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The presence of reactive bromine in polar regions is a widespread phenomenon that plays an important role in the photochemistry of the Arctic and Antarctic lower troposphere, including the destruction of ozone, the disturbance of radical cycles, and the oxidation of gaseous elemental mercury. The chemical mechanisms leading to the heterogeneous release of gaseous bromine compounds from saline surfaces are in principle well understood. There are, however, substantial uncertainties about the contribution of different potential sources to the release of reactive bromine, such as sea ice, brine, aerosols, and the snow surface, as well as about the seasonal and diurnal variation and the vertical distribution of reactive bromine. Here we use continuous long-term measurements of the vertical distribution of bromine monoxide (BrO) and aerosols at the two Antarctic sites Neumayer (NM) and Arrival Heights (AH), covering the periods of 2003–2021 and 2012–2021, respectively, to investigate how chemical and physical parameters affect the abundance of BrO. We find the strongest correlation between BrO and aerosol extinction (R=0.56 for NM and R=0.28 for AH during spring), suggesting that the heterogeneous release of Br2 from saline airborne particles (blowing snow and aerosols) is a dominant source for reactive bromine. Positive correlations between BrO and contact time of air masses, both with sea ice and the Antarctic ice sheet, suggest that reactive bromine is not only emitted by the sea ice surface but by the snowpack on the ice shelf and in the coastal regions of Antarctica. In addition, the open ocean appears to represent a source for reactive bromine during late summer and autumn when the sea ice extent is at its minimum. A source–receptor analysis based on back trajectories and sea ice maps shows that main source regions for BrO at NM are the Weddell Sea and the Filchner–Ronne Ice Shelf, as well as coastal polynyas where sea ice is newly formed. A strong morning peak in BrO frequently occurring during summer and that is particularly strong during autumn suggests a night-time build-up of Br2 by heterogeneous reaction of ozone on the saline snowpack in the vicinity of the measurement sites. We furthermore show that BrO can be sustained for at least 3 d while travelling across the Antarctic continent in the absence of any saline surfaces that could serve as a source for reactive bromine.

Aerosol particles are a complex component of the atmospheric system which influence climate directly by interacting with solar radiation, and indirectly by contributing to cloud formation. The variety of their sources, as well as the multiple transformations they may undergo during their transport (including wet and dry deposition), result in significant spatial and temporal variability of their properties. Documenting this variability is essential to provide a proper representation of aerosols and cloud condensation nuclei (CCN) in climate models. Using measurements conducted in 2016 or 2017 at 62 ground-based stations around the world, this study provides the most up-to-date picture of the spatial distribution of particle number concentration (Ntot) and number size distribution (PNSD, from 39 sites). A sensitivity study was first performed to assess the impact of data availability on Ntot's annual and seasonal statistics, as well as on the analysis of its diel cycle. Thresholds of 50 % and 60 % were set at the seasonal and annual scale, respectively, for the study of the corresponding statistics, and a slightly higher coverage (75 %) was required to document the diel cycle. Although some observations are common to a majority of sites, the variety of environments characterizing these stations made it possible to highlight contrasting findings, which, among other factors, seem to be significantly related to the level of anthropogenic influence. The concentrations measured at polar sites are the lowest (∼ 102 cm−3) and show a clear seasonality, which is also visible in the shape of the PNSD, while diel cycles are in general less evident, due notably to the absence of a regular day–night cycle in some seasons. In contrast, the concentrations characteristic of urban environments are the highest (∼ 103–104 cm−3) and do not show pronounced seasonal variations, whereas diel cycles tend to be very regular over the year at these stations. The remaining sites, including mountain and non-urban continental and coastal stations, do not exhibit as obvious common behaviour as polar and urban sites and display, on average, intermediate Ntot (∼ 102–103 cm−3). Particle concentrations measured at mountain sites, however, are generally lower compared to nearby lowland sites, and tend to exhibit somewhat more pronounced seasonal variations as a likely result of the strong impact of the atmospheric boundary layer (ABL) influence in connection with the topography of the sites. ABL dynamics also likely contribute to the diel cycle of Ntot observed at these stations. Based on available PNSD measurements, CCN-sized particles (considered here as either >50 nm or >100 nm) can represent from a few percent to almost all of Ntot, corresponding to seasonal medians on the order of ∼ 10 to 1000 cm−3, with seasonal patterns and a hierarchy of the site types broadly similar to those observed for Ntot. Overall, this work illustrates the importance of in situ measurements, in particular for the study of aerosol physical properties, and thus strongly supports the development of a broad global network of near surface observatories to increase and homogenize the spatial coverage of the measurements, and guarantee as well data availability and quality. The results of this study also provide a valuable, freely available and easy to use support for model comparison and validation, with the ultimate goal of contributing to improvement of the representation of aerosol–cloud interactions in models, and, therefore, of the evaluation of the impact of aerosol particles on climate.

Aerosol particles are essential constituents of the Earth's atmosphere, impacting the earth radiation balance directly by scattering and absorbing solar radiation, and indirectly by acting as cloud condensation nuclei. In contrast to most greenhouse gases, aerosol particles have short atmospheric residence times, resulting in a highly heterogeneous distribution in space and time. There is a clear need to document this variability at regional scale through observations involving, in particular, the in situ near-surface segment of the atmospheric observation system. This paper will provide the widest effort so far to document variability of climate-relevant in situ aerosol properties (namely wavelength dependent particle light scattering and absorption coefficients, particle number concentration and particle number size distribution) from all sites connected to the Global Atmosphere Watch network. High-quality data from almost 90 stations worldwide have been collected and controlled for quality and are reported for a reference year in 2017, providing a very extended and robust view of the variability of these variables worldwide. The range of variability observed worldwide for light scattering and absorption coefficients, single-scattering albedo, and particle number concentration are presented together with preliminary information on their long-term trends and comparison with model simulation for the different stations. The scope of the present paper is also to provide the necessary suite of information, including data provision procedures, quality control and analysis, data policy, and usage of the ground-based aerosol measurement network. It delivers to users of the World Data Centre on Aerosol, the required confidence in data products in the form of a fully characterized value chain, including uncertainty estimation and requirements for contributing to the global climate monitoring system.

In order to assess the evolution of aerosol parameters affecting climate change, a long-term trend analysis of aerosol optical properties was performed on time series from 52 stations situated across five continents. The time series of measured scattering, backscattering and absorption coefficients as well as the derived single scattering albedo, backscattering fraction, scattering and absorption Ångström exponents covered at least 10 years and up to 40 years for some stations. The non-parametric seasonal Mann–Kendall (MK) statistical test associated with several pre-whitening methods and with Sen's slope was used as the main trend analysis method. Comparisons with general least mean square associated with autoregressive bootstrap (GLS/ARB) and with standard least mean square analysis (LMS) enabled confirmation of the detected MK statistically significant trends and the assessment of advantages and limitations of each method. Currently, scattering and backscattering coefficient trends are mostly decreasing in Europe and North America and are not statistically significant in Asia, while polar stations exhibit a mix of increasing and decreasing trends. A few increasing trends are also found at some stations in North America and Australia. Absorption coefficient time series also exhibit primarily decreasing trends. For single scattering albedo, 52 % of the sites exhibit statistically significant positive trends, mostly in Asia, eastern/northern Europe and the Arctic, 22 % of sites exhibit statistically significant negative trends, mostly in central Europe and central North America, while the remaining 26 % of sites have trends which are not statistically significant. In addition to evaluating trends for the overall time series, the evolution of the trends in sequential 10-year segments was also analyzed. For scattering and backscattering, statistically significant increasing 10-year trends are primarily found for earlier periods (10-year trends ending in 2010–2015) for polar stations and Mauna Loa. For most of the stations, the present-day statistically significant decreasing 10-year trends of the single scattering albedo were preceded by not statistically significant and statistically significant increasing 10-year trends. The effect of air pollution abatement policies in continental North America is very obvious in the 10-year trends of the scattering coefficient – there is a shift to statistically significant negative trends in 2009–2012 for all stations in the eastern and central USA. This long-term trend analysis of aerosol radiative properties with a broad spatial coverage provides insight into potential aerosol effects on climate changes.

Abstract Background More than 90% of human immunodeficiency virus (HIV)‐infected patients will develop at least one type of skin disorder during the course of the disease. The prevalence and severity of skin disease commonly seen in HIV‐infected patients has decreased in the era of combination antiretroviral therapy (cART). Few studies in Ethiopia have shown the magnitude of skin problems among adult patients on cART. The aim of this study is to describe the pattern of skin disease among adult patients who are on cART. Methods Cross‐sectional observational study at ALERT Hospital from April 2018 to November 2018. Patterns of clinically diagnosed skin diseases were summarized descriptively. Result A total of 572 patients were evaluated. In total, 412 (72%) were female and the mean age of study participants was 40 (SD = 10.4). The median CD4 count at the time of diagnosis and start of cART were 178 (R 5‐2000) and 168 cells/μl (R 5‐1327), respectively. The mean duration of cART was 8 (SD = 3) years. 89.3% of patients were on first line and 7% on second line of cART regimen. Noninfectious inflammatory skin disorders (40.9%) were the most common concomitant diagnosis followed by infectious diseases (34.9%), infestation (7.7%), pigmentary disorders (6.3%) and cutaneous drug eruption (0.7%), respectively. Among the inflammatory skin disorders, 56.5% presented with eczema. One patient had Kaposi sarcoma. Conclusion Noninfectious inflammatory skin disorders are the most common concomitant skin disease in HIV‐infected patients, with eczema being most prevalent. Infectious skin diseases were also common presentations. In our study, AIDS‐defining skin conditions were rare.

Though the environmental conditions of the Weddell Sea region and Dronning Maud Land are still relatively stable compared to the fast-changing Antarctic Peninsula, we may suspect pronounced effects of global climate change for the near future (Thompson et al., 2011). Reducing the uncertainties in climate change modeling requires a better understanding of the aerosol optical properties, and for this we need accurate data on the aerosol refractive index (RI). Due to the remoteness of Antarctica only very few RI data are available from this region (Hogan et al., 1979; Virkkula et al., 2006; Shepherd et al., 2018). We calculate the real refractive index of natural atmospheric aerosols from number size distribution measurements at the German coastal Antarctic station Neumayer III. Given the high average scattering albedo of 0.992 (Weller et al., 2013), we assumed that the imaginary part of the RI is zero. Our method uses the overlapping size range (particle diameter D between 120 and 340 nm) of a scanning mobility particle sizer (SMPS), which sizes the particles by their electrical mobility, and a laser aerosol spectrometer (LAS), which sizes the particles by their optical scattering signal at the 633 nm wavelength. Based on almost a complete year of measurement, the average effective refractive index (RIeff, as we call our retrieved RI because of the used assumptions) for the dry aerosol particles turned out to be 1.44 with a standard deviation of 0.08, in a good agreement with the RI value of 1.47, which we derived from the chemical composition of bulk aerosol sampling measurements. At Neumayer the aerosol shows a pronounced seasonal pattern in both number concentration and chemical composition. Despite this, the variability of the monthly averaged RIeff values remained between 1.40 and 1.50. Compared to the annual mean, two austral winter months (July and September) showed slightly but significantly increased values (1.50 and 1.47, respectively). The size dependency of the RIeff could be determined from time-averaged LAS and SMPS number size distributions measured between December 2017 and January 2018. Here we calculated RIeff for four different particle size ranges and observed a slight decrease from 1.47 (D range 116–168 nm) to 1.37 (D range 346–478 nm). We find no significant dependence of the derived RIeff values on the wind direction. Thus we conclude that RIeff is largely independent of the general weather situation, roughly classified as (i) advection of marine boundary layer air masses during easterly winds caused by passing cyclones in contrast to (ii) air mass transport from continental Antarctica under southern katabatic winds. Neumayer, the only relevant contamination source, is located 1.5 km north of the air chemistry observatory, where the measurements were performed. Given that northerly winds are almost absent, the potential impact of local contamination is minimized in general. Indeed our data show no impact of local contamination on RIeff. Just in one case a temporary high-contamination episode with diesel engines operating right next to the measurement site resulted in an unusual high RIeff of 1.59, probably caused by the high black carbon content of the exhaust fumes. To conclude, our study revealed largely constant RIeff values throughout the year without any sign of seasonality. Therefore, it seems reasonable to use a single, constant RIeff value of 1.44 for modeling optical properties of natural, coastal Antarctic sub-micrometer aerosol.

We measured aerosol size distributions and conducted bulk and size-segregated aerosol sampling during two summer campaigns in January 2015 and January 2016 at the continental Antarctic station Kohnen (Dronning Maud Land). Physical and chemical aerosol properties differ conspicuously during the episodic impact of a distinctive low-pressure system in 2015 (LPS15) compared to the prevailing clear sky conditions. The approximately 3-day LPS15 located in the eastern Weddell Sea was associated with the following: marine boundary layer air mass intrusion; enhanced condensation particle concentrations (1400 ± 700 cm−3 compared to 250 ± 120 cm−3 under clear sky conditions; mean ± SD); the occurrence of a new particle formation event exhibiting a continuous growth of particle diameters (Dp) from 12 to 43 nm over 44 h (growth rate 0.6 nm h−1); peaking methane sulfonate (MS−), non-sea-salt sulfate (nss–SO42−), and Na+ concentrations (190 ng m−3 MS−, 137 ng m−3 nss–SO42−, and 53 ng m−3 Na+ compared to 24 ± 15, 107 ± 20, and 4.1 ± 2.2 ng m−3, respectively, during clear sky conditions); and finally an increased MS− ∕ nss–SO42− mass ratio βMS of 0.4 up to 2.3 (0.21 ± 0.1 under clear sky conditions) comparable to typical values found at coastal Antarctic sites. Throughout the observation period a larger part of MS− could be found in super-micron aerosol compared to nss–SO42−, i.e., (10 ± 2) % by mass compared to (3.2 ± 2) %, respectively. On the whole, under clear sky conditions aged aerosol characterized by usually mono-modal size distributions around Dp = 60 nm was observed. Although our observations indicate that the sporadic impacts of coastal cyclones were associated with enhanced marine aerosol entry, aerosol deposition on-site during austral summer should be largely dominated by typical steady clear sky conditions.

Multiple year-round (2006–2015) records of the bulk and size-segregated composition of aerosol were obtained at the inland site of Concordia located in East Antarctica. The well-marked maximum of non-sea-salt sulfate (nssSO4) in January (100 ± 28 ng m−3 versus 4.4 ± 2.3 ng m−3 in July) is consistent with observations made at the coast (280 ± 78 ng m−3 in January versus 16 ± 9 ng m−3 in July at Dumont d'Urville, for instance). In contrast, the well-marked maximum of MSA at the coast in January (60 ± 23 ng m−3 at Dumont d'Urville) is not observed at Concordia (5.2 ± 2.0 ng m−3 in January). Instead, the MSA level at Concordia peaks in October (5.6 ± 1.9 ng m−3) and March (14.9 ± 5.7 ng m−3). As a result, a surprisingly low MSA-to-nssSO4 ratio (RMSA) is observed at Concordia in mid-summer (0.05 ± 0.02 in January versus 0.25 ± 0.09 in March). We find that the low value of RMSA in mid-summer at Concordia is mainly driven by a drop of MSA levels that takes place in submicron aerosol (0.3 µm diameter). The drop of MSA coincides with periods of high photochemical activity as indicated by high ozone levels, strongly suggesting the occurrence of an efficient chemical destruction of MSA over the Antarctic plateau in mid-summer. The relationship between MSA and nssSO4 levels is examined separately for each season and indicates that concentration of non-biogenic sulfate over the Antarctic plateau does not exceed 1 ng m−3 in fall and winter and remains close to 5 ng m−3 in spring. This weak non-biogenic sulfate level is discussed in the light of radionuclides (210Pb, 10Be, and 7Be) also measured on bulk aerosol samples collected at Concordia. The findings highlight the complexity in using MSA in deep ice cores extracted from inland Antarctica as a proxy of past dimethyl sulfide emissions from the Southern Ocean.

Multiple year-round records of bulk and size-segregated composition of aerosol were obtained at the inland site of Concordia located at Dome C in East Antarctica. In parallel, sampling of acidic gases on denuder tubes was carried out to quantify the concentrations of HCl and HNO3 present in the gas phase. These time series are used to examine aerosol present over central Antarctica in terms of chloride depletion relative to sodium with respect to freshly emitted sea-salt aerosol as well as depletion of sulfate relative to sodium with respect to the composition of seawater. A depletion of chloride relative to sodium is observed over most of the year, reaching a maximum of ∼ 20 ng m−3 in spring when there are still large sea-salt amounts and acidic components start to recover. The role of acidic sulfur aerosol and nitric acid in replacing chloride from sea-salt particles is here discussed. HCl is found to be around twice more abundant than the amount of chloride lost by sea-salt aerosol, suggesting that either HCl is more efficiently transported to Concordia than sea-salt aerosol or re-emission from the snow pack over the Antarctic plateau represents an additional significant HCl source. The size-segregated composition of aerosol collected in winter (from 2006 to 2011) indicates a mean sulfate to sodium ratio of sea-salt aerosol present over central Antarctica of 0.16 ± 0.05, suggesting that, on average, the sea-ice and open-ocean emissions equally contribute to sea-salt aerosol load of the inland Antarctic atmosphere. The temporal variability of the sulfate depletion relative to sodium was examined at the light of air mass backward trajectories, showing an overall decreasing trend of the ratio (i.e., a stronger sulfate depletion relative to sodium) when air masses arriving at Dome C had traveled a longer time over sea ice than over open ocean. The findings are shown to be useful to discuss sea-salt ice records extracted at deep drilling sites located inland Antarctica.

Surface ozone has been measured since 2004 at the coastal East Antarctic site of Dumont d'Urville (DDU), and since 2007 at the Concordia station located on the high East Antarctic plateau. This paper discusses long-term changes, seasonal and diurnal cycles, as well as inter-annual summer variability observed at these two East Antarctic sites. At Concordia, near-surface ozone data were complemented by balloon soundings and compared to similar measurements done at the South Pole. The DDU record is compared to those obtained at the coastal site of Syowa, also located in East Antarctica, as well as the coastal sites of Neumayer and Halley, both located on the coast of the Weddell Sea in West Antarctica. Surface ozone mixing ratios exhibit very similar seasonal cycles at Concordia and the South Pole. However, in summer the diurnal cycle of ozone is different at the two sites with a drop of ozone in the afternoon at Concordia but not at the South Pole. The vertical distribution of ozone above the snow surface also differs. When present, the ozone-rich layer located near the ground is better mixed and deeper at Concordia (up to 400 m) than at the South Pole during sunlight hours. These differences are related to different solar radiation and wind regimes encountered at these two inland sites. DDU appears to be the coastal site where the impact of the late winter/spring bromine chemistry is the weakest, but where the impact of elevated ozone levels caused by NOx snow emissions from the high Antarctic plateau is the highest. The highest impact of the bromine chemistry is seen at Halley and Neumayer, and to a lesser extent at Syowa. These three sites are only weakly impacted by the NOx chemistry and the net ozone production occurring on the high Antarctic plateau. The differences in late winter/spring are attributed to the abundance of sea ice offshore from the sites, whereas those in summer are related to the topography of East Antarctica that promotes the katabatic flow bringing oxidant-rich inland air masses to the site. There appears to be a decreasing change in summer surface ozone at the two East Antarctic sites of Concordia and DDU over the most recent period (2004–2014 and 2007–2014). Further research, including continued monitoring, is needed at these two sites to better separate the effect of synoptic transport from possible change of NOx snow emissions in response to recovery of the stratospheric ozone layer leading to penetration of more UV radiation to the surface.

The applicability, methods and limitations of constrained peak fitting on mass spectra of low mass resolving power (m∕Δm50 ∼ 500) recorded with a time-of-flight aerosol chemical speciation monitor (ToF-ACSM) are explored. Calibration measurements as well as ambient data are used to exemplify the methods that should be applied to maximise data quality and assess confidence in peak-fitting results. Sensitivity analyses and basic peak fit metrics such as normalised ion separation are employed to demonstrate which peak-fitting analyses commonly performed in high-resolution aerosol mass spectrometry are appropriate to perform on spectra of this resolving power. Information on aerosol sulfate, nitrate, sodium chloride, methanesulfonic acid as well as semi-volatile metal species retrieved from these methods is evaluated. The constants in a commonly used formula for the estimation of the mass concentration of hydrocarbon-like organic aerosol may be refined based on peak-fitting results. Finally, application of a recently published parameterisation for the estimation of carbon oxidation state to ToF-ACSM spectra is validated for a range of organic standards and its use demonstrated for ambient urban data.

The Monitoring Atmospheric Composition and Climate (MACC) project represents the European Union's Copernicus Atmosphere Monitoring Service (CAMS) (http://www.copernicus.eu/), which became fully operational during 2015. The global near-real-time MACC model production run for aerosol and reactive gases provides daily analyses and 5-day forecasts of atmospheric composition fields. It is the only assimilation system worldwide that is operational to produce global analyses and forecasts of reactive gases and aerosol fields. We have investigated the ability of the MACC analysis system to simulate tropospheric concentrations of reactive gases covering the period between 2009 and 2012. A validation was performed based on carbon monoxide (CO), nitrogen dioxide (NO2) and ozone (O3) surface observations from the Global Atmosphere Watch (GAW) network, the O3 surface observations from the European Monitoring and Evaluation Programme (EMEP) and, furthermore, NO2 tropospheric columns, as well as CO total columns, derived from satellite sensors. The MACC system proved capable of reproducing reactive gas concentrations with consistent quality; however, with a seasonally dependent bias compared to surface and satellite observations – for northern hemispheric surface O3 mixing ratios, positive biases appear during the warm seasons and negative biases during the cold parts of the year, with monthly modified normalised mean biases (MNMBs) ranging between −30 and 30 % at the surface. Model biases are likely to result from difficulties in the simulation of vertical mixing at night and deficiencies in the model's dry deposition parameterisation. Observed tropospheric columns of NO2 and CO could be reproduced correctly during the warm seasons, but are mostly underestimated by the model during the cold seasons, when anthropogenic emissions are at their highest level, especially over the US, Europe and Asia. Monthly MNMBs of the satellite data evaluation range from values between −110 and 40 % for NO2 and at most −20 % for CO, over the investigated regions. The underestimation is likely to result from a combination of errors concerning the dry deposition parameterisation and certain limitations in the current emission inventories, together with an insufficiently established seasonality in the emissions.

We measured condensation particle (CP) concentrations and particle size distributions at the coastal Antarctic station Neumayer (70°39´ S, 8°15´ W) during two summer campaigns (from 20 January to 26 March 2012 and 1 February to 30 April 2014) and during the polar night between 12 August and 27 September 2014 in the particle diameter (Dp) range from 2.94 to 60.4 nm (2012) and from 6.26 to 212.9 nm (2014). During both summer campaigns we identified all in all 44 new particle formation (NPF) events. From 10 NPF events, particle growth rates could be determined to be around 0.90 ± 0.46 nm h−1 (mean ± SD; range: 0.4–1.9 nm h−1). With the exception of one case, particle growth was generally restricted to the nucleation mode (Dp < 25 nm) and the duration of NPF events was typically around 6.0 ± 1.5 h (mean ± SD; range: 4–9 h). Thus, in the surrounding area of Neumayer, particles did not grow up to sizes required for acting as cloud condensation nuclei. NPF during summer usually occurred in the afternoon in coherence with local photochemistry. During winter, two NPF events could be detected, though showing no ascertainable particle growth. A simple estimation indicated that apart from sulfuric acid, the derived growth rates required other low volatile precursor vapours.

We report on continuously measured 222Rn activity concentrations in near-surface air at Neumayer Station in the period 1995–2011. This 17-year record showed no long-term trend and has overall mean ± standard deviation of (0.019 ± 0.012) Bq m−3. A distinct and persistent seasonality could be distinguished with maximum values of (0.028 ± 0.013) Bq m−3 from January to March and minimum values of (0.015 ± 0.009) Bq m−3 from May to October. Elevated 222Rn activity concentrations were typically associated with air mass transport from the Antarctic Plateau. Our results do not support a relation between enhanced 222Rn activity concentrations at Neumayer and cyclonic activity or long-range transport from South America. The impact of oceanic 222Rn emissions could not be properly assessed but we tentatively identified regional sea ice extent (SIE) variability as a significant driver of the annual 222Rn cycle.

The social cost of carbon (SCC) has emerged as one of the relevant measures in integrated assessment models in climate economics, to quantify costs related to global warming and climate change. While the SCC is used in different models, including DICE (Dynamic Integrated model of Climate and Economy), PAGE (Policy Analysis of the Greenhouse Effect), and FUND (Climate Framework for Uncertainty, Negotiation, and Distribution), its exact definition and computation depend on the reference and, frequently lacking consistency within research streams whether focusing on a single model or on different models. In this study, we investigated three different methods for the computation of the SCC using the integrated assessment model DICE. While the first two methods are commonly known and used, the novel formula derived for the third method allows a direct analysis of the impact of the discount factor in the calculation of the SCC. We provide a detailed proof for the correctness of the third method and validate the consistency of all three methods by numerical experiments.

To probe the spatial extent of tropospheric ozone depletion events during Antarctic spring, a network of 10 autonomous ozone monitors was established around the Dronning Maud Land sector of Antarctica for a full calendar year. Together with manned stations in the area, the network covered a ~1200 km stretch of coast, as well as a transect ~300 km inland and to ~2000 m above sea level (a.s.l.). Here we present results from the spring period (August to October 2008). While some ozone depletion events were evident at only a single site, implying localised ozone destruction, others were evident across the network. The fact that, on occasions, ozone depletion events were observed at all coastal sites simultaneously, suggests the depleted air mass had a scale of at least 1200 km. As the ozone-poor air was advected from the Weddell Sea sea ice zone, the data imply that large areas over the Weddell Sea sea ice zone are significantly depleted in ozone on occasions during Antarctic spring.

Continuous black carbon (BC) observations were conducted from 1999 through 2009 by an Aethalometer (AE10) and from 2006 through 2011 by a Multi-Angle Absorption Photometer (MAAP) at Neumayer Station (NM) under stringent contamination control. Considering the respective observation period, BC concentrations measured by the MAAP were somewhat higher (median ± standard deviation: 2.1 ± 2.0 ng m−3) compared to the AE10 results (1.6 ± 2.1 ng m−3). Neither for the AE10 nor for the MAAP data set a significant long-term trend could be detected. Consistently a pronounced seasonality was observed with both instruments showing a primary annual maximum between October and November and a minimum in April with a maximum/minimum ratio of 4.5/1.6 = 3.8 and 2.7/0.64 = 4.2 for the MAAP and AE10 data, respectively. Occasionally a secondary summer maximum in January/February was visible. With the aim to assess the impact of BC on optical properties of the aerosol at NM, we evaluated the BC data along with particle scattering coefficients measured by an integrating nephelometer. We found the mean single scattering albedo of ω550 = 0.992 ± 0.0090 (median: 0.994) at a wavelength of 550 nm with a range of values from 0.95 to 1.0.

We have analysed the trends of total aerosol particle number concentrations (N) measured at long-term measurement stations involved either in the Global Atmosphere Watch (GAW) and/or EU infrastructure project ACTRIS. The sites are located in Europe, North America, Antarctica, and on Pacific Ocean islands. The majority of the sites showed clear decreasing trends both in the full-length time series, and in the intra-site comparison period of 2001–2010, especially during the winter months. Several potential driving processes for the observed trends were studied, and even though there are some similarities between N trends and air temperature changes, the most likely cause of many northern hemisphere trends was found to be decreases in the anthropogenic emissions of primary particles, SO2 or some co-emitted species. We could not find a consistent agreement between the trends of N and particle optical properties in the few stations with long time series of all of these properties. The trends of N and the proxies for cloud condensation nuclei (CCN) were generally consistent in the few European stations where the measurements were available. This work provides a useful comparison analysis for modelling studies of trends in aerosol number concentrations.

Currently many ground-based atmospheric stations include in-situ measurements of aerosol physical and optical properties, resulting in more than 20 long-term (> 10 yr) aerosol measurement sites in the Northern Hemisphere and Antarctica. Most of these sites are located at remote locations and monitor the aerosol particle number concentration, wavelength-dependent light scattering, backscattering, and absorption coefficients. The existence of these multi-year datasets enables the analysis of long-term trends of these aerosol parameters, and of the derived light scattering Ångström exponent and backscatter fraction. Since the aerosol variables are not normally distributed, three different methods (the seasonal Mann-Kendall test associated with the Sen's slope, the generalized least squares fit associated with an autoregressive bootstrap algorithm for confidence intervals, and the least-mean square fit applied to logarithms of the data) were applied to detect the long-term trends and their magnitudes. To allow a comparison among measurement sites, trends on the most recent 10 and 15 yr periods were calculated. No significant trends were found for the three continental European sites. Statistically significant trends were found for the two European marine sites but the signs of the trends varied with aerosol property and location. Statistically significant decreasing trends for both scattering and absorption coefficients (mean slope of −2.0% yr−1) were found for most North American stations, although positive trends were found for a few desert and high-altitude sites. The difference in the timing of emission reduction policy for the Europe and US continents is a likely explanation for the decreasing trends in aerosol optical parameters found for most American sites compared to the lack of trends observed in Europe. No significant trends in scattering coefficient were found for the Arctic or Antarctic stations, whereas the Arctic station had a negative trend in absorption coefficient. The high altitude Pacific island station of Mauna Loa presents positive trends for both scattering and absorption coefficients.

Continuous condensation particle (CP) observations were conducted from 1984 through 2009 at Neumayer Station under stringent contamination control. During this period, the CP concentration (median 258 cm−3) showed no significant long term trend but exhibited a pronounced seasonality characterized by a stepwise increase starting in September and reaching its annual maximum of around 103 cm−3 in March. Minimum values below 102 cm–3 were observed during June/July. Dedicated time series analyses in the time and frequency domain revealed no significant correlations between inter-annual CP concentration variations and atmospheric circulation indices like Southern Annular Mode (SAM) or Southern Ocean Index (SOI). The impact of the Pinatubo volcanic eruption and strong El Niño events did not affect CP concentrations. From thermodenuder experiments we deduced that the portion of volatile (at 125 °C) and semi-volatile (at 250 °C) particles which could be both associated with biogenic sulfur aerosol, was maximum during austral summer, while during winter non-volatile sea salt particles dominated. During September through April we could frequently observe enhanced concentrations of ultrafine particles within the nucleation mode (between 3 nm and 7 nm particle diameter), preferentially in the afternoon.

We synthesised observations of total particle number (CN) concentration from 36 sites around the world. We found that annual mean CN concentrations are typically 300–2000 cm−3 in the marine boundary layer and free troposphere (FT) and 1000–10 000 cm−3 in the continental boundary layer (BL). Many sites exhibit pronounced seasonality with summer time concentrations a factor of 2–10 greater than wintertime concentrations. We used these CN observations to evaluate primary and secondary sources of particle number in a global aerosol microphysics model. We found that emissions of primary particles can reasonably reproduce the spatial pattern of observed CN concentration (R2=0.46) but fail to explain the observed seasonal cycle (R2=0.1). The modeled CN concentration in the FT was biased low (normalised mean bias, NMB=−88%) unless a secondary source of particles was included, for example from binary homogeneous nucleation of sulfuric acid and water (NMB=−25%). Simulated CN concentrations in the continental BL were also biased low (NMB=−74%) unless the number emission of anthropogenic primary particles was increased or a mechanism that results in particle formation in the BL was included. We ran a number of simulations where we included an empirical BL nucleation mechanism either using the activation-type mechanism (nucleation rate, J, proportional to gas-phase sulfuric acid concentration to the power one) or kinetic-type mechanism (J proportional to sulfuric acid to the power two) with a range of nucleation coefficients. We found that the seasonal CN cycle observed at continental BL sites was better simulated by BL particle formation (R2=0.3) than by increasing the number emission from primary anthropogenic sources (R2=0.18). The nucleation constants that resulted in best overall match between model and observed CN concentrations were consistent with values derived in previous studies from detailed case studies at individual sites. In our model, kinetic and activation-type nucleation parameterizations gave similar agreement with observed monthly mean CN concentrations.

Emissions of sulphur hexafluoride (SF6), one of the strongest greenhouse gases on a per molecule basis, are targeted to be collectively reduced under the Kyoto Protocol. Because of its long atmospheric lifetime (estimated as 800 to 3200 years), the accumulation of SF6 in the atmosphere is a direct measure of its global emissions. Examination of our extended data set of globally distributed high-precision SF6 observations shows an increase in SF6 abundance from near zero in the 1970s to a global mean of 6.7 ppt by the end of 2008. In-depth evaluation of our long-term data records shows that the global source of SF6 decreased after 1995, most likely due to SF6 emission reductions in industrialised countries, but increased again after 1998. By subtracting those emissions reported by Annex I countries to the United Nations Framework Convention of Climatic Change (UNFCCC) from our observation-inferred SF6 source leaves a surprisingly large gap of more than 70–80% of non-reported SF6 emissions in the last decade. This suggests a strong under-estimation of emissions in Annex I countries and underlines the urgent need for independent atmospheric verification of greenhouse gases emissions accounting.

Recent ground-based and space borne observations suggest the presence of significant amounts of iodine monoxide in the boundary layer of Antarctica, which are expected to have an impact on the ozone budget and might contribute to the formation of new airborne particles. So far, the source of these iodine radicals has been unknown. This paper presents long-term measurements of iodine monoxide at the German Antarctic research station Neumayer, which indicate that high IO concentrations in the order of 50 ppb are present in the snow interstitial air. The measurements have been performed using multi-axis differential optical absorption spectroscopy (MAX-DOAS). Using a coupled atmosphere – snowpack radiative transfer model, the comparison of the signals observed from scattered skylight and from light reflected by the snowpack yields several ppb of iodine monoxide in the upper layers of the sunlit snowpack throughout the year. Snow pit samples from Neumayer Station contain up to 700 ng/l of total iodine, representing a sufficient reservoir for these extraordinarily high IO concentrations.

It has been shown that sunlit snow and ice plays an important role in processing atmospheric species. Photochemical production of a variety of chemicals has recently been reported to occur in snow/ice and the release of these photochemically generated species may significantly impact the chemistry of the overlying atmosphere. Nitrogen oxide and oxidant precursor fluxes have been measured in a number of snow covered environments, where in some cases the emissions significantly impact the overlying boundary layer. For example, photochemical ozone production (such as that occurring in polluted mid-latitudes) of 3–4 ppbv/day has been observed at South Pole, due to high OH and NO levels present in a relatively shallow boundary layer. Field and laboratory experiments have determined that the origin of the observed NOx flux is the photochemistry of nitrate within the snowpack, however some details of the mechanism have not yet been elucidated. A variety of low molecular weight organic compounds have been shown to be emitted from sunlit snowpacks, the source of which has been proposed to be either direct or indirect photo-oxidation of natural organic materials present in the snow. Although myriad studies have observed active processing of species within irradiated snowpacks, the fundamental chemistry occurring remains poorly understood. Here we consider the nature of snow at a fundamental, physical level; photochemical processes within snow and the caveats needed for comparison to atmospheric photochemistry; our current understanding of nitrogen, oxidant, halogen and organic photochemistry within snow; the current limitations faced by the field and implications for the future.