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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.

Stith, JL, Ramanathan V, Cooper WA, Roberts GC, DeMott PJ, Carmichael G, Hatch CD, Adhikary B, Twohy CH, Rogers DC, Baumgardner D, Prenni AJ, Campos T, Gao R, Anderson J, Feng Y.  2009.  An overview of aircraft observations from the Pacific Dust Experiment campaign. Journal of Geophysical Research-Atmospheres. 114   10.1029/2008jd010924   AbstractWebsite

Fourteen research flights were conducted in the Pacific Dust Experiment (PACDEX) during April and May 2007 to sample pollution and dust outbreaks from east Asia as they traveled across the northern Pacific Ocean into North America and interacted with maritime storms. Significant concentrations of black carbon (BC, consisting of soot and other light-absorbing particles measured with a soot photometer 2 instrument) and dust were observed both in the west and east Pacific Ocean from Asian plumes of dust and pollution. BC particles were observed through much of the troposphere, but the major finding is that the percentage of these particles compared with the total number of accumulation mode particles increased significantly (by a factor of 2-4) with increasing altitude, with peak values occurring between 5 and 10 km. Dust plumes had only a small impact on total cloud condensation nuclei at the sampling supersaturations but did exhibit high concentrations of ice nuclei (IN). IN concentrations in dust plumes exceeded typical tropospheric values by 4-20 times and were similar to previous studies in the Saharan aerosol layer when differences in the number concentrations of dust are accounted for. Enhanced IN concentrations were found in the upper troposphere off the coast of North America, providing a first direct validation of the transport of high-IN-containing dust layers near the tropopause entering the North American continent from distant sources. A source-specific chemical transport model was used to predict dust and other aerosols during PACDEX. The model was able to predict several features of the in situ observations, including the general altitudes where BC was found and a peak in the ratio of BC to sulfate between 5 and 10 km.

Roberts, GC, Nenes A.  2005.  A continuous-flow streamwise thermal-gradient CCN chamber for atmospheric measurements. Aerosol Science and Technology. 39:206-221.   10.1080/027868290913988   AbstractWebsite

We have addressed the need for improved measurements of cloud condensation nuclei (CCN) by developing a continuous-flow instrument that provides in situ measurements of CCN. The design presented in this article can operate between 0.1 and 3% supersaturation, at sampling rates sufficient for airborne operation. The design constitutes a cylindrical continuous-flow thermal-gradient diffusion chamber employing a novel technique of generating a supersaturation: by establishing a constant streamwise temperature gradient so that the difference in water vapor and thermal diffusivity yield a quasi-uniform centerline supersaturation. Our design maximizes the growth rate of activated droplets, thereby enhancing the performance of the instrument. The temperature gradient and the flow through the column control the supersaturation and may be modified to retrieve CCN spectra. The principle of the CCN instrument was validated in controlled laboratory experiments at different operating conditions using a monodisperse aerosols with known composition and size. These experiments yield sharp activation curves, even for those kinetically limited particles that have not exceeded their critical diameter. The performance of the CCN instrument was also assessed using polydisperse laboratory-generated aerosol of known composition and size distributions similar to ambient particulate matter. In all tests, the measured CCN concentrations compared well with predicted values and highlight the instrument's ability to measure CCN at various size distributions. The full potential of the new design has yet to be explored; however, model simulations suggest that direct measurements in the climatically important range of supersaturations of less than 0.1% (certainly down to 0.07%) are possible. The new instrument clearly offers a unique level of design simplicity, robustness, and flexilibity (temperature control, large range of supersaturations without flow reversal, and multiple configurations for same supersaturation) necessary for atmospheric studies.

Roberts, GC, Nenes A, Seinfeld JH, Andreae MO.  2003.  Impact of biomass burning on cloud properties in the Amazon Basin. Journal of Geophysical Research-Atmospheres. 108   10.1029/2001jd000985   AbstractWebsite

[1] We used a one-dimensional (1-D) cloud parcel model to assess the impact of biomass-burning aerosol on cloud properties in the Amazon Basin and to identify the physical and chemical properties of the aerosol that influence droplet growth. Cloud condensation nuclei (CCN) measurements were performed between 0.15% and 1.5% supersaturation at ground-based sites in the states of Amazonas and Rondonia, Brazil during several field campaigns in 1998 and 1999 as part of the Large-Scale Biosphere - Atmosphere (LBA) Experiment in Amazonia. CCN concentrations measured during the wet season were low and resembled concentrations more typical of marine conditions than most continental sites. During the dry season, smoke aerosol from biomass burning dramatically increased CCN concentrations. The modification of cloud properties, such as cloud droplet effective radius and maximum supersaturation, is most sensitive at low CCN concentrations. Hence, we could expect larger interannual variation of cloud properties during the wet season that the dry season. We found that differences between CCN spectra from forested and deforested regions during the wet season are modest and result in modifications of cloud properties that are small compared to those between wet and dry seasons. Our study suggests that the differences in surface albedo, rather than cloud albedo, between forested and deforested regions may dominate the impact of deforestation on the hydrological cycle and convective activity during the wet season. During the dry season, on the other hand, cloud droplet concentrations may increase by up to 7 times, which leads to a model-predicted decrease in cloud effective radius by a factor of 2. This could imply a maximum indirect radiative forcing due to aerosol as high as ca. -27 W m(-2) for a nonabsorbing cloud. Light-absorbing substances in smoke darken the Amazonian clouds and reduce the net radiative forcing, and a comparison of the Advanced Very High Resolution Radiometer (AVHRR) analysis and our modeling studies suggests that absorption of sunlight due to smoke aerosol may compensate for about half of the maximum aerosol effect. Sensitivity tests show that complete characterization of the aerosol is necessary when kinetic growth limitations become important. Subtle differences in the chemical and physical makeup are shown to be particularly influential in the activation and growth behavior of the aerosol. Knowledge of the CCN spectrum alone is not sufficient to fully capture the climatic influence of biomass burning.

Roberts, GC, Artaxo P, Zhou JC, Swietlicki E, Andreae MO.  2002.  Sensitivity of CCN spectra on chemical and physical properties of aerosol: A case study from the Amazon Basin. Journal of Geophysical Research-Atmospheres. 107   10.1029/2001jd000583   AbstractWebsite

Organic material, about half of which is water soluble, constitutes nearly 80% of the wet-season aerosol mass in the Amazon Basin, while soluble inorganic salts (predominantly ammonium bisulfate) represent about 15%. A detailed analysis of number distributions and the size-dependent chemical composition of the aerosol indicates that, in principle, the sulfate fraction could account for most of the cloud condensation nuclei (CCN) activity. Uncertainty about the chemical speciation of the water-soluble organic component precludes a rigorous analysis of its contribution to nucleation activity. Within reasonable assumptions, we can, however, predict a similar contribution of the organic component to CCN activity as that from sulfate. Because of the nonlinear dependence of droplet nucleation behavior on solute amount, the nucleation activity cannot be attributed uniquely to the inorganic or organic fractions. The role of water-soluble organic compounds as surfactants, however, may be significant (especially in the case of biomass-burning aerosol) and more field measurements are needed to quantify their effects on the surface tension of ambient aerosols. The parametric dependence of the CCN spectra on the physical and chemical properties of the aerosol show that the number distribution, soluble content of the aerosol, and surface tension effects all play an important role in determining CCN spectra.

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.