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上海冬春季含碳气溶胶消光特征及其及其演化

Light extinction characteristics and evolution of carbonaceous aerosols in Shanghai during winter and spring

  • 摘要: 上海冬春季气溶胶整体表现为散射主导特征,但短波段存在显著额外吸收,吸收波长指数(Absorption ?ngstr?m Exponent ,AAE)呈现AAE370-520 nm> AAE370-880 nm> AAE520-880 nm的光谱分布特征,证实棕碳(brown carbon ,BrC)在区域大气中的持续存在。剥离BrC影响后的黑碳(black carbon ,BC)吸收系数与其质量浓度具有更高相关性,表明改进AAE算法能够有效实现BC与BrC吸收分离。观测期间散射与吸收系数均呈现明显日变化,主要受交通排放及边界层演变共同控制;午后BrC吸收贡献相对增强,反映出光化学过程促进了二次有机发色团生成。总消光分析显示,二次无机盐累积是冬季高污染期间能见度恶化的主导因素,而春季散射性组分快速清除则导致BC相对吸收贡献增强。进一步分析发现,在高 AAE 条件下,BrC 的质量吸收截面(MAC)在午后明显下降,表现出典型的光漂白特征;然而,BC 的质量吸收截面在两季均保持相对稳定,不同 AAE 组之间未观察到一致的日间增强现象。这表明 BC 的吸收增强不仅受二次组分包覆影响,还受到颗粒老化程度、包覆结构及边界层演变等复杂因素的共同制约。

     

    Abstract: The aerosols in Shanghai during winter and spring generally exhibited scattering-dominated characteristics, although significant additional absorption was observed in the shortwave band. The Absorption ?ngstr?m Exponent (AAE) presented a spectral distribution of AAE370-520 nm > AAE370-880 nm > AAE520-880 nm, confirming the continuous presence of brown carbon (BrC) in the regional atmosphere. The segregated black carbon (BC) absorption showed a higher correlation with BC mass concentration, indicating that the improved AAE algorithm can effectively separate BC and BrC absorption. During the observation period, both scattering and absorption coefficients demonstrated distinct diurnal variations, which were primarily co-controlled by traffic emissions and boundary layer evolution. The relative contribution of BrC absorption increased in the afternoon, reflecting the promotion of secondary organic chromophore formation by photochemical processes. Total extinction analysis indicated that the accumulation of secondary inorganic salts was the dominant factor driving visibility deterioration during heavy winter pollution, whereas the rapid scavenging of scattering components in spring led to an enhanced relative absorption contribution of BC. Further analysis revealed that under high AAE conditions, the mass absorption cross-section (MAC) of BrC decreased significantly in the afternoon, demonstrating typical photobleaching characteristics. However, the MAC of BC remained relatively stable in both seasons, and no consistent diurnal enhancement was observed across different AAE groups. This suggests that the absorption enhancement of BC is not solely influenced by secondary component coatings, but is mutually constrained by complex factors including the degree of particle aging, coating structure, and boundary layer evolution.

     

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