A Physics-Constrained Deep-Learning Framework based on Long-Term Remote-Sensing Data for Retrieving Vertical Distribution of PM2.5 Chemical Components

Abstract

The vertical distribution of PM2.5 chemical components is crucial for identifying the causes of atmospheric pollution and its impact on climate change and extreme weather. By integrating long-term lidar measurements, deep-learning algorithms and a physics-constrained optimization method, this paper presents a novel lidar-based retrieval framework to obtain vertical mass concentration profiles of PM2.5 chemical components for the first time. Identifiable components include sulfate (SO42-), nitrate (NO3-), ammonium (NH4+), organic matter (OM) and black carbon (BC), which extend beyond the component types that traditional remote-sensing retrievals can identify. A 1-year retrieved surface mass concentrations of these components closely aligned with the observations, with Pearson correlation coefficient values ranging from 0.87 to 0.97. The retrieval framework applied to varying non-training spatiotemporal scenarios showed moderate generalization capability, although a tendency toward underestimation is observed. Tower and aircraft-based field campaigns indicate that the retrieved and observed vertical profiles of these components exhibited consistent patterns in mass concentrations and proportions. Subsequently, an explainable method was incorporated into the retrieval framework to quantify the multivariate driving effects on vertical profile retrieval. Results showed that the extinction coefficient and representative indicators within physiochemical processes contributed significantly to mass concentrations of these components. Finally, a dataset of vertical mass concentration profiles of these components over six years in a Chinese megacity (Beijing) was generated by the retrieval framework, revealing the dominant roles of OM and NO3- in PM2.5 throughout the entire boundary layer across all seasons. As a result of the continued implementation of clean air policies in China, these components exhibited significant decreases during 2021–2022 compared with 2017–2018. Our retrieval framework offers a novel approach for acquiring vertical profiles of PM2.5 chemical components, thereby providing a new perspective on elucidating the vertical evolution of atmospheric pollutants.