Evolution of the chemical fingerprint of biomass burning organic aerosol during aging

Bertrand, Amélie; Stefenelli, Giulia; Jen, Coty N.; Pieber, Simone M.; Bruns, Emily A.; Temime-Roussel, Brice; Slowik, Jay G.; Goldstein, Allen H.; Haddad, Imad El; Baltensperger, Urs; Prévôt, Andrê S. H.; Wortham, Henri; Marchand, Nicolas

doi:10.5194/acp-2017-1196

Cited by 9 publications

(12 citation statements)

References 47 publications

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“…The O/C increase also agrees with the rapid changes by photochemical oxidation of wood fire in chamber experiments (41), and the results were incorporated in the 2D volatility basis set (42). Finally, recent studies (43, 44) report that nitroaromatic compounds, a marker for ONC, increased in various BB smokes upon aging, which is consistent with our results.…”

Section: Resultssupporting

confidence: 93%

Spherical tarball particles form through rapid chemical and physical changes of organic matter in biomass-burning smoke

Adachi

Sedlacek

Kleinman

et al. 2019

Proc. Natl. Acad. Sci. U.S.A.

101

117

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Biomass burning (BB) emits enormous amounts of aerosol particles and gases into the atmosphere and thereby significantly influences regional air quality and global climate. A dominant particle type from BB is spherical organic aerosol particles commonly referred to as tarballs. Currently, tarballs can only be identified, using microscopy, from their uniquely spherical shapes following impaction onto a grid. Despite their abundance and potential significance for climate, many unanswered questions related to their formation, emission inventory, removal processes, and optical properties still remain. Here, we report analysis that supports tarball formation in which primary organic particles undergo chemical and physical processing within ∼3 h of emission. Transmission electron microscopy analysis reveals that the number fractions of tarballs and the ratios of N and O relative to K, the latter a conserved tracer, increase with particle age and that the more-spherical particles on the substrates had higher ratios of N and O relative to K. Scanning transmission X-ray spectrometry and electron energy loss spectrometry analyses show that these chemical changes are accompanied by the formation of organic compounds that contain nitrogen and carboxylic acid. The results imply that the chemical changes increase the particle sphericity on the substrates, which correlates with particle surface tension and viscosity, and contribute to tarball formation during aging in BB smoke. These findings will enable models to better partition tarball contributions to BB radiative forcing and, in so doing, better help constrain radiative forcing models of BB events.

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Section: Resultssupporting

confidence: 93%

Spherical tarball particles form through rapid chemical and physical changes of organic matter in biomass-burning smoke

Adachi

Sedlacek

Kleinman

et al. 2019

Proc. Natl. Acad. Sci. U.S.A.

101

117

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“…Fresh BB emissions can be quickly photochemically aged (in several hours), resulting in formation of the new OA with higher degree of oxygenation and a significant decrease of BB tracers as well as saturated hydrocarbon compounds. This has been observed in both laboratory (Bertrand et al, 2017;Bertrand et al, 2018;Grieshop et al, 2009a;Grieshop et al, 2009b) and 15 field measurements (Capes et al, 2008;DeCarlo et al, 2010). During the Polarstern cruises, the BB tracers in aPOA factor decayed severely, possibly due to the chemical aging in long-range (i.e.…”

Section: Aged Primary Organic Aerosol (Apoa)mentioning

confidence: 63%

Source apportionment of the submicron organic aerosols over the Atlantic Ocean from 53° N to 53° S using HR-ToF-AMS

Huang

Poulain

et al. 2018

Preprint

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PM1 filter samples with a sampling time of 24 hours. Our measurements show that the MBL aerosol particle mass is controlled by sulfate (50%), followed by organics (21%), sea salt (12%), ammonium (9%), Black Carbon (BC, 5%) and nitrate (3%). Only sulfate exhibits pronouncedly seasonal dependency, while no such trend was observed in other species.Source apportionment of the organic fraction was performed using Positive Matrix Factorization (PMF). Five factors were 20 identified, including three marine sources and two non-marine sources. Marine sources are linked to primary production (19% of total organic aerosol (OA) mass), marine dimethylsulfide (DMS)-oxidation (16%), and amine-related secondary formation (16%). The other two OA components are attributed to continental outflow (19%) and aged ship exhausts -biomass burning emissions (30%). Our study indicates that, on average, non-marine sources nearly have the equal importance to the Atlantic aerosols comparing with the marine sources, respectively contributing 49% and 51% to the total OA mass loadings. The 25 South Atlantic atmosphere is found to be less polluted than the North according to our source analysis. Detailed latitudinal distribution of OA sources showed that DMS oxidation contributes remarkably to the MBL aerosol over the South Atlantic during spring, while continental pollutants largely contaminate the marine atmosphere when near the west and middle Africa (15°N~15°S) as well as Europe. Based on our measurements, SOA produced from DMS oxidation over the Atlantic can be estimated as MSA mass concentration times a scaling factor 1.79 for spring season, which is derived from the strong 30 correlation (R 2 >0.85) between MSA and DMS-oxidation OA component.Atmos. Chem. Phys. Discuss., https://doi

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“…Biomass burning smoke is a significant source of primary and secondary atmospheric particles that have impacts on climate (Bond et al, ), air quality (e.g., Jaffe & Wigder, ; Nie et al, ; Xie et al, ), and health (e.g., Jassen et al, ; Johnston et al, ; Naeher et al, ; Zhang et al, ). Biomass burning emits primary carbonaceous aerosol (both as black carbon and primary organic aerosol; POA; Akagi et al, ; Reid, Koppmann, et al, , and references therein), inorganic aerosol, and vapors, where some vapors may serve as aerosol precursors (e.g., Alvarado & Prinn, ; Bertrand et al, ; Hatch et al, ; Jen et al, ). Biomass burning particle emissions are dominated by an accumulation mode, with a less‐concentrated coarse mode and occasionally a nucleation mode (Reid, Koppmann, et al, ).…”

Section: Introductionmentioning

confidence: 99%

More Than Emissions and Chemistry: Fire Size, Dilution, and Background Aerosol Also Greatly Influence Near‐Field Biomass Burning Aerosol Aging

et al. 2019

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Biomass burning emits particles (black carbon and primary organic aerosol) and precursor vapors to the atmosphere that chemically and physically age in the atmosphere. This theoretical study explores the relationships between fire size (determining the initial plume width and concentration), dilution rate, and entrainment of background aerosol on particle coagulation, organic aerosol (OA) evaporation, and secondary organic aerosol (SOA) condensation in smoke plumes. We examine the impacts of these processes on aged smoke OA mass, geometric mean diameter (Dg), peak lognormal modal width (σg), particle extinction (E), and cloud condensation nuclei (CCN) concentrations. In our simulations, aging OA mass is controlled by competition between OA evaporation and SOA condensation. Large, slowly diluting plumes evaporate little in our base set of simulations, which may allow for net increases in mass, E, CCN , and Dg from SOA condensation. Smaller, quickly diluting fire plumes lead to faster evaporation, which favors decreases in mass, E, CCN, and Dg. However, the SOA fraction of the smoke OA increases more rapidly in smaller fires due to faster primary organic aerosol evaporation leading to more SOA precursors. Net mass changes for smaller fires depend on background OA concentrations; increasing background aerosol concentrations decrease evaporation rates. Although coagulation does not change mass, it can decrease the number of particles in large/slowly diluting plumes, increasing Dg and E, and decreasing σg. While our conclusions are limited by being a theoretical study, we hope they help motivate future smoke‐plume analyses to consider the effects of fire size, meteorology, and background OA concentrations.

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Evolution of the chemical fingerprint of biomass burning organic aerosol during aging

Cited by 9 publications

References 47 publications

Spherical tarball particles form through rapid chemical and physical changes of organic matter in biomass-burning smoke

Spherical tarball particles form through rapid chemical and physical changes of organic matter in biomass-burning smoke

Source apportionment of the submicron organic aerosols over the Atlantic Ocean from 53° N to 53° S using HR-ToF-AMS

More Than Emissions and Chemistry: Fire Size, Dilution, and Background Aerosol Also Greatly Influence Near‐Field Biomass Burning Aerosol Aging

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