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Enhanced cold-season warming in semi-arid regions

This study examined surface air temperature trends over global land from 1901–2009. It is found that the warming trend was particularly enhanced, in the boreal cold season (November to March) over semi-arid regions (with precipitation of 200–600 mm yr−1) showing a temperature increase of 1.53 °C as compared to the global annual mean temperature increase of 1.13 °C over land. In mid-latitude semi-arid areas of Europe, Asia, and North America, temperatures in the cold season increased by 1.41, 2.42, and 1.5 °C, respectively. The semi-arid regions contribute 44.46% to global annual-mean land-surface temperature trend. The mid-latitude semi-arid regions in the Northern Hemisphere contribute by 27.0% of the total, with the mid-latitude semi-arid areas in Europe, Asia, and North America accounting for 6.29%, 13.81%, and 6.85%, respectively. Such enhanced semi-arid warming (ESAW) imply drier and warmer trend of these regions.
A closure study of cloud condensation nuclei in the North China Plain using droplet kinetic condensational growth model

Aerosol size distribution and cloud condensation nucleus (CCN) number concentration were measured in the North China Plain from 31 December 2009 to 20 January 2010. The CCN closure study was performed using these data and droplet kinetic condensational growth model. The calculated CCN concentration with the assumption of pure ammonium sulfate aerosol is 40–140% higher than that observed for the supersaturations in this study. A sensitivity test on aerosol solubility and mixing state indicates that 0.2–0.5 mass fraction of ammonium sulfate for internal mixture can lead to a ratio of 0.82–1.30 for the calculated to observed CCN concentrations, and that 0.4–0.7 mass fraction of ammonium sulfate for external mixture results in a ratio of 0.74–1.25 in the North China Plain during the time period of the field observations, suggesting that a relatively simple scheme may be used for CCN prediction in climate models for this region. Finally, we compare the calculated CCN concentrations from the kinetic condensational growth model and the equilibrium model. The kinetic condensational growth model can simulate droplet growth in a time period under a certain supersaturation, while the equilibrium model only predicts whether a certain aerosol can be activated as CCN under that supersaturation. The CCN concentration calculated with the kinetic model is higher than that with the equilibrium model at supersaturations of 0.056% and 0.083%, because some particles that are not activated from the equilibrium point-of-view can grow large enough to be considered as CCN in the kinetic model. While at a supersaturation of 0.17%, CCN concentration calculated with the kinetic model is lower than that with the equilibrium model, due to the limitation of droplet kinetic growth. The calculated CCN concentrations using the kinetic model and the equilibrium model are the same at supersaturations of 0.35% and 0.70%.
Introduction to the European Monitoring and Evaluation Programme (EMEP) and observed atmospheric composition change during 1972–2009

European scale harmonized monitoring of atmospheric composition was initiated in the early 1970s, and the activity has generated a comprehensive dataset (available at <a href="http://www.emep.int"target="_blank">http://www.emep.int</a>) which allows the evaluation of regional and spatial trends of air pollution during a period of nearly 40 yr. Results from the monitoring made within EMEP, the European Monitoring and Evaluation Programme, show large reductions in ambient concentrations and deposition of sulphur species during the last decades. Reductions are in the order of 70–90% since the year 1980, and correspond well with reported emission changes. Also reduction in emissions of nitrogen oxides (NOx) are reflected in the measurements, with an average decrease of nitrogen dioxide and nitrate in precipitation by about 23% and 25% respectively since 1990. Only minor reductions are however seen since the late 1990s. The concentrations of total nitrate in air have decreased on average only by 8% since 1990, and fewer sites show a significant trend. A majority of the EMEP sites show a decreasing trend in reduced nitrogen both in air and precipitation on the order of 25% since 1990. Deposition of base cations has decreased during the past 30 yr, and the pH in precipitation has increased across Europe. Large inter annual variations in the particulate matter mass concentrations reflect meteorological variability, but still there is a relatively clear overall decrease at several sites during the last decade. With few observations going back to the 1990s, the observed chemical composition is applied to document a change in particulate matter (PM) mass even since 1980. These data indicate an overall reduction of about 5 μg m−3 from sulphate alone. Despite the significant reductions in sulphur emissions, sulphate still remains one of the single most important compounds contributing to regional scale aerosol mass concentration. Long-term ozone trends at EMEP sites show a mixed pattern. The year-to-year variability in ozone due to varying meteorological conditions is substantial, making it hard to separate the trends caused by emission change from other effects. For the Nordic countries the data indicate a reduced occurrence of very low concentrations. The most pronounced change in the frequency distribution is seen at sites in the UK and the Netherlands, showing a reduction in the higher values. Smaller changes are seen in Germany, while in Switzerland and Austria, no change is seen in the frequency distribution of ozone. The lack of long-term data series is a major obstacle for studying trends in volatile organic compounds (VOC). The scatter in the data is large, and significant changes are only found for certain components and stations. Concentrations of the heavy metals lead and cadmium have decreased in both air and precipitation during the last 20 yr, with reductions in the order of 80–90% for Pb and 64–84% for Cd (precipitation and air respectively). The measurements of total gaseous mercury indicate a dramatic decrease in concentrations during 1980 to about 1993. Trends in hexachlorocyclohexanes (HCHs) show a significant decrease in annual average air concentrations. For other persistent organic pollutants (POPs) the patterns is mixed, and differs between sites and between measurements in air versus precipitation.
New representation of water activity based on a single solute specific constant to parameterize the hygroscopic growth of aerosols in atmospheric models

Water activity is a key factor in aerosol thermodynamics and hygroscopic growth. We introduce a new representation of water activity (aw), which is empirically related to the solute molality (μs) through a single solute specific constant, νi. Our approach is widely applicable, considers the Kelvin effect and covers ideal solutions at high relative humidity (RH), including cloud condensation nuclei (CCN) activation. It also encompasses concentrated solutions with high ionic strength at low RH such as the relative humidity of deliquescence (RHD). The constant νi can thus be used to parameterize the aerosol hygroscopic growth over a wide range of particle sizes, from nanometer nucleation mode to micrometer coarse mode particles. In contrast to other aw-representations, our νi factor corrects the solute molality both linearly and in exponent form x · ax. We present four representations of our basic aw-parameterization at different levels of complexity for different aw-ranges, e.g. up to 0.95, 0.98 or 1. νi is constant over the selected aw-range, and in its most comprehensive form, the parameterization describes the entire aw range (0–1). In this work we focus on single solute solutions. νi can be pre-determined with a root-finding method from our water activity representation using an aw−μs data pair, e.g. at solute saturation using RHD and solubility measurements. Our aw and supersaturation (Köhler-theory) results compare well with the thermodynamic reference model E-AIM for the key compounds NaCl and (NH4)2SO4 relevant for CCN modeling and calibration studies. Envisaged applications include regional and global atmospheric chemistry and climate modeling.
Lagrangian coherent structures in tropical cyclone intensification

Recent work has suggested that tropical cyclones intensify via a pathway of rotating deep moist convection in the presence of enhanced fluxes of moisture from the ocean. The rotating deep convective structures possessing enhanced cyclonic vorticity within their cores have been dubbed Vortical Hot Towers (VHTs). In general, the interaction between VHTs and the system-scale vortex, as well as the corresponding evolution of equivalent potential temperature (θe) that modulates the VHT activity, is a complex problem in moist helical turbulence. To better understand the structural aspects of the three-dimensional intensification process, a Lagrangian perspective is explored that focuses on the coherent structures seen in the flow field associated with VHTs and their vortical remnants, as well as the evolution and localized stirring of θe. Recently developed finite-time Lagrangian methods are limited in the three-dimensional turbulence and shear associated with the VHTs. In this paper, new Lagrangian techniques developed for three-dimensional velocity fields are summarized and we apply these techniques to study VHT and θe phenomenology in a high-resolution numerical tropical cyclone simulation. The usefulness of these methods is demonstrated by an analysis of particle trajectories. We find that VHTs create a locally turbulent mixing environment. However, associated with the VHTs are hyperbolic structures that span between adjacent VHTs or adjacent vortical remnants and represent coherent finite-time transport barriers in the flow field. Although the azimuthally-averaged inflow is responsible for the inward advection of boundary layer θe, attracting Lagrangian coherent structures are coincident with pools of high boundary layer θe. Extensions of boundary layer coherent structures grow above the boundary layer during episodes of convection and remain with the convective vortices. These hyperbolic structures form initially as boundaries between VHTs. As vorticity aggregates into a ring-like eyewall feature, the Lagrangian boundaries merge into a ring outside of the region of maximal vorticity.
DO3SE modelling of soil moisture to determine ozone flux to forest trees

The DO3SE (Deposition of O3 for Stomatal Exchange) model is an established tool for estimating ozone (O3) deposition, stomatal flux and impacts to a variety of vegetation types across Europe. It has been embedded within the EMEP (European Monitoring and Evaluation Programme) photochemical model to provide a policy tool capable of relating the flux-based risk of vegetation damage to O3 precursor emission scenarios for use in policy formulation. A key limitation of regional flux-based risk assessments has been the assumption that soil water deficits are not limiting O3 flux due to the unavailability of evaluated methods for modelling soil water deficits and their influence on stomatal conductance (gsto), and subsequent O3 flux. This paper describes the development and evaluation of a method to estimate soil moisture status and its influence on gsto for a variety of forest tree species. This DO3SE soil moisture module uses the Penman-Monteith energy balance method to drive water cycling through the soil-plant-atmosphere system and empirical data describing gsto relationships with pre-dawn leaf water status to estimate the biological control of transpiration. We trial four different methods to estimate this biological control of the transpiration stream, which vary from simple methods that relate soil water content or potential directly to gsto, to more complex methods that incorporate hydraulic resistance and plant capacitance that control water flow through the plant system. These methods are evaluated against field data describing a variety of soil water variables, gsto and transpiration data for Norway spruce (Picea abies), Scots pine (Pinus sylvestris), birch (Betula pendula), aspen (Populus tremuloides), beech (Fagus sylvatica) and holm oak (Quercus ilex) collected from ten sites across Europe and North America. Modelled estimates of these variables show consistency with observed data when applying the simple empirical methods, with the timing and magnitude of soil drying events being captured well across all sites and reductions in transpiration with the onset of drought being predicted with reasonable accuracy. The more complex methods, which incorporate hydraulic resistance and plant capacitance, perform less well, with predicted drying cycles consistently underestimating the rate and magnitude of water loss from the soil. A sensitivity analysis showed that model performance was strongly dependent upon the local parameterisation of key model drivers such as the maximum gsto, soil texture, root depth and leaf area index. The results suggest that the simple modelling methods that relate gsto directly to soil water content and potential provide adequate estimates of soil moisture and influence on gsto such that they are suitable to be used to assess the potential risk posed by O3 to forest trees across Europe.
High molecular weight SOA formation during limonene ozonolysis: insights from ultrahigh-resolution FT-ICR mass spectrometry characterization

The detailed molecular composition of laboratory generated limonene ozonolysis secondary organic aerosol (SOA) was studied using ultrahigh-resolution Fourier transform ion cyclotron resonance (FT-ICR) mass spectrometry. Approximately 1200 molecular formulas were identified in the SOA over the mass range of 140 to 850 Da. Four characteristic groups of high relative abundance species were observed; they indicate an array of accretion products that retain a large fraction of the limonene skeleton. The identified molecular formulas of each of the groups are related to one another by CH2, O and CH2O homologous series. The CH2 and O homologous series of the low molecular weight (MW) SOA (m/z < 300) are explained with a combination of functionalization and fragmentation of radical intermediates and reactive uptake of gas-phase carbonyls. They include isomerization and elimination reactions of Criegee radicals, reactions between alkyl peroxy radicals, and scission of alkoxy radicals resulting from the Criegee radicals. The presence of compounds with 10–15 carbon atoms in the first group (e.g. C11H18O6) provides evidence for SOA formation by the reactive uptake of gas-phase carbonyls during limonene ozonolysis. The high MW compounds (m/z > 300) were found to constitute a significant number fraction of the identified SOA components. The formation of high MW compounds was evaluated by molecular formula trends, fragmentation analysis of select high MW compounds and a comprehensive reaction matrix including the identified low MW SOA, hydroperoxides and Criegee radicals as building blocks. Although the formation of high MW SOA may occur via a variety of radical and non-radical reaction channels, the combined approach indicates a greater importance of the non-condensation reactions over aldol and ester condensation reaction channels. Among these hemi-acetal reactions appear to be most dominant followed by hydroperoxide and Criegee reaction channels.
Corrigendum to "Strongly sheared stratocumulus convection: an observationally based large-eddy simulation study" published in Atmos. Chem. Phys., 12, 5223–5235, 2012
Radiative forcing estimates of sulfate aerosol in coupled climate-chemistry models with emphasis on the role of the temporal variability

This paper describes the impact on the sulfate aerosol radiative effects of coupling the radiative code of a global circulation model with a chemistry-aerosol module. With this coupling, temporal variations of sulfate aerosol concentrations influence the estimate of aerosol radiative impacts. Effects of this coupling have been assessed on net fluxes, radiative forcing and temperature for the direct and first indirect effects of sulfate. The direct effect respond almost linearly to rapid changes in concentrations whereas the first indirect effect shows a strong non-linearity. In particular, sulfate temporal variability causes a modification of the short wave net fluxes at the top of the atmosphere of +0.24 and +0.22 W m−2 for the present and preindustrial periods, respectively. This change is small compared to the value of the net flux at the top of the atmosphere (about 240 W m−2). The effect is more important in regions with low-level clouds and intermediate sulfate aerosol concentrations (from 0.1 to 0.8 μg (SO4) m−3 in our model). The computation of the aerosol direct radiative forcing is quite straightforward and the temporal variability has little effect on its mean value. In contrast, quantifying the first indirect radiative forcing requires tackling technical issues first. We show that the preindustrial sulfate concentrations have to be calculated with the same meteorological trajectory used for computing the present ones. If this condition is not satisfied, it introduces an error on the estimation of the first indirect radiative forcing. Solutions are proposed to assess radiative forcing properly. In the reference method, the coupling between chemistry and climate results in a global average increase of 8% in the first indirect radiative forcing. This change reaches 50% in the most sensitive regions. However, the reference method is not suited to run long climate simulations. We present other methods that are simpler to implement in a coupled chemistry/climate model and that offer the possibility to assess radiative forcing.
Seasonal cycle and source analyses of aerosol optical properties in a semi-urban environment at Puijo station in Eastern Finland

We introduce a four-year (in 2006–2010) continuous data set of aerosol optical properties at Puijo in Kuopio, Finland. We study the annual and diurnal variation of the aerosol scattering and absorption coefficients, hemispheric backscattering fraction, scattering Ångström exponent, and single scattering albedo, whose median values over this period were 7.2 Mm−1 (at 550 nm), 1.0 Mm−1 (at 637 nm), 0.15, 1.93 (between 450 and 550 nm), and 0.85, respectively. The scattering coefficient peaked in the spring and autumn, being 2–4 times those in the summer and winter. An exception was the summer of 2010, when the scattering coefficient was elevated to ~300 Mm−1 by plumes from forest fires in Russia. The absorption coefficient peaked in the winter when soot-containing particles derived from biomass burning were present. The higher relative absorption coefficients resulted in lower single scattering albedo in winter. The optical properties varied also with wind direction and time of the day, indicating the effect of the local pollutant sources and the age of the particles. Peak values in the single scattering albedo were observed when the wind blew from a paper mill and from the sector without local pollutant sources. These observations were linked, respectively, to the sulphate-rich aerosol from the paper mill and the oxygenated organics in the aged aerosol, which both are known to increase the scattering characteristics of aerosols. Decreases in the single scattering albedo in the morning and afternoon, distinct in the summertime, were linked to the increased traffic density at these hours. The scattering and absorption coefficients of residential and long-range transported aerosol (two separate cloud events) were found to be decreased by clouds. The effect was stronger for the scattering than absorption, indicating preferential activation of the more hygroscopic aerosol with higher scattering characteristics.