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The scattering and backscattering enhancement factors (f(RH) and fb(RH)) describe how aerosol particle light scattering and backscattering, respectively, change with relative humidity (RH). They are important parameters in estimating direct aerosol radiative forcing (DARF). In this study we use a dataset presented in Burgos et al. (2019) that compiles f(RH) and fb(RH) measurements at three wavelengths (i.e. 450, 550 and 700 nm) performed with tandem nephelometer systems at multiple sites around the world. We present an overview of f(RH) and fb(RH) based on both long-term and campaign observations from 23 sites representing a range of aerosol types. The scattering enhancement shows a strong variability from site to site, with no clear pattern with respect to total scattering coefficient. In general, higher f(RH) is observed at Arctic and marine sites while lower values are found at urban and desert sites, although a consistent pattern as a function of site type is not observed. The backscattering enhancement fb(RH) is consistently lower tan f(RH) at all sites, with the difference between f(RH) and fb(RH) increasing for aerosol with higher f(RH). This is consistent with Mie theory which predicts higher enhancement of the light-scattering in the forward than in the backward direction as the particle takes up water. Our results show that the scattering enhancement is higher for PM1 than PM10 at most sites, which is also supported by theory due to the change in scattering efficiency with the size parameter that relates particle size and wavelength of incident light. At marine-influenced sites this difference is enhanced when coarse particles (likely sea salt) predominate. For most sites, f(RH) is observed to increase with increasing wavelength, except at sites with a known dust influence where the spectral dependence of f(RH) is found to be low or even exhibit the opposite pattern. The impact of RH on aerosol properties used to calculate radiative forcing (e.g., single scattering albedo, ω0, and backscattered fraction, b) is evaluated. The single scattering albedo generally increases with RH while b decreases. The net effect of aerosol hygroscopicity on radiative forcing efficiency (RFE) is an increase in the absolute forcing effect (negative sign) by a factor of up to 4 at RH = 90 % compared to dry conditions (RH

Given the sensitivity of the Arctic climate to short-lived climate forcers, long-term in situ surface measurements of aerosol parameters are useful in gaining insight into the magnitude and variability of these climate forcings. Seasonality of aerosol optical properties – including the aerosol light-scattering coefficient, absorption coefficient, single-scattering albedo, scattering Ångström exponent, and asymmetry parameter – are presented for six monitoring sites throughout the Arctic: Alert, Canada; Barrow, USA; Pallas, Finland; Summit, Greenland; Tiksi, Russia; and Zeppelin Mountain, Ny-Ålesund, Svalbard, Norway. Results show annual variability in all parameters, though the seasonality of each aerosol optical property varies from site to site. There is a large diversity in magnitude and variability of scattering coefficient at all sites, reflecting differences in aerosol source, transport, and removal at different locations throughout the Arctic. Of the Arctic sites, the highest annual mean scattering coefficient is measured at Tiksi (12.47 Mm−1), and the lowest annual mean scattering coefficient is measured at Summit (1.74 Mm−1). At most sites, aerosol absorption peaks in the winter and spring, and has a minimum throughout the Arctic in the summer, indicative of the Arctic haze phenomenon; however, nuanced variations in seasonalities suggest that this phenomenon is not identically observed in all regions of the Arctic. The highest annual mean absorption coefficient is measured at Pallas (0.48 Mm−1), and Summit has the lowest annual mean absorption coefficient (0.12 Mm−1). At the Arctic monitoring stations analyzed here, mean annual single-scattering albedo ranges from 0.909 (at Pallas) to 0.960 (at Barrow), the mean annual scattering Ångström exponent ranges from 1.04 (at Barrow) to 1.80 (at Summit), and the mean asymmetry parameter ranges from 0.57 (at Alert) to 0.75 (at Summit). Systematic variability of aerosol optical properties in the Arctic supports the notion that the sites presented here measure a variety of aerosol populations, which also experience different removal mechanisms. A robust conclusion from the seasonal cycles presented is that the Arctic cannot be treated as one common and uniform environment but rather is a region with ample spatiotemporal variability in aerosols. This notion is important in considering the design or aerosol monitoring networks in the region and is important for informing climate models to better represent short-lived aerosol climate forcers in order to yield more accurate climate predictions for the Arctic.

Several types of filter-based instruments are used to estimate aerosol light absorption coefficients. Two significant results are presented based on Aethalometer measurements at six Arctic stations from 2012 to 2014. First, an alternative method of post-processing the Aethalometer data is presented, which reduces measurement noise and lowers the detection limit of the instrument more effectively than boxcar averaging. The biggest benefit of this approach can be achieved if instrument drift is minimised. Moreover, by using an attenuation threshold criterion for data post-processing, the relative uncertainty from the electronic noise of the instrument is kept constant. This approach results in a time series with a variable collection time (Δt) but with a constant relative uncertainty with regard to electronic noise in the instrument. An additional advantage of this method is that the detection limit of the instrument will be lowered at small aerosol concentrations at the expense of temporal resolution, whereas there is little to no loss in temporal resolution at high aerosol concentrations ( > 2.1–6.7 Mm−1 as measured by the Aethalometers). At high aerosol concentrations, minimising the detection limit of the instrument is less critical. Additionally, utilising co-located filter-based absorption photometers, a correction factor is presented for the Arctic that can be used in Aethalometer corrections available in literature. The correction factor of 3.45 was calculated for low-elevation Arctic stations. This correction factor harmonises Aethalometer attenuation coefficients with light absorption coefficients as measured by the co-located light absorption photometers. Using one correction factor for Arctic Aethalometers has the advantage that measurements between stations become more inter-comparable.

Long-term measurements of changes in the aerosol scattering coefficient hygroscopic growth at the U.S. Department of Energy Southern Great Plains site provide information on the seasonal as well as size and chemical dependence of aerosol water uptake. Annual average sub-10 μm fRH values (the ratio of aerosol scattering at 85%/40% relative humidity (RH)) were 1.78 and 1.99 for the gamma and kappa fit algorithms, respectively. The study found higher growth rates in the winter and spring seasons that correlated with a high aerosol nitrate mass fraction. fRH exhibited strong, but differing, correlations with the scattering Angstrom exponent and backscatter fraction, two optical size-dependent parameters. The aerosol organic mass fraction had a strong influence on fRH. Increases in the organic mass fraction and absorption Angstrom exponent coincided with a decrease in fRH. Similarly, fRH declined with decreases in the aerosol single scatter albedo. Uncertainty analysis of the fit algorithms revealed high uncertainty at low scattering coefficients and increased uncertainty at high RH and fit parameters values.

Long-term measurements of the light absorption coefficient (b(abs)) obtained with a particle soot absorption photometer (PSAP), b(abs) (PSAP), have been previously reported for Barrow, Alaska, and ...

The Arctic is a rapidly changing ecosystem, with complex aerosol-cloud-climate feedbacks contributing to more rapid warming of the region as compared to the mid-latitudes. Understanding changes to particle number concentration and size distributions is important to constraining estimates of the effect of anthropogenic activity on the region. During six years of semi-continuous measurements of particle number size distributions conducted near Utqiaġvik (Barrow), Alaska, 37 particle-growth events were observed. The majority of events occurred during spring and summer with a monthly maximum in June, similar to other Arctic sites. Based on backward air mass trajectory analysis, similar numbers of particle-growth events were influenced by marine (46%) and Prudhoe Bay air masses (33%), despite air primarily coming from the Arctic Ocean (75 ± 2% of days) compared to Prudhoe Bay (8 ± 2% of days). The corresponding normalized particle-growth event frequency suggests that emissions from Prudhoe Bay could induce an average of 92 particle-growth events, more than all other air mass sources combined, at Barrow annually. Prudhoe Bay is currently the third largest oil and gas field in the United States, and development in the Arctic region is expected to expand throughout the 21st century as the extent of summertime sea ice decreases. Elevated particle number concentrations due to human activity are likely to have profound impacts on climate change in the Arctic through direct, indirect, and surface albedo feedbacks, particularly through the addition of cloud condensation nuclei.

The uptake of water by atmospheric aerosols has a pronounced effect on particle light scattering properties which in turn are strongly dependent on the ambient relative humidity (RH). Earth system models need to account for the aerosol water uptake and its influence on light scattering in order to properly capture the overall radiative effects of aerosols. Here we present a comprehensive model-measurement evaluation of the particle light scattering enhancement factor f(RH), defined as the particle light scattering coefficient at elevated RH (here set to 85 %) divided by its dry value. The comparison uses simulations from 10 Earth system models and a global dataset of surface-based in situ measurements. In general, we find a large diversity in the magnitude of predicted f(RH) amongst the different models which can not be explained by the site types. There is strong indication that differences in the model parameterizations of hygroscopicity and perhaps mixing state are driving at least some of the observed diversity in simulated f(RH). An important finding is that the models show a significantly larger discrepancy with the observations if RHref = 0 % is chosen as the model reference RH compared to when RHref = 40 % is used. The multi-site average ratio between model outputs and measurements is 1.64 in the former case and 1.16 in the latter. The overestimation by the models is believed to originate from the hygroscopicity parameterizations at the lower RH range which may not implement all phenomena taking place (i.e. not fully dried particles and hysteresis effects). Our results emphasize the need to consider the measurement conditions in such comparisons and recognize that measurements referred to as dry may not be dry in model terms.

A reference dataset of multi-wavelength particle light scattering and hemispheric backscattering coefficients for different relative humidities (RH) between RH = 30 and 95% and wavelengths between λ = 450 nm and 700 nm is described in this work. Tandem-humidified nephelometer measurements from 26 ground-based sites around the globe, covering multiple aerosol types, have been re-analysed and harmonized into a single dataset. The dataset includes multi-annual measurements from longterm monitoring sites as well as short-term field campaign data. The result is a unique collection of RH-dependent aerosol light scattering properties, presented as a function of size cut. This dataset is important for climate and atmospheric model-measurement inter-comparisons, as a means to improve model performance, and may be useful for satellite and remote sensing evaluation using surface-based, in-situ measurements., This work was essentially supported by the Department of Energy (USA) under the project DE-SC0016541. The humidified nephelometer measurements at BRW and SGP were funded by the U.S. Department of Energy Atmospheric Radiation Measurement (DOE/ARM) program via Argonne National Laboratory. The DOE/ARM Program Climate Research Facility and the DOE Atmospheric Sciences Program funded the AMF deployments (FKB, GRW, HFE, MAO, NIM, PGH, PVC, PYE). Measurements at KCO were supported by the National Science Foundation (Grant ATM-961288). The CBG humidified nephelometer measurements were supported by the NOAA Climate Goal program. The HLM measurements were supported by DOE’s ASP program under grant DE-A102-05ER63996. The GSN measurements were supported by NSF grant 0138250. The humidified nephelometer measurements operated by the Paul Scherrer Institute (CES, JFJ, MEL, MHD, ZEP, and HYY) and the instrument development itself were financially supported by the projects ESA Climate Change Initiative Aerosol cci (ESRIN/Contract No. 4000101545/10/I-AM), the Swiss National Science Foundation (Advanced Postdoc.Mobility fellowship; Grant No. P300P2_147776), and by the EC-projects Global Earth Observation and Monitoring (GEOmon, contract 036677) and European Supersites for Atmospheric Atmospheric Aerosol Research (EUSAAR, contract 026140). The measurements of the University of Granada (UGR) were supported by the Spanish Agencia Estatal de Investigación, AEI, through projects CGL2016-81092-R and CGL2017-90884- REDT and the European Union’s Horizon 2020 research and innovation program through project ACTRIS-2 (Grant Agreement No. 654109). The Lin’an site observation was supported by the National Natural Science Foundation of China (41475118). We thank Markus Fiebig, Richard Olav Rud, and Paul Eckhardt (NILU, Norway) for their great help to prepare and submit the data files to the EBAS and ACTRIS data centre. Open access funding provided by Stockholm University.

Cloud condensation nuclei (CCN) number concentrations alongside with submicrometer particle number size distributions and particle chemical composition have been measured at atmospheric observatories of the Aerosols, Clouds, and Trace gases Research InfraStructure (ACTRIS) as well as other international sites over multiple years. Here, harmonized data records from 11 observatories are summarized, spanning 98,677 instrument hours for CCN data, 157,880 for particle number size distributions, and 70,817 for chemical composition data. The observatories represent nine different environments, e.g., Arctic, Atlantic, Pacific and Mediterranean maritime, boreal forest, or high alpine atmospheric conditions. This is a unique collection of aerosol particle properties most relevant for studying aerosol-cloud interactions which constitute the largest uncertainty in anthropogenic radiative forcing of the climate. The dataset is appropriate for comprehensive aerosol characterization (e.g., closure studies of CCN), model-measurement intercomparison and satellite retrieval method evaluation, among others. Data have been acquired and processed following international recommendations for quality assurance and have undergone multiple stages of quality assessment.

The Two-Column Aerosol Project (TCAP), conducted from June 2012 through June 2013, was a unique study designed to provide a comprehensive data set that can be used to investigate a number of important climate science questions, including those related to aerosol mixing state and aerosol radiative forcing. The study was designed to sample the atmosphere between and within two atmospheric columns; one fixed near the coast of North America (over Cape Cod, MA) and a second moveable column over the Atlantic Ocean several hundred kilometers from the coast. The U.S. Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) Mobile Facility (AMF) was deployed at the base of the Cape Cod column, and the ARM Aerial Facility was utilized for the summer and winter intensive observation periods. One important finding from TCAP is that four of six nearly cloud-free flight days had aerosol layers aloft in both the Cape Cod and maritime columns that were detected using the nadir pointing second-generation NASA high-spectral resolution lidar (HSRL-2). These layers contributed up to 60% of the total observed aerosol optical depth (AOD). Many of these layers were also intercepted by the aircraft configured for in situ sampling, and the aerosol in the layers was found to have increased amounts of biomass burning material and nitrate compared to aerosol found near the surface. In addition, while there was a great deal of spatial and day-to-day variability in the aerosol chemical composition and optical properties, no systematic differences between the two columns were observed.

Hourly averaged aerosol optical properties (AOPs) measured over the years 2010–2013 at four continental North American NOAA Earth System Research Laboratory (NOAA/ESRL) cooperative aerosol network sites – Southern Great Plains near Lamont, OK (SGP), Bondville, IL (BND), Appalachian State University in Boone, NC (APP), and Egbert, Ontario, Canada (EGB) are analyzed. Aerosol optical properties measured over 1996–2009 at BND and 1997–2009 at SGP are also presented. The aerosol sources and types in the four regions differ enough so as to collectively represent rural, anthropogenically perturbed air conditions over much of eastern continental North America. Temporal AOP variability on monthly, weekly, and diurnal timescales is presented for each site. Differences in annually averaged AOPs and those for individual months at the four sites are used to examine regional AOP variability. Temporal and regional variability are placed in the context of reported aerosol chemistry at the sites, meteorological measurements (wind direction, temperature), and reported regional mixing layer heights. Basic trend analysis is conducted for selected AOPs at the long-term sites (BND and SGP). Systematic relationships among AOPs are also presented. Seasonal variability in PM1 (sub-1 μm particulate matter) scattering and absorption coefficients at 550 nm (σsp and σap, respectively) and most of the other PM1 AOPs is much larger than day of week and diurnal variability at all sites. All sites demonstrate summer σsp and σap peaks. Scattering coefficient decreases by a factor of 2–4 in September–October and coincides with minimum single-scattering albedo (ω0) and maximum hemispheric backscatter fraction (b). The co-variation of ω0 and b lead to insignificant annual cycles in top-of-atmosphere direct radiative forcing efficiency (DRFE) at APP and SGP. Much larger annual DRFE cycle amplitudes are observed at EGB (~ 40 %) and BND (~ 25 %), with least negative DRFE in September–October at both sites. Secondary winter peaks in σsp are observed at all sites except APP. Amplitudes of diurnal and weekly cycles in σap at the sites are larger for all seasons than those of σsp, with the largest differences occurring in summer. The weekly and diurnal cycle amplitudes of most intensive AOPs (e.g., those derived from ratios of measured σsp and σap) are minimal in most cases, especially those related to parameterizations of aerosol size distribution. Statistically significant trends in σsp (decreasing), PM1 scattering fraction (decreasing), and b (increasing) are found at BND from 1996 to 2013 and at SGP from 1997 to 2013. A statistically significant decreasing trend in PM10 scattering Ångström exponent is also observed for SGP but not BND. Most systematic relationships among AOPs are similar for the four sites and are adequately described for individual seasons by annually averaged relationships, although relationships involving absorption Ångström exponent vary with site and season.

We examine the relationship between the number concentration of boundary-layer cloud condensation nuclei (CCN) and light extinction to investigate underlying aerosol processes and satellite-based CCN estimates. For a variety of airborne and ground-based observations not dominated by dust, regression identifies the CCN (cm−3) at 0.4 ± 0.1% supersaturation with 100.3α +1.3σ0.75 where σ (Mm−1) is the 500 nm extinction coefficient by dried particles and α is the Angstrom exponent. The deviation of 1 km horizontal average data from this approximation is typically within a factor of 2.0. ∂logCCN / ∂logσ is less than unity because, among other explanations, growth processes generally make aerosols scatter more light without increasing their number. This, barring special meteorology–aerosol connections, associates a doubling of aerosol optical depth with less than a doubling of CCN, contrary to previous studies based on heavily averaged measurements or a satellite algorithm.

Capsule: A 21-month deployment to Graciosa Island in the northeastern Atlantic Ocean is providing an unprecedented record of the clouds, aerosols and meteorology in a poorly-sampled remote marine environment The Clouds, Aerosol, and Precipitation in the Marine Boundary Layer (CAP-MBL) deployment at Graciosa Island in the Azores generated a 21 month (April 2009- December 2010) comprehensive dataset documenting clouds, aerosols and precipitation using the Atmospheric Radiation Measurement (ARM) Mobile Facility (AMF). The scientific aim of the deployment is to gain improved understanding of the interactions of clouds, aerosols and precipitation in the marine boundary layer. Graciosa Island straddles the boundary between the subtropics and midlatitudes in the Northeast Atlantic Ocean, and consequently experiences a great diversity of meteorological and cloudiness conditions. Low clouds are the dominant cloud type, with stratocumulus and cumulus occurring regularly. Approximately half of all clouds contained precipitation detectable as radar echoes below the cloud base. Radar and satellite observations show that clouds with tops from 1- 11 km contribute more or less equally to surface-measured precipitation at Graciosa. A wide range of aerosol conditions was sampled during the deployment consistent with the diversity of sources as indicated by back trajectory analysis. Preliminary findings suggest important two-way interactions between aerosols and clouds at Graciosa, with aerosols affecting light precipitation and cloud radiative properties while being controlled in part by precipitation scavenging. The data from at Graciosa are being compared with short-range forecasts made a variety of models. A pilot analysis with two climate and two weather forecast models shows that they reproduce the observed time-varying vertical structure of lower-tropospheric cloud fairly well, but the cloud-nucleating aerosol concentrations less well. The Graciosa site has been chosen to be a permanent fixed ARM site that became operational in October 2013.

A 4-year record of aerosol size and hygroscopic growth factor distributions measured at the Department of Energy’s SGP ARM site in Oklahoma, U.S. were used to estimate supersaturation (S)-dependent cloud condensation nuclei concentrations (NCCN). Baseline or reference NCCN(S) spectra were estimated by using the data to create a matrix of size- and hygroscopicity-dependent number concentration (N) and then integrating for S > critical supersaturation (Sc) calculated for the same size and hygroscopicity pairs using κ-Köhler Theory. The accuracy of those estimates was assessed through comparison with the directly measured NCCN at the same site. Subsequently, NCCN was calculated using the same dataset but with an array of simplified treatments in which the aerosol was assumed to be either an internal or an external mixture and the hygroscopicity either assumed or based on averages derived from the growth factor distributions. The CCN spectra calculated using the simplified treatments were compared with those from the baseline approach to evaluate the impact of commonly used approximations. Among the simplified approaches, assuming the aerosol is an internal mixture with size-dependent hygroscopicity parameter (κ) resulted in estimates closest to those from the baseline approach over the range in S considered.

We propose here a novel approach for retrieving in parallel the effective density and real refractive index of weakly absorbing aerosol from optical and size distribution measurements. Here we define "weakly absorbing" as aerosol single-scattering albedos that exceed 0.95 at 0.5 μm. The required optical measurements are the scattering coefficient and the hemispheric backscatter fraction, obtained in this work from an integrating nephelometer. The required size spectra come from mobility and aerodynamic particle size spectrometers commonly referred to as a scanning mobility particle sizer and an aerodynamic particle sizer. The performance of this approach is first evaluated using a sensitivity study with synthetically generated but measurement-related inputs. The sensitivity study reveals that the proposed approach is robust to random noise; additionally the uncertainties of the retrieval are almost linearly proportional to the measurement errors, and these uncertainties are smaller for the real refractive index than for the effective density. Next, actual measurements are used to evaluate our approach. These measurements include the optical, microphysical, and chemical properties of weakly absorbing aerosol which are representative of a variety of coastal summertime conditions observed during the Two-Column Aerosol Project (TCAP; http://campaign.arm.gov/tcap/). The evaluation includes calculating the root mean square error (RMSE) between the aerosol characteristics retrieved by our approach, and the same quantities calculated using the conventional volume mixing rule for chemical constituents. For dry conditions (defined in this work as relative humidity less than 55%) and sub-micron particles, a very good (RMSE ~ 3%) and reasonable (RMSE ~ 28%) agreement is obtained for the retrieved real refractive index (1.49 ± 0.02) and effective density (1.68 ± 0.21), respectively. Our approach permits discrimination between the retrieved aerosol characteristics of sub-micron and sub-10-micron particles. The evaluation results also reveal that the retrieved density and refractive index tend to decrease with an increase of the relative humidity.

We have extensively evaluated the response of cloud base drizzle rate (Rcb; mm d−1) in warm clouds to liquid water path (LWP; g m−2) and to cloud condensation nuclei (CCN) number concentration (NCCN; cm−3), an aerosol proxy. This evaluation is based on a 19 month long data set of Doppler radar, lidar, microwave radiometers, and aerosol observing systems from the Atmospheric Radiation Measurement (ARM) Mobile Facility deployments at the Azores and in Germany. Assuming 0.55% supersaturation to calculate NCCN, we found a power law Rcb=0.0015±0.0009⋅LWP1.68±0.05NCCN−0.66±0.08, indicating that Rcb decreases by a factor of 2–3 as NCCN increases from 200 to 1000 cm−3 for fixed LWP. Additionally, the precipitation susceptibility to NCCN ranges between 0.5 and 0.9, in agreement with values from simulations and aircraft measurements. Surprisingly, the susceptibility of the probability of precipitation from our analysis is much higher than that from CloudSat estimates but agrees well with simulations from a multiscale high-resolution aerosol-climate model. Although scale issues are not completely resolved in the intercomparisons, our results are encouraging, suggesting that it is possible for multiscale models to accurately simulate the response of LWP to aerosol perturbations.

Aerosol-cloud interactions (ACI) constitute the single largest uncertainty in anthropogenic radiative forcing. To reduce the uncertainties and gain more confidence in the simulation of ACI, models need to be evaluated against observations, in particular against measurements of cloud condensation nuclei (CCN). Numerous observations of CCN number concentration exist, and many closure studies have been performed to predict CCN number concentrations based on particle number size distributions, chemical composition, and the κ-Köhler theory. Most of these studies provide details for short time periods or focus on special environmental conditions. These observations, however, cannot address questions of large-scale temporal and spatial CCN variability. Here we analyze long-term observations of CCN number concentrations, particle number size distributions and chemical composition from twelve sites on three continents. Eight of these stations are part of the European Aerosols, Clouds, and Trace gases Research InfraStructure (ACTRIS). We group the observatories into categories according to their official classification: coastal background (Barrow, Alaska; Mace Head, Ireland; Finokalia, Crete; Noto Peninsula, Japan), rural background (Melpitz, Germany; Cabauw, the Netherlands; Vavihill, Sweden), alpine sites (Puy de Dôme, France; Jungfraujoch, Switzerland), remote forest sites (ATTO, Brazil; SMEAR, Finland) and the urban environment (Seoul, South Korea). Expectedly, CCN characteristics are highly variable across regions. However, they also vary within categories, most strongly in the coastal background group, where CCN number concentrations can vary by up to a factor of 30 within one season. In terms of particle activation behavior, most continental stations exhibit very similar relative activation ratios across the range of 0.1 to 1.0 % supersaturation. At the coastal sites the activation ratios spread more widely across the SS spectrum. Several stations show strong seasonal cycles of CCN number concentrations and particle number size distributions, e.g., at Barrow (Arctic Haze in spring), at the alpine stations (stronger influence of polluted boundary layer air masses in summer), the rain forest (wet and dry season), or Finokalia (forest fire influence in fall). The rural background and urban sites exhibit relatively little variability throughout the year while short-term variability can be high especially at the urban site. The average hygroscopicity parameter, κ, calculated from the chemical composition of submicron particles, was highest at the coastal site of Mace Head (0.6) and the lowest at the rain forest station ATTO (0.2–0.3). We performed closure studies to predict CCN number concentrations from the particle number size distribution and chemical composition measurements. The prediction accuracy for the average concentrations is high. The ratio between predicted and measured CCN concentrations is between 0.87 and 1.4. The temporal variability is also well represented, as reflected by Pearson correlation coefficients > 0.87. We also conducted a series of sensitivity studies for the ratio of predicted versus measured CCN concentration, where we varied the hygroscopicity parameter κ, and made simple assumptions for aerosol particle number concentrations and size distributions. Uncertain particle number concentrations and their size distributions significantly impair the accuracy in predicting temporal variability and hence of absolute concentrations, while the effect of uncertain κ values is limited to the predicted CCN number concentration. Information on CCN number concentrations at many locations is important to better characterize ACI and their radiative forcing. Long-term comprehensive aerosol particle characterizations are labor intensive and costly. For observatories where such efforts are out of scope to obtain nevertheless long-term information of CCN number concentrations, we recommend conducting collocated CCN number concentration and particle number size distribution measurements at individual locations throughout one year at least to derive a seasonally resolved hygroscopicity parameter. This way, CCN number concentrations can be calculated based on continued particle number size distribution information only. This approach is a good alternative to deriving kappa from time-resolved chemical composition measurements which are costly and may still not cover the appropriate size range. Additionally, given the variability in observations at sites of the same category, a certain density in spatial coverage of observations is needed, especially along coastlines. We recommend operating "migrating-CCNCs" at priority locations, identified by model evaluation, around the globe where long-term particle number size distribution data are already available.

Cloud condensation nuclei (CCN) number concentrations alongside with submicrometer particle number size distributions and particle chemical composition have been measured at atmospheric observatories of the Aerosols, Clouds, and Trace gases Research InfraStructure (ACTRIS) as well as other international sites over multiple years. Here, harmonized data records from 11 observatories are summarized, spanning 98,677 instrument hours for CCN data, 157,880 for particle number size distributions, and 70,817 for chemical composition data. The observatories represent nine different environments, e.g., Arctic, Atlantic, Pacific and Mediterranean maritime, boreal forest, or high alpine atmospheric conditions. This is a unique collection of aerosol particle properties most relevant for studying aerosol-cloud interactions which constitute the largest uncertainty in anthropogenic radiative forcing of the climate. The dataset is appropriate for comprehensive aerosol characterization (e.g., closure studies of CCN), model-measurement intercomparison and satellite retrieval method evaluation, among others. Data have been acquired and processed following international recommendations for quality assurance and have undergone multiple stages of quality assessment.

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.

Several types of filter-based instruments are used to estimate aerosol light absorption coefficients.Two significant results are presented based on Aethalometer measurements at six Arctic station from 2012–2014. First, an alternative method of post-processing the Aethalometer data is presented which reduces measurement noise and lowers the detection limit of the instrument more effectively than boxcar averaging. The biggest benefit of this approach can be achieved if instrument drift is minimized. Moreover, by using an attenuation threshold criterion for data post-processing, the relative uncertainty from the electronic noise the instrument is kept constant. This approach results in a time series with a variable collection time (Δt), but with a constant relative uncertainty with regard to electronic noise in the instrument. An additional advantage of this method is that the detection limit of the instrument will be lowered at small aerosol concentrations at the expense of temporal resolution, whereas there is little to no loss in temporal resolution at high aerosol concentrations (>2.1–6.7 Mm−1 as measured by the Aethalometers). At high aerosol concentrations, minimizing the detection limit of the instrument is less critical. Second, utilizing co-located reference methods of aerosol absorption, a multiple cattering enhancement factor (Cref) of 3.10 specific to low elevation Arctic stations is found. Cref is a fundamental part of most of the Aethalometer corrections available in literature, and this is the first time a Cref value has been obtained for the Arctic.

Quantifying the aerosol/cloud-mediated radiative effect at a global scale requires simultaneous satellite retrievals of cloud condensation nuclei (CCN) concentrations and cloud base updraft velocities ( W b ). Hitherto, the inability to do so has been a major cause of high uncertainty regarding anthropogenic aerosol/cloud-mediated radiative forcing. This can be addressed by the emerging capability of estimating CCN and W b of boundary layer convective clouds from an operational polar orbiting weather satellite. Our methodology uses such clouds as an effective analog for CCN chambers. The cloud base supersaturation ( S ) is determined by W b and the satellite-retrieved cloud base drop concentrations ( N db ), which is the same as CCN ( S ). Validation against ground-based CCN instruments at Oklahoma, at Manaus, and onboard a ship in the northeast Pacific showed a retrieval accuracy of ±25% to ±30% for individual satellite overpasses. The methodology is presently limited to boundary layer not raining convective clouds of at least 1 km depth that are not obscured by upper layer clouds, including semitransparent cirrus. The limitation for small solar backscattering angles of

Background Despite increased recanalization rates in the treatment of acute ischemic stroke, the percentage of patients with a good clinical outcome of all those treated has not risen above 50%. This 50% barrier may be broken by improving the criteria for treatment selection. This study investigated the addition of the capillary index score (CIS), a new index for assessing remaining viable tissue in the ischemic area, to the existing criteria. Methods The Borgess Medical Center Ischemic Stroke Registry is a non-randomized single-center single-operator registry of consecutive subjects admitted for intra-arterial treatment of acute ischemic stroke. The CIS was calculated from a pre-intervention catheter cerebral angiogram in subjects with internal carotid artery (ICA) or middle cerebral artery (MCA) (M1) occlusion. Thrombolysis In Myocardial Infarction (TIMI) 2 or 3 was considered successful recanalization. A modified Rankin Scale (mRS) of 0–2 at 3 months was considered a good outcome. Results ICA or MCA (M1) occlusion was found in 46 of 58 consecutive patients treated by the same operator. Recanalization was successful in 72% of patients and 27% had a good outcome. CIS was available for 26 patients; 42% were favorable (2 or 3) and 58% were poor (0 or 1). A good outcome was found only in the favorable CIS group (p=0.0148). Successful recanalization (p=0.0029) and time from ictus to revascularization (p=0.0039) predicted a good outcome. Of patients with favorable CIS and TIMI 3, 83% had a good outcome. Conclusions Favorable CIS and recanalization were strong predictors of a good outcome. By using this new index as an adjunct to other criteria, the CIS may improve patient selection and help break the 50% barrier.

High altitude mountaintop observatories provide the opportunity to study aerosol properties in the free troposphere without the added expense and difficulty of making airborne measurements. Climatologies for free tropospheric aerosol radiative properties in cloud-free air, including light scattering, light absorption, light extinction, single scattering albedo, Angstrom exponent, hemispheric backscatter fraction and radiative forcing efficiency, from twelve high altitude (2.2–5.1 km) measurement platforms are presented at low relative humidity and at standard temperature and pressure. These climatologies utilize data from ten mountaintop observatories in the 20–50oN latitude band: Mauna Loa, USA; Lulin Mountain, Taiwan; Nepal Climate Observatory — Pyramid; Izana, Spain; Mount Waliguan, China; Beo Moussala, Bulgaria; Mount Bachelor, USA; Monte Cimone, Italy; Jungfraujoch, Switzerland; Whistler Mountain, Canada. Results are also included from two multi-year, in-situ aerosol vertical profiling programs: Southern Great Plains, USA and Bondville, USA. The amount of light absorption and scattering observed at these high altitude sites either peaks in the spring or it has a broad spring to summer enhancement. The seasonal variation of the aerosol single scattering albedo, backscatter fraction and Angstrom exponent changes from site to site but the timing can be related to aerosol sources and transport processes known to impact the individual sites. The seasonal variation of in-situ aerosol light extinction from these high altitude measurements is in excellent agreement with extinction values derived from CALIPSO lidar measurements. Analysis of the systematic variability among in-situ aerosol properties shows that these relationships can be used to infer aerosol types. In particular, the relationship between single scattering albedo and Angstrom exponent can indicate the presence of dust aerosol. Radiative forcing efficiency (RFE = aerosol forcing/aerosol optical depth) is used to assess the importance of single scattering albedo and backscatter fraction on aerosol forcing by eliminating aerosol amount (i.e., aerosol optical depth) from the calculation. Variability in monthly cycles of RFE corresponds with changes in single scattering albedo and hemispheric backscatter fraction. Utilizing site-specific, climatological values of single scattering albedo and backscatter fraction to calculate RFE results in departures from the monthly median values of RFE typically in the range 10–30%. The greatest discrepancy occurs for months with low aerosol loading where the observed variability of single scattering albedo and backscatter fraction is the greatest. At most sites the radiative forcing efficiency at low aerosol loading (light scattering −1 ) is slightly less negative (more warming) than at higher aerosol loading.

During April 2008, as part of the International Polar Year (IPY), a number of ground-based and aircraft campaigns were carried out in the North American Arctic region (e.g., ARCTAS, ARCPAC). The widespread presence during this period of biomass burning effluent, both gaseous and particulate, has been reported. Unusually high ozone readings for this time of year were recorded at surface ozone monitoring sites from northern Alaska to northern California. At Barrow, Alaska, the northernmost point in the United States, the highest April ozone readings recorded at the surface (hourly average values >55 ppbv) in 37 years of observation were measured on April 19, 2008. At Denali National Park in central Alaska, an hourly average of 79 ppbv was recorded during an 8-h period in which the average was over 75 ppbv, exceeding the ozone ambient air quality standard threshold value in the U.S. Elevated ozone (>60 ppbv) persisted almost continuously from April 19–23 at the monitoring site during this event. At a coastal site in northern California (Trinidad Head), hourly ozone readings were >50 ppbv almost continuously for a 35-h period from April 18–20. At several sites in northern California, located to the east of Trinidad Head, numerous occurrences of ozone readings exceeding 60 ppbv were recorded during April 2008. Ozone profiles from an extensive series of balloon soundings showed lower tropospheric features at ∼1–6 km with enhanced ozone during the times of elevated ozone amounts at surface sites in western Canada and the U.S. Based on extensive trajectory calculations, biomass burning in regions of southern Russia was identified as the likely source of the observed ozone enhancements. Ancillary measurements of atmospheric constituents and optical properties (aerosol optical thickness) supported the presence of a burning plume at several locations. At two coastal sites (Trinidad Head and Vancouver Island), profiles of a large suite of gases were measured from airborne flask samples taken during probable encounters with burning plumes. These profiles aided in characterizing the vertical thickness of the plumes, as well as confirming that the plumes reaching the west coast of North America were associated with biomass burning events.

This study presents an empirical method to estimate the CCN concentration as a function of percent supersaturation. The aerosol optical properties, backscatter fraction and single scatter albedo, function as proxies for the aerosol size and composition in a power law relationship to CCN. This method is tested at four sites with aged aerosol: SGP (Oklahoma, USA), FKB (Black Forest, Germany), HFE (Hefei, China) and GRW (Graciosa, Azores). Each site represents a different aerosol type and thus demonstrates the method robustness and limitations. Good agreement was found between the calculated and measured CCN with slopes between 0.81 and 1.03 and correlation coefficients (r2 values) between 0.59 and 0.67. The fit quality declined at low CCN concentrations.

In recent decades much attention has been given to the Arctic environment, where climate change is happening rapidly. Black carbon (BC) has been shown to be a major component of Arctic pollution that also affects the radiative balance. In the present study, we focused on how vegetation fires that occurred in Northern Eurasia during the period of 2002–2013 influenced the budget of BC in the Arctic. For simulating the transport of fire emissions from Northern Eurasia to the Arctic, we adopted BC fire emission estimates developed independently by GFED3 (Global Fire Emissions Database) and FEI-NE (Fire Emission Inventory – Northern Eurasia). Both datasets were based on fire locations and burned areas detected by MODIS (MODerate resolution Imaging Spectroradiometer) instruments on NASA's (National Aeronautics and Space Administration) Terra and Aqua satellites. Anthropogenic sources of BC were estimated using the MACCity (Monitoring Atmospheric Composition & Climate/megaCITY – Zoom for the ENvironment) emission inventory. During the 12-year period, an average area of 250,000 km2 yr−1 was burned in Northern Eurasia and the global emissions of BC ranged between 8.0 and 9.5 Tg yr−1. For the BC emitted in the Northern Hemisphere, about 70 % originated from anthropogenic sources and the rest from biomass burning (BB). Using the FEI-NE inventory, we found that 102 ± 29 kt yr−1 BC from biomass burning was deposited on the Arctic (defined here as the area north of 67º N) during the 12 years simulated, which was twice as much as when using MACCity inventory (56 ± 8 kt yr−1). The annual mass of BC deposited in the Arctic from all sources (FEI-NE in Northern Eurasia, MACCity elsewhere) is significantly higher by about 37 % in 2009 to 181 % in 2012, compared to the BC deposited using just the MACCity emission inventory. Deposition of BC in the Arctic from BB sources in the Northern Hemisphere thus represents 68 % of the BC deposited from all BC sources (the remaining being due to anthropogenic sources). Northern Eurasian vegetation fires (FEI-NE) contributed 85 % (79–91 %) to the BC deposited over the Arctic from all BB sources in the Northern Hemisphere. Arctic total BC burden showed strong seasonal variations, with highest values during the Arctic Haze season. High winter–spring values of BC burden were caused by transport of BC mainly from anthropogenic sources in Europe, whereas the peak in summer was mainly due to the fire emissions in Northern Eurasia. BC particles emitted from fires in lower latitudes (35° N–40° N) were found to remain the longest in the atmosphere due to the high release altitudes of smoke plumes, exhibit tropospheric transport resulting in a high summer peak of burden, and grow by condensation processes. In regards to the geographic contribution on the deposition of BC, we estimated that about 46 % of the BC deposited over the Arctic from vegetation fires in Northern Eurasia originated from Siberia, 6 % from Kazakhstan, 5 % from Europe, and about 1 % from Mongolia. The remaining 42 % originated from other areas in Northern Eurasia. For spring and summer, we computed that 42 % of the BC released from Northern Eurasian vegetation fires was deposited over the Arctic (annual average: 17 %). Vegetation fires in Northern Eurasia contributed to 14 % to 57 % of BC surface concentrations at the Arctic stations (Alert, Barrow, Zeppelin, Villum, and Tiksi), with fires in Siberia contributing the largest share. However, anthropogenic sources in the Northern Hemisphere remain essential, contributing 29 % to 54 % to the surface concentrations at the Arctic monitoring stations. The rest originated from North American fires.

The Clouds, Aerosol, and Precipitation in the Marine Boundary Layer (CAP-MBL) deployment at Graciosa Island in the Azores generated a 21-month (April 2009–December 2010) comprehensive dataset documenting clouds, aerosols, and precipitation using the Atmospheric Radiation Measurement Program (ARM) Mobile Facility (AMF). The scientific aim of the deployment is to gain improved understanding of the interactions of clouds, aerosols, and precipitation in the marine boundary layer.\ud \ud Graciosa Island straddles the boundary between the subtropics and midlatitudes in the northeast Atlantic Ocean and consequently experiences a great diversity of meteorological and cloudiness conditions. Low clouds are the dominant cloud type, with stratocumulus and cumulus occurring regularly. Approximately half of all clouds contained precipitation detectable as radar echoes below the cloud base. Radar and satellite observations show that clouds with tops from 1 to 11 km contribute more or less equally to surface-measured precipitation at Graciosa. A wide range of aerosol conditions was sampled during the deployment consistent with the diversity of sources as indicated by back-trajectory analysis. Preliminary findings suggest important two-way interactions between aerosols and clouds at Graciosa, with aerosols affecting light precipitation and cloud radiative properties while being controlled in part by precipitation scavenging.\ud \ud The data from Graciosa are being compared with short-range forecasts made with a variety of models. A pilot analysis with two climate and two weather forecast models shows that they reproduce the observed time-varying vertical structure of lower-tropospheric cloud fairly well but the cloud-nucleating aerosol concentrations less well. The Graciosa site has been chosen to be a permanent fixed ARM site that became operational in October 2013.

Shortwave direct aerosol radiative forcing (DARF) at the surface as well as aerosol optical depth (AOD) were estimated and chemically apportioned on the basis of ground-based aerosol and radiation measurements at the Gosan super-site in Korea during the Asian Pacific Regional Aerosol Characterization Experiment (ACE-Asia) in April 2001. An aerosol optical model and a radiative transfer model (RTM) were employed to calculate the aerosol extinction coefficient and radiative flux at the surface, respectively. The calculated scattering and absorption coefficients for Dp

The entrainment process of water vapor into the dust layer during Asian dust events and the effect of water vapor associated with the Asian dust layer (ADL) on aerosol hygroscopic properties are investigated. The entrainment processes of water vapor into the ADL is examined by using a PSU/NCAR MM5 together with the backward trajectory model, radiosonde data, and remotely sensed aerosol vertical distribution data. Two dust events in the spring of 1998 and 2001 are examined in detail. The results reveal that the water vapor mixing ratio (WVMR) derived by the MM5 fits in well with the WVMR observed by radiosonde, and is well coincident with the aerosol extinction coefficient (σep) measured by the micro-pulse lidar. The temporal evolution of the vertical distributions of WVMR and σep exhibited similar features. On the basis of a well simulation of the enhanced water vapor within the dust layer by the MM5, we trace the dust storms to examine the entrainment mechanism. The enhancement of WVMR within the ADL was initiated over the mountainous areas. The relatively moist air mass in the well-developed mixing layer over the mountainous areas is advected upward from the boundary layer by an ascending motion. However, a large portion of the water vapor within the ADL is enhanced over the edge of a highland and the plains in China. This is well supported by the simulated WVMR and the wind vectors. Aircraft-based in situ measurements of the chemical and optical properties of aerosol enable a quantitative estimation of the effect of the enhanced WVMR on the aerosol hygroscopic properties. The submicron aerosol accompanied by the dust storm caused an increase of aerosol scattering through water uptakes during the transport. This increase could be explained by the chemical fact that water-soluble submicron pollution aerosols are enriched in the ADL.

Measurements of the aerosol hygroscopic growth factor, f (RH), and the physical and optical properties of aerosols were made at Gosan, Korea during the aerosol characterization experiment (ACE)-Asia 2001 field campaign (April 2001). The optical and hygroscopic properties of aerosols were characterized in terms of the air mass transport pathways. During the Asian dust period, σ sp and σ ap were remarkably elevated with mean and standard deviation of 238.6±55.3 Mm −1 and 24.2±10.9 Mm −1 , respectively. The mean f (RH) for the pollution aerosols from Chinese sectors (2.75±0.38) in this study was much higher than that for the anthropogenic aerosols in Europe during ACE-2 (1.46±0.10) as well as that of the urban/industrial aerosols of the US east coast during TARFOX (1.81±0.37–2.30±0.24). The mean f (RH) during the smoke period (1.60±0.20) was comparable to that during INDOEX (1.58±0.21), and higher than that for SCAR-B in Brazil (1.16). We found a negative correlation ( r = 0.81 ) between f (RH) and OC concentration. This negative correlation suggests that organic aerosols have a strong influence on the smoke aerosol hygroscopicity.

This paper presents results of air mass characterization and the associated microphysical and optical properties of Asian aerosols, using the cluster analysis technique for classifying air mass back-trajectories arrived at Gosan on the Jeju Island, Korea during the ACE-Asia campaign. Five distinct clusters of trajectories were taken to explain each transport regime. The temporal variation of the transported air masses could be well explained by the consecutive and stepwise change of air masses between statistically classified clusters. The cluster-mean trajectory exhibited its close relationship with the synoptic-scale circulation pattern. In addition, it was shown that the composite of mean sea-level pressure field is useful for explaining favorable meteorological conditions for long-range transport of dust and anthropogenic pollution in East Asia. The highest light scattering and absorption coefficients for sub-10- and submicron aerosols as well as highest concentrations of 222Rn and condensation nuclei are associated with the air mass types accompanying dusts and pollutants. The cluster-mean single scattering albedo (SSA) for sub-10- and submicron aerosols ranged 0.88–0.90 and 0.81–0.86, respectively. This value of SSA indicates the large contribution of submicron aerosol for the light absorption in East Asia. The concentration of 222Rn and aerosol microphysical and optical properties for marine air mass suggests that the marine air masses are somewhat influenced by continental outflows. The minor differences in aerosol microphysical and optical properties among continental clusters with similar routes and different transport speed implies that the effect of transport speed may not be significant if the transport routes are similar.

In order to understand the influence of dust and anthropogenic pollution aerosols on regional climate in East Asia, we analyzed the aerosol optical, chemical and physical properties for two cases with high aerosol loading and assessed the radiative forcing of these cases. The 1st case study is a heavy dust episode (DE) in April (during ACE-Asia) 2001 and the 2nd case is a regional-scale pollution event in November 2001. The Angstrom exponent (A) for DE was 0.38 from sunphotometer measurements. The mean single scattering albedo (550 nm) at the surface reported during the pollution episode (PE, 0.88) was lower than that of DE (0.91). The concentrations of organic (OC) and elemental carbon (EC) measured during the PE were about 90% and 30% higher than DE. The aerosol mass scattering efficiency (αs) of PE is a factor of about 2 higher than that of the DE. The difference in the mass absorption efficiency (αa) of EC during DE and PE is small and within the measurement uncertainty. The diurnally averaged aerosol radiative forcing efficiency (ΔDFE, W m−2 τ−1) during DE is similar to results of other studies at Gosan.

The Continuous Light Absorption Photometer (CLAP) measures the aerosol absorption of radiation at three visible wavelengths; 461, 522, and 653 nanometers (nm). Data from this measurement is used in radiative forcing calculations, atmospheric heating rates, and as a prediction of the amount of equivalent black carbon in atmospheric aerosol and in models of aerosol semi-direct forcing. Aerosol absorption measurements are essential to modeling the energy balance of the atmosphere.

A steady state analysis of H2SO4 sources and sinks in the Antarctic marine boundary layer was performed using measurements from project SCATE, Sulfur Chemistry in the Antarctic Troposphere Experiment. The calculations show that the SO2 levels needed to account for the observed gas phase H2SO4 ranged from about 17 to 300 parts per trillion by volume (pptv) with an average SO2 concentration of 100 pptv, far more than previous measurements of SO2 in this region which range between 7 and 17 pptv [Berresheim, 1987; Pszenny et al., 1989; P. Quinn, personal communication, 1996]. Boundary layer oxidation of DMS via an SO2 intermediate was found to be an insufficient source of H2SO4 in this region. Likely alternative sources of H2SO4 include oxidation of boundary layer DMDS and vertical entrainment of air from higher altitudes.

Studies of dimethylsulfide (DMS) oxidation chemistry were conducted at Palmer Station on Anvers Island, Antarctica, during the austral summer of 1993/1994. Part of the study involved gas phase measurements of OH, methane sulfonic acid (MSA), and H2SO4 using a chemical ionization mass spectrometer, as well as measurements of the NO, CO, and 03 concentrations. Mean 24 hour concentrations from February 16-23 of OH, MSA, and H2SO4 were 1.1 x 105, 9.5 x 105, and 1.61 x 106 molecules cm -3, respectively. Model calculations of OH compared well with observed levels (e.g., within 30%). The modeling results suggest that the dominant source of OH is from the reaction of O(1D) with H20, where O(1D) is the product of 03 photolysis. Because of the clean atmospheric environment and predicted low nonmethyl hydrocarbon levels in Antarctica, the dominant OH sink was found to be reaction with CO and CH4. Particulate levels of MSA were higher than could be attributed to condensation of boundary layer (BL) gas phase MSA on to the aerosol surface. Alternate mechanisms for generating MSA in the particle phase were speculated to involve either in-cloud oxidation of dimethylsulfoxide or OH oxidation of DMS in the atmospheric buffer layer above the boundary layer followed by condensation of gas phase MSA on aerosols and transport back to the B L (Davis et al., this issue).

In January and February 1994, measurements of dimethylsulfide (DMS) in air and seawater were conducted at Palmer Station, Antarctica, during project SCATE (Sulfur Chemistry in the Antarctic Troposphere Experiment). Corresponding values ranged between 6 and 595 pptv (median: 94 pptv) and 0.7 and 3.7 nM (median: 2 nM), respectively. Atmospheric DMS levels were significantly enhanced during a storm episode in connection with large-scale low-pressure systems passing through the study area. DMS sea-to-air fluxes ranged between 0.03 and 19 (median: 1.1) μmol m−2 d−1 based on seawater DMS and wind speed measurements. The atmospheric DMS lifetime is estimated to be 9 days based on a 24-hour averaged OH concentration of 1.1 × 105 cm−3. Atmospheric dimethylsulfoxide (DMSO) and dimethylsulfone (DMSO2) mixing ratios varied mostly between