Abstract. Fresh and atmospherically aged biomass-burning (BB) aerosol mass is mostly comprised of strongly lightabsorbing black carbon (BC) and of organic carbon (OC) with its light-absorbing fraction -brown carbon (BrC). There is a lack of data on the physical and chemical properties of atmospheric BB aerosols, leading to high uncertainties in estimates of the BB impact on air quality and climate, especially for BrC. The polarity of chemical compounds influences their fate in the atmosphere including wet/dry deposition and chemical and physical processing. So far, most of the attention has been given to the water-soluble (polar) fraction of BrC, while the non-polar BrC fraction has been largely ignored. In the present study, the light absorption properties of polar and non-polar fractions of fresh and aged BB emissions were examined to estimate the contribution of differentpolarity organic compounds to the light absorption properties of BB aerosols.In our experiments, four globally and regionally important fuels were burned under flaming and smoldering conditions in the Desert Research Institute (DRI) combustion chamber. To mimic atmospheric oxidation processes (5-7 days), BB emissions were aged using an oxidation flow reactor (OFR). Fresh and OFR-aged BB aerosols were collected on filters and extracted with water and hexane to study absorption properties of polar and non-polar organic species. Results of spectrophotometric measurements (absorption weighted by the solar spectrum and normalized to mass of fuel consumed) over the 190 to 900 nm wavelength range showed that the non-polar (hexane-soluble) fraction is 2-3 times more absorbing than the polar (water-soluble) fraction. However, for emissions from fuels that undergo flaming combustion, an increased absorbance was observed for the water extracts of oxidized/aged emissions while the absorption of the hexane extracts was lower for the aged emissions for the same type of fuels. Absorption Ångström exponent (AAE) values, computed based on absorbance values from spectrophotometer measurements, were changed with aging and the nature of this change was fuel dependent. The light absorption by humic-like substances (HULIS) was found to be higher in fuels characteristic of the southwestern USA. The absorption of the HULIS fraction was lower for OFR-aged BB emissions. Comparison of the light absorption properties of different-polarity extracts (water, hexane, HULIS) provides insight into the chemical nature of BB BrC and its transformation during oxidation processes.

Biomass burning (BB) emissions and their atmospheric oxidation products can contribute significantly to direct aerosol radiative forcing of climate. Limited knowledge of BB organic aerosol chemical and optical properties leads to large uncertainties in climate models. In this article, we describe the experimental setup and the main findings of a laboratory BB study aimed at comprehensive optical, physical, and chemical characterization of fresh and aged BB emissions. An oxidation flow reactor (OFR) was used to mimic atmospheric oxidation processes. The OFR was characterized in terms of OHÁ production rate, particle transmission efficiency, and characteristic lifetimes of condensible compounds. Emission factors (EFs) of main air pollutants (particulate matter, organic carbon [OC], elemental carbon [EC], carbon monoxide [CO], and nitrogen oxides [NO x ]) were determined for five globally and regionally important biomass fuels: Siberian (Russia), Florida (USA), and Malaysian peats; mixed conifer and aspen fuel from Fishlake National Forest, Utah, USA; and mixed grass and brush fuel representative of the Great Basin, Nevada, USA. Measured fuel-based EFs for OC ranged from 0.85 ± 0.24 to 6.56 ± 1.40 mg g À1 . Measured EFs for EC ranged from 0.02 ± 0.01 to 0.16 ± 0.01 mg g À1 . The ratio of organic mass to total carbon mass for fresh emissions from these fuels ranged from 1.04 ± 0.04 to 1.34 ± 0.24. The effect of OFR aging on aerosol optical properties, size distribution, and concentration is also discussed.

Abstract. Fresh and atmospherically aged biomass-burning (BB) aerosol mass is mostly comprised of black carbon (BC) and organic carbon (OC) with its light-absorbing fraction -brown carbon (BrC). 10There is a lack of data on the physical and chemical properties of atmospheric BB aerosols, leading to high uncertainties in estimates of the BB impact on air quality and climate, especially for BrC. The polarity of chemical compounds influences their fate in the atmosphere including wet/dry deposition and chemical and physical processing. So far, most of the attention has been given to the water-soluble (polar) fraction of BrC, while the non-polar BrC fraction has been largely ignored. In the present study, 15 the light absorption properties of polar and non-polar fractions of fresh and aged BB emissions were examined to estimate the contribution of different-polarity organic compounds to the light absorption properties of BB aerosols.In our experiments, four globally and regionally important fuels were burned under flaming and smoldering conditions in DRI's combustion chamber. To mimic atmospheric oxidation processes (5-7 20 days), BB emissions were aged using an oxidation flow reactor (OFR). Fresh and OFR-aged BB aerosols were collected on filters and extracted with water and hexane to study absorption properties of polar and non-polar organic species. Spectrophotometric measurements over the 190 to 900 nm wavelength range showed that the non-polar (hexane-soluble) fraction is 2-3 times more absorbing than the polar (water-soluble) fraction. However, an increased absorbance was observed for the water 25 extracts of oxidized/aged emissions while the absorption of the hexane extracts was lower for the aged emissions. Comparing the absorption Ångström Exponent (AAE) values, we observed changes in the light absorption properties of BB aerosols with aging that was dependent on the fuel types. The light Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-161 Manuscript under review for journal Atmos. Chem. Phys.

Carbonaceous aerosols emitted from biomass burning influence radiative forcing and climate change. Of particular interest are emissions from high-latitude peat burning because amplified climate change makes the large carbon mass stored in these peatlands more susceptible to wildfires and their emission can affect cryosphere albedo and air quality after undergoing transport. We combusted Siberian peat in a laboratory biomass-burning facility and characterized the optical properties of freshly emitted combustion aerosols and those photochemically aged in an oxidation flow reactor (OFR) with a three-wavelength photoacoustic instrument. Total particle count increased with aging by a factor of 6 to 11 while the total particle volume either changed little (<8%) for 19 and 44 days of equivalent aging and increased by 88% for 61 days of equivalent aging. The aerosol single-scattering albedo (SSA) of both fresh and aged aerosol increased with the increasing wavelength. The largest changes in SSA due to OFR aging were observed at the shortest of the three wavelengths (i.e., at 405 nm) where SSA increased by less than ~2.4% for 19 and 44 days of aging. These changes were due to a decrease in the absorption coefficients by ~45%, with the effect on SSA somewhat reduced by a concurrent decrease in the scattering coefficients by 20 to 25%. For 61 days of aging, we observed very little change in SSA, namely an increase of 0.31% that was caused a ~56% increase in the absorption coefficients that was more than balanced by a somewhat larger (~71%) increase in the scattering coefficients. These large increases in the absorption and scattering coefficients for aging at 7 V are at least qualitatively consistent with the large increase in the particle volume (~88%). Overall, aging shifted the absorption toward longer wavelengths and decreased the absorption Ångström exponents, which ranged from ~5 to 9. Complex refractive index retrieval yielded real and imaginary parts that increased and decreased, respectively, with the increasing wavelength. The 405 nm real parts first increased and then decreased and imaginary parts decreased during aging, with little change at other wavelengths.

Combustion type can be characterized with different methods including calculating (modified) combustion efficiency (Yatavelli et al., 2017) and using an IR camera to monitor the thermal IR emissions (Freeborn et al., 2008). In this study, we have used the rate of fuel mass change to characterize combustion type.