Long-term Variation of Absorption and Total Aerosol Optical Properties over Typical Provinces of China from Satellite Observations

Increase of atmospheric aerosols has a profound impact on the Earth’s climate. It’s also one of the crucial factors that cuasesd more fequent air pollution events in China. Monthly average Aerosol Optical Depth (AOD) from MODIS and UltraViolet Absorbing aerosol Index (UVAI) from OMI during 2011 to 2019 are used to analyse the trend of absorption and total aerosol optical properties over three typical provinces of China, namely Shandong, Gansu and Guangdong provinces. The results show the average annual AOD of the three provinces are all decreasing while UVAI rises during this period. In addition, the monthly variation of AOD and UVAI are also obviously different over these provinces. In particular, the peak value of AOD appeared in July and the trough appeared in December over Shandong Province. And the peak appeared in April over Gansu Province, but AOD decrease slower then over Shandong Province. And there were two peaks in April and August over Guangdong Province. For UVAI, the peaks over Shandong and Gansu provinces both occur in January, while that over Guangdong Province appears in March. Above mentioned differences in the long-term trend and monthly variation of AOD and UVAI might be closely related to the meteorological conditions and aerosol emission of these three provinces.

Look−up tables resolved by complex refractive index to correct particle sizes measured by common research−grade optical particle counters

Optical particle counters (OPC) are widely used to measure the aerosol particle number size distribution at atmospheric ambient conditions and over a large size range. Their measurement principle is based on the dependence of light scattering on particle size. However, this dependence is not monotonic at all sizes and light scattering also depends on the particle composition (i.e., the complex refractive index, CRI) and morphology. Therefore, the conversion of the measured scattered intensity to the desired particle size depends on the microphysical properties of the sampled aerosol population and might not be unique at all sizes. While these complexities have been addressed before, corrections are typically applied ad-hoc and are not standardised. This paper addresses this issue by providing a consistent and extended database of pre−computed correction factors for a wide range of complex refractive index values representing the composition variability of atmospheric aerosols. These correction factors are calculated for five different commercial OPCs (USHAS, PCASP, FSSP, GRIMM and its airborne version Sky− GRIMM, CDP) by assuming Mie theory for homogeneous spherical particles, and by varying the real part of the CRI between 1.33 and 1.75 in steps of 0.01 and the imaginary part between 0.0 and 0.4 in steps of 0.001. Correction factors for mineral dust are provided at the CRI of 1.53 – 0.003i and account for the asphericity of these particles. The datasets described in this paper are distributed at open-access repository: https://doi.org/10.25326/234 (license CC BY, Formenti et al., 2021) maintained by the French national center for Atmospheric data and services AERIS to data users/geophysicists who number size distribution measurements from OPC for their research on atmospheric aerosols. Application and caveats of the CRI-corrections factors are presented and discussed. The dataset presented in this paper is not only useful for correcting the size distribution from an OPC when the particle refractive index is known, but even when only assumptions can be made. Furthermore, this dataset can be useful in calculating uncertainties or sensitivities of aerosol volume/mass/extinction from OPCs given no or limited knowledge of refractive index.

Chemical Transformation of α-Pinene derived Organosulfate via Heterogeneous OH Oxidation: Implications for Sources and Environmental Fates of Atmospheric Organosulfates

Organosulfur compounds are found to be ubiquitous in atmospheric aerosols — a majority of which are expected to be organosulfates (OSs). Given the atmospheric abundance of OSs, and their potential to form a variety of reaction products upon ageing, it is imperative to study the transformation kinetics and chemistry of OSs to better elucidate their atmospheric fates and impacts. In this work, we investigated the chemical transformation of an α-pinene derived organosulfate (C10H17O5SNa, αpOS-249) through heterogeneous OH oxidation at a relative humidity of 50 % in an oxidation flow reactor (OFR). The aerosol-phase reaction products were characterized using the high-performance liquid chromatography-electrospray ionization-high resolution mass spectrometry and the ion chromatography. By monitoring the decay rates of αpOS-249, the effective heterogeneous OH reaction rate was measured to be (6.72 ± 0.55) × 10−13 cm3 molecule−1 s−1. This infers an atmospheric lifetime of about two weeks at an average OH concentration of 1.5 × 106 molecules cm–3. Product analysis shows that OH oxidation of αpOS-249 can yield more oxygenated OSs having a nominal mass-to-charge ratio (m/z) at 247 (C10H15O5S−), 263 (C10H15O6S−), 265 (C10H17O6S−), 277 (C10H13O7S−), 279 (C10H15O7S−), and 281 (C10H17O7S−). The formation of fragmentation products, including both small OSs (C < 10) and inorganic sulfates, is found to be insignificant. These observations suggest that functionalization reactions are likely the dominant processes and that multigenerational oxidation possibly leads to formation of products with one or two hydroxyl and carbonyl functional groups adding to αpOS-249. Furthermore, all product ions except m/z = 277 have been detected in laboratory generated α-pinene derived secondary organic aerosols as well as in atmospheric aerosols. Our results reveal that OSs freshly formed from the photochemical oxidation of α-pinene could react further to form OSs commonly detected in atmospheric aerosols through heterogeneous OH oxidation. Overall, this study provides more insights into the sources, transformation, and fate of atmospheric OSs.

High latitude vegetation changes will determine future plant volatile impacts on atmospheric organic aerosols

Strong, ongoing high latitude-warming is causing changes to vegetation composition and plant productivity, modifying plant emissions of Biogenic Volatile Organic Compounds (BVOCs). In the sparsely populated high latitudes, climatic feedbacks resulting from BVOCs as precursors of atmospheric aerosols could be more important than elsewhere on the globe. Here, we quantitatively assess the linkages between vegetation changes, BVOC emissions and secondary organic aerosol (SOA) under different climate scenarios and show that warming-induced vegetation changes determine the spatial patterns of BVOC impacts on SOA. The northward advances of boreal needle-leaved trees and shrubs result in an increase of up to 45% in regional SOA optical depth, causing a cooling feedback. In contrast, areas dominated by temperate broad-leaved trees show a large decline in monoterpene emissions and SOA formation, causing a warming feedback. We highlight the necessity of considering vegetation shifts when assessing radiative feedbacks on climate following the BVOC-SOA pathway.