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The National Air Quality Forecast Capability (NAQFC) operated in the US National Oceanic and Atmospheric Administration (NOAA) provides the operational forecast guidance for ozone and fine particulate matter with aerodynamic diameters less than 2.5 µm (PM2.5) over the contiguous 48 US states (CONUS) using the Community Multi-scale Air Quality (CMAQ) model. The existing NAQFC uses climatological chemical lateral boundary conditions (CLBCs), which cannot capture pollutant intrusion events originating outside of the model domain. In this study, we developed a model framework to use dynamic CLBCs from the Goddard Earth Observing System Model, version 5 (GEOS) to drive NAQFC. A mapping of the GEOS chemical species to CMAQ's CB05–AERO6 (Carbon Bond 5; version 6 of the aerosol module) species was developed. The utilization of the GEOS dynamic CLBCs in NAQFC showed the best overall performance in simulating the surface observations during the Saharan dust intrusion and Canadian wildfire events in summer 2015. The simulated PM2.5 was improved from 0.18 to 0.37, and the mean bias was reduced from −6.74 to −2.96 µg m−3 over CONUS. Although the effect of CLBCs on the PM2.5 correlation was mainly near the inflow boundary, its impact on the background concentrations reached further inside the domain. The CLBCs could affect background ozone concentrations through the inflows of ozone itself and its precursors, such as CO. It was further found that the aerosol optical thickness (AOT) from satellite retrievals correlated well with the column CO and elemental carbon from GEOS. The satellite-derived AOT CLBCs generally improved the model performance for the wildfire intrusion events during a summer 2018 case study and demonstrated how satellite observations of atmospheric composition could be used as an alternative method to capture the air quality effects of intrusions when the CLBCs of global models, such as GEOS CLBCs, are not available.

We have derived values of the ultraviolet index (UVI) at solar noon using the Tropospheric Ultraviolet Model (TUV) driven by ozone, temperature and aerosol fields from climate simulations of the first phase of the Chemistry-Climate Model Initiative (CCMI-1). Since clouds remain one of the largest uncertainties in climate projections, we simulated only the clear-sky UVI. We compared the modelled UVI climatologies against present-day climatological values of UVI derived from both satellite data (the OMI-Aura OMUVBd product) and ground-based measurements (from the NDACC network). Depending on the region, relative differences between the UVI obtained from CCMI/TUV calculations and the ground-based measurements ranged between −5.9 % and 10.6 %. We then calculated the UVI evolution throughout the 21st century for the four Representative Concentration Pathways (RCPs 2.6, 4.5, 6.0 and 8.5). Compared to 1960s values, we found an average increase in the UVI in 2100 (of 2 %–4 %) in the tropical belt (30∘ N–30∘ S). For the mid-latitudes, we observed a 1.8 % to 3.4 % increase in the Southern Hemisphere for RCPs 2.6, 4.5 and 6.0 and found a 2.3 % decrease in RCP 8.5. Higher increases in UVI are projected in the Northern Hemisphere except for RCP 8.5. At high latitudes, ozone recovery is well identified and induces a complete return of mean UVI levels to 1960 values for RCP 8.5 in the Southern Hemisphere. In the Northern Hemisphere, UVI levels in 2100 are higher by 0.5 % to 5.5 % for RCPs 2.6, 4.5 and 6.0 and they are lower by 7.9 % for RCP 8.5. We analysed the impacts of greenhouse gases (GHGs) and ozone-depleting substances (ODSs) on UVI from 1960 by comparing CCMI sensitivity simulations (1960–2100) with fixed GHGs or ODSs at their respective 1960 levels. As expected with ODS fixed at their 1960 levels, there is no large decrease in ozone levels and consequently no sudden increase in UVI levels. With fixed GHG, we observed a delayed return of ozone to 1960 values, with a corresponding pattern of change observed on UVI, and looking at the UVI difference between 2090s values and 1960s values, we found an 8 % increase in the tropical belt during the summer of each hemisphere. Finally we show that, while in the Southern Hemisphere the UVI is mainly driven by total ozone column, in the Northern Hemisphere both total ozone column and aerosol optical depth drive UVI levels, with aerosol optical depth having twice as much influence on the UVI as total ozone column does.

The hydroxyl radical (OH) plays critical roles within the troposphere, such as determining the lifetime of methane (CH4), yet is challenging to model due to its fast cycling and dependence on a multitude of sources and sinks. As a result, the reasons for variations in OH and the resulting methane lifetime (τCH4), both between models and in time, are difficult to diagnose. We apply a neural network (NN) approach to address this issue within a group of models that participated in the Chemistry-Climate Model Initiative (CCMI). Analysis of the historical specified dynamics simulations performed for CCMI indicates that the primary drivers of τCH4 differences among 10 models are the flux of UV light to the troposphere (indicated by the photolysis frequency JO1D), the mixing ratio of tropospheric ozone (O3), the abundance of nitrogen oxides (NOx≡NO+NO2), and details of the various chemical mechanisms that drive OH. Water vapour, carbon monoxide (CO), the ratio of NO:NOx, and formaldehyde (HCHO) explain moderate differences in τCH4, while isoprene, methane, the photolysis frequency of NO2 by visible light (JNO2), overhead ozone column, and temperature account for little to no model variation in τCH4. We also apply the NNs to analysis of temporal trends in OH from 1980 to 2015. All models that participated in the specified dynamics historical simulation for CCMI demonstrate a decline in τCH4 during the analysed timeframe. The significant contributors to this trend, in order of importance, are tropospheric O3, JO1D, NOx, and H2O, with CO also causing substantial interannual variability in OH burden. Finally, the identified trends in τCH4 are compared to calculated trends in the tropospheric mean OH concentration from previous work, based on analysis of observations. The comparison reveals a robust result for the effect of rising water vapour on OH and τCH4, imparting an increasing and decreasing trend of about 0.5 % decade−1, respectively. The responses due to NOx, ozone column, and temperature are also in reasonably good agreement between the two studies.

Previous multi-model intercomparisons have shown that chemistry–climate models exhibit significant biases in tropospheric ozone compared with observations. We investigate annual-mean tropospheric column ozone in 15 models participating in the SPARC–IGAC (Stratosphere–troposphere Processes And their Role in Climate–International Global Atmospheric Chemistry) Chemistry-Climate Model Initiative (CCMI). These models exhibit a positive bias, on average, of up to 40 %–50 % in the Northern Hemisphere compared with observations derived from the Ozone Monitoring Instrument and Microwave Limb Sounder (OMI/MLS), and a negative bias of up to ∼ 30 % in the Southern Hemisphere. SOCOLv3.0 (version 3 of the Solar-Climate Ozone Links CCM), which participated in CCMI, simulates global-mean tropospheric ozone columns of 40.2 DU – approximately 33 % larger than the CCMI multi-model mean. Here we introduce an updated version of SOCOLv3.0, SOCOLv3.1, which includes an improved treatment of ozone sink processes, and results in a reduction in the tropospheric column ozone bias of up to 8 DU, mostly due to the inclusion of N2O5 hydrolysis on tropospheric aerosols. As a result of these developments, tropospheric column ozone amounts simulated by SOCOLv3.1 are comparable with several other CCMI models. We apply Gaussian process emulation and sensitivity analysis to understand the remaining ozone bias in SOCOLv3.1. This shows that ozone precursors (nitrogen oxides (NOx), carbon monoxide, methane and other volatile organic compounds, VOCs) are responsible for more than 90 % of the variance in tropospheric ozone. However, it may not be the emissions inventories themselves that result in the bias, but how the emissions are handled in SOCOLv3.1, and we discuss this in the wider context of the other CCMI models. Given that the emissions data set to be used for phase 6 of the Coupled Model Intercomparison Project includes approximately 20 % more NOx than the data set used for CCMI, further work is urgently needed to address the challenges of simulating sub-grid processes of importance to tropospheric ozone in the current generation of chemistry–climate models.

Major mid-winter stratospheric sudden warmings (SSWs) are the largest instance of wintertime variability in the Arctic stratosphere. Because SSWs are able to cause significant surface weather anomalies on intra-seasonal timescales, several previous studies have focused on their potential future change, as might be induced by anthropogenic forcings. However, a wide range of results have been reported, from a future increase in the frequency of SSWs to an actual decrease. Several factors might explain these contradictory results, notably the use of different metrics for the identification of SSWs and the impact of large climatological biases in single-model studies. To bring some clarity, we here revisit the question of future SSW changes, using an identical set of metrics applied consistently across 12 different models participating in the Chemistry–Climate Model Initiative. Our analysis reveals that no statistically significant change in the frequency of SSWs will occur over the 21st century, irrespective of the metric used for the identification of the event. Changes in other SSW characteristics – such as their duration, deceleration of the polar night jet, and the tropospheric forcing – are also assessed: again, we find no evidence of future changes over the 21st century., Blanca Ayarzagüena was funded by the European Project 603557-STRATOCLIM under the FP7-ENV.2013.6.1-2 programme and “Ayudas para la contratación de personal postdoctoral en formación en docencia e investigación en departamentos de la Universidad Complutense de Madrid”. Blanca Ayarzagüena and Ulrike Langematz wish to acknowledge the Deutsche Forschungsgemeinschaft (DFG) within the research programme SHARP under the grant LA 1025/15-1. Lorenzo M. Polvani is grateful for the continued support of the US National Science Foundation. The work of Neal Butchart, Steven C. Hardiman, and Fiona M. O'Connor was supported by the Joint BEIS/Defra Met Office Hadley Centre Climate Programme (GA01101). Neal Butchart and Steven C. Hardiman were supported by the European Community within the StratoClim project (grant 603557). Olaf Morgenstern and Guang Zeng acknowledge the UK Met Office for use of the Met Office Unified Model (MetUM). This research was supported by the New Zealand Government's Strategic Science Investment Fund (SSIF) through the NIWA programme CACV. Olaf Morgenstern acknowledges funding by the New Zealand Royal Society Marsden Fund (grant 12-NIW-006) and by the Deep South National Science Challenge (http://www.deepsouthchallenge.co.nz, last access: 21 March 2018). The authors wish to acknowledge the contribution of New Zealand eScience Infrastructure (NeSI) high-performance computing (HPC) facilities to the results of this research. New Zealand's national facilities are provided by NeSI and funded jointly by NeSI's collaborator institutions and through the Ministry of Business, Innovation & Employment's Research Infrastructure programme (https://www.nesi.org.nz, last access: 21 March 2018). The EMAC simulations were performed at the German Climate Computing Centre (DKRZ) through support from the Bundesministerium für Bildung und Forschung (BMBF). DKRZ and its Scientific Steering Committee are gratefully acknowledged for providing the HPC and data archiving resources for the consortial project ESCiMo (Earth System Chemistry integrated Modelling). CCSRNIES's research was supported by the Environment Research and Technology Development Funds of the Ministry of the Environment (2-1303) and Environment Restoration and Conservation Agency (2-1709), Japan, and computations were performed on NEC-SX9/A(ECO) and NEC SX-ACE computers at the Center for Global Environmental Research, NIES. The authors wish to thank two anonymous referees for their helpful comments.

Ozone within deep convective clouds is controlled by several factors involving photochemical reactions and transport. Gas-phase photochemical reactions and heterogeneous surface chemical reactions involving ice, water particles, and aerosols inside the clouds all contribute to the distribution and net production and loss of ozone. Ozone in clouds is also dependent on convective transport that carries low-troposphere/boundary-layer ozone and ozone precursors upward into the clouds. Characterizing ozone in thick clouds is an important step for quantifying relationships of ozone with tropospheric H2O, OH production, and cloud microphysics/transport properties. Although measuring ozone in deep convective clouds from either aircraft or balloon ozonesondes is largely impossible due to extreme meteorological conditions associated with these clouds, it is possible to estimate ozone in thick clouds using backscattered solar UV radiation measured by satellite instruments. Our study combines Aura Ozone Monitoring Instrument (OMI) and Microwave Limb Sounder (MLS) satellite measurements to generate a new research product of monthly-mean ozone concentrations in deep convective clouds between 30° S and 30° N for October 2004–April 2016. These measurements represent mean ozone concentration primarily in the upper levels of thick clouds and reveal key features of cloud ozone including: persistent low ozone concentrations in the tropical Pacific of ∼ 10 ppbv or less; concentrations of up to 60 pphv or greater over landmass regions of South America, southern Africa, Australia, and India/east Asia; connections with tropical ENSO events; and intraseasonal/Madden–Julian oscillation variability. Analysis of OMI aerosol measurements suggests a cause and effect relation between boundary-layer pollution and elevated ozone inside thick clouds over landmass regions including southern Africa and India/east Asia.

In this study we use ozone and stratospheric ozone tracer simulations from the high-resolution (0.5∘×0.5∘) Goddard Earth Observing System, Version 5 (GEOS-5), in a replay mode to study the impact of stratospheric ozone on tropospheric ozone interannual variability (IAV). We use these simulations in conjunction with ozonesonde measurements from 1990 to 2016 during the winter and spring seasons. The simulations include a stratospheric ozone tracer (StratO3) to aid in the evaluation of the impact of stratospheric ozone IAV on the IAV of tropospheric ozone at different altitudes and locations. The model is in good agreement with the observed interannual variation in tropospheric ozone, except for the post-Pinatubo period (1992–1994) over the region of North America. Ozonesonde data show a negative ozone anomaly in 1992–1994 following the Pinatubo eruption, with recovery thereafter. The simulated anomaly is only half the magnitude of that observed. Our analysis suggests that the simulated stratosphere–troposphere exchange (STE) flux deduced from the analysis might be too strong over the North American (50–70∘ N) region after the Mt. Pinatubo eruption in the early 1990s, masking the impact of lower stratospheric ozone concentration on tropospheric ozone. European ozonesonde measurements show a similar but weaker ozone depletion after the Mt. Pinatubo eruption, which is fully reproduced by the model. Analysis based on the stratospheric ozone tracer identifies differences in strength and vertical extent of stratospheric ozone impact on the tropospheric ozone interannual variation (IAV) between North America and Europe. Over North American stations, the StratO3 IAV has a significant impact on tropospheric ozone from the upper to lower troposphere and explains about 60 % and 66 % of the simulated ozone IAV at 400 hPa and ∼11 % and 34 % at 700 hPa in winter and spring, respectively. Over European stations, the influence is limited to the middle to upper troposphere and becomes much smaller at 700 hPa. The Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2), assimilated fields exhibit strong longitudinal variations over Northern Hemisphere (NH) mid-high latitudes, with lower tropopause height and lower geopotential height over North America than over Europe. These variations associated with the relevant variations in the location of tropospheric jet flows are responsible for the longitudinal differences in the stratospheric ozone impact, with stronger effects over North America than over Europe.

Understanding and modeling the large-scale transport of trace gases and aerosols is important for interpreting past (and projecting future) changes in atmospheric composition. Here we show that there are large differences in the global-scale atmospheric transport properties among the models participating in the IGAC SPARC Chemistry–Climate Model Initiative (CCMI). Specifically, we find up to 40 % differences in the transport timescales connecting the Northern Hemisphere (NH) midlatitude surface to the Arctic and to Southern Hemisphere high latitudes, where the mean age ranges between 1.7 and 2.6 years. We show that these differences are related to large differences in vertical transport among the simulations, in particular to differences in parameterized convection over the oceans. While stronger convection over NH midlatitudes is associated with slower transport to the Arctic, stronger convection in the tropics and subtropics is associated with faster interhemispheric transport. We also show that the differences among simulations constrained with fields derived from the same reanalysis products are as large as (and in some cases larger than) the differences among free-running simulations, most likely due to larger differences in parameterized convection. Our results indicate that care must be taken when using simulations constrained with analyzed winds to interpret the influence of meteorology on tropospheric composition.

We use a series of chemical transport model and chemistry climate model simulations to investigate the observed negative trends in MOPITT CO over several regions of the world, and to examine the consistency of time-dependent emission inventories with observations. We find that simulations driven by the MACCity inventory, used for the Chemistry Climate Modeling Initiative (CCMI), reproduce the negative trends in the CO column observed by MOPITT for 2000–2010 over the eastern United States and Europe. However, the simulations have positive trends over eastern China, in contrast to the negative trends observed by MOPITT. The model bias in CO, after applying MOPITT averaging kernels, contributes to the model–observation discrepancy in the trend over eastern China. This demonstrates that biases in a model's average concentrations can influence the interpretation of the temporal trend compared to satellite observations. The total ozone column plays a role in determining the simulated tropospheric CO trends. A large positive anomaly in the simulated total ozone column in 2010 leads to a negative anomaly in OH and hence a positive anomaly in CO, contributing to the positive trend in simulated CO. These results demonstrate that accurately simulating variability in the ozone column is important for simulating and interpreting trends in CO.

Ozone fields simulated for the first phase of the Chemistry-Climate Model Initiative (CCMI-1) will be used as forcing data in the 6th Coupled Model Intercomparison Project. Here we assess, using reference and sensitivity simulations produced for CCMI-1, the suitability of CCMI-1 model results for this process, investigating the degree of consistency amongst models regarding their responses to variations in individual forcings. We consider the influences of methane, nitrous oxide, a combination of chlorinated or brominated ozone-depleting substances, and a combination of carbon dioxide and other greenhouse gases. We find varying degrees of consistency in the models' responses in ozone to these individual forcings, including some considerable disagreement. In particular, the response of total-column ozone to these forcings is less consistent across the multi-model ensemble than profile comparisons. We analyse how stratospheric age of air, a commonly used diagnostic of stratospheric transport, responds to the forcings. For this diagnostic we find some salient differences in model behaviour, which may explain some of the findings for ozone. The findings imply that the ozone fields derived from CCMI-1 are subject to considerable uncertainties regarding the impacts of these anthropogenic forcings. We offer some thoughts on how to best approach the problem of generating a consensus ozone database from a multi-model ensemble such as CCMI-1.