Two extreme cases of aerosol optics from the Reno Aerosol Optics Experiment are used to develop a model-based calibration scheme for the 7-wavelength aethalometer. The cases include those of very white and very dark aerosol samples. The former allows for an assessment of the scattering offset associated with this filter-based method, with the wavelength-dependent scattering measured from a 3-wavelength nephelometer, and interpolated and extrapolated to the 7 wavelengths of the aethalometer. A photoacoustic instrument operating at 532 nm is used to evaluate the filter loading effect caused by aerosol light absorption. Multiple scattering theory is used to analytically obtain a filter-loading correction function. This theory shows that the exponential behavior of light absorption in the strong multiple scattering limit scales as the square root of the total absorption optical depth rather than linearly with optical depth as is commonly assumed with Beer's law. The multiple scattering model also provides a theoretical justification for subtracting a small fraction of aerosol light scattering away from measured apparent light absorption by the filter method. The model is tested against ambient measurements and is found to require coefficients that are situation specific. Several hypotheses are given for this specificity, and suggested methods for reducing it are discussed. Specific findings are as follows. Simultaneous aerosol light-scattering measurements are required for accurate interpretation of aethalometer data for high aerosol single-scattering albedo. Instantaneous errors of up to ±50% are possible for uncorrected data, depending on filter loading. The aethalometer overpredicts black carbon (BC) concentration on a fresh filter and underpredicts BC on a loaded filter. BC and photoacoustic light absorption can be tightly correlated if the data are averaged over the full range of filter loadings and the aerosol source is constant. Theory predicts that the Aethalometer response may be sensitive to filter face velocity, and hence flow rate, to the extent that particle penetration depth depends on face velocity.

We report the direct observation of laboratory production of spherical, carbonaceous particles – "tar balls" – from smoldering combustion of two commonly occurring dry mid-latitude fuels. Real-time measurements of spectrally varying absorption Ångström coefficients (AAC) indicate that a class of light absorbing organic carbon (OC) with wavelength dependent imaginary part of its refractive index – optically defined as "brown carbon" – is an important component of tar balls. The spectrum of the imaginary parts of their complex refractive indices can be described with a Lorentzian-like model with an effective resonance wavelength in the ultraviolet (UV) spectral region. Sensitivity calculations for aerosols containing traditional OC (no absorption at visible and UV wavelengths) and brown carbon suggest that accounting for near-UV absorption by brown carbon leads to an increase in aerosol radiative forcing efficiency and increased light absorption. Since particles from smoldering combustion account for nearly three-fourths of the total carbonaceous aerosol mass emitted globally, inclusion of the optical properties of tar balls into radiative forcing models has significance for the Earth's radiation budget, optical remote sensing, and understanding of anomalous UV absorption in the troposphere.

We characterized the gas‐ and speciated aerosol‐phase emissions from the open combustion of 33 different plant species during a series of 255 controlled laboratory burns during the Fire Laboratory at Missoula Experiments (FLAME). The plant species we tested were chosen to improve the existing database for U.S. domestic fuels: laboratory‐based emission factors have not previously been reported for many commonly burned species that are frequently consumed by fires near populated regions and protected scenic areas. The plants we tested included the chaparral species chamise, manzanita, and ceanothus, and species common to the southeastern United States (common reed, hickory, kudzu, needlegrass rush, rhododendron, cord grass, sawgrass, titi, and wax myrtle). Fire‐integrated emission factors for gas‐phase CO₂, CO, CH₄, C_2–4hydrocarbons, NH₃, SO₂, NO, NO₂, HNO₃, and particle‐phase organic carbon (OC), elemental carbon (EC), SO₄²⁻, NO₃⁻, Cl⁻, Na⁺, K⁺, and NH₄⁺generally varied with both fuel type and with the fire‐integrated modified combustion efficiency (MCE), a measure of the relative importance of flaming‐ and smoldering‐phase combustion to the total emissions during the burn. Chaparral fuels tended to emit less particulate OC per unit mass of dry fuel than did other fuel types, whereas southeastern species had some of the largest observed emission factors for total fine particulate matter. Our measurements spanned a larger range of MCE than prior studies, and thus help to improve estimates of the variation of emissions with combustion conditions for individual fuels.