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We use a simple model of a spherical biomass burning aerosol particle containing an internal mixture of black carbon (BC) and organic carbon (OC) with an effective refractive index calculated as a volume fraction‐weighted mean of refractive indices. Brown carbon (BrC) is considered to be an OC with an imaginary part of refractive index at the blue end of the solar spectrum higher (in absolute value) than at the red end. Mie‐scattering formalism is employed to calculate absorption Ångström exponent (AAE) as a function of single‐scattering albedo (SSA) for a set of BC refractive indices, BC volume fraction, and a set of effective refractive indices of BC and BrC mixtures. Ambient plumes are characterized by their mean SSA at 405 nm wavelength and two‐wavelength (405 and 781 nm) AAE values. Comparing observed and model‐calculated AAE and SSA values identifies the BC refractive index and its volume fraction and an effective refractive index of the BC and BrC mixture. From these values, the imaginary part of BrC refractive index is calculated. For observed southwestern ambient fires, the imaginary part of BrC refractive index is ≤0.016. In contrast, fires in the Amazon and from Africa are dominated by BC. We also use the Mie scattering model to establish the upper limit on AAE of BC (AAE ≤ 1.4) and the upper limit of the BC and OC mixture (AAE ≤ 1.7). Any AAE(405/781) > 1.7 requires the presence of BrC. We derive several relationships between AAE, SSA, BC fractions, and an imaginary part of BrC refractive index of ambient fires. Mie scattering model assuming spherical aerosol particles captures basic optical properties of ambient biomass burning aerosolsAbsorption Ångström exponent (AAE) of black carbon is limited to AAE <1.4, and AAE values >1.7 require the presence of brown carbonThe imaginary part of refractive index of brown carbon at the blue end of a solar spectrum is found to be between 0.005 and 0.016 for ambient plumes

Biomass burning (BB) is an important global source of aerosol and trace gases that degrade air quality, decrease visibility, and impact climate and human health. Refractory black carbon (rBC), brown carbon (BrC), and organic aerosol are major components of BB emissions. BB aerosol composition is highly variable at the source and depends on fuel composition and combustion phase. Atmospheric aging alters fresh BB aerosol through processes that are complex and dynamic. To better understand the variability in optical properties, we report fresh aerosol laboratory measurements from burning southwestern U.S. fuels and compare them to aged ambient BB aerosol from wildfires over a range of atmospheric time scales. Our BB aerosol analysis uses the relationship between the absorption Ångström exponent and single‐scattering albedo (SSA) to identify rBC, BrC, and organic aerosol‐dominated regimes that are defined using Mie theory. This model framework is used to interpret the large variability in optical properties measured in laboratory burns. In contrast, we find the observed absorption Ångström exponent‐SSA relationship for ambient BB aerosol to be less variable and more clustered together with increased atmospheric aging. This transition from fresh to aged behavior is attributed to the homogenization of the BB aerosol from mixing and aging over several hours. Finally, BB aerosol in ambient fire plumes that have aged for several hours exhibits larger SSAs than laboratory flaming burns. We conclude that BrC/OC mixtures play a larger role than rBC in the positive climate forcing of BB aerosol than what would be projected from laboratory results. A semiempirical Mie theory framework can be used to classify the chemical composition of biomass burning aerosol by optical propertiesSmoke optical properties in aged ambient fire plumes are more clustered and less variable than fresh laboratory burns due to mixing and agingAerosols from ambient fires are shifted toward the brown carbon and organic carbon mixing regime relative to those from laboratory fires