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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.

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.

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.

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.

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.

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.

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.

Biomass burning is a main source for primary carbonaceous particles in the atmosphere and acts as a crucial factor that alters Earth's energy budget and balance. It is also an important factor influencing air quality, regional climate and sustainability in the domain of Pan-Eurasian Experiment (PEEX). During the exceptionally intense agricultural fire season in mid-June 2012, accompanied by rapidly deteriorating air quality, a series of meteorological anomalies was observed, including a large decline in near-surface air temperature, spatial shifts and changes in precipitation in Jiangsu province of East China. To explore the underlying processes that link air pollution to weather modification, we conducted a numerical study with parallel simulations using the fully coupled meteorology–chemistry model WRF-Chem with a high-resolution emission inventory for agricultural fires. Evaluation of the modeling results with available ground-based measurements and satellite retrievals showed that this model was able to reproduce the magnitude and spatial variations of fire-induced air pollution. During the biomass-burning event in mid-June 2012, intensive emission of absorbing aerosols trapped a considerable part of solar radiation in the atmosphere and reduced incident radiation reaching the surface on a regional scale, followed by lowered surface sensible and latent heat fluxes. The perturbed energy balance and re-allocation gave rise to substantial adjustments in vertical temperature stratification, namely surface cooling and upper-air heating. Furthermore, an intimate link between temperature profile and small-scale processes like turbulent mixing and entrainment led to distinct changes in precipitation. On the one hand, by stabilizing the atmosphere below and reducing the surface flux, black carbon-laden plumes tended to dissipate daytime cloud and suppress the convective precipitation over Nanjing. On the other hand, heating aloft increased upper-level convective activity and then favored convergence carrying in moist air, thereby enhancing the nocturnal precipitation in the downwind areas of the biomass-burning plumes.

This work focuses on total organic carbon (TOC) and contributing species in cloud water over Southeast Asia using a rare airborne dataset collected during NASA's Cloud, Aerosol and Monsoon Processes Philippines Experiment (CAMP2Ex), in which a wide variety of maritime clouds were studied, including cumulus congestus, altocumulus, altostratus, and cumulus. Knowledge of TOC masses and their contributing species is needed for improved modeling of cloud processing of organics and to understand how aerosols and gases impact and are impacted by clouds. This work relies on 159 samples collected with an axial cyclone cloud-water collector at altitudes of 0.2–6.8 km that had sufficient volume for both TOC and speciated organic composition analysis. Species included monocarboxylic acids (glycolate, acetate, formate, and pyruvate), dicarboxylic acids (glutarate, adipate, succinate, maleate, and oxalate), methanesulfonic acid (MSA), and dimethylamine (DMA). TOC values range between 0.018 and 13.66 ppm C with a mean of 0.902 ppm C. The highest TOC values are observed below 2 km with a general reduction aloft. An exception is samples impacted by biomass burning for which TOC remains enhanced at altitudes as high as 6.5 km (7.048 ppm C). Estimated total organic matter derived from TOC contributes a mean of 30.7 % to total measured mass (inorganics + organics). Speciated organics contribute (on a carbon mass basis) an average of 30.0 % to TOC in the study region and account for an average of 10.3 % to total measured mass. The order of the average contribution of species to TOC, in decreasing contribution of carbon mass, is as follows (±1 standard deviation): acetate (14.7 ± 20.5 %), formate (5.4 ± 9.3 %), oxalate (2.8 ± 4.3 %), DMA (1.7 ± 6.3 %), succinate (1.6 ± 2.4 %), pyruvate (1.3 ± 4.5 %), glycolate (1.3 ± 3.7 %), adipate (1.0 ± 3.6 %), MSA (0.1 ± 0.1 %), glutarate (0.1 ± 0.2 %), and maleate (< 0.1 ± 0.1 %). Approximately 70 % of TOC remains unaccounted for, highlighting the complex nature of organics in the study region; in samples collected in biomass burning plumes, up to 95.6 % of TOC mass is unaccounted for based on the species detected. Consistent with other regions, monocarboxylic acids dominate the speciated organic mass (∼ 75 %) and are about 4 times more abundant than dicarboxylic acids. Samples are categorized into four cases based on back-trajectory history, revealing source-independent similarity between the bulk contributions of monocarboxylic and dicarboxylic acids to TOC (16.03 %–23.66 % and 3.70 %–8.75 %, respectively). Furthermore, acetate, formate, succinate, glutarate, pyruvate, oxalate, and MSA are especially enhanced during biomass burning periods, which is attributed to peat emissions transported from Sumatra and Borneo. Lastly, dust (Ca2+) and sea salt (Na+/Cl-) tracers exhibit strong correlations with speciated organics, supporting how coarse aerosol surfaces interact with these water-soluble organics.

In June and July 2016 the Dynamics–Aerosol–Chemistry–Cloud Interactions in West Africa (DACCIWA) project organised a major international field campaign in southern West Africa (SWA) including measurements from three inland ground supersites, urban sites in Cotonou and Abidjan, radiosondes, and three research aircraft. A significant range of different weather situations were encountered during this period, including the monsoon onset. The purpose of this paper is to characterise the large-scale setting for the campaign as well as synoptic and mesoscale weather systems affecting the study region in the light of existing conceptual ideas, mainly using objective and subjective identification algorithms based on (re-)analysis and satellite products. In addition, it is shown how the described synoptic variations influence the atmospheric composition over SWA through advection of mineral dust, biomass burning and urban pollution plumes.The boreal summer of 2016 was characterised by Pacific La Niña, Atlantic El Niño and warm eastern Mediterranean conditions, whose competing influences on precipitation led to an overall average rainy season. During the relatively dusty pre-onset Phase 1 (1–21 June 2016), three westward-propagating coherent cyclonic vortices between 4 and 13° N modulated winds and rainfall in the Guinea coastal area. The monsoon onset occurred in connection with a marked extratropical trough and cold surge over northern Africa, leading to a breakdown of the Saharan heat low and African easterly jet and a suppression of rainfall. During this period, quasi-stationary low-level vortices associated with the trough transformed into more tropical, propagating disturbances resembling an African easterly wave (AEW). To the east of this system, moist southerlies penetrated deep into the continent. The post-onset Phase 2 (22 June–20 July 2016) was characterised by a significant increase in low-level cloudiness, unusually dry conditions and strong northeastward dispersion of urban pollution plumes in SWA as well as rainfall modulation by westward-propagating AEWs in the Sahel. Around 12–14 July 2016 an interesting and so-far undocumented cyclonic–anticyclonic vortex couplet crossed SWA. The anticyclonic centre had its origin in the Southern Hemisphere and transported unusually dry air filled with aged aerosol into the region. During Phase 3 (21–26 July 2016), a similar vortex couplet slightly farther north created enhanced westerly moisture transports into SWA and extraordinarily wet conditions, accompanied by a deep penetration of the biomass burning plume from central Africa. Finally, a return to more undisturbed monsoon conditions took place during Phase 4 (27–31 July 2016). The in-depth synoptic analysis reveals that several significant weather systems during the DACCIWA campaign cannot be attributed unequivocally to any of the tropical waves and disturbances described in the literature and thus deserve further study.