The Common Representative Intermediates Mechanism Version 2 in the United Kingdom Chemistry and Aerosols Model

Funder: Met Office and the Natural Environment Research CouncilFunder: ESA Climate Change InitiativeAbstract: We document the implementation of the Common Representative Intermediates Mechanism version 2, reduction 5 into the United Kingdom Chemistry and Aerosol model (UKCA) version 10.9. The mechanism is merged with the stratospheric chemistry already used by the StratTrop mechanism, as used in UKCA and the UK Earth System Model, to create a new CRI‐Strat mechanism. CRI‐Strat simulates a more comprehensive treatment of non‐methane volatile organic compounds (NMVOCs) and provides traceability with the Master Chemical Mechanism. In total, CRI‐Strat simulates the chemistry of 233 species competing in 613 reactions (compared to 87 species and 305 reactions in the existing StratTrop mechanism). However, while more than twice as complex than StratTrop, the new mechanism is only 75% more computationally expensive. CRI‐Strat is evaluated against an array of in situ and remote sensing observations and simulations using the StratTrop mechanism in the UKCA model. It is found to increase production of ozone near the surface, leading to higher ozone concentrations compared to surface observations. However, ozone loss is also greater in CRI‐Strat, leading to less ozone away from emission sources and a similar tropospheric ozone burden compared to StratTrop. CRI‐Strat also produces more carbon monoxide than StratTrop, particularly downwind of biogenic VOC emission sources, but has lower burdens of nitrogen oxides as more is converted into reservoir species. The changes to tropospheric ozone and nitrogen budgets are sensitive to the treatment of NMVOC emissions, highlighting the need to reduce uncertainty in these emissions to improve representation of tropospheric chemical composition

Constraining regional greenhouse gas emissions using geostationary concentration measurements: a theoretical study

Abstract. We investigate the ability of column-integrated trace gas measurements from a geostationary satellite to constrain surface fluxes at regional scale. The proposed GEOCARB instrument measures CO2, CO and CH4 at a maximum resolution of 3 km east–west × 2.7 km north–south. Precisions are 3 ppm for CO2, 10 ppb for CO and 18 ppb for CH4. Sampling frequency is flexible. Here we sample a region at the location of Shanghai every 2 daylight hours for 6 days in June. We test the observing system by calculating the posterior uncertainty covariance of fluxes. We are able to constrain urban emissions at 3 km resolution including an isolated power plant. The CO measurement plays the strongest role; without it our effective resolution falls to 5 km. Methane fluxes are similarly well estimated at 5 km resolution. Estimating the errors for a full year suggests such an instrument would be a useful tool for both science and policy applications

Estimating CO<sub>2</sub> emissions from point sources: a case study of an isolated power station

Abstract. A methodology to estimate CO2 emissions from an isolated power plant is presented and illustrated for the Northern Power Station at Port Augusta, South Australia. The method involves measurement of in-situ and column-averaged CO2 at a site near the power plant, forward modelling (using WRF-Chem) of the observed signals and inverse modelling to obtain an estimate of the fluxes from the power plant. By subtracting the simulated background CO2 (obtained from Monitoring Atmospheric Composition and Climate CO2 fields) from the observed and simulated signals, we are able to account for fluxes from the power plant that are mainly responsible for the variations in the CO2 concentrations. Although the enhancements of the surface concentration of CO2 are a factor of 10 larger than the enhancements in the column-averaged concentration, the forward transport model has difficulty predicting the in-situ data, which is complicated by sea breeze effects and influence from other local sources. Better simulation is obtained for the column-averaged data leading to better estimates of fluxes. The ratio of our estimated emissions to the reported values is 1.06 ± 0.54. Modelling local biospheric fluxes makes little difference either to the estimated emissions or quality of the fit to the data. Variations in the large-scale concentration field have a larger impact highlighting the importance of good boundary conditions even in the relatively homogeneous Southern Hemisphere. The estimates are insensitive to details of the calculation such as stack height or modelling of plume injection. We conclude that column-integrated measurements offer a reasonable trade-off between sensitivity and model capability for estimating point sources