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All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Southern Ocean latitudinal gradients of cloud condensation nuclei

Abstract. The Southern Ocean region is one of the most pristine in the world and serves as an important proxy for the pre-industrial atmosphere. Improving our understanding of the natural processes in this region is likely to result in the largest reductions in the uncertainty of climate and earth system models. While remoteness from anthropogenic and continental sources is responsible for its clean atmosphere, this also results in the dearth of atmospheric observations in the region. Here we present a statistical summary of the latitudinal gradient of aerosol (condensation nuclei larger than 10 nm, CN10) and cloud condensation nuclei (CCN at various supersaturations) concentrations obtained from five voyages spanning the Southern Ocean between Australia and Antarctica from late spring to early autumn (October to March) of the 2017/18 austral seasons. Three main regions of influence were identified: the northern sector (40–45∘ S), where continental and anthropogenic sources coexisted with background marine aerosol populations; the mid-latitude sector (45–65∘ S), where the aerosol populations reflected a mixture of biogenic and sea-salt aerosol; and the southern sector (65–70∘ S), south of the atmospheric polar front, where sea-salt aerosol concentrations were greatly reduced and aerosol populations were primarily biologically derived sulfur species with a significant history in the Antarctic free troposphere. The northern sector showed the highest number concentrations with median (25th to 75th percentiles) CN10 and CCN0.5 concentrations of 681 (388–839) cm−3 and 322 (105–443) cm−3, respectively. Concentrations in the mid-latitudes were typically around 350 cm−3 and 160 cm−3 for CN10 and CCN0.5, respectively. In the southern sector, concentrations rose markedly, reaching 447 (298–446) cm−3 and 232 (186–271) cm−3 for CN10 and CCN0.5, respectively. The aerosol composition in this sector was marked by a distinct drop in sea salt and increase in both sulfate fraction and absolute concentrations, resulting in a substantially higher CCN0.5/CN10 activation ratio of 0.8 compared to around 0.4 for mid-latitudes. Long-term measurements at land-based research stations surrounding the Southern Ocean were found to be good representations at their respective latitudes; however this study highlighted the need for more long-term measurements in the region. CCN observations at Cape Grim (40∘39′ S) corresponded with CCN measurements from northern and mid-latitude sectors, while CN10 observations only corresponded with observations from the northern sector. Measurements from a simultaneous 2-year campaign at Macquarie Island (54∘30′ S) were found to represent all aerosol species well. The southernmost latitudes differed significantly from both of these stations, and previous work suggests that Antarctic stations on the East Antarctic coastline do not represent the East Antarctic sea-ice latitudes well. Further measurements are needed to capture the long-term, seasonal and longitudinal variability in aerosol processes across the Southern Ocean.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Cloud condensation nuclei concentrations derived from the CAMS reanalysis

Determining number concentrations of cloud condensation nuclei (CCN) is one of the first steps in the chain in analysis of cloud droplet formation, the direct microphysical link between aerosols and cloud droplets, and a process key for aerosol–cloud interactions (ACI). However, due to sparse coverage of in situ measurements and difficulties associated with retrievals from satellites, a global exploration of their magnitude, source as well as temporal and spatial distribution cannot be easily obtained. Thus, a better representation of CCN numbers is one of the goals for quantifying ACI processes and achieving uncertainty-reduced estimates of their associated radiative forcing. Here, we introduce a new CCN dataset which is derived based on aerosol mass mixing ratios from the latest Copernicus Atmosphere Monitoring Service reanalysis (CAMSRA) in a diagnostic model that uses CAMSRA aerosol properties and a simplified kappa-Köhler framework suitable for global models. The emitted aerosols in CAMSRA are not only based on input from emission inventories using aerosol observations, they also have a strong tie to satellite-retrieved aerosol optical depth (AOD) as this is assimilated as a constraining factor in the reanalysis. Furthermore, the reanalysis interpolates for cases of poor or missing retrievals and thus allows for a full spatiotemporal quantification of CCN numbers. The derived CCN dataset captures the general trend and spatial and temporal distribution of total CCN number concentrations and CCN from different aerosol species. A brief evaluation with ground-based in situ measurements demonstrates the improvement of the modelled CCN over the sole use of AOD as a proxy for CCN as the overall correlation coefficient improved from 0.37 to 0.71. However, we find the modelled CCN from CAMSRA to be generally high biased and find a particular erroneous overestimation at one heavily polluted site which emphasises the need for further validation. The CCN dataset (https://doi.org/10.26050/WDCC/QUAERERE_CCNCAMS_v1, Block, 2023), which is now freely available to users, features 3-D CCN number concentrations of global coverage for various supersaturations and aerosol species covering the years 2003–2021 with daily frequency. This dataset is one of its kind as it offers lots of opportunities to be used for evaluation in models and in ACI studies.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Cloud Condensation Nuclei Hygroscopicity Value-Added Product Report

The purpose of the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility’s Cloud Condensation Nuclei Hygroscopicity Parameter (AOSCCNSMPSKAPPA and AOSCCNUHSASKAPPA) Value-Added Product (VAP) is to calculate the hygroscopicity parameter, kappa, to quantify the ability of aerosols to activate into cloud water droplets. The hygroscopicity parameter is often used to model the cloud condensation nuclei (CCN) activity of atmospheric aerosols of different sizes and compositions, providing additional insight on the influence of aerosols on climate. The AOSCCNUHSASKAPPA VAP was recently developed to provides kappa data for ARM sites where AOSCCNSMPSKAPPA was missing.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Do Ultrafine Cloud Condensation Nuclei Invigorate Deep Convection?

Numerical simulations of the impact of ultrafine cloud condensation nuclei (CCN) on deep convection are analyzed herein to investigate the idea proposed by Fan et al. that addition of ultrafine CCN to an otherwise pristine environment leads to convective invigoration. The piggybacking methodology is applied, allowing rigorous separation of the impact of aerosols from different flow realizations that typically occur when even a small element of the model physics or modeling setup is changed. The setup follows the case of daytime convective development over land based on observations during the Large-Scale Biosphere–Atmosphere (LBA) experiment in Amazonia. Overall, the simulated impacts of ultrafine CCN are similar to the previous study by the authors on the impact of pollution on deep convection. There is no convective invigoration above the freezing level, but there is a small invigoration (increase in vertical velocities) below due to the supersaturation and buoyancy differences in conditions with additional ultrafine CCN compared to unperturbed pristine conditions. As in the previous study, the most significant impact is on the upper-tropospheric convective anvils that feature higher cloud fractions in conditions with ultrafine CCN. The increase comes from purely microphysical considerations as the increased cloud droplet concentrations from ultrafine CCN lead to increased ice crystal concentrations and, consequently, smaller sizes and fall velocities, and longer residence times. Mesoscale organization due to low-level shear has a small effect on the simulated ultrafine CCN impacts. Finally, an alternative explanation of increased lightning above oceanic shipping lines seen in satellite observations and argued to result from convective invigoration is provided.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Aerosol Hygroscopic Growth, Mixing State, and Cloud Condensation Nuclei Activity during TRACER (Field Campaign Report)

Convective clouds play a critical role in the Earth’s climate system. Recent research has shown that a realistic representation of convective processes is critical to constraining climate sensitivity in global climate models. Theoretical and modeling studies showed that aerosols could have strong dynamic feedback to convection in warm and humid environments through enhancing ice-related processes and condensational growth. A few observation-based studies also suggested the influence of aerosols on convective cloud and precipitation properties. However, robust observational quantification of an aerosol effect on convective clouds isolated from other factors remains elusive. Understanding the impact of aerosol on convective clouds requires knowledge of the cloud condensation nuclei (CCN) spectrum, which represents the number of particles that uptake water and form cloud droplets as a function of supersaturation. The water uptake by aerosol is also of critical importance for the direct interaction of aerosol with radiation (i.e., aerosol direct effect) due to light scattering and absorption by aerosol. While both droplet activation under supersaturated conditions (i.e., relative humidity RH > 100%) and the hygroscopic growth under sub-saturated conditions (i.e., RH < 100%) are strongly influenced by particle hygroscopicity, the thermodynamic regimes and measurement methods are quite different. Aerosol particles, especially organic particles, can exhibit higher hygroscopicity for droplet activation than that for hygroscopic growth. In the subsaturated regime, the hygroscopicity of organic particles can also vary strongly with RH. However, global climate models usually treat organic species in aerosols with a constant hygroscopicity, potentially introducing substantial uncertainties in the quantification of aerosol radiative effects.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Large contribution of organics to condensational growth and formation of cloud condensation nuclei (CCN) in the remote marine boundary layer

Marine low clouds strongly influence global climate, and their radiative effects are particularly susceptible to the concentration of cloud condensation nuclei (CCN). One major source of CCN is the condensational growth of pre-CCN particles, and sulfate has long been considered the major condensing species in the remote marine boundary layer. While some studies have suggested that secondary organic species can contribute to particle growth, its importance remains unclear. Here we present the first long-term observational evidence that organics play an important role in particle growth over remote oceans. To the contrary of traditional thinking, sulfate dominated condensational growth for only a small (~18 %) fraction of the 62 observed growth events, even fewer than the organic-dominated events (24 %). During most (58 %) growth events, the major condensing species included both organics and sulfate. Potential precursors of the secondary organics are volatile organic compounds from ocean biological activities and those produced by the air–sea interfacial oxidation. Our results indicate that the condensation of secondary organics contributes strongly to the growth of pre-CCN particles and thereby the CCN population over remote oceans.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Drivers of Cloud Condensation Nuclei in the Eastern North Atlantic as Observed at the ARM Site

Abstract Seven years of data collected at the Atmospheric Radiation Measurement's Eastern North Atlantic (ENA) site are analyzed to understand the controls of Cloud Condensation Nuclei (CCN) concentrations in the region. Day‐night differences in the aerosol data as segregated by wind direction demonstrate the aerosol observations to be impacted by local emissions when the wind direction (wdir) is between 90° and 310° (measured clockwise from the North where air is coming from). Data collected during marine conditions (wdir <90° or wdir >310°) show the CCN concentrations to be higher in the summer months as compared to the winter months. CCN budget analysis revealed advection and precipitation scavenging being primarily responsible for modulating the CCN concentrations at the site on monthly timescales, with rain rates driving the precipitation scavenging term. High (greater than 75th percentile) and low (lower than 25th percentile) CCN events were identified for each month to characterize the sub‐monthly variability of CCN concentrations. Low CCN events had thicker clouds, stronger rain rates, and lower reanalysis reported free‐tropospheric aerosol pseudo number concentration at the ENA site as compared to the high CCN events. Analysis of satellite data of air‐parcels 48 hr prior to their arrival at the ENA site demonstrated the air parcels during low CCN events to encounter higher cloudiness, stronger rain rates, and higher cloud top heights as compared to the high CCN events. The results presented herein provide key constraints for model evaluation studies and climatological studies conducted at the ENA site.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

Improving the Confidence in Retrievals of Vertical Distributions of Cloud Condensation Nuclei Number Concentration from ARM Supported by Aircraft In Situ Observations

Accurate quantification of the vertical distribution of cloud condensation nuclei (CCN) number concentrations is critical for improving our understanding of aerosol–cloud interactions. Ground-based Raman lidars operated by the Atmospheric Radiation Measurement (ARM) program, together with surface CCN measurements, are used to retrieve vertically resolved CCN number concentrations (Retrieved Number concentration of CCN, RNCCN). These retrievals rely on several assumptions, including that aerosol composition is vertically homogeneous. To assess this assumption, we developed and tested a framework to infer the dominant aerosol classes/types at different altitudes. This was done by applying a k-Nearest-Neighbors (kNN) algorithm to lidar ratio and linear depolarization ratio measurements from Raman lidar. We evaluated the framework using aircraft aerosol and CCN measurements from the ARM Holistic Interactions of Shallow Clouds, Aerosols, and Land Ecosystems (HI-SCALE) field campaign. The results show that RNCCN performance degrades as vertical aerosol complexity increases, i.e., RNCCN agrees with the aircraft CCN in vertically homogeneous conditions, but closure decreases in layered aerosol structures. To generalize beyond individual examples, we introduce a metric (heterogeneity index) that quantifies the vertical complexity by assessing the variation of inferred aerosol classes/types. Case-level statistics show a tendency for RNCCN and aircraft differences to increase with this metric. By detecting retrievals that are likely compromised by aerosol vertical heterogeneity, the proposed framework improves the interpretability and effective use of RNCCN used for long-term evaluation of models and aerosol–cloud interactions.

Tian, Jingjing↗
DOE OSTI2023

African smoke particles act as cloud condensation nuclei in the wintertime tropical North Atlantic boundary layer over Barbados

Abstract. The number concentration and properties of aerosol particles serving as cloud condensation nuclei (CCN) are important for understanding cloud properties, including in the tropical Atlantic marine boundary layer (MBL), where marine cumulus clouds reflect incoming solar radiation and obscure the low-albedo ocean surface. Studies linking aerosol source, composition, and water uptake properties in this region have been conducted primarily during the summertime dust transport season, despite the region receiving a variety of aerosol particle types throughout the year. In this study, we compare size-resolved aerosol chemical composition data to the hygroscopicity parameter κ derived from size-resolved CCN measurements made during the Elucidating the Role of Clouds–Circulation Coupling in Climate (EUREC4A) and Atlantic Tradewind Ocean-Atmosphere Mesoscale Interaction Campaign (ATOMIC) campaigns from January to February 2020. We observed unexpected periods of wintertime long-range transport of African smoke and dust to Barbados. During these periods, the accumulation-mode aerosol particle and CCN number concentrations as well as the proportions of dust and smoke particles increased, whereas the average κ slightly decreased (κ=0.46±0.10) from marine background conditions (κ=0.52±0.09) when the submicron particles were mostly composed of marine organics and sulfate. Size-resolved chemical analysis shows that smoke particles were the major contributor to the accumulation mode during long-range transport events, indicating that smoke is mainly responsible for the observed increase in CCN number concentrations. Earlier studies conducted at Barbados have mostly focused on the role of dust on CCN, but our results show that aerosol hygroscopicity and CCN number concentrations during wintertime long-range transport events over the tropical North Atlantic are also affected by African smoke. Our findings highlight the importance of African smoke for atmospheric processes and cloud formation over the Caribbean.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Assessment of Extinction‐, Satellite‐, and Model‐Based Vertical Cloud Condensation Nuclei (CCN) Retrieval Methods Using Airborne CCN Measurements Over the Southern Great Plains

Abstract Accurate estimates of the vertical profile of cloud condensation nuclei (CCN) concentration are crucial to better quantify aerosol‐cloud interactions. We assessed the correlation between the vertical CCN concentrations obtained from extinction‐, satellite‐, and model‐based retrieval methods and airborne CCN concentrations collected at 0.24% supersaturation within the 3, 9, 27, and 81 km regions centered over the U.S. Department of Energy's Atmospheric Radiation Measurement User Facility Southern Great Plains (SGP) site during the spring and summer of 2016. The extinction profiles at a wavelength 355 nm were provided by the ground‐based Raman lidar. Our analysis showed moderate correlation between dry‐corrected extinction and airborne CCN data. We found the retrieved number concentration of CCN (RNCCN) method showed regression best‐fit slopes close to unity and consistent prediction errors for the majority of the data. The Lenhardt et al. (2023, https://doi.org/10.5194/amt‐16‐2037‐2023 ) method showed similar conclusions but only during spring, whereas the Mamouri and Ansmann (2016, https://doi.org/10.5194/acp‐16‐5905‐2016 ) method showed poor correlation. The Shinozuka et al. (2015, https://doi.org/10.5194/acp‐15‐7585‐2015 ) satellite‐based method exhibited reasonable agreement during summer but poor correlation during periods where both high (∼1,400 #/cm 3 ) and low (∼50 #/cm 3 ) airborne CCN concentrations were observed. The Copernicus Atmosphere Monitoring Service reanalysis modeled 3‐D CCN data set showed a moderate to weak positive correlation but performed poorly at high airborne CCN concentrations. Our analysis suggests the extinction‐based RNCCN method performed better than other methods across most observation periods under the diverse meteorological conditions observed at the SGP site.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Cloud condensation nuclei characteristics at the Southern Great Plains site: role of particle size distribution and aerosol hygroscopicity

The activation ability of aerosols as cloud condensation nuclei (CCN) is crucial in climate and hydrological cycle studies, but their properties are not well known. We investigated the long-term measurements of atmospheric aerosol properties, CCN concentrations (N CCN ) at supersaturation (SS = 0.1%–1.0%), and hygroscopicity at the Department of Energy's Southern Great Plains (SGP) site to illustrate the dependence of N CCN on aerosol properties and transport pathways. Cluster analysis was applied to the back trajectories of air masses to investigate their respective source regions. The results showed that aged biomass burning aerosols from Central America were characterized by higher accumulation mode particles (N accu ; median value 805 cm -3 ) and relatively high aerosol hygroscopicity (κ; median value ~0.25) values that result in the higher CCN activation and relatively high N CCN (median value 258–1578 cm -3 at a SS of 0.1%–1.0%). Aerosols from the Gulf of Mexico were characterized by higher N accu (~35%), and N CCN (230–1721 cm -3 at a SS of 0.1%–1.0%) with the lowest κ (~0.17). In contrast, relatively high nucleation mode particles (N nucl ; ~20%) and low N CCN (128–1553 cm -3 at a SS of 0.1%–1.0%) with higher κ (~0.30) values were observed on the aerosols associated with a westerly wind. The results indicate particle size as the most critical factor influencing the ability of aerosols to activate, whereas the effect of chemical composition was secondary. Our CCN closure analysis suggests that chemical composition and mixing state information are more crucial at lower SS, whereas at higher SS, most particles become activated regardless of their chemical composition and size. This study affirms that soluble organic fraction information is required at higher SS for better N CCN prediction, but both the soluble organics fraction and mixing state are vital to reduce the N CCN prediction uncertainty at lower SS.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

Spatial Heterogeneity in Cloud Condensation Nuclei (SHINE) Field Campaign Report

Multiple land-atmosphere coupling processes influence the spatial distribution of boundary-layer energy, moisture, aerosol, or cloud condensation nuclei (CCN) properties. Accurately quantifying the spatial and temporal distributions of CCN concentrations is essential for investigating aerosol-cloud interactions and reducing uncertainties in aerosol radiative forcing estimates of Earth's system.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Enhancements in Cloud Condensation Nuclei Activity From Turbulent Fluctuations in Supersaturation

Abstract The effect of aerosols on the properties of clouds is a large source of uncertainty in predictions of weather and climate. These aerosol‐cloud interactions depend critically on the ability of aerosol particles to form cloud droplets. A challenge in modeling aerosol‐cloud interactions is the representation of interactions between turbulence and cloud microphysics. Turbulent mixing leads to small‐scale fluctuations in water vapor and temperature that are unresolved in large‐scale atmospheric models. To quantify the impact of turbulent fluctuations on cloud condensation nuclei (CCN) activation, we used a high‐resolution Large Eddy Simulation of a convective cloud chamber to drive particle‐based cloud microphysics simulations. We show small‐scale fluctuations strongly impact CCN activity. Once activated, the relatively long timescales of evaporation compared to fluctuations causes droplets to persist in subsaturated regions, which further increases droplet concentrations.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Cloud Condensation Nuclei Closure Study Using Airborne Measurements Over the Southern Great Plains

Abstract Airborne measurements of non‐refractory bulk aerosol chemical composition, aerosol size distributions, and cloud condensation nuclei (CCN) were conducted onboard a research aircraft during the Holistic Interactions of Shallow Clouds, Aerosols and Land Ecosystems field campaign in the spring and summer of 2016. A CCN closure study for the entire campaign period was performed where measured CCN concentrations at 0.24% and 0.46% supersaturation were compared with the predicted CCN concentrations calculated using κ ‐Köhler theory, three different assumptions of aerosol mixing state, and various assumptions about hygroscopicity, density, and the insoluble fraction of organic particles. We found that the Closure Ratio (CR), calculated as the ratio of predicted to measured CCN concentrations, was equal to one under two different aerosol mixing state assumptions: (a) all particles are composed of 100% organic particles, and (b) particles are externally mixed and composed of pure sulfates, nitrates, and organic particles assuming hygroscopicity values for organic particles ( ) between 0.04 and 0.17. The use of internal mixing state assumption often led to overprediction of CCN concentrations but the agreement within ±20% with the measured CCN concentrations was observed under certain closure permutations. A similar agreement, that is, within ±20%, was also observed using permuted parameters concerning density (1 and 1.5 g cm −3 ) and an insoluble fraction (0% and 20%) of organic particles. These findings may provide constraints on to predict CCN concentrations at a remote continental Southern Great Plains site.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Formation Process of Particles and Cloud Condensation Nuclei Over the Amazon Rainforest: The Role of Local and Remote New-Particle Formation

Understanding the formation processes of particles and cloud condensation nuclei (CCN) in pristine environments is a major challenge in accurately assessing anthropogenic radiative forcing. Here, using a state-of-the-art model that systematically simulates the chemical processes controlling new-particle formation (NPF) and multi-scale chemical transport, we find that NPF contributes ~90% of the particle number and ~80% of the CCN at 0.5% supersaturation (CCN0.5%) in the pristine Amazon boundary layer during the wet season. The corresponding contributions are only ~30% and ~20% during the dry season because of prevalent biomass burning. In both seasons, about half of the NPF-induced particles and ~85% of the NPF-induced CCN0.5% in the boundary layer originate from the long-range transport of new particles formed hundreds to thousands of kilometers away. Moreover, about 50–65% of the NPF-induced particles and 35–50% of the NPF induced CCN0.5% originate from the downward transport of new particles formed in the free troposphere.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Properties and Controlling Processes of Aerosol and Cloud Condensation Nuclei in Marine Boundary Layer Over Eastern North Atlantic (Final Report)

Remote marine low cloud systems have large spatial and temporal coverages. Because of their relatively low optical thickness and background aerosol concentrations, marine low clouds are particularly susceptible to perturbations in aerosols associated with anthropogenic emissions. Recent studies show that a large fraction of the global aerosol indirect forcing can be attributed to changes in marine low clouds, despite their relatively long distance from most anthropogenic sources. Currently, there remain large uncertainties in the magnitude of the global aerosol indirect radiative forcing. One major contribution to this large uncertainty derives from poor understanding of the aerosols under natural conditions, the perturbation by anthropogenic emissions, and the processes that drive them. In this project, we took advantage of the comprehensive, multi-dimensional characterization of meteorological parameters, trace gases, aerosol, cloud, and drizzle fields during the Aerosol and Cloud Experiments in Eastern North Atlantic (ACE-ENA) and the long-term measurements at the Atmospheric Radiation Measurement (ARM) Eastern North Atlantic (ENA) site on Graciosa Island. By synergistically combining in situ measurements, remote sensing retrievals, and model simulations, we quantified aerosol properties in the ENA, their vertical profiles, and variations with season, synoptic state, and airmass. We investigated key aerosol processes, including entrainment of free troposphere aerosol into marine boundary layer, new particle formation, growth of Aitken mode particles, and the influences of these processes on the cloud condensation nuclei (CCN) population in marine boundary layer. The representation of key aerosol processes in the Energy Exascale Earth System Model (E3SM) was evaluated using the observations. This project has led to 26 publications, which are listed at the end of this report.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Measurement report: Cloud condensation nuclei activity and its variation with organic oxidation level and volatility observed during an aerosol life cycle intensive operational period (ALC-IOP)

Abstract. Cloud condensation nuclei (CCN) spectrum and the CCN activated fraction of size-resolved aerosols (SR-CCN) were measured at a rural site on Long Island during the Department of Energy (DOE) aerosol life cycle intensive operational period (ALC-IOP) from 15 July to 15 August 2011. During the last week of the ALC-IOP, the dependence of the activated fraction on aerosol volatility was characterized by sampling downstream of a thermodenuder (TD) operated at temperatures up to 100 ∘C. Here we present aerosol properties, including aerosol total number concentration, CCN spectrum, and the CCN hygroscopicity, for air masses of representative origins during the ALC-IOP. The hygroscopicity of organic species in the aerosol is derived from CCN hygroscopicity and chemical composition. The dependence of organic hygroscopicity on the organic oxidation level (e.g., atomic O:C ratio) agrees well with theoretical predictions and results from previous laboratory and field studies. The derived κorg and O:C ratio first increase as TD temperature increases from 20 ∘C (i.e., ambient temperature) to 50 or 75 ∘C and then decrease as TD temperature further increases to 100 ∘C. The initial increases of O:C and κorg with TD temperature below 50 ∘C are likely due to evaporation of more volatile organics with relatively lower O:C and hygroscopicity such as primary organic aerosol. At the high TD temperatures, the decreases of O:C and κorg indicate that evaporated organics were more oxygenated and had lower molecular weights. These trends are different from previous laboratory experiments and field observations, which reported that organic O:C increased monotonically with increasing TD temperature, whereas κorg decreased with the TD temperature. One possible reason is that previous studies were either focused on laboratory-generated secondary organic aerosol (SOA) or based on field observations at locations more dominated by SOA.

54 ENVIRONMENTAL SCIENCES↗