Formaldehyde evolution in US wildfire plumes during the Fire Influence on Regional to Global Environments and Air Quality experiment (FIREX-AQ)

Liao, J.; Wolfe, G. M.; Hannun, Reem A.; Clair, J. M. St; Hanisco, T. F.; Gilman, J. B.; Lamplugh, Aaron; Selimovic, Vanessa; Diskin, G. S.; Nowak, John B.; Halliday, Hannah; DiGangi, J. P.; Hall, Samuel R.; Ullmann, Kirk; Holmes, Christopher D.; Fite, Charles H.; Agastra, Anxhelo; Ryerson, Thomas B.; Peischl, J.; Bourgeois, Ilann; Warneke, C.; Coggon, Matthew M.; Gkatzelis, Georgios I.; Sekimoto, Kanako; Fried, Alan; Richter, Dirk; Weibring, Petter; Apel, E. C.; Hornbrook, R. S.; Brown, Steven S.; Womack, Caroline C.; Robinson, Michael; Washenfelder, R. A.; Veres, P. R.; Neuman, J. A.

doi:10.5194/acp-21-18319-2021

Cited by 40 publications

(33 citation statements)

References 59 publications

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“…Chemical age can be estimated based on known differential reaction rates of species, or the physical age can be estimated. Here we estimate the physical age based on air mass trajectories comprising two components: advection age and plume rise age (Liao et al, 2021). The advection time was estimated by the HYbrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT; Rolph et al, 2017;Stein et al, 2015) from the DC-8 aircraft location relative to the smoke source identified using the MODIS-/ASTER airborne simulator (MASTER; Hook et al, 2001) with multiple high-resolution meteorological datasets, including High-Resolution Rapid Refresh (HRRR), the North American Mesoscale Forecast System (NAM CONUS nest) and the Global Forecast System (GFS).…”

Section: Age Of Smoke Plumesmentioning

confidence: 99%

Characteristics and evolution of brown carbon in western United States wildfires

et al. 2022

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Abstract. Brown carbon (BrC) associated with aerosol particles in western United States wildfires was measured between July and August 2019 aboard the NASA DC-8 research aircraft during the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) study. Two BrC measurement methods are investigated, highly spectrally resolved light absorption in solvent (water and methanol) extracts of particles collected on filters and in situ bulk aerosol particle light absorption measured at three wavelengths (405, 532 and 664 nm) with a photoacoustic spectrometer (PAS). A light-absorption closure analysis for wavelengths between 300 and 700 nm was performed. The combined light absorption of particle pure black carbon material, including enhancements due to internally mixed materials, plus soluble BrC and a Mie-predicted factor for conversion of soluble BrC to aerosol particle BrC, was compared to absorption spectra from a power law fit to the three PAS wavelengths. For the various parameters used, at a wavelength of roughly 400 nm they agreed, at lower wavelengths the individual component-predicted particle light absorption significantly exceeded the PAS and at higher wavelengths the PAS absorption was consistently higher but more variable. Limitations with extrapolation of PAS data to wavelengths below 405 nm and missing BrC species of low solubility that more strongly absorb at higher wavelengths may account for the differences. Based on measurements closest to fires, the emission ratio of PAS-measured BrC at 405 nm relative to carbon monoxide (CO) was on average 0.13 Mm−1 ppbv−1; emission ratios for soluble BrC are also provided. As the smoke moved away from the burning regions, the evolution over time of BrC was observed to be highly complex; BrC enhancement, depletion or constant levels with age were all observed in the first 8 h after emission in different plumes. Within 8 h following emissions, 4-nitrocatechol, a well-characterized BrC chromophore commonly found in smoke particles, was largely depleted relative to the bulk BrC. In a descending plume where temperature increased by 15 K, 4-nitrocatechol dropped, possibly due to temperature-driven evaporation, but bulk BrC remained largely unchanged. Evidence was found for reactions with ozone, or related species, as a pathway for secondary formation of BrC under both low and high oxides of nitrogen (NOx) conditions, while BrC was also observed to be bleached in regions of higher ozone and low NOx, consistent with complex behaviors of BrC observed in laboratory studies. Although the evolution of smoke in the first hours following emission is highly variable, a limited number of measurements of more aged smoke (15 to 30 h) indicate a net loss of BrC. It is yet to be determined how the near-field BrC evolution in smoke affects the characteristics of smoke over longer timescales and spatial scales, where its environmental impacts are likely to be greater.

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Section: Age Of Smoke Plumesmentioning

confidence: 99%

Characteristics and evolution of brown carbon in western United States wildfires

et al. 2022

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Section: Age Of Smoke Plumesmentioning

confidence: 99%

“…4-nitrophenol, 4-nitrocatechol, and their derivatives are now commonly identified BrC species (Bluvshtein et al, 2017;Hems and Abbatt, 2018); other identified chromophores include a range of polycyclic aromatic hydrocarbons (PAHs) derivatives and polyphenols that span wide molecular weights and structures (Lin et al, 2016). Carbonyl functional groups are a common feature of BrC chromophores (Laskin et al, 2015;Lin et al, 2015a;De Haan et al, 2017). Evidence suggests that strongly absorbing chromophores comprise a small mass fraction of OA in biomass burning smoke, but dominate the overall BrC absorption (Nguyen et al, 2012;Laskin et al, 2014).…”

Section: Introductionmentioning

confidence: 99%

“…A fraction of BrC is semi-volatile (Jai Devi et al, 2016) and may be a component of the secondary organic aerosol (SOA). This secondary BrC can be formed from a range of species and processes, such as reactions between aromatic VOCs with ozone (O3) or the hydroxyl (OH) or nitrate (NO3) radicals Jiang et al, 2019;Fan et al, 2020), aqueous reactions involving carbonyl function groups with ammonium sulfate or PAHs with illumination (Nguyen et al, 2012;Haynes et al, 2019), and heterogeneous reactions of isoprene on acidic particles (Limbeck et al, 2003).…”

Section: Introductionmentioning

confidence: 99%

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Characteristics and Evolution of Brown Carbon in Western United States Wildfires

Zeng

Dibb

Scheuer

et al. 2022

Preprint

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Abstract. Brown carbon (BrC) associated with aerosol particles in western United States wildfires was measured between Jul. and Aug. 2019 onboard the NASA DC-8 research aircraft during the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) study. Two BrC measurement methods are investigated; highly spectrally-resolved light absorption in solvent (water and methanol) extracts of particles collected on filters and in-situ bulk aerosol particle light absorption measured at three wavelengths (405, 532, 664 nm) with a photo acoustic spectrometer (PAS). A light absorption closure analysis for wavelengths between 300 and 700 nm was performed. The combined light absorption of particle pure black carbon material, including enhancements due to internally mixed materials, plus soluble BrC and a Mie-predicted factor for conversion of soluble BrC to aerosol particle BrC, was compared to absorption spectra from a power law fit to the three PAS wavelengths. For the various parameters used, at a wavelength of roughly 400 nm they agreed, at lower wavelengths the individual component-predicted particle light absorption significantly exceeded the PAS and at higher wavelengths the PAS absorption was consistently higher, but more variable. Limitations with extrapolation of PAS data to wavelengths below 405 nm and missing BrC species of low solubility that more strongly absorb at higher wavelengths may account for the differences. Based on measurements closest to fires, the emission ratio of PAS measured BrC at 405 nm relative to carbon monoxide (CO) was on average 0.13 Mm−1 ppbv−1, emission ratios for soluble BrC are also provided. As the smoke moved away from the burning regions the evolution over time of BrC was observed to be highly complex; BrC enhancement, depletion, or constant levels with age were all observed in the first 8 hours after emission in different plumes. Within 8 hours following emissions, 4-nitrocatechol, a well characterized BrC chromophore commonly found in smoke particles, was largely depleted relative to the bulk BrC. In a descending plume where temperature increased by 15 K, 4-nitrocatechol dropped possibly due to temperature-driven evaporation, but bulk BrC remained largely unchanged. Evidence was found for reactions with ozone, or related species, as a pathway for secondary formation of BrC under both low and high oxides of nitrogen (NOx) conditions, while BrC was also observed to be bleached in regions of higher ozone and low NOx, consistent with complex behaviors of BrC observed in laboratory studies. Although the evolution of smoke in the first hours following emission is highly variable, a limited number of measurements of more aged smoke (15 to 30 hours) indicate a net loss of BrC. It is yet to be determined how the near-field BrC evolution in smoke affects the characteristics of smoke over longer time and spatial scales, where its environmental impacts are likely to be greater.

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“…Plume ages for each transect were calculated using back trajectory analysis (Liao et al., 2021). Fire source locations were identified based on point of ignition reported by the National Interagency Fire Center, and confirmed with MODIS and VIIRS satellite detections.…”

Section: Experimental Approachmentioning

confidence: 99%

Complexity in the Evolution, Composition, and Spectroscopy of Brown Carbon in Aircraft Measurements of Wildfire Plumes

Washenfelder

Azzarello

Ball

et al. 2022

Geophysical Research Letters

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Biomass burning is a major source of light‐absorbing organic aerosol (brown carbon), but its composition, chemical evolution, and lifetime are not well known. We measured water‐soluble brown carbon absorption from 310 to 500 nm on the National Oceanic and Atmospheric Administration Twin Otter aircraft during flights downwind of western United States wildfires in summer 2019. The sampling strategy was near‐Lagrangian and the plume ages spanned 0–5 hr. Trends in brown carbon mass absorption coefficient with plume age varied between flights, and did not show an exponential decay over these short time scales. The measured absorption spectra were smoothly varying, without identifiable contributions from individual chromophores with structured absorption. Using aerosol tracer ions and reference absorption spectra, the calculated contribution of 4‐nitrocatechol to total absorption was <22 ± 9% and <11 ± 5%, although spectral fitting showed that it may be as low as <1.1% and <0.6% at 365 and 405 nm, respectively.

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Formaldehyde evolution in US wildfire plumes during the Fire Influence on Regional to Global Environments and Air Quality experiment (FIREX-AQ)

Cited by 40 publications

References 59 publications

Characteristics and evolution of brown carbon in western United States wildfires

Characteristics and evolution of brown carbon in western United States wildfires

Characteristics and Evolution of Brown Carbon in Western United States Wildfires

Complexity in the Evolution, Composition, and Spectroscopy of Brown Carbon in Aircraft Measurements of Wildfire Plumes

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