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Online coupled regional meteorology chemistry models in Europe: current status and prospects

Online coupled mesoscale meteorology atmospheric chemistry models have undergone a rapid evolution in recent years. Although mainly developed by the air quality modelling community, these models are also of interest for numerical weather prediction and regional climate modelling as they can consider not only the effects of meteorology on air quality, but also the potentially important effects of atmospheric composition on weather. Two ways of online coupling can be distinguished: online integrated and online access coupling. Online integrated models simulate meteorology and chemistry over the same grid in one model using one main time step for integration. Online access models use independent meteorology and chemistry modules that might even have different grids, but exchange meteorology and chemistry data on a regular and frequent basis. This article offers a comprehensive review of the current research status of online coupled meteorology and atmospheric chemistry modelling within Europe. Eighteen regional online coupled models developed or being used in Europe are described and compared. Topics discussed include a survey of processes relevant to the interactions between atmospheric physics, dynamics and composition; a brief overview of existing online mesoscale models and European model developments; an analysis on how feedback processes are treated in these models; numerical issues associated with coupled models; and several case studies and model performance evaluation methods. Finally, this article highlights selected scientific issues and emerging challenges that require proper consideration to improve the reliability and usability of these models for the three scientific communities: air quality, numerical meteorology modelling (including weather prediction) and climate modelling. This review will be of particular interest to model developers and users in all three fields as it presents a synthesis of scientific progress and provides recommendations for future research directions and priorities in the development, application and evaluation of online coupled models.
The Atmospheric Infrared Sounder version 6 cloud products

The version 6 cloud products of the Atmospheric Infrared Sounder (AIRS) and Advanced Microwave Sounding Unit (AMSU) instrument suite are described. The cloud top temperature, pressure, and height and effective cloud fraction are now reported at the AIRS field-of-view (FOV) resolution. Significant improvements in cloud height assignment over version 5 are shown with FOV-scale comparisons to cloud vertical structure observed by the CloudSat 94 GHz radar and the Cloud-Aerosol LIdar with Orthogonal Polarization (CALIOP). Cloud thermodynamic phase (ice, liquid, and unknown phase), ice cloud effective diameter (De), and ice cloud optical thickness (τ) are derived using an optimal estimation methodology for AIRS FOVs, and global distributions for 2007 are presented. The largest values of τ are found in the storm tracks and near convection in the tropics, while De is largest on the equatorial side of the midlatitude storm tracks in both hemispheres, and lowest in tropical thin cirrus and the winter polar atmosphere. Over the Maritime Continent the diurnal variability of τ is significantly larger than for the total cloud fraction, ice cloud frequency, and De, and is anchored to the island archipelago morphology. Important differences are described between northern and southern hemispheric midlatitude cyclones using storm center composites. The infrared-based cloud retrievals of AIRS provide unique, decadal-scale and global observations of clouds over portions of the diurnal and annual cycles, and capture variability within the mesoscale and synoptic scales at all latitudes.
Near-surface meteorology during the Arctic Summer Cloud Ocean Study (ASCOS): evaluation of reanalyses and global climate models

Atmospheric measurements from the Arctic Summer Cloud Ocean Study (ASCOS) are used to evaluate the performance of three atmospheric reanalyses (European Centre for Medium Range Weather Forecasting (ECMWF)-Interim reanalysis, National Center for Environmental Prediction (NCEP)-National Center for Atmospheric Research (NCAR) reanalysis, and NCEP-DOE (Department of Energy) reanalysis) and two global climate models (CAM5 (Community Atmosphere Model 5) and NASA GISS (Goddard Institute for Space Studies) ModelE2) in simulation of the high Arctic environment. Quantities analyzed include near surface meteorological variables such as temperature, pressure, humidity and winds, surface-based estimates of cloud and precipitation properties, the surface energy budget, and lower atmospheric temperature structure. In general, the models perform well in simulating large-scale dynamical quantities such as pressure and winds. Near-surface temperature and lower atmospheric stability, along with surface energy budget terms, are not as well represented due largely to errors in simulation of cloud occurrence, phase and altitude. Additionally, a development version of CAM5, which features improved handling of cloud macro physics, has demonstrated to improve simulation of cloud properties and liquid water amount. The ASCOS period additionally provides an excellent example of the benefits gained by evaluating individual budget terms, rather than simply evaluating the net end product, with large compensating errors between individual surface energy budget terms that result in the best net energy budget.
The direct and indirect radiative effects of biogenic secondary organic aerosol

We use a global aerosol microphysics model in combination with an offline radiative transfer model to quantify the radiative effect of biogenic secondary organic aerosol (SOA) in the present-day atmosphere. Through its role in particle growth and ageing, the presence of biogenic SOA increases the global annual mean concentration of cloud condensation nuclei (CCN; at 0.2% supersaturation) by 3.6–21.1%, depending upon the yield of SOA production from biogenic volatile organic compounds (BVOCs), and the nature and treatment of concurrent primary carbonaceous emissions. This increase in CCN causes a rise in global annual mean cloud droplet number concentration (CDNC) of 1.9–5.2%, and a global mean first aerosol indirect effect (AIE) of between +0.01 W m−2 and −0.12 W m−2. The radiative impact of biogenic SOA is far greater when biogenic oxidation products also contribute to the very early stages of new particle formation; using two organically mediated mechanisms for new particle formation, we simulate global annual mean first AIEs of −0.22 W m−2 and −0.77 W m−2. The inclusion of biogenic SOA substantially improves the simulated seasonal cycle in the concentration of CCN-sized particles observed at three forested sites. The best correlation is found when the organically mediated nucleation mechanisms are applied, suggesting that the first AIE of biogenic SOA could be as large as −0.77 W m−2. The radiative impact of SOA is sensitive to the presence of anthropogenic emissions. Lower background aerosol concentrations simulated with anthropogenic emissions from 1750 give rise to a greater fractional CCN increase and a more substantial first AIE from biogenic SOA. Consequently, the anthropogenic indirect radiative forcing between 1750 and the present day is sensitive to assumptions about the amount and role of biogenic SOA. We also calculate an annual global mean direct radiative effect of between −0.08 W m−2 and −0.78 W m−2 in the present day, with uncertainty in the amount of SOA produced from the oxidation of BVOCs accounting for most of this range.
Development of a source oriented version of the WRF/Chem model and its application to the California regional PM10 / PM2.5 air quality study

A source-oriented version of the Weather Research and Forecasting model with chemistry (SOWC, hereinafter) was developed. SOWC separately tracks primary particles with different hygroscopic properties rather than instantaneously combining them into an internal mixture. This approach avoids artificially mixing light absorbing black + brown carbon particles with materials such as sulfate that would encourage the formation of additional coatings. Source-oriented particles undergo coagulation and gas-particle conversion, but these processes are considered in a dynamic framework that realistically "ages" primary particles over hours and days in the atmosphere. SOWC more realistically predicts radiative feedbacks from anthropogenic aerosols compared to models that make internal mixing or other artificial mixing assumptions. A three-week stagnation episode (15 December 2000 to 6 January 2001) in the San Joaquin Valley (SJV) during the California Regional PM10 / PM2.5 Air Quality Study (CRPAQS) was chosen for the initial application of the new modeling system. Primary particles emitted from diesel engines, wood smoke, high-sulfur fuel combustion, food cooking, and other anthropogenic sources were tracked separately throughout the simulation as they aged in the atmosphere. Differences were identified between predictions from the source oriented vs. the internally mixed representation of particles with meteorological feedbacks in WRF/Chem for a number of meteorological parameters: aerosol extinction coefficients, downward shortwave flux, planetary boundary layer depth, and primary and secondary particulate matter concentrations. Comparisons with observations show that SOWC predicts particle scattering coefficients more accurately than the internally mixed model. Downward shortwave radiation predicted by SOWC is enhanced by ~1% at ground level chiefly because diesel engine particles in the source-oriented mixture are not artificially coated with material that increases their absorption efficiency. The extinction coefficient predicted by SOWC is reduced by an average of 0.012 km−1 (4.8%) in the SJV with a maximum reduction of ~0.2 km−1. Planetary boundary layer (PBL) height is increased by an average of 5.2 m (1.5%) with a~maximum of ~100 m in the SJV. Particulate matter concentrations predicted by SOWC are 2.23 μg m−3 (3.8%) lower than the average by the internally mixed version of the same model in the SJV because increased solar radiation at the ground increases atmospheric mixing. The changes in predicted meteorological parameters and particle concentrations identified in the current study stem from the mixing state of black carbon. The source-oriented model representation with realistic aging processes predicts that hydrophobic diesel engine particles remain largely uncoated over the +7 day simulation period, while the internal mixture model representation predicts significant accumulation of secondary nitrate and water on diesel engine particles. Similar results will likely be found in any air pollution stagnation episode that is characterized by significant particulate nitrate production. Future work should consider episodes where coatings are predominantly sulfate and/or secondary organic aerosol.
Estimation of cloud condensation nuclei concentration from aerosol optical quantities: influential factors and uncertainties

Large-scale measurements of cloud condensation nuclei (CCN) are difficult to obtain on a routine basis, whereas aerosol optical quantities are more readily available. This study investigates the relationship between CCN and aerosol optical quantities for some distinct aerosol types using extensive observational data collected at multiple Atmospheric Radiation Measurement (ARM) Climate Research Facility (CRF) sites around the world. The influences of relative humidity (RH), aerosol hygroscopicity (fRH) and single scattering albedo (SSA) on the relationship are analyzed. Better relationships are found between aerosol optical depth (AOD) and CCN at the Southern Great Plains (US), Ganges Valley (India) and Black Forest sites (Germany) than those at the Graciosa Island (the Azores) and Niamey (Niger) sites, where sea salt and dust aerosols dominate, respectively. In general, the correlation between AOD and CCN decreases as the wavelength of the AOD measurement increases, suggesting that AOD at a shorter wavelength is a better proxy for CCN. The correlation is significantly improved if aerosol index (AI) is used together with AOD. The highest correlation exists between CCN and aerosol scattering coefficients (σsp) and scattering AI measured in situ. The CCN–AOD (AI) relationship deteriorates with increasing RH. If RH exceeds 75%, the relationship where AOD is used as a proxy for CCN becomes invalid, whereas a tight σsp–CCN relationship exists for dry particles. Aerosol hygroscopicity has a weak impact on the σsp–CCN relationship. Particles with low SSA are generally associated with higher CCN concentrations, suggesting that SSA affects the relationship between CCN concentration and aerosol optical quantities. It may thus be used as a constraint to reduce uncertainties in the relationship. A significant increase in σsp and decrease in CCN with increasing SSA is observed, leading to a significant decrease in their ratio (CCN / σsp) with increasing SSA. Parameterized relationships are developed for estimating CCN, which account for RH, particle size, and SSA.
Long-range transport of giant particles in Asian dust identified by physical, mineralogical, and meteorological analysis

Giant particles transported over long distances are generally of limited concern in atmospheric studies due to their low number concentrations in mineral dust and possible local origin. However, they can play an important role in regional circulation of earth materials due to their enormous volume concentration. Asian dust laden with giant particles was observed in Korea on 31 March 2012, after a migration of about 2000 km across the Yellow Sea from the Gobi Desert. Scanning electron microscopy (SEM) revealed that 20% of the particles exceeded 10 μm in equivalent sphere diameter, with a maximum of 60 μm. The median diameter from the number distribution was 5.7 μm, which was larger than the diameters recorded of 2.5 and 2.9 μm in Asian dust storms in 2010 and 2011, respectively, and was consistent with independent optical particle counter data. Giant particles (>10 μm) contributed about 89% of the volume of the dust in the 2012 storm. Illite–smectite series clay minerals were the major mineral group followed by quartz, plagioclase, K-feldspar, and calcite. The total phyllosilicate content was ~52%. The direct long-range transport of giant particles was confirmed by calcite nanofibers closely associated with clays in a submicron scale identified by high-resolution SEM and transmission electron microscopy. Since giant particles consisted of clay agglomerates and clay-coated quartz, feldspars, and micas, the mineral composition varied little throughout the fine (<5 μm), coarse (5–10 μm), giant-S (10–20 μm), and giant-L (>20 μm) size bins. Analysis of the synoptic conditions of the 2012 dust event and its migration indicated that the mid-tropospheric strong wind belt directly stretching to Korea induced rapid transport of the dust, delivering giant particles. Giant dust particles with high settling velocity would be the major input into the terrestrial and marine sedimentary and ecological systems of East Asia and the western Pacific. Analysis of ancient aeolian deposits in Korea suggested the common deposition of giant particles from Asian dust through the late Quaternary Period. The roles of giant particles should be reviewed with regard to regional circulation of mineral particles and nutrients.
The changing oxidizing environment in London – trends in ozone precursors and their contribution to ozone production

Ground-level ozone is recognized to be a threat to human health (WHO, 2003), have a deleterious impact on vegetation (Fowler et al., 2009), is also an important greenhouse gas (IPCC, 2007) and key to the oxidative ability of the atmosphere (Monks et al., 2009). Owing to its harmful effect on health, much policy and mitigation effort has been put into reducing its precursors – the nitrogen oxides (NOx) and non-methane volatile organic compounds (NMVOCs). The non-linear chemistry of tropospheric ozone formation, dependent mainly on NOx and NMVOC concentrations in the atmosphere, makes controlling tropospheric ozone complex. Furthermore, the concentration of ozone at any given point is a complex superimposition of in-situ produced or destroyed ozone and transported ozone on the regional and hemispheric-scale. In order to effectively address ozone, a more detailed understanding of its origins is needed. Here we show that roughly half (5 μg m−3) of the observed increase in urban (London) ozone (10 μg m−3) in the UK from 1998 to 2008 is owing to factors of local origin, in particular, the change in NO : NO2 ratio, NMVOC : NOx balance, NMVOC speciation, and emission reductions (including NOx titration). In areas with previously higher large concentrations of nitrogen oxides, ozone that was previously suppressed by high concentrations of NO has now been "unmasked", as in London and other urban areas of the UK. The remaining half (approximately 5 μg m−3) of the observed ozone increase is attributed to non-local factors such as long-term transport of ozone, changes in background ozone, and meteorological variability. These results show that a two-pronged approach, local action and regional-to-hemispheric cooperation, is needed to reduce ozone and thereby population exposure, which is especially important for urban ozone.
Where do the air masses between double tropopauses come from?

An analysis of the origin of air masses that end up between double tropopauses (DT) in the subtropics and midlatitudes is presented. The double tropopauses were diagnosed in the ERA-Interim reanalysis (1979–2010), and the origin of air masses was analysed using the Lagrangian model FLEXPART. Different processes for the formation of double tropopauses (DT) have been suggested in the literature. Some studies have suggested that double tropopauses may occur as a response to the vertical profile of adiabatic heating, due to the residual meridional circulation, while others have put forward contradicting explanations. Whereas some studies have suggested that double tropopauses result from poleward excursions of the tropical tropopause over the extratropical one, others have argued that DTs develop in baroclinic unstable processes involving transport of air from high latitudes. In some regions, the DT structure has a semipermanent character which cannot be explained by excursions of the tropical tropopause alone. However, the results presented in this paper confirm that processes involving excursions of the tropical tropopause over the extratropical tropopause, which are therefore accompanied by intrusions of air from the tropical troposphere into the lower extratropical stratosphere, make a significant contribution for the occurrence of DTs in the subtropics and midlatitudes. Specifically, it is shown that the air between double tropopauses comes from equatorward regions, and has a higher percentage of tropospheric particles and a lower mean potential vorticity.
Two hundred fifty years of aerosols and climate: the end of the age of aerosols

Carbonaceous and sulfur aerosols have a substantial global and regional influence on climate, resulting in a net cooling to date, in addition to their impact on health and ecosystems. The magnitude of this influence has changed substantially over the past and is expected to continue to change into the future. An integrated picture of the changing climatic influence of black carbon, organic carbon and sulfate over the period 1850 through 2100, focusing on uncertainty, is presented using updated historical inventories and a coordinated set of emission projections. We describe, in detail, the aerosol emissions from the RCP4.5 scenario and its associated reference scenario. While aerosols have had a substantial impact on climate over the past century, we show that, by the end of the 21st century, aerosols will likely be only a minor contributor to radiative forcing due to increases in greenhouse gas forcing and a net global decrease in pollutant emissions. This outcome is even more certain under a successful implementation of a policy to limit greenhouse gas emissions as low-carbon energy technologies that do not emit appreciable aerosol or SO2 are deployed.