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The Arctic warms nearly four times faster than the global average, and aerosols play an increasingly important role in Arctic climate change. In the Arctic, sea salt is a major aerosol component in terms of mass concentration during winter and spring. However, the mechanisms of sea salt aerosol production remain unclear. Sea salt aerosols are typically thought to be relatively large in size but low in number concentration, implying that their influence on cloud condensation nuclei population and cloud properties is generally minor. Here we present observational evidence of abundant sea salt aerosol production from blowing snow in the central Arctic. Blowing snow was observed more than 20% of the time from November to April. The sublimation of blowing snow generates high concentrations of fine-mode sea salt aerosol (diameter below 300 nm), enhancing cloud condensation nuclei concentrations up to tenfold above background levels. Using a global chemical transport model, we estimate that from November to April north of 70° N, sea salt aerosol produced from blowing snow accounts for about 27.6% of the total particle number, and the sea salt aerosol increases the longwave emissivity of clouds, leading to a calculated surface warming of +2.30 W m⁻²under cloudy sky conditions.

 

Previous research on the health and air quality impacts of wildfire smoke has largely focused on the impact of smoke on outdoor air quality; however, many people spend a majority of their time indoors. The quality of indoor air on smoke-impacted days is largely unknown. In this analysis, we use publicly available data from an existing large network of low-cost indoor and outdoor fine particulate matter (PM_2.5) monitors to quantify the relationship between indoor and outdoor particulate air quality on smoke-impacted days in 2020 across the western United States (US). We also investigate possible regional and socioeconomic trends in this relationship for regions surrounding six major cities in the western US. We find indoor PM_2.5concentrations are 82% or 4.2µg m⁻³(median across all western US indoor monitors for the year 2020; interquartile range, IQR: 2.0–7.2µg m⁻³) higher on smoke-impacted days compared to smoke-free days. Indoor/outdoor PM_2.5ratios show variability by region, particularly on smoke-free days. However, we find the ratio of indoor/outdoor PM_2.5is less than 1 (i.e. indoor concentrations lower than outdoor) at nearly all indoor-outdoor monitor pairs on smoke-impacted days. Although typically lower than outdoor concentrations on smoke-impacted days, we find that on heavily smoke-impacted days (outdoor PM_2.5> 55µg m⁻³), indoor PM_2.5concentrations can exceed the 35µg m⁻³24 h outdoor standard set by the US Environmental Protection Agency. Further, total daily-mean indoor PM_2.5concentrations increase by 2.1µg m⁻³with every 10µg m⁻³increase in daily-mean outdoor PM_2.5.(median of statistically significant linear regression slopes across all western US monitor pairs; IQR: 1.0–4.3µg m⁻³) on smoke-impacted days. These results show that for indoor environments in the western US included in our analysis, remaining indoors during smoke events is currently an effective, but limited, strategy to reduce PM_2.5exposure.

 

Phase One of the Transportation and Transformation of Ammonia (TRANS²Am) field campaign took place in northeastern Colorado during the summer of 2021. One of the goals of TRANS²Am was to measure ammonia (NH₃) emissions from cattle feedlots and dairies. Most of these animal husbandry facilities are co‐located within oil and gas development, an important source of methane (CH₄) and ethane (C₂H₆) in the region. Phase One of TRANS²Am included 12 near‐source research flights. We present estimates of NH₃emissions ratios with respect to CH₄(NH₃EmR), with and without correction of CH₄from oil and gas, for 29 feedlots and dairies in the region. The data shows larger emissions ratios than previously reported in the literature with a large range of values (i.e., 0.1–2.6 ppbv ppbv⁻¹). Facilities housing cattle and dairy had a mean (std) of 1.20 (0.63) and 0.29 (0.08) ppbv ppbv⁻¹, respectively. We also found that only 15% of the total ammonia (NH_x) is in the particle phase (i.e., ) near major sources during the warm summertime months. We examined the evolution of NH₃in one plume that was sampled at different distances and altitudes up to 25 km downwind and estimated the NH₃lifetime against deposition and partitioning to the particle phase to be 87–120 min. Finally, we calculated estimates of NH₃emission rates from four optimally sampled facilities. These ranged from 4 to 29 g NH₃ · h⁻¹ · hd⁻¹.

 

Abstract. The impact of biomass burning (BB) on the atmospheric burden of volatile organic compounds (VOCs) is highly uncertain. Here we apply the GEOS-Chemchemical transport model (CTM) to constrain BB emissions in the western USA at ∼ 25 km resolution. Across three BB emission inventorieswidely used in CTMs, the inventory–inventory comparison suggests that the totals of 14 modeled BB VOC emissions in the western USA agree with eachother within 30 %–40 %. However, emissions for individual VOCs can differ by a factor of 1–5, driven by the regionally averaged emissionratios (ERs, reflecting both assigned ERs for specific biome and vegetation classifications) across the three inventories. We further evaluate GEOS-Chemsimulations with aircraft observations made during WE-CAN (Western Wildfire Experiment for Cloud Chemistry, Aerosol Absorption and Nitrogen) andFIREX-AQ (Fire Influence on Regional to Global Environments and Air Quality) field campaigns. Despite being driven by different global BBinventories or applying various injection height assumptions, the model–observation comparison suggests that GEOS-Chem simulations underpredictobserved vertical profiles by a factor of 3–7. The model shows small to no bias for most species in low-/no-smoke conditions. We thus attribute thenegative model biases mostly to underestimated BB emissions in these inventories. Tripling BB emissions in the model reproduces observed verticalprofiles for primary compounds, i.e., CO, propane, benzene, and toluene. However, it shows no to less significant improvements for oxygenatedVOCs, particularly for formaldehyde, formic acid, acetic acid, and lumped ≥ C3 aldehydes, suggesting the model is missing secondarysources of these compounds in BB-impacted environments. The underestimation of primary BB emissions in inventories is likely attributable tounderpredicted amounts of effective dry matter burned, rather than errors in fire detection, injection height, or ERs, as constrained by aircraftand ground measurements. We cannot rule out potential sub-grid uncertainties (i.e., not being able to fully resolve fire plumes) in the nestedGEOS-Chem which could explain the negative model bias partially, though back-of-the-envelope calculation and evaluation using longer-term groundmeasurements help support the argument of the dry matter burned underestimation. The total ERs of the 14 BB VOCs implemented in GEOS-Chem onlyaccount for half of the total 161 measured VOCs (∼ 75 versus 150 ppb ppm−1). This reveals a significant amount of missing reactiveorganic carbon in widely used BB emission inventories. Considering both uncertainties in effective dry matter burned (× 3) and unmodeledVOCs (× 2), we infer that BB contributed to 10 % in 2019 and 45 % in 2018 (240 and 2040 Gg C) of the total VOC primaryemission flux in the western USA during these two fire seasons, compared to only 1 %–10 % in the standard GEOS-Chem. 

Wildfires are an important atmospheric source of primary organic aerosol (POA) and precursors for secondary organic aerosol (SOA) at regional and global scales. However, there are large uncertainties surrounding the emissions and physicochemical processes that control the transformation, evolution, and properties of POA and SOA in large wildfire plumes. We develop a plume version of a kinetic model to simulate the dilution, oxidation chemistry, thermodynamic properties, and microphysics of organic aerosol (OA) in wildfire smoke. The model is applied to study the in-plume OA in four large wildfire smoke plumes intercepted during an aircraft-based field campaign in summer 2018 in the western United States. Based on estimates of dilution and oxidant concentrations before the aircraft first intercepted the plumes, we simulate the OA evolution from very close to the fire to several hours downwind. Our model results and sensitivity simulations suggest that dilution-driven evaporation of POA and simultaneous photochemical production of SOA are likely to explain the observed evolution in OA mass with physical age. The model, however, substantially underestimates the change in the oxygen-to-carbon ratio of the OA compared to measurements. In addition, we show that the rapid chemical transformation within the first hour after emission is driven by higher-than-ambient OH concentrations (3×10 6 -10 7 molecules cm -3 ) and the slower evolution over the next several hours is a result of lower-than-ambient OH concentrations (<10 6 molecules cm -3 ) and depleted SOA precursors. Model predictions indicate that the OA measured several hours downwind of the fire is still dominated by POA but with an SOA fraction that varies between 30% and 56% of the total OA. Semivolatile, heterocyclic, and oxygenated aromatic compounds, in that order, were found to contribute substantially (>90%) to SOA formation. Future work needs to focus on better understanding the dynamic evolution closer to the fire and resolving the rapid change in the oxidation state of OA with physical age. 

Abstract. The evolution of organic aerosol (OA) and aerosol sizedistributions within smoke plumes is uncertain due to the variability inrates of coagulation and OA condensation/evaporation between different smokeplumes and at different locations within a single plume. We use aircraftdata from the FIREX-AQ campaign to evaluate differences in evolving aerosolsize distributions, OA, and oxygen to carbon ratios (O:C) between and withinsmoke plumes during the first several hours of aging as a function of smokeconcentration. The observations show that the median particle diameterincreases faster in smoke of a higher initial OA concentration (>1000 µg m−3), with diameter growth of over 100 nm in 8 h – despite generally having a net decrease in OA enhancementratios – than smoke of a lower initial OA concentration (<100 µg m−3), which had net increases in OA. Observations of OA and O:Csuggest that evaporation and/or secondary OA formation was greater in lessconcentrated smoke prior to the first measurement (5–57 min afteremission). We simulate the size changes due to coagulation and dilution andadjust for OA condensation/evaporation based on the observed changes in OA.We found that coagulation explains the majority of the diameter growth, withOA evaporation/condensation having a relatively minor impact. We found thatmixing between the core and edges of the plume generally occurred ontimescales of hours, slow enough to maintain differences in aging betweencore and edge but too fast to ignore the role of mixing for most of our cases.