Comprehensive mass spectrometric analysis of unprecedented high levels of carbonaceous aerosol particles long-range transported from wildfires in the Siberian Arcticстатья
Аннотация:Wildfires in Siberia generate large amounts of aerosols, which may be transported over long distances and pose a18
threat to the sensitive ecosystem of the Arctic. Particulate matter (PM) of aged wildfire plumes with origin from19
Yakutia in August 2021 was collected in Nadym city and on Bely Island (both northwest Siberia). A20
comprehensive analysis of the chemical composition of aerosol particles was conducted by multi-wavelength21
thermal-optical carbon analyzer (TOCA) coupled to resonance-enhanced multiphoton ionization time-of-flight22
mass spectrometry (REMPI-TOFMS) as well as by ultra-high resolution Fourier-transform ion cyclotron23
resonance mass spectrometry (FT-ICR MS). In Nadym city, concentrations of organic carbon (OC) and elemental24
carbon (EC) were peaking at 100 μg m-3 and 40 μg m-3, respectively, associated with Angström Absorption25
Exponents for 405 and 808 nm (AAE405/808) between 1.5 and 3.3. The weekly average on Bely Island peaked at26
8.9 μg m-3 of OC and 0.3 μg m-3 of EC, and AAE405/808 close to unity. Particularly, ambient aerosol in Nadym city27
had a distinct biomass burning profile with pyrolysis products from carbohydrates, such as cellulose and hemi-28
cellulose, as well as lignin and resinoic acids. However, temporarily higher concentrations of 5- and 6-ring29
polycyclic aromatic hydrocarbons (PAHs), different from the PAH signature of biomass burning, suggests a30
contribution of regional gas flaring. FT-ICR MS with electrospray ionization (ESI) revealed a complex mixture of31
highly functionalized compounds, containing up to twenty oxygen atoms, as well as nitrogen- and sulfur-32
containing moieties. Concentrations of biomass burning markers on Bely Island were substantially lower than in33
Nadym city, flanked by appearance of unique compounds with higher oxygen content, higher molecular weight34
and lower aromaticity. Back trajectory analysis and satellite-derived aerosol optical depth suggested long-range35
transport of aerosol from the center of a Yakutian wildfire plume to Nadym city and the plume periphery to Bely36
Island. Owing to lower aerosol concentration in the plume periphery than in its center, it is demonstrated how37
dilution affects the chemical plume composition during atmospheric aging