Water vapor (H₂O) is the source of reactive hydrogen radicals in the middle atmosphere, whereas carbon monoxide (CO), being formed by CO₂photolysis, is suitable as a dynamical tracer. In the mesosphere, both H₂O and CO are sensitive to solar irradiance (SI) variability because of their destruction/production by solar radiation. This enables us to analyze the solar signal in both models and observed data. Here, we evaluate the mesospheric H₂O and CO response to solar irradiance variability using the Chemistry- Climate Model Initiative (CCMI-1) simulations and satellite observations. We analyzed the results of four CCMI models (CMAM, EMAC-L90MA, SOCOLv3, and CESM1- WACCM 3.5) operated in CCMI reference simulation REFC1SD in specified dynamics mode, covering the period from 1984-2017. Multiple linear regression analyses show a pronounced and statistically robust response of H₂O and CO to solar irradiance variability and to the annual and semiannual cycles. For periods with available satellite data, we compared the simulated solar signal against satellite observations, namely the GOZCARDS composite for 1992-2017 for H₂O and Aura/MLS measurements for 2005-2017 for CO. The model results generally agree with observations and reproduce an expected negative and positive correlation for H₂O and CO, respectively, with solar irradiance. However, the magnitude of the response and patterns of the solar signal varies among the considered models, indicating differences in the applied chemical reaction and dynamical schemes, including the representation of photolyzes. We suggest that there is no dominating thermospheric influence of solar irradiance in CO, as reported in previous studies, because the response to solar variability is comparable with observations in both low-top and high-top models. We stress the importance of this work for improving our understanding of the current ability and limitations of state-of-the-art models to simulate a solar signal in the chemistry and dynamics of the middle atmosphere.

Because tropospheric ozone is both a greenhouse gas and harmful air pollutant, it is important to understand how anthropogenic activities may influence its abundance and distribution through the 21st century. Here, we present model simulations performed with the chemistry-climate model SOCOL, in which spatially disaggregated chemistry and transport tracers have been implemented in order to better understand the distribution and projected changes in tropospheric ozone. We examine the influences of ozone precursor emissions (nitrogen oxides (NO_x), carbon monoxide (CO) and volatile organic compounds (VOCs)), climate change (including methane effects) and stratospheric ozone recovery on the tropospheric ozone budget, in a simulation following the climate scenario Representative Concentration Pathway (RCP) 6.0 (a medium-high, and reasonably realistic climate scenario). Changes in ozone precursor emissions have the largest effect, leading to a global-mean increase in tropospheric ozone which maximizes in the early 21st century at 23% compared to 1960. The increase is most pronounced at northern midlatitudes, due to regional emission patterns: between 1990 and 2060, northern midlatitude tropospheric ozone remains at constantly large abundances: 31% larger than in 1960. Over this 70-year period, attempts to reduce emissions in Europe and North America do not have an effect on zonally averaged northern midlatitude ozone because of increasing emissions from Asia, together with the long lifetime of ozone in the troposphere. A simulation with fixed anthropogenic ozone precursor emissions of NO_x, CO and non-methane VOCs at 1960 conditions shows a 6% increase in global-mean tropospheric ozone by the end of the 21st century, with an 11 % increase at northern midlatitudes. This increase maximizes in the 2080s and is mostly caused by methane, which maximizes in the 2080s following RCP 6.0, and plays an important role in controlling ozone directly, and indirectly through its influence on other VOCs and CO. Enhanced flux of ozone from the stratosphere to the troposphere as well as climate change-induced enhancements in lightning NO_x emissions also increase the tropospheric ozone burden, although their impacts are relatively small. Overall, the results show that under this climate scenario, ozone in the future is governed largely by changes in methane and NO_x; methane induces an increase in tropospheric ozone that is approximately one-third of that caused by NO_x. Climate impacts on ozone through changes in tropospheric temperature, humidity and lightning NO_x remain secondary compared with emission strategies relating to anthropogenic emissions of NO_x, such as fossil fuel burning. Therefore, emission policies globally have a critical role to play in determining tropospheric ozone evolution through the 21st century.