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53 pags., 19 figs., 1 tab., Our understanding of the processes that control the burden and budget of tropospheric ozone has changed dramatically over the last 60 years. Models are the key tools used to understand these changes, and these underscore that there are many processes important in controlling the tropospheric ozone budget. In this critical review, we assess our evolving understanding of these processes, both physical and chemical. We review model simulations from the International Global Atmospheric Chemistry Atmospheric Chemistry and Climate Model Intercomparison Project and Chemistry Climate Modelling Initiative to assess the changes in the tropospheric ozone burden and its budget from 1850 to 2010. Analysis of these data indicates that there has been significant growth in the ozone burden from 1850 to 2000 (approximately 43 ± 9%) but smaller growth between 1960 and 2000 (approximately 16 ± 10%) and that the models simulate burdens of ozone well within recent satellite estimates. The Chemistry Climate Modelling Initiative model ozone budgets indicate that the net chemical production of ozone in the troposphere plateaued in the 1990s and has not changed since then inspite of increases in the burden. There has been a shift in net ozone production in the troposphere being greatest in the northern mid and high latitudes to the northern tropics, driven by the regional evolution of precursor emissions. An analysis of the evolution of tropospheric ozone through the 21st century, as simulated by Climate Model Intercomparison Project Phase 5 models, reveals a large source of uncertainty associated with models themselves (i.e., in the way that they simulate the chemical and physical processes that control tropospheric ozone). This structural uncertainty is greatest in the near term (two to three decades), but emissions scenarios dominate uncertainty in the longer term (2050¿2100) evolution of tropospheric ozone. This intrinsic model uncertainty prevents robust predictions of near-term changes in the tropospheric ozone burden, and we review how progress can be made to reduce this limitation., ATA and PTG would like to acknowledge support from National Centre for Atmospheric Science. YE would like to acknowledge support from the National Science Foundation Atmospheric and Geospace Sciences awards # 1900795 and 1929368. TW acknowledges support from the Hong Kong Research Grants Council (T24-504/17-N) and the National Natural Science Foundation of China (91844301). ASL thanks European Executive Agency under the European Union’s Horizon 2020 Research Innovation programme (Project “ERC-2016-COG 726349 CLIMAHAL”). RH is supported by an NERC Independent Research Fellowship (NE/N014375/1). YMS is supported by an NERC PhD studentship. Part of this research was carried out at the Jet Propulsion Laboratory, California Institute of Technology, under a contract with the National Aeronautics and Space Administration.

Sesquiterpenes are one of the precursors of secondary organic aerosol (SOA) which can be an important global sources of organic aerosol (OA). Updating the chemistry scheme in the global chemistry transport model by incorporating an oxidation mechanism for β-caryophyllene (representing all sesquiterpenes), adding global sesquiterpene emissions of 29 Tg/yr and revising global monoterpene emissions up to 162 Tg/yr (Guenther et al., 2012) led to an increase of SOA burden by 95% and SOA production rate by 106% relative to the base case described in Utembe et al. (2011). Including the emissions of sesquiterpenes resulted in increase of SOA burden of 0.11 Tg and SOA production rate of 12.9 Tg/yr relative to the base case. The highest concentrations of sesquiterpene-derived SOA (by up to 1.2 µg/m3) were found over central Africa and South America, the regions having high levels of biogenic emissions with significant biomass burning. In the updated model simulation, the multi-generation oxidation products from sesquiterpenes and monoterpenes transported above the boundary layer and condensed to the aerosol phase at higher altitude led to an increase of OA by up to 30% over the tropics and northern mid to higher altitudes. The model evaluation showed an underestimation of model OA mostly for the campaigns dominated by regional anthropogenic pollution. The increase of SOA production from sesquiterpenes reduced the discrepancies between modelled and observed OA concentrations over the remote and rural areas. The increase of SOA concentrations by up to 200% from pre-industrial to present scenarios was found over the tropical oceans.

The impact of climate change between 2000 and 2095 SRES A2 climates on surface ozone (O)3 and on O3 source-receptor (S-R) relationships is quantified using three coupled climate-chemistry models (CCMs). The CCMs exhibit considerable variability in the spatial extent and location of surface O3 increases that occur within parts of high NOx emission source regions (up to 6 ppbv in the annual average and up to 14 ppbv in the season of maximum O3). In these source regions, all three CCMs show a positive relationship between surface O3 change and temperature change. Sensitivity simulations show that a combination of three individual chemical processes—(i) enhanced PAN decomposition, (ii) higher water vapor concentrations, and (iii) enhanced isoprene emission—largely reproduces the global spatial pattern of annual-mean surface O3 response due to climate change (R2 = 0.52). Changes in climate are found to exert a stronger control on the annual-mean surface O3 response through changes in climate-sensitive O3 chemistry than through changes in transport as evaluated from idealized CO-like tracer concentrations. All three CCMs exhibit a similar spatial pattern of annual-mean surface O3 change to 20% regional O3 precursor emission reductions under future climate compared to the same emission reductions applied under present-day climate. The surface O3 response to emission reductions is larger over the source region and smaller downwind in the future than under present-day conditions. All three CCMs show areas within Europe where regional emission reductions larger than 20% are required to compensate climate change impacts on annual-mean surface O3., JRC.H.4-Monitoring Agricultural Resources