Source and fate of atmospheric iron supplied to the subarctic North Pacific traced by stable iron isotope ratios

Abstract

The availability of dissolved iron (Fe) limits primary production over some regions of the surface ocean, especially in regions such as the subarctic North Pacific. In this work, we use Fe stable isotope ratios (δ56Fe) in bulk and size-fractionated marine aerosol particles and dissolved Fe of surface seawater in the subarctic North Pacific on Japanese GEOTRACES cruise GP02 (Summer 2017) as a tracer to clarify the relative contribution of combustion and natural Fe in both marine aerosol particles and surface seawater. The bulk aerosols collected in the coastal regions of both East Asia and western North Pacific have total δ56Fe values that are as low as −0.5 ‰ when compared to crustal (+0.1 ‰), with both the water-soluble phase and the fine particles even more fractionated (as low as −1.9 and −2.8 ‰, respectively). The negative correlation between the aerosol δ56Fe signatures and the enrichment factors of Fe and other elements dominated by anthropogenic sources (e.g., lead and cadmium) in these coastal regions indicates the presence of Fe emitted from high-temperature combustion sources, such as coal combustion and metal smelting. In these regions, combustion Fe accounts for 4–13 and 13–45 % of the total and water-soluble aerosol Fe, respectively. The results demonstrate that soluble aerosol Fe sourced from combustion Fe can be equivalent to that sourced from natural dust Fe in these coastal regions. By contrast, the aerosol particles in pelagic regions were near crustal δ56Fe in all particle size fractions, indicating the dominance of natural Fe and little to no combustion Fe. The relationships among the fractional Fe solubility, major ion concentration, Fe species, and δ56Fe indicate that the presence of combustion Fe is the dominant reason for the solubility increase in the coastal regions and that the atmospheric processing of mineral dust during transport is more important in the pelagic regions. The dissolved Fe of the surface seawater at 10 m depth had a consistently higher δ56Fe by up to +1.5 ‰ than that of the simultaneously collected water-soluble aerosol Fe. The pattern of the elevated δ56Fe in the surface seawater corresponds to decreasing Fe concentrations and can be approximated by Rayleigh fractionation; we attribute these elevated surface δ56Fe values to the effect of biological uptake. New Fe fluxes from both the atmosphere and deeper depths are limited at least in summer compared with the biological uptake in the open ocean of the subarctic North Pacific.