Distinct spatiotemporal patterns of atmospheric total and soluble iron from three sources revealed by shipboard online observations in the Northwest Pacific

Abstract

Non-dust emissions have been increasingly recognized as important contributors to atmospheric iron (Fe), influencing marine productivity through enhanced bioavailable Fe inputs. However, accurately quantifying the contributions and spatiotemporal variability of non-dust sources remains challenging due to relatively low time-resolution of traditional filter-based analytical methods. In this study, the contributions of non-dust emissions to atmospheric total and soluble Fe in the Northwest Pacific were quantified based on online measurements from three ship-based observation campaigns in 2021–2022. A Positive Matrix Factorization (PMF) model was applied for source apportionment. Results showed non-dust emissions were notable contributors to atmospheric total Fe, representing 24 %–41 % of total Fe in PM10 and 30 %–56 % in PM2.5 samples across different cruise legs. Importantly, their contributions to soluble Fe were significantly higher, reaching 88 %–97 % in PM10 and 85 %–98 % in PM2.5 samples. Among non-dust sources, land anthropogenic emissions contributed substantially to both total and soluble Fe, whereas ship emission contributed a small portion to total Fe but was a major source of soluble Fe, particularly in summer, when its contribution reached 79 % of soluble Fe in PM10 samples in coastal regions. Additionally, Fe from non-dust sources exhibited stronger spatial variability than dust source. The concentrations of land anthropogenic Fe differed by 3–5 times between coastal and open-ocean areas during the same cruises, while ship-derived Fe varied by an order of magnitude or more. This study offers critical observational evidence to advance understanding of how diverse emission sources shape atmospheric composition in Asian continental outflow regions.