Abstract. Biogenic volatile organic compound (BVOC) emissions are one of the essential inputs for chemical transport models (CTMs), but their estimates are associated with large uncertainties, leading to significant influence on air quality modelling. This study aims to investigate the effects of using different BVOC emission models on the performance of a CTM in simulating secondary pollutants, i.e. ozone, organic, and inorganic aerosols. European air quality was simulated for the year 2011 by the regional air quality model Comprehensive Air Quality Model with Extensions (CAMx) version 6.3, using BVOC emissions calculated by two emission models: the Paul Scherrer Institute (PSI) model and the Model of Emissions of Gases and Aerosol from Nature (MEGAN) version 2.1. Comparison of isoprene and monoterpene emissions from both models showed large differences in their general amounts, as well as their spatial distribution in both summer and winter. MEGAN produced more isoprene emissions by a factor of 3 while the PSI model generated 3 times the monoterpene emissions in summer, while there was negligible difference (∼4 %) in sesquiterpene emissions associated with the two models. Despite the large differences in isoprene emissions (i.e. 3-fold), the resulting impact in predicted summertime ozone proved to be minor (<10 %; MEGAN O3 was higher than PSI O3 by ∼7 ppb). Comparisons with measurements from the European air quality database (AirBase) indicated that PSI emissions might improve the model performance at low ozone concentrations but worsen performance at high ozone levels (>60 ppb). A much larger effect of the different BVOC emissions was found for the secondary organic aerosol (SOA) concentrations. The higher monoterpene emissions (a factor of ∼3) by the PSI model led to higher SOA by ∼110 % on average in summer, compared to MEGAN, and lead to better agreement between modelled and measured organic aerosol (OA): the mean bias between modelled and measured OA at nine measurement stations using Aerodyne aerosol chemical speciation monitors (ACSMs) or Aerodyne aerosol mass spectrometers (AMSs) was reduced by 21 %–83 % at rural or remote stations. Effects on inorganic aerosols (particulate nitrate, sulfate, and ammonia) were relatively small (<15 %).
Abstract. High surface ozone concentrations, which usually occur when photochemical ozone production takes place, pose a great risk to human health and vegetation. Air quality models are often used by policy makers as tools for the development of ozone mitigation strategies. However, the modeled ozone production is often not or not enough evaluated in many ozone modeling studies. The focus of this work is to evaluate the modeled ozone production in Europe indirectly, with the use of the ozone-temperature correlation for the summer of 2010 and to analyze its sensitivity to precursor emissions and meteorology by using the regional air quality model, the Comprehensive Air Quality Model with Extensions (CAMx). The results show that the model significantly underestimates the observed high afternoon surface ozone mixing ratios (≥ 60 ppb) by 10-20 ppb and overestimates the lower ones (< 40 ppb) by 5-15 ppb, resulting in a misleading good agreement with the observations for average ozone. The model also underestimates the ozone-temperature regression slope by about a factor of 2 for most of the measurement stations. To investigate the impact of emissions, four scenarios were tested: (i) increased volatile organic compound (VOC) emissions by a factor of 1.5 and 2 for the anthropogenic and biogenic VOC emissions, respectively, (ii) increased nitrogen oxide (NO x ) emissions by a factor of 2, (iii) a combination of the first two scenarios and (iv) increased trafficonly NO x emissions by a factor of 4. For southern, eastern, and central (except the Benelux area) Europe, doubling NO x emissions seems to be the most efficient scenario to reduce the underestimation of the observed high ozone mixing ratios without significant degradation of the model performance for the lower ozone mixing ratios. The model performance for ozone-temperature correlation is also better when NO x emissions are doubled. In the Benelux area, however, the third scenario (where both NO x and VOC emissions are increased) leads to a better model performance. Although increasing only the traffic NO x emissions by a factor of 4 gave very similar results to the doubling of all NO x emissions, the first scenario is more consistent with the uncertainties reported by other studies than the latter, suggesting that high uncertainties in NO x emissions might originate mainly from the road-transport sector rather than from other sectors. The impact of meteorology was examined with three sensitivity tests: (i) increased surface temperature by 4 • C, (ii) reduced wind speed by 50 % and (iii) doubled wind speed. The first two scenarios led to a consistent increase in all surface ozone mixing ratios, thus improving the model performance for the high ozone values but significantly degrading it for the low ozone values, while the third scenario had exactly the opposite effects. Overall, the modeled ozone is predicted to be more sensitive to its precursor emissions (especially traffic NO x ) and therefore their uncertainties, which seem to be responsible for the model un...
<p><strong>Abstract.</strong> Biogenic volatile organic compound (BVOC) emissions are one of the essential inputs for chemical transport models (CTMs), but their estimates are associated with large uncertainties leading to significant influences on air quality modelling. This study aims at investigating the effects of using different BVOC emission models on the performance of a CTM in simulating secondary pollutants, i.e. ozone, organic and inorganic aerosols. The European air quality was simulated for the year 2011 by the regional air quality model Comprehensive Air Quality Model with Extensions (CAMx) version 6.3, using BVOC emissions calculated by two emission models: the Paul Scherrer Institute (PSI) model and the Model of Emissions of Gases and Aerosol from Nature (MEGAN) v2.1. Comparison of isoprene and monoterpene emissions from both models showed large differences in their general amounts as well as their spatial distribution both in summer and winter. MEGAN produced more isoprene emissions by a factor of 3 while the PSI model generated three times of monoterpene emissions in summer, while there was negligible difference (~&#8201;4&#8201;%) in sesquiterpene emissions associated with the two models. Despite the large differences in isoprene emissions (i.e. 3-fold), the resulting impact in predicted summer-time ozone proved to be minor (<&#8201;10&#8201;%, O<sub>3</sub>-MEGAN was higher than O<sub>3</sub>-PSI by ~&#8201;7&#8201;ppb). Comparisons with measurements from the European air quality database (AirBase) indicated that PSI emissions might improve the model performance at low ozone concentrations, but worsen it at high ozone levels (>&#8201;60&#8201;ppb). A much larger effect of the different BVOC emissions was found for the secondary organic aerosol (SOA) concentrations. The higher monoterpene emissions (a factor of ~&#8201;3) by the PSI model led to higher SOA by ~&#8201;110&#8201;% on average in summer, compared to MEGAN, improving substantially the model performance for organic aerosol (OA): the mean bias between modelled and measured OA at 8 Aerodyne aerosol chemical speciation monitor (ACSM)/Aerodyne aerosol mass spectrometer (AMS) measurement stations was reduced by 21&#8201;%&#8211;83&#8201;% in rural/remote stations. Effects on inorganic aerosols (particulate nitrate, sulphate, and ammonia) were relatively smaller (<&#8201;15&#8201;%).</p>
<p><strong>Abstract.</strong> High surface ozone concentrations, which usually occur when photochemical ozone production takes place, pose a great risk to human health and vegetation. Air quality models are often used by policy makers as tools for the development of ozone mitigation strategies. However, the modeled ozone production is often not or not enough evaluated in many ozone modelling studies. The focus of this work is to evaluate the modeled ozone production in Europe indirectly, with the use of the ozone&#8211;temperature correlation for the summer of 2010 and to analyze its sensitivity to precursor emissions and meteorology by using the regional air quality model, CAMx. The results show that the model significantly underestimates the observed high afternoon surface ozone mixing ratios (&#8805;&#8201;60&#8201;ppb) by 10&#8211;20&#8201;ppb and overestimates the lower ones (<&#8201;40&#8201;ppb) by 5&#8211;15&#8201;ppb, resulting in a misleading good agreement with the observations for average ozone. The model also underestimates the ozone&#8211;temperature regression slope by about a factor of 2 for most of the measurement stations. To investigate the impact of emissions, three scenarios were tested: (i) increased VOC emissions by a factor of 1.5 and 2 for the anthropogenic and biogenic VOC emissions, respectively, (ii) increased NO<sub<x</sub> emissions by a factor of 2, and (iii) a combination of the first two scenarios. For southern and central (except the Benelux area) Europe, doubling NO<sub>x</sub> emissions seems to be the most efficient scenario to reduce the underestimation of the observed high ozone mixing ratios without significant degradation of the model performance for the lower ozone mixing ratios. The model performance for ozone&#8211;temperature correlation is also better when NO<sub>x</sub> emissions are doubled. In the Benelux area, however, the third scenario (where both NO<sub>x</sub> and VOC emissions are increased) leads to a better model performance. The impact of meteorology was examined with two sensitivity tests: (i) increased surface temperature by 4&#8201;&#176;C, and (ii) reduced wind speed by 50&#8201;%. Both scenarios lead to a consistent increase in all surface ozone mixing ratios, thus improving the model performance for the high ozone values but significantly degrading it for the low ozone values. Overall, the modeled ozone is predicted to be more sensitive to its precursor emissions (especially NO<sub>x</sub>) and therefore their uncertainties, which seem to be responsible for the model underestimation of the observed high ozone mixing ratios and ozone production.</p>
Abstract. Surface solar radiation (SSR) observations have indicated an increasing trend in Europe since the mid-1980s, referred to as solar “brightening”. In this study, we used the regional air quality model, CAMx (Comprehensive Air Quality Model with Extensions) to simulate and quantify, with various sensitivity runs (where the year 2010 served as the base case), the effects of increased radiation between 1990 and 2010 on photolysis rates (with the PHOT1, PHOT2 and PHOT3 scenarios, which represented the radiation in 1990) and biogenic volatile organic compound (BVOC) emissions (with the BIO scenario, which represented the biogenic emissions in 1990), and their consequent impacts on summer surface ozone concentrations over Europe between 1990 and 2010. The PHOT1 and PHOT2 scenarios examined the effect of doubling and tripling the anthropogenic PM2.5 concentrations, respectively, while the PHOT3 investigated the impact of an increase in just the sulfate concentrations by a factor of 3.4 (as in 1990), applied only to the calculation of photolysis rates. In the BIO scenario, we reduced the 2010 SSR by 3 % (keeping plant cover and temperature the same), recalculated the biogenic emissions and repeated the base case simulations with the new biogenic emissions. The impact on photolysis rates for all three scenarios was an increase (in 2010 compared to 1990) of 3–6 % which resulted in daytime (10:00–18:00 Local Mean Time – LMT) mean surface ozone differences of 0.2–0.7 ppb (0.5–1.5 %), with the largest hourly difference rising as high as 4–8 ppb (10–16 %). The effect of changes in BVOC emissions on daytime mean surface ozone was much smaller (up to 0.08 ppb, ∼ 0.2 %), as isoprene and terpene (monoterpene and sesquiterpene) emissions increased only by 2.5–3 and 0.7 %, respectively. Overall, the impact of the SSR changes on surface ozone was greater via the effects on photolysis rates compared to the effects on BVOC emissions, and the sensitivity test of their combined impact (the combination of PHOT3 and BIO is denoted as the COMBO scenario) showed nearly additive effects. In addition, all the sensitivity runs were repeated on a second base case with increased NOx emissions to account for any potential underestimation of modeled ozone production; the results did not change significantly in magnitude, but the spatial coverage of the effects was profoundly extended. Finally, the role of the aerosol–radiation interaction (ARI) changes in the European summer surface ozone trends was suggested to be more important when comparing to the order of magnitude of the ozone trends instead of the total ozone concentrations, indicating a potential partial damping of the effects of ozone precursor emissions' reduction.
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