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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 2.5µm (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_2.5in 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.

 

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.

 

Abstract. Fires emit a substantial amount of non-methane organic gases (NMOGs), theatmospheric oxidation of which can contribute to ozone and secondaryparticulate matter formation. However, the abundance and reactivity of thesefire NMOGs are uncertain and historically not well constrained. In thiswork, we expand the representation of fire NMOGs in a global chemicaltransport model, GEOS-Chem. We update emission factors to Andreae (2019) andthe chemical mechanism to include recent aromatic and ethene and ethyne modelimprovements(Bateset al., 2021; Kwon et al., 2021). We expand the representation of NMOGs byadding lumped furans to the model (including their fire emission andoxidation chemistry) and by adding fire emissions of nine species alreadyincluded 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 estimatethat our improved representation captures 72 % of emitted, identified NMOGcarbon mass and 49 % of OH reactivity from savanna and temperate forestfires, a substantial increase from the standard model (49 % of mass,28 % of OH reactivity). We evaluate fire NMOGs in our model withobservations 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 theTroposphere from Aircraft and Satellites (ARCTAS) in boreal Canada. We show that NMOGs,including furan, are well simulated in the eastern US with someunderestimates in the western US and that adding fire emissions improves ourability to simulate ethene in boreal Canada. We estimate that fires provide15 % of annual mean simulated surface OH reactivity globally, as well as morethan 75 % over fire source regions. Over continental regions about half ofthis simulated fire reactivity comes from NMOG species. We find that furansand ethene are important globally for reactivity, while phenol is moreimportant at a local level in the boreal regions. This is the first globalestimate of the impact of fire on atmospheric reactivity. 

We investigate and assess how well a global chemical transport model (GEOS‐Chem) simulates submicron aerosol mass concentrations in the remote troposphere. The simulated speciated aerosol (organic aerosol (OA), black carbon, sulfate, nitrate, and ammonium) mass concentrations are evaluated against airborne observations made during all four seasons of the NASA Atmospheric Tomography Mission (ATom) deployments over the remote Pacific and Atlantic Oceans. Such measurements over pristine environments offer fresh insights into the spatial (Northern [NH] and Southern Hemispheres [SH], Atlantic, and Pacific Oceans) and temporal (all seasons) variability in aerosol composition and lifetime, away from continental sources. The model captures the dominance of fine OA and sulfate aerosol mass concentrations in all seasons. There is a high bias across all species in the ATom‐2 (NH winter) simulations; implementing recent updates to the wet scavenging parameterization improves our simulations, eliminating the large ATom‐2 (NH winter) bias, improving the ATom‐1 (NH summer) and ATom‐3 (NH fall) simulations, but producing a model underestimate in aerosol mass concentrations for the ATom‐4 (NH spring) simulations. Following the wet scavenging updates, simulated global annual mean aerosol lifetimes vary from 1.9 to 4.0 days, depending on species. Aerosol lifetimes in each hemisphere vary by season, and are longest for carbonaceous aerosol during the southern hemispheric fire season. The updated wet scavenging parameterization brings simulated concentrations closer to observations and reduces global aerosol lifetime for all species, indicating the sensitivity of global aerosol lifetime and burden to wet removal processes.

 

Glyoxal is a volatile organic compound (VOC) in the atmosphere that is a precursor to ozone and secondary organic aerosol, can be a measure of photochemical activity, and is one of a small number of VOCs observable from space. However, the global budget of glyoxal is not well understood, and there has been limited exploration of whether current chemical transport models reproduce satellite observations of this VOC. In this work we take advantage of recent advances in the retrieval of glyoxal from the Ozone Monitoring Instrument along with retrieved formaldehyde and the GEOS‐Chem model to constrain global glyoxal sources. Model glyoxal is produced by direct emissions from fires (6.5 Tg/year) and secondary chemical production (32.9 Tg/year) from biogenic and anthropogenic precursors. The model reproduces the annual average terrestrial spatial variability in formaldehyde and glyoxal reasonably well, with anR²of 0.8 and 0.5, respectively. We find that the model representation of biomass burning, C₂H₂, glyocolaldehyde, and isoprene‐dominated glyoxal production is consistent with the observations of glyoxal and formaldehyde, and the ratio of glyoxal to formaldehyde to within ~20%. However, the observations suggest that glyoxal production from the high monoterpene‐emitting boreal regions is underestimated in the model, with concentrations low by more than a factor of 3. This suggests that the oxidative chemistry of monoterpenes is not well represented in the GEOS‐Chem model and that more laboratory work is needed to constrain the impact of monoterpene emissions on atmospheric composition.