Abstract. 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 ω o 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.
[1] A multitude of sensitivity studies in the literature point to the importance of proper chemical and morphological characterization of particles when the radiative impacts of airborne dusts are modeled. However, the community data set is based on heterogeneous measurement methods relying on varying aerodynamic, chemical, morphological, and optical means. During the Puerto Rico Dust Experiment, size distributions of dust particles from Africa were measured using a variety of aerodynamic, optical, and geometric means. Consistent with the literature, comparisons of these size distributions showed quite dissimilar results. ''Measured'' volume median diameters varied from 2.5 to 9 mm for various geometric, aerodynamic, optical, and optical inversion methods. Aerodynamic systems showed mixed performance. Column integrated size distributions inverted from AERONET Sun/sky radiance data produced somewhat reasonable results in the coarse mode when given proper constraints and taken in the proper context. The largest systematic errors were found in optical particle counters due to insensitivities to particle size in the 4-10 mm region with further complications due to dust particle morphology and index of refraction issues. As these methods can produce quite dissimilar size distributions, considerable errors in calculated radiative properties can occur if incorrectly modeled into dust parameters. None of the methods compared in this study can adequately reproduce the measured mass extinction or mass scattering efficiency of the dust using spherical geometry methods. Given all of the uncertainties in the sizing methods, we promote the use of fundamental and quantifiable descriptors of particles such as mass as a function of aerodynamic diameter.
[1] As part of the Puerto Rico Dust Experiment (PRIDE), airborne and surface dust particle samples from Africa were collected and subjected to bulk elemental and singleparticle analysis. Airborne samples were collected on polycarbonate filters at various altitudes and underwent single-particle scanning electron microscopy with energy dispersive analysis with X-rays (EDAX) to derive elemental ratios of key soil elements. Particle chemistry was related to size and morphological characteristics. At the principle surface site, particles were collected on a Davis Rotating Drum (DRUM) cascade impactor strips in eight stages from 0.1 to 12 mm at 4 hour time resolution. These samples were subjected to X-ray florescence (XRF) to determine bulk elemental composition from Al through Zn. The elemental data showed good correlation between the DRUM and the aircraft samples. Cluster analysis of single-particle data resulted in 63 statistically significant clusters. Several clusters can be easily related to their parent mineralogical species. However, as dust particles are to a large extent aggregates, most clusters are based on a continuum of varied mineralogical species and cannot be easily categorized. With 60,500 total particles counted from the airborne filters, a statistically significant number of large particles could be analyzed. Estimated mean surface area modal diameter is $5 mm, with an average aspect ratio of 1.9. An apparent change in source region is seen in the morphological data and non alumino-silicate minerals but is not seen in the aluminum to silicon ratio. We suspect homogenization during long-range transport.
For 26 days in mid‐June and July 2000, a research group comprised of U.S. Navy, NASA, and university scientists conducted the Puerto Rico Dust Experiment (PRIDE). In this paper we give a brief overview of mean meteorological conditions during the study. We focus on our findings on African dust transported into the Caribbean utilizing a Navajo aircraft and AERONET Sun photometer data. During the study midvisible aerosol optical thickness (AOT) in Puerto Rico averaged 0.25, with a maximum >0.5 and with clean marine periods of ∼0.08. Dust AOTs near the coast of Africa (Cape Verde Islands and Dakar) averaged ∼0.4, 30% less than previous years. By analyzing dust vertical profiles in addition to supplemental meteorology and MPLNET lidar data we found that dust transport cannot be easily categorized into any particular conceptual model. Toward the end of the study period, the vertical distribution of dust was similar to the commonly assumed Saharan Air Layer (SAL) transport. During the early periods of the study, dust had the highest concentrations in the marine and convective boundary layers with only a weak dust layer in the SAL being present, a state usually associated with wintertime transport patterns. We corroborate the findings of Maring et al. [2003] that in most cases, there was an unexpected lack of vertical stratification of dust particle size. We systematically analyze processes that may impact dust vertical distribution and speculate that dust vertical distribution predominately influenced by flow patterns over Africa and differential advection coupled with fair weather cloud entrainment, mixing by easterly waves, and regional subsidence.
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