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The recent ACE-2, EPIC and DYCOMS-II field experiments showed that the drizzle precipitation rate of marine stratocumulus scales with the cloud geometrical thickness or liquid water path, and the droplet concentration, when averaged over a domain typical of a GCM grid. This feature is replicated here with large-eddy-simulations using state-of-the-art bulk parameterizations of precipitation formation in stratocumulus clouds. The set of numerical simulations shows scaling relationships similar to the ones derived from the field experiments, especially the one derived from the DYCOMS-II data set. This result suggests that the empirical relationships were not fortuitous and that they reflect the mean effect of cloud physical processes. Such relationships might be more suited to GCM parameterizations of precipitation from shallow clouds than bulk parameterizations of autoconversion, that were initially developed for cloud resolving models.
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Some effects in the biosphere from the Total Solar Eclipse of 29 March 2006 were investigated in field crops and marine zooplankton. Taking into account the decisive role of light on plant life and productivity, measurements of photosynthesis and stomatal behaviour were conducted on seven important field-grown cereal and leguminous crops. A drop in photosynthetic rates, by more than a factor of 5 in some cases, was observed, and the minimum values of photosynthetic rates ranged between 3.13 and 10.13 μmol CO<sub>2</sub> m<sup>−2</sup> s<sup>−1</sup>. The drop in solar irradiance and the increase in mesophyll CO<sub>2</sub>-concentration during the eclipse did not induce stomatal closure thus not blocking CO<sub>2</sub> uptake by plants. Light effects on the photochemical phase of photosynthesis may be responsible for the observed depression in photosynthetic rates. Field studies addressing the migratory responses of marine zooplankton (micro-zooplankton (ciliates), and meso-zooplankton) due to the rapid changes in underwater light intensity were also performed. The light intensity attenuation was simulated with the use of accurate underwater radiative transfer modeling techniques. Ciliates, responded to the rapid decrease in light intensity during the eclipse adopting night-time behaviour. From the meso-zooplankton assemblage, various vertical migratory behaviours were adopted by different species.
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A new parameterization of the lightning-produced NO<sub>x</sub> has been developed for cloud-resolving models. This parameterization is based on the unique characteristics of identifying which convective cells are capable of producing lightning based on a vertical velocity threshold and estimating the lightning flash rate in each convective cell from the non-precipitation and precipitation ice mass flux product. Further, the source location is filamentary instead of volumetric as in most previous parameterizations. <br><br> This parameterization has been tested on the 10 July 1996 Stratospheric-Tropospheric Experiment: Radiation, Aerosols and Ozone (STERAO) storm. Comparisons of the simulated flash rate and NO mixing ratio (control experiment) with observations at different locations and stages of the storm show good agreement. An individual flash produces on average 121±41 moles of NO (7.3±2.5×10<sup>25</sup> molecules NO) for the simulated high cloud base, high shear storm that is dominated by intra-cloud flash activity. Sensitivity tests have been performed to study the impact of the flash rate, the cloud-to-ground flash ratio, the flash length, the spatial distribution of the NO molecules, and the production rate per flash on the NO concentration and distribution. Results show a strong impact from the flash rate, the spatial placement of the lightning-NO<sub>x</sub> source and the number of moles produced per flash. On the other hand, the simulations show almost no impact from the different cloud-to-ground (<i>CG</i>) ratios and the lightning-NO<sub>x</sub> production rates per <i>CG</i> flash used as input to the model.
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Measurements of the submicron fraction of the atmospheric aerosol in the marine boundary layer were performed from January to March 2007 (Southern Hemisphere summer) onboard the French research vessel <i>Marion Dufresne</i> in the Southern Atlantic and Indian Ocean (20° S–60° S, 70° W–60° E). We used an Aerodyne High-Resolution-Time-of-Flight AMS to characterize the chemical composition and to measure species-resolved size distributions of non-refractory aerosol components in the submicron range. <br><br> Within the "standard" AMS compounds (ammonium, chloride, nitrate, sulfate, organics) "sulfate" is the dominant species in the marine boundary layer with concentrations ranging between 50 ng m<sup>−3</sup> and 3 μg m<sup>−3</sup>. Furthermore, what is seen as "sulfate" by the AMS is likely comprised mostly of sulfuric acid. <br><br> Another sulfur containing species that is produced in marine environments is methanesulfonic acid (MSA). There have been previously measurements of MSA using an Aerodyne AMS. However, due to the use of an instrument equipped with a quadrupole detector with unit mass resolution it was not possible to physically separate MSA from other contributions to the same <i>m/z</i>. In order to identify MSA within the HR-ToF-AMS raw data and to extract mass concentrations for MSA from the field measurements the standard high-resolution MSA fragmentation patterns for the measurement conditions during the ship campaign (e.g. vaporizer temperature) needed to be determined. <br><br> To identify characteristic air masses and their source regions backwards trajectories were used and averaged concentrations for AMS standard compounds were calculated for each air mass type. Sulfate mass size distributions were measured for these periods showing a distinct difference between oceanic air masses and those from African outflow. While the peak in the mass distribution was roughly at 250 nm (vacuum aerodynamic diameter) in marine air masses, it was shifted to 470 nm in African outflow air. Correlations between the mass concentrations of sulfate, organics and MSA show a narrow correlation for MSA with sulfate/sulfuric acid coming from the ocean, but not with continental sulfate.
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The concern of adverse health impacts from exposure to vehicle-emitted nanoparticles has been escalating over the past few years. In order to meet more stringent EPA emission standards for particle mass emissions, advanced exhaust after-treatment systems such as continuously regenerating diesel particle filters (CRDPFs) have to be employed on vehicles and fuel with ultra-low sulfur is to be used. Although CRDPFs were found to be effective in reducing particle mass emissions, they were revealed to increase the potential of volatile nanoparticle formation. Significant nanoparticle concentrations have also been detected for vehicles running on ultra-low sulfur fuel but without CRDPFs. The main focus of this paper is the formation and evolution of nanoparticles in an exhaust plume under ultra-low sulfur conditions. Such a study is necessary to project future nanoparticle emissions as fuel compositions and after-treatment systems change. We have carried out a comprehensive quantitative assessment of the effects of enhanced sulfur conversion efficiency, sulfur storage/release, and presence of non-volatile cores on nanoparticle formation using a detailed composition resolved aerosol microphysical model with a recently improved H<sub>2</sub>SO<sub>4</sub>-H<sub>2</sub>O homogeneous nucleation (BHN) module. Two well-controlled case studies show good agreement between model predictions and measurements in terms of particle size distribution and temperature dependence of particle formation rate, which leads us to conclude that BHN is the main source of nanoparticles for vehicles equipped with CRDPFs. We found that the employment of CRDPFs may lead to the higher number concentration of nanoparticles (but smaller size) in the exhaust of vehicles running on ultra-low sulfur fuel compared to those emitted from vehicles running on high sulfur fuel. We have also shown that the sulfate storage and release effect can lead to significant enhancement in nanoparticle production under favorable conditions. For vehicles running on ultra-low sulfur fuel but without CRDPFs, the BHN is negligible; however, the condensation of low volatile organic compounds on nanometer-sized non-volatile cores may explain the observed nucleation mode particles.
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The cloud scanner sensor is a central part of a recently proposed satellite remote sensing concept – the three-dimensional (3-D) cloud and aerosol interaction mission (CLAIM-3D) combining measurements of aerosol characteristics in the vicinity of clouds and profiles of cloud microphysical characteristics. Such a set of collocated measurements will allow new insights in the complex field of cloud-aerosol interactions affecting directly the development of clouds and precipitation, especially in convection. The cloud scanner measures radiance reflected or emitted by cloud sides at several wavelengths to derive a profile of cloud particle size and thermodynamic phase. For the retrieval of effective size a Bayesian approach was adopted and introduced in a preceding paper. <br><br> In this paper the potential of the approach, which has to account for the complex three-dimensional nature of cloud geometry and radiative transfer, is tested in realistic cloud observing situations. In a fully simulated environment realistic cloud resolving modelling provides complex 3-D structures of ice, water, and mixed phase clouds, from the early stage of convective development to mature deep convection. A three-dimensional Monte Carlo radiative transfer is used to realistically simulate the aspired observations. <br><br> A large number of cloud data sets and related simulated observations provide the database for an experimental Bayesian retrieval. An independent simulation of an additional cloud field serves as a synthetic test bed for the demonstration of the capabilities of the developed retrieval techniques. For this test case only a minimal overall bias in the order of 1% as well as pixel-based uncertainties in the order of 1 μm for droplets and 8 μm for ice particles were found for measurements at a high spatial resolution of 250 m.
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Unsaturated fatty acids are important constituents of the organic fraction of atmospheric aerosols originating from biogenic or combustion sources. Oxidative processing of these may change their interaction with water and thus affect their effect on climate. The ozonolysis of oleic and arachidonic acid aerosol particles was studied under humid conditions in a flow reactor at ozone exposures close to atmospheric levels, at concentrations between 0.5 and 2 ppm. While oleic acid is a widely used proxy for such studies, arachidonic acid represents polyunsaturated fatty acids, which may decompose into hygroscopic products. The hygroscopic (diameter) growth factor at 93% relative humidity (RH) of the oxidized arachidonic particles increased up to 1.09 with increasing RH during the ozonolysis. In contrast, the growth factor of oleic acid was very low (1.03 at 93% RH) and was almost invariant to the ozonolysis conditions, so that oleic acid is not a good model to observe oxidation induced changes of hygroscopicity under atmospheric conditions. We show for arachidonic acid particles that the hygroscopic changes induced by humidity during ozonolysis are accompanied by about a doubling of the ratio of carboxylic acid protons to aliphatic protons. We suggest that, under humid conditions, the reaction of water with the Criegee intermediates might open a pathway for the formation of smaller acids that lead to more significant changes in hygroscopicity. Thus the effect of water to provide a competing pathway during ozonolysis observed in this study should be motivation to include water, which is ubiquitously present in and around atmospheric particles, in future studies related to aerosol particle aging.
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The optical properties of sea-salt aerosol have been parameterized at shortwave and longwave wavelengths. The optical properties were parameterized in a simple functional form in terms of the ambient relative humidity based on Mie optical property calculations. The proposed parameterization is tested relative to Mie calculations and is found to be accurate to within a few percent. In the parameterization, the effects of the size distribution on the optical properties are accounted for in terms of effective radius of the sea-salt size distribution. This parameterization differs from previous works by being formulated directly with the wet sea-salt size distribution and, to our knowledge, this is the first published sea-salt parameterization to provide a parameterization for both shortwave and longwave wavelengths. <br><br> We have used this parameterization in a set of idealized 1-D radiative transfer calculations to investigate the sensitivity of various attributes of sea-salt forcing, including the dependency on sea-salt column loading, effective variance, solar angle, and surface albedo. From these sensitivity tests, it is found that sea-salt forcings for both shortwave and longwave spectra are linearly related to the sea-salt loading for realistic values of loadings. The radiative forcing results illustrate that the shortwave forcing is an order of magnitude greater than the longwave forcing results and opposite in sign, for various loadings. Forcing sensitivity studies show that the influence of effective variance for sea-salt is minor; therefore, only one value of effective variance is used in the parameterization. The dependence of sea-salt forcing with solar zenith angle illustrates an interesting result that sea-salt can generate a positive top-of-the-atmosphere result (i.e. warming) when the solar zenith angle is relatively small (i.e. <30°). Finally, it is found that the surface albedo significantly affects the shortwave radiative forcing, with the forcing diminishing to zero as the surface albedo tends to unity.
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The Atmospheric Chemistry Experiment (ACE), also known as SCISAT, was launched on 12 August 2003, carrying two instruments that measure vertical profiles of atmospheric constituents using the solar occultation technique. One of these instruments, the ACE Fourier Transform Spectrometer (ACE-FTS), is measuring volume mixing ratio (VMR) profiles of nitrous oxide (N<sub>2</sub>O) from the upper troposphere to the lower mesosphere at a vertical resolution of about 3–4 km. In this study, the quality of the ACE-FTS version 2.2 N<sub>2</sub>O data is assessed through comparisons with coincident measurements made by other satellite, balloon-borne, aircraft, and ground-based instruments. These consist of vertical profile comparisons with the SMR, MLS, and MIPAS satellite instruments, multiple aircraft flights of ASUR, and single balloon flights of SPIRALE and FIRS-2, and partial column comparisons with a network of ground-based Fourier Transform InfraRed spectrometers (FTIRs). Between 6 and 30 km, the mean absolute differences for the satellite comparisons lie between −42 ppbv and +17 ppbv, with most within ±20 ppbv. This corresponds to relative deviations from the mean that are within ±15%, except for comparisons with MIPAS near 30 km, for which they are as large as 22.5%. Between 18 and 30 km, the mean absolute differences for the satellite comparisons are generally within ±10 ppbv. From 30 to 60 km, the mean absolute differences are within ±4 ppbv, and are mostly between −2 and +1 ppbv. Given the small N<sub>2</sub>O VMR in this region, the relative deviations from the mean are therefore large at these altitudes, with most suggesting a negative bias in the ACE-FTS data between 30 and 50 km. In the comparisons with the FTIRs, the mean relative differences between the ACE-FTS and FTIR partial columns (which cover a mean altitude range of 14 to 27 km) are within ±5.6% for eleven of the twelve contributing stations. This mean relative difference is negative at ten stations, suggesting a small negative bias in the ACE-FTS partial columns over the altitude regions compared. Excellent correlation (<i>R</i>=0.964) is observed between the ACE-FTS and FTIR partial columns, with a slope of 1.01 and an intercept of −0.20 on the line fitted to the data.
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We have analyzed one year (July 2006–July 2007) of measurement data from a relatively clean background site located in dry savannah in South Africa. The annual-median trace gas concentrations were equal to 0.7 ppb for SO<sub>2</sub>, 1.4 ppb for NO<sub>x</sub>, 36 ppb for O<sub>3</sub> and 105 ppb for CO. The corresponding PM<sub>1</sub>, PM<sub>2.5</sub> and PM<sub>10</sub> concentrations were 9.0, 10.5 and 18.8 μg m<sup>−3</sup>, and the annual median total particle number concentration in the size range 10–840 nm was 2340 cm<sup>−3</sup>. During Easterly winds, influence of industrial sources approximately 150 km away from the measurement site was clearly visible, especially in SO<sub>2</sub> and NO<sub>x</sub> concentrations. Of gases, NO<sub>x</sub> and CO had a clear annual, and SO<sub>2</sub>, NO<sub>x</sub> and O<sub>3</sub> clear diurnal cycle. Atmospheric new-particle formation was observed to take place in more than 90% of the analyzed days. The days with no new particle formation were cloudy or rainy days. The formation rate of 10 nm particles varied in the range of 0.1–28 cm<sup>−3</sup> s<sup>−1</sup> (median 1.9 cm<sup>−3</sup> s<sup>−1</sup>) and nucleation mode particle growth rates were in the range 3–21 nm h<sup>−1</sup> (median 8.5 nm h<sup>−1</sup>). Due to high formation and growth rates, observed new particle formation gives a significant contribute to the number of cloud condensation nuclei budget, having a potential to affect the regional climate forcing patterns.
