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Techniques for Estimating Emissions Factors from Forest Burning: ARCTAS and SEAC4RS Airborne Measurements Indicate Which Fires Produce Ozone

Previous studies of emission factors from biomass burning are prone to large errors since they ignore the interplay of mixing and varying pre-fire background CO2 levels. Such complications severely affected our studies of 446 forest fire plume samples measured in the Western US by the science teams of NASA's SEAC4RS and ARCTAS airborne missions. Consequently we propose a Mixed Effects Regression Emission Technique (MERET) to check techniques like the Normalized Emission Ratio Method (NERM), where use of sequential observations cannot disentangle emissions and mixing. We also evaluate a simpler "consensus" technique. All techniques relate emissions to fuel burned using C(sub burn) = delta C(sub tot) added to the fire plume, where C(sub tot) approximately equals (CO2 + CO). Mixed-effects regression can estimate pre-fire background values of Ctot (indexed by observation j) simultaneously with emissions factors indexed by individual species i, delta epsilon lambda tau alpha−x(sub i)/(C(sub burn))i,j., MERET and "consensus" require more than two emissions indicators. Our studies excluded samples where exogenous CO or CH4 might have been fed into a fire plume, mimicking emission. We sought to let the data on 13 gases and particulate properties suggest clusters of variables and plume types, using non-negative matrix factorization (NMF). While samples were mixtures, the NMF unmixing suggested purer burn types. Particulate properties (bscat, babs, SSA, AAE) and gas-phase emissions were interrelated. Finally, we sought a simple categorization useful for modeling ozone production in plumes. Two kinds of fires produced high ozone: those with large fuel nitrogen as evidenced by remnant CH3CN in the plumes, and also those from very intense large burns. Fire types with optimal ratios of delta-NOy/delta- HCHO associate with the highest additional ozone per unit Cburn, Perhaps these plumes exhibit limited NOx binding to reactive organics. Perhaps these plumes exhibit limited NOx binding to reactive organics.

fires↗

Techniques for Estimating Emissions Factors from Forest Burning: ARCTAS and SEAC4RS Airborne Measurements Indicate which Fires Produce Ozone

Previous studies of emission factors from biomass burning are prone to large errors since they ignore the interplay of mixing and varying pre-fire background CO2 levels. Such complications severely affected our studies of 446 forest fire plume samples measured in the Western US by the science teams of NASA's SEAC4RS and ARCTAS airborne missions. Consequently we propose a Mixed Effects Regression Emission Technique (MERET) to check techniques like the Normalized Emission Ratio Method (NERM), where use of sequential observations cannot disentangle emissions and mixing. We also evaluate a simpler "consensus" technique. All techniques relate emissions to fuel burned using C(burn) = delta C(tot) added to the fire plume, where C(tot) approximately equals (CO2 = CO). Mixed-effects regression can estimate pre-fire background values of C(tot) (indexed by observation j) simultaneously with emissions factors indexed by individual species i, delta, epsilon lambda tau alpha-x(sub I)/C(sub burn))I,j. MERET and "consensus" require more than emissions indicators. Our studies excluded samples where exogenous CO or CH4 might have been fed into a fire plume, mimicking emission. We sought to let the data on 13 gases and particulate properties suggest clusters of variables and plume types, using non-negative matrix factorization (NMF). While samples were mixtures, the NMF unmixing suggested purer burn types. Particulate properties (b scant, b abs, SSA, AAE) and gas-phase emissions were interrelated. Finally, we sought a simple categorization useful for modeling ozone production in plumes. Two kinds of fires produced high ozone: those with large fuel nitrogen as evidenced by remnant CH3CN in the plumes, and also those from very intense large burns. Fire types with optimal ratios of delta-NOy/delta- HCHO associate with the highest additional ozone per unit Cburn, Perhaps these plumes exhibit limited NOx binding to reactive organics. Perhaps these plumes exhibit limited NOx binding to reactive organics

ozone↗

Planning, Implementation, and Scientific Goals of the Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) Field Missions

The Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) field mission based at Ellington Field, Texas, during August and September 2013 employed the most comprehensive airborne payload to date to investigate atmospheric composition over North America. The NASA ER-2, DC-8, and SPEC Inc. Learjet flew 57 science flights from the surface to 20 km. The ER-2 employed seven remote sensing instruments as a satellite surrogate and eight in situ instruments. The DC-8 employed 23 in situ and five remote sensing instruments for radiation, chemistry, and microphysics. The Learjet used 11 instruments to explore cloud microphysics. SEAC4RS launched numerous balloons, augmented Aerosol RObotic NETwork, and collaborated with many existing ground measurement sites. Flights investigating convection included close coordination of all three aircraft. Coordinated DC-8 and ER-2 flights investigated the optical properties of aerosols, the influence of aerosols on clouds, and the performance of new instruments for satellite measurements of clouds and aerosols. ER-2 sorties sampled stratospheric injections of water vapor and other chemicals by local and distant convection. DC-8 flights studied seasonally evolving chemistry in the Southeastern U.S., atmospheric chemistry with lower emissions of NOx and SO2 than in previous decades, isoprene chemistry under high and low NOx conditions at different locations, organic aerosols, air pollution near Houston and in petroleum fields, smoke from wildfires in western forests and from agricultural fires in the Mississippi Valley, and the ways in which the chemistry in the boundary layer and the upper troposphere were influenced by vertical transport in convective clouds.

Toon, Owen B.↗

Agricultural Fires in the Southeastern U.S. During SEAC4RS: Emissions of Trace Gases and Particles and Evolution of Ozone, Reactive Nitrogen, and Organic Aerosol

Emissions from 15 agricultural fires in the southeastern U.S. were measured from the NASA DC-8 research aircraft during the summer 2013 Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) campaign. This study reports a detailed set of emission factors (EFs) for 25 trace gases and 6 fine particle species. The chemical evolution of the primary emissions in seven plumes was examined in detail for ~1.2 h. A Lagrangian plume cross-section model was used to simulate the evolution of ozone (O3), reactive nitrogen species, and organic aerosol (OA). Observed EFs are generally consistent with previous measurements of crop residue burning, but the fires studied here emitted high amounts of SO2 and fine particles, especially primary OA and chloride. Filter-based measurements of aerosol light absorption implied that brown carbon (BrC) was ubiquitous in the plumes. In aged plumes, rapid production of O3, peroxyacetyl nitrate (PAN), and nitrate was observed with (Delta)O3/(Delta)CO, (Delta)PAN/(Delta)NOy, and (Delta)nitrate/(Delta)NOy reaching approx. 0.1, approx. 0.3, and approx.0.3. For five selected cases, the model reasonably simulated O3 formation but underestimated PAN formation. No significant evolution of OA mass or BrC absorption was observed. However, a consistent increase in oxygen-to-carbon (O/C) ratios of OA indicated that OA oxidation in the agricultural fire plumes was much faster than in urban and forest fire plumes. Finally, total annual SO2, NOx, and CO emissions from agricultural fires in Arkansas, Louisiana, Mississippi, and Missouri were estimated (within a factor of approx. 2) to be equivalent to approx. 2% SO2 from coal combustion and approx. 1% NOx and approx. 9% CO from mobile sources.

OA mass or BrC absorption↗

Tropospheric Ozone Change from 1980 to 2010 Dominated by Equatorward Redistribution of Emissions

Ozone is an important air pollutant at the surface, and the third most important anthropogenic greenhouse gas in the troposphere. Since 1980, anthropogenic emissions of ozone precursors methane, non-methane volatile organic compounds, carbon monoxide and nitrogen oxides (NOx) have shifted from developed to developing regions. Emissions have thereby been redistributed equatorwards, where they are expected to have a stronger effect on the tropospheric ozone burden due to greater convection, reaction rates and NOx sensitivity. Here we use a global chemical transport model to simulate changes in tropospheric ozone concentrations from 1980 to 2010, and to separate the influences of changes in the spatial distribution of global anthropogenic emissions of short-lived pollutants, the magnitude of these emissions, and the global atmospheric methane concentration. We estimate that the increase in ozone burden due to the spatial distribution change slightly exceeds the combined influences of the increased emission magnitude and global methane. Emission increases in Southeast, East and South Asia may be most important for the ozone change, supported by an analysis of statistically significant increases in observed ozone above these regions. The spatial distribution of emissions dominates global tropospheric ozone, suggesting that the future ozone burden will be determined mainly by emissions from low latitudes.

Zhang, Yuqiang↗

Daily Ambient Air Pollution Metrics for Five Cities: Evaluation of Data Fusion-Based Estimates and Uncertainties

Spatiotemporal characterization of ambient air pollutant concentrations is increasingly relying on the combination of observations and air quality models to provide well-constrained, spatially and temporally complete pollutant concentration fields. Air quality models, in particular, are attractive, as they characterize the emissions, meteorological, and physiochemical process linkages explicitly while providing continuous spatial structure. However, such modeling is computationally intensive and has biases. The limitations of spatially sparse and temporally incomplete observations can be overcome by blending the data with estimates from a physically and chemically coherent model, driven by emissions and meteorological inputs. We recently developed a data fusion method that blends ambient ground observations and chemical transport-modeled (CTM) data to estimate daily, spatially resolved pollutant concentrations and associatedcorrelations. In this study, we assess the ability of the data fusion method to produce daily metrics (i.e., 1-hr max, 8-hr max, and 24-hr average) of ambient air pollution that capture spatiotemporal air pollution trends for 12 pollutants (CO, NO2, NOx, O3, SO2, PM (sub10), PM (sub 2.5), and five PM (sub 2.5) components) across five metropolitan areas (Atlanta, Birmingham, Dallas, Pittsburgh, and St. Louis), from 2002 to 2008. Three sets of comparisons are performed: (1) the CTM concentrations are evaluated for each pollutant and metropolitan domain, (2) the data fusion concentrations are compared with the monitor data, (3) a comprehensive cross-validation analysis against observed data evaluates the quality of the data fusion model simulations across multiple metropolitan domains. The resulting daily spatial field estimates of air pollutant concentrations and uncertainties are not only consistent with observations, emissions, andmeteorology, but substantially improve CTM-derived results for nearly all pollutants and all cities, with the exception of NO2 for Birmingham. The greatest improvements occur for O3 and PM (sub 2.5). Squared spatiotemporal correlation coefficients range between simulations and observations determined using cross-validation across all cities for air pollutants of secondary and mixed origins are R-squared equal to 0.88-0.93 (O3), 0.81-0.89 (SO4), 0.67-0.83 (PM (sub 2.5)), 0.52-0.72 (NO3), 0.43-0.80 (NH4), 0.32-0.51 (OC), and 0.14-0.71 (PM (sub 10)). Results for relatively homogeneous pollutants of secondary origin, tend to be better than those for more spatially heterogeneous (larger spatial gradients) pollutants of primary origin (NOx, CO, SO2 and EC). Generally, background concentrations and spatial concentration gradients reflect interurban airshed complexity and the effects of regional transport, whereas daily spatial pattern variability shows intra urban consistency in the fused data. With sufficiently high CTM spatial resolution, traffic-related pollutants exhibit gradual concentration gradients that peak toward the urban centers. Ambient pollutant concentration uncertainty estimates for the fused data are both more accurate and smaller than those for either the observations or the model simulations alone.

spatiotemporal fusion↗

Fuel Sensitivity of Gas Emissions, Lean Blowout and Combustion Dynamics for a 9-Point LDI Combustor

Fuel sensitivity of gaseous emissions, approach to lean blowout and combustion dynamics are evaluated in this study. Experiments were conducted at the NASA Glenn Research Center's CE-5 flame tube test facility with a 9-point Swirl-Venturi Lean Direct Injection (SV-LDI) combustor. A reference jet fuel (A2) and two test fuels (C1 and C3) from were provided by the National Jet Fuels Combustion Program (NJFCP). C1 is essentially a 2-component iso-paraffin test fuel with a low cetane number of 17, and C3 is a high viscosity test fuel. Approach to lean blowout was monitored in terms of the rapid increase in CO emissions index as equivalence ratio decreased, but testing did not proceed all the way to lean blowout (LBO). Burning C1 was found to produce lower NOx emissions, but C1 flame temperatures were about 25 K higher relative to A2 at near LBO points (where CO emissions increased very rapidly). The NOx emissions of C3 were similar to A2. At low power conditions where fuel injector performance is not optimized for this 9-point LDI combustor, C3 had higher CO emissions than A2 and C1, likely due to C3's higher viscosity relative to A2 and C1. No discernable difference in combustion dynamics was observed between the three fuels tested in the 9-point LDI combustor. While a systematic ignition test campaign was not conducted, it was observed that C1 required a higher equivalence ratio and inlet air temperature for test rig ignition compared to A2 and C3.

Lean Direct Injection↗

Fundamental Study of a 7-Element Fuel Injector Configuration for Gas Turbine Combustors - A Look at Cold Flow and Burning Measurements

Lean direct injection (LDI) is a combustion concept to reduce oxides of nitrogen (NOx) for next generation aircraft gas turbine engines. These newer engines have cycles that increase fuel efficiency through increased operating pressures, which increase combustor inlet temperatures. NOx formation rates increase with higher temperatures, and the LDI strategy is to avoid high temperature by staying fuel lean and away from stoichiometric burning. Thus, LDI relies on rapid and uniform fuel/air mixing. Additionally, in combustors for smaller core engines, the area and volume bring about mixing and time scale challenges not found in larger engines. As part of our parametric study in which we vary swirler angle and orientation and look at their effect on fluid mixing and combustion, we examine one configuration of a 7-point lean direct injector by looking at the non-combusting 2-D velocity field using PIV, and combusting system for chemical species using chemiluminescent imaging and flame spectroscopy. The circular 7-point array consists of axial swirlers, with the center 60° swirler surrounded by six 52° swirlers. The velocity results for this configuration show that the outer swirlers serve to isolate the center flow field near the injector exit. A recirculation zone forms downstream of the center swirler, but not behind the outer swirlers. The combusting results also show an isolated zone directly downstream of the center injector. The flame spectra show variation in speciation of combustion species such as OH*, C3*, CH*, and C2* as a function of position within the combustor.

lean direct injection↗

Emissions Relationships Among Western Forest Fire Plumes: I. Emission Factors Free from Mixing Errors

Previous studies of emission factors from biomass burning are prone to largeerrors since they ignore the interplay of mixing and varying pre-fire backgroundCO2 levels. Such complications severely affected our studies of 446 forest fireplume samples measured in the Western US by the science teams of NASAsSEAC4RS and ARCTAS airborne missions. Consequently we propose a MixedEffects Regression Emission Technique (MERET) to check techniques like theNormalized Emission Ratio Method (NERM), where use of sequentialobservations cannot disentangle emissions and mixing. We also evaluate asimpler consensus technique. All techniques relate emissions to fuel burnedusing C burn = Δ Ctot added to the fire plume, where ≈ Ctot (CO2 + CO). Mixed-effectsregression can estimate pre-fire background values of Ctot (indexed byobservation j) simultaneously with emissions factors indexed by individual species i, δέλτα-xi (Cburn )i,j., MERET and consensus require more than twoemissions indicators. Our studies excluded samples where exogenous CO orCH4 might have been fed into a fire plume, mimicking emission.We sought to let the data on 13 gases and particulate properties suggest clustersof variables and plume types, using non-negative matrix factorization (NMF).While samples were mixtures, the NMF unmixing suggested purer burn types.Particulate properties (bscat, babs, SSA, AÅE) and gas-phase emissions were interrelated.Finally, we sought a simple categorization useful for modeling ozone productionin plumes. Two kinds of fires produced high ozone: those with large fuel nitrogenas evidenced by remnant CH3CN in the plumes, and also those from veryintense large burns. Fire types with optimal ratios of delta-NOydelta-HCHO associate with the highest additional ozone per unit Cburn, Perhaps theseplumes exhibit limited NOx binding to reactive organics. Perhaps these plumesexhibit limited NOx binding to reactive organics.

plumes↗

Emissions Relationships Among Western Forest Fire Plumes: II. Plume Typing for Sources of Ozone and Aerosol Absorption

Previous studies of emission factors from biomass burning are prone to largeerrors since they ignore the interplay of mixing and varying pre-fire backgroundCO2 levels. Such complications severely affected our studies of 446 forest fireplume samples measured in the Western US by the science teams of NASAs SEAC4RS and ARCTAS airborne missions. Consequently we propose a MixedEffects Regression Emission Technique (MERET) to check techniques like theNormalized Emission Ratio Method (NERM), where use of sequentialobservations cannot disentangle emissions and mixing. We also evaluate asimpler consensus technique. All techniques relate emissions to fuel burnedusing Cburn Ctot added to the fire plume, where Ctot (CO2 + CO). Mixed-effectsregression can estimate pre-fire background values of Ctot (indexed byobservation j) simultaneously with emissions factors indexed by individualspecies i, xi (Cburn )i,j., MERET and consensus require more than twoemissions indicators. Our studies excluded samples where exogenous CO orCH4 might have been fed into a fire plume, mimicking emission.We sought to let the data on 13 gases and particulate properties suggest clustersof variables and plume types, using non-negative matrix factorization (NMF).While samples were mixtures, the NMF unmixing suggested purer burn types.Particulate properties (bscat, babs, SSA, AE) and gas-phase emissions were interrelated.Finally, we sought a simple categorization useful for modeling ozone productionin plumes. Two kinds of fires produced high ozone: those with large fuel nitrogenas evidenced by remnant CH3CN in the plumes, and also those from veryintense large burns. Fire types with optimal ratios of delta-NOydelta-HCHO associate with the highest additional ozone per unit Cburn, Perhaps theseplumes exhibit limited NOx binding to reactive organics. Perhaps these plumesexhibit limited NOx binding to reactive organics.

ozone↗

Fuel Sensitivity of Gas Emissions, Lean Blowout and Combustion Dynamics for a 9-Point LDI Combustor

Fuel sensitivity of gaseous emissions, approach to lean blowout and combustion dynamics are evaluated in this study. Experiments were conducted at the NASA Glenn Research Center's CE-5 flame tube test facility with a 9-point Swirl-Venturi Lean Direct Injection (SV-LDI) combustor. A reference jet fuel (A2) and two test fuels (C1 and C3) from were provided by the National Jet Fuels Combustion Program (NJFCP). C1 is essentially a 2-component iso-paraffin test fuel with a low cetane number of 17, and C3 is a high viscosity test fuel. Approach to lean blowout was monitored in terms of the rapid increase in CO emissions index as equivalence ratio decreased, but testing did not proceed all the way to lean blowout (LBO). Burning C1 was found to produce lower NOx emissions, but C1 flame temperatures were about 25 K higher relative to A2 at near LBO points (where CO emissions increased very rapidly). The NOx emissions of C3 were similar to A2. At low power conditions where fuel injector performance is not optimized for this 9-point LDI combustor, C3 had higher CO emissions than A2 and C1, likely due to C3's higher viscosity relative to A2 and C1. No discernable difference in combustion dynamics was observed between the three fuels tested in the 9-point LDI combustor. While a systematic ignition test campaign was not conducted, it was observed that C1 required a higher equivalence ratio and inlet air temperature for test rig ignition compared to A2 and C3.

Combustion dynamics↗

Long Term Biological Treatment of Space Habitation Waste Waters in a One Stage MABR: Comparison of Operation for N and C Oxidation With and Without Simultaneous Denitrification

Aerobic biological stabilization has been previously demonstrated for full size MABR?s (CoMANDR 1.0, CoMANDR 2.0, and R-CoMANDR) over operating periods of ~1 year. These systems have successfully treated a variety of possible habitation waste streams including an ISS (urine + flush and humidity condensate) and Early Planetary Base (EPB) wastewater (urine, flush water, hygiene wastewater, and laundry). Biological stabilization has a number of advantages including: 1) elimination of hazardous pre-treat chemicals; 2) production of NOx species (that can be easily rejected by evaporative or membrane systems); 3) elimination of volatile organic constituents; 4) a low pH effluent that facilitates membrane and distillation processes; and 5) a effluent that produces a better quality and less hazardous brine for water recovery. Previous work has primarily evaluated aerobic operation in which organic carbon and nitrogen is converted to CO2 and NOx-, respectively. An alternative to aerobic operation would be to include anoxic operation to promote denitrification and production of N2 gas. This allows for production of make-up gas as well as reduces the O2 demand and can increase ammonia oxidation efficiency. We evaluated the operation of a full scale (2 crew/day) MABR operated to perform oxidation of organic carbon and nitrogen with and without simultaneous reduction of oxidized N to N2 gas, simultaneous nitrification denitrification (SNDN). The system was challenged with a variety of space habitation wastewaters ranging from an ISS composition to a possible EPB waste stream under both continuous and on-production feeding modes. The system has been operated for over 2.5 years. We report on an overall comparison of aerobic oxidation and SNDN operational regimes to evaluate the system with the best overall attributes to support recycling of space habitation waste streams.

Biological water processing↗

Aircraft Trajectory Design Based on Reducing the Combined Effects of Carbon-di-oxide, Nitrogen and Contrails

Aircraft operations need to meet the combined requirements of safety, efficiency, capacity and reduced environmental impact. Aircraft routes can be made efficient by flying wind optimal routes. However, the desire to reduce the impact of aviation emissions and contrails may result in trajectories, which deviate from wind optimal trajectories leading to extra fuel use. The lifetime associated with different emissions and contrails varies from a few hours to several hundred years. The impact of certain gases depends on the amount and location of the emission, and the decision-making horizon, in years, when the impact is estimated. The Absolute Global Temperature Potential (AGTP) is used as a metric to measure the combined effects of emissions and contrails. This paper extends earlier work by the authors to include the effect of oxides of nitrogen in the development of aircraft trajectories to reduce the combined effects of carbon dioxide, oxides of nitrogen (NOX) and contrails. The methodology is applied to air traffic in the continental US. The paper shows the trade-offs between reducing emissions and the cost of extra fuel using a fuel sensitivity index, defined as the reduction in AGTP per kg of fuel. The paper shows the performance of the optimization strategy for decision intervals of 10, 25 and 100 years. Based on the simplified models, the inclusion of NOX emissions has a slight influence on the minimal climate impact trajectories when the decision horizons are around 25 years.

Sridhar, Banavar↗

Biomass burning declines lead to large net reductions in NO2 concentrations over north equatorial Africa in spite of growing fossil fuel emissions

Socio-economic development in low and middle-income countries has been accompanied by increased emissions of air pollutants such as nitrogen oxides (NOx: nitrogen dioxide (NO2) + nitric oxide (NO)), which affect human health. In sub-Saharan Africa, fossil fuel combustion has nearly doubled since 2000. At the same time, biomass burning—another important NOx source—has declined in Africa’s northern biomass burning region, attributed to changes in climate and anthropogenic fire management associated with agricultural development. Here we use satellite observations of tropospheric NO2 vertical column densities (VCDs) and burned area to identify NO2 trends and drivers over Africa. Across the northern ecosystems where biomass burning occurs—home to over 350 million people—mean annual tropospheric NO2 VCDs decreased by 4.5% from 2005 through 2017 during the biomass burning season of November through February. Reductions in burned area explained the majority of these change in NO2 VCDs, but there were also weaker relationships between changes in NO2 VCDs and fossil fuel emissions over parts of West Africa, which were stronger during rainy season. Over Africa’s biomass burning regions, NO2 VCDs tended to decrease with increasing population density up to a threshold of approximately 180 people per km2, suggesting that anthropogenic activity causes a net reduction in NO2 emissions across roughly 90% of the continent’s biomass burning regions. In contrast to the widely-held perception that socio-economic development worsens air quality in low and middle-income nations, our results suggest that countries in Africa’s northern biomass burning region are following a different pathway, resulting in regional air quality benefits. However, these benefits may be lost with increasing fossil fuel use.

Biomass burning↗

Isotopically Tracking Nitrogen Oxides, Nitrous Acid, And Nitric Acid, Particulate Nitrate from Wildfire During FIREX-AQ

Wildfires are an important source of reactive nitrogen species including nitrogen oxides (NOx = NO + NO2) and nitrous acid (HONO), as well as products such as nitric acid (HNO3) and particulate nitrate (p-NO3-). These species have strongly influence air quality and climate. In summer of 2019 (July 25 —August 21), as part of the FIREX-AQ ground mission, we drove ~3000 miles and sampled smoke of different ages in both daytime and nighttime from 5 different wildfires in the western US. Using recently developed methods that have been validated in both laboratory and field settings, we conducted high time resolution collection of NOx, NO2, HONO, HNO3, and p-NO3- for off-line characterization of isotopic composition δ15N, δ18O and Δ17O (=δ17O−0.52 δ18O). δ15N serves as a potential tracer for tracking sources and reactive nitrogen cycling pathways, δ18O and Δ17O provide key information about oxidation pathways (i.e. O3 versus RO2). Our measured δ15N for HONO ranges from -4.9‰ to +5.2‰ and -8‰ to +5.2‰ respectively, in the majority overlapping with our prior lab controlled burning results, which suggests the capability of δ15N for tracing the biomass burning emissions against other sources including vehicular emissions and soil emissions. In addition, our measurements show δ18O and Δ17O for NO2 and HONO vary significantly day vs night, as well as in young smoke vs aged smoke, likely reflecting different oxidizing mechanisms under different smoke conditions. Preliminary results of isotopic signatures of all the above reactive nitrogen species will be presented, and their relationships will be explored to identify wildfire derived reactive nitrogen source signatures and to constrain atmospheric processing pathways (e.g. secondary formation of HONO) for different fires under various smoke conditions depending on fuel types, fire conditions and meteorological conditions.

Jiajue Chai↗

Global Environmental Impact of Supersonic Cruise Aircraft in the Stratosphere

We analyze the climate and ozone impacts of commercial supersonic aircraft using state-of-the-science modeling capabilities ranging from plume to global scale. A scenario-based approach captures variability and uncertainty in the impacts with market adoption, aircraft design choices and regulatory scenarios, focusing on different overland flight restrictions. We find that the notional aircraft considered could attract a market of up to 2.5% of year-2035 seat-kilometers. Overland flight restrictions reduce this market by 80–100%. In comparison to subsonic aircraft, contrails are found to be∼10 times less likely to form behind supersonic jets. A Mach 1.6 jet cruising at 17 km altitude causes 0.85 mDU of depletion per billion seat-km, with 54% of this impact attributable to sulfur emissions and 35% to NOx emissions. Asa result, we find a net non-CO2, non-contrail radiative forcing of−0.020 mW m−2per billion seat-km. Long-term adjoint simulations show that net ozone-neutral cruise can be achieved by flying near 14 km, subject to fuel sulfur content and NOx emissions index.

supersonic, Stratosphere, environment↗

Global Environmental Impact of Supersonic Cruise Aircraft in the Stratosphere

We analyze the climate and ozone impacts of commercial supersonic aircraft using state-of-the-science modeling capabilities ranging from plume to global scale. A scenario-based approach captures variability and uncertainty in the impacts with market adoption, aircraft design choices and regulatory scenarios, focusing on different overland flight restrictions. We find that the notional aircraft considered could attract a market of up to 2.5% of year-2035 seat-kilometers. Overland flight restrictions reduce this market by 80–100%. In comparison to subsonic aircraft, contrails are found to be ∼ 10 times less likely to form behind supersonic jets. A Mach 1.6 jet cruising at 17 km altitude causes 0.85 mDU of depletion per billion seat-km, with 54% of this impact attributable to sulfur emissions and 35% to NOx emissions. As a result, we find a net non-CO2, non-contrail radiative forcing of −0.020mWm−2 per billion seat-km. Long-term adjoint simulations show that net ozone-neutral cruise can be achieved by flying near 14 km, subject to fuel sulfur content and NOx emissions index.

Raymond L Speth↗

Effective radiative forcing from emissions of reactive gases and aerosols - a multi-model comparison

This paper quantifies the pre-industrial (1850) to present-day (2014) effective radiative forcing (ERF) of anthropogenic emissions of NOX, volatile organic compounds (VOCs; including CO), SO2, NH3, black carbon, organic carbon, and concentrations of methane, N2O and ozone-depleting halocarbons, using CMIP6 models. Concentration and emission changes of reactive species can cause multiple changes in the composition of radiatively active species: tropospheric ozone, stratospheric ozone, stratospheric water vapour, secondary inorganic and organic aerosol, and methane. Where possible we break down the ERFs from each emitted species into the contributions from the composition changes. The ERFs are calculated for each of the models that participated in the AerChemMIP experiments as part of the CMIP6 project, where the relevant model output was available. The 1850 to 2014 multi-model mean ERFs (± standard deviations) are −1.03 ± 0.37 W/sq.m for SO2 emissions, −0.25 ± 0.09 W/sq.m for organic carbon (OC), 0.15 ± 0.17 W/sq.m for black carbon (BC) and −0.07 ± 0.01 W/sq.m for NH3. For the combined aerosols (in the piClim-aer experiment) it is −1.01 ± 0.25 W/sq.m. The multi-model means for the reactive well-mixed greenhouse gases (including any effects on ozone and aerosol chemistry) are 0.67 ± 0.17 W/sq.m for methane (CH4), 0.26 ± 0.07 W/sq.m for nitrous oxide (N2O) and 0.12 ± 0.2 W/sq.m for ozone-depleting halocarbons (HC). Emissions of the ozone precursors nitrogen oxides (NOx), volatile organic compounds and both together (O3) lead to ERFs of 0.14 ± 0.13, 0.09 ± 0.14 and 0.20 ± 0.07 W/sq.m respectively. The differences in ERFs calculated for the different models reflect differences in the complexity of their aerosol and chemistry schemes, especially in the case of methane where tropospheric chemistry captures increased forcing from ozone production.

radiative forcing↗