Solar radiation modification (SRM) is increasingly discussed as a potential method to ameliorate some negative effects of climate change. However, unquantified uncertainties in physical and environmental impacts of SRM impede informed debate and decision making. Some uncertainties are due to lack of understanding of processes determining atmospheric effects of SRM and/or a lag in development of their representation in models, meaning even high-quality model intercomparisons will not necessarily reveal or address them. Although climate models at multiple scales are advancing in complexity, there are specific areas of uncertainty where additional model development (often requiring new observations) could significantly advance understanding of SRM's effects, and improve our ability to assess and weigh potential risks against those of choosing to not use SRM. We convene expert panels in the areas of atmospheric science most critical to understanding the three most widely discussed forms of SRM. Each identifies three key modeling gaps relevant to either stratospheric aerosols, cirrus, or low-altitude marine clouds. Within each area, key challenges remain in capturing impacts due to complex interactions in aerosol physics, atmospheric chemistry/dynamics, and aerosol-cloud interactions. Across all three, in addition to arguing for more observations, the panels argue that model development work to either leverage different capabilities of existing models, bridge scales across which relevant processes operate, or address known modeling gaps could advance understanding. By focusing on these knowledge gaps we believe the modeling community could advance understanding of SRM's physical risks and potential benefits, allowing better-informed decision-making about whether and how to use SRM.

Atmospheric sensitivities (gradients), quantifying the atmospheric response to emissions or other perturbations, can provide meaningful insights on the underlying atmospheric chemistry or transport processes. Atmospheric adjoint modeling enables the calculation of receptor-oriented sensitivities of model outputs of interest to input parameters (e.g., emissions), overcoming the numerical cost of conventional (forward) modeling. The adjoint of the GEOS-Chem atmospheric chemistry-transport model is a widely used such model, but prior to v36 it lacked extensive stratospheric capabilities. Here, we present the development and evaluation of the discrete adjoint of the global chemistry-transport model (CTM) GEOS-Chem unified chemistry extension (UCX) for stratospheric applications, which extends the existing capabilities of the GEOS-Chem adjoint to enable the calculation of sensitivities that include stratospheric chemistry and interactions. This development adds 37 new tracers, 273 kinetic and photolysis reactions, an updated photolysis scheme, treatment of stratospheric aerosols, and all other features described in the original UCX paper. With this development the GEOS-Chem adjoint model is able to capture the spatial, temporal, and speciated variability in stratospheric ozone depletion processes, among other processes. We demonstrate its use by calculating 2-week sensitivities of stratospheric ozone to precursor species and show that the adjoint captures the Antarctic ozone depletion potential of active halogen species, including the chlorine activation and deactivation process. The spatial variations in the sensitivity of stratospheric ozone to NOx emissions are also described. This development expands the scope of research questions that can be addressed by allowing stratospheric interactions and feedbacks to be considered in the tropospheric sensitivity and inversion applications.

Contrails are potentially the largest contributor to aviation-attributable climate change, but estimates of their coverage are highly uncertain. No study has provided observation-based continental-scale estimates of the diurnal, seasonal, and regional variability in contrail coverage. We present contrail coverage estimates for the years 2018, 2019 and 2020 for the contiguous United States, derived by developing and applying a deep learning algorithm to over 100 000 satellite images. We estimate that contrails covered an area the size of Massachusetts and Connecticut combined in the years 2018 and 2019. Comparing 2019 and 2020, we quantify a 35.8% reduction in distance flown above 8 km altitude and an associated reduction in contrail coverage of 22.3%. We also find that the diurnal pattern in contrail coverage aligns with that of flight traffic, but that the amount of contrail coverage per distance flown decreases in the afternoon.

Model-based estimates of aviation’s climate impacts have found that contrails contribute 36%–81% of aviation’s instantaneous radiative forcing. These estimates depend on the accuracy of meteorological data provided by reanalyses like ECMWF Reanalysis 5th Generation (ERA5) and Modern Era Retrospective analysis for Research and Applications V2 (MERRA-2). Using data from 793 044 radiosondes, we find persistent contrails forming at cruise altitudes in 30° N–60° S are overestimated by factors of 2.0 and 3.5 for ERA5 and MERRA-2, respectively. Seasonal and inter-annual trends are well-reproduced by both models (R2 = 0.79 and 0.74). We also find a contrail lifetime metric is overestimated by 17% in ERA5 and 45% in MERRA-2. Finally, the reanalyses incorrectly identify individual regions that could form persistent contrails 87% and 52% of the time, respectively. These results suggest that contrail models currently overestimate the number and lifetime of persistent contrails. Additional observations are needed for future models in order to provide locally accurate estimates of contrails or to support mitigation strategies.

Depletion of stratospheric ozone, and the associated increase in population exposure to UV radiation, is an environmental consequence of high-altitude, supersonic aviation. Assessments of the impacts of emissions from subsonic aircraft – which fly at lower altitudes – have instead shown that they produce a net increase, rather than decrease, in global net ozone, suggesting the existence of an intermediate “column ozone neutral” cruise altitude. Knowing this altitude and its variation with factors such as latitude, season, and fuel composition could provide a pathway towards reducing the environmental impacts of aviation, but would require a prohibitive number of atmospheric simulations. We instead use the newly developed GEOS-Chem tropospheric-stratospheric adjoint to identify the location of the column ozone-neutral aircraft cruise altitude as a function of these factors. We show that, although the mean ozone neutral altitude is at 13.5 km globally, this varies from 14.6 km to 12.5 km between the equator and 60°N. This altitude varies by less than a kilometer between seasons, but the net depletion resulting from flying at greater altitudes varies by a factor of two. We also find that eliminating fuel sulfur would result in a neutral altitude 0.5–1.0 km greater than when conventional jet fuel is burned. Our results imply that a low Mach number supersonic aircraft burning low-sulfur fuel (e.g. biofuels) may be able to achieve net zero global ozone change. However, for a fleet to achieve ozone neutrality will require careful consideration of the non-linear variation in sensitivity with altitude and latitude.

Outdoor air pollution adversely affects human health and is estimated to be responsible for five to ten per cent of the total annual premature mortality in the contiguous United States^1-3. Combustion emissions from a variety of sources, such as power generation or road traffic, make a large contribution to harmful air pollutants such as ozone and fine particulate matter (PM2.5)⁴. Efforts to mitigate air pollution have focused mainly on the relationship between local emission sources and local air quality². Air quality can also be affected by distant emission sources, however, including emissions from neighbouring federal states^5,6. This cross-state exchange of pollution poses additional regulatory challenges. Here we quantify the exchange of air pollution among the contiguous United States, and assess its impact on premature mortality that is linked to increased human exposure to PM_2.5 and ozone from seven emission sectors for 2005 to 2018. On average, we find that 41 to 53 per cent of air-quality-related premature mortality resulting from a state's emissions occurs outside that state. We also find variations in the cross-state contributions of different emission sectors and chemical species to premature mortality, and changes in these variations over time. Emissions from electric power generation have the greatest cross-state impacts as a fraction of their total impacts, whereas commercial/residential emissions have the smallest. However, reductions in emissions from electric power generation since 2005 have meant that, by 2018, cross-state premature mortality associated with the commercial/residential sector was twice that associated with power generation. In terms of the chemical species emitted, nitrogen oxides and sulfur dioxide emissions caused the most cross-state premature deaths in 2005, but by 2018 primary PM_2.5 emissions led to cross-state premature deaths equal to three times those associated with sulfur dioxide emissions. These reported shifts in emission sectors and emission species that contribute to premature mortality may help to guide improvements to air quality in the contiguous United States.

Aviation emissions have been found to cause5%of global anthropogenic radiative forcing and ∼16 000 premature deaths annually due to impaired air quality. When aiming to reduce these impacts, decision makers often face trade-offs between different emission species or impacts in different times and locations. To inform rational decision-making, this study computes aviation’s marginal climate and air quality impacts per tonne of species emitted and accounts for the altitude, location, and chemical composition of emissions. Climate impacts are calculated using a reduced-order climate model, and air quality-related health impacts are quantified using marginal atmospheric sensitivities to emissions from the adjoint of the global chemistry-transport model GEOS-Chem in combination with concentration response functions and the value of statistical life. The results indicate that 90% of the global impacts per unit of fuel burn are attributable to cruise emissions, and that 64% of all damages are the result of air quality impacts. Furthermore, nitrogen oxides (NOx), carbon dioxide (CO2), and contrails are collectively responsible for 97% of the total impact. Applying our result metrics to an example, we find that a 20%NOx stringency scenario for new aircraft would reduce the net atmospheric impacts by 700mUSD during the first year of operation, even if theNOx emission reductions cause a small increase inCO2 emissions of 2%. In such a way, the damage metrics can be used to rapidly evaluate the atmospheric impacts of market growth as well as emissions trade-offs of aviation-related policies or technology improvements.

In September 2015, the Volkswagen Group (VW) admitted the use of 'defeat devices' designed to lower emissions measured during VW vehicle testing for regulatory purposes. Globally, 11 million cars sold between 2008 and 2015 are affected, including about 2.6 million in Germany. On-road emissions tests have yielded mean on-road NO _x emissions for these cars of 0.85 g km ^-1 , over four times the applicable European limit of 0.18 g km ^-1 . This study estimates the human health impacts and costs associated with excess emissions from VW cars driven in Germany. A distribution of on-road emissions factors is derived from existing measurements and combined with sales data and a vehicle fleet model to estimate total excess NO _x emissions. These emissions are distributed on a 25 by 28 km grid covering Europe, using the German Federal Environmental Protection Agency's (UBA) estimate of the spatial distribution of NO _x emissions from passenger cars in Germany. We use the GEOS-Chem chemistry-transport model to predict the corresponding increase in population exposure to fine particulate matter and ozone in the European Union, Switzerland, and Norway, and a set of concentration-response functions to estimate mortality outcomes in terms of early deaths and of life-years lost. Integrated over the sales period (2008-2015), we estimate median mortality impacts from VW excess emissions in Germany to be 1200 premature deaths in Europe, corresponding to 13 000 life-years lost and 1.9 billion EUR in costs associated with life-years lost. Approximately 60% of mortality costs occur outside Germany. For the current fleet, we estimate that if on-road emissions for all affected VW vehicles in Germany are reduced to the applicable European emission standard by the end of 2017, this would avert 29 000 life-years lost and 4.1 billion 2015 EUR in health costs (median estimates) relative to a counterfactual case with no recall.

The US Environmental Protection Agency (EPA) has alleged that Volkswagen Group of America (VW) violated the Clean Air Act (CAA) by developing and installing emissions control system 'defeat devices' (software) in model year 2009-2015 vehicles with 2.0 litre diesel engines. VW has admitted the inclusion of defeat devices. On-road emissions testing suggests that in-use NO_x emissions for these vehicles are a factor of 10 to 40 above the EPA standard. In this paper we quantify the human health impacts and associated costs of the excess emissions. We propagate uncertainties throughout the analysis. A distribution function for excess emissions is estimated based on available in-use NO_x emissions measurements. We then use vehicle sales data and the STEP vehicle fleet model to estimate vehicle distance traveled per year for the fleet. The excess NO_x emissions are allocated on a 50 km grid using an EPA estimate of the light duty diesel vehicle NO_x emissions distribution. We apply a GEOS-Chem adjoint-based rapid air pollution exposure model to produce estimates of particulate matter and ozone exposure due to the spatially resolved excess NO_x emissions. A set of concentration-response functions is applied to estimate mortality and morbidity outcomes. Integrated over the sales period (2008-2015) we estimate that the excess emissions will cause 59 (95% CI: 10 to 150) early deaths in the US. When monetizing premature mortality using EPA-recommended data, we find a social cost of ∼$450m over the sales period. For the current fleet, we estimate that a return to compliance for all affected vehicles by the end of 2016 will avert ∼130 early deaths and avoid ∼$840m in social costs compared to a counterfactual case without recall.