Abstract. We implemented a tagged tracer method of black carbon (BC) into a global chemistry transport model, GEOSChem, examined the pathways and efficiency of long-range transport from a variety of anthropogenic and biomass burning emission sources to the Arctic, and quantified the source contributions of individual emissions. Firstly, we evaluated the simulated BC by comparing it with observations at the Arctic sites and examined the sensitivity of an aging parameterization and wet scavenging rate by ice clouds. For tagging BC, we added BC tracers distinguished by source types (anthropogenic and biomass burning) and regions; the global domain was divided into 16 and 27 regions for anthropogenic and biomass burning emissions, respectively. Our simulations showed that BC emitted from Europe and Russia was transported to the Arctic mainly in the lower troposphere during winter and spring. In particular, BC transported from Russia was widely spread over the Arctic in winter and spring, leading to a dominant contribution of 62 % to the Arctic BC near the surface as the annual mean. In contrast, BC emitted from East Asia was found to be transported in the middle troposphere into the Arctic mainly over the Sea of Okhotsk and eastern Siberia during winter and spring. We identified an important "window" area, which allowed a strong incoming of East Asian BC to the Arctic (130-180 • E and 3-8 km of altitude at 66 • N). The model demonstrated that the contribution from East Asia to the Arctic had a maximum at about 5 km of altitude due to uplifting during long-range transport in early spring. The efficiency of BC transport from East Asia to the Arctic was lower than that from other large source regions such as Europe, Russia, and North America. However, the East Asian contribution was the most important for BC in the middle troposphere (41 %) and the BC burden over the Arctic (27 %) because of the large emissions from this region. These results suggested that the main sources of Arctic BC differed with altitude. The contribution of all the anthropogenic sources to Arctic BC concentrations near the surface was dominant (90 %) on an annual basis. The contributions of biomass burning in boreal regions (Siberia, Alaska, and Canada) to the annual total BC deposition onto the Arctic were estimated to be 12-15 %, which became the maximum during summer.
Abstract. A long-term, robust observational record of atmospheric black carbon (BC) concentrations at Fukue Island for 2009–2019 was produced by unifying the data from a continuous soot monitoring system (COSMOS) and a Multi-Angle Absorption Photometer (MAAP). This record was then used to analyze emission trends from China. We identified a rapid reduction in BC concentrations of (-5.8±1.5) % yr−1 or −48 % from 2010 to 2018. We concluded that an emission change of (-5.3±0.7) % yr−1, related to changes in China of as much as −4.6 % yr−1, was the main underlying driver. This evaluation was made after correcting for the interannual meteorological variability (IAV) by using the regional atmospheric chemistry model simulations from the Weather Research and Forecasting (WRF) and Community Multiscale Air Quality (CMAQ) models (collectively WRF/CMAQ) with the constant emissions. This resolves the current fundamental disagreements about the sign of the BC emissions trend from China over the past decade as assessed from bottom-up emission inventories. Our analysis supports inventories reflecting the governmental clean air actions after 2010 (e.g., MEIC1.3, ECLIPSE versions 5a and 6b, and the Regional Emission inventory in ASia (REAS) version 3.1) and recommends revisions to those that do not (e.g., Community Emissions Data System – CEDS). Our estimated emission trends were fairly uniform across seasons but diverse among air mass origins. Stronger BC reductions, accompanied by a reduction in carbon monoxide (CO) emissions, occurred in regions of south-central East China, while weaker BC reductions occurred in north-central East China and northeastern China. Prior to 2017, the BC and CO emissions trends were both unexpectedly positive in northeastern China during winter months, which possibly influenced the climate at higher latitudes. The pace of the estimated emissions reduction over China surpasses the Shared Socioeconomic Pathways (SSPs with reference to SSP1, specifically) scenarios for 2015–2030, which suggests highly successful emission control policies. At Fukue Island, the BC fraction of fine particulate matter (PM2.5) also steadily decreased over the last decade. This suggests that reductions in BC emissions started without significant delay when compared to other pollutants such as NOx and SO2, which are among the key precursors of scattering PM2.5.
The contribution from several source regions in East Asia to PM2.5 concentration at Fukue Island, a remote island located in the western part of Japan and close to the Asian continent, is estimated using a three-dimensional chemical transport model. The model results suggest that PM2.5 that is attributed to foreign anthropogenic sources have a larger contribution than that of domestic pollution and have a substantial impact on attainment of the atmospheric environmental standard of Japan at Fukue Island.
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