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Abstract Future anthropogenic land use change (LUC) may alter atmospheric carbonaceous aerosol (black carbon and organic aerosol) burden by perturbing biogenic and fire emissions. However, there has been little investigation of this effect. We examine the global evolution of future carbonaceous aerosol under the Shared Socioeconomic Pathways projected reforestation and deforestation scenarios using the CESM2 model from present‐day to 2100. Compared to present‐day, the change in future biogenic volatile organic compounds emission follows changes in forest coverage, while fire emissions decrease in both projections, driven by trends in deforestation fires. The associated carbonaceous aerosol burden change produces moderate aerosol direct radiative forcing (−0.021 to +0.034 W/m²) and modest mean reduction in PM_2.5exposure (−0.11 μg/m³to −0.23 μg/m³) in both scenarios. We find that future anthropogenic LUC may be more important in determining atmospheric carbonaceous aerosol burden than direct anthropogenic emissions, highlighting the importance of further constraining the impact of LUC. 

Abstract 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. 

Abstract. Secondary inorganic aerosols (sulfate, nitrate, and ammonium, SNA) are major contributors to fine particulate matter. Predicting concentrations of these species is complicated by the cascade of processes that control their abundance, including emissions, chemistry, thermodynamic partitioning, and removal. In this study, we use 11 flight campaigns to evaluate the GEOS-Chem model performance for SNA. Across all the campaigns, the model performance is best for sulfate (R2 = 0.51; normalized mean bias (NMB) = 0.11) and worst for nitrate (R2=0.22; NMB = 1.76), indicating substantive model deficiencies in the nitrate simulation. Thermodynamic partitioning reproduces the total particulate nitrate well (R2=0.79; NMB = 0.09), but actual partitioning (i.e., ε(NO3-)= NO3- / TNO3) is challenging to assess given the limited sets of full gas- and particle-phase observations needed for ISORROPIA II. In particular, ammonia observations are not often included in aircraft campaigns, and more routine measurements would help constrain sources of SNA model bias. Model performance is sensitive to changes in emissions and dry and wet deposition, with modest improvements associated with the inclusion of different chemical loss and production pathways (i.e., acid uptake on dust, N2O5 uptake, and NO3- photolysis). However, these sensitivity tests show only modest reduction in the nitrate bias, with no improvement to the model skill (i.e., R2), implying that more work is needed to improve the description of loss and production of nitrate and SNA as a whole. 

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.