Cloud condensation nuclei in pristine tropical rainforest air of Amazonia: size-resolved measurements and modeling of atmospheric aerosol composition and CCN activity

Atmospheric aerosol particles serving as cloud condensation nuclei (CCN) are key elements of the hydrological cycle and climate. We have measured and characterized CCN at water vapor supersaturations in the range of S=0.10-0.82% in pristine tropical rainforest air during the AMAZE-08 campaign in central Amazonia. The effective hygroscopicity parameters describing the influence of chemical composition on the CCN activity of aerosol particles varied in the range of kappa approximate to 0.1-0.4 (0.16+/-0.06 arithmetic mean and standard deviation). The overall median value of kappa approximate to 0.15 was by a factor of two lower than the values typically observed for continental aerosols in other regions of the world. Aitken mode particles were less hygroscopic than accumulation mode particles (kappa approximate to 0.1 at D approximate to 50 nm; kappa approximate to 0.2 at D approximate to 200 nm), which is in agreement with earlier hygroscopicity tandem differential mobility analyzer (H-TDMA) studies. The CCN measurement results are consistent with aerosol mass spectrometry (AMS) data, showing that the organic mass fraction (f(org)) was on average as high as similar to 90% in the Aitken mode (D <= 100 nm) and decreased with increasing particle diameter in the accumulation mode (similar to 80% at D approximate to 200 nm). The kappa values exhibited a negative linear correlation with f(org) (R(2)=0.81), and extrapolation yielded the following effective hygroscopicity parameters for organic and inorganic particle components: kappa(org)approximate to 0.1 which can be regarded as the effective hygroscopicity of biogenic secondary organic aerosol (SOA) and kappa(inorg)approximate to 0.6 which is characteristic for ammonium sulfate and related salts. Both the size dependence and the temporal variability of effective particle hygroscopicity could be parameterized as a function of AMS-based organic and inorganic mass fractions (kappa(p)=kappa(org) x f(org)+kappa(inorg) x f(inorg)). The CCN number concentrations predicted with kappa(p) were in fair agreement with the measurement results (similar to 20% average deviation). The median CCN number concentrations at S=0.1-0.82% ranged from N(CCN,0.10)approximate to 35 cm(-3) to N(CCN,0.82)approximate to 160 cm(-3), the median concentration of aerosol particles larger than 30 nm was N(CN,30)approximate to 200 cm(-3), and the corresponding integral CCN efficiencies were in the range of N(CCN,0.10/NCN,30)approximate to 0.1 to N(CCN,0.82/NCN,30)approximate to 0.8. Although the number concentrations and hygroscopicity parameters were much lower in pristine rainforest air, the integral CCN efficiencies observed were similar to those in highly polluted megacity air. Moreover, model calculations of N(CCN,S) assuming an approximate global average value of kappa approximate to 0.3 for continental aerosols led to systematic overpredictions, but the average deviations exceeded similar to 50% only at low water vapor supersaturation (0.1%) and low particle number concentrations (<= 100 cm(-3)). Model calculations assuming aconstant aerosol size distribution led to higher average deviations at all investigated levels of supersaturation: similar to 60% for the campaign average distribution and similar to 1600% for a generic remote continental size distribution. These findings confirm earlier studies suggesting that aerosol particle number and size are the major predictors for the variability of the CCN concentration in continental boundary layer air, followed by particle composition and hygroscopicity as relatively minor modulators. Depending on the required and applicable level of detail, the information and parameterizations presented in this paper should enable efficient description of the CCN properties of pristine tropical rainforest aerosols of Amazonia in detailed process models as well as in large-scale atmospheric and climate models.

Aerosol number fluxes over the Amazon rain forest during the wet season

Number fluxes of particles with diameter larger than 10 nm were measured with the eddy covariance method over the Amazon rain forest during the wet season as part of the LBA (The Large Scale Biosphere Atmosphere Experiment in Amazonia) campaign 2008. The primary goal was to investigate whether sources or sinks dominate the aerosol number flux in the tropical rain forest-atmosphere system. During the measurement campaign, from 12 March to 18 May, 60% of the particle fluxes pointed downward, which is a similar fraction to what has been observed over boreal forests. The net deposition flux prevailed even in the absolute cleanest atmospheric conditions during the campaign and therefore cannot be explained only by deposition of anthropogenic particles. The particle transfer velocity v(t) increased with increasing friction velocity and the relation is described by the equation v(t) = 2.4x10(-3)xu(*) where u(*) is the friction velocity. Upward particle fluxes often appeared in the morning hours and seem to a large extent to be an effect of entrainment fluxes into a growing mixed layer rather than primary aerosol emission. In general, the number source of primary aerosol particles within the footprint area of the measurements was small, possibly because the measured particle number fluxes reflect mostly particles less than approximately 200 nm. This is an indication that the contribution of primary biogenic aerosol particles to the aerosol population in the Amazon boundary layer may be low in terms of number concentrations. However, the possibility of horizontal variations in primary aerosol emission over the Amazon rain forest cannot be ruled out.

Remote sensing the vertical profile of cloud droplet effective radius, thermodynamic phase, and temperature

Cloud-aerosol interaction is a key issue in the climate system, affecting the water cycle, the weather, and the total energy balance including the spatial and temporal distribution of latent heat release. Information on the vertical distribution of cloud droplet microphysics and thermodynamic phase as a function of temperature or height, can be correlated with details of the aerosol field to provide insight on how these particles are affecting cloud properties and their consequences to cloud lifetime, precipitation, water cycle, and general energy balance. Unfortunately, today's experimental methods still lack the observational tools that can characterize the true evolution of the cloud microphysical, spatial and temporal structure in the cloud droplet scale, and then link these characteristics to environmental factors and properties of the cloud condensation nuclei. Here we propose and demonstrate a new experimental approach (the cloud scanner instrument) that provides the microphysical information missed in current experiments and remote sensing options. Cloud scanner measurements can be performed from aircraft, ground, or satellite by scanning the side of the clouds from the base to the top, providing us with the unique opportunity of obtaining snapshots of the cloud droplet microphysical and thermodynamic states as a function of height and brightness temperature in clouds at several development stages. The brightness temperature profile of the cloud side can be directly associated with the thermodynamic phase of the droplets to provide information on the glaciation temperature as a function of different ambient conditions, aerosol concentration, and type. An aircraft prototype of the cloud scanner was built and flew in a field campaign in Brazil. The CLAIM-3D (3-Dimensional Cloud Aerosol Interaction Mission) satellite concept proposed here combines several techniques to simultaneously measure the vertical profile of cloud microphysics, thermodynamic phase, brightness temperature, and aerosol amount and type in the neighborhood of the clouds. The wide wavelength range, and the use of multi-angle polarization measurements proposed for this mission allow us to estimate the availability and characteristics of aerosol particles acting as cloud condensation nuclei, and their effects on the cloud microphysical structure. These results can provide unprecedented details on the response of cloud droplet microphysics to natural and anthropogenic aerosols in the size scale where the interaction really happens.

Spectral dependence of aerosol light absorption over the Amazon Basin

In this study, we examine the spectral dependence of aerosol absorption at different sites and seasons in the Amazon Basin. The analysis is based on measurements performed during three intensive field experiments at a pasture site (Fazenda Nossa Senhora, Rondonia) and at a primary forest site (Cuieiras Reserve, Amazonas), from 1999 to 2004. Aerosol absorption spectra were measured using two Aethalometers: a 7-wavelength Aethalometer (AE30) that covers the visible (VIS) to near-infrared (NIR) spectral range, and a 2-wavelength Aethalometer (AE20) that measures absorption in the UV and in the NIR. As a consequence of biomass burning emissions, about 10 times greater absorption values were observed in the dry season in comparison to the wet season. Power law expressions were fitted to the measurements in order to derive the absorption Angstrom exponent, defined as the negative slope of absorption versus wavelength in a log-log plot. At the pasture site, about 70% of the absorption Angstrom exponents fell between 1.5 and 2.5 during the dry season, indicating that biomass burning aerosols have a stronger spectral dependence than soot carbon particles. Angstrom exponents decreased from the dry to the wet season, in agreement with the shift from biomass burning aerosols, predominant in the fine mode, to biogenic and dust aerosols, predominant in the coarse mode. The lowest absorption Angstrom exponents (90% of data below 1.5) were observed at the forest site during the dry season. Also, results indicate that low absorption coefficients were associated with low Angstrom exponents. This finding suggests that biogenic aerosols from Amazonia have a weaker spectral dependence for absorption than biomass burning aerosols, contradicting our expectations of biogenic particles behaving as brown carbon. In a first order assessment, results indicate a small (<1 %) effect of variations in absorption Angstrom exponents on 24-h aerosol forcings, at least in the spectral range of 450-880 nm. Further studies should be taken to assess the corresponding impact in the UV spectral range. The assumption that soot spectral properties represent all ambient light absorbing particles may cause a misjudgment of absorption towards the UV, especially in remote areas. Therefore, it is recommended to measure aerosol absorption at several wavelengths to accurately assess the impact of non-soot aerosols on climate and on photochemical atmospheric processes.

Sources of carbonaceous aerosol in the Amazon basin

The quantification of sources of carbonaceous aerosol is important to understand their atmospheric concentrations and regulating processes and to study possible effects on climate and air quality, in addition to develop mitigation strategies. In the framework of the European Integrated Project on Aerosol Cloud Climate Interactions (EUCAARI) fine (D(p) < 2.5 mu m) and coarse (2.5 mu m < Dp < 10 mu m) aerosol particles were sampled from February to June (wet season) and from August to September (dry season) 2008 in the central Amazon basin. The mass of fine particles averaged 2.4 mu g m(-3) during the wet season and 4.2 mu g m(-3) during the dry season. The average coarse aerosol mass concentration during wet and dry periods was 7.9 and 7.6 mu g m(-3), respectively. The overall chemical composition of fine and coarse mass did not show any seasonality with the largest fraction of fine and coarse aerosol mass explained by organic carbon (OC); the average OC to mass ratio was 0.4 and 0.6 in fine and coarse aerosol modes, respectively. The mass absorbing cross section of soot was determined by comparison of elemental carbon and light absorption coefficient measurements and it was equal to 4.7 m(2) g(-1) at 637 nm. Carbon aerosol sources were identified by Positive Matrix Factorization (PMF) analysis of thermograms: 44% of fine total carbon mass was assigned to biomass burning, 43% to secondary organic aerosol (SOA), and 13% to volatile species that are difficult to apportion. In the coarse mode, primary biogenic aerosol particles (PBAP) dominated the carbonaceous aerosol mass. The results confirmed the importance of PBAP in forested areas. The source apportionment results were employed to evaluate the ability of global chemistry transport models to simulate carbonaceous aerosol sources in a regional tropical background site. The comparison showed an overestimation of elemental carbon (EC) by the TM5 model during the dry season and OC both during the dry and wet periods. The overestimation was likely due to the overestimation of biomass burning emission inventories and SOA production over tropical areas.

Sources of particulate matter: emission profile of biomass burning

Biomass burning is an important source of atmospheric Particulate Matter (PM) in Brazil: the burning of forests in the northwest and of sugar cane plantations in the southeast are important examples. The objective of this work is the measurement of the PM emission profile of burning of sugar cane and other characteristic vegetative burning in the region of Sao Carlos-SP/Brazil. Samples of PM(10) and PM(2.5) were collected in different conditions, including small laboratory controlled burnings and real ones. The samples were analysed by X-Ray Fluorescence (XRF) and 14 chemical elements quantified. t-Student tests were performed to compare the obtained profiles, using as a reference a vegetative burn profile taken from the USEPA data bank SPECIATE. All measured profiles presented significant amounts of Cl and K, which are confirmed as tracers of sugar cane foliage burning.

The effect of the generation and handling in the acquired electrostatic charge in airborne particles

The measurement of the charge distribution in laboratory generated aerosols particles was carried out. Four cases of electrostatic charge acquisition by aerosol particles were evaluated. In two of these cases. the charges acquired by the particles were naturally derived from the aerosol generation procedure itself, without using any additional charging method. Ill the other two cases, a corona charger and an impact charger were utilized as Supplementary methods for charge generation. Two types of aerosol generators were used in the dispersion of particles in the gas Stream: the vibrating orifice generator TSI model 3450 and the rotating plate generator TSI model 3433. In the vibrating orifice generator. a Solution of methylene blue Was used and the generated particles were mono-dispersed. Different mono-aerosols were generated with particle diameters varying from 6.0 x 10(-6) m to 1.4 x 10(-5) m. In the rotating plate generator, a poly-dispersed phosphate rock concentrate with Stokes mean diameter of 1.30 x 10(-6) m and size range between 1.5 x 10(-7) m and 8.0 x 10(-6) m Was utilized as powder material in all tests. In the tests performed with the mono-dispersed particles. the median charges of the particles varied between -3.0 x 10-(16) C and -5.0 x 10(-18) degrees C and a weak dependence between particle size and charge was observed. The particles were predominantly negatively charged. In the tests with the poly-dispersed particles the median charges varied fairly linearly with the particle diameter and were negative. The order of magnitude of the results obtained is in accordance with data reported in the literature. The charge distribution, in this case, was wider, so that an appreciable amount of particles were positively charged. The relative spread of the distribution varied with the charging method. It was also noticed that the corona charger acted very effectively in charging the particles. (C) 2008 Elsevier BY. All rights reserved.

A positive growth response to NaCl applications in Eucalyptus plantations established on K-deficient soils

Contrasting responses of Eucalyptus trees to K fertilizer applications have been reported on soils with low K contents. A complete randomized block experiment was set up in Brazil to test the hypothesis that large atmospheric deposits of NaCl in coastal regions might lead to a partial substitution of K by Na in Eucalyptus physiology and enhance tree growth. Treatments with application of 1.5, 3.0, 4.5 kmol K ha(-1) (K(1.5), K(3.0), 1(4.5, respectively) as KCl, 3.0 kmol K ha(-1) applied as K(2)SO(4), 3.0 kmol Na ha(-1) (Na(3.0)) as NaCl commercialized for cattle feeding, and a mixture of 1.5 kmol K + 1.5 kmol Na ha(-1) (K(1.5) + Na(1.5)) were compared to a control treatment (C) with no K and Na applications. All the plots were fertilized with large amounts of the other nutrients. A positive effect of NaCl applications on the growth of E. grandis trees was observed. NaCl and KCl additions in treatments Na(3.0) and K(3.0) increased above-ground biomass by 56% and 130% three years after planting, respectively, in comparison with the C treatment. By contrast, accumulated litterfall up to age 3 years was not significantly modified. NaCl applications in the Na(3.0) treatment significantly increased Na accumulation in above-ground tree components but did not modify K accumulation, whatever the sampling age. A partial substitution of K by Na in tree physiology, as observed for various agricultural crops, might explain this behaviour. Our results suggest the possibility of applying inexpensive K fertilizers, which are less purified in Na, and explain why high yields are achieved without K fertilizer applications in areas with large dry depositions of marine aerosols. Further investigations are necessary to identify the processes involving Na in Eucalyptus tree physiology. (C) 2009 Elsevier B.V. All rights reserved.

Model for gas-liquid flow through wet porous medium

A method involving bubbling of air through a fibrous filter immersed in water has recently been investigated (Agranovski et al. [1]). Experimental results showed that the removal efficiency for ultra-fine aerosols by such filters was greatly increased compared to dry filters. Nuclear Magnetic Resonance (NMR) imaging was used to examine the wet filter and to determine the nature of the gas flow inside the filter (Agranovski et al. [2]). It was found that tortuous preferential pathways (or flow tubes) develop within the filter through which the air flows and the distribution of air and water inside the porous medium has been investigated. The aim of this paper is to investigate the geometry of the pathways and to make estimates of the flow velocities and particle removal efficiency in such pathways. A mathematical model of the flow of air along the preferred pathways has been developed and verified experimentally. Even for the highest realistic gas velocity the flow field was essentially laminar (Re approximate to 250). We solved Laplace's equation for stream function to map trajectories of particles and gas molecules to investigate the possibility of their removal from the carrier.

Wet deposition of major ions in a rural area impacted by biomass burning emissions

This work concerns the influence of industrialized agriculture in the tropics on precipitation chemistry. A total of 264 rain events were sampled using a wet-only collector in central Sao Paulo State, Brazil, between January 2003 and July 2007. Electroneutrality balance calculations (considering H(+), K(+), Na(+), NH(4)(+), Ca(2)(+), Mg(2)(+), Cl(-), NO(3)(-), SO(4)(2-), F(-), PO(4)(3-), H(3)CCOO(-), HCOO(-), C(2)O(4)(2-) and HCO(3)(-)) showed that there was an excess of cations (similar to 15%), which was attributed to the presence of unmeasured organic anion species originating from biomass burning and biogenic emissions. On average, the three ions NH(4)(+), NO(3)(-) and H(+) were responsible for >55% of the total ion concentrations in the rainwater samples. Concentrations (except of H(+)) were significantly higher (t-test; P = 0.05), by between two to six-fold depending on species, during the winter sugar cane harvest period, due to the practice of pre-harvest burning of the crop. Principal component analysis showed that three components could explain 88% of the variance for measurements made throughout the year: PC1 (52%, biomass burning and soil dust resuspension); PC2 (26%, secondary aerosols); PC3 (10%, road transport emissions). Differences between harvest and non-harvest periods appeared to be mainly due to an increased relative importance of road transport/industrial emissions during the summer (non-harvest) period. The volume-weighted mean (VWM) concentrations of ammonium (23.4 mu mol L(-1)) and nitrate (17.5 mu mol L(-1)) in rainwater samples collected during the harvest period were similar to those found in rainwater from Sao Paulo city, which emphasizes the importance of including rural agro-industrial emissions in regional-scale atmospheric chemistry and transport models. Since there was evidence of a biomass burning source throughout the year, it appears that rainwater composition will continue to be affected by vegetation fires, even after sugar cane burning is phased out as envisaged by recent Sao Paulo State legislation. (C) 2011 Elsevier Ltd. All rights reserved.

The effects of air pollution on hospitalizations for cardiovascular disease in elderly people in Australian and New Zealand cities

OBJECTIVE: The goal of this study was to estimate the associations between outdoor air pollution and cardiovascular hospital admissions for the elderly. DESIGN: Associations were assessed using the case-crossover method for seven cities: Auckland and Christchurch, New Zealand; and Brisbane, Canberra, Melbourne, Perth, and Sydney Australia. Results were combined across cities using a random-effects meta-analysis and stratified for two adult age groups: 15-64 years and >= 65 years of age (elderly). Pollutants considered were nitrogen dioxide, carbon monoxide, daily measures of particulate matter (PM) and ozone. Where multiple pollutant associations were found, a matched case-control analysis was used to identify the most consistent association. RESULTS: In the elderly, all pollutants except 03 were significantly associated with five categories or cardiovascular disease admissions. No associations were found for arrhythmia and stroke. For a 0.9-ppm increase in CO, there were significant increases in elderly hospital admissions for total cardiovascular disease (2.2%), all cardiac disease (2.8%), cardiac failure (6.0%), ischemic heart disease (2.3%), and myocardial infarction (2.9%). There was some heterogeneity between cities, possibly due to differences in humidity and the percentage of elderly people. In matched analyses, CO had the most consistent association. CONCLUSIONS. The results suggest that air pollution arising from common emission sources for CO, NO2, and PM (e.g., motor vehicle exhausts) has significant associations with adult cardiovascular hospital admissions, especially in the elderly, at air pollution concentrations below normal health guidelines. RELEVANCE TO CLINICAL AND PROFESSIONAL PRACTICE: Elderly populations in Australia need to be protected from air pollution arising from outdoor sources to reduce cardiovascular disease.

Associations involving delays (particularly long delays) between certain weather parameters and geomagnetic activity

Four sunspot-minimum periods (1963-1966, 1971-1977, 1983-1987 and 1992-1997) have been examined for the results which are presented. Using several different weather parameters, tropospheric gravity waves, enhanced cold fronts and two rainfall data sets in Eastern Australia, associations at reasonably high levels of significance have been found with enhanced geomagnetic activity (EGA). Statistically this EGA involved either short delays of several days or long delays of about 20 days. The geomagnetic parameters used were (a) the AE index (b) the hourly H component for a number of stations and (c) the daily K-P-sum value. The K-P-sum analyses have shown that the EGA associated with the delays form part of four or five cycles of recurrent geomagnetic activity for 27-day periodicities. Furthermore statistically two recurrent cycles are found to exist concurrently, one apparently related to the short delays and the other to the long delays. Periodicities of 13.5 days are created because the two sets are displaced from each other by approximately this interval. A brief reference is made to the 13.5 periodicity known to exist for geomagnetic activity and the evidence in the literature for active regions on the sun to be displaced by 180 degrees of solar longitude.

Aerosolization of protein solutions using thermal inkjet technology

Vapotronics Inc. is developing the thermal inkjet (TIJ) technology used extensively in the printer industry to create a digital aerosol inhaler for the inhalation of therapeutics for local and systemic delivery. The operation of thermal inkjet printers requires generation of high temperatures and vaporization of the liquid formulation to effect droplet ejection. A study was conducted to develop formulations that would permit the generation of aerosols of therapeutic proteins without damage to the inkjet system or degradation of the proteins. Two proteins, human growth hormone and insulin, were formulated and aerosolized. The aerosol was collected and subjected to assays to compare the physicochemical and biological activities of these proteins before and after aerosolization. In each case, there was no significant changes to the proteins as a result of the aerosolization, providing evidence that TIJ can be used for aerosolizing solutions of protein therapeutics.

Study of wet porous filtration

A growing demand for efficient air quality management calls for the development of technologies capable of meeting the stringent requirements now being applied in areas of chemical, biological and medical activities. Currently, filtration is the most effective process available for removal of fine particles from carrier gases. Purification of gaseous pollutants is associated with adsorption, absorption and incineration. In this paper we discuss a new technique for highly efficient simultaneous purification of gaseous and particulate pollutants from carrier gases, and investigate the utilization of Nuclear Magnetic Resonance (NMR) imaging for the study of the dynamic processes associated with gas-liquid flow in porous media. Our technique involves the passage of contaminated carrier gases through a porous medium submerged into a liquid, leading to the formation of narrow and tortuous pathways through the medium. The wet walls of these pathways result in outstanding purification of gaseous, liquid and solid alien additives. NMR imaging was successfully used to map the gas pathways inside the porous medium submerged into the liquid layer. (C) 2002 Elsevier Science B.V. All rights reserved.

Parâmetros bioquímicos foliares das espécies Licania tomentosa (Benth.) e Bauhinia forficata (Link.) para avaliação da qualidade do ar

Foliar analysis of biochemical parameters were carried out in order to investigate the influence of air pollutants on two tropical tree species (Licania tomentosa (Benth.) and Bauhinia forfícata (Link.)). Special attention was given to tropospheric ozone due to the fact that concentration levels in the region were found to be up to 140 µg m-3 for a 4 h average time, which is well above the value that can cause injuries to orchides and tobacco (59 µg m-3). Other pollutants such as nitrogen and sulphur oxides were measured and their ambient concentrations were also associated to biochemical alterations in the investigated species.