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Amouroux, D, Roberts G, Rapsomanikis S, Andreae MO.  2002.  Biogenic gas (CH4, N2O, DMS) emission to the atmosphere from near-shore and shelf waters of the north-western Black Sea. Estuarine Coastal and Shelf Science. 54:575-587.   10.1006/ecss.2000.0666   AbstractWebsite

The marine emissions of biogenic gases (CH4, N2O, DMS) were determined on the north-western shelf of the Black Sea in July 1995. Methane (CH,) saturation ratios (SR) averaged 930% (173-10 500%) and were inversely proportional to salinity. The mean nitrous oxide (N2O) SR was 111% (96-149%), which is similar to the values found in other coastal water masses, and did not present any significant variability as a function of salinity. Dimethyl sulphide (DMS) concentrations ranged between 2.96 and 11.9 nM and chlorophyll a-normalized DIMS concentrations were found to increase exponentially with salinity, illustrating the influence of plankton speciation. Coastal and shelf waters affected by riverine inputs, which represent 30% of the Black Sea surface area, contributed up to 53% of the CH4 flux during the summer period. Biogenic sulphur emissions, primarily as DMS, showed a strong gradient, increasing from open Black Sea waters to estuarine Danube waters. There was less variation in the flux densities of N2O for the different water masses. By extrapolating values obtained during summer 1995, upper limits for the emissions from the Black Sea to the atmosphere were estimated to be 6.7-11.7 Gmol yr(-1) of CH4, 0.45-0.75 Gmol yr(-1) of N2O and 0.30-0.80 Gmol yr(-1) of DMS, using two different air-sea gas exchange models. (C) 2002 Elsevier Science Ltd. All rights reserved.

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

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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
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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.

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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.

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.

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.

Conant, WC, VanReken TM, Rissman TA, Varutbangkul V, Jonsson HH, Nenes A, Jimenez JL, Delia AE, Bahreini R, Roberts GC, Flagan RC, Seinfeld JH.  2004.  Aerosol-cloud drop concentration closure in warm cumulus. Journal of Geophysical Research-Atmospheres. 109   10.1029/2003jd004324   AbstractWebsite

[1] Our understanding of the activation of aerosol particles into cloud drops during the formation of warm cumulus clouds presently has a limited observational foundation. Detailed observations of aerosol size and composition, cloud microphysics and dynamics, and atmospheric thermodynamic state were collected in a systematic study of 21 cumulus clouds by the Center for Interdisciplinary Remotely-Piloted Aircraft Studies (CIRPAS) Twin Otter aircraft during NASA's Cirrus Regional Study of Tropical Anvils and Cirrus Layers - Florida Area Cirrus Experiment (CRYSTAL-FACE). An "aerosol-cloud'' closure study was carried out in which a detailed cloud activation parcel model, which predicts cloud drop concentration using observed aerosol concentration, size distribution, cloud updraft velocity, and thermodynamic state, is evaluated against observations. On average, measured droplet concentration in adiabatic cloud regions is within 15% of the predictions. This agreement is corroborated by independent measurements of aerosol activation carried out by two cloud condensation nucleus (CCN) counters on the aircraft. Variations in aerosol concentration, which ranged from 300 to 3300 cm(-3), drives large microphysical differences ( 250 2300 cm(-3)) observed among continental and maritime clouds in the South Florida region. This is the first known study in which a cloud parcel model is evaluated in a closure study using a constraining set of data collected from a single platform. Likewise, this is the first known study in which relationships among aerosol size distribution, CCN spectrum, and cloud droplet concentration are all found to be consistent with theory within experimental uncertainties much less than 50%. Vertical profiles of cloud microphysical properties ( effective radius, droplet concentration, dispersion) clearly demonstrate the boundary layer aerosol's effect on cloud microphysics throughout the lowest 1 km of cloud depth. Onboard measurements of aerosol hygroscopic growth and the organic to sulfate mass ratio are related to CCN properties. These chemical data are used to quantify the range of uncertainty associated with the simplified treatment of aerosol composition assumed in the closure study.

Corrigan, CE, Roberts GC, Ramana MV, Kim D, Ramanathan V.  2008.  Capturing vertical profiles of aerosols and black carbon over the Indian Ocean using autonomous unmanned aerial vehicles. Atmospheric Chemistry and Physics. 8:737-747.   10.5194/acp-8-737-2008   AbstractWebsite

Measurements of the vertical distribution of aerosol properties provide essential information for generating more accurate model estimates of radiative forcing and atmospheric heating rates compared with employing remotely sensed column averaged properties. A month long campaign over the Indian Ocean during March 2006 investigated the interaction of aerosol, clouds, and radiative effects. Routine vertical profiles of aerosol and water vapor were determined using autonomous unmanned aerial vehicles equipped with miniaturized instruments. Comparisons of these airborne instruments with established ground-based instruments and in aircraft-to-aircraft comparisons demonstrated an agreement within 10%. Aerosol absorption optical depths measured directly using the unmanned aircraft differed from columnar AERONET sun-photometer results by only 20%. Measurements of total particle concentration, particle size distributions, aerosol absorption and black carbon concentrations are presented along with the trade wind thermodynamic structure from the surface to 3000 m above sea level. Early March revealed a well-mixed layer up to the cloud base at 500 m above mean sea level (m a.s.l.), followed by a decrease of aerosol concentrations with altitude. The second half of March saw the arrival of a high altitude plume existing above the mixed layer that originated from a continental source and increased aerosol concentrations by more than tenfold, yet the surface air mass showed little change in aerosol concentrations and was still predominantly influenced by marine sources. Black carbon concentrations at 1500 m above sea level increased from 70 ng/m(3) to more than 800 ng/m(3) with the arrival of this polluted plume. The absorption aerosol optical depth increased from as low as 0.005 to as much as 0.035 over the same period. The spectral dependence of the aerosol absorption revealed an absorption Angstrom exponent of 1.0, which is typical of an aerosol with most of its absorption attributed to black carbon and generally indicates the absorbing component originated from fossil fuel sources and other high-temperature combustion sources. The results indicate that surface measurements do not represent the aerosol properties within the elevated layers, especially if these layers are influenced by long range transport.

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.

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.

Crumeyrolle, S, Manninen HE, Sellegri K, Roberts G, Gomes L, Kulmala M, Weigel R, Laj P, Schwarzenboeck A.  2010.  New particle formation events measured on board the ATR-42 aircraft during the EUCAARI campaign. Atmospheric Chemistry and Physics. 10:6721-6735.   10.5194/acp-10-6721-2010   AbstractWebsite

Aerosol properties were studied during an intensive airborne measurement campaign that took place at Rotterdam in Netherlands in May 2008 within the framework of the European Aerosol Cloud Climate and Air Quality Interactions project (EUCAARI). The objective of this study is to illustrate seven events of new particle formation (NPF) observed with two Condensation Particle Counters (CPCs) operated on board the ATR-42 research aircraft in airsectors around Rotterdam, and to provide information on the spatial extent of the new particle formation phenomenon based on 1-s resolution measurements of ultra-fine particle (in the size range 3-10 nm diameter, denoted N(3-10) hereafter) concentrations. The results show that particle production occurred under the influence of different air mass origins, at different day times and over the North Sea as well as over the continent. The number concentration of freshly nucleated particles (N(3-10)) varied between 5000 and 100 000 cm(-3) within the boundary layer (BL). Furthermore the vertical extension for all nucleation events observed on the ATR-42 never exceeded the upper limit of the BL. The horizontal extent of N(3-10) could not be delimited due to inflexible flight plans which could not be modified to accommodate real-time results. However, the NPF events were observed over geographically large areas; typically the horizontal extension was about 100 km and larger.

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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
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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.

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.

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Graham, B, Mayol-Bracero OL, Guyon P, Roberts GC, Decesari S, Facchini MC, Artaxo P, Maenhaut W, Koll P, Andreae MO.  2002.  Water-soluble organic compounds in biomass burning aerosols over Amazonia - 1. Characterization by NMR and GC-MS. Journal of Geophysical Research-Atmospheres. 107   10.1029/2001jd000336   AbstractWebsite

[1] As part of the European contribution to the Large-Scale Atmosphere-Biosphere Experiment in Amazonia (LBA-EUSTACH), aerosols were sampled at representative pasture and primary rainforest sites in Rondonia, Brazil, during the 1999 "burning season" and dry-to-wet season transition (September-October). Water-soluble organic compounds (WSOCs) within the samples were characterized using a combination of H-1 Nuclear Magnetic Resonance (NMR) spectroscopy for chemical functional group analysis, and Gas Chromatography-Mass Spectrometry (GC-MS) for identification and quantification of individual low-molecular-weight compounds. The H-1 NMR analysis indicates that WSOCs are predominantly aliphatic or oxygenated aliphatic compounds (alcohols, carboxylic acids, etc.), with a minor content of aromatic rings carrying carboxylic and phenolic groups. Levoglucosan (1,6-anhydro-beta-D-glucose), a well-known cellulose combustion product, was the most abundant individual compound identified by GC-MS (0.04-6.90 mug m(-3)), accounting for 1-6% of the total carbon (TC) and 2-8% of the water-soluble organic carbon (WSOC). Other anhydrosugars, produced by hemicellulose breakdown, were detected in much smaller amounts, in addition to series of acids, hydroxyacids, oxoacids, and polyalcohols (altogether 2-5% of TC, 3-6% of WSOC). Most correlated well with organic carbon, black carbon, and potassium, indicating biomass burning to be the major source. A series of sugar alcohols (mannitol, arabitol, erythritol) and sugars (glucose, fructose, mannose, galactose, sucrose, trehalose) were identified as part of the natural background aerosol and are probably derived from airborne microbes and other biogenic material. The bulk of the WSOCs (86-91% WSOC) eluded analysis by GC-MS and may be predominantly high-molecular weight in nature.

Guyon, P, Boucher O, Graham B, Beck J, Mayol-Bracero OL, Roberts GC, Maenhaut W, Artaxo P, Andreae MO.  2003.  Refractive index of aerosol particles over the Amazon tropical forest during LBA-EUSTACH 1999. Journal of Aerosol Science. 34:883-907.   10.1016/s0021-8502(03)00052-1   AbstractWebsite

Optical properties of aerosol particles were characterized during two field campaigns at a remote rainforest site in Rond (o) over cap nia, Brazil, as part of the project European Studies on Trace Gases and Atmospheric Chemistry, a contribution to the Large-Scale Biosphere-Atmosphere Experiment in Amazonia (LBA-EUSTACH). The measurements included background (wet season), biomass burning (dry season), and transition period conditions. Optical measurements of light scattering and absorption were combined with data on number/size distributions in a new iterative method, which retrieves the effective imaginary refractive index of the particles at a wavelength of 545 nm. For ambient relative humidities lower than 80%, background aerosols exhibited an average refractive index of 1.42 - 0.006i. Biomass burning aerosols displayed a much larger imaginary part, with an average refractive index of 1.41 - 0.013i. Other climate-relevant parameters were estimated from Mie calculations. These include single-scattering albedos of 0.93 +/- 0.03 and 0.90 +/- 0.03 (at ambient humidity), asymmetry parameters of 0.63 +/- 0.02 and 0.70 +/- 0.03, and backscatter ratios of 0.12 +/- 0.01 and 0.08 +/- 0.01 for background and biomass burning aerosols, respectively. (C) 2003 Published by Elsevier Ltd.

Guyon, P, Graham B, Roberts GC, Mayol-Bracero OL, Maenhaut W, Artaxo P, Andreae MO.  2004.  Sources of optically active aerosol particles over the Amazon forest. Atmospheric Environment. 38:1039-1051.   10.1016/j.atmosenv.2003.10.051   AbstractWebsite

Size-fractionated ambient aerosol samples were collected at a pasture site and a primary rainforest site in the Brazilian Amazon Basin during two field campaigns (April-May and September-October 1999), as part of the European contribution to the Large-Scale Biosphere-Atmosphere Experiment in Amazonia (LBA-EUSTACH). The samples were analyzed for up to 19 trace elements by particle-induced X-ray emission analysis (PIXE), for equivalent black carbon (BCe) by a light reflectance technique and for mass concentration by gravimetric analysis. Additionally, we made continuous measurements of absorption and light scattering by aerosol particles. The vertical chemical composition gradients at the forest site have been discussed in a companion article (Journal of Geophysical Research-Atmospheres 108 (1318), 4591 (doi:4510.1029/2003JD003465)). In this article, we present the results of a source identification and quantitative apportionment study of the wet and dry season aerosols, including an apportionment of the measured scattering and absorption properties of the total aerosol in terms of the identified aerosol sources. Source apportionments (obtained from absolute principal component analysis) revealed that the wet and dry season aerosols contained the same three main components, but in different (absolute and relative) amounts: the wet season aerosol consisted mainly of a natural biogenic component, whereas pyrogenic aerosols dominated the dry season aerosol mass. The third component identified was soil dust, which was often internally mixed with the biomass-burning aerosol. All three components contributed significantly to light extinction during both seasons. At the pasture site, up to 47% of the light absorption was attributed to biogenic particles during the wet season, and up to 35% at the tower site during the wet-to-dry transition period. The results from the present study suggest that, in addition to pyrogenic particles, biogenic and soil dust aerosols must be taken into account when modeling the physical and optical properties of aerosols in forested regions such the Amazon Basin. (C) 2003 Published by Elsevier Ltd.

Guyon, P, Graham B, Beck J, Boucher O, Gerasopoulos E, Mayol-Bracero OL, Roberts GC, Artaxo P, Andreae MO.  2003.  Physical properties and concentration of aerosol particles over the Amazon tropical forest during background and biomass burning conditions. Atmospheric Chemistry and Physics. 3:951-967.   10.5194/acp-3-951-2003   AbstractWebsite

We investigated the size distribution, scattering and absorption properties of Amazonian aerosols and the optical thickness of the aerosol layer under the pristine background conditions typical of the wet season, as well as during the biomass-burning-influenced dry season. The measurements were made during two campaigns in 1999 as part of the European contribution to the Large-Scale BiosphereAtmosphere Experiment in Amazonia (LBA-EUSTACH). In moving from the wet to the dry season, median particle numbers were observed to increase from values comparable to those of the remote marine boundary layer (similar to400 cm(-3)) to values more commonly associated with urban smog (similar to4000 cm(-3)), due to a massive injection of submicron smoke particles. Aerosol optical depths at 500 nm increased from 0.05 to 0.8 on average, reaching a value of 2 during the dry season. Scattering and absorption coefficients, measured at 550 nm, showed a concomitant increase from average values of 6.8 and 0.4 Mm(-1) to values of 91 and 10 Mm(-1), respectively, corresponding to an estimated decrease in single-scattering albedo from ca. 0.97 to 0.91. The roughly tenfold increase in many of the measured parameters attests to the dramatic effect that extensive seasonal biomass burning (deforestation, pasture cleaning) is having on the composition and properties of aerosols over Amazonia. The potential exists for these changes to impact on regional and global climate through changes to the extinction of solar radiation as well as the alteration of cloud properties.

Guyon, P, Graham B, Roberts GC, Mayol-Bracero OL, Maenhaut W, Artaxo P, Andreae MO.  2003.  In-canopy gradients, composition, sources, and optical properties of aerosol over the Amazon forest. Journal of Geophysical Research-Atmospheres. 108   10.1029/2003jd003465   AbstractWebsite

[1] As part of the Large-Scale Biosphere-Atmosphere Experiment in Amazonia-European Studies on Trace Gases and Atmospheric Chemistry (LBA-EUSTACH), size-fractionated aerosol samples were collected at a primary rain forest in the Brazilian Amazon during two field campaigns in April - May and September - October 1999. These two periods encompassed parts of the wet and dry seasons, respectively. Daytime-nighttime-segregated sampling was carried out at three different heights ( above, within, and below canopy level) on a 54-m meteorological tower at the forest site in order to better characterize the aerosol sources. The samples were analyzed for up to 19 trace elements by particle-induced X-ray emission analysis and for carbonaceous components by thermal-optical analysis. Equivalent black carbon (BCe) and gravimetric analyses were also performed. The average mass concentrations for particles < 2 μm diameter were 2.2 and 33.5 μg m(-3) for the wet and the dry seasons, respectively. The elements related to biomass burning and soil dust generally exhibited highest concentrations above the canopy and during daytime, while forest-derived aerosol was more concentrated underneath the canopy and during nighttime. These variations can be largely attributed to daytime convective mixing and the formation of a shallow nocturnal boundary layer, along with the possibility of enhanced nighttime release of biogenic aerosol particles. Mass scattering (α(s)) and mass absorption efficiency (α(a)) data indicate that scattering was dominated by fine aerosol, while fine and coarse aerosol both contributed significantly to absorption during both seasons. The data also suggest that components other than elemental carbon were responsible for a substantial fraction of the absorption.

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Hadley, OL, Ramanathan V, Carmichael GR, Tang Y, Corrigan CE, Roberts GC, Mauger GS.  2007.  Trans-Pacific transport of black carbon and fine aerosols (D < 2.5 µm) into North America. Journal of Geophysical Research-Atmospheres. 112   10.1029/2006jd007632   AbstractWebsite

[1] This study presents estimates of long-range transport of black carbon (BC) and aerosol fine mass (diameter less than 2.5 mm) across the Pacific Ocean into North America during April 2004. These transport estimates are based on simulations by the Chemical Weather Forecast System (CFORS) model and evaluated across 130 degrees W, (30 degrees N-60 degrees N) from 26 March through 25 April 2004. CFORS calculates BC transport into North America at 25-32 Gg of which over 75% originates from Asia. Modeled fine aerosol mass transport is between 900 and 1100 Gg. The BC transport amounts to about 77% of the published estimates of North American BC emissions. Approximately 78% of the BC and 82% of the fine aerosol mass transport occur in the midtroposphere above 2 km. Given the relatively large magnitude of the estimated BC transport, we undertake a detailed validation of the model simulations of fine aerosol mass and BC over the west coast of North America. In situ aircraft data were available for the month of April 2004 to assess the accuracy of model simulations of aerosols in the lower troposphere. Aircraft data for aerosol mass collected in the eastern Pacific Ocean during April 2004 as part of the Cloud Indirect Forcing Experiment, as well as surface measurements of fine mass and BC at 30 west coast locations, are compared to CFORS predictions. These surface sites are part of the Interagency Monitoring of Protected Visual Environments (IMPROVE) network. Both the aircraft and the IMPROVE data sets reveal similar patterns of good agreement near and above the boundary layer accompanied by large overprediction within the boundary layer. The observational data validate the CFORS simulations of BC and fine aerosol mass above the boundary layer. The near-surface overprediction does not impair the major conclusions of this study regarding long-range aerosol and BC transport, as most of the long-range transport occurs above 2 km. From this we conclude that the transport of BC from Asia and other regions west is a major source of BC at high elevations over North America. The simulated concentrations of BC between 1 and 3 km, as well as the measured BC concentrations over the elevated IMPROVE sites, range from 0.1 to 0.3 mu g/m(3). Direct radiative forcing over North America due to the modeled BC concentration between 1 and 15 km is estimated at an additional 2.04-2.55 W/m(2) absorbed in the atmosphere and a dimming of-1.45 to-1.47 W/m(2) at the surface. The impact of transported BC on the regional radiation budget through direct and indirect effects of the transported BC and other aerosols warrants further study.

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.

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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.

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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.

Kubatova, A, Vermeylen R, Claeys M, Cafmeyer J, Maenhaut W, Roberts G, Artaxo P.  2000.  Carbonaceous aerosol characterization in the Amazon basin, Brazil: novel dicarboxylic acids and related compounds. Atmospheric Environment. 34:5037-5051.   10.1016/s1352-2310(00)00320-4   AbstractWebsite

High-resolution capillary gas chromatography (GC) and GC/mass spectrometry (MS) were employed for the quantitative determination of dichloromethane-extractable organic compounds in total and size-fractionated aerosol samples which were collected in the Amazon basin, Brazil, during the wet season, as part of the LBA-CLAIRE-98 experiment. Special emphasis was placed on the characterization and identification of several novel unknown dicarboxylic acids and related oxidative degradation products. This class of acidic products was enriched in the fine size fraction, suggesting that they were secondary organic aerosol products formed by gas-to-particle conversion. Some of the unknowns contributed more to the class of dicarboxylic acids than the major known compound, nonadioic acid (azelaic acid). The same unknowns were also observed in urban aerosol samples collected on hot summer days in Gent, Belgium. For the characterization and structure elucidation of the unknowns, various types of derivatizations and Fractionation by solid-phase extraction were employed in combination with GC/MS. Four unknowns were identified. The most abundant were two derivatives of glutaric acid, 3-isopropyl pentanedioic acid and 3-acetyl pentanedioic acid. The other two identified unknowns were another oxo homologue, 3-acetyl hexanedioic acid, and, interestingly, 3-carboxy heptanedioic acid. To our knowledge, the occurrence of these four compounds in atmospheric aerosols has not yet been reported. The biogenic precursors of the novel identified compounds could not be pinpointed. but most likely include monoterpenes and fatty acids. (C) 2000 Elsevier Science Ltd. All rights reserved.