Predictions of the Optical Properties of Brown Carbon Aerosol by Machine Learning with Typical Chromophores

The linkages between BrC optical properties and chemical composition remain inadequately understood, with quantified chromophores explaining less than 25% of ambient aerosol light absorption. This study characterized 38 typical chromophores in aerosols collected in Xi'an, with light absorption contributions to BrC ranging from 1.6 +/- 0.3 to 5.8 +/- 2.6% at 365 nm. Based on these quantified chromophores, an interpretable machine learning model and the Shapley Additive Explanation (SHAP) method were employed to explore the relationships between BrC optical properties and chemical composition. The model attained high accuracy with Pearson correlation coefficients (r) exceeding 0.93 for the absorption coefficient (Abs lambda) and surpassing 0.57 for mass absorption efficiency (MAE lambda) of BrC. It explains more than 80% of the variance in Abs and over 50% in MAE, significantly improving the understanding of BrC light absorption. Polycyclic aromatic hydrocarbons (PAHs) and oxygenated PAHs (OPAHs) with four and five rings exhibit significant positive effects on Abs lambda, suggesting that similar unidentified chromophores may also notably impact BrC optical characteristics. The model based on chromophore mass concentrations further simplifies studying BrC optical characteristics. This study advances understanding of the relationship between BrC composition and optical properties and guides the investigation of unrecognized chromophores.