Biomass Burning Smoke Plumes Research Articles

Optical Properties of Individual Tar Balls in the Free Troposphere.

Tar balls are brown carbonaceous particles that are highly viscous, spherical, amorphous, and light absorbing. They are believed to form in biomass burning smoke plumes during transport in the troposphere. Tar balls are also believed to have a significant impact on the Earth's radiative balance, but due to poorly characterized optical properties, this impact is highly uncertain. Here, we used two nighttime samples to investigate the chemical composition and optical properties of individual tar balls transported in the free troposphere to the Climate Observatory "Ottavio Vittori" on Mt. Cimone, Italy, using multimodal microspectroscopy. In our two samples, tar balls contributed 50% of carbonaceous particles by number. Of those tar balls, 16% were inhomogeneously mixed with other constituents. Using electron energy loss spectroscopy, we retrieved the complex refractive index (RI) for a wavelength range from 200 to 1200 nm for both inhomogeneously and homogeneously mixed tar balls. We found no significant difference in the average RI of inhomogeneously and homogeneously mixed tar balls (1.40-0.03i and 1.36-0.03i at 550 nm, respectively). Furthermore, we estimated the top of the atmosphere radiative forcing using the Santa Barbara DISORT Atmospheric Radiative Transfer model and found that a layer of only tar balls with an optical depth of 0.1 above vegetation would exert a positive radiative forcing ranging from 2.8 W m-2 (on a clear sky day) to 9.5 W m-2 (when clouds are below the aerosol layer). Understanding the optical properties of tar balls can help reduce uncertainties associated with the contribution of biomass-burning aerosol in current climate models.

Near-source grid-based measurement of CO and PM2.5 concentration during a full-scale fire experiment in southern European shrubland

There is limited research on the exposure of wildland firefighters to smoke because of the operational obstacles when monitoring air pollutants in the field. In this work, a grid of portable sensors was used to measure PM2.5 and CO concentrations in the near-source region during the burn of two shrubland research blocks in Central Portugal. Strong spatial variability of smoke levels was observed in the analysis of the ratios between mean concentrations of neighbouring sensors, with values as high as 4.4 for PM2.5 and 7.4 for CO. These large gradients were registered at a distance of only 5 m suggesting that considerable differences on individual exposure can occur depending on the location of that individual in relation to the smoke plume trajectory. Also, peak events of 2–3 times the mean were observed in periods exceeding 6 min. In the two experiments, the average concentrations of both PM2.5 and CO were higher during smouldering, which represents a risk of acute exposure due to the closer proximity of firefighters to the emission source during mop-up, stressing the importance of wearing portable gas detectors for managing critical exposure. The collected data constitutes a step forward in the effort to understand the mechanisms controlling the exposure during firefighting operations, by providing a source of information on near-ground concentration fluctuations within a biomass-burning smoke plume at a fine spatial-temporal resolution.

Investigating the links between ozone and organic aerosol chemistry in a biomass burning plume from a prescribed fire in California chaparral

Abstract. Within minutes after emission, complex photochemistry in biomass burning smoke plumes can cause large changes in the concentrations of ozone (O3) and organic aerosol (OA). Being able to understand and simulate this rapid chemical evolution under a wide variety of conditions is a critical part of forecasting the impact of these fires on air quality, atmospheric composition, and climate. Here we use version 2.1 of the Aerosol Simulation Program (ASP) to simulate the evolution of O3 and secondary organic aerosol (SOA) within a young biomass burning smoke plume from the Williams prescribed fire in chaparral, which was sampled over California in November 2009. We demonstrate the use of a method for simultaneously accounting for the impact of the unidentified intermediate volatility, semi-volatile, and extremely low volatility organic compounds (here collectively called "SVOCs") on the formation of OA (using the Volatility Basis Set – VBS) and O3 (using the concept of mechanistic reactivity). We show that this method can successfully simulate the observations of O3, OA, NOx, ethylene (C2H4), and OH to within measurement uncertainty using reasonable assumptions about the average chemistry of the unidentified SVOCs. These assumptions were (1) a reaction rate constant with OH of ~ 10-11 cm3 s−1; (2) a significant fraction (up to ~ 50 %) of the RO2 + NO reaction resulted in fragmentation, rather than functionalization, of the parent SVOC; (3) ~ 1.1 molecules of O3 were formed for every molecule of SVOC that reacted; (4) ~ 60 % of the OH that reacted with the unidentified non-methane organic compounds (NMOC) was regenerated as HO2; and (5) that ~ 50 % of the NO that reacted with the SVOC peroxy radicals was lost, presumably to organic nitrate formation. Additional evidence for the fragmentation pathway is provided by the observed rate of formation of acetic acid (CH3COOH), which is consistent with our assumed fragmentation rate. However, the model overestimates peroxyacetyl nitrate (PAN) formation downwind by about 50 %, suggesting the need for further refinements to the chemistry. This method could provide a way for classifying different smoke plume observations in terms of the average chemistry of their SVOCs, and could be used to study how the chemistry of these compounds (and the O3 and OA they form) varies between plumes.

Tropical biomass burning smoke plume size, shape, reflectance, and age based on 2001–2009 MISR imagery of Borneo

Abstract. Land clearing for crops, plantations and grazing results in anthropogenic burning of tropical forests and peatlands in Indonesia, where images of fire-generated aerosol plumes have been captured by the Multi-angle Imaging SpectroRadiometer (MISR) since 2001. Here we analyze the size, shape, optical properties, and age of distinct fire-generated plumes in Borneo from 2001–2009. The local MISR overpass at 10:30 a.m. misses the afternoon peak of Borneo fire emissions, and may preferentially sample longer plumes from persistent fires burning overnight. Typically the smoke flows with the prevailing southeasterly surface winds at 3–4 m s−1, and forms ovoid plumes whose mean length, height, and cross-plume width are 41 km, 708 m, and 27% of the plume length, respectively. 50% of these plumes have length between 24 and 50 km, height between 523 and 993 m and width between 18% and 30% of plume length. Length and cross-plume width are lognormally distributed, while height follows a normal distribution. Borneo smoke plume heights are similar to previously reported plume heights, yet Borneo plumes are on average nearly three times longer than previously studied plumes. This could be due to sampling or to more persistent fires and greater fuel loads in peatlands than in other tropical forests. Plume area (median 169 km2, with 25th and 75th percentiles at 99 km2 and 304 km2, respectively) varies exponentially with length, though for most plumes a linear relation provides a good approximation. The MISR-estimated plume optical properties involve greater uncertainties than the geometric properties, and show patterns consistent with smoke aging. Optical depth increases by 15–25% in the down-plume direction, consistent with hygroscopic growth and nucleation overwhelming the effects of particle dispersion. Both particle single-scattering albedo and top-of-atmosphere reflectance peak about halfway down-plume, at values about 3% and 10% greater than at the origin, respectively. The initially oblong plumes become brighter and more circular with time, increasingly resembling smoke clouds. Wind speed does not explain a significant fraction of the variation in plume geometry. We provide a parameterization of plume shape that can help atmospheric models estimate the effects of plumes on weather, climate, and air quality. Plume age, the age of smoke furthest down-plume, is lognormally distributed with a median of 2.8 h (25th and 75th percentiles at 1.3 h and 4.0 h), different from the median ages reported in other studies. Intercomparison of our results with previous studies shows that the shape, height, optical depth, and lifetime characteristics reported for tropical biomass burning plumes on three continents are dissimilar and distinct from the same characteristics of non-tropical wildfire plumes.

Emission Ratios for Ammonia and Formic Acid and Observations of Peroxy Acetyl Nitrate (PAN) and Ethylene in Biomass Burning Smoke as Seen by the Tropospheric Emission Spectrometer (TES).

We use the Tropospheric Emission Spectrometer (TES) aboard the NASA Aura satellite to determine the concentrations of the trace gases ammonia (NH3) and formic acid (HCOOH) within boreal biomass burning plumes, and present the first detection of peroxy acetyl nitrate (PAN) and ethylene (C2H4) by TES. We focus on two fresh Canadian plumes observed by TES in the summer of 2008 as part of the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS-B) campaign. We use TES retrievals of NH3 and HCOOH within the smoke plumes to calculate their emission ratios (1.0% ± 0.5% and 0.31% ± 0.21%, respectively) relative to CO for these Canadian fires. The TES derived emission ratios for these gases agree well with previous aircraft and satellite estimates, and can complement ground-based studies that have greater surface sensitivity. We find that TES observes PAN mixing ratios of ~2 ppb within these mid-tropospheric boreal biomass burning plumes when the average cloud optical depth is low (<0.1) and that TES can detect C2H4 mixing ratios of ~2 ppb in fresh biomass burning smoke plumes.

Formation of ozone and growth of aerosols in young smoke plumes from biomass burning: 1. Lagrangian parcel studies

We have developed a new model of the gas‐ and aerosol‐phase chemistry of biomass burning smoke plumes called Aerosol Simulation Program (ASP). Here we use ASP combined with a Lagrangian parcel model to simulate the chemistry in smoke plumes from three fires: the Otavi savannah fire in Namibia, an Alaska boreal forest fire, and the Timbavati savannah fire. Our model explained the observations of ozone in the Otavi and Alaska plumes fairly well, but our initial model simulation of the Timbavati plume underestimated the concentrations of ozone, OH, and secondary aerosol matter. The Timbavati simulation agrees with observations if we increase OH to equal its observed levels. Heterogeneous reactions of NO2 and SO2 could explain the needed higher concentrations of OH and the rapid formation of ozone, nitrate, and sulfate in the smoke plume if the uptake coefficients on smoke aerosols are large (O(10−3) and O(10−4), respectively). Uncharacterized organic species in the smoke plume were likely responsible for the rapid formation of aerosol organic carbon. The changes in the aerosol size distribution were dominated by plume dilution and condensational growth. The single scattering albedo of the modeled smoke increases from 0.866 to 0.902 over 1 h of aging. The change in aerosol scattering with relative humidity for the modeled fresh smoke matches observations up to 66% RH, but the model greatly overestimates the humidification factor at 80% RH (2.88 versus an observed value of 1.70–1.79). For the aged smoke, the modeled humidification factor is 1.22, slightly below the observed value of 1.40.

Intercomparison of Two Box Models of the Chemical Evolution in Biomass-Burning Smoke Plumes

Results from two independently developed biomass-burning smoke plume models are compared. Model results were obtained for the temporal evolution of two nascent smoke plumes originating from significantly different fire environments (an Alaskan boreal forest and an African savanna). The two smoke plume models differed by 1%–10% for [O3], with similar differences for NO x and formaldehyde (relative percent differences). Smaller intermodel differences were observed for the African savanna smoke plume as compared to the plume from the Alaskan boreal fire. Mechanistic differences between the models are heightened for the Alaskan smoke plume due to the higher VOC emission ratios as compared to the African savanna fire. The largest deviations result from the differences in oxidative photochemical mechanisms, with a smaller contribution attributable to the calculation of photolysis frequencies. The differences between the two smoke plume models are significantly smaller than the uncertainties of available photokinetic data or field measurements. Model accuracy depends most significantly on having the fullest possible VOC data, a requirement that is constrained by currently available instrumentation.