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Cloud-resolving modelling of aerosol indirect effects in idealised radiative-convective equilibrium with interactive and fixed sea surface temperature

The study attempts to evaluate the aerosol indirect effects over tropical oceans in regions of deep convection applying a three-dimensional cloud-resolving model run over a doubly-periodic domain. The Tropics are modelled using a radiative-convective equilibrium idealisation when the radiation, turbulence, cloud microphysics and surface fluxes are explicitly represented while the effects of large-scale circulation are ignored. The aerosol effects are modelled by varying the number concentration of cloud condensation nuclei (CCN) at 1% supersaturation, which serves as a proxy for the aerosol amount in the environment, over a wide range, from pristine maritime (50 cm−3) to polluted (1000 cm−3) conditions. No direct effects of aerosol on radiation are included. Two sets of simulations have been run: fixed (non-interactive) sea surface temperature (SST) and interactive SST as predicted by a simple slab-ocean model responding to the surface radiative fluxes and surface enthalpy flux. Both sets of experiments agree on the tendency of increased aerosol concentrations to make the shortwave cloud forcing more negative and reduce the longwave cloud forcing in response to increasing CCN concentration. These, in turn, tend to cool the SST in interactive-SST case. It is interesting that the absolute change of the SST and most other bulk quantities depends only on relative change of CCN concentration; that is, same SST change can be the result of doubling CCN concentration regardless of clean or polluted conditions. It is found that the 10-fold increase of CCN concentration can cool the SST by as much as 1.5 K. This is quite comparable to 2.1–2.3 K SST warming obtained in a simulation for clean maritime conditions, but doubled CO2 concentration. Assuming the aerosol concentration has increased from preindustrial time by 30%, the radiative forcing due to indirect aerosol effects is estimated to be −0.3 W m−2. It is found that the indirect aerosol effect is dominated by the first (Twomey) effect. Qualitative differences between the interactive and fixed SST cases have been found in sensitivity of the hydrological cycle to the increase in CCN concentration; namely, the precipitation rate shows some tendency to increase in fixed SST case, but robust tendency to decrease in interactive SST case.
Urediospores of rust fungi are ice nucleation active at > −10 °C and harbor ice nucleation active bacteria

Various features of the biology of the rust fungi and of the epidemiology of the plant diseases they cause illustrate the important role of rainfall in their life history. Based on this insight we have characterized the ice nucleation activity (INA) of the aerially disseminated spores (urediospores) of this group of fungi. Urediospores of this obligate plant parasite were collected from natural infections of 7 species of weeds in France, from coffee in Brazil and from field and greenhouse-grown wheat in France, the USA, Turkey and Syria. Immersion freezing was used to determine freezing onset temperatures and the abundance of ice nuclei in suspensions of washed spores. Microbiological analyses of spores from France, the USA and Brazil, and subsequent tests of the ice nucleation activity of the bacteria associated with spores were deployed to quantify the contribution of bacteria to the ice nucleation activity of the spores. All samples of spores were ice nucleation active, having freezing onset temperatures as high as −4 °C. Spores in most of the samples carried cells of ice nucleation-active strains of the bacterium Pseudomonas syringae (at rates of less than 1 bacterial cell per 100 urediospores), but bacterial INA accounted for only a small fraction of the INA observed in spore suspensions. Changes in the INA of spore suspensions after treatment with lysozyme suggest that the INA of urediospores involves a polysaccharide. Based on data from the literature, we have estimated the concentrations of urediospores in air at cloud height and in rainfall. These quantities are very similar to those reported for other biological ice nucleators in these same substrates. However, at cloud level convective activity leads to widely varying concentrations of particles of surface origin, so that mean concentrations can underestimate their possible effects on clouds. We propose that spatial and temporal concentrations of biological ice nucleators active at temperatures > −10 °C and the specific conditions under which they can influence cloud glaciation need to be further evaluated so as to understand how evolutionary processes could have positively selected for INA.
Analysis of upper-tropospheric humidity in tropical descent regions using observed and modelled radiances

We use multiple observations and climate model simulations to study upper tropospheric humidity (UTH) in tropical descent regions. A satellite simulator is used to generate UTH from model fields to ensure a like-to-like comparison. We have shown that HadGEM2 is generally able to reproduce the patterns and magnitude of UTH in these regions. In both models and observations, the major mode of UTH variability in these regions is associated with El Nino and Southern Oscillation (ENSO); a negative UTH anomaly is seen during El Nino years. There is no significant trend in UTH in these regions, where even a small negative trend would lead to an important reduction of the positive water vapour feedback on global warming.
Stratospheric loss and atmospheric lifetimes of CFC-11 and CFC-12 derived from satellite observations

The lifetimes of CFC-11 and CFC-12 have been evaluated using global observations of their stratospheric distributions from satellite-based instruments over the time period from 1992 to 2010. The chlorofluorocarbon (CFC) datasets are from the Cryogen Limb Array Etalon Spectrometer (CLAES), the Cryogenic Infrared Spectrometers and Telescopes for the Atmosphere (CRISTA-1 and CRISTA-2), the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS), and the Atmospheric Chemistry Experiment (ACE). Stratospheric loss rates were calculated using an ultraviolet radiative transfer code with updated cross section and solar irradiance data. Mean steady-state lifetimes based on these observations are 44.7 (36–58) yr for CFC-11 and 106.6 (90–130) yr for CFC-12, which are in good agreement with the most recent WMO ozone assessment. There are two major sources of error in calculating lifetimes using this method. The first important error arises from uncertainties in tropical stratospheric observations, particularly for CFC-11. Another large contribution to the error is due to uncertainties in the penetration of solar ultraviolet radiation at wavelengths between 185 and 220 nm, primarily in the tropical stratosphere between 20 and 35 km altitude.
Droplet number uncertainties associated with CCN: an assessment using observations and a global model adjoint

We use the Global Modelling Initiative (GMI) chemical transport model with a cloud droplet parameterisation adjoint to quantify the sensitivity of cloud droplet number concentration to uncertainties in predicting CCN concentrations. Published CCN closure uncertainties for six different sets of simplifying compositional and mixing state assumptions are used as proxies for modelled CCN uncertainty arising from application of those scenarios. It is found that cloud droplet number concentrations (Nd) are fairly insensitive to the number concentration (Na) of aerosol which act as CCN over the continents (∂lnNd/∂lnNa ~10–30%), but the sensitivities exceed 70% in pristine regions such as the Alaskan Arctic and remote oceans. This means that CCN concentration uncertainties of 4–71% translate into only 1–23% uncertainty in cloud droplet number, on average. Since most of the anthropogenic indirect forcing is concentrated over the continents, this work shows that the application of Köhler theory and attendant simplifying assumptions in models is not a major source of uncertainty in predicting cloud droplet number or anthropogenic aerosol indirect forcing for the liquid, stratiform clouds simulated in these models. However, it does highlight the sensitivity of some remote areas to pollution brought into the region via long-range transport (e.g., biomass burning) or from seasonal biogenic sources (e.g., phytoplankton as a source of dimethylsulfide in the southern oceans). Since these transient processes are not captured well by the climatological emissions inventories employed by current large-scale models, the uncertainties in aerosol-cloud interactions during these events could be much larger than those uncovered here. This finding motivates additional measurements in these pristine regions, for which few observations exist, to quantify the impact (and associated uncertainty) of transient aerosol processes on cloud properties.
Dynamic evaluation of a multi-year model simulation of particulate matter concentrations over Europe

A 9 yr air quality simulation is conducted from 2000 to 2008 over Europe using the Polyphemus/Polair3D chemical-transport model (CTM) and then evaluated against the measurements of the European Monitoring and Evaluation Programme (EMEP). The spatial distribution of PM2.5 over Europe shows high concentrations over northern Italy (36 μg m−3) and some areas of Eastern Europe, France, and Benelux, and low concentrations over Scandinavia, Spain, and the easternmost part of Europe. PM2.5 composition differs among regions. The operational evaluation shows satisfactory model performance for ozone (O3). PM2.5, PM10, and sulfate (SO4=) meet the performance goal of Boylan and Russell (2006). Nitrate (NO3−) and ammonium (NH4+) are overestimated, although NH4+ meets the performance criterion. The correlation coefficients between simulated and observed data are 63% for O3, 57% for PM10, 59% for PM2.5, 57% for SO4=, 42% for NO3−, and 58% for NH4+. The comparison with other recent 1 yr model simulations shows that all models overestimate nitrate. The performance of PM2.5, sulfate, and ammonium is comparable to that of the other models. The dynamic evaluation shows that the response of PM2.5 to changes in meteorology differs depending on location and the meteorological variable considered. Wind speed and precipitation show a strong negative day-to-day correlation with PM2.5 and its components (except for sea salt, which shows a positive correlation), which tends towards 0 as the day lag increases. On the other hand, the correlation coefficient is near constant for temperature, for any day lag and PM2.5 species, but it may be positive or negative depending on the species and, for sulfate, depending on the location. The effects of precipitation and wind speed on PM2.5 and its components are better reproduced by the model than the effects of temperature. This is mainly due to the fact that temperature has different effects on the PM2.5 components, unlike precipitation and wind speed, which impact most of the PM2.5 components in the same way. These results suggest that state-of-the-science air quality models reproduce satisfactorily the effect of meteorology on PM2.5 and therefore are suitable to investigate the effects of climate change on particulate air quality, although uncertainties remain concerning semivolatile PM2.5 components.
Seasonal and spatial variability of the OM/OC mass ratios and high regional correlation between oxalic acid and zinc in Chinese urban organic aerosols

We calculated the organic matter to organic carbon mass ratios (OM/OC mass ratios) in PM2.5 collected from 14 Chinese cities during summer and winter of 2003 and analyzed the causes for their seasonal and spatial variability. The OM/OC mass ratios were calculated two ways. Using a mass balance method, the calculated OM/OC mass ratios averaged 1.92 ± 0.39 year-round, with no significant seasonal or spatial variation. The second calculation was based on chemical species analyses of the organic compounds extracted from the PM2.5 samples using dichloromethane/methanol and water. The calculated OM/OC mass ratio in summer was relatively high (1.75 ± 0.13) and spatially-invariant due to vigorous photochemistry and secondary organic aerosol (OA) production throughout the country. The calculated OM/OC mass ratio in winter (1.59 ± 0.18) was significantly lower than that in summer, with lower values in northern cities (1.51 ± 0.07) than in southern cities (1.65 ± 0.15). This likely reflects the wider usage of coal for heating purposes in northern China in winter, in contrast to the larger contributions from biofuel and biomass burning in southern China in winter. On average, organic matter constituted 36% and 34% of Chinese urban PM2.5 mass in summer and winter, respectively. We report, for the first time, a high regional correlation between Zn and oxalic acid in Chinese urban aerosols in summer. This is consistent with the formation of stable Zn oxalate complex in the aerosol phase previously proposed by Furukawa and Takahashi (2011). We found that many other dicarboxylic acids were also highly correlated with Zn in the summer Chinese urban aerosol samples, suggesting that they may also form stable organic complexes with Zn. Such formation may have profound implications for the atmospheric abundance and hygroscopic properties of aerosol dicarboxylic acids.
Volatile organic compounds in the western Mediterranean basin: urban and rural winter measurements during the DAURE campaign

Atmospheric volatile organic compounds (VOCs) have key environmental and biological roles, but little is known about the daily VOC mixing ratios in Mediterranean urban and natural environments. We measured VOC mixing ratios concurrently at an urban and a rural site during the winter DAURE campaign in the northeastern Iberian Peninsula, by means of PTR-MS at both locations: a PTR-Quad-MS at the urban site and a PTR-ToF-MS at the rural site. All VOC mixing ratios measured were higher at the urban site (e.g. acetaldehyde, isoprene, benzene, and toluene with averages up to 1.68, 0.31, 0.58 and 2.71 ppbv, respectively), with the exception of some short-chain oxygenated VOCs such as acetone (with similar averages of 0.7–1.6 ppbv at both sites). The average diurnal pattern also differed between the sites. Most of the VOCs at the urban location showed their highest mixing ratios in the morning and evening. These peaks coincided with traffic during rush hour, the main origin of most of the VOCs analyzed. Between these two peaks, the sea breeze transported the urban air inland, thus helping to lower the VOC loading at the urban site. At the rural site, most of the measured VOCs were advected by the midday sea breeze, yielding the highest daily VOC mixing ratios (e.g. acetaldehyde, isoprene, benzene, and toluene with averages up to 0.65, 0.07, 0.19, and 0.41 ppbv, respectively). Only biogenic monoterpenes showed a clear local origin at this site. In addition, the concentrations of fine particulate matter observed at both sites, together with the synoptic meteorological conditions and radio-sounding data, allowed the identification of different atmospheric scenarios that had a clear influence on the measured VOC mixing ratios. These results highlight the differences and relationships in VOC mixing ratios between nearby urban and rural areas in Mediterranean regions. Further research in other urban-rural areas is warranted to better understand the urban-rural influence on atmospheric VOC mixing ratios under different atmospheric conditions.
The 2007–2011 evolution of tropical methane in the mid-troposphere as seen from space by MetOp-A/IASI

Since July 2007, monthly averages of mid-tropospheric methane have been retrieved in the tropics over land and sea, by day and night, from IASI onboard MetOp-A, yielding a complete view of the geographical distribution, seasonality and long-term tendency of methane in the mid-troposphere. Retrieved methane displays a clear seasonal cycle of ~25 ppbv in the northern tropics, with a maximum in November and a minimum in April–May, a more complex cycle of ~15 ppbv in the southern tropics, and a south-to-north latitudinal variation of ~30 ppbv – in good agreement with regular aircraft measurements of the CONTRAIL program. Comparisons with CARIBIC aircraft measurements made at ~11 km yield an averaged difference between collocated IASI estimates and CARIBIC measurements of 7.2 ppbv with a standard deviation of 13.1 ppbv. Comparisons with aircraft measurements made above 6 km during five HIPPO campaigns give an averaged difference between collocated IASI estimates and HIPPO measurements of 5.1 ppbv with a standard deviation of 16.3 ppbv. These comparisons show that IASI captures well the evolution of mid-tropospheric methane. In particular, in 2007 and 2008, IASI shows an increase of mid-tropospheric methane in the tropical region of 9.5 ± 2.8 and 6.3 ± 1.7 ppbv yr−1, respectively – in excellent agreement with the rate of increase measured at the surface after almost a decade of near-zero growth. IASI also indicates a slowing down of this increase in the following years to ~2 ppbv yr−1, with the highest increase in 2010. Assuming that the recent evolution of methane is mostly due to an increase in surface emissions, IASI might indicate a decrease in tropical wetland emissions for the period 2009–2011 compared to 2007–2008, in agreement with decreasing tropical precipitation over this period, together with an increase in biomass burning emissions in 2010 in the southern tropics.
A three-dimensional variational data assimilation system for multiple aerosol species with WRF/Chem and an application to PM2.5 prediction

A three-dimensional variational data assimilation (3-DVAR) algorithm for aerosols in a WRF/Chem model is presented. The WRF/Chem model uses the MOSAIC (Model for Simulating Aerosol Interactions and Chemistry) scheme, which explicitly treats eight major species (elemental/black carbon, organic carbon, nitrate, sulfate, chloride, ammonium, sodium and the sum of other inorganic, inert mineral and metal species) and represents size distributions using a sectional method with four size bins. The 3-DVAR scheme is formulated to take advantage of the MOSAIC scheme in providing comprehensive analyses of species concentrations and size distributions. To treat the large number of state variables associated with the MOSAIC scheme, this 3-DVAR algorithm first determines the analysis increments of the total mass concentrations of the eight species, defined as the sum of the mass concentrations across all size bins, and then distributes the analysis increments over four size bins according to the background error variances. The number concentrations for each size bin are adjusted based on the ratios between the mass and number concentrations of the background state. Additional flexibility is incorporated to further lump the eight mass concentrations, and five lumped species are used in the application presented. The system is evaluated using the analysis and prediction of PM2.5 in the Los Angeles basin during the CalNex 2010 field experiment, with assimilation of surface PM2.5 and speciated concentration observations. The results demonstrate that the data assimilation significantly reduces the errors in comparison with a simulation without data assimilation and improved forecasts of the concentrations of PM2.5 as well as individual species for up to 24 h. Some implementation difficulties and limitations of the system are discussed.