this experiment have revealed a similar level of aerosol pollution of about AODurb=0.015–0.019, which comprised 15 %–19 % of the total AOD at 550 nm. The urban component of PM10 (PM10urb) was about 16 µg m−3 according to the measurements and 6 µg m−3 according to the COSMO-ART simulations. We obtained a pronounced diurnal cycle of PM10urb and urban BC (BCurb) as well as their strong correlation with the IPDs. With the IPD index change from 3 to 1 at night, there was about a 4 times increase in PM10urb (up to 30–40 µg m−3) and a 3 times increase in BCurb (up to 3–3.5 µg m−3). At the same time, no pronounced daily cycle was found for the columnar urban aerosol component (AODurb), although there was a slight increase in model AODurb at night.

Lagrangian models are fundamental tools to study atmospheric transport processes and for practical applications such as dispersion modeling for anthropogenic and natural emission sources. However, conducting large-scale Lagrangian transport simulations with millions of air parcels or more can become rather numerically costly. In this study, we assessed the potential of exploiting graphics processing units (GPUs) to accelerate Lagrangian transport simulations. We ported the Massive-Parallel Trajectory Calculations (MPTRAC) model to GPUs using the open accelerator (OpenACC) programming model. The trajectory calculations conducted within the MPTRAC model were fully ported to GPUs, i.e., except for feeding in the meteorological input data and for extracting the particle output data, the code operates entirely on the GPU devices without frequent data transfers between CPU and GPU memory. Model verification, performance analyses, and scaling tests of the Message Passing Interface (MPI) – Open Multi-Processing (OpenMP) – OpenACC hybrid parallelization of MPTRAC were conducted on the Jülich Wizard for European Leadership Science (JUWELS) Booster supercomputer operated by the Jülich Supercomputing Centre, Germany. The JUWELS Booster comprises 3744 NVIDIA A100 Tensor Core GPUs, providing a peak performance of 71.0 PFlop s−1. As of June 2021, it is the most powerful supercomputer in Europe and listed among the most energy-efficient systems internationally. For large-scale simulations comprising 108 particles driven by the European Centre for Medium-Range Weather Forecasts' fifth-generation reanalysis (ERA5), the performance evaluation showed a maximum speed-up of a factor of 16 due to the utilization of GPUs compared to CPU-only runs on the JUWELS Booster. In the large-scale GPU run, about 67 % of the runtime is spent on the physics calculations, conducted on the GPUs. Another 15 % of the runtime is required for file I/O, mostly to read the large ERA5 data set from disk. Meteorological data preprocessing on the CPUs also requires about 15 % of the runtime. Although this study identified potential for further improvements of the GPU code, we consider the MPTRAC model ready for production runs on the JUWELS Booster in its present form. The GPU code provides a much faster time to solution than the CPU code, which is particularly relevant for near-real-time applications of a Lagrangian transport model.

In June 2019, the Raikoke volcano, Kuril Islands, emitted 0.4–1.8×109 kg of very fine ash and 1–2×109 kg of SO2 up to 14 km into the atmosphere. The eruption was characterized by several eruption phases of different duration and height summing up to a total eruption length of about 5.5 h. Resolving such complex eruption dynamics is required for precise volcanic plume dispersion forecasts. To address this issue, we coupled the atmospheric model system ICON-ART (ICOsahedral Nonhydrostatic with the Aerosols and Reactive Trace gases module) with the 1D plume model FPlume to calculate the eruption source parameters (ESPs) online. The main inputs are the plume heights for the different eruption phases that are geometrically derived from satellite data. An empirical relationship is used to derive the amount of very fine ash (particles µm), which is relevant for long-range transport in the atmosphere. On the first day after the onset of the eruption, the modeled ash loading agrees very well with the ash loading estimated from AHI (Advanced Himawari Imager) observations due to the resolution of the eruption phases and the online treatment of the ESPs. In later hours, aerosol dynamical processes (nucleation, condensation, and coagulation) explain the loss of ash in the atmosphere in agreement with the observations. However, a direct comparison is partly hampered by water and ice clouds overlapping the ash cloud in the observations. We compared 6-hourly means of model and AHI data with respect to the structure, amplitude, and location (SAL method) to further validate the simulated dispersion of SO2 and ash. In the beginning, the structure and amplitude values for SO2 differed largely because the dense ash cloud leads to an underestimation of the SO2 amount in the satellite data. On the second and third day, the SAL values are close to zero for all parameters (except for the structure value of ash), indicating a very good agreement of the model and observations. Furthermore, we found a separation of the ash and SO2 plume after 1 d due to particle sedimentation, chemistry, and aerosol–radiation interaction. The results confirm that coupling the atmospheric model system and plume model enables detailed treatment of the plume dynamics (phases and ESPs) and leads to significant improvement of the ash and SO2 dispersion forecast. This approach can benefit the operational forecast of ash and SO2 especially in the case of complex and noncontinuous volcanic eruptions like that of Raikoke in 2019.

Efficient transport pathways for ozone-depleting very short-lived substances (VSLSs) from their source regions into the stratosphere are a matter of current scientific debate; however they have yet to be fully identified on an observational basis. Understanding the increasing impact of chlorine-containing VSLSs (Cl-VSLSs) on stratospheric ozone depletion is important in order to validate and improve model simulations and future predictions. We report on a transport study using airborne in situ measurements of the Cl-VSLSs dichloromethane (CH2Cl2) and trichloromethane (chloroform, CHCl3) to derive a detailed description of two transport pathways from (sub)tropical source regions into the extratropical upper troposphere and lower stratosphere (Ex-UTLS) in the Northern Hemisphere (NH) late summer. The Cl-VSLS measurements were obtained in the upper troposphere and lower stratosphere (UTLS) above western Europe and the midlatitude Atlantic Ocean in the frame of the WISE (Wave-driven ISentropic Exchange) aircraft campaign in autumn 2017 and are combined with the results from a three-dimensional simulation of a Lagrangian transport model as well as back-trajectory calculations. Compared to background measurements of similar age we find up to 150 % enhanced CH2Cl2 and up to 100 % enhanced CHCl3 mixing ratios in the extratropical lower stratosphere (Ex-LS). We link the measurements of enhanced CH2Cl2 and CHCl3 mixing ratios to emissions in the region of southern and eastern Asia. Transport from this area to the Ex-LS at potential temperatures in the range of 370–400 K takes about 6–11 weeks via the Asian summer monsoon anticyclone (ASMA). Our measurements suggest anthropogenic sources to be the cause of these strongly elevated Cl-VSLS concentrations observed at the top of the lowermost stratosphere (LMS). A faster transport pathway into the Ex-LS is derived from particularly low CH2Cl2 and CHCl3 mixing ratios in the UTLS. These low mixing ratios reflect weak emissions and a local seasonal minimum of both species in the boundary layer of Central America and the tropical Atlantic. We show that air masses uplifted by hurricanes, the North American monsoon, and general convection above Central America into the tropical tropopause layer to potential temperatures of about 360–370 K are transported isentropically within 5–9 weeks from the boundary layer into the Ex-LS. This transport pathway linked to the North American monsoon mainly impacts the middle and lower part of the LMS with particularly low CH2Cl2 and CHCl3 mixing ratios. In a case study, we specifically analyze air samples directly linked to the uplift by the Category 5 Hurricane Maria that occurred during October 2017 above the Atlantic Ocean. CH2Cl2 and CHCl3 have similar atmospheric sinks and lifetimes, but the fraction of biogenic emissions is clearly higher for CHCl3 than for the mainly anthropogenically emitted CH2Cl2; consequently lower CHCl3 : CH2Cl2 ratios are expected in air parcels showing a higher impact of anthropogenic emissions. The observed CHCl3 : CH2Cl2 ratio suggests clearly stronger anthropogenic emissions in the region of southern and eastern Asia compared to those in the region of Central America and the tropical Atlantic. Overall, the transport of strongly enhanced CH2Cl2 and CHCl3 mixing ratios from southern and eastern Asia via the ASMA is the main factor in increasing the chlorine loading from the analyzed VSLSs in the Ex-LS during the NH late summer. Thus, further increases in Asian CH2Cl2 and CHCl3 emissions, as frequently reported in recent years, will further increase the impact of Cl-VSLSs on stratospheric ozone depletion.

We report on measurements of total bromine (Brtot) in the upper troposphere and lower stratosphere taken during 15 flights with the German High Altitude and LOng range research aircraft (HALO). The research campaign WISE (Wave-driven ISentropic Exchange) included regions over the North Atlantic, Norwegian Sea, and northwestern Europe in fall 2017. Brtot is calculated from measured total organic bromine (Brorg) added to inorganic bromine (Bryinorg), evaluated from measured BrO and photochemical modeling. Combining these data, the weighted mean [Brtot] is 19.2±1.2 ppt in the northern hemispheric lower stratosphere (LS), in agreement with expectations for Brtot in the middle stratosphere (Engel and Rigby et al., 2018). The data reflect the expected variability in Brtot in the LS due to variable influx of shorter lived brominated source and product gases from different regions of entry. A closer look into Brorg and Bryinorg, as well as simultaneously measured transport tracers (CO and N2O) and an air mass lag time tracer (SF6), suggests that bromine-rich air masses persistently protruded into the lowermost stratosphere (LMS) in boreal summer, creating a high bromine region (HBrR). A subsection, HBrR∗, has a weighted average of [Brtot] = 20.9±0.8 ppt. The most probable source region is air recently transported from the tropical upper troposphere and tropopause layer (UT/TTL) with a weighted mean of [Brtot] = 21.6±0.7 ppt. CLaMS Lagrangian transport modeling shows that the HBrR air mass consists of 51.2 % from the tropical troposphere, 27.1 % from the stratospheric background, and 6.4 % from the midlatitude troposphere (as well as contributions from other domains). The majority of the surface air reaching the HBrR is from the Asian monsoon and its adjacent tropical regions, which greatly influences trace gas transport into the LMS in boreal summer and fall. Tropical cyclones from Central America in addition to air associated with the Asian monsoon region contribute to the elevated Brtot observed in the UT/TTL. TOMCAT global 3-D model simulations of a concurrent increase of Brtot show an associated O3 change of -2.6±0.7 % in the LS and -3.1±0.7 % near the tropopause. Our study of varying Brtot in the LS also emphasizes the need for more extensive monitoring of stratospheric Brtot globally and seasonally to fully understand its impact on LMS O3 and its radiative forcing of climate, as well as in aged air in the middle stratosphere to elucidate the stratospheric trend in bromine.

During the monsoon season of the year 2017 the airborne StratoClim mission took place in Kathmandu, Nepal, with eight mission flights of the M-55 Geophysica in the upper troposphere–lower stratosphere (UTLS) of the Asian monsoon anticyclone (AMA) over northern India, Nepal, and Bangladesh. More than 100 events of new particle formation (NPF) were observed. In total, more than 2 h of flight time was spent under NPF conditions as indicated by the abundant presence of nucleation-mode aerosols, i.e. with particle diameters dp smaller than 15 nm, which were detected in situ by means of condensation nuclei counting techniques. Mixing ratios of nucleation-mode particles (nnm) of up to ∼ 50 000 mg−1 were measured at heights of 15–16 km (θ ≈ 370 K). NPF was most frequently observed at ∼ 12–16 km altitude (θ ≈ 355–380 K) and mainly below the tropopause. Resulting nnm remained elevated (∼ 300–2000 mg−1) up to altitudes of ∼ 17.5 km (θ ≈ 400 K), while under NPF conditions the fraction (f) of sub-micrometre-sized non-volatile residues (dp > 10 nm) remained below 50 %. At ∼ 12–14 km (θ ≈ 355–365 K) the minimum of f (< 15 %) was found, and underneath, the median f generally remains below 25 %. The persistence of particles at nucleation-mode sizes is limited to a few hours, mainly due to coagulation, as demonstrated by a numerical simulation. The frequency of NPF events observed during StratoClim 2017 underlines the importance of the AMA as a source region for UTLS aerosols and for the formation and maintenance of the Asian tropopause aerosol layer (ATAL). The observed abundance of NPF-produced nucleation-mode particles within the AMA is not unambiguously attributable to (a) specific source regions in the boundary layer (according to backward trajectory analyses), or (b) the direct supply with precursor material by convective updraught (from correlations of NPF with carbon monoxide), or (c) the recent release of NPF-capable material from the convective outflow (according to air mass transport times in the tropical tropopause layer, TTL). Temperature anomalies with ΔT of 2 K (peak-to-peak amplitude), as observed at a horizontal wavelength of ∼ 70–100 km during a level flight of several hours, match with NPF detections and represent an additional mechanism for local increases in supersaturation of the NPF precursors. Effective precursor supply and widely distributed temperature anomalies within the AMA can explain the higher frequency of intense NPF observed during StratoClim 2017 than all previous NPF detections with COPAS (COndensation PArticle counting System) at TTL levels over Brazil, northern Australia, or West Africa.

This paper presents measurements of ozone, water vapour and nitric acid (HNO3) in the upper troposphere/lower stratosphere (UTLS) over North Atlantic and Europe. The measurements were acquired with the Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) during the Wave Driven Isentropic Exchange (WISE) campaign in October 2017. GLORIA is an airborne limb imager capable of acquiring both 2-D data sets (curtains along the flight path) and, when the carrier aircraft is flying around the observed air mass, spatially highly resolved 3-D tomographic data. Here, we present a case study of a Rossby wave (RW) breaking event observed during two subsequent flights 2 d apart. RW breaking is known to steepen tracer gradients and facilitate stratosphere–troposphere exchange (STE). Our measurements reveal complex spatial structures in stratospheric tracers (ozone and nitric acid) with multiple vertically stacked filaments. Backward-trajectory analysis is used to demonstrate that these features are related to several previous Rossby wave breaking events and that the small-scale structure of the UTLS in the Rossby wave breaking region, which is otherwise very hard to observe, can be understood as stirring and mixing of air masses of tropospheric and stratospheric origin. It is also shown that a strong nitric acid enhancement observed just above the tropopause is likely a result of NOx production by lightning activity. The measurements showed signatures of enhanced mixing between stratospheric and tropospheric air near the polar jet with some transport of water vapour into the stratosphere. Some of the air masses seen in 3-D data were encountered again 2 d later, stretched to very thin filament (horizontal thickness down to 30 km at some altitudes) rich in stratospheric tracers. This repeated measurement allowed us to directly observe and analyse the progress of mixing processes in a thin filament over 2 d. Our results provide direct insight into small-scale dynamics of the UTLS in the Rossby wave breaking region, which is of great importance to understanding STE and poleward transport in the UTLS.

Measurements of the pollution trace gases ethane (C2H6), ethyne (C2H2), formic acid (HCOOH), and peroxyacetyl nitrate (PAN) were performed in the North Atlantic upper troposphere and lowermost stratosphere (UTLS) region with the airborne limb imager GLORIA (Gimballed Limb Observer for Radiance Imaging of the Atmosphere) with high spatial resolution down to cloud top. Observations were made during flights with the German research aircraft HALO (High Altitude and LOng Range Research Aircraft) in the frame of the WISE (Wave-driven ISentropic Exchange) campaign, which was carried out in autumn 2017 from Shannon (Ireland) and Oberpfaffenhofen (Germany). Enhanced volume mixing ratios (VMRs) of up to 2.2 ppbv C2H6, 0.2 ppbv C2H2, 0.9 ppbv HCOOH, and 0.4 ppbv PAN were detected during the flight on 13 September 2017 in the upper troposphere and around the tropopause above the British Isles. Elevated quantities of PAN were measured even in the lowermost stratosphere (locally up to 14 km), likely reflecting the fact that this molecule has the longest lifetime of the four species discussed herein. Backward trajectory calculations as well as global three-dimensional Chemical Lagrangian Model of the Stratosphere (CLaMS) simulations with artificial tracers of air mass origin have shown that the main sources of the observed pollutant species are forest fires in North America and anthropogenic pollution in South Asia and Southeast Asia uplifted and moved within the Asian monsoon anticyclone (AMA) circulation system. After release from the AMA, these species or their precursor substances are transported by strong tropospheric winds over large distances, depending on their particular atmospheric lifetime of up to months. Observations are compared to simulations with the atmospheric models EMAC (ECHAM5/MESSy Atmospheric Chemistry) and CAMS (Copernicus Atmosphere Monitoring Service). These models are qualitatively able to reproduce the measured VMR enhancements but underestimate the absolute amount of the increase. Increasing the emissions in EMAC by a factor of 2 reduces the disagreement between simulated and measured results and illustrates the importance of the quality of emission databases used in chemical models.

The potential of heterogeneous chlorine activation in the midlatitude lowermost stratosphere during summer is a matter of debate. The occurrence of heterogeneous chlorine activation through the presence of aerosol particles could cause ozone destruction. This chemical process requires low temperatures and is accelerated by an enhancement of the stratospheric water vapour and sulfate amount. In particular, the conditions present in the lowermost stratosphere during the North American Summer Monsoon season (NAM) are expected to be cold and moist enough to cause the occurrence of heterogeneous chlorine activation. Furthermore, the temperatures, the water vapour mixing ratio and the sulfate aerosol abundance are affected by future global warming and by the potential application of sulfate geoengineering. Hence, both future scenarios could promote this ozone destruction process. We investigate the likelihood of the occurrence of heterogeneous chlorine activation and its impact on ozone in the lowermost-stratospheric mixing layer between tropospheric and stratospheric air above central North America (30.6–49.6∘ N, 72.25–124.75∘ W) in summer for conditions today, at the middle and at the end of the 21st century. Therefore, the results of the Geoengineering Large Ensemble Simulations (GLENS) for the lowermost-stratospheric mixing layer between tropospheric and stratospheric air are considered together with 10-day box-model simulations performed with the Chemical Lagrangian Model of the Stratosphere (CLaMS). In GLENS two future scenarios are simulated: the RCP8.5 global warming scenario and a geoengineering scenario, where sulfur is additionally injected into the stratosphere to keep the global mean surface temperature from changing. In the GLENS simulations, the mixing layer will warm and moisten in both future scenarios with a larger effect in the geoengineering scenario. The likelihood of chlorine activation occurring in the mixing layer is highest in the years 2040–2050 if geoengineering is applied, accounting for 3.3 %. In comparison, the likelihood of conditions today is 1.0 %. At the end of the 21st century, the likelihood of this ozone destruction process occurring decreases. We found that 0.1 % of the ozone mixing ratios in the mixing layer above central North America is destroyed for conditions today. A maximum ozone destruction of 0.3 % in the mixing layer occurs in the years 2040–2050 if geoengineering is applied. Comparing the southernmost latitude band (30–35∘ N) and the northernmost latitude band (44–49∘ N) of the considered region, we found a higher likelihood of the occurrence of heterogeneous chlorine activation in the southernmost latitude band, causing a higher impact on ozone as well. However, the ozone loss process is found to have a minor impact on the midlatitude ozone column.

A correct and reliable forecast of volcanic plume dispersion is vital for aviation safety. This can only be achieved by representing all responsible physical and chemical processes (sources, sinks, and interactions) in the forecast models. The representation of the sources has been enhanced over the last decade, while the sinks and interactions have received less attention. In particular, aerosol dynamic processes and aerosol–radiation interaction are neglected so far. Here we address this gap by further developing the ICON-ART (ICOsahedral Nonhydrostatic – Aerosols and Reactive Trace gases) global modeling system to account for these processes. We use this extended model for the simulation of volcanic aerosol dispersion after the Raikoke eruption in June 2019. Additionally, we validate the simulation results with measurements from AHI (Advanced Himawari Imager), CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization), and OMPS-LP (Ozone Mapping and Profiling Suite-Limb Profiler). Our results show that around 50 % of very fine volcanic ash mass (particles with diameter d µm) is removed due to particle growth and aging. Furthermore, the maximum volcanic cloud top height rises more than 6 km over the course of 4 d after the eruption due to aerosol–radiation interaction. This is the first direct evidence that shows how cumulative effects of aerosol dynamics and aerosol–radiation interaction lead to a more precise forecast of very fine ash lifetime in volcanic clouds.

The South Asian summer monsoon is associated with a large-scale anticyclonic circulation in the upper troposphere and lower stratosphere (UTLS), which confines the air mass inside. During boreal summer, the confinement of this air mass leads to an accumulation of aerosol between about 13 and 18 km (360 and 440 K potential temperature); this accumulation of aerosol constitutes the Asian Tropopause Aerosol Layer (ATAL). We present balloon-borne aerosol backscatter measurements of the ATAL performed by the Compact Optical Backscatter Aerosol Detector (COBALD) instrument in Nainital in northern India in August 2016, and compare these with COBALD measurements in the post-monsoon time in November 2016. The measurements demonstrate a strong variability of the ATAL's altitude, vertical extent, aerosol backscatter intensity and cirrus cloud occurrence frequency. Such a variability cannot be deduced from climatological means of the ATAL as they are derived from satellite measurements. To explain this observed variability we performed a Lagrangian back-trajectory analysis using the Chemical Lagrangian Model of the Stratosphere (CLaMS). We identify the transport pathways as well as the source regions of air parcels contributing to the ATAL over Nainital in August 2016. Our analysis reveals a variety of factors contributing to the observed day-to-day variability of the ATAL: continental convection, tropical cyclones (maritime convection), dynamics of the anticyclone and stratospheric intrusions. Thus, the air in the ATAL is a mixture of air masses coming from different atmospheric altitude layers. In addition, contributions from the model boundary layer originate in different geographic source regions. The location of the strongest updraft along the backward trajectories reveals a cluster of strong upward transport at the southern edge of the Himalayan foothills. From the top of the convective outflow level (about 13 km; 360 K) the air parcels ascend slowly to ATAL altitudes within a large-scale upward spiral driven by the diabatic heating in the anticyclonic flow of the South Asian summer monsoon at UTLS altitudes. Cases with a strong ATAL typically show boundary layer contributions from the Tibetan Plateau, the foothills of the Himalayas and other continental regions below the Asian monsoon. Weaker ATAL cases show higher contributions from the maritime boundary layer, often related to tropical cyclones, indicating a mixing of clean maritime and polluted continental air. On the one hand increasing anthropogenic emissions in the future are expected due to the strong growth of Asian economies; on the other hand the implementation of new emission control measures (in particular in China) has reduced the anthropogenic emissions of some pollutants contributing to the ATAL substantially. It needs to be monitored in the future whether the thickness and intensity of the ATAL will further increase, which will likely impact the surface climate.

This study underlines the important role of the transported black carbon (BC) mass concentration in the West African monsoon (WAM) area. BC was measured with a micro-aethalometer integrated in the payload bay of the unmanned research aircraft ALADINA (Application of Light-weight Aircraft for Detecting IN situ Aerosol). As part of the DACCIWA (Dynamics–Aerosol–Chemistry–Cloud Interactions in West Africa) project, 53 measurement flights were carried out at Savè, Benin, on 2–16 July 2016. A high variability of BC (1.79 to 2.42±0.31 µg m−3) was calculated along 155 vertical profiles that were performed below cloud base in the atmospheric boundary layer (ABL). In contrast to initial expectations of primary emissions, the vertical distribution of BC was mainly influenced by the stratification of the ABL during the WAM season. The article focuses on an event (14 and 15 July 2016) which showed distinct layers of BC in the lowermost 900 m above ground level (a.g.l.). Low concentrations of NOx and CO were sampled at the Savè supersite near the aircraft measurements and suggested a marginal impact of local sources during the case study. The lack of primary BC emissions was verified by a comparison of the measured BC with the model COSMO-ART (Consortium for Small-scale Modelling–Aerosols and Reactive Trace gases) that was applied for the field campaign period. The modelled vertical profiles of BC led to the assumption that the measured BC was already altered, as the size was mainly dominated by the accumulation mode. Further, calculated vertical transects of wind speed and BC presume that the observed BC layer was transported from the south with maritime inflow but was mixed vertically after the onset of a nocturnal low-level jet at the measurement site. This report contributes to the scope of DACCIWA by linking airborne BC data with ground observations and a model, and it illustrates the importance of a more profound understanding of the interaction between BC and the ABL in the WAM region.

Between June and September large amounts of biomass burning aerosol are released into the atmosphere from agricultural fires in central and southern Africa. Recent studies have suggested that this plume is carried westward over the Atlantic Ocean at altitudes between 2 and 4 km and then northward with the monsoon flow at low levels to increase the atmospheric aerosol load over coastal cities in southern West Africa (SWA), thereby exacerbating air pollution problems. However, the processes by which these fire emissions are transported into the planetary boundary layer (PBL) are still unclear. One potential factor is the large-scale subsidence related to the southern branch of the monsoon Hadley cell over the tropical Atlantic. Here we use convection-permitting model simulations with COSMO-ART to investigate for the first time the contribution of downward mixing induced by clouds, a process we refer to as downward cloud venting in contrast to the more common process of upward transport from a polluted PBL. Based on a monthly climatology, model simulations compare satisfactory with wind fields from reanalysis data, cloud observations, and satellite-retrieved carbon monoxide (CO) mixing ratio. For a case study on 2 July 2016, modelled clouds and rainfall show overall good agreement with Spinning Enhanced Visible and InfraRed Imager (SEVIRI) cloud products and Global Precipitation Measurement Integrated Multi-satellitE Retrievals (GPM-IMERG) rainfall estimates. However, there is a tendency for the model to produce too much clouds and rainfall over the Gulf of Guinea. Using the CO dispersion as an indicator for the biomass burning plume, we identify individual mixing events south of the coast of Côte d'Ivoire due to midlevel convective clouds injecting parts of the biomass burning plume into the PBL. Idealized tracer experiments suggest that around 15 % of the CO mass from the 2–4 km layer is mixed below 1 km within 2 d over the Gulf of Guinea and that the magnitude of the cloud venting is modulated by the underlying sea surface temperatures. There is even stronger vertical mixing when the biomass burning plume reaches land due to daytime heating and a deeper PBL. In that case, the long-range-transported biomass burning plume is mixed with local anthropogenic emissions. Future work should provide more robust statistics on the downward cloud venting effect over the Gulf of Guinea and include aspects of aerosol deposition.

Low ozone and high water vapour mixing ratios are common features in the Asian summer monsoon (ASM) anticyclone; however, low ozone and low water vapour values were observed near the tropopause over Kunming, China, within the ASM using balloon-borne measurements performed during the SWOP (sounding water vapour, ozone, and particle) campaign in August 2009 and 2015. Here, we investigate low ozone and water vapour signatures in the upper troposphere and lower stratosphere (UTLS) using FengYun-2D, FengYun-2G, and Aura Microwave Limb Sounder (MLS) satellite measurements and backward trajectory calculations. Trajectories with kinematic and diabatic vertical velocities were calculated using the Chemical Lagrangian Model of the Stratosphere (CLaMS) trajectory module driven by both ERA-Interim and ERA5 reanalysis data. All trajectory calculations show that air parcels with low ozone and low water vapour values in the UTLS over Kunming measured by balloon-borne instruments originate from the western Pacific boundary layer. Deep convection associated with tropical cyclones over the western Pacific transports ozone-poor air from the marine boundary layer to the cold tropopause region. Subsequently, these air parcels are mixed into the strong easterlies on the southern side of the Asian summer monsoon anticyclone. Air parcels are dehydrated when passing the lowest temperature region ( K) at the convective outflow of tropical cyclones. However, trajectory calculations show different vertical transport via deep convection depending on the employed reanalysis data (ERA-Interim, ERA5) and vertical velocities (diabatic, kinematic). Both the kinematic and the diabatic trajectory calculations using ERA5 data show much faster and stronger vertical transport than ERA-Interim primarily because of ERA5's better spatial and temporal resolution, which likely resolves convective events more accurately. Our findings show that the interplay between the ASM anticyclone and tropical cyclones has a significant impact on the chemical composition of the UTLS during summer.

Severe hailstorms have the potential to damage buildings and crops. However, important processes for the prediction of hailstorms are insufficiently represented in operational weather forecast models. Therefore, our goal is to identify model input parameters describing environmental conditions and cloud microphysics, such as the vertical wind shear and strength of ice multiplication, which lead to large uncertainties in the prediction of deep convective clouds and precipitation. We conduct a comprehensive sensitivity analysis simulating deep convective clouds in an idealized setup of a cloud-resolving model. We use statistical emulation and variance-based sensitivity analysis to enable a Monte Carlo sampling of the model outputs across the multi-dimensional parameter space. The results show that the model dynamical and microphysical properties are sensitive to both the environmental and microphysical uncertainties in the model. The microphysical parameters lead to larger uncertainties in the output of integrated hydrometeor mass contents and precipitation variables. In particular, the uncertainty in the fall velocities of graupel and hail account for more than 65 % of the variance of all considered precipitation variables and for 30 %–90 % of the variance of the integrated hydrometeor mass contents. In contrast, variations in the environmental parameters – the range of which is limited to represent model uncertainty – mainly affect the vertical profiles of the diabatic heating rates.

Vast stretches of agricultural land in southern and central Africa are burnt between June and September each year, which releases large quantities of aerosol into the atmosphere. The resulting smoke plumes are carried west over the Atlantic Ocean at altitudes between 2 and 4 km. As only limited observational data in West Africa have existed until now, whether this pollution has an impact at lower altitudes has remained unclear. The Dynamics-aerosol-chemistry-cloud interactions in West Africa (DACCIWA) aircraft campaign took place in southern West Africa during June and July 2016, with the aim of observing gas and aerosol properties in the region in order to assess anthropogenic and other influences on the atmosphere. Results presented here show that a significant mass of aged accumulation mode aerosol was present in the southern West African monsoon layer, over both the ocean and the continent. A median dry aerosol concentration of 6.2 µg m−3 (standard temperature and pressure, STP) was observed over the Atlantic Ocean upwind of the major cities, with an interquartile range from 5.3 to 8.0 µg m−3. This concentration increased to a median of 11.1 µg m−3 (8.6 to 15.7 µg m−3) in the immediate outflow from cities. In the continental air mass away from the cities, the median aerosol loading was 7.5 µg m−3 (5.9 to 10.5 µg m−3). The accumulation mode aerosol population over land displayed similar chemical properties to the upstream population, which implies that upstream aerosol is a significant source of aerosol pollution over the continent. The upstream aerosol is found to have most likely originated from central and southern African biomass burning. This demonstrates that biomass burning plumes are being advected northwards, after being entrained into the monsoon layer over the eastern tropical Atlantic Ocean. It is shown observationally for the first time that they contribute up to 80 % to the regional aerosol loading in the monsoon layer over southern West Africa. Results from the COSMO-ART (Consortium for Small-scale Modeling – Aerosol and Reactive Trace gases) and GEOS-Chem models support this conclusion, showing that observed aerosol concentrations over the northern Atlantic Ocean can only be reproduced when the contribution of transported biomass burning aerosol is taken into account. As a result, the large and growing emissions from the coastal cities are overlaid on an already substantial aerosol background. Simulations using COSMO-ART show that cloud droplet number concentrations can increase by up to 27 % as a result of transported biomass burning aerosol. On a regional scale this renders cloud properties and precipitation less sensitive to future increases in anthropogenic emissions. In addition, such high background loadings will lead to greater pollution exposure for the large and growing population in southern West Africa. These results emphasise the importance of including aerosol from across country borders in the development of air pollution policies and interventions in regions such as West Africa.

We conducted a 6-week measurement campaign in summer 2016 at a rural site about 11 km north of the city of Karlsruhe in southwest Germany in order to study the chemical composition and origin of aerosols in the upper Rhine valley. In particular, we deployed a single-particle mass spectrometer (LAAPTOF) and an aerosol mass spectrometer (AMS) to provide complementary chemical information on aerosol particles smaller than 2.5 µm. For the entire measurement period, the total aerosol particle mass was dominated by sodium salts, contributing on average (36±27) % to the total single particles measured by the LAAPTOF. The total particulate organic compounds, sulfate, nitrate, and ammonium contributed on average (58±12) %, (22±7) %, (10±1) %, and (9±3) % to the total non-refractory particle mass measured by the AMS. Positive matrix factorization (PMF) analysis for the AMS data suggests that the total organic aerosol (OA) consisted of five components, including (9±7) % hydrocarbon-like OA (HOA), (16±11) % semi-volatile oxygenated OA (SV-OOA), and (75±15) % low-volatility oxygenated OA (LV-OOA). The regional transport model COSMO-ART was applied for source apportionment and to achieve a better understanding of the impact of complex transport patterns on the field observations. Combining field observations and model simulations, we attributed high particle numbers and SO2 concentrations observed at this rural site to industrial emissions from power plants and a refinery in Karlsruhe. In addition, two characteristic episodes with aerosol particle mass dominated by sodium salts particles comprising (70±24) % of the total single particles and organic compounds accounting for (77±6) % of total non-refractory species, respectively, were investigated in detail. For the first episode, we identified relatively fresh and aged sea salt particles originating from the Atlantic Ocean more than 800 km away. These particles showed markers like m∕z 129 C5H7NO3+, indicating the influence of anthropogenic emissions modifying their composition, e.g. from chloride to nitrate salts during the long-range transport. For a 3 d episode including high organic mass concentrations, model simulations show that on average (74±7) % of the particulate organics at this site were of biogenic origin. Detailed model analysis allowed us to find out that three subsequent peaks of high organic mass concentrations originated from different sources, including local emissions from the city and industrial area of Karlsruhe, regional transport from the city of Stuttgart (∼64 km away), and potential local night-time formation and growth. Biogenic (forest) and anthropogenic (urban) emissions were mixed during transport and contributed to the formation of organic particles. In addition, topography, temperature inversion, and stagnant meteorological conditions also played a role in the build-up of higher organic particle mass concentrations. Furthermore, the model was evaluated using field observations and corresponding sensitivity tests. The model results show good agreement with trends and concentrations observed for several trace gases (e.g. O3, NO2, and SO2) and aerosol particle compounds (e.g. ammonium and nitrate). However, the model underestimates the number of particles by an order of magnitude and underestimates the mass of organic particles by a factor of 2.3. The discrepancy was expected for particle number since the model does not include all nucleation processes. The missing organic mass indicates either an underestimated regional background or missing sources and/or mechanisms in the model, like night-time chemistry. This study demonstrates the potential of combining comprehensive field observations with dedicated transport modelling to understand the chemical composition and complex origin of aerosols.

Water vapour convectively injected into the mid-latitude lowermost stratosphere could affect stratospheric ozone. The associated potential ozone loss process requires low temperatures together with elevated water vapour mixing ratios. Since this ozone loss is initiated by heterogeneous chlorine activation on liquid aerosols, an increase in sulfate aerosol surface area due to a volcanic eruption or geoengineering could increase the likelihood of its occurrence. However, the chemical mechanism of this ozone loss process has not yet been analysed in sufficient detail and its sensitivity to various conditions is not yet clear. Under conditions of climate change associated with an increase in greenhouse gases, both a stratospheric cooling and an increase in water vapour convectively injected into the stratosphere are expected. Understanding the influence of low temperatures, elevated water vapour and enhanced sulfate particles on this ozone loss mechanism is a key step in estimating the impact of climate change and potential sulfate geoengineering on mid-latitude ozone. Here, we analyse the ozone loss mechanism and its sensitivity to various stratospheric conditions in detail. By conducting a box-model study with the Chemical Lagrangian Model of the Stratosphere (CLaMS), chemistry was simulated along a 7 d backward trajectory. This trajectory was calculated neglecting mixing of neighbouring air masses. Chemical simulations were initialized using measurements taken during the Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) aircraft campaign (2013, Texas), which encountered an elevated water vapour mixing ratio of 10.6 ppmv at a pressure level around 100 hPa. We present a detailed analysis of the ozone loss mechanism, including the chlorine activation, chlorine-catalysed ozone loss cycles, maintenance of activated chlorine and the role of active nitrogen oxide radicals (NOx). Focussing on a realistic trajectory in a temperature range from 197 to 202 K, a threshold in water vapour of 10.6 ppmv has to be exceeded and maintained for stratospheric ozone loss to occur. We investigated the sensitivity of the water vapour threshold to temperature, sulfate content, inorganic chlorine (Cly), inorganic nitrogen (NOy) and inorganic bromine (Bry). The water vapour threshold is mainly determined by the temperature and sulfate content. However, the amount of ozone loss depends on Cly, Bry and the duration of the time period over which chlorine activation can be maintained. NOy affects both the potential of ozone formation and the balance between reactions yielding chlorine activation and deactivation, which determines the water vapour threshold. Our results show that in order to deplete ozone, a chlorine activation time of 24 to 36 h for conditions of the water vapour threshold with low temperatures must be maintained. A maximum ozone loss of 9 % was found for a 20 ppmv water vapour mixing ratio using North American Monsoon (NAM) tropopause standard conditions with a chemical box-model simulation along a realistic trajectory. For the same trajectory, using observed conditions (of 10.6 ppmv H2O), the occurrence of simulated ozone loss was dependent on the sulfate amount assumed. Detailed analysis of current and future possibilities is needed to assess whether enhanced water vapour conditions in the summertime mid-latitude lower stratosphere lead to significant ozone loss.

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  months) at the top of the Asian monsoon anticyclone and of air masses within the tropical pipe (6 months < age  months) during summer 2008. The occurrence of young air masses ( 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 European Centre for Medium-Range Weather Forecasts' (ECMWF's) next-generation reanalysis ERA5 provides many improvements, but it also confronts the community with a “big data” challenge. Data storage requirements for ERA5 increase by a factor of ∼80 compared with the ERA-Interim reanalysis, introduced a decade ago. Considering the significant increase in resources required for working with the new ERA5 data set, it is important to assess its impact on Lagrangian transport simulations. To quantify the differences between transport simulations using ERA5 and ERA-Interim data, we analyzed comprehensive global sets of 10-day forward trajectories for the free troposphere and the stratosphere for the year 2017. The new ERA5 data have a considerable impact on the simulations. Spatial transport deviations between ERA5 and ERA-Interim trajectories are up to an order of magnitude larger than those caused by parameterized diffusion and subgrid-scale wind fluctuations after 1 day and still up to a factor of 2–3 larger after 10 days. Depending on the height range, the spatial differences between the trajectories map into deviations as large as 3 K in temperature, 30 % in specific humidity, 1.8 % in potential temperature, and 50 % in potential vorticity after 1 day. Part of the differences between ERA5 and ERA-Interim is attributed to the better spatial and temporal resolution of the ERA5 reanalysis, which allows for a better representation of convective updrafts, gravity waves, tropical cyclones, and other meso- to synoptic-scale features of the atmosphere. Another important finding is that ERA5 trajectories exhibit significantly improved conservation of potential temperature in the stratosphere, pointing to an improved consistency of ECMWF's forecast model and observations that leads to smaller data assimilation increments. We conducted a number of downsampling experiments with the ERA5 data, in which we reduced the numbers of meteorological time steps, vertical levels, and horizontal grid points. Significant differences remain present in the transport simulations, if we downsample the ERA5 data to a resolution similar to ERA-Interim. This points to substantial changes of the forecast model, observations, and assimilation system of ERA5 in addition to improved resolution. A comparison of two Lagrangian trajectory models allowed us to assess the readiness of the codes and workflows to handle the comprehensive ERA5 data and to demonstrate the consistency of the simulation results. Our results will help to guide future Lagrangian transport studies attempting to navigate the increased computational complexity and leverage the considerable benefits and improvements of ECMWF's new ERA5 data set.

Water in the atmosphere can exist in the solid, liquid or gas phase. At high humidities, if the aerosol population remains constant, more water vapour will condense onto the particles and cause them to swell, sometimes up to several times their original size. This significant change in size and chemical composition is termed hygroscopic growth and alters a particle's optical properties. Even in unsaturated conditions, this can change the aerosol direct effect, for example by increasing the extinction of incoming sunlight. This can have an impact on a region's energy balance and affect visibility. Here, aerosol and relative humidity measurements collected from aircraft and radiosondes during the Dynamics–Aerosol–Chemistry–Cloud Interactions in West Africa (DACCIWA) campaign were used to estimate the effect of highly humid layers of air on aerosol optical properties during the monsoon season in southern West Africa. The effects of hygroscopic growth in this region are of particular interest due to the regular occurrence of high humidity and the high levels of pollution in the region. The Zdanovskii, Stokes and Robinson (ZSR) mixing rule is used to estimate the hygroscopic growth of particles under different conditions based on chemical composition. These results are used to estimate the aerosol optical depth (AOD) at λ=525 nm for 63 relative humidity profiles. The median AOD in the region from these calculations was 0.36, the same as that measured by sun photometers at the ground site. The spread in the calculated AODs was less than the spread from the sun photometer measurements. In both cases, values above 0.5 were seen predominantly in the mornings and corresponded with high humidities. Observations of modest variations in aerosol load and composition are unable to explain the high and variable AODs observed using sun photometers, which can only be recreated by accounting for the very elevated and variable relative humidities (RHs) in the boundary layer. Most importantly, the highest AODs present in the mornings are not possible without the presence of high RH in excess of 95 %. Humid layers are found to have the most significant impact on AOD when they reach RH greater than 98 %, which can result in a wet AOD more than 1.8 times the dry AOD. Unsaturated humid layers were found to reach these high levels of RH in 37 % of observed cases. It can therefore be concluded that the high AODs present across the region are driven by the high humidities and are then moderated by changes in aerosol abundance. Aerosol concentrations in southern West Africa are projected to increase substantially in the coming years; results presented here show that the presence of highly humid layers in the region is likely to enhance the consequent effect on AOD significantly.

Balloon-borne measurements of ozone in Lhasa (29.66∘ N, 91.14∘ E; 3650 m above sea level) in August 2013 are investigated using backward trajectory calculations performed with the Chemical Lagrangian Model of the Stratosphere (CLaMS). Measurements show three time periods characterized by high ozone mixing ratios (OMRs) in the troposphere on 8, 11, and 18–20 August 2013 during the Asian summer monsoon (ASM) season. Here, we verified two different sources for the enhanced ozone values in the troposphere. First, transport of polluted air from the boundary layer, and second downward transport from the stratosphere by stratospheric intrusions. Air pollution from South Asia through convective and long-range transport plays a key role in enhancing middle tropospheric OMRs up to 90 % on 8 August and up to 125 % on 11 August 2013 compared to monthly mean ozone of August 2013. Stratospheric air intruded from the northern high-latitudes to the southeastern flank of the ASM anticyclone to the troposphere and is identified as the source of enhanced ozone according to backward trajectory calculation and satellite measurements by the Ozone Monitoring Instrument (OMI) and the Atmospheric Infrared Sounder (AIRS). Air parcels with high ozone moved from the high-latitude lower stratosphere to the middle and upper troposphere. These air parcels are then transported to Lhasa over long distances and enhanced upper and middle tropospheric ozone over Lhasa during 18–20 August 2013. Our findings demonstrate that the strong variability of ozone within the ASM anticyclone in the free troposphere is caused by transport from very different regions of the atmosphere.

Background: The Global Anticoagulant Registry in the FIELD–Atrial Fibrillation (GARFIELD-AF) is an ongoing prospective noninterventional registry, which is providing important information on the baseline characteristics, treatment patterns, and 1-year outcomes in patients with newly diagnosed non-valvular atrial fibrillation (NVAF). This report describes data from Indian patients recruited in this registry. Methods and results: A total of 52,014 patients with newly diagnosed AF were enrolled globally; of these, 1388 patients were recruited from 26 sites within India (2012–2016). In India, the mean age was 65.8 years at diagnosis of NVAF. Hypertension was the most prevalent risk factor for AF, present in 68.5% of patients from India and in 76.3% of patients globally (P

Water uptake can significantly increase the size and therefore alters the optical properties of aerosols. In this study, the regional-scale model framework COSMO-ART is applied to southern West Africa (SWA) for a summer monsoon process study on 2–3 and 6–7 July 2016. The high moisture and aerosol burden in the monsoon layer makes SWA favorable to quantify properties that determine the aerosol liquid water content and its impact on radiative transfer. Given the marked diurnal cycle in SWA, the analysis is separated into three characteristic phases: (a) the Atlantic inflow progression phase (15:00–02:00 UTC), when winds from the Gulf of Guinea accelerate in the less turbulent evening and nighttime boundary layer, (b) the moist morning phase (03:00–08:00 UTC), when the passage of the Atlantic inflow front leads to overall cool and moist conditions over land, and (c) the daytime drying phase (09:00–15:00 UTC), in which the Atlantic inflow front reestablishes with the inland heating initiated after sunrise. This diurnal cycle also impacts, via relative humidity, the aerosol liquid water content. We analyzed the impact of relative humidity and clouds on the aerosol liquid water content. As shown by other studies, accumulation-mode particles are the dominant contributor of aerosol liquid water. We find aerosol growth factors of 2 (4) for submicron (coarse-mode) particles, leading to a substantial increase in mean aerosol optical depth from 0.2 to 0.7. Considering the aerosol liquid water content leads to a decrease in shortwave radiation of about 20 W m−2, while longwave effects appear to be insignificant, especially during nighttime. The estimated relationships between total column aerosol liquid water and radiation are −305±39 W g−1 (shortwave in-cloud), −114±42 W g−1 (shortwave off-cloud) and about −10 W g−1 (longwave). The results highlight the need to consider the relative humidity dependency of aerosol optical depth in atmospheric models, particularly in moist tropical environments where their effect on radiation can be very large.

Atmospheric composition studies on weather and climate timescales require flexible, scalable models. The ICOsahedral Nonhydrostatic model with Aerosols and Reactive Trace gases (ICON-ART) provides such an environment. Here, we introduce the most up-to-date version of the flexible tracer framework for ICON-ART and explain its application in one numerical weather forecast and one climate related case study. We demonstrate the implementation of idealised tracers and chemistry tendencies of different complexity using the ART infrastructure. Using different ICON physics configurations for weather and climate with ART, we perform integrations on different timescales, illustrating the model's performance. First, we present a hindcast experiment for the 2002 ozone hole split with two different ozone chemistry schemes using the numerical weather prediction physics configuration. We compare the hindcast with observations and discuss the confinement of the vortex split using an idealised tracer diagnostic. Secondly, we study AMIP-type integrations using a simplified chemistry scheme in conjunction with the climate physics configuration. We use two different simulations: the interactive simulation, where modelled ozone is coupled back to the radiation scheme, and the non-interactive simulation that uses a default background climatology of ozone. Additionally, we introduce changes of water vapour by methane oxidation for the interactive simulation. We discuss the impact of stratospheric ozone and water vapour variations in the interactive and non-interactive integrations on the water vapour tape recorder, as a measure of tropical upwelling changes. Additionally we explain the seasonal evolution and latitudinal distribution of the age of air. The age of air is a measure of the strength of the meridional overturning circulation with young air in the tropical upwelling region and older air in polar winter downwelling regions. We conclude that our flexible tracer framework allows for tailor-made configurations of ICON-ART in weather and climate applications that are easy to configure and run well.

Southern West Africa (SWA) is undergoing rapid and significant socioeconomic changes associated with a massive increase in air pollution. Still, the impact of atmospheric pollutants, in particular that of aerosol particles, on weather and climate in this region is virtually unexplored. In this study, the regional-scale model framework COSMO-ART is applied to SWA for a summer monsoon process study on 2–3 July 2016 to assess the aerosol direct and indirect effect on clouds and atmospheric dynamics. The modeling study is supported by observational data obtained during the extensive field campaign of the project DACCIWA (Dynamics–Aerosol–Chemistry–Cloud Interactions in West Africa) in June–July 2016. As indicated in previous studies, a coastal front is observed that develops during daytime and propagates inland in the evening (Atlantic inflow). Increasing the aerosol amount in COSMO-ART leads to reduced propagation velocities with frontal displacements of 10–30 km and a weakening of the nocturnal low-level jet. This is related to a subtle balance of processes related to the decrease in near-surface heating: (1) flow deceleration due to reduced land–sea temperature contrast and thus local pressure gradient, (2) reduced turbulence favoring frontal advance inland and (3) delayed stratus-to-cumulus transition of 1–2 h via a later onset of the convective boundary layer. The spatial shift of the Atlantic inflow and the temporal shift of the stratus-to-cumulus transition are synergized in a new conceptual model. We hypothesize a negative feedback of the stratus-to-cumulus transition on the Atlantic inflow with increased aerosol. The results exhibit radiation as the key player governing the aerosol affects on SWA atmospheric dynamics via the aerosol direct effect and the Twomey effect, whereas impacts on precipitation are small.

A high-resolution regional-scale numerical model was extended by a parameterization that allows for both the generation and the life cycle of contrails and contrail cirrus to be calculated. The life cycle of contrails and contrail cirrus is described by a two-moment cloud microphysical scheme that was extended by a separate contrail ice class for a better representation of the high concentration of small ice crystals that occur in contrails. The basic input data set contains the spatially and temporally highly resolved flight trajectories over Central Europe derived from real-time data. The parameterization provides aircraft-dependent source terms for contrail ice mass and number. A case study was performed to investigate the influence of contrails and contrail cirrus on the shortwave radiative fluxes at the earth's surface. Accounting for contrails produced by aircraft enabled the model to simulate high clouds that were otherwise missing on this day. The effect of these extra clouds was to reduce the incoming shortwave radiation at the surface as well as the production of photovoltaic power by up to 10 %.

The impact of air masses originating in Asia and influenced by the Asian monsoon anticyclone on the Northern Hemisphere stratosphere is investigated based on in situ measurements. A statistically significant increase in water vapor (H2O) of about 0.5 ppmv (11 %) and methane (CH4) of up to 20 ppbv (1.2 %) in the extratropical stratosphere above a potential temperature of 380 K was detected between August and September 2012 during the HALO aircraft missions Transport and Composition in the UT/LMS (TACTS) and Earth System Model Validation (ESMVal). We investigate the origin of the increased water vapor and methane using the three-dimensional Chemical Lagrangian Model of the Stratosphere (CLaMS). We assign the source of the moist air masses in the Asian region (northern and southern India, eastern China, southeast Asia, and the tropical Pacific) based on tracers of air mass origin used in CLaMS. The water vapor increase is correlated with an increase of the simulated Asian monsoon air mass contribution from about 10 % in August to about 20 % in September, which corresponds to a doubling of the influence from the Asian monsoon region. Additionally, back trajectories starting at the aircraft flight paths are used to differentiate transport from the Asian monsoon anticyclone and other source regions by calculating the Lagrangian cold point (LCP). The geographic location of the LCPs, which indicates the region where the set point of water vapor mixing ratio along these trajectories occurs, can be predominantly attributed to the Asian monsoon region.

The importance for reliable forecasts of incoming solar radiation is growing rapidly, especially for those countries with an increasing share in photovoltaic (PV) power production. The reliability of solar radiation forecasts depends mainly on the representation of clouds and aerosol particles absorbing and scattering radiation. Especially under extreme aerosol conditions, numerical weather prediction has a systematic bias in the solar radiation forecast. This is caused by the design of numerical weather prediction models, which typically account for the direct impact of aerosol particles on radiation using climatological mean values and the impact on cloud formation assuming spatially and temporally homogeneous aerosol concentrations. These model deficiencies in turn can lead to significant economic losses under extreme aerosol conditions. For Germany, Saharan dust outbreaks occurring 5 to 15 times per year for several days each are prominent examples for conditions, under which numerical weather prediction struggles to forecast solar radiation adequately. We investigate the impact of mineral dust on the PV-power generation during a Saharan dust outbreak over Germany on 4 April 2014 using ICON-ART, which is the current German numerical weather prediction model extended by modules accounting for trace substances and related feedback processes. We find an overall improvement of the PV-power forecast for 65 % of the pyranometer stations in Germany. Of the nine stations with very high differences between forecast and measurement, eight stations show an improvement. Furthermore, we quantify the direct radiative effects and indirect radiative effects of mineral dust. For our study, direct effects account for 64 %, indirect effects for 20 % and synergistic interaction effects for 16 % of the differences between the forecast including mineral dust radiative effects and the forecast neglecting mineral dust.

In September 2015 one of the severest and most unusual dust events on record occurred in the Eastern Mediterranean. Surprisingly, operational dust transport models were unable to forecast the event. This study details the reasons for this failure and presents simulations of the event at convection-permitting resolution using the modelling system ICON-ART. The results allow for an in-depth analysis of the influence of the synoptic situation, the complex interaction of multiple driving atmospheric systems and the mineral dust radiative effect on the dust event. A comparison of the results with observations reveals the quality of the simulation results with respect to structure and timing of the dust transport. The forecast of the dust event is improved decisively. The event is triggered by the unusually early occurrence of an active Red Sea trough situation with an easterly axis over Mesopotamia. The connected sustained organized mesoscale convection produces multiple cold-pool outflows responsible for intense dust emissions. Complexity is added by the interaction with an intense heat low, the inland-penetrating Eastern Mediterranean sea breeze and the widespread occurrence of supercritical flow conditions and subsequent hydraulic jumps in the vicinity of the Dead Sea Rift Valley. The newly implemented mineral dust radiation interaction leads to systematically more intense and faster propagating cold-pool outflows.

For the past 8 years, Greece has been experiencing a major financial crisis which, among other side effects, has led to a shift in the fuel used for residential heating from fossil fuel towards biofuels, primarily wood. This study simulates the fate of the residential wood burning aerosol plume (RWB smog) and the implications on atmospheric chemistry and radiation, with the support of detailed aerosol characterization from measurements during the winter of 2013–2014 in Athens. The applied model system (TNO-MACC_II emissions and COSMO-ART model) and configuration used reproduces the measured frequent nighttime aerosol spikes (hourly PM10 > 75 µg m−3) and their chemical profile (carbonaceous components and ratios). Updated temporal and chemical RWB emission profiles, derived from measurements, were used, while the level of the model performance was tested for different heating demand (HD) conditions, resulting in better agreement with measurements for Tmin −2 at the surface), followed by a minor feedback to the concentration levels of aerosol species. The low radiative cooling of a period with such intense air pollution conditions is attributed to the timing of the smog plume appearance, both directly (longwave radiation increases during nighttime) and indirectly (the mild effect of the residual plume on solar radiation during the next day, due to removal and dispersion processes).

The complexity of atmospheric aerosol causes large uncertainties in its parameterization in atmospheric models. In a process-based comparison of two aerosol and chemistry schemes within the regional atmospheric modeling framework COSMO-ART (Consortium for Small-Scale Modelling, Aersosol and Reactive Trace gases extension), we identify key sensitivities of aerosol parameterizations. We consider the aerosol module MADE (Modal Aerosol Dynamics model for Europe) in combination with full gas-phase chemistry and the aerosol module M7 in combination with a constant-oxidant-field-based sulfur cycle. For a Saharan dust outbreak reaching Europe, modeled aerosol populations are more sensitive to structural differences between the schemes, in particular the consideration of aqueous-phase sulfate production, the selection of aerosol species and modes, and modal composition, than to parametric choices like modal standard deviation and the parameterization of aerosol dynamics. The same observation applies to aerosol optical depth (AOD) and the concentrations of cloud condensation nuclei (CCN). Differences in the concentrations of ice-nucleating particles (INPs) are masked by uncertainties between two ice-nucleation parameterizations and their coupling to the aerosol scheme. Differences in cloud droplet and ice crystal number concentrations are buffered by cloud microphysics as we show in a susceptibility analysis.

We present a recently developed emission module for the ICON (ICOsahedral Non-hydrostatic)-ART (Aerosols and Reactive Trace gases) modelling framework. The emission module processes external flux data sets and increments the tracer volume mixing ratios in the boundary layer accordingly. The performance of the emission module is illustrated with simulations of acetone, using a simplified chemical depletion mechanism based on a reaction with OH and photolysis only. In our model setup, we calculate a tropospheric acetone lifetime of 33 days, which is in good agreement with the literature. We compare our results with ground-based as well as with airborne IAGOS-CARIBIC measurements in the upper troposphere and lowermost stratosphere (UTLS) in terms of phase and amplitude of the annual cycle. In all our ICON-ART simulations the general seasonal variability is well represented but uncertainties remain concerning the magnitude of the acetone mixing ratio in the UTLS region. In addition, the module for online calculations of biogenic emissions (MEGAN2.1) is implemented in ICON-ART and can replace the offline biogenic emission data sets. In a sensitivity study we show how different parametrisations of the leaf area index (LAI) change the emission fluxes calculated by MEGAN2.1 and demonstrate the importance of an adequate treatment of the LAI within MEGAN2.1. We conclude that the emission module performs well with offline and online emission fluxes and allows the simulation of the annual cycles of emissions-dominated substances.

In the frame of the SWOP (sounding water vapour, ozone, and particle) campaign during the Asian summer monsoon (ASM), ozone and water vapour profiles were measured by balloon-borne sensors launched from Lhasa (29.66° N, 91.14° E, elevation 3650 m), China, in August 2013. In total, 24 soundings were launched, nearly half of which show strong variations in the relationship between ozone and water vapour in the tracer–tracer correlation in the upper troposphere and lower stratosphere (UTLS). For each sounding, 20-day backward trajectories were calculated using the trajectory module of the Chemical Lagrangian Model of the Stratosphere (CLaMS) to analyse these variations. The trajectory calculations demonstrate that three tropical cyclones (tropical storm Jebi, typhoons Utor and Trami), which occurred over the western Pacific Ocean during August 2013, had a considerable impact on the vertical distribution of ozone and water vapour by uplifting marine air masses to altitudes of the ASM anticyclone. Air parcels subsequently arrived at the observation site via two primary pathways: firstly via direct horizontal transport from the location of the typhoon to the station within approximately 3 days, and secondly via transport following the clockwise wind flow of the ASM within a timescale of 1 week. Furthermore, the interplay between the spatial position of the ASM anticyclone and tropical cyclones plays a key role in controlling the transport pathways of air parcels from the boundary layer of the western Pacific to Lhasa in horizontal and vertical transport. Moreover, the statistical analysis shows that the strongest impact by typhoons is found at altitudes between 14.5 and 17 km (365–375 K). Low ozone values (50–80 ppbv) were observed between 370 and 380 K due to the strong vertical transport within tropical cyclones.

A new gas-flaring emission parameterization has been developed, which combines remote sensing observations using Visible Infrared Imaging Radiometer Suite (VIIRS) nighttime data with combustion equations. The parameterization has been applied to southern West Africa, including the Niger Delta as a region that is highly exposed to gas flaring. Two 2-month datasets for June–July 2014 and 2015 were created. The parameterization delivers emissions of CO, CO2, NO, NO2 and SO2. A flaring climatology for both time periods has been derived. The uncertainties owing to cloud cover, parameter selection, natural gas composition and the interannual differences are assessed. The largest uncertainties in the emission estimation are linked to the parameter selection. It can be shown that the flaring emissions in Nigeria have significantly decreased by 25 % from 2014 to 2015. Existing emission inventories were used for validation. CO2 emissions with the estimated uncertainty in parentheses of 2.7 (3. 6∕0. 5) Tg yr−1 for 2014 and 2.0 (2. 7∕0. 4) Tg yr−1 for 2015 were derived. Regarding the uncertainty range, the emission estimate is in the same order of magnitude compared to existing emission inventories with a tendency for underestimation. The deviations might be attributed to a shortage in information about the combustion efficiency within southern West Africa, the decreasing trend in gas flaring or inconsistent emission sector definitions. The parameterization source code is available as a package of R scripts.

Global simulations with the Chemical Lagrangian Model of the Stratosphere (CLaMS) using artificial tracers of air mass origin are used to analyze transport mechanisms from the Asian monsoon region into the lower stratosphere. In a case study, the transport of air masses from the Asian monsoon anticyclone originating in India/China by an eastward-migrating anticyclone which broke off from the main anticyclone on 20 September 2012 and filaments separated at the northeastern flank of the anticyclone are analyzed. Enhanced contributions of young air masses (younger than 5 months) are found within the separated anticyclone confined at the top by the thermal tropopause. Further, these air masses are confined by the anticyclonic circulation and, on the polar side, by the subtropical jet such that the vertical structure resembles a bubble within the upper troposphere. Subsequently, these air masses are transported eastwards along the subtropical jet and enter the lower stratosphere by quasi-horizontal transport in a region of double tropopauses most likely associated with Rossby wave breaking events. As a result, thin filaments with enhanced signatures of tropospheric trace gases were measured in the lower stratosphere over Europe during the TACTS/ESMVal campaign in September 2012 in very good agreement with CLaMS simulations. Our simulations demonstrate that source regions in Asia and in the Pacific Ocean have a significant impact on the chemical composition of the lower stratosphere of the Northern Hemisphere. Young, moist air masses, in particular at the end of the monsoon season in September/October 2012, flooded the extratropical lower stratosphere in the Northern Hemisphere with contributions of up to ≈ 30 % at 380 K (with the remaining fraction being aged air). In contrast, the contribution of young air masses to the Southern Hemisphere is much lower. At the end of October 2012, approximately 1.5 ppmv H2O is found in the lower Northern Hemisphere stratosphere (at 380 K) from source regions both in Asia and in the tropical Pacific compared to a mean water vapor content of ≈ 5 ppmv. In addition to this main transport pathway from the Asian monsoon anticyclone to the east along the subtropical jet and subsequent transport into the northern lower stratosphere, a second horizontal transport pathway out of the anticyclone to the west into the tropics (TTL) is found in agreement with MIPAS HCFC-22 measurements.

Both climate forcing and climate sensitivity persist as stubborn uncertainties limiting the extent to which climate models can provide actionable scientific scenarios for climate change. A key, explicit control on cloud–aerosol interactions, the largest uncertainty in climate forcing, is the vertical velocity of cloud-scale updrafts. Model-based studies of climate sensitivity indicate that convective entrainment, which is closely related to updraft speeds, is an important control on climate sensitivity. Updraft vertical velocities also drive many physical processes essential to numerical weather prediction.Vertical velocities and their role in atmospheric physical processes have been given very limited attention in models for climate and numerical weather prediction. The relevant physical scales range down to tens of meters and are thus frequently sub-grid and require parameterization. Many state-of-science convection parameterizations provide mass fluxes without specifying vertical velocities, and parameterizations that do provide vertical velocities have been subject to limited evaluation against what have until recently been scant observations. Atmospheric observations imply that the distribution of vertical velocities depends on the areas over which the vertical velocities are averaged. Distributions of vertical velocities in climate models may capture this behavior, but it has not been accounted for when parameterizing cloud and precipitation processes in current models.New observations of convective vertical velocities offer a potentially promising path toward developing process-level cloud models and parameterizations for climate and numerical weather prediction. Taking account of the scale dependence of resolved vertical velocities offers a path to matching cloud-scale physical processes and their driving dynamics more realistically, with a prospect of reduced uncertainty in both climate forcing and sensitivity.

The transport of air masses originating from the Asian monsoon anticyclone into the extratropical upper troposphere and lower stratosphere (Ex-UTLS) above potential temperatures Θ = 380 K was identified during the HALO aircraft mission TACTS in August and September 2012. In situ measurements of CO, O3 and N2O during TACTS flight 2 on 30 August 2012 show the irreversible mixing of aged stratospheric air masses with younger (recently transported from the troposphere) ones within the Ex-UTLS. Backward trajectories calculated with the trajectory module of CLaMS indicate that these tropospherically affected air masses originate from the Asian monsoon anticyclone. These air masses are subsequently transported above potential temperatures Θ = 380 K from the monsoon circulation region into the Ex-UTLS, where they subsequently mix with stratospheric air masses. The overall trace gas distribution measured during TACTS shows that this transport pathway had affected the chemical composition of the Ex-UTLS during boreal summer and autumn 2012. This leads to an intensification of the tropospheric influence on the extratropical lower stratosphere with PV > 8 pvu within 3 weeks during the TACTS mission. During the same time period a weakening of the tropospheric influence on the lowermost stratosphere (LMS) is determined. The study shows that the transport of air masses originating from the Asian summer monsoon region within the lower stratosphere affects the change in the chemical composition of the Ex-UTLS over Europe and thus contributes to the flushing of the LMS during summer 2012.

We quantified the effects of the plume rise of biomass burning aerosol and gases for the forest fires that occurred in Saskatchewan, Canada, in July 2010. For this purpose, simulations with different assumptions regarding the plume rise and the vertical distribution of the emissions were conducted. Based on comparisons with observations, applying a one-dimensional plume rise model to predict the injection layer in combination with a parametrization of the vertical distribution of the emissions outperforms approaches in which the plume heights are initially predefined. Approximately 30 % of the fires exceed the height of 2 km with a maximum height of 8.6 km. Using this plume rise model, comparisons with satellite images in the visible spectral range show a very good agreement between the simulated and observed spatial distributions of the biomass burning plume. The simulated aerosol optical depth (AOD) with data of an AERONET station is in good agreement with respect to the absolute values and the timing of the maximum. Comparison of the vertical distribution of the biomass burning aerosol with CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation) retrievals also showed the best agreement when the plume rise model was applied. We found that downwelling surface short-wave radiation below the forest fire plume is reduced by up to 50 % and that the 2 m temperature is decreased by up to 6 K. In addition, we simulated a strong change in atmospheric stability within the biomass burning plume.

This paper presents an analysis of trace gases in the Asian summer monsoon (ASM) region on the basis of observations by the CRISTA infrared limb sounder taken in low-earth orbit in August 1997. The spatially highly resolved measurements of peroxyacetyl nitrate (PAN) and O3 allow a detailed analysis of an eddy-shedding event of the ASM anticyclone. We identify enhanced PAN volume mixing ratios (VMRs) within the main anticyclone and within the eddy, which are suitable as a tracer for polluted air originating in India and China. Plotting the retrieved PAN VMRs against potential vorticity (PV) and potential temperature reveals that the PV value at which the PAN VMRs exhibit the strongest decrease with respect to PV increases with potential temperature. These PV values might be used to identify the extent of the ASM. Using temperature values also derived from CRISTA measurements, we also computed the location of the thermal tropopause according to the WMO criterion and find that it confines the PAN anomaly vertically within the main ASM anticyclone. In contrast, the shed eddy exhibits enhanced PAN VMRs for 1 to 2 km above the thermal tropopause. Using the relationship between PAN as a tropospheric tracer and O3 as a stratospheric tracer to identify mixed air parcels, we further found the anticyclone to contain few such air parcels, whereas the region between the anticyclone and the eddy as well as the eddy itself contains many mixed air parcels. In combination, this implies that while the anticyclone confines polluted air masses well, eddy shedding provides a very rapid horizontal transport pathway of Asian pollution into the extratropical lowermost stratosphere with a timescale of only a few days.

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 the aircraft M-55 Geophysica, which was operated from Kiruna, Sweden. Flights were performed at a height of up to 21 km and some of the particle samples were taken within distinct polar stratospheric clouds (PSCs). 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 in early winter, during the late-winter RECONCILE mission the air masses were subsiding inside the Arctic winter vortex from the 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 the presence of soot was also 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 large refractory particles in the stratosphere, as well as the experimental finding that these particles were not observed in the particle samples (upper size limit ∼ 5 µm) taken during PSC events, strengthens the hypothesis that such particles are present in the lower polar stratosphere in late winter and have provided a surface for heterogeneous nucleation during PSC formation.