Jeffrey S. Reid

A review of biomass burning emissions part III: intensive optical properties of biomass burning particles

Because of its wide coverage over much of the globe, biomass burning has been widely studied in the context of direct radiative forcing. Such study is warranted as smoke particles scatter and at times absorb solar radiation efficiently. Further, as much of what is known about smoke transport and impacts is based on remote sensing measurements, the optical properties of smoke particles have far reaching effects into numerous aspects of biomass burning studies. Global estimates of direct forcing have been widely varying, ranging from near zero to −1 W m−2. A significant part of this difference can be traced to varying assumptions on the optical properties of smoke. This manuscript is the third part of four examining biomass-burning emissions. Here we review and discuss the literature concerning measurement and modeling of optical properties of biomassburning particles. These include available data from published sensitivity studies, field campaigns, and inversions from the Aerosol Robotic Network (AERONET) of Sun photometer sites. As a whole, optical properties reported in the literature are varied, reflecting both the dynamic nature of fires, variations in smoke aging processes and differences in measurement technique. We find that forward modeling or “internal closure” studies ultimately are of little help in resolving outstanding measurement issues due to the high degree of degeneracy in solutions when using “reasonable” input parameters. This is particularly notable with respect to index of refraction and the treatment of black carbon. Consequently, previous claims of column closure may in fact be more ambiguous. Differences between in situ and retrieved ωo values have implications for estimates of mass scattering and mass absorption efficiencies. In this manuscript we Correspondence to: J. S. Reid (reidj@nrlmry.navy.mil) review and discuss this community dataset. Strengths and lapses are pointed out, future research topics are prioritized, and best estimates and uncertainties of key smoke particle parameters are provided.

Physical, chemical, and optical properties of regional hazes dominated by smoke in Brazil

Gas and particle measurements are described for optically thick regional hazes, dominated by aged smoke from biomass burning, in the cerrado and rain forested regions of Brazil. The hazes tended to be evenly mixed from the surface to the trade wind inversion at 3–4 km in altitude. The properties of aged gases and particles in the regional hazes were significantly different from those of young smoke (<4 min old). As the smoke aged, the total amount of carbon in non-methane hydrocarbon species (C<11) was depleted by about one third due to transformations into CO2, CO, and reactive molecules, and removed by dry deposition and/or by conversion to particulate matter. As the smoke particles aged, their sizes increased significantly due to coagulation and mass growth by secondary species (e.g., ammonium, organic acids and sulfate). During aging, condensation and gas-to-particle conversion of inorganic and organic vapors increased the aerosol mass by ∼20–40%. One third to one half of this mass growth likely occurred in the first few hours of aging due to the condensation of large organic molecules. The remaining mass growth was probably associated with photochemical and cloud-processing mechanisms operating over several days. Changes in particle sizes and compositions during aging had a large impact on the optical properties of the aerosol. Over a 2 to 4 day period, the fine particle mass-scattering efficiency and single-scattering albedo increased by 1 m2 g−1, and ∼0.06, respectively. Conversely, the Angstrom coefficient, backscatter ratio, and mass absorption efficiency decreased significantly with age.

Emission factors of hydrocarbons, halocarbons, trace gases and particles from biomass burning in Brazil

Airborne measurements of the emissions of gases and particles from 19 individual forest, cerrado, and pasture fires in Brazil were obtained during the Smoke, Clouds, and Radiation-Brazil (SCAR-B) study in August-September 1995. Emission factors were determined for a number of major and minor gaseous and particulate species, including carbon dioxide, carbon monoxide, sulfur dioxide, nitrogen oxides, methane, nonmethane hydrocarbons, halocarbons, particulate (black and organic) carbon, and particulate ionic species. The magnitude of the emission factors for gaseous species were determined primarily by the relative amounts of flaming and smoldering combustion, rather than differences in vegetation type. Hydrocarbons and halocarbons were well correlated with CO, which is indicative of emissions primarily associated with smoldering combustion. Although there was large variability between fires, higher emission factors for SO2 and NOχ were associated with an increased ratio of flaming to smoldering combustion; this could be due to variations in the amounts of sulfur and nitrogen in the fuels. Emission factors for particles were not so clearly associated with smoldering combustion as those for hydrocarbons. The emission factors measured in this study are similar to those measured previously in Brazil and Africa. However, particle emission factors from fires in Brazil appear to be roughly 20 to 40% lower than those from North American boreal forest fires.

Effects of black carbon content, particle size, and mixing on light absorption by aerosols from biomass burning in Brazil

Black carbon mass absorption efficiencies of smoke particles were measured for various types of biomass fires during the Smoke, Clouds, and Radiation-Brazil (SCAR-B) experiment using thermal evolution measurements for black carbon and optical absorption methods. The obtained results range between 5.2 and 19.3 m2 g−1 with an average value of 12.1±4.0 m2 g−1. Particle size distributions and optical properties were also measured to provide a full set of physical parameters for modeling calculations. Mie theory was used to model the optical properties of the particles assuming both internal and external mixtures coupling the modeling calculations with the experimental results obtained during the campaign. For internal mixing, a particle model with a layered structure consisting of an absorbing black carbon core, surrounded by a nonabsorbing shell, was assumed. Also, for internal mixing, a discrete dipole approximation code was used to simulate packed soot clusters commonly found in electron microscopy photographs of filters collected during the experiment. The modeled results for layered spheres and packed clusters explain black carbon mass absorption coefficients up to values of about 25 m2 g−1, but measurements show even higher values which were correlated with the chemical composition and characteristics of the structure of the particles. Unrealistic high values of black carbon absorption efficiencies were linked to high concentrations of K, which influence the volatilization of black carbon (BC) at lower temperatures than usual, possibly causing artifacts in the determination of BC by thermal technique. The modeling results are compared with nephelometer and light absorption measurements.

Climatological aspects of the optical properties of fine/coarse mode aerosol mixtures

[1] Aerosol mixtures composed of coarse mode desert dust combined with fine mode combustion generated aerosols (from fossil fuel and biomass burning sources) were investigated at three locations that are in and/or downwind of major global aerosol emission source regions. Multiyear monitoring data at Aerosol Robotic Network sites in Beijing (central eastern China), Kanpur (Indo-Gangetic Plain, northern India), and Ilorin (Nigeria, Sudanian zone of West Africa) were utilized to study the climatological characteristics of aerosol optical properties. Multiyear climatological averages of spectral single scattering albedo (SSA) versus fine mode fraction (FMF) of aerosol optical depth at 675 nm at all three sites exhibited relatively linear trends up to ~50% FMF. This suggests the possibility that external linear mixing of both fine and coarse mode components (weighted by FMF) dominates the SSA variation, where the SSA of each component remains relatively constant for this range of FMF only. However, it is likely that a combination of other factors is also involved in determining the dynamics of SSA as a function of FMF, such as fine mode particles adhering to coarse mode dust. The spectral variation of the climatological averaged aerosol absorption optical depth (AAOD) was nearly linear in logarithmic coordinates over the wavelength range of 440-870 nm for both the Kanpur and Ilorin sites. However, at two sites in China (Beijing and Xianghe), a distinct nonlinearity in spectral AAOD in logarithmic space was observed, suggesting the possibility of anomalously strong absorption in coarse mode aerosols increasing the 870 nm AAOD.

Physical and optical properties of young smoke from individual biomass fires in Brazil

Physical and optical characteristics of particles in smoke from 19 fires were measured in Brazil during the 1995 burning season as part of the Smoke, Clouds, and Radiation-Brazil (SCAR-B) project. The University of Washington C-131A measured particle sizes and absorption and scattering properties in very young smoke (<4 min old). These properties are related to fuel type, fire intensity, combustion efficiency, and particle composition. The count median diameter (CMD) of particles from tropical forest fires were strongly and positively correlated with the combustion efficiency. The particle volume median diameter (VMD) of the particles from forest fires did not correlate well with combustion efficiency, but it was highly correlated with the emission factors of particles and unsaturated hydrocarbons. The median diameter and standard deviation of the particle size spectra for smoke from grass and cerrado fires did not correlate with either the combustion efficiency or any emission factor. The measured particle radiative properties correlated well with the measured particle sizes and compositions, and the relationships between these parameters are described fairly well by Mie theory. The optical properties of smoke from individual biomass fires in Brazil differ significantly from those of smoke from biomass burning in North America. In particular, the total light-scattering coefficient for smoke particles in Brazil is, on average, 15% less than for smoke particles in North America. Also, the average values of the single-scattering albedos of smoke particles in Brazil are 0.05 to 0.1 less than those in North America.

Use of the Ångstrom exponent to estimate the variability of optical and physical properties of aging smoke particles in Brazil

In situ airborne measurements from the Smoke, Clouds and Radiation-Brazil (SCAR-B) study show that during aging over 1–4 days the physical and optical properties of smoke particles are correlated. Consequently, if one optical or physical property of the smoke particles is determined, other properties can be derived. This methodology is validated using multiwavelength Angstrom exponents determined from the ground-based Sun photometer measurements in SCAR-B. It is shown that the Angstrom exponent determined from Sun photometers for the wavelength intervals 339–437 nm and 437–669 nm are well correlated with particle size, single-scattering albedo, and the backscatter ratio (r2>0.8). Therefore, when almucantar sky radiance data are not available and for remote sensing applications (such as MODIS), some of the uncertainties in the properties of smoke particles can be reduced by applying these relationships. Using this methodology, major oscillations were observed in smoke particle properties in Brazil on timescales of ∼5–15 days, resulting in variations of the volume median diameter and single-scattering albedo of ±0.04 μm and ±0.05, respectively. In comparison, the mean value of the dry smoke particle volume median diameter and single-scattering albedo over all of Brazil was 0.27 μm and 0.86, respectively. A daily cycle in smoke particle properties was also observed. The weekly and seasonal variability in the single-scattering albedo is shown to have significant consequences for retrieving aerosol optical depths from satellite measurements.

Global Monitoring and Forecasting of Biomass-Burning Smoke: Description of and Lessons From the Fire Locating and Modeling of Burning Emissions (FLAMBE) Program

Recently, global biomass-burning research has grown from what was primarily a climate field to include a vibrant air quality observation and forecasting community. While new fire monitoring systems are based on fundamental Earth Systems Science (ESS) research, adaptation to the forecasting problem requires special procedures and simplifications. In a reciprocal manner, results from the air quality research community have contributed scientifically to basic ESS. To help exploit research and data products in climate, ESS, meteorology and air quality biomass burning communities, the joint Navy, NASA, NOAA, and University Fire Locating and Modeling of Burning Emissions (FLAMBE) program was formed in 1999. Based upon the operational NOAA/NESDIS Wild-Fire Automated Biomass Burning Algorithm (WF_ABBA) and the near real time University of Maryland/NASA MODIS fire products coupled to the operational Navy Aerosol Analysis and Prediction System (NAAPS) transport model, FLAMBE is a combined ESS and operational system to study the nature of smoke particle emissions and transport at the synoptic to continental scales. In this paper, we give an overview of the FLAMBE system and present fundamental metrics on emission and transport patterns of smoke. We also provide examples on regional smoke transport mechanisms and demonstrate that MODIS optical depth data assimilation provides significant variance reduction against observations. Using FLAMBE as a context, throughout the paper we discuss observability issues surrounding the biomass burning system and the subsequent propagation of error. Current indications are that regional particle emissions estimates still have integer factors of uncertainty.

Characterization of the optical properties of biomass burning aerosols in Zambia during the 1997 ZIBBEE field campaign

The physical and optical properties of biomass burning aerosols in a savanna region in south central Africa (Zambia) were analyzed from measurements made during the Zambian International Biomass Burning Emissions Experiment (ZIBBEE) during August-September 1997. Due to the large spatial extent of African savannas and the high frequency of occurrence of burning in the annual dry seasons, characterization of the optical properties of the resultant biomass burning aerosols is important for the study of atmospheric radiative processes and for remote sensing of both surface and atmospheric properties in these regions. Aerosol Robotic Network Sun-sky radiometer spectral measurements of direct Sun observations and directional sky radiances were utilized to infer spectral aerosol optical depths (τa), aerosol size distributions, and single-scattering albedos. During the primary ZIBBEE study period, which coincided with the peak period of biomass burning in the region, there was a high correlation between the measured τa and the total column water vapor or precipitable water vapor (PWV), suggesting transport of smoke aerosol from regions with higher PWV. Size distribution retrievals of the biomass burning smoke show that the accumulation mode dominated and a comparison with smoke from Amazonia (Bolivia) shows a shift toward smaller particles for African savanna smoke. This may be the result of differences in mode of combustion (flaming versus smoldering), fuel type and moisture content, and the aging processes of the aerosol. The single-scattering albedo (ω0) of the aerosols were retrieved using several approaches, yielding average values of ω0 at ∼550 nm during ZIBBEE varying from ∼0.82 to ∼0.85, thus showing good agreement within the retrieval uncertainty of ∼0.03 of these methods. In general, ω0 was relatively constant as a function of aerosol loading, with very little change occurring for τa at 440 nm ranging from 0.7 to 1.7. African savanna smoke exhibits significantly higher absorption than smoke from Amazonian forested regions and also a greater rate of decrease of ω0 with increasing wavelength. Variations in the spectral change of the Angstrom wavelength exponent were also investigated with respect to the degree of aerosol absorption and changes in the accumulation mode size distributions.

High aerosol optical depth biomass burning events: A comparison of optical properties for different source regions

Received 29 May 2003; revised 8 September 2003; accepted 17 September 2003; published 21 October 2003. [1] The optical properties of aerosols such as smoke from biomass burning vary due to aging processes and these particles reach larger sizes at high concentrations. We compare the spectra of aerosol optical depth (ta), columnintegrated volume size distributions, refractive indices, and single scattering albedo retrieved from AERONET observations for four selected events of very high smoke optical depth (ta � 2 at 500 nm). Two case studies are from tropical biomass burning regions (Brazil and Zambia) and two are cases of boreal forest and peat fire smoke transported long distances to sites in the US and Moldova. Smoke properties for these extreme events can be significantly different from those reported in more typical plumes. In particular, large differences in smoke fine mode particle radius (� 0.17 to 0.25 mm) and single scattering albedo (� 0.88 to 0.99 at 440 nm) were observed as a result of differences in fuels burned, combustion phase, and aging. INDEX TERMS: 0305 Atmospheric Composition and Structure: Aerosols and particles (0345, 4801); 0345 Atmospheric Composition and Structure: Pollution—urban and regional (0305); 0360 Atmospheric Composition and Structure: Transmission and scattering of radiation. Citation: Eck, T. F., B. N. Holben, J. S. Reid, N. T. O’Neill, J. S. Schafer, O. Dubovik, A. Smirnov, M. A. Yamasoe, and P. Artaxo, High aerosol optical depth biomass burning events: A comparison of optical properties for different source regions, Geophys. Res. Lett., 30(20), 2035, doi:10.1029/ 2003GL017861, 2003.