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  1. Wildfire smoke contains numerous different reactive organic gases, many of which have only recently been identified and quantified. Consequently, their relative importance as an oxidant sink is poorly constrained, resulting in incomplete representation in both global chemical transport models (CTMs) and explicit chemical mechanisms. Leveraging 160 gas-phase measurements made during the Western Wildfire Experiment for Cloud Chemistry, Aerosol Absorption, and Nitrogen (WE-CAN) aircraft campaign, we calculate OH reactivities (OHRs) for western U.S. wildfire emissions, smoke aged >3 days, smoke-impacted and low/no smoke-impacted urban atmospheres, and the clean free troposphere. VOCs were found to account for ∼80% of the total calculated OHR in wildfire emissions, with at least half of the field VOC OHR not currently implemented for biomass burning (BB) emissions in the commonly used GEOS-Chem CTM. To improve the representation of OHR, we recommend CTMs implement furan-containing species, butadienes, and monoterpenes for BB. The Master Chemical Mechanism (MCM) was found to account for 88% of VOC OHR in wildfire emissions and captures its observed decay in the first few hours of aging, indicating that most known VOC OH sinks are included in the explicit mechanisms. We find BB smoke enhanced the average total OHR by 53% relative to themore »low/no smoke urban background, mainly due to the increase in VOCs and CO thus promoting urban ozone production. This work highlights the most important VOC species for daytime BB plume oxidation and provides a roadmap for which species should be prioritized in next-generation CTMs to better predict the downwind air quality and health impacts of BB smoke.« less
    Free, publicly-accessible full text available January 19, 2024
  2. Abstract

    The known effects of thermodynamics and aerosols can well explain the thunderstorm activity over land, but fail over oceans. Here, tracking the full lifecycle of tropical deep convective cloud clusters shows that adding fine aerosols significantly increases the lightning density for a given rainfall amount over both ocean and land. In contrast, adding coarse sea salt (dry radius > 1 μm), known as sea spray, weakens the cloud vigor and lightning by producing fewer but larger cloud drops, which accelerate warm rain at the expense of mixed-phase precipitation. Adding coarse sea spray can reduce the lightning by 90% regardless of fine aerosol loading. These findings reconcile long outstanding questions about the differences between continental and marine thunderstorms, and help to understand lightning and underlying aerosol-cloud-precipitation interaction mechanisms and their climatic effects.

  3. Free, publicly-accessible full text available April 21, 2023
  4. We examined the reactive uptake of dinitrogen pentoxide (N 2 O 5 ) to authentic biomass-burning aerosol (BBA) using a small chamber reservoir in combination with an entrained aerosol flow tube. BBA was generated from four different fuel types and the reactivity of N 2 O 5 was probed from 30 to 70% relative humidity (RH). The N 2 O 5 reactive uptake coefficient, γ (N 2 O 5 ), depended upon RH, fuel type, and to a lesser degree on aerosol chloride mass fractions. The γ (N 2 O 5 ) ranged from 2.0 (±0.4) ×10 −3 on black needlerush derived BBA at 30% RH to 6.0 (±0.6) ×10 −3 on wiregrass derived BBA at 65% RH. Major N 2 O 5 reaction products were observed including gaseous ClNO 2 and HNO 3 and particulate nitrate, and used to create a reactive nitrogen budget. Black needlerush BBA had the most particulate chloride, and the only measured ClNO 2 yield > 1%. The ClNO 2 yield on black needlerush decayed from an initial value of ∼100% to ∼30% over the course of the burn experiment, suggesting a depletion of BBA chloride over time. Black needlerush was also the only fuelmore »for which the reactive nitrogen budget indicated other N-containing products were generated. Generally, the results suggest limited chloride availability for heterogeneous reaction for BBA in the RH range probed here, including BBA with chloride mass fractions on the higher end of previously reported values (∼17–34%). Though less than fresh sea spray aerosol, ∼50%. We use these measured quantities to discuss the implications for nocturnal aerosol nitrate formation, the chemical fate of N 2 O 5 (g), and the availability of particulate chloride for activation in biomass burning plumes.« less
  5. Abstract. We present an updated mechanism for tropospheric halogen (Cl + Br + I) chemistry in the GEOS-Chem global atmospheric chemical transportmodel and apply it to investigate halogen radical cycling and implications for tropospheric oxidants. Improved representation of HOBr heterogeneouschemistry and its pH dependence in our simulation leads to less efficient recycling and mobilization of bromine radicals and enables the model toinclude mechanistic sea salt aerosol debromination without generating excessive BrO. The resulting global mean tropospheric BrO mixingratio is 0.19 ppt (parts per trillion), lower than previous versions of GEOS-Chem. Model BrO shows variable consistency and biases in comparison tosurface and aircraft observations in marine air, which are often near or below the detection limit. The model underestimates the daytimemeasurements of Cl2 and BrCl from the ATom aircraft campaign over the Pacific and Atlantic, which if correct would imply a very largemissing primary source of chlorine radicals. Model IO is highest in the marine boundary layer and uniform in the free troposphere, with a globalmean tropospheric mixing ratio of 0.08 ppt, and shows consistency with surface and aircraft observations. The modeled global meantropospheric concentration of Cl atoms is 630 cm−3, contributing 0.8 % of the global oxidation of methane, 14 % of ethane,8 % of propane, and 7 % of highermore »alkanes. Halogen chemistry decreases the global tropospheric burden of ozone by 11 %,NOx by 6 %, and OH by 4 %. Most of the ozone decrease is driven by iodine-catalyzed loss. The resulting GEOS-Chem ozonesimulation is unbiased in the Southern Hemisphere but too low in the Northern Hemisphere.« less