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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.

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.

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.

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

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

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, 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.

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.

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.