Effect of sulfate aerosol on tropospheric NOx and ozone budgets: Model simulations and TOPSE evidence

The distributions of NOx and O3 are analyzed during TOPSE (Tropospheric Ozone Production about the Spring Equinox). In this study these data are compared with the calculations of a global chemical/transport model (Model for OZone And Related chemical Tracers (MOZART)). Specifically, the effect that hydrolysis of N2O5 on sulfate aerosols has on tropospheric NOx and O3 budgets is studied. The results show that without this heterogeneous reaction, the model significantly overestimates NOx concentrations at high latitudes of the Northern Hemisphere (NH) in winter and spring in comparison to the observations during TOPSE; with this reaction, modeled NOx concentrations are close to the measured values. This comparison provides evidence that the hydrolysis of N2O5 on sulfate aerosol plays an important role in controlling the tropospheric NOx and O3 budgets. The calculated reduction of NOx attributed to this reaction is 80 to 90% in winter at high latitudes over North America. Because of the reduction of NOx, O3 concentrations are also decreased. The maximum O3reduction occurs in spring although the maximum NOx reduction occurs in winter when photochemical O3 production is relatively low. The uncertainties related to uptake coefficient and aerosol loading in the model is analyzed. The analysis indicates that the changes in NOxdue to these uncertainties are much smaller than the impact of hydrolysis of N2O5 on sulfate aerosol. The effect that hydrolysis of N2O5 on global NOx and O3 budgets are also assessed by the model. The results suggest that in the Northern Hemisphere, the average NOx budget decreases 50% due to this reaction in winter and 5% in summer. The average O3 budget is reduced by 8% in winter and 6% in summer. In the Southern Hemisphere (SH), the sulfate aerosol loading is significantly smaller than in the Northern Hemisphere. As a result, sulfate aerosol has little impact on NOx and O3 budgets of the Southern Hemisphere

Ozone, aerosol, potential vorticity, and trace gas trends observed at high‐latitudes over North America from February to May 2000

Ozone (O3) and aerosol scattering ratio profiles were obtained from airborne lidar measurements on thirty‐eight flights over seven deployments covering the latitudes of 40°–85°N between 4 February and 23 May 2000 as part of the Tropospheric Ozone Production about the Spring Equinox (TOPSE) field experiment. Each deployment started from Broomfield, Colorado, with bases in Churchill, Canada, and on most deployments, Thule Air Base, Greenland. Nadir and zenith lidar O3 measurements were combined with in situ O3 measurements to produce vertically continuous O3 profiles from near the surface to above the tropopause. Potential vorticity (PV) distributions along the flight track were obtained from several different meteorological analyses. Ozone, aerosol, and PV distributions were used together to identify the presence of pollution plumes and stratospheric intrusions. Ozone was found to increase in the middle free troposphere (4–6 km) at high latitudes (60°–85°N) by an average of 4.6 ppbv/mo (parts per billion by volume per month) from about 54 ppbv in early February to over 72 ppbv in mid‐May. The average aerosol scattering ratios at 1064 nm in the same region increased rapidly at an average rate of 0.36/mo from about 0.38 to over 1.7. Ozone and aerosol scattering were highly correlated over the entire field experiment, and PV and beryllium (7Be) showed no significant positive trend over the same period. The primary cause of the observed O3 increase in the mid troposphere at high latitudes was determined to be the photochemical production of O3 in pollution plumes with less than 20% of the increase from stratospherically‐derived O3

French/Belgian Scientific Contribution to Tropospheric Studies using the METOP Sensors

International audienceWe propose to combine the tropospheric measurements provided by the IASI and GOME2 instruments aboard METOP, together with data from ground-based stations, airborne and spaceborne remote sensors, along with atmospheric chemistry models (CTMs) in order to improve our knowledge of processes constraining the chemical composition of the troposphere and to study the regional and global scale air quality. The measurements of ozone (O3), carbon monoxide (CO), nitrogen dioxide (NO2), formaldehyde (CH2O), and methane (CH4) will be used in conjunction with the 3D tropospheric LMDz-INCA, MOZART, IMAGES and CHIMERE CTM models, using data assimilation and inversion modeling techniques, to study the global distribution of these species and to derive improved emissions estimates. Before the METOP launch, all the tools developed in the framework of this project will be used to analyse the AURA TES and OMI tropospheric products. After the launch of METOP, the data provided by both satellites will then be analyzed with the CTMs. The resulting global distributions will be used to perform detailed studies of the role of biomass burning in the budget of tropospheric species, the emissions of ozone precursors, the role of convective transport of pollutants, and its consequences in terms of air quality

Uncertainties in the simulation of XCO2 plumes from power plant emissions: A comparison between 6 high-resolution atmospheric transport models

Power plants are a major source of CO2 globally. Although their emissions are routinely monitored in many countries especially in the developed world, these numbers are often not publicly available and a complete global record is still far from reality. An important goal of Europe's planned Copernicus CO2 satellite mission CO2M is therefore to provide an independent quantification of power plant emissions worldwide. Emissions may be estimated from satellite XCO2 observations by simulating the plumes with an atmospheric transport model and finding those emissions that minimize a cost function of the differences between simulation and observations. Here we present a comparison of CO2 plume simulations from six high-resolution models, three Large Eddy Simulation models, two mesoscale Eulerian models, and one Lagrangian particle dispersion model. Simulations were conducted for two large coal-fired power plants, Belchatow in Poland and Jänschwalde in Germany, which were extensively observed with aircraft in situ and remote sensing measurements during the CoMet campaign in May-June 2018. The observations provide a unique opportunity to study the capability of the models to simulate such plumes in a realistic manner and to design optimal modelling and emission quantification strategies. The Belchatow plume was sampled under highly convective and turbulent conditions whereas the Jänschwalde plume was observed in a more stable weather situation. The models are able to reproduce these differences by simulating a highly structured turbulent plume for Belchatow and a more Gaussian-shaped plume for Jänschwalde. However, the models differ in many details including the horizontal and vertical spread of the plumes, suggesting that in addition to resolution the specific choices of turbulence and advection scheme have a significant impact on the results. Our findings suggest that estimating emissions from individual images is particularly challenging for turbulent plumes. Since turbulence intensity evolves with the build-up of the convective boundary layer, a satellite overpass well before noon would likely be an advantage

Error Budget of the MEthane Remote LIdar missioN and Its Impact on the Uncertainties of the Global Methane Budget

International audienceMEthane Remote LIdar missioN (MERLIN) is a German‐French space mission, scheduled for launch in 2024 and built around an innovative light detecting and ranging instrument that will retrieve methane atmospheric weighted columns. MERLIN products will be assimilated into chemistry transport models to infer methane emissions and sinks. Here the expected performance of MERLIN to reduce uncertainties on methane emissions is estimated. A first complete error budget of the mission is proposed based on an analysis of the plausible causes of random and systematic errors. Systematic errors are spatially and temporally distributed on geophysical variables and then aggregated into an ensemble of 32 scenarios. Observing System Simulation Experiments are conducted, originally carrying both random and systematic errors. Although relatively small (±2.9 ppb), systematic errors are found to have a larger influence on MERLIN performances than random errors. The expected global mean uncertainty reduction on methane emissions compared to the prior knowledge is found to be 32%, limited by the impact of systematic errors. The uncertainty reduction over land reaches 60% when the largest desert regions are removed. At the latitudinal scale, the largest uncertainty reductions are achieved for temperate regions (84%) and then tropics (56%) and high latitudes (53%). Similar Observing System Simulation Experiments based on error scenarios for Greenhouse Gases Observing SATellite reveal that MERLIN should perform better than Greenhouse Gases Observing SATellite for most continental regions. The integration of error scenarios for MERLIN in another inversion system suggests similar results, albeit more optimistic in terms of uncertainty reduction