Abstract. We present here the optical properties of humiclike substances (HULIS) isolated from the fine fraction of biomass-burning aerosol collected in the Amazon basin during the LBA-SMOCC (Large scale Biosphere atmosphere experiment in Amazonia -SMOke aerosols, Clouds, rainfall and Climate) experiment in September 2002. From the isolated HULIS, aerosol particles were generated and their scattering and absorption coefficients measured. The size distribution and mass of the particles were also recorded. The value of the index of refraction was derived from "closure" calculations based on particle size, scattering and absorption measurements. On average, the complex index of refraction at 532 nm of HULIS collected during day and nighttime was 1.65-0.0019i and 1.69-0.0016i, respectively. In addition, the imaginary part of the complex index of refraction was calculated using the measured absorption coefficient of the bulk HULIS.The mass absorption coefficient of the HULIS at 532 nm was found to be quite low (0.031 and 0.029 m 2 g −1 for the day and night samples, respectively). However, due to the high absorptionÅngström exponent (6-7) of HULIS, the specific absorption increases substantially towards shorter wavelengths (∼2-3 m 2 g −1 at 300 nm), causing a relatively high (up to 50%) contribution to the light absorption of our Amazonian aerosol at 300 nm. For the relative contribution of HULIS to light absorption in the entire solar spectrum, lower values (6.4-8.6%) are obtained, but those are still not negligible.

The aerosol light absorption coefficient is an essential parameter involved in atmospheric radiation budget calculations. The Aethalometer (AE) has the great advantage of measuring the aerosol light absorption coefficient at several wavelengths, but the derived absorption coefficients are systematically too high when compared to reference methods. Up to now, four different correction algorithms of the AE absorption coefficients have been proposed by several authors. A new correction scheme based on these previously published methods has been developed, which accounts for the optical properties of the aerosol particles embedded in the filter. All the corrections have been tested on six datasets representing different aerosol types and loadings and include multi-wavelength AE and white-light AE. All the corrections have also been evaluated through comparison with a Multi-Angle Absorption Photometer (MAAP) for four datasets lasting between 6 months and five years. The modification of the wavelength dependence by the different corrections is analyzed in detail. The performances and the limits of all AE corrections are determined and recommendations are given

This study addresses the cellular uptake and intracellular trafficking of 15-nm gold nanoparticles (NPs), either plain (i.e., stabilized with citrate) or coated with polyethylene glycol (PEG), exposed to human alveolar epithelial cells (A549) at the air-liquid interface for 1, 4, and 24 h. Quantitative analysis by stereology on transmission electron microscopy images reveals a significant, nonrandom intracellular distribution for both NP types. No particles are observed in the nucleus, mitochondria, endoplasmic reticulum, or golgi. The cytosol is not a preferred cellular compartment for both NP types, although significantly more PEG-coated than citrate-stabilized NPs are present there. The preferred particle localizations are vesicles of different sizes (<150, 150-1000, >1000 nm). This is observed for both NP types and indicates a predominant uptake by endocytosis. Subsequent inhibition of caveolin- and clathrin-mediated endocytosis by methyl-beta-cyclodextrin (MbetaCD) results in a significant reduction of intracellular NPs. The inhibition, however, is more pronounced for PEG-coated than citrate-stabilized NPs. The latter are mostly found in larger vesicles; therefore, they are potentially taken up by macropinocytosis, which is not inhibited by MbetaCD. With prolonged exposure times, both NPs are preferentially localized in larger-sized intracellular vesicles such as lysosomes, thus indicating intracellular particle trafficking. This quantitative evaluation reveals that NP surface coatings modulate endocytotic uptake pathways and cellular NP trafficking. Other nonendocytotic entry mechanisms are found to be involved as well, as indicated by localization of a minority of PEG-coated NPs in the cytosol.

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Abstract. Spectral aerosol light absorption is an important parameter for the assessment of the radiation budget of the atmosphere. Although on-line measurement techniques for aerosol light absorption, such as the Aethalometer and the Particle Soot Absorption Photometer (PSAP), have been available for two decades, they are limited in accuracy and spectral resolution because of the need to deposit the aerosol on a filter substrate before measurement. Recently, a 7-wavelength (λ) Aethalometer became commercially available, which covers the visible (VIS) to near-infrared (NIR) spectral range (λ=450-950 nm), and laboratory calibration studies improved the degree of confidence in these measurement techniques. However, the applicability of the laboratory calibration factors to ambient conditions has not been investigated thoroughly yet.As part of the LBA-SMOCC (Large scale Biosphere atmosphere experiment in Amazonia -SMOke aerosols, Clouds, rainfall and Climate) campaign from September to November 2002 in the Amazon basin we performed an extensive field calibration of a 1-λ PSAP and a 7-λ Aethalometer utilizing a photoacoustic spectrometer (PAS, 532 nm) as reference device. Especially during the dry period of the campaign, the aerosol population was dominated by pyrogenic emissions. The most pronounced artifact of integrating-plate type attenuation techniques (e.g. Aethalometer, PSAP) is due to multiple scattering effects within the filter matrix. ForCorrespondence to: O. Schmid (oschmid@mpch-mainz.mpg.de) the PSAP, we essentially confirmed the laboratory calibration factor by Bond et al. (1999). On the other hand, for the Aethalometer we found a multiple scattering enhancement of 5.23 (or 4.55, if corrected for aerosol scattering), which is significantly larger than the factors previously reported (∼2) for laboratory calibrations. While the exact reason for this discrepancy is unknown, the available data from the present and previous studies suggest aerosol mixing (internal versus external) as a likely cause. For Amazonian aerosol, we found no absorption enhancement due to hygroscopic particle growth in the relative humidity (RH) range between 40% and 80%. However, a substantial bias in PSAP sensitivity that correlated with both RH and temperature (T) was observed for 20%

BackgroundEngineered nanoparticles are becoming increasingly ubiquitous and their toxicological effects on human health, as well as on the ecosystem, have become a concern. Since initial contact with nanoparticles occurs at the epithelium in the lungs (or skin, or eyes), in vitro cell studies with nanoparticles require dose-controlled systems for delivery of nanoparticles to epithelial cells cultured at the air-liquid interface.ResultsA novel air-liquid interface cell exposure system (ALICE) for nanoparticles in liquids is presented and validated. The ALICE generates a dense cloud of droplets with a vibrating membrane nebulizer and utilizes combined cloud settling and single particle sedimentation for fast (~10 min; entire exposure), repeatable (<12%), low-stress and efficient delivery of nanoparticles, or dissolved substances, to cells cultured at the air-liquid interface. Validation with various types of nanoparticles (Au, ZnO and carbon black nanoparticles) and solutes (such as NaCl) showed that the ALICE provided spatially uniform deposition (<1.6% variability) and had no adverse effect on the viability of a widely used alveolar human epithelial-like cell line (A549). The cell deposited dose can be controlled with a quartz crystal microbalance (QCM) over a dynamic range of at least 0.02-200 μg/cm2. The cell-specific deposition efficiency is currently limited to 0.072 (7.2% for two commercially available 6-er transwell plates), but a deposition efficiency of up to 0.57 (57%) is possible for better cell coverage of the exposure chamber.Dose-response measurements with ZnO nanoparticles (0.3-8.5 μg/cm2) showed significant differences in mRNA expression of pro-inflammatory (IL-8) and oxidative stress (HO-1) markers when comparing submerged and air-liquid interface exposures. Both exposure methods showed no cellular response below 1 μg/cm2 ZnO, which indicates that ZnO nanoparticles are not toxic at occupationally allowed exposure levels.ConclusionThe ALICE is a useful tool for dose-controlled nanoparticle (or solute) exposure of cells at the air-liquid interface. Significant differences between cellular response after ZnO nanoparticle exposure under submerged and air-liquid interface conditions suggest that pharmaceutical and toxicological studies with inhaled (nano-)particles should be performed under the more realistic air-liquid interface, rather than submerged cell conditions.

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