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Chamber oxidation experiments conducted at the Fire Sciences Laboratory in 2016 are evaluated to identify important chemical processes contributing to the hydroxy radical (OH) chemistry of biomass burning non-methane organic gases (NMOGs). Based on the decay of primary carbon measured by proton transfer reaction time-of-flight mass spectrometry (PTR-ToF-MS), it is confirmed that furans and oxygenated aromatics are among the NMOGs emitted from western United States fuel types with the highest reactivities towards OH. The oxidation processes and formation of secondary NMOG masses measured by PTR-ToF-MS and iodide-clustering time-of-flight chemical ionization mass spectrometry (I-CIMS) is interpreted using a box model employing a modified version of the Master Chemical Mechanism (v. 3.3.1) that includes the OH oxidation of furan, 2-methylfuran, 2,5-dimethylfuran, furfural, 5-methylfurfural, and guaiacol. The model supports the assignment of major PTR-ToF-MS and I-CIMS signals to a series of anhydrides and hydroxy furanones formed primarily through furan chemistry. This mechanism is applied to a Lagrangian box model used previously to model a real biomass burning plume. The customized mechanism reproduces the decay of furans and oxygenated aromatics and the formation of secondary NMOGs, such as maleic anhydride. Based on model simulations conducted with and without furans, it is estimated that furans contributed up to 10 % of ozone and over 90 % of maleic anhydride formed within the first 4 h of oxidation. It is shown that maleic anhydride is present in a biomass burning plume transported over several days, which demonstrates the utility of anhydrides as markers for aged biomass burning plumes.

From June to October, southern Africa produces one-third of the global biomass burning (BB) emissions by widespread fires. BB aerosols are transported westward over the south-eastern Atlantic with the mid-tropospheric winds, resulting in significant radiative effects. Ascension Island (ASI) is located midway between Africa and South America. From June 2016 to October 2017, a 17-month in situ observation campaign on ASI found a low single-scattering albedo (SSA) as well as a high mass absorption cross-section of black carbon (MACBC), demonstrating the strong absorbing marine boundary layer in the south-eastern Atlantic. Here we investigate the monthly variations of critical optical properties of BB aerosols, i.e. SSA and MACBC, during the BB seasons and the driving factors behind these variations. Both SSA and MACBC increase from June to August and decrease in September and October. The average SSA during the BB seasons is 0.81 at 529 nm wavelength, with the highest mean ∼ 0.85 in October and the lowest ∼ 0.78 in August. The absorption enhancement (Eabs) derived from the MACBC shows similar trends with SSA, with the average during the whole of the BB seasons at ∼ 1.96 and ∼ 2.07 in 2016 and 2017, respectively. As the Eabs is higher than the ∼ 1.5 commonly adopted value by climate models, this result suggests the marine boundary layer in the south-eastern Atlantic is more absorbing than model simulations. We find the enhanced ratio of BC to CO (ΔBC/ΔCO, equal to BC/ΔCO as the BC background concentration is considered to be 0) is well correlated with SSA and MACBC, providing a simple way to estimate the aerosol optical characteristics in the south-eastern Atlantic. The exponential function we proposed can approximate SSA and MACBC with BC/ΔCO, and when BC/ΔCO is small it can capture the rapid growth of SSA as BC/ΔCO decreases. BC/ΔCO is influenced by combustion conditions and aerosol scavenging. From the analysis of the location of BB, the primary source fuel, the water content in the fuel, combined with the mean cloud cover and precipitation in the transport areas of the BB plume, we conclude that the increase in BC/ΔCO from June to August is likely to be caused by burning becoming more flaming. The reduction in the water content of fuels may be responsible for the change in the burning conditions from June to August. The decrease in BC/ΔCO in September and October may be caused by two factors, one being a lower proportion of flaming conditions, possibly associated with a decrease in mean surface wind speed in the burning area, and the other being an increase in precipitation in the BB transport pathway, leading to enhanced aerosol scavenging, which ultimately results in an increase in SSA and MACBC.

Marine stratocumulus clouds cover nearly one-quarter of the ocean surface and thus play an extremely important role in determining the global radiative balance. The semipermanent marine stratocumulus deck over the southeastern Atlantic Ocean is of particular interest, because of its interactions with seasonal biomass burning aerosols that are emitted in southern Africa. Understanding the impacts of biomass burning aerosols on stratocumulus clouds and the implications for regional and global radiative balance is still very limited. Previous studies have focused on assessing the magnitude of the warming caused by solar scattering and absorption by biomass burning aerosols over stratocumulus (the direct radiative effect) or cloud adjustments to the direct radiative effect (the semidirect effect). Here, using a nested modeling approach in conjunction with observations from multiple satellites, we demonstrate that cloud condensation nuclei activated from biomass burning aerosols entrained into the stratocumulus (the microphysical effect) can play a dominant role in determining the total radiative forcing at the top of the atmosphere, compared with their direct and semidirect radiative effects. Biomass burning aerosols over the region and period with heavy loadings can cause a substantial cooling (daily mean −8.05 W m−2), primarily as a result of clouds brightening by reducing the cloud droplet size (the Twomey effect) and secondarily through modulating the diurnal cycle of cloud liquid water path and coverage (the cloud lifetime effect). Our results highlight the importance of realistically representing the interactions of stratocumulus with biomass burning aerosols in global climate models in this region.

The radiative impact of organic aerosols (OA) is a large source of uncertainty in estimating the global direct radiative effect (DRE) of aerosols. This radiative impact includes not only light scattering but also light absorption from a subclass of OA referred to as brown carbon (BrC). However, the absorption properties of BrC are poorly understood, leading to large uncertainties in modeling studies. To obtain observational constraints from measurements, a simple absorption Ångström exponent (AAE) method is often used to separate the contribution of BrC absorption from that of black carbon (BC). However, this attribution method is based on assumptions regarding the spectral dependence of BC that are often violated in the ambient atmosphere. Here we develop a new AAE method which improves upon previous approaches by using the information from the wavelength-dependent measurements themselves and by allowing for an atmospherically relevant range of BC properties, rather than fixing these at a single assumed value. We note that constraints on BC optical properties and mixing state would help further improve this method. We apply this method to multiwavelength absorption aerosol optical depth (AAOD) measurements at AERONET sites worldwide and surface aerosol absorption measurements at multiple ambient sites. We estimate that BrC globally contributes up to 40 % of the seasonally averaged absorption at 440 nm. We find that the mass absorption coefficient of OA (OA-MAC) is positively correlated with the BC ∕ OA mass ratio. Based on the variability in BC properties and BC ∕ OA emission ratio, we estimate a range of 0.05–1.5 m2 g−1 for OA-MAC at 440 nm. Using the combination of AERONET and OMI UV absorption observations we estimate that the AAE388∕440 nm for BrC is generally  ∼ 4 worldwide, with a smaller value in Europe (< 2). Our analyses of observations at two surface sites (Cape Cod, to the southeast of Boston, and the GoAmazon2014/5 T3 site, to the west of Manaus, Brazil) reveal no significant relationship between BrC absorptivity and photochemical aging in urban-influenced conditions. However, the absorption of BrC measured during the biomass burning season near Manaus is found to decrease with photochemical aging with a lifetime of  ∼ 1 day. This lifetime is comparable to previous observations within a biomass burning plume but much slower than estimated from laboratory studies. Given the large uncertainties associated with AERONET retrievals of AAOD, the most challenging aspect of our analysis is that an accurate, globally distributed, multiple-wavelength aerosol absorption measurement dataset is unavailable at present. Thus, achieving a better understanding of the properties, evolution, and impacts of global BrC will rely on the future deployment of accurate multiple-wavelength absorption measurements to which AAE methods, such as the approach developed here, can be applied.

This study characterizes single-particle aerosol composition from filters collected during the ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) and CLoud–Aerosol–Radiation Interaction and Forcing: Year 2017 (CLARIFY-2017) campaigns. In particular the study describes aged biomass burning aerosol (BBA), its interaction with the marine boundary layer and the influence of biomass burning (BB) air on marine aerosol. The study finds evidence of BBA influenced by marine boundary layer processing as well as sea salt influenced by BB air. Secondary chloride aerosols were observed in clean marine air as well as in BB-influenced air in the free troposphere. Higher-volatility organic aerosol appears to be associated with increased age of biomass burning plumes, and photolysis or oxidation may be a mechanism for the apparent increased volatility. Aqueous processing and interaction with the marine boundary layer air may be a mechanism for the presence of sodium on many aged potassium salts. By number, biomass burning potassium salts and modified sea salts are the most observed particles on filter samples. The most commonly observed BC coatings are inorganic salts. These results suggest that atmospheric processes such as photolysis, oxidation and cloud processing are key drivers in the elemental composition and morphology of aged BBA. Fresh BBA inorganic salt content, as it has an important role in the particles' ability to uptake water, may be a key driver in how aqueous processing and atmospheric aging proceed.

We present global airborne observations of acetyl peroxynitrate (CH3C(O)OONO2, PAN) in the remote troposphere from the Atmospheric Tomography (ATom) campaign. These observations show that biomass burning is the dominant source of PAN in the Southern Hemisphere (SH). In the Northern Hemisphere, anthropogenic emissions from Asia and Europe also contribute significantly to PAN over the Pacific and Atlantic Oceans. Model simulations underestimate PAN in the lower troposphere, in part, due to the underestimation of local production driven by acetaldehyde oxidation and βNO2 ${\\beta }_{{\\text{NO}}_{2}}$ (the ratio of acetyl peroxy radicals reacting with NO2 relative to other pathways). The significant impacts of biomass burning evident in the ATom PAN observations suggest that improving model treatment of plume transport and the conversion of NOx to PAN in biomass burning plumes is a viable focus for better simulating PAN. Global observations of PAN provide a benchmark for the evaluation of satellite observations and model simulations of PAN.

This study describes a quite special and interesting atmospheric event characterized by the simultaneous presence of fresh and aged smoke layers. These peculiar conditions occurred on 16 July 2024 at the CNR-IMAA atmospheric observatory (CIAO) in Potenza (Italy), and represent an ideal case for the evaluation of the impact of aging and transport mechanisms on both the optical and microphysical properties of biomass burning aerosol. The fresh smoke was originated by a local wildfire about 2 km from the measurement site and observed about one hour after its ignition. The other smoke layer was due to a wide wildfire occurring in Canada that, according to backward trajectory analysis, traveled for about 5–6 days before reaching the observatory. Synergetic use of lidar, ceilometer, radar, and microwave radiometer measurements revealed that particles from the local wildfire, located at about 3 km a.s.l., acted as condensation nuclei for cloud formation as a result of high humidity concentrations at this altitude range. Optical characterization of the fresh smoke layer based on Raman lidar measurements provided lidar ratio (LR) values of 46 ± 4 sr and 34 ± 3 sr, at 355 and 532 nm, respectively. The particle linear depolarization ratio (PLDR) at 532 nm was 0.067 ± 0.002, while backscatter-related Ångström exponent (AEβ) values were 1.21 ± 0.03, 1.23 ± 0.03, and 1.22 ± 0.04 in the spectral ranges of 355–532 nm, 355–1064 nm and 532–1064 nm, respectively. Microphysical inversion caused by these intensive optical parameters indicates a low contribution of black carbon (BC) and, despite their small size, particles remained outside the ultrafine range. Moreover, a combined use of CIAO remote sensing and in situ instrumentation shows that the particle properties are affected by humidity variations, thus suggesting a marked particle hygroscopic behavior. In contrast, the smoke plume from the Canadian wildfire traveled at altitudes between 6 and 8 km a.s.l., remaining unaffected by local humidity. Absorption in this case was higher, and, as observed in other aged wildfires, the LR at 532 nm was larger than that at 355 nm. Specifically, the LR at 355 nm was 55 ± 2 sr, while at 532 nm it was 82 ± 3 sr. The AEβ values were 1.77 ± 0.13 and 1.41 ± 0.07 at 355–532 nm and 532–1064 nm, respectively and the PLDR at 532 nm was 0.040 ± 0.003. Microphysical analysis suggests the presence of larger, yet much more absorbent particles. This analysis indicates that both optical and microphysical properties of smoke can vary significantly depending on its origin, persistence, and transport in the atmosphere. These factors that must be carefully incorporated into future climate models, especially considering the frequent occurrences of fire events worldwide.

Furans are emitted to the atmosphere during biomass burning from the pyrolysis of cellulose. They are one of the major contributing volatile organic compound (VOC) classes to OH and NO3 reactivity in biomass burning plumes. The major removal process of furans from the atmosphere at night is reaction with the nitrate radical, NO3. Here, we report a series of relative rate experiments in the 7300 L indoor simulation chamber at Institut de Combustion Aérothermique Réactivité et Environnement, Centre national de la recherche scientifique (ICARE-CNRS), Orléans, using a number of different reference compounds to determine NO3 reaction rate coefficients for four furans, two furanones, and pyrrole. In the case of the two furanones, this is the first time that NO3 rate coefficients have been reported. The recommended values (cm3 molec.-1 s-1) are as follows: furan, (1.49 ± 0.23) × 10-12; 2-methylfuran, (2.26 ± 0.52) × 10-11; 2,5-dimethylfuran, (1.02 ± 0.31) × 10-10; furfural (furan-2-aldehyde), (9.07 ± 2.3) × 10-14; α-angelicalactone (5-methyl-2(3H)-furanone), (3.01 ± 0.45) × 10-12; γ-crotonolactone (2(5H)-furanone), <1.4 × 10-16; and pyrrole, (6.94 ± 1.9) × 10-11. The furfural + NO3 reaction rate coefficient is found to be an order of magnitude smaller than previously reported. These experiments show that for furan, alkyl-substituted furans, α-angelicalactone, and pyrrole, reaction with NO3 will be the dominant removal process at night and may also contribute during the day. For γ-crotonolactone, reaction with NO3 is not an important atmospheric sink.

The evolution of organic aerosol (OA) and aerosol size distributions within smoke plumes is uncertain due to the variability in rates of coagulation and OA condensation/evaporation between different smoke plumes and at different locations within a single plume. We use aircraft data from the FIREX-AQ campaign to evaluate differences in evolving aerosol size distributions, OA, and oxygen to carbon ratios (O:C) between and within smoke plumes during the first several hours of aging as a function of smoke concentration. The observations show that the median particle diameter increases faster in smoke of a higher initial OA concentration (>1000 µg m−3), with diameter growth of over 100 nm in 8 h – despite generally having a net decrease in OA enhancement ratios – than smoke of a lower initial OA concentration (<100 µg m−3), which had net increases in OA. Observations of OA and O:C suggest that evaporation and/or secondary OA formation was greater in less concentrated smoke prior to the first measurement (5–57 min after emission). We simulate the size changes due to coagulation and dilution and adjust for OA condensation/evaporation based on the observed changes in OA. We found that coagulation explains the majority of the diameter growth, with OA evaporation/condensation having a relatively minor impact. We found that mixing between the core and edges of the plume generally occurred on timescales of hours, slow enough to maintain differences in aging between core and edge but too fast to ignore the role of mixing for most of our cases.

Open biomass burning contributes significantly to air quality degradation and associated human health impacts over large areas. It is one of the largest sources of reactive trace gases and fine particles to Earth’s atmosphere and consequently a major source of cloud condensation nuclei on a global scale. However, there is a large uncertainty in the climate effect of open biomass burning aerosols due to the complexity of their constituents. Here, we present an exceptionally large dataset on southern African savannah and grassland fire plumes and their atmospheric evolution, based on 5.5 years of continuous measurements from 2010 to 2015. We find that the mass of submicrometre aerosols more than doubles on average, in only three hours of daytime ageing. We also evaluate biomass burning aerosol particle size distributions and find a large discrepancy between the observations and current model parameterizations, especially in the 30–100 nm range. We conclude that accounting for near-source secondary organic aerosol formation and using measurement-based size distribution parameterizations in smoke plumes is essential to better constrain the climate and air quality effects of savannah and grassland fires.