Therese S. Carter’s research while affiliated with George Washington University and other places

Communities of color and lower income are often found to experience disproportionate levels of fine particulate matter (PM2.5) air pollution in the US.1–3 The federal and several state governments use relatively coarsely resolved (12km) PM2.5 concentration estimates to identify overburdened communities. Newly available PM2.5 datasets estimate concentrations at increasingly high spatial resolutions (50m - 1km), with different magnitudes and spatial patterns, potentially affecting assessments of racial, ethnic, and socioeconomic exposure disparities. We show that two recently available high-resolution datasets from the scientific community and the 12km dataset are consistent for national and regional average, but not intraurban, PM2.5 concentration disparities in 2019. The datasets consistently indicate that regional average PM2.5 concentrations are higher in the least White (by 3-65%) and most Hispanic census tracts (2-47%), compared with in the most Non-Hispanic White tracts. However, in nine of the 10 most populous cities, the three datasets differ on the order of least-to-most exposed population subgroups. We identified 1029 tracts (representing ~4.5 million people) as disadvantaged (≥65th percentile for poverty and ≥90th percentile PM2.5) in all three datasets, 335 tracts (~1.5 million people) as disadvantaged using both high-resolution datasets but not the 12km dataset, and 695 tracts (~2.7 million people) as disadvantaged in the 12km dataset but not the high-resolution datasets. The 12km dataset does not capture intraurban disparities and may mischaracterize disproportionately exposed neighborhoods. The high-resolution PM2.5 datasets can be further improved by ground-truthing with observations from rapidly expanding ground and mobile monitoring and by integrating across available datasets.

Increasing fire activity and the associated degradation in air quality in the United States has been indirectly linked to human activity via climate change. In addition, direct attribution of fires to human activities may provide opportunities for near term smoke mitigation by focusing policy, management, and funding efforts on particular ignition sources. We analyze how fires associated with human ignitions (agricultural fires and human-initiated wildfires) impact fire particulate matter under 2.5 µ m (PM 2.5 ) concentrations in the contiguous United States (CONUS) from 2003 to 2018. We find that these agricultural and human-initiated wildfires dominate fire PM 2.5 in both a high fire and human ignition year (2018) and low fire and human ignition year (2003). Smoke from these human levers also makes meaningful contributions to total PM 2.5 (∼5%–10% in 2003 and 2018). Across CONUS, these two human ignition processes account for more than 80% of the population-weighted exposure and premature deaths associated with fire PM 2.5 . These findings indicate that a large portion of the smoke exposure and impacts in CONUS are from fires ignited by human activities with large mitigation potential that could be the focus of future management choices and policymaking.

Fires emit a substantial amount of non-methane organic gases (NMOGs), the atmospheric oxidation of which can contribute to ozone and secondary particulate matter formation. However, the abundance and reactivity of these fire NMOGs are uncertain and historically not well constrained. In this work, we expand the representation of fire NMOGs in a global chemical transport model, GEOS-Chem. We update emission factors to Andreae (2019) and the chemical mechanism to include recent aromatic and ethene and ethyne model improvements (Bates et al., 2021; Kwon et al., 2021). We expand the representation of NMOGs by adding lumped furans to the model (including their fire emission and oxidation chemistry) and by adding fire emissions of nine species already included in the model, prioritized for their reactivity using data from the Fire Influence on Regional to Global Environments (FIREX) laboratory studies. Based on quantified emissions factors, we estimate that our improved representation captures 72 % of emitted, identified NMOG carbon mass and 49 % of OH reactivity from savanna and temperate forest fires, a substantial increase from the standard model (49 % of mass, 28 % of OH reactivity). We evaluate fire NMOGs in our model with observations from the Amazon Tall Tower Observatory (ATTO) in Brazil, Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) and DC3 in the US, and Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) in boreal Canada. We show that NMOGs, including furan, are well simulated in the eastern US with some underestimates in the western US and that adding fire emissions improves our ability to simulate ethene in boreal Canada. We estimate that fires provide 15 % of annual mean simulated surface OH reactivity globally, as well as more than 75 % over fire source regions. Over continental regions about half of this simulated fire reactivity comes from NMOG species. We find that furans and ethene are important globally for reactivity, while phenol is more important at a local level in the boreal regions. This is the first global estimate of the impact of fire on atmospheric reactivity.

Biomass burning organic aerosol (BBOA) in the atmosphere contains many compounds that absorb solar radiation, called brown carbon (BrC). While BBOA is in the atmosphere, BrC can undergo reactions with oxidants such as ozone which decrease absorbance, or whiten. The effect of temperature and relative humidity (RH) on whitening has not been well constrained, leading to uncertainties when predicting the direct radiative effect of BrC on climate. Using an aerosol flow-tube reactor, we show that the whitening of BBOA by oxidation with ozone is strongly dependent on RH and temperature. Using a poke-flow technique, we show that the viscosity of BBOA also depends strongly on these conditions. The measured whitening rate of BrC is described well with the viscosity data, assuming that the whitening is due to oxidation occurring in the bulk of the BBOA, within a thin shell beneath the surface. Using our combined datasets, we developed a kinetic model of this whitening process, and we show that the lifetime of BrC is 1 d or less below ∼1 km in altitude in the atmosphere but is often much longer than 1 d above this altitude. Including this altitude dependence of the whitening rate in a chemical transport model causes a large change in the predicted warming effect of BBOA on climate. Overall, the results illustrate that RH and temperature need to be considered to understand the role of BBOA in the atmosphere.

Fires emit a substantial amount of non-methane organic gases (NMOGs); the atmospheric oxidation of which can contribute to ozone and secondary particulate matter formation. However, the abundance and reactivity of these fire NMOGs are uncertain and historically not well constrained. In this work, we expand the representation of fire NMOGs in a global chemical transport model, GEOS-Chem. We update emission factors to Andreae (2019) and the chemical mechanism to include recent aromatic and ethene/ethyne model improvements (Bates et al., 2021; Kwon et al., 2021). We expand the representation of NMOGs by adding lumped furans to the model (including their fire emission and oxidation chemistry) and by adding fire emissions of nine species already included in the model, prioritized for their reactivity using data from the FIREX laboratory studies. Based on quantified emissions factors, we estimate that our improved representation captures 72 % of emitted, identified NMOG carbon mass and 49 % of OH reactivity from savanna and temperate forest fires, a substantial increase from the standard model (49 % of mass, 28 % of OH reactivity). We evaluate fire NMOGs in our model with observations from the Amazon Tall Tower Observatory (ATTO), FIREX-AQ and DC3 in the US, and ARCTAS in boreal Canada. We show that NMOGs, including furan, are well simulated in the eastern US with some underestimates in the western US and that adding fire emissions improves our ability to simulate ethene in boreal Canada. We estimate that fires provide 15 % of annual mean simulated surface OH reactivity globally, and exceeding 75 % over fire source regions. Over continental regions about half of this simulated fire reactivity comes from NMOG species. We find that furans and ethene are important globally for reactivity, while phenol is more important at a local level in the boreal regions. This is the first global estimate of the impact of fire on atmospheric reactivity.

The World Health Organization recently updated their air quality guideline for annual fine particulate matter (PM2.5) exposure from 10 to 5 μg m-3, citing global health considerations. We explore if this guideline is attainable across different regions of the world using a series of model sensitivity simulations for 2019. Our results indicate that >90% of the global population is exposed to PM2.5 concentrations that exceed the 5 μg m-3 guideline and that only a few sparsely populated regions (largely in boreal North America and Asia) experience annual average concentrations of <5 μg m-3. We find that even under an extreme abatement scenario, with no anthropogenic emissions, more than half of the world's population would still experience annual PM2.5 exposures above the 5 μg m-3 guideline (including >70% and >60% of the African and Asian populations, respectively), largely due to fires and natural dust. Our simulations demonstrate the large heterogeneity in PM2.5 composition across different regions and highlight how PM2.5 composition is sensitive to reductions in anthropogenic emissions. We thus suggest the use of speciated aerosol exposure guidelines to help facilitate region-specific air quality management decisions and improve health-burden estimates of fine aerosol exposure.

This study aims to better our collective understanding of the oxidative capacity and atmospheric chemistry over the equatorial Pacific. Bulk and size-segregated filter samples were collected during the GEOTRACES Eastern Tropical Pacific transect (4.1° S, 81.9° W to 10.5° S, 152.0° W; October–December 2013) and measured for aerosol concentration and complete isotopic composition of nitrate (δ¹⁵N, δ¹⁸O, Δ¹⁷O where Δ¹⁷O = δ¹⁷O – 0.52 × δ¹⁸O). Combined size-segregated filters produced data similar to that found in bulk filter samples, and notably neither δ¹⁵N nor δ¹⁸O showed any trends based on aerosol size. Similar to other studies, NO3– is concentrated (>80%) in the coarse size fractions (>1.5 μm). Bulk aerosol concentrations ranged from 6.6 to 89.8 nmol/m³. The bulk δ¹⁵N-, δ¹⁸O-, and Δ¹⁷O-nitrate ranged from −13.1 to −3.2‰, 68.5 to 79.3‰, and 23.5 to 28.4‰, respectively. Higher δ¹⁵N values near the coast are best explained by the influence of continental sources; lower δ¹⁵N values far from the coast may be associated with chemical fractionation during long-range transport or an oceanic source. Both Δ¹⁷O and δ¹⁸O are interpreted using kinetic analysis and gas concentrations from a global atmospheric chemical transport model (GEOS-Chem), which showed that nitrate production in this environment is dominated by OH oxidation (60%) and RONO2 hydrolysis (15%). To best match the δ¹⁸O and Δ¹⁷O observations in this study, the terminal oxygen isotopic values for ozone must be higher than those suggested by available observations and/or halogen-mediated chemistry must be more important than the models currently suggest.

Biomass burning (BB) produces large quantities of carbonaceous aerosol (black carbon and organic aerosol, BC and OA, respectively), which significantly degrade air quality and impact climate. BC absorbs radiation, warming the atmosphere, while OA typically scatters radiation, leading to cooling. However, some OA, termed brown carbon (BrC), also absorbs visible and near UV radiation; although, its properties are not well constrained. We explore three aircraft campaigns from important BB regions with different dominant fuel and fire types (Western Wildfire Experiment for Cloud Chemistry, Aerosol Absorption, and Nitrogen [WE‐CAN] in the western United States and ObseRvations of Aerosols above CLouds and their intEractionS and Cloud‐Aerosol‐Radiation Interactions and Forcing for Year downwind of southern Africa) and compare them with simulations from the global chemical transport model, GEOS‐Chem using GFED4s. The model generally captures the observed vertical profiles of carbonaceous BB aerosol concentrations; however, we find that BB BC emissions are underestimated in southern Africa. Our comparisons suggest that BC and/or BrC absorption is substantially higher downwind of Africa than in the western United States and, while the Saleh et al. (2014, https://doi.org/10.1038/ngeo2220) and FIREX parameterizations based on the BC:OA ratio improve model‐observation agreement in some regions, they do not sufficiently differentiate absorption characteristics at short wavelengths. We find that photochemical whitening substantially decreases the burden and direct radiative effect of BrC (annual mean of +0.29 W m⁻² without whitening and +0.08 W m⁻² with). Our comparisons suggest that whitening is required to explain WE‐CAN observations; however, the importance of whitening for African fires cannot be confirmed. Qualitative comparisons with the OMI UV aerosol index suggest our standard BrC whitening scheme may be too fast over Africa.

Fires and the aerosols that they emit impact air quality, health, and climate, but the abundance and properties of carbonaceous aerosol (both black carbon and organic carbon) from biomass burning (BB) remain uncertain and poorly constrained. We aim to explore the uncertainties associated with fire emissions and their air quality and radiative impacts from underlying dry matter consumed and emissions factors. To investigate this, we compare model simulations from a global chemical transport model, GEOS-Chem, driven by a variety of fire emission inventories with surface and airborne observations of black carbon (BC) and organic aerosol (OA) concentrations and satellite-derived aerosol optical depth (AOD). We focus on two fire-detection-based and/or burned-area-based (FD-BA) inventories using burned area and active fire counts, respectively, i.e., the Global Fire Emissions Database version 4 (GFED4s) with small fires and the Fire INventory from NCAR version 1.5 (FINN1.5), and two fire radiative power (FRP)-based approaches, i.e., the Quick Fire Emission Dataset version 2.4 (QFED2.4) and the Global Fire Assimilation System version 1.2 (GFAS1.2). We show that, across the inventories, emissions of BB aerosol (BBA) differ by a factor of 4 to 7 over North America and that dry matter differences, not emissions factors, drive this spread. We find that simulations driven by QFED2.4 generally overestimate BC and, to a lesser extent, OA concentrations observations from two fire-influenced aircraft campaigns in North America (ARCTAS and DC3) and from the Interagency Monitoring of Protected Visual Environments (IMPROVE) network, while simulations driven by FINN1.5 substantially underestimate concentrations. The GFED4s and GFAS1.2-driven simulations provide the best agreement with OA and BC mass concentrations at the surface (IMPROVE), BC observed aloft (DC3 and ARCTAS), and AOD observed by MODIS over North America. We also show that a sensitivity simulation including an enhanced source of secondary organic aerosol (SOA) from fires, based on the NOAA Fire Lab 2016 experiments, produces substantial additional OA; however, the spread in the primary emissions estimates implies that this magnitude of SOA can be neither confirmed nor ruled out when comparing the simulations against the observations explored here. Given the substantial uncertainty in fire emissions, as represented by these four emission inventories, we find a sizeable range in 2012 annual BBA PM2.5 population-weighted exposure over Canada and the contiguous US (0.5 to 1.6 µg m-3). We also show that the range in the estimated global direct radiative effect of carbonaceous aerosol from fires (-0.11 to -0.048 W m-2) is large and comparable to the direct radiative forcing of OA (-0.09 W m-2) estimated in the Fifth Assessment Report (AR5) of the Intergovernmental Panel on Climate Change (IPCC). Our analysis suggests that fire emissions uncertainty challenges our ability to accurately characterize the impact of smoke on air quality and climate.

Abstract. Fires and the aerosols that they emit impact air quality, health, and climate, but the abundance and properties of carbonaceous aerosol (both black carbon and organic carbon) from biomass burning (BB) remain uncertain and poorly constrained. We aim to quantify the uncertainties associated with fire emissions and their air quality and radiative impacts from underlying dry matter consumed and emissions factors. To explore this, we compare model simulations from a global chemical transport model, GEOS-Chem, driven by a variety of fire emission inventories with surface and airborne observations of black carbon (BC) and organic aerosol (OA) concentrations and satellite-derived aerosol optical depth (AOD). We focus on two fire detection/burned area-based (FD/BA) inventories using burned area and active fire counts, respectively: the Global Fire Emissions Database version 4 (GFED4s) with small fires and the Fire INventory from NCAR version 1.5 (FINN1.5) and two fire radiative power (FRP)-based approaches: the Quick Fire Emission Dataset version 2.4 (QFED2.4) and the Global Fire Assimilation System version 1.2 (GFAS1.2). We show that, across the inventories, emissions of BB aerosol (BBA) differ by a factor of 4 to 7 over North America and that dry matter differences, not emissions factors, drive this spread. We find that simulations driven by QFED2.4 generally overestimate BC and, to a lesser extent, OA concentrations observations from two fire-influenced aircraft campaigns in North America (ARCTAS and DC3) and from the Interagency Monitoring of Protected Visual Environments (IMPROVE) network, while simulations driven by FINN1.5 substantially underestimate concentrations. The GFED4s and GFAS1.2-driven simulations provide the best agreement with OA and BC mass concentrations at the surface (IMPROVE), BC observed aloft (DC3 and ARCTAS), and AOD observed by MODIS over North America. We also show that a sensitivity simulation including an enhanced source of secondary organic aerosol (SOA) from fires based on the NOAA Fire Lab 2016 experiments produces substantial additional OA; however, the spread in the primary emissions estimates implies that this magnitude of SOA cannot be either confirmed or ruled out when comparing the simulations against the observations explored here. Given the substantial uncertainty in fire emissions, as represented by these four emission inventories, we find a sizeable range in BBA population-weighted exposure over Canada and the contiguous United States (0.5 to 1.6 µg m⁻³). We also show that the range in the estimated global direct radiative effect of carbonaceous aerosol from fires (−0.11 to −0.048 W m⁻²) is large and comparable to the direct radiative forcing of OA (−0.09 W m⁻²) estimated in AR5. Our analysis suggests that fire emissions uncertainty challenges our ability to accurately characterize the impact of smoke on air quality and climate.