ALBERT

Description: Cheatgrass (Bromus Tectorum) is a highly invasive species in the Great Basin of the Western USA that is increasing the frequency and intensity of wildland fires. Though cheatgrass plays a significant role in the fire ecology of the Great Basin, very little is known about its combustion emissions. The fresh smoke from 16 open laboratory burns of cheatgrass was analyzed using real-time measurements and filter analysis. We presented measured intensive optical properties of the emitted smoke, including absorption Ångström exponent (AAE), scattering Ångström exponent (SAE), single scattering albedo (SSA), and other combustion properties, such as modified combustion efficiency (MCE) and fuel-based emission factors (EFs). In addition, we gave a detailed chemical analysis of polar organic species in cheatgrass combustion emissions. We presented EFs that showed a large variation between fuels and demonstrated that analysis of combustion emissions for specific fuels was important for studying and modeling the chemistry of biomass-burning emissions.

Description: Light-absorbing organic carbon aerosol – colloquially known as brown carbon (BrC) – is emitted from combustion processes and has a brownish or yellowish visual appearance, caused by enhanced light absorption at shorter visible and ultraviolet wavelengths (0.3 µm≲λ≲0.5 µm). Recently, optical properties of atmospheric BrC aerosols have become the topic of intense research, but little is known about how BrC deposition onto snow surfaces affects the spectral snow albedo, which can alter the resulting radiative forcing and in-snow photochemistry. Wildland fires in close proximity to the cryosphere, such as peatland fires that emit large quantities of BrC, are becoming more common at high latitudes, potentially affecting nearby snow and ice surfaces. In this study, we describe the artificial deposition of BrC aerosol with known optical, chemical, and physical properties onto the snow surface, and we monitor its spectral radiative impact and compare it directly to modeled values. First, using small-scale combustion of Alaskan peat, BrC aerosols were artificially deposited onto the snow surface. UV–Vis absorbance and total organic carbon (TOC) concentration of snow samples were measured for samples with and without artificial BrC deposition. These measurements were used to first derive a BrC (mass) specific absorption (m2 g−1) across the UV–Vis spectral range. We then estimate the imaginary part of the refractive index of deposited BrC aerosol using a volume mixing rule. Single-particle optical properties were calculated using Mie theory, and these values were used to show that the measured spectral snow albedo of snow with deposited BrC was in general agreement with modeled spectral snow albedo using calculated BrC optical properties. The instantaneous radiative forcing per unit mass of total organic carbon deposited to the ambient snowpack was found to be 1.23 (+0.14/-0.11) W m−2 per part per million (ppm). We estimate the same deposition onto a pure snowpack without light-absorbing impurities would have resulted in an instantaneous radiative forcing per unit mass of 2.68 (+0.27/-0.22) W m−2 per ppm of BrC deposited.

Description: Semivolatile organic compounds (SVOCs) emitted from open biomass burning (BB) can contribute to chemical and physical properties of atmospheric aerosols and also may cause adverse health effects. The polar fraction of SVOCs is a prominent part of BB organic aerosols, and thus it is important to characterize the chemical composition and reactivity of this fraction. In this study, globally and regionally important representative fuels (Alaskan peat, Moscow peat, Pskov peat, eucalyptus, Malaysian peat, and Malaysian agricultural peat) were burned under controlled conditions using the combustion chamber facility at the Desert Research Institute (DRI). Gas- and particle-phase biomass-burning emissions were aged in an oxidation flow reactor (OFR) to mimic 5–7 d of atmospheric aging. Fresh and OFR-aged biomass-burning aerosols were collected on Teflon-impregnated glass fiber filters (TIGF) in tandem with XAD resin media for organic carbon speciation. The polar fraction extracted with dichloromethane and acetone was analyzed with gas chromatography mass spectrometry (GC-MS) for 84 polar organic compounds – including mono- and dicarboxylic acids, methoxylated phenols, aromatic acids, anhydrosugars, resin acids, and sterols. For all these compounds, fuel-based emission factors (EFs) were calculated for fresh and OFR-aged samples. The carbon mass of the quantified polar compounds was found to constitute 5 % to 7 % of the total organic compound mass. A high abundance of methoxyphenols (239 mg kg−1 for Pskov peat; 22.6 % of total GC-MS characterized mass) and resin acids (118 mg kg−1 for Alaskan peat; 14.5 % of total GC-MS characterized mass) was found in peat-burning emissions (smoldering combustion). The concentration of some organic compounds (e.g., tetracosanoic acid) with a molecular weight (MW) above 350 g mol−1 decreased after OFR aging, while abundances of low-MW compounds (e.g., hexanoic acid) increased. This indicated a significant extent of fragmentation reactions in the OFR. Methoxyphenols decreased after OFR aging, while a significant increase (3.7 to 8.6 times) in the abundance of dicarboxylic acids emission factors (EFs), especially maleic acid (10 to 60 times), was observed. EFs for fresh and ratios from fresh-to-aged BB samples reported in this study can be used to perform source apportionment and predict processes occurring during atmospheric transport.

Description: Fresh and atmospherically aged biomass-burning (BB) aerosol mass is mostly comprised of strongly light-absorbing 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 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 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.

Description: Light-absorbing organic carbon aerosol – colloquially known as brown carbon (BrC) – is emitted from combustion processes and has a brownish or yellowish visual appearance, caused by enhanced light absorption at shorter visible and ultraviolet wavelengths (0.3 μm ≲ λ ≲ 0.5 μm). Recently, optical properties of atmospheric BrC aerosols have become the topic of intense research, but little is known about how BrC deposition onto snow surfaces affects the spectral snow albedo, which can alter the resulting radiative forcing and in-snow photochemistry. Wildland fires in close proximity to the cryosphere, such as peatland fires that emit large quantities of BrC, are becoming more common at high latitudes, potentially affecting nearby snow and ice surfaces. In this study, we describe the artificial deposition of BrC aerosol with known optical, chemical, and physical properties onto the snow surface and we monitor its spectral radiative impact and compare it directly to modeled values. First, using small-scale combustion of Alaskan peat, BrC aerosols were artificially deposited onto the snow surface. UV-vis absorbance and total organic carbon (TOC) concentration of snow samples were measured for samples with and without artificial BrC deposition. These measurements were used to estimate the imaginary part of the refractive index of deposited BrC aerosol with a volume mixing rule. Single particle optical properties were calculated using Mie theory, and these values were used to show that the measured spectral snow albedo of snow with deposited BrC was in general agreement with modeled spectral snow albedo using calculated BrC optical properties. The instantaneous radiative forcing by impurities present in the snow before the deposition experiments was found to increase the instantaneous radiative forcing at the surface of the natural snow at our site by 1.23 (+0.14/−0.11) W m−2 per ppm of BrC deposited. However, we estimate that deposition onto a clean snowpack without light-absorbing impurities would have resulted in a more than twice as large instantaneous radiative forcing of 2.68 (+0.27/−0.22) W m−2 per ppm of BrC deposited.

Description: 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). 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 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 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 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 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.

Description: Wildfires have become an important source of particulate matter (PM2.5 〈 2.5-µm diameter), leading to unhealthy air quality index occurrences in the western United States. Since people mainly shelter indoors during wildfire smoke events, the infiltration of wildfire PM2.5 into indoor environments is a key determinant of human exposure and is potentially controllable with appropriate awareness, infrastructure investment, and public education. Using time-resolved observations outside and inside more than 1,400 buildings from the crowdsourced PurpleAir sensor network in California, we found that the geometric mean infiltration ratios (indoor PM2.5 of outdoor origin/outdoor PM2.5) were reduced from 0.4 during non-fire days to 0.2 during wildfire days. Even with reduced infiltration, the mean indoor concentration of PM2.5 nearly tripled during wildfire events, with a lower infiltration in newer buildings and those utilizing air conditioning or filtration.