Evolution of Acyl Peroxynitrates (PANs) in Wildfire Smoke Plumes Detected by the Cross‐Track Infrared Sounder (CrIS) Over the Western U.S. During Summer 2018
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We characterise the vertical distribution of biomass-burning emissions across the Amazon during the biomass-burning season (July–November) with an extensive climatology of smoke plumes derived from MISR and MODIS (2005–2012) and CALIOP (2006–2012) observations. Smoke plume heights exhibit substantial variability, spanning a few hundred metres up to 6 km above the terrain. However, the majority of the smoke is located at altitudes below 2.5 km. About 60 % of smoke plumes are observed in drought years, 40 %–50 % at the peak month of the burning season (September) and 94 % over tropical forest and savanna regions, with respect to the total number of smoke plume observations. At the time of the MISR observations (10:00–11:00 LT), the highest plumes are detected over grassland fires (with an averaged maximum plume height of ∼1100 m) and the lowest plumes occur over tropical forest fires (∼800 m). A similar pattern is found later in the day (14:00–15:00 LT) with CALIOP, although at higher altitudes (2300 m grassland vs. 2000 m tropical forest), as CALIOP typically detects smoke at higher altitudes due to its later overpass time, associated with a deeper planetary boundary layer, possibly more energetic fires, and greater sensitivity to thin aerosol layers. On average, 3 %–20 % of the fires inject smoke into the free troposphere; this percentage tends to increase toward the end of the burning season (November: 15 %–40 %). We find a well-defined seasonal cycle between MISR plume heights, MODIS fire radiative power and atmospheric stability across the main biomes of the Amazon, with higher smoke plumes, more intense fires and reduced atmospheric stability conditions toward the end of the burning season. Lower smoke plume heights are detected during drought (800 m) compared to non-drought (1100 m) conditions, in particular over tropical forest and savanna fires. Drought conditions favour understory fires over tropical forest, which tend to produce smouldering combustion and low smoke injection heights. Droughts also seem to favour deeper boundary layers and the percentage of smoke plumes that reach the free troposphere is lower during these dry conditions. Consistent with previous studies, the MISR mid-visible aerosol optical depth demonstrates that smoke makes a significant contribution to the total aerosol loading over the Amazon, which in combination with lower injection heights in drought periods has important implications for air quality. This work highlights the importance of biome type, fire properties and atmospheric and drought conditions for plume dynamics and smoke loading. In addition, our study demonstrates the value of combining observations of MISR and CALIOP constraints on the vertical distribution of smoke from biomass burning over the Amazon.
The Pacific Northwest region of the United States and Canada has become more vulnerable to intense wildfire regimes due to years of fire suppression and climatic changes. Smoke from fires exposes communities to hazardous aerosols and pollutants known to trigger asthma symptoms and exacerbate other respiratory and cardiovascular diseases. In partnership with The Nature Conservancy’s Washington Chapter and the Puget Sound Clean Air Agency, NASA DEVELOP investigated the impacts of wildfire smoke on air quality from 2008 to 2020 using NASA Earth observations. To explore the various dimensions of smoke and its relation to air quality, the team looked at the vertical extent of smoke plumes and the resulting changes in air quality. The team evaluated the potential relationship between plume height of wildfire smoke and fire radiative power using the Moderate Resolution Imaging Spectroradiometer (MODIS) aboard the Aqua and Terra satellites and Terra’s Multi-angle Imaging SpectroRadiometer (MISR) using the MISR INteractive eXplorer (MINX). The team determined that there was no regional relationship between fire radiative power and smoke plume height. To investigate changes in air quality resulting from wildfire smoke, the team utilized data from NASA’s Fire Information for Resource Management System, from the European Space Agency’s Sentinel-5P Tropospheric Monitoring Instrument (TROPOMI), and true color imagery from Landsat 8 Operational Land Imager (OLI). The team created a Google Earth Engine-based (GEE) web tool to visualize changes in atmospheric pollutants and aerosol optical depth. Results of case study fires showed varying increases in pollutant concentrations when compared to a baseline map. The end products provided the partners with tools to quantify plume height using MINX and to visualize recent air quality patterns relating to variations in wildfire extent and severity in the Pacific Northwest
In order to improve aerosol representation in the NASA Goddard Earth Observing System (GEOS) model, we evaluated simulations of the aerosol properties and transport over the southern African biomass burning source and outflow region using observations made during the first deployment of the ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) field campaign in September 2016. An example case study of September 24 was analyzed in detail, during which aircraft-based in-situ and remote sensing observations showed the presence of a multi-layered smoke plume structure with significant vertical variation in single scattering albedo (SSA). Our baseline GEOS simulations were not able to represent the observed SSA variation, nor the observed organic aerosol-to-black carbon ratio (OA : BC). Analyzing the simulated smoke age suggests that the higher altitude, less absorbing smoke plume was younger (~4 days), while the lower altitude and more absorbing smoke plume was older (~7 days). We hypothesize a chemical or microphysical loss process exists to explain the change in aerosol absorption as the smoke plume ages, and we apply a simple 6-day e-folding loss rate to the model hydrophilic biomass burning OA to mimic this process. Adding this loss process required some adjustment to the model assumed scaling factors of aerosol emissions to conserve the regional aerosol loading and further improve the simulated OA : BC ratio. Accordingly, we have increased our biomass burning emissions of OA by 60 % and biomass burning BC by 15 %. We also utilized the ORACLES airborne observations to better constrain the simulation of aerosol optical properties, adjusting the assumed particle size, hygroscopic growth, and absorption. Our final GEOS model simulation with additional OA loss and updated optics showed a better performance in simulating AOD and SSA compared to independent ground and space-based retrievals for the entire month of September 2016, including the OMI Aerosol Index. In terms of radiative implications of our model adjustments, the final GEOS simulation suggested a decreased atmospheric warming of about 10 % (~2 W m -2 ) over the south-east Atlantic region and above the stratocumulus cloud decks compared to the model baseline simulations. These results improve the representation of the smoke age, transport, and optical properties in Earth system models.
Abstract. The evolution of organic aerosol (OA) and aerosol size distributions within smoke plumes is uncertain due to the variability in rates of coagulation and OA condensation/evaporation between different smoke plumes and at different locations within a single plume. We use aircraft data from the FIREX-AQ campaign to evaluate differences in evolving aerosol size distributions, OA, and oxygen to carbon ratios (O:C) between and within smoke plumes during the first several hours of aging as a function of smoke concentration. The observations show that the median particle diameter increases 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 enhancement ratios – than smoke of a lower initial OA concentration (<100 µg m−3), which had net increases in OA. Observations of OA and O:C suggest that evaporation and/or secondary OA formation was greater in less concentrated smoke prior to the first measurement (5–57 min after emission). We simulate the size changes due to coagulation and dilution and adjust for OA condensation/evaporation based on the observed changes in OA. We found that coagulation explains the majority of the diameter growth, with OA evaporation/condensation having a relatively minor impact. We found that mixing between the core and edges of the plume generally occurred on timescales of hours, slow enough to maintain differences in aging between core and edge but too fast to ignore the role of mixing for most of our cases.
NASA's ERTS-1 satellite, with its high resolution and multispectral capabilities, has been found useful in the detection and analysis of smoke from large point sources (power plants, steel mills, etc.), and widespread atmospheric turbidity associated with atmospheric stagnations. Smoke plumes from the Chicago-Northern Indiana industrial complex have been tracked over Lake Michigan for over 100 km. Experience has shown that smoke plumes are relatively easy to detect over water (in the 0.6-0.7 micrometer band) but much more difficult over land surfaces. Pattern recognition techniques (cluster analysis) were applied to the digital ERTS data, and it was found that the smoke plumes indeed had a unique spectral signature. Studies are currently underway to use measured plume geometries to obtain quantitative estimates of diffusion over water surfaces.
In this paper, we present aerosol retrieval results from the ACEPOL (Aerosol Characterization from Polarimeter and Lidar) campaign, which was a joint initiative between NASA and SRON – the Netherlands Institute for Space Research. The campaign took place in October–November 2017 over the western part of the United States. During ACEPOL six different instruments were deployed on the NASA ER-2 high-altitude aircraft, including four multi-angle polarimeters (MAPs): SPEX airborne, the Airborne Hyper Angular Rainbow Polarimeter (AirHARP), the Airborne Multi-angle SpectroPolarimetric Imager (AirMSPI), and the Research Scanning Polarimeter (RSP). Also, two lidars participated: the High Spectral Resolution Lidar-2 (HSRL-2) and the Cloud Physics Lidar (CPL). Flights were conducted mainly for scenes with low aerosol load over land, but some cases with higher AOD were also observed. We perform aerosol retrievals from SPEX airborne, RSP (410–865 nm range only), and AirMSPI using the SRON aerosol retrieval algorithm and compare the results against AERONET (AErosol RObotic NETwork) and HSRL-2 measurements (for SPEX airborne and RSP). All three MAPs compare well against AERONET for the aerosol optical depth (AOD), with a mean absolute error (MAE) between 0.014 and 0.024 at 440 nm. For the fine-mode effective radius the MAE ranges between 0.021 and 0.028 µm. For the comparison with HSRL-2 we focus on a day with low AOD (0.02–0.14 at 532 nm) over the California Central Valley, Arizona, and Nevada (26 October) as well as a flight with high AOD (including measurements with AOD>1.0 at 532 nm) over a prescribed forest fire in Arizona (9 November). For the day with low AOD the MAEs in AOD (at 532 nm) with HSRL-2 are 0.014 and 0.022 for SPEX and RSP, respectively, showing the capability of MAPs to provide accurate AOD retrievals for the challenging case of low AOD over land. For the retrievals over the smoke plume a reasonable agreement in AOD between the MAPs and HSRL-2 was also found (MAE 0.088 and 0.079 for SPEX and RSP, respectively), despite the fact that the comparison is hampered by large spatial variability in AOD throughout the smoke plume. A good comparison is also found between the MAPs and HSRL-2 for the aerosol depolarization ratio (a measure of particle sphericity), with an MAE of 0.023 and 0.016 for SPEX and RSP, respectively. Finally, SPEX and RSP agree very well for the retrieved microphysical and optical properties of the smoke plume.
During the 2019/2020 fire season, Australian bushfires burned 46 million acres, killed 39 people and billions of animals, and became the costlier fire season in Australian history. Between the end of December and early January, a series of pyrocumulonimbus injected thick smoke layers in the upper troposphere and lower stratosphere which were observed over the Tasmanian Sea and New Zealand by the Ozone Mapping and Profiler Suite (OMPS) and the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO). The smoke plume crossed the tropopause and was further dispersed across the Eastern Pacific Ocean rising up to 30 km height after two weeks. . In this study, we use CALIPSO and the NASA Langley Trajectory Model (LaTM), driven by Modern-Era Retrospective analysis for Research and Application, Version 2 (MERRA-2) meteorological data, to track the dispersion of Australian fire smoke plumes in both the troposphere and the stratosphere. Trajectory mapping is used to re-construct the 3-dimension structure of the smoke plumes. Results are compared with independent observations from the Stratospheric Aerosol and Gas Experiment (SAGE) III on the International Space Station (ISS) to understand the complex transport of the plume into the stratosphere and its lifetime. Using trajectory maps, the impact of the Australian bushfires on the Earth’s radiative energy budget is assessed with the Clouds and the Earth’s Radiant Energy System (CERES).
During the 2019/2020 fire season, Australian bushfires burned 46 million acres, killed 39 people and billions of animals, and became the costlier fire season in Australian history. Between the end of December and early January, a series of pyrocumulonimbus injected thick smoke layers in the upper troposphere and lower stratosphere which were observed over the Tasmanian Sea and New Zealand by the Ozone Mapping and Profiler Suite (OMPS) and the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO). The smoke plume crossed the tropopause and was further dispersed across the Eastern Pacific Ocean rising up to 30 km height after two weeks. . In this study, we use CALIPSO and the NASA Langley Trajectory Model (LaTM), driven by Modern-Era Retrospective analysis for Research and Application, Version 2 (MERRA-2) meteorological data, to track the dispersion of Australian fire smoke plumes in both the troposphere and the stratosphere. Trajectory mapping is used to re-construct the 3-dimension structure of the smoke plumes. Results are compared with independent observations from the Stratospheric Aerosol and Gas Experiment (SAGE) III on the International Space Station (ISS) to understand the complex transport of the plume into the stratosphere and its lifetime. Using trajectory maps, the impact of the Australian bushfires on the Earth’s radiative energy budget is assessed with the Clouds and the Earth’s Radiant Energy System (CERES).
During the 2019 Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) study, the NASA DC-8 carried out in situ chemical measurements in smoke plumes emitted from wildfires and agricultural fires in the contiguous United States. The DC-8 payload included a modified proton-transfer-reaction time-of-flight mass spectrometer (PTR-ToF-MS) for the fast measurement of gaseous ammonia (NH 3 ) and a high-resolution time-of-flight aerosol mass spectrometer (AMS) for the fast measurement of submicron particulate ammonium (NH 4 + ). We herein report data collected in smoke plumes emitted from 6 wildfires in the Western United States, 2 prescribed grassland fires in the Central United States, 1 prescribed forest fire in the Southern United States, and 66 small agricultural fires in the Southeastern United States. Smoke plumes contained double to triple digit ppb levels of NH 3 . In the wildfire plumes, a significant fraction of NH 3 had already been converted to NH 4 + at the time of sampling (≥2 h after emission). Substantial amounts of NH 4 + were also detected in freshly emitted smoke from corn and rice field fires. We herein present a comprehensive set of emission factors of NH 3 and NH x , with NH x = NH 3 + NH 4 + . Average NH 3 and NH x emission factors for wildfires in the Western United States were 1.86±0.75 g kg −1 and 2.47±0.80 g kg −1 of fuel burned, respectively. Average NH 3 and NH x emission factors for agricultural fires in the Southeastern United States were 0.89±0.58 and 1.74±0.92 g kg −1 , respectively. Our data show no clear inverse correlation between modified combustion efficiency (MCE) and NH 3 emissions. The observed NH 3 emissions were significantly higher than measured in previous laboratory experiments in the FIREX FireLab 2016 study.
Wildfire activity in the western United States during August to October 2020 was exceptional in terms of the fire severity and area burned. Extremely dry biomass fuels from near historic multi-year drought conditions were further exacerbated with very hot and dry conditions in 2020. These conditions when coupled with strong offshore flow allowed many ignitions to grow into extremely large and severe wildfires. Long-term monitoring at a few AERONET sites in California showed that the number of days with high Aerosol Optical Depth at 440 nm (AOD 440 >1) in 2020 was greater than any other year going back to the beginning of the data records in 2002. A wide range of fine mode particle volume median radii were retrieved from AERONET data over the course of these fires suggesting significant variability in combustion conditions and aging processes. Additionally, the fine mode radii in some of these smoke plumes in 2020 were very large especially at high AOD (∼0.22–0.32 μm volume median radius), likely due to both coagulation and condensation occurring during aging at very high particulate concentrations. The largest fine mode particle radii combined with narrow distributions resulted in some very rare AOD spectra showing peak AOD at 500 nm and decreasing to lower AOD at both shorter and longer wavelengths. The most extreme retrieved size distributions and associated measured AOD spectra were principally observed in long-distance transported smoke plumes from these western United States fires at sites in Colorado, Maryland and Virginia, possibly due to further aging during transport. Additionally, strong absorption was sometimes observed at short wavelengths with much lower single scattering albedo at 440 nm compared to 675 nm in some plumes consistent with significant brown carbon (BrC) and/or coated black carbon (BC) absorption in biomass burning particles. This strong spectral absorption signature observed at some California sites and dates remained similarly strong in some smoke plumes observed at some east coast sites in Maryland and Virginia, thereby suggesting that the lifetime of these particular BrC and/or coated BC absorbing species was greater than 5 days.
The effects of biomass burning aerosols (BBA) on radiative forcing and cloud formation depend on chemical composition and the internal structures of individual particles within smoke plumes. To improve our understanding of the chemical and physical properties of BBA emitted at different times of the day and their evolution during atmospheric aging, we conducted a study as a part of the Fire Influence on Regional to Global Environments and Air Quality field campaign. Particle samples were collected onboard a research aircraft from smoke plumes from a wildfire in eastern Oregon during late afternoon and nighttime flights on August 28, 2019. A time-resolved aerosol collector was used to collect samples on substrates for offline spectromicroscopic imaging to investigate the single-particle characteristics of BBA particles. Approximately 20,400 individual particles from 10 selected samples were analyzed using computer-controlled scanning electron microscopy coupled with energy-dispersive X-ray microanalysis, revealing their elemental composition, morphology, and viscosity. Elemental microanalysis indicated that aged potassium is likely found in the form of K 2 SO 4 , KNO 3 , and possible K-organic salts. Further chemical speciation and carbon bonding mapping within individual particles were conducted using synchrotron-based scanning transmission X-ray microscopy (STXM) coupled with near edge X-ray absorption fine structure (NEXAFS) spectroscopy. Real-time, water-soluble light absorption measurements were acquired using a particle-into-liquid sampler instrument coupled to a liquid waveguide capillary cell and total organic analyzer. In the late afternoon samples, 65% of the total particle number population consisted entirely of organic components, compared to 46% in the nighttime particles. These differences were attributed to discrepancies in composition at the time of emission and to the daytime condensation and accumulation of photochemically formed secondary organic material on existing BBA particles, a process that halts at night. Microscopy images indicated that particle viscosity was lower in the nighttime particles (<10 1 Pa·s), likely due to increased relative humidity and a higher contribution from hygroscopic inorganic components. The chemical heterogeneity of individual particles was quantified using STXM-derived mixing state parameters. The nature of carbon bonding within individual particles was inferred from the extent of carbon sp 2 hybridization derived from NEXAFS spectra. Average percentages of sp 2 hybridization range between 40% and 60%, with no noticeable differences between late afternoon and nighttime flights. These findings were compared with the online optical properties of both late afternoon and nighttime smoke plumes, providing valuable insights into the complex relationship between chemical composition and optical properties of BBA particles at different times of the day.
The optical and chemical properties of biomass burning (BB) smoke particles greatly affect the impact that wildfires have on climate and air quality. Previous work has demonstrated some links between smoke properties and factors such as fuel type and meteorology. However, the factors controlling BB particle speciation at emission are not adequately understood nor are the factors driving particle aging during atmospheric transport. As such, modeling wildfire smoke impacts on climate and air quality remains challenging. The potential to provide robust, statistical characterizations of BB particles based on ecosystem type and ambient environmental conditions with remote sensing data is investigated here. Space-based Multi-angle Imaging SpectroRadiometer (MISR) observations, combined with the MISR Research Aerosol (RA) algorithm and the MISR Interactive Explorer (MINX) tool, are used to retrieve smoke plume aerosol optical depth (AOD) and to provide constraints on plume vertical extent; smoke age; and particle size, shape, light-absorption properties, and absorption spectral dependence. These tools are applied to numerous wildfire plumes in Canada and Alaska, across a range of conditions, to create a regional inventory of BB particle-type temporal and spatial distribution. We then statistically compare these results with satellite measurements of fire radiative power (FRP) and land cover characteristics, as well as short-term climate, meteorological, and drought information from the Modern-Era Retrospective analysis for Research and Applications (MERRA-2) reanalysis and the North American Drought Monitor. We find statistically significant differences in the retrieved smoke properties based on land cover type, with fires in forests producing the thickest plumes containing the largest, brightest particles and fires in savannas and grasslands exhibiting the opposite. Additionally, the inferred dominant aging mechanisms and the timescales over which they occur vary systematically between land types. This work demonstrates the potential of remote sensing to constrain BB particle properties and the mechanisms governing their evolution over entire ecosystems. It also begins to realize this potential, as a means of improving regional and global climate and air quality modeling in a rapidly changing world.