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It is important to understand how future environmental policies will impact both climate change and air pollution. Although targeting near-term climate forcers (NTCFs), defined here as aerosols, tropospheric ozone, and precursor gases, should improve air quality, NTCF reductions will also impact climate. Prior assessments of the impact of NTCF mitigation on air quality and climate have been limited. This is related to the idealized nature of some prior studies, simplified treatment of aerosols and chemically reactive gases, as well as a lack of a sufficiently large number of models to quantify model diversity and robust responses. Here, we quantify the 2015–2055 climate and air quality effects of non-methane NTCFs using nine state-of-the-art chemistry–climate model simulations conducted for the Aerosol and Chemistry Model Intercomparison Project (AerChemMIP). Simulations are driven by two future scenarios featuring similar increases in greenhouse gases (GHGs) but with “weak” (SSP3-7.0) versus “strong” (SSP3-7.0-lowNTCF) levels of air quality control measures. As SSP3-7.0 lacks climate policy and has the highest levels of NTCFs, our results (e.g., surface warming) represent an upper bound. Unsurprisingly, we find significant improvements in air quality under NTCF mitigation (strong versus weak air quality controls). Surface fine particulate matter (PM2.5) and ozone (O3) decrease by -2.2±0.32 µg m−3 and -4.6±0.88 ppb, respectively (changes quoted here are for the entire 2015–2055 time period; uncertainty represents the 95 % confidence interval), over global land surfaces, with larger reductions in some regions including south and southeast Asia. Non-methane NTCF mitigation, however, leads to additional climate change due to the removal of aerosol which causes a net warming effect, including global mean surface temperature and precipitation increases of 0.25±0.12 K and 0.03±0.012 mm d−1, respectively. Similarly, increases in extreme weather indices, including the hottest and wettest days, also occur. Regionally, the largest warming and wetting occurs over Asia, including central and north Asia (0.66±0.20 K and 0.03±0.02 mm d−1), south Asia (0.47±0.16 K and 0.17±0.09 mm d−1), and east Asia (0.46±0.20 K and 0.15±0.06 mm d−1). Relatively large warming and wetting of the Arctic also occur at 0.59±0.36 K and 0.04±0.02 mm d−1, respectively. Similar surface warming occurs in model simulations with aerosol-only mitigation, implying weak cooling due to ozone reductions. Our findings suggest that future policies that aggressively target non-methane NTCF reductions will improve air quality but will lead to additional surface warming, particularly in Asia and the Arctic. Policies that address other NTCFs including methane, as well as carbon dioxide emissions, must also be adopted to meet climate mitigation goals.

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.

We investigate the sensitivity of aerosol representation in the regional climate model RegCM4 for two dust parameterizations for the period 2007–2014 over the Sahara and the Mediterranean. We apply two discretization methods of the dust size distribution keeping the total mass constant: (1) the default RegCM4 4-bin approach, where the size range of each bin is calculated using an equal, logarithmic separation of the total size range of dust, using the diameter of dust particles, and (2) a newly implemented 12-bin approach with each bin defined according to an isogradient method where the size ranges are dependent on the dry deposition velocity of dust particles. Increasing the number of transported dust size bins theoretically improves the representation of the physical properties of dust particles within the same size bin. Thus, more size bins improve the simulation of atmospheric processes. The radiative effects of dust over the area are discussed and evaluated with the CALIPSO dust optical depth (DOD). This study is among the first studies evaluating the vertical profile of simulated dust with a pure dust product. Reanalysis winds from ERA-Interim and the total precipitation flux from the Climate Research Unit (CRU) observational gridded database are used to evaluate and explain the discrepancies between model and observations. The new dust binning approach increases the dust column burden by 4 and 3 % for fine and coarse particles, respectively, which increases DOD by 10 % over the desert and the Mediterranean. Consequently, negative shortwave radiative forcing (RF) is enhanced by more than 10 % at the top of the atmosphere and by 1 to 5 % on the surface. Positive longwave RF locally increases by more than 0.1 W m−2 in a large portion of the Sahara, the northern part of the Arabian Peninsula and the Middle East. The four-bin isolog method is to some extent numerically efficient, nevertheless our work highlights that the simplified representation of the four-bin approach produces less dust optical depth and RF, a fact that should be taken into account by future studies of the same region.

This study characterizes the spatiotemporal variability and relative contribution of different types of aerosols to the Aerosol Optical Depth (AOD) over the Eastern Mediterranean as derived from MODIS Terra (3/2000–12/2012) and Aqua (7/2002–12/2012) satellite instruments. For this purpose, a 0.1°×0.1° gridded MODIS dataset was compiled and validated against AERONET sunphotometric observations. The high spatial resolution and long temporal coverage of the dataset allows for the determination of local hot spots like megacities, medium sized cities, industrial zones, and power plant complexes, seasonal variabilities, and decadal averages. The average AOD at 550 nm (AOD550) for the entire region is ~ 0.22 ± 0.19 with maximum values in summer and seasonal variabilities that can be attributed to precipitation, photochemical production of secondary organic aerosols, transport of pollution and smoke from biomass burning in Central and Eastern Europe, and transport of dust from the Sahara Desert and the Middle East. The MODIS data were analyzed together with data from other satellite sensors, reanalysis projects and a chemistry-aerosol-transport model using an optimized algorithm tailored for the region and capable of estimating the contribution of different aerosol types to the total AOD550. The spatial and temporal variability of anthropogenic, dust and fine mode natural aerosols over land and anthropogenic, dust and marine aerosols over the sea is examined. The relative contribution of the different aerosol types to the total AOD550 exhibits a low/high seasonal variability over land/oceanic areas, respectively. Overall, anthropogenic aerosols, dust and fine mode natural aerosols account for ~ 51 %, ~ 34 % and ~ 15 % of the total AOD550 over land, while, anthropogenic aerosols, dust and marine aerosols account ~ 40 %, ~ 34 % and ~ 26 % of the total AOD550 over the sea, based on MODIS Terra and Aqua observations.

In this work, we assess the ability of RegCM4 regional climate model to simulate surface solar radiation (SSR) patterns over Europe. A decadal RegCM4 run (2000–2009) was implemented and evaluated against satellite-based observations from the Satellite Application Facility on Climate Monitoring (CM SAF), showing that the model simulates adequately the SSR patterns over the region. The SSR bias between RegCM4 and CM SAF is +1.5 % for MFG (Meteosat First Generation) and +3.3 % for MSG (Meteosat Second Generation) observations. The relative contribution of parameters that determine the transmission of solar radiation within the atmosphere to the deviation appearing between RegCM4 and CM SAF SSR is also examined. Cloud macrophysical and microphysical properties such as cloud fractional cover (CFC), cloud optical thickness (COT) and cloud effective radius (Re) from RegCM4 are evaluated against data from CM SAF. Generally, RegCM4 underestimates CFC by 24.3 % and Re for liquid/ice clouds by 36.1 %/28.3 % and overestimates COT by 4.3 %. The same procedure is repeated for aerosol optical properties such as aerosol optical depth (AOD), asymmetry factor (ASY) and single-scattering albedo (SSA), as well as other parameters, including surface broadband albedo (ALB) and water vapor amount (WV), using data from MACv1 aerosol climatology, from CERES satellite sensors and from ERA-Interim reanalysis. It is shown here that the good agreement between RegCM4 and satellite-based SSR observations can be partially attributed to counteracting effects among the above mentioned parameters. The potential contribution of each parameter to the RegCM4–CM SAF SSR deviations is estimated with the combined use of the aforementioned data and a radiative transfer model (SBDART). CFC, COT and AOD are the major determinants of these deviations on a monthly basis; however, the other parameters also play an important role for specific regions and seasons. Overall, for the European domain, CFC, COT and AOD are the most important factors, since their underestimations and overestimations by RegCM4 cause an annual RegCM4–CM SAF SSR absolute deviation of 8.4, 3.8 and 4.5 %, respectively.

This study provides a new look at the observed and calculated long-term temperature changes from the lower troposphere to the lower stratosphere since 1958 over the Northern Hemisphere. The data sets include the NCEP/NCAR reanalysis, the Free University of Berlin (FU-Berlin) and the RICH radiosonde data sets as well as historical simulations with the CESM1-WACCM global model participating in CMIP5. The analysis is mainly based on monthly layer mean temperatures derived from geopotential height thicknesses in order to take advantage of the use of the independent FU-Berlin stratospheric data set of geopotential height data since 1957. This approach was followed to extend the records for the investigation of the stratospheric temperature trends to the earliest possible time. After removing the natural variability with an autoregressive multiple regression model our analysis shows that the period 1958–2011 can be divided into two distinct sub-periods of long-term temperature variability and trends: before and after 1980. By calculating trends for the summer time to reduce interannual variability, the two periods are as follows. From 1958 until 1979, a non-significant trend (0.06 ± 0.06 °C decade−1 for NCEP) and slightly cooling trends (−0.12 ± 0.06 °C decade−1 for RICH) are found in the lower troposphere. The second period from 1980 to the end of the records shows significant warming (0.25 ± 0.05 °C decade−1 for both NCEP and RICH). Above the tropopause a significant cooling trend is clearly seen in the lower stratosphere both in the pre-1980 period (−0.58 ± 0.17 °C decade−1 for NCEP, −0.30 ± 0.16 °C decade−1 for RICH and −0.48 ± 0.20 °C decade−1 for FU-Berlin) and the post-1980 period (−0.79 ± 0.18 °C decade−1 for NCEP, −0.66 ± 0.16 °C decade−1 for RICH and −0.82 ± 0.19 °C decade−1 for FU-Berlin). The cooling in the lower stratosphere persists throughout the year from the tropics up to 60° N. At polar latitudes competing dynamical and radiative processes reduce the statistical significance of these trends. Model results are in line with reanalysis and the observations, indicating a persistent cooling (−0.33 °C decade−1) in the lower stratosphere during summer before and after 1980; a feature that is also seen throughout the year. However, the lower stratosphere CESM1-WACCM modelled trends are generally lower than reanalysis and the observations. The contrasting effects of ozone depletion at polar latitudes in winter/spring and the anticipated strengthening of the Brewer–Dobson circulation from man-made global warming at polar latitudes are discussed. Our results provide additional evidence for an early greenhouse cooling signal in the lower stratosphere before 1980, which appears well in advance relative to the tropospheric greenhouse warming signal. The suitability of early warning signals in the stratosphere relative to the troposphere is supported by the fact that the stratosphere is less sensitive to changes due to cloudiness, humidity and man-made aerosols. Our analysis also indicates that the relative contribution of the lower stratosphere versus the upper troposphere low-frequency variability is important for understanding the added value of the long-term tropopause variability related to human-induced global warming.

Observations show that the Mediterranean troposphere is characterized by a marked enhancement in summertime ozone, with a maximum over the eastern Mediterranean. This has been linked to enhanced photochemical ozone production and subsidence under cloud-free anticyclonic conditions. The eastern Mediterranean is among the regions with the highest levels of background tropospheric ozone worldwide. A 12 yr climatological analysis (1998–2009) of free-tropospheric ozone was carried out over the region based on the ECMWF (European Centre for Medium-Range Weather Forecasts) ERA-Interim reanalysis data and simulations with the EMAC (ECHAM5–MESSy) atmospheric chemistry–climate model. EMAC is nudged towards the ECMWF analysis data and includes a stratospheric ozone tracer. A characteristic summertime pool with high ozone concentrations is found in the middle troposphere over the eastern Mediterranean–Middle East (EMME) in the ERA-Interim ozone data, Tropospheric Emission Spectrometer (TES) satellite ozone data and simulations with EMAC. The enhanced ozone over the EMME during summer is a robust feature, extending down to lower free-tropospheric levels. The investigation of ozone in relation to potential vorticity and water vapour and the stratospheric ozone tracer indicates that the dominant mechanism causing the free-tropospheric ozone pool is the downward transport from the upper troposphere and lower stratosphere, in association with the enhanced subsidence and the limited horizontal divergence observed over the region. The implications of these high free-tropospheric ozone levels on the seasonal cycle of near-surface ozone over the Mediterranean are discussed.

High frequency of agricultural fires is observed every year during the summer months over SW Russia and Eastern Europe. This study investigates the initial injection height of aerosol generated by the fires over these regions during the biomass burning season, which determines the potential for long-range transport of the smoke. This information is critical for aerosol transport modeling, as it determines the smoke plume evolution. The study focuses on the period 2006–2008, and is based on observations made by the CALIOP instrument on board the NASA CALIPSO satellite. MODIS data are synergistically used for the detection of the fires and the characterization of their intensity. CALIPSO aerosol vertical distributions generated by the active fires are analyzed to investigate the aerosol top height which is considered dependent on the heat generated by the fires and can be associated with the initial injection height. Aerosol top heights of the vertically homogenous smoke layers are found to range between 1.6 and 5.9 km. Smoke injection heights from CALIPSO are compared with mixing layer heights taken by the European Centre for Medium-range Weather Forecast (ECMWF), to investigate the direct injection of smoke particles into the free troposphere. Our results indicate that the aerosol plumes are observed within the boundary layer for the 50% of the cases examined. For the rest of the cases, the strong updrafts generated by the fires resulted to smoke injection heights greater than the ECMWF estimated mixing layer by 0.5 to 3.0 km, indicating a direct smoke injection into the free troposphere. The smoke injection height showed a dependence on the MODIS-Land Fire Radiative Power product which is indicative of the fire intensity, especially in the cases of lower static stability in the upper part of the boundary layer and the free troposphere.

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.

This study investigates the effects of the total solar eclipse of 29 March 2006 on surface air-quality levels over Greece based on observations at a number of sites in conjunction with chemical box modelling and 3-D air-quality modelling. Emphasis is given on surface ozone and other photooxidants at four Greek sites Kastelorizo, Finokalia (Crete), Pallini (Athens) and Thessaloniki, which are located at gradually increasing distances from the path of the eclipse totality and are characterized by different air pollution levels. The eclipse offered the opportunity to test our understanding of air pollution build-up and the response of the gas-phase chemistry of photo-oxidants during a photolytical perturbation using both a photochemical box model and a regional air-quality offline model based on the modeling system WRF/CAMx. At the relatively unpolluted sites of Kastelorizo and Finokalia no clear signal of the solar eclipse on surface O 3 , NO 2 and NO concentrations can be deduced from the observations while there is no correlation of observed O 3 , NO 2 and NO with observed global radiation. The box and regional model simulations for the two relatively unpolluted sites indicate that the calculated changes in net ozone production rates between eclipse and non eclipse conditions are rather small compared to the observed short-term ozone variability. Furthermore the simulated ozone lifetime is in the range of a few days at these sites and hence the solar eclipse effects on ozone can be easily masked by local and regional transport. At the polluted sites of Thessaloniki and Pallini, the solar eclipse effects on O 3 , NO 2 and NO concentrations are revealed from both the measurements and modeling with the net effect being a decrease in O 3 and NO and an increase in NO 2 as NO 2 formed from the reaction of O 3 with NO while at the same time NO 2 is not efficiently photolysed. This result is also supported by a positive correlation of observed global radiation with O 3 and NO and a negative correlation with NO 2 . It is evident from the 3-D air quality modeling over Greece that the maximum effects of the eclipse on O 3 , NO 2 and NO are reflected on the large urban agglomerations of Athens, and Thessaloniki where the maximum of the emissions occur.

In this study we present the seasonal variability of ozone production efficiencies (EN), defined as the net number of ozone molecules produced per molecule of nitrogen oxides (nitrogen oxide (NO) + nitrogen dioxide (NO2)=NOx) oxidized to NOz (total reactive nitrogen (NOy)–NOx) determined from field measurements of a seven-year period (1998–2004) at the Swiss high-alpine research station Jungfraujoch (JFJ), 3580 m a.s.l. This dataset is a unique long-term data series of nitrogen levels in the free troposphere over Central Europe and hence it offers an excellent opportunity to perform such an analysis and provide further evidence to the photochemical origin of the ozone spring maximum at locations of the northern hemisphere distant from nearby pollution sources. Experimentally derived daily EN values have been selected for 571 days out of the 2557 days from 1998 to 2004, from which an average ozone production efficiency of 18.8±1.3 molecules of O3 produced per molecule of NOx oxidized was calculated. This value indicates the great potential and importance of photochemical ozone production in the free troposphere. The monthly means of experimentally derived daily EN values show a seasonal variation with lower values from May to August, which can be probably attributed to more efficient vertical transport of polluted air masses from the atmospheric boundary layer up to JFJ. In agreement, theoretically derived monthly EN values show similar seasonal variation. The ratio NOy/CO, a parameter to assess the aging process that has occurred in an air parcel, was used as a criterion to disaggregate the 571 selected days between undisturbed and disturbed free tropospheric (FT). The monthly means of experimentally derived EN values for the undisturbed FT conditions show a distinct seasonal cycle with higher values in the cold season from November to April. The EN values for undisturbed FT conditions are particularly higher than the respective monthly EN values for disturbed FT conditions from February to October. It should be noted that the monthly EN values of March (EN=35.8) and April (EN=34.9) are among the highest values throughout the year for undisturbed FT conditions at JFJ. These results highlight the key and possibly the dominant role for photochemistry in the observed build-up of tropospheric ozone in the winter-spring transition period.

This work examines changes in cirrus cloud cover (CCC) in possible association with aviation activities at congested air corridors. The analysis is based on the latest version of the International Satellite Cloud Climatology Project D2 data set and covers the period 1984-1998. Over the studied areas, the effect of large-scale modes of natural climate variability such as ENSO, QBO and NAO as well as the possible influence of the tropopause variability, were first removed from the cloud data set in order to calculate long-term changes of observed cirrus cloudiness. The results show increasing trends in (CCC) between 1984 and 1998 over the high air traffic corridors of North America, North Atlantic and Europe. Of these upward trends, only in the summertime over the North Atlantic and only in the wintertime over North America are statistically significant (exceeding +2.0% per decade). Over adjacent locations with low air traffic, the calculated trends are statistically insignificant and in most cases negative both during winter and summer in the regions studied. These negative trends, over low air traffic regions, are consistent with the observed large scale negative trends seen in (CCC) over most of the northern middle latitudes and over the tropics. Moreover, further investigation of vertical velocities over high and low air traffic regions provide evidence that the trends of opposite signs in (CCC) over these regions, do not seem to be caused by different trends in dynamics. It is also shown that the longitudinal distribution of decadal changes in (CCC) along the latitude belt centered at the North Atlantic air corridor, parallels the spatial distribution of fuel consumption from highflying air traffic, providing an independent test of possible impact of aviation on contrail cirrus formation. The correlation between the fuel consumption and the longitudinal variability of (CCC) is significant (+0.7) over the middle latitudes but not over the tropics. This could be explained by the fact that over the tropics the variability of (CCC) is dominated by dynamics while at middle latitudes microphysics explain most of its variability. Results from this study are compared with other studies and for different periods of records and it appears that there exists general agreement as to the evidence of a possible aviation effect on high cloud positive trends over regions with congested air traffic.

A wide range of measurements was carried out in central and southeastern Europe within the framework of the EU project STACCATO (Influence of Stratosphere-Troposphere Exchange in a Changing Climate on Atmospheric Transport and Oxidation Capacity) with the principle goal to create a comprehensive data set on stratospheric air intrusions into the troposphere along a rather frequently observed pathway over central Europe from the North Sea to the Mediterranean Sea. The measurements were based on predictions by suitable quasi-operational trajectory calculations using ECMWF forecast data. A predicted deep Stratosphere to Troposphere Transport (STT) event, encountered during the STACCATO period on 20-21 June 2001, was followed by the measurements network almost from its inception. Observations provide evidence that the intrusion affected large parts of central and southeastern Europe. Especially, the ozone lidar observations on 20-21 June 2001 at Garmisch-Partenkirchen, Germany captured the evolution of two marked tongues of high ozone with the first one descending to nearly 2 km, thus providing an excellent data set for model intercomparisons and validation. In addition, for the first time to our knowledge concurrent surface measurements of the cosmogenic radionuclides 10Be and 7Be and their ratio 10Be/7Be are presented together as stratospheric tracers in a case study of a stratospheric intrusion. The ozone tracer columns calculated with the FLEXPART model were found to be in good agreement with water vapour satellite images, capturing the evolution of the observed dry streamers of stratospheric origin. Furthermore, the time-height cross section of ozone tracer simulated with FLEXPART over Garmisch-Partenkirchen captures many details of the evolution of the two observed high-ozone filaments measured with the IFU lidar, thus demonstrating the considerable progress in model simulations. Finally, the modelled ozone (operationally available since October 1999) from the ECMWF (European Centre for Medium-Range Weather Forecasts) atmospheric model is shown to be in very good agreement with the observations during this case study, which provides the first successful validation of a chemical tracer that is derived operationally from a weather forecast model. This suggests that coupling chemistry and weather forecast models may significantly improve both weather and chemical forecasts in the future.