Stratospheric Aerosol Loading Research Articles

Aerosol particle size distribution in the stratosphere retrieved from SCIAMACHY limb measurements

Abstract. Information about aerosols in the Earth's atmosphere is of a great importance in the scientific community. While tropospheric aerosol influences the radiative balance of the troposphere and affects human health, stratospheric aerosol plays an important role in atmospheric chemistry and climate change. In particular, information about the amount and distribution of stratospheric aerosols is required to initialize climate models, as well as validate aerosol microphysics models and investigate geoengineering. In addition, good knowledge of stratospheric aerosol loading is needed to increase the retrieval accuracy of key trace gases (e.g. ozone or water vapour) when interpreting remote sensing measurements of the scattered solar light. The most commonly used characteristics to describe stratospheric aerosols are the aerosol extinction coefficient and Ångström coefficient. However, the use of particle size distribution parameters along with the aerosol number density is a more optimal approach. In this paper we present a new retrieval algorithm to obtain the particle size distribution of stratospheric aerosol from space-borne observations of the scattered solar light in the limb-viewing geometry. While the mode radius and width of the aerosol particle size distribution are retrieved, the aerosol particle number density profile remains unchanged. The latter is justified by a lower sensitivity of the limb-scattering measurements to changes in this parameter. To our knowledge this is the first data set providing two parameters of the particle size distribution of stratospheric aerosol from space-borne measurements of scattered solar light. Typically, the mode radius and w can be retrieved with an uncertainty of less than 20 %. The algorithm was successfully applied to the tropical region (20° N–20° S) for 10 years (2002–2012) of SCIAMACHY observations in limb-viewing geometry, establishing a unique data set. Analysis of this new climatology for the particle size distribution parameters showed clear increases in the mode radius after the tropical volcanic eruptions, whereas no distinct behaviour of the absolute distribution width could be identified. A tape recorder, which describes the time lag as the perturbation propagates to higher altitudes, was identified for both parameters after the volcanic eruptions. A quasi-biannual oscillation (QBO) pattern at upper altitudes (28–32 km) is prominent in the anomalies of the analysed parameters. A comparison of the aerosol effective radii derived from SCIAMACHY and SAGE II data was performed. The average difference is found to be around 30 % at the lower altitudes, decreasing with increasing height to almost zero around 30 km. The data sample available for the comparison is, however, relatively small.

Stratospheric Smoke With Unprecedentedly High Backscatter Observed by Lidars Above Southern France

AbstractExtreme pyroconvection events triggered by wildfires in northwest Canada and United States during August 2017 resulted in vast injection of combustion products into the stratosphere. The plumes of stratospheric smoke were observed by lidars at Observatoire de Haute‐Provence (OHP) for many weeks that followed the fires as distinct aerosol layers with backscatter reaching unprecedentedly high values for a nonvolcanic aerosol layer. We use spaceborne CALIOP lidar to track the spatiotemporal evolution of the smoke plumes before their detection at OHP. A remarkable agreement between ground‐ and spaced‐based lidars sampling the same smoke plume on a particular date allowed us to extrapolate the OHP observations to a regional scale, where CALIOP reported extreme aerosol optical depth values as high as 0.21. On a monthly time scale, the lidar observations indicate that boreal summer 2017 forest fires had a hemisphere‐scale impact on stratospheric aerosol load, similar to that of moderate volcanic eruptions.

Equatorward dispersion of a high-latitude volcanic plume and its relation to the Asian summer monsoon: a case study of the Sarychev eruption in 2009

Abstract. Tropical volcanic eruptions have been widely studied for their significant contribution to stratospheric aerosol loading and global climate impacts, but the impact of high-latitude volcanic eruptions on the stratospheric aerosol layer is not clear and the pathway of transporting aerosol from high latitudes to the tropical stratosphere is not well understood. In this work, we focus on the high-latitude volcano Sarychev (48.1° N, 153.2° E), which erupted in June 2009, and the influence of the Asian summer monsoon (ASM) on the equatorward dispersion of the volcanic plume. First, the sulfur dioxide (SO2) emission time series and plume height of the Sarychev eruption are estimated with SO2 observations of the Atmospheric Infrared Sounder (AIRS) and a backward trajectory approach using the Lagrangian particle dispersion model Massive–Parallel Trajectory Calculations (MPTRAC). Then, the transport and dispersion of the plume are simulated using the derived SO2 emission time series. The transport simulations are compared with SO2 observations from AIRS and validated with aerosol observations from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS). The MPTRAC simulations show that about 4 % of the sulfur emissions were transported to the tropical stratosphere within 50 days after the beginning of the eruption, and the plume dispersed towards the tropical tropopause layer (TTL) through isentropic transport above the subtropical jet. The MPTRAC simulations and MIPAS aerosol data both show that between the potential temperature levels of 360 and 400 K, the equatorward transport was primarily driven by anticyclonic Rossby wave breaking enhanced by the ASM in boreal summer. The volcanic plume was entrained along the anticyclone flows and reached the TTL as it was transported southwestwards into the deep tropics downstream of the anticyclone. Further, the ASM anticyclone influenced the pathway of aerosols by isolating an aerosol hole inside of the ASM, which was surrounded by aerosol-rich air outside. This transport barrier was best indicated using the potential vorticity gradient approach. Long-term MIPAS aerosol detections show that after entering the TTL, aerosol from the Sarychev eruption remained in the tropical stratosphere for about 10 months and ascended slowly. The ascent speed agreed well with the ascent speed of the water vapor tape recorder. Furthermore, a hypothetical MPTRAC simulation for a wintertime eruption was carried out. It is shown that under winter atmospheric circulations, the equatorward transport of the plume would be suppressed by the strong subtropical jet and weak wave breaking events. In this hypothetical scenario, a high-latitude volcanic eruption would not be able to contribute to the tropical stratospheric aerosol layer.

Particulate sulfur in the upper troposphere and lowermost stratosphere – sources and climate forcing

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.

Global warming and ocean stratification: A potential result of large extraterrestrial impacts

AbstractThe prevailing paradigm for the climatic effects of large asteroid or comet impacts is a reduction in sunlight and significant short‐term cooling caused by atmospheric aerosol loading. Here we show, using global climate model experiments, that the large increases in stratospheric water vapor that can occur upon impact with the ocean cause radiative forcings of over +20 W m−2 in the case of 10 km sized bolides. The result of such a positive forcing is rapid climatic warming, increased upper ocean stratification, and potentially disruption of upper ocean ecosystems. Since two thirds of the world's surface is ocean, we suggest that some bolide impacts may actually warm climate overall. For impacts producing both stratospheric water vapor and aerosol loading, radiative forcing by water vapor can reduce or even cancel out aerosol‐induced cooling, potentially causing 1–2 decades of increased temperatures in both the upper ocean and on the land surface. Such a response, which depends on the ratio of aerosol to water vapor radiative forcing, is distinct from many previous scenarios for the climatic effects of large bolide impacts, which mostly account for cooling from aerosol loading. Finally, we discuss how water vapor forcing from bolide impacts may have contributed to two well‐known phenomena: extinction across the Cretaceous/Paleogene boundary and the deglaciation of the Neoproterozoic snowball Earth.

Impact of a moderate volcanic eruption on chemistry in the lower stratosphere: balloon-borne observations and model calculations

Abstract. 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.

Long-Term Variation of Stratospheric Aerosols Observed With Lidar from 1982 to 2014 Over Tsukuba, Japan

The vertical distribution of stratospheric aerosols has been measured with lidars at the Meteorological Research Institute (MRI) over Tsukuba since 1982. After two major volcanic eruptions (Mt. El Chichon in 1982 and Mt. Pinatubo in 1991), stratospheric aerosol loading increased about 50–100 times compared with the background level which was observed for 1997-2000. From 2000 to 2012, a slight increase (5.3% year–1) was observed by some volcanic eruptions. This long-term lidar data have been used for assessing of impact of the stratospheric aerosols on climate and the ozone layer.

Positive trends in Southern Hemisphere carbonyl sulfide

AbstractTransport of carbonyl sulfide (OCS) from the troposphere to the stratosphere contributes sulfur to the stratospheric aerosol layer, which reflects incoming short‐wave solar radiation, cooling the climate system. Previous analyses of OCS observations have shown no significant trend, suggesting that OCS is unlikely to be a major contributor to the reported increases in stratospheric aerosol loading and indicating a balanced OCS budget. Here we present analyses of ground‐based Fourier transform spectrometer measurements of OCS at three Southern Hemisphere sites spanning 34.45°S to 77.80°S. At all three sites statistically significant positive trends are seen from 2001 to 2014 with an observed overall trend in total column OCS at Wollongong of 0.73 ± 0.03%/yr, at Lauder of 0.43 ± 0.02%/yr, and at Arrival Heights of 0.45 ± 0.05%/yr. These observed trends in OCS imply that the OCS budget is not balanced and could contribute to constraints on current estimates of sources and sinks.

Evaluation of Erythemal ultraviolet solar radiation over Saudi Arabia

To characterize and reduce the harmful effects of Erythemal ultraviolet radiation (EUV), it is vital to recognize the spatial distribution and temporal variation of EUV radiation under various meteorological conditions. In light of these requirements, the problem we address here is to understand the results of a study performed to assess the influence of stratospheric ozone and aerosol loading on the receipt of EUV at six sites located in Saudi Arabia. The selected sites were chosen to represent the climatic zones of the north, middle, and south of Saudi Arabia. Intensive satellite-based measurements of the atmosphere over the period 1979–2005 obtained from the Total Ozone Mapping Spectrometer (TOMS) website (ftp://toms.gsfc.nasa.gov) were used, with a four year gap from 1993 to 1996. The results hint that, in spite of the significant decrease in stratospheric ozone, there is a clear decreasing trend in the EUV data series due to the increase in the aerosol loading during summer months. For the other months the correlation is not clear and in all cases there was no decrease in the EUV radiation trend outside summer months, with few exceptions.

Global atmospheric sulfur budget under volcanically quiescent conditions: Aerosol‐chemistry‐climate model predictions and validation

AbstractThe global atmospheric sulfur budget and its emission dependence have been investigated using the coupled aerosol‐chemistry‐climate model SOCOL‐AER. The aerosol module comprises gaseous and aqueous sulfur chemistry and comprehensive microphysics. The particle distribution is resolved by 40 size bins spanning radii from 0.39 nm to 3.2 μm, including size‐dependent particle composition. Aerosol radiative properties required by the climate model are calculated online from the aerosol module. The model successfully reproduces main features of stratospheric aerosols under nonvolcanic conditions, including aerosol extinctions compared to Stratospheric Aerosol and Gas Experiment II (SAGE II) and Halogen Occultation Experiment, and size distributions compared to in situ measurements. The calculated stratospheric aerosol burden is 109 Gg of sulfur, matching the SAGE II‐based estimate (112 Gg). In terms of fluxes through the tropopause, the stratospheric aerosol layer is due to about 43% primary tropospheric aerosol, 28% SO2, 23% carbonyl sulfide (OCS), 4% H2S, and 2% dimethyl sulfide (DMS). Turning off emissions of the short‐lived species SO2, H2S, and DMS shows that OCS alone still establishes about 56% of the original stratospheric aerosol burden. Further sensitivity simulations reveal that anticipated increases in anthropogenic SO2 emissions in China and India have a larger influence on stratospheric aerosols than the same increase in Western Europe or the U.S., due to deep convection in the western Pacific region. However, even a doubling of Chinese and Indian emissions is predicted to increase the stratospheric background aerosol burden only by 9%. In contrast, small to moderate volcanic eruptions, such as that of Nabro in 2011, may easily double the stratospheric aerosol loading.

Total ozone trends and variability during 1979–2012 from merged data sets of various satellites

Abstract. The study presents a long-term statistical trend analysis of total ozone data sets obtained from various satellites. A multi-variate linear regression was applied to annual mean zonal mean data using various natural and anthropogenic explanatory variables that represent dynamical and chemical processes which modify global ozone distributions in a changing climate. The study investigated the magnitude and zonal distribution of the different atmospheric chemical and dynamical factors contributing to long-term total ozone changes. The regression model included the equivalent effective stratospheric chlorine (EESC), the 11-year solar cycle, the quasi-biennial oscillation (QBO), stratospheric aerosol loading describing the effects from major volcanic eruptions, the El Niño–Southern Oscillation (ENSO), the Arctic and Antarctic oscillation (AO/AAO), and accumulated eddy heat flux (EHF), the latter representing changes due to the Brewer–Dobson circulation. The total ozone column data set used here comprises the Solar Backscater Ultraviolet SBUV/SBUV-2 merged ozone data set (MOD) V8.6, the merged data set of the Solar Backscaterr Ultraviolet, the Total Ozone Mapping Spectrometer and the Ozone Monitoring Instrument SBUV/TOMS/OMI (1979–2012) MOD V8.0 and the merged data set of the Global Ozone Monitoring Experiment, the Scanning Imaging Absorption spectroMeter for Atmospheric ChartograpHY and the Global Ozone Monitoring Experiment 2 GOME/SCIAMACHY/GOME-2 (GSG) (1995–2012). The trend analysis was performed for twenty-six 5° wide latitude bands from 65° S to 65° N, and the analysis explained most of the ozone variability to within 70 to 90%. The results show that QBO dominates the ozone variability in the tropics (±7 DU) while at higher latitudes, the dynamical indices, AO/AAO and eddy heat flux, have substantial influence on total ozone variations by up to ±10 DU. The contribution from volcanic aerosols is only prominent during the major eruption periods (El Chichón and Mt. Pinatubo), and together with the ENSO signal, is more evident in the Northern Hemisphere. The signature of the solar cycle covers all latitudes and contributes about 10 DU from solar maximum to solar minimum. EESC is found to be a main contributor to the long-term ozone decline and the trend changes after the end of the 1990s. From the EESC fits, statistically significant upward trends after 1997 were found in the extratropics, which points at the slowing of ozone decline and the onset of ozone recovery. The EESC based trends are compared with the trends obtained from the statistical piecewise linear trend (PWLT) model (known as hockey stick) with a turnaround in 1997 to examine the differences between both approaches. In case of the SBUV merged V8.6 data the EESC and PWLT trends before and after 1997 are in good agreement (within 2 σ), however, the positive post-1997 linear trends from the PWLT regression are not significant within 2 σ. A sensitivity study is carried out by comparing the regression results, using SBUV/SBUV-2 MOD V8.6 merged time series (1979–2012) and a merged data set combining SBUV/SBUV-2 (1979–June 1995) and GOME/SCIAMACHY/GOME-2 ("GSG") WFDOAS (Weighting Function DOAS) (July 1995–2012) as well as SBUV/TOMS/OMI MOD V8.0 (1979–2012) in the regression analysis in order to investigate the uncertainty in the long-term trends due to different ozone data sets and data versions. Replacing the late SBUV/SBUV-2 merged data record with GSG data (unscaled and adjusted) leads to very similar results demonstrating the high consistency between satellite data sets. However, the comparison of the new SBUV/SBUV-2 MOD V8.6 with the MOD V8.0 and MOD8.6/GSG data showed somewhat smaller sensitivities with regard to several proxies as well as the linear EESC trends. On the other hand, the PWLT trends after 1997 show some differences, however, within the 2 σ error bars the PWLT trends agree with each other for all three data sets.

A tropical West Pacific OH minimum and implications for stratospheric composition

Abstract. Most of the short-lived biogenic and anthropogenic chemical species that are emitted into the atmosphere break down efficiently by reaction with OH and do not reach the stratosphere. Here we show the existence of a pronounced minimum in the tropospheric column of ozone over the West Pacific, the main source region for stratospheric air, and suggest a corresponding minimum of the tropospheric column of OH. This has the potential to amplify the impact of surface emissions on the stratospheric composition compared to the impact when assuming globally uniform OH conditions. Specifically, the role of emissions of biogenic halogenated species for the stratospheric halogen budget and the role of increasing emissions of SO2 in Southeast Asia or from minor volcanic eruptions for the increasing stratospheric aerosol loading need to be reassessed in light of these findings. This is also important since climate change will further modify OH abundances and emissions of halogenated species. Our study is based on ozone sonde measurements carried out during the TransBrom cruise with the RV Sonne roughly along 140–150° E in October 2009 and corroborating ozone and OH measurements from satellites, aircraft campaigns and FTIR instruments. Model calculations with the GEOS-Chem Chemistry and Transport Model (CTM) and the ATLAS CTM are used to simulate the tropospheric OH distribution over the West Pacific and the transport pathways to the stratosphere. The potential effect of the OH minimum on species transported into the stratosphere is shown via modeling the transport and chemistry of CH2Br2 and SO2.

Odin–OSIRIS detection of the Chelyabinsk meteor

Abstract. On 15 February 2013 an 11 000 ton meteor entered Earth's atmosphere southeast of Chelyabinsk, creating a large fireball at 23 km altitude. The resulting stratospheric aerosol loading was detected by the Ozone Mapping and Profiler Suite (OMPS) in a high-altitude polar belt. This work confirms the presence and lifetime of the stratospheric debris using the Optical Spectrograph and InfraRed Imaging System (OSIRIS) onboard the Odin satellite. Although OSIRIS coverage begins in mid-March, the measurements show a belt of enhanced scattering near 35 km altitude between 50° N and 70° N. Initially, enhancements show increased scattering of up to 15% over the background conditions, decaying in intensity and dropping in altitude until they are indistinguishable from background conditions by mid-May. An inversion is also attempted using the standard OSIRIS processing algorithm to determine the extinction in the meteoric debris.

Effects on winter circulation of short and long term solar wind changes

Indices of the North Atlantic Oscillation and the Arctic Oscillation show correlations on the day-to-day timescale with the solar wind speed (SWS). Minima in the indices were found on days of SWS minima during years of high stratospheric aerosol loading. The spatial distribution of surface pressure changes during 1963–2011 with day-to-day changes in SWS shows a pattern resembling the NAO. Such a pattern was noted for year-to-year variations by Boberg and Lundstedt (2002), who compared NAO variations with the geo-effective solar wind electric field (the monthly average SWS multiplied by the average southward component, i.e., negative Bz component, of the interplanetary magnetic field). The spatial distribution of the correlations of geopotential height changes in the troposphere and stratosphere with the SWS; the geo-effective electric field (SWS∗Bz); and the solar 10.7cm flux suggests that solar wind inputs connected to the troposphere via the global electric circuit, together with solar ultraviolet irradiance acting on the stratosphere, affect regional atmospheric dynamics.

The effect of aerosols on long wave radiation and global warming

The effect of aerosols on long wave (LW) radiation was studied based on narrowband LW calculations in a reference mid-latitude summer atmosphere with and without aerosols. Aerosols were added to the narrowband LW scheme based on their typical schematic observed spectral and vertical behaviour over European land areas. This was found to agree also with the spectral aerosol data from the Lan Zhou University Semi-Arid Climate Observatory and Laboratory measurement stations in the north-western China.A volcanic stratospheric aerosol load was found to induce local LW warming and a stronger column “greenhouse effect” than a doubled CO2 concentration. A heavy near-surface aerosol load was found to increase the downwelling LW radiation to the surface and to reduce the outgoing LW radiation, acting very much like a thin low cloud in increasing the LW greenhouse effect of the atmosphere. The short wave reflection of white aerosol has, however, stronger impact in general, but the aerosol LW greenhouse effect is non-negligible under heavy aerosol loads.

35 yr of stratospheric aerosol measurements at Garmisch-Partenkirchen: from Fuego to Eyjafjallajökull, and beyond

Abstract. Lidar measurements at Garmisch-Partenkirchen (Germany) have almost continually delivered backscatter coefficients of stratospheric aerosol since 1976. The time series is dominated by signals from the particles injected into or formed in the stratosphere due to major volcanic eruptions, in particular those of El Chichon (Mexico, 1982) and Mt Pinatubo (Philippines, 1991). Here, we focus more on the long-lasting background period since the late 1990s and 2006, in view of processes maintaining a residual lower-stratospheric aerosol layer in absence of major eruptions, as well as the period of moderate volcanic impact afterwards. During the long background period the stratospheric backscatter coefficients reached a level even below that observed in the late 1970s. This suggests that the predicted potential influence of the strongly growing air traffic on the stratospheric aerosol loading is very low. Some correlation may be found with single strong forest-fire events, but the average influence of biomass burning seems to be quite limited. No positive trend in background aerosol can be resolved over a period as long as that observed by lidar at Mauna Loa. We conclude that the increase of our integrated backscatter coefficients starting in 2008 is mostly due to volcanic eruptions with explosivity index 4, penetrating strongly into the stratosphere. Most of them occurred in the mid-latitudes. A key observation for judging the role of eruptions just reaching the tropopause region was that of the plume from the Icelandic volcano Eyjafjallajökull above Garmisch-Partenkirchen (April 2010) due to the proximity of that source. The top altitude of the ash above the volcano was reported just as 9.3 km, but the lidar measurements revealed enhanced stratospheric aerosol up to 14.3 km. Our analysis suggests for two or three of the four measurement days the presence of a stratospheric contribution from Iceland related to quasi-horizontal transport, differing from the strong descent of the layers entering Central Europe at low altitudes. The backscatter coefficients within the first 2 km above the tropopause exceed the stratospheric background by a factor of four to five. In addition, Asian and Saharan dust layers were identified in the free troposphere, Asian dust most likely even in the stratosphere.

Effects of stratospheric sulfate aerosol geo‐engineering on cirrus clouds

Cooling the Earth through the injection of sulphate into the stratosphere is one of the most discussed geo‐engineering (GE) schemes. Stratospheric aerosols can sediment into the troposphere, modify the aerosol composition and thus might impact cirrus clouds. We use a global climate model with a physically based parametrization for cirrus clouds in order to investigate possible microphysical and dynamical effects. We find that enhanced stratospheric aerosol loadings as proposed by several GE approaches will likely lead to a reduced ice crystal nucleation rate and thus optically thinner cirrus clouds. These optically thinner cirrus clouds exert a strong negative cloud forcing in the long‐wave which contributes by 60% to the overall net GE forcing. This shows that indirect effects of stratospheric aerosols on cirrus clouds may be important and need to be considered in order to estimate the maximum cooling derived from stratospheric GE.

Analysis of stratospheric NO<sub>2</sub> trends above Jungfraujoch using ground-based UV-visible, FTIR, and satellite nadir observations

Abstract. The trend in stratospheric NO2 column at the NDACC (Network for the Detection of Atmospheric Composition Change) station of Jungfraujoch (46.5° N, 8.0° E) is assessed using ground-based FTIR and zenith-scattered visible sunlight SAOZ measurements over the period 1990 to 2009 as well as a composite satellite nadir data set constructed from ERS-2/GOME, ENVISAT/SCIAMACHY, and METOP-A/GOME-2 observations over the 1996–2009 period. To calculate the trends, a linear least squares regression model including explanatory variables for a linear trend, the mean annual cycle, the quasi-biennial oscillation (QBO), solar activity, and stratospheric aerosol loading is used. For the 1990–2009 period, statistically indistinguishable trends of −3.7 ± 1.1% decade−1 and −3.6 ± 0.9% decade−1 are derived for the SAOZ and FTIR NO2 column time series, respectively. SAOZ, FTIR, and satellite nadir data sets show a similar decrease over the 1996–2009 period, with trends of −2.4 ± 1.1% decade−1, −4.3 ± 1.4% decade−1, and −3.6 ± 2.2% decade−1, respectively. The fact that these declines are opposite in sign to the globally observed +2.5% decade−1 trend in N2O, suggests that factors other than N2O are driving the evolution of stratospheric NO2 at northern mid-latitudes. Possible causes of the decrease in stratospheric NO2 columns have been investigated. The most likely cause is a change in the NO2/NO partitioning in favor of NO, due to a possible stratospheric cooling and a decrease in stratospheric chlorine content, the latter being further confirmed by the negative trend in the ClONO2 column derived from FTIR observations at Jungfraujoch. Decreasing ClO concentrations slows the NO + ClO → NO2 + Cl reaction and a stratospheric cooling slows the NO + O3 → NO2 + O2 reaction, leaving more NOx in the form of NO. The slightly positive trends in ozone estimated from ground- and satellite-based data sets are also consistent with the decrease of NO2 through the NO2 + O3 → NO3 + O2 reaction. Finally, we cannot rule out the possibility that a strengthening of the Dobson-Brewer circulation, which reduces the time available for N2O photolysis in the stratosphere, could also contribute to the observed decline in stratospheric NO2 above Jungfraujoch.

Temperature thresholds for chlorine activation and ozone loss in the polar stratosphere

Abstract. Low stratospheric temperatures are known to be responsible for heterogeneous chlorine activation that leads to polar ozone depletion. Here, we discuss the temperature threshold below which substantial chlorine activation occurs. We suggest that the onset of chlorine activation is dominated by reactions on cold binary aerosol particles, without the formation of polar stratospheric clouds (PSCs), i.e. without any significant uptake of HNO3 from the gas phase. Using reaction rates on cold binary aerosol in a model of stratospheric chemistry, a chlorine activation threshold temperature, TACL, is derived. At typical stratospheric conditions, TACL is similar in value to TNAT (within 1–2 K), the highest temperature at which nitric acid trihydrate (NAT) can exist. TNAT is still in use to parameterise the threshold temperature for the onset of chlorine activation. However, perturbations can cause TACL to differ from TNAT: TACL is dependent upon H2O and potential temperature, but unlike TNAT is not dependent upon HNO3. Furthermore, in contrast to TNAT, TACL is dependent upon the stratospheric sulfate aerosol loading and thus provides a means to estimate the impact on polar ozone of strong volcanic eruptions and some geo-engineering options, which are discussed. A parameterisation of TACL is provided here, allowing it to be calculated for low solar elevation (or high solar zenith angle) over a comprehensive range of stratospheric conditions. Considering TACL as a proxy for chlorine activation cannot replace a detailed model calculation, and polar ozone loss is influenced by other factors apart from the initial chlorine activation. However, TACL provides a more accurate description of the temperature conditions necessary for chlorine activation and ozone loss in the polar stratosphere than TNAT.

Global electric circuit modulation of winter cyclone vorticity in the northern high latitudes

Small changes in extended winter (November–March) 500hPa vorticity area index (VAI) values for the 60–80°N latitude band are shown to be positively correlated with changes in a proxy for the high latitude ionosphere-to-surface current density Jz.The proxy was obtained from low latitude Jz values, measured at Mauna Loa Observatory (MLO) during the years 1960–1961 and 1977–1982, which were taken as proportional to the global ionospheric potential Vi. Such MLO Jz values may also serve as proxies for high latitude Jz, provided that they are not used during Forbush decreases or during periods of high stratospheric aerosol loading. The MLO data were of sufficient quantity and quality to obtain high latitude Jz proxies for five northern hemisphere winters. These proxies were used in linear regressions with lagged values of anomalies in the VAI (with lags extending from −150 to +150days). For the regression analysis using VAI values from the four 1977–1982 winters, the largest R2 value occurred for a lag of +2days, and the corresponding regression coefficient was the second largest in magnitude for the 301day interval. An ANOVA test showed this result to have a statistical significance of greater than 95%. For the regression analysis using data from only the 1960–1961 winter, both the maximum slope and R2 value occurred for a lag of −3 days. However, the autocorrelation of the VAI has a width of ∼15 days, and the noise associated with the small number of data points for 1960–1961 suggests that the maxima were displaced to negative lags by noise. The overall results are consistent with Tinsley’s hypothesis that higher Jz values enhance the vorticities of relatively intense winter cyclones when latent heat is important for their development. Electric charge deposited in clouds by Jz modulates the scavenging rates for both cloud condensation nuclei and ice-forming nuclei. The hypothesis is that these modulate the updraft vigor by the Rosenfeld mechanism, thus increasing the cyclonic vorticity.