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Satellite-Based Evaluation of AeroCom Model Bias in Biomass Burning Regions

Global models are widely used to simulate biomass burning aerosol (BBA). Exhaustive evaluations on model representation of aerosol distributions and properties are fundamental to assess health and climate impacts of BBA. Here we conducted a comprehensive comparison of Aerosol Comparisons between Observations and Models (AeroCom) project model simulations with satellite observations. A total of 59 runs by 18 models from three AeroCom Phase-III experiments (i.e., biomass burning emissions, CTRL16, and CTRL19) and 14 satellite products of aerosols were used in the study. Aerosol optical depth (AOD) at 550 nm was investigated during the fire season over three key fire regions reflecting different fire dynamics (i.e., deforestation-dominated Amazon, Southern Hemisphere Africa where savannas are the key source of emissions, and boreal forest burning in boreal North America). The 14 satellite products were first evaluated against AErosol RObotic NETwork (AERONET) observations, with large uncertainties found. But these uncertainties had small impacts on the model evaluation that was dominated by modeling bias. Through a comparison with Polarization and Directionality of the Earth’s Reflectances measurements with the Generalized Retrieval of Aerosol and Surface Properties algorithm (POLDER-GRASP), we found that the modeled AOD values were biased by −93 % to 152 %, with most models showing significant underestimations even for the state-of-the-art aerosol modeling techniques (i.e., CTRL19). By scaling up BBA emissions, the negative biases in modeled AOD were significantly mitigated, although it yielded only negligible improvements in the correlation between models and observations, and the spatial and temporal variations in AOD biases did not change much. For models in CTRL16 and CTRL19, the large diversity in modeled AOD was in almost equal measures caused by diversity in emissions, lifetime, and the mass extinction coefficient (MEC). We found that in the AeroCom ensemble, BBA lifetime correlated significantly with particle deposition (as expected) and in turn correlated strongly with precipitation. Additional analysis based on Cloud-Aerosol LIdar with Orthogonal Polarization (CALIOP) aerosol profiles suggested that the altitude of the aerosol layer in the current models was generally too low, which also contributed to the bias in modeled lifetime. Modeled MECs exhibited significant correlations with the Ångström exponent (AE, an indicator of particle size). Comparisons with the POLDER-GRASP-observed AE suggested that the models tended to overestimate the AE (underestimated particle size), indicating a possible underestimation of MECs in models. The hygroscopic growth in most models generally agreed with observations and might not explain the overall underestimation of modeled AOD. Our results imply that current global models contain biases in important aerosol processes for BBA (e.g., emissions, removal, and optical properties) that remain to be addressed in future research.

biomass burning aerosols↗

Energy Budget Constraints on the Time History of Aerosol Forcing and Climate Sensitivity

Abstract An observationally constrained time series of historical aerosol effective radiative forcing (ERF) from 1750 to 2019 is developed in this study. We find that the time history of aerosol ERFs diagnosed in CMIP6 models exhibits considerable variation and explore how the time history of aerosol forcing influences the probability distributions of present‐day aerosol forcing and emergent metrics such as climate sensitivity. Using a simple energy balance model, trained on CMIP6 climate models and constrained by observed near‐surface warming and ocean heat uptake, we derive estimates for the historical aerosol forcing. We find 2005–2014 mean aerosol ERF to be −1.1 (−1.8 to −0.5) W m −2 relative to 1750. Assuming recently published historical emissions from fossil fuel and industrial sectors and biomass burning emissions from SSP2‐4.5, aerosol ERF in 2019 is −0.9 (−1.5 to −0.4) W m −2 . There is a modest recovery in aerosol forcing (+0.025 W m −2 decade −1 ) between 1980 and 2014. This analysis also gives a 5%–95% range of equilibrium climate sensitivity of 1.8°C –5.1°C (best estimate 3.1°C) with a transient climate response of 1.2°C –2.6°C (best estimate 1.8°C).

54 ENVIRONMENTAL SCIENCES↗

The Effect of Future Ambient Air Pollution on Human Premature Mortality to 2100 Using Output from the ACCMIP Model Ensemble

Ambient air pollution from ground-level ozone and fine particulate matter (PM(sub 2.5)) is associated with premature mortality. Future concentrations of these air pollutants will be driven by natural and anthropogenic emissions and by climate change. Using anthropogenic and biomass burning emissions projected in the four Representative Concentration Pathway scenarios (RCPs), the ACCMIP ensemble of chemistry climate models simulated future concentrations of ozone and PM(sub 2.5) at selected decades between 2000 and 2100. We use output from the ACCMIP ensemble, together with projections of future population and baseline mortality rates, to quantify the human premature mortality impacts of future ambient air pollution. Future air-pollution-related premature mortality in 2030, 2050 and 2100 is estimated for each scenario and for each model using a health impact function based on changes in concentrations of ozone and PM(sub 2.5) relative to 2000 and projected future population and baseline mortality rates. Additionally, the global mortality burden of ozone and PM(sub 2.5) in 2000 and each future period is estimated relative to 1850 concentrations, using present-day and future population and baseline mortality rates. The change in future ozone concentrations relative to 2000 is associated with excess global premature mortality in some scenarios/periods, particularly in RCP8.5 in 2100 (316 thousand deaths per year), likely driven by the large increase in methane emissions and by the net effect of climate change projected in this scenario, but it leads to considerable avoided premature mortality for the three other RCPs. However, the global mortality burden of ozone markedly increases from 382000 (121000 to 728000) deaths per year in 2000 to between 1.09 and 2.36 million deaths per year in 2100, across RCPs, mostly due to the effect of increases in population and baseline mortality rates. PM(sub 2.5) concentrations decrease relative to 2000 in all scenarios, due to projected reductions in emissions, and are associated with avoided premature mortality, particularly in 2100: between 2.39 and 1.31 million deaths per year for the four RCPs. The global mortality burden of PM(sub 2.5) is estimated to decrease from 1.70 (1.30 to 2.10) million deaths per year in 2000 to between 0.95 and 1.55 million deaths per year in 2100 for the four RCPs due to the combined effect of decreases in PM(sub 2.5) concentrations and changes in population and baseline mortality rates. Trends in future air-pollution-related mortality vary regionally across scenarios, reflecting assumptions for economic growth and air pollution control specific to each RCP and region. Mortality estimates differ among chemistry climate models due to differences in simulated pollutant concentrations, which is the greatest contributor to overall mortality uncertainty for most cases assessed here, supporting the use of model ensembles to characterize uncertainty. Increases in exposed population and baseline mortality rates of respiratory diseases magnify the impact on premature mortality of changes in future air pollutant concentrations and explain why the future global mortality burden of air pollution can exceed the current burden, even where air pollutant concentrations decrease.

Silva, Raquel A.↗

Building the Fire Energetics and Emissions Research (FEER) Smoke Emissions Inventory Version 1.0

The Fire Energetics and Emissions Research (FEER) group's new coefficient of emission global gridded product at 1x1 resolution that directly relates fire readiative energy (FRE) to smoke aerosol release, FEERv1.0 Ce, made its public debut in August 2013. Since then, steps have been taken to generate corresponding maps and totals of total particulate matter (PM) emissions using different sources of FRE, and subsequently to simulate the resulting PM(sub 2.5) in the WRF-Chem 3.5 model using emission rates from FEERv1.0 as well as other standard biomass burning emission inventories. An flowchart of the FEER algorithm to calculate Ce is outlined here along with a display of the resulting emissions of total PM globally and also regionally. The modeling results from the WRF-Chem3.5 simulations are also shown.

particulate matter↗

Aircraft measurements of aerosol and trace gas chemistry in the eastern North Atlantic

The Aerosol and Cloud Experiment in the Eastern North Atlantic (ACE-ENA) investigated properties of aerosols and subtropical marine boundary layer (MBL) clouds. Low subtropical marine clouds can have a large effect on Earth's radiative budget, but they are poorly represented in global climate models. In order to understand their radiative effects, it is imperative to understand the composition and sources of the MBL cloud condensation nuclei (CCN). The campaign consisted of two intensive operation periods (IOPs) (June–July 2017 and January–February 2018) during which an instrumented G-1 aircraft was deployed from Lajes Field on Terceira Island in the Azores, Portugal. The G-1 conducted research flights in the vicinity of the Atmospheric Radiation Measurement (ARM) Eastern North Atlantic (ENA) atmospheric observatory on Graciosa Island. An Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and Ionicon proton-transfer-reaction mass spectrometer (PTR-MS) were deployed aboard the aircraft, characterizing chemistry of non-refractory aerosol and trace gases, respectively. The eastern North Atlantic region was found to be very clean, with an average non-refractory submicrometer aerosol mass loading of 0.6 µg m −3 in the summer and 0.1 µg m −3 in the winter, measured by the AMS. Average concentrations of the trace reactive gases methanol and acetone were 1–2 ppb; benzene, toluene and isoprene were even lower, <1 ppb. Mass fractions of sulfate, organics, ammonium and nitrate in the boundary layer were 69 %, 23 %, 7 % and 1 % and remained largely similar between seasons. The aerosol chemical composition was dominated by sulfate and highly processed organics. Particulate methanesulfonic acid (MSA), a well-known secondary biogenic marine species, was detected, with an average boundary layer concentration of 0.021 µg m −3 , along with its gas-phase precursor, dimethyl sulfide (DMS). MSA accounted for no more than 3 % of the submicron, non-refractory aerosol in the boundary layer. Examination of vertical profiles of aerosol and gas chemistry during ACE-ENA reveals an interplay of local marine emissions and long-range-transported aged aerosol. A case of transport of biomass burning emissions from North American fires has been identified using back-trajectory analysis. In the summer, the non-refractory portion of the background CCN budget was heavily influenced by aerosol associated with ocean productivity, in particular sulfate formed from DMS oxidation. Episodic transport from the continents, particularly of biomass burning aerosol, periodically increased CCN concentrations in the free troposphere. In the winter, with ocean productivity lower, CCN concentrations were overall much lower and dominated by remote transport. These results show that anthropogenic emissions perturb CCN concentrations in remote regions that are sensitive to changes in CCN number and illustrate that accurate predictions of both transport and regional aerosol formation from the oceans are critical to accurately modeling clouds in these regions.

54 ENVIRONMENTAL SCIENCES↗

Composition and Evolution of Southeast Asian Biomass Burning Trace Gas Emissions during a September 2019 Borneo Burning Event

Biomass burning in Southeast Asia is a major pollutant source contributing to poor air quality throughout the region. Thus, understanding these emissions is critical for predicting and mitigating their health impacts. While there have been many studies reporting ground-based and satellite measurements, regional scale measurements to tie the two together have not been common in this region. The 2019 Cloud, Aerosol and Monsoon Processes Philippines Experiment (CAMP2Ex) field campaign examined Southeast Asian regional sources and their effects on aerosol/cloud interactions using a combination of airborne, shipborne, and ground-based measurements. On 16 September, a major biomass burning event primarily located on Borneo was sampled via aircraft in the near-field over the Sulu Sea, while on 17 September, the aged plume from the event was sampled again east of the Philippines over the Philippine Sea. We discuss the emissions from this event, using tracer-tracer ratios (e.g. MCE, NOy/CO), HYSPLIT back trajectories, and HSRL-2 lidar retrievals to differentiate sources and provide insight into the composition and chemical evolution of the plume. This case study provides a valuable perspective into the accuracy of emission inventories as well as a rare opportunity for satellite validation.

Joshua P DiGangi↗

Revised (Mixed-Effects) Estimation for Forest Burning Emissions of Gases and Smoke, Fire/Emission Factor Typology, and Potential Remote Sensing Classification of Types for Ozone and Black-Carbon Simulation

We summarize recent progress (a) in correcting biomass burning emissions factors deduced from airborne sampling of forest fire plumes, (b) in understanding the variability in reactivity of the fresh plumes sampled in ARCTAS (2008), DC3 (2012), and SEAC4RS (2013) airborne missions, and (c) in a consequent search for remotely sensed quantities that help classify forest-fire plumes. Particle properties, chemical speciation, and smoke radiative properties are related and mutually informative, as pictures below suggest (slopes of lines of same color are similar). (a) Mixed-effects (random-effects) statistical modeling provides estimates of both emission factors and a reasonable description of carbon-burned simultaneously. Different fire plumes will have very different contributions to volatile organic carbon reactivity; this may help explain differences of free NOx(both gas- and particle-phase), and also of ozone production, that have been noted for forest-fire plumes in California. Our evaluations check or correct emission factors based on sequential measurements (e.g., the Normalized Ratio Enhancement and similar methods). We stress the dangers of methods relying on emission-ratios to CO. (b) This work confirms and extends many reports of great situational variability in emissions factors. VOCs vary in OH reactivity and NOx-binding. Reasons for variability are not only fuel composition, fuel condition, etc., but are confused somewhat by rapid transformation and mixing of emissions. We use "unmixing" (distinct from mixed-effects) statistics and compare briefly to approaches like neural nets. We focus on one particularly intense fire the notorious Yosemite Rim Fire of 2013. In some samples, NOx activity was not so suppressed by binding into nitrates as in other fires. While our fire-typing is evolving and subject to debate, the carbon-burned delta(CO2+CO) estimates that arise from mixed effects models, free of confusion by background-CO2 variation, should provide a solid base for discussion. (c) We report progress using promising links we find between emissions-related "fire types" and promising features deducible from remote observations of plumes, e.g., single scatter albedo, Angstrom exponent of scattering, Angstrom exponent of absorption, (CO column density)/(aerosol optical depth).

Remote sensing↗

A New Method of Deriving Time-Averaged Tropospheric Column Ozone over the Tropics Using Total Ozone Mapping Spectrometer (TOMS) Radiances: Intercomparison and Analysis Using TRACE A Data

Error analysis of archived total 03 from total ozone mapping spectrometer (TOMS) (version 6) presented. Daily total 03 maps for the tropics, from the period October 6-21, 1992, are derived from TOMS radiances following correction for these errors. These daily maps, averaged together, show a wavelike feature, which is observed in all latitude bands, underlying sharp peaks which occur at different longitudes depending on the latitude. The wave pattern is used to derive both time-averaged stratospheric and tropospheric 03 fields. The nature of the wave pattern (stratospheric or tropospheric) cannot be determined with certainty due to missing data (no Pacific sondes, no lower stratospheric Stratospheric Aerosol and Gas Experiment (SAGE) ozone for 18 months after the Mt. Pinatubo eruption) and significant uncertainties in the corroborative satellite record in the lower stratosphere (solar backscattered ultraviolet (SBUV), microwave limb sounder (MLS)). However, the time- averaged tropospheric ozone field, based on the assumption that the wave feature is stratospheric, agrees within 10% with ultraviolet differential absorption laser Transport and Atmospheric Chemistry near the Equator-Atlantic) (TRACE A) 03 measurements from the DC-8 and with ozonesonde measurements over Brazzaville, Congo, Ascension Island, and Natal, Brazil, for the period October 6-21, 1992. The derived background (nonpolluted) Indian Ocean tropospheric ozone amount, 26 Dobson units (DU), agrees with the cleanest African ozonesonde profiles for September-October 1992. The assumption of a totally tropospheric wave (flat stratosphere) gives 38 DU above the western Indian Ocean and 15-40% disagreements with the sondes. Tropospheric column 03 is high from South America to Africa, owing to interaction of dynamics with biomass burning emissions. Comparison with fire distributions from advanced very high resolution radiometer (AVHHR) during October 1992 suggests that tropospheric 03 produced from biomass burning in South America and Africa dominates the 03 budget in the tropical southern hemisphere during the study period.

Kim, J. H.↗

Update on GOCART Model Development and Applications

Recent results from the GOCART and GMI models are reported. They include: Updated emission inventories for anthropogenic and volcano sources, satellite-derived vegetation index for seasonal variations of dust emission, MODIS-derived smoke AOT for assessing uncertainties of biomass-burning emissions, long-range transport of aerosol across the Pacific Ocean, and model studies on the multi-decadal trend of regional and global aerosol distributions from 1980 to 2010, volcanic aerosols, and nitrate aerosols. The document was presented at the 2013 AEROCENTER Annual Meeting held at the GSFC Visitors Center, May 31, 2013. The Organizers of the meeting are posting the talks to the public Aerocentr website, after the meeting.

emission inventories↗

Characterization of Wildfire Emissions in California: Analysis of Airborne Measurements of Trace Gases from 2013 to 2016

Biomass burning, which includes wildfires, prescribed, and agricultural fires, is an important source of trace gases and particles, and can influence air quality on a local, regional, and global scale. Biomass burning emissions are an important source of several key trace gases including carbon dioxide (CO2) and methane (CH4). With the threat of wildfire events increasing due to changes in land use, increasing population, and climate change, the importance of characterizing wildfire emissions is vital. In this work we characterize trace gas emissions from 9 wildfire events in California between 2013 – 2016, in some cases with multiple measurements performed during different burn periods of a specific wildfire. During this period airborne measurements of CO2, CH4, water vapor (H2O), ozone (O3), and formaldehyde (HCHO) were made by the Alpha Jet Atmospheric eXperiment (AJAX). Located in the Bay Area of California, AJAX is a joint effort between NASA Ames Research Center and H211, LLC. AJAX makes in-situ airborne measurements of trace gases 2-4 times per month, resulting in 229 flights to date since 2011. Results presented include emission ratios (ER) of trace gases measured by AJAX during fire flights, and comparisons of ERs are made for each fire, which differ in time, location, burning intensity, and fuel type. We also use our airborne measurements to compare with photochemical grid model results to assess model approximations of plume transport and chemical evolution from select wildfires.

Parworth, Caroline L.↗

Using Satellite‐Derived Fire Arrival Times for Coupled Wildfire‐Air Quality Simulations at Regional Scales of the 2020 California Wildfire Season

Abstract Wildfire frequency has increased in the Western US over recent decades, driven by climate change and a legacy of forest management practices. Consequently, human structures, health, and life are increasingly at risk due to wildfires. Furthermore, wildfire smoke presents a growing hazard for regional and national air quality. In response, many scientific tools have been developed to study and forecast wildfire behavior, or test interventions that may mitigate risk. In this study, we present a retrospective analysis of 1 month of the 2020 Northern California wildfire season, when many wildfires with varying environments and behavior impacted regional air quality. We simulated this period using a coupled numerical weather prediction model with online atmospheric chemistry, and compare two approaches to representing smoke emissions: an online fire spread model driven by remotely sensed fire arrival times and a biomass burning emissions inventory. First, we quantify the differences in smoke emissions and timing of fire activity, and characterize the subsequent impact on estimates of smoke emissions. Next, we compare the simulated smoke to surface observations and remotely sensed smoke; we find that despite differences in the simulated smoke surface concentrations, the two models achieve similar levels of accuracy. We present a detailed comparison between the performance and relative strengths of both approaches, and discuss potential refinements that could further improve future simulations of wildfire smoke. Finally, we characterize the interactions between smoke and meteorology during this event, and discuss the implications that increases in regional smoke may have on future meteorological conditions.

54 ENVIRONMENTAL SCIENCES↗

Cloud processing and weeklong ageing affect biomass burning aerosol properties over the south-eastern Atlantic

Abstract Southern Africa produces a third of global biomass burning emissions, which have a long atmospheric lifetime and influence regional radiation balance and climate. Here, we use airmass trajectories to link different aircraft observations to investigate the evolution of biomass-burning aerosols during their westward transport from Southern Africa over the south-eastern Atlantic, where a semi-permanent stratocumulus cloud deck is located. Our results show secondary organic aerosol formation during the initial 3 days of transport, followed by decreases in organic aerosol via photolysis before reaching equilibrium. Aerosol absorption wavelength dependency decreases with ageing, due to an increase in particle size and photochemical bleaching of brown carbon. Cloud processing, including aqueous-phase reaction and scavenging, contributes to the oxidation of organic aerosols, while it strongly reduces large diameter particles and single-scattering albedo of biomass burning aerosols. Together, these processes resulted in a marine boundary layer with fewer yet more oxidized and absorbing aerosols.

54 ENVIRONMENTAL SCIENCES↗

Influence of plumes from biomass burning on atmospheric chemistry over the equatorial and tropical South Atlantic during CITE 3

During all eight flights conducted over the equatorial and tropical South Atlantic in the course of the Chemical Instrumentation Test and Evaluation (CITE 3) experiment, we observed haze layers with elevated concentrations of aerosols, O3, CO, and other trace gases related to biomass burning emissions. They occurred at altitudes between 1000 and 5200 m and were usually only some 100-300 m thick. These layers extended horizontally over several 100 km and were marked by the presence of visible brownish haze. Air mass trajectories indicate that these layers originate in the biomass burning regions of Africa and South America and typically have aged at least 10 days since the time of emission. In the haze layers, O3 and CO concentrations up to 90 and 210 ppb were observed, respectively. The two species were highly correlated. The ratio concentrations in plume minus background concentrations of O3/CO is typically in the range 0.2-0.7, much higher than the ratios in the less aged plumes investigated previously in Amazonia. In most cases, aerosol (0.12-3 micrometer diameter) number concentrations were also elevated by up to 400/cu cm in the layers; aerosol enrichments were also strongly correlated with elevated CO levels. Clear correlations between CO and NO(x) enrichments were not apparent due to the age of the plumes, in which most NO(x) would have already reacted away within 1-2 days. Only in some of the plumes could clear correlations between NO(y) and CO be identified; the absence of a general correlation between NO(y) and CO may be due to instrumental limitations and to variable sinks for NO(y). The average enrichment of the ratio concentrations in plume minus background concentrations of NO(y)/CO was quite high, consistent with the efficient production of ozone observed in the plumes. The chemical characteristics of the haze layers, together with remote sensing information and trajectory calculations, suggest that fire emissions (in Africa and/or South America) are the primary source of the haze layer components.

Andreae, M. O.↗

In Situ Measurements of Ammonia In Plumes Emitted From Wildfires And Agricultural Fires in the US

Emissions of trace gases and particles from fires have a major impact on climate, visibility, air quality, and public health. Biomass burning emissions include reactive nitrogen gases, among which ammonia (NH3) plays a prominent role. NH3 is a short-lived gas that acts as precursor for secondary inorganic aerosols. This process is still poorly constrained in downwind fire plumes. In summer 2019, NASA and NOAA carried out the joint airborne FIREX-AQ (Fire Influence on Regional to global Environments and Air Quality) mission over the continental US to sample plumes from wildfires and agricultural fires. On board the NASA DC-8, we used a modified PTR-ToF-MS instrument for measuring NH3 in situ and at high time resolution. Over the course of the mission, we collected a large set of NH3 data in plumes emitted from fires differing in fuel type and burning stage. Herein, we will present the measured NH3 emissions ratios and factors, compare them with the literature, and investigate the dependence of NH3 emissions on fuel type and burning conditions.

ammonia↗

Aerosol characteristics at the Southern Great Plains site during the HI-SCALE campaign

Abstract. Large uncertainties exist in global climate model predictions of radiative forcing due to insufficient understanding and simplified numerical representation of cloud formation and cloud–aerosol interactions. The Holistic Interactions of Shallow Clouds, Aerosols and Land Ecosystems (HI-SCALE) campaign was conducted near the DOE's Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) site in north-central Oklahoma to provide a better understanding of land–atmosphere interactions, aerosol and cloud properties, and the influence of aerosol and land–atmosphere interactions on cloud formation. The HI-SCALE campaign consisted of two intensive observational periods (IOPs) (April–May and August–September, 2016), during which coincident measurements were conducted both on the G-1 aircraft platform and at the SGP ground site. In this study we focus on the observations at the SGP ground site. An Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and an Ionicon proton-transfer-reaction mass spectrometer (PTR-MS) were deployed, characterizing chemistry of non-refractory aerosol and trace gases, respectively. Contributions from various aerosol sources, including biogenic and biomass burning emissions, were retrieved using factor analysis of the AMS data. In general, the organic aerosols at the SGP site was highly oxidized, with oxygenated organic aerosol (OOA) identified as the dominant factor for both the spring and summer IOP though more aged in spring. Cases of isoprene-epoxydiol-derived secondary organic aerosol (IEPOX SOA) and biomass burning events were further investigated to understand additional sources of organic aerosol. Unlike other regions largely impacted by IEPOX chemistry, the IEPOX SOA at SGP was more highly oxygenated, likely due to the relatively weak local emissions of isoprene. Biogenic emissions appear to largely control the formation of organic aerosol (OA) during the HI-SCALE campaign. Potential HOM (highly oxygenated molecule) chemistry likely contributes to the highly oxygenated feature of aerosols at the SGP site, with impacts on new particle formation and global climate.

54 ENVIRONMENTAL SCIENCES↗

True Emission Factors for Forest Fires and the Role of Non-Fire NOx

True Emission Factors for Forest Fires and the Role of Non-Fire NOx Robert B. Chatfield and Meinrat Andreae The standard way to estimate biomass burning emissions factors from airborne, surface, or laboratory data is to relate the emitted pollutant concentration to the carbon burned, C(sub tot), and liberated to the air, mostly CO2. We approximate total emitted carbon C(sub tot) ~ (CO2 + CO). Emission ratios that are based on CO, describing burning effects, delta-parameter delta-CO, are often used to quantify fire emissions. These are not as useful as emission factors, for they often complicate analyses, since delta-CO delta-CO2 may vary by unto tenfold, and can have bias artifacts of similar magnitude. We present a methodology that estimates both emission factors and a reasonable description of background C(sub tot). High O3 values require a history of the balanced interaction of two pollutant types, nitrogen oxides (NOx) and a radical source, VOCs. However, high VOC NOx ratios seen in many plumes, especially from smoldering-dominated fires, make substantial O3 formation less likely. One particularly intense fire we analyzed, the notorious Rim Fire of 2013, near Yosemite, California. It produced notable quantities of free NOx and (both gas- and particle-phase) Cl species. Consequently, we also outline a quantitative way to assess the effects of anthropogenic or lightning NOx. We provide the example of California burning emissions using measurements of HCHO, NO, and the photolysis rate j(sub HCHO).

Chatfield, Robert B.↗

Global Partitioning of NOx Sources Using Satellite Observations: Relative Roles of Fossil Fuel Combustion, Biomass Burning and Soil Emissions

This document contains the following abstract for the paper "Global partitioning of NOx sources using satellite observations: Relative roles of fossil fuel combustion, biomass burning and soil emissions." Satellite observations have been used to provide important new information about emissions of nitrogen oxides. Nitrogen oxides (NOx) are significant in atmospheric chemistry, having a role in ozone air pollution, acid deposition and climate change. We know that human activities have led to a three- to six-fold increase in NOx emissions since pre-industrial times, and that there are three main surface sources of NOx: fuel combustion, large-scale fires, and microbial soil processes. How each of these sources contributes to the total NOx emissions is subject to some doubt, however. The problem is that current NOx emission inventories rely on bottom-up approaches, compiling large quantities of statistical information from diverse sources such as fuel and land use, agricultural data, and estimates of burned areas. This results in inherently large uncertainties. To overcome this, Lyatt Jaegle and colleagues from the University of Washington, USA, used new satellite observations from the Global Ozone Monitoring Experiment (GOME) instrument. As the spatial and seasonal distribution of each of the sources of NOx can be clearly mapped from space, the team could provide independent topdown constraints on the individual strengths of NOx sources, and thus help resolve discrepancies in existing inventories. Jaegle's analysis of the satellite observations, presented at the recent Faraday Discussion on "Atmospheric Chemistry", shows that fuel combustion dominates emissions at northern mid-latitudes, while fires are a significant source in the Tropics. Additionally, she discovered a larger than expected role for soil emissions, especially over agricultural regions with heavy fertilizer use. Additional information is included in the original extended abstract.

Jaegle, Lyatt↗

North African savanna fires and atmospheric carbon dioxide

The effect of north African savanna fires on atmospheric CO2 is investigated using a tracer transport model. The model uses winds from operational numerical weather prediction analyses and provides CO2 concentrations as a function of space and time. After a spin-up period of several years, biomass-burning sources are added, and model experiments are run for an additional year, utilizing various estimates of CO2 sources. The various model experiments show that biomass burning in the north African savannas significantly affects CO2 concentrations in South America. The effect is more pronounced during the period from January through March, when biomass burning in South America is almost nonexistent. During this period, atmospheric CO2 concentrations in parts of South America typically may increase by 0.5 to 0.75 ppm at 970 mbar, the average pressure of the lowest model layer. These figures are above the probable uncertainty level, as model runs with biomass-burning sources estimated from independent studies using distinct data sets and techniques indicate. From May through September, when severe biomass burning occurs in South America, the effect of north African savanna fires over South America has become generally small at 970 mbar, but north of the equator it may be of the same magnitude or larger than the effect of South American fires. The CO2 concentration increase in the extreme northern and southern portions of South America, however, is mostly due to southern African fires, whose effect may be 2-3 times larger than the effect of South American fires at 970 mbar. Even in the central part of the continent, where local biomass-burning emissions are maximum, southern African fires contribute to at least 15% of the CO2 concentration increase at 970 mbar. At higher levels in the atmosphere, less CO2 emitted by north African savanna fires reaches South America, and at 100 mbar no significant amount of CO2 is transported across the Atlantic Ocean. The vertical structure of the CO2 concentration increase due to biomass burning differs substantially, depending on whether sources are local or remote. A prominent maximum of CO2 concentration increase in the lower layers characterizes the effect of local sources, whereas a more homogeneous profile of CO2 concentration increase characterizes the effect of remote sources. The results demonstrate the strong remote effects of African biomoass burning which, owing to the general circulation of the atmosphere, are felt as far away as South America.

Iacobellis, Sam F.↗