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NASA NTRS2022

Wetland Emission and Atmospheric Sink Changes Explain Methane Growth in 2020

Atmospheric methane growth reached an exceptionally high rate of 15.1 ± 0.4 parts per billion per year in 2020 despite a probable decrease in anthropogenic methane emissions during COVID-19 lockdowns(1). Here we quantify changes in methane sources and in its atmospheric sink in 2020 compared with 2019. We find that, globally, total anthropogenic emissions decreased by 1.2 ± 0.1 teragrams of methane per year (Tg CH4 yr−1), fire emissions decreased by 6.5 ± 0.1 Tg CH4 yr−1 and wetland emissions increased by 6.0 ± 2.3 Tg CH4 yr−1. Tropospheric OH concentration decreased by 1.6 ± 0.2 per cent relative to 2019, mainly as a result of lower anthropogenic nitrogen oxide (NOx) emissions and associated lower free tropospheric ozone during pandemic lockdowns(2). From atmospheric inversions, we also infer that global net emissions increased by 6.9 ± 2.1 Tg CH4 yr−1 in 2020 relative to 2019, and global methane removal from reaction with OH decreased by 7.5 ± 0.8 Tg CH4 yr−1. Therefore, we attribute the methane growth rate anomaly in 2020 relative to 2019 to lower OH sink (53 ± 10 per cent) and higher natural emissions (47 ± 16 per cent), mostly from wetlands. In line with previous findings(3,4,) our results imply that wetland methane emissions are sensitive to a warmer and wetter climate and could act as a positive feedback mechanism in the future. Our study also suggests that nitrogen oxide emission trends need to be taken into account when implementing the global anthropogenic methane emissions reduction pledge(5).

Shushi Peng↗

NASA NTRS2019

Integrating Remote Sensing Observations with NASA's GEOS-5 Modeling Framework in Support of Retrospective Analyses and Seasonal Prediction of Biosphere-Atmosphere CO2 Flux

The absorption of nearly half of all anthropogenic carbon dioxide (CO2) emissions by terrestrial and marine ecosystems has played a critical role in mitigating climate change. However, a persistent lack of understanding of these uptake processes impedes attribution, and thereby introduces large uncertainties into projections of the trajectory of carbon and climate in coming decades. A better understanding and quantification of the seasonal and interannual variability of carbon flux between the atmosphere and ocean and terrestrial biospheres is critically needed to improve predictions from Earth system models. We propose to bring together a diverse suite of remote sensing observations, mechanistic models, and NASA's Goddard Earth Observing System, version 5 (GEOS-5) model to address two objective 1) quantify the processes controlling the temporal variability of biosphere-atmosphere CO2 flux on seasonal and interannual timescales from 1989 to 2018 and 2) evaluating the predictability of the components of carbon flux on seasonal timescales. Because GEOS-5 has been developed to incorporate a variety of Earth system observations and includes a complete and physically consistent depiction of the atmosphere, land, and ocean carbon cycles, it represents a unique and ideal synthesis framework for this effort. By expanding the realism of processes that could be included in GEOS-5 seasonal forecasts, this effort supports NASA's goals toward an integrated Earth system modeling and prediction framework.We propose to integrate a number of observations into the GEOS-5 modeling system to refine retrospective estimates of both terrestrial and marine carbon flux and to test hypotheses regarding the effects of climate drivers on terrestrial carbon flux. This will include assimilating several satellite ocean color products in the NASA Ocean Biogeochemistry Model (NOBM) to improve the representation of ocean biology. We will also utilize remote sensing datasets to increase the temporal resolution of global land-use change estimates and fire emissions to better constrain the temporal variability of the terrestrial carbon cycle. This information will be incorporated into two NASA terrestrial biosphere models Catchment-CN, a dynamic vegetation model that is integrated within GEOS-5 and the Ecosystem Demography (ED) model, a core modeling resource supporting the Global Ecosystem Dynamics Investigation (GEDI) mission to map biomass. Fluxes will be evaluated through 1) comparison to top-down flux estimates inferred from surface CO2 observations and 2) comparison against available aircraft and satellite observations.By combining predictions of net ecosystem exchange and air-sea CO2 flux from land and ocean models with statistical predictions of land use change, fire, and fossil fuel emissions, we propose to create the first dynamical CO2 forecast on seasonal timescales. Because of the experimental nature of this endeavor, an important project objective will be to evaluate the limits to the predictability of different carbon cycle processes over lead times of 1-12 months using different satellite and surface data streams.

Ott, Lesley↗

DOE OSTI2024

Improving North American Wildfire Prediction by Integrating a Machine-Learning Fire Model in a Land Surface Model

Wildfires have shown increasing trends in both frequency and severity across the Contiguous United States (CONUS). However, process-based fire models have difficulties in accurately simulating the burned area over the CONUS due to a simplification of the physical process and cannot capture the interplay among fire, ignition, climate, and human activities. The deficiency of burned area simulation deteriorates the description of fire impact on energy balance, water budget, and carbon fluxes in the Earth System Models (ESMs). Alternatively, machine learning (ML) based fire models, which capture statistical relationships between the burned area and environmental factors, have shown promising burned area predictions and corresponding fire impact simulation. We develop a hybrid framework (ML4Fire-XGB) that integrates a pretrained eXtreme Gradient Boosting (XGBoost) wildfire model with the Energy Exascale Earth System Model (E3SM) land model (ELM) version 2.1. A Fortran-C-Python deep learning bridge is adapted to support online communication between ELM and the ML fire model. Specifically, the burned area predicted by the ML-based wildfire model is directly passed to ELM to adjust the carbon pool and vegetation dynamics after disturbance, which are then used as predictors in the ML-based fire model in the next time step. Evaluated against the historical burned area from Global Fire Emissions Database 5 from 2001-2020, the ML4Fire-XGB model outperforms process-based fire models in terms of spatial distribution and seasonal variations. Sensitivity analysis confirms that the ML4Fire-XGB well captures the responses of the burned area to rising temperatures. The ML4Fire-XGB model has proved to be a new tool for studying vegetation-fire interactions, and more importantly, enables seamless exploration of climate-fire feedback, working as an active component in E3SM.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Simulated wildfire burned area over the CONUS during 2001-2020

Wildfires have shown increasing trends in both frequency and severity across the Contiguous United States (CONUS). However, process-based fire models have difficulties in accurately simulating the burned area over the CONUS due to a simplification of the physical process and cannot capture the interplay among fire, ignition, climate, and human activities. The deficiency of burned area simulation deteriorates the description of fire impact on energy balance, water budget, and carbon fluxes in the Earth System Models (ESMs). Alternatively, machine learning (ML) based fire models, which capture statistical relationships between the burned area and environmental factors, have shown promising burned area predictions and corresponding fire impact simulation. We develop a hybrid framework (ML4Fire-XGB) that integrates a pretrained eXtreme Gradient Boosting (XGBoost) wildfire model with the Energy Exascale Earth System Model (E3SM) land model (ELM). A Fortran-C-Python deep learning bridge is adapted to support online communication between ELM and the ML fire model. Specifically, the burned area predicted by the ML-based wildfire model is directly passed to ELM to adjust the carbon pool and vegetation dynamics after disturbance, which are then used as predictors in the ML-based fire model in the next time step. Evaluated against the historical burned area from Global Fire Emissions Database 5 from 2001-2020, the ML4Fire-XGB model outperforms process-based fire models in terms of spatial distribution and seasonal variations. Sensitivity analysis confirms that the ML4Fire-XGB well captures the responses of the burned area to rising temperatures. The ML4Fire-XGB model has proved to be a new tool for studying vegetation-fire interactions, and more importantly, enables seamless exploration of climate-fire feedback, working as an active component in E3SM.

Liu, Ye↗

NASA NTRS2012

Carbon Consequences of Forest Disturbance and Recovery Across the Conterminous United States

Forests of North America are thought to constitute a significant long term sink for atmospheric carbon. The United States Forest Service Forest Inventory and Analysis (FIA) program has developed a large data base of stock changes derived from consecutive estimates of growing stock volume in the US. These data reveal a large and relatively stable increase in forest carbon stocks over the last two decades or more. The mechanisms underlying this national increase in forest stocks may include recovery of forests from past disturbances, net increases in forest area, and growth enhancement driven by climate or fertilization by CO2 and Nitrogen. Here we estimate the forest recovery component of the observed stock changes using FIA data on the age structure of US forests and carbon stocks as a function of age. The latter are used to parameterize forest disturbance and recovery processes in a carbon cycle model. We then apply resulting disturbance/recovery dynamics to landscapes and regions based on the forest age distributions. The analysis centers on 28 representative climate settings spread about forested regions of the conterminous US. We estimate carbon fluxes for each region and propagate uncertainties in calibration data through to the predicted fluxes. The largest recovery-driven carbon sinks are found in the South central, Pacific Northwest, and Pacific Southwest regions, with spatially averaged net ecosystem productivity (NEP) of about 100 g C / square m / a driven by forest age structure. Carbon sinks from recovery in the Northeast and Northern Lake States remain moderate to large owing to the legacy of historical clearing and relatively low modern disturbance rates from harvest and fire. At the continental scale, we find a conterminous U.S. forest NEP of only 0.16 Pg C/a from age structure in 2005, or only 0.047 Pg C/a of forest stock change after accounting for fire emissions and harvest transfers. Recent estimates of NEP derived from inventory stock change, harvest, and fire data show twice the NEP sink we derive from forest age distributions. We discuss possible reasons for the discrepancies including modeling errors and the possibility of climate and/or fertilization (CO2 or N) growth enhancements.

Williams, Christopher A.↗

NASA NTRS1991

Characteristics of smoke emissions from biomass fires of the Amazon region - BASE-A experiment

The Biomass Burning Airborne and Spaceborne Experiment-Amazonia was designed for study of both aerosol and gaseous emissions from fires using an airborne sampling platform. The emission factors for combustion products from four fires suggest that the proportion of carbon released in the form of CO2 is higher than for fires of logging which has been burned in the western U.S. Combustion efficiency was of the order of 97 percent for the Amazonian test fire and 86-94 percent for deforestation fires. The inorganic content of particles from tropical fires are noted to be different from those of fires in the U.S.

Ward, Darold E.↗

NASA NTRS1988

Particulate emissions from a mid-latitude prescribed chaparral fire

Particulate emission from a 400-acre prescribed chaparral fire in the San Dimas Experimental Forest was investigated by collecting smoke aerosol on Teflon and glass-fiber filters from a helicopter, and using SEM and EDAX to study the features of the particles. Aerosol particles ranged in size from about 0.1 to 100 microns, with carbon, oxygen, magnesium, aluminum, silicon, calcium, and iron as the primary elements. The results of ion chromatographic analysis of aerosol-particle extracts (in water-methanol) revealed the presence of significant levels of NO2(-), NO3(-), SO4(2-), Cl(-), PO4(3-), C2O4(2-), Na(+), NH4(+), and K(+). The soluble ionic portion of the aerosol was estimated to be about 2 percent by weight.

Cofer, Wesley R., III↗

NASA NTRSDate not supplied

Comparing the Regional Variability of Emission Factors of Greenhouse Gases Over Different Landscape During FIREX-AQ Campaign

Biomass burning (wildfires, prescribed and agricultural burning) is one of the major sources of trace gases and particulate emissions and annual variability in growth rates. Biomass burning can impact local, regional, and global air quality, as well as climate. Measurements of emissions from biomass burning are crucial to a better understanding of how it influences and interacts with biogeochemical cycles. High resolution in-situ measurements were recorded onboard the NASA DC-8 aircraft during the FIREX-AQ (Fire Influence on Regional to Global Environments and Air Quality) airborne field campaign July-September, 2019, which was conducted over the continental U.S. Fire emission factors (EF) are essential input for emissions models used to develop biomass burning emission inventories. Here we present the Emission Ratio (ER), MCE (Modified Combustion Efficiency), and EF (Emission Factor) of CO2, CO, and CH4, which constitute the majority of carbon emitted from the wildland, prescribed, and agricultural fires. EFCO2, EFCO, and EFCH4 from the Wildland fires at Williams Flats, WA (primarily Douglas Fir, Ponderosa pine, wheatgrass: 50-75%), ranged from 1527 – 1820 g/kg (Avg. 1641±42), 6.5 – 174.1 g/kg (110.5±24.1), and 0.7 – 11.3 g/kg (6.2±1.9), respectively. EFs from the Arizona CASTLE fire, with somewhat different fuel sources (primarily Ponderosa pine, Douglas fir: 40-70%) ranged from 1266 – 1667 g/kg (1596±59), 99.5 – 344.5 g/kg (136.7±36.8), and 0.4 – 9.2 g/kg (7.2±1.7), respectively. Another primary driver of EFs is likely fire weather. Detailed variability of greenhouse gas EFs will be examined and presented in accordance with different fuels and fire conditions at burned areas, specifically within unique wildland and croplands, using the FCCS (Fuel Characteristic Classification System) 30m land cover identification and the Cropland Data Layer (CDL).

Biomass burning↗

NASA NTRSDate not supplied

Comparing the regional variability of emission factors of greenhouse gases over different landscape during FIREX-AQ campaign

Biomass burning↗

NASA NTRS2021

Research Questions and Challenges for Improved Spacecraft Fire Detection

This paper describes challenges and recommendations for research to improve spacecraft fire detection. Because crew safety is critical to every spaceflight mission, effective fire detectors must detect a wide variety of fires to ensure the success of future space exploration. Fire emissions are affected by fuel type, heating conditions, gravity and exploration atmosphere. Advances in sensing technology provide a promising basis for future detectors, which must selectively detect a broad variety of fires. Addressing these areas will secure the success of future lunar and deep space missions.

Claire Fortenberry↗

DOE OSTI2025

Sensitivity of Regional WRF‐Chem Air Quality and Weather Simulations to Biomass‐Burning Emission Data Sets: A Case Study of the Impact of Canadian Wildfire on the US°

This study focuses on the period from June 26 to 29, 2023, when record‐breaking Canadian wildfires severely impacted air quality in the Midwest United States. Using the Weather Research and Forecasting Model with Chemistry (WRF‐Chem) and four biomass‐burning data sets (Fire Inventory from NCAR version 1, Fire Inventory from NCAR version 2.5, Quick Fire Emissions Data set [QFED], and Regional ABI‐VIIRS Emission), we analyzed aerosol transport from Canada to the US and assessed the model's accuracy in predicting PM 2.5 , O 3 , CO and aerosol weather feedback. Model simulations were compared with ground‐based and remote sensing observations as well as field measurements from the Community Research on Climate and Urban Science (CROCUS) project. Our findings show that the movement of a low‐pressure system from the Great Lakes to the Atlantic, combined with the high‐pressure system over the Atlantic, caused the transport of aerosols from Canadian wildfires to the US. Results show WRF‐Chem significantly underestimated key atmospheric components: aerosol optical depth (AOD) by over 50%, PM 2.5 by 65%–90% and peak O 3 concentrations by 50%–55% across four biomass burning data sets. Additionally, CO and NO 2 concentrations were underpredicted. The substantial underestimation of PM 2.5 led to an overestimation of temperature by up to 3.6 °C primarily due to excessive downward shortwave radiation, which resulted from the underestimation of direct aerosol effects and an increase in sensible heat flux. Among the biomass‐burning data sets, QFED produced the most accurate AOD and PM 2.5 predictions due to improved wildfire emission estimates, leading to a 1.0 to 1.5 °C reduction in temperature overestimation during the daytime. These findings underscore the need for improving wildfire emission estimates for trace gases and aerosols to enhance air quality and weather feedback predictions.

WRF-chem model↗

NASA NTRS2012

Satellite-based Assessment of Climate Controls on US Burned Area

Climate regulates fire activity through the buildup and drying of fuels and the conditions for fire ignition and spread. Understanding the dynamics of contemporary climate-fire relationships at national and sub-national scales is critical to assess the likelihood of changes in future fire activity and the potential options for mitigation and adaptation. Here, we conducted the first national assessment of climate controls on US fire activity using two satellite-based estimates of monthly burned area (BA), the Global Fire Emissions Database (GFED, 1997 2010) and Monitoring Trends in Burn Severity (MTBS, 1984 2009) BA products. For each US National Climate Assessment (NCA) region, we analyzed the relationships between monthly BA and potential evaporation (PE) derived from reanalysis climate data at 0.5 resolution. US fire activity increased over the past 25 yr, with statistically significant increases in MTBS BA for entire US and the Southeast and Southwest NCA regions. Monthly PE was strongly correlated with US fire activity, yet the climate driver of PE varied regionally. Fire season temperature and shortwave radiation were the primary controls on PE and fire activity in the Alaska, while water deficit (precipitation PE) was strongly correlated with fire activity in the Plains regions and Northwest US. BA and precipitation anomalies were negatively correlated in all regions, although fuel-limited ecosystems in the Southern Plains and Southwest exhibited positive correlations with longer lead times (6 12 months). Fire season PE in creased from the 1980s 2000s, enhancing climate-driven fire risk in the southern and western US where PE-BA correlations were strongest. Spatial and temporal patterns of increasing fire season PE and BA during the 1990s 2000s highlight the potential sensitivity of US fire activity to climate change in coming decades. However, climatefire relationships at the national scale are complex, based on the diversity of fire types, ecosystems, and ignition sources within each NCA region. Changes in the seasonality or magnitude of climate anomalies are therefore unlikely to result in uniform changes in US fire activity.

Morton, D. C.↗

DOE OSTI2024

Enhanced Carbon Flux Response to Atmospheric Aridity and Water Storage Deficit During the 2015–2016 El Niño Compromised Carbon Balance Recovery in Tropical South America

During the 2015–2016 El Niño, the Amazon basin released almost one gigaton of carbon (GtC) into the atmosphere due to extreme temperatures and drought. The link between the drought impact and recovery of the total carbon pools and its biogeochemical drivers is still unknown. With satellite-constrained net carbon exchange and its component fluxes including gross primary production and fire emissions, we show that the total carbon loss caused by the 2015–2016 El Niño had not recovered by the end of 2018. Forest ecosystems over the Northeastern (NE) Amazon suffered a cumulative total carbon loss of ~0.6 GtC through December 2018, driven primarily by a suppression of photosynthesis whereas southeastern savannah carbon loss was driven in part by fire. We attribute the slow recovery to the unexpected large carbon loss caused by the severe atmospheric aridity coupled with a water storage deficit during drought. We show the attenuation of carbon uptake is three times higher than expected from the pre-drought sensitivity to atmospheric aridity and ground water supply. Our study fills an important knowledge gap in our understanding of the unexpectedly enhanced response of carbon fluxes to atmospheric aridity and water storage deficit and its impact on regional post-drought recovery as a function of the vegetation types and climate perturbations. Our results suggest that the disproportionate impact of water supply and demand could compromise resiliency of the Amazonian carbon balance to future increases in extreme events.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRSDate not supplied

PyroCbs from Australia Fires and its Impact Using Satellite Observations from CrIS and TROPOMI and Reanalysis Data

Pyrocumulonimbus (pyroCb) clouds are thunder clouds created by intense heat from the Earth’s surface. They are formed similarly to cumulonimbus clouds, but the intense heat that results in the vigorous updraft comes from fire, either large wildfires or volcanic eruptions. Australia’s unprecedented fire disasters at the end of 2019 to early 2020 emitted huge amounts of carbon monoxide (CO) and fire aerosol particles to the atmosphere, particularly during the pyroCb outbreak that occurred in southeast Australia between 29 December 2019 and 4 January 2020. It was estimated that at least 18 pyroCbs were generated during this episode, and some of them injected ice, smoke, and biomass burning gases above the local tropopause. An unprecedented abundance of H2O and CO in the stratosphere, and the displacement of background ozone (O3) and N2O from rapid ascent of air from the troposphere and lower stratosphere were found from satellite observations. Some other studies also found that the fire emissions and their long-range transport resulted in stratospheric aerosol, temperature, and O3 anomalies after the 2020 Australian bushfires and altered the Antarctic ozone and vortex, posing great impact to local air quality and climate change. Further study on the atmospheric thermodynamic status of atmosphere associated with these pyroCbs, and the change of the cloud properties and trace gases during this unprecedented Australia fires will be made using a new single Field of View (SFOV) Sounder Atmospheric Products (SiFSAP). SiFSAP was developed by NASA using the Cross-track Infrared Sounder (CrIS) and Advanced Technology Microwave Sounder (ATMS) onboard SNPP and JPSS-1, and will soon be available to the public at NASA DAAC. Since this product has a spatial resolution of 15 km at nadir, which is better than most global weather and climate models and other current operational sounding products, a process-oriented analysis of the dynamic transport of CO and fire plumes during this unprecedented fire disasters will be made in this study. Based on a Principal Component Radiative Transfer Model (PCRTM) and an optimized estimation retrieval algorithm, a simultaneously retrieval is made using the whole spectral information measured by CrIS, and the derived SiFSAP include temperature, water vapor, trace gases (such as O3, CO2, CO, CH4 and N2O), cloud properties and surface properties. Use of ATMS together with CrIS allows SiFSAP to get accurate retrieval products under thick pyroCb conditions, and an algorithm to detect pyroCb based on the hyperspectral infrared sounder spectrum from CrIS will be developed and verified. In addition to SiFSAP sounding products, other products like CO, O3, NO2 from TROPOMI, O3 from OMPS will be used for retrospective analysis. The wind fields from the NASA’s Modern-Era Retrospective Analysis for Research and Applications Version-2 (MERRA-2) and ERA5 will be used to characterize the transport, and the SiFSAP temperature and water vapor profiles within and around pyroCbs will be compared with MERRA-2 and ERA5 products.

Xiaozhen (Shawn) Xiong↗

NASA NTRS2024

Multi-Agency Ensemble Forecast of Wildfire Air Quality in the United States: Toward Community Consensus of Early Warning

Wildfires pose increasing risks to human health and properties in North America. Due to large uncertainties in fire emission, transport, and chemical transformation, it remains challenging to accurately predict air quality during wildfire events, hindering our collective capability to issue effective early warnings to protect public health and welfare. Here we present a new real-time Hazardous Air Quality Ensemble System (HAQES) by leveraging various wildfire smoke forecasts from three U.S. federal agencies (NOAA, NASA, and Navy). Compared to individual models, the HAQES ensemble forecast significantly enhances forecast accuracy. To further enhance forecasting performance, a weighted ensemble forecast approach was introduced and tested. Compared to the unweighted ensemble mean, the multilinear regression weighted ensemble reduced fractional bias by 34% in the major fire regions, false alarm rate by 72%, and increased hit rate by 17%. Finally, we improved the weighted ensemble using quantile regression and weighted regression methods to enhance the forecast of extreme air quality events. The advanced weighted ensemble increased the PM2.5 exceedance hit rate by 55% compared to the ensemble mean. Our findings provide insights into the development of advanced ensemble forecast methods for wildfire air quality, offering a practical way to enhance decision-making support to protect public health.

Yunyao Li↗

NASA NTRS2022

Climate Drivers of Global Wildfire Burned Area

Wildfire is an integral part of the Earth system, but at the same time it can pose serious threats to human society and to certain types of terrestrial ecosystems. Meteorological conditions are a key driver of wildfire activity and extent, which led to the emergence of the use of fire danger indices that depend solely on weather conditions. The Canadian Fire Weather Index (FWI) is a widely used fire danger index of this kind. Here, we evaluate how well the FWI, its components, and the climate variables from which it is derived, correlate with observation-based burned area (BA) for a variety of world regions. We use a novel technique, according to which monthly BA are grouped by size for each Global Fire Emissions Database (GFED) pyrographic region. We find strong correlations of BA anomalies with the FWI anomalies, as well as with the underlying deviations from their climatologies for the four climate variables from which FWI is estimated, namely, temperature, relative humidity, precipitation, and wind. We quantify the relative sensitivity of the observed BA to each of the four climate variables, finding that this relationship strongly depends on the pyrographic region and land type. Our results indicate that the BA anomalies strongly correlate with FWI anomalies at a GFED region scale, compared to the strength of the correlation with individual climate variables. Additionally, among the individual climate variables that comprise the FWI, relative humidity and temperature are the most influential factors that affect the observed BA. Our results support the use of the composite fire danger index FWI, as well as its sub-indices, the Build-Up Index (BUI) and the Initial Spread Index (ISI), comparing to single climate variables, since they are found to correlate better with the observed forest or non-forest BA, for the most regions across the globe.

Wildfire↗

DOE OSTI2022

Pan-Arctic seasonal cycles and long-term trends of aerosol properties from 10 observatories

Even though the Arctic is remote, aerosol properties observed there are strongly influenced by anthropogenic emissions from outside the Arctic. This is particularly true for the so-called Arctic haze season (January through April). In summer (June through September), when atmospheric transport patterns change, and precipitation is more frequent, local Arctic sources, i.e., natural sources of aerosols and precursors, play an important role. Over the last few decades, significant reductions in anthropogenic emissions have taken place. At the same time a large body of literature shows evidence that the Arctic is undergoing fundamental environmental changes due to climate forcing, leading to enhanced emissions by natural processes that may impact aerosol properties. In this study, we analyze 9 aerosol chemical species and 4 particle optical properties from 10 Arctic observatories (Alert, Kevo, Pallas, Summit, Thule, Tiksi, Barrow/Utgiavik, Villum, and Gruvebadet and Zeppelin Observatory – both at Ny-Ålesund Research Station) to understand changes in anthropogenic and natural aerosol contributions. Variables include equivalent black carbon, particulate sulfate, nitrate, ammonium, methanesulfonic acid, sodium, iron, calcium and potassium, as well as scattering and absorption coefficients, single scattering albedo and scattering Ångström exponent. First, annual cycles are investigated, which despite anthropogenic emission reductions still show the Arctic haze phenomenon. Second, long-term trends are studied using the Mann–Kendall Theil–Sen slope method. We find in total 41 significant trends over full station records, i.e., spanning more than a decade, compared to 26 significant decadal trends. The majority of significantly declining trends is from anthropogenic tracers and occurred during the haze period, driven by emission changes between 1990 and 2000. For the summer period, no uniform picture of trends has emerged. Twenty-six percent of trends, i.e., 19 out of 73, are significant, and of those 5 are positive and 14 are negative. Negative trends include not only anthropogenic tracers such as equivalent black carbon at Kevo, but also natural indicators such as methanesulfonic acid and non-sea-salt calcium at Alert. Positive trends are observed for sulfate at Gruvebadet. No clear evidence of a significant change in the natural aerosol contribution can be observed yet. However, testing the sensitivity of the Mann–Kendall Theil–Sen method, we find that monotonic changes of around 5 % yr –1 in an aerosol property are needed to detect a significant trend within one decade. This highlights that long-term efforts well beyond a decade are needed to capture smaller changes. It is particularly important to understand the ongoing natural changes in the Arctic, where interannual variability can be high, such as with forest fire emissions and their influence on the aerosol population. To investigate the climate-change-induced influence on the aerosol population and the resulting climate feedback, long-term observations of tracers more specific to natural sources are needed, as well as of particle microphysical properties such as size distributions, which can be used to identify changes in particle populations which are not well captured by mass-oriented methods such as bulk chemical composition.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1994

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.↗