skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.


Title: Observationally constrained representation of brown carbon emissions from wildfires in a chemical transport model
The month of August 2015 featured extensive wildfires in the Northwestern U.S. and no significant fires in Alaska and Canada. With the majority of carbonaceous aerosols (CA), including black carbon (BC) and brown carbon (BrC), over the U.S. dominated by emissions from Northwestern wildfires, this month presented a unique opportunity for testing wildfire BrC representation in the Weather Research and Forecasting model with chemistry (WRF-Chem). We performed parallel simulations that (1) did not account for BrC absorption, (2) accounted for BrC absorption, and (3) accounted for BrC absorption as well as its decay due to photobleaching. We used a comprehensive set of extensive and pseudo-intensive optical properties, namely the aerosol optical depth (AOD), aerosol absorption optical depth (AAOD), absorption Ångström exponent (AAE), and single scattering albedo (SSA) to constrain the model output against observations from the Aerosol Robotic Network (AERONET). We found that accounting for BrC absorption and photobleaching resulted in the best agreement with observations in terms of aerosol absorption (AAOD and AAE). However, the model severely underestimated AOD and SSA compared to observations. We attributed this discrepancy to missing scattering due to missing secondary organic aerosol (SOA) formation from wildfire emissions in the model. To test this hypothesis, we applied a zeroth-order representation of wildfire SOA, which significantly improved the AOD and SSA model-observation comparison. Our findings indicate that BrC absorption, the decay of its absorption due to photobleaching, as well as SOA formation should be accounted for in chemical transport models in order to accurately represent CA emissions from wildfires.  more » « less
Award ID(s):
1748080
PAR ID:
10323030
Author(s) / Creator(s):
;
Date Published:
Journal Name:
Environmental Science: Atmospheres
Volume:
2
Issue:
2
ISSN:
2634-3606
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. null (Ed.)
    Deriving aerosol optical depth (AOD) from space-borne observations is still challenging due to uncertainties associated with sensor calibration drift, cloud screening, aerosol type classification, and surface reflectance characterization. As an initial step to understanding the physical processes impacting these uncertainties in satellite AOD retrievals, this study outlines a theoretical approach to estimate biases in the satellite aerosol retrieval algorithm affected by surface albedo and prescribed aerosol optical properties using a simplified radiative transfer model with a traditional error propagation approach. We expand the critical surface reflectance concept to obtain the critical surface albedo (CSA), critical single scattering albedo (CSSA), and critical asymmetry parameter (CAP). The top-of-atmosphere (TOA) reflectance is not sensitive to significant variability in aerosol loading (AOD) at the critical value; thus, the AOD cannot be determined. Results show that 5% bias in surface albedo (A), single scattering albedo (SSA), or asymmetry parameter (g) lead to large retrieved AOD errors, especially high under conditions when A, SSA, or g are close to their critical values. The results can be useful for future research related to improvements of satellite aerosol retrieval algorithms and provide a preliminary framework to analytically quantify AOD uncertainties from satellite retrievals. 
    more » « less
  2. Nitrogen-containing heterocyclic volatile organic compounds (VOCs) are important components of wildfire emissions that are readily reactive toward nitrate radicals (NO3) during nighttime, but the oxidation mechanism and the potential formation of secondary organic aerosol (SOA) and brown carbon (BrC) are unclear. Here, NO3 oxidation of three nitrogen-containing heterocyclic VOCs, pyrrole, 1-methylyrrole (1-MP), and 2-methylpyrrole (2-MP), was investigated in chamber experiments to determine the effect of precursor structures on SOA and BrC formation. The SOA chemical compositions and the optical properties were analyzed using a suite of online and offline instrumentation. Dinitro- and trinitro-products were found to be the dominant SOA constituents from pyrrole and 2-MP, but not observed from 1-MP. Furthermore, the SOA from 2-MP and pyrrole showed strong light absorption, while that from 1-MP were mostly scattering. From these results, we propose that NO3-initiated hydrogen abstraction from the 1-position in pyrrole and 2-MP followed by radical shift and NO2 addition leads to light-absorbing nitroaromatic products. In the absence of a 1-position hydrogen, NO3 addition likely dominates the 1-MP chemistry. We also estimate that the total SOA mass and light absorption from pyrrole and 2-MP are comparable to those from phenolic VOCs and toluene in biomass burning, underscoring the importance of considering nighttime oxidation of pyrrole and methylpyrroles in air quality and climate models. 
    more » « less
  3. Brown carbon (BrC) plays an important role in global radiative budget but there have been few studies on BrC in Arctic despite rapid warming and increasing wildfires in this region. Here we investigate the optical properties of BrC from boreal fires in Alaska summer, with two sets of measurements from PILS-LWCC-TOC (Particle-Into-Liquid-Sampler – Liquid-Waveguide Capillary flow-through optical Cell - Total-Organic-Carbon analyzer) and filter measurements. We show that during intense wildfires, the mass absorption coefficient at 365 nm (MAC365) from water soluble organic carbon (WSOC) remained stable at ∼1 m2 g−1. With all plumes sampled and derived transport time, we show a decrease of MAC365 with plume age, with a shorter photobleaching lifetime (∼11 h) at 365 nm compared to 405 nm (∼20 h). The total absorption by organic aerosols measured from filters at 365 nm is higher than the absorption by WSOC by a factor 2–3, suggesting a dominant role of insoluble organic carbon. Overall BrC dominates absorption in the near-ultraviolet and visible radiation during wildfire season in Alaska summer. 
    more » « less
  4. Abstract. We characterize the aerosol physical and optical properties of 13 transported biomass burning (BB) events. BB events included long-rangeinfluence from fires in Alaskan and Siberian boreal forests transported to Mt. Bachelor Observatory (MBO) in the free troposphere (FT) over 8–14+ d and regional wildfires in northern California and southwestern Oregon transported to MBO in the boundary layer (BL) over 10 h to 3 d. Intensive aerosol optical properties and normalized enhancement ratios for BB events were derived from measured aerosol light scattering coefficients (σscat), aerosol light-absorbing coefficients (σabs), fine particulate matter (PM1), and carbon monoxide (CO) measurements made from July to September 2019, with particle size distribution collected from August to September. The observations showed that the Siberian BB events had a lower scattering Ångström exponent (SAE), a higher mass scattering efficiency (MSE; Δσscat/ΔPM1), and a bimodal aerosol size distribution with a higher geometric mean diameter (Dg). We hypothesize that the larger particles and associated scatteringproperties were due to the transport of fine dust alongside smoke in addition to contributions from condensation of secondary aerosol, coagulation of smaller particles, and aqueous-phase processing duringtransport. Alaskan and Siberian boreal forest BB plumes were transported long distances in the FT and characterized by lower absorptionÅngström exponent (AAE) values indicative of black carbon (BC)dominance in the radiative budget. Significantly elevated AAE values wereonly observed for BB events with <1 d transport, which suggests strong production of brown carbon (BrC) in these plumes but limited radiative forcing impacts outside of the immediate region. 
    more » « less
  5. Guaiacol, present in wood smoke, readily forms secondary organic aerosol (SOA), and, in the aqueous phase, brown carbon (BrC) species. Here, BrC is produced in an illuminated chamber containing guaiacol(g), HOOH(g) as an OH radical source, and either deliquesced salt particles or guaiacol SOA at 50% relative humidity. BrC production slows without an OH source (HOOH), likely due to low levels of radical generation by photosensitization, perhaps involving surface-adsorbed guaiacol and dissolved oxygen. With or without HOOH, BrC mass absorption coefficients at 365 nm generated by the guaiacol + OH reaction reach a maximum at ~6 h of atmospheric OH exposure, after which photobleaching becomes dominant. In the presence of soluble iron but no HOOH, more BrC is produced, likely due to insoluble polymer production observed in previous studies. However, with both soluble iron and HOOH (enabling Fenton chemistry), significantly less SOA and BrC are produced due to very high oxidation rates, and the average SOA carbon oxidation state reaches 2, indicating carboxylate products like oxalate. These results indicate that SOA and BrC formation by guaiacol photooxidation can take place over a wider range of atmospheric conditions than previously thought, and that the effects of iron(II) depend on HOOH. Multiphase guaiacol photooxidation likely makes a significant contribution to producing highly oxidized SOA material in smoke plumes. 
    more » « less