Evolution of perturbations in 3D air quality models

The deterministic approach of sensitivity analysis is applied on the solution vector of an Air Quality Model. In particular, the photochemical CAMx code is augmented with derivatives utilising the automatic differentiation software ADIFOR. The enhanced with derivatives version of the model is then adopted in a study of the effect of perturbations at the boundary conditions on the predicted ozone concentrations. The calculated derivative matrix provides valuable information e.g., on the ordering of the infl uential factors or the localisation of highly affected regions. Two fundamentally different domains of the Auto-Oil II programme were used as test cases for the simulations, namely Athens and Milan. The results suggest that ozone concentration be highly affected by its own boundary conditions and subsequently, with an order of magnitude less, by the boundary conditions of NOX and VOC

Effects of methane outgassing on the Black Sea atmosphere

International audienceMethane in air and seawater was measured in the Eastern Black Sea during the 10?18 December 1999 BIGBLACK project cruise. The measurements allowed for the calculation of supersaturation ratios and methane fluxes across the air-sea interface. CH4 mixing ratios in air were generally in the 1.8?2.0 ppmv range, while surface (4 m depth) seawater concentrations varied from 5 to 100 ppmv. Above active seep areas, the water was supersaturated at around 500% with respect to the overlying atmosphere. Accordingly, flux densities varied greatly and were up to 4000 umol m-2 day-1. In the Sevastopol harbour, supersaturations up to around 3000%, similar to those at the Danube Delta, were observed, while in the Istanbul harbour supersaturations could not be determined because the very high values of water concentrations have led to detector saturation. Simple modelling shows that the observed fluxes do not have any substantial impact in the methane content of the Black Sea atmosphere, as they could only raise its concentrations by less than 1 ppb. On the other hand, calculations performed as part of the CRIMEA project, show that mud volcano eruptions could episodically raise the methane concentrations well above their regional background for several tens of kilometres downwind

Decadal regional air quality simulations over Europe in present climate: near surface ozone sensitivity to external meteorological forcing

Abstract. Regional climate-air quality decadal simulations over Europe were carried out with the RegCM3/CAMx modeling system for the time slice 1991–2000, in order to study the impact of different meteorological forcing on surface ozone. The RegCM3 regional climate model was firstly constrained by the ERA40 reanalysis dataset which is considered as an experiment with perfect meteorological boundary conditions and then it was constrained by the global circulation model ECHAM5. A number of meteorological parameters were examined including the 500 mb geopotential height, solar radiation, temperature, cloud liquid water path, planetary boundary layer height and surface wind. The different RegCM meteorological forcing resulted in changes of near surface ozone over Europe ranging between ± 4 ppb for winter and summer. The area showing the greatest sensitivity in O3 during winter is central and southern Europe while in summer central north continental Europe. The different meteorological forcing impacts on the atmospheric circulation, which in turn affects cloudiness and solar radiation, temperature, wind patterns and the meteorology depended biogenic emissions. For comparison reasons, the impact of chemical boundary conditions on surface ozone was additionally examined with a series of sensitivity studies, indicating that surface ozone changes are comparable to those caused by the different meteorological forcing. These findings suggest that, when it comes to regional climate-air quality simulations, the selection of external meteorological forcing can be as important as the selection of adequate chemical lateral boundary conditions

Changes in PM2.5 concentrations and their sources in the US from 1990 to 2010

Significant reductions in emissions of SO2, NOx, volatile organic compounds (VOCs), and primary particulate matter (PM) took place in the US from 1990 to 2010. We evaluate here our understanding of the links between these emissions changes and corresponding changes in concentrations and health outcomes using a chemical transport model, the Particulate Matter Comprehensive Air Quality Model with Extensions (PMCAMx), for 1990, 2001, and 2010. The use of the Particle Source Apportionment Algorithm (PSAT) allows us to link the concentration reductions to the sources of the corresponding primary and secondary PM. The reductions in SO2 emissions (64 %, mainly from electric-generating units) during these 20 years have dominated the reductions in PM2.5, leading to a 45 % reduction in sulfate levels. The predicted sulfate reductions are in excellent agreement with the available measurements. Also, the reductions in elemental carbon (EC) emissions (mainly from transportation) have led to a 30 % reduction in EC concentrations. The most important source of organic aerosol (OA) through the years according to PMCAMx is biomass burning, followed by biogenic secondary organic aerosol (SOA). OA from on-road transport has been reduced by more than a factor of 3. On the other hand, changes in biomass burning OA and biogenic SOA have been modest. In 1990, about half of the US population was exposed to annual average PM2.5 concentrations above 20 µg m−3, but by 2010 this fraction had dropped to practically zero. The predicted changes in concentrations are evaluated against the observed changes for 1990, 2001, and 2010 in order to understand whether the model represents reasonably well the corresponding processes caused by the changes in emissions.This work was supported by the Center for Air, Climate, and Energy Solutions (CACES), which was supported under assistance agreement no. R835873 awarded by the U.S. Environmental Protection Agency and the Horizon-2020 Project REMEDIA of the European Union under grant agreement no. 874753.Peer ReviewedPostprint (published version

Evaluation of high-resolution predictions of fine particulate matter and its composition in an urban area using PMCAMx-v2.0

Accurately predicting urban PM2.5 concentrations and composition has proved challenging in the past, partially due to the resolution limitations of computationally intensive chemical transport models (CTMs). Increasing the resolution of PM2.5 predictions is desired to support emissions control policy development and address issues related to environmental justice. A nested grid approach using the CTM PMCAMx-v2.0 was used to predict PM2.5 at increasing resolutions of 36 km × 36 km, 12 km × 12 km, 4 km × 4 km, and 1 km × 1 km for a domain largely consisting of Allegheny County and the city of Pittsburgh in southwestern Pennsylvania, US, during February and July 2017. Performance of the model in reproducing PM2.5 concentrations and composition was evaluated at the finest scale using measurements from regulatory sites as well as a network of low-cost monitors. Novel surrogates were developed to allocate emissions from cooking and on-road traffic sources to the 1 km × 1 km resolution grid. Total PM2.5 mass is reproduced well by the model during the winter period with low fractional error (0.3) and fractional bias (+0.05) when compared to regulatory measurements. Comparison with speciated measurements during this period identified small underpredictions of PM2.5 sulfate, elemental carbon (EC), and organic aerosol (OA) offset by a larger overprediction of PM2.5 nitrate. In the summer period, total PM2.5 mass is underpredicted due to a large underprediction of OA (bias = −1.9 µg m−3, fractional bias = −0.41). In the winter period, the model performs well in reproducing the variability between urban measurements and rural measurements of local pollutants such as EC and OA. This effect is less consistent in the summer period due to a larger fraction of long-range-transported OA. Comparison with total PM2.5 concentration measurements from low-cost sensors showed improvements in performance with increasing resolution. Inconsistencies in PM2.5 nitrate predictions in both periods are believed to be due to errors in partitioning between PM2.5 and PM10 modes and motivate improvements to the treatment of dust particles within the model. The underprediction of summer OA would likely be improved by updates to biogenic secondary organic aerosol (SOA) chemistry within the model, which would result in an increase of long-range transport SOA seen in the inner modeling domain. These improvements are obvious topics for future work towards model improvement. Comparison with regulatory monitors showed that increasing resolution from 36 to 1 km improved both fractional error and fractional bias in both modeling periods. Improvements at all types of measurement locations indicated an improved ability of the model to reproduce urban–rural PM2.5 gradients at higher resolutions.</p

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

© 2016. This is an Open Access article, distributed under the terms of the Creative Commons Attribution licence (http://creativecommons.org/licenses/by/4.0/), which permits unrestricted re-use, distribution, and reproduction in any medium, provided the original work is properly cited. Ioannis Kioutsioukis, et al, ‘Insights into the deterministic skill of air quality ensembles from the analysis of AQMEII data’, Atmospheric Chemistry and Physics, Vol 16(24): 15629-15652, published 20 December 2016, the version of record is available at doi:10.5194/acp-16-15629-2016 Published by Copernicus Publications on behalf of the European Geosciences Union.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.Peer reviewedFinal Published versio

Corrigendum to "Satellite observations and model simulations of tropospheric NO₂ columns over south-eastern Europe" published in Atmos. Chem. Phys., 9, 6119–6134, 2009

No abstract available

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&thinsp;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&thinsp;hPa for the lower-tropospheric ozone mixing ratios (0–2&thinsp;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&thinsp;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.</p

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

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 (O$_{3}$), nitrogen dioxide (NO$_{2}$) and particulate matter (PM$_{10}$). 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 O$_{3}$ than NO$_{2}$ and PM$_{10}$, 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 O$_{3}$ and lower for PM$_{10}$, 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

Statistical assessment of changes in climate extremes over Greece (1955-2002)

This article focuses on extreme events of high and low temperatures and precipitation and their amplitude and frequency changes over the last 50 years in Greece. Sixteen climate indices have been calculated and their trends were analysed to identify possible changes over a network of measurement stations covering the region quite homogeneously. Furthermore, the changes in the probability distribution of the indices were examined. In addition, we analyzed the temporal evolution of the amplitude and frequency of extreme events through the parameters of extreme value distribution. The temporal stability of the fitted distributions is examined and the spatial distribution of their trend as well as the changes in the 5-year return levels is investigated. Half of the examined climatic indices exhibit significant regional trend; most of them are sole functions of minimum temperature or precipitation. A shift was found in the tail distribution of the peak minimum temperatures, with the 5-year return value in the last quartile of the twientieth century to be equal to the 7-year return value in the previous quartile. Warming was also apparent for the maximum temperature, mainly in the summer months, but of smaller magnitude. Total precipitation shifted towards drier climate over the domain while extreme rainfall events exhibit increased variability without following any coherent regional pattern. The changes in the peak temperature extremes are most sensitive to the changes in the location of the distribution of annual extremes. Changes in the precipitation extremes are associated with changes in both the scale and location of the fitted distribution. The highest range of change was found for the scale parameter for both temperature and precipitation extremes, pointing out that the most influenced factor is the interannual variability of the extremes. © 2009 Royal Meteorological Society