Knowledge-guided machine learning reveals pivotal drivers for gas-to-particle conversion of atmospheric nitrate

Abstract

Particulate nitrate, a key component of fine particles, forms through the intricate gas-to-particle conversion process. This process is regulated by the gas-to-particle conversion coefficient of nitrate (ε(NO ₃ ⁻)). The mechanism between ε(NO ₃ ⁻) and its drivers is highly complex and nonlinear, and can be characterized by machine learning methods. However, conventional machine learning often yields results that lack clear physical meaning and may even contradict established physical/chemical mechanisms due to the influence of ambient factors. It urgently needs an alternative approach that possesses transparent physical interpretations and provides deeper insights into the impact of ε(NO ₃ ⁻). Here we introduce a supervised machine learning approach—the multilevel nested random forest guided by theory approaches. Our approach robustly identifies NH ₄ ⁺, SO ₄ ²⁻, and temperature as pivotal drivers for ε(NO ₃ ⁻). Notably, substantial disparities exist between the outcomes of traditional random forest analysis and the anticipated actual results. Furthermore, our approach underscores the significance of NH ₄ ⁺ during both daytime (30%) and nighttime (40%) periods, while appropriately downplaying the influence of some less relevant drivers in comparison to conventional random forest analysis. This research underscores the transformative potential of integrating domain knowledge with machine learning in atmospheric studies.

Graphical abstract

Highlights

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  Multilevel nested random forest guided by theory approaches yields reliable results.

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  Pivotal variables are screened automatically via recursive feature elimination.

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  The approach rectifies the outcomes of RF and thoroughly discourses G/P conversion.

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  The significance of NH ₄ ⁺ is underscored during both daytime (30%) and nighttime (40%).

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  Integrating domain knowledge into machine learning is a research hotspot in the future.