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Biomass burning smoke aerosols are efficient at attenuating incoming solar radiation. The Layered Atlantic Smoke Interactions with Clouds campaign was conducted from June 2016 to October 2017. The U. S. Department of Energy mobile Atmospheric Radiation Measurement site located on Ascension Island (AMF‐ASI) identified several instances of smoke plume intrusions. Increases in surface and column measurements of aerosol loading were directly related to increases in fine mode fraction, number concentrations of aerosols (Na), and cloud condensation nuclei (NCCN). During periods of weak lower tropospheric stability, smoke particles were more likely to be advected downward either by boundary layer turbulence or cloud top entrainment under non‐overcast sky conditions. Backward trajectory analysis illustrated that smoke aerosols reaching the AMF‐ASI site were fine mode, less aged, strongly absorbing, and had shorter boundary layer trajectories while longer boundary layer trajectories denoted mixtures of weakly absorbing smoke and coarse mode marine aerosols. The most polluted smoke cases of August 2016 and 2017 revealed a notable contrast in radiative forcing per unit aerosol optical depth or radiative forcing efficiency (ΔFeff) at the top of the atmosphere (TOA) and near‐surface (BOA). The weakly (strongly) absorbing 2016 cases exhibited weaker (stronger) ΔFeff at the TOA and BOA suggesting a warming (cooling) effect within the boundary layer. The 2017 cases featured the strongest ΔFeff suggesting more of a cooling effect at the TOA and BOA due to mixing of fresh smoke with marine aerosols during transport. Plain Language Summary: Fires are often observed in Central Africa throughout the year due to agricultural and natural processes. As a result of changes in pressure patterns along with wind direction and strength, the smoke aerosols can transport to regions thousands of kilometers away from the fires. The aerosols can aid in cloud development while at the same time, have variable impacts on the amount of solar radiation reaching the surface and returning to space which can cause either warming or cooling along their transport pathway. In the Southern Hemisphere tropics, there are few observations to document aerosol radiative forcing impacts on global climate. This study uses short‐term and long‐term measurements of aerosol physical properties in conjunction with meteorological analysis to diagnose the impact of smoke aerosols on incoming solar radiation and cloud development during transport. Key Points: African biomass burning smoke plumes feature highly variable top of the atmosphere and BOA radiative forcing efficiencies when mixed with marine aerosolsSmoke aerosols with stronger radiative forcing efficiencies present a cooling effect which can stabilize the marine boundary layerLonger back trajectories suggest aging of smoke aerosols and mixing with marine aerosols which facilitate cloud development [ABSTRACT FROM AUTHOR]

Understanding the driving factors for the change of climatic patterns is crucial for the implementation of mitigation and adaptation measures. Significant effort has been made to understand changes in climatic patterns; however, less has been done to investigate the driving factors that influence the trends of early rainfall over Malawi. Hence, a substantial research gap exists concerning in the implementation of mitigation and adaptation measures. The present study investigates the implications of atmospheric aerosols on precipitation during the early rainfall season over Malawi. Open burning, such as bushfires and burning of crop residues by local farmers, are the major anthropogenic activities enhancing aerosol accumulation in the atmosphere and hence need to be strictly controlled over the domain and the surrounding region. The present results show that rainfall generally starts between October and November and gradually increases with the maximum observed in January and ends in March in most areas. Monthly aerosol optical depth (AOD550) has an opposite pattern to that of rainfall with high AOD550 (>0.4) between September and October, mostly over southern areas and along with Lake Malawi. An analysis of rainfall during the beginning of the season indicates a significant decrease of rainfall over the southern areas of Malawi, associated with high AOD550, while insignificant change is observed over the central and northern areas associated with low AOD550 values. Statistical analyses among AOD550, cloud effective radius (CER), and precipitation demonstrates that negative trends of rainfall are strongly associated with a high concentration of anthropogenic aerosols from biomass burning during October. These aerosols might have absorbed excess moisture and disrupted local convective processes associated with the first rainfall that the domain receives, between the months of October and November. Therefore, regional control measures are required to reduce the excess emissions of anthropogenic aerosols into the atmosphere, such as controlling open burning during the active fire period (July-October). [ABSTRACT FROM AUTHOR]

Abstract Biomass burning smoke aerosols are efficient at attenuating incoming solar radiation. The Layered Atlantic Smoke Interactions with Clouds campaign was conducted from June 2016 to October 2017. The U. S. Department of Energy mobile Atmospheric Radiation Measurement site located on Ascension Island (AMF‐ASI) identified several instances of smoke plume intrusions. Increases in surface and column measurements of aerosol loading were directly related to increases in fine mode fraction, number concentrations of aerosols (Na), and cloud condensation nuclei (NCCN). During periods of weak lower tropospheric stability, smoke particles were more likely to be advected downward either by boundary layer turbulence or cloud top entrainment under non‐overcast sky conditions. Backward trajectory analysis illustrated that smoke aerosols reaching the AMF‐ASI site were fine mode, less aged, strongly absorbing, and had shorter boundary layer trajectories while longer boundary layer trajectories denoted mixtures of weakly absorbing smoke and coarse mode marine aerosols. The most polluted smoke cases of August 2016 and 2017 revealed a notable contrast in radiative forcing per unit aerosol optical depth or radiative forcing efficiency (ΔFeff) at the top of the atmosphere (TOA) and near‐surface (BOA). The weakly (strongly) absorbing 2016 cases exhibited weaker (stronger) ΔFeff at the TOA and BOA suggesting a warming (cooling) effect within the boundary layer. The 2017 cases featured the strongest ΔFeff suggesting more of a cooling effect at the TOA and BOA due to mixing of fresh smoke with marine aerosols during transport.

The fractal dimension is a key parameter in quantifying the morphology of aerosol aggregates, which is necessary to understand their radiative impact. Here we used Transmission Electron Microscopy (TEM) images to determine 2D fractal dimensions using the nested square and box-grid method and used two different empirical equations to obtain the 3D fractal dimensions. The values ranged from 1.70 ± 0.05 for pine to 1.82 ± 0.07 for Eucalyptus, with both methods giving nearly identical results using one of the empirical equations and the other overestimated the 3D values significantly when compared to other values in the literature. The values we obtained are comparable to the fractal dimensions of fresh aerosols in the literature and were dependent on fuel type and combustion condition. Although these methods accurately calculated the fractal dimension, they have shortcomings if the images are not of the highest quality. While there are many ways of determining the fractal dimension of linear features, we conclude that the application of every method requires careful consideration of a range of methodological concerns. [ABSTRACT FROM AUTHOR]

Physicochemical and toxicological properties of biomass burning are of great importance for the assessment of the impacts of wildfires on the environment. However, the data on Siberian wildfires are limited. The composition of aerosols originating during Siberian biomass burning is studied in the Large Aerosol Chamber (LAC) of the Institute of Atmospheric Optics, Siberian Branch, Russian Academy of Sciences, Tomsk. In this work, we study the composition of organic compounds in Siberian pine and forest debris smoke produced during smoldering and flaming phases and aging with the use of FTIR spectroscopy, gas chromatography-mass spectrometry, and liquid chromatography. Markers which allow identifying the combustion conditions and biomass type are suggested, namely, characteristic absorption bands, ratios of carboxyl and aliphatic functionalities, and diagnostic ratios of polycyclic aromatic hydrocarbons (PAHs). Emission factors and carcinogenic risk of smoke PAHs are estimated. [ABSTRACT FROM AUTHOR]

Increased wildfire events constitute a significant threat to life and property in the United States. Wildfire impact on severe storms and weather hazards is another pathway that threatens society, and our understanding of which is very limited. Here, we use unique modeling developments to explore the effects of wildfires in the western US (mainly California and Oregon) on precipitation and hail in the central US. We find that the western US wildfires notably increase the occurrences of heavy precipitation rates by 38% and significant severe hail (≥2 in.) by 34% in the central United States. Both heat and aerosols from wildfires play an important role. By enhancing surface high pressure and increasing westerly and southwesterly winds, wildfires in the western United States produce (1) stronger moisture and aerosol transport to the central United States and (2) larger wind shear and storm-relative helicity in the central United States. Both the meteorological environment more conducive to severe convective storms and increased aerosols contribute to the enhancements of heavy precipitation rates and large hail. Moreover, the local wildfires in the central US also enhance the severity of storms, but their impact is notably smaller than the impact of remote wildfires in California and Oregon because of the lessened severity of the local wildfires. As wildfires are projected to be more frequent and severe in a warmer climate, the influence of wildfires on severe weather in downwind regions may become increasingly important. [ABSTRACT FROM AUTHOR]

In the present study, we present the aerosol optical properties and radiative forcing (RF) of the tropospheric and stratospheric smoke layers, observed by the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) satellite, during the extraordinary Australian biomass burning (BB) event in 2019–2020. These BB layers were studied and analyzed within the longitude range 140° E–20° W and the latitude band 20°–60° S, as they were gradually transported from the Australian banks to the South American continent. These layers were found to be trapped within the Andes circulation, staying for longer time periods in the same longitude region. The BB aerosols reached altitudes even up to 22 km amsl., and regarding their optical properties, they were found to be nearly spherical (particle linear depolarization ratio (PLDR) < 0.10) in the troposphere; while, in the stratosphere, they were more depolarizing with PLDR values reaching up to 0.20. Fine and ultrafine smoke particles were dominant in the stratosphere, according to the observed Ångström exponent, related to the backscatter coefficients obtained by the pair of wavelengths 532 and 1064 nm (Åb up to 3), in contrast to the Åb values in the troposphere (Åb < 1) indicative of the presence of coarser particles. As the aerosols fend off the source, towards North America, a slightly descending trend was observed in the tropospheric Åb values, while the stratospheric ones were lightly increased. A maximum aerosol optical depth (AOD) value of 0.54 was recorded in the lower troposphere over the fire spots, while, in the stratosphere, AOD values up to 0.29 were observed. Sharp changes of carbon monoxide (CO) and ozone (O3) concentrations were also recorded by the Copernicus Atmosphere Monitoring Service (CAMS) in various atmospheric heights over the study region, associated with fire smoke emissions. The tropospheric smoke layers were found to have a negative mean radiative effect, ranging from −12.83 W/m2 at the top of the atmosphere (TOA), to −32.22 W/m2 on the surface (SRF), while the radiative effect of the stratospheric smoke was estimated between −7.36 at the TOA to −18.51 W/m2 at the SRF. [ABSTRACT FROM AUTHOR]

The fractal dimension is a key parameter in quantifying the morphology of aerosol aggregates, which is necessary to understand their radiative impact. Here we used Transmission Electron Microscopy (TEM) images to determine 2D fractal dimensions using the nested square and box-grid method and used two different empirical equations to obtain the 3D fractal dimensions. The values ranged from 1.70 ± 0.05 for pine to 1.82 ± 0.07 for Eucalyptus, with both methods giving nearly identical results using one of the empirical equations and the other overestimated the 3D values significantly when compared to other values in the literature. The values we obtained are comparable to the fractal dimensions of fresh aerosols in the literature and were dependent on fuel type and combustion condition. Although these methods accurately calculated the fractal dimension, they have shortcomings if the images are not of the highest quality. While there are many ways of determining the fractal dimension of linear features, we conclude that the application of every method requires careful consideration of a range of methodological concerns.

• Warmer, drier weather due to climate change increases the risk of large wildfires. • Unprecedently large wildfires broke out earlier than the usual forest fire season. • Wildfires increased PM 2.5 by more than 20 times and CO by 4–12 times more than usual. • Biomass burning aerosols have a high fraction of PM 1.0 , contributing 95.7 % to PM 2.5. • Climate change makes fire-prone conditions and causes more severe fires than before. In March 2022, three weeks earlier than the usual forest fire season, a wildfire of unprecedented scale broke out in South Korea, spreading rapidly over a large forest area and burning 22,477 hectares in two weeks. This event was likely related to climate change; however, the relevance of climate change in the occurrence of such large fire events is not yet clearly understood. In this study, we assessed how climate change affects the regional climate and the extent to which it enhances the potential risk of wildfires based on the analysis of long-term meteorological observation data from 1923 to 2022 and the calculation of fire weather indices (FWIs). Results showed that the climate regime has shifted from cold and wet to warm and dry winters, with this shift involving a 4 °C increase in temperature, an 8 % decrease in relative humidity, and a 17 mm decrease in precipitation. Dry winter weather has become increasingly severe, resulting in extreme drought in winter 2021 and early spring 2022, with the FWI calculations revealing great potential dangers from fires. However, no major fires were reported in 2021, which is attributable to a reduction in accidental ignition sources owing to the restrictions on human activity caused by the COVID-19 pandemic. This demonstrates the importance of managing artificial ignition. The 2022 wildfires produced substantial quantities of ultrafine aerosols, which consisted mainly of particles smaller than 1.0 µm. These particles have raised the level of air pollution by more than 20 times compared to before the fires. The CO concentrations were also found to be 4 to 12 times higher than the typical local background concentrations. This study highlights that climate change may make forests more vulnerable to fire in temperate and mid-latitude monsoon-affected regions, where large-scale wildfires were not previously a concern. [Display omitted] [ABSTRACT FROM AUTHOR]

The impacts of vertical distribution of biomass burning (BB) emissions on aerosol distributions and direct radiative effects over the BB source regions of Mainland Southeast Asia (MSEA) and downwind East Asian regions during spring (March to May) 2019 were investigated by applying an online coupled regional chemistry-aerosol-climate model (RIEMS-Chem). Model validation against a variety of observations demonstrated a generally good skill of the model in simulating aerosol chemical components, aerosol optical depth (AOD), and vertical distribution of aerosol extinction coefficient (EXT) when BB emissions were included. Four methods were adopted to represent injection height of BB emissions, including (1) a physical process-based parameterization (BB_param), (2) satellite-based prescribed profiles (BB_prof), (3) temporal-spatial varied injection profiles from the GFAS (Global Fire Assimilation System) dataset (BB_GFAS), and (4) BB emissions released at a fixed altitude (BB_high). The BB_param experiment generally produced better statistics compared to observations. Different BB injection height treatments considerably affected concentrations and distributions of BB aerosols, aerosol optical properties, direct radiative effects of BB aerosols (DRE BB), atmospheric heating rate, and cloud fractions. The simulated sub-regional (100–120°E and 19–26°N, including major BB source and downwind areas) and seasonal mean DRE BB at the top of the atmosphere (TOA) were +1.7 W m−2, +1.3 W m−2, +1.2 W m−2, and +1.7 W m−2 in the BB_param, BB_prof, BB_GFAS, and BB_high experiments, respectively, while the corresponding mean DRE BB at the surface were −30.3 W m−2, -19.1 W m−2, -19.0 W m−2, and -22.1 W m−2. It is noticed that the DRE BB at TOA and at the surface in BB_GFAS were just 68% and 63% of the values in BB_param, and the different injection height treatment had larger influences on DRE BB at the surface than at TOA. The BB aerosol-induced atmospheric heating rate was up to 0.8–1.2 K/day in BB_param, which was larger than those in other experiments. Low cloud was enhanced while middle and high clouds were reduced by BB aerosols over northern MSEA. The BB aerosol-induced changes in cloud fractions in the BB_param experiment (up to 0.15 for low cloud and −0.05 for middle and high cloud) were approximately twice those in the other experiments. This study demonstrates the importance and necessity of properly representing the injection height of BB emissions in model estimation of radiative and climatic effects of BB aerosols. [Display omitted] • The direct radiative effects of four methods for BB injection height were explored. • Surface direct radiative effect of BB aerosols varied from −19 to −30 W m-2 among the methods. • BB aerosols induced the largest HR of 0.8–1.2 K/day at 3–5 km by the physically based method. • The BB aerosol-induced changes in cloud fraction with these methods varied by a factor of two. [ABSTRACT FROM AUTHOR]

Black carbon emitted from incomplete combustion of biomass and fossil fuel burning is an important aerosol; however, available long-term black carbon data are limited to remote polar and high-alpine ice cores from few geographic regions. Black carbon records from lake sediments fill geographic gaps but such records are still scarce, particularly in the Southern Hemisphere. We applied a new incandescence-based methodology to develop Holocene refractory black carbon (rBC) records from four lake-sediment archives in New Zealand and compare these with macroscopic charcoal records. Our rBC records suggest periods with substantial rBC deposition during the Holocene before human arrival in the 13th century reflecting long-range transport and possibly local wetland fires. With Polynesian settlement, rBC deposition increased on the South Island in agreement with macroscopic charcoal records, and it is this period of burning that is proposed as the source of rBC increases evident in Antarctic ice cores. However, sites on the North Island show no contemporaneous rBC increase suggesting regional differences in biomass burning patterns between the North and South islands. None of the New Zealand records show an increase in rBC from fossil fuel sources during the Industrial Era post-1850 CE. • Refractory black carbon (rBC) links lake sediment and ice core fire record. • New Zealand lake-sediment rBC suggests fire activity before human arrival. • Regional patterns of past rBC differ between the South and North Island. • rBC from the South Island contributed to Antarctic rBC increase. • New Zealand lake sediments show no rBC signal from fossil fuel sources. [ABSTRACT FROM AUTHOR]

In the present study, we present the aerosol optical properties and radiative forcing (RF) of the tropospheric and stratospheric smoke layers, observed by the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) satellite, during the extraordinary Australian biomass burning (BB) event in 2019–2020. These BB layers were studied and analyzed within the longitude range 140° E–20° W and the latitude band 20°–60° S, as they were gradually transported from the Australian banks to the South American continent. These layers were found to be trapped within the Andes circulation, staying for longer time periods in the same longitude region. The BB aerosols reached altitudes even up to 22 km amsl., and regarding their optical properties, they were found to be nearly spherical (particle linear depolarization ratio (PLDR) < 0.10) in the troposphere; while, in the stratosphere, they were more depolarizing with PLDR values reaching up to 0.20. Fine and ultrafine smoke particles were dominant in the stratosphere, according to the observed Ångström exponent, related to the backscatter coefficients obtained by the pair of wavelengths 532 and 1064 nm (Åb up to 3), in contrast to the Åb values in the troposphere (Åb < 1) indicative of the presence of coarser particles. As the aerosols fend off the source, towards North America, a slightly descending trend was observed in the tropospheric Åb values, while the stratospheric ones were lightly increased. A maximum aerosol optical depth (AOD) value of 0.54 was recorded in the lower troposphere over the fire spots, while, in the stratosphere, AOD values up to 0.29 were observed. Sharp changes of carbon monoxide (CO) and ozone (O3) concentrations were also recorded by the Copernicus Atmosphere Monitoring Service (CAMS) in various atmospheric heights over the study region, associated with fire smoke emissions. The tropospheric smoke layers were found to have a negative mean radiative effect, ranging from −12.83 W/m2 at the top of the atmosphere (TOA), to −32.22 W/m2 on the surface (SRF), while the radiative effect of the stratospheric smoke was estimated between −7.36 at the TOA to −18.51 W/m2 at the SRF.

Previous evaluations of simulated aerosol transport over the south‐east Atlantic by global aerosol models, including the Goddard Earth Observing System (GEOS) atmospheric general circulation model, showed that the bulk of the modeled smoke aerosol layer resided ~1–2 km lower than Cloud‐Aerosol Lidar with Orthogonal Polarization (CALIOP) lidar observations. Using this finding as the motivation, this study examines the changes in model‐simulated cloud properties in response to redistributing the vertical placement of the aerosol over the ocean. Ten years (2006–2015) of CALIOP‐retrieved smoke aerosol extinction profiles were used to redistribute the model‐simulated aerosol mass on a monthly mean basis, keeping the column aerosol mass conserved. The results from the model sensitivity experiments show that elevating the aerosol layer to higher levels in agreement with CALIOP observations causes an increase in cloud fractions by ~33% for shallow marine boundary layers (MBL) and a decrease by ~30% for deeper MBL. For a shallow MBL, aerosol‐induced warming within the cloud layers for the lower altitude aerosol case decreases relative humidity at these levels and leads to a reduction of overall cloud amount compared to the elevated aerosol case. For a deeper MBL, however, aerosol heating within the upper cloud levels in the lower altitude aerosol case increases the underlying MBL stability, which suppresses the cloud vertical extent, enhances cloud cover, and delays the stratocumulus to cumulus transition. Finally, aerosol redistribution impacts on radiative forcing are investigated, which appear to be mainly driven by the changes in cloud area fractions rather than in‐cloud liquid water path changes between the model experiments. Key Points: Model cloud responses to aerosol‐radiation interactions strongly depend on the vertical placement of smoke with respect to the cloudsFor shallow stratocumulus, aerosol‐induced warming within the clouds reduces cloud amounts by decreasing relative humidityFor deeper stratocumulus, increase in stability due to aerosol heating overwhelms cloud burn‐off and delays its transition to cumulus [ABSTRACT FROM AUTHOR]

Mean optical and microphysical aerosol properties of long-range transported biomass burning (BB) particles and mixtures are presented from a 9-year (2011–2019) data set of multiwavelength Raman lidar data, obtained by the EOLE lidar over the city of Athens (37.58° N, 23.47° E), Greece. We studied 34 aerosol layers characterized as: (1) smoke; (2) smoke + continental polluted, and (3) smoke + mixed dust. We found, mainly, small-sized aerosols with mean backscatter-related (355 nm/532 nm, 532 nm/1064 nm) values and Ångström exponent (AE) values in the range 1.4–1.7. The lidar ratio (LR) value at 355 nm was found to be 57 ± 10 sr, 51 ± 5 sr, and 38 ± 9 sr for the aerosol categories (1), (2), and (3), respectively; while at 532 nm, we observed LR values of 73 ± 11 sr, 59 ± 10 sr, and 62 ± 12 for the same categories. Regarding the retrieved microphysical properties, the effective radius (reff) ranged from 0.24 ± 0.11 to 0.24 ± 0.14 μm for all aerosol categories, while the volume density (vd) ranged from 8.6 ± 3.2 to 20.7 ± 14.1 μm−3cm−3 with the higher values linked to aerosol categories (1) and (2); the real part of the refractive index (mR) ranged between 1.49 and 1.53, while for the imaginary part (mI), we found values within 0.0108 i and 0.0126 i. Finally, the single scattering albedo (SSA) of the propped particles varied from 0.915 to 0.936 at all three wavelengths (355–532–1064 nm). The novelty of this study is the provision of typical values of BB aerosol properties from the UV to the near IR, which can be used in forecasting the aerosol climatic effects in the European region.

In this paper, we have applied an extensive back-trajectory calculation to describe a complex atmospheric circulation pattern in the Central Mediterranean, registered in late spring 2013, which led to successive advections of biomass burning and Saharan dust aerosols over Italy. We based our study on chemical results obtained at the two background Italian sites of Monte Martano and Lampedusa. The two sites feature different local aerosol sources and are geographically distant. In order to distinguish the contribution of long-range sources associated with the advection event, we set up a potential source contribution function analysis of the chemical composition of PM10 sampled at both sites. The main goal was to individuate the variability of the aerosol composition associated with the long-range transport and to trace back the source areas. We discussed the case of study in the context of the unusual synoptic meteorological conditions during the observational period. The wide geographical scale covered in this study allowed us to explore the extent to which an aerosol intrusion from Eastern Europe may impact on the Central Mediterranean. Also, we pointed out how a sudden shift of the synoptic meteorological conditions can induce, in a few days, a complete change in the chemistry of airborne dust, due to a contribution from Sahara, which was more significant in Central Italy with respect to lower latitudes. [ABSTRACT FROM AUTHOR]

In this paper, we present long-term observations of the multiwavelength Raman lidar PollyXT conducted in the framework of the DACAPO-PESO campaign. Regardless of the relatively clean atmosphere in the southern mid-latitude oceans region, we regularly observed events of long-range transported smoke, originating either from regional sources in South America or from Australia. Two case studies will be discussed, both identified as smoke events that occurred on 5 February 2019 and 11 March 2019. For the first case considered, the lofted smoke layer was located at an altitude between 1.0 and 4.2 km, and apart from the predominance of smoke particles, particle linear depolarization values indicated the presence of dust particles. Mean lidar ratio values at 355 and 532 nm were 49 ± 12 and 24 ± 18 sr respectively, while the mean particle linear depolarization was 7.6 ± 3.6% at 532 nm. The advection of smoke and dust particles above Punta Arenas affected significantly the available cloud condensation nuclei (CCN) and ice nucleating particles (INP) in the lower troposphere, and effectively triggered the ice crystal formation processes. Regarding the second case, the thin smoke layers were observed at altitudes 5.5–7.0, 9.0 and 11.0 km. The particle linear depolarization ratio at 532 nm increased rapidly with height, starting from 2% for the lowest two layers and increasing up to 9.5% for the highest layer, indicating the possible presence of non-spherical coated soot aggregates. INP activation was effectively facilitated. The long-term analysis of the one year of observations showed that tropospheric smoke advection over Punta Arenas occurred 16 times (lasting from 1 to 17 h), regularly distributed over the period and with high potential to influence cloud formation in the otherwise pristine environment of the region.

In this paper the authors discuss the changes of aerosol optical depth (AOD) in the region of eastern Europe and the Baltic Sea due to wild fire episodes which occurred in the area of Belarus and Ukraine in 2002. The authors discuss how the biomass burning aerosols were advected over the Baltic area and changed the composition of aerosol ensemble for a period of several summer weeks. The air pressure situation and slow wind speeds also facilitated the development of such conditions. As a consequence very high AOD levels were recorded, by an order of 3–4 higher versus normal conditions and they significantly increased the annual averages. On particular days of August 2002 the AOD values reached a level of over 0.7. On these days fine particles fully dominated the entire ensemble of aerosol particles. They were either sulfates or smoke particles. Such situation was unique over a period of many years and it had its serious consequences for the region and especially for the Baltic Sea.

Biomass burning (BB) aerosols contribute to climate forcing, but much is still unknown about the extent of this forcing, owing partially to the high level of uncertainty regarding BB aerosol optical properties. A key optical parameter is the refractive index (RI), which influences the absorbing and scattering properties of aerosols. This quantity is not measured directly, but it is obtained by fitting the measured scattering cross section and extinction cross section to a theoretical model using the RI as a fitting parameter. We used the Rayleigh−Debye−Gans (RDG) approximation to retrieve the complex RI of freshly emitted BB aerosol from two fuels (eucalyptus and olive) from Africa in the spectral range of 500−580 nm. Experimental measurements were carried out using cavity ring-down spectroscopy to measure extinction over the range of wavelengths of 500−580 nm and nephelometry to measure scattering at three wavelengths of 450, 550, and 700 nm for size-selected BB aerosol particles. The fuels were combusted in a tube furnace at a temperature of 800 °C, which is representative of the flaming stage of burning. Filter samples were collected and imaged using tunneling electron microscopy to obtain information on the morphology and size of the particles, which was used in the RDG calculations. The mean radii of the monomers were 27.8 and 31.5 nm for the eucalyptus and the olive fuels, respectively. The components of the retrieved complex RI were in the range of 1.31 ≤ n ≤ 1.56 and 0.045 ≤ k ≤ 0.468. The real and complex parts of the RI increase with increasing particle mobility diameter. The real part of the RI is lower, and the imaginary part is higher than what was recommended in literature for black carbon generated by propane or field measurements from fires of mixed wood samples. Fuel dependent results from controlled laboratory experiments can be used in climate modeling efforts and to constrain field measurements from biomass burning.

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. [ABSTRACT FROM AUTHOR]

Abstract: A coupled weather‐aerosol model is used to study the effect of biomass burning aerosols on deep convection over the Borneo Island and surrounding oceans. Simulations are performed at the convection‐permitting scale (4 km) for 40 days during the boreal summer and include interactive fire emissions and the aerosol effect on radiative and microphysical processes. Intense burning occurs daily in the southern part of the island, and smoke propagates northward to regions of deep convection. The model captures well the observed diurnal cycle of precipitation and high cloud cover. Cloud microphysics and radiative aerosol impacts are considered separately. Modifications of the cloud microphysics by smoke aerosols reinforce deep convection near the central Borneo mountainous region. This reinforced convection is due to reduced shallow precipitation in the afternoon that leads to a warm planetary boundary layer anomaly at sunset enhancing deep convection at night. Aerosol absorptive properties strongly affect local and synoptic atmospheric responses. The radiative processes of moderately absorbing aerosols tend to reduce deep convection over most regions due to local surface cooling and atmosphere warming that increase the static stability. For more absorbing aerosols, however, the impact is reversed with increased nighttime convection over most regions. This is partly related to changes in the vertical water vapor divergence profiles that decrease the convergence toward Borneo for moderately absorbing aerosols and increase it for more absorbing ones. These changes in the synoptic circulation due to large‐scale aerosol perturbations are as important as local processes to explain the observed rainfall perturbation patterns. [ABSTRACT FROM AUTHOR]

The refractive index (RI) is an important parameter in describing the radiative impacts of aerosols. It is important to constrain the RI of aerosol components, since there is still significant uncertainty regarding the RI of biomass burning aerosols. Experimentally measured extinction cross-sections, scattering cross-sections, and single scattering albedos for white pine biomass burning (BB) aerosols under two different burning and sampling conditions were modeled using T-matrix theory. The refractive indices were extracted from these calculations. Experimental measurements were conducted using a cavity ring-down spectrometer to measure the extinction, and a nephelometer to measure the scattering of size-selected aerosols. BB aerosols were obtained by burning white pine using (1) an open fire in a burn drum, where the aerosols were collected in distilled water using an impinger, and then re-aerosolized after several days, and (2) a tube furnace to directly introduce the BB aerosols into an indoor smog chamber, where BB aerosols were then sampled directly. In both cases, filter samples were also collected, and electron microscopy images were used to obtain the morphology and size information used in the T-matrix calculations. The effective radius of the particles collected on filter media from the open fire was approximately 245 nm, whereas it was approximately 76 nm for particles from the tube furnace burns. For samples collected in distilled water, the real part of the RI increased with increasing particle size, and the imaginary part decreased. The imaginary part of the RI was also significantly larger than the reported values for fresh BB aerosol samples. For the particles generated in the tube furnace, the real part of the RI decreased with particle size, and the imaginary part was much smaller and nearly constant. The RI is sensitive to particle size and sampling method, but there was no wavelength dependence over the range considered (500-680 nm). Our values for the RI of fresh (white pine) biomass burning aerosols ranged from 1.33 + i0.008 to 1.74 + i0.008 for 200-nm, 300-nm, and 400-nm diameter particles. These are within the range of RI values in the most recent study conducted during the Fire Laboratory at Missoula Experiments (FLAME I and II), which were 1.55 to 1.80 for the real part, and 0.01-0.50 for the imaginary part, for fresh BB aerosols with diameters of 200-570 nm. There is no clear trend on the dependence of the RI values on particle size. The RI values derived from measurements of aerosols produced from the combustion of hydrocarbons and diesel cannot be used for BB aerosols. [ABSTRACT FROM AUTHOR]

Southeast Asia (SEA) biomass-burning could exert considerable influences on air quality and stability in the Guangdong-Hong Kong-Macao Great Bay Area (GBA) through long-range transport, while such impacts were typically quantified with numerical modeling which may suffer uncertainties in emissions and model parameterizations. Here we present an observation-based method to quantify such influences of SEA biomass-burning by analyzing 2009–2019 satellite-observed aerosol vertical structure which has enough data records to distinguish the conditions with or without severe biomass-burning impacts based on fire point counts in SEA. Results suggest that the observation-based method successfully captured the SEA biomass-burning days in spring, excluding the irrelevant days as more as possible and avoiding underestimation. Substantial increase of aloft AOD (by 0.21) in GBA is found during the severe SEA biomass-burning days comparing to less severe days, suggesting the enhanced aerosol loading in GBA contributed from the SEA biomass burning. Meanwhile, the near-surface particle size in GBA was increased (CR from 0.606 to 0.673) during severe SEA biomass-burning days, which is opposite to that for the aloft particle size which was decreased (CR from 0.693 to 0.621) driven by the small aerosols originated from biomass-burning SEA. Such phenomenal might be associated with the enhancement of atmospheric static stability in GBA (N2 from 1.34 × 10−4 s−2 to 1.66 × 10−4 s−2) as the abundant aloft aerosols transported from SEA modulates the aerosol vertical structure and associate radiative effects and atmospheric dynamic, results in enhanced aging processes and aerosol particle aggregation under weak ventilation condition. Further, the air pollution in GBA is also aggravated due to the reduced ventilation driven by the enhanced aerosol radiative effects associated with the transported aerosols, as the surface PM 2.5 concentrations were increased by 17% (from 29.27 μg /m3 to 34.15 μg /m3) during severe biomass-burning days. Such results demonstrate that our observation-based method with abundant satellites-retrieved aerosol vertical structure information can successfully quantify the influences of SEA biomass-burning on aerosol–radiation interactions and local air pollution over the GBA, which can also be applied in other regions to identify the influences of local sources and regional transport pollution. • CALIPSO-observed aerosol vertical structure reveals the influences of SEA biomass burning on GBA • GBA suffers SEA biomass burning influences during almost half of biomass-burning season. • Particle sizes in GBA decrease at aloft but increase near surface due to SEA biomass-burning fires • Imported aerosol from SEA increased atmospheric stability and air pollution in GBA [ABSTRACT FROM AUTHOR]

As an important source of pollutants in Beijing, biomass burning (BB) aerosols emitted by BB have a strong absorption and scattering effect on surface solar radiation (SSR). However, the existence of meteorological factors has a powerful impact on the estimation of the BB aerosol radiation effect. In this paper, a deweathered technique based on machine learning is presented to quantitatively isolate the influence of weather conditions from the radiative effect of BB aerosols. Furthermore, the seasonal trend of SSR is constrained by removing the general seasonal changes by the detrending method. The BB event on October 7–11, 2014, in Beijing was used as a case to validate the effectiveness of the proposed method. Experimental results show that meteorological factors aggravate the influence of BB events on SSR. Specifically, during the BB event, meteorological factors led to an additional increase of 10.9% in diffuse radiation and an additional decrease of 17.5%, 13.1%, 181.3%, 9.7% and 86.9% in global radiation, net radiation, horizontal direct radiation, reflected radiation and vertical direct radiation, respectively. After isolating the impact of meteorological factors on SSR in the BB event, we found that the average effects of BB aerosols on global radiation, net radiation, diffuse radiation, horizontal direct solar radiation, reflected radiation and vertical direct solar radiation during the BB event were −35.6 Wm−2 (−3.1 MJm−2day−1), −14.1 Wm−2 (−1.2 MJm−2day−1), 20.7 Wm−2 (1.8 MJm−2day−1), −67.3 Wm−2 (−5.8 MJm−2day−1), −8.9 Wm−2 (−0.8MJm−2day−1), and −132.9 Wm−2 (−11.5 MJm−2day−1), respectively. In conclusion, the weather normalization and detrended methods in this study provide a new idea for the accurate estimation of the impact of aerosols on SSR. This provides a quantitative reference for further understanding the impacts of atmospheric pollution on SSR. • The impact of meteorology on surface solar radiation is decoupled by weather normalization. • The seasonal trend of surface solar radiation in this study is removed by the detrending method. • The diffuse radiation increased up to 20.7 Wm−2 during the biomass burning (BB) event. • The global radiation decreased by 36.5 Wm−2 due to BB aerosols. [ABSTRACT FROM AUTHOR]

A smoke plume originating from the massive wildfires near Moscow was clearly detected in northern Finland on 30 July 2010. Measurements made with remote sensing instruments demonstrated how the biomass burning aerosols affected the chemical and optical characteristics of the atmosphere in regions hundreds of kilometers away from the actual fires. In this study, we used MODIS, AIRS, CALIOP, PFR, ceilometers, FTS and Brewer data to quantify the properties of the transported smoke plume. In addition, in situ measurements of aerosol concentration (DMPS), absorption (aethalometer) and scattering (nephelometer) are presented. We found that due to the smoke plume in northern Finland, the daily averaged optical thickness of aerosols increased fourfold, and MODIS retrieved AOD as high as 4.5 for the thickest part of the plume. FTS measurements showed that CO concentration increased by 100% during the plume. CALIOP and ceilometer measurements revealed that the smoke plume was located close to the surface, below 3 km, and that the plume was not homogeneously mixed. In addition, in situ measurements showed that the scattering and absorption coefficients were almost 20 times larger in the smoke plume than on average, and that the number of particles larger than 320 nm increased 14-fold. Moreover, a comparison with in situ measurements recorded in eastern Finland on the previous day showed that the transport from eastern to northern Finland decreased the scattering coefficient, black carbon concentration, and total number concentration 0.5%/h, 1.5%/h and 2.0%/h, respectively.

The purpose of this study is to evaluate the strength of the near-UV wavelength of 380 nm relative to visible and near-IR bands, and to find the suitable wavelength for detecting aerosols by using the Global Imager (GLI) sensor aboard the Advanced Earth Observing Satellite-II (ADEOS-II). Sensitivity analysis is performed for the retrieval of biomass burning aerosols by employing the radiative transfer model Rstar5b. It is determined that background surface reflectance in the blue band is similar to that in the near-UV band, and that wavelengths in the blue bands are more sensitive to the Aerosol Optical Thickness (AOT) than wavelengths in the near-UV band. The Total Ozone Mapping Spectrometer (TOMS) Aerosol Index (AI) is used in the indirect method used for aerosol retrieval, and the wavelength pair 380 nm and 460 nm is determined to be the most sensitive to the AOT. The results of this study suggest that wavelengths in the blue bands are suitable for detecting biomass burning aerosols over the Korean peninsula.

We examine the 2002 Yakutsk wildfire event and simulate the impacts of smoke aerosols on local radiative energy budget, using the WRF-Chem-SMOKE model. When comparing satellite retrievals (the Surface Radiation Budget (SRB) dataset) with model simulations, we found that the agreement is generally good, except for the regions where the model predicts too few clouds or SRB misclassifies strong smoke plumes as clouds. We also found that the smoke-induced changes in upward shortwave fluxes at top of atmosphere (TOA) vary under different burning and meteorological conditions. In the first period of the fire season (9–12 August), smoke particles cause a warming effect around 3 W/m2, mainly through functioning as ice nuclei, which deplete the cloud water amount in the frontal system. At the beginning of the second period of the fire season (19–20 August), large amounts of pre-existing smoke particles cause a strong cooling effect of −8 W/m2. This is offset by the warming effect caused by relatively small amounts of cloud condensation nuclei increases, which promotes the rain formation and depletes the cloud water amount. After the cloud decks are well mixed with smoke plumes (21–22 August), the first indirect and direct effects of smoke together lead to a cooling of −10 W/m2. These results highlight the importance of meso-scale modeling efforts in estimating the smoke-induced changes in the radiative energy budget over high latitudes.

The refractive index (RI) is an important parameter in describing the radiative impacts of aerosols. It is important to constrain the RI of aerosol components, since there is still significant uncertainty regarding the RI of biomass burning aerosols. Experimentally measured extinction cross-sections, scattering cross-sections, and single scattering albedos for white pine biomass burning (BB) aerosols under two different burning and sampling conditions were modeled using T-matrix theory. The refractive indices were extracted from these calculations. Experimental measurements were conducted using a cavity ring-down spectrometer to measure the extinction, and a nephelometer to measure the scattering of size-selected aerosols. BB aerosols were obtained by burning white pine using (1) an open fire in a burn drum, where the aerosols were collected in distilled water using an impinger, and then re-aerosolized after several days, and (2) a tube furnace to directly introduce the BB aerosols into an indoor smog chamber, where BB aerosols were then sampled directly. In both cases, filter samples were also collected, and electron microscopy images were used to obtain the morphology and size information used in the T-matrix calculations. The effective radius of the particles collected on filter media from the open fire was approximately 245 nm, whereas it was approximately 76 nm for particles from the tube furnace burns. For samples collected in distilled water, the real part of the RI increased with increasing particle size, and the imaginary part decreased. The imaginary part of the RI was also significantly larger than the reported values for fresh BB aerosol samples. For the particles generated in the tube furnace, the real part of the RI decreased with particle size, and the imaginary part was much smaller and nearly constant. The RI is sensitive to particle size and sampling method, but there was no wavelength dependence over the range considered (500–680 nm). Our values for the RI of fresh (white pine) biomass burning aerosols ranged from 1.33 + i0.008 to 1.74 + i0.008 for 200-nm, 300-nm, and 400-nm diameter particles. These are within the range of RI values in the most recent study conducted during the Fire Laboratory at Missoula Experiments (FLAME I and II), which were 1.55 to 1.80 for the real part, and 0.01–0.50 for the imaginary part, for fresh BB aerosols with diameters of 200–570 nm. There is no clear trend on the dependence of the RI values on particle size. The RI values derived from measurements of aerosols produced from the combustion of hydrocarbons and diesel cannot be used for BB aerosols.

Organic aerosols (OA) are universally regarded as an important component of the atmosphere that have far-ranging impacts on climate forcing and human health. Many of these impacts are related to OA molecular characteristics. Despite the acknowledged importance, current uncertainties related to the source apportionment of molecular properties and environmental impacts make it difficult to confidently predict the net impacts of OA. Here we evaluate the specific molecular compounds as well as bulk structural properties of total suspended particulates in ambient OA collected from key emission sources (marine, biomass burning, and urban) using ultrahigh resolution mass spectrometry (UHR-MS) and proton nuclear magnetic resonance spectroscopy (¹H NMR). UHR-MS and ¹H NMR show that OA within each source is structurally diverse, and the molecular characteristics are described in detail. Principal component analysis (PCA) revealed that (1) aromatic nitrogen species are distinguishing components for these biomass burning aerosols; (2) these urban aerosols are distinguished by having formulas with high O/C ratios and lesser aromatic and condensed aromatic formulas; and (3) these marine aerosols are distinguished by lipid-like compounds of likely marine biological origin. This study provides a unique qualitative approach for enhancing the chemical characterization of OA necessary for molecular source apportionment. [ABSTRACT FROM AUTHOR]

Organic aerosol (OA) is one of the major components of fine atmospheric aerosol particles. Recent field campaigns and modeling studies in Colombia have demonstrated the presence of a large OA fraction in urban and rural aerosols. In this work we focus on constraining the sources associated with OA and its precursors over the city of Bogotá, Colombia. We used PM 2.5 chemical speciation data from field campaigns carried out during 2018 to evaluate the ability of a regional transport model to reproduce and explain the observed OA. The samples were collected at three sites during high- and low-aerosol concentration seasons in the region. We used The Weather Research and Forecasting Model coupled with Chemistry (WRF-Chem) with two different chemical mechanisms and aerosol schemes, RACM/MADE-VBS and MOZART/MOSAIC, in conjunction with the detailed in-situ aerosol chemical speciation observations to analyze the seasonality of OA in the city of Bogotá, and to establish the most relevant sources. Simulations were carried out for the same periods for which data is available, spanning a high biomass burning (BB) season (February 2018) and a low biomass burning season (September 2018). We demonstrated that long-range transport of BB emissions from Northern Amazonia can episodically increase aerosol loading during September, while BB activity in the Grasslands of the Orinoco River Basin are the main source during February. The two aerosol schemes utilized in this work reproduce the observed seasonal variations in total fine aerosol concentration, with a difference between February and September of 10 μ g m−3. The comparison between aerosol schemes demonstrated that MOZART/MOSAIC consistently predicted more OA with a larger SOA:OA ratio than in the RACM/MADE-VBS experiment. SOA dominates the OA fraction by 66% for RACM/MADE-VBS and 74% for MOZART/MOSAIC during February and 69% for RACM/MADE-VBS and 71% for MOZART/MOSAIC during September. These differences between organic aerosol burden between the mechanisms used in this study may be attributed to the different treatment of SOA gas/particle partitioning in the schemes. • WRF-Chem simulations and in-situ PM 2.5 chemical composition data were used to understand the contribution of OA over Bogotá. • Biomass burning plumes from Northern Amazonia and from the Orinoco River Grassland can severely impact the region. • Field data shows that OA contributes over 40% to PM 2.5 in the city. • The model underpredicts organic aerosols, with the MOZART/MOSAIC scheme predicting higher POA and SOA than RACM/MADE-VBS. [ABSTRACT FROM AUTHOR]

Increased wildfire events constitute a significant threat to life and property in the United States. Wildfire impact on severe storms and weather hazards is another pathway that threatens society, and our understanding of which is very limited. Here, we use unique modeling developments to explore the effects of wildfires in the western US (mainly California and Oregon) on precipitation and hail in the central US. We find that the western US wildfires notably increase the occurrences of heavy precipitation rates by 38% and significant severe hail (≥2 in.) by 34% in the central United States. Both heat and aerosols from wildfires play an important role. By enhancing surface high pressure and increasing westerly and southwesterly winds, wildfires in the western United States produce (1) stronger moisture and aerosol transport to the central United States and (2) larger wind shear and storm-relative helicity in the central United States. Both the meteorological environment more conducive to severe convective storms and increased aerosols contribute to the enhancements of heavy precipitation rates and large hail. Moreover, the local wildfires in the central US also enhance the severity of storms, but their impact is notably smaller than the impact of remote wildfires in California and Oregon because of the lessened severity of the local wildfires. As wildfires are projected to be more frequent and severe in a warmer climate, the influence of wildfires on severe weather in downwind regions may become increasingly important.

Organic aerosols (OA) are universally regarded as an important component of the atmosphere that have far-ranging impacts on climate forcing and human health. Many of these impacts are related to OA molecular characteristics. Despite the acknowledged importance, current uncertainties related to the source apportionment of molecular properties and environmental impacts make it difficult to confidently predict the net impacts of OA. Here we evaluate the specific molecular compounds as well as bulk structural properties of total suspended particulates in ambient OA collected from key emission sources (marine, biomass burning, and urban) using ultrahigh resolution mass spectrometry (UHR-MS) and proton nuclear magnetic resonance spectroscopy (1H NMR). UHR-MS and 1H NMR show that OA within each source is structurally diverse, and the molecular characteristics are described in detail. Principal component analysis (PCA) revealed that (1) aromatic nitrogen species are distinguishing components for these biomass burning aerosols; (2) these urban aerosols are distinguished by having formulas with high O/C ratios and lesser aromatic and condensed aromatic formulas; and (3) these marine aerosols are distinguished by lipid-like compounds of likely marine biological origin. This study provides a unique qualitative approach for enhancing the chemical characterization of OA necessary for molecular source apportionment.

The lifecycle of black carbon (BC)-containing particles from biomass burns is examined using aircraft and surface observations of the BC mixing state for plume ages from ∼15 min to 10 days. Because BC is nonvolatile and chemically inert, changes in the mixing state of BC-containing particles are driven solely by changes in particle coating, which is mainly secondary organic aerosol (SOA). The coating mass initially increases rapidly ( k growth = 0.84 h -1 ), then remains relatively constant for 1-2 days as plume dilution no longer supports further growth, and then decreases slowly until only ∼30% of the maximum coating mass remains after 10 days ( k loss = 0.011 h -1 ). The mass ratio of coating-to-core for a BC-containing particle with a 100 nm mass-equivalent diameter BC core reaches a maximum of ∼20 after a few hours and drops to ∼5 after 10 days of aging. The initial increase in coating mass can be used to determine SOA formation rates. The slow loss of coating material, not captured in global models, comprises the dominant fraction of the lifecycle of these particles. Coating-to-core mass ratios of BC particles in the stratosphere are much greater than those in the free troposphere indicating a different lifecycle.

Abstract: Size-resolved measurements of particulate matter (PM) emissions from 10 biomass materials (rice straw, soybean stem, green perilla stem, red pepper stem, pine needles, cherry leaves, cherry stem, maple leaves, gingko leaves and gingko stem) were conducted in a laboratory hood chamber environment using a 10-stage MOUDI. Samples were analyzed to determine the mass, water soluble organic carbon (WSOC), and water soluble inorganic species. This study examines how particle emissions and size distributions of chemical components vary with biomass materials. Mass fractions of water soluble organic mass (WSOM) (=1.6 × WSOC) and ionic species to the PM1.8 emissions varied significantly depending on the biomass type burned. The percent mass of WSOM in PM1.8 emissions ranged from 19.8% (green perilla stem) to 41.9% (red pepper stem) for agricultural crop residues, while the tree category accounted for 9.6% (gingko leaves) to 44.0% (gingko stem) of the PM1.8 emissions. Total ionic species contents in the PM1.8 mass ranged from 7.4% (rice straw) to 26.9% (green perilla stem) for the agricultural waste category, and 5.8% (maple leaves) to 23.5% (gingko stem) for the tree category. The ionic species fraction of the PM1.8 emission was dominated by K+, Cl−, and , while Ca2+ was important in the coarse mode particles (>3.1 μm). PM1.8 emissions of K+, Cl−, and were as high as 16.9%, 9.0%, and 5.8%, respectively, and were from the green perilla stem, red pepper stem, and gingko stem emissions. Normalized size distributions of mass, WSOC, K+, Cl−, , and oxalate in the biomass burning emissions showed a unimodal size distribution, peaking in the size ranges of 0.32–0.55 μm and 0.55–1.0 μm. Size-resolved PM mass fractions of WSOM, K+, Cl−, and showed fairly consistent distributions for each biomass type, with higher fractions in the ultrafine mode (<0.10 μm) and lower fractions in the accumulation mode of 0.32–1.0 μm. The size distributions of WSOC were strongly correlated (mostly R 2 > 0.90) with those of K+ in the particle size range of <0.1 μm and 0.1–1.8 μm and the biomass types. Strong correlations between the concentrations of K+–Cl− and were observed for the following size ranges; <0.1 μm, 0.1–1.0 μm, 1.0–1.8 μm, and 1.8–3.1 μm for most biomass burning emissions. Regression line slopes for K+/WSOC (i.e., mass of K+/mass of WSOC from biomass burning emissions) were not significantly changed for particle size and biomass type, but slopes for Cl−/K+ and /K+ varied significantly with the particle size (ultrafine, condensation, droplet, and coarse modes) and biomass type. [Copyright &y& Elsevier]

A smoke plume originating from the massive wildfires near Moscow was clearly detected in northern Finland on 30 July 2010. Measurements made with remote sensing instruments demonstrated how the biomass burning aerosols affected the chemical and optical characteristics of the atmosphere in regions hundreds of kilometers away from the actual fires. In this study, we used MODIS, AIRS, CALIOP, PFR, ceilometers, FTS and Brewer data to quantify the properties of the transported smoke plume. In addition, in situ measurements of aerosol concentration (DMPS), absorption (aethalometer) and scattering (nephelometer) are presented. We found that due to the smoke plume in northern Finland, the daily averaged optical thickness of aerosols increased fourfold, and MODIS retrieved AOD as high as 4.5 for the thickest part of the plume. FTS measurements showed that CO concentration increased by 100% during the plume. CALIOP and ceilometer measurements revealed that the smoke plume was located close to the surface, below 3 km, and that the plume was not homogeneously mixed. In addition, in situ measurements showed that the scattering and absorption coefficients were almost 20 times larger in the smoke plume than on average, and that the number of particles larger than 320 nm increased 14-fold. Moreover, a comparison with in situ measurements recorded in eastern Finland on the previous day showed that the transport from eastern to northern Finland decreased the scattering coefficient, black carbon concentration, and total number concentration 0.5%/h, 1.5%/h and 2.0%/h, respectively. [ABSTRACT FROM AUTHOR]

Abstract: Nitrogen-containing organic compounds in the atmosphere have drawn attention owing to their impact on aerosol chemistry and physics and their potential adverse effects on the biosphere. Among them, nitrocatechols and their homologs have recently been associated with biomass burning. In the present study, nitrocatechols, nitrophenols, nitroguaiacols and nitrosalicylic acids (NSAs) were simultaneously quantified for the first time by using a new analytical method based on liquid chromatography/tandem mass spectrometry, which was systematically optimized and validated. Several analyte specific issues regarding the sample preparation and chromatographic analysis were addressed in order to ensure method sensitivity, precision, and accuracy. Sample matrix effects were thoroughly investigated in order to ensure method specificity. The method was found to be sensitive with limits of detection ranging from 0.1 to 1.0μgL−1, and with accuracy generally between 90 and 104%. The relative standard deviations for repeatability and intermediate precision were better than 4% and 9%, respectively. The method was applied to the analysis of winter and summer PM10 samples from the city of Ljubljana, Slovenia. Aerosol concentrations as high as 152 and 134ngm−3 were obtained for the major aerosol nitro-aromatics: 4-nitrocatechol (4NC) and methyl-nitrocatechols (MNCs), respectively. Up to 500-times higher concentrations of 4NC and MNCs were found in winter compared to summer aerosols. The correlation analysis for winter samples showed that 4NC, MNCs, and NSAs are strongly inter-correlated (R 2 =0.84–0.96). Significant correlations between these analytes and anhydrosugars support their proposed origin from biomass burning. The studied nitro-aromatics were found to constitute a non-negligible fraction (around 1%) of the organic carbon. [Copyright &y& Elsevier]

Abstract: Although particulate emissions from residential wood burning have become a subject of great scientific concern for a few years, data related to their impact on the air quality of large European urban centres are still missing. In the present study, we investigated the chemical and optical properties of fine (PM2.5) carbonaceous aerosols in Paris during the 2005 winter season in order to track the presence of wood burning emissions in such a large city. The use of a seven wavelength Aethalometer allowed us to document shortwave light absorption by brown-carbon-containing organic aerosols of biomass burning origin. In particular, a well-marked diurnal pattern of the spectral dependence of light absorption, with maxima during the night, could be observed every day of the campaign and attributed to wood burning emissions. Relatively high absorption Ångstrom exponents and WSOC/OC ratios (respectively 1.25 and 0.35 on average for the period of study) also indicated the importance of biomass burning aerosols in the Paris atmosphere in winter. Finally, a rough estimate of the contribution of wood burning carbonaceous aerosols to PM2.5 could be achieved. This contribution was found to be as high as 20 ± 10% on average at the Paris background site investigated here. [Copyright &y& Elsevier]

Abstract: A new aerosol parameterization was developed and implemented for operational use with the BRASIL-SR model. The goal is to improve the assessment of solar energy resources in Brazil. Optical properties of the aerosols from burning biomass were obtained using software package OPAC and are in good agreement with previous field measurements made in Brazil. Three different mixture ratios of black carbon were used to cover the full range of typical measured values. The atmospheric transport model SMOKE provided the aerosol profile. An evaluating period of 11days in August/1995 and ground measurements from six sites situated in Amazon region was used to validate the results. The global solar irradiation estimates obtained with new aerosol parameterization, presented smaller mean bias error in all ground sites. The correlation among estimates and measured values for surface global solar irradiation improved about 2.5 times by adopting an aerosol composition with 5% of black carbon. [Copyright &y& Elsevier]

Mean optical and microphysical aerosol properties of long-range transported biomass burning (BB) particles and mixtures are presented from a 9-year (2011–2019) data set of multiwavelength Raman lidar data, obtained by the EOLE lidar over the city of Athens (37.58° N, 23.47° E), Greece. We studied 34 aerosol layers characterized as: (1) smoke; (2) smoke + continental polluted, and (3) smoke + mixed dust. We found, mainly, small-sized aerosols with mean backscatter-related (355 nm/532 nm, 532 nm/1064 nm) values and Ångström exponent (AE) values in the range 1.4–1.7. The lidar ratio (LR) value at 355 nm was found to be 57 ± 10 sr, 51 ± 5 sr, and 38 ± 9 sr for the aerosol categories (1), (2), and (3), respectively; while at 532 nm, we observed LR values of 73 ± 11 sr, 59 ± 10 sr, and 62 ± 12 for the same categories. Regarding the retrieved microphysical properties, the effective radius (reff) ranged from 0.24 ± 0.11 to 0.24 ± 0.14 μm for all aerosol categories, while the volume density (vd) ranged from 8.6 ± 3.2 to 20.7 ± 14.1 μm−3cm−3 with the higher values linked to aerosol categories (1) and (2); the real part of the refractive index (mR) ranged between 1.49 and 1.53, while for the imaginary part (mI), we found values within 0.0108 i and 0.0126 i. Finally, the single scattering albedo (SSA) of the propped particles varied from 0.915 to 0.936 at all three wavelengths (355–532–1064 nm). The novelty of this study is the provision of typical values of BB aerosol properties from the UV to the near IR, which can be used in forecasting the aerosol climatic effects in the European region. [ABSTRACT FROM AUTHOR]

• ROS and chemical composition for fresh and aged BB particles were determined. • ROS production induced by BB aerosols increase by 11 %–64 % after two days of aging. • PAHs and metals are important contributors to OS of fresh BB aerosols. • Enhanced OS of aged particles possibly relates to OM evolution in aging processes. Biomass burning (BB) has an important impact on local/regional air quality and human health in China, but most previous studies overlooked the influence of atmospheric aging processes on cytotoxicity and chemical composition of BB aerosols. In this study, we combined a combustion chamber and an oxidation flow reactor to generate fresh and aged BB PM 2.5. Human bronchial epithelial BEAS-2B cells were exposed to PM 2.5 preparation for 24 h, and then determined for particle-induced reactive oxygen species (ROS) in vitro. The particle-induced ROS production increased by 11 %–64 % after two days of aging, suggesting an enhancement of in vitro -induced oxidative stress (OS) of aged BB particles. Chemical analysis showed that organic matter (OM) was the dominant component with no changes in relative abundance for the fresh and aged BB particles. Organic polycyclic aromatic compounds and some metals showed strong correlations with ROS in fresh particles, indicating the important effects of these harmful components on the OS of fresh BB aerosols. However, such correlations were not found for the aged particles, which is possibly related to the loss of non- or low-toxic semivolatile compounds and the formation of secondary harmful OM (such as some N-containing organic compounds) during the atmospheric aging processes. [ABSTRACT FROM AUTHOR]

In this paper, we present long-term observations of the multiwavelength Raman lidar Polly X T conducted in the framework of the DACAPO-PESO campaign. Regardless of the relatively clean atmosphere in the southern mid-latitude oceans region, we regularly observed events of long-range transported smoke, originating either from regional sources in South America or from Australia. Two case studies will be discussed, both identified as smoke events that occurred on 5 February 2019 and 11 March 2019. For the first case considered, the lofted smoke layer was located at an altitude between 1.0 and 4.2 km, and apart from the predominance of smoke particles, particle linear depolarization values indicated the presence of dust particles. Mean lidar ratio values at 355 and 532 nm were 49 ± 12 and 24 ± 18 sr respectively, while the mean particle linear depolarization was 7.6 ± 3.6% at 532 nm. The advection of smoke and dust particles above Punta Arenas affected significantly the available cloud condensation nuclei (CCN) and ice nucleating particles (INP) in the lower troposphere, and effectively triggered the ice crystal formation processes. Regarding the second case, the thin smoke layers were observed at altitudes 5.5–7.0, 9.0 and 11.0 km. The particle linear depolarization ratio at 532 nm increased rapidly with height, starting from 2% for the lowest two layers and increasing up to 9.5% for the highest layer, indicating the possible presence of non-spherical coated soot aggregates. INP activation was effectively facilitated. The long-term analysis of the one year of observations showed that tropospheric smoke advection over Punta Arenas occurred 16 times (lasting from 1 to 17 h), regularly distributed over the period and with high potential to influence cloud formation in the otherwise pristine environment of the region. [ABSTRACT FROM AUTHOR]

Biomass burning (BB) aerosols contribute to climate forcing, but much is still unknown about the extent of this forcing, owing partially to the high level of uncertainty regarding BB aerosol optical properties. A key optical parameter is the refractive index (RI), which influences the absorbing and scattering properties of aerosols. This quantity is not measured directly, but it is obtained by fitting the measured scattering cross section and extinction cross section to a theoretical model using the RI as a fitting parameter. We used the Rayleigh–Debye–Gans (RDG) approximation to retrieve the complex RI of freshly emitted BB aerosol from two fuels (eucalyptus and olive) from Africa in the spectral range of 500–580 nm. Experimental measurements were carried out using cavity ring-down spectroscopy to measure extinction over the range of wavelengths of 500–580 nm and nephelometry to measure scattering at three wavelengths of 450, 550, and 700 nm for size-selected BB aerosol particles. The fuels were combusted in a tube furnace at a temperature of 800 °C, which is representative of the flaming stage of burning. Filter samples were collected and imaged using tunneling electron microscopy to obtain information on the morphology and size of the particles, which was used in the RDG calculations. The mean radii of the monomers were 27.8 and 31.5 nm for the eucalyptus and the olive fuels, respectively. The components of the retrieved complex RI were in the range of 1.31 ≤ n ≤ 1.56 and 0.045 ≤ k ≤ 0.468. The real and complex parts of the RI increase with increasing particle mobility diameter. The real part of the RI is lower, and the imaginary part is higher than what was recommended in literature for black carbon generated by propane or field measurements from fires of mixed wood samples. Fuel dependent results from controlled laboratory experiments can be used in climate modeling efforts and to constrain field measurements from biomass burning. [ABSTRACT FROM AUTHOR]