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Calmer, R, Roberts GC, Preissler J, Sanchez KJ, Derrien S, O'Dowd C.  2018.  Vertical wind velocity measurements using a five-hole probe with remotely piloted aircraft to study aerosol-cloud interactions. Atmospheric Measurement Techniques. 11:2583-2599.   10.5194/amt-11-2583-2018   AbstractWebsite

The importance of vertical wind velocities (in particular positive vertical wind velocities or updrafts) in atmospheric science has motivated the need to deploy multi-hole probes developed for manned aircraft in small remotely piloted aircraft (RPA). In atmospheric research, lightweight RPAs ( < 2.5 kg) are now able to accurately measure atmospheric wind vectors, even in a cloud, which provides essential observing tools for understanding aerosol-cloud interactions. The European project BACCHUS (impact of Biogenic versus Anthropogenic emissions on Clouds and Climate: towards a Holistic UnderStanding) focuses on these specific interactions. In particular, vertical wind velocity at cloud base is a key parameter for studying aerosol-cloud interactions. To measure the three components of wind, a RPA is equipped with a five-hole probe, pressure sensors, and an inertial navigation system (INS). The five-hole probe is calibrated on a multi-axis platform, and the probe-INS system is validated in a wind tunnel. Once mounted on a RPA, power spectral density (PSD) functions and turbulent kinetic energy (TKE) derived from the five-hole probe are compared with sonic anemometers on a meteorological mast. During a BACCHUS field campaign at Mace Head Atmospheric Research Station (Ireland), a fleet of RPAs was deployed to profile the atmosphere and complement ground-based and satellite observations of physical and chemical properties of aerosols, clouds, and meteorological state parameters. The five-hole probe was flown on straight-and-level legs to measure vertical wind velocities within clouds. The vertical velocity measurements from the RPA are validated with vertical velocities derived from a ground-based cloud radar by showing that both measurements yield model-simulated cloud droplet number concentrations within 10 %. The updraft velocity distributions illustrate distinct relationships between vertical cloud fields in different meteorological conditions.

Crispel, P, Roberts G.  2018.  All-sky photogrammetry techniques to georeference a cloud field. Atmospheric Measurement Techniques. 11:593-609.   10.5194/amt-11-593-2018   AbstractWebsite

In this study, we present a novel method of identifying and geolocalizing cloud field elements from a portable all-sky camera stereo network based on the ground and oriented towards zenith. The methodology is mainly based on stereophotogrammetry which is a 3-D reconstruction technique based on triangulation from corresponding stereo pixels in rectified images. In cases where clouds are horizontally separated, identifying individual positions is performed with segmentation techniques based on hue filtering and contour detection algorithms. Macroscopic cloud field characteristics such as cloud layer base heights and velocity fields are also deduced. In addition, the methodology is fitted to the context of measurement campaigns which impose simplicity of implementation, auto-calibration, and portability. Camera internal geometry models are achieved a priori in the laboratory and validated to ensure a certain accuracy in the peripheral parts of the all-sky image. Then, stereophotogrammetry with dense 3-D reconstruction is applied with cameras spaced 150m apart for two validation cases. The first validation case is carried out with cumulus clouds having a cloud base height at 1500ma. g.l. The second validation case is carried out with two cloud layers: a cumulus fractus layer with a base height at 1000ma. g.l. and an altocumulus stratiformis layer with a base height of 2300ma. g.l. Velocity fields at cloud base are computed by tracking image rectangular patterns through successive shots. The height uncertainty is estimated by comparison with a Vaisala CL31 ceilometer located on the site. The uncertainty on the horizontal coordinates and on the velocity field are theoretically quantified by using the experimental uncertainties of the cloud base height and camera orientation. In the first cumulus case, segmentation of the image is performed to identify individuals clouds in the cloud field and determine the horizontal positions of the cloud centers.

Sanchez, KJ, Roberts GC, Calmer R, Nicoll K, Hashimshoni E, Rosenfeld D, Ovadnevaite J, Preissler J, Ceburnis D, O'Dowd C, Russell LM.  2017.  Top-down and bottom-up aerosol-cloud closure: towards understanding sources of uncertainty in deriving cloud shortwave radiative flux. Atmospheric Chemistry and Physics. 17:9797-9814.   10.5194/acp-17-9797-2017   AbstractWebsite

Top-down and bottom-up aerosol-cloud shortwave radiative flux closures were conducted at the Mace Head Atmospheric Research Station in Galway, Ireland, in August 2015. This study is part of the BACCHUS (Impact of Biogenic versus Anthropogenic emissions on Clouds and Climate: towards a Holistic UnderStanding) European collaborative project, with the goal of understanding key processes affecting aerosol-cloud shortwave radiative flux closures to improve future climate predictions and develop sustainable policies for Europe. Instrument platforms include ground-based unmanned aerial vehicles (UAVs)(1) and satellite measurements of aerosols, clouds and meteorological variables. The ground-based and airborne measurements of aerosol size distributions and cloud condensation nuclei (CCN) concentration were used to initiate a 1-D microphysical aerosol-cloud parcel model (ACPM). UAVs were equipped for a specific science mission, with an optical particle counter for aerosol distribution profiles, a cloud sensor to measure cloud extinction or a five-hole probe for 3D wind vectors. UAV cloud measurements are rare and have only become possible in recent years through the miniaturization of instrumentation. These are the first UAV measurements at Mace Head. ACPM simulations are compared to in situ cloud extinction measurements from UAVs to quantify closure in terms of cloud shortwave radiative flux. Two out of seven cases exhibit sub-adiabatic vertical temperature profiles within the cloud, which suggests that entrainment processes affect cloud microphysical properties and lead to an overestimate of simulated cloud shortwave radiative flux. Including an entrainment parameterization and explicitly calculating the entrainment fraction in the ACPM simulations both improved cloud-top radiative closure. Entrainment reduced the difference between simulated and observation-derived cloud-top shortwave radiative flux (delta RF) by between 25 and 60Wm(-2). After accounting for entrainment, satellite-derived cloud droplet number concentrations (CDNCs) were within 30% of simulated CDNC. In cases with a well-mixed boundary layer, delta RF is no greater than 20Wm(-2) after accounting for cloud-top entrainment and up to 50Wm(-2) when entrainment is not taken into account. In cases with a decoupled boundary layer, cloud microphysical properties are inconsistent with ground-based aerosol measurements, as expected, and delta RF is as high as 88Wm(-2), even high (> 30Wm(-2)) after accounting for cloud-top entrainment. This work demonstrates the need to take in situ measurements of aerosol properties for cases where the boundary layer is decoupled as well as consider cloud-top entrainment to accurately model stratocumulus cloud radiative flux.

Claeys, M, Roberts G, Mallet M, Arndt J, Sellegri K, Sciare J, Wenger J, Sauvage B.  2017.  Optical, physical and chemical properties of aerosols transported to a coastal site in the western Mediterranean: a focus on primary marine aerosols. Atmospheric Chemistry and Physics. 17:7891-7915.   10.5194/acp-17-7891-2017   AbstractWebsite

As part of the ChArMEx-ADRIMED campaign (summer 2013), ground-based in situ observations were conducted at the Ersa site (northern tip of Corsica; 533 m a.s.l.) to characterise the optical, physical and chemical properties of aerosols. During the observation period, a major influence of primary marine aerosols was detected (22-26 June), with a mass concentration reaching up to 6.5 mu g m(-3) and representing more than 40% of the total PM10 mass concentration. Its relatively low ratio of chloride to sodium (average of 0.57) indicates a fairly aged sea salt aerosol at Ersa. In this work, an original data set, obtained from online real-time instruments (ATOFMS, PILS-IC) has been used to characterise the ageing of primary marine aerosols (PMAs). During this PMA period, the mixing of fresh and aged PMAs was found to originate from both local and regional (Gulf of Lion) emissions, according to local wind measurements and FLEXPART back trajectories. Two different aerosol regimes have been identified: a dust outbreak (dust) originating from Algeria/Tunisia, and a pollution period with aerosols originating from eastern Europe, which includes anthropogenic and biomass burning sources (BBP). The optical, physical and chemical properties of the observed aerosols, as well as their local shortwave (SW) direct radiative effect (DRE) in clear-sky conditions, are compared for these three periods in order to assess the importance of the direct radiative impact of PMAs compared to other sources above the western Mediterranean Basin. As expected, AERONET retrievals indicate a relatively low local SW DRF during the PMA period with mean values of -11 +/- 4 at the surface and -8 +/- 3W m(-2) at the top of the atmosphere (TOA). In comparison, our results indicate that the dust outbreak observed at our site during the campaign, although of moderate intensity (AOD of 0.3-0.4 at 440 nm and column-integrated SSA of 0.90-0.95), induced a local instantaneous SW DRF that is nearly 3 times the effect calculated during the PMA period, with maximum values up to -40 W m(-2) at the surface. A similar range of values were found for the BBP period to those during the dust period (SW DRF at the surface and TOA of -23 +/- 6 and -15 +/- 4 W m(-2) respectively). The multiple sources of measurements at Ersa allowed the detection of a PMA-dominant period and their characterisation in terms of ageing, origin, transport, optical and physical properties and direct climatic impact.

Arndt, J, Sciare J, Mallet M, Roberts GC, Marchand N, Sartelet K, Sellegri K, Dulac F, Healy RM, Wenger JC.  2017.  Sources and mixing state of summertime background aerosol in the north-western Mediterranean basin. Atmospheric Chemistry and Physics. 17:6975-7001.   10.5194/acp-17-6975-2017   AbstractWebsite

An aerosol time-of-flight mass spectrometer (ATOFMS) was employed to provide real-time single particle mixing state and thereby source information for aerosols impacting the western Mediterranean basin during the ChArMEx-ADRIMED and SAF-MED campaigns in summer 2013. The ATOFMS measurements were made at a ground-based remote site on the northern tip of Corsica. Twenty-seven distinct ATOFMS particle classes were identified and subsequently grouped into eight general categories: EC-rich (elemental carbon), K-rich, Na-rich, amines, OC-rich (organic carbon), V-rich, Fe-rich and Ca-rich particles. Mass concentrations were reconstructed for the ATOFMS particle classes and found to be in good agreement with other co-located quantitative measurements (PM1, black carbon (BC), organic carbon, sulfate mass and ammonium mass). Total ATOFMS reconstructed mass (PM2.5) accounted for 70-90% of measured PM10 mass and was comprised of regionally transported fossil fuel (EC-rich) and biomass burning (K-rich) particles. The accumulation of these transported particles was favoured by repeated and extended periods of air mass stagnation over the western Mediterranean during the sampling campaigns. The single particle mass spectra proved to be valuable source markers, allowing the identification of fossil fuel and biomass burning combustion sources, and was therefore highly complementary to quantitative measurements made by Particle into Liquid Sampler ion chromatography (PILS-IC) and an aerosol chemical speciation monitor (ACSM), which have demonstrated that PM1 and PM10 were comprised predominantly of sulfate, ammonium and OC. Good temporal agreement was observed between ATOFMS EC-rich and K-rich particle mass concentrations and combined mass concentrations of BC, sulfate, ammonium and low volatility oxygenated organic aerosol (LV-OOA). This combined information suggests that combustion of fossil fuels and biomass produced primary EC- and OC-containing particles, which then accumulated ammonium, sulfate and alkylamines during regional transport. Three other sources were also identified: local biomass burning, marine and shipping. Local combustion particles

Ovadnevaite, J, Zuend A, Laaksonen A, Sanchez KJ, Roberts G, Ceburnis D, Decesari S, Rinaldi M, Hodas N, Facchini MC, Seinfeld JH, Dowd CO.  2017.  Surface tension prevails over solute effect in organic-influenced cloud droplet activation. Nature. 546:637-641.   10.1038/nature22806   AbstractWebsite

The spontaneous growth of cloud condensation nuclei (CCN) into cloud droplets under supersaturated water vapour conditions is described by classic Kohler theory(1,2). This spontaneous activation of CCN depends on the interplay between the Raoult effect, whereby activation potential increases with decreasing water activity or increasing solute concentration, and the Kelvin effect, whereby activation potential decreases with decreasing droplet size or increases with decreasing surface tension, which is sensitive to surfactants(1). Surface tension lowering caused by organic surfactants, which diminishes the Kelvin effect, is expected to be negated by a concomitant reduction in the Raoult effect, driven by the displacement of surfactant molecules from the droplet bulk to the droplet-vapour interface(3,4). Here we present observational and theoretical evidence illustrating that, in ambient air, surface tension lowering can prevail over the reduction in the Raoult effect, leading to substantial increases in cloud droplet concentrations. We suggest that consideration of liquid-liquid phase separation, leading to complete or partial engulfing of a hygroscopic particle core by a hydrophobic organic-rich phase, can explain the lack of concomitant reduction of the Raoult effect, while maintaining substantial lowering of surface tension, even for partial surface coverage. Apart from the importance of particle size and composition in droplet activation, we show by observation and modelling that incorporation of phase-separation effects into activation thermodynamics can lead to a CCN number concentration that is up to ten times what is predicted by climate models, changing the properties of clouds. An adequate representation of the CCN activation process is essential to the prediction of clouds in climate models, and given the effect of clouds on the Earth's energy balance, improved prediction of aerosol-cloud-climate interactions is likely to result in improved assessments of future climate change.

Wex, H, Dieckmann K, Roberts GC, Conrath T, Izaguirre MA, Hartmann S, Herenz P, Schafer M, Ditas F, Schmeissner T, Henning S, Wehner B, Siebert H, Stratmann F.  2016.  Aerosol arriving on the Caribbean island of Barbados: physical properties and origin. Atmospheric Chemistry and Physics. 16:14107-14130.   10.5194/acp-16-14107-2016   AbstractWebsite

The marine aerosol arriving at Barbados (Ragged Point) was characterized during two 3-week long measurement periods in November 2010 and April 2011, in the context of the measurement campaign CARRIBA (Cloud, Aerosol, Radiation and tuRbulence in the trade wInd regime over BArbados). Through a comparison between ground-based and airborne measurements it was shown that the former are representative of the marine boundary layer at least up to cloud base. In general, total particle number concentrations (N-total) ranged from as low as 100 up to 800 cm(-3), while number concentrations for cloud condensation nuclei (N-CCN) at a supersaturation of 0.26% ranged from some 10 to 600 cm(-3). N-total and N-CCN depended on the air mass origin. Three distinct types of air masses were found. One type showed elevated values for both N-total and N-CCN and could be attributed to long-range transport from Africa, by which biomass burning particles from the Sahel region and/or mineral dust particles from the Sahara were advected. The second and third type both had values for N-CCN below 200 cm(-3) and a clear minimum in the particle number size distribution (NSD) around 70 to 80 nm (Hoppel minimum). While for one of these two types the accumulation mode was dominating (albeit less so than for air masses advected from Africa), the Aitken mode dominated the other and contributed more than 50% of all particles. These Aitken mode particles likely were formed by new particle formation no more than 3 days prior to the measurements. Hygroscopicity of particles in the CCN size range was determined from CCN measurements to be kappa = 0.66 on average, which suggests that these particles contain mainly sulfate and do not show a strong influence from organic material, which might generally be the case for the months during which measurements were made. The average kappa could be used to derive N-CCN from measured number size distributions, showing that this is a valid approach to obtain N-CCN. Although the total particulate mass sampled on filters was found to be dominated by Na+ and Cl-, this was found to be contributed by a small number of large particles (> 500 nm, mostly even in the super-micron size range). Based on a three-modal fit, a sea spray mode observed in the NSDs was found to contribute 90% to the total particulate mass but only 4 to 10% to N-total and up to 15% to N-CCN. This is in accordance with finding no correlation between N-total and wind speed.

Sanchez, KJ, Russell LM, Modini RL, Frossard AA, Ahlm L, Corrigan CE, Roberts GC, Hawkins LN, Schroder JC, Bertram AK, Zhao R, Lee AKY, Lin JJ, Nenes A, Wang Z, Wonaschutz A, Sorooshian A, Noone KJ, Jonsson H, Toom D, Macdonald AM, Leaitch WR, Seinfeld JH.  2016.  Meteorological and aerosol effects on marine cloud microphysical properties. Journal of Geophysical Research-Atmospheres. 121:4142-4161.   10.1002/2015jd024595   AbstractWebsite

Meteorology and microphysics affect cloud formation, cloud droplet distributions, and shortwave reflectance. The Eastern Pacific Emitted Aerosol Cloud Experiment and the Stratocumulus Observations of Los-Angeles Emissions Derived Aerosol-Droplets studies provided measurements in six case studies of cloud thermodynamic properties, initial particle number distribution and composition, and cloud drop distribution. In this study, we use simulations from a chemical and microphysical aerosol-cloud parcel (ACP) model with explicit kinetic drop activation to reproduce observed cloud droplet distributions of the case studies. Four cases had subadiabatic lapse rates, resulting in fewer activated droplets, lower liquid water content, and higher cloud base height than an adiabatic lapse rate. A weighted ensemble of simulations that reflect measured variation in updraft velocity and cloud base height was used to reproduce observed droplet distributions. Simulations show that organic hygroscopicity in internally mixed cases causes small effects on cloud reflectivity (CR) (<0.01), except for cargo ship and smoke plumes, which increased CR by 0.02 and 0.07, respectively, owing to their high organic mass fraction. Organic hygroscopicity had larger effects on droplet concentrations for cases with higher aerosol concentrations near the critical diameter (namely, polluted cases with a modal peak near 0.1 mu m). Differences in simulated droplet spectral widths (k) caused larger differences in CR than organic hygroscopicity in cases with organic mass fractions of 60% or less for the cases shown. Finally, simulations from a numerical parameterization of cloud droplet activation suitable for general circulation models compared well with the ACP model, except under high organic mass fraction.

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.

Hammer, E, Gysel M, Roberts GC, Elias T, Hofer J, Hoyle CR, Bukowiecki N, Dupont JC, Burnet F, Baltensperger U, Weingartner E.  2014.  Size-dependent particle activation properties in fog during the ParisFog 2012/13 field campaign. Atmospheric Chemistry and Physics. 14:10517-10533.   10.5194/acp-14-10517-2014   AbstractWebsite

Fog-induced visibility reduction is responsible for a variety of hazards in the transport sector. Therefore there is a large demand for an improved understanding of fog formation and thus improved forecasts. Improved fog forecasts require a better understanding of the numerous complex mechanisms during the fog life cycle. During winter 2012/13 a field campaign called ParisFog aiming at fog research took place at SIRTA (Instrumented Site for Atmospheric Remote Sensing Research). SIRTA is located about 20 km southwest of the Paris city center, France, in a semi-urban environment. In situ activation properties of the prevailing fog were investigated by measuring (1) total and interstitial (non-activated) dry particle number size distributions behind two different inlet systems; (2) interstitial hydrated aerosol and fog droplet size distributions at ambient conditions; and (3) cloud condensation nuclei (CCN) number concentration at different supersaturations (SS) with a CCN counter. The aerosol particles were characterized regarding their hygroscopic properties, fog droplet activation behavior and contribution to light scattering for 17 developed fog events. Low particle hygroscopicity with an overall median of the hygroscopicity parameter, kappa, of 0.14 was found, likely caused by substantial influence from local traffic and wood burning emissions. Measurements of the aerosol size distribution at ambient RH re-vealed that the critical wet diameter, above which the hydrated aerosols activate to fog droplets, is rather large (with a median value of 2.6 mu m) and is highly variable (ranging from 1 to 5 mu m) between the different fog events. Thus, the number of activated fog droplets was very small and the nonactivated hydrated particles were found to contribute significantly to the observed light scattering and thus to the reduction in visibility. Combining all experimental data, the effective peak supersaturation, SSpeak, a measure of the peak supersaturation during the fog formation, was determined. The median SSpeak value was estimated to be in the range from 0.031 to 0.046% (upper and lower limit estimations), which is in good agreement with previous experimental and modeling studies of fog.

Werner, F, Ditas F, Siebert H, Simmel M, Wehner B, Pilewskie P, Schmeissner T, Shaw RA, Hartmann S, Wex H, Roberts GC, Wendisch M.  2014.  Twomey effect observed from collocated microphysical and remote sensing measurements over shallow cumulus. Journal of Geophysical Research-Atmospheres. 119:1534-1545.   10.1002/2013jd020131   AbstractWebsite

Clear experimental evidence of the Twomey effect for shallow trade wind cumuli near Barbados is presented. Effective droplet radius (r(eff)) and cloud optical thickness (), retrieved from helicopter-borne spectral cloud-reflected radiance measurements, and spectral cloud reflectivity () are correlated with collocated in situ observations of the number concentration of aerosol particles from the subcloud layer (N). N denotes the concentration of particles larger than 80 nm in diameter and represents particles in the activation mode. In situ cloud microphysical and aerosol parameters were sampled by the Airborne Cloud Turbulence Observation System (ACTOS). Spectral cloud-reflected radiance data were collected by the Spectral Modular Airborne Radiation measurement sysTem (SMART-HELIOS). With increasing N a shift in the probability density functions of and toward larger values is observed, while the mean values and observed ranges of retrieved r(eff) decrease. The relative susceptibilities (RS) of r(eff), , and to N are derived for bins of constant liquid water path. The resulting values of RS are in the range of 0.35 for r(eff) and , and 0.27 for . These results are close to the maximum susceptibility possible from theory. Overall, the shallow cumuli sampled near Barbados show characteristics of homogeneous, plane-parallel clouds. Comparisons of RS derived from in situ measured r(eff) and from a microphysical parcel model are in close agreement.

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.

Juranyi, Z, Tritscher T, Gysel M, Laborde M, Gomes L, Roberts G, Baltensperger U, Weingartner E.  2013.  Hygroscopic mixing state of urban aerosol derived from size-resolved cloud condensation nuclei measurements during the MEGAPOLI campaign in Paris. Atmospheric Chemistry and Physics. 13:6431-6446.   10.5194/acp-13-6431-2013   AbstractWebsite

Ambient aerosols are a complex mixture of particles with different physical and chemical properties and consequently distinct hygroscopic behaviour. The hygroscopicity of a particle determines its water uptake at subsaturated relative humidity (RH) and its ability to form a cloud droplet at supersaturated RH. These processes influence Earth's climate and the atmospheric lifetime of the particles. Cloud condensation nuclei (CCN) number size distributions (i.e. CCN number concentrations as a function of dry particle diameter) were measured close to Paris during the MEGAPOLI campaign in January-February 2010, covering 10 different supersaturations (SS = 0.1-1.0%). The time-resolved hygroscopic mixing state with respect to CCN activation was also derived from these measurements. Simultaneously, a hygroscopicity tandem differential mobility analyser (HTDMA) was used to measure the hygroscopic growth factor (ratio of wet to dry mobility diameter) distributions at RH = 90%. The aerosol was highly externally mixed and its mixing state showed significant temporal variability. The average particle hygroscopicity was relatively low at subsaturation (RH = 90%; mean hygroscopicity parameter kappa = 0.12-0.27) and increased with increasing dry diameter in the range 35-265 nm. The mean kappa value, derived from the CCN measurements at supersaturation, ranged from 0.08 to 0.24 at SS = 1.0-0.1%. Two types of mixing-state resolved hygroscopicity closure studies were performed, comparing the water uptake ability measured below and above saturation. In the first type the CCN counter was connected in series with the HTDMA and and closure was achieved over the whole range of probed dry diameters, growth factors and supersaturations using the kappa-parametrization for the water activity and assuming surface tension of pure water in the Kohler theory. In the second closure type we compared hygroscopicity distributions derived from parallel monodisperse CCN measurements and HTDMA measurements. Very good agreement was found at all supersaturations, which shows that monodisperse CCN measurements are a reliable alternative to determine the hygroscopic mixing state of ambient aerosols.

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.

Siebert, H, Beals M, Bethke J, Bierwirth E, Conrath T, Dieckmann K, Ditas F, Ehrlich A, Farrell D, Hartmann S, Izaguirre MA, Katzwinkel J, Nuijens L, Roberts G, Schafer M, Shaw RA, Schmeissner T, Serikov I, Stevens B, Stratmann F, Wehner B, Wendisch M, Werner F, Wex H.  2013.  The fine-scale structure of the trade wind cumuli over Barbados - an introduction to the CARRIBA project. Atmospheric Chemistry and Physics. 13:10061-10077.   10.5194/acp-13-10061-2013   AbstractWebsite

The CARRIBA (Cloud, Aerosol, Radiation and tuRbulence in the trade wInd regime over BArbados) project, focused on high resolution and collocated measurements of thermodynamic, turbulent, microphysical, and radiative properties of trade wind cumuli over Barbados, is introduced. The project is based on two one-month field campaigns in November 2010 (climatic wet season) and April 2011 (climatic dry season). Observations are based on helicopterborne and ground-based measurements in an area of 100 km(2) off the coast of Barbados. CARRIBA is accompanied by long-term observations at the Barbados Cloud Observatory located at the East coast of Barbados since early in 2010 and which provides a longer-term context for the CARRIBA measurements. The deployed instrumentation and sampling strategy are presented together with a classification of the meteorological conditions. The two campaigns were influenced by different air masses advected from the Caribbean area, the Atlantic Ocean, and the African continent which led to distinct aerosol conditions. Pristine conditions with low aerosol particle number concentrations of similar to 100 cm(3) were alternating with periods influenced by Saharan dust or aerosol from biomass burning resulting in comparably high number concentrations of similar to 500 cm(3). The biomass burning aerosol was originating from both the Caribbean area and Africa. The shallow cumulus clouds responded to the different aerosol conditions with a wide range of mean droplet sizes and number concentrations. Two days with different aerosol and cloud microphysical properties but almost identical meteorological conditions have been analyzed in detail. The differences in the droplet number concentration and droplet sizes appear not to show any significant change for turbulent cloud mixing, but the relative roles of droplet inertia and sedimentation in initiating coalescence, as well as the cloud reflectivity, do change substantially.

Wonaschutz, A, Coggon M, Sorooshian A, Modini R, Frossard AA, Ahlm L, Mulmenstadt J, Roberts GC, Russell LM, Dey S, Brechtel FJ, Seinfeld JH.  2013.  Hygroscopic properties of smoke-generated organic aerosol particles emitted in the marine atmosphere. Atmospheric Chemistry and Physics. 13:9819-9835.   10.5194/acp-13-9819-2013   AbstractWebsite

During the Eastern Pacific Emitted Aerosol Cloud Experiment (E-PEACE), a plume of organic aerosol was produced by a smoke generator and emitted into the marine atmosphere from aboard the R/V Point Sur. In this study, the hygroscopic properties and the chemical composition of the plume were studied at plume ages between 0 and 4 h in different meteorological conditions. In sunny conditions, the plume particles had very low hygroscopic growth factors (GFs): between 1.05 and 1.09 for 30 nm and between 1.02 and 1.1 for 150 nm dry size at a relative humidity (RH) of 92 %, contrasted by an average marine background GF of 1.6. New particles were produced in large quantities (several 10 000 cm(-3)), which lead to substantially increased cloud condensation nuclei (CCN) concentrations at super-saturations between 0.07 and 0.88 %. Ratios of oxygen to carbon (O : C) and water-soluble organic mass (WSOM) increased with plume age: from <0.001 to 0.2, and from 2.42 to 4.96 mu g m(-3), respectively, while organic mass fractions decreased slightly (similar to 0.97 to similar to 0.94). High-resolution aerosol mass spectrometer (AMS) spectra show that the organic fragment m/z 43 was dominated by C2H3O+ in the small, new particle mode and by C3H7+ in the large particle mode. In the marine background aerosol, GFs for 150 nm particles at 40% RH were found to be enhanced at higher organic mass fractions: an average GF of 1.06 was observed for aerosols with an organic mass fraction of 0.53, and a GF of 1.04 for an organic mass fraction of 0.35.

DeMott, PJ, Hudson JG, Roberts GC, Bundke U.  2013.  Cloud condensation and ice nuclei. Airborne Measurements for Environmental Research. ( Wendisch M, Brenguier JL, Kohkhanovsky A, Eds.).:157-223.: John Wiley & Sons Abstract
Begue, N, Tulet P, Chaboureau JP, Roberts G, Gomes L, Mallet M.  2012.  Long-range transport of Saharan dust over northwestern Europe during EUCAARI 2008 campaign: Evolution of dust optical properties by scavenging. Journal of Geophysical Research-Atmospheres. 117   10.1029/2012jd017611   AbstractWebsite

The evolution of dust optical properties is illustrated in this paper through a case of long-range transport of Saharan dust over northwestern Europe during the European Integrated Project on Aerosol-Cloud-Climate and Air Quality Interactions (EUCAARI) experimental campaign in 2008. This spread of dust over northwestern Europe is investigated by combining satellite, airborne, ground-based observations and the non-hydrostatic meso-scale model Meso-NH. The total dust amount emitted during the study period is estimated to 185 Tg. The analysis of the removal processes reveals that only 12.5 Tg is lost by dry deposition, and that wet deposition is the main process of dust removal (73 Tg). The observed aerosol optical thickness ranged from 0.1 to 0.5 at the wavelength of 440 nm, with a maximum value close to 1 is found over the Netherlands (51.97 degrees N, 4.93 degrees E). Over that site, the main dust layer is located between 2.5 and 5.2 km above sea level (asl), moreover dust was also present at 0.9 km asl. The nephelometer measurements on board the ATR-42 aircraft revealed a strong wavelength dependence of the scattering coefficient over the Netherlands. The Angstrom exponent is greater than 0.5, whereas usually it approaches zero in presence of Saharan dust. This is due to high precipitation scavenging efficiency for the coarse mode, particularly below 4 km. Our results confirm that atmospheric conditions govern the life cycle of dust microphysical phenomena, providing conditions for transformation processes during transport, and removal of particles from the atmosphere.

Baumgardner, D, Avallone L, Bansemer A, Borrmann S, Brown P, Bundke U, Chuang PY, Cziczo D, Field P, Gallagher M, Gayet JF, Heymsfield A, Korolev A, Kramer M, McFarquhar G, Mertes S, Mohler O, Lance S, Lawson P, Petters MD, Pratt K, Roberts G, Rogers D, Stetzer O, Stith J, Strapp W, Twohy C, Wendisch M.  2012.  In situ, airborne instrumentation: addressing and solving measurement problems in ice clouds. Bulletin of the American Meteorological Society. 93:E529-E534.   10.1175/bams-d-11-00123.1   AbstractWebsite
Russell, LM, Sorooshian A, Seinfeld JH, Albrecht BA, Nenes A, Ahlm L, Chen Y-C, Coggon M, Craven JS, Flagan RC, Frossard AA, Jonsson H, Jung E, Lin JJ, Metcalf AR, Modini R, Mülmenstädt J, Roberts GC, Shingler T, Song S, Wang Z, Wonaschütz A.  2012.  Eastern Pacific Emitted Aerosol Cloud Experiment (E-PEACE). Bulletin of the American Meteorological Society. : American Meteorological Society   10.1175/BAMS-D-12-00015   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 on 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 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 (i) shipboard smoke-generated particles with 0.05–1 μm diameters (which produced tracks measured by satellite and had drop composition characteristic of organic smoke), (ii) combustion particles from container ships with 0.05–0.2 μm diameters (which were measured in a variety of conditions with droplets containing both organic and sulfate components), and (iii) aircraft-based milled salt particles with 3–5 μm 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.

Moore, MJK, Furutani H, Roberts GC, Moffet RC, Gilles MK, Palenik B, Prather KA.  2011.  Effect of organic compounds on cloud condensation nuclei (CCN) activity of sea spray aerosol produced by bubble bursting. Atmospheric Environment. 45:7462-7469.   10.1016/j.atmosenv.2011.04.034   AbstractWebsite

The ocean comprises over 70% of the surface of the earth and thus sea spray aerosols generated by wave processes represent a critical component of our climate system. The manner in which different complex oceanic mixtures of organic species and inorganic salts are distributed between individual particles in sea spray directly determines which particles will effectively form cloud nuclei. Controlled laboratory experiments were undertaken to better understand the full range of particle properties produced by bubbling solutions composed of simplistic model organic species, oleic acid and sodium dodecyl sulfate (SDS), mixed with NaCl to more complex artificial seawater mixed with complex organic mixtures produced by common oceanic microorganisms. Simple mixtures of NaCl and oleic acid or SDS had a significant effect on CCN activity, even in relatively small amounts. However, an artificial seawater (ASW) solution containing microorganisms, the common cyanobacteria (Synechococcus) and DMS-producing green algae (Ostreococcus), produced particles containing similar to 34 times more carbon than the particles produced from pure ASW, yet no significant change was observed in the overall CCN activity. We hypothesize that these microorganisms produce diverse mixtures of organic species with a wide range of properties that produced offsetting effects, leading to no net change in the overall average measured hygroscopicity of the collection of sea spray particles. Based on these observations, changes in CCN activity due to "bloom" conditions would be predicted to lead to small changes in the average CCN activity, and thus have a negligible impact on cloud formation. However, each sea spray particle will contain a broad spectrum of different species, and thus further studies are needed of the CCN activity of individual sea spray particles and biological processes under a wide range of controllable conditions. (C) 2011 Published by Elsevier Ltd.

Kulmala, M, Asmi A, Lappalainen HK, Baltensperger U, Brenguier JL, Facchini MC, Hansson HC, Hov O, O'Dowd CD, Poschl U et al..  2011.  General overview: European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) - integrating aerosol research from nano to global scales. Atmos Chem Phys. 11:13061-13143.   doi:10.5194/acp-11-13061-2011   Abstract

In this paper we describe and summarize the main achievements of the European Aerosol Cloud Climate and Air Quality Interactions project (EUCAARI). EUCAARI started on 1 January 2007 and ended on 31 December 2010 leaving a rich legacy including: (a) a comprehensive database with a year of observations of the physical, chemical and optical properties of aerosol particles over Europe, (b) comprehensive aerosol measurements in four developing countries, (c) a database of airborne measurements of aerosols and clouds over Europe during May 2008, (d) comprehensive modeling tools to study aerosol processes fron nano to global scale and their effects on climate and air quality. In addition a new Pan-European aerosol emissions inventory was developed and evaluated, a new cluster spectrometer was built and tested in the field and several new aerosol parameterizations and computations modules for chemical transport and global climate models were developed and evaluated. These achievements and related studies have substantially improved our understanding and reduced the uncertainties of aerosol radiative forcing and air quality-climate interactions. The EUCAARI results can be utilized in European and global environmental policy to assess the aerosol impacts and the corresponding abatement strategies.

Martin, ST, Andreae MO, Artaxo P, Baumgardner D, Chen Q, Goldstein AH, Guenther A, Heald CL, Mayol-Bracero OL, McMurry PH, Pauliquevis T, Poschl U, Prather KA, Roberts GC, Saleska SR, Dias MAS, Spracklen DV, Swietlicki E, Trebs I.  2010.  Sources and properties of Amazonian aerosol particles. Reviews of Geophysics. 48   10.1029/2008rg000280   AbstractWebsite

This review provides a comprehensive account of what is known presently about Amazonian aerosol particles and concludes by formulating outlook and priorities for further research. The review is organized to follow the life cycle of Amazonian aerosol particles. It begins with a discussion of the primary and secondary sources relevant to the Amazonian particle burden, followed by a presentation of the particle properties that characterize the mixed populations present over the Amazon Basin at different times and places. These properties include number and mass concentrations and distributions, chemical composition, hygroscopicity, and cloud nucleation ability. The review presents Amazonian aerosol particles in the context of natural compared to anthropogenic sources as well as variability with season and meteorology. This review is intended to facilitate an understanding of the current state of knowledge on Amazonian aerosol particles specifically and tropical continental aerosol particles in general and thereby to enhance future research in this area.

Roberts, GC, Day DA, Russell LM, Dunlea EJ, Jimenez JL, Tomlinson JM, Collins DR, Shinozuka Y, Clarke AD.  2010.  Characterization of particle cloud droplet activity and composition in the free troposphere and the boundary layer during INTEX-B. Atmospheric Chemistry and Physics. 10:6627-6644.   10.5194/acp-10-6627-2010   AbstractWebsite

Measurements of cloud condensation nuclei (CCN), aerosol size distributions, and submicron aerosol composition were made as part of the Intercontinental Chemical Transport Experiment Phase B (INTEX-B) campaign during spring 2006. Measurements were conducted from an aircraft platform over the northeastern Pacific and western North America with a focus on how the transport and evolution of Asian pollution across the Pacific Ocean affected CCN properties. A broad range of air masses were sampled and here we focus on three distinct air mass types defined geographically: the Pacific free troposphere (FT), the marine boundary layer (MBL), and the polluted continental boundary layer in the California Central Valley (CCV). These observations add to the few observations of CCN in the FT. CCN concentrations showed a large range of concentrations between air masses, however CCN activity was similar for the MBL and CCV (kappa similar to 0.2-0.25). FT air masses showed evidence of long-range transport from Asia and CCN activity was consistently higher than for the boundary layer air masses. Bulk chemical measurements predicted CCN activity reasonably well for the CCV and FT air masses. Decreasing trends in kappa with organic mass fraction were observed for the combination of the FT and CCV air masses and can be explained by the measured soluble inorganic chemical components. Changes in hygroscopicity associated with differences in the non-refractory organic composition were too small to be distinguished from the simultaneous changes in inorganic ion composition in the FT and MBL, although measurements for the large organic fractions (0.6-0.8) found in the CCV showed values of the organic fraction hygroscopicity consistent with other polluted regions (kappa(org)similar to 0.1-0.2). A comparison of CCN-derived kappa (for particles at the critical diameter) to H-TDMA-derived kappa (for particles at 100 nm diameter) showed similar trends, however the CCN-derived kappa values were significantly higher.