Abstract. We compare a full-year (2006) record of surface air NO 2 concentrations measured in Israeli cities to coinciding retrievals of tropospheric NO 2 columns from satellite sensors (SCIAMACHY aboard ENVISAT and OMI aboard Aura). This provides a large statistical data set for validation of NO 2 satellite measurements in urban air, where validation is difficult yet crucial for using these measurements to infer NO x emissions by inverse modeling. Assuming that NO 2 is well-mixed throughout the boundary layer (BL), and using observed average seasonal boundary layer heights, near-surface NO 2 concentrations are converted into BL NO 2 columns. The agreement between OMI and (13:45) BL NO 2 columns (slope=0.93, n=542), and the comparable results at 10:00 h for SCIAMACHY, allow a validation of the seasonal, weekly, and diurnal cycles in satellite-derived NO 2 . OMI and BL NO 2 columns show consistent seasonal cycles (winter NO 2 1.6-2.7× higher than summer). BL and coinciding OMI columns both show a strong weekly cycle with 45-50% smaller NO 2 columns on Saturday relative to the weekday mean, reflecting the reduced weekend activity, and validating the weekly cycle observed from space. The diurnal difference between SCIAMACHY (10:00) and OMI (13:45) NO 2 is maximum in summer when SCIAMACHY is up to 40% higher than OMI, and minimum in winter when OMI slightly exceeds SCIAMACHY. A similar seasonal variation in the diurnal difference is found in the source region of Cairo. The surface measurements in Israel cities confirm this seasonal variation in the diurnal cycle. Using simulations from Correspondence to: F. Boersma (boersma@knmi.nl) a global 3-D chemical transport model (GEOS-Chem), we show that this seasonal cycle can be explained by a much stronger photochemical loss of NO 2 in summer than in winter.
Abstract. The heterogeneous reaction between gas phase glyoxal and ammonium sulfate (AS) aerosols, a proxy for inorganic atmospheric aerosol, was studied in terms of the dependence of the optical, physical and chemical properties of the product aerosols on initial particle size and ambient relative humidity (RH). Our experiments imitate an atmospheric scenario of a dry particle hydration at ambient RH conditions in the presence of glyoxal gas followed by efflorescence due to decrease of the ambient RH. The reactions were studied under different RH conditions, starting from dry conditions (∼20 % RH) and up to 90 % RH, covering conditions prevalent in many atmospheric environments, and followed by consequent drying of the reacted particles before their analysis by the aerosol mass spectrometer (AMS), cavity ring down (CRD) and scanning mobility particle sizer (SMPS) systems. At λ = 355 nm, the reacted aerosols demonstrate a substantial growth in optical extinction cross section, as well as in mobility diameter under a broad range of RH values (35-90 %). The ratio of the product aerosol to seed aerosol geometric cross section reached up to ∼3.5, and the optical extinction cross-section up to ∼250. The reactions show a trend of increasing physical and optical growth with decreasing seed aerosol size, from 100 nm to 300 nm, as well as with decreasing RH values from 90 % to ∼40 %. Optically inactive aerosols, at the limit of the Mie range (100 nm diameter) become optically active as they grow due to the reaction. AMS analyses of the reaction of 300 nm AS at RH values of 50 %, 75 % and 90 % show that the main products of the reaction are glyoxal oligomers, formed by acetal formation in the presence of AS. In addition, imidaCorrespondence to: Y. Rudich (yinon.rudich@weizmann.ac.il) zole formation, which is a minor channel, is observed for all reactions, yielding a product which absorbs at λ = 290 nm, with possible implications on the radiative properties of the product aerosols. The ratio of absorbing substances (C-N compounds, including imidazoles) increases with increasing RH value. A core/shell model used for the investigation of the optical properties of the reaction products of AS with gas phase glyoxal, shows that the refractive index (RI) of the reaction products are n = 1.68(±0.10) + 0.01(±0.02) at 50 % RH and n = 1.65(±0.06) + 0.02(±0.01) at 75 % RH at 355 nm. The observed increase in the ratio of the absorbing substances is not indicated in the imaginary part of the products at RH 50 % and 75 %. A further increase in the ratio of absorbing substances and a resulting increase in the imaginary part of the RI at higher RH values is expected, and may become even more substantial after longer reaction times, possibly in cloud or fog droplets. This study shows that the reaction of abundant substances present in atmospheric aerosols, such as AS, and gas phase glyoxal alters the aerosols' optical, physical and chemical properties and may have implications on the radiative effect of these aerosols.
Phytoplankton blooms are ephemeral events of exceptionally high primary productivity that regulate the flux of carbon across marine food webs [1-3]. Quantification of bloom turnover [4] is limited by a fundamental difficulty to decouple between physical and biological processes as observed by ocean color satellite data. This limitation hinders the quantification of bloom demise and its regulation by biological processes [5, 6], which has important consequences on the efficiency of the biological pump of carbon to the deep ocean [7-9]. Here, we address this challenge and quantify algal blooms' turnover using a combination of satellite and in situ data, which allows identification of a relatively stable oceanic patch that is subject to little mixing with its surroundings. Using a newly developed multisatellite Lagrangian diagnostic, we decouple the contributions of physical and biological processes, allowing quantification of a complete life cycle of a mesoscale (∼10-100 km) bloom of coccolithophores in the North Atlantic, from exponential growth to its rapid demise. We estimate the amount of organic carbon produced during the bloom to be in the order of 24,000 tons, of which two-thirds were turned over within 1 week. Complimentary in situ measurements of the same patch area revealed high levels of specific viruses infecting coccolithophore cells, therefore pointing at the importance of viral infection as a possible mortality agent. Application of the newly developed satellite-based approaches opens the way for large-scale quantification of the impact of diverse environmental stresses on the fate of phytoplankton blooms and derived carbon in the ocean.
This study focuses on the heterogeneous reactions of gas phase glyoxal with aerosols of glycine, the most abundant amino acid in atmospheric aerosols, as well as with a mixture of glycine and ammonium sulfate (AS) at a molar ratio of 1:100 (glycine-AS 1:100). Aerosols were exposed to varying relative humidity (RH) conditions in the presence of gas phase glyoxal for ∼1 h, followed by drying and efflorescence. The changes in size, chemical composition, and optical properties were consequently measured. The reactions occur over a wide range of relative humidities, from ∼30% up to 90% RH, covering values that are substantially lower as well as above the deliquescence point of the investigated aerosols. The product aerosols exhibit a trend of increasing growth in size, in optical extinction cross sections, and in extinction efficiencies (at λ = 355 nm) with decreasing seed aerosol size, and with decreasing RH values from 90% to ∼50%. For glycine-AS 1:100 particles, the ratio of the geometric cross section of the product aerosol to the original seed aerosol reached a value of ∼3, the optical extinction cross section ratio was up to ∼25, and the Q(ext) ratio was up to ∼8, exceeding those of both AS and glycine separately, suggesting a synergistic effect. Aerosol mass spectrometer analyses show that the main products of all the studied reactions are glyoxal oligomers (light scattering compounds), with a minor contribution from imidazoles (absorbing compounds at λ = 355 nm). These findings imply that the changes in the optical properties are likely due to enhanced scattering by the reaction products. The fraction of absorbing substances in the reacted aerosol increases with increasing RH, suggesting that the absorption component may become more substantial after longer reaction times, possibly in cloud or fog droplets. The results suggest that these reactions are possibly important in low RH regions, plausibly due to the reaction occurring in a few interfacial monolayers of water well before deliquescence.
Anthropogenic pollution from marine microplastic particles is a growing concern, both as a source of toxic compounds, and because they can transport pathogens and other pollutants. Airborne microplastic particles were previously observed over terrestrial and coastal locations, but not in the remote ocean. Here, we collected ambient aerosol samples in the North Atlantic Ocean, including the remote marine atmosphere, during the Tara Pacific expedition in May-June 2016, and chemically characterized them using micro-Raman spectroscopy. We detected a range of airborne microplastics, including polystyrene, polyethylene, polypropylene, and poly-silicone compounds. Polyethylene and polypropylene were also found in seawater, suggesting local production of airborne microplastic particles. Terminal velocity estimations and back trajectory analysis support this conclusion. For technical reasons, only particles larger than 5 µm, at the upper end of a typical marine atmospheric size distribution, were analyzed, suggesting that our analyses underestimate the presence of airborne microplastic particles in the remote marine atmosphere.
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