Quality Model Evaluation International Initiative Research Articles

A single-point modeling approach for the intercomparison and evaluation of ozone dry deposition across chemical transport models (Activity 2 of AQMEII4).

A primary sink of air pollutants and their precursors is dry deposition. Dry deposition estimates differ across chemical transport models, yet an understanding of the model spread is incomplete. Here, we introduce Activity 2 of the Air Quality Model Evaluation International Initiative Phase 4 (AQMEII4). We examine 18 dry deposition schemes from regional and global chemical transport models as well as standalone models used for impact assessments or process understanding. We configure the schemes as single-point models at eight Northern Hemisphere locations with observed ozone fluxes. Single-point models are driven by a common set of site-specific meteorological and environmental conditions. Five of eight sites have at least 3 years and up to 12 years of ozone fluxes. The interquartile range across models in multiyear mean ozone deposition velocities ranges from a factor of 1.2 to 1.9 annually across sites and tends to be highest during winter compared with summer. No model is within 50 % of observed multiyear averages across all sites and seasons, but some models perform well for some sites and seasons. For the first time, we demonstrate how contributions from depositional pathways vary across models. Models can disagree with respect to relative contributions from the pathways, even when they predict similar deposition velocities, or agree with respect to the relative contributions but predict different deposition velocities. Both stomatal and nonstomatal uptake contribute to the large model spread across sites. Our findings are the beginning of results from AQMEII4 Activity 2, which brings scientists who model air quality and dry deposition together with scientists who measure ozone fluxes to evaluate and improve dry deposition schemes in the chemical transport models used for research, planning, and regulatory purposes.

Technical note: AQMEII4 Activity 1: evaluation of wet and dry deposition schemes as an integral part of regional-scale air quality models

We present in this technical note the research protocol for phase 4 of the Air Quality Model Evaluation International Initiative (AQMEII4). This research initiative is divided into two activities, collectively having three goals: (i) to define the current state of the science with respect to representations of wet and especially dry deposition in regional models, (ii) to quantify the extent to which different dry deposition parameterizations influence retrospective air pollutant concentration and flux predictions, and (iii) to identify, through the use of a common set of detailed diagnostics, sensitivity simulations, model evaluation, and reduction of input uncertainty, the specific causes for the current range of these predictions. Activity 1 is dedicated to the diagnostic evaluation of wet and dry deposition processes in regional air quality models (described in this paper), and Activity 2 to the evaluation of dry deposition point models against ozone flux measurements at multiple towers with multiyear observations (to be described in future submissions as part of the special issue on AQMEII4). The scope of this paper is to present the scientific protocols for Activity 1, as well as to summarize the technical information associated with the different dry deposition approaches used by the participating research groups of AQMEII4. In addition to describing all common aspects and data used for this multi-model evaluation activity, most importantly, we present the strategy devised to allow a common process-level comparison of dry deposition obtained from models using sometimes very different dry deposition schemes. The strategy is based on adding detailed diagnostics to the algorithms used in the dry deposition modules of existing regional air quality models, in particular archiving diagnostics specific to land use–land cover (LULC) and creating standardized LULC categories to facilitate cross-comparison of LULC-specific dry deposition parameters and processes, as well as archiving effective conductance and effective flux as means for comparing the relative influence of different pathways towards the net or total dry deposition. This new approach, along with an analysis of precipitation and wet deposition fields, will provide an unprecedented process-oriented comparison of deposition in regional air quality models. Examples of how specific dry deposition schemes used in participating models have been reduced to the common set of comparable diagnostics defined for AQMEII4 are also presented.

A reflection on 10 years of the Air Quality Model Evaluation International Initiative

Editor’s Note:The authors document the progress that they made in evaluating the performance of regional air quality models within the framework of AQMEII and how this international collaborative e...

Aerosol optical properties over Europe: an evaluation of the AQMEII Phase 3 simulations against satellite observations

Abstract. The main uncertainties regarding the estimation of changes in the Earth's energy budget are related to the role of atmospheric aerosols. These changes are caused by aerosol–radiation (ARIs) and aerosol–cloud interactions (ACIs), which heavily depend on aerosol properties. Since the 1980s, many international modeling initiatives have studied atmospheric aerosols and their climate effects. Phase 3 of the Air Quality Modelling Evaluation International Initiative (AQMEII) focuses on evaluating and intercomparing regional and linked global/regional modeling systems by collaborating with the Task Force on the Hemispheric Transport of Air Pollution Phase 2 (HTAP2) initiative. Within this framework, the main aim of this work is the assessment of the representation of aerosol optical depth (AOD) and the Ångström exponent (AE) in AQMEII Phase 3 simulations over Europe. The evaluation was made using remote-sensing data from the Moderate Resolution Imaging Spectroradiometer (MODIS) sensors aboard the Terra and Aqua platforms, and the instruments belonging to the ground-based Aerosol Robotic Network (AERONET) and the Maritime Aerosol Network (MAN). Overall, the skills of AQMEII simulations when representing AOD (mean absolute errors from 0.05 to 0.30) produced lower errors than for the AE (mean absolute errors from 0.30 to 1). Regardless of the models or the emissions used, models were skillful at representing the low and mean AOD values observed (below 0.5). However, high values (around 1.0) were overpredicted for biomass burning episodes, due to an underestimation in the common fires' emissions, and were overestimated for coarse particles – principally desert dust – related to the boundary conditions. Despite this behavior, the spatial and temporal variability of AOD was better represented by all the models than AE variability, which was strongly underestimated in all the simulations. Noticeably, the impact of the model selection when representing aerosol optical properties is higher than the use of different emission inventories. On the other hand, the influence of ARIs and ACIs has a little visible impact compared to the impact of the model used.

Assessment and economic valuation of air pollution impacts on human health over Europe and the United States as calculated by a multi-model ensemble in the framework of AQMEII3.

The impact of air pollution on human health and the associated external costs in Europe and the United States (US) for the year 2010 are modeled by a multi-model ensemble of regional models in the frame of the third phase of the Air Quality Modelling Evaluation International Initiative (AQMEII3). The modeled surface concentrations of O3, CO, SO2 and PM2.5 are used as input to the Economic Valuation of Air Pollution (EVA) system to calculate the resulting health impacts and the associated external costs from each individual model. Along with a base case simulation, additional runs were performed introducing 20 % anthropogenic emission reductions both globally and regionally in Europe, North America and east Asia, as defined by the second phase of the Task Force on Hemispheric Transport of Air Pollution (TF-HTAP2).Health impacts estimated by using concentration inputs from different chemistry–transport models (CTMs) to the EVA system can vary up to a factor of 3 in Europe (12 models) and the United States (3 models). In Europe, the multi-model mean total number of premature deaths (acute and chronic) is calculated to be 414 000, while in the US, it is estimated to be 160 000, in agreement with previous global and regional studies. The economic valuation of these health impacts is calculated to be EUR 300 billion and 145 billion in Europe and the US, respectively. A subset of models that produce the smallest error compared to the surface observations at each time step against an all-model mean ensemble results in increase of health impacts by up to 30 % in Europe, while in the US, the optimal ensemble mean led to a decrease in the calculated health impacts by ~ 11 %.A total of 54 000 and 27 500 premature deaths can be avoided by a 20 % reduction of global anthropogenic emissions in Europe and the US, respectively. A 20 % reduction of North American anthropogenic emissions avoids a total of ~ 1000 premature deaths in Europe and 25 000 total premature deaths in the US. A 20 % decrease of anthropogenic emissions within the European source region avoids a total of 47 000 premature deaths in Europe. Reducing the east Asian anthropogenic emissions by 20 % avoids ~ 2000 total premature deaths in the US. These results show that the domestic anthropogenic emissions make the largest impacts on premature deaths on a continental scale, while foreign sources make a minor contribution to adverse impacts of air pollution.

Evaluation and uncertainty estimation of the impact of air quality modelling on crop yields and premature deaths using a multi-model ensemble

This study promotes the critical use of air pollution modelling results for health and agriculture impacts, with the primary goal of providing more reliable estimates to decision makers. To date, the accuracy of air quality (AQ) models and the effects of model-to-model result variability (which we will refer to as model uncertainty) on impact assessment studies have been often ignored, thus undermining the robustness of the information used in the decision making process and the confidence in the results obtained.A suite of twelve PM2.5 and ozone concentration fields produced by regional-scale chemistry transport Air Quality (AQ) models during the third phase of the Air Quality Model Evaluation International Initiative (AQMEII) has been used to calculate the impact of air pollution on premature deaths and crop yields. An innovative technique is applied to bias-adjust the models to available observations.The model results for ozone and PM2.5 are combined in a multi-model (MM) ensemble, which is used to estimate the damage and economic cost to human health and crop yields, as well as the associated uncertainties. The MM ensemble quantifies directly the uncertainty introduced by AQ models into the air pollution impact assessment chain, while the indirect use of experimental information through a bias adjustment, reduces the uncertainty in the ozone and PM2.5 fields and subsequently the uncertainty of the final impact assessment and cost valuation.The analysis over the European countries analysed in this study shows a mean number of premature deaths due to exposure to PM2.5 and ozone of approximately 370,000 (inter-quantile range between 260,000 and 415,000) and a relative yield loss of approximately 7% to 9% (depending on the exposure metrics used, for wheat and maize together). Furthermore, the results indicate that a reduction in the uncertainty of the modelled ozone by 61% and by 80% (depending on the aggregation metric used) and by 46% for PM2.5, produces a reduction in the uncertainty in premature mortality and crop loss of >60%, and of an equivalent percentage in the final uncertainty of cost valuation, providing decision makers with more accurate estimations for more targeted interventions.

Impacts of different characterizations of large-scale background on simulated regional-scale ozone over the continental United States.

This study analyzes simulated regional-scale ozone burdens both near the surface and aloft, estimates process contributions to these burdens, and calculates the sensitivity of the simulated regional-scale ozone burden to several key model inputs with a particular emphasis on boundary conditions derived from hemispheric or global-scale models. The Community Multiscale Air Quality (CMAQ) model simulations supporting this analysis were performed over the continental US for the year 2010 within the context of the Air Quality Model Evaluation International Initiative (AQMEII) and Task Force on Hemispheric Transport of Air Pollution (TF-HTAP) activities. CMAQ process analysis (PA) results highlight the dominant role of horizontal and vertical advection on the ozone burden in the mid-to-upper troposphere and lower stratosphere. Vertical mixing, including mixing by convective clouds, couples fluctuations in free-tropospheric ozone to ozone in lower layers. Hypothetical bounding scenarios were performed to quantify the effects of emissions, boundary conditions, and ozone dry deposition on the simulated ozone burden. Analysis of these simulations confirms that the characterization of ozone outside the regional-scale modeling domain can have a profound impact on simulated regional-scale ozone. This was further investigated by using data from four hemispheric or global modeling systems (Chemistry - Integrated Forecasting Model (C-IFS), CMAQ extended for hemispheric applications (H-CMAQ), the Goddard Earth Observing System model coupled to chemistry (GEOS-Chem), and AM3) to derive alternate boundary conditions for the regional-scale CMAQ simulations. The regional-scale CMAQ simulations using these four different boundary conditions showed that the largest ozone abundance in the upper layers was simulated when using boundary conditions from GEOS-Chem, followed by the simulations using C-IFS, AM3, and H-CMAQ boundary conditions, consistent with the analysis of the ozone fields from the global models along the CMAQ boundaries. Using boundary conditions from AM3 yielded higher springtime ozone columns burdens in the middle and lower troposphere compared to boundary conditions from the other models. For surface ozone, the differences between the AM3-driven CMAQ simulations and the CMAQ simulations driven by other large-scale models are especially pronounced during spring and winter where they can reach more than 10 ppb for seasonal mean ozone mixing ratios and as much as 15 ppb for domain-averaged daily maximum 8 h average ozone on individual days. In contrast, the differences between the C-IFS-, GEOS-Chem-, and H-CMAQ-driven regional-scale CMAQ simulations are typically smaller. Comparing simulated sur face ozone mixing ratios to observations and computing seasonal and regional model performance statistics revealed that boundary conditions can have a substantial impact on model performance. Further analysis showed that boundary conditions can affect model performance across the entire range of the observed distribution, although the impacts tend to be lower during summer and for the very highest observed percentiles. The results are discussed in the context of future model development and analysis opportunities.

Influence of anthropogenic emissions and boundary conditions on multi-model simulations of major air pollutants over Europe and North America in the framework of AQMEII3.

In the framework of the third phase of the Air Quality Model Evaluation International Initiative (AQMEII3), and as contribution to the second phase of the Hemispheric Transport of Air Pollution (HTAP2) activities for Europe and North America, the impacts of a 20 % decrease of global and regional anthropogenic emissions on surface air pollutant levels in 2010 are simulated by an international community of regional-scale air quality modeling groups, using different state-of-the-art chemistry and transport models (CTMs). The emission perturbations at the global level, as well as over the HTAP2-defined regions of Europe, North America and East Asia, are first simulated by the global Composition Integrated Forecasting System (C-IFS) model from European Centre for Medium-Range Weather Forecasts (ECMWF), which provides boundary conditions to the various regional CTMs participating in AQMEII3. On top of the perturbed boundary conditions, the regional CTMs used the same set of perturbed emissions within the regional domain for the different perturbation scenarios that introduce a 20 % reduction of anthropogenic emissions globally as well as over the HTAP2-defined regions of Europe, North America and East Asia.Results show that the largest impacts over both domains are simulated in response to the global emission perturbation, mainly due to the impact of domestic emission reductions. The responses of NO2, SO2 and PM concentrations to a 20 % anthropogenic emission reduction are almost linear (~ 20 % decrease) within the global perturbation scenario with, however, large differences in the geographical distribution of the effect. NO2, CO and SO2 levels are strongly affected over the emission hot spots. O3 levels generally decrease in all scenarios by up to ~ 1 % over Europe, with increases over the hot spot regions, in particular in the Benelux region, by an increase up to ~ 6 % due to the reduced effect of NOx titration. O3 daily maximum of 8 h running average decreases in all scenarios over Europe, by up to ~ 1 %. Over the North American domain, the central-to-eastern part and the western coast of the US experience the largest response to emission perturbations. Similar but slightly smaller responses are found when domestic emissions are reduced. The impact of intercontinental transport is relatively small over both domains, however, still noticeable particularly close to the boundaries. The impact is noticeable up to a few percent, for the western parts of the North American domain in response to the emission reductions over East Asia. O3 daily maximum of 8 h running average decreases in all scenarios over north Europe by up to ~ 5 %. Much larger reductions are calculated over North America compared to Europe.In addition, values of the Response to Extra-Regional Emission Reductions (RERER) metric have been calculated in order to quantify the differences in the strengths of nonlocal source contributions to different species among the different models. We found large RERER values for O3 (~ 0.8) over both Europe and North America, indicating a large contribution from non-local sources, while for other pollutants including particles, low RERER values reflect a predominant control by local sources. A distinct seasonal variation in the local vs. non-local contributions has been found for both O3 and PM2.5, particularly reflecting the springtime long-range transport to both continents.

Seasonal ozone vertical profiles over North America using the AQMEII3 group of air quality models: model inter-comparison and stratospheric intrusions.

This study evaluates simulated vertical ozone profiles produced in the framework of the third phase of the Air Quality Model Evaluation International Initiative (AQMEII3) against ozonesonde observations in North America for the year 2010. Four research groups from the United States (US) and Europe have provided modeled ozone vertical profiles to conduct this analysis. Because some of the modeling systems differ in their meteorological drivers, wind speed and temperature are also included in the analysis. In addition to the seasonal ozone profile evaluation for 2010, we also analyze chemically inert tracers designed to track the influence of lateral boundary conditions on simulated ozone profiles within the modeling domain. Finally, cases of stratospheric ozone intrusions during May–June 2010 are investigated by analyzing ozonesonde measurements and the corresponding model simulations at Intercontinental Chemical Transport Experiment Ozonesonde Network Study (IONS) experiment sites in the western United States. The evaluation of the seasonal ozone profiles reveals that, at a majority of the stations, ozone mixing ratios are underestimated in the 1–6 km range. The seasonal change noted in the errors follows the one seen in the variance of ozone mixing ratios, with the majority of the models exhibiting less variability than the observations. The analysis of chemically inert tracers highlights the importance of lateral boundary conditions up to 250 hPa for the lower-tropospheric ozone mixing ratios (0–2 km). Finally, for the stratospheric intrusions, the models are generally able to reproduce the location and timing of most intrusions but underestimate the magnitude of the maximum mixing ratios in the 2–6 km range and overestimate ozone up to the first kilometer possibly due to marine air influences that are not accurately described by the models. The choice of meteorological driver appears to be a greater predictor of model skill in this altitude range than the choice of air quality model.

Advanced error diagnostics of the CMAQ and Chimere modelling systems within the AQMEII3 model evaluation framework.

The work here complements the overview analysis of the modelling systems participating in the third phase of the Air Quality Model Evaluation International Initiative (AQMEII3) by focusing on the performance for hourly surface ozone by two modelling systems, Chimere for Europe and CMAQ for North America. The evaluation strategy outlined in the course of the three phases of the AQMEII activity, aimed to build up a diagnostic methodology for model evaluation, is pursued here and novel diagnostic methods are proposed. In addition to evaluating the "base case" simulation in which all model components are configured in their standard mode, the analysis also makes use of sensitivity simulations in which the models have been applied by altering and/or zeroing lateral boundary conditions, emissions of anthropogenic precursors, and ozone dry deposition. To help understand of the causes of model deficiencies, the error components (bias, variance, and covariance) of the base case and of the sensitivity runs are analysed in conjunction with timescale considerations and error modelling using the available error fields of temperature, wind speed, and NO x concentration. The results reveal the effectiveness and diagnostic power of the methods devised (which remains the main scope of this study), allowing the detection of the timescale and the fields that the two models are most sensitive to. The representation of planetary boundary layer (PBL) dynamics is pivotal to both models. In particular, (i) the fluctuations slower than ~ 1.5 days account for 70-85 % of the mean square error of the full (undecomposed) ozone time series; (ii) a recursive, systematic error with daily periodicity is detected, responsible for 10-20 % of the quadratic total error; (iii) errors in representing the timing of the daily transition between stability regimes in the PBL are responsible for a covariance error as large as 9 ppb (as much as the standard deviation of the network-average ozone observations in summer in both Europe and North America); (iv) the CMAQ ozone error has a weak/negligible dependence on the errors in NO2, while the error in NO2 significantly impacts the ozone error produced by Chimere; (v) the response of the models to variations of anthropogenic emissions and boundary conditions show a pronounced spatial heterogeneity, while the seasonal variability of the response is found to be less marked. Only during the winter season does the zeroing of boundary values for North America produce a spatially uniform deterioration of the model accuracy across the majority of the continent.

Source-sector contributions to European ozone and fine PM in 2010 using AQMEII modeling data

Abstract. Source apportionment modeling provides valuable information on the contributions of different source sectors and/or source regions to ozone (O3) or fine particulate matter (PM2.5) concentrations. This information can be useful in designing air quality management strategies and in understanding the potential benefits of reducing emissions from a particular source category. The Comprehensive Air quality Model with Extensions (CAMx) offers unique source attribution tools, called the Ozone and Particulate Source Apportionment Technology (OSAT/PSAT), which track source contributions. We present results from a CAMx source attribution modeling study for a summer month and a winter month using a recently evaluated European CAMx modeling database developed for Phase 3 of the Air Quality Model Evaluation International Initiative (AQMEII). The contributions of several source sectors (including model boundary conditions of chemical species representing transport of emissions from outside the modeling domain as well as initial conditions of these species) to O3 or PM2.5 concentrations in Europe were calculated using OSAT and PSAT, respectively. A 1-week spin-up period was used to reduce the influence of initial conditions. Evaluation focused on 16 major cities and on identifying source sectors that contributed above 5 %. Boundary conditions have a large impact on summer and winter ozone in Europe and on summer PM2.5, but they are only a minor contributor to winter PM2.5. Biogenic emissions are important for summer ozone and PM2.5. The important anthropogenic sectors for summer ozone are transportation (both on-road and non-road), energy production and conversion, and industry. In two of the 16 cities, solvent and product also contributed above 5 % to summertime ozone. For summertime PM2.5, the important anthropogenic source sectors are energy, transportation, industry, and agriculture. Residential wood combustion is an important anthropogenic sector in winter for PM2.5 over most of Europe, with larger contributions in central and eastern Europe and the Nordic cities. Other anthropogenic sectors with large contributions to wintertime PM2.5 include energy, transportation, and agriculture.

Evaluation and error apportionment of an ensemble of atmospheric chemistry transport modeling systems: multivariable temporal and spatial breakdown.

Through the comparison of several regional-scale chemistry transport modeling systems that simulate meteorology and air quality over the European and North American continents, this study aims at (i) apportioning error to the responsible processes using timescale analysis, (ii) helping to detect causes of model error, and (iii) identifying the processes and temporal scales most urgently requiring dedicated investigations. The analysis is conducted within the framework of the third phase of the Air Quality Model Evaluation International Initiative (AQMEII) and tackles model performance gauging through measurement-to-model comparison, error decomposition, and time series analysis of the models biases for several fields (ozone, CO, SO2, NO, NO2, PM10, PM2.5, wind speed, and temperature). The operational metrics (magnitude of the error, sign of the bias, associativity) provide an overallsense of model strengths and deficiencies, while apportioning the error to its constituent parts (bias, variance, and covariance) can help assess the nature and quality of the error. Each of the error components is analyzed independently and apportioned to specific processes based on the corresponding timescale (long scale, synoptic, diurnal, and intraday) using the error apportionment technique devised in the former phases of AQMEII. The application of the error apportionment method to the AQMEII Phase 3 simulations provides several key insights. In addition to reaffirming the strong impact of model inputs (emission and boundary conditions) and poor representation of the stable boundary layer on model bias, results also highlighted the high interdependencies among meteorological and chemical variables, as well as among their errors. This indicates that the evaluation of air quality model performance for individual pollutants needs to be supported by complementary analysis of meteorological fields and chemical precursors to provide results that are more insightful from a model development perspective. This will require evaluaion methods that are able to frame the impact on error of processes, conditions, and fluxes at the surface. For example, error due to emission and boundary conditions is dominant for primary species (CO, particulate matter (PM)), while errors due to meteorology and chemistry are most relevant to secondary species, such as ozone. Some further aspects emerged whose interpretation requires additional consideration, such as the uniformity of the synoptic error being region- and model-independent, observed for several pollutants; the source of unexplained variance for the diurnal component; and the type of error caused by deposition and at which scale.

Technical note: Coordination and harmonization of the multi-scale, multi-model activities HTAP2, AQMEII3, and MICS-Asia3: simulations, emission inventories, boundary conditions, and model output formats.

We present an overview of the coordinated global numerical modelling experiments performed during 2012–2016 by the Task Force on Hemispheric Transport of Air Pollution (TF HTAP), the regional experiments by the Air Quality Model Evaluation International Initiative (AQMEII) over Europe and North America, and the Model Intercomparison Study for Asia (MICS-Asia). To improve model estimates of the impacts of intercontinental transport of air pollution on climate, ecosystems, and human health and to answer a set of policy-relevant questions, these three initiatives performed emission perturbation modelling experiments consistent across the global, hemispheric, and continental/regional scales. In all three initiatives, model results are extensively compared against monitoring data for a range of variables (meteorological, trace gas concentrations, and aerosol mass and composition) from different measurement platforms (ground measurements, vertical profiles, airborne measurements) collected from a number of sources. Approximately 10 to 25 modelling groups have contributed to each initiative, and model results have been managed centrally through three data hubs maintained by each initiative. Given the organizational complexity of bringing together these three initiatives to address a common set of policy-relevant questions, this publication provides the motivation for the modelling activity, the rationale for specific choices made in the model experiments, and an overview of the organizational structures for both the modelling and the measurements used and analysed in a number of modelling studies in this special issue.

Insights into the deterministic skill of air quality ensembles from the analysis of AQMEII data

Abstract. Simulations from chemical weather models are subject to uncertainties in the input data (e.g. emission inventory, initial and boundary conditions) as well as those intrinsic to the model (e.g. physical parameterization, chemical mechanism). Multi-model ensembles can improve the forecast skill, provided that certain mathematical conditions are fulfilled. In this work, four ensemble methods were applied to two different datasets, and their performance was compared for ozone (O3), nitrogen dioxide (NO2) and particulate matter (PM10). Apart from the unconditional ensemble average, the approach behind the other three methods relies on adding optimum weights to members or constraining the ensemble to those members that meet certain conditions in time or frequency domain. The two different datasets were created for the first and second phase of the Air Quality Model Evaluation International Initiative (AQMEII). The methods are evaluated against ground level observations collected from the EMEP (European Monitoring and Evaluation Programme) and AirBase databases. The goal of the study is to quantify to what extent we can extract predictable signals from an ensemble with superior skill over the single models and the ensemble mean. Verification statistics show that the deterministic models simulate better O3 than NO2 and PM10, linked to different levels of complexity in the represented processes. The unconditional ensemble mean achieves higher skill compared to each station's best deterministic model at no more than 60 % of the sites, indicating a combination of members with unbalanced skill difference and error dependence for the rest. The promotion of the right amount of accuracy and diversity within the ensemble results in an average additional skill of up to 31 % compared to using the full ensemble in an unconditional way. The skill improvements were higher for O3 and lower for PM10, associated with the extent of potential changes in the joint distribution of accuracy and diversity in the ensembles. The skill enhancement was superior using the weighting scheme, but the training period required to acquire representative weights was longer compared to the sub-selecting schemes. Further development of the method is discussed in the conclusion.

Error apportionment for atmospheric chemistry-transport models – a new approach to model evaluation

Abstract. In this study, methods are proposed to diagnose the causes of errors in air quality (AQ) modelling systems. We investigate the deviation between modelled and observed time series of surface ozone through a revised formulation for breaking down the mean square error (MSE) into bias, variance and the minimum achievable MSE (mMSE). The bias measures the accuracy and implies the existence of systematic errors and poor representation of data complexity, the variance measures the precision and provides an estimate of the variability of the modelling results in relation to the observed data, and the mMSE reflects unsystematic errors and provides a measure of the associativity between the modelled and the observed fields through the correlation coefficient. Each of the error components is analysed independently and apportioned to resolved processes based on the corresponding timescale (long scale, synoptic, diurnal, and intra-day) and as a function of model complexity.The apportionment of the error is applied to the AQMEII (Air Quality Model Evaluation International Initiative) group of models, which embrace the majority of regional AQ modelling systems currently used in Europe and North America.The proposed technique has proven to be a compact estimator of the operational metrics commonly used for model evaluation (bias, variance, and correlation coefficient), and has the further benefit of apportioning the error to the originating timescale, thus allowing for a clearer diagnosis of the processes that caused the error.

Funcionamiento del Sistema WRF-CMAQ para Bulgaria con tres subdominios en Europa

The air quality modelling system WRF-CMAQ running at the National Institute of Meteorology and Hydrology (NIMH) in Sofia was applied to the European domain for the year 2010 in the frame of the Air Quality Model Evaluation International Initiative (AQMEII), Phase 2. The model system was set up for a domain of 5000x5000 km2 size with horizontal resolution of 25 km. The models’ options used and the emission input are briefly outlined. The model performance was investigated based on graphical plots and statistical indexes obtained by the web-based model evaluation platform ENSEMBLE. A preliminary operational model evaluation for ozone and particulate matter was conducted, comparing simulated and observed concentrations at ground level in three sub-domains of Europe. The analysis shows model overestimation for ozone and model underestimation for particulate matter. The best statistical indicators are for ozone concentrations during summer, when comparing data for EMEP stations in the EU domain. The worse results are for PM10 winter concentration in the region of the Balkan countries.

Application of WRF/Chem over North America under the AQMEII Phase 2 – Part 2: Evaluation of 2010 application and responses of air quality and meteorology–chemistry interactions to changes in emissions and meteorology from 2006 to 2010

Abstract. The Weather Research and Forecasting model with Chemistry (WRF/Chem) simulation with the 2005 Carbon Bond (CB05) gas-phase mechanism coupled to the Modal for Aerosol Dynamics for Europe (MADE) and the volatility basis set approach for secondary organic aerosol (SOA) are conducted over a domain in North America for 2006 and 2010 as part of the Air Quality Model Evaluation International Initiative (AQMEII) Phase 2 project. Following the Part 1 paper that focuses on the evaluation of the 2006 simulations, this Part 2 paper focuses on a comparison of model performance in 2006 and 2010 as well as analysis of the responses of air quality and meteorology–chemistry interactions to changes in emissions and meteorology from 2006 to 2010. In general, emissions for gaseous and aerosol species decrease from 2006 to 2010, leading to a reduction in gaseous and aerosol concentrations and associated changes in radiation and cloud variables due to various feedback mechanisms. WRF/Chem is able to reproduce most observations and the observed variation trends from 2006 to 2010, despite its slightly worse performance than WRF that is likely due to inaccurate chemistry feedbacks resulting from less accurate emissions and chemical boundary conditions (BCONs) in 2010. Compared to 2006, the performance for most meteorological variables in 2010 gives lower normalized mean biases but higher normalized mean errors and lower correlation coefficients. The model also shows poorer performance for most chemical variables in 2010. This could be attributed to underestimations in emissions of some species, such as primary organic aerosol in some areas of the US in 2010, and inaccurate chemical BCONs and meteorological predictions. The inclusion of chemical feedbacks in WRF/Chem reduces biases in meteorological predictions in 2010; however, it increases errors and weakens correlations comparing to WRF simulations. Sensitivity simulations show that the net changes in meteorological variables from 2006 to 2010 are mostly influenced by changes in meteorology and those of ozone and fine particulate matter are influenced to a large extent by emissions and/or chemical BCONs and to a lesser extent by changes in meteorology. Using a different set of emissions and/or chemical BCONs helps improve the performance of individual variables, although it does not improve the degree of agreement with observed interannual trends. These results indicate a need to further improve the accuracy and consistency of emissions and chemical BCONs, the representations of SOA and chemistry–meteorology feedbacks in the online-coupled models.

Sensitivity of feedback effects in CBMZ/MOSAIC chemical mechanism

To investigate the impact of the aerosol effects on meteorological variables and pollutant concentrations two simulations with the WRF-Chem model have been performed over Europe for year 2010. We have performed a baseline simulation without any feedback effects and a second simulation including the direct as well as the indirect aerosol effect. The paper describes the full configuration of the model, the simulation design, special impacts and evaluation. Although low aerosol particle concentrations are detected, the inclusion of the feedback effects results in an increase of solar radiation at the surface over cloudy areas (North-West, including the Atlantic) and decrease over more sunny locations (South-East). Aerosol effects produce an increase of the water vapor and decrease the planet boundary layer height over the whole domain except in the Sahara area, where the maximum particle concentrations are detected. Significant ozone concentrations are found over the Mediterranean area. Simulated feedback effects between aerosol concentrations and meteorological variables and on pollutant distributions strongly depend on the aerosol concentrations and the clouds. Further investigations are necessary with higher aerosol particle concentrations. WRF-Chem variables are evaluated using available hourly observations in terms of performance statistics. Standardized observations from the ENSEMBLE system web-interface were used. The research was developed under the second phase of Air Quality Model Evaluation International Initiative (AQMEII). WRF-Chem demonstrates its capability in capturing temporal and spatial variations of the major meteorological variables and pollutants, except the wind speed over complex terrain. The wind speed bias may affect the accuracy in the chemical predictions (NO2, SO2). The analysis of the correlations between simulated data sets and observational data sets indicates that the simulation with aerosol effects performs slightly better. These results indicate potential importance of the aerosol feedback effects and an urgent need to further improve the representations in current atmospheric models to reduce uncertainties at all scales.

A comparison between 2010 and 2006 air quality and meteorological conditions, and emissions and boundary conditions used in simulations of the AQMEII-2 North American domain

Several participants in Phase 2 of the Air Quality Model Evaluation International Initiative (AQMEII-2) who are applying coupled models to the North American domain are comparing model results for two years, 2006 and 2010, with the goal of performing dynamic model evaluation. From a modeling perspective, the differences of interest are the large reductions in domain total emissions of NOx (21%) and SO2 (37%) from 2006 to 2010 and significant differences in meteorological conditions between these two years. The emission reductions occurred mostly in the eastern U.S, with some reduction in emissions from western wildfires in 2010. Differences in meteorological conditions both confound the impact of emission reductions on ambient air quality and provide an opportunity to examine how models respond to changing meteorology. This study is aimed at documenting changes in emissions, modeled large-scale background concentrations used as boundary conditions for the regional models, and observed meteorology and air quality to provide a context for the dynamic model evaluation studies performed within AQMEII-2. In addition to warmer summer temperatures, conditions in the eastern U.S. summer of 2010 were characterized by less precipitation than in 2006, while western portions of the U.S. and Canada were much cooler in 2010 due to a strengthening of the thermal trough over the Southwest and associated onshore flow. Summer ozone levels in many portions of the Northeast and Midwest were largely unchanged in 2010 despite reductions in precursor emissions. Normalization of the ozone trend, to account for differences in meteorological conditions, including warmer summer temperatures in 2010, shows that the emission reductions would have resulted in lower ozone levels at these locations if not for the countervailing influence of meteorological conditions. Winter mean surface temperatures were generally above average in 2006 whereas below average temperatures were noted in the Southeast and northern plains in 2010, consistent with a greater frequency of cold arctic air outbreaks. In general, changes in observed air quality as measured at U.S. monitoring sites appear to be consistent with differences in emissions and meteorological conditions between 2006 and 2010. Two potential inconsistencies were noted which warrant further investigation: 1) an increase in particulate nitrate during the winter in the Midwest despite lower emissions of NOx and 2) lower than expected SO2 reductions in the Southeast during the winter.

Assessment of the MACC reanalysis and its influence as chemical boundary conditions for regional air quality modeling in AQMEII-2

The Air Quality Model Evaluation International Initiative (AQMEII) has now reached its second phase which is dedicated to the evaluation of online coupled chemistry-meteorology models. Sixteen modeling groups from Europe and five from North America have run regional air quality models to simulate the year 2010 over one European and one North American domain. The MACC re-analysis has been used as chemical initial (IC) and boundary conditions (BC) by all participating regional models in AQMEII-2. The aim of the present work is to evaluate the MACC re-analysis along with the participating regional models against a set of ground-based measurements (O3, CO, NO, NO2, SO2, SO42−) and vertical profiles (O3 and CO). Results indicate different degrees of agreement between the measurements and the MACC re-analysis, with an overall better performance over the North American domain. The influence of BC on regional air quality simulations is analyzed in a qualitative way by contrasting model performance for the MACC re-analysis with that for the regional models. This approach complements more quantitative approaches documented in the literature that often have involved sensitivity simulations but typically were limited to only one or only a few regional scale models. Results suggest an important influence of the BC on ozone for which the underestimation in winter in the MACC re-analysis is mimicked by the regional models. For CO, it is found that background concentrations near the domain boundaries are rather close to observations while those over the interior of the two continents are underpredicted by both MACC and the regional models over Europe but only by MACC over North America. This indicates that emission differences between the MACC re-analysis and the regional models can have a profound impact on model performance and points to the need for harmonization of inputs in future linked global/regional modeling studies.