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The impact of ocean ecosystems on marine boundary layer aerosols and clouds has been the subject of much research but remains uncertain. Five experiments were recently conducted in the western North Atlantic to assess if the seasonally recurring phytoplankton bloom affects aerosol properties. These experiments include the second Western Atlantic Climate Study and four North Atlantic Aerosols and Marine Ecosystem Study cruises. Measurements of unheated and heated number size distributions, cloud condensation nucleus (CCN) concentrations, and aerosol composition were used to identify primary and secondary aerosol components that could be related to the state of the bloom. Only periods of clean marine air, as defined by radon, particle number concentrations, aerosol light absorption coefficient, and back trajectories, were included in the analysis. Nonvolatile material was found to be prevalent in the Aitken mode size range after heating to 230°, likely due to downward mixing from the free troposphere. CCN concentrations at 0.1% supersaturation were best correlated (r2 = 0.73) with accumulation mode nss SO4=. Sea spray aerosol was only correlated with CCN during November when bloom accumulation had not yet occurred and dimethylsulfide concentrations were at a minimum. The fraction of CCN attributable to sea spray aerosol was less than 20% during March, May/June, and September, indicating the limited contribution of sea spray aerosol to the CCN population of the western North Atlantic atmosphere. The strongest link between the plankton bloom and aerosol and cloud properties appears to be due to biogenic non-sea salt SO4=.

The domain of the surface ocean and lower atmosphere is a complex, highly dynamic component of the Earth system. Better understanding of the physics and biogeochemistry of the air-sea interface and the processes that control the exchange of mass and energy across that boundary define the scope of the Surface Ocean-Lower Atmosphere Study (SOLAS) project. The scientific questions driving SOLAS research, as laid out in the SOLAS Science Plan and Implementation Strategy for the period 2004-2014, are highly challenging, inherently multidisciplinary and broad. During that decade, SOLAS has significantly advanced our knowledge. Discoveries related to the physics of exchange, global trace gas budgets and atmospheric chemistry, the CLAW hypothesis (named after its authors, Charlson, Lovelock, Andreae and Warren), and the influence of nutrients and ocean productivity on important biogeochemical cycles, have substantially changed our views of how the Earth system works and revealed knowledge gaps in our understanding. As such SOLAS has been instrumental in contributing to the International Geosphere-Biosphere Programme (IGBP) mission of identification and assessment of risks posed to society and ecosystems by major changes in the Earth's biological, chemical and physical cycles and processes during the Anthropocene epoch. SOLAS is a bottom-up organization, whose scientific priorities evolve in response to scientific developments and community needs, which has led to the launch of a new 10-year phase. SOLAS (2015-2025) will focus on five core science themes that will provide a scientific basis for understanding and projecting future environmental change and for developing tools to inform societal decision-making.

Organic nitrates in both gas and condensed (aerosol) phases were measured during the Uintah Basin Winter Ozone Study from January to February in 2012. A high degree of correlation between total aerosol volume at diameters less than 500 nm and the particulate organic nitrate concentration indicates that organic nitrates are a consistent, if not dominant, fraction of fine aerosol mass. In contrast, a similar correlation with sub-2.5 μm aerosol volume is weaker. The C : N atomic ratio inferred from field measurements of PM2.5 and particulate organic nitrate is 34 : 1. Calculations constrained by the observations indicate that both condensation of gas-phase nitrates and heterogeneous reactions of NO3/N2O5 are responsible for introducing organic nitrate functionality into the aerosol and that the source molecules are alkanes. Extrapolating the results to urban aerosol suggests organic nitrate production from alkanes may be a major secondary organic aerosol source.

Physical and biogeochemical processes in seawater controlling primary marine aerosol (PMA) production and composition are poorly understood and associated with large uncertainties in estimated fluxes into the atmosphere. PMA production was investigated in the biologically productive NE Pacific Ocean and in biologically productive and oligotrophic regions of the NW Atlantic Ocean. Physicochemical properties of model PMA, produced by aeration of fresh seawater under controlled conditions, were quantified. Diel variability in model PMA mass and number fluxes was observed in biologically productive waters, increasing following sunrise and decreasing to predawn levels overnight. Such variability was not seen in oligotrophic waters. During daytime, surfactant scavenging by aeration in the aerosol generator without replenishing the seawater in the reservoir reduced the model PMA production in productive waters to nighttime levels but had no influence on production from oligotrophic waters. Results suggest bubble plume interactions with sunlight-mediated biogenic surfactants in productive seawater significantly enhanced model PMA production. Key Points Surface ocean biogeochemistry mediates physics of marine aerosol production Diel cycles in biologically productive surface seawater mediate production Observations show chemical processes affecting mass and number production fluxes © 2014. American Geophysical Union. All Rights Reserved.

Frost flowers are clusters of highly saline ice crystals growing on newly formed sea ice or frozen lakes. Based on observations of particles derived from frost flowers in the Arctic, we formulate an observation-based parameterization of salt aerosol source function from frost flowers. The particle flux from frost flowers in winter has the order of 106 m-2 s-1 at the wind speed of 10 m s-1, but the source flux is highly localized to new sea ice regions and strongly dependent on wind speed. We have implemented this parameterization into the regional Weather Research and Forecasting model with Chemistry initialized for two wintertime scenarios. The addition of sea salt aerosol emissions from frost flowers increases averaged sea salt aerosol mass and number concentration and subsequent cloud droplet number. This change of cloud droplet number concentration increases downward longwave cloud radiative forcing through enhanced cloud optical depth and emissivity. The magnitude of this forcing of sea salt aerosols from frost flowers on clouds and radiation, however, contributes negligibly to surface warming in Barrow, Alaska, in the wintertime scenarios studied here. Key Points We evaluate a parameterization of salt aerosol from frost flowers in WRF-Chem The modeled salt explains half of the observed submicron salt aerosol Longwave cloud forcing increases but does not add to Arctic surface warming ©2013. American Geophysical Union. All Rights Reserved.

This review focuses on critical issues in ocean-atmosphere exchange that will be addressed by new research strategies developed by the international Surface Ocean-Lower Atmosphere Study (SOLAS) research community. Eastern boundary upwelling systems are important sites for CO2 and trace gas emission to the atmosphere, and the proposed research will examine how heterotrophic processes in the underlying oxygen-deficient waters interact with the climate system. The second regional research focus will examine the role of sea-ice biogeochemistry and its interaction with atmospheric chemistry. Marine aerosols are the focus of a research theme directed at understanding the processes that determine their abundance, chemistry and radiative properties. A further area of aerosol-related research examines atmospheric nutrient deposition in the surface ocean, and how differences in origin, atmospheric processing and composition influence surface ocean biogeochemistry. Ship emissions are an increasing source of aerosols, nutrients and toxins to the atmosphere and ocean surface, and an emerging area of research will examine their effect on ocean biogeochemistry and atmospheric chemistry. The primary role of SOLAS is to coordinate coupled multi-disciplinary research within research strategies that address these issues, to achieve robust representation of critical ocean-atmosphere exchange processes in Earth System models. © 2013 CSIRO.

Marine cloud brightening (MCB) is the deliberate injection of aerosol particles into shallow marine clouds to increase their reflection of solar radiation and reduce the amount of energy absorbed by the climate system. From the physical science perspective, the consensus of a broad international group of scientists is that the viability of MCB will ultimately depend on whether observations and models can robustly assess the scale-up of local-to-global brightening in today's climate and identify strategies that will ensure an equitable geographical distribution of the benefits and risks associated with projected regional changes in temperature and precipitation. To address the physical science knowledge gaps required to assess the societal implications of MCB, we propose a substantial and targeted program of research-field and laboratory experiments, monitoring, and numerical modeling across a range of scales.

In-situ marine cloud droplet number concentrations (CDNCs), cloud condensation nuclei (CCN), and CCN proxies, based on particle sizes and optical properties, are accumulated from seven field campaigns: ACTIVATE; NAAMES; CAMP 2 EX; ORACLES; SOCRATES; MARCUS; and CAPRICORN2. Each campaign involves aircraft measurements, ship-based measurements, or both. Measurements collected over the North and Central Atlantic, Indo-Pacific, and Southern Oceans, represent a range of clean to polluted conditions in various climate regimes. With the extensive range of environmental conditions sampled, this data collection is ideal for testing satellite remote detection methods of CDNC and CCN in marine environments. Remote measurement methods are vital to expanding the available data in these difficult-to-reach regions of the Earth and improving our understanding of aerosol-cloud interactions. The data collection includes particle composition and continental tracers to identify potential contributing CCN sources. Several of these campaigns include High Spectral Resolution Lidar (HSRL) and polarimetric imaging measurements and retrievals that will be the basis for the next generation of space-based remote sensors and, thus, can be utilized as satellite surrogates., (© 2023. This is a U.S. Government work and not under copyright protection in the US; foreign copyright protection may apply.)

SignificancePhysical and chemical properties of individual atmospheric particles determine their climate impacts. Hygroscopic inorganic salt particles mixed with trace amounts of organic material are predicted to be liquid under typical tropospheric conditions in the summertime Arctic. Yet, we unexpectedly observed a significant concentration of solid particles composed of ammonium sulfate with an organic coating under conditions of high relative humidity and low temperature. These particle properties are consistent with marine biogenic-derived new particle formation and growth, with particle collision hypothesized to result in the solid phase. This particle source is predicted to have increasing relevance in the context of declining Arctic sea ice and increasing open water, with impacts on clouds, and therefore climate.

Four North Atlantic Aerosol and Marine Ecosystems Study (NAAMES) field campaigns from winter 2015 through spring 2018 sampled an extensive set of oceanographic and atmospheric parameters during the annual phytoplankton bloom cycle. This unique dataset provides four seasons of open-ocean observations of wind speed, sea surface temperature (SST), seawater particle attenuation at 660 nm ( c p,660 , a measure of ocean particulate organic carbon), bacterial production rates, and sea-spray aerosol size distributions and number concentrations ( N SSA ). The NAAMES measurements show moderate to strong correlations (0.56 < R < 0.70) between N SSA and local wind speeds in the marine boundary layer on hourly timescales, but this relationship weakens in the campaign averages that represent each season, in part because of the reduction in range of wind speed by multiday averaging. N SSA correlates weakly with seawater c p,660 ( R = 0.36, P << 0.01), but the correlation with c p,660 , is improved ( R = 0.51, P < 0.05) for periods of low wind speeds. In addition, NAAMES measurements provide observational dependence of SSA mode diameter ( d m ) on SST, with d m increasing to larger sizes at higher SST ( R = 0.60, P << 0.01) on hourly timescales. These results imply that climate models using bimodal SSA parameterizations to wind speed rather than a single SSA mode that varies with SST may overestimate SSA number concentrations (hence cloud condensation nuclei) by a factor of 4 to 7 and may underestimate SSA scattering (hence direct radiative effects) by a factor of 2 to 5, in addition to overpredicting variability in SSA scattering from wind speed by a factor of 5., Competing Interests: The authors declare no conflict of interest.

Biogenic sources contribute to cloud condensation nuclei (CCN) in the clean marine atmosphere, but few measurements exist to constrain climate model simulations of their importance. The chemical composition of individual atmospheric aerosol particles showed two types of sulfate-containing particles in clean marine air masses in addition to mass-based Estimated Salt particles. Both types of sulfate particles lack combustion tracers and correlate, for some conditions, to atmospheric or seawater dimethyl sulfide (DMS) concentrations, which means their source was largely biogenic. The first type is identified as New Sulfate because their large sulfate mass fraction (63% sulfate) and association with entrainment conditions means they could have formed by nucleation in the free troposphere. The second type is Added Sulfate particles (38% sulfate), because they are preexisting particles onto which additional sulfate condensed. New Sulfate particles accounted for 31% (7 cm -3 ) and 33% (36 cm -3 ) CCN at 0.1% supersaturation in late-autumn and late-spring, respectively, whereas sea spray provided 55% (13 cm -3 ) in late-autumn but only 4% (4 cm -3 ) in late-spring. Our results show a clear seasonal difference in the marine CCN budget, which illustrates how important phytoplankton-produced DMS emissions are for CCN in the North Atlantic.

Background: Advances in single-cell sequencing provide unprecedented opportunities for clinical examination of circulating tumor cells, cancer stem cells, and other rare cells responsible for disease progression and drug resistance. On the genomic level, single-cell whole exome sequencing (scWES) started to gain popularity with its unique potentials in characterizing mutational landscapes at a single-cell level. Currently, there is little known about the performance of different exome capture kits in scWES. Nextera rapid capture (NXT; Illumina, Inc.) has been the only exome capture kit recommended for scWES by Fluidigm C1, a widely accessed system in single-cell preparation., Results: In this study, we compared the performance of NXT following Fluidigm's protocol with Agilent SureSelectXT Target Enrichment System (AGL), another exome capture kit widely used for bulk sequencing. We created DNA libraries of 192 single cells isolated from spheres grown from a melanoma specimen using Fluidigm C1. Twelve high-yield cells were selected to perform dual-exome capture and sequencing using AGL and NXT in parallel. After mapping and coverage analysis, AGL outperformed NXT in coverage uniformity, mapping rates of reads, exome capture rates, and low PCR duplicate rates. For germline variant calling, AGL achieved better performance in overlap with known variants in dbSNP and transition-transversion ratios. Using calls from high coverage bulk sequencing from blood DNA as the golden standard, AGL-based scWES demonstrated high positive predictive values, and medium to high sensitivity. Lastly, we evaluated somatic mutation calling by comparing single-cell data with the matched blood sequence as control. On average, 300 mutations were identified in each cell. In 10 of 12 cells, higher numbers of mutations were identified using AGL than NXT, probably caused by coverage depth. When mutations are adequately covered in both AGL and NXT data, the two methods showed very high concordance (93-100% per cell)., Conclusions: Our results suggest that AGL can also be used for scWES when there is sufficient DNA, and it yields better data quality than the current Fluidigm's protocol using NXT., (© 2019 S. Karger AG, Basel.)

Aerosol particles influence global climate by determining cloud droplet number concentrations, brightness, and lifetime. Primary aerosol particles, such as those produced from breaking waves in the ocean, display large particle-particle variability in chemical composition, morphology, and physical phase state, all of which affect the ability of individual particles to accommodate water and grow into cloud droplets. Despite such diversity in molecular composition, there is a paucity of methods available to assess how particle-particle variability in chemistry translates to corresponding differences in aerosol hygroscopicity. Here, an approach has been developed that allows for characterization of the distribution of aerosol hygroscopicity within a chemically complex population of atmospheric particles. This methodology, when applied to the interpretation of nascent sea spray aerosol, provides a quantitative framework for connecting results obtained using molecular mimics generated in the laboratory with chemically complex ambient aerosol. We show that nascent sea spray aerosol, generated in situ in the Atlantic Ocean, displays a broad distribution of particle hygroscopicities, indicative of a correspondingly broad distribution of particle chemical compositions. Molecular mimics of sea spray aerosol organic material were used in the laboratory to assess the volume fractions and molecular functionality required to suppress sea spray aerosol hygroscopicity to the extent indicated by field observations. We show that proper accounting for the distribution and diversity in particle hygroscopicity and composition are important to the assessment of particle impacts on clouds and global climate.

We present a sensitive, compact detector that measures total reactive nitrogen (NOy), as well as NO2, NO, and O3. In all channels, NO2 is directly detected by laser diode based cavity ring-down spectroscopy (CRDS) at 405 nm. Ambient O3 is converted to NO2 in excess NO for the O3 measurement channel. Likewise, ambient NO is converted to NO2 in excess O3. Ambient NOy is thermally dissociated at ∼700 °C to form NO2 or NO in a heated quartz inlet. Any NO present in ambient air or formed from thermal dissociation of other reactive nitrogen compounds is converted to NO2 in excess O3 after the thermal converter. We measured thermal dissociation profiles for six of the major NOy components and compared ambient measurements with other instruments during field campaigns in Utah and Alabama. Alabama measurements were made in a rural location with high biogenic emissions, and Utah measurements were made in the wintertime in unusual conditions that form high ozone levels from emissions related to oil and gas production. The NOy comparison in Alabama, to an accepted standard measurement method (a molybdenum catalytic converter/chemiluminescence instrument), agreed to within 12%, which we define as an upper limit to the accuracy of the NOy channel. The 1σ precision is <30 pptv at 1 s and <4 pptv at 1 min time resolution for all measurement channels. The accuracy is 3% for the NO2 and O3 channels and 5% for the NO channel. The precision and accuracy of this instrument make it a versatile alternative to standard chemiluminescence-based NOy instruments.

Jacobson argues that our statement that "many climate models may overestimate warming by BC" has not been demonstrated. Jacobson challenges our results on the basis that we have misinterpreted some model results, omitted optical focusing under high relative humidity conditions and by involatile components, and because our measurements consist of only two locations over short atmospheric time periods. We address each of these arguments, acknowledging important issues and clarifying some misconceptions, and stand by our observations. We acknowledge that Jacobson identified one detail in our experimental technique that places an additional constraint on the interpretation of our observations and reduces somewhat the potential consequences of the stated implications.

Atmospheric black carbon (BC) warms Earth's climate, and its reduction has been targeted for near-term climate change mitigation. Models that include forcing by BC assume internal mixing with non-BC aerosol components that enhance BC absorption, often by a factor of ~2; such model estimates have yet to be clearly validated through atmospheric observations. Here, direct in situ measurements of BC absorption enhancements (E(abs)) and mixing state are reported for two California regions. The observed E(abs) is small-6% on average at 532 nm-and increases weakly with photochemical aging. The E(abs) is less than predicted from observationally constrained theoretical calculations, suggesting that many climate models may overestimate warming by BC. These ambient observations stand in contrast to laboratory measurements that show substantial E(abs) for BC are possible.

More than twenty years ago, a biological regulation of climate was proposed whereby emissions of dimethyl sulphide from oceanic phytoplankton resulted in the formation of aerosol particles that acted as cloud condensation nuclei in the marine boundary layer. In this hypothesis--referred to as CLAW--the increase in cloud condensation nuclei led to an increase in cloud albedo with the resulting changes in temperature and radiation initiating a climate feedback altering dimethyl sulphide emissions from phytoplankton. Over the past two decades, observations in the marine boundary layer, laboratory studies and modelling efforts have been conducted seeking evidence for the CLAW hypothesis. The results indicate that a dimethyl sulphide biological control over cloud condensation nuclei probably does not exist and that sources of these nuclei to the marine boundary layer and the response of clouds to changes in aerosol are much more complex than was recognized twenty years ago. These results indicate that it is time to retire the CLAW hypothesis.

Atmospheric emissions of gas and particulate matter from a large ocean-going container vessel were sampled as it slowed and switched from high-sulfur to low-sulfur fuel as it transited into regulated coastal waters of California. Reduction in emission factors (EFs) of sulfur dioxide (SO₂), particulate matter, particulate sulfate and cloud condensation nuclei were substantial (≥ 90%). EFs for particulate organic matter decreased by 70%. Black carbon (BC) EFs were reduced by 41%. When the measured emission reductions, brought about by compliance with the California fuel quality regulation and participation in the vessel speed reduction (VSR) program, are placed in a broader context, warming from reductions in the indirect effect of SO₄ would dominate any radiative changes due to the emissions changes. Within regulated waters absolute emission reductions exceed 88% for almost all measured gas and particle phase species. The analysis presented provides direct estimations of the emissions reductions that can be realized by California fuel quality regulation and VSR program, in addition to providing new information relevant to potential health and climate impact of reduced fuel sulfur content, fuel quality and vessel speed reductions.

Oceans cover over two-thirds of the Earth's surface, and the particles emitted to the atmosphere by waves breaking on sea surfaces provide an important contribution to the planetary albedo. During the International Chemistry Experiment in the Arctic LOwer Troposphere (ICEALOT) cruise on the R/V Knorr in March and April of 2008, organic mass accounted for 15-47% of the submicron particle mass in the air masses sampled over the North Atlantic and Arctic Oceans. A majority of this organic component (0.1-0.4 microm(-3)) consisted of organic hydroxyl (including polyol and other alcohol) groups characteristic of saccharides, similar to biogenic carbohydrates found in seawater. The large fraction of organic hydroxyl groups measured during ICEALOT in submicron atmospheric aerosol exceeded those measured in most previous campaigns but were similar to particles in marine air masses in the open ocean (Southeast Pacific Ocean) and coastal sites at northern Alaska (Barrow) and northeastern North America (Appledore Island and Chebogue Point). The ocean-derived organic hydroxyl mass concentration during ICEALOT correlated strongly to submicron Na concentration and wind speed. The observed submicron particle ratios of marine organic mass to Na were enriched by factors of approximately 10(2)-approximately 10(3) over reported sea surface organic to Na ratios, suggesting that the surface-controlled process of film bursting is influenced by the dissolved organic components present in the sea surface microlayer. Both marine organic components and Na increased with increasing number mean diameter of the accumulation mode, suggesting a possible link between organic components in the ocean surface and aerosol-cloud interactions.

Halogen atoms and oxides are highly reactive and can profoundly affect atmospheric composition. Chlorine atoms can decrease the lifetimes of gaseous elemental mercury and hydrocarbons such as the greenhouse gas methane. Chlorine atoms also influence cycles that catalytically destroy or produce tropospheric ozone, a greenhouse gas potentially toxic to plant and animal life. Conversion of inorganic chloride into gaseous chlorine atom precursors within the troposphere is generally considered a coastal or marine air phenomenon. Here we report mid-continental observations of the chlorine atom precursor nitryl chloride at a distance of 1,400 km from the nearest coastline. We observe persistent and significant nitryl chloride production relative to the consumption of its nitrogen oxide precursors. Comparison of these findings to model predictions based on aerosol and precipitation composition data from long-term monitoring networks suggests nitryl chloride production in the contiguous USA alone is at a level similar to previous global estimates for coastal and marine regions. We also suggest that a significant fraction of tropospheric chlorine atoms may arise directly from anthropogenic pollutants.

We have studied the influence of the peripheral vasodilator hydralazine (HDZ) on the vasculature and blood perfusion of two members of a series of subcutaneous murine adenocarcinomata of the colon (MAC tumours), and the influence of HDZ on the efficacy and/or toxicity of TCNU and melphalan. The fluorescent DNA stain Hoechst 33342, showed that HDZ caused a shutdown of tumour vasculature, related in magnitude to both dose and tumour differentiation state; 10 mg kg-1 caused an 80% vascular shutdown of well differentiated MAC 26 tumours, but only a 50% shutdown of the poorly differentiated MAC 15A tumours. 2.5 mg kg-1 was ineffective. The blood perfusion marker 99mTc-HMPAO showed that the normal perfusion of MAC tumours was consistently markedly less than that of lung, liver or kidneys (4-5% of lung perfusion). HDZ (10 mg kg-1) decreased MAC 26 perfusion by 63%, and that of MAC 15A by 20%. Again, 2.5 mg kg-1) was ineffective. Use of in vivo to in vitro clonogenic assays showed that HDZ (10 mg kg-1) potentiated the efficacy of melphalan (1-10 mg kg-1 i.p.) by a factor of 2.1, and increased the efficacy of TCNU (1-10 mg kg-1 i.v., factor = 1.7) when given 10 or 15 min respectively after dosing. However, the addition of HDZ increased the acute bone marrow toxicity of melphalan, but not that of TCNU. The clinical relevance of these results is discussed.

The present study explored the relationship between participants' level of anxiety about death and both their sense of purposefulness in life and their personal experience of time controlling for the effects of participants' general anxiety and social desirability set. Participants were 145 women aged sixty to eighty-five, members of senior citizens clubs in suburban New Jersey, who agreed to complete a booklet of questionnaires at home and return them anonymously. As hypothesized, respondents high in measured death anxiety were found to be more likely to express less sense of purposefulness to their lives, a sense that time is moving forward, a feeling of being harassed and pressured by the passage of time, an experienced discontinuity and lack of direction in their lives, an inclination to procrastinate and be inefficient in their use of time, and a reported disposition towards being inconsistent. For the most part, the relationship between death anxiety and the other variables was found to hold even when the effects of general anxiety and social desirability were partialed out.