scholarly journals Undersizing of aged African biomass burning aerosol by an ultra-high-sensitivity aerosol spectrometer

2021 ◽  
Vol 14 (11) ◽  
pp. 7381-7404
Author(s):  
Steven G. Howell ◽  
Steffen Freitag ◽  
Amie Dobracki ◽  
Nikolai Smirnow ◽  
Arthur J. Sedlacek III

Abstract. The ultra-high-sensitivity aerosol spectrometer (UHSAS) differs from most other optical particle spectrometers by using a high-power infrared (IR) laser to detect small particles and reduce the sizing ambiguity due to the non-monotonicity of scattering with particle size. During the NASA ORACLES project (ObseRvations of Aerosols above CLouds and their intEractionS) over the southeast Atlantic Ocean, the UHSAS clearly undersized particles in the biomass burning plume extending from southern Africa. Since the horizontal and vertical extent of the plume was vast, the NASA P-3B research aircraft often flew through a fairly uniform biomass burning plume for periods exceeding 30 min, sufficient time to explore the details of the UHSAS response by selecting single particle sizes with a differential mobility analyzer (DMA) and passing them to the UHSAS. This was essentially an in-flight calibration of the UHSAS using the particles of interest. Two modes of responses appeared. Most particles were undersized by moderate amounts, ranging from not at all for 70 nm aerosols to 15 % for 280 nm particles. Mie scattering calculations show that composition-dependent refractive index of the particles cannot explain the pattern. Heating of brown carbon or tarballs in the beam causing evaporation and shrinking of the particles is the most plausible explanation, though mis-sizing due to non-sphericity cannot be ruled out. A small fraction (10 %–30 %) of the particles were undersized by 25 % to 35 %. Those were apparently the particles containing refractory black carbon. Laboratory calibrations confirm that black carbon is drastically undersized by the UHSAS, because particles heat to their vaporization point and shrink. A simple empirical correction equation was implemented that dramatically improves agreement with DMA distributions between 100 and 500 nm. It raised the median particle diameter by 18 nm, from 163 to 181 nm, during the August 2017 deployment and by smaller amounts during deployments with less intense pollution. Calculated scattering from UHSAS size distributions increased by about 130 %, dramatically improving agreement with scattering measured by nephelometers. The correction is only valid in polluted instances; clean marine boundary layer and free troposphere aerosols behaved more like the calibration spheres. We were unable to directly test the correction between 500 and 1000 nm, though aerodynamic particle sizer (APS) data appear to show that the correction is poor at the largest diameters, which is no surprise as the composition of those particles is likely to be quite different than that of the accumulation mode. This adds to the evidence that UHSAS data must be treated cautiously whenever the aerosol may absorb infrared light. Similar corrections may be required whenever brown carbon aerosol is present.

2020 ◽  
Author(s):  
Steven G. Howell ◽  
Steffen Freitag ◽  
Amie Dobracki ◽  
Nikolai Smirnow ◽  
Arthur J. Sedlacek III

Abstract. The Ultra-High Sensitivity Aerosol Spectrometer (UHSAS) differs from most other optical particle spectrometers by using a high-power infrared (IR) laser to detect small particles and reduce the sizing ambiguity due to the non-monotonicity of scattering with particle size. During the NASA ORACLES project (ObseRvations of Aerosols above CLouds and their intEractionS) over the southeast Atlantic Ocean, the UHSAS clearly undersized particles in the biomass burning plume extending from Southern Africa. Since the horizontal and vertical extent of the plume was vast, the NASA P-3B research aircraft often flew through a fairly uniform biomass burning plume for periods exceeding 30 minutes, sufficient time to explore the details of the UHSAS response by selecting single particle sizes with a Differential Mobility Analyzer (DMA) and passing them to the UHSAS. This was essentially an in-flight calibration of the UHSAS using the particles of interest. Two modes of responses appeared. Most particles were undersized by moderate amounts, ranging from not at all for 70 nm aerosols to 15 % for 280 nm particles. Mie scattering calculations show that composition-dependent refractive index of the particles is unlikely to explain the pattern. Heating of brown carbon or tarballs in the beam causing evaporation and shrinking of the particles is the most plausible explanation, though that requires greater IR absorption than is usually attributed to brown carbon. 10–30 % of the particles were undersized by 25 to 35 %. Those were apparently the particles containing refractory black carbon. Laboratory calibrations confirm that black carbon is drastically undersized by the UHSAS, though the mechanism is not entirely clear. A simple empirical correction equation was implemented that dramatically improves agreement with DMA distributions between 100 and 500 nm. It raised median particle diameter 18 nm, from 163 to 181 nm during the August 2017 deployment and by smaller amounts during deployments with less intense pollution. Calculated scattering from UHSAS size distributions increased by about 130 %, dramatically improving agreement with scattering measured by nephelometers. The correction is only valid in polluted instances; clean marine boundary layer and free troposphere aerosols behaved more like the calibration spheres. We were unable to directly test the correction between 500 and 1000 nm, though APS data appear to show that the correction is poor at the largest diameters, which is no surprise as the composition of those particles is likely to be quite different than that of the accumulation mode. This adds to the evidence that UHSAS data must be treated cautiously whenever the aerosol may absorb infrared light. Similar corrections may be required whenever brown carbon aerosol is present.


2020 ◽  
Author(s):  
HuiHui Wu ◽  
Jonathan Taylor ◽  
Justin Langridge ◽  
Chenjie Yu ◽  
Paul Williams ◽  
...  

<p>The biomass burning over West Africa during the dry season (December – February) is a globally significant source of trace gases and carbonaceous aerosol particles in the atmosphere. The MOYA-2017 (Methane Observations Yearly Assessments 2017) campaign were conducted using the UK FAAM Bae-146 airborne research aircraft, to investigate biomass burning emissions in this region. Research sorties were flown out of Senegal, with some flights directly over terrestrial fires and others sampling transported smokes over the Atlantic ocean.</p><p>The aircraft was equipped with a variety of aerosol-related instruments to measure submicron aerosol chemical properties (aerosol mass spectrometer, AMS and single-particle soot photometer, SP2) and absorption at different wavelengths (Photoacoustic spectrometer, PAS, measure at 405, 514 and 658 nm). In this study, we focus on the aging process of ambient black carbon (BC) and brown carbon (BrC) from biomass burning, in time scale from (<0.5) h to (9 – 15) h. The transport age of smokes was estimated using Met Office's Numerical Atmospheric-dispersion Modelling Environment (NAME).</p><p>The sampled smokes during MOYA-2017 were controlled by flaming-phase combustion. The enhancement ratios of BC with respect to CO ranged from 14 to 26 (ng m<sup>–3</sup> / ppbv) at sources. Our measurements show that count and mass median diameters of BC core size were relatively stable, which were around 106 and 190 nm respectively. Average BC coating thickness increased from (1.16 ± 0.03) to (1.71 ± 0.06) after approximately half-day transport. Average absorption angstrom exponents (AAE<sub>405-658</sub>) increased from (1.1 ± 0.1) to (1.8 ± 0.3), suggesting that BrC contributed little in the very freshly emitted aerosols (<0.5 h) and were formed during aging process. In order to investigate the importance of BrC in this area, we also attributed the measured aerosol absorption into BC and BrC separately. By linking AAE<sub>405-658</sub> with organic (OA) composition measured by the AMS, we found that the increasing AAE<sub>405-658</sub> is positively correlated with O/C ratio (oxygenation) of the OA. These data indicate that BrC in smokes controlled by flaming combustion is likely to be from the condensation of semi-volatile OA during cooling stage of smokes, and from the aged primary OA or secondary OA formation.</p>


2016 ◽  
Vol 9 (1) ◽  
pp. 103-114 ◽  
Author(s):  
G. I. Gkatzelis ◽  
D. K. Papanastasiou ◽  
K. Florou ◽  
C. Kaltsonoudis ◽  
E. Louvaris ◽  
...  

Abstract. An experimental methodology was developed to measure the nonvolatile particle number concentration using a thermodenuder (TD). The TD was coupled with a high-resolution time-of-flight aerosol mass spectrometer, measuring the chemical composition and mass size distribution of the submicrometer aerosol and a scanning mobility particle sizer (SMPS) that provided the number size distribution of the aerosol in the range from 10 to 500 nm. The method was evaluated with a set of smog chamber experiments and achieved almost complete evaporation (> 98 %) of secondary organic as well as freshly nucleated particles, using a TD temperature of 400 °C and a centerline residence time of 15 s. This experimental approach was applied in a winter field campaign in Athens and provided a direct measurement of number concentration and size distribution for particles emitted from major pollution sources. During periods in which the contribution of biomass burning sources was dominant, more than 80 % of particle number concentration remained after passing through the thermodenuder, suggesting that nearly all biomass burning particles had a nonvolatile core. These remaining particles consisted mostly of black carbon (60 % mass contribution) and organic aerosol (OA; 40 %). Organics that had not evaporated through the TD were mostly biomass burning OA (BBOA) and oxygenated OA (OOA) as determined from AMS source apportionment analysis. For periods during which traffic contribution was dominant 50–60 % of the particles had a nonvolatile core while the rest evaporated at 400 °C. The remaining particle mass consisted mostly of black carbon with an 80 % contribution, while OA was responsible for another 15–20 %. Organics were mostly hydrocarbon-like OA (HOA) and OOA. These results suggest that even at 400 °C some fraction of the OA does not evaporate from particles emitted from common combustion processes, such as biomass burning and car engines, indicating that a fraction of this type of OA is of extremely low volatility.


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.


2020 ◽  
Vol 20 (19) ◽  
pp. 11625-11637
Author(s):  
Antonios Tasoglou ◽  
Evangelos Louvaris ◽  
Kalliopi Florou ◽  
Aikaterini Liangou ◽  
Eleni Karnezi ◽  
...  

Abstract. A month-long set of summertime measurements in a remote area in the Mediterranean is used to quantify aerosol absorption and the role of black and brown carbon. The suite of instruments included a high-resolution aerosol mass spectrometer (HR-ToF-AMS) and a scanning mobility particle sizer (SMPS), both coupled to a thermodenuder and an Aethalometer, a photoacoustic extinctiometer (PAX405), and a single particle soot photometer (SP2). The average refractory black carbon (rBC) concentration during the campaign was 0.14 µg m−3, representing 3 % of the fine aerosol mass. The measured light absorption was two or more times higher than that of fresh black carbon (BC). Mie theory indicated that the absorption enhancement due to the coating of BC cores by nonrefractory material could explain only part of this absorption enhancement. The role of brown carbon (BrC) and other non-BC light-absorbing material was then investigated. A good correlation (R2=0.76) between the unexplained absorption and the concentration of extremely low volatility organic compounds (ELVOCs) mass was found.


2018 ◽  
Vol 18 (23) ◽  
pp. 17003-17016 ◽  
Author(s):  
Paola Formenti ◽  
Stuart John Piketh ◽  
Andreas Namwoonde ◽  
Danitza Klopper ◽  
Roelof Burger ◽  
...  

Abstract. Continuous measurements between July 2012 and December 2015 at the Henties Bay Aerosol Observatory (HBAO; 22∘ S, 14∘05′ E), Namibia, show that, during the austral wintertime, transport of light-absorbing black carbon aerosols occurs at low level into the marine boundary layer. The average of daily concentrations of equivalent black carbon (eBC) over the whole sampling period is 53 (±55) ng m−3. Peak values above 200 ng m−3 and up to 800 ng m−3 occur seasonally from May to August, ahead of the dry season peak of biomass burning in southern Africa (August to October). Analysis of 3-day air mass back-trajectories show that air masses from the South Atlantic Ocean south of Henties Bay are generally cleaner than air having originated over the ocean north of Henties Bay, influenced by the outflow of the major biomass burning plume, and from the continent, where wildfires occur. Additional episodic peak concentrations, even for oceanic transport, indicate that pollution from distant sources in South Africa and maritime traffic along the Atlantic ship tracks could be important. While we expect the direct radiative effect to be negligible, the indirect effect on the microphysical properties of the stratocumulus clouds and the deposition to the ocean could be significant and deserve further investigation, specifically ahead of the dry season.


2013 ◽  
Vol 13 (5) ◽  
pp. 2415-2422 ◽  
Author(s):  
D. A. Lack ◽  
R. Bahreini ◽  
J. M. Langridge ◽  
J. B. Gilman ◽  
A. M. Middlebrook

Abstract. Traditional gas and particle phase chemical markers used to identify the presence of biomass burning (BB) emissions were measured for a large forest fire near Boulder, Colorado. Correlation of the organic matter mass spectroscopic m/z 60 with measured particle light absorption properties found no link at 532 nm, and a strong correlation at 404 nm. Non-black carbon absorption at 404 nm was well correlated to the ratio of the mass fractions of particulate organic matter (POM) that was m/z 60 (f60) to m/z 44 (f44). The f60 to f44 ratio did not fully explain the variability in non-BC absorption, due to contributions of brown carbon (BrC) absorption and absorption due to internal mixing of POM with black carbon (BC). The absorption Ångstrom exponent (ÅAbs) showed a good correlation to f60/f44; however the best correlation resulted from the mass absorption efficiency (MAE) of BrC at 404 nm (MAEPOM-404 nm) and f60/f44. This result indicates that the absorption of POM at low visible and UV wavelengths is linked to emissions of organic matter that contribute to the m/z 60 mass fragment, although they do not contribute to 532 nm absorption. m/z 60 is often attributed to levoglucosan and related compounds. The linear relationship between MAEPOM-404 nm and f60/f44 suggests that the strength of BrC absorption for this fire can be predicted by emissions of f60-related organic matter.


2020 ◽  
Author(s):  
Antonios Tasoglou ◽  
Evangelos Louvaris ◽  
Kalliopi Florou ◽  
Aikaterini Liangou ◽  
Eleni Karnezi ◽  
...  

Abstract. A month-long set of summertime measurements in a remote area in the Mediterranean is used to quantify aerosol absorption and the role of black and brown carbon. The suite of instruments included a high-resolution Aerosol Mass Spectrometer (HR-ToF-AMS), and a Scanning Mobility Particle Sizer (SMPS) both coupled to a thermodenuder and an aethalometer, a photoacoustic extinctiometer (PAX405), a Multi-Angle Absorption Photometer (MAAP), and a Single Particle Soot Photometer (SP2). The average refractory black carbon (rBC) concentration during the campaign was 0.14 μg m−3, representing 3 % of the fine aerosol mass. The measured light absorption was two or more times higher than that of fresh black carbon (BC). Mie theory indicated that the absorption enhancement due to the coating of BC cores by non-refractory material could explain only part of this absorption enhancement. The role of brown carbon (BrC) and other non-BC light-absorbing material was then investigated. A good correlation (R2 = 0.65) between the unexplained absorption and the concentration of extremely low volatility organic compounds (ELVOCs) mass was found.


2015 ◽  
Vol 15 (3) ◽  
pp. 1367-1383 ◽  
Author(s):  
J. C. Schroder ◽  
S. J. Hanna ◽  
R. L. Modini ◽  
A. L. Corrigan ◽  
S. M. Kreidenwies ◽  
...  

Abstract. Size-resolved observations of aerosol particles and cloud droplet residuals were studied at a marine boundary layer site (251 m a.m.s.l.) in La Jolla, San Diego, California, during 2012. A counterflow virtual impactor (CVI) was used as the inlet to sample cloud residuals while a total inlet was used to sample both cloud residuals and interstitial particles. Two cloud events totaling 10 h of in-cloud sampling were analyzed. Based on bulk aerosol particle concentrations, mass concentrations of refractory black carbon (rBC), and back trajectories, the two air masses sampled were classified as polluted marine air. Since the fraction of cloud droplets sampled by the CVI was less than 100%, the measured activated fractions of rBC should be considered as lower limits to the total fraction of rBC activated during the two cloud events. Size distributions of rBC and a coating analysis showed that sub-100 nm rBC cores with relatively thick coatings were incorporated into the cloud droplets (i.e., 95 nm rBC cores with median coating thicknesses of at least 65 nm were incorporated into the cloud droplets). Measurements also show that the coating volume fraction of rBC cores is relatively large for sub-100 nm rBC cores. For example, the median coating volume fraction of 95 nm rBC cores incorporated into cloud droplets was at least 0.9, a result that is consistent with κ-Köhler theory. Measurements of the total diameter of the rBC-containing particles (rBC core and coating) suggest that the total diameter of rBC-containing particles needed to be at least 165 nm to be incorporated into cloud droplets when the core rBC diameter is ≥ 85 nm. This result is consistent with previous work that has shown that particle diameter is important for activation of non-rBC particles. The activated fractions of rBC determined from the measurements ranged from 0.01 to 0.1 for core rBC diameters ranging from 70 to 220 nm. This type of data is useful for constraining models used for predicting rBC concentrations in the atmosphere.


2019 ◽  
Author(s):  
Aoxing Zhang ◽  
Yuhang Wang ◽  
Yuzhong Zhang ◽  
Rodney J. Weber ◽  
Yongjia Song ◽  
...  

Abstract. Carbonaceous aerosols significantly affect global radiative forcing and climate through absorption and scattering of sunlight. Black carbon (BC) and brown carbon (BrC) are light-absorbing carbonaceous aerosols. The direct radiative effect (DRE) of BrC is uncertain. A recent study suggests that BrC absorption is comparable to BC in the upper troposphere over biomass burning regions and that the resulting radiative heating tends to stabilize the atmosphere. Yet current climate models do not include proper physical and chemical treatments of BrC. In this study, we derived a BrC global biomass burning emission inventory on the basis of the Global Fire Emissions Database 4 (GFED4), developed a BrC module in the Community Atmosphere Model version 5 (CAM5) of Community Earth System Model (CESM) model, and investigated the photo-bleaching effect and convective transport of BrC on the basis of Studies of Emissions, Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) and Deep Convective Clouds and Chemistry Project (DC-3) measurements. The model simulations of BC were also evaluated using HIAPER (High-Performance Instrumented Airborne Platform for Environmental Research) Pole-to-Pole Observations (HIPPO) measurements. We found that globally BrC is a significant absorber, the DRE of which is 0.10 W/m2, more than 25 % of BC DRE (+0.39 W/m2). Most significantly, model results indicated that BrC atmospheric heating in the tropical mid and upper troposphere is larger than that of BC. The source of tropical BrC is mainly from wildfires, which are more prevalent in the tropical regions than higher latitudes and release much more BrC relative to BC than industrial sources. While BC atmospheric heating is skewed towards northern mid-latitude lower atmosphere, BrC heating is more centered in the tropical free troposphere. The contribution of BrC heating to the Hadley circulation and latitudinal expansion of the tropics is comparable to BC heating.


Sign in / Sign up

Export Citation Format

Share Document