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The investigation of the impact of aircraft parameters on contrail properties helps to better understand the climate impact from aviation. Yet, in observations, it is a challenge to separate aircraft and meteorological influences on contrail formation. During the CONCERT campaign in November 2008, contrails from 3 Airbus passenger aircraft of types A319-111, A340-311 and A380-841 were probed at cruise under similar meteorological conditions with in situ instruments on board DLR research aircraft Falcon. Within the 2 min-old contrails detected near ice saturation, we find similar effective diameters <i>D</i><sub>eff</sub> (5.2–5.9 μm), but differences in particle number densities <i>n</i><sub>ice</sub> (162–235 cm<sup>−3</sup>) and in vertical contrail extensions (120–290 m), resulting in large differences in contrail optical depths τ at 550 nm (0.25–0.94). Hence larger aircraft produce optically thicker contrails. <br><br> Based on the observations, we apply the EULAG-LCM model with explicit ice microphysics and, in addition, the Contrail and Cirrus Prediction (CoCiP) model to calculate the aircraft type impact on young contrails under identical meteorological conditions. The observed increase in τ for heavier aircraft is confirmed by the models, yet for generally smaller τ. CoCiP model results suggest that the aircraft dependence of climate-relevant contrail properties persists during contrail lifetime, adding importance to aircraft-dependent model initialization. We finally derive an analytical relationship between contrail, aircraft and meteorological parameters. Near ice saturation, contrail width × τ scales linearly with the fuel flow rate, as confirmed by observations. For higher relative humidity with respect to ice (RHI), the analytical relationship suggests a non-linear increase in the form (RHI-1<sup>2/3</sup>. Summarized, our combined results could help to more accurately assess the climate impact from aviation using an aircraft-dependent contrail parameterization.
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Biological aerosol particles have become increasingly important for atmospheric study, but continuous measurements at high time and size resolution have not been available until recently. Here we report seasonal cycles of fluorescent biological aerosol particles (FBAP) from the boreal forest in Hyytiälä, Finland (18 months) and the semi-arid Manitou Experimental Forest, Colorado (10 months). FBAP at both locations were observed to be highest in summer and lowest in winter, increasing by factors of 12 and 5 between these seasons, respectively. In addition to the low temperatures and reduced sunlight during winter, we suggest that snow cover inhibited FBAP release from local terrestrial surfaces and that more extensive snow cover at the Finland site contributed to lower winter FBAP concentrations. Average size distributions at each site exhibited peaks between 1.5 and 6 μm in aerodynamic diameter. The Finland site consistently showed a dominant, narrow FBAP peak at ~ 3 μm in addition to discreet modes at ~ 1.5 and ~ 5 μm, whereas the Colorado site showed broader peaks at 1.5 and 5 μm, suggesting different modes of biological particles at the two sites. FBAP concentrations in both locations were shown to correlate with daily patterns of relative humidity (RH) during each season. Also during summer at each site, average FBAP concentration scaled with RH, but at the Finland site RH values above ~ 82% led to a significant decrease in FBAP concentration. We hypothesize that this is due to dew formation that inhibits bioparticle release. Lastly we show that rain during summer at each location led to pronounced increases in both fluorescent and total particle concentrations with FBAP peak particle size at ~ 2 μm and concentration scaling with rain intensity. We suggest that these particles are primarily fungal spores and other bioparticles lofted from splashing of rain droplets hitting soil and leaf surfaces. During the summer at the Colorado site we consistently observed a mode of ~ 4 μm particles appearing several hours after rain events that we suggest are fungal spores actively emitted when ambient conditions are most advantageous for spread and germination. The pronounced patterns of fluorescent bioparticles observed here suggest that parameterizations of both daily and seasonal cycles will be important to accurately reflect bioparticle emissions in future studies of atmospheric bioaerosols and their potential effects on clouds and precipitation.
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Aerosol particles from shipping emissions both cool the climate and cause adverse health effects. The cooling effect is, however, declining because of shipping emission controls aiming to improve air quality. We used an aerosol-climate model ECHAM-HAMMOZ to test whether by altering ship fuel sulfur content, the present-day aerosol-induced cooling effect from shipping could be preserved, while at the same time reducing premature mortality rates related to shipping emissions. We compared the climate and health effects of a present-day shipping emission scenario (ship fuel sulfur content of 2.7%) with (1) a simulation with strict emission controls in the coastal waters (ship fuel sulfur content of 0.1%) and twofold the present-day fuel sulfur content (i.e. 5.4%) elsewhere; and (2) a scenario with global strict shipping emission controls (ship fuel sulfur content of 0.1% in coastal waters and 0.5% elsewhere) roughly corresponding to international agreements to be enforced by the year 2020. Scenario 1 had a slightly stronger aerosol-induced effective radiative forcing (ERF) from shipping than the present-day scenario (−0.43 W m<sup>−2</sup> vs. −0.39 W m<sup>−2</sup>) while reducing premature mortality from shipping by 69% (globally 34 900 deaths avoided per year). Scenario 2 decreased the ERF to −0.06 W m<sup>−2</sup> and annual deaths by 96% (globally 48 200 deaths avoided per year) compared to present-day. Our results show that the cooling effect of present-day emissions could be retained with simultaneous notable improvements in air quality, even though the shipping emissions from the open ocean clearly have a significant effect on continental air quality. However, increasing ship fuel sulfur content in the open ocean would violate existing international treaties, could cause detrimental side-effects, and could be classified as geoengineering.
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Persistent organic pollutants, such as polychlorinated biphenyls, reach the Southern Ocean atmosphere through long-range atmospheric transport. In this study we report the largest dataset available for the atmospheric occurrence of PCBs in the Southern Ocean surrounding the Antarctic Peninsula from samples obtained during three cruises in 2005, 2008 and 2009. The gas phase concentrations of total PCBs (Σ<sub>25</sub>PCBs) ranged from 1 to 70 pg m<sup>−3</sup>, while the aerosol phase concentrations were significantly lower (0.04 to 0.4 pg m<sup>−3</sup>). The aerosol phase is enriched in the more hydrophobic congeners consistent with the model predictions of gas-particle partitioning. There is a net air-to-water diffusive flux of PCBs to the Southern Ocean, up to 100 times higher than the dry deposition flux of aerosol-bound PCBs. The air-water disequilibrium is higher for the more hydrophobic congeners consistent with the role of the biological pump removing PCBs from the water column by settling of PCBs bound to organic matter. The atmospheric half-lives of PCB 52 and 180 are of 3.8 and 1 days, respectively, as calculated from the measured atmospheric concentration and depositional fluxes. The volatilization of PCBs from Antarctic soils during the austral summer drives higher gas phase concentrations in the atmosphere over Antarctica during the warmer periods. This temperature dependence is not observed for PCBs over the adjacent Southern Ocean, probably due to the importance of long-range atmospheric transport and atmospheric deposition modulating the atmospheric occurrence of PCBs.
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An earlier method to determine the mean response of upper-tropospheric water to localised deep convective systems (DC systems) is improved and applied to the EC-Earth climate model. Following Zelinka and Hartmann (2009), several fields related to moist processes and radiation from various satellites are composited with respect to the local maxima in rain rate to determine their spatio-temporal evolution with deep convection in the central Pacific Ocean. Major improvements to the earlier study are the isolation of DC systems in time so as to prevent multiple sampling of the same event, and a revised definition of the mean background state that allows for better characterisation of the DC-system-induced anomalies. <br><br> The observed DC systems in this study propagate westward at ~4 m s<sup>−1</sup>. Both the upper-tropospheric relative humidity and the outgoing longwave radiation are substantially perturbed over a broad horizontal extent and for periods >30 h. The cloud fraction anomaly is fairly constant with height but small maximum can be seen around 200 hPa. The cloud ice water content anomaly is mostly confined to pressures greater than 150 hPa and reaches its maximum around 450 hPa, a few hours after the peak convection. Consistent with the large increase in upper-tropospheric cloud ice water content, albedo increases dramatically and persists about 30 h after peak convection. <br><br> Applying the compositing technique to EC-Earth allows an assessment of the model representation of DC systems. The model captures the large-scale responses, most notably for outgoing longwave radiation, but there are a number of important differences. DC systems appear to propagate eastward in the model, suggesting a strong link to Kelvin waves instead of equatorial Rossby waves. The diurnal cycle in the model is more pronounced and appears to trigger new convection further to the west each time. Finally, the modelled ice water content anomaly peaks at pressures greater than 500 hPa and in the upper troposphere between 250 hPa and 500 hPa, there is less ice than the observations and it does not persist as long after peak convection. The modelled upper-tropospheric cloud fraction anomaly, however, is of a comparable magnitude and exhibits a similar longevity as the observations.
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New-particle formation in the plumes of coal-fired power plants and other anthropogenic sulfur sources may be an important source of particles in the atmosphere. It remains unclear, however, how best to reproduce this formation in global and regional aerosol models with grid-box lengths that are tens of kilometres and larger. Based on the results of the System for Atmospheric Modelling (SAM), a large-eddy simulation/cloud-resolving model (LES/CRM) with online two-moment aerosol sectional (TOMAS) microphysics, we have developed a computationally efficient, but physically based, parameterization that predicts the characteristics of aerosol formed within sulfur-rich plumes based on parameters commonly available in global- and regional-scale models. Given large-scale mean meteorological parameters ((1) wind speed, (2) boundary-layer height and (3) downward shortwave radiative flux), (4) emissions of SO<sub>2</sub> and (5) NO<sub>x</sub> from the source, (6) mean background condensation sink, (7) background SO<sub>2</sub> and (8) NO<sub>x</sub> concentrations, and (9) the desired distance from the source, the parameterization will predict (1) the fraction of the emitted SO<sub>2</sub> that is oxidized to H<sub>2</sub>SO<sub>4</sub>, (2) the fraction of that H<sub>2</sub>SO<sub>4</sub> that forms new particles instead of condensing onto pre-existing particles, (3) the mean mass per particle of the newly formed particles, and (4) the number of newly formed particles per kilogram SO<sub>2</sub> emitted. The parameterization we describe here should allow for more accurate predictions of aerosol size distributions and a greater confidence in the effects of aerosols in climate and health studies.
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Despite critical importance for air quality and climate predictions, accurate representation of secondary organic aerosol (SOA) formation remains elusive. An essential addition to the ongoing discussion of improving model predictions is an acknowledgement of the linkages between experimental conditions, parameter optimization and model output, as well as the linkage between empirically-derived partitioning parameters and the physicochemical properties of SOA they represent in models. In this work, a "best available" set of SOA modeling parameters is selected by comparing predicted SOA yields and mass concentrations with observed yields and mass concentrations from a comprehensive list of published smog chamber studies. Evaluated SOA model parameters include existing parameters for two product (2p) and volatility basis set (VBS) modeling frameworks, and new 2p-VBS parameters; 2p-VBS parameters are developed to exploit advantages of the VBS approach within the computationally-economical and widely-used 2p framework. Fine particulate matter (PM<sub>2.5</sub>) and SOA mass concentrations are simulated for the continental United States using CMAQv.4.7.1; results are compared for a base case (with default CMAQ parameters) and two best available parameter cases to illustrate the high- and low-NO<sub>x</sub> limits of biogenic SOA formation from monoterpenes. Results are discussed in terms of implications for current chemical transport model simulations and recommendations are provided for future modeling and measurement efforts. The comparisons of SOA yield predictions with data from 22 published chamber studies illustrate that: (1) SOA yields for naphthalene, and cyclic and > C5 straight-chain/branched alkanes are not well represented using either the newly developed or existing parameters for low-yield aromatics and lumped alkanes, respectively; and (2) for four of seven volatile organic compound+oxidant systems, the 2p-VBS parameters better represent chamber data than do the default CMAQ v.4.7.1 parameters. Using the "best available" parameters (combination of published 2p and newly derived 2p-VBS), predicted SOA mass and PM<sub>2.5</sub> concentrations increase by up to 15% and 7%, respectively, for the high-NO<sub>x</sub> case and up to 215% (~3 μg m<sup>−3</sup>) and 55%, respectively, for the low-NO<sub>x</sub> case. Percent bias between model-based and observationally-based secondary organic carbon (SOC) improved from −63% for the base case to −15% for the low-NO<sub>x</sub> case. The ability to robustly assign "best available" parameters in all volatile organic compound+oxidant systems, however, is critically limited due to insufficient data; particularly for photo-oxidation of diverse monoterpenes, sesquiterpenes, and alkanes under a range of atmospherically relevant conditions.
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We demonstrate improvements in CALIPSO (Cloud–Aerosol Lidar and Infrared Pathfinder Satellite Observations) dust extinction retrievals over northern Africa and Europe when corrections are applied regarding the Saharan dust lidar ratio assumption, the separation of the dust portion in detected dust mixtures, and the averaging scheme introduced in the Level 3 CALIPSO product. First, a universal, spatially constant lidar ratio of 58 sr instead of 40 sr is applied to individual Level 2 dust-related backscatter products. The resulting aerosol optical depths show an improvement compared with synchronous and collocated AERONET (Aerosol Robotic Network) measurements. An absolute bias of the order of −0.03 has been found, improving on the statistically significant biases of the order of −0.10 reported in the literature for the original CALIPSO product. When compared with the MODIS (Moderate-Resolution Imaging Spectroradiometer) collocated aerosol optical depth (AOD) product, the CALIPSO negative bias is even less for the lidar ratio of 58 sr. After introducing the new lidar ratio for the domain studied, we examine potential improvements to the climatological CALIPSO Level 3 extinction product: (1) by introducing a new methodology for the calculation of pure dust extinction from dust mixtures and (2) by applying an averaging scheme that includes zero extinction values for the nondust aerosol types detected. The scheme is applied at a horizontal spatial resolution of 1° × 1° for ease of comparison with the instantaneous and collocated dust extinction profiles simulated by the BSC-DREAM8b dust model. Comparisons show that the extinction profiles retrieved with the proposed methodology reproduce the well-known model biases per subregion examined. The very good agreement of the proposed CALIPSO extinction product with respect to AERONET, MODIS and the BSC-DREAM8b dust model makes this dataset an ideal candidate for the provision of an accurate and robust multiyear dust climatology over northern Africa and Europe.
