Abstract. This paper presents a first comprehensive analysis of long-term measurements of atmospheric aerosol components from Aerosol Chemical Speciation Monitor (ACSM) and multi-wavelength Aethalometer (AE33) instruments collected between 2015 and 2021 at 13 (sub)urban sites as part of the French CARA program. The datasets contain the mass concentrations of major chemical species within PM₁, namely organic aerosols (OA), nitrate (NO₃^-), ammonium (NH₄⁺), sulfate (SO₄^2-), non-sea-salt chloride (Cl^-), and equivalent black carbon (eBC). Rigorous quality control, technical validation, and environmental evaluation processes were applied, adhering to both the guidance from the French reference laboratory for air quality monitoring and the Aerosol, Clouds, and Trace gases Research Infrastructure (ACTRIS) standard operating procedures. Key findings include geographical differences in aerosol chemical composition, seasonal variations, and diel patterns, which are influenced by meteorological conditions, anthropogenic activities, and proximity to emission sources. Overall, OA dominates PM₁ at each site (43–60 %), showing distinct seasonality with higher concentrations (i) in winter, due to enhanced residential heating emissions, and (ii) in summer, due to increased photochemistry favoring secondary aerosol formation. NO₃ is the second most important contributor to PM₁ (15–30 %), peaking in late winter and early spring, especially in northern France, and playing a significant role during pollution episodes. SO₄ (8–14 %) and eBC (5–11 %) complement the major fine aerosol species, with their relative contributions strongly influenced by the origin of air masses and the stability of meteorological conditions, respectively. Such chemically-speciated multi-year datasets have significant value for the scientific community, offering opportunities for future research, including source apportionment studies, trend analyses, and epidemiological investigations. They are also vital for evaluating and validating regional air quality models. In this regard, a comparison with the CHIMERE Chemical Transport Model shows high correlations between simulations and measurements, albeit underestimating OA concentrations by 46–76 %. Regional discrepancies in NO₃ concentration levels emphasize the importance of these datasets in validating air quality models and tailoring air pollution mitigation strategies.

中文翻译：

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法国运营网络（CARA 计划）13 个地点的细颗粒物的多年高时间分辨率测量：数据处理和化学成分

摘要。本文首次全面分析了 2015 年至 2021 年间在法国 13 个（郊区）城市站点收集的气溶胶化学形态监测仪 (ACSM) 和多波长空气浓度计 (AE33) 仪器对大气气溶胶成分的长期测量结果。卡拉计划。数据集包含 PM ₁中主要化学物质的质量浓度，即有机气溶胶 (OA)、硝酸盐 (NO ₃ ^- )、铵 (NH ₄ ⁺ )、硫酸盐 (SO ₄ ^2- )、非海盐氯化物 ( Cl ^- ) 和等效黑炭 (eBC)。采用严格的质量控制、技术验证和环境评估流程，遵循法国空气质量监测参考实验室的指导以及气溶胶、云和微量气体研究基础设施 (ACTRIS) 标准操作程序。主要发现包括气溶胶化学成分、季节变化和昼夜模式的地理差异，这些差异受到气象条件、人类活动和与排放源的接近程度的影响。总体而言，OA 在每个地点的 PM ₁中占主导地位(43-60%)，表现出明显的季节性，浓度较高 (i) 冬季，由于住宅供暖排放增加；(ii) 夏季，由于光化学作用增强，有利于二次气溶胶形成。 NO _{3是 PM 1}的第二重要贡献者(15-30%)，在冬末和早春达到峰值，尤其是在法国北部，并在污染事件期间发挥着重要作用。 SO ₄ (8–14%) 和 eBC (5–11%) 补充了主要的细气溶胶种类，它们的相对贡献分别受到气团起源和气象条件稳定性的强烈影响。这种化学成分多年的数据集对科学界具有重要价值，为未来的研究提供了机会，包括来源解析研究、趋势分析和流行病学调查。它们对于评估和验证区域空气质量模型也至关重要。在这方面，与 CHIMERE 化学传递模型的比较显示模拟和测量之间具有高度相关性，尽管低估了 OA 浓度 46-76%。 NO ₃浓度水平的区域差异强调了这些数据集在验证空气质量模型和制定空气污染缓解策略方面的重要性。