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

Influence of transport and ocean ice extent on biogenic aerosol sulfur in the Arctic atmosphere

The recent decline in sea ice cover in the Arctic Ocean could affect the regional radiative forcing via changes in sea ice-atmosphere exchange of dimethyl sulfide (DMS) and biogenic aerosols formed from its atmospheric oxidation, such as methanesulfonic acid (MSA). This study examines relationships between changes in total sea ice extent north of 70 degrees N and atmospheric MSA measurement at Alert, Nunavut, during 1980-2009; at Barrow, Alaska, during 1997-2008; and at Ny-Alesund, Svalbard, for 1991-2004. During the 1980-1989 and 1990-1997 periods, summer (July-August) and June MSA concentrations at Alert decreased. In general, MSA concentrations increased at all locations since 2000 with respect to 1990 values, specifically during June and summer at Alert and in summer at Barrow and Ny-Alesund. Our results show variability in MSA at all sites is related to changes in the source strengths of DMS, possibly linked to changes in sea ice extent as well as to changes in atmospheric transport patterns. Since 2000, a late spring increase in atmospheric MSA at the three sites coincides with the northward migration of the marginal ice edge zone where high DMS emissions from ocean to atmosphere have previously been reported. Significant negative correlations are found between sea ice extent and MSA concentrations at the three sites during the spring and June. These results suggest that a decrease in seasonal ice cover influencing other mechanisms of DMS production could lead to higher atmospheric MSA concentrations

Primary marine aerosol-cloud interactions off the coast of California

Primary marine aerosol (PMA)-cloud interactions off the coast of California were investigated using observations of marine aerosol, cloud condensation nuclei (CCN), and stratocumulus clouds during the Eastern Pacific Emitted Aerosol Cloud Experiment (E-PEACE) and the Stratocumulus Observations of Los-Angeles Emissions Derived Aerosol-Droplets (SOLEDAD) studies. Based on recently reported measurements of PMA size distributions, a constrained lognormal-mode-fitting procedure was devised to isolate PMA number size distributions from total aerosol size distributions and applied to E-PEACE measurements. During the 12 day E-PEACE cruise on the R/V Point Sur, PMA typically contributed less than 15% of total particle concentrations. PMA number concentrations averaged 12 cm^(−3) during a relatively calmer period (average wind speed 12 m/s^1) lasting 8 days, and 71 cm^(−3) during a period of higher wind speeds (average 16 m/s^1) lasting 5 days. On average, PMA contributed less than 10% of total CCN at supersaturations up to 0.9% during the calmer period; however, during the higher wind speed period, PMA comprised 5–63% of CCN (average 16–28%) at supersaturations less than 0.3%. Sea salt was measured directly in the dried residuals of cloud droplets during the SOLEDAD study. The mass fractions of sea salt in the residuals averaged 12 to 24% during three cloud events. Comparing the marine stratocumulus clouds sampled in the two campaigns, measured peak supersaturations were 0.2 ± 0.04% during E-PEACE and 0.05–0.1% during SOLEDAD. The available measurements show that cloud droplet number concentrations increased with >100 nm particles in E-PEACE but decreased in the three SOLEDAD cloud events

Biogenic oxidized organic functional groups in aerosol particles from a mountain forest site and their similarities to laboratory chamber products

Submicron particles collected at Whistler, British Columbia, at 1020 m a.s.l. during May and June 2008 on Teflon filters were analyzed by Fourier transform infrared (FTIR) and X-ray fluorescence (XRF) techniques for organic functional groups (OFG) and elemental composition. Organic mass (OM) concentrations ranged from less than 0.5 to 3.1 μg m<sup>−3</sup>, with a project mean and standard deviation of 1.3±1.0 μg m<sup>−3</sup> and 0.21±0.16 μg m<sup>−3</sup> for OM and sulfate, respectively. On average, organic hydroxyl, alkane, and carboxylic acid groups represented 34%, 33%, and 23% of OM, respectively. Ketone, amine and organosulfate groups constituted 6%, 5%, and <1% of the average organic aerosol composition, respectively. Measurements of volatile organic compounds (VOC), including isoprene and monoterpenes from biogenic VOC (BVOC) emissions and their oxidation products (methyl-vinylketone / methacrolein, MVK/MACR), were made using co-located proton transfer reaction mass spectrometry (PTR-MS). We present chemically-specific evidence of OFG associated with BVOC emissions. Positive matrix factorization (PMF) analysis attributed 65% of the campaign OM to biogenic sources, based on the correlations of one factor to monoterpenes and MVK/MACR. The remaining fraction was attributed to anthropogenic sources based on a correlation to sulfate. The functional group composition of the biogenic factor (consisting of 32% alkane, 25% carboxylic acid, 21% organic hydroxyl, 16% ketone, and 6% amine groups) was similar to that of secondary organic aerosol (SOA) reported from the oxidation of BVOCs in laboratory chamber studies, providing evidence that the magnitude and chemical composition of biogenic SOA simulated in the laboratory is similar to that found in actual atmospheric conditions. The biogenic factor OM is also correlated to dust elements, indicating that dust may act as a non-acidic SOA sink. This role is supported by the organic functional group composition and morphology of single particles, which were analyzed by scanning transmission X-ray microscopy near edge X-ray absorption fine structure (STXM-NEXAFS)

Cloud partitioning of isocyanic acid (HNCO) and evidence of secondary source of HNCO in ambient air

Although isocyanic acid (HNCO) may cause a variety of health issues via protein carbamylation and has been proposed as a key compound in smoke-related health issues, our understanding of the atmospheric sources and fate of this toxic compound is currently incomplete. To address these issues, a field study was conducted at Mount Soledad, La Jolla, CA, to investigate partitioning of HNCO to clouds and fogs using an Acetate Chemical Ionization Mass Spectrometer coupled to a ground-based counterflow virtual impactor. The first field evidence of cloud partitioning of HNCO is presented, demonstrating that HNCO is dissolved in cloudwater more efficiently than expected based on the effective Henry's law solubility. The measurements also indicate evidence for a secondary, photochemical source of HNCO in ambient air at this site. Key PointsThe first field observation of cloud scavenging of isocyanic acid (HNCO)HNCO may be partitioning to clouds more efficiently than expectedA secondary, photochemical source of HNCO is observe

Cloud albedo increase from carbonaceous aerosol

Airborne measurements from two consecutive days, analysed with the aid of an aerosol-adiabatic cloud parcel model, are used to study the effect of carbonaceous aerosol particles on the reflectivity of sunlight by water clouds. The measurements, including aerosol chemistry, aerosol microphysics, cloud microphysics, cloud gust velocities and cloud light extinction, were made below, in and above stratocumulus over the northwest Atlantic Ocean. On the first day, the history of the below-cloud fine particle aerosol was marine and the fine particle sulphate and organic carbon mass concentrations measured at cloud base were 2.4 \u3bcg m 123 and 0.9 \u3bcg m 123 respectively. On the second day, the below-cloud aerosol was continentally influenced and the fine particle sulphate and organic carbon mass concentrations were 2.3 \u3bcg m 123 and 2.6 \u3bcg m 123 respectively. Over the range 0.06\u20130.8 \u3bcm diameter, the shapes of the below-cloud size distributions were similar on both days and the number concentrations were approximately a factor of two higher on the second day. The cloud droplet number concentrations (CDNC) on the second day were approximately three times higher than the CDNC measured on the first day. Using the parcel model to separate the influence of the differences in gust velocities, we estimate from the vertically integrated cloud light scattering measurements a 6% increase in the cloud albedo principally due to the increase in the carbonaceous components on the second day. Assuming no additional absorption by this aerosol, a 6% albedo increase translates to a local daytime radiative cooling of 3c12 W m 122. This result provides observational evidence that the role of anthropogenic carbonaceous components in the cloud albedo effect can be much larger than that of anthropogenic sulphate, as some global simulations have indicated.Peer reviewed: YesNRC publication: Ye