Fine Ash-Bearing Particles as a Major Aerosol Component in Biomass Burning Smoke

Biomass burning (BB) events are occurring globally with increasing frequency, and their emissions are having more impacts on human health and climate. Large ash particles are recognized as a BB product with major influences on soil and water environments. However, fine-ash particles, which have diameters smaller than several microns and characteristic morphologies and compositions (mainly Ca and Mg carbonates), have not yet been explicitly considered as a major BB aerosol component either in field observations or climate models. This study measured BB aerosol samples using transmission electron microscopy (TEM) and ion chromatography during the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) campaign. We show that significant amounts of fine ash-bearing particles are transported \u3e100 km from their fire sources. Our environmental chamber experiments suggest that they can act as cloud condensation and ice nuclei. We also found considerable amounts of fine ash-bearing particles in the TEM samples collected during previous campaigns (Biomass Burning Observation Project and Megacity Initiative: Local and Global Research Observations). These ash particles are commonly mixed with organic matter and make up ∼8% and 5% of BB smoke by number and mass, respectively, in samples collected during the FIREX-AQ campaign. The measured ash-mass concentrations are approximately five times and six times greater than those of BB black carbon and potassium, respectively, scaling to an estimated global emission of 11.6 Tg yr−1 with a range of 8.8–16.3 Tg yr−1. Better characterization and constraints on these fine ash-bearing particles will improve BB aerosol measurements and strengthen assessments of BB impacts on human health and climate

Seasonal variations in fire conditions are important drivers in the trend of aerosol optical properties over the south-eastern Atlantic

From June to October, southern Africa produces one-third of the globalbiomass burning (BB) emissions by widespread fires. BB aerosols aretransported westward over the south-eastern Atlantic with the mid-tropospheric winds,resulting in significant radiative effects. Ascension Island (ASI) islocated midway between Africa and South America. From June 2016 to October 2017, a 17-month in situ observation campaign on ASI found a lowsingle-scattering albedo (SSA) as well as a high mass absorptioncross-section of black carbon (MACBC), demonstrating the strongabsorbing marine boundary layer in the south-eastern Atlantic. Here weinvestigate the monthly variations of critical optical properties of BBaerosols, i.e. SSA and MACBC, during the BB seasons and the drivingfactors behind these variations. Both SSA and MACBC increase fromJune to August and decrease in September and October. The average SSA duringthe BB seasons is 0.81 at 529 nm wavelength, with the highest mean∼ 0.85 in October and the lowest ∼ 0.78 inAugust. The absorption enhancement (Eabs) derived from the MACBCshows similar trends with SSA, with the average during the whole of the BB seasonsat ∼ 1.96 and ∼ 2.07 in 2016 and 2017, respectively. As theEabs is higher than the ∼ 1.5 commonly adopted value byclimate models, this result suggests the marine boundary layer in thesouth-eastern Atlantic is more absorbing than model simulations. We find theenhanced ratio of BC to CO (ΔBC/ΔCO, equal to BC/ΔCOas the BC background concentration is considered to be 0) is well correlatedwith SSA and MACBC, providing a simple way to estimate the aerosoloptical characteristics in the south-eastern Atlantic. The exponentialfunction we proposed can approximate SSA and MACBC with BC/ΔCO, and when BC/ΔCO is small it can capture the rapid growth of SSAas BC/ΔCO decreases. BC/ΔCO is influenced by combustionconditions and aerosol scavenging. From the analysis of the location of BB, the primary source fuel, the water content in the fuel, combinedwith the mean cloud cover and precipitation in the transport areas of the BBplume, we conclude that the increase in BC/ΔCO from June to Augustis likely to be caused by burning becoming more flaming. The reduction inthe water content of fuels may be responsible for the change in the burningconditions from June to August. The decrease in BC/ΔCO in Septemberand October may be caused by two factors, one being a lower proportion offlaming conditions, possibly associated with a decrease in mean surface windspeed in the burning area, and the other being an increase in precipitationin the BB transport pathway, leading to enhanced aerosol scavenging, whichultimately results in an increase in SSA and MACBC

Light absorption by brown carbon over the South-East Atlantic Ocean

International audienceBiomass burning emissions often contain brown carbon (BrC), which represents a large family of light-absorbing organics that are chemically complex, thus making it difficult to estimate their absorption of incoming solar radiation, resulting in large uncertainties in the estimation of the global direct radiative effect of aerosols. Here we investigate the contribution of BrC to the total light absorption of biomass burning aerosols over the South-East Atlantic Ocean with different optical models, utilizing a suite of airborne measurements from the ORACLES 2018 campaign. An effective refractive index of black carbon (BC), meBC=1.95+ikeBC, that characterizes the absorptivity of all absorbing components at 660 nm wavelength was introduced to facilitate the attribution of absorption at shorter wavelengths, i.e. 470 nm. Most values of the imaginary part of the effective refractive index, keBC, were larger than those commonly used for BC from biomass burning emissions, suggesting contributions from absorbers besides BC at 660 nm. The TEM-EDX single-particle analysis further suggests that these long-wavelength absorbers might include iron oxides, as iron is found to be present only when large values of keBC are derived. Using this effective BC refractive index, we find that the contribution of BrC to the total absorption at 470 nm (RBrC,470) ranges from ∼8 %-22 %, with the organic aerosol mass absorption coefficient (MACOA,470) at this wavelength ranging from 0.30±0.27 to 0.68±0.08 m2 g-1. The core-shell model yielded much higher estimates of MACOA,470 and RBrC,470 than homogeneous mixing models, underscoring the importance of model treatment. Absorption attribution using the Bruggeman mixing Mie model suggests a minor BrC contribution of 4 % at 530 nm, while its removal would triple the BrC contribution to the total absorption at 470 nm obtained using the AAE (absorption Ångström exponent) attribution method. Thus, it is recommended that the application of any optical properties-based attribution method use absorption coefficients at the longest possible wavelength to minimize the influence of BrC and to account for potential contributions from other absorbing materials

Intercomparison of biomass burning aerosol optical properties from in-situ and remote-sensing instruments in ORACLES-2016

Abstract. The total effect of aerosols, both directly and on cloud properties, remains the biggest source of uncertainty in anthropogenic radiative forcing on the climate. Correct characterization of intensive aerosol optical properties, particularly in conditions where absorbing aerosol is present, is a crucial factor in quantifying these effects. The Southeast Atlantic Ocean (SEA), with seasonal biomass burning smoke plumes overlying and mixing with a persistent stratocumulus cloud deck, offers an excellent natural laboratory to make the observations necessary to understand the complexities of aerosol-cloud-radiation interactions. The first field deployment of the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) campaign was conducted in September of 2016 out of Walvis Bay, Namibia. Data collected during ORACLES-2016 are used to derive aerosol properties from an unprecedented number of simultaneous measurement techniques over this region. Here we present results from six of the eight independent instruments or instrument combinations, all applied to measure or retrieve aerosol absorption and single scattering albedo. Most but not all of the biomass-burning aerosol was located in the free troposphere, in relative humidities typically ranging up to 60 %. We present the single scattering albedo (SSA), absorbing and total aerosol optical depth (AOD and AAOD), and absorption, scattering, and extinction Ångström exponents (AAE, SAE, EAE) for specific case studies looking at near-coincident and -colocated measurements from multiple instruments, and SSAs for the broader campaign average over the monthlong deployment. For the case studies, we find that SSA agrees within the measurement uncertainties between multiple instruments, though, over all cases, there is no strong correlation between values reported by one instrument and another. We also find that agreement between the instruments is more robust at higher aerosol loading (AOD 400  > 0.4). The campaign-wide average and range shows differences in the values measured by each instrument. We find the ORACLES-2016 campaign-average SSA at 500 nm (SSA 500 ) to be between 0.85 and 0.88, depending on the instrument considered (4STAR, AirMSPI, or in situ measurements), with the inter-quartile ranges for all instruments between 0.83 and 0.89. This is consistent with previous September values reported over the region (between 0.84 and 0.90 for SSA at 550 nm). The results suggest that the differences observed in the campaign-average values may be dominated by instrument-specific spatial sampling differences and the natural physical variability in aerosol conditions over the SEA, rather than fundamental methodological differences

Intercomparison of biomass burning aerosol optical properties from in situ and remote-sensing instruments in ORACLES-2016

The total effect of aerosols, both directly and on cloud properties, remains the biggest source of uncertainty in anthropogenic radiative forcing on the climate. Correct characterization of intensive aerosol optical properties, particularly in conditions where absorbing aerosol is present, is a crucial factor in quantifying these effects. The southeast Atlantic Ocean (SEA), with seasonal biomass burning smoke plumes overlying and mixing with a persistent stratocumulus cloud deck, offers an excellent natural laboratory to make the observations necessary to understand the complexities of aerosol–cloud–radiation interactions. The first field deployment of the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) campaign was conducted in September of 2016 out of Walvis Bay, Namibia. Data collected during ORACLES-2016 are used to derive aerosol properties from an unprecedented number of simultaneous measurement techniques over this region. Here, we present results from six of the eight independent instruments or instrument combinations, all applied to measure or retrieve aerosol absorption and single-scattering albedo. Most but not all of the biomass burning aerosol was located in the free troposphere, in relative humidities typically ranging up to 60%. We present the single-scattering albedo (SSA), absorbing and total aerosol optical depth (AAOD and AOD), and absorption, scattering, and extinction Ångström exponents (AAE, SAE, and EAE, respectively) for specific case studies looking at near-coincident and near-colocated measurements from multiple instruments, and SSAs for the broader campaign average over the month-long deployment. For the case studies, we find that SSA agrees within the measurement uncertainties between multiple instruments, though, over all cases, there is no strong correlation between values reported by one instrument and another. We also find that agreement between the instruments is more robust at higher aerosol loading (AOD 400 > 0.4 ).The campaign-wide average and range shows differences in the values measured by each instrument. We find the ORACLES-2016 campaign-average SSA at 500 > nm (SSA 500 ) to be between 0.85 and 0.88, depending on the instrument considered (4STAR, AirMSPI, or in situ measurements), with the interquartile ranges for all instruments between 0.83 and 0.89. This is consistent with previous September values reported over the region (between 0.84 and 0.90 for SSA at 550nm). The results suggest that the differences observed in the campaign-average values may be dominated by instrument-specific spatial sampling differences and the natural physical variability in aerosol conditions over the SEA, rather than fundamental methodological differences

The Two-Column Aerosol Project: Phase I - Overview and Impact of Elevated Aerosol Layers on Aerosol Optical Depth

The Two-Column Aerosol Project (TCAP), conducted from June 2012 through June 2013, was a unique study designed to provide a comprehensive data set that can be used to investigate a number of important climate science questions, including those related to aerosol mixing state and aerosol radiative forcing. The study was designed to sample the atmosphere be tween and within two atmospheric columns; one fixed near the coast of North America (over Cape Cod, MA) and a second moveable column over the Atlantic Ocean several hundred kilometers from the coast. The U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Mobile Facility (AMF) was deployed at the base of the Cape Cod column, and the ARM Aerial Facility was utilized for the summer and winter intensive observation periods. One important finding from TCAP is that four of six nearly cloud-free flight days had aerosol layers aloft in both the Cape Cod and maritime columns that were detected using the nadir pointing second-generation NASA high-spectral resolution lidar (HSRL-2).These layer s contributed up to 60 of the total observed aerosol optical depth (AOD). Many of these layers were also intercepted by the aircraft configured for in situ sampling, and the aerosol in the layers was found to have increased amounts of biomass burning material and nitrate compared to aerosol found near the surface. In addition, while there was a great deal of spatial and day-to-day variability in the aerosol chemical composition and optical properties, no systematic differences between the two columns were observed