| 1. |
- Ciarelli, Giancarlo, et al.
(författare)
-
Trends of inorganic and organic aerosols and precursor gases in Europe: Insights from the EURODELTA multi-model experiment over the 1990-2010 period
- 2019
-
Ingår i: Geoscientific Model Development. - : Copernicus GmbH. - 1991-959X .- 1991-9603. ; 12:12, s. 4923-4954
-
Tidskriftsartikel (refereegranskat)abstract
- In the framework of the EURODELTA-Trends (EDT) modeling experiment, several chemical transport models (CTMs) were applied for the 1990-2010 period to investigate air quality changes in Europe as well as the capability of the models to reproduce observed long-term air quality trends. Five CTMs have provided modeled air quality data for 21 continuous years in Europe using emission scenarios prepared by the International Institute for Applied Systems Analysis/Greenhouse Gas - Air Pollution Interactions and Synergies (IIASA/GAINS) and corresponding year-by-year meteorology derived from ERA-Interim global reanalysis. For this study, long-term observations of particle sulfate (SO2 4-), total nitrate (TNO3), total ammonium (TNHx) as well as sulfur dioxide (SO2) and nitrogen dioxide (NO2) for multiple sites in Europe were used to evaluate the model results. The trend analysis was performed for the full 21 years (referred to as PT) but also for two 11-year subperiods: 1990-2000 (referred to as P1) and 2000-2010 (referred to as P2). The experiment revealed that the models were able to reproduce the faster decline in observed SO2 concentrations during the first decade, i.e., 1990-2000, with a 64%-76% mean relative reduction in SO2 concentrations indicated by the EDT experiment (range of all the models) versus an 82% mean relative reduction in observed concentrations. During the second decade (P2), the models estimated a mean relative reduction in SO2 concentrations of about 34%-54%, which was also in line with that observed (47%). Comparisons of observed and modeled NO2 trends revealed a mean relative decrease of 25% and between 19% and 23% (range of all the models) during the P1 period, and 12% and between 22% and 26% (range of all the models) during the P2 period, respectively. Comparisons of observed and modeled trends in SO4 2- concentrations during the P1 period indicated that the models were able to reproduce the observed trends at most of the sites, with a 42%-54% mean relative reduction indicated by the EDT experiment (range of all models) versus a 57% mean relative reduction in observed concentrations and with good performance also during the P2 and PT periods, even though all the models overpredicted the number of statistically significant decreasing trends during the P2 period. Moreover, especially during the P1 period, both modeled and observational data indicated smaller reductions in SO42- concentrations compared with their gas-phase precursor (i.e., SO2), which could be mainly attributed to increased oxidant levels and pH-dependent cloud chemistry. An analysis of the trends in TNO3 concentrations indicated a 28%-39% and 29% mean relative reduction in TNO3 concentrations for the full period for model data (range of all the models) and observations, respectively. Further analysis of the trends in modeled HNO3 and particle nitrate (NO-3 ) concentrations revealed that the relative reduction in HNO3 was larger than that for NO-3 during the P1 period, which was mainly attributed to an increased availability of "free ammonia". By contrast, trends in modeled HNO3 and NO-3 concentrations were more comparable during the P2 period. Also, trends of TNHx concentrations were, in general, underpredicted by all models, with worse performance for the P1 period than for P2. Trends in modeled anthropogenic and biogenic secondary organic aerosol (ASOA and BSOA) concentrations together with the trends in available emissions of biogenic volatile organic compounds (BVOCs) were also investigated. A strong decrease in ASOA was indicated by all the models, following the reduction in anthropogenic non-methane VOC (NMVOC) precursors. Biogenic emission data provided by the modeling teams indicated a few areas with statistically significant increase in isoprene emissions and monoterpene emissions during the 1990-2010 period over Fennoscandia and eastern European regions (i.e., around 14 %-27 %), which was mainly attributed to the increase of surface temperature. However, the modeled BSOA concentrations did not linearly follow the increase in biogenic emissions. Finally, a comprehensive evaluation against positive matrix factorization (PMF) data, available during the second period (P2) at various European sites, revealed a systematic underestimation of the modeled SOA fractions of a factor of 3 to 11, on average, most likely because of missing SOA precursors and formation pathways, with reduced biases for the models that accounted for chemical aging of semi-volatile SOA components in the atmosphere.
|
|
| 2. |
- Colette, Augustin, et al.
(författare)
-
EURODELTA-Trends, a multi-model experiment of air quality hindcast in Europe over 1990–2010
- 2017
-
Ingår i: Geoscientific Model Development. - : Copernicus GmbH. - 1991-959X .- 1991-9603. ; 10:9, s. 3255-3276
-
Tidskriftsartikel (refereegranskat)abstract
- The EURODELTA-Trends multi-model chemistry-transport experiment has been designed to facilitate a better understanding of the evolution of air pollution and its drivers for the period 1990–2010 in Europe. The main objective of the experiment is to assess the efficiency of air pollutant emissions mitigation measures in improving regional-scale air quality. The present paper formulates the main scientific questions and policy issues being addressed by the EURODELTA-Trends modelling experiment with an emphasis on how the design and technical features of the modelling experiment answer these questions. The experiment is designed in three tiers, with increasing degrees of computational demand in order to facilitate the participation of as many modelling teams as possible. The basic experiment consists of simulations for the years 1990, 2000, and 2010. Sensitivity analysis for the same three years using various combinations of (i) anthropogenic emissions, (ii) chemical boundary conditions, and (iii) meteorology complements it. The most demanding tier consists of two complete time series from 1990 to 2010, simulated using either time-varying emissions for corresponding years or constant emissions. Eight chemistry-transport models have contributed with calculation results to at least one experiment tier, and five models have – to date – completed the full set of simulations (and 21-year trend calculations have been performed by four models). The modelling results are publicly available for further use by the scientific community. The main expected outcomes are (i) an evaluation of the models' performances for the three reference years, (ii) an evaluation of the skill of the models in capturing observed air pollution trends for the 1990–2010 time period, (iii) attribution analyses of the respective role of driving factors (e.g. emissions, boundary conditions, meteorology), (iv) a dataset based on a multi-model approach, to provide more robust model results for use in impact studies related to human health, ecosystem, and radiative forcing.
|
|
| 3. |
- Genberg, Johan, et al.
(författare)
-
Source apportionment of carbonaceous aerosol in southern Sweden
- 2011
-
Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11:22, s. 11387-11400
-
Tidskriftsartikel (refereegranskat)abstract
- A one-year study was performed at the Vavihill background station in southern Sweden to estimate the anthropogenic contribution to the carbonaceous aerosol. Weekly samples of the particulate matter PM10 were collected on quartz filters, and the amounts of organic carbon, elemental carbon, radiocarbon (14C) and levoglucosan were measured. This approach enabled source apportionment of the total carbon in the PM10 fraction using the concentration ratios of the sources. The sources considered in this study were emissions from the combustion of fossil fuels and biomass, as well as biogenic sources. During the summer, the carbonaceous aerosol mass was dominated by compounds of biogenic origin (80%), which are associated with biogenic primary and secondary organic aerosols. During the winter months, biomass combustion (32%) and fossil fuel combustion (28%) were the main contributors to the carbonaceous aerosol. Elemental carbon concentrations in winter were about twice as large as during summer, and can be attributed to biomass combustion, probably from domestic wood burning. The contribution of fossil fuels to elemental carbon was stable throughout the year, although the fossil contribution to organic carbon increased during the winter. Thus, the organic aerosol originated mainly from natural sources during the summer and from anthropogenic sources during the winter. The result of this source apportionment was compared with results from the EMEP MSC-W chemical transport model. The model and measurements were generally consistent for total atmospheric organic carbon, however, the contribution of the sources varied substantially. E.g. the biomass burning contributions of OC were underestimated by the model by a factor of 2.2 compared to the measurements.
|
|
| 4. |
- Jenkin, M. E., et al.
(författare)
-
The CRI v2.2 reduced degradation scheme for isoprene
- 2019
-
Ingår i: Atmospheric Environment. - : Elsevier BV. - 1873-2844 .- 1352-2310. ; 212:1 Sept., s. 172-182
-
Tidskriftsartikel (refereegranskat)abstract
- The reduced representation of isoprene degradation in the Common Representative Intermediates (CRI)mechanism has been systematically updated, using the Master Chemical Mechanism (MCM v3.3.1)as a reference benchmark, with the updated mechanism being released as CRI v2.2. The complete isoprene degradation mechanism in CRI v2.2 consists of 186 reactions of 56 closed shell and free radical species, this being an order of magnitude reduction in size compared with MCM v3.3.1. The chemistry initiated by reaction with OH radicals, NO3 radicals and ozone (O3)is treated. An overview of the updates is provided, within the context of reported kinetic and mechanistic information. The revisions mainly relate to the OH-initiated chemistry, which tends to dominate under atmospheric conditions, although these include updates to the chemistry of products that are also generated from the O3- and NO3-initiated oxidation. The revisions have impacts in a number of key areas, including recycling of HOx and NOx. The performance of the CRI v2.2 isoprene mechanism has been compared with those of the preceding version (CRI v2.1)and the reference MCM v3.3.1 over a range of relevant conditions, using a box model of the tropical forested boundary layer. In addition, tests are carried out to ensure that the performance of MCM v3.3.1 remains robust to more recently reported information. CRI v2.2 has also been implemented into the STOCHEM chemistry-transport model, with a customized close-variant of CRI v2.2 implemented into the EMEP MSC-W chemistry-transport model. The results of these studies are presented and used to illustrate the global-scale impacts of the mechanistic updates on HOx radical concentrations.
|
|
| 5. |
- Langner, J., et al.
(författare)
-
Model-simulated source contributions to PM2.5 in Santiago and the central region of Chile
- 2020
-
Ingår i: Aerosol and Air Quality Research. - : Taiwan Association for Aerosol Research. - 2071-1409 .- 1680-8584. ; 20:5, s. 1111-1126
-
Tidskriftsartikel (refereegranskat)abstract
- The contributions to PM2.5 from different emission sectors across central Chile and the Santiago metropolitan area during summer/fall and winter have been evaluated using a chemical transport model. The simulations generally underestimate the mean PM2.5 concentrations compared to measurements conducted at stations in Santiago that belong to the Chilean National Air Quality Information System (SINCA). The potential reasons for this discrepancy include underestimated direct PM2.5 emissions, missing emissions for semi-and intermediately volatile organic compounds (SVOCs and IVOCs) and overestimated wind speeds in the simulations. The simulated winter PM2.5 concentrations in Santiago are lower and higher than the values observed during nighttime, and daytime and late evening, respectively, which may be related to excessive simulated wind speeds, as well as to uncertainties in the diurnal variation in the emissions. During summer/fall, the simulated diurnal variation better agrees with the observations, but the peak concentrations during the morning are underestimated, whereas those during the evening are overestimated. The simulated contributions of different aerosol components to the PM2.5 at one station in Santiago are all lower than the observed values, except for elemental carbon equivalent black carbon (BCe), which exhibit comparable or higher levels in the simulations. The absolute differences are the largest for the total organic matter, whereas the relative differences are the largest for BCe and ammonium. The simulated sector contributions indicate that emissions originating from transport and construction machinery dominate the PM2.5 in Santiago; however, residential wood combustion is the primary source in other urban areas of central Chile, except near major point sources. Away from urban areas, traffic routes and major industrial sources, secondary inorganic aerosol (SIA) is estimated to be the largest component of the aerosol, whereas the simulated secondary organic aerosol (SOA) only contributes a small fraction.
|
|
| 6. |
- McFiggans, Gordon, et al.
(författare)
-
Secondary organic aerosol reduced by mixture of atmospheric vapours
- 2019
-
Ingår i: Nature. - : Springer Science and Business Media LLC. - 0028-0836 .- 1476-4687. ; 565:7741, s. 587-593
-
Tidskriftsartikel (refereegranskat)abstract
- Secondary organic aerosol contributes to the atmospheric particle burden with implications for air quality and climate. Biogenic volatile organic compounds such as terpenoids emitted from plants are important secondary organic aerosol precursors with isoprene dominating the emissions of biogenic volatile organic compounds globally. However, the particle mass from isoprene oxidation is generally modest compared to that of other terpenoids. Here we show that isoprene, carbon monoxide and methane can each suppress the instantaneous mass and the overall mass yield derived from monoterpenes in mixtures of atmospheric vapours. We find that isoprene 'scavenges' hydroxyl radicals, preventing their reaction with monoterpenes, and the resulting isoprene peroxy radicals scavenge highly oxygenated monoterpene products. These effects reduce the yield of low-volatility products that would otherwise form secondary organic aerosol. Global model calculations indicate that oxidant and product scavenging can operate effectively in the real atmosphere. Thus highly reactive compounds (such as isoprene) that produce a modest amount of aerosol are not necessarily net producers of secondary organic particle mass and their oxidation in mixtures of atmospheric vapours can suppress both particle number and mass of secondary organic aerosol. We suggest that formation mechanisms of secondary organic aerosol in the atmosphere need to be considered more realistically, accounting for mechanistic interactions between the products of oxidizing precursor molecules (as is recognized to be necessary when modelling ozone production).
|
|
| 7. |
- Noda, Jun, 1969, et al.
(författare)
-
Aerosol from Biomass Combustion in Northern Europe: Influence of Meteorological Conditions and Air Mass History
- 2019
-
Ingår i: Atmosphere. - 2073-4433. ; 10:12
-
Tidskriftsartikel (refereegranskat)abstract
- Alkali-containing submicron particles were measured continuously during three months, including late winter and spring seasons in Gothenburg, Sweden. The overall aims were to characterize the ambient concentrations of combustion-related aerosol particles and to address the importance of local emissions and long-range transport for atmospheric concentrations in the urban background environment. K and Na concentrations in the particulate matter PM1 size range were measured by an Alkali aerosol mass spectrometer (Alkali-AMS) and a cluster analysis was conducted. Local meteorological conditions and trace gas and PM concentrations were also obtained for a nearby location. In addition, back trajectory analyses and chemical transport model (CTM) simulations were included for the evaluation. The Alkali-AMS cluster analysis indicated three major clusters: (1) biomass burning origin, (2) mixture of other combustion sources, and (3) marine origin. Low temperatures and low wind speed conditions correlated with high concentrations of K-containing particles, mainly owing to local and regional emissions from residential biomass combustion; transport of air masses from continental Europe also contribute to Cluster 1. The CTM results indicate that open biomass burning in the eastern parts of Europe may have contributed substantially to high PM2.5 concentrations (and to Cluster 1) during an episode in late March. According to the CTM results, the mixed cluster (2) is likely to include particles emitted from different source types and no single geographical source region seems to dominate for this cluster. The back trajectory analysis and meteorological conditions indicated that the marine origin cluster was correlated with westerly winds and high wind speed; this cluster had high concentrations of Na-containing particles, as expected for sea salt particles.
|
|
| 8. |
- Otero, Noelia, et al.
(författare)
-
A multi-model comparison of meteorological drivers of surface ozone over Europe
- 2018
-
Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 18:16, s. 12269-12288
-
Tidskriftsartikel (refereegranskat)abstract
- The implementation of European emission abatement strategies has led to a significant reduction in the emissions of ozone precursors during the last decade. Ground-level ozone is also influenced by meteorological factors such as temperature, which exhibit interannual variability and are expected to change in the future. The impacts of climate change on air quality are usually investigated through air-quality models that simulate interactions between emissions, meteorology and chemistry. Within a multi-model assessment, this study aims to better understand how air-quality models represent the relationship between meteorological variables and surface ozone concentrations over Europe. A multiple linear regression (MLR) approach is applied to observed and modelled time series across 10 European regions in springtime and summertime for the period of 2000-2010 for both models and observations. Overall, the air-quality models are in better agreement with observations in summertime than in springtime and particularly in certain regions, such as France, central Europe or eastern Europe, where local meteorological variables show a strong influence on surface ozone concentrations. Larger discrepancies are found for the southern regions, such as the Balkans, the Iberian Peninsula and the Mediterranean basin, especially in springtime. We show that the air-quality models do not properly reproduce the sensitivity of surface ozone to some of the main meteorological drivers, such as maximum temperature, relative humidity and surface solar radiation. Specifically, all air-quality models show more limitations in capturing the strength of the ozone-relative-humidity relationship detected in the observed time series in most of the regions, for both seasons. Here, we speculate that dry-deposition schemes in the air-quality models might play an essential role in capturing this relationship. We further quantify the relationship between ozone and maximum temperature (m(o3-T), climate penalty) in observations and air-quality models. In summertime, most of the air-quality models are able to reproduce the observed climate penalty reasonably well in certain regions such as France, central Europe and northern Italy. However, larger discrepancies are found in springtime, where air-quality models tend to overestimate the magnitude of the observed climate penalty.
|
|
| 9. |
- Simpson, David, 1961, et al.
(författare)
-
GenChem v1.0-a chemical pre-processing and testing system for atmospheric modelling
- 2020
-
Ingår i: Geoscientific Model Development. - : Copernicus GmbH. - 1991-959X .- 1991-9603. ; 13:12, s. 6447-6465
-
Tidskriftsartikel (refereegranskat)abstract
- This paper outlines the structure and usage of the GenChem system, which includes a chemical preprocessor GenChem.py) and a simple box model (box-Chem). GenChem provides scripts and input files for converting chemical equations into differential form for use in atmospheric chemical transport models (CTMs) and/or the boxChem system. Although GenChem is primarily intended for users of the Meteorological Synthesizing Centre - West of the European Monitoring and Evaluation Programme (EMEP MSC-W) CTM and related systems, boxChem can be run as a stand-alone chemical solver, enabling for example easy testing of chemical mechanisms against each other. This paper presents an outline of the usage of the GenChem system, explaining input and output files, and presents some examples of usage. The code needed to run GenChem is released as opensource code under the GNU license.
|
|
| 10. |
- Theobald, M. R., et al.
(författare)
-
An evaluation of European nitrogen and sulfur wet deposition and their trends estimated by six chemistry transport models for the period 1990–2010
- 2019
-
Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 19:1, s. 379-405
-
Tidskriftsartikel (refereegranskat)abstract
- The wet deposition of nitrogen and sulfur in Europe for the period 1990–2010 was estimated by six atmospheric chemistry transport models (CHIMERE, CMAQ, EMEP MSC-W, LOTOS-EUROS, MATCH and MINNI) within the framework of the EURODELTA-Trends model intercomparison. The simulated wet deposition and its trends for two 11-year periods (1990–2000 and 2000–2010) were evaluated using data from observations from the EMEP European monitoring network. For annual wet deposition of oxidised nitrogen (WNOx), model bias was within 30 % of the average of the observations for most models. There was a tendency for most models to underestimate annual wet deposition of reduced nitrogen (WNHx), although the model bias was within 40 % of the average of the observations. Model bias for WNHx was inversely correlated with model bias for atmospheric concentrations of NH3 + NH4+, suggesting that an underestimation of wet deposition partially contributed to an overestimation of atmospheric concentrations. Model bias was also within about 40 % of the average of the observations for the annual wet deposition of sulfur (WSOx) for most models. Decreasing trends in WNOx were observed at most sites for both 11-year periods, with larger trends, on average, for the second period. The models also estimated predominantly decreasing trends at the monitoring sites and all but one of the models estimated larger trends, on average, for the second period. Decreasing trends were also observed at most sites for WNHx, although larger trends, on average, were observed for the first period. This pattern was not reproduced by the models, which estimated smaller decreasing trends, on average, than those observed or even small increasing trends. The largest observed trends were for WSOx, with decreasing trends at more than 80 % of the sites. On average, the observed trends were larger for the first period. All models were able to reproduce this pattern, although some models underestimated the trends (by up to a factor of 4) and others overestimated them (by up to 40 %), on average. These biases in modelled trends were directly related to the tendency of the models to under- or overestimate annual wet deposition and were smaller for the relative trends (expressed as % yr−1 relative to the deposition at the start of the period). The fact that model biases were fairly constant throughout the time series makes it possible to improve the predictions of wet deposition for future scenarios by adjusting the model estimates using a bias correction calculated from past observations. An analysis of the contributions of various factors to the modelled trends suggests that the predominantly decreasing trends in wet deposition are mostly due to reductions in emissions of the precursors NOx, NH3 and SOx. However, changes in meteorology (e.g. precipitation) and other (non-linear) interactions partially offset the decreasing trends due to emission reductions during the first period but not the second. This suggests that the emission reduction measures had a relatively larger effect on wet deposition during the second period, at least for the sites with observations.
|
|
| 11. |
- Yttri, Karl Espen, et al.
(författare)
-
The EMEP Intensive Measurement Period campaign, 2008-2009: characterizing carbonaceous aerosol at nine rural sites in Europe
- 2019
-
Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 19:7, s. 4211-4233
-
Tidskriftsartikel (refereegranskat)abstract
- Carbonaceous aerosol (total carbon, TCp) was source apportioned at nine European rural background sites, as part of the European Measurement and Evaluation Programme (EMEP) Intensive Measurement Periods in fall 2008 and winter/spring 2009. Five predefined fractions were apportioned based on ambient measurements: elemental and organic carbon, from combustion of biomass (ECbb and OCbb) and from fossil-fuel (ECff and OCff) sources, and remaining non-fossil organic carbon (OCrnf), dominated by natural sources. OCrnf made a larger contribution to TCp than anthropogenic sources (ECbb, OCbb, ECff, and OCff) at four out of nine sites in fall, reflecting the vegetative season, whereas anthropogenic sources dominated at all but one site in winter/spring. Biomass burning (OCbb + ECbb) was the major anthropogenic source at the central European sites in fall, whereas fossil-fuel (OCff + ECff) sources dominated at the southernmost and the two northernmost sites. Residential wood burning emissions explained 30 %-50 % of TCp at most sites in the first week of sampling in fall, showing that this source can be the dominant one, even outside the heating season. In winter/spring, biomass burning was the major anthropogenic source at all but two sites, reflecting increased residential wood burning emissions in the heating season. Fossil-fuel sources dominated EC at all sites in fall, whereas there was a shift towards biomass burning for the southernmost sites in winter/spring. Model calculations based on base-case emissions (mainly officially reported national emissions) strongly underpredicted observational derived levels of OCbb and ECbb outside Scandinavia. Emissions based on a consistent bottom-up inventory for residential wood burning (and including intermediate volatility compounds, IVOCs) improved model results compared to the base-case emissions, but modeled levels were still substantially underestimated compared to observational derived OCbb and ECbb levels at the southernmost sites. Our study shows that natural sources are a major contributor to carbonaceous aerosol in Europe, even in fall and in winter/spring, and that residential wood burning emissions are equally as large as or larger than that of fossil-fuel sources, depending on season and region. The poorly constrained residential wood burning emissions for large parts of Europe show the obvious need to improve emission inventories, with harmonization of emission factors between countries likely being the most important step to improve model calculations for biomass burning emissions, and European PM2.5 concentrations in general.
|
|
