Constraining surface emissions of air pollutants using inverse modelling: method intercomparison and a new two-step two-scale regularization approach

Abstract

When constraining surface emissions of air pollutants using inverse modelling one often encounters spurious corrections to the inventory at places where emissions and observations are colocated, referred to here as the colocalization problem. Several approaches have been used to deal with this problem: coarsening the spatial resolution of emissions; adding spatial correlations to the covariance matrices; adding constraints on the spatial derivatives into the functional being minimized; and multiplying the emission error covariance matrix by weighting factors. Intercomparison of methods for a carbon monoxide inversion over a city shows that even though all methods diminish the colocalization problem and produce similar general patterns, detailed information can greatly change according to the method used ranging from smooth, isotropic and short range modifications to not so smooth, non-isotropic and long range modifications. Poisson (non-Gaussian) and Gaussian assumptions both show these patterns, but for the Poisson case the emissions are naturally restricted to be positive and changes are given by means of multiplicative correction factors, producing results closer to the true nature of emission errors. Finally, we propose and test a new two-step, two-scale, fully Bayesian approach that deals with the colocalization problem and can be implemented for any prior density distribution. DOI: 10.1111/j.1600-0889.2011.00529.x