Chemical composition of tropospheric air masses encountered during high altitude flights (>11.5 km) during the 2009 fall Operation Ice Bridge field campaign

Mountain and high-altitude sites provide representative data for the lower free troposphere and various pathways for aerosol interactions, changing boundary layer heights useful in understanding atmospheric composition. However, few studies exist in African regions despite its diversity in both natural and anthropogenic emissions. For this reason, the ATLAS Mohamed V (AM5) observatory in the Middle Atlas region was established to provide the necessary infrastructure for detailed atmospheric studies in the North African high-altitude region. Here, results of a field study conducted to determine the aerosol chemical composition in this region, understand its variations, and importance in assessing global and regional changes in the atmospheric composition is reported. Particulate matter (PM10) filter samples (200) were collected using a high-volume (500l/min) collector in a 12h sampling interval from August to December 2017. The chemical composition of the samples was analyzed for trace metals, ions, elemental carbon, organic carbon, aliphatic hydrocarbons, and polycyclic aromatic hydrocarbon (PAHs) content. The results show that the high-altitude aerosol composition is influenced by regional and transregional transport of different pollutants. Local sources play an important role during periods when the wind speed is low, especially during autumn. Despite the proximity of the site to the Saharan Desert, its influence on the atmospheric composition was mainly seasonal and accounted for only 14% of the sampling duration. The chemical composition was dominated by inorganic elements, mainly suspended dust (47%) and ionic species (16%), and followed by organic matter (15%), water content (12%), and indeterminate mass (9%). Biogenic organics contributed up to 7% of the organic matter with high contributions from compounds such as Nonacosane, Heptacosane, and 2-Pentadecanone. Four main air masses characterized the inflow to the site, which often leads to different aerosol chemical compositions. Mineral dust influenced was seasonal and ranged between 20 and 70% of the PM mass with peaks observed during the summer and was accompanied by high concentrations of SO42- of up to 1.3 &#181;g/m&#179;. PM10 concentrations during winter were low (< 30 &#181;g/m&#179;), with a dominance of marine air masses (53%) carrying aerosols rich in sea salt and polluted anthropogenic aerosols from the coastal regions (Rabat and Casablanca). During the day-time, mineral dust contribution to PM increased by about 42% due to road dust resuspension. In contrast, during night-time, an increase in the concentrations of PAHs, ketones, and anthropogenic metals such as Pb, Ni, and Cu was found due to variations in the boundary layer height. The results provide first insights into typical North African high-altitude background aerosol chemical composition useful for long-term assessment of climate and regional influence of air pollution in North Africa.&#160;

Download Full-text

Aerosol characterization in an oceanic context around Reunion island (AEROMARINE field campaign)

10.5194/egusphere-egu21-2729 ◽

2021 ◽

Author(s):

Faustine Mascaut ◽

Olivier Pujol ◽

Jérôme Brioude ◽

Bert Verreyken ◽

Raphaël Peroni ◽

...

Keyword(s):

Indian Ocean ◽

High Altitude ◽

Atmospheric Environment ◽

Reunion Island ◽

Free Troposphere ◽

Marine Aerosols ◽

Field Campaign ◽

Air Masses ◽

Major Interest ◽

Réunion Island

We present the results of the AEROMARINE field campaign which took place in the boreal spring 2019 off the coast of Reunion island in the South West Indian Ocean basin. The southern Indian Ocean is of major interest for the study of marine aerosols, their distribution and variability [1]. Nine instrumented light plane flights and a ground-based microwave radiometer were used during the AEROMARINE field campaign. These measurements were compared with the long-term measurements of the AERONET sun-photometer (based in Saint Denis, Reunion Island) and various instruments of the high altitude Maido Observatory (2200m above sea level, Reunion island). These results were analyzed using different model outputs: (i) the AROME mesoscale weather forecast model to work on the thermodynamics of the boundary layer, (ii) the FLEXPART-AROME Lagrangian particle dispersion model to assess the geographical and vertical origin of air masses, and (iii) the chemical transport model CAMS (Copernicus Atmosphere Monitoring Service) to work on the aerosol chemical composition of air masses. These measurements allowed us to determine the background concentration of natural marine aerosols and to highlight that (1) the atmospheric layers above 1500m are in the free troposphere and are mainly composed of aerosols from the regional background and (2) that the local environment (ocean or island) has little impact on the measured concentrations. Marine aerosols emitted locally are mostly measured in the lower atmospheric layers (below 500m). The daytime marine aerosol distributions in the free troposphere measured by the aircraft were compared to the aerosol distribution measured at the high altitude Maido observatory at night when the observatory is located in the free troposphere.&#160; We also found that the CAMS reanalyses overestimated the aerosol optical depth in this region. Finally, our study confirms, with no ambiguity, that the AERONET station in Saint Denis (Reunion island) can be considered as a representative marine station in the tropics [2].&#160; References [1]&#160; I.&#160; Koren,&#160; G.&#160; Dagan,&#160; and&#160; O.&#160; Altaratz. &#160; From&#160; aerosol-limited&#160; to&#160; invigoration&#160; of&#160; warm&#160; convective clouds. Science, 344 (6188) : 1143&#8211;1146, 2014. [2]&#160; P. Hamill, M. Giordano, C. Ward, D. Giles, and B. Holben.&#160; An aeronet-based aerosol classification using the mahalanobis distance. Atmospheric Environment, 140 : 213&#8211;233,2016.

Download Full-text

Processing of biomass burning aerosol in the Eastern Mediterranean during summertime

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-13-25969-2013 ◽

2013 ◽

Vol 13 (10) ◽

pp. 25969-25999 ◽

Cited By ~ 2

Author(s):

A. Bougiatioti ◽

I. Stavroulas ◽

E. Kostenidou ◽

P. Zarmpas ◽

C. Theodosi ◽

...

Keyword(s):

Chemical Composition ◽

Biomass Burning ◽

Eastern Mediterranean ◽

Late Summer ◽

Organic Aerosol ◽

High Temporal Resolution ◽

Night Time ◽

Air Masses ◽

Aerosol Mass ◽

Atmospheric Processing

Abstract. The aerosol chemical composition in air masses affected by wildfires from the Greek islands of Chios, Euboea and Andros, the Dalmatian Coast and Sicily, during late summer of 2012 was characterized at the remote background site of Finokalia, Crete. Air masses were transported several hundreds of kilometers, arriving at the measurement station after approximately half a day of transport, mostly during night-time. The chemical composition of the particulate matter was studied by different high temporal resolution instruments, including an Aerosol Chemical Speciation Monitor (ACSM) and a seven-wavelength aethalometer. Despite the large distance from emission and long atmospheric processing, a clear biomass burning organic aerosol (BBOA) profile containing characteristic markers is derived from BC measurements and Positive Matrix Factorization (PMF) analysis of the ACSM mass spectra. The ratio of fresh to aged BBOA decreases with increasing atmospheric processing time and BBOA components appear to be converted to oxygenated organic aerosol (OOA). Given that the smoke was mainly transported overnight, it appears that the processing can take place in the dark. These results show that a significant fraction of the BBOA loses its characteristic AMS signature and is transformed to OOA in less than a day. This implies that biomass burning can contribute almost half of the organic aerosol mass in the area during summertime.

Download Full-text

Impact of different Asian source regions on the composition of the Asian monsoon anticyclone and of the extratropical lowermost stratosphere

Atmospheric Chemistry and Physics ◽

10.5194/acp-15-13699-2015 ◽

2015 ◽

Vol 15 (23) ◽

pp. 13699-13716 ◽

Cited By ~ 41

Author(s):

B. Vogel ◽

G. Günther ◽

R. Müller ◽

J.-U. Grooß ◽

M. Riese

Keyword(s):

Chemical Composition ◽

Southeast Asia ◽

Asian Monsoon ◽

Monsoon Season ◽

Intraseasonal Variability ◽

Air Masses ◽

Northern India ◽

Source Regions ◽

The Tropics ◽

Emission Tracers

Abstract. The impact of different boundary layer source regions in Asia on the chemical composition of the Asian monsoon anticyclone, considering its intraseasonal variability in 2012, is analysed by simulations of the Chemical Lagrangian Model of the Stratosphere (CLaMS) using artificial emission tracers. The horizontal distribution of simulated CO, O3, and artificial emission tracers for India/China are in good agreement with patterns found in satellite measurements of O3 and CO by the Aura Microwave Limb Sounder (MLS). Using in addition, correlations of artificial emission tracers with potential vorticity demonstrates that the emission tracer for India/China is a very good proxy for spatial distribution of trace gases within the Asian monsoon anticyclone. The Asian monsoon anticyclone constitutes a horizontal transport barrier for emission tracers and is highly variable in location and shape. From the end of June to early August, a northward movement of the anticyclone and, during September, a strong broadening of the spatial distribution of the emission tracer for India/China towards the tropics are found. In addition to the change of the location of the anticyclone, the contribution of different boundary source regions to the composition of the Asian monsoon anticyclone in the upper troposphere strongly depends on its intraseasonal variability and is therefore more complex than hitherto believed. The largest contributions to the composition of the air mass in the anticyclone are found from northern India and Southeast Asia at a potential temperature of 380 K. In the early (mid-June to mid-July) and late (September) period of the 2012 monsoon season, contributions of emissions from Southeast Asia are highest; in the intervening period (early August), emissions from northern India have the largest impact. Our findings show that the temporal variation of the contribution of different convective regions is imprinted in the chemical composition of the Asian monsoon anticyclone. Air masses originating in Southeast Asia are found both within and outside of the Asian monsoon anticyclone because these air masses experience, in addition to transport within the anticyclone, upward transport at the southeastern flank of the anticyclone and in the tropics. Subsequently, isentropic poleward transport of these air masses occurs at around 380 K with the result that the extratropical lowermost stratosphere in the Northern Hemisphere is flooded by the end of September with air masses originating in Southeast Asia. Even after the breakup of the anticyclonic circulation (around the end of September), significant contributions of air masses originating in India/China are still found in the upper troposphere over Asia. Our results demonstrate that emissions from India, China, and Southeast Asia have a significant impact on the chemical composition of the lowermost stratosphere of the Northern Hemisphere, in particular at the end of the monsoon season in September/October 2012.

Download Full-text

Trace gases and organic aerosol at a rural site in Vietnam during large scale biomass burning

10.5194/egusphere-egu21-181 ◽

2021 ◽

Author(s):

Simone M. Pieber ◽

Dac-Loc Nguyen ◽

Hendryk Czech ◽

Stephan Henne ◽

Nicolas Bukowiecki ◽

...

Keyword(s):

Air Quality ◽

Chemical Composition ◽

Biomass Burning ◽

Large Scale ◽

Trace Gases ◽

Organic Aerosol ◽

Trace Gas ◽

Rural Site ◽

Air Masses ◽

Mixing Ratios

Open biomass burning (BB) is a globally widespread phenomenon. The fires release pollutants, which are harmful for human and ecosystem health and alter the Earth's radiative balance. Yet, the impact of various types of BB on the global radiative forcing remains poorly constrained concerning greenhouse gas emissions, BB organic aerosol (OA) chemical composition and related light absorbing properties. Fire emissions composition is influenced by multiple factors (e.g., fuel and thereby vegetation-type, fuel moisture, fire temperature, available oxygen). Due to regional variations in these parameters, studies in different world regions are needed. Here we investigate the influence of seasonally recurring BB on trace gas concentration and air quality at the regional Global Atmosphere Watch (GAW) station Pha Din (PDI) in rural Northwestern Vietnam. PDI is located in a sparsely populated area on the top of a hill (1466 m a.s.l.) and is well suited to study the large-scale fires on the Indochinese Peninsula, whose pollution plumes are frequently transported towards the site [1]. We present continuous trace gas observations of CO2, CH4, CO, and O3 conducted at PDI since 2014 and interpret the data with atmospheric transport simulations. Annually recurrent large scale BB leads to hourly time-scale peaks CO mixing ratios at PDI of 1000 to 1500 ppb around every April since the start of data collection in 2014. We complement this analysis with carbonaceous PM2.5 chemical composition analyzed during an intensive campaign in March-April 2015. This includes measurements of elemental and organic carbon (EC/OC) and more than 50 organic markers, such as sugars, PAHs, fatty acids and nitro-aromatics [2]. For the intensive campaign, we linked CO, CO2, CH4 and O3 mixing ratios to a statistical classification of BB events, which is based on OA composition. We found increased CO and O3 levels during medium and high BB influence during the intensive campaign. A backward trajectory analysis confirmed different source regions for the identified periods based on the OA cluster. Typically, cleaner air masses arrived from northeast, i.e., mainland China and Yellow sea during the intensive campaign. The more polluted periods were characterized by trajectories from southwest, with more continental recirculation of the medium cluster, and more westerly advection for the high cluster. These findings highlight that BB activities in Northern Southeast Asia significantly enhances the regional OA loading, chemical PM2.5 composition and the trace gases in northwestern Vietnam. The presented analysis adds valuable data on air quality in a region of scarce data availability.&#160;REFERENCES[1] Bukowiecki, N. et al. Effect of Large-scale Biomass Burning on Aerosol Optical Properties at the GAW Regional Station Pha Din, Vietnam. AAQR. 19, 1172&#8211;1187 (2019).[2] Nguyen, D. L, et al. Carbonaceous aerosol composition in air masses influenced by large-scale biomass burning: a case-study in Northwestern Vietnam. ACPD., https://doi.org/10.5194/acp-2020-1027, in review, 2020.

Download Full-text

Hygroscopic properties and cloud condensation nuclei activity of atmospheric aerosols under the influences of Asian continental outflow and new particle formation at a coastal site in eastern Asia

Atmospheric Chemistry and Physics ◽

10.5194/acp-20-5911-2020 ◽

2020 ◽

Vol 20 (10) ◽

pp. 5911-5922 ◽

Cited By ~ 4

Author(s):

Hing Cho Cheung ◽

Charles Chung-Kuang Chou ◽

Celine Siu Lan Lee ◽

Wei-Chen Kuo ◽

Shuenn-Chin Chang

Keyword(s):

Chemical Composition ◽

Cloud Condensation Nuclei ◽

Particle Formation ◽

Number Concentration ◽

Pollution Sources ◽

New Particle Formation ◽

Condensation Nuclei ◽

Air Masses ◽

Hygroscopic Properties ◽

Aerosol Hygroscopicity

Abstract. The chemical composition of fine particulate matter (PM2.5), the size distribution and number concentration of aerosol particles (NCN), and the number concentration of cloud condensation nuclei (NCCN) were measured at the northern tip of Taiwan during an intensive observation experiment from April 2017 to March 2018. The parameters of aerosol hygroscopicity (i.e., activation ratio, activation diameter and kappa of CCN) were retrieved from the measurements. Significant variations were found in the hygroscopicity of aerosols (kappa – κ – of 0.18–0.56, for water vapor supersaturation – SS – of 0.12 %–0.80 %), which were subject to various pollution sources, including aged air pollutants originating in eastern and northern China and transported by the Asian continental outflows and fresh particles emitted from local sources and distributed by land–sea breeze circulations as well as produced by processes of new particle formation (NPF). Cluster analysis was applied to the back trajectories of air masses to investigate their respective source regions. The results showed that aerosols associated with Asian continental outflows were characterized by lower NCN and NCCN values and by higher kappa values of CCN, whereas higher NCN and NCCN values with lower kappa values of CCN were observed in the aerosols associated with local air masses. Besides, it was revealed that the kappa value of CCN exhibited a decrease during the early stage of an event of new particle formation, which turned to an increasing trend over the later period. The distinct features in the hygroscopicity of aerosols were found to be consistent with the characteristics in the chemical composition of PM2.5. This study has depicted a clear seasonal characteristic of hygroscopicity and CCN activity under the influence of a complex mixture of pollutants from different regional and/or local pollution sources. Nevertheless, the mixing state and chemical composition of the aerosols critically influence the aerosol hygroscopicity, and further investigations are necessary to elucidate the atmospheric processing involved in the CCN activation in coastal areas.

Download Full-text

Aerosol hygroscopicity and its link to chemical composition in the coastal atmosphere of Mace Head: marine and continental air masses

Atmospheric Chemistry and Physics ◽

10.5194/acp-20-3777-2020 ◽

2020 ◽

Vol 20 (6) ◽

pp. 3777-3791 ◽

Cited By ~ 1

Author(s):

Wei Xu ◽

Jurgita Ovadnevaite ◽

Kirsten N. Fossum ◽

Chunshui Lin ◽

Ru-Jin Huang ◽

...

Keyword(s):

Chemical Composition ◽

Growth Factor ◽

Time Resolution ◽

Sea Salt ◽

High Time ◽

High Time Resolution ◽

Marine Aerosol ◽

Diurnal Pattern ◽

Air Masses ◽

Aerosol Hygroscopicity

Abstract. Chemical composition and hygroscopicity closure of marine aerosol in high time resolution has not been achieved yet due to the difficulty involved in measuring the refractory sea-salt concentration in near-real time. In this study, attempts were made to achieve closure for marine aerosol based on a humidified tandem differential mobility analyser (HTDMA) and a high-resolution time-of-flight aerosol mass spectrometer (AMS) for wintertime aerosol at Mace Head, Ireland. The aerosol hygroscopicity was examined as a growth factor (GF) at 90 % relative humidity (RH). The corresponding GFs of 35, 50, 75, 110 and 165 nm particles were 1.54±0.26, 1.60±0.29, 1.66±0.31, 1.72±0.29 and 1.78±0.30 (mean ± standard deviation), respectively. Two contrasting air masses (continental and marine) were selected to study the temporal variation in hygroscopicity; the results demonstrated a clear diurnal pattern in continental air masses, whereas no diurnal pattern was found in marine air masses. In addition, wintertime aerosol was observed to be largely externally mixed in both of the contrasting air masses. Concurrent high time resolution PM1 (particulate matter <1 µm) chemical composition data from combined AMS and MAAP measurements, comprising organic matter, non-sea-salt sulfate, nitrate, ammonium, sea salt and black carbon (BC), were used to predict aerosol hygroscopicity with the Zdanovskii–Stokes–Robinson (ZSR) mixing rule. Overall, good agreement (an R2 value of 0.824 and a slope of 1.02) was found between the growth factor of 165 nm particles measured by the HTDMA (GF_HTDMA) and the growth factor derived from the AMS + MAAP bulk chemical composition (GF_AMS). Over 95 % of the estimated GF values exhibited less than a 10 % deviation for the whole dataset, and this deviation was mostly attributed to the neglected mixing state as a result of the bulk PM1 composition.

Download Full-text

Comparison between simulated and observed chemical composition of fine aerosols in Paris (France) during springtime: contribution of regional versus continental emissions

Atmospheric Chemistry and Physics ◽

10.5194/acp-10-11987-2010 ◽

2010 ◽

Vol 10 (24) ◽

pp. 11987-12004 ◽

Cited By ~ 70

Author(s):

J. Sciare ◽

O. d'Argouges ◽

Q. J. Zhang ◽

R. Sarda-Estève ◽

C. Gaimoz ◽

...

Keyword(s):

Chemical Composition ◽

Secondary Organic Aerosols ◽

Transport Model ◽

Organic Aerosols ◽

Carbonaceous Material ◽

Chemical Components ◽

Carbonaceous Aerosols ◽

Time Resolved ◽

Air Masses ◽

North Western

Abstract. Hourly concentrations of inorganic salts (ions) and carbonaceous material in fine aerosols (aerodynamic diameter, A.D. <2.5 μm) have been determined experimentally from fast measurements performed for a 3-week period in spring 2007 in Paris (France). The sum of these two chemical components (ions and carbonaceous aerosols) has shown to account for most of the fine aerosol mass (PM2.5). This time-resolved dataset allowed investigating the factors controlling the levels of PM2.5 in Paris and showed that polluted periods with PM2.5 > 15 μg m−3 were characterized by air masses of continental (North-Western Europe) origin and chemical composition made by 75% of ions. By contrast, periods with clean marine air masses have shown the lowest PM2.5 concentrations (typically of about 10 μg m−3); carbonaceous aerosols contributing for most of this mass (typically 75%). In order to better discriminate between local and continental contributions to the observed chemical composition and concentrations of PM2.5 over Paris, a comparative study was performed between this time-resolved dataset and the outputs of a chemistry transport model (CHIMERE), showing a relatively good capability of the model to reproduce the time-limited intense maxima observed in the field for PM2.5 and ion species. Different model scenarios were then investigated switching off local and European (North-Western and Central) emissions. Results of these scenarios have clearly shown that most of the ions observed over Paris during polluted periods, were either transported or formed in-situ from gas precursors transported from Northern Europe. On the opposite, long-range transport from Europe appeared to weakly contribute to the levels of carbonaceous aerosols observed over Paris. The model failed to properly account for the concentration levels and variability of secondary organic aerosols (SOA) determined experimentally by the EC-tracer method. The abundance of SOA (relatively to organic aerosol, OA) was as much as 75%, showing a weak dependence on air masses origin. Elevated SOA/OA ratios were also observed for air masses having residence time above ground of less than 10 h, suggesting intense emissions and/or photochemical processes leading to rapid formation of secondary organic aerosols.

Download Full-text

Classification of clouds sampled at the puy de Dôme (France) based on 10 yr of monitoring of their physicochemical properties

Atmospheric Chemistry and Physics ◽

10.5194/acp-14-1485-2014 ◽

2014 ◽

Vol 14 (3) ◽

pp. 1485-1506 ◽

Cited By ~ 58

Author(s):

L. Deguillaume ◽

T. Charbouillot ◽

M. Joly ◽

M. Vaïtilingom ◽

M. Parazols ◽

...

Keyword(s):

Statistical Analysis ◽

Chemical Composition ◽

Inorganic Compounds ◽

Average Concentration ◽

Anthropogenic Sources ◽

Back Trajectory ◽

Data Set ◽

Air Masses ◽

High Concentrations ◽

Inorganic Constituents

Abstract. Long-term monitoring of the chemical composition of clouds (73 cloud events representing 199 individual samples) sampled at the puy de Dôme (pdD) station (France) was performed between 2001 and 2011. Physicochemical parameters, as well as the concentrations of the major organic and inorganic constituents, were measured and analyzed by multicomponent statistical analysis. Along with the corresponding back-trajectory plots, this allowed for distinguishing four different categories of air masses reaching the summit of the pdD: polluted, continental, marine and highly marine. The statistical analysis led to the determination of criteria (concentrations of inorganic compounds, pH) that differentiate each category of air masses. Highly marine clouds exhibited high concentrations of Na+ and Cl−; the marine category presented lower concentration of ions but more elevated pH. Finally, the two remaining clusters were classified as "continental" and "polluted"; these clusters had the second-highest and highest levels of NH4+, NO3−, and SO24−, respectively. This unique data set of cloud chemical composition is then discussed as a function of this classification. Total organic carbon (TOC) is significantly higher in polluted air masses than in the other categories, which suggests additional anthropogenic sources. Concentrations of carboxylic acids and carbonyls represent around 10% of the organic matter in all categories of air masses and are studied for their relative importance. Iron concentrations are significantly higher for polluted air masses and iron is mainly present in its oxidation state (+II) in all categories of air masses. Finally, H2O2 concentrations are much more varied in marine and highly marine clouds than in polluted clouds, which are characterized by the lowest average concentration of H2O2. This data set provides concentration ranges of main inorganic and organic compounds for modeling purposes on multiphase cloud chemistry.

Download Full-text

Analysis of CCN activity of Arctic aerosol and Canadian biomass burning during summer 2008

Atmospheric Chemistry and Physics ◽

10.5194/acp-13-2735-2013 ◽

2013 ◽

Vol 13 (5) ◽

pp. 2735-2756 ◽

Cited By ~ 92

Author(s):

T. L. Lathem ◽

A. J. Beyersdorf ◽

K. L. Thornhill ◽

E. L. Winstead ◽

M. J. Cubison ◽

...

Keyword(s):

Chemical Composition ◽

Biomass Burning ◽

Industrial Pollution ◽

Physical Aging ◽

Volume Fraction ◽

Cloud Condensation Nuclei ◽

Water Soluble ◽

The Arctic ◽

High Concentration ◽

Air Masses

Abstract. The NASA DC-8 aircraft characterized the aerosol properties, chemical composition, and cloud condensation nuclei (CCN) concentrations of the summertime Arctic during the 2008 NASA Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaign. Air masses characteristic of fresh and aged biomass burning, boreal forest, Arctic background, and anthropogenic industrial pollution were sampled. Observations were spatially extensive (50–85° N and 40–130° W) and exhibit significant variability in aerosol and CCN concentrations. The chemical composition was dominated by highly oxidized organics (66–94% by volume), with a water-soluble mass fraction of more than 50%. The aerosol hygroscopicity parameter, κ, ranged between κ = 0.08–0.32 for all air mass types. Industrial pollution had the lowest κ of 0.08 ± 0.01, while the Arctic background had the highest and most variable κ of 0.32 ± 0.21, resulting from a lower and more variable organic fraction. Both fresh and aged (long-range transported) biomass burning air masses exhibited remarkably similar κ (0.18 ± 0.13), consistent with observed rapid chemical and physical aging of smoke emissions in the atmosphere, even in the vicinity of fresh fires. The organic hygroscopicity (κorg) was parameterized by the volume fraction of water-soluble organic matter (εWSOM), with a κ = 0.12, such that κorg = 0.12εWSOM. Assuming bulk (size-independent) composition and including the κorg parameterization enabled CCN predictions to within 30% accuracy for nearly all environments sampled. The only exception was for industrial pollution from Canadian oil sands exploration, where an external mixture and size-dependent composition was required. Aerosol mixing state assumptions (internal vs. external) in all other environments did not significantly affect CCN predictions; however, the external mixing assumption provided the best results, even though the available observations could not determine the true degree of external mixing and therefore may not always be representative of the environments sampled. No correlation was observed between κorg and O : C. A novel correction of the CCN instrument supersaturation for water vapor depletion, resulting from high concentrations of CCN, was also employed. This correction was especially important for fresh biomass burning plumes where concentrations exceeded 1.5×104 cm−3 and introduced supersaturation depletions of &geq;25%. Not accounting for supersaturation depletion in these high concentration environments would therefore bias CCN closure up to 25% and inferred κ by up to 50%.

Download Full-text