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Abstract. Aerosols over Earth's remote and spatially extensive ocean surfaces have important influences on planetary climate. However, these aerosols and their effects remain poorly understood, in part due to the remoteness and limited observations over these regions. In this study, we seek to understand factors that shape marine aerosol size distributions and composition in the Northwest Atlantic Ocean region. We use the GEOS-Chem-TOMAS model to interpret measurements collected from ship and aircraft during the four seasonal campaigns of the North Atlantic Aerosols and Marine Ecosystems Study (NAAMES) conducted between 2015 and 2018. Observations from the NAAMES campaigns show enhancements in aerosol total number concentration at atmospheric altitudes of about 1 km, most pronounced during the phytoplankton bloom maxima (May/June). Our simulations, combined with NAAMES ship and aircraft measurements, suggest several key factors contribute to aerosol number and size in the Northwest Atlantic lower troposphere, with significant regional-mean (40–60° N, 20–50° W) aerosol-cloud albedo indirect effects (AIE) and direct radiative effects (DRE) during the phytoplankton bloom. These key factors and their associated radiative effects in the region are: (1) particle formation above/near the marine boundary layer (MBL) top (AIE: −3.37 W m−2, DRE: −0.62 W m−2), (2) particle growth due to marine secondary organic aerosol (MSOA) as the nascent particles subside into the MBL, enabling them to become cloud-condensation-nuclei-size particles (AIE: −2.27 W m−2, DRE: −0.10 W m−2), (3) particle formation/growth due to the products of dimethyl sulfide, above/within the MBL (−1.29 W m−2, DRE: −0.06 W m−2), and (4) ship emissions (AIE: −0.62 W m−2, DRE: −0.05 W m−2). Our results suggest a synergy of particle formation near the MBL top and growth by MSOA that contributes strongly to cloud-condensation-nuclei-sized particles with significant regional radiative effects in the Northwest Atlantic. Future work is needed to understand the sources and temperature-dependence of condensable marine vapors forming MSOA and to understand the species that can form new particles at the boundary layer top and grow these particles as they descend into the marine boundary layer.

Summertime Arctic aerosol size distributions are strongly controlled by natural regional emissions. Within this context, we use a chemical transport model with sizeresolved aerosol microphysics (GEOS-Chem-TOMAS) to interpret measurements of aerosol size distributions from the Canadian Arctic Archipelago during the summer of 2016, as part of the "NETwork on Climate and Aerosols: Addressing key uncertainties in Remote Canadian Environments" (NETCARE) project. Our simulations suggest that condensation of secondary organic aerosol (SOA) from precursor vapors emitted in the Arctic and near Arctic marine (ice-free seawater) regions plays a key role in particle growth events that shape the aerosol size distributions observed at Alert (82.5° N, 62.3° W), Eureka (80.1° N, 86.4° W), and along a NETCARE ship track within the Archipelago. We refer to this SOA as Arctic marine SOA (AMSOA) to reflect the Arctic marine-based and likely biogenic sources for the precursors of the condensing organic vapors. AMSOA from a simulated flux (500 μgm-2 day-1, north of 50° N) of precursor vapors (with an assumed yield of unity) reduces the summertime particle size distribution model-observation mean fractional error 2- to 4-fold, relative to a simulation without this AMSOA. Particle growth due to the condensable organic vapor flux contributes strongly (30 %-50 %) to the simulated summertime-mean number of particles with diameters larger than 20 nm in the study region. This growth couples with ternary particle nucleation (sulfuric acid, ammonia, and water vapor) and biogenic sulfate condensation to account for more than 90% of this simulated particle number, which represents a strong biogenic influence. The simulated fit to summertime size-distribution observations is further improved at Eureka and for the ship track by scaling up the nucleation rate by a factor of 100 to account for other particle precursors such as gas-phase iodine and/or amines and/or fragmenting primary particles that could be missing from our simulations. Additionally, the fits to the observed size distributions and total aerosol number concentrations for particles larger than 4 nm improve with the assumption that the AMSOA contains semivolatile species: the model-observation mean fractional error is reduced 2- to 3-fold for the Alert and ship track size distributions. AMSOA accounts for about half of the simulated particle surface area and volume distributions in the summertime Canadian Arctic Archipelago, with climaterelevant simulated summertime pan-Arctic-mean top-of-theatmosphere aerosol direct (-0:04Wm-2) and cloud-albedo indirect (-0:4Wm-2) radiative effects, which due to uncertainties are viewed as an order of magnitude estimate. Future work should focus on further understanding summertime Arctic sources of AMSOA.

High-latitude ecosystems have the capacity to release large amounts of carbon dioxide (CO2) to the atmosphere in response to increasing temperatures, representing a potentially significant positive feedback within the climate system. Here, we combine aircraft and tower observations of atmospheric CO2 with remote sensing data and meteorological products to derive temporally and spatially resolved year-round CO2 fluxes across Alaska during 2012-2014. We find that tundra ecosystems were a net source of CO2 to the atmosphere annually, with especially high rates of respiration during early winter (October through December). Long-term records at Barrow, AK, suggest that CO2 emission rates from North Slope tundra have increased during the October through December period by 73% ± 11% since 1975, and are correlated with rising summer temperatures. Together, these results imply increasing early winter respiration and net annual emission of CO2 in Alaska, in response to climate warming. Our results provide evidence that the decadal-scale increase in the amplitude of the CO2 seasonal cycle may be linked with increasing biogenic emissions in the Arctic, following the growing season. Early winter respiration was not well simulated by the Earth System Models used to forecast future carbon fluxes in recent climate assessments. Therefore, these assessments may underestimate the carbon release from Arctic soils in response to a warming climate.

Global modeling of aerosol‐particle number and size is important for understanding aerosol effects on Earth's climate and air quality. Fine‐resolution global models are desirable for representing nonlinear aerosol‐microphysical processes, their nonlinear interactions with dynamics and chemistry, and spatial heterogeneity. However, aerosol‐microphysical simulations are computationally demanding, which can limit the achievable global horizontal resolution. Here, we present the first coupling of the TwO‐Moment Aerosol Sectional (TOMAS) microphysics scheme with the High‐Performance configuration of the GEOS‐Chem model of atmospheric composition (GCHP), a coupling termed GCHP‐TOMAS. GCHP's architecture allows massively parallel GCHP‐TOMAS simulations including on the cloud, using hundreds of computing cores, faster runtimes, more memory, and finer global horizontal resolution (e.g., 25 km × 25 km, 7.8 × 105 model columns) versus the previous single‐node capability of GEOS‐Chem‐TOMAS (tens of cores, 200 km × 250 km, 1.3 × 104 model columns). GCHP‐TOMAS runtimes have near‐ideal scalability with computing‐core number. Simulated global‐mean number concentrations increase (dominated by free‐tropospheric over‐ocean sub‐10‐nm‐diameter particles) toward finer GCHP‐TOMAS horizontal resolution. Increasing the horizontal resolution from 200 km × 200–50 km × 50 km increases the global monthly mean free‐tropospheric total particle number by 18.5%, and over‐ocean sub‐10‐nm‐diameter particles by 39.8% at 4‐km altitude. With a cascade of contributing factors, free‐tropospheric particle‐precursor concentrations increase (32.6% at 4‐km altitude) with resolution, promoting new‐particle formation and growth that outweigh coagulation changes. These nonlinear effects have the potential to revise current understanding of processes controlling global aerosol number and aerosol impacts on Earth's climate and air quality. Plain Language Summary: Small particles in the air have important effects on Earth's climate and air quality. Representing the number and size of these particles in global models is challenging because their processes are complex. This factor has often limited global‐model horizontal resolution because fine global resolution models (e.g., 25 km × 25 km or smaller) generally ran too slowly but would be useful for representing details missed at traditional coarse resolution (e.g., 200 km × 250 km). We start with a detailed particle scheme that previously only ran at coarse global resolution because fine resolution would take too long. We present the initial use of this scheme in an updated model version, with a structure allowing a fast‐running, high‐memory model with fine resolution, by using hundreds to thousands of computer cores. In the updated structure, model speed increases with the number of cores used. We find that the total number of particles in the model is more with fine compared to coarse model resolution. These increases are most in Earth's remote regions and for particles which come from gas. Using fine model resolution globally when representing particles could change our understanding of how they impact Earth's climate and air quality. Key Points: We couple aerosol microphysics with GEOS‐Chem's High‐Performance configuration for fine (25 km × 25 km) global‐resolution capabilityGlobal‐mean aerosol number increases with model resolution, dominated by particles smaller than 10 nm in the over‐ocean free troposphereToward finer horizontal resolution, enhanced particle precursor loading in the free troposphere promotes particle formation and growth [ABSTRACT FROM AUTHOR]

With rapid changes in climate and the seasonal amplitude of carbon dioxide (CO2) in the Arctic, it is critical that we detect and quantify the underlying processes controlling the changing amplitude of CO2 to better predict carbon cycle feedbacks in the Arctic climate system. We use satellite and airborne observations of atmospheric CO2 with climatically forced CO2 flux simulations to assess the detectability of Alaskan carbon cycle signals as future warming evolves. We find that current satellite remote sensing technologies can detect changing uptake accurately during the growing season but lack sufficient cold season coverage and near-surface sensitivity to constrain annual carbon balance changes at regional scale. Airborne strategies that target regular vertical profile measurements within continental interiors are more sensitive to regional flux deeper into the cold season but currently lack sufficient spatial coverage throughout the entire cold season. Thus, the current CO2 observing network is unlikely to detect potentially large CO2 sources associated with deep permafrost thaw and cold season respiration expected over the next 50 y. Although continuity of current observations is vital, strategies and technologies focused on cold season measurements (active remote sensing, aircraft, and tall towers) and systematic sampling of vertical profiles across continental interiors over the full annual cycle are required to detect the onset of carbon release from thawing permafrost.

Wetlands are the largest global natural methane (CH4/ source, and emissions between 50 and 70° N latitude contribute 10-30% to this source. Predictive capability of land models for northern wetland CH4 emissions is still low due to limited site measurements, strong spatial and temporal variability in emissions, and complex hydrological and biogeochemical dynamics. To explore this issue, we compare wetland CH4 emission predictions from the Community Land Model 4.5 (CLM4.5-BGC) with siteto regional-scale observations. A comparison of the CH4 fluxes with eddy flux data highlighted needed changes to the model's estimate of aerenchyma area, which we implemented and tested. The model modification substantially reduced biases in CH4 emissions when compared with CarbonTracker CH4 predictions. CLM4.5 CH4 emission predictions agree well with growing season (May-September) CarbonTracker Alaskan regional-level CH4 predictions and sitelevel observations. However, CLM4.5 underestimated CH4 emissions in the cold season (October-April). The monthly atmospheric CH4 mole fraction enhancements due to wetland emissions are also assessed using the Weather Research and Forecasting-Stochastic Time-Inverted Lagrangian Transport (WRF-STILT) model coupled with daily emissions from CLM4.5 and compared with aircraft CH4 mole fraction measurements from the Carbon in Arctic Reservoirs Vulnerability Experiment (CARVE) campaign. Both the tower and aircraft analyses confirm the underestimate of cold-season CH4 emissions by CLM4.5. The greatest uncertainties in predicting the seasonal CH4 cycle are from the wetland extent, coldseason CH4 production and CH4 transport processes. We recommend more cold-season experimental studies in highlatitude systems, which could improve the understanding and parameterization of ecosystem structure and function during this period. Predicted CH4 emissions remain uncertain, but we show here that benchmarking against observations across spatial scales can inform model structural and parameter improvements.

Accurate representation of aerosol optical properties is essential for the modeling and remote sensing of atmospheric aerosols. Although aerosol optical properties are strongly dependent upon the aerosol size distribution, the use of detailed aerosol microphysics schemes in global atmospheric models is inhibited by associated computational demands. Computationally efficient parameterizations for aerosol size are needed. In this study, airborne measurements over the United States (DISCOVER-AQ) and South Korea (KORUS-AQ) are interpreted with a global chemical transport model (GEOS-Chem) to investigate the variation in aerosol size when organic matter (OM) and sulfate–nitrate–ammonium (SNA) are the dominant aerosol components. The airborne measurements exhibit a strong correlation (r=0.83) between dry aerosol size and the sum of OM and SNA mass concentration (MSNAOM). A global microphysical simulation (GEOS-Chem-TOMAS) indicates that MSNAOM and the ratio between the two components (OM/SNA) are the major indicators for SNA and OM dry aerosol size. A parameterization of the dry effective radius (Reff) for SNA and OM aerosol is designed to represent the airborne measurements (R2=0.74 ; slope = 1.00) and the GEOS-Chem-TOMAS simulation (R2=0.72 ; slope = 0.81). When applied in the GEOS-Chem high-performance model, this parameterization improves the agreement between the simulated aerosol optical depth (AOD) and the ground-measured AOD from the Aerosol Robotic Network (AERONET; R2 from 0.68 to 0.73 and slope from 0.75 to 0.96). Thus, this parameterization offers a computationally efficient method to represent aerosol size dynamically. [ABSTRACT FROM AUTHOR]

Accurate representation of aerosol optical properties is essential for modeling and remote sensing of atmospheric aerosols. Although aerosol optical properties are strongly dependent upon the aerosol size distribution, use of detailed aerosol microphysics schemes in global atmospheric models is inhibited by associated computational demands. Computationally efficient parameterizations for aerosol size are needed. In this study, airborne measurements over the United States (DISCOVER-AQ) and South Korea (KORUS-AQ) are interpreted with a global chemical transport model (GEOS-Chem) to investigate the variation in aerosol size when organic matter (OM) and sulfate-nitrate-ammonium (SNA) are the dominant aerosol components. The airborne measurements exhibit a strong correlation (r = 0.83) between dry aerosol size and the sum of OM and SNA mass concentration (MSNAOM). A global microphysical simulation (GEOS-Chem-TOMAS) indicates that MSNAOM, and the ratio between the two components (OM/SNA) are the major indicators for SNA and OM dry aerosol size. A parameterization of dry effective radius (Reff) for SNA and OM aerosol is proposed, which well represents the airborne measurements (R² = 0.74, slope = 1.00) and the GEOS-Chem-TOMAS simulation (R² = 0.72, slope = 0.81). When applied in the GEOS-Chem high-performance model, this parameterization improves the agreement between the simulated aerosol optical depth (AOD) and the ground-measured AOD from the Aerosol Robotic Network (AERONET; R² from 0.68 to 0.73, slope from 0.75 to 34 0.96). Thus, this parameterization offers a computationally efficient method to represent aerosol size dynamically. [ABSTRACT FROM AUTHOR]

Detailed knowledge of the physical and chemical properties and sources of particles that form clouds is especially important in pristine areas like the Arctic, where particle concentrations are often low and observations are sparse. Here, we present in situ cloud and aerosol measurements from the central Arctic Ocean in August–September 2018 combined with air parcel source analysis. We provide direct experimental evidence that Aitken mode particles (particles with diameters ≲70 nm) significantly contribute to cloud condensation nuclei (CCN) or cloud droplet residuals, especially after the freeze‐up of the sea ice in the transition toward fall. These Aitken mode particles were associated with air that spent more time over the pack ice, while size distributions dominated by accumulation mode particles (particles with diameters ≳70 nm) showed a stronger contribution of oceanic air and slightly different source regions. This was accompanied by changes in the average chemical composition of the accumulation mode aerosol with an increased relative contribution of organic material toward fall. Addition of aerosol mass due to aqueous‐phase chemistry during in‐cloud processing was probably small over the pack ice given the fact that we observed very similar particle size distributions in both the whole‐air and cloud droplet residual data. These aerosol–cloud interaction observations provide valuable insight into the origin and physical and chemical properties of CCN over the pristine central Arctic Ocean. Key Points: Aitken‐mode particles contributed significantly to cloud droplet formation in the high Arctic, especially after the transition to fallResidence time over the pack ice and the relative contribution of organics both increased when average particle size decreasedAddition of aerosol mass due to aqueous‐phase chemistry was probably small over the pack ice [ABSTRACT FROM AUTHOR]

The impact of aerosols on clouds is a well-studied, although still poorly constrained, part of the atmospheric system. New particle formation (NPF) is thought to contribute 40 %–80 % of the global cloud droplet number concentration, although it is extremely difficult to observe an air mass from NPF to cloud formation. NPF and growth occurs frequently in the Canadian Arctic summer atmosphere, although only a few studies have characterized the source and properties of these aerosols. This study presents cloud condensation nuclei (CCN) concentrations measured on board the CCGS Amundsen in the eastern Canadian Arctic Archipelago from 23 July to 23 August 2016 as part of the Network on Climate and Aerosols: Addressing Uncertainties in Remote Canadian Environments (NETCARE). The study was dominated by frequent ultrafine particle and/or growth events, and particles smaller than 100 nm dominated the size distribution for 92 % of the study period. Using κ -Köhler theory and aerosol size distributions, the mean hygroscopicity parameter (κ) calculated for the entire study was 0.12 (0.06–0.12, 25th–75th percentile), suggesting that the condensable vapours that led to particle growth were primarily slightly hygroscopic, which we infer to be organic. Based on past measurement and modelling studies from NETCARE and the Canadian Arctic, it seems likely that the source of these slightly hygroscopic, organic, vapours is the ocean. Examining specific growth events suggests that the mode diameter (Dmax) had to exceed 40 nm before CCN concentrations at 0.99 % supersaturation (SS) started to increase, although a statistical analysis shows that CCN concentrations increased 13–274 cm -3 during all ultrafine particle and/or growth times (total particle concentrations >500 cm -3 , Dmax<100 nm) compared with background times (total concentrations <500 cm -3) at SS of 0.26 %–0.99 %. This value increased to 25–425 cm -3 if the growth times were limited to times when Dmax was also larger than 40 nm. These results support past results from NETCARE by showing that the frequently observed ultrafine particle and growth events are dominated by a slightly hygroscopic fraction, which we interpret to be organic vapours originating from the ocean, and that these growing particles can increase the background CCN concentrations at SS as low as 0.26 %, thus pointing to their potential contribution to cloud properties and thus climate through the radiation balance. [ABSTRACT FROM AUTHOR]

The impact of aerosols on clouds is a well-studied, although still poorly constrained, part of the atmospheric system. New particle formation (NPF) is thought to contribute 40-80 % of the global cloud droplet number concentration, although it is extremely difficult to observe an air mass from NPF to cloud formation. NPF and growth occurs frequently in the Canadian Arctic summer atmosphere, although only a few studies have characterized the source and properties of these aerosols. This study presents cloud condensation nuclei (CCN) concentrations measured on board the CCGS Amundsen in the eastern Canadian Arctic Archipelago from 23 July to 23 August 2016 as part of the Network on Climate and Aerosols: Addressing Uncertainties in Remote Canadian Environments (NETCARE). The study was dominated by frequent ultrafine particle and/or growth events, and particles smaller than 100 nm dominated the size distribution for 92 % of the study period. Using κ-Kohler theory and aerosol size distributions, the mean hygroscopicity parameter (κ) calculated for the entire study was 0.12 (0.06-0.12, 25th-75th percentile), suggesting that the condensable vapours that led to particle growth were primarily non-hygroscopic, which we infer to be organic. Based on past measurement and modelling studies from NETCARE and the Canadian Arctic, it seems likely that the source of these non-hygroscopic, organic, vapours is the ocean. Examining specific growth events suggests that the mode diameter (Dmax) had to exceed 40 nm before CCN concentrations at 0.99 % SS started to increase, although a statistical analysis shows that CCN concentrations increased 13-274 cm−3 during all ultrafine particle and/or growth times (total particle concentrations > 500 cm−3, Dmax < 100 nm) compared to Background times (total concentrations < 500 cm−3) at SS of 0.26-0.99 %. This value increased to 25-425 cm−3 if the growth times were limited to times when Dmax was also larger than 40 nm. These results support past results from NETCARE by showing that the frequently observed ultrafine particle and growth events are dominated by a highly non-hygroscopic fraction, which we interpret to be organic vapours originating from the ocean, and that these growing particles can increase the background CCN concentrations at SS as low as 0.26 %, thus pointing to their potential contribution to cloud properties and thus climate through the radiation balance. [ABSTRACT FROM AUTHOR]

Environmental supersaturation is a key parameter in the formation of fog and clouds, yet it cannot be measured directly and must be inferred. Calculating the ambient supersaturation in fog requires knowledge of the aerosol hygroscopicity as well as particle size distribution, and relatively few values have been reported in the literature. Here we use κ‐Köhler theory to derive aerosol activation properties based on particle hygroscopicity and dry particle size distributions, and then estimate the effective peak supersaturation during eight cases of radiative fog at the Southern Great Plains site in rural north‐central Oklahoma, USA. The mean hygroscopicity parameter κ of particles likely to act as cloud condensation nuclei varied from 0.14 to 0.43. Ambient effective peak supersaturation during the fog episodes was between 0.01%–0.07%, with most values below 0.04%. The minimum 50% dry activation diameter generally ranged between 300–400 nm with little activation of particles with diameters below 300 nm. Key Points: Supersaturation during eight radiation fog cases at a rural site in Oklahoma, USA is found to vary from 0.01% to 0.06%Evidence of initial dry particle size distribution and aerosol hygroscopicity affects nucleation scavenging efficiencyThe lowest dry activation diameter during each fog event was typically between 300–400 nm and wet activation diameters ranged from 2 to 7 µm [ABSTRACT FROM AUTHOR]

Aerosols over Earth's remote and spatially extensive ocean surfaces have important influences on planetary climate. However, these aerosols and their effects remain poorly understood, in part due to the remoteness and limited observations over these regions. In this study, we seek to understand factors that shape marine aerosol size distributions and composition in the Northwest Atlantic Ocean region. We use the GEOS-Chem-TOMAS model to interpret measurements collected from ship and aircraft during the four seasonal campaigns of the North Atlantic Aerosols and Marine Ecosystems Study (NAAMES) conducted between 2015 and 2018. Observations from the NAAMES campaigns show enhancements in aerosol total number concentration at atmospheric altitudes of about 1 km, most pronounced during the phytoplankton bloom maxima (May/June). Our simulations, combined with NAAMES ship and aircraft measurements, suggest several key factors contribute to aerosol number and size in the Northwest Atlantic lower troposphere, with significant regional-mean (40-60° N, 20-50° W) aerosol-cloud albedo indirect effects (AIE) and direct radiative effects (DRE) during the phytoplankton bloom. These key factors and their associated radiative effects in the region are: (1) particle formation above/near the marine boundary layer (MBL) top (AIE: -3.37 W m-2, DRE: -0.62 W m-2), (2) particle growth due to marine secondary organic aerosol (MSOA) as the nascent particles subside into the MBL, enabling them to become cloud-condensation-nuclei-size particles (AIE: -2.27 W m-2, DRE: -0.10 W m-2), (3) particle formation/growth due to the products of dimethyl sulfide, above/within the MBL (-1.29 W m-2, DRE: -0.06 W m-2), and (4) ship emissions (AIE: -0.62 W m-2, DRE: -0.05 W m-2). Our results suggest a synergy of particle formation near the MBL top and growth by MSOA that contributes strongly to cloud-condensation-nuclei-sized particles with significant regional radiative effects in the Northwest Atlantic. Future work is needed to understand the sources and temperature-dependence of condensable marine vapors forming MSOA and to understand the species that can form new particles at the boundary layer top and grow these particles as they descend into the marine boundary layer. [ABSTRACT FROM AUTHOR]

Low clouds persist in the summer Arctic with important consequences for the radiation budget. In this study, we simulate the linear relationship between liquid water content (LWC) and cloud droplet number concentration (CDNC) observed during an aircraft campaign based out of Resolute Bay, Canada, conducted as part of the Network on Climate and Aerosols: Addressing Key Uncertainties in Remote Canadian Environments study in July 2014. Using a single-column model, we find that autoconversion can explain the observed linear relationship between LWC and CDNC. Of the three autoconversion schemes we examined, the scheme using continuous drizzle (Khairoutdinov and Kogan, 2000) appears to best reproduce the observed linearity in the tenuous cloud regime (Mauritsen et al., 2011), while a scheme with a threshold for rain (Liu and Daum, 2004) best reproduces the linearity at higher CDNC. An offline version of the radiative transfer model used in the Canadian Atmospheric Model version 4.3 is used to compare the radiative effects of the modelled and observed clouds. We find that there is no significant difference in the upward longwave cloud radiative effect at the top of the atmosphere from the three autoconversion schemes (p=0.05) but that all three schemes differ at p=0.05 from the calculations based on observations. In contrast, the downward longwave and shortwave cloud radiative effect at the surface for the Wood (2005b) and Khairoutdinov and Kogan (2000) schemes do not differ significantly (p=0.05) from the observation-based radiative calculations, while the Liu and Daum (2004) scheme differs significantly from the observation-based calculation for the downward shortwave but not the downward longwave fluxes. [ABSTRACT FROM AUTHOR]

During September–October 2016, a marine aerosol generator configured with forced‐air Venturis was deployed at two biologically productive and two oligotrophic regions of the western North Atlantic Ocean to investigate factors that modulate primary marine aerosol (PMA) production. The generator produced representative bubble size distributions with Hinze scales (0.32 to 0.95 mm radii) and void fractions (0.011 to 0.019 Lair Lsw‐1) that overlapped those of plumes produced in the surface ocean by breaking wind waves. Hinze scales and void fractions of bubble plumes varied among seawater hydrographic regions, whereas corresponding peaks and widths of bubble size distributions did not, suggesting that variability in seawater surfactants drove variability in plume dynamics. Peaks in size‐resolved number production efficiencies for model PMA (mPMA) emitted via bubble bursting in the generator were within a narrow range (0.059 to 0.069 μm geometric mean diameter) over wide ranges in subsurface bubble characteristics, suggesting that subsurface bubble size distributions were not the primary controlling factors as was suggested by previous work. Total mass production efficiencies for mPMA decreased with increasing air detrainment rates, supporting the hypothesis that surface bubble rafts attenuate mPMA mass production. Total mass and Na+ production efficiencies for mPMA from biologically productive seawater were significantly greater than those from oligotrophic seawater. Corresponding mPMA number distributions peaked at smaller sizes during daytime, suggesting that short‐lived surfactants of biological and/or photochemical origin modulated diel variability in marine aerosol production. Key Points: Aerosol mass production efficiencies decreased with increasing rates of bubble air detrainment in seawaterProduction efficiencies and enrichment factors of particulate organic mass were higher for productive relative to oligotrophic seawaterAerosol number production efficiencies were insensitive to relative variability in subsurface bubble size distributions [ABSTRACT FROM AUTHOR]

The occurrence of frequent aerosol nucleation and growth events in the Arctic during summertime may impact the region's climate through increasing the number of cloud condensation nuclei in the Arctic atmosphere. Measurements of aerosol size distributions and aerosol composition were taken during the summers of 2015 and 2016 at Eureka and Alert on Ellesmere Island in Nunavut, Canada. These results provide a better understanding of the frequency and spatial extent of elevated Aitken mode aerosol concentrations as well as of the composition and sources of aerosol mass during particle growth. Frequent appearances of small particles followed by growth occurred throughout the summer. These particle growth events were observed beginning in June with the melting of the sea ice rather than with the polar sunrise, which strongly suggests that influence from the marine boundary layer was the primary cause of the events. Correlated particle growth events at the two sites, separated by 480 km, indicate conditions existing over large scales play a key role in determining the timing and the characteristics of the events. In addition, aerosol mass spectrometry measurements were used to analyze the size-resolved chemical composition of aerosols during two selected growth events. It was found that particles with diameters between 50 and 80 nm (physical diameter) during these growth events were predominately organic with only a small sulfate contribution. The oxidation of the organics also changed with particle size, with the fraction of organic acids increasing with diameter from 80 to 400 nm. The growth events at Eureka were observed most often when the temperature inversion between the sea and the measurement site (at 610 m a.s.l.) was non-existent or weak, presumably creating conditions with low aerosol condensation sink and allowing fresh marine emissions to be mixed upward to the observatory's altitude. While the nature of the gaseous precursors responsible for the growth events is still poorly understood, oxidation of dimethyl sulfide alone to produce particle-phase sulfate or methanesulfonic acid was inconsistent with the measured aerosol composition, suggesting the importance of other gas-phase organic compounds condensing for particle growth. [ABSTRACT FROM AUTHOR]

Low clouds persist in the summer Arctic with important consequences for the radiation budget. In this study, we simulate the linear relationship between liquid water content (LWC) and cloud droplet number concentration (CDNC) observed during an aircraft campaign based out of Resolute Bay, Canada conducted as part of the NETCARE study in July 2014. Using a single column model, we find that autoconversion can explain the observed linear relationship between LWC and CDNC. Of the three schemes we examined, the autoconversion scheme using continuous drizzle (Khairoutdinov and Kogan, 2000) appears to best reproduce the observed linearity in the tenuous-cloud regime (Mauritsen et al., 2011), while a scheme with a threshold for rain (Liu and Daum, 2004) best reproduces the linearity at higher CDNC. An offline version of the radiative transfer model used in the Canadian Atmospheric Model version 4.3 is used to compare the radiative effects of the modelled and observed clouds. We find that there is no significant difference in the upward longwave fluxes at the top of the atmosphere from the three autoconversion schemes (p=0.05), but that all three schemes differ at p=0.05 from the calculations based on observations. In contrast, the downward longwave and shortwave fluxes at the surface for all three schemes do not differ significantly (p=0.01) from the observation-based radiative calculations. [ABSTRACT FROM AUTHOR]

Motivated by the need to predict how the Arctic atmosphere will change in a warming world, this article summarizes recent advances made by the research consortium NETCARE (Network on Climate and Aerosols: Addressing Key Uncertainties in Remote Canadian Environments) that contribute to our fundamental understanding of Arctic aerosol particles as they relate to climate forcing. The overall goal of NETCARE research has been to use an interdisciplinary approach encompassing extensive field observations and a range of chemical transport, earth system, and biogeochemical models. Several major findings and advances have emerged from NETCARE since its formation in 2013. (1) Unexpectedly high summertime dimethyl sulfide (DMS) levels were identified in ocean water (up to 75 nM) and the overlying atmosphere (up to 1 ppbv) in the Canadian Arctic Archipelago (CAA). Furthermore, melt ponds, which are widely prevalent, were identified as an important DMS source (with DMS concentrations of up to 6 nM and a potential contribution to atmospheric DMS of 20 % in the study area). (2) Evidence of widespread particle nucleation and growth in the marine boundary layer was found in the CAA in the summertime, with these events observed on 41 % of days in a 2016 cruise. As well, at Alert, Nunavut, particles that are newly formed and grown under conditions of minimal anthropogenic influence during the months of July and August are estimated to contribute 20 % to 80 % of the 30–50 nm particle number density. DMS-oxidation-driven nucleation is facilitated by the presence of atmospheric ammonia arising from seabird-colony emissions, and potentially also from coastal regions, tundra, and biomass burning. Via accumulation of secondary organic aerosol (SOA), a significant fraction of the new particles grow to sizes that are active in cloud droplet formation. Although the gaseous precursors to Arctic marine SOA remain poorly defined, the measured levels of common continental SOA precursors (isoprene and monoterpenes) were low, whereas elevated mixing ratios of oxygenated volatile organic compounds (OVOCs) were inferred to arise via processes involving the sea surface microlayer. (3) The variability in the vertical distribution of black carbon (BC) under both springtime Arctic haze and more pristine summertime aerosol conditions was observed. Measured particle size distributions and mixing states were used to constrain, for the first time, calculations of aerosol–climate interactions under Arctic conditions. Aircraft- and ground-based measurements were used to better establish the BC source regions that supply the Arctic via long-range transport mechanisms, with evidence for a dominant springtime contribution from eastern and southern Asia to the middle troposphere, and a major contribution from northern Asia to the surface. (4) Measurements of ice nucleating particles (INPs) in the Arctic indicate that a major source of these particles is mineral dust, likely derived from local sources in the summer and long-range transport in the spring. In addition, INPs are abundant in the sea surface microlayer in the Arctic, and possibly play a role in ice nucleation in the atmosphere when mineral dust concentrations are low. (5) Amongst multiple aerosol components, BC was observed to have the smallest effective deposition velocities to high Arctic snow (0.03 cm s -1). [ABSTRACT FROM AUTHOR]

Motivated by the need to predict how the Arctic atmosphere will change in a warming world, this article summarizes recent advances made by the research consortium NETCARE (Network on Climate and Aerosols: Addressing Key Uncertainties in Remote Canadian Environments) that contribute to our fundamental understanding of Arctic aerosol particles as they relate to climate forcing. The overall goal of NETCARE research has been to use an interdisciplinary approach encompassing extensive field observations and a range of chemical transport, earth system, and biogeochemical models. Several major findings and advances have emerged from NETCARE since its formation in 2013 . (1) Unexpectedly high summertime dimethyl sulfide (DMS) levels were identified in ocean water and the overlying atmosphere in the Canadian Arctic Archipelago (CAA). Furthermore, melt ponds, which are widely prevalent, were identified as an important DMS source. (2) Evidence was found of widespread particle nucleation and growth in the marine boundary layer in the CAA in the summertime. DMS-oxidation-driven nucleation is facilitated by the presence of atmospheric ammonia arising from sea bird colony emissions, and potentially also from coastal regions, tundra, and biomass burning. Via accumulation of secondary organic material (SOA), a significant fraction of the new particles grow to sizes that are active in cloud droplet formation. Although the gaseous precursors to Arctic marine SOA remain poorly defined, the measured levels of common continental SOA precursors (isoprene and monoterpenes) were low, whereas elevated mixing ratios of oxygenated volatile organic compounds were inferred to arise via processes involving the sea surface microlayer. (3) The variability in the vertical distribution of black carbon (BC) under both springtime Arctic haze and more pristine summertime aerosol conditions was observed. Measured particle size distributions and mixing states were used to constrain, for the first time, calculations of aerosol-climate interactions under Arctic conditions. Aircraft- and ground-based measurements were used to better establish the BC source regions that supply the Arctic via long-range transport mechanisms. (4) Measurements of ice nucleating particles (INPs) in the Arctic indicate that a major source of these particles is mineral dust, likely derived from local sources in the summer and long-range transport in the spring. In addition, INPs are abundant in the sea surface microlayer in the Arctic, and possibly play a role in ice nucleation in the atmosphere when mineral dust concentrations are low. (5) Amongst multiple aerosol components, BC was observed to have the smallest effective deposition velocities to high Arctic snow. [ABSTRACT FROM AUTHOR]

Summertime Arctic aerosol size distributions are strongly controlled by natural regional emissions. Within this context, we use a chemical transport model with size-resolved aerosol microphysics (GEOS-Chem-TOMAS) to interpret measurements of aerosol size distributions from the Canadian Arctic Archipelago during the summer of 2016, as part of the NETwork on Climate and Aerosols: addressing key uncertainties in Remote Canadian Environments (NETCARE). Our simulations suggest that condensation of secondary organic aerosol (SOA) from precursor vapors emitted in the Arctic and near Arctic marine (open ocean and coastal) regions plays a key role in particle growth events that shape the aerosol size distributions observed at Alert (82.5° N, 62.3° W), Eureka (80.1° N, 86.4° W), and along a NETCARE ship track within the Archipelago. We refer to this SOA as Arctic marine SOA (Arctic MSOA) to reflect the Arctic marine-based and likely biogenic sources for the precursors of the condensing organic vapors. Arctic MSOA from a simulated flux (500 μg m-2 d-1, north of 50° N) of precursor vapors (assumed yield of unity) reduces the summertime particle size distribution model-observation mean fractional error by 2- to 4-fold, relative to a simulation without this Arctic MSOA. Particle growth due to the condensable organic vapor flux contributes strongly (30-50 %) to the simulated summertime-mean number of particles with diameters larger than 20 nm in the study region, and couples with ternary particle nucleation (sulfuric acid, ammonia, and water vapor) and biogenic sulfate condensation to account for more than 90 % of this simulated particle number, a strong biogenic influence. The simulated fit to summertime size-distribution observations is further improved at Eureka and for the ship track by scaling up the nucleation rate by a factor of 100 to account for other particle precursors such as gas-phase iodine and/or amines and/or fragmenting primary particles that could be missing from our simulations. Additionally, the fits to observed size distributions and total aerosol number concentrations for particles larger than 4 nm improve with the assumption that the Arctic MSOA contains semi-volatile species; reducing model-observation mean fractional error by 2- to 3-fold for the Alert and ship track size distributions. Arctic MSOA accounts for more than half of the simulated total particulate organic matter mass concentrations in the summertime Canadian Arctic Archipelago, and this Arctic MSOA has strong simulated summertime pan-Arctic-mean top-of-the-atmosphere aerosol direct (-0.04 W m-2) and cloud-albedo indirect (-0.4 W m-2) radiative effects. Future work should focus on further understanding summertime Arctic sources of Arctic MSOA. [ABSTRACT FROM AUTHOR]

The occurrence of frequent aerosol nucleation and growth events in the Arctic during summertime may impact the region’s climate through increasing the number of cloud condensation nuclei in the Arctic atmosphere. Measurements of aerosol size distributions and aerosol composition were taken during the summers of 2015 and 2016 at Eureka and Alert on Ellesmere Island in Nunavut, Canada. The corresponding results provide a better understanding of the frequency and spatial extent of these nucleation and growth events as well as of the composition and sources of aerosol mass during particle growth. These events are observed beginning in June with the melting of the sea ice rather than with polar sunrise, which strongly suggests emissions from marine sources are the primary cause of the events. Frequent particle nucleation followed by growth occurs throughout the summer. Correlated particle growths events at the two sites, separated by 480 km, indicate conditions existing over such large scales play a key role in determining the timing and the characteristics of the events. In addition, aerosol mass spectrometry measurements are used to analyze the size-resolved chemical composition of aerosols during two selected growth events. It is found that particles with diameters smaller than 100 nm are predominately organic with only a small sulphate contribution. The oxidation of the organic fraction also changes with particle size with larger particles containing a greater fraction of organic acids relative to other non-acid oxygenates (e.g. alcohols or aldehydes). It is also observed that the relative amount of m / z 44 in the measured mass spectra increases during the growth events suggesting increases in organic acid concentrations in the particle phase. The nucleation and growth events at Eureka are observed most often when the temperature inversion between the sea and the measurement site (at 610 m a.s.l.) is non-existent or weak allowing presumably fresh marine emissions to be mixed upward to the observatory altitude. While the nature of the gaseous precursors responsible for the growth events are poorly understood, oxidation of dimethyl sulphide alone to produce particle phase sulphate or methanesulphonic acid is not consistent with the measured aerosol composition, suggesting the importance of condensation of other gas phase organic compounds for particle growth. [ABSTRACT FROM AUTHOR]

Methane (CH4) is the second most important greenhouse gas but its emissions from northern regions are still poorly constrained. In this study, we analyze a subset of in situ CH4 aircraft observations made over Alaska during the growing seasons of 2012-2014 as part of the Carbon in Arctic Reservoirs Vulnerability Experiment (CARVE). Net surface CH4 fluxes are estimated using a Lagrangian particle dispersion model which quantitatively links surface emissions from Alaska and the western Yukon with observations of enhanced CH4 in the mixed layer. We estimate that between May and September, net CH4 emissions from the region of interest were 2.2±0.5 Tg, 1.9±0.4 Tg, and 2.3±0.6 Tg of CH4 for 2012, 2013, and 2014, respectively. If emissions are only attributed to two biogenic eco-regions within our domain, then tundra regions were the predominant source, accounting for over half of the overall budget despite only representing 18% of the total surface area. Boreal regions, which cover a large part of the study region, accounted for the remainder of the emissions. Simple multiple linear regression analysis revealed that, overall, CH4 fluxes were largely driven by soil temperature and elevation. In regions specifically dominated by wetlands, soil temperature and moisture at 10 cm depth were important explanatory variables while in regions that were not wetlands, soil temperature and moisture at 40 cm depth were more important, suggesting deeper methanogenesis in drier soils. Although similar environmental drivers have been found in the past to control CH4 emissions at local scales, this study shows that they can be used to generate a statistical model to estimate the regional-scale net CH4 budget. [ABSTRACT FROM AUTHOR]

The source strength and capability of aerosol particles in the Arctic to act as cloud condensation nuclei have important implications for understanding the indirect aerosol-cloud effect within the polar climate system. It has been shown in several Arctic regions that ultrafine particle (UFP) formation and growth is a key contributor to aerosol number concentrations during the summer. This study uses aerosol number size distribution measurements from ship-board measurement expeditions aboard the research icebreaker CCGS Amundsen in the summers of 2014 and 2016 throughout the Canadian Arctic to gain a deeper understanding of the drivers of UFP formation and growth within this marine boundary layer. UFP number concentrations (diameter > 4 nm) in the range of 101-104 cm-3 were observed across the two seasons, with concentrations greater than 103 cm-3 occurring more frequently in 2016. Higher concentrations in 2016 were associated with UFP formation and growth, with events occurring on 41 % of days, while events were only observed on 6 % of days in 2014. Assessment of relevant parameters for aerosol nucleation showed that the median condensation sink in this region was approximately 1.2 h-1 in 2016 and 2.2 h-1 in 2014, which lie at the lower end of ranges observed at even the most remote stations reported in the literature. Apparent growth rates of all observed events in both expeditions averaged 4.3 ±â€‰4.1 nm h-1, in general agreement with other recent studies at similar latitudes. Higher solar radiation, lower cloud fractions, and lower sea ice concentrations combined with differences in the developmental stage and activity of marine microbial communities within the Canadian Arctic were documented and help explain differences between the aerosol measurements made during the 2014 and 2016 expeditions. These findings help to motivate further studies of biosphere-atmosphere interactions within the Arctic marine environment to explain the production of UFP and their growth to sizes relevant for cloud droplet activation. [ABSTRACT FROM AUTHOR]

Methane (CH4) is the second most important greenhouse gas but its emissions from northern regions is still poorly constrained. In this study, we analyze a subset of in situ CH4 aircraft observations made over Alaska during the growing seasons of 2012-2014 as part of the Carbon in Arctic Reservoir Vulnerability Experiment (CARVE). Surface CH4 fluxes are estimated using an atmospheric particle transport model which quantitatively links surface emissions from Alaska and the western Yukon with observations of enhanced CH4 in the boundary layer. We estimate that between May and September, 2.1 ± 0.5 Tg, 1.7 ± 0.4 Tg and 2.0 ± 0.3 Tg of CH4 were emitted from the region of interest for 2012-2014, respectively. The predominant sources of the CH4 budget were two broadly classed eco-regions within our domain, with CH4 from the tundra region accounting for over half of the overall budget, despite only representing 18 % of the total surface area. Boreal regions, which cover a large part of the study region, accounted for the remainder of the emissions. Simple multiple linear regression analysis revealed that overall, CH4 flux were largely driven by soil temperature and elevation. In regions specifically dominated by wetlands, soil temperature and moisture at 10 cm depth were important explanatory variables while in regions that were not wetlands, soil temperature and moisture at 40 cm depth were more important, reflecting the depth at which methanogenesis occurs. Although similar variables have been found in the past to control CH4 emissions at local scales, this study shows that they can be used to generate a statistical model to estimate the regional scale CH4 budget. [ABSTRACT FROM AUTHOR]

Methane (CH4) fluxes from Alaska and other arctic regions may be sensitive to thawing permafrost and future climate change, but estimates of both current and future fluxes from the region are uncertain. This study estimates CH4 fluxes across Alaska for 2012-2014 using aircraft observations from the Carbon in Arctic Reservoirs Vulnerability Experiment (CARVE) and a geostatistical inverse model (GIM). We find that a simple flux model based on a daily soil temperature map and a static map of wetland extent reproduces the atmospheric CH4 observations at the statewide, multiyear scale more effectively than global-scale process-based models. This result points to a simple and effective way of representing CH4 fluxes across Alaska. It further suggests that process-based models can improve their representation of key processes and that more complex processes included in these models cannot be evaluated given the information content of available atmospheric CH4 observations. In addition, we find that CH4 emissions from the North Slope of Alaska account for 24% of the total statewide flux of 1.74 ± 0.26 Tg CH4 (for May-October). Global-scale process models only attribute an average of 3% of the total flux to this region. This mismatch occurs for two reasons: process models likely underestimate wetland extent in regions without visible surface water, and these models prematurely shut down CH4 fluxes at soil temperatures near 0°C. Lastly, we find that the seasonality of CH4 fluxes varied during 2012-2014 but that total emissions did not differ significantly among years, despite substantial differences in soil temperature and precipitation. [ABSTRACT FROM AUTHOR]

Wetlands are the largest global natural methane (CH4) source, and emissions between 50 and 70° N latitude contribute 10-30% to this source. Predictive capability of land models for northern wetland CH4 emissions is still low due to limited site measurements, strong spatial and temporal variability in emissions, and complex hydrological and biogeochemical dynamics. To explore this issue, we compare wetland CH4 emission predictions from the Community Land Model 4.5 (CLM4.5-BGC) with siteto regional-scale observations. A comparison of the CH4 fluxes with eddy flux data highlighted needed changes to the model's estimate of aerenchyma area, which we implemented and tested. The model modification substantially reduced biases in CH4 emissions when compared with CarbonTracker CH4 predictions. CLM4.5 CH4 emission predictions agree well with growing season (May-September) CarbonTracker Alaskan regional-level CH4 predictions and sitelevel observations. However, CLM4.5 underestimated CH4 emissions in the cold season (October-April). The monthly atmospheric CH4 mole fraction enhancements due to wetland emissions are also assessed using the Weather Research and Forecasting-Stochastic Time-Inverted Lagrangian Transport (WRF-STILT) model coupled with daily emissions from CLM4.5 and compared with aircraft CH4 mole fraction measurements from the Carbon in Arctic Reservoirs Vulnerability Experiment (CARVE) campaign. Both the tower and aircraft analyses confirm the underestimate of cold-season CH4 emissions by CLM4.5. The greatest uncertainties in predicting the seasonal CH4 cycle are from the wetland extent, coldseason CH4 production and CH4 transport processes. We recommend more cold-season experimental studies in highlatitude systems, which could improve the understanding and parameterization of ecosystem structure and function during this period. Predicted CH4 emissions remain uncertain, but we show here that benchmarking against observations across spatial scales can inform model structural and parameter improvements. [ABSTRACT FROM AUTHOR]

With rapid changes in climate and the seasonal amplitude of carbon dioxide (CO2) in the Arctic, it is critical that we detect and quantify the underlying processes controlling the changing amplitude of CO2 to better predict carbon cycle feedbacks in the Arctic climate system. We use satellite and airborne observations of atmospheric CO2 with climatically forced CO2 flux simulations to assess the detectability of Alaskan carbon cycle signals as future warming evolves. We find that current satellite remote sensing technologies can detect changing uptake accurately during the growing season but lack sufficient cold season coverage and near-surface sensitivity to constrain annual carbon balance changes at regional scale. Airborne strategies that target regular vertical profile measurements within continental interiors are more sensitive to regional flux deeper into the cold season but currently lack sufficient spatial coverage throughout the entire cold season. Thus, the current CO2 observing network is unlikely to detect potentially large CO2 sources associated with deep permafrost thaw and cold season respiration expected over the next 50 y. Although continuity of current observations is vital, strategies and technologies focused on cold season measurements (active remote sensing, aircraft, and tall towers) and systematic sampling of vertical profiles across continental interiors over the full annual cycle are required to detect the onset of carbon release from thawing permafrost. [ABSTRACT FROM AUTHOR]

Wetlands are the single largest global natural methane (CH4) source, and emissions between 50°N and 70°N latitude contribute 10-30% to this source. Predictive capability of northern wetland CH4 emissions is still low due to limited site measurements, strong spatial and temporal variability in emissions, and complex hydrological and biogeochemical dynamics. To explore this issue, we compare wetland CH4 emission predictions from the Community Land Model 4.5 (CLM4.5-BGC) with site to regional scale observations. A comparison of the CH4 fluxes with eddy flux data highlighted needed changes to the model's estimate of aerenchyma area, which we implemented and tested. The model modification substantially reduced biases in CH4 emissions when compared with CarbonTracker CH4 predictions. CLM4.5 CH4 emission predictions agree well with growing season (May-September) CarbonTracker Alaskan regional-level CH4 predictions and site-level observations. However, CLM4.5 underestimated CH4 emissions in the cold season (October-April). The monthly CH4 mole fraction enhancements due to wetland emissions are also assessed using the WRF-STILT Lagrangian transport model coupled with daily emission priors from CLM4.5 and compared with aircraft CH4 mole fraction measurements from the Carbon in Arctic Reservoirs Vulnerability Experiment (CARVE) campaign. Both the tower and aircraft analyses confirm the underestimate of cold season CH4 emissions by CLM4.5. The greatest uncertainties in predicting the seasonal CH4 cycle are from the wetland extent, cold season CH4 production and CH4 transport processes. We recommend more cold-season experimental studies in high latitude systems, which could improve understanding and parameterization of ecosystem structure and function during this period. Predicted CH4 emissions remain uncertain, but we show here that benchmarking against observations across spatial scales can inform model structural and parameter improvements. [ABSTRACT FROM AUTHOR]

While sea spray particles are highly soluble by nature, and are thus excellent seeds for nascent cloud droplets, organic compounds such as surfactants have previously been identified within aerosol particles, bulk seawater, and the sea-surface microlayer in various oceans and seas. As the presence of dissolved surfactants within spray particles may limit their ability to act as cloud condensation nuclei (CCN), and since the abundance of CCN available during cloud formation is known to affect cloud albedo, the presence of surfactants in the marine environment can affect the local radiation balance. In this work, we added a model surfactant commonly used in households and industry (sodium dodecyl benzene sulfonate, SDBS) to a control solution of NaCl and observed its effects on the number of CCN produced by artificial breaking waves. We found that the addition of SDBS modified the number of CCN produced by a breaking wave analogue in three main ways: (I) by reducing the hygroscopicity of the resulting particulate; (II) by producing finer particulates than the control NaCl solution; and (III) by reducing the total number of particles produced overall. In addition, measurements of the absorption of ultraviolet light (λ = 224 nm) were used to quantify the concentration of SDBS in bulk water samples and aerosol extracts. We found that SDBS was significantly enriched in aerosol extracts relative to the bulk water even when the concentration of SDBS in the bulk water was below the limit of detection (LOD) of our quantitation methods. Thus, the surfactant studied will influence the production of CCN even when present in minute concentrations., Competing Interests: The authors declare no competing financial interest., (© 2022 The Authors. Published by American Chemical Society.)

Breaking waves produce bubble plumes that burst at the sea surface, injecting primary marine aerosol (PMA) highly enriched with marine organic carbon (OC) into the atmosphere. It is widely assumed that this OC is modern, produced by present-day biological activity, even though nearly all marine OC is thousands of years old, produced by biological activity long ago. We used natural abundance radiocarbon ( 14 C) measurements to show that 19 to 40% of the OC associated with freshly produced PMA was refractory dissolved OC (RDOC). Globally, this process removes 2 to 20 Tg of RDOC from the oceans annually, comparable to other RDOC losses. This process represents a major removal pathway for old OC from the sea, with important implications for oceanic and atmospheric biogeochemistry, the global carbon cycle, and climate., (Copyright © 2019 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).)

Surfactants account for minor fractions of total organic carbon in the ocean but can significantly influence the production of primary marine aerosol particles (PMA) at the sea surface via modulation of bubble surface tension. During September and October 2016, model PMA (mPMA) were produced from seawater by bursting bubbles at two biologically productive and two oligotrophic stations in the western North Atlantic Ocean. Total concentrations of surfactants extracted from mPMA and seawater were quantified and characterized via measurements of surface tension isotherms and critical micelle concentrations (CMCs). Surfactant CMCs in biologically productive seawater were lower than those in the oligotrophic seawater suggesting that surfactant mixtures in the two regions were chemically distinct. mPMA surfactants were enriched in all regions relative to those in the associated seawater. Surface tension isotherms indicate that mPMA surfactants were weaker than corresponding seawater surfactants. mPMA from biologically productive seawater contained higher concentrations of surfactants than those produced from oligotrophic seawater, supporting the hypothesis that seawater surfactant properties modulate mPMA surfactant concentrations. Diel variability in concentrations of seawater and mPMA surfactants in some regions is consistent with biological and/or photochemical processing. This work demonstrates direct links between surfactants in mPMA and those in the associated seawater.

Methane (CH 4 ) fluxes from Alaska and other arctic regions may be sensitive to thawing permafrost and future climate change, but estimates of both current and future fluxes from the region are uncertain. This study estimates CH 4 fluxes across Alaska for 2012-2014 using aircraft observations from the Carbon in Arctic Reservoirs Vulnerability Experiment (CARVE) and a geostatistical inverse model (GIM). We find that a simple flux model based on a daily soil temperature map and a static map of wetland extent reproduces the atmospheric CH 4 observations at the state-wide, multi-year scale more effectively than global-scale, state-of-the-art process-based models. This result points to a simple and effective way of representing CH 4 flux patterns across Alaska. It further suggests that contemporary process-based models can improve their representation of key processes that control fluxes at regional scales, and that more complex processes included in these models cannot be evaluated given the information content of available atmospheric CH 4 observations. In addition, we find that CH 4 emissions from the North Slope of Alaska account for 24% of the total statewide flux of 1.74 ± 0.44 Tg CH 4 ( for May-Oct.). Contemporary global-scale process models only attribute an average of 3% of the total flux to this region. This mismatch occurs for two reasons: process models likely underestimate wetland area in regions without visible surface water, and these models prematurely shut down CH 4 fluxes at soil temperatures near 0°C. As a consequence, wetlands covered by vegetation and wetlands with persistently cold soils could be larger contributors to natural CH 4 fluxes than in process estimates. Lastly, we find that the seasonality of CH 4 fluxes varied during 2012-2014, but that total emissions did not differ significantly among years, despite substantial differences in soil temperature and precipitation; year-to-year variability in these environmental conditions did not affect obvious changes in total CH 4 fluxes from the state.