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At least 523 records · Page 29

Hydrodynamic Suppression of Soot Formation in Laminar Coflowing Jet Diffusion Flames

Effects of flow (hydrodynamic) properties on limiting conditions for soot-free laminar non-premixed hydrocarbon/air flames (called laminar soot-point conditions) were studied, emphasizing non-buoyant laminar coflowing jet diffusion flames. Effects of air/fuel-stream velocity ratios were of particular interest; therefore, the experiments were carried out at reduced pressures to minimize effects of flow acceleration due to the intrusion of buoyancy. Test conditions included reactant temperatures of 300 K; ambient pressures of 3.7-49 8 kPa; methane-, acetylene-, ethylene-, propane-, and methane-fueled flames burning in coflowing air with fuel-port diameters of 1.7, 3.2, and 6.4 mm, fuel jet Reynolds numbers of 18-121; air coflow velocities of 0-6 m/s; and air/fuel-stream velocity ratios of 0.003-70. Measurements included laminar soot-point flame lengths, laminar soot-point fuel flow rates, and laminar liftoff conditions. The measurements show that laminar soot-point flame lengths and fuel flow rates can be increased, broadening the range of fuel flow rates where the flames remain soot free, by increasing air/fuel-stream velocity ratios. The mechanism of this effect involves the magnitude and direction of flow velocities relative to the flame sheet where increased air/fuel-stream velocity ratios cause progressive reduction of flame residence times in the fuel-rich soot-formation region. The range of soot-free conditions is limited by both liftoff, particularly at low pressures, and the intrusion of effects of buoyancy on effective air/fuel-stream velocity ratios, particularly at high pressures. Effective correlations of laminar soot- and smoke-point flame lengths were also found in terms of a corrected fuel flow rate parameter, based on simplified analysis of laminar jet diffusion flame structure. The results show that laminar smoke-point flame lengths in coflowing air environments are roughly twice as long as soot-free (blue) flames under comparable conditions due to the presence of luminous soot particles under fuel-lean conditions when smoke-point conditions are approached. This is very similar to earlier findings concerning differences between laminar smoke- and sootpoint flame lengths in still environments.

Dai, Z.↗

Flame and Soot Boundaries of Laminar Jet Diffusion Flames

The shapes (flame-sheet and luminous-flame boundaries) or steady weakly buoyant round hydrocarbon-fueled laminar-jet diffusion flames in still and coflowing air were studied both experimentally and theoretically. Flame-sheet shapes were measured from photographs using a CH optical filter to distinguish flame-sheet boundaries in the presence of blue CO2 and OH emissions and yellow continuum radiation from soot. Present experimental conditions included acetylene-, methane-, propane-, and ethylene-fueled flames having initial reactant temperatures of 300 K. ambient pressures of 4-50 kPa, jet-exit Reynolds numbers of 3-54, initial air/fuel velocity ratios of 0-9, and luminous flame lengths of 5-55 mm; earlier measurements for propylene- and 1,3-butadiene-fueled flames for similar conditions were considered as well. Nonbuoyant flames in still air were observed at microgravity conditions; essentially nonbuoyant flames in coflowing air were observed at small pressures to control effects of buoyancy. Predictions of luminous flame boundaries from soot luminosity were limited to laminar smoke-point conditions, whereas predictions of flame-sheet boundaries ranged from soot-free to smoke-point conditions. Flame-shape predictions were based on simplified analyses using the boundary-layer approximations along with empirical parameters to distinguish flame-sheet and luminous-flame (at the laminar smoke point) boundaries. The comparison between measurements and predictions was remarkably good and showed that both flame-sheet and luminous-flame lengths are primarily controlled by fuel flow rates with lengths in coflowing air approaching 2/3 of the lengths in still air as coflowing air velocities are increased. Finally, luminous flame lengths at laminar smoke-point conditions were roughly twice as long as flame-sheet lengths at comparable conditions because of the presence of luminous soot particles in the fuel-lean region of the flames.

Xu, F.↗

Microphysics of Pyrocumulonimbus Clouds

The intense heat from forest fires can generate explosive deep convective cloud systems that inject pollutants to high altitudes. Both satellite and high-altitude aircraft measurements have documented cases in which these pyrocumulonimbus clouds inject large amounts of smoke well into the stratosphere (Fromm and Servranckx 2003; Jost et al. 2004). This smoke can remain in the stratosphere, be transported large distances, and affect lower stratospheric chemistry. In addition recent in situ measurements in pyrocumulus updrafts have shown that the high concentrations of smoke particles have significant impacts on cloud microphysical properties. Very high droplet number densities result in delayed precipitation and may enhance lightning (Andrew et al. 2004). Presumably, the smoke particles will also lead to changes in the properties of anvil cirrus produces by the deep convection, with resulting influences on cloud radiative forcing. In situ sampling near the tops of mature pyrocumulonimbus is difficult due to the high altitude and violence of the storms. In this study, we use large eddy simulations (LES) with size-resolved microphysics to elucidate physical processes in pyrocumulonimbus clouds.

Jensen, Eric↗

Estimation of Fire Emissions from Satellite-Based Measurements

Biomass burning is a worldwide phenomenon affecting many vegetated parts of the globe regularly. Fires emit large quantities of aerosol and trace gases into the atmosphere, thus influencing the atmospheric chemistry and climate. Traditional methods of fire emissions estimation achieved only limited success, because they were based on peripheral information such as rainfall patterns, vegetation types and changes, agricultural practices, and surface ozone concentrations. During the last several years, rapid developments in satellite remote sensing has allowed more direct estimation of smoke emissions using remotely-sensed fire data. However, current methods use fire pixel counts or burned areas, thereby depending on the accuracy of independent estimations of the biomass fuel loadings, combustion efficiency, and emission factors. With the enhanced radiometric range of its 4-micron fire channel, the Moderate Resolution Imaging Spectroradiometer (MODIS) sensor, which flies aboard both of the Earth Observing System EOS) Terra and Aqua Satellites, is able to measure the rate of release of fire radiative energy (FRE) in MJ/s (something that older sensors could not do). MODIS also measures aerosol distribution. Taking advantage of these new resources, we have developed a procedure combining MODIS fire and aerosol products to derive FRE-based smoke emission coefficients (C(e), in kg/MJ) for different regions of the globe. These coefficients are simply used to multiply FRE from MODIS to derive the emitted smoke aerosol mass. Results from this novel methodology are very encouraging. For instance, it was found that the smoke total particulate mass emission coefficient for the Brazilian Cerrado ecosystem (approximately 0.022 kg/MJ) is about twice the value for North America, Western Europe, or Australia, but about 50% lower than the value for southern Africa.

Ichoku, Charles↗

Tropospheric Carbon Monoxide Measurements from the Scanning High-resolution Interferometer Sounder on 7 September 2000 in Southern Africa during SAFARI 2000

Retrieved tropospheric carbon monoxide (CO) column densities are presented for more than 9000 spectra obtained by the University of Wisconsin-Madison (UWis) Scanning High-Resolution Interferometer Sounder (SHIS) during a flight on the NASA ER-2 on 7 September 2000 as part of the Southern African Regional Science Initiative (SAFARI 2000) dry season field campaign. Enhancements in tropospheric column CO were detected in the vicinity of a controlled biomass burn in the Timbavati Game Reserve in northeastern South Africa and over the edge of the river of smoke in south central Mozambique. Relatively clean air was observed over the far southern coast of Mozambique. Quantitative comparisons are presented with in situ measurements from five different instruments flying on two other aircraft: the University of Washington Convair-580 (CV) and the South African Aerocommander JRB in the vicinity of the Timbavati fire. Measured tropospheric CO columns (extrapolated from 337 to 100 mb) of 2.1 x 10(exp 18) per square centimeter in background air and up to 1.5 x 10(exp 19) per square centimeter in the smoke plume agree well with SHIS retrieved tropospheric CO columns of (2.3 plus or minus 0.25) x 10(exp 18) per square centimeter over background air near the fire and (1.5 plus or minus 0.35) x 10(exp 19) per square centimeter over the smoke plume. Qualitative comparisons are presented with three other in situ CO profiles obtained by the South African JRA aircraft over Mozambique and northern South Africa showing the influence of the river of smoke.

McMillan, W. W.↗

Informing Aerosol Transport Models With Satellite Multi-Angle Aerosol Measurements

As the aerosol products from the NASA Earth Observing System's Multi-angle Imaging SpectroRadiometer (MISR) mature, we are placing greater focus on ways of using the aerosol amount and type data products, and aerosol plume heights, to constrain aerosol transport models. We have demonstrated the ability to map aerosol air-mass-types regionally, and have identified product upgrades required to apply them globally, including the need for a quality flag indicating the aerosol type information content, that varies depending upon retrieval conditions. We have shown that MISR aerosol type can distinguish smoke from dust, volcanic ash from sulfate and water particles, and can identify qualitative differences in mixtures of smoke, dust, and pollution aerosol components in urban settings. We demonstrated the use of stereo imaging to map smoke, dust, and volcanic effluent plume injection height, and the combination of MISR and MODIS aerosol optical depth maps to constrain wildfire smoke source strength. This talk will briefly highlight where we stand on these application, with emphasis on the steps we are taking toward applying the capabilities toward constraining aerosol transport models, planet-wide.

Limbacher, J.↗

Space-based Observational Constraints for 1-D Plume Rise Models

We use a space-based plume height climatology derived from observations made by the Multi-angle Imaging SpectroRadiometer (MISR) instrument aboard the NASA Terra satellite to evaluate the ability of a plume-rise model currently embedded in several atmospheric chemical transport models (CTMs) to produce accurate smoke injection heights. We initialize the plume-rise model with assimilated meteorological fields from the NASA Goddard Earth Observing System and estimated fuel moisture content at the location and time of the MISR measurements. Fire properties that drive the plume-rise model are difficult to estimate and we test the model with four estimates for active fire area and four for total heat flux, obtained using empirical data and Moderate Resolution Imaging Spectroradiometer (MODIS) re radiative power (FRP) thermal anomalies available for each MISR plume. We show that the model is not able to reproduce the plume heights observed by MISR over the range of conditions studied (maximum r2 obtained in all configurations is 0.3). The model also fails to determine which plumes are in the free troposphere (according to MISR), key information needed for atmospheric models to simulate properly smoke dispersion. We conclude that embedding a plume-rise model using currently available re constraints in large-scale atmospheric studies remains a difficult proposition. However, we demonstrate the degree to which the fire dynamical heat flux (related to active fire area and sensible heat flux), and atmospheric stability structure influence plume rise, although other factors less well constrained (e.g., entrainment) may also be significant. Using atmospheric stability conditions, MODIS FRP, and MISR plume heights, we offer some constraints on the main physical factors that drive smoke plume rise. We find that smoke plumes reaching high altitudes are characterized by higher FRP and weaker atmospheric stability conditions than those at low altitude, which tend to remain confined below the BL, consistent with earlier results. We propose two simplified parameterizations for computing injection heights for fires in CTMs and discuss current challenges to representing plume injection heights in large scale atmospheric models.

Martin, Maria Val↗

Aerosol Meteorology of Maritime Continent for the 2012 7SEAS Southwest Monsoon Intensive Study - Part 2: Philippine Receptor Observations of Fine-Scale Aerosol Behavior

The largest 7 Southeast Asian Studies (7SEAS) operations period within the Maritime Continent (MC) occurred in the August-September 2012 biomass burning season. Data included were observations aboard the MY Vasco, dispatched to the Palawan Archipelago and Sulu Sea of the Philippines for September 2012. At these locations, the Vasco observed MC smoke and pollution entering the southwest monsoon (SWM) monsoonal trough. Here we describe the research cruise findings and the finer-scale aerosol meteorology of this convectively active region. This 2012 cruise complemented a 2-week cruise in 2011 and was generally consistent with previous findings in terms of how smoke emission and transport related to monsoonal flows, tropical cyclones (TC), and the covariance between smoke transport events and the atmosphere's thermodynamic structure. Biomass burning plumes were usually mixed with significant amounts of anthropogenic pollution. Also key to aerosol behavior were squall lines and cold pools propagating across the South China Sea (SCS) and scavenging aerosol particles in their path. However, the 2012 cruise showed much higher modulation in aerosol frequency than its 2011 counterpart. Whereas in 2011 large synoptic-scale aerosol events transported high concentrations of smoke into the Philippines over days, in 2012 measured aerosol events exhibited a much shorter-term variation, sometimes only 312h. Strong monsoonal flow reversals were also experienced in 2012. Nucleation events in cleaner and polluted conditions, as well as in urban plumes, were observed. Perhaps most interestingly, several cases of squall lines preceding major aerosol events were observed, as opposed to 2011 observations where these lines largely scavenged aerosol particles from the marine boundary layer. Combined, these observations indicate pockets of high and low particle counts that are not uncommon in the region. These perturbations are difficult to observe by satellite and very difficult to model. Indeed, the Navy Aerosol Analysis and Prediction System (NAAPS) simulations captured longer period aerosol events quite well but largely failed to capture the timing of high-frequency phenomena. Ultimately, the research findings of these cruises demonstrate the real world challenges of satellite-based missions, significant aerosol life cycle questions such as those the future Aerosol/Clouds/Ecosystems (ACE) will investigate, and the importance of small-scale phenomena such as sea breezes, squall lines, and nucleation events embedded within SWM patterns in dominating aerosol life cycle and potential relationships to clouds.

Reid, Jeffrey S.↗

Radiative Characteristics of Aerosol During Extreme Fire Event over Siberia in Summer 2012

Microphysical and optical properties of aerosol were studied during a mega-fire event in summer 2012 over Siberia using ground-based measurements of spectral solarradiation at the AERONET site in Tomsk and satellite observations. The data were analyzed using multi-year (2003-2013) measurements of aerosol characteristics under back-ground conditions and for less intense fires, differing in burning biomass type, stage of fire, remoteness from observation site, etc. (ordinary smoke). In June-August 2012, the average aerosol optical depth (AOD, 500 nm) had been 0.95+/-0.86, about a factor of 6 larger than background values (0.16+/-0.08), and a factor of 2.5 larger than in ordinary smoke. The AOD values were extremely high on 24-28 July and reached 3-5. A comparison with satellite observations showed that ground-based measurements in the region of Tomsk not only reflect the local AOD features, but are also characteristic for the territory of Western Siberia as a whole. Single scattering albedo (SSA, 440 nm) in this period ranged from 0.91 to 0.99 with an average of approx. 0.96 in the entire wavelength range of 440-1020 nm. The increase in absorptance of aerosol particles (SSA(440 nm)=0.92) and decrease in SSA with wavelength observed in ordinary smoke agree with the data from multi-year observations in analogous situations in the boreal zone of USA and Canada. Volume aerosol size distribution in extreme and ordinary smoke had a bimodal character with significant prevalence of fine-mode particles, but in summer 2012 the mean median radius and the width of the fine-mode distribution somewhat increased. In contrast to data from multi-year observations, in summer 2012 an increase in the volume concentration and median radius of the coarse mode was observed with growing AOD.

Zhuravleva, Tatiana B.↗

Assessing the Radiative Impact of the 2019 – 2020 Australian Bushfires using Trajectory-Mapped CALIPSO Observations.

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).

Australian Bushfires↗

Assessing the Radiative Impact of the 2019 – 2020 Australian Bushfires using Trajectory-Mapped CALIPSO and SAGE III/ISS Observations.

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).

Australian bushfire↗

Variability of Lidar-Derived Particle Properties Over West Africa Due to Changes in Absorption: Towards an Understanding

Measurements performed in western Africa (Senegal) during the SHADOW field campaign are analyzed to show that spectral dependence of the imaginary part of the complex refractive index (CRI) of dust can be revealed by lidar-measured particle parameters. Observations in April 2015 provide good opportunity for such study, because, due to high optical depth of the dust, exceeding 0.5, the extinction coefficient could be derived from lidar measurements with high accuracy and the contribution of other aerosol types, such as biomass burning, was negligible. For instance, in the second half of April 2015, AERONET observations demonstrated a temporal decrease in the imaginary part of the CRI at 440 nm from approximately 0.0045 to 0.0025. This decrease is in line with a change in the relationship between the lidar ratios (the extinction-to-backscattering ratio) at 355 and 532 nm (S(355) and S(532)). For instance in the first half of April, S(355)∕S(532) is as high as 1.5 and the backscatter Angstrom exponent, A(β), is as low as −0.75, while after 15 April S(355)/S(532)=1.0 and A(β) is close to zero. The aerosol depolarization ratio δ(532) for the whole of April exceeded 30 % in the height range considered, implying that no other aerosol, except dust, occurred. The performed modeling confirmed that the observed S(355)∕S(532) and Aβ values match the spectrally dependent imaginary part of the refractive index as can be expected for mineral dust containing iron oxides. The second phase of the SHADOW campaign was focused on evaluation of the lidar ratio of smoke and estimates of its dependence on relative humidity (RH). For five studied smoke episodes the lidar ratio increases from 44±5 to 66±7 sr at 532 nm and from 62±6 to 80±8 sr at 355 nm, when RH varied from 25 % to 85 %. Performed numerical simulations demonstrate that observed ratio S(355)∕S(532), exceeding 1.0 in the smoke plumes, can indicate an increase in the imaginary part of the smoke particles in the ultraviolet (UV) range.

Lidar-Derived Particle Properties↗

Southern Idaho Health & Air Quality II: Evaluating Atmospheric Mixing Height Estimations in the Western United States

Wildfires in the western United States have caused immense infrastructure damage and loss of human life in recent years. Wildfire smoke, which travels far from its original source, is also harmful to human health. Mixing height, which acts as a lid and prevents smoke from rising above a certain altitude in the lower troposphere, is a critical input in smoke dispersion and air quality models used by agencies that monitor wildfires. These models, coupled with forecaster expertise, are also used to decide when it is safe to execute a prescribed burn. The DEVELOPID team partnered with the National Weather Service (NWS) Fire Weather Program, Bureau of Land Management (BLM), National Interagency Fire Center (NIFC), and National Park Service (NPS) Fire Management Program Center (FMPC) to help improve reliability and confidence in mixing height estimations, and therefore the burn prescription decision-making process. To that end, the team developed a toolbox for measuring smoke-related aerosol mixing heights using Cloud-Aerosol LiDAR and Infrared Pathfinder Satellite Observations (CALIPSO) Vertical Feature Mask granules. CALIPSO mixing heights and NWS estimations covaried significantly and positively. However, substantial disagreement between the methods stymied the team’s attempts to quantify systematic bias in a meaningful way. The relative error between the methods was especially large at low mixing heights, which suggests that this method of validation may only be suitable at higher altitudes.

Dean Berkowitz↗

Variations in radiative heating of humid biomass burning aerosols in the southeast Atlantic from airborne observations and reanalysis

The atmosphere over the southeast Atlantic Ocean (SEA) experiences consistent springtime biomass burning (BB) smoke from widespread agricultural fires on the African continent. This smoke layer is initially lofted high in a continental mixed layer (~5-6km) and is then transported westward into the free troposphere where it overlies and ultimately mixes into a stratocumulus-topped oceanic boundary layer. Coincident with this smoke is an elevated humidity signal which is present from the time a given airmass is over the continental source region. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) was a NASA Earth Venture Suborbital mission with the goal of measuring aerosol, cloud, and atmospheric properties over this region over three deployments in September 2016, August 2017, and October 2018. Measurements included in situ profile measurements of aerosol physical and optical properties, trace gas concentrations, and cloud properties, as well as column measurements of aerosol optical depth and trace gas concentrations from an airborne sun photometer. Here we present results from each of the ORACLES deployments over the southeast Atlantic Ocean. Despite the differing locations and season of each deployment, we show that there is good agreement between the airborne ORACLES dataset and large-scale reanalyses, specifically the ECMWF ERA5 reanalyses (and, to a degree, the CAMS product) as compared to other available products. This agreement allows us to examine multi-year seasonal patterns and trends beyond the three months with available aircraft data. In both the data and reanalysis, we find distinct variations between each deployment in terms of vertical smoke distribution and correlation to atmospheric specific humidity, due to changing conditions over the BB season. We trace the origin and the history of these smoky airmasses and finally, we briefly discuss the broader radiative and dynamical implications of these results for conditions of aerosols overlying stratocumulus clouds.

K. Pistone↗

Variation and evolution of atmospheric structure over the SEA BB season as seen from aircraft and reanalysis

The presence of absorbing aerosols and atmospheric water vapor will impact clouds both radiatively and dynamically. The atmosphere over the southeast Atlantic Ocean (SEA) experiences consistent springtime biomass burning (BB) smoke from widespread agricultural fires on the African continent. This smoke layer is initially lofted high in a continental mixed layer (~5-6km) and is then transported westward into the free troposphere where it overlies and ultimately mixes into the underlying stratocumulus-topped oceanic boundary layer. Coincident with this smoke is an elevated humidity signal which is present from the time a given airmass is over the continental source region. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) was a NASA Earth Venture Suborbital mission with the goal of measuring aerosol, cloud, and atmospheric properties over this region over three deployments in September 2016, August 2017, and October 2018. Measurements included in situ profile measurements of aerosol physical and optical properties, trace gas concentrations, and cloud properties, as well as column measurements of aerosol optical depth and trace gas concentrations from an airborne sun photometer, allowing for calculation of radiative heating at different altitudes. Here we present results from the three ORACLES deployments over the southeast Atlantic Ocean. The airborne observations capture both seasonal patterns (August through October) and spatial patterns (north/south and east/west) in the vertical smoke distribution and its correlation to atmospheric specific humidity over the SEA basin. We describe the observed variations and show that the variability in both meteorological and emissions is largely captured in the European Centre for Medium-range Weather Forecasting Copernicus Atmosphere Monitoring Service (ECMWF CAMS) reanalysis, which allows for a more systematic examination of the relative frequency of observed conditions and their radiative impact over the region. Finally, we discuss the broader radiative and dynamical implications of these results for conditions of biomass burning aerosols overlying stratocumulus clouds.

Kristina Marie Myers Pistone↗

Simultaneous Retrievals of Biomass Burning Aerosols and Trace Gases From the Ultraviolet to Near-Infrared Over Northern Thailand During the 2019 Pre-Monsoon Season

With the advent of spaceborne spectroradiometers in a geostationary constellation, measuring high spectral resolution ultraviolet–visible (UV-VIS) and selected near-/shortwave-infrared (NIR/SWIR) radiances can enable the probing of the life cycle of key atmospheric trace gases and aerosols at higher temporal resolutions over the globe. The UV-VIS measurements are important for retrieving several key trace gases (e.g., O 3 , SO 2 , NO 2 , and HCHO) and particularly for deriving aerosol characteristics (e.g., aerosol absorption and vertical profile). This study examines the merit of simultaneous retrievals of trace gases and aerosols using a ground-based spectroradiometer covering the UV-NIR to monitor their physicochemical processes and to obtain reliable aerosol information for various applications. During the 2019 pre-monsoon season over northern Thailand, we deployed a ground-based SMART–s (Spectral Measurements for Atmospheric Radiative Transfer–spectroradiometer) instrument, which is an extended-range Pandora with reliable radiometric calibration in the 330–820 nm range, to retrieve remotely sensed chemical and aerosol properties for the first time near biomass burning sources. The high spectral resolution (∼ 1.0 nm full width half maximum with ∼ 3.7 × oversampling) of sun and sky measurements from SMART–s provides several key trace gases (e.g., O 3 , NO 2 , and H 2 O) and aerosol properties covering the UV where significant light absorption occurs by the carbonaceous particles. During the measurement period, highly correlated total column amounts of NO 2 and aerosol optical thickness (т aer ) retrieved from SMART–s (correlation coefficient, R=0.74) indicated their common emissions from biomass burning events. The SMART–s retrievals of the spectral single scattering albedo (ω 0 ) of smoke aerosols showed an abrupt decrease in the UV, which is an important parameter dictating photochemical processes in the atmosphere. The values of ω 0 and column precipitable water vapor (H 2 O) gradually increase with the mixing of biomass burning smoke particles and higher water vapor concentrations when approaching the monsoon season. The retrieved ω 0 and weighted mean radius of fine-mode aerosols from SMART–s showed positive correlations with the H 2 O (R=0.81 for ω 0 at 330 nm and 0.56 for the volume-weighted mean radius), whereas the real part of the refractive index of fine-mode aerosol (n f ) showed negative correlations (R = -0.61 at 330 nm), which suggest that aerosol aging processes including hygroscopic growth (e.g., humidification and cloud processing) can be a major factor affecting the temporal trends of aerosol optical properties. Retrieved n f and ω 0 were closer to those of the water droplet (i.e., n f of about 1.33 and ω 0 of about 1.0) under lower amounts of NO 2 during the measurement period; considering that the NO 2 amounts in the smoke may indicate the aging of the plume after emission due to its short lifetime, the tendency is also consistent with active hygroscopic processes of the aerosols over this area. Retrieved UV aerosol properties from SMART–s generally support the assumed smoke aerosol models (i.e., the spectral shape of aerosol absorption) used in NASA's current satellite algorithms, and their spectral ω 0 retrievals from ground and satellites showed good agreements (R = 0.73–0.79). However, temporal and spectral variabilities in the aerosol absorption properties in the UV emphasize the importance of a realistic optical model of aerosols for further improvements in satellite retrievals.

biomass burning↗

Measurement Report :Emission Factors of NH3 and NHx for Wildfires and Agricultural Fires in the United States

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.

Laura Tomsche↗