The impact of atmospheric motions on source-specific black carbon and the induced direct radiative effects over a river-valley region

Abstract

Black carbon (BC) is one of the most important short-lived climate forcers, and atmospheric motions play an important role in determining its mass concentrations of pollutants. Here an intensive observation was launched in a typical river-valley city to investigate relationships between atmospheric motions and BC aerosols. Equivalent BC (eBC) source apportionment was based on an aethalometer model with the site-dependent absorption Ångström exponents (AAEs) and the mass absorption cross sections (MACs) retrieved using a positive matrix factorization (PMF) model based on observed chemical components (i.e., EC, POC, K+, Mg, Al, Si, S, Cl, Ca, V, Mn, Fe, Ni, Cu, As, Se, Br, Sr, Pb, Ga, and Zn) and primary absorption coefficients at selected wavelengths from λ=370 to 880 nm. The derived AAEs from 370 to 880 nm were 1.07 for diesel vehicular emissions, 2.13 for biomass burning, 1.74 for coal combustion, and 1.78 for mineral dust. The mean values for eBCfossil and eBCbiomass were 2.46 and 1.17 µg m−3, respectively. Wind run distances and the vector displacements of the wind in 24 h were used to construct a self-organizing map, from which four atmospheric motion categories were identified (local-scale dominant, local-scale strong and regional-scale weak, local-scale weak and regional-scale strong, and regional-scale dominant). BC pollution was found to be more likely when the influence of local-scale motions outweighed that of regional-scale motions. Cluster analysis for the back-trajectories of air mass calculated by the Hybrid Single-Particle Lagrangian Integrated Trajectory model at the study site indicated that the directions of air flow can have different impacts for different scales of motion. The direct radiative effects (DREs) of source-specific eBC were lower when the influence of regional-scale motions outweighed that of the local ones. However, due to chemical aging of the particles during transport – the DRE efficiencies under regional-scale motions were ∼ 1.5 times higher than those under more local influences. The finding that the DRE efficiency of BC increased during the regional transport suggested significant consequences in regions downwind of pollution sources and emphasizes the importance of regionally transported BC for potential climatic effects.