Isotopic fingerprinting of dissolved iron sources in the deep western Pacific since the late Miocene

Iron (Fe) is a productivity-limiting nutrient in the ocean. However, the sources of dissolved Fe (dFe) in the deep ocean and how they respond to tectonic and climate changes are still poorly understood. In the northern hemisphere, dust flux to the low-latitude western Pacific has increased dramatically since the late Miocene associated with intense aridification of the Asian inland. Meanwhile, the terrigenous material supply to the open ocean might have also changed as a result of the reorganization of the Pacific circulation due to the gradual closure of seaways in the low latitudes. Therefore, the western Pacific is a characteristic region for understanding the sources of dFe in the deep ocean and their responses to long term climate changes. Here, we present data on isotopic evolution of dFe and dissolved Pb since similar to 8 Ma based on ferromanganese crust METG-03 (16.0 degrees N, 152.0 degrees E, 3850 m water depth) in the western Pacific deep water. Our results show that delta Fe-56 of the crust remains fairly stable since the late Miocene, i.e., about -0.32 +/- 0.08 parts per thousand (2SD). We infer that delta Fe-56 of dFe in the deep western Pacific is relatively invariant at similar to 0.45 +/- 0.1 parts per thousand based on the Fe isotopic fractionation between hydrogenetic crust and the seawater dissolved component. The reconstructed isotope signature is similar to the measured delta Fe-56 value (0.37 +/- 0.15 parts per thousand) of the intermediate to deep waters in the modern low-latitude western Pacific region close to the island arcs, but is significantly higher than that of the eastern Pacific deep waters near South America which is controlled by the reductive dissolution of continental shelf sediments and the hydrothermal inputs (delta Fe-56<-0.1 parts per thousand). The deep-water(206)Pb/Pb-204 ratio recorded by METG-03 displays systematic increase at about 8-4 Ma, reflecting increased input from sediment dissolution of low-latitude island arcs associated with reorganization of the western Pacific deep circulation. Notably, Fe isotopes of terrigenous materials from different sources are similar, while their dissolved Fe isotopic signatures released to the ocean are mainly controlled by the mechanism of particle dissolution. The stability of delta Fe-56 and systematic changes in Pb isotopes over the last similar to 8 Ma thus suggest that Asian dust dissolution and hydrothermal inputs are likely only minor sources of dFe in the low-latitude deep western Pacific, while the acquisition and transport of dFe from shelf sediments by organic ligand binding in the oxic environment is the major dFe source which keeps stable on tectonic time scales since the late Miocene.