Abstract. In June 2019 a stratospheric eruption occurred at Raikoke (48∘ N, 153∘ E). Satellite observations show the injection of ash and SO2 into the lower stratosphere and an early entrainment of the plume into a cyclone. Following the Raikoke eruption, stratospheric aerosol optical depth (sAOD) values increased in the whole Northern Hemisphere and tropics and remained enhanced for more than 1 year, with peak values at 0.040 (short-wavelength, high northern latitudes) to 0.025 (short-wavelength, Northern Hemisphere average). Discrepancies between observations and global model simulations indicate that ash may have influenced the extent and evolution of the sAOD. Top of the atmosphere radiative forcings are estimated at values between −0.3 and -0.4Wm-2 (clear-sky) and of −0.1 to -0.2Wm-2 (all-sky), comparable to what was estimated for the Sarychev eruption in 2009. Almost simultaneously two significantly smaller stratospheric eruptions occurred at Ulawun (5∘ S, 151∘ E) in June and August. Aerosol enhancements from the Ulawun eruptions mainly had an impact on the tropics and Southern Hemisphere. The Ulawun plume circled the Earth within 1 month in the tropics. Peak shorter-wavelength sAOD values at 0.01 are found in the tropics following the Ulawun eruptions and a radiative forcing not exceeding −0.15 (clear-sky) and −0.05 (all-sky). Compared to the Canadian fires (2017), Ambae eruption (2018), Ulawun (2019) and the Australian fires (2019/2020), the highest sAOD and radiative forcing values are found for the Raikoke eruption.

We describe and show results from a series of field campaigns that used balloonborne instruments launched from India and Saudi Arabia during the summers 2014–17 to study the nature, formation, and impacts of the Asian Tropopause Aerosol Layer (ATAL). The campaign goals were to i) characterize the optical, physical, and chemical properties of the ATAL; ii) assess its impacts on water vapor and ozone; and iii) understand the role of convection in its formation. To address these objectives, we launched 68 balloons from four locations, one in Saudi Arabia and three in India, with payload weights ranging from 1.5 to 50 kg. We measured meteorological parameters; ozone; water vapor; and aerosol backscatter, concentration, volatility, and composition in the upper troposphere and lower stratosphere (UTLS) region. We found peaks in aerosol concentrations of up to 25 cm–3 for radii > 94 nm, associated with a scattering ratio at 940 nm of ∼1.9 near the cold-point tropopause. During medium-duration balloon flights near the tropopause, we collected aerosols and found, after offline ion chromatography analysis, the dominant presence of nitrate ions with a concentration of about 100 ng m–3. Deep convection was found to influence aerosol loadings 1 km above the cold-point tropopause. The Balloon Measurements of the Asian Tropopause Aerosol Layer (BATAL) project will continue for the next 3–4 years, and the results gathered will be used to formulate a future National Aeronautics and Space Administration–Indian Space Research Organisation (NASA–ISRO) airborne campaign with NASA high-altitude aircraft.

Abstract. The Chemistry-Aerosol Mediterranean Experiment (ChArMEx; http://charmex.lsce.ipsl.fr) is a collaborative research program federating international activities to investigate Mediterranean regional chemistry-climate interactions. A special observing period (SOP-1a) including intensive airborne measurements was performed in the framework of the Aerosol Direct Radiative Impact on the regional climate in the MEDiterranean region (ADRIMED) project during the Mediterranean dry season over the western and central Mediterranean basins, with a focus on aerosol-radiation measurements and their modeling. The SOP-1a took place from 11 June to 5 July 2013. Airborne measurements were made by both the ATR-42 and F-20 French research aircraft operated from Sardinia (Italy) and instrumented for in situ and remote-sensing measurements, respectively, and by sounding and drifting balloons, launched in Minorca. The experimental setup also involved several ground-based measurement sites on islands including two ground-based reference stations in Corsica and Lampedusa and secondary monitoring sites in Minorca and Sicily. Additional measurements including lidar profiling were also performed on alert during aircraft operations at EARLINET/ACTRIS stations at Granada and Barcelona in Spain, and in southern Italy. Remote-sensing aerosol products from satellites (MSG/SEVIRI, MODIS) and from the AERONET/PHOTONS network were also used. Dedicated meso-scale and regional modeling experiments were performed in relation to this observational effort. We provide here an overview of the different surface and aircraft observations deployed during the ChArMEx/ADRIMED period and of associated modeling studies together with an analysis of the synoptic conditions that determined the aerosol emission and transport. Meteorological conditions observed during this campaign (moderate temperatures and southern flows) were not favorable to producing high levels of atmospheric pollutants or intense biomass burning events in the region. However, numerous mineral dust plumes were observed during the campaign, with the main sources located in Morocco, Algeria and Tunisia, leading to aerosol optical depth (AOD) values ranging between 0.2 and 0.6 (at 440 nm) over the western and central Mediterranean basins. One important point of this experiment concerns the direct observations of aerosol extinction onboard the ATR-42, using the CAPS system, showing local maxima reaching up to 150 M m −1 within the dust plume. Non-negligible aerosol extinction (about 50 M m −1 ) has also been observed within the marine boundary layer (MBL). By combining the ATR-42 extinction coefficient observations with absorption and scattering measurements, we performed a complete optical closure revealing excellent agreement with estimated optical properties. This additional information on extinction properties has allowed calculation of the dust single scattering albedo (SSA) with a high level of confidence over the western Mediterranean. Our results show a moderate variability from 0....

Abstract.Carbon aerosols are produced by all combustion processes. This paper investigates some possible effects of heterogeneous reduction of atmospheric constituents on carbon aerosols. Reduction of HNO3, NO2, and 03 on carbon aerosols may be an important effect of increased air traffic that has not been considered to date. It is shown that if HNO3, NO2 and 03 are heterogeneously reduced on atmospheric amorphous carbon aerosols, then a significant, lower stratospheric ozone loss mechanism could exist. This ozone loss mechanism is almost independent of temperature and does not require the presence of sunlight. The mechanism can operate at all latitudes where amorphous carbon aerosols are present. The relative importance of the mechanism increases with nightlength. The reduction of HNO3 on carbon aerosols could also be a significant renoxification process wherever carbon aerosols are present. Owing to the very different soot levels in the two hemispheres, this implies that there should be a hemispheric assymetry in the role of these mechanisms. The renoxification lea, ds to simulated tropospheric HNO3/NO• ratios that are close to those observed. In contrast to the stratospheric response, the tropospheric production of NO• due to the reduction of HNO3 would lead to tropospheric ozone production.

Abstract. The study of aerosols in the troposphere and in the stratosphere is of major importance both for climate and air quality studies. Among the numerous instruments available, optical aerosol particles counters (OPCs) provide the size distribution in diameter range from about 100 nm to a few tens of µm. Most of them are very sensitive to the nature of aerosols, and this can result in significant biases in the retrieved size distribution. We describe here a new versatile optical particle/sizer counter named LOAC (Light Optical Aerosol Counter), which is light and compact enough to perform measurements not only at the surface but under all kinds of balloons in the troposphere and in the stratosphere. LOAC is an original OPC performing observations at two scattering angles. The first one is around 12 • , and is almost insensitive to the refractive index of the particles; the second one is around 60 • and is strongly sensitive to the refractive Published by Copernicus Publications on behalf of the European Geosciences Union. J.-B. Renard et al.: Size distribution and nature of atmospheric particlesindex of the particles. By combining measurement at the two angles, it is possible to retrieve the size distribution between 0.2 and 100 µm and to estimate the nature of the dominant particles (droplets, carbonaceous, salts and mineral particles) when the aerosol is relatively homogeneous. This typology is based on calibration charts obtained in the laboratory. The uncertainty for total concentrations measurements is ±20 % when concentrations are higher than 1 particle cm −3 (for a 10 min integration time). For lower concentrations, the uncertainty is up to about ±60 % for concentrations smaller than 10 −2 particle cm −3 . Also, the uncertainties in size calibration are ±0.025 µm for particles smaller than 0.6 µm, 5 % for particles in the 0.7-2 µm range, and 10 % for particles greater than 2 µm. The measurement accuracy of submicronic particles could be reduced in a strongly turbid case when concentration of particles > 3 µm exceeds a few particles cm −3 . Several campaigns of cross-comparison of LOAC with other particle counting instruments and remote sensing photometers have been conducted to validate both the size distribution derived by LOAC and the retrieved particle number density. The typology of the aerosols has been validated in well-defined conditions including urban pollution, desert dust episodes, sea spray, fog, and cloud. Comparison with reference aerosol mass monitoring instruments also shows that the LOAC measurements can be successfully converted to mass concentrations.

Stratospheric aerosols play a significant role in stratospheric chemistry. In the past, it was assumed that only liquid droplets are present in the stratosphere. Nevertheless, a few lidar measurements have shown that sudden enhancement of aerosol content in the middle stratosphere could be due to meteoritic debris. Aircraft measurements have shown that solid particles can be found in the lower stratosphere; these particles are mainly soot, but also include some interplanetary material. In order to better document the various characteristics of aerosols in the unperturbed stratosphere (i.e., free of volcanic aerosols), we have performed observations using different balloon-borne instruments (Stratospheric and Tropospheric Aerosol Counter (STAC), Spectroscopie d'Absorption Lunaire pour l'Observation des Minoritaires Ozone et NOx (SALOMON), and Micro Radiometre Ballon (MicroRADIBAL)) and also some satellite data (Global ozone monitoring by occultation of stars Envisat (GOMOS-Envisat)). These instruments allow us to obtain the number of particles in different size classes, the wavelength dependence of aerosol extinction, and the radiance of the light scattered by aerosols. Combining all the data together, it appears that significant amounts of particles are ubiquitous in the middle stratosphere, above the canonical sulfate aerosol layer. "Background'' interplanetary dusts in low concentration are likely present in the stratosphere. Above 30 km, interplanetary dust and largest grains from meteoroid disintegration dominate. Although the disintegration of meteoroids occurs in the upper stratosphere or in the mesosphere at all latitudes, these solid aerosols can be transported to the polar regions by the general circulation and can descend into the middle and lower stratosphere during winter mesospheric descents. Between about 22 km and 30 km, soot particles contribute to the population of aerosols at all latitudes. These soot, likely originating from biomass burning at all latitudes, could be injected into the lower stratosphere by the pyroconvective effect and can then reach the middle stratosphere perhaps owing to the gravitophotophoresis effect as was theoretically proposed. In the lower unperturbed stratosphere, liquid sulfate aerosols dominate, although soot particles are still present. Local horizontal and vertical enhancements of solid aerosols have sometimes been detected, although their origin is not yet determined. The presence of these solid particles can strongly bias the interpretation of in situ and remote sensing measurements when only the presence of liquid aerosols is assumed. Therefore, a new strategy of measurement will be necessary in the future to better characterize the stratospheric aerosol content free of volcanic particles

The ice giants Uranus and Neptune are the least understood class of planets in our solar system but the most frequently observed type of exoplanets. Presumed to have a small rocky core, a deep interior comprising ∼70% heavy elements surrounded by a more dilute outer envelope of H 2 and He, Uranus and Neptune are fundamentally different from the better-explored gas giants Jupiter and Saturn. Because of the lack of dedicated exploration missions, our knowledge of the composition and atmospheric processes of these distant worlds is primarily derived from remote sensing from Earth-based observatories and space telescopes. As a result, Uranus's and Neptune's physical and atmospheric properties remain poorly constrained and their roles in the evolution of the Solar System not well understood. Exploration of an ice giant system is therefore a highpriority science objective as these systems (including the magnetosphere, satellites, rings, atmosphere, and interior) challenge our understanding of planetary formation and evolution. Here we describe the main scientific goals to be addressed by a future in situ exploration of an ice giant. An atmospheric entry probe targeting the 10-bar level, about 5 scale heights beneath the tropopause, would yield insight into two broad themes : i) the formation history of the ice giants and, in a broader extent, that of the Solar System, and ii) the processes at play in planetary atmospheres. The probe would descend under parachute to measure composition, structure, and dynamics, with data returned to Earth using a Carrier Relay Spacecraft as a relay station. In addition, possible mission concepts and partnerships are presented, and a strawman ice-giant probe payload is described. An ice-giant atmospheric probe could represent a significant ESA contribution to a future NASA ice-giant flagship mission.

The underwater Hunga Tonga-Hunga Ha-apai volcano erupted in the early hours of 15th January 2022, and injected volcanic gases and aerosols to over 50 km altitude. Here we synthesise satellite, ground-based, in situ and radiosonde observations of the eruption to investigate the strength of the stratospheric aerosol and water vapour perturbations in the initial weeks after the eruption and we quantify the net radiative impact across the two species using offline radiative transfer modelling. We find that the Hunga Tonga-Hunga Ha-apai eruption produced the largest global perturbation of stratospheric aerosols since the Pinatubo eruption in 1991 and the largest perturbation of stratospheric water vapour observed in the satellite era. Immediately after the eruption, water vapour radiative cooling dominated the local stratospheric heating/cooling rates, while at the top-of-the-atmosphere and surface, volcanic aerosol cooling dominated the radiative forcing. However, after two weeks, due to dispersion/dilution, water vapour heating started to dominate the top-of-the-atmosphere radiative forcing, leading to a net warming of the climate system.