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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.

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.

Furutani, H, Dall'osto M, Roberts GC, Prather KA.  2008.  Assessment of the relative importance of atmospheric aging on CCN activity derived from field observations. Atmospheric Environment. 42:3130-3142.   10.1016/j.atmosenv.2007.09.024   AbstractWebsite

The effect of atmospheric aging on the cloud condensation nuclei (CCN) activity of atmospheric aerosols was studied by comparing different air masses with different degrees of aging along the southern coast of California over the Pacific Ocean during a research cruise on the R/V Roger Revelle from 2-19 November 2004. Activation diameters (D(act)) were calculated using the measured CCN concentrations, condensation nuclei (CN) concentrations, and particle size distributions. Measurements of single particle size and chemistry, as well as black carbon (BC) concentrations with an aethalometer, were made to provide further insight into aerosol chemistry. A gradient of aerosol concentrations was encountered: along the coast of California, the highest BC and CN concentrations (1000-6000 ng m(-3) and 2000-15,000 cm(-3)) were measured which decreased as the ship moved away from shore to much lower values (<100 ng m(-3), similar to 300 cm(-3)). In all regions, external mixtures of organic carbon, elemental carbon, sea salt, and dust aerosols frequently associated with nitrate and sulfate were observed. A correlation plot between the CCN/CN ratio and D(act) exhibits a clear linear correlation, showing a distinct relationship between the extent of anthropogenic aging and CCN activity with the most highly aged air masses showing the highest CCN activity and smallest D(act). These results show changes in aerosol chemistry due to atmospheric aging that play an important role in determining the CCN activity of atmospheric aerosols. The present study demonstrates that variations in aerosol chemistry must be taken into account in models to adequately account for the physicochemical properties of atmospheric aerosols and their CCN activity. (C) 2007 Published by Elsevier Ltd.

Yum, SS, Roberts G, Kim JH, Song KY, Kim DY.  2007.  Submicron aerosol size distributions and cloud condensation nuclei concentrations measured at Gosan, Korea, during the Atmospheric brown clouds - East Asian Regional Experiment 2005. Journal of Geophysical Research-Atmospheres. 112   10.1029/2006jd008212   AbstractWebsite

Submicron aerosol size distributions, CN and CCN concentrations at a constant supersaturation of 0.6% were measured at a relatively remote coastal site at Gosan in Jeju Island, Korea, during the ABC-EAREX from 11 March to 8 April 2005. The average CN concentrations were 6088 +/- 3988, 5231 +/- 2454 and 3513 +/- 1790 cm(-3), respectively, for the three major air mass types classified by their origins. The corresponding CCN concentrations were 2393 +/- 1156, 2897 +/- 1226 and 1843 +/- 585 cm(-3). The type III air mass was the closest to maritime origins, but these lowest concentrations at Gosan were an order of magnitude higher than those of clean marine boundary layer, indicating that regardless of air mass designation springtime submicron aerosols at Gosan were under steady continental influences. Distinct new particle formation and growth events occurred on 6 d, when clear sky weather conditions prevailed that brought air from northern China, Mongolia or Russia by anticyclonic circulations. Simultaneous occurrence of these events at a western coastal site in the Korean Peninsula 350 km north of Gosan suggests that these events were not local but at least regional-scale events. CCN concentrations were predicted with the aerosol size distributions and the assumption of particles being composed of ( NH(4))(2)SO(4). The predicted to measured CCN concentration ratio was 1.27 +/- 0.29 and the r(2) was 0.77 for the whole measurement period. The type I air mass that has the most continental influences showed a slight tendency to overpredict CCN concentrations but the good agreement overall suggests that springtime Gosan aerosols act almost like ammonium sulfate as far as CCN activity is concerned, almost regardless of air mass origin.

Roberts, G, Mauger G, Hadley O, Ramanathan V.  2006.  North American and Asian aerosols over the eastern Pacific Ocean and their role in regulating cloud condensation nuclei. Journal of Geophysical Research-Atmospheres. 111   10.1029/2005jd006661   AbstractWebsite

[ 1] Measurements of aerosol and cloud properties in the Eastern Pacific Ocean were taken during an airborne experiment on the University of Wyoming's King Air during April 2004 as part of the Cloud Indirect Forcing Experiment (CIFEX). We observed a wide variety of aerosols, including those of long-range transport from Asia, clean marine boundary layer, and North American emissions. These aerosols, classified by their size distribution and history, were found in stratified layers between 500 to 7500 m above sea level and thicknesses from 100 to 3000 m. A comparison of the aerosol size distributions to measurements of cloud condensation nuclei (CCN) provides insight to the CCN activity of the different aerosol types. The overall ratio of measured to predicted CCN concentration (NCCN) is 0.56 +/- 0.41 with a relationship of N-CCN,N- measured = N-CCN, predicted(0.846 +/- 0.002) for 23 research flights and 1884 comparisons. Such a relationship does not accurately describe a CCN closure; however, it is consistent with our measurements that high CCN concentrations are more influenced by anthropogenic sources, which are less CCN active. While other CCN closures have obtained results closer to the expected 1: 1 relationship, the different aerosol types ( and presumably differences in aerosol chemistry) are responsible for the discrepancy. The measured N-CCN at 0.3% supersaturation (S-c) ranged from 20 cm(-3) (pristine) to 350 cm(-3) ( anthropogenic) with an average of 106 +/- 54 cm(-3) over the experiment. The inferred supersaturation in the clouds sampled during this experiment is similar to 0.3%. CCN concentrations of cloud-processed aerosol were well predicted using an ammonium sulfate approximation for S-c <= 0.4%. Predicted N-CCN for other aerosol types (i.e., Asian and North American aerosols) were high compared to measured values indicating a less CCN active aerosol. This study highlights the importance of chemical effects on CCN measurements and introduces a CCN activation index as a method of classifying the efficiency of an aerosol to serve as CCN relative to an ammonium sulfate particle. This index ranged from close to unity for cloud processed aerosols to as low as 0.31 for aged aerosols transported from Asia. We also compare the performance of two CCN instruments ( static thermal diffusion chamber and streamwise continuous flow chamber) on a 45 minute level leg where we observe an aged layer and a nucleation event. More than 50% of the aged aerosol served as CCN at 0.2% S-c, primarily owing to their large size, while CCN concentrations during the nucleation event were close to 0 cm(-3). CCN concentrations from both instruments agreed within instrument errors; however, the continuous flow chamber effectively captured the rapid transition in aerosol properties.

Rissler, J, Swietlicki E, Zhou J, Roberts G, Andreae MO, Gatti LV, Artaxo P.  2004.  Physical properties of the sub-micrometer aerosol over the Amazon rain forest during the wet-to-dry season transition - comparison of modeled and measured CCN concentrations. Atmospheric Chemistry and Physics. 4:2119-2143.   10.5194/acp-4-2119-2004   AbstractWebsite

Sub-micrometer atmospheric aerosol particles were studied in the Amazon region, 125 km northeast of Manaus, Brazil (-1degrees55.2'S, 59degrees28.1'W). The measurements were performed during the wet-to-dry transition period, 4-28 July 2001 as part of the LBA (Large-Scale Biosphere Atmosphere Experiment in Amazonia) CLAIRE-2001 (Cooperative LBA Airborne Regional Experiment) experiment. The number size distribution was measured with two parallel differential mobility analyzers, the hygroscopic growth at 90% RH with a Hygroscopic Tandem Mobility Analyzer (H-TDMA) and the concentrations of cloud condensation nuclei (CCN) with a cloud condensation nuclei counter. A model was developed that uses the H-TDMA data to predict the number of soluble molecules or ions in the individual particles and the corresponding minimum particle diameter for activation into a cloud droplet at a certain supersaturation. Integrating the number size distribution above this diameter, CCN concentrations were predicted with a time resolution of 10 min and compared to the measured concentrations. During the study period, three different air masses were identified and compared: clean background, air influenced by aged biomass burning, and moderately polluted air from recent local biomass burning. For the clean period 2001, similar number size distributions and hygroscopic behavior were observed as during the wet season at the same site in 1998, with mostly internally mixed particles of low diameter growth factor (similar to1.3 taken from dry to 90% RH). During the periods influenced by biomass burning the hygroscopic growth changed slightly, but the largest difference was seen in the number size distribution. The CCN model was found to be successful in predicting the measured CCN concentrations, typically within 25%. A sensitivity study showed relatively small dependence on the assumption of which model salt that was used to predict CCN concentrations from H-TDMA data. One strength of using H-TDMA data to predict CCN concentrations is that the model can also take into account soluble organic compounds, insofar as they go into solution at 90% RH. Another advantage is the higher time resolution compared to using size-resolved chemical composition data.

Formenti, P, Andreae MO, Lange L, Roberts G, Cafmeyer J, Rajta I, Maenhaut W, Holben BN, Artaxo P, Lelieveld J.  2001.  Saharan dust in Brazil and Suriname during the Large-Scale Biosphere-Atmosphere Experiment in Amazonia (LBA) - Cooperative LBA Regional Experiment (CLAIRE) in March 1998. Journal of Geophysical Research-Atmospheres. 106:14919-14934.   10.1029/2000jd900827   AbstractWebsite

Advection of Saharan dust was observed via chemical and optical measurements during March 1998 in Brazil and Suriname during the Large-Scale Biosphere-Atmosphere Experiment in Amazonia (LBA)-Cooperative LBA Airborne Regional Experiment (CLAIRE)-98 experiment. In Brazil the dust outbreak produced an increase of a factor of 3 in the daily mean mass concentration (up to 26 +/- 7 mug m(-3)) of particles smaller than 10 mum equivalent aerodynamic diameter (EAD), and in the daily mean aerosol particle scattering coefficient sigma (N) (up to 26 +/- 8 Mm(-1) STP, ambient humidity). Background levels of aerosol scattering (ambient) were sigma (s) similar to 10 Mm(-1). The effect of dust advection was evident for all major crustal elements (Al, Si, Ca, Ti, Mn, and Fe), as well as the sea-salt elements (Na, Cl, and S), as the dust layer was transported at low altitude (below 800 hPa). Coarse P and organic carbon (OC) concentrations were not influenced by the occurrence of dust, and were mainly emitted by the rain forest. The dry scattering mass efficiency of dust (particles smaller than 10 mum EAD) was estimated to be between 0.65 (+/- 0.06) and 0.89 (+/- 0.08) m(2) g(-1). Airborne profiles of aerosol scattering showed two distinct types of vertical structure in the dust layer over Suriname, either vertically uniform (15, 26 March), or plume-like (25 March). Dust layers extended generally up to 700 hPa, while scattering layers occasionally encountered at higher altitudes resulted from smoke emitted by biomass burning in Venezuela and Colombia, Observations in South America were supported by measurements in Israel and Tenerife (Canary Islands), where the dust outbreaks were also detected.

Kettle, AJ, Andreae MO, Amouroux D, Andreae TW, Bates TS, Berresheim H, Bingemer H, Boniforti R, Curran MAJ, DiTullio GR, Helas G, Jones GB, Keller MD, Kiene RP, Leck C, Levasseur M, Malin G, Maspero M, Matrai P, McTaggart AR, Mihalopoulos N, Nguyen BC, Novo A, Putaud JP, Rapsomanikis S, Roberts G, Schebeske G, Sharma S, Simo R, Staubes R, Turner S, Uher G.  1999.  A global database of sea surface dimethylsulfide (DMS) measurements and a procedure to predict sea surface DMS as a function of latitude, longitude, and month. Global Biogeochemical Cycles. 13:399-444.   10.1029/1999gb900004   AbstractWebsite

A database of 15,617 point measurements of dimethylsulfide (DMS) in surface waters along with lesser amounts of data for aqueous and particulate dimethylsulfoniopropionate concentration, chlorophyll concentration, sea surface salinity and temperature, and wind speed has been assembled. The database was processed to create a series of climatological annual and monthly 1 degrees x1 degrees latitude-longitude squares of data. The results were compared to published fields of geophysical and biological parameters. No significant correlation was found between DMS and these parameters, and no simple algorithm could be found to create monthly fields of sea surface DMS concentration based on these parameters. Instead, an annual map of sea surface DMS was produced using an algorithm similar to that employed by Conkright et al. [1994]. In this approach, a first-guess field of DMS sea surface concentration measurements is created and then a correction to this field is generated based on actual measurements. Monthly sea surface grids of DMS were obtained using a similar scheme, but the sparsity of DMS measurements made the method difficult to implement. A scheme was used which projected actual data into months of the year where no data were otherwise present.