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We analyze cirrus cloud measurements from two dual-instrument cloud spectrometers, two hygrometers and a backscattersonde with the goal of connecting cirrus optical parameters usually accessible by remote sensing with microphysical size-resolved and bulk properties accessible in situ. Specifically, we compare the particle backscattering coefficient and depolarization ratio to the particle size distribution, effective and mean radius, surface area density, particle aspherical fraction, and ice water content. Data were acquired by instruments on board the M55 Geophysica research aircraft in July and August 2017 during the Asian Monsoon campaign based in Kathmandu, Nepal, in the framework of the StratoClim (Stratospheric and upper tropospheric processes for better climate predictions) project. Cirrus clouds have been observed over the Himalayan region between 10 km and the tropopause, situated at 17–18 km. The observed particle number densities varied between 10 and 10−4 cm−3 in the dimensional range from 1.5 to 468.5 µm in radius. Correspondingly, backscatter ratios from 1.1 up to 50 have been observed. Optical-scattering theory has been used to compare the backscattering coefficients computed from the measured particle size distribution with those directly observed by the backscattersonde. The aspect ratio of the particles, modeled as spheroids for the T-matrix approach, was left as a free parameter to match the calculations to the optical measures. The computed backscattering coefficient can be brought into good agreement with the observed one, but the match between simulated and measured depolarization ratios is insufficient. Relationships between ice particle concentration, mean and effective radius, surface area density, and ice water content with the measured backscattering coefficient are investigated for an estimate of the bulk microphysical parameters of cirrus clouds from remote sensing lidar data. The comparison between particle depolarization and aspherical fraction as measured by one of the cloud spectrometers equipped with a detector for polarization represents a novelty since it was the first time the two instruments were operated simultaneously on an aircraft. The analysis shows the difficulty of establishing an univocal link between depolarization values and the presence and amount of aspherical scatterers. This suggests the need for further investigation that could take into consideration not only the fraction of aspheric particles but also their predominant morphology.

Scattering codes are used to study the optical properties of polar stratospheric clouds (PSCs). Particle backscattering and depolarization coefficients can be computed with available scattering codes once the particle size distribution (PSD) is known and a suitable refractive index is assumed. However, PSCs often appear as external mixtures of supercooled ternary solution (STS) droplets, solid nitric acid trihydrate (NAT) and possibly ice particles, making the assumption of a single refractive index and a single morphology to model the scatterers questionable. Here we consider a set of 15 coincident measurements of PSCs above McMurdo Station, Antarctica, using ground-based lidar, a balloon-borne optical particle counter (OPC) and in situ observations taken by a laser backscattersonde and OPC during four balloon stratospheric flights from Kiruna, Sweden. This unique dataset of microphysical and optical observations allows us to test the performances of optical scattering models when both spherical and aspherical scatterers of different composition and, possibly, shapes are present. We consider particles as STS if their radius is below a certain threshold value Rth and NAT or possibly ice if it is above it. The refractive indices are assumed known from the literature. Mie scattering is used for the STS, assumed spherical. Scattering from NAT particles, considered spheroids of different aspect ratio (AR), is treated with T-matrix results where applicable. The geometric-optics–integral-equation approach is used whenever the particle size parameter is too large to allow for a convergence of the T-matrix method. The parameters Rth and AR of our model have been varied between 0.1 and 2 µm and between 0.3 and 3, respectively, and the calculated backscattering coefficient and depolarization were compared with the observed ones. The best agreement was found for Rth between 0.5 and 0.8 µm and for AR less than 0.55 and greater than 1.5. To further constrain the variability of AR within the identified intervals, we have sought an agreement with the experimental data by varying AR on a case-by-case basis and further optimizing the agreement by a proper choice of AR smaller than 0.55 and greater than 1.5 and Rth within the interval 0.5 and 0.8 µm. The ARs identified in this way cluster around the values 0.5 and 2.5. The comparison of the calculations with the measurements is presented and discussed. The results of this work help to set limits to the variability of the dimensions and asphericity of PSC solid particles, within the limits of applicability of our model based on the T-matrix theory of scattering and on assumptions on a common particle shape in a PSD and a common threshold radius for all the PSDs.

In situ measurements in the climatically important upper troposphere–lower stratosphere (UTLS) are critical for understanding controls on cloud formation, the entry of water into the stratosphere, and hydration–dehydration of the tropical tropopause layer. Accurate in situ measurement of water vapor in the UTLS however is difficult because of low water vapor concentrations ( ppmv) and a challenging low temperature–pressure environment. The StratoClim campaign out of Kathmandu, Nepal, in July and August 2017, which made the first high-altitude aircraft measurements in the Asian Summer Monsoon (ASM), also provided an opportunity to intercompare three in situ hygrometers mounted on the M-55 Geophysica: ChiWIS (Chicago Water Isotope Spectrometer), FISH (Fast In situ Stratospheric Hygrometer), and FLASH (Fluorescent Lyman-α Stratospheric Hygrometer). Instrument agreement was very good, suggesting no intrinsic technique-dependent biases: ChiWIS measures by mid-infrared laser absorption spectroscopy and FISH and FLASH by Lyman-α induced fluorescence. In clear-sky UTLS conditions (H2O ppmv), mean and standard deviations of differences in paired observations between ChiWIS and FLASH were only (-1.4±5.9) % and those between FISH and FLASH only (-1.5±8.0) %. Agreement between ChiWIS and FLASH for in-cloud conditions is even tighter, at (+0.7±7.6) %. Estimated realized instrumental precision in UTLS conditions was 0.05, 0.2, and 0.1 ppmv for ChiWIS, FLASH, and FISH, respectively. This level of accuracy and precision allows the confident detection of fine-scale spatial structures in UTLS water vapor required for understanding the role of convection and the ASM in the stratospheric water vapor budget.

The Asian monsoon anticyclone (AMA) represents one of the wettest regions in the lower stratosphere (LS) and is a key contributor to the global annual maximum in LS water vapour. While the AMA wet pool is linked with persistent convection in the region and horizontal confinement of the anticyclone, there remain ambiguities regarding the role of tropopause-overshooting convection in maintaining the regional LS water vapour maximum. This study tackles this issue using a unique set of observations from aboard the high-altitude M55-Geophysica aircraft deployed in Nepal in summer 2017 within the EU StratoClim project. We use a combination of airborne measurements (water vapour, ice water, water isotopes, cloud backscatter) together with ensemble trajectory modelling coupled with satellite observations to characterize the processes controlling water vapour and clouds in the confined lower stratosphere (CLS) of the AMA. Our analysis puts in evidence the dual role of overshooting convection, which may lead to hydration or dehydration depending on the synoptic-scale tropopause temperatures in the AMA. We show that all of the observed CLS water vapour enhancements are traceable to convective events within the AMA and furthermore bear an isotopic signature of the overshooting process. A surprising result is that the plumes of moist air with mixing ratios nearly twice the background level can persist for weeks whilst recirculating within the anticyclone, without being subject to irreversible dehydration through ice settling. Our findings highlight the importance of convection and recirculation within the AMA for the transport of water into the stratosphere.

The Asian summer monsoon is an effective pathway for aerosol particles and precursors from the planetary boundary layer over Central, South, and East Asia into the upper troposphere and lower stratosphere. An enhancement of aerosol particles within the Asian monsoon anticyclone (AMA), called the Asian tropopause aerosol layer (ATAL), has been observed by satellites. We discuss airborne in situ and remote sensing observations of aerosol microphysical properties conducted during the 2017 StratoClim field campaign within the AMA region. The aerosol particle measurements aboard the high-altitude research aircraft M55 Geophysica (maximum altitude reached of ∼20.5 km) were conducted with a modified ultra-high-sensitivity aerosol spectrometer – airborne (UHSAS-A; particle diameter detection range of 65 nm to 1 µm), the COndensation PArticle counting System (COPAS, detecting total concentrations of submicrometer-sized particles), and the New Ice eXpEriment – Cloud and Aerosol Spectrometer with Detection of POLarization (NIXE-CAS-DPOL). In the COPAS and UHSAS-A vertical particle mixing ratio (PMR) profiles and the size distribution profiles (for number, surface area, and volume concentration), the ATAL is evident as a distinct layer between ∼370 and 420 K potential temperature (Θ). Within the ATAL, the maximum detected PMRs (from the median profiles) were ∼700 mg−1 for particle diameters between 65 nm and 1 µm (UHSAS-A) and higher than 2500 mg−1 for diameters larger than 10 nm (COPAS). These values are up to 2 times higher than those previously found at similar altitudes in other tropical locations. The difference between the PMR profiles measured by the UHSAS-A and the COPAS indicate that the region below the ATAL at Θ levels from 350 to 370 K is influenced by the nucleation of aerosol particles (diameter nm). We provide detailed analyses of the vertical distribution of the aerosol particle size distributions and the PMR and compare these with previous tropical and extratropical measurements. The backscatter ratio (BR) was calculated based on the aerosol particle size distributions measured in situ. The resulting data set was compared with the vertical profiles of the BR detected by the multiwavelength aerosol scatterometer (MAS) and an airborne miniature aerosol lidar (MAL) aboard the M55 Geophysica and by the satellite-borne Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP). The data of all four methods largely agree with one another, showing enhanced BR values in the altitude range of the ATAL (between ∼15 and 18.5 km) with a maximum at 17.5 km altitude. By means of the AMA-centered equivalent latitude calculated from meteorological reanalysis data, it is shown that such enhanced values of the BR larger than 1.1 could only be observed within the confinement of the AMA.

A polarization diversity elastic backscatter lidar was deployed on the equatorial island of Palau in February and March 2016 in the framework of the EU StratoClim project. The system operated unattended in the Palau Atmosferic Observatory from 15 February to 25 March 2016 during the nighttime. Each lidar profile extends from the ground to 30 km height. Here, the dataset is presented and discussed in terms of the temperature structure of the upper troposphere–lower stratosphere (UTLS) obtained from co-located radiosoundings. The cold-point tropopause (CPT) was higher than 17 km. During the campaign, several high-altitude clouds were observed, peaking approximately 3 km below the CPT. Their occurrence was associated with cold anomalies in the upper troposphere (UT). Conversely, when warm UT anomalies occurred, the presence of cirrus was restricted to a 5 km thick layer centred 5 km below the CPT. Thin and subvisible cirrus (SVC) were frequently detected close to the CPT. The particle depolarization ratios of these cirrus were generally lower than the values detected in the UT clouds. CPT cirrus occurrence showed a correlation with cold anomalies likely triggered by stratospheric wave activity penetrating the UT. The back-trajectories study revealed a thermal and convective history compatible with the convective outflow formation for most of the cirrus clouds, suggesting that the majority of air masses related to the clouds had encountered convection in the past and had reached the minimum temperature during its transport in less than 48 h before the observation. A subset of SVC with low depolarization and no sign of significative recent uplifting may have originated in situ.

Polar stratospheric clouds (PSCs) have been observed from 2014 to 2018 from the lidar observatory at the Antarctic Concordia station (Dome C), included as a primary station in the NDACC (Network for Detection of Atmospheric Climate Change). Many of these measurements have been performed in coincidence with overpasses of the satellite-borne CALIOP (Cloud Aerosol Lidar with Orthogonal Polarization) lidar, in order to perform a comparison in terms of PSC detection and composition classification. Good agreement has been obtained, despite intrinsic differences in observation geometry and data sampling. This study reports, to our knowledge, the most extensive comparison of PSC observations by ground-based and satellite-borne lidars. The PSCs observed by the ground-based lidar and CALIOP form a complementary and congruent dataset and allow us to study the seasonal and interannual variations in PSC occurrences at Dome C. Moreover, a strong correlation with the formation temperature of NAT (nitric acid trihydrate), TNAT, calculated from local temperature, pressure, and H2O and HNO3 concentrations is shown. PSCs appear at Dome C at the beginning of June up to 26 km and start to disappear in the second half of August, when the local temperatures start to rise above TNAT. Rare PSC observations in September coincide with colder air masses below 18 km.

The StratoClim stratospheric aircraft campaign took place in summer 2017 in Nepal (27 July–10 August) and provided for the first time a wide dataset of observations of air composition inside the Asian monsoon anticyclone (AMA). In the framework of this project, with the purpose of modelling the injection of pollutants and natural compounds into the stratosphere, we performed a series of diffusive back trajectory runs along the flights' tracks. The availability of in situ measurements of trace gases has been exploited to evaluate the capability of the trajectory system to reproduce the transport in the upper troposphere–lower stratosphere (UTLS) region. The diagnostics of the convective sources and mixing in the air parcel samples have been derived by integrating the trajectory output with high-resolution observations of cloud tops from the Meteosat Second Generation (MSG1) and Himawari geostationary satellites. Back trajectories have been calculated using meteorological fields from European Centre for Medium-Range Weather Forecasts (ECMWF) reanalysis (ERA-Interim and ERA5) at 3 and 1 h resolution, using both kinematic and diabatic vertical motion. The comparison among the different trajectory runs shows, in general, a higher consistency with observed data as well as a better agreement between the diabatic and kinematic version when using ERA5-based runs with respect to ERA-Interim. Overall, a better capacity in reproducing the pollution features is finally found in the diabatic version of the ERA5 runs. We therefore adopt this setting to analyse the convective influence in the UTLS starting from the StratoClim observations. A large variety of transport conditions have been individuated during the eight flights of the campaign. The larger influence by convective injections is found from the continental sources of China and India. Only a small contribution appears to be originated from maritime regions, in particular the South Pacific and the Bay of Bengal, which, unexpectedly, was not particularly active during the period of the campaign. In addition, a mass of clean air injected from a typhoon has also been detected at around 18 km. Thin filamentary structures of polluted air, characterized by peaks in CO, are observed, mostly associated with young convective air (age less than a few days) and with a predominant South China origin. The analysis revealed a case of direct injection of highly polluted air close to the level of the tropopause (anomalies of around 80 ppbv injected at 16 km) that then kept rising inside the anticyclonic circulation. Due to the location of the campaign, air from continental India, in contrast, has been only observed to be linked to air masses that recirculated within the anticyclone for 10 to 20 d, resulting in a lower concentration of the trace gas. The analysis of a flight overpassing an intense convective system close to the southern Nepalese border revealed the injection of very young air (few hours of age) directly in the tropopause region (∼18 km), visible in the trace gases as an enhancement in CO and a depletion in the O3 one. From the whole campaign, a vertical stratification in the age of air is observed: up to 15 km, the age is less than 3 d, and these fresh air masses constitute almost the totality of the air composition. A transition layer is then individuated between 15 and 17 km, where the convective contribution is still dominant, and the ages vary between 1 and 2 weeks. Above this level, the mean age of the air sampled by the aircraft is estimated to be 20 d. There, the convective contribution rapidly decreases with height and finally becomes negligible around 20 km.

A comparison of polar stratospheric cloud (PSC) occurrence from 2006 to 2010 is presented, as observed from the ground-based lidar station at McMurdo (Antarctica) and by the satellite-borne CALIOP lidar (Cloud-Aerosol Lidar with Orthogonal Polarization) measuring over McMurdo. McMurdo (Antarctica) is one of the primary lidar stations for aerosol measurements of the NDACC (Network for Detection of Atmospheric Climate Change). The ground-based observations have been classified with an algorithm derived from the recent v2 detection and classification scheme, used to classify PSCs observed by CALIOP. A statistical approach has been used to compare ground-based and satellite-based observations, since point-to-point comparison is often troublesome due to the intrinsic differences in the observation geometries and the imperfect overlap of the observed areas. A comparison of space-borne lidar observations and a selection of simulations obtained from chemistry–climate models (CCMs) has been made by using a series of quantitative diagnostics based on the statistical occurrence of different PSC types. The distribution of PSCs over Antarctica, calculated by several CCMVal-2 and CCMI chemistry–climate models has been compared with the PSC coverage observed by the satellite-borne CALIOP lidar. The use of several diagnostic tools, including the temperature dependence of the PSC occurrences, evidences the merits and flaws of the different models. The diagnostic methods have been defined to overcome (at least partially) the possible differences due to the resolution of the models and to identify differences due to microphysics (e.g., the dependence of PSC occurrence on T−TNAT). A significant temperature bias of most models has been observed, as well as a limited ability to reproduce the longitudinal variations in PSC occurrences observed by CALIOP. In particular, a strong temperature bias has been observed in CCMVal-2 models with a strong impact on PSC formation. The WACCM-CCMI (Whole Atmosphere Community Climate Model – Chemistry-Climate Model Initiative) model compares rather well with the CALIOP observations, although a temperature bias is still present.

Studying the vertical distribution of aerosol particle physical and chemical properties in the troposphere is essential to understand the relative importance of local emission processes vs. long-range transport for column-integrated aerosol properties (e.g. the aerosol optical depth, AOD, affecting regional climate) as well as for the aerosol burden and its impacts on air quality at the ground. The main objective of this paper is to investigate the transport of desert dust in the middle troposphere and its intrusion into the planetary boundary layer (PBL) over the Po Valley (Italy), a region considered one of the greatest European pollution hotspots for the frequency that particulate matter (PM) limit values are exceeded. Events of mineral aerosol uplift from local (soil) sources and phenomena of hygroscopic growth at the ground are also investigated, possibly affecting the PM concentration in the region as well. During the PEGASOS 2012 field campaign, an integrated observing–modelling system was set up based on near-surface measurements (particle concentration and chemistry), vertical profiling (backscatter coefficient profiles from lidar and radiosoundings) and Lagrangian air mass transport simulations by FLEXPART model. Measurements were taken at the San Pietro Capofiume supersite (44°39′ N, 11°37′ E; 11 m a.s.l.), located in a rural area relatively close to some major urban and industrial emissive areas in the Po Valley. Mt. Cimone (44°12′ N, 10°42′ E; 2165 m a.s.l.) WMO/GAW station observations are also included in the study to characterize regional-scale variability. Results show that, in the Po Valley, aerosol is detected mainly below 2000 m a.s.l. with a prevalent occurrence of non-depolarizing particles ( > 50 % throughout the campaign) and a vertical distribution modulated by the PBL daily evolution. Two intense events of mineral dust transport from northern Africa (19–21 and 29 June to 2 July) are observed, with layers advected mainly above 2000 m, but subsequently sinking and mixing in the PBL. As a consequence, a non-negligible occurrence of mineral dust is observed close to the ground ( ∼ 7 % of occurrence during a 1-month campaign). The observations unambiguously show Saharan dust layers intruding the Po Valley mixing layer and directly affecting the aerosol concentrations near the surface. Finally, lidar observations also indicate strong variability in aerosol on shorter timescales (hourly). Firstly, these highlight events of hygroscopic growth of anthropogenic aerosol, visible as shallow layers of low depolarization near the ground. Such events are identified during early morning hours at high relative humidity (RH) conditions (RH > 80 %). The process is observed concurrently with high PM1 nitrate concentration (up to 15 µg cm−3) and hence mainly explicable by deliquescence of fine anthropogenic particles, and during mineral dust intrusion episodes, when water condensation on dust particles could instead represent the dominant contribution. Secondly, lidar images show frequent events (mean daily occurrence of ∼ 22 % during the whole campaign) of rapid uplift of mineral depolarizing particles in afternoon–evening hours up to 2000 m a.s.l. height. The origin of such particles cannot be directly related to long-range transport events, being instead likely linked to processes of soil particle resuspension from agricultural lands.

Vertical profiles of aerosol particle optical properties were explored in a case study near the San Pietro Capofiume (SPC) ground station during the PEGASOS Po Valley campaign in the summer of 2012. A Zeppelin NT airship was employed to investigate the effect of the dynamics of the planetary boundary layer at altitudes between ∼ 50 and 800 m above ground. Determined properties included the aerosol particle size distribution, the hygroscopic growth factor, the effective index of refraction and the light absorption coefficient. The first three parameters were used to retrieve the light scattering coefficient. Simultaneously, direct measurements of both the scattering and absorption coefficient were carried out at the SPC ground station. Additionally, a single wavelength polarization diversity elastic lidar system provided estimates of aerosol extinction coefficients using the Klett method to accomplish the inversion of the signal, for a vertically resolved comparison between in situ and remote-sensing results. Note, however, that the comparison was for the most part done in the altitude range where the overlap function is incomplete and accordingly uncertainties are larger. First, the airborne results at low altitudes were validated with the ground measurements. Agreement within approximately ±25 and ±20 % was found for the dry scattering and absorption coefficient, respectively. The single scattering albedo, ranged between 0.83 and 0.95, indicating the importance of the absorbing particles in the Po Valley region. A clear layering of the atmosphere was observed during the beginning of the flight (until ∼ 10:00 LT – local time) before the mixing layer (ML) was fully developed. Highest extinction coefficients were found at low altitudes, in the new ML, while values in the residual layer, which could be probed at the beginning of the flight at elevated altitudes, were lower. At the end of the flight (after ∼ 12:00 LT) the ML was fully developed, resulting in constant extinction coefficients at all altitudes measured on the Zeppelin NT. Lidar estimates captured these dynamic features well and good agreement was found for the extinction coefficients compared to the in situ results, using fixed lidar ratios (LR) between 30 and 70 sr for the altitudes probed with the Zeppelin. These LR are consistent with values for continental aerosol particles that can be expected in this region.

We investigated chemical and microphysical processes in the late winter in the Antarctic lower stratosphere, after the first chlorine activation and initial ozone depletion. We focused on a time interval when both further chlorine activation and ozone loss, but also chlorine deactivation, occur. We performed a comprehensive Lagrangian analysis to simulate the evolution of an air mass along a 10-day trajectory, coupling a detailed microphysical box model to a chemistry model. Model results have been compared with in situ and remote sensing measurements of particles and ozone at the start and end points of the trajectory, and satellite measurements of key chemical species and clouds along it. Different model runs have been performed to understand the relative role of solid and liquid polar stratospheric cloud (PSC) particles for the heterogeneous chemistry, and for the denitrification caused by particle sedimentation. According to model results, under the conditions investigated, ozone depletion is not affected significantly by the presence of nitric acid trihydrate (NAT) particles, as the observed depletion rate can equally well be reproduced by heterogeneous chemistry on cold liquid aerosol, with a surface area density close to background values. Under the conditions investigated, the impact of denitrification is important for the abundances of chlorine reservoirs after PSC evaporation, thus stressing the need to use appropriate microphysical models in the simulation of chlorine deactivation. We found that the effect of particle sedimentation and denitrification on the amount of ozone depletion is rather small in the case investigated. In the first part of the analyzed period, when a PSC was present in the air mass, sedimentation led to a smaller available particle surface area and less chlorine activation, and thus less ozone depletion. After the PSC evaporation, in the last 3 days of the simulation, denitrification increases ozone loss by hampering chlorine deactivation.

The case study presented here focuses on the life cycle of clouds in the anvil region of a tropical deep convective system. During the SCOUT-O3 campaign from Darwin, Northern Australia, the Hector storm system has been probed by the Geophysica high-altitude aircraft. Clouds were observed by in situ particle probes, a backscatter sonde, and a miniature lidar. Additionally, aerosol number concentrations have been measured. On 30 November 2005 a double flight took place and Hector was probed throughout its life cycle in its developing, mature, and dissipating stage. The two flights were four hours apart and focused on the anvil region of Hector in altitudes between 10.5 and 18.8 km (i.e. above 350 K potential temperature). Trajectory calculations, satellite imagery, and ozone measurements have been used to ensure that the same cloud air masses have been probed in both flights. The size distributions derived from the measurements show a change not only with increasing altitude but also with the evolution of Hector. Clearly different cloud to aerosol particle ratios as well as varying ice crystal morphology have been found for the different development stages of Hector, indicating different freezing mechanisms. The development phase exhibits the smallest ice particles (up to 300 μm) with a rather uniform morphology. This is indicative for rapid glaciation during Hector's development. Sizes of ice crystals are largest in the mature stage (larger than 1.6 mm) and even exceed those of some continental tropical deep convective clouds, also in their number concentrations. The backscatter properties and particle images show a change in ice crystal shape from the developing phase to rimed and aggregated particles in the mature and dissipating stages; the specific shape of particles in the developing phase cannot be distinguished from the measurements. Although optically thin, the clouds in the dissipating stage have a large vertical extent (roughly 6 km) and persist for at least 6 h. Thus, the anvils of these high-reaching deep convective clouds have a high potential for affecting the tropical tropopause layer by modifying the humidity and radiative budget, as well as for providing favourable conditions for subvisible cirrus formation. The involved processes may also influence the amount of water vapour that ultimately reaches the stratosphere in the tropics.

In January 2010 and December 2011, synoptic-scale polar stratospheric cloud (PSC) fields were probed during seven flights of the high-altitude research aircraft M-55 Geophysica within the RECONCILE (Reconciliation of essential process parameters for an enhanced predictability of Arctic stratospheric ozone loss and its climate interaction) and the ESSenCe (ESSenCe: ESA Sounder Campaign) projects. Particle size distributions in a diameter range between 0.46 and 40μm were recorded by four different optical in situ instruments. Three of these particle instruments are based on the detection of forward-scattered light by single particles. The fourth instrument is a grayscale optical array imaging probe. Optical particle diameters of up to 35μm were detected with particle number densities and total particle volumes exceeding previous Arctic measurements. Also, gas-phase and particle-bound NOy was measured, as well as water vapor concentrations. The optical characteristics of the clouds were measured by the remote sensing lidar MAL (Miniature Aerosol Lidar) and by the in situ backscatter sonde MAS (Multiwavelength Aerosol Scatterometer), showing the synoptic scale of the encountered PSCs. The particle mode below 2μm in size diameter has been identified as supercooled ternary solution (STS) droplets. The PSC particles in the size range above 2μm in diameter are considered to consist of nitric acid hydrates, and the particles' high HNO3 content was confirmed by the NOy instrument. Assuming a particle composition of nitric acid trihydrate (NAT), the optically measured size distributions result in particle-phase HNO3 mixing ratios exceeding available stratospheric values. Therefore the measurement uncertainties concerning probable overestimations of measured particle sizes and volumes are discussed in detail. We hypothesize that either a strong asphericity or an alternate particle composition (e.g., water ice coated with NAT) could explain our observations. In particular, with respect to the denitrification by sedimentation of large HNO3-containing particles, generally considered to be NAT, our new measurements raise questions concerning composition, shape and nucleation pathways. Answering these would improve the numerical simulation of PSC microphysical processes like cloud particle formation, growth and denitrification, which is necessary for better predictions of future polar ozone losses, especially under changing global climate conditions. Generally, it seems that the occurrence of large NAT particles – sometimes termed "NAT rocks" – are a regular feature of synoptic-scale PSCs in the Arctic.

This work quantifies the spatial distribution of different aerosol types, their seasonal variability and sources.The analysis of four years of CALIOP (Cloud–Aerosol LIdar with Orthogonal Polarization) vertically resolved aerosol data allows the identification of spatial patterns of desert dust and carbonaceous particles in different atmospheric layers. Clusters of Lagrangian back trajectories highlight the transport pathways from source regions during the dusty spring season. The analysis shows a prevalence of dust; at low heights it occurs frequently (up to 70% of available observations) and is distributed north of the Tibetan Plateau with a main contribution from the Gobi and Taklamakan deserts, and west of the Tibetan Plateau, originating from the deserts of southwest Asia and advected by the Westerlies. Above the Himalayas the dust amount is minor but still not negligible (occurrence around 20%) and mainly affected by the transport from more distant deserts sources (Sahara and Arabian Peninsula). Carbonaceous aerosol, produced mainly in northern India and eastern China, is subject to shorter-range transport and is indeed observed closer to the sources, while there is a limited amount reaching the top of the plateau. Data analysis reveals a clear seasonal variability in the frequencies of occurrence for the main aerosol types; dust is regulated principally by the monsoon dynamics, with maximal occurrence in spring. We also highlight relevant interannual differences, showing a larger presence of aerosol in the region during 2007 and 2008. The characterization of the aerosol spatial and temporal distribution in terms of observational frequency is a key piece of information that can be directly used for the evaluation of global aerosol models.

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.

We describe an airborne lidar for the characterization of atmospheric aerosol. The system has been set up in response to the need to monitor extended regions where the air traffic may be posed at risk by the presence of potentially harmful volcanic ash, and to study the characteristics of volcanic emissions both near the source region and when transported over large distances. The lidar provides backscatter and linear depolarization profiles at 532 nm, from which aerosol and cloud properties can be derived. The paper presents the characteristics and capabilities of the lidar system and gives examples of its airborne deployment. Observations from three flights, aimed at assessing the system capabilities in unperturbed atmospheric conditions, and at characterizing the emissions near a volcanic ash source (Mt. Etna) and transported far away from the source, are presented and discussed.

New particle formation (NPF), which generates nucleation mode aerosol, was observed in the tropical Upper Troposphere (UT) and Tropical Tropopause Layer (TTL) by in situ airborne measurements over South America (January–March 2005), Australia (November–December 2005), West Africa (August 2006) and Central America (2004–2007). Particularly intense NPF was found at the bottom of the TTL. Measurements with a set of condensation particle counters (CPCs) with different dp50 (50% lower size detection efficiency diameter or "cut-off diameter") were conducted on board the M-55 Geophysica in the altitude range of 12.0–20.5 km and on board the DLR Falcon-20 at up to 11.5 km altitude. On board the NASA WB-57F size distributions were measured over Central America in the 4 to 1000 nm diameter range with a system of nucleation mode aerosol spectrometers. Nucleation mode particle concentrations (NNM) were derived from these measurements which allow for identifying many NPF events with NNM in the range of thousands of particles per cm3. Over Australia and West Africa, we identified NPF in the outflow of tropical convection, in particular of a Mesoscale Convective System (MCS). Newly formed particles with NNM > 1000 cm−3 were found to coexist with ice cloud particles (dp > 2 μm) as long as cloud particle concentrations remained below 2 cm−3. The occurrence of NPF within the upper troposphere and the TTL was generally confined within 340 K to 380 K potential temperature, but NPF was of particular strength between 350 K and 370 K (i.e. ~1–4 km below the cold point tropopause). Analyses of the aerosol volatility (at 250 °C) show that in the TTL on average 75–90% of the particles were volatile, compared to typically only 50% in the extra-tropical UT, indicative for the particles to mainly consist of H2SO4-H2O and possibly organic compounds. Along two flight segments over Central and South America (24 February 2005 and 7 August 2006, at 12.5 km altitude) in cloud free air, above thin cirrus, particularly high NNM were observed. Recent lifting had influenced the probed air masses, and NNM reached up to 16 000 particles cm−3 (ambient concentration). A sensitivity study using an aerosol model, which includes neutral and ion induced nucleation processes, simulates NNM in reasonable agreement with the in situ observations of clear-air NPF. Based on new, stringent multi-CPC criteria, our measurements corroborate the hypothesis that the tropical UT and the TTL are regions supplying freshly nucleated particles. Our findings narrow the altitude of the main source region to the bottom TTL, i.e. to the level of main tropical convection outflow, and, by means of measurements of carbon monoxide, they indicate the importance of anthropogenic emissions in NPF. After growth and/or coalescence the nucleation mode particles may act as cloud condensation nuclei in the tropical UT, or, upon ascent into the stratosphere, contribute to maintain the stratospheric background aerosol.

In situ measurements of ice crystal size distributions in tropical upper troposphere/lower stratosphere (UT/LS) clouds were performed during the SCOUT-AMMA campaign over West Africa in August 2006. The cloud properties were measured with a Forward Scattering Spectrometer Probe (FSSP-100) and a Cloud Imaging Probe (CIP) operated aboard the Russian high altitude research aircraft M-55 Geophysica with the mission base in Ouagadougou, Burkina Faso. A total of 117 ice particle size distributions were obtained from the measurements in the vicinity of Mesoscale Convective Systems (MCS). Two to four modal lognormal size distributions were fitted to the average size distributions for different potential temperature bins. The measurements showed proportionately more large ice particles compared to former measurements above maritime regions. With the help of trace gas measurements of NO, NOy, CO2, CO, and O3 and satellite images, clouds in young and aged MCS outflow were identified. These events were observed at altitudes of 11.0 km to 14.2 km corresponding to potential temperature levels of 346 K to 356 K. In a young outflow from a developing MCS ice crystal number concentrations of up to (8.3 ± 1.6) cm−3 and rimed ice particles with maximum dimensions exceeding 1.5 mm were found. A maximum ice water content of 0.05 g m−3 was observed and an effective radius of about 90 μm. In contrast the aged outflow events were more diluted and showed a maximum number concentration of 0.03 cm−3, an ice water content of 2.3 × 10−4 g m−3, an effective radius of about 18 μm, while the largest particles had a maximum dimension of 61 μm. Close to the tropopause subvisual cirrus were encountered four times at altitudes of 15 km to 16.4 km. The mean ice particle number concentration of these encounters was 0.01 cm−3 with maximum particle sizes of 130 μm, and the mean ice water content was about 1.4 × 10−4 g m−3. All known in situ measurements of subvisual tropopause cirrus are compared and an exponential fit on the size distributions is established for modelling purposes. A comparison of aerosol to ice crystal number concentrations, in order to obtain an estimate on how many ice particles may result from activation of the present aerosol, yielded low ratios for the subvisual cirrus cases of roughly one cloud particle per 30 000 aerosol particles, while for the MCS outflow cases this resulted in a high ratio of one cloud particle per 300 aerosol particles.

An FSSP-100 Optical Particle Counter designed to count and size particles in the micron range and a backscattersonde that measures in-situ particle optical properties such as backscatter and depolarization ratio, are part of the payload of the high altitude research aircraft M55 Geophysica. This aircraft was deployed in tropical field campaigns in Bauru, Brasil (TROCCINOX, 2004) Darwin, Australia (SCOUT-Darwin, 2005) and Ouagadougou, Burkina Faso (SCOUT-AMMA, 2006). In those occasions, measurements of particle size distributions and optical properties within cirrus cloud were performed. Scope of the present work is to assess and discuss the consistency between the particle volume backscatter coefficient observed by the backscattersonde and the same parameter retrieved by optical scattering theory applied to particle size distributions as measured by the FSSP-100. In addition, empirical relationships linking the optical properties measured in-situ by the backscattersonde, which generally can be obtained by remote sensing techniques (LIDAR), and microphysical bulk properties like total particle number, surface and volume density will be presented and discussed.

The EU HIBISCUS project consisted of a series of field campaigns during the intense convective summers in 2001, 2003 and 2004 in the State of São Paulo in Brazil. Its objective was to investigate the impact of deep convection on the Tropical Tropopause Layer (TTL) and the lower stratosphere by providing a new set of observational data on meteorology, tracers of horizontal and vertical transport, water vapour, clouds, and chemistry in the tropical Upper Troposphere/Lower Stratosphere (UT/LS). This was achieved using short duration research balloons to study local phenomena associated with convection over land, and long-duration balloons circumnavigating the globe to study the contrast between land and oceans. Analyses of observations of short-lived tracers, ozone and ice particles show strong episodic local updraughts of cold air across the lapse rate tropopause up to 18 or 19 km (420–440 K) in the lower stratosphere by overshooting towers. The long duration balloon and satellite measurements reveal a contrast between the composition of the lower stratosphere over land and oceanic areas, suggesting significant global impact of such events. The overshoots are shown to be well captured by non-hydrostatic meso-scale Cloud Resolving Models indicating vertical velocities of 50–60 m s−1 at the top of the Neutral Buoyancy Level (NBL) at around 14 km, but, in contrast, are poorly represented by global Chemistry-Transport Models (CTM) forced by Numerical Weather Forecast Models (NWP) underestimating the overshooting process. Finally, the data collected by the HIBISCUS balloons have allowed a thorough evaluation of temperature NWP analyses and reanalyses, as well as satellite ozone, nitrogen oxide, water vapour and bromine oxide measurements in the tropics.

We present the analysis of the impact of convection on the composition of the tropical tropopause layer region (TTL) in West-Africa during the AMMA-SCOUT campaign. Geophysica M55 aircraft observations of water vapor, ozone, aerosol and CO2 during August 2006 show perturbed values at altitudes ranging from 14 km to 17 km (above the main convective outflow) and satellite data indicates that air detrainment is likely to have originated from convective cloud east of the flights. Simulations of the BOLAM mesoscale model, nudged with infrared radiance temperatures, are used to estimate the convective impact in the upper troposphere and to assess the fraction of air processed by convection. The analysis shows that BOLAM correctly reproduces the location and the vertical structure of convective outflow. Model-aided analysis indicates that convection can influence the composition of the upper troposphere above the level of main outflow for an event of deep convection close to the observation site. Model analysis also shows that deep convection occurring in the entire Sahelian transect (up to 2000 km E of the measurement area) has a non negligible role in determining TTL composition.

Airborne in-situ observations of ClO in the tropics were made during the TROCCINOX (Aracatuba, Brazil, February 2005) and SCOUT-O3 (Darwin, Australia, November/December 2005) field campaigns. While during most flights significant amounts of ClO (≈10–20 parts per trillion, ppt) were present only in aged stratospheric air, instances of enhanced ClO mixing ratios of up to 40 ppt – significantly exceeding those expected from gas phase chemistry – were observed in air masses of a more tropospheric character. Most of these observations are associated with low temperatures or with the presence of cirrus clouds (often both), suggesting that cirrus ice particles and/or liquid aerosol at low temperatures may promote significant heterogeneous chlorine activation in the tropical upper troposphere lower stratosphere (UTLS). In two case studies, particularly high levels of ClO observed were reproduced by chemistry simulations only under the assumption that significant denoxification had occurred in the observed air. However, to reproduce the ClO observations in these simulations, O3 mixing ratios higher than observed had to be assumed, and at least for one of these flights, a significant denoxification is in contrast to the observed NO levels, suggesting that the coupling of chlorine and nitrogen compounds in the tropical UTLS may not be completely understood.

In this work, we have studied the seasonal and inter-annual variability of the aerosol vertical distribution over Sahelian Africa for the years 2006, 2007 and 2008, characterizing the different kind of aerosols present in the atmosphere in terms of their optical properties observed by ground-based and satellite instruments, and their sources searched for by using trajectory analysis. This study combines data acquired by three ground-based micro lidar systems located in Banizoumbou (Niger), Cinzana (Mali) and M'Bour (Senegal) in the framework of the African Monsoon Multidisciplinary Analysis (AMMA), by the AEROsol RObotic NETwork (AERONET) sun-photometers and by the space-based Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) onboard the CALIPSO satellite (Cloud-Aerosol Lidar and Infrared Pathfinder Observations). During winter, the lower levels air masses arriving in the Sahelian region come mainly from North, North-West and from the Atlantic area, while in the upper troposphere air flow generally originates from West Africa, crossing a region characterized by the presence of large biomass burning sources. The sites of Cinzana, Banizoumbou and M'Bour, along a transect of aerosol transport from East to West, are in fact under the influence of tropical biomass burning aerosol emission during the dry season, as revealed by the seasonal pattern of the aerosol optical properties, and by back-trajectory studies. Aerosol produced by biomass burning are observed mainly during the dry season and are confined in the upper layers of the atmosphere. This is particularly evident for 2006, which was characterized by a large presence of biomass burning aerosols in all the three sites. Biomass burning aerosol is also observed during spring when air masses originating from North and East Africa pass over sparse biomass burning sources, and during summer when biomass burning aerosol is transported from the southern part of the continent by the monsoon flow. During summer months, the entire Sahelian region is under the influence of Saharan dust aerosols: the air masses in low levels arrive from West Africa crossing the Sahara desert or from the Southern Hemisphere crossing the Guinea Gulf while in the upper layers air masses still originate from North, North-East. The maximum of the desert dust activity is observed in this period which is characterized by large AOD (above 0.2) and backscattering values. It also corresponds to a maximum in the extension of the aerosol vertical distribution (up to 6 km of altitude). In correspondence, a progressive cleaning up of the lowermost layers of the atmosphere is occurring, especially evident in the Banizoumbou and Cinzana sites. Summer is in fact characterized by extensive and fast convective phenomena. Lidar profiles show at times large dust events loading the atmosphere with aerosol from the ground up to 6 km of altitude. These events are characterized by large total attenuated backscattering values, and alternate with very clear profiles, sometimes separated by only a few hours, indicative of fast removal processes occurring, likely due to intense convective and rain activity. The inter-annual variability in the three year monitoring period is not very significant. An analysis of the aerosol transport pathways, aiming at detecting the main source regions, revealed that air originated from the Saharan desert is present all year long and it is observed in the lower levels of the atmosphere at the beginning and at the end of the year. In the central part of the year it extends upward and the lower levels are less affected by air masses from Saharan desert when the monsoon flow carries air from the Guinea Gulf and the Southern Hemisphere inland.

Trace gas and aerosol data collected in the tropical tropopause layer (TTL) between 12–18.5 km by the M55 Geophysica aircraft as part of the SCOUT-AMMA campaign over West Africa during the summer monsoon in August 2006 have been analysed in terms of their air mass origins. Analysis of domain filling back trajectories arriving over West Africa, and in the specific region of the flights, showed that the M55 flights were generally representative of air masses arriving over West Africa during the first 2 weeks of August, 2006. Air originating from the mid-latitude lower stratosphere was under-sampled (in the mid-upper TTL) whilst air masses uplifted from central Africa (into the lower TTL) were over-sampled in the latter part of the campaign. Signatures of recent (previous 10 days) origins were superimposed on the large-scale westward flow over West Africa. In the lower TTL, air masses were impacted by recent local deep convection over Africa at the level of main convective outflow (350 K, 200 hPa) and on certain days up to 370 K (100 hPa). Estimates of the fraction of air masses influenced by local convection vary from 10 to 50% depending on the method applied and from day to day during the campaign. The analysis shows that flights on 7, 8 and 11 August were more influenced by local convection than on 4 and 13 August allowing separation of trace gas and aerosol measurements into "convective" and "non-convective" flights. Strong signatures, particularly in species with short lifetimes (relative to CO2) like CO, NO and fine-mode aerosols were seen during flights most influenced by convection up to 350–365 K. Observed profiles were also constantly perturbed by uplift (as high as 39%) of air masses from the mid to lower troposphere over Asia, India, and oceanic regions resulting in import of clean oceanic (e.g. O3-poor) or polluted air masses from Asia (high O3, CO, CO2) into West Africa. Thus, recent uplift of CO2 over Asia may contribute to the observed positive CO2 gradients in the TTL over West Africa. This suggests a more significant fraction of younger air masses in the TTL and needs to taken into consideration in derivations of mean age of air. Transport of air masses from the mid-latitude lower stratosphere had an impact from the mid-TTL upwards (20–40% above 370 K) during the campaign period importing air masses with high O3 and NOy. Ozone profiles show a less pronounced lower TTL minimum than observed previously by regular ozonesondes at other tropical locations. Concentrations are less than 100 ppbv in the lower TTL and vertical gradients less steep than in the upper TTL. The air mass origin analysis and simulations of in-situ net photochemical O3 production, initialised with observations, suggest that the lower TTL is significantly impacted by uplift of O3 precursors (over Africa and Asia) leading to positive production rates (up to 2 ppbv per day) in the lower and mid TTL even at moderate NOx levels. Photochemical O3 production increases with higher NOx and H2O in air masses with O3 less than 150 ppbv.

During June, July and August 2006 five aircraft took part in a campaign over West Africa to observe the aerosol content and chemical composition of the troposphere and lower stratosphere as part of the African Monsoon Multidisciplinary Analysis (AMMA) project. These are the first such measurements in this region during the monsoon period. In addition to providing an overview of the tropospheric composition, this paper provides a description of the measurement strategy (flights performed, instrumental payloads, wing-tip to wing-tip comparisons) and points to some of the important findings discussed in more detail in other papers in this special issue. The ozone data exhibits an "S" shaped vertical profile which appears to result from significant losses in the lower troposphere due to rapid deposition to forested areas and photochemical destruction in the moist monsoon air, and convective uplift of ozone-poor air to the upper troposphere. This profile is disturbed, particularly in the south of the region, by the intrusions in the lower and middle troposphere of air from the southern hemisphere impacted by biomass burning. Comparisons with longer term data sets suggest the impact of these intrusions on West Africa in 2006 was greater than in other recent wet seasons. There is evidence for net photochemical production of ozone in these biomass burning plumes as well as in urban plumes, in particular that from Lagos, convective outflow in the upper troposphere and in boundary layer air affected by nitrogen oxide emissions from recently wetted soils. This latter effect, along with enhanced deposition to the forested areas, contributes to a latitudinal gradient of ozone in the lower troposphere. Biogenic volatile organic compounds are also important in defining the composition both for the boundary layer and upper tropospheric convective outflow. Mineral dust was found to be the most abundant and ubiquitous aerosol type in the atmosphere over Western Africa. Data collected within AMMA indicate that injection of dust to altitudes favourable for long-range transport (i.e. in the upper Sahelian planetary boundary layer) can occur behind the leading edge of mesoscale convective system (MCS) cold-pools. Research within AMMA also provides the first estimates of secondary organic aerosols across the West African Sahel and have shown that organic mass loadings vary between 0 and 2 μg m−3 with a median concentration of 1.07 μg m−3. The vertical distribution of nucleation mode particle concentrations reveals that significant and fairly strong particle formation events did occur for a considerable fraction of measurement time above 8 km (and only there). Very low concentrations were observed in general in the fresh outflow of active MCSs, likely as the result of efficient wet removal of aerosol particles due to heavy precipitation inside the convective cells of the MCSs. This wet removal initially affects all particle size ranges as clearly shown by all measurements in the vicinity of MCSs.

Processes occurring in the tropical upper troposphere (UT), the Tropical Transition Layer (TTL), and the lower stratosphere (LS) are of importance for the global climate, for stratospheric dynamics and air chemistry, and for their influence on the global distribution of water vapour, trace gases and aerosols. In this contribution we present aerosol and trace gas (in-situ) measurements from the tropical UT/LS over Southern Brazil, Northern Australia, and West Africa. The instruments were operated on board of the Russian high altitude research aircraft M-55 "Geophysica" and the DLR Falcon-20 during the campaigns TROCCINOX (Araçatuba, Brazil, February 2005), SCOUT-O3 (Darwin, Australia, December 2005), and SCOUT-AMMA (Ouagadougou, Burkina Faso, August 2006). The data cover submicron particle number densities and volatility from the COndensation PArticle counting System (COPAS), as well as relevant trace gases like N2O, ozone, and CO. We use these trace gas measurements to place the aerosol data into a broader atmospheric context. Also a juxtaposition of the submicron particle data with previous measurements over Costa Rica and other tropical locations between 1999 and 2007 (NASA DC-8 and NASA WB-57F) is provided. The submicron particle number densities, as a function of altitude, were found to be remarkably constant in the tropical UT/LS altitude band for the two decades after 1987. Thus, a parameterisation suitable for models can be extracted from these measurements. Compared to the average levels in the period between 1987 and 2007 a slight increase of particle abundances was found for 2005/2006 at altitudes with potential temperatures, Θ, above 430 K. The origins of this increase are unknown except for increases measured during SCOUT-AMMA. Here the eruption of the Soufrière Hills volcano in the Caribbean caused elevated particle mixing ratios. The vertical profiles from Northern hemispheric mid-latitudes between 1999 and 2006 also are compact enough to derive a parameterisation. The tropical profiles all show a broad maximum of particle mixing ratios (between Θ≈340 K and 390 K) which extends from below the TTL to above the thermal tropopause. Thus these particles are a "reservoir" for vertical transport into the stratosphere. The ratio of non-volatile particle number density to total particle number density was also measured by COPAS. The vertical profiles of this ratio have a maximum of 50% above 370 K over Australia and West Africa and a pronounced minimum directly below. Without detailed chemical composition measurements a reason for the increase of non-volatile particle fractions cannot yet be given. However, half of the particles from the tropical "reservoir" contain compounds other than sulphuric acid and water. Correlations of the measured aerosol mixing ratios with N2O and ozone exhibit compact relationships for the tropical data from SCOUT-AMMA, TROCCINOX, and SCOUT-O3. Correlations with CO are more scattered probably because of the connection to different pollution source regions. We provide additional data from the long distance transfer flights to the campaign sites in Brazil, Australia, and West-Africa. These were executed during a time window of 17 months within a period of relative volcanic quiescence. Thus the data represent a "snapshot picture" documenting the status of a significant part of the global UT/LS fine aerosol at low concentration levels 15 years after the last major (i.e., the 1991 Mount Pinatubo) eruption. The corresponding latitudinal distributions of the measured particle number densities are presented in this paper to provide data of the UT/LS background aerosol for modelling purposes.

Pollutant plumes with enhanced concentrations of trace gases and aerosols were observed over the southern coast of West Africa during August 2006 as part of the AMMA wet season field campaign. Plumes were observed both in the mid and upper troposphere. In this study we examined the origin of these pollutant plumes, and their potential to photochemically produce ozone (O3) downwind over the Atlantic Ocean. Their possible contribution to the Atlantic O3 maximum is also discussed. Runs using the BOLAM mesoscale model including biomass burning carbon monoxide (CO) tracers were used to confirm an origin from central African biomass burning fires. The plumes measured in the mid troposphere (MT) had significantly higher pollutant concentrations over West Africa compared to the upper tropospheric (UT) plume. The mesoscale model reproduces these differences and the two different pathways for the plumes at different altitudes: transport to the north-east of the fire region, moist convective uplift and transport to West Africa for the upper tropospheric plume versus north-west transport over the Gulf of Guinea for the mid-tropospheric plume. Lower concentrations in the upper troposphere are mainly due to enhanced mixing during upward transport. Model simulations suggest that MT and UT plumes are 16 and 14 days old respectively when measured over West Africa. The ratio of tracer concentrations at 600 hPa and 250 hPa was estimated for 14–15 August in the region of the observed plumes and compares well with the same ratio derived from observed carbon dioxide (CO2) enhancements in both plumes. It is estimated that, for the period 1–15 August, the ratio of Biomass Burning (BB) tracer concentration transported in the UT to the ones transported in the MT is 0.6 over West Africa and the equatorial South Atlantic. Runs using a photochemical trajectory model, CiTTyCAT, initialized with the observations, were used to estimate in-situ net photochemical O3 production rates in these plumes during transport downwind of West Africa. The mid-troposphere plume spreads over altitude between 1.5 and 6 km over the Atlantic Ocean. Even though the plume was old, it was still very photochemically active (mean net O3 production rates over 10 days of 2.6 ppbv/day and up to 7 ppbv/day during the first days) above 3 km especially during the first few days of transport westward. It is also shown that the impact of high aerosol loads in the MT plume on photolysis rates serves to delay the peak in modelled O3 concentrations. These results suggest that a significant fraction of enhanced O3 in mid-troposphere over the Atlantic comes from BB sources during the summer monsoon period. According to simulated occurrence of such transport, BB may be the main source for O3 enhancement in the equatorial south Atlantic MT, at least in August 2006. The upper tropospheric plume was also still photochemically active, although mean net O3 production rates were slower (1.3 ppbv/day). The results suggest that, whilst the transport of BB pollutants to the UT is variable (as shown by the mesoscale model simulations), pollution from biomass burning can make an important contribution to additional photochemical production of O3 in addition to other important sources such as nitrogen oxides (NOx) from lightning.

A multi-platform field measurement campaign involving aircraft and balloons took place over West Africa between 26 July and 25 August 2006, in the frame of the concomitant AMMA Special Observing Period and SCOUT-O3 African tropical activities. Specifically aiming at sampling the upper troposphere and lower stratosphere, the high-altitude research aircraft M55 Geophysica was deployed in Ouagadougou (12.3° N, 1.7° W), Burkina Faso, in conjunction with the German D-20 Falcon, while a series of stratospheric balloons and sonde flights were conducted from Niamey (13.5° N, 2.0° E), Niger. Altogether, these measurements were intended to provide experimental evidence for a better understanding of large scale transport, assessing the effect of lightning on NOx production, and studying the impact of intense mesoscale convective systems on water, aerosol, dust and chemical species in the upper troposphere and lower stratosphere. The M55 Geophysica carried out five local and four transfer flights between southern Europe and the Sahel and back, while eight stratospheric balloons and twenty-nine sondes were flown from Niamey. These experiments allowed a characterization of the tropopause and lower stratosphere of the region. The paper provides an overview of SCOUT-AMMA campaign activities together with a description of the meteorology of the African monsoon and the situation prevailing during the flights and a brief summary of the observations accomplished.

A suite of diagnostics is applied to in-situ aircraft measurements and one Chemistry-Climate Model (CCM) data to characterize the vertical structure of the Tropical Tropopause Layer (TTL). The diagnostics are based on vertical tracer profiles and relative vertical tracer gradients, using tropopause-referenced coordinates, and tracer-tracer relationships in the tropical Upper Troposphere/Lower Stratosphere (UT/LS). Observations were obtained during four tropical campaigns performed from 1999 to 2006 with the research aircraft Geophysica and have been compared to the output of the ECHAM5/MESSy CCM. The model vertical resolution in the TTL (~500 m) allows for appropriate comparison with high-resolution aircraft observations and the diagnostics used highlight common TTL features between the model and the observational data. The analysis of the vertical profiles of water vapour, ozone, and nitrous oxide, in both the observations and the model, shows that concentration mixing ratios exhibit a strong gradient change across the tropical tropopause, due to the role of this latter as a transport barrier and that transition between the tropospheric and stratospheric regimes occurs within a finite layer. The use of relative vertical ozone and carbon monoxide gradients, in addition to the vertical profiles, helps to highlight the region where this transition occurs and allows to give an estimate of its thickness. The analysis of the CO-O3 and H2O-O3 scatter plots and of the Probability Distribution Function (PDF) of the H2O-O3 pair completes this picture as it allows to better distinguish tropospheric and stratospheric regimes that can be identified by their different chemical composition. The joint analysis and comparison of observed and modelled data allows to state that the model can represent the background TTL structure and its seasonal variability rather accurately. The model estimate of the thickness of the interface region between tropospheric and stratospheric regimes agrees well with average values inferred from observations. On the other hand, the measurements can be influenced by regional scale variability, local transport processes as well as deep convection, that can not be captured by the model.

Light-weight microlidar and water vapour measurements were taken on-board a stratospheric balloon during the HIBISCUS 2004 campaign, held in Bauru, Brazil (49° W, 22° S). Cirrus clouds were observed throughout the flight between 12 and 15 km height with a high mesoscale variability in optical and microphysical properties. It was found that the cirrus clouds were composed of different layers characterized by marked differences in height, thickness and optical properties. Simultaneous water vapour observations show that the different layers are characterized by different values of the saturation with respect to ice. A mesoscale simulation and a trajectory analysis clearly revealed that the clouds had formed in the outflow of a large and persistent convective region and that the observed variability of the optical properties and of the cloud structure is likely linked to the different residence times of the convectively-processed air in the upper troposphere.

During the APE-THESEO mission in the Indian Ocean the Myasishchev Design Bureau stratospheric research aircraft M55 Geophysica performed a flight over and within the inner core region of tropical cyclone Davina. Measurements of total water, water vapour, temperature, aerosol backscattering, ozone and tracers were made and are discussed here in comparison with the averages of those quantities acquired during the campaign time frame. Temperature anomalies in the tropical tropopause layer (TTL), warmer than average in the lower part and colder than average in the upper TTL were observed. Ozone was strongly reduced compared to its average value, and thick cirrus decks were present up to the cold point, sometimes topped by a layer of very dry air. Evidence for meridional transport of trace gases in the stratosphere above the cyclone was observed and perturbed water distribution in the TTL was documented. The paper discuss possible processes of dehydration induced by the cirrus forming above the cyclone, and change in the chemical tracer and water distribution in the lower stratosphere 400–430 K due to meridional transport from the mid-latitudes and link with Davina. Moreover it compares the data prior and after the cyclone passage to discuss its actual impact on the atmospheric chemistry and thermodynamics.

We report in situ and remote observations proving occasional occurrence of solid particles in the tropical lowest stratosphere, 200 km from deep convective events. The particles were found during field campaigns in Southeast Brazil (49.03 W 22.36 S). They occur in the altitude range from 17.5 to 20.8 km, at temperatures up to at least 10 K above the expected frost point temperature. While stability of ice particles at these altitudes is unexpected from a theoretical point of view, it is argued that these observations are indications of tropospheric air masses penetrating into the stratosphere during convective overshoots. It is argued that the intrusion of tropospheric air must have carried a large amount of water with it, which effectively hydrated the lowest stratosphere, and consequently suppressed sublimation. This conclusion is further supported by a separate water vapor mixing ratio profile obtained at the same observation site.

We have analyzed mid-infrared limb-emission measurements of polar stratospheric clouds (PSCs) by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) during the Antarctic winter 2003 with respect to PSC composition. Coincident Lidar observations from McMurdo were used for comparison with PSC types 1a, 1b and 2. Application of new refractive index data of β-NAT have allowed to accurately simulate the prominent spectral band at 820 cm-1 observed by MIPAS at the location where the Lidar instrument observed type 1a PSCs. Broadband spectral fits covering the range from 780 to 960 cm-1 and from 1220 to 1490 cm-1 showed best agreement with the MIPAS measurements when spectroscopic data of NAT were used to simulate the MIPAS spectra. MIPAS measurements collocated with Lidar observations of Type 1b and Type 2 PSCs could only be reproduced by assuming a composition of supercooled ternary H2SO4/HNO3/H2O solution (STS) and of ice, respectively. Particle radius and number density profiles derived from MIPAS were generally consistent with the Lidar observations. Only in the case of ice clouds, PSC volumes are partly underestimated by MIPAS due to large cloud optical thickness in the limb-direction. A comparison of MIPAS cloud composition and Lidar PSC-type determination based on all available MIPAS-Lidar coincident measurements revealed good agreement between PSC-types 1a, 1b and 2, and NAT, STS and ice, respectively. We could not find spectroscopic evidence for the presence of nitric acid dihydrate (NAD) from MIPAS observations of PSCs over Antarctica in 2003.

Mountain wave polar stratospheric clouds (PSCs) were detected on 8 February 2003 above the Scandinavian Mountains by in-situ instruments onboard the M55 Geophysica aircraft. PSC particle composition, backscatter and chlorine activation for this case are studied with a recently developed non-equilibrium microphysical box model for liquid aerosol. Results from the microphysical model, run on quasi-lagrangian trajectories, show that the PSC observed was composed of supercooled ternary (H2O/HNO3/H2SO4) solution (STS) particles, which are out of equilibrium with the gas phase. The measured condensed nitric acid and aerosol backscatter of the PSC can well be simulated with the model. Up to 0.15 ppbv Cl2 can be released by the PSC within 2 h, showing the propensity of these small-scale clouds for chlorine activation. Equilibrium calculations – of the sort commonly used in large scale chemistry transport models – overestimate the measured condensed nitrate by up to a factor of 3, and overestimates chlorine activation by 10%, in this mountain wave cloud.

Space borne infrared limb emission measurements by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) reveal the formation of a belt of polar stratospheric clouds (PSCs) of nitric acid trihydrate (NAT) particles over Antarctica in mid-June 2003. By mesoscale microphysical simulations we show that this sudden onset of NAT PSCs was caused by heterogeneous nucleation on ice in the cooling phases of large-amplitude stratospheric mountain waves over the Antarctic Peninsula and the Ellsworth Mountains. MIPAS observations of PSCs before this event show no indication for the presence of NAT clouds with volume densities larger than about 0.3 µm3/cm3 and radii smaller than 3 µm, but are consistent with supercooled droplets of ternary H2SO4/HNO3/H2O solution (STS). Simulations indicate that homogeneous surface nucleation rates have to be reduced by three orders of magnitude to comply with the observations.

Synoptic scale polar stratospheric clouds (PSCs) that formed without the presence of mountain lee waves were observed in early December 2002 from Kiruna/Sweden using balloon-borne instruments. The physical, chemical, and optical properties of the particles were measured. Within the PSC solid particles existed whenever the temperature was below the equilibrium temperature for nitric acid trihydrate and liquid particles appeared when the temperature fell below an even lower threshold about 3 K above the frost point with solid particles still present. The correlation of liquid supercooled ternary solution aerosols with local temperatures is a pronounced feature observed during this flight; average molar ratios H2O/HNO3 were somewhat higher than predicted by models. In addition HCl has been measured for the first time in liquid aerosols. The chlorine isotope signature served as a unique tool to identify unambiguously HCl dissolved in STS particles. Within a narrow temperature range of about three degrees above the frost point, the measured average amount of HCl in liquid particles is below 1 weight%.

The extent of springtime Arctic ozone loss does not reach Antarctic ``ozone hole'' dimensions because of the generally higher temperatures in the northern hemisphere vortex and consequent less polar stratospheric cloud (PSC) particle surface for heterogeneous chlorine activation. Yet, with increasing greenhouse gases stratospheric temperatures are expected to further decrease. To infer if present Antarctic PSC occurrence can be applied to predict future Arctic PSC occurrence, lidar observations from McMurdo station (78° S, 167° E) and NyÅlesund (79° N, 12° E) have been analysed for the 9 winters between 1995 (1995/1996) and 2003 (2003/2004). Although the statistics may not completely cover the overall hemispheric PSC occurrence, the observations are considered to represent the main synoptic cloud features as both stations are mostly situated in the centre or at the inner edge of the vortex. Since the focus is set on the occurrence frequency of solid and liquid particles, the analysis has been restricted to volcanic aerosol free conditions. In McMurdo, by far the largest part of PSC observations is associated with NAT PSCs. The observed persistent background of NAT particles and their potential ability to cause denoxification and irreversible denitrification is presumably more important to Antarctic ozone chemistry than the scarcely observed ice PSCs. Meanwhile in Ny-Ålesund, ice PSCs have never been observed, while solid NAT and liquid STS clouds both occur in large fraction. Although they are also found solely, the majority of observations reveals solid and liquid particle layers in the same profile. For the Ny-Ålesund measurements, the frequent occurrence of liquid PSC particles yields major significance in terms of ozone chemistry, as their chlorine activation rates are more efficient. The relationship between temperature, PSC formation, and denitrification is nonlinear and the McMurdo and Ny-Ålesund PSC observations imply that for predicted stratospheric cooling it is not possible to directly apply current Antarctic PSC occurrence to the Arctic stratosphere. Future Arctic PSC occurrence, and thus ozone loss, is likely to depend on the shape and barotropy of the vortex rather than on minimum temperature alone.

Polar stratospheric clouds (PSC) have been observed in early winter (December 2002) during the SOLVE II/Vintersol campaign, both from balloons carrying comprehensive instrumentation for measurements of chemical composition, size distributions, and optical properties of the particles, as well as from individual backscatter soundings from Esrange and Sodankylä. The observations are unique in the sense that the PSC particles seem to have formed in the early winter under synoptic temperature conditions and not being influenced by mountain lee waves. A sequence of measurements during a 5-days period shows a gradual change between liquid and solid type PSCs with the development of a well-known sandwich structure. It appears that all PSC observations show the presence of a background population of solid particles, occasionally mixed in with more optically dominating liquid particles. The measurements have been compared with results from a detailed microphysical and optical simulation of the formation processes. Calculated extinctions are in good agreement with SAGE-III measurements from the same period. Apparently the solid particles are controlled by the synoptic temperature history while the presence of liquid particles is controlled by the local temperatures at the time of observation. The temperature histories indicate that the solid particles are nucleated above the ice frost point, and a surface freezing mechanism for this is included in the model. Reducing the calculated freezing rates by a factor 10-20, the model is able to simulate the observed particle size distributions and reproduce observed HNO3 gas phase concentrations.

Mechanisms by which subvisible cirrus clouds (SVCs) might contribute to dehydration close to the tropical tropopause are not well understood. Recently Ultrathin Tropical Tropopause Clouds (UTTCs) with optical depths around 10-4 have been detected in the western Indian ocean. These clouds cover thousands of square kilometers as 200-300 m thick distinct and homogeneous layer just below the tropical tropopause. In their condensed phase UTTCs contain only 1-5% of the total water, and essentially no nitric acid. A new cloud stabilization mechanism is required to explain this small fraction of the condensed water content in the clouds and their small vertical thickness. This work suggests a mechanism, which forces the particles into a thin layer, based on upwelling of the air of some mm/s to balance the ice particles, supersaturation with respect to ice above and subsaturation below the UTTC. In situ measurements suggest that these requirements are fulfilled. The basic physical properties of this mechanism are explored by means of a single particle model. Comprehensive 1-D cloud simulations demonstrate this stabilization mechanism to be robust against rapid temperature fluctuations of +/- 0.5 K. However, rapid warming (Delta T > 2 K) leads to evaporation of the UTTC, while rapid cooling (Delta T < -2 K) leads to destabilization of the particles with the potential for significant dehydration below the cloud

Subvisible cirrus clouds (SVCs) may contribute to dehydration close to the tropical tropopause. The higher and colder SVCs and the larger their ice crystals, the more likely they represent the last efficient point of contact of the gas phase with the ice phase and, hence, the last dehydrating step, before the air enters the stratosphere. The first simultaneous in situ and remote sensing measurements of SVCs were taken during the APE-THESEO campaign in the western Indian ocean in February/March 1999. The observed clouds, termed Ultrathin Tropical Tropopause Clouds (UTTCs), belong to the geometrically and optically thinnest large-scale clouds in the Earth's atmosphere. Individual UTTCs may exist for many hours as an only 200--300 m thick cloud layer just a few hundred meters below the tropical cold point tropopause, covering up to 105 km2. With temperatures as low as 181 K these clouds are prime representatives for defining the water mixing ratio of air entering the lower stratosphere.

A new automated small size lidar system (microlidar or MULID) has been developed and employed to perform aerosol measurements since March 2010 at Ny Ålesund (78.9°N, 11.9°E), Svalbard. The lidar observations have been used to estimate the PBL height by using the gradient method based on abrupt changes in the vertical aerosol profile and monitor its temporal evolution. The scope of the present study is to compare several approaches to estimate the PBL height, by using lidar observations, meteorological measurements by radio soundings, and a zero-order one-dimensional model based on a parameterization of the turbulent kinetic energy budget within the mixing layer, under the assumptions of horizontal homogeneity, and neglecting radiation and latent heat effects. A case study is presented here for a convective PBL, observed in June 2010 in order to verify whether the Gradient Method can be applied to lidar measurements in the Arctic region to obtain the PBL height. The results obtained are in good agreement with the PBL height estimated by the analysis of thermodynamic measurements obtained from radio sounding and with the model.

Multiwavelength laser backscattersondes (MAS) have been widely used from a variety of airborne platforms for in situ measurements of optical properties of clouds and atmospheric particulate as well as their phase and composition. Recently, a new miniaturized LIDAR (MULID) has been developed using state-of-art technology for balloon borne profiling of the same quantities. A description of the two instruments, a survey of preliminary results obtained during test flights and indications for future use are given.

No abstract available.

In this study, the first postpartum heat, termed the foal heat, characteristics and performance in female donkey (jenny) of Martina Franca are described. To this end, the follicular development of 42 jennies during foal heat was compared with that of 31 jennies at the third estrus after foaling. Estrus length (7.1±0.9 and 6.8±0.7 days), follicular development and preovulatory follicle size (43.7±3.5 and 45.1±2.5 mm) were similar between jennies during the foal heat and during the third estrus after foaling. The pregnancy rate at day 14 was significantly lower in the foal heat jennies (57.1%) than the third estrus jennies (82.3%). However, the pregnancy rate at day 14 in foal heat jennies increased significantly when the onset of foal heat was ⩾8 days after foaling (93.8%) or when the ovulation happened ⩾12 days after foaling (85.7%). The data provided in the present study suggest that the foal heat in the endangered jennies of Martina Franca could be successfully utilized to reduce the interpartum period if the onset of foal heat occurs >8 days after foaling.