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  1. Abstract. Observations over the last decade have demonstrated that theatmosphere contains potentially hundreds of compounds that can react withsulfuric acid to nucleate stable aerosol particles. Consequently, modelingatmospheric nucleation requires detailed knowledge of nucleation reactionkinetics and spatially and temporally resolved measurements of numerousprecursor compounds. This study introduces the Nucleation Potential Model(NPM), a novel nucleation model that dramatically simplifies the diversereactions between sulfuric acid and any combination of precursor gases. The NPMpredicts 1 nm nucleation rates from only two measurable gas concentrations,regardless of whether all precursor gases are known. The NPM describes sulfuricacid nucleating with a parameterized base compound at an effective baseconcentration, [Beff]. [Beff] captures the ability of a compoundor mixture to form stable clusters with sulfuric acid and is estimated frommeasured 1 nm particle concentrations. The NPM is applied to experimental andfield observations of sulfuric acid nucleation to demonstrate how[Beff] varies for different stabilizing compounds, mixtures, andsampling locations. Analysis of previous field observations shows distinctdifferences in [Beff] between locations that follow the emissionsources and stabilizing compound concentrations for that region. Overall,the NPM allows researchers to easily model nucleation across diverseenvironments and estimate the concentration of non-sulfuric acid precursorsusing a condensation particle counter. 
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  3. Wildfires are an important atmospheric source of primary organic aerosol (POA) and precursors for secondary organic aerosol (SOA) at regional and global scales. However, there are large uncertainties surrounding the emissions and physicochemical processes that control the transformation, evolution, and properties of POA and SOA in large wildfire plumes. We develop a plume version of a kinetic model to simulate the dilution, oxidation chemistry, thermodynamic properties, and microphysics of organic aerosol (OA) in wildfire smoke. The model is applied to study the in-plume OA in four large wildfire smoke plumes intercepted during an aircraft-based field campaign in summer 2018 in the western United States. Based on estimates of dilution and oxidant concentrations before the aircraft first intercepted the plumes, we simulate the OA evolution from very close to the fire to several hours downwind. Our model results and sensitivity simulations suggest that dilution-driven evaporation of POA and simultaneous photochemical production of SOA are likely to explain the observed evolution in OA mass with physical age. The model, however, substantially underestimates the change in the oxygen-to-carbon ratio of the OA compared to measurements. In addition, we show that the rapid chemical transformation within the first hour after emission is driven by higher-than-ambient OH concentrations (3×10 6 -10 7 molecules cm -3 ) and the slower evolution over the next several hours is a result of lower-than-ambient OH concentrations (<10 6 molecules cm -3 ) and depleted SOA precursors. Model predictions indicate that the OA measured several hours downwind of the fire is still dominated by POA but with an SOA fraction that varies between 30% and 56% of the total OA. Semivolatile, heterocyclic, and oxygenated aromatic compounds, in that order, were found to contribute substantially (>90%) to SOA formation. Future work needs to focus on better understanding the dynamic evolution closer to the fire and resolving the rapid change in the oxidation state of OA with physical age. 
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  4. Abstract. Western US wildlands experience frequent and large-scale wildfires which arepredicted to increase in the future. As a result, wildfire smoke emissionsare expected to play an increasing role in atmospheric chemistry whilenegatively impacting regional air quality and human health. Understanding theimpacts of smoke on the environment is informed by identifying andquantifying the chemical compounds that are emitted during wildfires and byproviding empirical relationships that describe how the amount andcomposition of the emissions change based upon different fire conditions andfuels. This study examined particulate organic compounds emitted from burningcommon western US wildland fuels at the US Forest Service Fire ScienceLaboratory. Thousands of intermediate and semi-volatile organic compounds(I/SVOCs) were separated and quantified into fire-integrated emission factors(EFs) using a thermal desorption, two-dimensional gas chromatograph withonline derivatization coupled to an electron ionization/vacuum ultraviolethigh-resolution time-of-flight mass spectrometer(TD-GC × GC-EI/VUV-HRToFMS). Mass spectra, EFs as a function ofmodified combustion efficiency (MCE), fuel source, and other definingcharacteristics for the separated compounds are provided in the accompanyingmass spectral library. Results show that EFs for total organic carbon (OC),chemical families of I/SVOCs, and most individual I/SVOCs span 2–5 orders ofmagnitude, with higher EFs at smoldering conditions (low MCE) than flaming.Logarithmic fits applied to the observations showed that log (EFs) forparticulate organic compounds were inversely proportional to MCE. Thesemeasurements and relationships provide useful estimates of EFs for OC,elemental carbon (EC), organic chemical families, and individual I/SVOCs as afunction of fire conditions. 
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