A Nudge to the Truth: Atom Conservation as a Hard Constraint in Models of Atmospheric Composition Using a Species-Weighted Correction

Abstract

Computational models of atmospheric composition are not always physically consistent. For example, not all models respect fundamental conservation laws such as conservation of atoms in an interconnected chemical system. In well performing models, these unphysical deviations are often ignored because they are frequently minor, and thus only need a small nudge to perfectly conserve mass. Here we introduce a method that anchors a prediction from any numerical model to physically consistent hard constraints, nudging concentrations to the nearest solution that respects the conservation laws. This closed-form model-agnostic correction uses a single matrix operation to minimally perturb the predicted concentrations to ensure that atoms are conserved to machine precision. To demonstrate this approach, we train a gradient boosting decision tree ensemble to emulate a small reference model of ozone photochemistry and test the effect of the correction on accurate but nonconservative predictions. The nudging approach minimally perturbs the already well-predicted results for most species, but decreases the accuracy of important oxidants, including radicals. We develop a weighted extension of this nudging approach that considers the uncertainty and magnitude of each species in the correction. This species-level weighting approach is essential to accurately predict important low concentration species such as radicals. We find that applying the species-weighted correction slightly improves overall accuracy by nudging unphysical predictions to a more likely mass-conserving solution.

Computational models of atmospheric composition do not always make scientifically trustworthy predictions. This corrective approach minimally adjusts the predicted concentrations of chemical species to guarantee conservation of mass.