Estimates of global terrestrial isoprene emissions using MEGAN (Model of Emissions of Gases and Aerosols from Nature)

Reactive gases and aerosols are produced by terrestrial ecosystems, processed within plant canopies, and can then be emitted into the above-canopy atmosphere. Estimates of the above-canopy fluxes are needed for quantitative earth system studies and assessments of past, present and future air quality and climate. The Model of Emissions of Gases and Aerosols from Nature (MEGAN) is described and used to quantify net terrestrial biosphere emission of isoprene into the atmosphere. MEGAN is designed for both global and regional emission modeling and has global coverage with ~1 km² spatial resolution. Field and laboratory investigations of the processes controlling isoprene emission are described and data available for model development and evaluation are summarized. The factors controlling isoprene emissions include biological, physical and chemical driving variables. MEGAN driving variables are derived from models and satellite and ground observations. Tropical broadleaf trees contribute almost half of the estimated global annual isoprene emission due to their relatively high emission factors and because they are often exposed to conditions that are conducive for isoprene emission. The remaining flux is primarily from shrubs which have a widespread distribution. The annual global isoprene emission estimated with MEGAN ranges from about 500 to 750 Tg isoprene (440 to 660 Tg carbon) depending on the driving variables which include temperature, solar radiation, Leaf Area Index, and plant functional type. The global annual isoprene emission estimated using the standard driving variables is ~600 Tg isoprene. Differences in driving variables result in emission estimates that differ by more than a factor of three for specific times and locations. It is difficult to evaluate isoprene emission estimates using the concentration distributions simulated using chemistry and transport models, due to the substantial uncertainties in other model components, but at least some global models produce reasonable results when using isoprene emission distributions similar to MEGAN estimates. In addition, comparison with isoprene emissions estimated from satellite formaldehyde observations indicates reasonable agreement. The sensitivity of isoprene emissions to earth system changes (e.g., climate and land-use) demonstrates the potential for large future changes in emissions. Using temperature distributions simulated by global climate models for year 2100, MEGAN estimates that isoprene emissions increase by more than a factor of two. This is considerably greater than previous estimates and additional observations are needed to evaluate and improve the methods used to predict future isoprene emissions

Emissions of Volatile Organic Compounds Inferred From Airborne Flux Measurements over a Megacity

Toluene and benzene are used for assessing the ability to measure disjunct eddy covariance (DEC) fluxes of Volatile Organic Compounds (VOC) using Proton Transfer Reaction Mass Spectrometry (PTR-MS) on aircraft. Statistically significant correlation between vertical wind speed and mixing ratios suggests that airborne VOC eddy covariance (EC) flux measurements using PTR-MS are feasible. City-median midday toluene and benzene fluxes are calculated to be on the order of 14.1±4.0 mg/m<sup>2</sup>/h and 4.7±2.3 mg/m<sup>2</sup>/h, respectively. For comparison the adjusted CAM2004 emission inventory estimates toluene fluxes of 10 mg/m<sup>2</sup>/h along the footprint of the flight-track. Wavelet analysis of instantaneous toluene and benzene measurements during city overpasses is tested as a tool to assess surface emission heterogeneity. High toluene to benzene flux ratios above an industrial district (e.g. 10–15 g/g) including the International airport (e.g. 3–5 g/g) and a mean flux (concentration) ratio of 3.2±0.5 g/g (3.9±0.3 g/g) across Mexico City indicate that evaporative fuel and industrial emissions play an important role for the prevalence of aromatic compounds. Based on a tracer model, which was constrained by BTEX (BTEX– Benzene/Toluene/Ethylbenzene/m, p, o-Xylenes) compound concentration ratios, the fuel marker methyl-tertiary-butyl-ether (MTBE) and the biomass burning marker acetonitrile (CH<sub>3</sub>CN), we show that a combination of industrial, evaporative fuel, and exhaust emissions account for >87% of all BTEX sources. Our observations suggest that biomass burning emissions play a minor role for the abundance of BTEX compounds in the MCMA (2–13%)

Estimation of mercury emissions from forest fires, lakes, regional and local sources using measurements in Milwaukee and an inverse method

Gaseous elemental mercury is a global pollutant that can lead to serious health concerns via deposition to the biosphere and bio-accumulation in the food chain. Hourly measurements between June 2004 and May 2005 in an urban site (Milwaukee, WI) show elevated levels of mercury in the atmosphere with numerous short-lived peaks as well as longer-lived episodes. The measurements are analyzed with an inverse model to obtain information about mercury emissions. The model is based on high resolution meteorological simulations (WRF), hourly back-trajectories (WRF-FLEXPART) and a chemical transport model (CAMx). The hybrid formulation combining back-trajectories and Eulerian simulations is used to identify potential source regions as well as the impacts of forest fires and lake surface emissions. Uncertainty bounds are estimated using a bootstrap method on the inversions. Comparison with the US Environmental Protection Agency's National Emission Inventory (NEI) and Toxic Release Inventory (TRI) shows that emissions from coal-fired power plants are properly characterized, but emissions from local urban sources, waste incineration and metal processing could be significantly under-estimated. Emissions from the lake surface and from forest fires were found to have significant impacts on mercury levels in Milwaukee, and to be underestimated by a factor of two or more

Emission factors for open and domestic biomass burning for use in atmospheric models

Biomass burning (BB) is the second largest source of trace gases and the largest source of primary fine carbonaceous particles in the global troposphere. Many recent BB studies have provided new emission factor (EF) measurements. This is especially true for non-methane organic compounds (NMOC), which influence secondary organic aerosol (SOA) and ozone formation. New EF should improve regional to global BB emissions estimates and therefore, the input for atmospheric models. In this work we present an up-to-date, comprehensive tabulation of EF for known pyrogenic species based on measurements made in smoke that has cooled to ambient temperature, but not yet undergone significant photochemical processing. All EFs are converted to one standard form (g compound emitted per kg dry biomass burned) using the carbon mass balance method and they are categorized into 14 fuel or vegetation types. Biomass burning terminology is defined to promote consistency. We compile a large number of measurements of biomass consumption per unit area for important fire types and summarize several recent estimates of global biomass consumption by the major types of biomass burning. Post emission processes are discussed to provide a context for the emission factor concept within overall atmospheric chemistry and also highlight the potential for rapid changes relative to the scale of some models or remote sensing products. Recent work shows that individual biomass fires emit significantly more gas-phase NMOC than previously thought and that including additional NMOC can improve photochemical model performance. A detailed global estimate suggests that BB emits at least 400 Tg yr^(−1) of gas-phase NMOC, which is almost 3 times larger than most previous estimates. Selected recent results (e.g. measurements of HONO and the BB tracers HCN and CH_3CN) are highlighted and key areas requiring future research are briefly discussed

A decadal satellite analysis of the origins and impacts of smoke in Colorado

We analyze the record of aerosol optical depth (AOD) measured by the MODerate resolution Imaging Spectroradiometer (MODIS) aboard the Terra satellite in combination with surface PM[subscript 2.5] to investigate the impact of fires on aerosol loading and air quality over Colorado from 2000 to 2012, and to evaluate the contribution of local versus transported smoke. Fire smoke contributed significantly to the AOD levels observed over Colorado. During the worst fire seasons of 2002 and 2012, average MODIS AOD over the Colorado Front Range corridor were 20–50% larger than the other 11 yr studied. Surface PM[subscript 2.5] was also unusually elevated during fire events and concentrations were in many occasions above the daily National Ambient Air Quality Standard (35 μg m[superscript −3]) and even reached locally unhealthy levels (> 100 μg m[superscript −3]) over populated areas during the 2012 High Park fire and the 2002 Hayman fire. Over the 13 yr examined, long-range transport of smoke from northwestern US and even California (> 1500 km distance) occurred often and affected AOD and surface PM[subscript 2.5]. During most of the transport events, MODIS AOD and surface PM[subscript 2.5] were reasonable correlated (r[superscript 2] = 0.2–0.9), indicating that smoke subsided into the Colorado boundary layer and reached surface levels. However, that is not always the case since at least one event of AOD enhancement was disconnected from the surface (r[superscript 2]<0.01 and low PM[subscript 2.5] levels). Observed plume heights from the Multi-angle Imaging SpectroRadiometer (MISR) satellite instrument and vertical aerosol profiles measured by the space-based Cloud-Aerosol LIdar with Orthogonal Polarization (CALIOP) showed a complex vertical distribution of smoke emitted by the High Park fire in 2012. Smoke was detected from a range of 1.5 to 7.5 km altitude at the fire origin and from ground levels to 12.3 km altitude far away from the source. The variability of smoke altitude as well as the local meteorology were key in determining the aerosol loading and air quality over the Colorado Front Range region. Our results underline the importance of accurate characterization of the vertical distribution of smoke for estimating the air quality degradation associated with fire activity and its link to human health.United States. National Park Service (Grant H2370 094000/J2350103006

Aerosol microphysical impact on summertime convective precipitation in the Rocky Mountain region

We present an aerosol-cloud-precipitation modeling study of convective clouds using the Weather Research and Forecasting model fully coupled with Chemistry (WRF-Chem) version 3.1.1. Comparison of the model output with measurements from a research site in the Rocky Mountains in Colorado revealed that the fraction of organics in the model is underpredicted. This is most likely due to missing processes in the aerosol module in the model version used, such as new particle formation and growth of secondary organic aerosols. When boundary conditions and domain-wide initial conditions of aerosol loading are changed in the model (factors of 0.1, 0.2, and 10 of initial aerosol mass of SO4-2, NH4+, and NO3-), the domain-wide precipitation changes by about 5%. Analysis of the model results reveals that the Rocky Mountain region and Front Range environment is not conducive for convective invigoration to play a major role, in increasing precipitation, as seen in some other studies. When localized organic aerosol emission are increased to mimic new particle formation, the resulting increased aerosol loading leads to increases in domain-wide precipitation, opposite to what is seen in the model simulations with changed boundary and initial conditions

Quantifying black carbon deposition over the Greenland ice sheet from forest fires in Canada

Black carbon (BC) concentrations observed in 22 snowpits sampled in the northwest sector of the Greenland ice sheet in April 2014 have allowed us to identify a strong and widespread BC aerosol deposition event, which was dated to have accumulated in the pits from two snow storms between 27 July and 2 August 2013. This event comprises a significant portion (57% on average across all pits) of total BC deposition over 10 months (July 2013 to April 2014). Here we link this deposition event to forest fires burning in Canada during summer 2013 using modeling and remote sensing tools. Aerosols were detected by both the Cloud‐Aerosol Lidar with Orthogonal Polarization (on board CALIPSO) and Moderate Resolution Imaging Spectroradiometer (Aqua) instruments during transport between Canada and Greenland. We use high‐resolution regional chemical transport modeling (WRF‐Chem) combined with high‐resolution fire emissions (FINNv1.5) to study aerosol emissions, transport, and deposition during this event. The model captures the timing of the BC deposition event and shows that fires in Canada were the main source of deposited BC. However, the model underpredicts BC deposition compared to measurements at all sites by a factor of 2–100. Underprediction of modeled BC deposition originates from uncertainties in fire emissions and model treatment of wet removal of aerosols. Improvements in model descriptions of precipitation scavenging and emissions from wildfires are needed to correctly predict deposition, which is critical for determining the climate impacts of aerosols that originate from fires

Aerosol plume transport and transformation in high spectral resolution lidar measurements and WRF-Flexpart simulations during the MILAGRO Field Campaign

The Mexico City Metropolitan Area (MCMA) experiences high loadings of atmospheric aerosols from anthropogenic sources, biomass burning and wind-blown dust. This paper uses a combination of measurements and numerical simulations to identify different plumes affecting the basin and to characterize transformation inside the plumes. The High Spectral Resolution Lidar on board the NASA LaRC B-200 King Air aircraft measured extinction coefficients and extinction to backscatter ratio at 532 nm, and backscatter coefficients and depolarization ratios at 532 and 1064 nm. These can be used to identify aerosol types. The measurement curtains are compared with particle trajectory simulations using WRF-Flexpart for different source groups. The good correspondence between measurements and simulations suggests that the aerosol transport is sufficiently well characterized by the models to estimate aerosol types and ages. Plumes in the basin undergo complex transport, and are frequently mixed together. Urban aerosols are readily identifiable by their low depolarization ratios and high lidar ratios, and dust by the opposite properties. Fresh biomass burning plumes have very low depolarization ratios which increase rapidly with age. This rapid transformation is consistent with the presence of atmospheric tar balls in the fresh plumes

Population exposure to hazardous air quality due to the 2015 fires in Equatorial Asia.

Vegetation and peatland fires cause poor air quality and thousands of premature deaths across densely populated regions in Equatorial Asia. Strong El-Niño and positive Indian Ocean Dipole conditions are associated with an increase in the frequency and intensity of wildfires in Indonesia and Borneo, enhancing population exposure to hazardous concentrations of smoke and air pollutants. Here we investigate the impact on air quality and population exposure of wildfires in Equatorial Asia during Fall 2015, which were the largest over the past two decades. We performed high-resolution simulations using the Weather Research and Forecasting model with Chemistry based on a new fire emission product. The model captures the spatio-temporal variability of extreme pollution episodes relative to space- and ground-based observations and allows for identification of pollution sources and transport over Equatorial Asia. We calculate that high particulate matter concentrations from fires during Fall 2015 were responsible for persistent exposure of 69 million people to unhealthy air quality conditions. Short-term exposure to this pollution may have caused 11,880 (6,153-17,270) excess mortalities. Results from this research provide decision-relevant information to policy makers regarding the impact of land use changes and human driven deforestation on fire frequency and population exposure to degraded air quality.This research was supported in part by a L’Oréal-UNESCO UK and Ireland Fellowship For Women In Science (to PC), the Natural Environmental Research Council (NERC) through the LICS the SAMBBA project (ref. NE/J009822/1), the EPA STAR program (R835422), and the National Research Fellow Award (NRF2012NRFNRFF001-031). EB is partly supported by funding from UBoC. Further support was provided by the Lilly Endowment, Inc., through its support for the Indiana University Pervasive Technology Institute and the Indiana METACyt Initiative. This work makes use of the LandScan (2013)™ High Resolution global Population Data Set copyrighted by UT-Battelle, LLC, operator of Oak Ridge National Laboratory under Contract No. DE-AC05- 00OR22725 with the United States Department of Energy. Global Burden of Disease used in this study have been accessed from the Institute for Health Metric and Evaluation website: http://ghdx.healthdata.org/ihme_data. We gratefully acknowledge the National Environment Agency (NEA) of Singapore for collecting and providing PM2.5 and PSI data (available at http://www.nea.gov.sg/anti-pollution-radiation-protection/air-pollution-control/psi/historical-psi-readings). The National Center for Atmospheric Research is operated by the University Corporation for Atmospheric Research under the sponsorship of the National Science Foundation. We thank Louisa Emmons for providing the boundary conditions for dust from CAM-Chem. We also acknowledge the NASA scientists responsible for MODIS products, WRF-Chem developers and ACOM scientists at NCAR for useful discussion on model set-up