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Modini, RL, Frossard AA, Ahlm L, Russell LM, Corrigan CE, Roberts GC, Hawkins LN, Schroder JC, Bertram AK, Zhao R, Lee AKY, Abbatt JPD, Lin J, Nenes A, Wang Z, Wonaschutz A, Sorooshian A, Noone KJ, Jonsson H, Seinfeld JH, Toom-Sauntry D, Macdonald AM, Leaitch WR.  2015.  Primary marine aerosol-cloud interactions off the coast of California. Journal of Geophysical Research-Atmospheres. 120:4282-4303.   10.1002/2014jd022963   AbstractWebsite

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 12m/s(1)) lasting 8 days, and 71cm(-3) during a period of higher wind speeds (average 16m/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 0.20.04% 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.

Collins, DB, Ault AP, Moffet RC, Ruppel MJ, Cuadra-Rodriguez LA, Guasco TL, Corrigan CE, Pedler BE, Azam F, Aluwihare LI, Bertram TH, Roberts GC, Grassian VH, Prather KA.  2013.  Impact of marine biogeochemistry on the chemical mixing state and cloud forming ability of nascent sea spray aerosol. Journal of Geophysical Research-Atmospheres. 118:8553-8565.   10.1002/jgrd.50598   AbstractWebsite

The composition and properties of sea spray aerosol, a major component of the atmosphere, are often controlled by marine biological activity; however, the scope of impacts that ocean chemistry has on the ability for sea spray aerosol to act as cloud condensation nuclei (CCN) is not well understood. In this study, we utilize a mesocosm experiment to investigate the impact of marine biogeochemical processes on the composition and mixing state of sea spray aerosol particles with diameters<0.2 mu m produced by controlled breaking waves in a unique ocean-atmosphere facility. An increase in relative abundance of a distinct, insoluble organic particle type was observed after concentrations of heterotrophic bacteria increased in the seawater, leading to an 86 +/- 5% reduction in the hygroscopicity parameter () at 0.2% supersaturation. Aerosol size distributions showed very little change and the submicron organic mass fraction increased by less than 15% throughout the experiment; as such, neither of these typical metrics can explain the observed reduction in hygroscopicity. Predictions of the hygroscopicity parameter that make the common assumption that all particles have the same bulk organic volume fractions lead to overpredictions of CCN concentrations by 25% in these experiments. Importantly, key changes in sea spray aerosol mixing state that ultimately influenced CCN activity were driven by bacteria-mediated alterations to the organic composition of seawater.

Russell, LM, Sorooshian A, Seinfeld JH, Albrecht BA, Nenes A, Ahlm L, Chen YC, Coggon M, Craven JS, Flagan RC, Frossard AA, Jonsson H, Jung E, Lin JJ, Metcalf AR, Modini R, Mulmenstadt J, Roberts GC, Shingler T, Song S, Wang Z, Wonaschutz A.  2013.  Eastern Pacific emitted aerosol cloud experiment. Bulletin of the American Meteorological Society. 94:709-+.   10.1175/bams-d-12-00015.1   AbstractWebsite

Aerosol-cloud-radiation interactions are widely held to be the largest single source of uncertainty in climate model projections of future radiative forcing due to increasing anthropogenic emissions. The underlying causes of this uncertainty among modeled predictions of climate are the gaps in our fundamental understanding of cloud processes. There has been significant progress with both observations and models in addressing these important questions but quantifying them correctly is nontrivial, thus limiting our ability to represent them in global climate models. The Eastern Pacific Emitted Aerosol Cloud Experiment (E-PEACE) 2011 was a targeted aircraft campaign with embedded modeling studies, using the Center for Interdisciplinary Remotely-Piloted Aircraft Studies (CIRPAS) Twin Otter aircraft and the research vessel Point Sur in July and August 2011 off the central coast of California, with a full payload of instruments to measure particle and cloud number, mass, composition, and water uptake distributions. E-PEACE used three emitted particle sources to separate particle-induced feedbacks from dynamical variability, namely 1) shipboard smoke-generated particles with 0.05-1-mu m diameters (which produced tracks measured by satellite and had drop composition characteristic of organic smoke), 2) combustion particles from container ships with 0.05-0.2-mu m diameters (which were measured in a variety of conditions with droplets containing both organic and sulfate components), and 3) aircraft-based milled salt particles with 3-5-mu m diameters (which showed enhanced drizzle rates in some clouds). The aircraft observations were consistent with past large-eddy simulations of deeper clouds in ship tracks and aerosol cloud parcel modeling of cloud drop number and composition, providing quantitative constraints on aerosol effects on warm-cloud microphysics.

Creamean, JM, Ault AP, Ten Hoeve JE, Jacobson MZ, Roberts GC, Prather KA.  2011.  Measurements of aerosol chemistry during new particle formation events at a remote rural mountain site. Environmental Science & Technology. 45:8208-8216.   10.1021/es103692f   AbstractWebsite

Determining the major sources of particles that act as cloud condensation nuclei (CCN) represents a critical step in the development of a more fundamental understanding of aerosol impacts on cloud formation and climate. Reported herein are direct measurements of the CCN activity of newly formed ambient particles, measured at a remote rural site in the Sierra Nevada Mountains of Northern California. Nucleation events in the winter of 2009 occurred during two pristine periods following precipitation, with higher gas-phase SO(2) concentrations during the second period, when faster particle growth occurred (7-8 nm/h). Amines, as opposed to ammonia, and sulfate were detected in the particle phase throughout new particle formation (NPF) events, increasing in number as the particles grew to larger sizes. Interestingly, long-range transport of SO(2) from Asia appeared to potentially play a role in NPF during faster particle growth. Understanding the propensity of newly formed particles to act as CCN is critical for predicting the effects of NPF on orographic cloud formation during winter storms along the Sierra Nevada Mountain range. The potential impact of newly formed particles in remote regions needs to be compared with that of transported urban aerosols when evaluating the impact of aerosols on clouds and climate.

Sullivan, RC, Moore MJK, Petters MD, Kreidenweis SM, Roberts GC, Prather KA.  2009.  Timescale for hygroscopic conversion of calcite mineral particles through heterogeneous reaction with nitric acid. Physical Chemistry Chemical Physics. 11:7826-7837.   10.1039/b904217b   AbstractWebsite

Atmospheric heterogeneous reactions can potentially change the hygroscopicity of atmospheric aerosols as they undergo chemical aging processes in the atmosphere. A particle's hygroscopicity influences its cloud condensation nuclei (CCN) properties with potential impacts on cloud formation and climate. In this study, size-selected calcite mineral particles were reacted with controlled amounts of nitric acid vapour over a wide range of relative humidities in an aerosol flow tube to study the conversion of insoluble and thus apparently non-hygroscopic calcium carbonate into soluble and hygroscopic calcium nitrate. The rate of hygroscopic change particles undergo during a heterogeneous reaction is derived from experimental measurements for the first time. The chemistry of the reacted particles was determined using an ultra. ne aerosol time-of-flight mass spectrometer (UF-ATOFMS) while the particles' hygroscopicity was determined through measuring CCN activation curves fit to a single parameter of hygroscopicity, kappa. The reaction is rapid, corresponding to atmospheric timescales of hours. At low to moderate HNO(3) exposures, the increase in the hygroscopicity of the particles is a linear function of the HNO(3)(g) exposure. The experimentally observed conversion rate was used to constrain a simple but accurate kinetic model. This model predicts that calcite particles will be rapidly converted into hygroscopic particles (kappa > 0.1) within 4 h for low HNO(3) mixing ratios (10 pptv) and in less than 3 min for 1000 pptv HNO(3). This suggests that the hygroscopic conversion of the calcite component of atmospheric mineral dust aerosol will be controlled by the availability of nitric acid and similar reactants, and not by the atmospheric residence time.

VanReken, TM, Rissman TA, Roberts GC, Varutbangkul V, Jonsson HH, Flagan RC, Seinfeld JH.  2003.  Toward aerosol/cloud condensation nuclei (CCN) closure during CRYSTAL-FACE. Journal of Geophysical Research-Atmospheres. 108   10.1029/2003jd003582   AbstractWebsite

[1] During July 2002, measurements of cloud condensation nuclei were made in the vicinity of southwest Florida as part of the Cirrus Regional Study of Tropical Anvils and Cirrus Layers-Florida Area Cirrus Experiment (CRYSTAL-FACE) field campaign. These observations, at supersaturations of 0.2 and 0.85%, are presented here. The performance of each of the two CCN counters was validated through laboratory calibration and an in situ intercomparison. The measurements indicate that the aerosol sampled during the campaign was predominantly marine in character: the median concentrations were 233 cm(-3) (at S = 0.2%) and 371 cm(-3) (at S = 0.85%). Three flights during the experiment differed from this general trend; the aerosol sampled during the two flights on 18 July was more continental in character, and the observations on 28 July indicate high spatial variability and periods of very high aerosol concentrations. This study also includes a simplified aerosol/CCN closure analysis. Aerosol size distributions were measured simultaneously with the CCN observations, and these data are used to predict a CCN concentration using Kohler theory. For the purpose of this analysis, an idealized composition of pure ammonium sulfate was assumed. The analysis indicates that in this case, there was good general agreement between the predicted and observed CCN concentrations: at S = 0.2%, N-predicted/N-observed = 1.047 (R-2 = 0.911); at S = 0.85%, N-predicted/N-observed = 1.201 (R-2 = 0.835). The impacts of the compositional assumption and of including in-cloud data in the analysis are addressed. The effect of removing the data from the 28 July flight is also examined; doing so improves the result of the closure analysis at S = 0.85%. When omitting that atypical flight, N-predicted/N-observed = 1.085 (R-2 = 0.770) at S = 0.85%.