Strong increase in mortality attributable to ozone pollution under a climate change and demographic scenario
Tropopause folds are the key process underlying stratosphere-to-troposphere transport (STT) of ozone, and thus they affect tropospheric ozone levels and variability. In the present study we perform a process-oriented evaluation of Copernicus Atmosphere Monitoring Service (CAMS) reanalysis (CAMSRA) O3 during folding events over Europe and for the time period from 2003 to 2018. A 3-D labeling algorithm is applied to detect tropopause folds in CAMSRA, while ozonesonde data from WOUDC (World Ozone and Ultraviolet Radiation Data Centre) and aircraft measurements from IAGOS (In-service Aircraft for a Global Observing System) are used for CAMSRA O3 evaluation. The profiles of observed and CAMSRA O3 concentrations indicate that CAMSRA reproduces the observed O3 increases in the troposphere during the examined folding events. Nevertheless, at most of the examined sites, CAMSRA overestimates the observed O3 concentrations, mostly at the upper portion of the observed increases, with a median fractional gross error (FGE) among the examined sites >0.2 above 400 hPa. The use of a control run without data assimilation reveals that the aforementioned overestimation of CAMSRA O3 arises from the data assimilation implementation. Overall, although data assimilation assists CAMSRA O3 to follow the observed O3 enhancements in the troposphere during the STT events, it introduces biases in the upper troposphere resulting in no clear quantitative improvement compared to the control run without data assimilation. Less biased assimilated O3 products, with finer vertical resolution in the troposphere, in addition to higher IFS (Integrated Forecasting System) vertical resolution, are expected to provide a better representation of O3 variability during tropopause folds.
A process-oriented evaluation of CAMS reanalysis ozone during tropopause folds over Europe for the period 2003-2018
Tropopause folds are the key process underlying stratosphere-to-troposphere transport (STT) of ozone, and thus they affect tropospheric ozone levels and variability. In the present study we perform a process-oriented evaluation of Copernicus Atmosphere Monitoring Service (CAMS) reanalysis (CAMSRA) O3 during folding events over Europe and for the time period from 2003 to 2018. A 3-D labeling algorithm is applied to detect tropopause folds in CAMSRA, while ozonesonde data from WOUDC (World Ozone and Ultraviolet Radiation Data Centre) and aircraft measurements from IAGOS (In-service Aircraft for a Global Observing System) are used for CAMSRA O3 evaluation. The profiles of observed and CAMSRA O3 concentrations indicate that CAMSRA reproduces the observed O3 increases in the troposphere during the examined folding events. Nevertheless, at most of the examined sites, CAMSRA overestimates the observed O3 concentrations, mostly at the upper portion of the observed increases, with a median fractional gross error (FGE) among the examined sites >0.2 above 400 hPa. The use of a control run without data assimilation reveals that the aforementioned overestimation of CAMSRA O3 arises from the data assimilation implementation. Overall, although data assimilation assists CAMSRA O3 to follow the observed O3 enhancements in the troposphere during the STT events, it introduces biases in the upper troposphere resulting in no clear quantitative improvement compared to the control run without data assimilation. Less biased assimilated O3 products, with finer vertical resolution in the troposphere, in addition to higher IFS (Integrated Forecasting System) vertical resolution, are expected to provide a better representation of O3 variability during tropopause folds.
Implications of COVID-19 Restriction Measures in Urban Air Quality of Thessaloniki, Greece: A Machine Learning Approach
Following the rapid spread of COVID-19, a lockdown was imposed in Thessaloniki, Greece, resulting in an abrupt reduction of human activities. To unravel the impact of restrictions on the urban air quality of Thessaloniki, NO2 and O3 observations are compared against the business-as-usual (BAU) concentrations for the lockdown period. BAU conditions are modeled, applying the XGBoost (eXtreme Gradient Boosting) machine learning algorithm on air quality and meteorological surface measurements, and reanalysis data. A reduction in NO2 concentrations is found during the lockdown period due to the restriction policies at both AGSOFIA and EGNATIA stations of −24.9 [−26.6, −23.2]% and −18.4 [−19.6, −17.1]%, respectively. A reverse effect is revealed for O3 concentrations at AGSOFIA with an increase of 12.7 [10.8, 14.8]%, reflecting the reduced O3 titration by NOx. The implications of COVID-19 lockdowns in the urban air quality of Thessaloniki are in line with the results of several recent studies for other urban areas around the world, highlighting the necessity of more sophisticated emission control strategies for urban air quality management.
A global climatology of tropopause folds in CAMS and MERRA-2 Reanalyses
Tropopause folds are the main mechanism underlying stratosphere-to-troposphere transport and influence tropospheric composition and weather systems by triggering convection. Here, we present the global climatology of tropopause folds in Copernicus Atmosphere Monitoring Service (CAMS) and Modern-Era Retrospective analysis for Research and Applications, version 2 (MERRA-2) reanalysis of atmospheric composition products for the time period from 2003 to 2018. We applied a 3-D labeling algorithm in CAMS and MERRA-2 reanalysis data to detect tropopause folding events. In constructing their climatologies, we show that the bulk of the folds are vertically shallow and are mainly found at the subtropical zones in the vicinity of the jet streams, while deeper folds also occur over the storm tracks, consistent with previous studies. The spatiotemporal characteristics of fold climatology are captured in a similar manner in CAMS and MERRA-2, with MERRA-2 capturing slightly higher frequencies during all seasons. In quantitative terms, there is a good agreement between CAMS and MERRA-2 fold frequencies with spatiotemporal R2 values of ∼0.9 for DJF, MAM, and JJA, and 0.75 for SON. The two reanalysis products are in close agreement regarding the intra- and interannual variability in fold frequency, with temporal correlation scores higher than 0.7 over the subtropical bands where the majority of folds are found. The agreement between the two reanalyses is lower in the Southern Hemisphere compared to the Northern Hemisphere. Thus, the global climatology of tropopause folds in both CAMS and MERRA-2 reanalyses are similar to those of previous studies.
A complex aerosol transport event over Europe during the 2017 Storm Ophelia in CAMS forecast systems: analysis and evaluation
animation_Ophelia.mp4In mid-October 2017 Storm Ophelia crossed over western coastal Europe, inducing the combined transport of Saharan dust and Iberian biomass burning aerosols over several European areas. In this study we assess the performance of the Copernicus Atmosphere Monitoring Service (CAMS) forecast systems during this complex aerosol transport event and the potential benefits that data assimilation and regional models could bring. To this end, CAMS global and regional forecast data are analysed and compared against observations from passive (MODIS: Moderate Resolution Imaging Spectroradiometer aboard Terra and Aqua) and active (CALIOP/CALIPSO: Cloud-Aerosol LIdar with Orthogonal Polarization aboard Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations) satellite sensors and ground-based measurements (EMEP: European Monitoring and Evaluation Programme). The analysis of the CAMS global forecast indicates that dust and smoke aerosols, discretely located on the warm and cold fronts of Ophelia, respectively, were affecting the aerosol atmospheric composition over Europe during the passage of the Storm. The observed MODIS aerosol optical depth (AOD) values are satisfactorily reproduced by the CAMS global forecast system, with a correlation coefficient of 0.77 and a fractional gross error (FGE) of 0.4. The comparison with a CAMS global control simulation not including data assimilation indicates a significant improvement in the bias due to data assimilation implementation, as the FGE decreases by 32 %. The qualitative evaluation of the IFS (Integrated Forecast System) dominant-aerosol type and location against the CALIPSO observations overall reveals a good agreement. Regarding the footprint on air quality, both CAMS global and regional forecast systems are generally able to reproduce the observed signal of increase in surface particulate matter concentrations. The regional component performs better in terms of bias and temporal variability, with the correlation deteriorating over forecast time. Yet, both products exhibit inconsistencies on the quantitative and temporal representation of the observed surface particulate matter enhancements, stressing the need for further development of the air quality forecast systems for even more accurate and timely support of citizens and policy-makers.
On the impact of future climate change on tropopause folds and tropospheric ozone
Using a transient simulation for the period 1960–2100 with the state-of-the-art ECHAM5/MESSy Atmospheric Chemistry (EMAC) global model and a tropopause fold identification algorithm, we explore the future projected changes in tropopause folds, stratosphere-to-troposphere transport (STT) of ozone, and tropospheric ozone under the RCP6.0 scenario. Statistically significant changes in tropopause fold frequencies from 1970–1999 to 2070–2099 are identified in both hemispheres, regionally exceeding 3 %, and are associated with the projected changes in the position and intensity of the subtropical jet streams. A strengthening of ozone STT is projected for the future in both hemispheres, with an induced increase in transported stratospheric ozone tracer throughout the whole troposphere, reaching up to 10 nmol mol−1 in the upper troposphere, 8 nmol mol−1 in the middle troposphere, and 3 nmol mol−1 near the surface. Notably, the regions exhibiting the largest changes of ozone STT at 400 hPa coincide with those with the highest fold frequency changes, highlighting the role of the tropopause folding mechanism in STT processes under a changing climate. For both the eastern Mediterranean and Middle East (EMME) and Afghanistan (AFG) regions, which are known as hotspots of fold activity and ozone STT during the summer period, the year-to-year variability of middle-tropospheric ozone with stratospheric origin is largely explained by the short-term variations in ozone at 150 hPa and tropopause fold frequency. Finally, ozone in the lower troposphere is projected to decrease under the RCP6.0 scenario during MAM (March, April, and May) and JJA (June, July, and August) in the Northern Hemisphere and during DJF (December, January, and February) in the Southern Hemisphere, due to the decline of ozone precursor emissions and the enhanced ozone loss from higher water vapour abundances, while in the rest of the troposphere ozone shows a remarkable increase owing mainly to the STT strengthening and the stratospheric ozone recovery.
A deep stratosphere-to-troposphere ozone transport event over Europe simulated in CAMS global and regional forecast systems: analysis and evaluation
Stratosphere-to-troposphere transport (STT) is an important natural source of tropospheric ozone, which can occasionally influence ground-level ozone concentrations relevant for air quality. Here, we analyse and evaluate the Copernicus Atmosphere Monitoring Service (CAMS) global and regional forecast systems during a deep STT event over Europe for the time period from 4 to 9 January 2017. The predominant synoptic condition is described by a deep upper level trough over eastern and central Europe, favouring the formation of tropopause folding events along the jet stream axis and therefore the intrusion of stratospheric ozone into the troposphere. Both global and regional CAMS forecast products reproduce the “hook-shaped” streamer of ozone-rich and dry air in the middle troposphere depicted from the observed satellite images of water vapour. The CAMS global model successfully reproduces the folding of the tropopause at various European sites, such as Trapani (Italy), where a deep folding down to 550 hPa is seen. The stratospheric ozone intrusions into the troposphere observed by WOUDC ozonesonde and IAGOS aircraft measurements are satisfactorily forecasted up to 3 days in advance by the CAMS global model in terms of both temporal and vertical features of ozone. The fractional gross error (FGE) of CAMS ozone day 1 forecast between 300 and 500 hPa is 0.13 over Prague, while over Frankfurt it is 0.04 and 0.19, highlighting the contribution of data assimilation, which in most cases improves the model performance. Finally, the meteorological and chemical forcing of CAMS global forecast system in the CAMS regional forecast systems is found to be beneficial for predicting the enhanced ozone concentrations in the middle troposphere during a deep STT event.
On the role of tropopause folds in summertime tropospheric ozone over sthe eastern Mediterranean and the Middle East
We study the contribution of tropopause folds in the summertime pool of tropospheric ozone over the eastern Mediterranean and the Middle East (EMME) with the aid of the ECHAM5/MESSy Atmospheric Chemistry (EMAC) model. Tropopause fold events in EMAC simulations were identified with a 3-D labeling algorithm that detects folds at grid points where multiple crossings of the dynamical tropopause are computed. Subsequently the events featuring the largest horizontal and vertical extent were selected for further study. For the selection of these events we identified a significant contribution of the stratospheric ozone reservoir to the high concentrations of ozone in the middle and lower free troposphere over the EMME. A distinct increase of ozone is found over the EMME in the middle troposphere during summer as a result of the fold activity, shifting towards the southeast and decreasing altitude. We find that the interannual variability of near-surface ozone over the eastern Mediterranean (EM) during summer is related to that of both tropopause folds and ozone in the free troposphere.
Near-surface ozone trends over Europe in RegCM3/CAMx simulations for the time period 1996-2006
The RegCM3/CAMx modeling system is applied to estimate near surface ozone trends over Europe for the time period 1996–2006. In order to assess the impact of changing anthropogenic emissions and meteorology on modeled ozone trends two simulations were performed: The first simulation (CONEM) was forced from constant anthropogenic emissions based on the EMEP emissions of the year 1996, while the second simulation (VAREM) was forced from year to year varying anthropogenic emissions based on the EMEP emissions of the years 1996–2006.
Near surface ozone measurements from the EMEP database are used for assessing the skill of the modeling system to reproduce the observed ozone trends. Concerning VAREM simulation the main pattern is a significant positive annual trend over southern UK and Benelux which is also detected in the observations, attributed to the reduction of ozone titration by NO as a result of NOx emissions control policies. Significant negative ozone trends are found over the Mediterranean due to reduction of ozone precursors emissions over continental Europe. As far as it concerns CONEM simulation a significant increase of ozone is found during summer associated with the heatwave event of 2003. Overall, the observed ozone trends are captured fairly well by the RegCM3/CAMx modeling system over the highly polluted areas of central and western Europe but only partially reproduced or not captured at all at the rest of Europe, probably due to limitations of the model setup to capture background ozone variability related to processes such as intercontinental transport and stratosphere–troposphere exchange.
Evaluating the impact of chemical boundary conditions on near surface ozone in regional climate-air quality simulations over Europe
A modeling system based on the air quality model CAMx driven off-line by the regional climate model RegCM3 is used for assessing the impact of chemical lateral boundary conditions (LBCs) on near surface ozone over Europe for the period 1996–2000. The RegCM3 and CAMx simulations were performed on a 50 km × 50 km grid over Europe with RegCM3 driven by the NCEP meteorological reanalysis fields and CAMx with chemical LBCs from ECHAM5/MOZART global model. The recent past period (1996–2000) was simulated in three experiments. The first simulation was forced using time and space invariant LBCs, the second was based on ECHAM5/MOZART chemical LBCs fixed for the year 1996 and the third was based on ECHAM5/MOZART chemical LBCs with interannual variability. Anthropogenic and biogenic emissions were kept identical for the three sensitivity runs.
In order to evaluate the ability of the RegCM3/CAMx modeling system and assess the impact of varying chemical LBCs, simulated surface ozone concentrations are compared against measurements from the EMEP network using various statistical metrics. The evaluation indicates that implementation of time and space variant chemical LBCs of a global chemistry transport model (CTM) improves the RegCM/CAMx performance with respect to seasonal variability, especially at stations close to the borders of the model domain over north and northwestern Europe. The modeling system reproduces the seasonal variability of ozone when LBCs from ECHAM5/MOZART model are applied for the vast majority of stations. On a seasonal basis, the varying chemical LBCs resulted in improvement of both model bias and variance of simulated versus observed ozone for all seasons. Finally taking into account all the statistical measures assessed for the comparison of RegCM3/CAMx and ECHAM5/MOZART with observed ozone, a slight improvement for the regional air quality model is indicated but this finding should be perceived with caution as the regional scale simulation and the global scale simulation have a different meteorological forcing.
A deep stratospheric intrusion event down to the earth's surface of the megacity of Athens
flexpart.aviThis case study investigates a stratospheric intrusion event down to the earth’s surface (near sea-level pressure) of the greater area of Athens (23.43°E 37.58°N), which occurred on 9 October 2003 and caused a remarkable increase in surface ozone concentrations not related to photochemical production. This event is among the rare case studies investigating, on the one hand, a deep stratospheric intrusion down to the earth’s surface at near sea-level pressure and, on the other, an event affecting the near surface ozone of a megacity such as Athens. The synoptic situation is described by a deep upper lever trough at 300 and 500 hPa extending over Greece, which is related to a deep tropopause fold as revealed by vertical cross sections of potential vorticity, relative humidity, divergence and vertical velocity. The analysis of potential vorticity at several isentropic levels indicates a hook-shaped streamer of high PV values (greater than 4 pvu at the 315 K isentropic level) over southeast Europe, which coincides with a streamer of dry air as observed from satellite images of water vapor. The aforementioned structure characterizes a textbook case study of stratosphere-to-troposphere transport. The Lagrangian particle dispersion model FLEXPART was used to calculate the trajectories of air particles reaching the receptor site and the fraction of particles with stratospheric origin. It reveals an important direct stratospheric impact within 1 day related to the tropopause fold described in this study with the fraction of stratospheric particles reaching maximum values of 1.9 and 4.5% for threshold values of the dynamical tropopause 2 and 1.5 pvu, respectively. Furthermore, a larger indirect aged stratospheric contribution is also revealed 4 to 5 days prior to the release, related to stratospheric intrusion events at the western Atlantic Ocean, reaching maximum values of 2.5 and 6.9% of particles crossing the 2 and 1.5 pvu potential vorticity surfaces, respectively.