Global O3-CO Correlations in a Chemistry and Transport Model During July-August: Evaluation with TES Satellite Observations and Sensitivity to Input Meteorological Data and Emissions.

We examine the capability of the Global Modeling Initiative (GMI) chemistry and transport model to reproduce global mid-tropospheric (618hPa) O3-CO correlations determined by the measurements from Tropospheric Emission Spectrometer (TES) aboard NASA's Aura satellite during boreal summer (July-August). The model is driven by three meteorological data sets (fvGCM with sea surface temperature for 1995, GEOS4-DAS for 2005, and MERRA for 2005), allowing us to examine the sensitivity of model O3-CO correlations to input meteorological data. Model simulations of radionuclide tracers (222Rn, 210Pb, and 7Be) are used to illustrate the differences in transport-related processes among the meteorological data sets. Simulated O3 values are evaluated with climatological ozone profiles from ozonesonde measurements and satellite tropospheric O3 columns. Despite the fact that three simulations show significantly different global and regional distributions of O3 and CO concentrations, all simulations show similar patterns of O3-CO correlations on a global scale. These patterns are consistent with those derived from TES observations, except in the tropical easterly biomass burning outflow regions. Discrepancies in regional O3-CO correlation patterns in the three simulations may be attributed to differences in convective transport, stratospheric influence, and subsidence, among other processes. To understand how various emissions drive global O3-CO correlation patterns, we examine the sensitivity of GMI/MERRA model-calculated O3 and CO concentrations and their correlations to emission types (fossil fuel, biomass burning, biogenic, and lightning NOx emissions). Fossil fuel and biomass burning emissions are mainly responsible for the strong positive O3-CO correlations over continental outflow regions in both hemispheres. Biogenic emissions have a relatively smaller impact on O3-CO correlations than other emissions, but are largely responsible for the negative correlations over the tropical eastern Pacific, reflecting the fact that O3 is consumed and CO generated during the atmospheric oxidation process of isoprene under low NOx conditions. We find that lightning NOx emissions degrade both positive correlations at mid-/high- latitudes and negative correlations in the tropics because ozone production downwind of lightning NOx emissions is not directly related to the emission and transport of CO. Our study concludes that O3-CO correlations may be used effectively to constrain the sources of regional tropospheric O3 in global 3-D models, especially for those regions where convective transport of pollution plays an important role.

Origins of tropospheric ozone interannual variation (IAV) over Réunion: A model investigation.

Observations from long-term ozonesonde measurements show robust variations and trends in the evolution of ozone in the middle and upper troposphere over Réunion Island (21.1°S, 55.5°E) in June-August. Here we examine possible causes of the observed ozone variation at Réunion Island using hindcast simulations by the stratosphere-troposphere Global Modeling Initiative chemical transport model (GMI-CTM) for 1992-2014, driven by assimilated Modern-Era Retrospective Analysis for Research and Applications (MERRA) meteorological fields. Réunion Island is at the edge of the subtropical jet, a region of strong stratospheric-tropospheric exchange (STE). Our analysis implies that the large interannual variation (IAV) of upper tropospheric ozone over Réunion is driven by the large IAV of the stratospheric influence. The IAV of the large-scale, quasi-horizontal wind patterns also contributes to the IAV of ozone in the upper troposphere. Comparison to a simulation with constant emissions indicates that increasing emissions do not lead to the maximum trend in the middle and upper troposphere over Réunion during austral winter implied by the sonde data. The effects of increasing emission over southern Africa are limited to the lower troposphere near the surface in August - September.

Evaluation of the aerosol vertical distribution in global aerosol models through comparison against CALIOP measurements: AeroCom phase II results.

The ability of 11 models in simulating the aerosol vertical distribution from regional to global scales, as part of the second phase of the AeroCom model intercomparison initiative (AeroCom II), is assessed and compared to results of the first phase. The evaluation is performed using a global monthly gridded data set of aerosol extinction profiles built for this purpose from the CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) Layer Product 3.01. Results over 12 subcontinental regions show that five models improved, whereas three degraded in reproducing the interregional variability in Z α0-6 km, the mean extinction height diagnostic, as computed from the CALIOP aerosol profiles over the 0-6 km altitude range for each studied region and season. While the models' performance remains highly variable, the simulation of the timing of the Z α0-6 km peak season has also improved for all but two models from AeroCom Phase I to Phase II. The biases in Z α0-6 km are smaller in all regions except Central Atlantic, East Asia, and North and South Africa. Most of the models now underestimate Z α0-6 km over land, notably in the dust and biomass burning regions in Asia and Africa. At global scale, the AeroCom II models better reproduce the Z α0-6 km latitudinal variability over ocean than over land. Hypotheses for the performance and evolution of the individual models and for the intermodel diversity are discussed. We also provide an analysis of the CALIOP limitations and uncertainties contributing to the differences between the simulations and observations.

Measuring and modeling the lifetime of nitrous oxide including its variability.

Nitrous oxide lifetime is computed empirically from MLS satellite dataEmpirical N2O lifetimes compared with models including interannual variabilityResults improve values for present anthropogenic and preindustrial emissions.

Quantifying errors in trace species transport modeling.

One expectation when computationally solving an Earth system model is that a correct answer exists, that with adequate physical approximations and numerical methods our solutions will converge to that single answer. With such hubris, we performed a controlled numerical test of the atmospheric transport of CO(2) using 2 models known for accurate transport of trace species. Resulting differences were unexpectedly large, indicating that in some cases, scientific conclusions may err because of lack of knowledge of the numerical errors in tracer transport models. By doubling the resolution, thereby reducing numerical error, both models show some convergence to the same answer. Now, under realistic conditions, we identify a practical approach for finding the correct answer and thus quantifying the advection error.