Comparison between ozone column depths and methane lifetimes computed by one- and three-dimensional models at different atmospheric O2 levels.

Recently, Cooke et al. (Cooke et al. 2022 R. Soc. Open Sci. 9, 211165. (doi:10.1098/rsos.211165)) used a three-dimensional coupled chemistry-climate model (WACCM6) to calculate ozone column depths at varied atmospheric O2 levels. They argued that previous one-dimensional (1-D) photochemical model studies, e.g. Segura et al. (Segura et al. 2003 Astrobiology 3, 689-708. (doi:10.1089/153110703322736024)), may have overestimated the ozone column depth at low pO2, and hence also overestimated the lifetime of methane. We have compared new simulations from an updated version of the Segura et al. model with those from WACCM6, together with some results from a second three-dimensional model. The discrepancy in ozone column depths is probably due to multiple interacting parameters, including H2O in the upper troposphere, lower boundary conditions, vertical and meridional transport rates, and different chemical mechanisms, especially the treatment of O2 photolysis in the Schumann-Runge (SR) bands (175-205 nm). The discrepancy in tropospheric OH concentrations and methane lifetime between WACCM6 and the 1-D model at low pO2 is reduced when absorption from CO2 and H2O in this wavelength region is included in WACCM6. Including scattering in the SR bands may further reduce this difference. Resolving these issues can be accomplished by developing an accurate parametrization for O2 photolysis in the SR bands and then repeating these calculations in the various models.

The response of the ozone layer to quadrupled CO2 concentrations.

An accurate quantification of the stratospheric ozone feedback in climate change simulations requires knowledge of the ozone response to increased greenhouse gases. Here, we present an analysis of the ozone layer response to an abrupt quadrupling of CO2 concentrations in four chemistry-climate models. We show that increased CO2 levels lead to a decrease in ozone concentrations in the tropical lower stratosphere, and an increase over the high latitudes and throughout the upper stratosphere. This pattern is robust across all models examined here, although important inter-model differences in the magnitude of the response are found. As a result of the cancellation between upper and lower stratospheric ozone, the total column ozone response in the tropics is small, and appears to be model dependent. A substantial portion of the spread in the tropical column ozone is tied to inter-model spread in upwelling. The high latitude ozone response is strongly seasonally dependent, and shows increases peaking in late-winter and spring of each hemisphere, with prominent longitudinal asymmetries. The range of ozone responses to CO2 reported in this paper has the potential to induce significant radiative and dynamical effects on the simulated climate. Hence, these results highlight the need of using an ozone dataset consistent with CO2 forcing in models involved in climate sensitivity studies.

Interactive nature of climate change and aerosol forcing.

The effect of changing cloud cover on climate, based on cloud-aerosol interactions, is one of the major unknowns for climate forcing and climate sensitivity. It has two components: (1) the impact of aerosols on clouds and climate due to in situ interactions (i.e., rapid response) and (2) the effect of aerosols on the cloud feedback that arises as climate changes-climate feedback response. We examine both effects utilizing the NASA Goddard Institute for Space Studies ModelE2 to assess the indirect effect, with both mass-based and microphysical aerosol schemes, in transient twentieth century simulations. We separate the rapid response and climate feedback effects by making simulations with a coupled version of the model as well as one with no sea surface temperature or sea ice response ("atmosphere-only" simulations). We show that the indirect effect of aerosols on temperature is altered by the climate feedbacks following the ocean response, and this change differs depending upon which aerosol model is employed. Overall, the effective radiative forcing (ERF) for the "direct effect" of aerosol-radiation interaction (ERFari) ranges between -0.2 and -0.6 W m-2 for atmosphere-only experiments, while the total effective radiative forcing, including[C0]the indirect effect (ERFari+aci) varies between about -0.4 and -1.1 W m-2 for atmosphere-only simulations; both ranges are in agreement with those given in Intergovernmental Panel on Climate Change (2013). Including the full feedback of the climate system lowers these ranges to -0.2 to -0.5 W m-2 for ERFari and -0.3 to -0.74 W m-2 for ERFari+aci. With both aerosol schemes, the climate change feedbacks have reduced the global average indirect radiative effect of atmospheric aerosols relative to what the emission changes would have produced, at least partially due to its effect on tropical upper tropospheric clouds.

Past, Present and Future Atmospheric Nitrogen Deposition.

Reactive nitrogen emissions into the atmosphere are increasing due to human activities, affecting nitrogen deposition to the surface and impacting the productivity of terrestrial and marine ecosystems. An atmospheric chemistry-transport model (TM4-ECPL) is here used to calculate the global distribution of total nitrogen deposition, accounting for the first time for both its inorganic and organic fractions in gaseous and particulate phases, and past and projected changes due to anthropogenic activities. The anthropogenic and biomass burning ACCMIP historical and RCP6.0 and RCP8.5 emissions scenarios are used. Accounting for organic nitrogen (ON) primary emissions, the present-day global nitrogen atmospheric source is about 60% anthropogenic, while total N deposition increases by about 20% relative to simulations without ON primary emissions. About 20-25% of total deposited N is ON. About 10% of the emitted nitrogen oxides are deposited as ON instead of inorganic nitrogen (IN) as is considered in most global models. Almost a 3-fold increase over land (2-fold over the ocean) has been calculated for soluble N deposition due to human activities from 1850 to present. The investigated projections indicate significant changes in the regional distribution of N deposition and chemical composition, with reduced compounds gaining importance relative to oxidized ones, but very small changes in the global total flux. Sensitivity simulations quantify uncertainties due to the investigated model parameterizations of IN partitioning onto aerosols and of N chemically fixed on organics to be within 10% for the total soluble N deposition and between 25-35% for the dissolved ON deposition. Larger uncertainties are associated with N emissions.