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  1. Rapid production of formic acid in biomass burning smoke is not captured by the Master Chemical Mechanism (MCM) nor simplified GEOS-Chem chemistry, likely due to missing secondary chemical production.

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    Free, publicly-accessible full text available November 9, 2024
  2. Atmospheric oxidation of monoterpenes (C10H16) contributes to ambient particle number and mass concentrations due, in part, to the resulting peroxy radicals undergoing auto-oxidation to low-volatility highly oxygenated molecules (HOMs).

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  3. Abstract

    Exceptionally high‐energy lightning strokes >106 J (X1000 stronger than average) in the very low‐frequency band between 5 and 18 kHz, also known as superbolts (SB), occur mostly during winter over the North‐East Atlantic, the Mediterranean Sea, and over the Altiplano in South America. Here we compare the World‐Wide Lightning Location Network database with meteorological and aerosol data to examine the causes of lightning stroke high energies. Our results show that the energy per stroke increases sharply as the distance between the cloud'scharging zone(where the cloud electrification occurs) and the surface decreases. Since thecharging zoneoccurs above the 0°C isotherm, this distance is shorter when the 0°C isotherm is closer to the surface. This occurs either due to cold air mass over the ocean during winter or high surface altitude in the Altiplano during summer thunderstorms. Stroke energy decreases with the warm phase of the cloud, as proxied by the cloud base temperature, and increases with a more developed cloud, as proxied by the cloud top temperature, but to a much lesser extent than the distance between the surface and 0°C isotherm. Aerosols play no significant role. It is hypothesized that a shorter distance between thecharging zoneand the ground represents less electrical resistance that allows stronger discharge currents.

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  4. Free, publicly-accessible full text available January 23, 2025
  5. 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 the 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. 
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  6. 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.

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  7. 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 fuel 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. 
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