Estimating transboundary transported anthropogenic sulfate deposition in Japan using the sulfur isotopic ratio.

High emissions of air pollutants from Northeast Asia are strongly influenced by air quality as well as by ecosystems. This study investigated the spatiotemporal variations in the sulfur isotopic ratio (δS) in atmospheric deposition at eleven monitoring stations in Japan from 2011 to 2016 and estimated the amount of transboundary transported anthropogenic sulfate (TRB) deposition using mass balance calculations. The δS of sulfate in precipitation ranged from -0.42 to +22.7‰. Sea salt (SS), TRB, and domestic anthropogenic sources (DOM) were the dominant sources of sulfate deposition in Japan. TRB sulfate deposition was largest on the Sea of Japan side, with an annual average value of 1.5 ± 0.3-6.9 ± 0.5 mg m d (36-44%), followed by Mt. Happo (4.5 ± 0.1 mg m d; 88%), the Pacific Ocean side (1.5 ± 0.8, 4.3 ± 0.9 mg m d; 24-50%), and the remote islands in the North Pacific Ocean (1.1 ± 0.2, 2.0 ± 0.8 mg m d; 19-32%). TRB sulfate deposition on the Sea of Japan side was 2-12 times higher in winter and 1-2 times higher in summer than that of DOM. In contrast, TRB sulfate deposition on the Pacific Ocean side was 1.5-3 times higher in summer than in winter due to high precipitation levels. In Tokyo, the annual contribution from DOM sulfate deposition is approximately three times higher than that from TRB. Annual TRB sulfate deposition is lowest at Ogasawara at 1.1 ± 0.2 mg m d, and the annual oceanic DMS contribution to sulfate deposition is high, accounting for 1.3 mg m d (20 ± 6%). The contribution of Asian dust was estimated to be 1-5.2 mg m d(3-6%), which occurred in a single Asian dust event on the Sea of Japan side.