Advanced insights into biomass burning aerosols during the 2023 Canadian wildfires from dual-site Raman and fluorescence lidar observations

IF 5.7 1区 地球科学 Q1 ENVIRONMENTAL SCIENCES
Qiaoyun Hu,Philippe Goloub,Igor Veselovskii,Thierry Podvin,Gaël Dubois,Sergey Khaykin,William Boissière,Fabrice Ducos,Mikhail Korenskiy
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Abstract

Wildfires, as a major source of aerosols, affect air quality and climate at regional and global scales. Fluorescence lidar is a promising technique for characterizing biomass burning aerosols (BBAs) from wildfires, as it detects signals from fluorescent organic compounds in BBAs in addition to elastic and Raman backscatter. However, published fluorescence lidar studies on BBAs remain largely limited to sparse single-site case studies, hindering the development of the technique and a systematic characterization of BBA properties. This study presents dual-site observations of transported BBAs from the exceptional 2023 Canadian wildfires, recorded between May and September at the ATOLL observatory (France) and the GPI site (Russia). ATOLL operates a multi-wavelength Raman lidar with one fluorescence channel at 466 nm; GPI operates a five-channel broadband fluorescence lidar excited at 355 nm. This dual-site dataset combines elastic, depolarization, and fluorescence observations in free troposphere (FT) and upper troposphere–lower stratosphere (UTLS). Compared with FT layers, UTLS layers exhibit higher depolarization, slightly lower lidar ratios, lower Ångström exponents, and a redshift in fluorescence spectral peaks. Cross-site comparisons reveal consistent fluorescence magnitudes and spectral shapes. Depolarization ratio, Ångström exponent, and fluorescence color ratio are moderately correlated with altitude ( r 2 ≈0.61–0.68), although altitude likely acts as an intermediate variable governed by plume injection height, in-layer temperature, and plume origin. Finally, the near-absence of hygroscopic growth at RH of 90 %–100 % challenges the assumption that aged BBAs are typically hygroscopic, suggesting their water uptake properties may be more complex than currently represented in climate models.
通过双站点拉曼和荧光激光雷达观测,深入了解2023年加拿大野火期间生物质燃烧气溶胶
野火是气溶胶的主要来源,在区域和全球范围内影响空气质量和气候。荧光激光雷达是表征野火中生物质燃烧气溶胶(BBAs)的一种很有前途的技术,因为它可以检测到BBAs中荧光有机化合物的信号以及弹性和拉曼反向散射。然而,BBA荧光激光雷达研究发表在很大程度上仍局限于稀疏的单案例研究,阻碍发展的技术和系统描述BBA属性。本研究介绍了在5月至9月期间在法国ATOLL天文台和俄罗斯GPI站点记录的2023年加拿大特殊野火中传输的BBAs的双站点观测结果。ATOLL操作一个多波长拉曼激光雷达,在466 nm处有一个荧光通道;GPI操作一个五通道宽带荧光激光雷达,激发波长为355nm。该双站点数据集结合了自由对流层(FT)和对流层上层-平流层下层(UTLS)的弹性、去极化和荧光观测。与FT层相比,UTLS层具有更高的去极化、略低的激光雷达比、更低的Ångström指数和荧光光谱峰的红移。跨点比较显示一致的荧光强度和光谱形状。退极化比、Ångström指数和荧光色比与海拔高度有一定的相关性(r2≈0.61-0.68),海拔高度可能作为一个中间变量,受羽流注入高度、层内温度和羽流起源的控制。最后,在相对湿度为90% - 100%时几乎没有吸湿性生长,这挑战了陈年BBAs典型吸湿性的假设,表明它们的吸水特性可能比目前气候模型中所代表的更为复杂。
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来源期刊
Atmospheric Chemistry and Physics
Atmospheric Chemistry and Physics 地学-气象与大气科学
CiteScore
10.70
自引率
20.60%
发文量
702
审稿时长
6 months
期刊介绍: Atmospheric Chemistry and Physics (ACP) is a not-for-profit international scientific journal dedicated to the publication and public discussion of high-quality studies investigating the Earth''s atmosphere and the underlying chemical and physical processes. It covers the altitude range from the land and ocean surface up to the turbopause, including the troposphere, stratosphere, and mesosphere. The main subject areas comprise atmospheric modelling, field measurements, remote sensing, and laboratory studies of gases, aerosols, clouds and precipitation, isotopes, radiation, dynamics, biosphere interactions, and hydrosphere interactions. The journal scope is focused on studies with general implications for atmospheric science rather than investigations that are primarily of local or technical interest.
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