scholarly journals Atmospheric aging enhances the ice nucleation ability of biomass-burning aerosol

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.

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.


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 ◽  
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.


2002 ◽  
Vol 107 (D21) ◽  
pp. LAC 12-1-LAC 12-15 ◽  
Author(s):  
Markus Fiebig ◽  
Andreas Petzold ◽  
Ulla Wandinger ◽  
Manfred Wendisch ◽  
Christoph Kiemle ◽  
...  

2021 ◽  
Author(s):  
Igor B. Konovalov ◽  
Nikolai A. Golovushkin ◽  
Tatyana B. Zhuravleva ◽  
Ilmir M. Nastrdinov ◽  
Daria A. Lvova ◽  
...  

2015 ◽  
Vol 15 (5) ◽  
pp. 6771-6819
Author(s):  
J. H. Slade ◽  
R. Thalman ◽  
J. Wang ◽  
D. A. Knopf

Abstract. Multiphase OH and O3 oxidation reactions with atmospheric organic aerosol (OA) can influence particle physicochemical properties including composition, morphology, and lifetime. Chemical aging of initially insoluble or low soluble single-component OA by OH and O3 can increase their water-solubility and hygroscopicity, making them more active as cloud condensation nuclei (CCN) and susceptible to wet deposition. However, an outstanding problem is whether the effects of chemical aging on their CCN activity are preserved when mixed with other organic or inorganic compounds exhibiting greater water-solubility. In this work, the CCN activity of laboratory-generated biomass burning aerosol (BBA) surrogate-particles exposed to OH and O3 is evaluated by determining the hygroscopicity parameter, κ, as a function of particle type, mixing state, and OH/O3 exposure applying a CCN counter (CCNc) coupled to an aerosol flow reactor (AFR). Levoglucosan (LEV), 4-methyl-5-nitrocatechol (MNC), and potassium sulfate (KS) serve as representative BBA compounds that exhibit different hygroscopicity, water solubility, chemical functionalities, and reactivity with OH radicals, and thus exemplify the complexity of mixed inorganic/organic aerosol in the atmosphere. The CCN activities of all of the particles were unaffected by O3 exposure. Following exposure to OH, κ of MNC was enhanced by an order of magnitude, from 0.009 to ~0.1, indicating that chemically-aged MNC particles are better CCN and more prone to wet deposition than pure MNC particles. No significant enhancement in κ was observed for pure LEV particles following OH exposure. κ of the internally-mixed particles was not affected by OH oxidation. Furthermore, the CCN activity of OH exposed MNC-coated KS particles is similar to the OH unexposed atomized 1 : 1 by mass MNC : KS binary-component particles. Our results strongly suggest that when OA is dominated by water-soluble organic carbon (WSOC) or inorganic ions, chemical aging has no significant impact on OA hygroscopicity. The organic compounds exhibiting low solubility behave as if they are infinitely soluble when mixed with a sufficient amount of water-soluble compounds. At and beyond this point, the particles' CCN activity is governed entirely by the water-soluble fraction and not influenced by the oxidized organic fraction. Our results have important implications for heterogeneous oxidation and its impact on cloud formation given that atmospheric aerosol is a complex mixture of organic and inorganic compounds exhibiting a wide-range of solubilities.


2013 ◽  
Vol 13 (5) ◽  
pp. 11509-11536 ◽  
Author(s):  
R. Saleh ◽  
C. J. Hennigan ◽  
G. R. McMeeking ◽  
W. K. Chuang ◽  
E. S. Robinson ◽  
...  

Abstract. Experiments were conducted to investigate light absorption of organic aerosol (OA) in fresh and photo-chemically aged biomass-burning emissions. The experiments considered residential hardwood fuel (oak) and fuels commonly consumed in wild-land and prescribed fires in the United States (pocosin pine and gallberry). Photo-chemical aging was performed in an environmental chamber. We constrained the light-absorption properties of the OA using conservative limiting assumptions, and found that both primary organic aerosol (POA) in the fresh emissions and secondary organic aerosol (SOA) produced by photo-chemical aging absorb light to a significant extent, and are categorized as brown carbon. This work presents the first direct evidence that SOA produced in aged biomass-burning emissions is absorptive. For the investigated fuels, SOA is less absorptive than POA in the long visible, but exhibits steeper wavelength-dependence (larger Absorption Ångström Exponent) and is more absorptive in the short visible and near-UV. Light absorption by SOA in biomass-burning emissions might be an important contributor to the global radiative forcing budget.


2015 ◽  
Vol 15 (17) ◽  
pp. 10183-10201 ◽  
Author(s):  
J. H. Slade ◽  
R. Thalman ◽  
J. Wang ◽  
D. A. Knopf

Abstract. Multiphase OH and O3 oxidation reactions with atmospheric organic aerosol (OA) can influence particle physicochemical properties including composition, morphology, and lifetime. Chemical aging of initially insoluble or low-soluble single-component OA by OH and O3 can increase their water solubility and hygroscopicity, making them more active as cloud condensation nuclei (CCN) and susceptible to wet deposition. However, an outstanding problem is whether the effects of chemical aging on their CCN activity are preserved when mixed with other organic or inorganic compounds exhibiting greater water solubility. In this work, the CCN activity of laboratory-generated biomass burning aerosol (BBA) surrogate particles exposed to OH and O3 is evaluated by determining the hygroscopicity parameter, κ, as a function of particle type, mixing state, and OH and O3 exposure applying a CCN counter (CCNc) coupled to an aerosol flow reactor (AFR). Levoglucosan (LEV), 4-methyl-5-nitrocatechol (MNC), and potassium sulfate (KS) serve as representative BBA compounds that exhibit different hygroscopicity, water solubility, chemical functionalities, and reactivity with OH radicals, and thus exemplify the complexity of mixed inorganic/organic aerosol in the atmosphere. The CCN activities of all of the particles were unaffected by O3 exposure. Following exposure to OH, κ of MNC was enhanced by an order of magnitude, from 0.009 to ~ 0.1, indicating that chemically aged MNC particles are better CCN and more prone to wet deposition than pure MNC particles. No significant enhancement in κ was observed for pure LEV particles following OH exposure. κ of the internally mixed particles was not affected by OH oxidation. Furthermore, the CCN activity of OH-exposed MNC-coated KS particles is similar to the OH unexposed atomized 1 : 1 by mass MNC : KS binary-component particles. Our results strongly suggest that when OA is dominated by water-soluble organic carbon (WSOC) or inorganic ions, chemical aging has no significant impact on OA hygroscopicity. The organic compounds exhibiting low solubility behave as if they are infinitely soluble when mixed with a sufficient number of water-soluble compounds. At and beyond this point, the particles' CCN activity is governed entirely by the water-soluble fraction and is not influenced by the oxidized organic fraction. Our results have important implications for heterogeneous oxidation and its impact on cloud formation given that atmospheric aerosol is a complex mixture of organic and inorganic compounds exhibiting a wide range of solubilities.


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