scholarly journals Non-reversible aging can increase solar absorption in African biomass burning aerosol plumes of intermediate age

2022 ◽  
Author(s):  
Amie Dobracki ◽  
Paquita Zuidema ◽  
Steve Howell ◽  
Pablo Saide ◽  
Steffen Freitag ◽  
...  

Abstract. Recent studies highlight that biomass-burning aerosol over the remote southeast Atlantic is some of the most sunlight-absorbing aerosol on the planet. In-situ measurements of single-scattering albedo at the 530 nm wavelength (SSA530nm) range from 0.83 to 0.89 within six flights (five in September, 2016 and one in late August, 2017) of the ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) aircraft campaign, increasing with the organic aerosol to black carbon (OA : BC) mass ratio. OA : BC mass ratios of 10 to 14 are lower than some model values and consistent with BC-enriched source emissions, based on indirect inferences of fuel type (savannah grasslands) and dry, flame-efficient combustion conditions. These primarily explain the low single-scattering albedos. We investigate whether continued chemical aging of aerosol plumes of intermediate age (4–7 days after emission, as determined from model tracers) within the free troposphere can further lower the SSA530nm. A mean OA to organic carbon mass ratio of 2.2 indicates highly oxygenated aerosol with the chemical marker f44 indicating the free-tropospheric aerosol continues to oxidize after advecting offshore of continental Africa. Two flights, for which BC to carbon monoxide (CO) ratios remain constant with increasing chemical age, are analyzed further. In both flights, the OA : BC mass ratio decreases over the same time span, indicating continuing net aerosol loss. One flight sampled younger (∼ 4 days) aerosol within the strong zonal outflow of the 4–6 km altitude African Easterly Jet-South. This possessed the highest OA : BC mass ratio of the 2016 campaign and overlaid slightly older aerosol with proportionately less OA, although the age difference of one day is not enough to attribute to a large-scale recirculation and subsidence pattern. The other flight sampled aerosol constrained closer to the coast by a mid-latitude disturbance and found older aerosol aloft overlying younger aerosol. Its vertical increase in OA : BC and nitrate to BC was less pronounced than when younger aerosol overlaid older aerosol, consistent with compensation between a net aerosol loss through aging and a thermodynamical partitioning. Organic nitrate provided 68 % on average of the total nitrate for the 6 flights, in contrast to measurements made at Ascension Island that only found inorganic nitrate. Some evidence for the thermodynamical partitioning to the particle phase at higher altitudes with higher relative humidities for nitrate is still found. The 470–660 nm absorption Angstrom exponent is slightly higher near the African coast than further offshore (approximately 1.2 versus 1.0–1.1), indicating some brown carbon may be present near the coast. The data support the following parameterization: SSA530nm = 0.80+0056*(OA : BC). This indicates a 20 % decrease in SSA can be attributed to chemical aging, or the net 25 % reduction in OA : BC documented for constant BC : CO ratios.

2019 ◽  
Vol 19 (14) ◽  
pp. 9181-9208 ◽  
Author(s):  
Kristina Pistone ◽  
Jens Redemann ◽  
Sarah Doherty ◽  
Paquita Zuidema ◽  
Sharon Burton ◽  
...  

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 (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 (AOD400>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 (SSA500) 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.


2006 ◽  
Vol 6 (10) ◽  
pp. 2911-2925 ◽  
Author(s):  
D. Chand ◽  
P. Guyon ◽  
P. Artaxo ◽  
O. Schmid ◽  
G. P. Frank ◽  
...  

Abstract. As part of the Large Scale Biosphere-Atmosphere Experiment in Amazonia – Smoke, Aerosols, Clouds, Rainfall and Climate (LBA-SMOCC) campaign, detailed surface and airborne aerosol measurements were performed over the Amazon Basin during the dry to wet season from 16 September to 14 November 2002. Optical and physical properties of aerosols at the surface, and in the boundary layer (BL) and free troposphere (FT) during the dry season are discussed in this article. Carbon monoxide (CO) is used as a tracer for biomass burning emissions. At the surface, good correlation among the light scattering coefficient (σs at 545 nm), PM2.5, and CO indicates that biomass burning is the main source of aerosols. Accumulation of haze during some of the large-scale biomass burning events led to high PM2.5 (225 μg m−3), σs (1435 Mm−1), aerosol optical depth at 500 nm (3.0), and CO (3000 ppb). A few rainy episodes reduced the PM2.5, number concentration (CN) and CO concentration by two orders of magnitude. The correlation analysis between σs and aerosol optical thickness shows that most of the optically active aerosols are confined to a layer with a scale height of 1617 m during the burning season. This is confirmed by aircraft profiles. The average mass scattering and absorption efficiencies (545 nm) for small particles (diameter Dp<1.5 μm) at surface level are found to be 5.0 and 0.33 m2 g−1, respectively, when relating the aerosol optical properties to PM2.5 aerosols. The observed mean single scattering albedo (ωo at 545 nm) for submicron aerosols at the surface is 0.92±0.02. The light scattering by particles (Δσs/Δ CN) increase 2–10 times from the surface to the FT, most probably due to the combined affects of coagulation and condensation.


2016 ◽  
Vol 16 (15) ◽  
pp. 9549-9561 ◽  
Author(s):  
Rudra P. Pokhrel ◽  
Nick L. Wagner ◽  
Justin M. Langridge ◽  
Daniel A. Lack ◽  
Thilina Jayarathne ◽  
...  

Abstract. Single-scattering albedo (SSA) and absorption Ångström exponent (AAE) are two critical parameters in determining the impact of absorbing aerosol on the Earth's radiative balance. Aerosol emitted by biomass burning represent a significant fraction of absorbing aerosol globally, but it remains difficult to accurately predict SSA and AAE for biomass burning aerosol. Black carbon (BC), brown carbon (BrC), and non-absorbing coatings all make substantial contributions to the absorption coefficient of biomass burning aerosol. SSA and AAE cannot be directly predicted based on fuel type because they depend strongly on burn conditions. It has been suggested that SSA can be effectively parameterized via the modified combustion efficiency (MCE) of a biomass burning event and that this would be useful because emission factors for CO and CO2, from which MCE can be calculated, are available for a large number of fuels. Here we demonstrate, with data from the FLAME-4 experiment, that for a wide variety of globally relevant biomass fuels, over a range of combustion conditions, parameterizations of SSA and AAE based on the elemental carbon (EC) to organic carbon (OC) mass ratio are quantitatively superior to parameterizations based on MCE. We show that the EC ∕ OC ratio and the ratio of EC ∕ (EC + OC) both have significantly better correlations with SSA than MCE. Furthermore, the relationship of EC ∕ (EC + OC) with SSA is linear. These improved parameterizations are significant because, similar to MCE, emission factors for EC (or black carbon) and OC are available for a wide range of biomass fuels. Fitting SSA with MCE yields correlation coefficients (Pearson's r) of  ∼  0.65 at the visible wavelengths of 405, 532, and 660 nm while fitting SSA with EC / OC or EC / (EC + OC) yields a Pearson's r of 0.94–0.97 at these same wavelengths. The strong correlation coefficient at 405 nm (r =  0.97) suggests that parameterizations based on EC / OC or EC / (EC + OC) have good predictive capabilities even for fuels in which brown carbon absorption is significant. Notably, these parameterizations are effective for emissions from Indonesian peat, which have very little black carbon but significant brown carbon (SSA  =  0.990 ± 0.001 at 532 and 660 nm, SSA  =  0.937 ± 0.011 at 405 nm). Finally, we demonstrate that our parameterization based on EC / (EC + OC) accurately predicts SSA during the first few hours of plume aging with data from Yokelson et al. (2009) gathered during a biomass burning event in the Yucatán Peninsula of Mexico.


2019 ◽  
Author(s):  
Kristina Pistone ◽  
Jens Redemann ◽  
Sarah Doherty ◽  
Paquita Zuidema ◽  
Sharon Burton ◽  
...  

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 (AOD400 > 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 (SSA500) 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.


2021 ◽  
Vol 7 (9) ◽  
pp. eabd3440
Author(s):  
Lydia G. Jahl ◽  
Thomas A. Brubaker ◽  
Michael J. Polen ◽  
Leif G. Jahn ◽  
Kerrigan P. Cain ◽  
...  

Ice-nucleating particles (INPs) in biomass-burning aerosol (BBA) that affect cloud glaciation, microphysics, precipitation, and radiative forcing were recently found to be driven by the production of mineral phases. BBA experiences extensive chemical aging as the smoke plume dilutes, and we explored how this alters the ice activity of the smoke using simulated atmospheric aging of authentic BBA in a chamber reactor. Unexpectedly, atmospheric aging enhanced the ice activity for most types of fuels and aging schemes. The removal of organic carbon particle coatings that conceal the mineral-based ice-active sites by evaporation or oxidation then dissolution can increase the ice activity by greater than an order of magnitude. This represents a different framework for the evolution of INPs from biomass burning where BBA becomes more ice active as it dilutes and ages, making a larger contribution to the INP budget, resulting cloud microphysics, and climate forcing than is currently considered.


Atmosphere ◽  
2021 ◽  
Vol 12 (12) ◽  
pp. 1700
Author(s):  
Shuaiyi Shi ◽  
Yanjun Ma ◽  
Fangwen Bao ◽  
Faisal Mumtaz

Due to its unique natural conditions and agricultural tradition, northeast China (NEC) has formed a distinctive open biomass burning habit with local-specific biomass burning aerosol features. In this research, with the help of a newly optimized biomass burning aerosol identification method, which combines satellite aerosol and fire observational products with the HYSPLIT model forward trajectories, a systematic and quantitative analysis of aerosol emitted from open biomass burning in the NEC region are conducted to determine in detail its local-specific features, such as influence region, aging characteristics, and seasonal variation. During the 72-h aging process after biomass burning emission, aerosol particle size growth found with the Angstrom exponent declines from 1.6 to 1.54. Additionally, the volume fraction of black carbon decreases from 4.5% to 3.1%, leading to the Single Scattering Albedo (SSA) increasing from the fresh state of 0.84 to the aged state of 0.89. The cooling effect at TOA, due to the existence of aerosol, is enhanced by more than 70%, indicating its severe and dynamic influence on climate change. The average AOD in spring is 0.63, which is higher than autumn’s value of 0.52, indicating that biomass burning is more intensive in spring. Compared to autumn, aerosols emitted from spring biomass burning in the NEC region have lower sphere fraction, smaller particle size, higher volume fraction of black carbon, higher absorbability, and weaker cooling effect at TOA, which can be partly explained by the drier ambient environment and lower water content of the burned crop straw in spring.


2016 ◽  
Author(s):  
B. T. Johnson ◽  
J. M. Haywood ◽  
J. M. Langridge ◽  
E. Darbyshire ◽  
W. T. Morgan ◽  
...  

Abstract. We present observations of biomass burning aerosol from the South American Biomass Burning Analysis (SAMBBA) and other measurement campaigns, and use these to evaluate the representation of biomass burning aerosol properties and processes in a state-of-the-art climate model. The evaluation includes detailed comparisons with aircraft and ground data, along with remote sensing observations from MODIS and AERONET. We demonstrate several improvements to aerosol properties following the implementation of the GLOMAP-mode modal aerosol scheme in the HadGEM3 climate model. This predicts the particle size distribution, composition and optical properties, giving increased accuracy in the representation of aerosol properties and physical-chemical processes over the CLASSIC bulk aerosol scheme previously used in HadGEM2. Although both models give similar regional distributions of carbonaceous aerosol mass and Aerosol Optical Depth (AOD), GLOMAP-mode is better able to capture the observed size distribution, single scattering albedo, and Ångström exponent across different tropical biomass burning source regions. Both aerosol schemes overestimate the uptake of water compared to recent observations, CLASSIC more so than GLOMAP-mode, leading to a likely overestimation of aerosol scattering, AOD and single scattering albedo at high relative humidity. Observed aerosol vertical distributions were well captured when biomass burning aerosol emissions were injected uniformly from the surface to 3 km. Finally, good agreement between observed and modelled AOD was gained only after scaling up GFED3 emissions by a factor of 1.6 for CLASSIC and 2.0 for GLOMAP-mode. We attribute this difference in scaling factor mainly to different assumptions for the growth of aerosol mass during ageing via oxidation and condensation of organics.


2009 ◽  
Vol 9 (20) ◽  
pp. 8017-8038 ◽  
Author(s):  
S.-W. Kim ◽  
P. Chazette ◽  
F. Dulac ◽  
J. Sanak ◽  
B. Johnson ◽  
...  

Abstract. We present observations of tropospheric aerosol and water vapor transport over West Africa and the associated meteorological conditions during the AMMA SOP-0 dry season experiment, which was conducted in West Africa in January–February 2006. This study combines data from ultra-light aircraft (ULA)-based lidar, airborne in-situ aerosol and gas measurements, standard meteorological measurements, satellite-based aerosol measurements, airmass trajectories, and radiosonde measurements. At Niamey (13.5° N, 2.2° E) the prevailing surface wind (i.e. Harmattan) was from the northeast bringing dry dusty air from the Sahara desert. High concentrations of mineral dust aerosol were typically observed from the surface to 1.5 or 2 km associated with the Saharan airmasses. At higher altitudes the prevailing wind veered to the south or southeast bringing relatively warm and humid airmasses from the biomass burning regions to the Sahel (<10° N). These elevated layers had high concentrations of biomass burning aerosol and were typically observed between altitudes of 2–5 km. Meteorological analyses show these airmasses were advected upwards over the biomass burning regions through ascent in Inter-Tropical Discontinuity (ITD) zone. Aerosol vertical profiles obtained from the space-based lidar CALIOP onboard CALIPSO during January 2007 also showed the presence of dust particles (particle depolarization (δ)~30%, lidar Ångström exponent (LAE)<0, aerosol backscatter to extinction ratio (BER): 0.026~0.028 sr−1) at low levels (<1.5 km) and biomass burning smoke aerosol (δ<10%, LAE: 0.6~1.1, BER: 0.015~0.018 sr−1) between 2 and 5 km. CALIOP data indicated that these distinct continental dust and biomass burning aerosol layers likely mixed as they advected further south over the tropical Atlantic Ocean, as indicated an intermediate values of δ (10~17%), LAE (0.16~0.18) and BER (0.0021~0.0022 sr−1).


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