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Satellite observations have revealed an enhanced aerosol layer near the tropopause over Asia during the summer monsoon, called the “Asian Tropopause Aerosol Layer” (ATAL). In this work, aerosol particles in the ATAL were collected with a balloon-borne impactor near the tropopause region over India, using extended-duration balloon flights, in summer 2017 and winter 2018. The chemical composition of these particles was further investigated by quantitative analysis using offline ion chromatography. Nitrate (NO3-) and nitrite (NO2-) were found to be the dominant ions in the collected aerosols with values ranging between 87 and 343 ng m−3 at STP (standard temperature and pressure) during the summer campaign. In contrast, sulfate (SO42-) levels were found to be above the detection limit (>10 ng m−3 at STP) only in winter. In addition, we determined the origin of the air masses sampled during the flights using the analysis of back trajectories as well as a convective proxy from cloud-top temperature fields derived from a geostationary satellite. The results obtained from this analysis were put into the context of large-scale transport and aerosol distribution using GEOS-Chem chemical transport model simulations. The first flight in summer 2017 which sampled an air mass within the Asian monsoon anticyclone (AMA), influenced by convection over Western China, was associated with particle size diameters from 0.05 to 0.15 µm. In contrast, the second flight sampled air masses at the edge of the AMA associated with a larger particle size radius (>2 µm) with a higher NO2- concentration. The sampled air masses in winter 2018 were likely affected by smoke from the Pacific Northwest fire event in Canada, which occurred 7 months before our campaign, associated with concentration enhancements of SO42- and Ca2+. Overall, our results suggest that nitrogen-containing particles represent a large fraction of cloud-free and in-cloud aerosols populating the ATAL, which is partially in agreement with the results from aircraft measurements during the StratoClim (Stratospheric and upper tropospheric processes for better climate predictions) campaign. The exact nature of those particles is still unknown, but their coincidences with subvisible cirrus clouds and their sizes suggest nitric acid trihydrate (NAT) as a possible candidate, as NAT has already been observed in the tropical upper troposphere and lower stratosphere in other studies. Furthermore, GEOS-Chem model simulations indicate that lightning NOx emissions could have significantly impacted the production of nitrate aerosols sampled during the summer of 2017.

Remote-sensing measurements by light detection and ranging (lidar) instruments are fundamental for the monitoring of altitude-resolved aerosol optical properties. Here we validate vertical profiles of aerosol backscatter coefficient (βaer) measured by two independent lidar systems using co-located balloon-borne measurements performed by Compact Optical Backscatter Aerosol Detector (COBALD) sondes. COBALD provides high-precision in situ measurements of βaer at two wavelengths (455 and 940 nm). The two analyzed lidar systems are the research Raman Lidar for Meteorological Observations (RALMO) and the commercial CHM15K ceilometer (Lufft, Germany). We consider in total 17 RALMO and 31 CHM15K profiles, co-located with simultaneous COBALD soundings performed throughout the years 2014–2019 at the MeteoSwiss observatory of Payerne (Switzerland). The RALMO (355 nm) and CHM15K (1064 nm) measurements are converted to 455 and 940 nm, respectively, using the Ångström exponent profiles retrieved from COBALD data. To account for the different receiver field-of-view (FOV) angles between the two lidars (0.01–0.02∘) and COBALD (6∘), we derive a custom-made correction using Mie-theory scattering simulations. Our analysis shows that both lidar instruments achieve on average a good agreement with COBALD measurements in the boundary layer and free troposphere, up to 6 km altitude. For medium-high-aerosol-content measurements at altitudes below 3 km, the mean ± standard deviation difference in βaer calculated from all considered soundings is −2 % ± 37 % (−0.018 ± 0.237 Mm−1 sr−1 at 455 nm) for RALMO−COBALD and +5 % ± 43 % (+0.009 ± 0.185 Mm−1 sr−1 at 940 mm) for CHM15K−COBALD. Above 3 km altitude, absolute deviations generally decrease, while relative deviations increase due to the prevalence of air masses with low aerosol content. Uncertainties related to the FOV correction and spatial- and temporal-variability effects (associated with the balloon's drift with altitude and different integration times) contribute to the large standard deviations observed at low altitudes. The lack of information on the aerosol size distribution and the high atmospheric variability prevent an accurate quantification of these effects. Nevertheless, the excellent agreement observed in individual profiles, including fine and complex structures in the βaer vertical distribution, shows that under optimal conditions, the discrepancies with the in situ measurements are typically comparable to the estimated statistical uncertainties in the remote-sensing measurements. Therefore, we conclude that βaer profiles measured by the RALMO and CHM15K lidar systems are in good agreement with in situ measurements by COBALD sondes up to 6 km altitude.

The South Asian summer monsoon is associated with a large-scale anticyclonic circulation in the upper troposphere and lower stratosphere (UTLS), which confines the air mass inside. During boreal summer, the confinement of this air mass leads to an accumulation of aerosol between about 13 and 18 km (360 and 440 K potential temperature); this accumulation of aerosol constitutes the Asian Tropopause Aerosol Layer (ATAL). We present balloon-borne aerosol backscatter measurements of the ATAL performed by the Compact Optical Backscatter Aerosol Detector (COBALD) instrument in Nainital in northern India in August 2016, and compare these with COBALD measurements in the post-monsoon time in November 2016. The measurements demonstrate a strong variability of the ATAL's altitude, vertical extent, aerosol backscatter intensity and cirrus cloud occurrence frequency. Such a variability cannot be deduced from climatological means of the ATAL as they are derived from satellite measurements. To explain this observed variability we performed a Lagrangian back-trajectory analysis using the Chemical Lagrangian Model of the Stratosphere (CLaMS). We identify the transport pathways as well as the source regions of air parcels contributing to the ATAL over Nainital in August 2016. Our analysis reveals a variety of factors contributing to the observed day-to-day variability of the ATAL: continental convection, tropical cyclones (maritime convection), dynamics of the anticyclone and stratospheric intrusions. Thus, the air in the ATAL is a mixture of air masses coming from different atmospheric altitude layers. In addition, contributions from the model boundary layer originate in different geographic source regions. The location of the strongest updraft along the backward trajectories reveals a cluster of strong upward transport at the southern edge of the Himalayan foothills. From the top of the convective outflow level (about 13 km; 360 K) the air parcels ascend slowly to ATAL altitudes within a large-scale upward spiral driven by the diabatic heating in the anticyclonic flow of the South Asian summer monsoon at UTLS altitudes. Cases with a strong ATAL typically show boundary layer contributions from the Tibetan Plateau, the foothills of the Himalayas and other continental regions below the Asian monsoon. Weaker ATAL cases show higher contributions from the maritime boundary layer, often related to tropical cyclones, indicating a mixing of clean maritime and polluted continental air. On the one hand increasing anthropogenic emissions in the future are expected due to the strong growth of Asian economies; on the other hand the implementation of new emission control measures (in particular in China) has reduced the anthropogenic emissions of some pollutants contributing to the ATAL substantially. It needs to be monitored in the future whether the thickness and intensity of the ATAL will further increase, which will likely impact the surface climate.

We measured the vertical profiles of backscatter ratio (BSR) using the balloon-borne, lightweight Compact Optical Backscatter AerosoL Detector (COBALD) instruments above Linzhi, located in the southeastern Tibetan Plateau, in the summer of 2014. An enhanced aerosol layer in the upper troposphere–lower stratosphere (UTLS), with BSR (455 nm) > 1.1 and BSR (940 nm) > 1.4, was observed. The color index (CI) of the enhanced aerosol layer, defined as the ratio of aerosol backscatter ratios (ABSRs) at wavelengths of 940 and 455 nm, varied from 4 to 8, indicating the prevalence of fine particles with a mode radius of less than 0.1 µm. We find that unlike the very small particles (mode radius smaller than 0.04 µm) at low relative humidity (RHi < 40 %), the relatively large particles in the aerosol layer were generally very hydrophilic as their size increased dramatically with relative humidity. This result indicates that water vapor can play a very important role in increasing the size of fine particles in the UTLS over the Tibetan Plateau. Our observations provide observation-based evidence supporting the idea that aerosol particle hygroscopic growth is an important factor influencing the radiative properties of the Asian Tropopause Aerosol Layer (ATAL) during the Asian summer monsoon.

The Asian summer monsoon anticyclone (ASMA) is a major meteorological system of the upper troposphere–lower stratosphere (UTLS) during boreal summer. It is known to contain enhanced tropospheric trace gases and aerosols, due to rapid lifting from the boundary layer by deep convection and subsequent horizontal confinement. Given its dynamical structure, the ASMA represents an efficient pathway for the transport of pollutants to the global stratosphere. A detailed understanding of the thermal structure and processes in the ASMA requires accurate in situ measurements. Within the StratoClim project we performed state-of-the-art balloon-borne measurements of temperature, water vapor, ozone and aerosol backscatter from two stations on the southern slopes of the Himalayas. In total, 63 balloon soundings were conducted during two extensive monsoon-season campaigns, in August 2016 in Nainital, India (29.4° N, 79.5° E), and in July–August 2017 in Dhulikhel, Nepal (27.6° N, 85.5° E); one shorter post-monsoon campaign was also carried out in November 2016 in Nainital. These measurements provide unprecedented insights into the UTLS thermal structure, the vertical distributions of water vapor, ozone and aerosols, cirrus cloud properties and interannual variability in the ASMA. Here we provide an overview of all of the data collected during the three campaign periods, with focus on the UTLS region and the monsoon season. We analyze the vertical structure of the ASMA in terms of significant levels and layers, identified from the temperature and potential temperature lapse rates and Lagrangian backward trajectories, which provides a framework for relating the measurements to local thermodynamic properties and the large-scale anticyclonic flow. Both the monsoon-season campaigns show evidence of deep convection and confinement extending up to 1.5–2 km above the cold-point tropopause (CPT), yielding a body of air with high water vapor and low ozone which is prone to being lifted further and mixed into the free stratosphere. Enhanced aerosol backscatter also reveals the signature of the Asian tropopause aerosol layer (ATAL) over the same region of altitudes. The Dhulikhel 2017 campaign was characterized by a 5 K colder CPT on average than in Nainital 2016 and a local water vapor maximum in the confined lower stratosphere, about 1 km above the CPT. Data assessment and modeling studies are currently ongoing with the aim of fully exploring this dataset and its implications with respect to stratospheric moistening via the ASMA system and related processes.

High-resolution in situ balloon measurements of water vapour, aerosol, methane and temperature in the upper tropical tropopause layer (TTL) and lower stratosphere are used to evaluate the processes affecting the stratospheric water budget: horizontal transport (in-mixing) and hydration by cross-tropopause overshooting updrafts. The obtained in situ evidence of these phenomena are analysed using satellite observations by Aura MLS (Microwave Limb Sounder) and CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation) together with trajectory and transport modelling performed using CLaMS (Chemical Lagrangian Model of the Stratosphere) and HYSPLIT (Hybrid Single-Particle Lagrangian Integrated Trajectory) model. Balloon soundings were conducted during March 2012 in Bauru, Brazil (22.3° S) in the frame of the TRO-Pico campaign for studying the impact of convective overshooting on the stratospheric water budget. The balloon payloads included two stratospheric hygrometers: FLASH-B (Fluorescence Lyman-Alpha Stratospheric Hygrometer for Balloon) and Pico-SDLA instrument as well as COBALD (Compact Optical Backscatter Aerosol Detector) sondes, complemented by Vaisala RS92 radiosondes. Water vapour vertical profiles obtained independently by the two stratospheric hygrometers are in excellent agreement, ensuring credibility of the vertical structures observed. A signature of in-mixing is inferred from a series of vertical profiles, showing coincident enhancements in water vapour (of up to 0.5 ppmv) and aerosol at the 425 K (18.5 km) level. Trajectory analysis unambiguously links these features to intrusions from the Southern Hemisphere extratropical stratosphere, containing more water and aerosol, as demonstrated by MLS and CALIPSO global observations. The in-mixing is successfully reproduced by CLaMS simulations, showing a relatively moist filament extending to 20° S. A signature of local cross-tropopause transport of water is observed in a particular sounding, performed on a convective day and revealing water vapour enhancements of up to 0.6 ppmv as high as the 404 K (17.8 km) level. These are shown to originate from convective overshoots upwind detected by an S-band weather radar operating locally in Bauru. The accurate in situ observations uncover two independent moisture pathways into the tropical lower stratosphere, which are hardly detectable by space-borne sounders. We argue that the moistening by horizontal transport is limited by the weak meridional gradients of water, whereas the fast convective cross-tropopause transport, largely missed by global models, can have a substantial effect, at least at a regional scale.

Observations of high supersaturations with respect to ice inside cirrus clouds with high ice water content (> 0.01 g kg−1) and high crystal number densities (> 1 cm−3) are challenging our understanding of cloud microphysics and of climate feedback processes in the upper troposphere. However, single measurements of a cloudy air mass provide only a snapshot from which the persistence of ice supersaturation cannot be judged. We introduce here the "cirrus match technique" to obtain information about the evolution of clouds and their saturation ratio. The aim of these coordinated balloon soundings is to analyze the same air mass twice. To this end the standard radiosonde equipment is complemented by a frost point hygrometer, "SnowWhite", and a particle backscatter detector, "COBALD" (Compact Optical Backscatter AerosoL Detector). Extensive trajectory calculations based on regional weather model COSMO (Consortium for Small-Scale Modeling) forecasts are performed for flight planning, and COSMO analyses are used as a basis for comprehensive microphysical box modeling (with grid scale of 2 and 7 km, respectively). Here we present the results of matching a cirrus cloud to within 2–15 km, realized on 8 June 2010 over Payerne, Switzerland, and a location 120 km downstream close to Zurich. A thick cirrus cloud was detected over both measurement sites. We show that in order to quantitatively reproduce the measured particle backscatter ratios, the small-scale temperature fluctuations not resolved by COSMO must be superimposed on the trajectories. The stochastic nature of the fluctuations is captured by ensemble calculations. Possibilities for further improvements in the agreement with the measured backscatter data are investigated by assuming a very slow mass accommodation of water on ice, the presence of heterogeneous ice nuclei, or a wide span of (spheroidal) particle shapes. However, the resulting improvements from these microphysical refinements are moderate and comparable in magnitude with changes caused by assuming different regimes of temperature fluctuations for clear-sky or cloudy-sky conditions, highlighting the importance of proper treatment of subscale fluctuations. The model yields good agreement with the measured backscatter over both sites and reproduces the measured saturation ratios with respect to ice over Payerne. Conversely, the 30% in-cloud supersaturation measured in a massive 4 km thick cloud layer over Zurich cannot be reproduced, irrespective of the choice of meteorological or microphysical model parameters. The measured supersaturation can only be explained by either resorting to an unknown physical process, which prevents the ice particles from consuming the excess humidity, or – much more likely – by a measurement error, such as a contamination of the sensor housing of the SnowWhite hygrometer by a precipitation drop from a mixed-phase cloud just below the cirrus layer or from some very slight rain in the boundary layer. This uncertainty calls for in-flight checks or calibrations of hygrometers under the special humidity conditions in the upper troposphere.

Large areas of synoptic-scale ice PSCs (polar stratospheric clouds) distinguished the Arctic winter 2009/2010 from other years and revealed unprecedented evidence of water redistribution in the stratosphere. A unique snapshot of water vapor repartitioning into ice particles was obtained under extremely cold Arctic conditions with temperatures around 183 K. Balloon-borne, aircraft and satellite-based measurements suggest that synoptic-scale ice PSCs and concurrent reductions and enhancements in water vapor are tightly linked with the observed de- and rehydration signatures, respectively. In a companion paper (Part 1), water vapor and aerosol backscatter measurements from the RECONCILE (Reconciliation of essential process parameters for an enhanced predictability of Arctic stratospheric ozone loss and its climate interactions) and LAPBIAT-II (Lapland Atmosphere–Biosphere Facility) field campaigns have been analyzed in detail. This paper uses a column version of the Zurich Optical and Microphysical box Model (ZOMM) including newly developed NAT (nitric acid trihydrate) and ice nucleation parameterizations. Particle sedimentation is calculated in order to simulate the vertical redistribution of chemical species such as water and nitric acid. Despite limitations given by wind shear and uncertainties in the initial water vapor profile, the column modeling unequivocally shows that (1) accounting for small-scale temperature fluctuations along the trajectories is essential in order to reach agreement between simulated optical cloud properties and observations, and (2) the use of recently developed heterogeneous ice nucleation parameterizations allows the reproduction of the observed signatures of de- and rehydration. Conversely, the vertical redistribution of water measured cannot be explained in terms of homogeneous nucleation of ice clouds, whose particle radii remain too small to cause significant dehydration.

We present high-resolution measurements of water vapour, aerosols and clouds in the Arctic stratosphere in January and February 2010 carried out by in situ instrumentation on balloon sondes and high-altitude aircraft combined with satellite observations. The measurements provide unparalleled evidence of dehydration and rehydration due to gravitational settling of ice particles. An extreme cooling of the Arctic stratospheric vortex during the second half of January 2010 resulted in a rare synoptic-scale outbreak of ice polar stratospheric clouds (PSCs) remotely detected by the lidar aboard the CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation) satellite. The widespread occurrence of ice clouds was followed by sedimentation and consequent sublimation of ice particles, leading to vertical redistribution of water inside the vortex. A sequence of balloon and aircraft soundings with chilled mirror and Lyman- α hygrometers (Cryogenic Frostpoint Hygrometer, CFH; Fast In Situ Stratospheric Hygrometer, FISH; Fluorescent Airborne Stratospheric Hygrometer, FLASH) and backscatter sondes (Compact Optical Backscatter Aerosol Detector, COBALD) conducted in January 2010 within the LAPBIAT (Lapland Atmosphere-Biosphere Facility) and RECONCILE (Reconciliation of Essential Process Parameters for an Enhanced Predictability of Arctic Stratospheric Ozone Loss and its Climate Interactions) campaigns captured various phases of this phenomenon: ice formation, irreversible dehydration and rehydration. Consistent observations of water vapour by these independent measurement techniques show clear signatures of irreversible dehydration of the vortex air by up to 1.6 ppmv in the 20–24 km altitude range and rehydration by up to 0.9 ppmv in a 1 km thick layer below. Comparison with space-borne Aura MLS (Microwave Limb Sounder) water vapour observations allow the spatiotemporal evolution of dehydrated air masses within the Arctic vortex to be derived and upscaled.

The international research project RECONCILE has addressed central questions regarding polar ozone depletion, with the objective to quantify some of the most relevant yet still uncertain physical and chemical processes and thereby improve prognostic modelling capabilities to realistically predict the response of the ozone layer to climate change. This overview paper outlines the scope and the general approach of RECONCILE, and it provides a summary of observations and modelling in 2010 and 2011 that have generated an in many respects unprecedented dataset to study processes in the Arctic winter stratosphere. Principally, it summarises important outcomes of RECONCILE including (i) better constraints and enhanced consistency on the set of parameters governing catalytic ozone destruction cycles, (ii) a better understanding of the role of cold binary aerosols in heterogeneous chlorine activation, (iii) an improved scheme of polar stratospheric cloud (PSC) processes that includes heterogeneous nucleation of nitric acid trihydrate (NAT) and ice on non-volatile background aerosol leading to better model parameterisations with respect to denitrification, and (iv) long transient simulations with a chemistry-climate model (CCM) updated based on the results of RECONCILE that better reproduce past ozone trends in Antarctica and are deemed to produce more reliable predictions of future ozone trends. The process studies and the global simulations conducted in RECONCILE show that in the Arctic, ozone depletion uncertainties in the chemical and microphysical processes are now clearly smaller than the sensitivity to dynamic variability.

In this work, we present the first study resolving the temporal evolution of δ2H and δ18O values in cloud droplets during 13 different cloud events. The cloud events were probed on a 937 m high mountain chain in Germany in the framework of the Hill Cap Cloud Thuringia 2010 campaign (HCCT-2010) in September and October 2010. The δ values of cloud droplets ranged from −77‰ to −15‰ (δ2H) and from −12.1‰ to −3.9‰ (δ18O) over the whole campaign. The cloud water line of the measured δ values was δ2H=7.8×δ18O+13×10−3, which is of similar slope, but with higher deuterium excess than other Central European Meteoric Water Lines. Decreasing δ values in the course of the campaign agree with seasonal trends observed in rain in central Europe. The deuterium excess was higher in clouds developing after recent precipitation revealing episodes of regional moisture recycling. The variations in δ values during one cloud event could either result from changes in meteorological conditions during condensation or from variations in the δ values of the water vapor feeding the cloud. To test which of both aspects dominated during the investigated cloud events, we modeled the variation in δ values in cloud water using a closed box model. We could show that the variation in δ values of two cloud events was mainly due to changes in local temperature conditions. For the other eleven cloud events, the variation was most likely caused by changes in the isotopic composition of the advected and entrained vapor. Frontal passages during two of the latter cloud events led to the strongest temporal changes in both δ2H (≈ 6‰ per hour) and δ18O (≈ 0.6‰ per hour). Moreover, a detailed trajectory analysis for the two longest cloud events revealed that variations in the entrained vapor were most likely related to rain out or changes in relative humidity and temperature at the moisture source region or both. This study illustrates the sensitivity of stable isotope composition of cloud water to changes in large scale air mass properties and regional recycling of moisture.

In this work, we present the first observations of stable water isotopologue ratios in cloud droplets of different sizes collected simultaneously. We address the question whether the isotope ratio of droplets in a liquid cloud varies as a function of droplet size. Samples were collected from a ground intercepted cloud (= fog) during the Hill Cap Cloud Thuringia 2010 campaign (HCCT-2010) using a three-stage Caltech Active Strand Cloud water Collector (CASCC). An instrument test revealed that no artificial isotopic fractionation occurs during sample collection with the CASCC. Furthermore, we could experimentally confirm the hypothesis that the δ values of cloud droplets of the relevant droplet sizes (μm-range) were not significantly different and thus can be assumed to be in isotopic equilibrium immediately with the surrounding water vapor. However, during the dissolution period of the cloud, when the supersaturation inside the cloud decreased and the cloud began to clear, differences in isotope ratios of the different droplet sizes tended to be larger. This is likely to result from the cloud's heterogeneity, implying that larger and smaller cloud droplets have been collected at different moments in time, delivering isotope ratios from different collection times.

Advanced measurement and modelling techniques are employed to estimate the partitioning of atmospheric water between the gas phase and the condensed phase in and around cirrus clouds, and thus to identify in-cloud and out-of-cloud supersaturations with respect to ice. In November 2008 the newly developed balloon-borne backscatter sonde COBALD (Compact Optical Backscatter and AerosoL Detector) was flown 14 times together with a CFH (Cryogenic Frost point Hygrometer) from Lindenberg, Germany (52° N, 14° E). The case discussed here in detail shows two cirrus layers with in-cloud relative humidities with respect to ice between 50% and 130%. Global operational analysis data of ECMWF (roughly 1° × 1° horizontal and 1 km vertical resolution, 6-hourly stored fields) fail to represent ice water contents and relative humidities. Conversely, regional COSMO-7 forecasts (6.6 km × 6.6 km, 5-min stored fields) capture the measured humidities and cloud positions remarkably well. The main difference between ECMWF and COSMO data is the resolution of small-scale vertical features responsible for cirrus formation. Nevertheless, ice water contents in COSMO-7 are still off by factors 2–10, likely reflecting limitations in COSMO's ice phase bulk scheme. Significant improvements can be achieved by comprehensive size-resolved microphysical and optical modelling along backward trajectories based on COSMO-7 wind and temperature fields, which allow accurate computation of humidities, homogeneous ice nucleation, resulting ice particle size distributions and backscatter ratios at the COBALD wavelengths. However, only by superimposing small-scale temperature fluctuations, which remain unresolved by the numerical weather prediction models, can we obtain a satisfying agreement with the observations and reconcile the measured in-cloud non-equilibrium humidities with conventional ice cloud microphysics. Conversely, the model-data comparison provides no evidence that additional changes to ice-cloud microphysics – such as heterogeneous nucleation or changing the water vapour accommodation coefficient on ice – are required.

This paper presents results of the extensive field campaign CLACE 2010 (Cloud and Aerosol Characterization Experiment) performed in summer 2010 at the Jungfraujoch (JFJ) and the Kleine Scheidegg (KLS) in the Swiss Alps. The main goal of this campaign was to investigate the vertical variability of aerosol optical properties around the JFJ and to show the consistency of the different employed measurement techniques considering explicitly the effects of relative humidity (RH) on the aerosol light scattering. Various aerosol optical and microphysical parameters were recorded using in-situ and remote sensing techniques. In-situ measurements of aerosol size distribution, light scattering, light absorption and scattering enhancement due to water uptake were performed at the JFJ at 3580 m a.s.l.. A unique set-up allowed remote sensing measurements of aerosol columnar and vertical properties from the KLS located about 1500 m below and within the line of sight to the JFJ (horizontal distance of approx. 4.5 km). In addition, two satellite retrievals from the Spinning Enhanced Visible and Infrared Imager (SEVIRI) and the Moderate Resolution Imaging Spectroradiometer (MODIS) as well as back trajectory analyses were added to the comparison to account for a wider geographical context. All in-situ and remote sensing measurements were in clear correspondence. The ambient extinction coefficient measured in situ at the JFJ agreed well with the KLS-based LIDAR (Light Detection and Ranging) retrieval at the altitude-level of the JFJ under plausible assumptions on the LIDAR ratio. However, we can show that the quality of this comparison is affected by orographic effects due to the exposed location of the JFJ on a saddle between two mountains and next to a large glacier. The local RH around the JFJ was often higher than in the optical path of the LIDAR measurement, especially when the wind originated from the south via the glacier, leading to orographic clouds which remained lower than the LIDAR beam. Furthermore, the dominance of long-range transported Saharan dust was observed in all measurements for several days, however only for a shorter time period in the in-situ measurements due to the vertical structure of the dust plume. The optical properties of the aerosol column retrieved from SEVIRI and MODIS showed the same magnitude and a similar temporal evolution as the measurements at the KLS and the JFJ. Remaining differences are attributed to the complex terrain and simplifications in the aerosol retrieval scheme in general.

The volcanic aerosol plume resulting from the Eyjafjallajökull eruption in Iceland in April and May 2010 was detected in clear layers above Switzerland during two periods (17–19 April 2010 and 16–19 May 2010). In-situ measurements of the airborne volcanic plume were performed both within ground-based monitoring networks and with a research aircraft up to an altitude of 6000 m a.s.l. The wide range of aerosol and gas phase parameters studied at the high altitude research station Jungfraujoch (3580 m a.s.l.) allowed for an in-depth characterization of the detected volcanic aerosol. Both the data from the Jungfraujoch and the aircraft vertical profiles showed a consistent volcanic ash mode in the aerosol volume size distribution with a mean optical diameter around 3 ± 0.3 μm. These particles were found to have an average chemical composition very similar to the trachyandesite-like composition of rock samples collected near the volcano. Furthermore, chemical processing of volcanic sulfur dioxide into sulfate clearly contributed to the accumulation mode of the aerosol at the Jungfraujoch. The combination of these in-situ data and plume dispersion modeling results showed that a significant portion of the first volcanic aerosol plume reaching Switzerland on 17 April 2010 did not reach the Jungfraujoch directly, but was first dispersed and diluted in the planetary boundary layer. The maximum PM10 mass concentrations at the Jungfraujoch reached 30 μgm−3 and 70 μgm−3 (for 10-min mean values) duri ng the April and May episode, respectively. Even low-altitude monitoring stations registered up to 45 μgm−3 of volcanic ash related PM10 (Basel, Northwestern Switzerland, 18/19 April 2010). The flights with the research aircraft on 17 April 2010 showed one order of magnitude higher number concentrations over the northern Swiss plateau compared to the Jungfraujoch, and a mass concentration of 320 (200–520) μgm−3 on 18 May 2010 over the northwestern Swiss plateau. The presented data significantly contributed to the time-critical assessment of the local ash layer properties during the initial eruption phase. Furthermore, dispersion models benefited from the detailed information on the volcanic aerosol size distribution and its chemical composition.

This paper shows that most of the so far identified constituents of the tropospheric organic particulate matter belong to a semivolatile fraction for which gas phase diffusion in the lower troposphere is sufficiently fast to establish thermodynamic equilibrium between aerosol particles. For the first time analytical expressions for this process are derived. Inspection of vapor pressure data of a series of organic substances allows a rough estimate for which substances this mixing process must be considered. As general benchmarks we conclude that for typical aerosol radii between 0.1 and 1 µm this mixing process is efficient at 25°C for polar species with molecular weights up to 200 and for non-polar species up to 320. At −10°C, these values are shifted to 150 for polar and to 270 for non-polar substances. The extent of mixing of this semivolatile fraction is governed by equilibrium thermodynamics, leading to a selectively, though not completely, internally mixed aerosol. The internal mixing leads to a systematic depression of melting and deliquescence points of organic and mixed organic/inorganic aerosols, thus leading to an aerosol population in the lower troposphere which is predominantly liquid.