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One year of Raman lidar observations of free-tropospheric aerosol layers over South Africa

Raman lidar data obtained over a 1 year period has been analysed in relation to aerosol layers in the free troposphere over the Highveld in South Africa. In total, 375 layers were observed above the boundary layer during the period 30 January 2010 to 31 January 2011. The seasonal behaviour of aerosol layer geometrical characteristics, as well as intensive and extensive optical properties were studied. The highest centre heights of free-tropospheric layers were observed during the South African spring (2520 ± 970 m a.g.l., also elsewhere). The geometrical layer depth was found to be maximum during spring, while it did not show any significant difference for the rest of the seasons. The variability of the analysed intensive and extensive optical properties was high during all seasons. Layers were observed at a mean centre height of 2100 ± 1000 m with an average lidar ratio of 67 ± 25 sr (mean value with 1 standard deviation) at 355 nm and a mean extinction-related Ångström exponent of 1.9 ± 0.8 between 355 and 532 nm during the period under study. Except for the intensive biomass burning period from August to October, the lidar ratios and Ångström exponents are within the range of previous observations for urban/industrial aerosols. During Southern Hemispheric spring, the biomass burning activity is clearly reflected in the optical properties of the observed free-tropospheric layers. Specifically, lidar ratios at 355 nm were 89 ± 21, 57 ± 20, 59 ± 22 and 65 ± 23 sr during spring (September–November), summer (December–February), autumn (March–May) and winter (June–August), respectively. The extinction-related Ångström exponents between 355 and 532 nm measured during spring, summer, autumn and winter were 1.8 ± 0.6, 2.4 ± 0.9, 1.8 ± 0.9 and 1.8 ± 0.6, respectively. The mean columnar aerosol optical depth (AOD) obtained from lidar measurements was found to be 0.46 ± 0.35 at 355 nm and 0.25 ± 0.2 at 532 nm. The contribution of free-tropospheric aerosols on the AOD had a wide range of values with a mean contribution of 46%.
Sources of black carbon aerosols in South Asia and surrounding regions during the Integrated Campaign for Aerosols, Gases and Radiation Budget (ICARB)

This study examines differences in the surface black carbon (BC) aerosol loading between the Bay of Bengal (BoB) and the Arabian Sea (AS) and identifies dominant sources of BC in South Asia and surrounding regions during March–May 2006 (Integrated Campaign for Aerosols, Gases and Radiation Budget, ICARB) period. A total of 13 BC tracers are introduced in the Weather Research and Forecasting Model coupled with Chemistry to address these objectives. The model reproduced the temporal and spatial variability of BC distribution observed over the AS and the BoB during the ICARB ship cruise and captured spatial variability at the inland sites. In general, the model underestimates the observed BC mass concentrations. However, the model–observation discrepancy in this study is smaller compared to previous studies. Model results show that ICARB measurements were fairly well representative of the AS and the BoB during the pre-monsoon season. Elevated BC mass concentrations in the BoB are due to 5 times stronger influence of anthropogenic emissions on the BoB compared to the AS. Biomass burning in Burma also affects the BoB much more strongly than the AS. Results show that anthropogenic and biomass burning emissions, respectively, accounted for 60 and 37% of the average ± standard deviation (representing spatial and temporal variability) BC mass concentration (1341 ± 2353 ng m−3) in South Asia. BC emissions from residential (61%) and industrial (23%) sectors are the major anthropogenic sources, except in the Himalayas where vehicular emissions dominate. We find that regional-scale transport of anthropogenic emissions contributes up to 25% of BC mass concentrations in western and eastern India, suggesting that surface BC mass concentrations cannot be linked directly to the local emissions in different regions of South Asia.
Impacts of emission reductions on aerosol radiative effects

The global aerosol–climate model ECHAM-HAMMOZ was used to investigate changes in the aerosol burden and aerosol radiative effects in the coming decades. Four different emissions scenarios were applied for 2030 (two of them applied also for 2020) and the results were compared against the reference year 2005. Two of the scenarios are based on current legislation reductions: one shows the maximum potential of reductions that can be achieved by technical measures, and the other is targeted to short-lived climate forcers (SLCFs). We have analyzed the results in terms of global means and additionally focused on eight subregions. Based on our results, aerosol burdens show an overall decreasing trend as they basically follow the changes in primary and precursor emissions. However, in some locations, such as India, the burdens could increase significantly. The declining emissions have an impact on the clear-sky direct aerosol effect (DRE), i.e. the cooling effect. The DRE could decrease globally 0.06–0.4 W m−2 by 2030 with some regional increases, for example, over India (up to 0.84 W m−2). The global changes in the DRE depend on the scenario and are smallest in the targeted SLCF simulation. The aerosol indirect radiative effect could decline 0.25–0.82 W m−2 by 2030. This decrease takes place mostly over the oceans, whereas the DRE changes are greatest over the continents. Our results show that targeted emission reduction measures can be a much better choice for the climate than overall high reductions globally. Our simulations also suggest that more than half of the near-future forcing change is due to the radiative effects associated with aerosol–cloud interactions.
Free amino acids in Antarctic aerosol: potential markers for the evolution and fate of marine aerosol

To investigate the impact of marine aerosols on global climate change it is important to study their chemical composition and size distribution. Amino acids are a component of the organic nitrogen in aerosols and particles containing amino acids have been found to be efficient ice nuclei. The main aim of this study was to investigate the L- and D-free amino acid composition as possible tracers of primary biological production in Antarctic aerosols from three different areas: two continental bases, Mario Zucchelli Station (MZS) on the coast of the Ross Sea, Concordia Station at Dome C on the Antarctic Plateau, and the Southern Ocean near the Antarctic continent. Studying the size distribution of amino acids in aerosols allowed us to characterize this component of the water-soluble organic carbon (WSOC) in marine aerosols near their source and after long-range transport. The presence of only free L-amino acids in our samples is indicative of the prevalence of phytoplanktonic material. Sampling at these three points allowed us to study the reactivity of these compounds during long-range transport. The mean total amino acid concentration detected at MZS was 11 pmol m−3, a higher percentage of amino acids were found in the fine fraction. The aerosol samples collected at Dome C had the lowest amino acid values (0.7 and 0.8 pmol m−3), and the coarse particles were found to have higher concentrations of amino acids compared to the coastal site. The amino acid composition in the aerosol collected at Dome C had also changed compared to the coastal site, suggesting that physical and chemical transformations had occurred during long range transport. During the sampling cruise on the R/V Italica on the Southern Ocean, high concentrations of amino acids were found in the total suspended particles, this we attribute to the presence of intact biological material (as microorganisms or plant material) in the sample.
AOD trends during 2001–2010 from observations and model simulations

The aerosol optical depth (AOD) trend between 2001 and 2010 is estimated globally and regionally from observations and results from simulations with the EMAC (ECHAM5/MESSy Atmospheric Chemistry) model. Although interannual variability is applied only to anthropogenic and biomass-burning emissions, the model is able to quantitatively reproduce the AOD trends as observed by the MODIS (Moderate Resolution Imaging Spectroradiometer) satellite sensor, while some discrepancies are found when compared to MISR (Multi-angle Imaging SpectroRadiometer) and SeaWIFS (Sea-viewing Wide Field-of-view Sensor) observations. Thanks to an additional simulation without any change in emissions, it is shown that decreasing AOD trends over the US and Europe are due to the decrease in the emissions, while over the Sahara Desert and the Middle East region, the meteorological changes play a major role. Over Southeast Asia, both meteorology and emissions changes are equally important in defining AOD trends. Additionally, decomposing the regional AOD trends into individual aerosol components reveals that the soluble components are the most dominant contributors to the total AOD, as their influence on the total AOD is enhanced by the aerosol water content.
Iodine observed in new particle formation events in the Arctic atmosphere during ACCACIA

Accurately accounting for new particle formation (NPF) is crucial to our ability to predict aerosol number concentrations in many environments and thus cloud properties, which is in turn vital in simulating radiative transfer and climate. Here we present an analysis of NPF events observed in the Greenland Sea during the summertime as part of the Aerosol-Cloud Coupling And Climate Interactions in the Arctic (ACCACIA) project. While NPF events have been reported in the Arctic before, we were able, for the first time, to detect iodine in the growing particles using an Aerosol Mass Spectrometer (AMS) during a persistent event in the region of the coastal sea-ice near Greenland. Given the potency of iodine as a nucleation precursor, the results imply that iodine was responsible for the initial NPF, a phenomenon that has been reported at lower latitudes and associated with molecular iodine emissions from coastal macroalgae. The initial source of iodine in this instance is not clear, but it was associated with air originating approximately 1 day previously over melting coastal sea-ice. These results show that atmospheric models must consider iodine as a source of new particles in addition to established precursors such as sulfur compounds.
Evaluation of a regional air quality model using satellite column NO2: treatment of observation errors and model boundary conditions and emissions

We compare tropospheric column NO2 between the UK Met Office operational Air Quality in the Unified Model (AQUM) and satellite observations from the Ozone Monitoring Instrument (OMI) for 2006. Column NO2 retrievals from satellite instruments are prone to large uncertainty from random, systematic and smoothing errors. We present an algorithm to reduce the random error of time-averaged observations, once smoothing errors have been removed with application of satellite averaging kernels to the model data. This reduces the total error in seasonal mean columns by 10–70%, which allows critical evaluation of the model. The standard AQUM configuration evaluated here uses chemical lateral boundary conditions (LBCs) from the GEMS (Global and regional Earth-system Monitoring using Satellite and in situ data) reanalysis. In summer the standard AQUM overestimates column NO2 in northern England and Scotland, but underestimates it over continental Europe. In winter, the model overestimates column NO2 across the domain. We show that missing heterogeneous hydrolysis of N2O5 in AQUM is a significant sink of column NO2 and that the introduction of this process corrects some of the winter biases. The sensitivity of AQUM summer column NO2 to different chemical LBCs and NOx emissions data sets are investigated. Using Monitoring Atmospheric Composition and Climate (MACC) LBCs increases AQUM O3 concentrations compared with the default GEMS LBCs. This enhances the NOx–O3 coupling leading to increased AQUM column NO2 in both summer and winter degrading the comparisons with OMI. Sensitivity experiments suggest that the cause of the remaining northern England and Scotland summer column NO2 overestimation is the representation of point source (power station) emissions in the model.
Precipitation effects of giant cloud condensation nuclei artificially introduced into stratocumulus clouds

To study the effect of giant cloud condensation nuclei (GCCN) on precipitation processes in stratocumulus clouds, 1–10 μm diameter salt particles (salt powder) were released from an aircraft while flying near the cloud top on 3 August 2011 off the central coast of California. The seeded area was subsequently sampled from the aircraft that was equipped with aerosol, cloud, and precipitation probes and an upward-facing cloud radar. During post-seeding sampling, made 30–60 min after seeding, the mean cloud droplet size increased, the droplet number concentration decreased, and large drop (e.g., diameter larger than 10 μm) concentration increased. Average drizzle rates increased from about 0.05 to 0.20 mm h−1, and the liquid water path decreased from about 52 to 43 g m−2. Strong radar returns associated with drizzle were observed on the post-seeding cloud-base level-leg flights and were accompanied by a substantial depletion of the cloud liquid water content. The changes were large enough to suggest that the salt particles with concentrations estimated to be 10−2 to 10-4 cm−3 resulted in a four-fold increase in the cloud-base rainfall rate and depletion of the cloud water due to rainout. In contrast, a case is shown where the cloud was already precipitating (on 10 August) and the effect of adding GCCN to the cloud was insignificant.
OClO and BrO observations in the volcanic plume of Mt. Etna – implications on the chemistry of chlorine and bromine species in volcanic plumes

Spatial and temporal profiles of chlorine dioxide (OClO), bromine monoxide (BrO) and sulfur dioxide (SO2) of the volcanic plume at Mt. Etna, Italy, were investigated in September 2012 using Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS). OClO was detected in 119 individual measurements covering plume ages up to 6 min. BrO could be detected in 452 spectra up to 23 min downwind. The retrieved slant column densities (SCDs) reached maximum values of 2.0 × 1014 molecules cm-2 (OClO) and 1.1 × 1015 molecules cm-2 (BrO). Mean mixing ratios of BrO and OClO were estimated assuming a circular plume cross section. Furthermore, ClO mixing ratios were derived directly from the BrO and OClO-SCDs. Average abundances of BrO = 1.35 ppb, OClO = 300 ppt and ClO = 139 ppt were found in the young plume (plume age τ < 4 min) with peak values of 2.7 ppb (BrO), 600 ppt (OClO) and 235 ppt (ClO) respectively. The chemical evolution of BrO and OClO in the plume was investigated in great detail by analysing the OClO/SO2 and BrO/SO2 ratios as a function of plume age τ. A marked increase of both ratios was observed in the young plume (τ < 142 s) and a levelling off at larger plume ages showing mean SO2 ratios of 3.17 × 10-5 (OClO/SO2) and 1.65 × 10-4 (BrO/SO2). OClO was less abundant in the plume compared to BrO with a mean OClO/BrO ratio of 0.16 at plume ages exceeding 3 min. A measurement performed in the early morning at low solar radiances revealed BrO/SO2 and OClO/SO2 ratios increasing with time. This observation substantiates the importance of photochemistry regarding the formation of BrO and OClO in volcanic plumes. These findings support the current understanding of the underlying chemistry, namely, that BrO is formed in an autocatalytic, heterogeneous reaction mechanism (in literature often referred to as "bromine explosion") and that OClO is formed in the reaction of OClO with BrO. These new findings, especially the very detailed observation of the BrO and OClO formation in the young plume, were used to infer the prevailing Cl-atom concentrations in the plume. Relatively small values ranging from [Cl] = 2.5 × 106 cm-3 (assuming 80 ppb background O3) to [Cl] = 2.0 × 108 cm-3 (at 1 ppb O3) were calculated at plume ages of about 2 min. Based on these Cl abundances, a potential – chlorine-induced – depletion of tropospheric methane (CH4) in the plume was investigated. CH4 lifetimes between 14 h (at 1 ppb O3) and 47 days (at 80 ppb O3) were derived. While these lifetimes are considerably shorter than the atmospheric lifetime of CH4, the impact of gaseous chlorine on the CH4 budget in the plume environment should nevertheless be relatively small due to plume dispersion (decreasing Cl concentrations) and ongoing mixing of the plume with the surrounding atmosphere (replenishing O3 and CH4). In addition, all spectra were analysed for signatures of IO, OIO and BrO. None of these species could be detected. Upper limits for IO/SO2, OIO/SO2 and OBrO/SO2 are 1.8 × 10-6, 2.0 × 10-5 and 1.1 × 10-5 respectively.
Molecular composition of fresh and aged secondary organic aerosol from a mixture of biogenic volatile compounds: a high-resolution mass spectrometry study

Field observations over the past decade indicate that a significant fraction of organic aerosol in remote areas may contain highly oxidized molecules. Aerosol processing or further oxidation (aging) of organic aerosol has been suggested to be responsible for their formation through heterogeneous reaction with oxidants and multigenerational oxidation of vapours by OH radicals. In this study we investigated the influence of several aging processes on the molecular composition of secondary organic aerosols (SOA) using direct infusion and liquid chromatography high-resolution mass spectrometry. SOA was formed in simulation chamber experiments from ozonolysis of a mixture of four biogenic volatile organic compounds (BVOC): α-pinene, β-pinene, Δ3-carene and isoprene. The SOA was subsequently aged under three different sets of conditions: in the dark in the presence of residual ozone, with UV irradiation and OH radicals, and using UV light only. Among all studied conditions, only OH radical-initiated aging was found to influence the molecular composition of the aerosol and showed an increase in carbon oxidation state (OSC) and elemental O / C ratios of the SOA components. None of the aging processes produced an observable effect on the oligomers formed from ozonolysis of the BVOC mixture, which were found to be equally abundant in both "fresh" and "aged" SOA. Additional experiments using α-pinene as the sole precursor demonstrated that oligomers are an important group of compounds in SOA produced from both ozonolysis and OH radical-initiated oxidation processes; however, a completely different set of oligomers is formed under these two oxidation regimes. SOA from the OH-initiated oxidation of α-pinene had a significantly higher overall OSC and O / C compared to that from pure ozonolysis experiments confirming that the OH radical reaction is more likely to be responsible for the occurrence of highly oxidized species in ambient biogenic SOA.