Spatiotemporal variations of tropospheric ozone in Spain (2008-2019).

This study aims to support the development of Spain's Ozone Mitigation Plan by evaluating the present-day spatial variation (2015-2019) and trends (2008-2019) for seven ground-level ozone (O3) metrics relevant for human/ecosystems exposure and regulatory purposes. Results indicate that the spatial variation of O3 depends on the part of the O3 distribution being analyzed. Metrics associated with moderate O3 concentrations depict an increasing O3 gradient between the northern and Mediterranean coasts due to climatic factors, while for metrics considering the upper end of the O3 distribution, this climatic gradient tends to attenuate in favor of hotspot regions pointing to relevant local/regional O3 formation. A classification of atmospheric regions in Spain is proposed based on their O3 pollution patterns, to identify priority areas (or O3 hotspots) where local/regional precursor abatement might significantly reduce O3 during pollution episodes. The trends assessment reveals a narrowing of the O3 distribution at the national level, with metrics influenced by lower concentrations tending to increase over time, and those reflecting the higher end of the O3 distribution tending to decrease. While most stations show no statistically significant variations, contrasting O3 trends are evident among the O3 hotspots. The Madrid area exhibits the majority of upward trends across all metrics, frequently with the highest increasing rates, implying increasing O3 associated with both chronic and episodic exposure. The Valencian Community area exhibits a mixed variation pattern, with moderate to high O3 metrics increasing and peak metrics decreasing, while O3 in areas downwind of Barcelona, the Guadalquivir Valley and Puertollano shows no variations. Sevilla is the only large Spanish city with generalized O3 decreasing trends. The different O3 trends among hotspots highlight the need for mitigation measures to be designed at a local/regional scale to be effective. This approach may offer valuable insights for other countries developing O3 mitigation plans.

Multi-sectoral impact assessment of an extreme African dust episode in the Eastern Mediterranean in March 2018.

In late March 2018, a large part of the Eastern Mediterranean experienced an extraordinary episode of African dust, one of the most intense in recent years, here referred to as the "Minoan Red" event. The episode mainly affected the Greek island of Crete, where the highest aerosol concentrations over the past 15 yeas were recorded, although impacts were also felt well beyond this core area. Our study fills a gap in dust research by assessing the multi-sectoral impacts of sand and dust storms and their socioeconomic implications. Specifically, we provide a multi-sectoral impact assessment of Crete during the occurrence of this exceptional African dust event. During the day of the occurrence of the maximum dust concentration in Crete, i.e. March 22nd, 2018, we identified impacts on meteorological conditions, agriculture, transport, energy, society (including closing of schools and cancellation of social events), and emergency response systems. As a result, the event led to a 3-fold increase in daily emergency responses compare to previous days associated with urban emergencies and wildfires, a 3.5-fold increase in hospital visits and admissions for Chronic Obstructive Pulmonary Disease (COPD) exacerbations and dyspnoea, a reduction of visibility causing aircraft traffic disruptions (eleven cancellations and seven delays), and a reduction of solar energy production. We estimate the cost of direct and indirect effects of the dust episode, considering the most affected socio-economic sectors (e.g. civil protection, aviation, health and solar energy production), to be between 3.4 and 3.8 million EUR for Crete. Since such desert dust transport episodes are natural, meteorology-driven and thus to a large extent unavoidable, we argue that the efficiency of actions to mitigate dust impacts depends on the accuracy of operational dust forecasting and the implementation of relevant early warning systems for social awareness.

To what extent the traffic restriction policies applied in Barcelona city can improve its air quality?

Barcelona city (Spain) is applying a series of traffic restriction measures that aim at renewing and reducing the amount of circulating vehicles to improve air quality. The measures include changes in the built environment to reduce private vehicle space in specific areas through the so-called "superblocks" and tactical urban planning actions, along with the implementation of a city-wide Low Emission Zone (LEZ) that restricts the entry of the most polluting vehicles to the city. Our study quantifies the impact of these measures in the greater area of Barcelona combining a coupled macroscopic traffic and pollutant emission model with a multi-scale air quality model. Our modelling system allows estimating the effect of different traffic restrictions upon traffic and the associated emissions and air quality levels at a very high resolution (20 m). The measures were evaluated both individually and collectively to assess both their relative and overall impact upon emissions and air quality. We show that in the absence of traffic demand reductions, the application of isolated measures that reduce private vehicle space, either through superblocks or tactical urban planning, have no overall emission impacts; only localized street-level NOx positive and negative changes (±17%) are found due to traffic re-routing and the generation of new bottlenecks. It is only when these measures are combined with optimistic fleet renewal as a result of the LEZ implementation and demand reductions, that relevant global emission reductions in NOx are obtained (-13% and -30%, respectively) with estimated NO2 reductions of -36% and -23% at the two traffic air quality monitoring stations. Despite the potential improvements, our simulations suggest that current measures are insufficient to comply with EU air quality standards and that further traffic restriction policies to reduce traffic demand are needed.

Improved representation of the global dust cycle using observational constraints on dust properties and abundance.

Even though desert dust is the most abundant aerosol by mass in Earth's atmosphere, atmospheric models struggle to accurately represent its spatial and temporal distribution. These model errors are partially caused by fundamental difficulties in simulating dust emission in coarse-resolution models and in accurately representing dust microphysical properties. Here we mitigate these problems by developing a new methodology that yields an improved representation of the global dust cycle. We present an analytical framework that uses inverse modeling to integrate an ensemble of global model simulations with observational constraints on the dust size distribution, extinction efficiency, and regional dust aerosol optical depth. We then compare the inverse model results against independent measurements of dust surface concentration and deposition flux and find that errors are reduced by approximately a factor of two relative to current model simulations of the Northern Hemisphere dust cycle. The inverse model results show smaller improvements in the less dusty Southern Hemisphere, most likely because both the model simulations and the observational constraints used in the inverse model are less accurate. On a global basis, we find that the emission flux of dust with geometric diameter up to 20 µm (PM20) is approximately 5,000 Tg/year, which is greater than most models account for. This larger PM20 dust flux is needed to match observational constraints showing a large atmospheric loading of coarse dust. We obtain gridded data sets of dust emission, vertically integrated loading, dust aerosol optical depth, (surface) concentration, and wet and dry deposition fluxes that are resolved by season and particle size. As our results indicate that this data set is more accurate than current model simulations and the MERRA-2 dust reanalysis product, it can be used to improve quantifications of dust impacts on the Earth system.

GISS-E2.1: Configurations and Climatology.

This paper describes the GISS-E2.1 contribution to the Coupled Model Intercomparison Project, Phase 6 (CMIP6). This model version differs from the predecessor model (GISS-E2) chiefly due to parameterization improvements to the atmospheric and ocean model components, while keeping atmospheric resolution the same. Model skill when compared to modern era climatologies is significantly higher than in previous versions. Additionally, updates in forcings have a material impact on the results. In particular, there have been specific improvements in representations of modes of variability (such as the Madden-Julian Oscillation and other modes in the Pacific) and significant improvements in the simulation of the climate of the Southern Oceans, including sea ice. The effective climate sensitivity to 2 × CO2 is slightly higher than previously at 2.7-3.1°C (depending on version) and is a result of lower CO2 radiative forcing and stronger positive feedbacks.

Ozone source apportionment during peak summer events over southwestern Europe.

It is well established that in Europe, high O3 concentrations are most pronounced in southern/Mediterranean countries due to the more favourable climatological conditions for its formation. However, the contribution of the different sources of precursors to O3 formation within each country relative to the imported (regional and hemispheric) O3 is poorly quantified. This lack of quantitative knowledge prevents local authorities from effectively designing plans that reduce the exceedances of the O3 target value set by the European air quality directive. O3 source attribution is a challenge because the concentration at each location and time results not only from local biogenic and anthropogenic precursors, but also from the transport of O3 and precursors from neighbouring regions, O3 regional and hemispheric transport and stratospheric O3 injections. The main goal of this study is to provide a first quantitative estimation of the contribution of the main anthropogenic activity sectors to peak O3 events in Spain relative to the contribution of imported (regional and hemispheric) O3. We also assess the potential of our source apportionment method to improve O3 modelling. Our study applies and thoroughly evaluates a countrywide O3 source apportionment method implemented in the CALIOPE air quality forecast system for Spain at high resolution (4 × 4 km2) over a 10-day period characterized by typical summer conditions in the Iberian Peninsula (IP). The method tags both O3 and its gas precursor emissions from source sectors within one simulation, and each tagged species is subject to the typical physico-chemical processes (advection, vertical mixing, deposition, emission and chemistry) as the actual conditions remain unperturbed. We quantify the individual contributions of the largest NO x local sources to high O3 concentrations compared with the contribution of imported O3. We show, for the first time, that imported O3 is the largest input to the ground-level O3 concentration in the IP, accounting for 46 %-68 % of the daily mean O3 concentration during exceedances of the European target value. The hourly imported O3 increases during typical northwestern advections (70 %-90 %, 60-80 µg m-3), and decreases during typical stagnant conditions (30 %-40 %, 30-60 µg m-3) due to the local NO titration. During stagnant conditions, the local anthropogenic precursors control the O3 peaks in areas downwind of the main urban and industrial regions (up to 40 % in hourly peaks). We also show that ground-level O3 concentrations are strongly affected by vertical mixing of O3-rich layers present in the free troposphere, which result from local/regional layering and accumulation, and continental/hemispheric transport. Indeed, vertical mixing largely explains the presence of imported O3 at ground level in the IP. Our results demonstrate the need for detailed quantification of the local and remote contributions to high O3 concentrations for local O3 management, and show O3 source apportionment to be an essential analysis prior to the design of O3 mitigation plans in any non-attainment area. Achieving the European O3 objectives in southern Europe requires not only ad hoc local actions but also decided national and European-wide strategies.

Predicting the mineral composition of dust aerosols: Insights from elemental composition measured at the Izaña Observatory.

Regional variations of dust mineral composition are fundamental to climate impacts but generally neglected in climate models. A challenge for models is that atlases of soil composition are derived from measurements following wet sieving, which destroys the aggregates potentially emitted from the soil. Aggregates are crucial to simulating the observed size distribution of emitted soil particles. We use an extension of brittle fragmentation theory in a global dust model to account for these aggregates. Our method reproduces the size-resolved dust concentration along with the approximately size-invariant fractional abundance of elements like Fe and Al in the decade-long aerosol record from the Izaña Observatory, off the coast of West Africa. By distinguishing between Fe in structural and free forms, we can attribute improved model behavior to aggregation of Fe and Al-rich clay particles. We also demonstrate the importance of size-resolved measurements along with elemental composition analysis to constrain models.

Atmospheric transport and deposition of mineral dust to the ocean: implications for research needs.

This paper reviews our knowledge of the measurement and modeling of mineral dust emissions to the atmosphere, its transport and deposition to the ocean, the release of iron from the dust into seawater, and the possible impact of that nutrient on marine biogeochemistry and climate. Of particular concern is our poor understanding of the mechanisms and quantities of dust deposition as well as the extent of iron solubilization from the dust once it enters the ocean. Model estimates of dust deposition in remote oceanic regions vary by more than a factor of 10. The fraction of the iron in dust that is available for use by marine phytoplankton is still highly uncertain. There is an urgent need for a long-term marine atmospheric surface measurement network, spread across all oceans. Because the southern ocean is characterized by large areas with high nitrate but low chlorophyll surface concentrations, that region is particularly sensitive to the input of dust and iron. Data from this region would be valuable, particularly at sites downwind from known dust source areas in South America, Australia, and South Africa. Coordinated field experiments involving both atmospheric and marine measurements are recommended to address the complex and interlinked processes and role of dust/Fe fertilization on marine biogeochemistry and climate.