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 $-\mathrm{0.4}\mathrm{W}{\mathrm{m}}^{-\mathrm{2}}$ (clear-sky) and of −0.1 to $-\mathrm{0.2}\mathrm{W}{\mathrm{m}}^{-\mathrm{2}}$ (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 investigate the impact of the 2015 Mount Calbuco eruption and previous eruptions on stratospheric aerosols, polar stratospheric clouds, and ozone depletion using the Community Earth System Model coupled with the Community Aerosol and Radiation Model for Atmospheres compared with several satellite and balloon observations. The modeled volcanic sulfate aerosol size distribution agrees with the Light Optical Aerosol Counter observation at the Reunion Island site (21°S, 55°E) on 19 August at 20 km within estimated 0.1‐ to 1‐μm radius error bars. Both the observed and simulated backscatter and extinction show that volcanic sulfate aerosol from the Mount Calbuco eruption was transported from midlatitude toward the Antarctic and slowly descended during transport. They also indicate that the SO₂ emission into the stratosphere from Mount Calbuco is 0.2–0.4 Tg. The modeled number density indicates that the volcanic sulfate aerosol from the Mount Calbuco eruption penetrated into the Antarctic polar vortex in May and thereafter and reduced the polar stratospheric clouds effective radius. In the simulations, the Antarctic stratosphere denitrified too early and by too much compared with Microwave Limb Sounder observations. Heterogeneous nucleation of nitric acid trihydrate or sophisticated gravity wave representations may be required to simulate nitric acid trihydrate particles with smaller falling velocity. The volcanic sulfate aerosol increases the ozone depletion in September especially around 100 hPa and 70°S, relative to a case without any volcanic eruptions. The simulated surface area density, earlier ozone loss, and larger area of the ozone hole are consistent with the presence of volcanic sulfate layers observed at 16 km as well as previous studies.

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 index 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.

We show that a fire plume injected into the lower stratosphere at high northern latitudes during the Canadian wildfire event in August 2017 partly reached the tropics. The transport to the tropics was mediated by the anticyclonic flow of the Asian monsoon circulation. The fire plume reached the Asian monsoon area in late August/early September, when the Asian monsoon anticyclone (AMA) was still in place. While there is no evidence of mixing into the center of the AMA, we show that a substantial part of the fire plume is entrained into the anticyclonic flow at the AMA edge and is transported from the extratropics to the tropics, and possibly the Southern Hemisphere particularly following the north–south flow on the eastern side of the AMA. In the tropics the fire plume is lifted by ∼5 km in 7 months. Inside the AMA we find evidence of the Asian tropopause aerosol layer (ATAL) in August, doubling background aerosol conditions with a calculated top of the atmosphere shortwave radiative forcing of −0.05 W m⁻². The regional climate impact of the fire signal in the wider Asian monsoon area in September exceeds the impact of the ATAL by a factor of 2–4 and compares to that of a plume coming from an advected moderate volcanic eruption. The stratospheric, trans-continental transport of this plume to the tropics and the related regional climate impact point to the importance of long-range dynamical interconnections of pollution sources.

In the companion (Part I) paper, we have described and evaluated a new versatile optical particle counter/sizer named LOAC (Light Optical Aerosol Counter), based on scattering measurements at angles of 12 and 60°. That allows for some typology identification of particles (droplets, carbonaceous, salts, and mineral dust) in addition to size-segregated counting in a large diameter range from 0.2 µm up to possibly more than 100 µm depending on sampling conditions (Renard et al., 2016). Its capabilities overpass those of preceding optical particle counters (OPCs) allowing the characterization of all kind of aerosols from submicronic-sized absorbing carbonaceous particles in polluted air to very coarse particles (> 10–20 µm in diameter) in desert dust plumes or fog and clouds. LOAC's light and compact design allows measurements under all kinds of balloons, on-board unmanned aerial vehicles (UAVs) and at ground level. We illustrate here the first LOAC airborne results obtained from a UAV and a variety of scientific balloons. The UAV was deployed in a peri-urban environment near Bordeaux in France. Balloon operations include (i) tethered balloons deployed in urban environments in Vienna (Austria) and Paris (France), (ii) pressurized balloons drifting in the lower troposphere over the western Mediterranean (during the Chemistry-Aerosol Mediterranean Experiment – ChArMEx campaigns), (iii) meteorological sounding balloons launched in the western Mediterranean region (ChArMEx) and from Aire-sur-l'Adour in south-western France (VOLTAIRE-LOAC campaign). More focus is put on measurements performed in the Mediterranean during (ChArMEx) and especially during African dust transport events to illustrate the original capability of balloon-borne LOAC to monitor in situ coarse mineral dust particles. In particular, LOAC has detected unexpected large particles in desert sand plumes.