Biomass burning (BB) is a large source of primary and secondary organic aerosols (POA and SOA). This study addresses the physical and chemical evolution of BB organic aerosols. Firstly, the evolution and lifetime of BB POA and SOA signatures observed with the Aerodyne Aerosol Mass Spectrometer are investigated, focusing on measurements at high-latitudes acquired during the 2008 NASA ARCTAS mission, in comparison to data from other field studies and from laboratory aging experiments. The parameter <i>f</i><sub>60</sub>, the ratio of the integrated signal at <i>m/z</i> 60 to the total signal in the organic component mass spectrum, is used as a marker to study the rate of oxidation and fate of the BB POA. A background level of <i>f</i><sub>60</sub>~0.3% ± 0.06% for SOA-dominated ambient OA is shown to be an appropriate background level for this tracer. Using also <i>f</i><sub>44</sub> as a tracer for SOA and aged POA and a surrogate of organic O:C, a novel graphical method is presented to characterise the aging of BB plumes. Similar trends of decreasing <i>f</i><sub>60</sub> and increasing <i>f</i><sub>44</sub> with aging are observed in most field and lab studies. At least some very aged BB plumes retain a clear <i>f</i><sub>60</sub> signature. A statistically significant difference in <i>f</i><sub>60</sub> between highly-oxygenated OA of BB and non-BB origin is observed using this tracer, consistent with a substantial contribution of BBOA to the springtime Arctic aerosol burden in 2008. Secondly, a summary is presented of results on the net enhancement of OA with aging of BB plumes, which shows large variability. The estimates of net OA gain range from ΔOA/ΔCO(mass) = −0.01 to ~0.05, with a mean ΔOA/POA ~19%. With these ratios and global inventories of BB CO and POA a global net OA source due to aging of BB plumes of ~8 ± 7 Tg OA yr<sup>−1</sup> is estimated, of the order of 5 % of recent total OA source estimates. Further field data following BB plume advection should be a focus of future research in order to better constrain this potentially important contribution to the OA burden
Biomass burning (BB) is a large source of primary and secondary organic aerosols (POA and SOA). This study addresses the physical and chemical evolution of BB organic aerosols. Firstly, the evolution and lifetime of BB POA and SOA signatures observed with the Aerodyne Aerosol Mass Spectrometer are investigated, focusing on measurements at high-latitudes acquired during the 2008 NASA ARCTAS mission, in comparison to data from other field studies and from laboratory aging experiments. The parameter <i>f</i><sub>60</sub>, the ratio of the integrated signal at <i>m/z</i> 60 to the total signal in the organic component mass spectrum, is used as a marker to study the rate of oxidation and fate of the BB POA. A background level of <i>f</i><sub>60</sub>~0.3% ±0.06% for SOA-dominated ambient OA is shown to be an appropriate background level for this tracer. Using also <i>f</i><sub>44</sub> as a tracer for SOA and aged POA, a novel graphical method is presented to characterise the aging of BB plumes. Similar trends of decreasing <i>f</i><sub>60</sub> and increasing <i>f</i><sub>44</sub> with aging are observed in most field and lab studies. At least some very aged BB plumes retain a clear <i>f</i><sub>60</sub> signature. A statistically significant difference in <i>f</i><sub>60</sub> between highly-oxygenated OA of BB and non-BB origin is observed using this tracer, consistent with a substantial contribution of BBOA to the springtime Arctic aerosol burden in 2008. Secondly, a summary is presented of results on the net enhancement of OA with aging of BB plumes, which shows large variability. The estimates of net OA gain range from ΔOA/ΔCO(mass) =−0.01 to ~0.07, with a mean ΔOA/POA ~25%. With these ratios and global inventories of BB CO and POA a global net OA source due to aging of BB plumes of ~9 Tg OA yr<sup>−1</sup> is estimated, of the order of 5% of recent total OA source estimates. Further field data following BB plume advection should be a focus of future research in order to better constrain this potentially important contribution to the OA burden
[1] Airborne Multi-AXis Differential Optical Absorption Spectroscopy (AMAX-DOAS) measurements of NO 2 tropospheric vertical columns were performed over California for two months in summer 2010. The observations are compared to the NASA Ozone Monitoring Instrument (OMI) tropospheric vertical columns (data product v2.1) in two ways: (1) Median data were compared for the whole time period for selected boxes, and the agreement was found to be fair (R = 0.97, slope = 1.4 ± 0.1, N = 10). (2) A comparison was performed on the mean of coincident AMAX-DOAS measurements within the area of the corresponding OMI pixels with the tropospheric NASA OMI NO 2 assigned to that pixel. The effects of different data filters were assessed. Excellent agreement and a strong correlation (R = 0.85, slope = 1.05 ± 0.09, N = 56) was found for (2) when the data were filtered to eliminate large pixels near the edge of the OMI orbit, the cloud radiance fraction was <50%, the OMI overpass occurred within 2 h of the AMAX-DOAS measurements, the flight altitude was >2 km, and a representative sample of the footprint was taken by the AMAX-DOAS instrument. The AMAX-DOAS and OMI data sets both show a reduction of NO 2 tropospheric columns on weekends by 38 ± 24% and 33 ± 11%, respectively. The assumptions in the tropospheric satellite air mass factor simulations were tested using independent measurements of surface albedo, aerosol extinction, and NO 2 profiles for Los Angeles for July 2010 indicating an uncertainty of 12%.
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