Search for: All records

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 Atmospheric ice nucleating particles (INPs) influence global climate by altering cloud formation, lifetime, and precipitation efficiency. The role of secondary organic aerosol (SOA) material as a source of INPs in the ambient atmosphere has not been well defined. Here, we demonstrate the potential for biogenic SOA to activate as depositional INPs in the upper troposphere by combining field measurements with laboratory experiments. Ambient INPs were measured in a remote mountaintop location at –46 °C and an ice supersaturation of 30% with concentrations ranging from 0.1 to 70 L –1 . Concentrations of depositional INPs were positively correlated with the mass fractions and loadings of isoprene-derived secondary organic aerosols. Compositional analysis of ice residuals showed that ambient particles with isoprene-derived SOA material can act as depositional ice nuclei. Laboratory experiments further demonstrated the ability of isoprene-derived SOA to nucleate ice under a range of atmospheric conditions. We further show that ambient concentrations of isoprene-derived SOA can be competitive with other INP sources. This demonstrates that isoprene and potentially other biogenically-derived SOA materials could influence cirrus formation and properties. 

Abstract Weather and climate models are challenged by uncertainties and biases in simulating Southern Ocean (SO) radiative fluxes that trace to a poor understanding of cloud, aerosol, precipitation and radiative processes, and their interactions. Projects between 2016 and 2018 used in-situ probes, radar, lidar and other instruments to make comprehensive measurements of thermodynamics, surface radiation, cloud, precipitation, aerosol, cloud condensation nuclei (CCN) and ice nucleating particles over the SO cold waters, and in ubiquitous liquid and mixed-phase cloudsnucleating particles over the SO cold waters, and in ubiquitous liquid and mixed-phase clouds common to this pristine environment. Data including soundings were collected from the NSF/NCAR G-V aircraft flying north-south gradients south of Tasmania, at Macquarie Island, and on the RV Investigator and RSV Aurora Australis. Synergistically these data characterize boundary layer and free troposphere environmental properties, and represent the most comprehensive data of this type available south of the oceanic polar front, in the cold sector of SO cyclones, and across seasons. Results show a largely pristine environments with numerous small and few large aerosols above cloud, suggesting new particle formation and limited long-range transport from continents, high variability in CCN and cloud droplet concentrations, and ubiquitous supercooled water in thin, multi-layered clouds, often with small-scale generating cells near cloud top. These observations demonstrate how cloud properties depend on aerosols while highlighting the importance of confirmed low clouds were responsible for radiation biases. The combination of models and observations is examining how aerosols and meteorology couple to control SO water and energy budgets. 

Abstract Maritime boundary‐layer clouds over the Southern Ocean (SO) have a large shortwave radiative effect. Yet, climate models have difficulties in representing these clouds and, especially, their phase in this observationally sparse region. This study aims to increase the knowledge of SO cloud phase by presenting in‐situ cloud microphysical observations from the Southern Ocean Clouds, Radiation, Aerosol, Transport Experimental Study (SOCRATES). We investigate the occurrence of ice in summertime marine stratocumulus and cumulus clouds in the temperature range between 6 and −25°C. Our observations show that in ice‐containing clouds, maximum ice number concentrations of up to several hundreds per liter were found. The observed ice crystal concentrations were on average one to two orders of magnitude higher than the simultaneously measured ice nucleating particle (INP) concentrations in the temperature range below −10°C and up to five orders of magnitude higher than estimated INP concentrations in the temperature range above −10°C. These results highlight the importance of secondary ice production (SIP) in SO summertime marine boundary‐layer clouds. Evidence for rime splintering was found in the Hallett‐Mossop (HM) temperature range but the exact SIP mechanism active at lower temperatures remains unclear. Finally, instrument simulators were used to assess simulated co‐located cloud ice concentrations and the role of modeled HM rime‐splintering. We found that CAM6 is deficient in simulating number concentrations across the HM temperature range with little sensitivity to the model HM process, which is inconsistent with the aforementioned observational evidence of highly active SIP processes in SO low‐level clouds. 

Abstract Small cumulus clouds over the western United States were measured via airborne instruments during the wildfire season in summer of 2018. Statistics of the sampled clouds are presented and compared to smoke aerosol properties. Cloud droplet concentrations were enhanced in regions impacted by biomass burning smoke, at times exceeding 3,000 cm⁻³. Images and elemental composition of individual smoke particles and cloud droplet residuals are presented and show that most are dominantly organic, internally mixed with some inorganic elements. Despite their high organic content and relatively low hygroscopicity, on average about half of smoke aerosol particles >80 nm diameter formed cloud droplets. This reduced cloud droplet size in small, smoke‐impacted clouds. A number of complex and competing climatic impacts may result from wide‐spread reductions in cloud droplet size due to wildfires prevalent across the region during summer months. 

Abstract Wildfires in the western United States are large sources of particulate matter, and the area burned by wildfires is predicted to increase in the future. Some particles released from wildfires can affect cloud formation by serving as ice‐nucleating particles (INPs). INPs have numerous impacts on cloud radiative properties and precipitation development. Wildfires are potentially important sources of INPs, as indicated from previous measurements, but their abundance in the free troposphere has not been quantified. The Western Wildfire Experiment for Cloud Chemistry, Aerosol Absorption, and Nitrogen campaign sampled free tropospheric immersion‐freezing INPs from smoke plumes near their source and downwind, along with widespread aged smoke. The results indicate an enhancement of INPs in smoke plumes relative to out‐of‐plume background air, but the magnitude of enhancement was both temperature and fire dependent. The majority of INPs were inferred to be predominately organic in composition with some contribution from biological sources at modest super cooling, and contributions from minerals at deeper super cooling. A fire involving primarily sagebrush shrub land and aspen forest fuels had the highest INP concentrations measured in the campaign, which is partially attributed to the INP characteristics of lofted, uncombusted plant material. Electron microscopy analysis of INPs also indicated tar balls present in this fire. Parameterization of the plume INP data on a per‐unit‐aerosol surface area basis confirmed that smoke is not an efficient source of INPs. Nevertheless, the high numbers of particles released from, and ubiquity of western US wildfires in summertime, regionally elevate INP concentrations in the free troposphere. 

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.