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1. Exploring the Increasing Trend of Organic Carbon in the Atmospheric Aqueous Phase

   Lawrence, C; Lance, S; Casson, P; Tripathy, A; Brandt, R; Synder, P; Kelting, D; Yerger, E; Murray, G; Campbell, J; et al (November 2024, National Atmospheric Deposition Program)

   Organic carbon (OC) is a highly diverse class of compounds that represents a small but critical fraction of the atmosphere’s chemical composition. Volatile organic compounds (VOCs), when combined with nitrogen oxides (NOx), can produce tropospheric ozone (O3), a regulated air pollutant. OC also represents a large and growing fraction of aerosol mass, either through direct emissions from sources like fossil combustion and biomass burning, or through secondary chemistry by the oxidation and subsequent reduction of vapor pressure of VOCs leading to condensational growth. Clouds droplets and precipitation can contain additional OC due to the dissolution of soluble organic gases to the aqueous phase. OC has abundantly been found in aqueous samples of clouds, fog, and precipitation, exposing these compounds to unique aqueous chemical reactions and wet deposition. However, the concentrations and controlling factors of atmospheric aqueous organic carbon remain highly unconstrained. Cloud water measurements at Whiteface Mountain in the Adirondack Mountains in upstate New York have revealed an increasing trend of Total Organic Carbon (TOC), with annual median concentrations doubling in 14 years, possibly signaling a growing trend in atmospheric OC. However, the causes and potential consequences of this trend remain unclear. Another question that has yet to be explored is if this trend in OC extends beyond WFM. To answer this question, this work explores the trends of WFM cloud water and 4 additional long-term cloud water and wet deposition datasets that have measured TOC or dissolved OC (DOC) throughout the Northeast US. These sites include Mt Washington, NH, Hubbard Brook NH, Thompson Farm NH, and Sleepers River Vermont. This work will also discuss potential hypotheses driving this increasing trend including increased biomass burning influence and increased biogenic emissions in the region. 

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2. Measurements of Total OH Reactivity During CalNex‐LA

   https://doi.org/10.1029/2020JD032988  

   Hansen, R. F.; Griffith, S. M.; Dusanter, S.; Gilman, J. B.; Graus, M.; Kuster, W. C.; Veres, P. R.; de Gouw, J. A.; Warneke, C.; Washenfelder, R. A.; et al (June 2021, Journal of Geophysical Research: Atmospheres)

   Abstract Total OH reactivity was measured during the California Research at the Nexus of Air Quality and Climate Change field campaign at the Pasadena ground site using a turbulent flow tube reactor with laser‐induced fluorescence detection of the OH radical. Collocated measurements of volatile organic compounds (VOCs), inorganic species, and meteorological parameters were made and used to calculate the total OH reactivity, which was then compared to the measured values. An analysis of the OH reactivity measurements finds that although the measured reactivity correlated well with the calculated reactivity, the measurements were consistently greater than the calculations for all times during the day, with an average missing OH reactivity of 8–10 s⁻¹, accounting for approximately 40% of the measured total OH reactivity. An analysis of correlations with both anthropogenic tracers of combustion and oxygenated VOCs as well as air trajectories during the campaign suggest that the missing OH reactivity was likely due to a combination of both unmeasured local emissions and unmeasured oxidation products transported to the site. Approximately 50% of the missing OH reactivity may have been due to emissions of unmeasured volatile chemical products, such as pesticides, cleaning agents, and personal care products. 

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3. Reconciling the total carbon budget for boreal forest wildfire emissions using airborne observations

   https://doi.org/10.5194/acp-22-12493-2022  

   Hayden, Katherine L.; Li, Shao-Meng; Liggio, John; Wheeler, Michael J.; Wentzell, Jeremy J.; Leithead, Amy; Brickell, Peter; Mittermeier, Richard L.; Oldham, Zachary; Mihele, Cristian M.; et al (September 2022, Atmospheric Chemistry and Physics)

   Wildfire impacts on air quality and climate are expected to be exacerbatedby climate change with the most pronounced impacts in the boreal biome.Despite the large geographic coverage, there is limited information onboreal forest wildfire emissions, particularly for organic compounds, whichare critical inputs for air quality model predictions of downwind impacts.In this study, airborne measurements of 193 compounds from 15 instruments,including 173 non-methane organics compounds (NMOG), were used to providethe most detailed characterization, to date, of boreal forest wildfireemissions. Highly speciated measurements showed a large diversity ofchemical classes highlighting the complexity of emissions. Usingmeasurements of the total NMOG carbon (NMOGT), the ΣNMOG wasfound to be 50 % ± 3 % to 53 % ± 3 % of NMOGT, of which, theintermediate- and semi-volatile organic compounds (I/SVOCs) were estimatedto account for 7 % to 10 %. These estimates of I/SVOC emission factorsexpand the volatility range of NMOG typically reported. Despite extensivespeciation, a substantial portion of NMOGT remained unidentified(47 % ± 15 % to 50 % ± 15 %), with expected contributions from morehighly-functionalized VOCs and I/SVOCs. The emission factors derived in thisstudy improve wildfire chemical speciation profiles and are especiallyrelevant for air quality modelling of boreal forest wildfires. Theseaircraft-derived emission estimates were further linked with those derivedfrom satellite observations demonstrating their combined value in assessingvariability in modelled emissions. These results contribute to theverification and improvement of models that are essential for reliablepredictions of near-source and downwind pollution resulting from borealforest wildfires. 

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4. Sulfur isotopes of sulfate measurements from a Greenland ice core (1200-1850) and volcanic gas measurements from various volcanoes and hot springs in Iceland

   https://doi.org/10.18739/A2N873162  

   Jongebloed, Ursula; Alexander, Becky; Cole-Dai, Jihong; Schauer, Andrew; Larrick, Carleigh; Wood, Robert; Fischer, Tobias; Carn, Simon; Salimi, Sara; Edouard, Shana; et al (January 2022, NSF Arctic Data Center)

   The Arctic is warming at almost four times the global rate. Cooling caused by anthropogenic aerosols has been estimated to offset sixty percent of greenhouse-gas-induced Arctic warming, but the contribution of aerosols to radiative forcing (RF) represents the largest uncertainty in estimating total RF, largely due to unknown preindustrial aerosol abundance. Here, sulfur isotope measurements in a Greenland ice core show that passive volcanic degassing contributes up to 66 ± 10% of preindustrial ice core sulfate in years without major eruptions. A state-of-the-art model indicates passive volcanic sulfur emissions influencing the Arctic are underestimated by up to a factor of three, possibly because many volcanic inventories do not include hydrogen sulfide emissions. Higher preindustrial volcanic sulfur emissions reduce modeled anthropogenic Arctic aerosol cooling by up to a factor of two (+0.11 to +0.29 W m-2 (watts per square meter)), suggesting that underestimating passive volcanic sulfur emissions has significant implications for anthropogenic-induced Arctic climate change. These data include sulfur isotopes of sulfate measurements from a Greenland ice core and volcanic gas measurements (CO2:S (carbon dioxide:sulfur) ratios) from various volcanoes and hot springs in Iceland. 

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5. Emissions of Trace Organic Gases From Western U.S. Wildfires Based on WE‐CAN Aircraft Measurements

   https://doi.org/10.1029/2020JD033838  

   Permar, Wade; Wang, Qian; Selimovic, Vanessa; Wielgasz, Catherine; Yokelson, Robert J.; Hornbrook, Rebecca S.; Hills, Alan J.; Apel, Eric C.; Ku, I‐Ting; Zhou, Yong; et al (June 2021, Journal of Geophysical Research: Atmospheres)

   Abstract We present emission measurements of volatile organic compounds (VOCs) for western U.S. wildland fires made on the NSF/NCAR C‐130 research aircraft during the Western Wildfire Experiment for Cloud Chemistry, Aerosol Absorption, and Nitrogen (WE‐CAN) field campaign in summer 2018. VOCs were measured with complementary instruments onboard the C‐130, including a proton‐transfer‐reaction time‐of‐flight mass spectrometer (PTR‐ToF‐MS) and two gas chromatography (GC)‐based methods. Agreement within combined instrument uncertainties (<60%) was observed for most co‐measured VOCs. GC‐based measurements speciated the isomeric contributions to selected PTR‐ToF‐MS ion masses and generally showed little fire‐to‐fire variation. We report emission ratios (ERs) and emission factors (EFs) for 161 VOCs measured in 31 near‐fire smoke plume transects of 24 specific individual fires sampled in the afternoon when burning conditions are typically most active. Modified combustion efficiency (MCE) ranged from 0.85 to 0.94. The measured campaign‐average total VOC EF was 26.1 ± 6.9 g kg⁻¹, approximately 67% of which is accounted for by oxygenated VOCs. The 10 most abundantly emitted species contributed more than half of the total measured VOC mass. We found that MCE alone explained nearly 70% of the observed variance for total measured VOC emissions (r² = 0.67) and >50% for 57 individual VOC EFs representing more than half the organic carbon mass. Finally, we found little fire‐to‐fire variability for the mass fraction contributions of individual species to the total measured VOC emissions, suggesting that a single speciation profile can describe VOC emissions for the wildfires in coniferous ecosystems sampled during WE‐CAN. 

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