Abstract. We present a study on the stratospheric aerosol load during 2006–2015, discuss the influence from volcanism and other sources, and reconstruct an aerosol optical depth (AOD) data set in a resolution of 1∘ latitudinally and 8 days timewise. The purpose is to include the “entire” stratosphere, from the tropopause to the almost particle-free altitudes of the midstratosphere. A dynamic tropopause of 1.5 PVU was used, since it enclosed almost all of the volcanic signals in the CALIOP data set. The data were successfully cleaned from polar stratospheric clouds using a temperature threshold of 195 K. Furthermore, a method was developed to correct data when the CALIOP laser beam was strongly attenuated by volcanic aerosol, preventing a negative bias in the AOD data set. Tropospheric influence, likely from upwelling dust, was found in the extratropical transition layer in spring. Eruptions of both extratropical and tropical volcanoes that injected aerosol into the stratosphere impacted the stratospheric aerosol load for up to a year if their clouds reached lower than 20 km altitude. Deeper-reaching tropical injections rose in the tropical pipe and impacted it for several years. Our AODs mostly compare well to other long-term studies of the stratospheric AOD. Over the years 2006–2015, volcanic eruptions increased the stratospheric AOD on average by ∼40 %. In absolute numbers the stratospheric AOD and radiative forcing amounted to 0.008 and −0.2 W m−2, respectively.

Abstract. We present a study on the stratospheric aerosol load during 2006-2015, discuss the influence from volcanism and other sources, and reconstruct an AOD data-set in a resolution of 1° latitudinally and 8 days timewise. Our attempt is to include the "entire" stratosphere, from the tropopause to the almost particle free altitudes of the mid-stratosphere. A dynamic tropopause of 1.5 PVU was found to be the best suited one, enclosing almost all of the volcanic signals in the CALIOP dataset. New methods were developed to handle bias in the data. The data were successfully cleaned from polar stratospheric 10 clouds using a temperature threshold of 195 K. Furthermore, a method was developed to correct data when the CALIPSO laser beam was strongly attenuated by volcanic aerosol, preventing a negative bias in the AOD data-set. Tropospheric influence, likely from upwelling dust, was found in the extratropical transition layer in spring. Eruptions of both extratropical and tropical volcanoes that injected aerosol into the stratosphere impacted the stratospheric aerosol load for up to a year if their clouds reached lower than 20 km altitudes, whereas deeper reaching tropical injections rose in the tropical pipe and 15 impacted it for several years. Over the years 2006-2015, volcanic eruptions increased the stratospheric AOD on average by ~40%. In absolute numbers the stratospheric AOD and radiative forcing amounted to 0.008 and -0.2 Wm -2 , respectively.

Abstract. Smoke from western North American wildfires reached the stratosphere in large amounts in August 2017. Limb-oriented satellite-based sensors are commonly used for studies of wildfire aerosol injected into the stratosphere (OMPS-LP (Ozone Mapping and Profiler Suite Limb Profiler) and SAGE III/ISS (Stratospheric Aerosol and Gas Experiment III on the International Space Station)). We find that these methods are inadequate for studies of the first 1–2 months after such a strong fire event due to event termination (“saturation”). The nadir-viewing lidar CALIOP (Cloud-Aerosol LIdar with Orthogonal Polarization) is less affected due to shorter path in the smoke; furthermore, it provides a means to develop a method to correct for strong attenuation of the signal. After the initial phase, the aerosol optical depth (AOD) from OMPS-LP and CALIOP show very good agreement above the 380 K isentrope, whereas OMPS-LP tends to produce higher AOD than CALIOP in the lowermost stratosphere (LMS), probably due to reduced sensitivity at altitudes below 17 km. Time series from CALIOP of attenuation-corrected stratospheric AOD of wildfire smoke show an exponential decline during the first month after the fire, which coincides with highly significant changes in the wildfire aerosol optical properties. The AOD decline is verified by the evolution of the smoke layer composition, comparing the aerosol scattering ratio (CALIOP) to the water vapor concentration from MLS (Microwave Limb Sounder). Initially the stratospheric wildfire smoke AOD is comparable with the most important volcanic eruptions during the last 25 years. Wildfire aerosol declines much faster, 80 %–90 % of the AOD is removed with a half-life of approximately 10 d. We hypothesize that this dramatic decline is caused by photolytic loss. This process is rarely observed in the atmosphere. However, in the stratosphere this process can be studied with practically no influence from wet deposition, in contrast to the troposphere where this is the main removal path of submicron aerosol particles. Despite the loss, the aerosol particles from wildfire smoke in the stratosphere are relevant for the climate.

Stratospheric aerosol has long been seen as a pure mixture of sulfuric acid and water. Recent measurements, however, found a considerable carbonaceous fraction extending at least 8 km into the stratosphere. This fraction affects the aerosol optical depth (AOD) and the radiative properties, and hence the radiative forcing and climate impact of the stratospheric aerosol. Here we present an investigation based on a decade (2005-2014) of airborne aerosol sampling at 9-12 km altitude in the tropics and the northern hemisphere (NH) aboard the IAGOS-CARIBIC passenger aircraft. We find that the chemical composition of tropospheric aerosol in the tropics differs markedly from that at NH midlatitudes, and, that the carbonaceous stratospheric aerosol is oxygenpoor compared to the tropospheric aerosol. Furthermore, the carbonaceous and sulfurous components of the aerosol in the lowermost stratosphere (LMS) show strong increases in concentration connected with springtime subsidence from overlying stratospheric layers. The LMS concentrations significantly exceed those in the troposphere, thus clearly indicating a stratospheric production of not only the well-established sulfurous aerosol, but also a considerable but less understood carbonaceous component.npj Climate and Atmospheric Science (2019)2:40 ; https://doi.

Abstract. This study is based on fine-mode aerosol samples collected in the upper troposphere (UT) and the lowermost stratosphere (LMS) of the Northern Hemisphere extratropics during monthly intercontinental flights at 8.8–12 km altitude of the IAGOS-CARIBIC platform in the time period 1999–2014. The samples were analyzed for a large number of chemical elements using the accelerator-based methods PIXE (particle-induced X-ray emission) and PESA (particle elastic scattering analysis). Here the particulate sulfur concentrations, obtained by PIXE analysis, are investigated. In addition, the satellite-borne lidar aboard CALIPSO is used to study the stratospheric aerosol load. A steep gradient in particulate sulfur concentration extends several kilometers into the LMS, as a result of increasing dilution towards the tropopause of stratospheric, particulate sulfur-rich air. The stratospheric air is diluted with tropospheric air, forming the extratropical transition layer (ExTL). Observed concentrations are related to the distance to the dynamical tropopause. A linear regression methodology handled seasonal variation and impact from volcanism. This was used to convert each data point into stand-alone estimates of a concentration profile and column concentration of particulate sulfur in a 3 km altitude band above the tropopause. We find distinct responses to volcanic eruptions, and that this layer in the LMS has a significant contribution to the stratospheric aerosol optical depth and thus to its radiative forcing. Further, the origin of UT particulate sulfur shows strong seasonal variation. We find that tropospheric sources dominate during the fall as a result of downward transport of the Asian tropopause aerosol layer (ATAL) formed in the Asian monsoon, whereas transport down from the Junge layer is the main source of UT particulate sulfur in the first half of the year. In this latter part of the year, the stratosphere is the clearly dominating source of particulate sulfur in the UT during times of volcanic influence and under background conditions.

Aerosol composition and optical scattering from particles in the lowermost stratosphere (LMS) have been studied by comparing in-situ aerosol samples from the IAGOS-CARIBIC passenger aircraft with vertical profiles of aerosol backscattering obtained from the CALIOP lidar aboard the CALIPSO satellite. Concentrations of the dominating fractions of the stratospheric aerosol, being sulphur and carbon, have been obtained from post-flight analysis of IAGOS-CARIBIC aerosol samples. This information together with literature data on black carbon concentrations were used to calculate the aerosol backscattering which subsequently is compared with measurements by CALIOP. Vertical optical profiles were taken in an altitude range of several kilometres from and above the northern hemispheric extratropical tropopause for the years 2006-2014. We find that the two vastly different measurement platforms yield different aerosol backscattering, especially close to the tropopause where the influence from tropospheric aerosol is strong. The best agreement is found when the LMS is affected by volcanism, i.e., at elevated aerosol loadings. At background conditions, best agreement is obtained some distance (>2 km) above the tropopause in winter and spring, i.e., at likewise elevated aerosol loadings from subsiding aerosol-rich stratospheric air. This is to our knowledge the first time the CALIPSO lidar measurements have been compared to in-situ long-term aerosol measurements.

Abstract. In this study we describe a methodology to create high-vertical-resolution SO2 profiles from volcanic emissions. We demonstrate the method's performance for the volcanic clouds following the eruption of Sarychev in June 2009. The resulting profiles are based on a combination of satellite SO2 and aerosol retrievals together with trajectory modelling. We use satellite-based measurements, namely lidar backscattering profiles from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) satellite instrument, to create vertical profiles for SO2 swaths from the Atmospheric Infrared Sounder (AIRS) aboard the Aqua satellite. Vertical profiles are created by transporting the air containing volcanic aerosol seen in CALIOP observations using the FLEXible PARTicle dispersion model (FLEXPART) while preserving the high vertical resolution using the potential temperatures from the MERRA-2 (Modern-Era Retrospective analysis for Research and Application) meteorological data for the original CALIOP swaths. For the Sarychev eruption, air tracers from 75 CALIOP swaths within 9 d after the eruption are transported forwards and backwards and then combined at a point in time when AIRS swaths cover the complete volcanic SO2 cloud. Our method creates vertical distributions for column density observations of SO2 for individual AIRS swaths, using height information from multiple CALIOP swaths. The resulting dataset gives insight into the height distribution in the different sub-clouds of SO2 within the stratosphere. We have compiled a gridded high-vertical-resolution SO2 inventory that can be used in Earth system models, with a vertical resolution of 1 K in potential temperature, 61 ± 56 m, or 1.8 ± 2.9 mbar.

Abstract. In this study we describe a methodology to create high vertical resolution SO2 profiles from volcanic emissions. We demonstrate the method’s performance for the volcanic clouds following the eruption of Sarychev in June 2009. The resulting profiles are based on a combination of satellite SO2 and aerosol retrievals together with trajectory modelling. We use satellite-based measurements, namely lidar back-scattering profiles from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) satellite instrument to create vertical profiles for SO2 swaths from the Atmospheric Infrared Sounder (AIRS) aboard the Aqua satellite. Vertical profiles are created by transporting the air containing volcanic aerosol seen in CALIOP observations using the dispersion model FLEXPART, while preserving the high vertical resolution by using the potential temperatures from the MERRA-2 meteorological data for the original CALIOP swaths. For the Sarychev eruption, air tracers from 75 CALIOP swaths within 9 days after the eruption are transported forwards and backwards, and then combined at a point in time when AIRS swaths cover the complete volcanic SO2 cloud. Our method creates vertical distributions for column density observations of SO2 for individual AIRS swaths. The resulting dataset gives insight to the height distribution in the different sub-clouds of SO2 within the stratosphere. We have compiled a gridded high vertical resolution SO2 inventory that can be used in Earth system models, with vertical resolution of 1 K in potential temperature or 61 ± 56 m and 1.8 ± 2.9 mbar.