The global aerosol extinction from the CALIOP space lidar was used to compute aerosol optical depth (AOD) over a 9-year period (2007-2015) and partitioned between the boundary layer (BL) and the free troposphere (FT) using BL heights obtained from the ERA-Interim archive. The results show that the vertical distribution of AOD does not follow the diurnal cycle of the BL but remains similar between day and night highlighting the presence of a residual layer during night. The BL and FT contribute 69 and 31 %, respectively, to the global tropospheric AOD during daytime in line with observations obtained in Aire sur l'Adour (France) using the Light Optical Aerosol Counter (LOAC) instrument. The FT AOD contribution is larger in the tropics than at mid-latitudes which indicates that convective transport largely controls the vertical profile of aerosols. Over oceans, the FT AOD contribution is mainly governed by long-range transport of aerosols from emission sources located within neighboring continents. According to the CALIOP aerosol classification, dust and smoke particles are the main aerosol types transported into the FT. Overall, the study shows that the fraction of AOD in the FT - and thus potentially located above low-level clouds - is substantial and deserves more attention when evaluating the radiative effect of aerosols in climate models. More generally, the results have implications for processes determining the overall budgets, sources, sinks and transport of aerosol particles and their description in atmospheric models.

Mineral dust from arid areas is a major component of global aerosol and has strong interactions with climate and biogeochemistry. As part of the Chemistry-Aerosol Mediterranean Experiment (ChArMEx) to investigate atmospheric chemistry and its impacts in the Mediterranean region, an intensive field campaign was performed from mid-June to early August 2013 in the western basin including in situ balloon-borne aerosol measurements with the light optical aerosol counter (LOAC). LOAC is a counter/sizer that provides the aerosol concentrations in 19 size classes between 0.2 and 100 mu m, and an indication of the nature of the particles based on dual-angle scattering measurements. A total of 27 LOAC flights were conducted mainly from Minorca Island (Balearic Islands, Spain) but also from Ile du Levant off Hyeres city (SE France) under 17 light dilatable balloons (meteorological sounding balloons) and 10 boundary layer pressurised balloons (quasi-Lagrangian balloons). The purpose was to document the vertical extent of the plume and the time evolution of the concentrations at constant altitude (air density) by in situ observations. LOAC measurements are in agreement with ground-based measurements (lidar, photometer), aircraft measurements (counters), and satellite measurements (CALIOP) in the case of fair spatial and temporal coincidences. LOAC has often detected three modes in the dust particle volume size distributions fitted by lognormal laws at roughly 0.2, 4 and 30 mu m in modal diameter. Thanks to the high sensitivity of LOAC, particles larger than 40 mu m were observed, with concentrations up to about 10(-4) cm(-3). Such large particles were lifted several days before and their persistence after transport over long distances is in conflict with calculations of dust sedimentation. We did not observe any significant evolution of the size distribution during the transport from quasi-Lagrangian flights, even for the longest ones (similar to 1 day). Finally, the presence of charged particles is inferred from the LOAC measurements and we speculate that electrical forces might counteract gravitational settling of the coarse particles.

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 similar to 45% and increases of similar to 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 (similar to 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.

Clouds are crucial for Earth's climate and radiation budget. Great attention has been paid to low, high and vertically thick tropospheric clouds such as stratus, cirrus and deep convective clouds. However, much less is known about tropospheric mid-level clouds as these clouds are challenging to observe in situ and difficult to detect by remote sensing techniques. Here we use Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) satellite observations to show that thin mid-level clouds (TMLCs) are ubiquitous in the tropics. Supported by high-resolution regional model simulations, we find that TMLCs are formed by detrainment from convective clouds near the zero-degree isotherm. Calculations using a radiative transfer model indicate that tropical TMLCs have a cooling effect on climate that could be as large in magnitude as the warming effect of cirrus. We conclude that more effort has to be made to understand TMLCs, as their influence on cloud feedbacks, heat and moisture transport, and climate sensitivity could be substantial.

Six years (200702012) of data from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) satellite instrument were used to investigate the vertical distribution and transport of aerosols over the tropical South American continent and the southeast Pacific Ocean. The multiyear aerosol extinction assessment indicates that aerosols, mainly biomass burning particles emitted during the dry season in the Amazon Basin, are lifted in significant amounts over the Andes. The aerosols are mainly transported in the planetary boundary layer between the surface and 2 km altitude with an aerosol extinction maximum near the surface. During the transport toward the Andes, the aerosol extinction decreases at a rate of 0.02 km(-1) per kilometer of altitude likely due to dilution and deposition processes. Aerosols reaching the top of the Andes, at altitudes typically between 4 and 5 km, are entrained into the free troposphere (FT) over the southeast Pacific Ocean. A comparison between CALIOP observations and ERA-Interim reanalysis data indicates that during their long-range transport over the tropical Pacific Ocean, these aerosols are slowly transported toward the marine boundary layer by the large-scale subsidence at a rate of 0.4 cm s(-1). The observed vertical/horizontal transport ratio is 0.700.8 m km(-1) Continental aerosols linked to transport over the Andes can be traced on average over 4000 km away from the continent indicating an aerosol residence time of 809 days in the FT over the Pacific Ocean. The FT aerosol optical depth (AOD) above the Pacific Ocean near South American coast accounts on average for 6% and 25% of the total AOD during the season of low and high biomass burning, respectively. This result shows that, during the biomass burning season, continental aerosols largely influence the AOD over the remote southeast Pacific Ocean. Overall, FT AOD decrease exponentially with the distance to continental sources at a rate of about 10% per degree of longitude over the Pacific Ocean.