Chemical and physical transformations of organic aerosol from the photo-oxidation of open biomass burning emissions in an environmental chamber

Hennigan, Christopher J.; Miracolo, Marissa A.; Engelhart, G. J.; May, Andrew A.; Presto, Albert A.; Lee, Taesam; Sullivan, A.; McMeeking, G. R.; Coe, Hugh; Wold, Cyle; Hao, Wei Min; Gilman, J. B.; Kuster, W. C.; Gouw, J. A. de; Schichtel, B. A.; Collett, Jeffrey L.; Kreidenweis, Sonia M.; Robinson, Allen L.

doi:10.5194/acp-11-7669-2011

Cited by 341 publications

(457 citation statements)

References 62 publications

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“…Since the organic/ CO ratio was relatively constant, it is likely the aerosol transformed by: (1) repartitioning of more volatile, less oxygenated organic species to the gas phase following heterogeneous reactions and/or dilution, resulting in a more oxidized organic aerosol (Kroll et al, 2009), as well as (2) condensation of oxidized organics (Donahue et al, 2006), such as dicarboxylic acids, as discussed below. As noted by Capes et al (2008) and Hennigan et al (2011) for similar observations of the aging of biomass burning organic aerosol, the mechanisms must balance one another to keep the organic/ CO ratio constant.…”

Section: Organicsmentioning

confidence: 99%

Flight-based chemical characterization of biomass burning aerosols within two prescribed burn smoke plumes

et al. 2011

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Abstract. Biomass burning represents a major global source of aerosols impacting direct radiative forcing and cloud properties. Thus, the goal of a number of current studies involves developing a better understanding of how the chemical composition and mixing state of biomass burning aerosols evolve during atmospheric aging processes. During the Ice in Clouds Experiment-Layer Clouds (ICE-L) in the fall of 2007, smoke plumes from two small Wyoming Bureau of Land Management prescribed burns were measured by online aerosol instrumentation aboard a C-130 aircraft, providing a detailed chemical characterization of the particles. After ∼2-4 min of aging, submicron smoke particles, produced primarily from sagebrush combustion, consisted predominantly of organics by mass, but were comprised primarily of internal mixtures of organic carbon, elemental carbon, potassium chloride, and potassium sulfate. Significantly, the fresh biomass burning particles contained minor mass fractions of nitrate and sulfate, suggesting that hygroscopic material is incorporated very near or at the point of emission. The mass fractions of ammonium, sulfate, and nitrate increased with aging up to ∼81-88 min and resulted in acidic particles. Decreasing black carbon mass concentrations occurred due to Correspondence to: K. A. Prather (kprather@ucsd.edu) dilution of the plume. Increases in the fraction of oxygenated organic carbon and the presence of dicarboxylic acids, in particular, were observed with aging. Cloud condensation nuclei measurements suggested all particles >100 nm were active at 0.5 % water supersaturation in the smoke plumes, confirming the relatively high hygroscopicity of the freshly emitted particles. For immersion/condensation freezing, ice nuclei measurements at −32 • C suggested activation of ∼0.03-0.07 % of the particles with diameters greater than 500 nm.

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Section: Organicsmentioning

confidence: 99%

Flight-based chemical characterization of biomass burning aerosols within two prescribed burn smoke plumes

et al. 2011

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“…Coagulation is a driving factor in size-distribution evolution due to the high concentrations of particles within plumes (Andreae and Merlet, 2001;Capes et al, 2008). Production of secondary organic aerosol (SOA) in-plume has been observed in chamber studies Grieshop et al, 2009;Hennigan et al, 2011;Heringa et al, 2011;Ortega et al, 2013) and in the field (DeCarlo et al, 2010;Lee et al, 2008;Reid et al, 1998;Yokelson et al, 2009), and this SOA will condense onto the particles, increasing their size. In addition, the primary organic aerosol (POA) emitted by the fires may evaporate during the dilution of the plume (Huffman et al, 2009;May et al, 2013).…”

Section: Biomass-burning Particlesmentioning

confidence: 99%

“…In addition to releasing high levels of greenhouse gases (CO 2 , CO) and volatile organic compounds, biomass burning releases smoke particles that have climate impacts through the direct and indirect aerosol effects. These particles are primarily composed of a mixture of black carbon (BC) and organic carbon (OC), with inorganics contributing some mass (Capes et al, 2008;Carrico et al, 2010;Cubison et al, 2011;Hennigan et al, 2011;Hudson et al, 2004;Reid et al, 2005). These particles directly affect Earth's radiation balance and climate by scattering and absorbing incoming solar radiation (Haywood, 2000;Jacobson, 2001).…”

Section: Biomass-burning Particlesmentioning

confidence: 99%

Aged boreal biomass-burning aerosol size distributions from BORTAS 2011

et al. 2015

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Abstract. Biomass-burning aerosols contribute to aerosol radiative forcing on the climate system. The magnitude of this effect is partially determined by aerosol size distributions, which are functions of source fire characteristics (e.g. fuel type, MCE) and in-plume microphysical processing. The uncertainties in biomass-burning emission number-size distributions in climate model inventories lead to uncertainties in the CCN (cloud condensation nuclei) concentrations and forcing estimates derived from these models.The BORTAS-B (Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellite) measurement campaign was designed to sample boreal biomass-burning outflow over eastern Canada in the summer of 2011. Using these BORTAS-B data, we implement plume criteria to isolate the characteristic size distribution of aged biomass-burning emissions (aged ∼ 1-2 days) from boreal wildfires in northwestern Ontario. The composite median size distribution yields a single dominant accumulation mode with D pm = 230 nm (numbermedian diameter) and σ = 1.5, which are comparable to literature values of other aged plumes of a similar type. The organic aerosol enhancement ratios ( OA / CO) along the path of Flight b622 show values of 0.09-0.17 µg m −3 ppbv −1 (parts per billion by volume) with no significant trend with distance from the source. This lack of enhancement ratio increase/decrease with distance suggests no detectable net OA (organic aerosol) production/evaporation within the aged plume over the sampling period (plume age: 1-2 days), though it does not preclude OA production/loss at earlier stages. A Lagrangian microphysical model was used to determine an estimate of the freshly emitted size distribution corresponding to the BORTAS-B aged size distributions. The model was restricted to coagulation and dilution processes based on the insignificant net OA production/evaporation derived from the OA / CO enhancement ratios. We estimate that the young-plume median diameter was in the range of 59-94 nm with modal widths in the range of 1.7-2.8 (the ranges are due to uncertainty in the entrainment rate). Thus, the size of the freshly emitted particles is relatively unconstrained due to the uncertainties in the plume dilution rates.

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“…Improved projection of climate change impacts through global climate model simulation is dependent on more robust parameterisation of the constituent drivers, constrained by direct measurements. Several fundamental aspects of the BBOA lifecycle remain poorly characterised (Hallquist et al, 2009), including the conditions and processes controlling formation and the effects of transformations occurring during aging, such as gas-particle partitioning of low volatility organic compounds following photo-oxidation, heterogeneous reactions with existing OA and losses through dilution-based evaporation or volatilisation (Reid et al, 2005;Grieshop et al, 2009;Hennigan et al, 2011). Variability at source has been shown to be extensive, in response to changes in both fuel properties and combustion conditions (McMeeking et al, 2009;Jolleys et al, 2012Jolleys et al, , 2014.…”

Section: Introductionmentioning

confidence: 99%

Properties and evolution of biomass burning organic aerosol from Canadian boreal forest fires

et al. 2015

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Abstract. Airborne measurements of biomass burning organic aerosol (BBOA) from boreal forest fires reveal highly contrasting properties for plumes of different ages. These measurements, performed using an Aerodyne Research Inc. compact time-of-flight aerosol mass spectrometer (C-ToF-AMS) during the BORTAS (quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites) experiment in the summer of 2011, have been used to derive normalised excess organic aerosol (OA) mass concentrations ( OA / CO), with higher average ratios observed closer to source (0.190 ± 0.010) than in the far-field (0.097 ± 0.002). The difference in OA / CO between fresh and aged plumes is influenced by a change in dominant combustion conditions throughout the campaign. Measurements at source comprised 3 plume interceptions during a single research flight and sampled largely smouldering fires. Twentythree interceptions were made across four flights in the farfield, with plumes originating from fires occurring earlier in the campaign when fire activity had been more intense, creating an underlying contrast in emissions prior to any transformations associated with aging. Changing combustion conditions also affect the vertical distribution of biomass burning emissions, as aged plumes from more flaming-dominated fires are injected to higher altitudes of up to 6000 m. Proportional contributions of the mass-to-charge ratio (m/z) 60 and 44 peaks in the AMS mass spectra to the total OA mass (denoted f 60 and f 44 ) are used as tracers for primary and oxidised BBOA, respectively. f 44 is lower on average in near-field plumes than those sampled in the far-field, in accordance with longer aging times as plumes are transported a greater distance from source. However, high levels of O 3 / CO and −log(NO x / NO y ) close to source indicate that emissions can be subject to very rapid oxidation over short timescales. Conversely, the lofting of plumes into the upper troposphere can lead to the retention of source profiles after transportation over extensive temporal and spatial scales, with f 60 also higher on average in aged plumes. Evolution of OA composition with aging is comparable to observations of BB tracers in previous studies, revealing a consistent progression from f 60 to f 44 . The elevated levels of oxygenation in aged plumes, and their association with lower average OA / CO, are consistent with OA loss through evaporation during aging due to a combination of dilution and chemical processing, while differences in combustion conditions throughout the campaign also have a significant influence on BBOA production and composition.

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Chemical and physical transformations of organic aerosol from the photo-oxidation of open biomass burning emissions in an environmental chamber

Cited by 341 publications

References 62 publications

Flight-based chemical characterization of biomass burning aerosols within two prescribed burn smoke plumes

Flight-based chemical characterization of biomass burning aerosols within two prescribed burn smoke plumes

Aged boreal biomass-burning aerosol size distributions from BORTAS 2011

Properties and evolution of biomass burning organic aerosol from Canadian boreal forest fires

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