Importance of vertical velocity variations in the cloud droplet nucleation process of marine stratus clouds

Eleven cloud cases through marine stratus, obtained during two field experiments in the North Atlantic Ocean, are used to study the sensitivity of cloud droplet nucleation to the vertical gust velocity. Selected cloud microphysical data, size-distributed aerosol properties and particle chemistry are applied in an adiabatic parcel model. The nucleated cloud droplet number concentrations (N) predicted using the probability density function (PDF) of the measured in-cloud vertical velocities are compared to predictions using a characteristic velocity value. In this study, the model-predicted N from the PDF of the measured in-cloud vertical velocities agrees with the observed maximum N (Nmax) to within 8.6%. The average N (Navg) can be related to Nmax using a power law (Leaitch et al., 1996). If a relationship between Nmax and Navg based on the measurements is applied to obtain the average N from the model-predicted N, then the model-predicted average N agrees with the observed average N to within 13.3%. When a characteristic vertical velocity (0.8 times the standard deviation of the vertical velocity distribution in this study) is used in the parcel model to simulate N, the model-predicted N agrees with the observed maximum N to within 5.7% and the model-predicted average N agrees with the observed average N within 8.8%. This indicates that using a characteristic value of the vertical velocity distribution instead of its PDF is a good approximation for simulating the nucleated cloud droplet number of marine stratus on a cloud scal

Contributions from DMS and ship emissions to CCN observed over the summertime North Pacific

Measurements of cloud condensation nuclei (CCN) made over the North Pacific Ocean in July 2002 are analysed with concurrent measurements of aerosol number, mass and composition. Overall the CCN are controlled by the sulphate, including one case that suggests particle nucleation and growth resulting from dimethyl sulphide oxidation that enhanced CCN concentrations. Hourly CCN concentrations are correlated with concentrations of sulphate plus methanesulphonic acid (MSA) over the entire study period (<i>r</i><sup>2</sup>=0.43 and 0.52 for supersaturations of 0.34% and 0.19%, respectively), and are not well correlated with other organics (<i>r</i><sup>2</sup><0.2). One case study reveals elevated mass and number concentrations of ultrafine and fine organic particles due to regional ship emissions, identified through quadrupole aerosol mass spectrometer (Q-AMS) measurements, during which organic mass concentrations are correlated with CCN values (<i>r</i><sup>2</sup>=0.39 and 0.46 for supersaturations of 0.19% and 0.34%, respectively). The evolution of the time series and mass distributions of organics, sulphate and MSA over this timeframe indicate that the regional distribution of small, diffuse ship-sourced organic particles act as condensation sites for sulphur species, resulting in a subsequent increase in number concentrations of CCN. We conclude that, where present, direct emissions of anthropogenic organic particles may exert a strong control on marine CCN concentrations once diffused into the marine atmosphere, by acting as condensation sites for biogenic and anthropogenic sulphur species

Atmospheric mercury speciation and mercury in snow over time at Alert, Canada

Ten years of atmospheric mercury speciation data and 14 years of mercury in snow data from Alert, Nunavut, Canada, are examined. The speciation data, collected from 2002 to 2011, includes gaseous elemental mercury (GEM), particulate mercury (PHg) and reactive gaseous mercury (RGM). During the winter-spring period of atmospheric mercury depletion events (AMDEs), when GEM is close to being completely depleted from the air, the concentration of both PHg and RGM rise significantly. During this period, the median concentrations for PHg is 28.2 pgm⁻³ and RGM is 23.9 pgm⁻³, from March to June, in comparison to the annual median concentrations of 11.3 and 3.2 pgm⁻³ for PHg and RGM, respectively. In each of the ten years of sampling, the concentration of PHg increases steadily from January through March and is higher than the concentration of RGM. This pattern begins to change in April when the levels of PHg peak and RGM begin to increase. In May, the high PHg and low RGM concentration regime observed in the early spring undergoes a transition to a regime with higher RGM and much lower PHg concentrations. The higher RGM concentration continues into June. The transition is driven by the atmospheric conditions of air temperature and particle availability. Firstly, a high ratio of the concentrations of PHg to RGM is reported at low temperatures which suggests that oxidized gaseous mercury partitions to available particles to form PHg. Prior to the transition, the median air temperature is −24.8 °C and after the transition the median air temperature is −5.8 °C. Secondly, the high PHg concentrations occur in the spring when high particle concentrations are present. The high particle concentrations are principally due to Arctic haze and sea salts. In the snow, the concentrations of mercury peak in May for all years. Springtime deposition of total mercury to the snow at Alert peaks in May when atmospheric conditions favour higher levels of RGM. Therefore, the conditions in the atmosphere directly impact when the highest amount of mercury will be deposited to the snow during the Arctic spring

The effect of organic compounds on the growth rate of cloud droplets in marine and forest settings

International audienceOrganic matter represents an important fraction of the fine particle aerosol, yet our knowledge of the roles of organics in the activation of aerosol particles into cloud droplets is poor. A cloud condensation nucleus (CCN) counter is used to examine the relative growth rates of cloud droplets for case studies from field measurements on the North Pacific Ocean and in a coniferous forest. A model of the condensational growth of water droplets, on particles dissolving according to their solubility in water, is used to simulate the initial scattering of the droplets as they grow in the CCN counter. Simulations of the growth rates of fine particles sampled in the marine boundary layer of the North Pacific Ocean indicate that the main influence of the marine organic material on the water uptake rate is from its effect on the size distribution of the sulphate. Simulations of the observations of water uptake on biogenic organic aerosol particles sampled in a coniferous forest indicate an impact of the organic on the water uptake rates, but one that is still smaller than that of pure sulphate. The solubility of the organic becomes an important factor in determining the water uptake as the organic mass increases relative to sulphate. The values of the organic component of the hygroscopicity parameter ? that describes the CCN activity were found to be negligible for the marine particles and 0.02?0.05 for the forest particles

Trans-Pacific dust events observed at Whistler, British Columbia during INTEX-B

International audienceThe meteorology and physico-chemical characteristics of aerosol associated with two new cases of long range dust transport affecting western Canada during spring 2006 are described. Each event showed enhancements of both sulfate aerosol and crustal material of Asian origin. However, the events were of quite different character and demonstrate the highly variable nature of such events. The April event was a significant dust event with moderate sulfate enhancement while the May event was a weak dust event with very significant sulfate enhancement. The latter event was interesting in the sense that it was of short duration and was quickly followed by significant enhancement of organic material likely of regional origin. Comparison of these two events with other documented cases extending back to 1993, suggests that all dust events show coincident enhancements of sulfate and crustal aerosol. However, events vary across a wide continuum based on the magnitude of aerosol enhancements and their sulfate to calcium ratios. At one extreme, events are dominated by highly significant crustal enhancements (e.g. the well-documented 1998 and 2001 "dust" events) while at the other are events with some dust transport, but where sulfate enhancements are of very high magnitude (e.g. the 1993 event at Crater Lake and the 15 May 2006 event at Whistler). Other events represent a "mix". It is likely that this variability is a function of the comparative strengths of the dust and anthropogenic SO2 sources, the transport pathway and in particular the extent to which dust is transported across industrial SO2 sources, and finally, meteorological and chemical processes

Ground-based remote sensing of an elevated forest fire aerosol layer at Whistler, BC: implications for interpretation of mountaintop chemistry

On 30 August 2009, intense forest fires in interior British Columbia (BC) coupled with winds from the east and northeast resulted in transport of a broad forest fire plume across southwestern BC. The physico-chemical and optical characteristics of the plume as observed from Saturna Island (AERONET), CORALNet-UBC and the Whistler Mountain air chemistry facility were consistent with forest fire plumes that have been observed elsewhere in continental North America. However, the importance of three-dimensional transport in relation to the interpretation of mountaintop chemistry observations is highlighted on the basis of deployment of both a <i>CL31</i> ceilometer and a single particle mass spectrometer (SPMS) in a mountainous setting. The SPMS is used to identify the biomass plume based on levoglucosan and potassium markers. Data from the SPMS are also used to show that the biomass plume was correlated with nitrate, but not correlated with sulphate or sodium. This study not only provides baseline measurements of biomass burning plume physico-chemical characteristics in western Canada, but also highlights the importance of lidar remote sensing methods in the interpretation of mountaintop chemistry measurements

Evaluation of an entraining droplet activation parameterization using in situ cloud data

This study investigates the ability of a droplet activation parameterization (which considers the effects of entrainment and mixing) to reproduce observed cloud droplet number concentration (CDNC) in ambient clouds. Predictions of the parameterization are compared against cloud averages of CDNC from ambient cumulus and stratocumulus clouds sampled during CRYSTAL‐FACE (Key West, Florida, July 2002) and CSTRIPE (Monterey, California, July 2003), respectively. The entrainment parameters required by the parameterization are derived from the observed liquid water content profiles. For the cumulus clouds considered in the study, CDNC is overpredicted by 45% with the adiabatic parameterization. When entrainment is accounted for, the predicted CDNC agrees within 3.5%. Cloud‐averaged CDNC for stratocumulus clouds is well captured when entrainment is not considered. In all cases considered, the entraining parameterization compared favorably against a statistical correlation developed from observations to treat entrainment effects on droplet number. These results suggest that including entrainment effects in the calculation of CDNC, as presented here, could address important overprediction biases associated with using adiabatic CDNC to represent cloud‐scale average values

Corrigendum to &quot;Size-resolved observations of refractory black carbon particles in cloud droplets at a marine boundary layer site&quot; published in Atmos. Chem. Phys., 15, 1367–1383, 2015

No abstract available

Analysis of aircraft and satellite measurements from the Intercontinental Chemical Transport Experiment (INTEX-B) to quantify long-range transport of East Asian sulfur to Canada

We interpret a suite of satellite, aircraft, and ground-based measurements over the North Pacific Ocean and western North America during April&amp;ndash;May 2006 as part of the Intercontinental Chemical Transport Experiment Phase B (INTEX-B) campaign to understand the implications of long-range transport of East Asian emissions to North America. The Canadian component of INTEX-B included 33 vertical profiles from a Cessna 207 aircraft equipped with an aerosol mass spectrometer. Long-range transport of organic aerosols was insignificant, contrary to expectations. Measured sulfate plumes in the free troposphere over British Columbia exceeded 2 μg/m&lt;sup&gt;3&lt;/sup&gt;. We update the global anthropogenic emission inventory in a chemical transport model (GEOS-Chem) and use it to interpret the observations. Aerosol Optical Depth (AOD) retrieved from two satellite instruments (MISR and MODIS) for 2000&amp;ndash;2006 are analyzed with GEOS-Chem to estimate an annual growth in Chinese sulfur emissions of 6.2% and 9.6%, respectively. Analysis of aircraft sulfate measurements from the NASA DC-8 over the central Pacific, the NSF C-130 over the east Pacific and the Cessna over British Columbia indicates most Asian sulfate over the ocean is in the lower free troposphere (800&amp;ndash;600 hPa), with a decrease in pressure toward land due to orographic effects. We calculate that 56% of the measured sulfate between 500&amp;ndash;900 hPa over British Columbia is due to East Asian sources. We find evidence of a 72&amp;ndash;85% increase in the relative contribution of East Asian sulfate to the total burden in spring off the northwest coast of the United States since 1985. Campaign-average simulations indicate anthropogenic East Asian sulfur emissions increase mean springtime sulfate in Western Canada at the surface by 0.31 μg/m&lt;sup&gt;3&lt;/sup&gt; (~30%) and account for 50% of the overall regional sulfate burden between 1 and 5 km. Mean measured daily surface sulfate concentrations taken in the Vancouver area increase by 0.32 μg/m&lt;sup&gt;3&lt;/sup&gt; per 10% increase in the simulated fraction of Asian sulfate, and suggest current East Asian emissions episodically degrade local air quality by more than 1.5 μg/m&lt;sup&gt;3&lt;/sup&gt;

Overview of the Second Texas Air Quality Study (TexAQS II) and the Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS)

The Second Texas Air Quality Study (TexAQS II) was conducted in eastern Texas during 2005 and 2006. This 2-year study included an intensive field campaign, TexAQS 2006/Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS), conducted in August–October 2006. The results reported in this special journal section are based on observations collected on four aircraft, one research vessel, networks of ground-based air quality and meteorological (surface and radar wind profiler) sites in eastern Texas, a balloon-borne ozonesonde-radiosonde network (part of Intercontinental Transport Experiment Ozonesonde Network Study (IONS-06)), and satellites. This overview paper provides operational and logistical information for those platforms and sites, summarizes the principal findings and conclusions that have thus far been drawn from the results, and directs readers to appropriate papers for the full analysis. Two of these findings deserve particular emphasis. First, despite decreases in actual emissions of highly reactive volatile organic compounds (HRVOC) and some improvements in inventory estimates since the TexAQS 2000 study, the current Houston area emission inventories still underestimate HRVOC emissions by approximately 1 order of magnitude. Second, the background ozone in eastern Texas, which represents the minimum ozone concentration that is likely achievable through only local controls, can approach or exceed the current National Ambient Air Quality Standard of 75 ppbv for an 8-h average. These findings have broad implications for air quality control strategies in eastern Texas