Simulation of the evolution of biomass burning organic aerosol with different volatility basis set schemes in PMCAMx-SRv1.0

Theodoritsi, Georgia N.; Ciarelli, Giancarlo; Pandis, Spyros Ν.

doi:10.5194/gmd-14-2041-2021

Cited by 3 publications

(2 citation statements)

References 49 publications

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“…The evaporation of BBOA is modeled using the kinetic TD model of Cappa, which takes a VBS and temperature conditions as inputs and outputs the MFR. We evaluated multiple BBOA VBS from the literature ,− and also fitted a basis set as part of this work (Supporting Information Section III, Figures S7–S9). The fitted basis set is presented in Table S2.…”

Section: Resultsmentioning

confidence: 99%

Impact of Biomass Burning Organic Aerosol Volatility on Smoke Concentrations Downwind of Fires

Pagonis,

Selimovic,

Campuzano-Jost

et al. 2023

Environ. Sci. Technol.

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Biomass burning particulate matter (BBPM) affects regional air quality and global climate, with impacts expected to continue to grow over the coming years. We show that studies of North American fires have a systematic altitude dependence in measured BBPM normalized excess mixing ratio (NEMR; ΔPM/ΔCO), with airborne and high-altitude studies showing a factor of 2 higher NEMR than ground-based measurements. We report direct airborne measurements of BBPM volatility that partially explain the difference in the BBPM NEMR observed across platforms. We find that when heated to 40− 45 °C in an airborne thermal denuder, 19% of lofted smoke PM 1 evaporates. Thermal denuder measurements are consistent with evaporation observed when a single smoke plume was sampled across a range of temperatures as the plume descended from 4 to 2 km altitude. We also demonstrate that chemical aging of smoke and differences in PM emission factors can not fully explain the platformdependent differences. When the measured PM volatility is applied to output from the High Resolution Rapid Refresh Smoke regional model, we predict a lower PM NEMR at the surface compared to the lofted smoke measured by aircraft. These results emphasize the significant role that gas-particle partitioning plays in determining the air quality impacts of wildfire smoke.

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Section: Resultsmentioning

confidence: 99%

Impact of Biomass Burning Organic Aerosol Volatility on Smoke Concentrations Downwind of Fires

Pagonis,

Selimovic,

Campuzano-Jost

et al. 2023

Environ. Sci. Technol.

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“…Different analytical and computational techniques exist for the determination of the chemical composition of OM and especially secondary organic aerosols (SOAs). Modeling all important SOA-related reactions and species is not feasible for three-dimensional models (Jathar et al, 2015), and simple models do not always reproduce the measured concentrations of OM (Volkamer et al, 2006;Theodoritsi et al, 2021). Among the analytical techniques, aerosol mass spectrometry (AMS) and mid-infrared (MIR) spectroscopy are able to provide bulk chemical information for most of the OM mass (Hallquist et al, 2009).…”

Section: Introductionmentioning

confidence: 99%

Fragment ion–functional group relationships in organic aerosols using aerosol mass spectrometry and mid-infrared spectroscopy

et al. 2022

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Abstract. Aerosol mass spectrometry (AMS) and mid-infrared spectroscopy (MIR) are two analytical methods for characterizing the chemical composition of organic matter (OM). While AMS provides high-temporal-resolution bulk measurements, the extensive fragmentation during the electron ionization makes the characterization of OM components limited. The analysis of aerosols collected on polytetrafluoroethylene (PTFE) filters using MIR, on the other hand, provides functional group information with reduced sample alteration but results in a relatively low temporal resolution. In this work, we compared and combined MIR and AMS measurements for several environmental chamber experiments of combustion-related aerosols to achieve a better understanding of the AMS spectra and the OM chemical evolution with aging. Fresh emissions of wood and coal burning were injected into an environmental simulation chamber and aged with hydroxyl and nitrate radicals. A high-resolution time-of-flight AMS measured the bulk chemical composition of fine OM. Fine aerosols were also sampled on PTFE filters before and after aging for the offline MIR analysis. After comparing AMS and MIR bulk measurements, we used multivariate statistics to identify the functional groups associated the most with the AMS OM for different aerosol sources and oxidants. We also identified the key fragment ions resulting from molecules containing each functional group for the complex OM generated from biomass and fossil fuel combustion. Finally, we developed a statistical model that enables the estimation of the high-time-resolution functional group composition of OM using collocated AMS and MIR measurements. AMS spectra can be used to interpolate the functional group measurements by MIR using this approach. The latter allows us to better understand the evolution of OM during the aging process.

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Chemical evolution of primary and secondary biomass burning aerosols during daytime and nighttime

et al. 2023

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Abstract. Primary emissions from wood and pellet stoves were aged in an atmospheric simulation chamber under daytime and nighttime conditions. The aerosol was analyzed with online aerosol mass spectrometry and offline Fourier transform infrared spectroscopy (FTIR). Measurements using the two techniques agreed reasonably well in terms of the organic aerosol (OA) mass concentration, OA:OC trends, and concentrations of biomass burning markers – lignin-like compounds and anhydrosugars. Based on aerosol mass spectrometry, around 15 % of the primary organic aerosol (POA) mass underwent some form of transformation during daytime oxidation conditions after 6–10 h of atmospheric exposure. A lesser extent of transformation was observed during the nighttime oxidation. The decay of certain semi-volatile (e.g., levoglucosan) and less volatile (e.g., lignin-like) POA components was substantial during aging, highlighting the role of heterogeneous reactions and gas–particle partitioning. Lignin-like compounds were observed to degrade under both daytime and nighttime conditions, whereas anhydrosugars degraded only under daytime conditions. Among the marker mass fragments of primary biomass burning OA (bbPOA), heavy ones (higher m/z) were relatively more stable during aging. The biomass burning secondary OA (bbSOA) became more oxidized with continued aging and resembled that of aged atmospheric organic aerosols. The bbSOA formed during daytime oxidation was dominated by acids. Organonitrates were an important product of nighttime reactions in both humid and dry conditions. Our results underline the importance of changes to both the primary and secondary biomass burning aerosols during their atmospheric aging. Heavier fragments from aerosol mass spectrometry seldom used in atmospheric chemistry can be used as more stable tracers of bbPOA and, in combination with the established levoglucosan marker, can provide an indication of the extent of bbPOA aging.

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Simulation of the evolution of biomass burning organic aerosol with different volatility basis set schemes in PMCAMx-SRv1.0

Cited by 3 publications

References 49 publications

Impact of Biomass Burning Organic Aerosol Volatility on Smoke Concentrations Downwind of Fires

Impact of Biomass Burning Organic Aerosol Volatility on Smoke Concentrations Downwind of Fires

Fragment ion–functional group relationships in organic aerosols using aerosol mass spectrometry and mid-infrared spectroscopy

Chemical evolution of primary and secondary biomass burning aerosols during daytime and nighttime

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