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A test bench has been developed allowing to simulate air flow in a 20 L cylindrical stainless‐steel chamber under conditions of the stratosphere and the troposphere: pressure from about 500 to 30 hPa, air temperature from 293 to 223 K and air flow velocity of about 5 m/s. Humidity of the air flow is controlled in the range of frost temperature from 253 to 193 K with accuracy better than 0.3 K for a frost temperature of 198 K. Specifically designed to test a newly developed frost point hygrometer, this facility may as well be used for testing instruments with suitable dimensions especially those operating with sounding balloons. A test bench has been developed allowing for the simulation of air flow in a 20 L cylindrical stainless‐steel chamber under conditions of the stratosphere and the troposphere: pressure from about 500 to 30 hPa, air temperature from 20°C to −50°C, and air flow velocity of about 5 m/s.

Most major field campaigns, such as the Southern Africa Fire Atmosphere Research Initiative (SAFARI-92 and SAFARI-2000) and AErosol, RadiatiOn and CLOuds in southern Africa (AEROCLO-sA), have focused on the west coast of southern Africa, leaving the east coast underexplored. To address this, the Biomass Burning Aerosol Campaign (BiBAC) was initiated by the IRP ARSAIO (International Research Project – Atmospheric Research in Southern Africa and Indian Ocean) during the 2022 biomass burning season to study aerosol optical properties over southern Africa and the southwestern Indian Ocean (SWIO). This study analyzes aerosol properties during the intensive observation period (IOP) of BiBAC at Skukuza in Kruger National Park during two events: 18–23 September (Event 1) and 9–17 October (Event 2). Sun-photometer data, consistent with CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization), revealed a predominance of biomass burning aerosols. Transport analyses show southeastward movement of carbon monoxide (CO) and aerosols, reaching up to 6 km during Event 1 and 10 km during Event 2. Synoptic conditions, including frontal systems and baroclinic waves, drove regional and intercontinental pollutant transport, impacting the Mozambique Channel and surrounding areas. A “river of smoke” observed in Event 1 suggests novel synoptic conditions compared to previous studies. This study is the first to highlight two distinct transport mechanisms of aerosol plumes and CO from southern Africa and South America toward the SWIO basin, underscoring the significance of east-coast observations in understanding regional and global atmospheric dynamics.

The Gradient in Longitude of Atmospheric constituents above the Mediterranean basin (GLAM) campaign was set up in August 2014, as part of the Chemistry and Aerosol Mediterranean Experiment (ChArMEx) project. This campaign aimed to study the chemical variability of gaseous pollutants and aerosols in the troposphere along a west–east transect above the Mediterranean Basin (MB). In the present work, we focus on two biomass burning events detected at 5.4 and 9.7 km altitude above sea level (a.s.l.) over Sardinia (from 39∘12′ N–9∘15′ E to 35∘35′ N–12∘35′ E and at 39∘30′ N–8∘25′ E, respectively). Concentration variations in trace gas carbon monoxide (CO), ozone (O3) and aerosols were measured thanks to the standard instruments on board the Falcon 20 aircraft operated by the Service des Avions Français Instrumentés pour la Recherche en Environnement (SAFIRE) and the Spectromètre InfraRouge In situ Toute Altitude (SPIRIT) developed by LPC2E. Twenty-day backward trajectories with Lagrangian particle dispersion model FLEXPART (FLEXible PARTicle) help to understand the transport processes and the origin of the emissions that contributed to this pollution detected above Sardinia. Biomass burning emissions came (i) on 10 August from the North American continent with air masses transported during 5 days before arriving over the MB, and (ii) on 6 August from Siberia, with air masses travelling during 12 days and enriched in fire emission products above Canada 5 days before arriving over the MB. In combination with the Global Fire Assimilation System (GFAS) inventory and the Moderate Resolution Imaging Spectroradiometer (MODIS) satellite fire locations, FLEXPART reproduces well the contribution of those fires to CO and aerosols enhancements under adjustments of the injection height to 10 km in both cases and application of an amplification factor of 2 on CO GFAS emissions for the 10 August event. The chemistry transport model (CTM) MOCAGE is used as a complementary tool for the case of 6 August to confirm the origin of the emissions by tracing the CO global atmospheric composition reaching the MB. For this event, both models agree on the origin of air masses with CO concentrations simulated with MOCAGE lower than the observed ones, likely caused by the coarse model horizontal resolution that yields the dilution of the emissions and diffusion during transport. In combination with wind fields, the analysis of the transport of the air mass documented on 6 August suggests the subsidence of CO pollution from Siberia towards North America and then a transport to the MB via fast jet winds located at around 5.5 km in altitude. Finally, using the ratio ΔO3 ∕ ΔCO, the plume age can be estimated and the production of O3 during the transport of the air mass is studied using the MOCAGE model.

We present a global carbonyl sulfide (OCS) data set covering the period June 2002 to April 2012, derived from FTIR (Fourier transform infrared) limb emission spectra measured with the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on the ENVISAT satellite. The vertical resolution is 4–5 km in the height region 6–15 km and 15 at 40 km altitude. The total estimated error amounts to 40–50 pptv between 10 and 20 km and to 120 pptv at 40 km altitude. MIPAS OCS data show no systematic bias with respect to balloon observations, with deviations mostly below ±50 pptv. However, they are systematically higher than the OCS volume mixing ratios of the ACE-FTS instrument on SCISAT, with maximum deviations of up to 100 pptv in the altitude region 13–16 km. The data set of MIPAS OCS exhibits only moderate interannual variations and low interhemispheric differences. Average concentrations at 10 km altitude range from 480 pptv at high latitudes to 500–510 pptv in the tropics and at northern mid-latitudes. Seasonal variations at 10 km altitude amount to up to 35 pptv in the Northern and up to 15 pptv in the Southern Hemisphere. Northern hemispheric OCS abundances at 10 km altitude peak in June in the tropics and around October at high latitudes, while the respective southern hemispheric maxima were observed in July and in November. Global OCS distributions at 250 hPa (∼ 10–11 km) show enhanced values at low latitudes, peaking during boreal summer above the western Pacific and the Indian Ocean, which indicates oceanic release. Further, a region of depleted OCS amounts extending from Brazil to central and southern Africa was detected at this altitude, which is most pronounced in austral summer. This depletion is related to seasonally varying vegetative uptake by the tropical forests. Typical signatures of biomass burning like the southern hemispheric biomass burning plume are not visible in MIPAS data, indicating that this process is only a minor source of upper tropospheric OCS. At the 150 hPa level (∼ 13–14 km) enhanced amounts of OCS were also observed inside the Asian monsoon anticyclone, but this enhancement is not especially outstanding compared to other low latitude regions at the same altitude. At the 80 hPa level (∼ 17–18 km), equatorward transport of mid-latitude air masses containing lower OCS amounts around the summertime anticyclones was observed. A significant trend could not be detected in upper tropospheric MIPAS OCS amounts, which points to globally balanced sources and sinks. Simulations with the ECHAM-MESSy model reproduce the observed latitudinal cross sections fairly well.

During the 2020 austral summer, the pristine atmosphere of the southwest Indian Ocean (SWIO) basin experienced significant perturbations. This study examines the variability of aerosols and carbon monoxide (CO) over this remote oceanic region and investigates the underlying processes in the upper troposphere–lower stratosphere (UT-LS). Aerosol profiles in January and February 2020 revealed a multi-layer structure in the tropical UT-LS. Numerical models – the FLEXible PARTicle dispersion model (FLEXPART) and the Modèle Isentropique de transport Mésoéchelle de l'Ozone Stratosphérique par Advection (MIMOSA) – indicated that the lower-stratospheric aerosol content was influenced by the intense and persistent stratospheric aerosol layer generated during the 2019–2020 extreme Australian bushfire events. A portion of this layer was transported eastward by prevailing easterly winds, leading to increased aerosol extinction profiles over Réunion on 27 and 28 January. Analysis of advected potential vorticity revealed isentropic transport of air masses containing Australian biomass burning aerosols from extratropical latitudes to Réunion at the 400 K isentropic level on 28 January. Interestingly, we found that biomass burning (BB) activity in eastern Africa, though weak during this season, significantly influenced (contributed up to 90 % of) the vertical distribution of CO and aerosols in the upper troposphere over the SWIO basin. Ground-based observations at Réunion confirmed the simultaneous presence of African and Australian aerosol layers. This study provides the first evidence of African BB emissions impacting the CO and aerosol distribution in the upper troposphere over the SWIO basin during the convective season.

Atmospheric aerosols significantly influence the Earth’s climate, yet they remain a major source of uncertainty in climate projections. Here, we present a set of unique offline analysis of organics collected from the ground to the stratosphere with ultimate sensitivity using a new balloon-borne sampling technique deployed on simple weather balloons. Activated and functionalized carbon fabrics were used to target chemical compounds in the gaseous and aerosol forms during three flights over France. Ultra-high-resolution mass spectrometry, enabling the detection of thousands of organic compounds, and highlighted high-carbon-number organics, indicating oligomerization in long-lived tropical stratospheric air masses. Our measurements suggest that large stratospheric sulfate aerosols from volcanic eruptions could play a role in the formation of secondary aerosols in internally mixed particles and may explain the presence of organics with higher carbon numbers. These measurements revealed a drop in the number of unsaturated carbons at higher altitudes.

The historically large and severe wildfires in Australia from September 2019 to March 2020 are known to have injected a smoke plume into the stratosphere around New Year, due to pyro-cumulonimbus (pyro-Cb) activity, that was subsequently distributed throughout the Southern Hemisphere (SH). We show with satellite, ground based remote sensing, and in situ observations that the fires before New Year, had already a substantial impact on the SH atmosphere, starting as early as September 2019, with subsequent long-range transport of trace gas plumes in the upper-troposphere. Airborne in situ measurements above Southern Argentina in November 2019 show elevated CO mixing ratios at an altitude of 11 km and can be traced back using FLEXPART trajectories to the Australian fires in mid-November 2019. Ground based solar-FTS (Fourier Transform Spectroscopy) observations of biomass burning tracers CO, HCN and C 2 H 6 at Lauder, South Island, New Zealand show enhanced tropospheric columns already starting in September 2019. In MLS observations averaged over 30°–60°S, enhanced CO mixing ratios compared to previous years become visible in late October 2019 only at and below the 147 hPa pressure level. Peak differences are found with satellite and ground-based observations for all altitude levels in the Southern Hemisphere in January. With still increased aerosol values following the Ulawun eruption in 2019, averaged satellite observations show no clear stratospheric and upper-tropospheric aerosol enhancements from the Australian fires, before the pyro-Cb events at the end of December 2019. However, with the clear enhancement of fire tracers, we suggest the period September to December 2019 (prior to the major pyro-Cb events) should be taken into account in terms of fire pollutant emissions when studying the impact of the Australian fires on the SH atmosphere.

The major volcanic eruption of Mount Pinatubo in 1991 has been shown to have significant effects on stratospheric chemistry and ozone depletion even at midlatitudes. Since then, only moderate but recurrent volcanic eruptions have modulated the stratospheric aerosol loading and are assumed to be one cause for the reported increase in the global aerosol content over the past 15 years. This particularly enhanced aerosol context raises questions about the effects on stratospheric chemistry which depend on the latitude, altitude and season of injection. In this study, we focus on the midlatitude Sarychev volcano eruption in June 2009, which injected 0.9 Tg of sulfur dioxide (about 20 times less than Pinatubo) into a lower stratosphere mainly governed by high-stratospheric temperatures. Together with in situ measurements of aerosol amounts, we analyse high-resolution in situ and/or remote-sensing observations of NO2, HNO3 and BrO from balloon-borne infrared and UV–visible spectrometers launched in Sweden in August–September 2009. It is shown that differences between observations and three-dimensional (3-D) chemistry-transport model (CTM) outputs are not due to transport calculation issues but rather reflect the chemical impact of the volcanic plume below 19 km altitude. Good measurement–model agreement is obtained when the CTM is driven by volcanic aerosol loadings derived from in situ or space-borne data. As a result of enhanced N2O5 hydrolysis in the Sarychev volcanic aerosol conditions, the model calculates reductions of ∼ 45 % and increases of ∼ 11 % in NO2 and HNO3 amounts respectively over the August–September 2009 period. The decrease in NOx abundances is limited due to the expected saturation effect for high aerosol loadings. The links between the various chemical catalytic cycles involving chlorine, bromine, nitrogen and HOx compounds in the lower stratosphere are discussed. The increased BrO amounts (∼ 22 %) compare rather well with the balloon-borne observations when volcanic aerosol levels are accounted for in the CTM and appear to be mainly controlled by the coupling with nitrogen chemistry rather than by enhanced BrONO2 hydrolysis. We show that the chlorine partitioning is significantly controlled by enhanced BrONO2 hydrolysis. However, simulated effects of the Sarychev eruption on chlorine activation are very limited in the high-temperature conditions in the stratosphere in the period considered, inhibiting the effect of ClONO2 hydrolysis. As a consequence, the simulated chemical ozone loss due to the Sarychev aerosols is low with a reduction of −22 ppbv (−1.5 %) of the ozone budget around 16 km. This is at least 10 times lower than the maximum ozone depletion from chemical processes (up to −20 %) reported in the Northern Hemisphere lower stratosphere over the first year following the Pinatubo eruption. This study suggests that moderate volcanic eruptions have limited chemical effects when occurring at midlatitudes (restricted residence times) and outside winter periods (high-temperature conditions). However, it would be of interest to investigate longer-lasting tropical volcanic plumes or sulfur injections in the wintertime low-temperature conditions.

Very short-lived substances (VSLS) contribute as source gases significantly to the tropospheric and stratospheric bromine loading. At present, an estimated 25 % of stratospheric bromine is of oceanic origin. In this study, we investigate how climate change may impact the ocean–atmosphere flux of brominated VSLS, their atmospheric transport, and chemical transformations and evaluate how these changes will affect stratospheric ozone over the 21st century. Under the assumption of fixed ocean water concentrations and RCP6.0 scenario, we find an increase of the ocean–atmosphere flux of brominated VSLS of about 8–10 % by the end of the 21st century compared to present day. A decrease in the tropospheric mixing ratios of VSLS and an increase in the lower stratosphere are attributed to changes in atmospheric chemistry and transport. Our model simulations reveal that this increase is counteracted by a corresponding reduction of inorganic bromine. Therefore the total amount of bromine from VSLS in the stratosphere will not be changed by an increase in upwelling. Part of the increase of VSLS in the tropical lower stratosphere results from an increase in the corresponding tropopause height. As the depletion of stratospheric ozone due to bromine depends also on the availability of chlorine, we find the impact of bromine on stratospheric ozone at the end of the 21st century reduced compared to present day. Thus, these studies highlight the different factors influencing the role of brominated VSLS in a future climate.

The present study contributes to the scientific effort for a better understanding of the potential of the Australian biomass burning events to influence tropospheric trace gas abundances at the regional scale. In order to exclude the influence of the long-range transport of ozone precursors from biomass burning plumes originating from Southern America and Africa, the analysis of the Australian smoke plume has been driven over the period December 2019 to January 2020. This study uses satellite (IASI, MLS, MODIS, CALIOP) and ground-based (sun-photometer, FTIR, ozone radiosondes) observations. The highest values of aerosol optical depth (AOD) and carbon monoxide total columns are observed over Southern and Central Australia. Transport is responsible for the spatial and temporal distributions of aerosols and carbon monoxide over Australia, and also the transport of the smoke plume outside the continent. The dispersion of the tropospheric smoke plume over Oceania and Southern Pacific extends from tropical to extratropical latitudes. Ozone radiosonde measurements performed at Samoa (14.4°S, 170.6°W) and Lauder (45.0°S, 169.4°E) indicate an increase in mid-tropospheric ozone (6–9 km) (from 10% to 43%) linked to the Australian biomass burning plume. This increase in mid-tropospheric ozone induced by the transport of the smoke plume was found to be consistent with MLS observations over the tropical and extratropical latitudes. The smoke plume over the Southern Pacific was organized as a stretchable anticyclonic rolling which impacted the ozone variability in the tropical and subtropical upper-troposphere over Oceania. This is corroborated by the ozone profile measurements at Samoa which exhibit an enhanced ozone layer (29%) in the upper-troposphere. Our results suggest that the transport of Australian biomass burning plumes have significantly impacted the vertical distribution of ozone in the mid-troposphere southern tropical to extratropical latitudes during the 2019–20 extreme Australian bushfires.