Accelerating models for multiphase chemical kinetics through machine learning with polynomial chaos expansion and neural networks

The heterogeneous chemistry of atmospheric aerosols involves multiphase chemical kinetics that can be described by kinetic multi-layer models (KMs) that explicitly resolve mass transport and chemical reactions. However, KMs are computationally too expensive to be used as sub-modules in large-scale atmospheric models, and the computational costs also limit their utility in inverse-modeling approaches commonly used to infer aerosol kinetic parameters from laboratory studies. In this study, we show how machine learning methods can generate inexpensive surrogate models for the kinetic multi-layer model of aerosol surface and bulk chemistry (KM-SUB) to predict reaction times in multiphase chemical systems. We apply and compare two common and openly available methods for the generation of surrogate models, polynomial chaos expansion (PCE) with UQLab and neural networks (NNs) through the Python package Keras. We show that the PCE method is well suited to determining global sensitivity indices of the KMs, and we demonstrate how inverse-modeling applications can be enabled or accelerated with NN-suggested sampling. These qualities make them suitable supporting tools for laboratory work in the interpretation of data and the design of future experiments. Overall, the KM surrogate models investigated in this study are fast, accurate, and robust, which suggests their applicability as sub-modules in large-scale atmospheric models.

Automated summary

This study demonstrates how machine learning methods can be used to generate inexpensive surrogate models for predicting reaction times in multiphase chemical systems. Two common methods, polynomial chaos expansion (PCE) and neural networks (NNs), were applied and compared in generating these surrogate models. The results show that PCE is suitable for determining global sensitivity indices, while NNs can accelerate inverse modeling applications. Overall, the investigated surrogate models are fast, accurate, and robust, indicating their potential applicability as sub-modules in large-scale atmospheric models.