Abstract
The refractive index (RI) is an important parameter in describing the radiative impacts of aerosols. It is important to constrain the RI of aerosol components, since there is still significant uncertainty regarding the RI of biomass burning aerosols. Experimentally measured extinction cross-sections, scattering cross-sections, and single scattering albedos for white pine biomass burning (BB) aerosols under two different burning and sampling conditions were modeled using T-matrix theory. The refractive indices were extracted from these calculations. Experimental measurements were conducted using a cavity ring-down spectrometer to measure the extinction, and a nephelometer to measure the scattering of size-selected aerosols. BB aerosols were obtained by burning white pine using (1) an open fire in a burn drum, where the aerosols were collected in distilled water using an impinger, and then re-aerosolized after several days, and (2) a tube furnace to directly introduce the BB aerosols into an indoor smog chamber, where BB aerosols were then sampled directly. In both cases, filter samples were also collected, and electron microscopy images were used to obtain the morphology and size information used in the T-matrix calculations. The effective radius of the particles collected on filter media from the open fire was approximately 245 nm, whereas it was approximately 76 nm for particles from the tube furnace burns. For samples collected in distilled water, the real part of the RI increased with increasing particle size, and the imaginary part decreased. The imaginary part of the RI was also significantly larger than the reported values for fresh BB aerosol samples. For the particles generated in the tube furnace, the real part of the RI decreased with particle size, and the imaginary part was much smaller and nearly constant. The RI is sensitive to particle size and sampling method, but there was no wavelength dependence over the range considered (500–680 nm). Our values for the RI of fresh (white pine) biomass burning aerosols ranged from 1.33 + i0.008 to 1.74 + i0.008 for 200-nm, 300-nm, and 400-nm diameter particles. These are within the range of RI values in the most recent study conducted during the Fire Laboratory at Missoula Experiments (FLAME I and II), which were 1.55 to 1.80 for the real part, and 0.01–0.50 for the imaginary part, for fresh BB aerosols with diameters of 200–570 nm. There is no clear trend on the dependence of the RI values on particle size. The RI values derived from measurements of aerosols produced from the combustion of hydrocarbons and diesel cannot be used for BB aerosols.
Highlights
With an estimated total climate forcing of +1.1 W·m−2, black carbon (BC) is the second most important human emission in terms of its climate forcing in the present-day atmosphere, second to CO2 [1]
In biomass burning, flaming combustion is characterized by the production of BC, while smoldering combustion is dominated by the production of organic carbon (OC), including brown carbon (BrC)
For the initial T-matrix calculations, we considered the biomass burning (BB) aerosols obtained from our experiments to have higher concentrations of black carbon
Summary
With an estimated total climate forcing of +1.1 W·m−2 , black carbon (BC) is the second most important human emission in terms of its climate forcing in the present-day atmosphere, second to CO2 [1]. The values of efficiencies Qabs , Qscatt , and Qext are calculated using the Mie code for values of the real and imaginary parts of the index of refraction, and using experimental values of extinction and scattering cross-sections, a best fit is found by minimizing the error between the calculated and measured values [48] This assumes the particles are pure spheres, which is not the case for real BB aerosols. Theory, which treats particles as fractal-like aggregates of small spheres, and Mie theory, to study the optical properties of combustion particles from propane This method produced single scattering albedo (SSA) values that were underestimated by 56% when compared with the experimental results [46]. Filter samples were collected from both types of burning, and electron microscopy images were used to obtain morphology and size information to conduct T-matrix calculations
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