Abstract. 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 absorptionÅngström 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.

[1] A dual-wavelength photoacoustic instrument operating at 405 and 870 nm was used during the 2006 Fire Lab at Missoula Experiment to measure light scattering and absorption by smoke from the combustion of a variety of biomass fuels. Simultaneous measurements of aerosol light scattering by reciprocal nephelometry within the instrument's acoustic resonator accompany photoacoustic aerosol light absorption measurements. Single scattering albedo values at 405 nm ranging from 0.37 to 0.95 were measured for different fuel types, and the spectral dependence of absorption was quantified using the Å ngström exponent of absorption. An absorption Å ngström exponent near unity is commonly observed for motor vehicle emission-generated black carbon aerosol. For biomass smoke, Å ngström exponents as high as 3.5 were found in association with smoke having single scattering albedo near unity. The measurements strongly suggest that light-absorbing organic material is present in wood smoke. A second singlewavelength photoacoustic instrument with reciprocal nephelometry was used to quantify aerosol scattering and absorption at 532 nm. Absorption Å ngström exponents calculated using 532 and 870 nm data were as large as 2.5 for smoke with single scattering albedos near unity. The spectral variation in optical properties provides insight into the differentiation of aerosols from mobile or industrial sources versus those from biomass burning. Optical properties of biomass smokes could be classified by general fuel type such as flowering shrubs versus pine needle litter.Citation: Lewis, K., W. P. Arnott, H. Moosmüller, and C. E. Wold (2008), Strong spectral variation of biomass smoke light absorption and single scattering albedo observed with a novel dual-wavelength photoacoustic instrument,

Abstract. Hundreds of wildfires in Northern California were sparked by lightning during the summer of 2008, resulting in downwind smoke for the months of June and July. Comparisons are reported for aerosol optics measurements in Reno, Nevada made during the very smoky month of July and the relatively clean month of August. Photoacoustic instruments equipped with integrating nephelometers were used to measure aerosol light scattering and absorption coefficients at wavelengths of 405 nm and 870 nm, revealing a strong variation of aerosol light absorption with wavelength. Insight on fuels burned is gleaned from comparison ofÅngström exponents of absorption (AEA) versus single scattering albedo (SSA) of the ambient measurements with laboratory biomass smoke measurements for many fuels. Measurements during the month of August, which were largely unaffected by fire smoke, exhibit surprisingly low AEA for aerosol light absorption when the SSA is highest, again likely as a consequence of the underappreciated wavelength dependence of aerosol light absorption by particles coated with nonabsorbing organic and inorganic matter. Coated sphere calculations were used to show that AEA as large as 1.6 are possible for wood smoke even with non-absorbing organic coatings on black carbon cores, suggesting care be exercised when diagnosing AEA.

Abstract. We report the direct observation of large-scale production of spherical, carbonaceous particles – "tar balls" – from smoldering combustion of two commonly occurring dry mid-latitude fuels. Real-time measurements indicate that 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 organic carbon (no absorption at visible and UV wavelengths) and brown carbon suggest that accounting for UV absorption by brown carbon leads to a significant increase in aerosol radiative forcing efficiency and increased atmospheric warming. 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.

Abstract. Smoke particle emissions from the combustion of biomass fuels typical for the western and southeastern United States were studied and compared under high humidity and ambient conditions in the laboratory. The fuels used were Montana ponderosa pine (Pinus ponderosa), southern California chamise (Adenostoma fasciculatum), and Florida saw palmetto (Serenoa repens). Information on the nonrefractory chemical composition of biomass burning aerosol from each fuel was obtained with an aerosol mass spectrometer and through estimation of the black carbon concentration from light absorption measurements at 870 nm. Changes in the optical and physical particle properties under high humidity conditions were observed for hygroscopic smoke particles containing substantial inorganic mass fractions that were emitted from combustion of chamise and palmetto fuels. Light scattering cross sections increased under high humidity for these particles, consistent with the hygroscopic growth measured for 100 nm particles in HTDMA measurements.

[1] Aerosols generated from burning different plant fuels were characterized to determine relationships between chemical, optical and physical properties. Single scattering albedo (w) and Angstrom absorption coefficients (a ap ) were measured using a photoacoustic technique combined with a reciprocal nephelometer. Carbon-to-oxygen atomic ratios, sp 2 hybridization, elemental composition and morphology of individual particles were measured using scanning transmission X-ray microscopy coupled with near-edge X-ray absorption fine structure spectroscopy (STXM/ NEXAFS) and scanning electron microscopy with energy dispersion of X-rays (SEM/EDX). Particles were grouped into three categories based on sp 2 hybridization and chemical composition. Measured w (0.4 À 1.0 at 405 nm) and a ap (1.0 À 3.5) values displayed a fuel dependence. The category with sp 2 hybridization >80% had values of w (<0.5) and a ap ($1.25) characteristic of light absorbing soot. Other categories with lower sp 2 hybridization (20 to 60%) exhibited higher w (>0.8) and a ap (1.0 to 3.5) values, indicating increased absorption spectral selectivity.

Abstract.A series of laboratory experiments at the Fire Laboratory at Missoula (FLAME) investigated chemical, physical, and optical properties of fresh smoke samples from combustion of wildland fuels that are burned annually in the western and southeastern US The burns were conducted in the combustion chamber of the US Forest Service Fire Sciences Laboratory in Missoula, Montana. Here we discuss retrieval of optical properties for a variety of fuels burned in FLAME 2, using nephelometer-measured scattering coefficients, photoacoustically-measured aerosol absorption coefficients, and size distribution measurements. Uncertainties are estimated from various instrument characteristics and instrument calibration studies. Our estimates of single scattering albedo for different dry smoke samples varied from 0.428 to 0.990, indicative of observed wide variations in smoke aerosol chemical composition. In selected case studies, we retrieved the complex refractive index from measurements but show that these are highly sensitive to uncertainties in measured size distributions.

Abstract. Smoke particle emissions from the combustion of biomass fuels typical for the western and southeastern United States were studied and compared under high humidity and ambient conditions in the laboratory. The fuels used are Montana ponderosa pine (Pinus ponderosa), southern California chamise (Adenostoma fasciculatum), and Florida saw palmetto (Serenoa repens). Information on the non-refractory chemical composition of biomass burning aerosol from each fuel was obtained with an aerosol mass spectrometer and through estimation of the black carbon concentration from light absorption measurements at 870 nm. Changes in the optical and physical particle properties under high humidity conditions were observed for hygroscopic smoke particles containing substantial inorganic mass fractions that were emitted from combustion of chamise and palmetto fuels. Light scattering cross sections increased under high humidity for these particles, consistent with the hygroscopic growth measured for 100 nm particles in HTDMA measurements. Photoacoustic measurements of aerosol light absorption coefficients reveal a 20% reduction with increasing relative humidity, contrary to the expectation of light absorption enhancement by the liquid coating taken up by hygroscopic particles. This reduction is hypothesized to arise from two mechanisms: 1. Shielding of inner monomers after particle consolidation or collapse with water uptake; 2. The contribution of mass transfer through evaporation and condensation at high relative humidity to the usual heat transfer pathway for energy release by laser-heated particles in the photoacoustic measurement of aerosol light absorption. The mass transfer contribution is used to evaluate the fraction of aerosol surface covered with liquid water solution as a function of RH.