Undersizing of aged African biomass burning aerosol by an ultra-high-sensitivity aerosol spectrometer
Explore the source record for details and available documents.
54 ENVIRONMENTAL SCIENCES↗
SEARCH · Search NASA
Results for “aerosol aging”
Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.
Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.
Marine Shallow Cloud Adjustments to the Presence of Shortwave-Absorbing Aerosols: Advancing Understanding Through a Combined Analysis of Lasic Datasets and Process Modeling (Final Report)
This is a final report for this award, whose purpose was to support the analysis of data emanating from the LASIC (Layered Atlantic Smoke Interaction with Clouds) campaign. (Layered Atlantic Smoke Interactions with Clouds) is a strategy to improve our understanding of aged carbonaceous aerosol, its seasonal evolution, and the mechanisms by which clouds adjust to the presence of the aerosol. The observational strategy centers on deploying the AMF1 cloud, aerosol, and atmospheric profiling instrumentation to Ascension Island, located within the trade-wind shallow cumulus regime (14.50W, 80S) 3000 km offshore of continental Africa. The location is within the latitude zone of the maximum outflow of aerosol, with the deepening boundary layer known to entrain free-tropospheric smoke. The primary activities for LASIC are: 1) to improve current knowledge on aged biomass burning aerosol and its radiative properties as a function of the seasonal cycle; 2) to use surface-based remote sensing to sensitively interrogate the atmosphere for the relative vertical location of aerosol and clouds; 3) to improve our understanding of the cloud adjustments to the presence of shortwave-absorbing aerosol within the vertical column, both through aerosol-radiation and through aerosol-cloud interactions; 4) to aid low cloud parameterization efforts for climate models. This award serves to further these activities and includes a sub-award to Dr. Pablo Saide at UCLA for activities 3) and 4).
54 ENVIRONMENTAL SCIENCES↗
Ocean observations with EOS/MODIS: Algorithm development and post launch studies
Several significant accomplishments were made during the present reporting period. (1) Initial simulations to understand the applicability of the MODerate Resolution Imaging Spectrometer (MODIS) 1380 nm band for removing the effects of stratospheric aerosols and thin cirrus clouds were completed using a model for an aged volcanic aerosol. The results suggest that very simple procedures requiring no a priori knowledge of the optical properties of the stratospheric aerosol may be as effective as complex procedures requiring full knowledge of the aerosol properties, except the concentration which is estimated from the reflectance at 1380 nm. The limitations of this conclusion will be examined in the next reporting period; (2) The lookup tables employed in the implementation of the atmospheric correction algorithm have been modified in several ways intended to improve the accuracy and/or speed of processing. These have been delivered to R. Evans for implementation into the MODIS prototype processing algorithm for testing; (3) A method was developed for removal of the effects of the O2 'A' absorption band from SeaWiFS band 7 (745-785 nm). This is important in that SeaWiFS imagery will be used as a test data set for the MODIS atmospheric correction algorithm over the oceans; and (4) Construction of a radiometer, and associated deployment boom, for studying the spectral reflectance of oceanic whitecaps at sea was completed. The system was successfully tested on a cruise off Hawaii on which whitecaps were plentiful during October-November. This data set is now under analysis.
Gordon, Howard R.↗
Modeling Volatility-Based Aerosol Phase State Predictions in the Amazon Rainforest
Organic aerosol (OA) is a complex matrix of various constituents—fresh (primary organic aerosols—POA) and aged via oxidation (secondary organic aerosols—SOA), generated from biogenic, anthropogenic, and biomass burning sources. The viscosity of OA can be critical in influencing new particle formation, reactive uptake processes that impact evaporation-growth kinetics, and the lifetime of particles in the atmosphere. We report this work utilizes a well-defined relationship between volatility and viscosity for pure compounds, which we incorporated within the Weather Research and Forecasting Model coupled to chemistry (WRF-Chem) to simulate the phase state and viscosity of bulk OA during the dry-to-wet transition season (September–October) in the Amazon rainforest during 2014. Our simulations indicate spatial and temporal heterogeneity in aerosol phase state often not captured by global-scale models. We show the strong role of water associated with organic aerosol ($w_s$) as the dominant factor that can be used to quantitatively estimate OA viscosity. Analysis of WRF-Chem simulations across the entire atmospheric column indicates a strong inverse log-linear relationship between $w_s$ and OA viscosity with a correlation coefficient approaching 1, in the background and biomass burning-influenced conditions. At high altitudes where relative humidity (RH) and temperatures are low, our simulations indicate that OA exists in a semisolid-/solid-like phase state, consistent with previous studies. OA hygroscopicity is strongly correlated (ca. –0.8) with OA viscosity at RH ca. 30–50%, but this RH range is found mostly at low OA concentrations and the middle troposphere (ca. 6–10 km altitudes) in our simulated domain. OA hygroscopicity is uncorrelated with viscosity at higher-RH (near surface) and lower-RH (upper troposphere) regimes. At the urban site near surface, where day–night differences in RH are significant, RH is found to drive the phase state. At the background forested site near surface, where day–night RH differences are small, biomass burning-influenced OA is semisolid and a significant OA associated with background conditions is liquid-like. Simulations indicate a long tail of OA viscosity frequency distributions extending in the semisolid/solid regimes over background biogenic-influenced conditions due to the role of low-volatility OA components such as monoterpene oxidation products.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
African dust transported to Barbados in the wintertime lacks indicators of chemical aging
The chemical processing (“aging”) of mineral dust is thought to increase dust light-scattering efficiency, cloud droplet activation, and nutrient solubility. However, the extent of African dust aging during long-range transport to the western Atlantic is poorly understood. Here, we explore African dust aging in wintertime samples collected from Barbados when dust is transported at lower altitudes. Ion chromatography (IC) analysis indicates that the mass concentrations of bulk nitrate, sulfate, and oxalate increase, relative to background conditions, when African dust reaches Barbados after transatlantic transport, indicating dust aging. However, aerosol mixing-state analysis from computer-controlled scanning electron microscopy with energy dispersive X-ray spectroscopy (CCSEM/EDX) indicates that approximately 67 % of dust particles are internally mixed with sea salt, while only about 26 % of dust particles contain no internally mixed components. SEM/EDX elemental mapping and time-of-flight secondary ion mass spectrometry (TOF-SIMS) reveals that within internally mixed dust and sea salt particles, only sea salt components contain signs of aging as indicated by the loss of chloride and acquisition of nitrate and/or sulfate. Our results suggest that chemical aging may only modestly increase the solubility of nutrients in African dust during long-range transport. Because most dust that we measured was internally mixed with sea salt, chemical aging is not necessarily required to increase the hygroscopicity of dust, at least in the lower boundary layer. Further, our findings have implications for understanding the release of halogens from sea salts, which may be enhanced in internally mixed dust and sea salt particles.
54 ENVIRONMENTAL SCIENCES↗
Novel Application of Machine Learning Techniques for Rapid Source Apportionment of Aerosol Mass Spectrometer Datasets
In this work, we apply machine learning approaches sparse multinomial logistic regression to classify aerosol mass spectrometer (AMS) unit mass resolution (UMR) data followed by an ensemble regression technique for source apportionment of organic aerosols (OA). The classifier was trained on 60 well characterized laboratory and positive matrix factorization (PMF) deconvolved reference spectra to identify eight OA types. These include four laboratory-derived secondary organic aerosol (SOA) spectra, which include isoprene photooxidation SOA, isoprene epoxydiols (IEPOX) SOA, a monoterpene SOA type that includes a-pinene and ß-pinene SOA, and aromatic SOA from oxidation of naphthalene and m-xylene precursors, as well as PMF deconvolved spectra for three primary organic aerosol (POA) types, namely, hydrocarbon-like organic aerosol (HOA), biomass burning organic aerosol (BBOA), and cooking OA (COA), and a more oxidized oxygenated OA type (MO-OOA). A 5-fold cross-validation strategy, repeated 10 times, was used to assess the classifier’s performance. The classifier had high classification accuracy for COA, aromatic SOA, and isoprene SOA spectra but incorrectly classified ~9% by number of MO-OOA spectra as BBOA, 12% of BBOA spectra as HOA (and vice versa), and 18% of IEPOX-SOA spectra as aromatic SOA. Next, an ensemble regression model was trained on an artificially generated dataset consisting of mixtures of different OA types to assess its ability to predict fractional mass abundances from classification probabilities of various OA species obtained from the multinomial logistic regression classifier trained on the reference spectra. Ultimately, the proposed approach was applied for source apportionment of aircraft-based AMS measurements of OA UMR spectra during the HI-SCALE field campaign. On two representative days (May 6th and 18th, 2016), the algorithm determined that ~50-60% of OA by mass was MO-OOA, which represented a highly aged organic aerosol mixture from different sources. On both days, BBOA was determined to contribute less than 10% to OA by mass. However, on May 18th, the aromatic SOA fraction was higher compared to that on May 6th. The proposed approach is capable of rapidly analyzing AMS data in real time, making it suitable for applications where rapid source apportionment of AMS OA spectra is desirable.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Individual Aerosol Particles from Biomass Burning in Southern Africa Compositions and Aging of Inorganic Particles: Compositions and Aging of Inorganic Particles - 2
Individual aerosol particles collected over southern Africa during the SAFARI 2000 field study were studied using transmission electron microscopy and field-emission scanning electron microscopy. The sizes, shapes, compositions, mixing states, surface coatings, and relative abundances of aerosol particles from biomass burning, in boundary layer hazes, and in the free troposphere were compared, with emphasis on aging and reactions of inorganic smoke particles. Potassium salts and organic particles were the predominant species in the smoke, and most were internally mixed. More KCl particles occur in young smoke, whereas more K2SO4 and KNO3 particles were present in aged smoke. This change indicates that with the aging of the smoke, KCl particles from the fires were converted to K2SO4 and KNO3 through reactions with sulfur- and nitrogen- bearing species from biomass burning as well as other sources. More soot was present in smoke from flaming grass fires than bush and wood fires, probably due to the predominance of flaming combustion in grass fires. The high abundance of organic particles and soluble salts can affect the hygroscopic properties of biomass-burning aerosols and therefore influence their role as cloud condensation nuclei. Particles from biomass burning were important constituents of the regional hazes.
Li, Jia↗
Biomass burning and marine aerosol processing over the southeast Atlantic Ocean: a TEM single-particle analysis
This study characterizes single-particle aerosol composition from filters collected during the ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) and CLoud–Aerosol–Radiation Interaction and Forcing: Year 2017 (CLARIFY-2017) campaigns. In particular the study describes aged biomass burning aerosol (BBA), its interaction with the marine boundary layer and the influence of biomass burning (BB) air on marine aerosol. The study finds evidence of BBA influenced by marine boundary layer processing as well as sea salt influenced by BB air. Secondary chloride aerosols were observed in clean marine air as well as in BB-influenced air in the free troposphere. Higher-volatility organic aerosol appears to be associated with increased age of biomass burning plumes, and photolysis or oxidation may be a mechanism for the apparent increased volatility. Aqueous processing and interaction with the marine boundary layer air may be a mechanism for the presence of sodium on many aged potassium salts. By number, biomass burning potassium salts and modified sea salts are the most observed particles on filter samples. The most commonly observed BC coatings are inorganic salts. These results suggest that atmospheric processes such as photolysis, oxidation and cloud processing are key drivers in the elemental composition and morphology of aged BBA. Fresh BBA inorganic salt content, as it has an important role in the particles' ability to uptake water, may be a key driver in how aqueous processing and atmospheric aging proceed.
54 ENVIRONMENTAL SCIENCES↗
Chemical composition of the atmospheric aerosol in the troposphere over the Hudson Bay lowlands and Quebec-Labrador regions of Canada
Atmospheric aerosols were collected in the boundary layer and free troposphere over continental and coastal subarctic regions of Canada during the July - August 1990 joint U.S.-Canadian Arctic Boundary Layer Expedition (ABLE) 3B/Northern Wetlands Study (NOWES). The samples were analyzed for the following water soluble species: sulfate, nitrate, ammonium, potassium, sodium, chloride, oxalate, methylsulfonate, and total amine nitrogen. Ammonium and sulfate were the major water soluble components of these aerosols. The nearly neutral (overall) chemical composition of summertime aerosol particles contrasts their strongly acidic wintertime composition. Aerosol samples were separated into several air mass categories and characterized in terms of chemical composition, associated mixing ratios of gaseous compounds, and meteorological parameters. The fundamental category represented particles associated with 'background' air masses. The summertime atmospheric aerosols in background air over the North American subarctic and Arctic regions were characterized by relatively small and spatially uniform mixing ratios of the measured species. These aerosol particles were aged to the extent that they had lost their primary source signature. The chemical profile of the background air aerosols was frequently modified by additions from biomass fire plumes, aged tropical marine air, and intrusions of upper tropospheric/lower stratospheric air. Aerosols in boundary layer background air over the boreal forest region of Quebec-Labrador had significantly larger mixing ratios of ammonium and sulfate relative to the Hudson Bay region. This may reflect infiltration of anthropogenic pollution or be due to natural emissions from this region.
Gorzelska, K.↗
Interfacial Dark Aging Is an Overlooked Source of Aqueous Secondary Organic Aerosol
In this work, the relative yields of aqueous secondary organic aerosols (aqSOAs) at the air–liquid (a–l) interface are investigated between photochemical and dark aging using in situ time-of-flight secondary ion mass spectrometry (ToF-SIMS). Our results show that dark aging is an important source of aqSOAs despite a lack of photochemical drivers. Photochemical reactions of glyoxal and hydroxyl radicals (•OH) produce oligomers and cluster ions at the aqueous surface. Interestingly, different oligomers and cluster ions form intensely in the dark at the a–l interface, contrary to the notion that oligomer formation mainly depends on light irradiation. Furthermore, cluster ions form readily during dark aging and have a higher water molecule adsorption ability. This finding is supported by the observation of more frequent organic water cluster ion formation. The relative yields of water clusters in the form of protonated and hydroxide ions are presented using van Krevelen diagrams to explore the underlying formation mechanisms of aqSOAs. Large protonated and hydroxide water clusters (e.g., (H2O)nH+, 17 < n ≤ 44) have reasonable yields during UV aging. In contrast, small protonated and hydroxide water clusters (e.g., (H2O)nH+, 1 ≤ n ≤ 17) form after several hours of dark aging. Moreover, cluster ions have higher yields in dark aging, indicating the overlooked influence of dark aging interfacial products on aerosol optical properties. Molecular dynamic simulation shows that cluster ions form stably in UV and dark aging. AqSOAs molecules produced from dark and photochemical aging can enhance UV absorption of the aqueous surface, promote cloud condensation nuclei (CCN) activities, and affect radiative forcing.
Van Krevelen diagram↗
Studies of optical and chemical properties of aged and fresh biomass burning absorbing aerosols for climate models
Particulate emissions from burning fuels from sub-Saharan Africa is currently poorly characterized. With increasing population and industrialization, emissions are expected to grow. Optical methods for measuring light absorption in the ultraviolet (UV) and visible (vis) regions of the spectrum are crucial for understanding the optical properties of BB aerosols (Bond and Bergstrom, 2006; Lack and Cappa, 2010; Moschos et al., 2021). One such instrument is the dual-spot AE33 model aethalometer is a common filter-based instrument that can be used to measure aerosol absorption properties (Hansen et al., 1984). This instrument has many figures of merit; however, the method's limitations include potential biases from scattering within the filter material, multiple scattering effects of the particles, filter loading (i.e. particle shadowing), and the need for wavelength-specific correction factors (Cλ), which depend on accurate intercomparison with other in situ techniques (Bond et al., 1999; Collaud Coen et al., 2010). This work aims to: 1. Optically characterize BB aerosol generated from African fuel 2. Correct the aethalometer at multiple wavelengths 3. Parametrize these correction factors. 4. Combusting the same fuels with two difference tube furnace systems assess the general applicability of this flexible means of producing BB aerosol. This was accomplished by conducting laboratory studies at Los Alamos National Laboratory (LANL) and North Carolina A&T State University (NCA&T), where aethalometer measurements were compared to in situ optical measurements. Mass cross sections of BB aerosol from these under-studied fuels will be determined along with their wavelength dependence.
09 BIOMASS FUELS↗
Validation and Expected Error Estimation of Suomi-NNP VIIRS Aerosol Optical Thickness and Angstrom Exponent with AERONET
The new-generation polar-orbiting operational environmental sensor, the Visible Infrared Imaging Radiometer Suite (VIIRS) on board the Suomi National Polar-orbiting Partnership (S-NPP) satellite, provides critical daily global aerosol observations. As older satellite sensors age out, the VIIRS aerosol product will become the primary observational source for global assessments of aerosol emission and transport, aerosol meteorological and climatic effects, air quality monitoring, and public health. To prove their validity and to assess their maturity level, the VIIRS aerosol products were compared to the spatiotemporally matched Aerosol Robotic Network (AERONET)measurements. Over land, the VIIRS aerosol optical thickness (AOT) environmental data record (EDR) exhibits an overall global bias against AERONET of 0.0008 with root-mean-square error(RMSE) of the biases as 0.12. Over ocean, the mean bias of VIIRS AOT EDR is 0.02 with RMSE of the biases as 0.06.The mean bias of VIIRS Ocean Angstrom Exponent (AE) EDR is 0.12 with RMSE of the biases as 0.57. The matchups between each product and its AERONET counterpart allow estimates of expected error in each case. Increased uncertainty in the VIIRS AOT and AE products is linked to specific regions, seasons, surface characteristics, and aerosol types, suggesting opportunity for future modifications as understanding of algorithm assumptions improves. Based on the assessment, the VIIRS AOT EDR over land reached Validated maturity beginning 23 January 2013; the AOT EDR and AE EDR over ocean reached Validated maturity beginning 2 May 2012, excluding the processing error period 15 October to 27 November 2012. These findings demonstrate the integrity and usefulness of the VIIRS aerosol products that will transition from S-NPP to future polar-orbiting environmental satellites in the decades to come and become the standard global aerosol data set as the previous generations missions come to an end.
Huang, Jingfeng↗
Effects of El Chichon on stratospheric aerosols late 1982 to early 1984
Stratospheric aerosols collected over the western U.S. from late 1982 to early 1984 show the strong effects of El Chichon's eruption. Although mineral particles disappeared during this period, large acid droplets were still common. Because these have never been seen in prevolcanic, background-level collections, they apparently result from increased droplet growth made possible by the unusual abundance of sulfate. Aerosol size distributions show a wide variety of multimodal curves due to mixing of air masses containing aerosols of various ages or histories. Toward the end of the study time there are fewer large aerosols because of gravitational settling and poleward transport. The result is a steady reduction in sulfate, as most aerosol mass is concentrated in a small number of large droplets. Even the later sulfate levels are, however, five times typical prevolcanic background contents. Thus the influence of El Chichon on high-altitude was still considerable 22 months after eruption.
Snetsinger, K. G.↗
Water-soluble Organic Components in Aerosols Associated with Savanna Fires in Southern Africa: Identification, Evolution and Distribution
During the SAFARI 2000 field campaign, both smoke aerosols from savanna fires and haze aerosols in the boundary layer and in the free troposphere were collected from an aircraft in southern Africa. These aerosol samples were analyzed for their water-soluble chemical components, particularly the organic species. A novel technique, electrospray ionization-ion trap mass spectrometry, was used concurrently with an ion chromatography system to analyze for carbohydrate species. Seven carbohydrates, seven organic acids, five metallic elements, and three inorganic anions were identified and quantified. On the average, these 22 species comprised 36% and 27% of the total aerosol mass in haze and smoke aerosols, respectively. For the smoke aerosols, levoglucosan was the most abundant carbohydrate species, while gluconic acid was tentatively identified as the most abundant organic acid. The mass abundance and possible source of each class of identified species are discussed, along with their possible formation pathways. The combustion phase of a fire had an impact on the chemical composition of the emitted aerosols. Secondary formation of sulfate, nitrate, levoglucosan, and several organic acids occurred during the initial aging of smoke aerosols. It is likely that under certain conditions, some carbohydrate species in smoke aerosols, such as levoglucosan, were converted to organic acids during upward transport.
Gao, Song↗
Observations of Smoke Aerosol from Biomass Burning in Mexico: Effect of Particle Aging on Radiative Forcing and Remote Sensing
We take advantage of the May 1998 biomass burning event in Southern Mexico to test the global applicability of a smoke aerosol size model developed from data observed in South America. The Mexican event is an unique opportunity to observe well-aged, residual smoke. Observations of smoke aerosol size distribution made from vertical profiles of airborne in situ measurements show an inverse relationship between concentration and particle size that suggests the aging process continues more than a week after the smoke is separated from its fire sources. The ground-based radiometer retrievals show that the column-averaged, aged, Mexican smoke particles are larger (diameter = 0.28 - 0.33 micrometers) than the mean smoke particles in South America (diameter = 0.22 - 0.30 micrometers). However, the difference (delta - 0.06 micrometer) translates into differences in backscattering coefficient of only 4-7% and an increase of direct radiative forcing of only 10%.
Remer, Lorraine A.↗
Cloud condensation nuclei characteristics at the Southern Great Plains site: role of particle size distribution and aerosol hygroscopicity
The activation ability of aerosols as cloud condensation nuclei (CCN) is crucial in climate and hydrological cycle studies, but their properties are not well known. We investigated the long-term measurements of atmospheric aerosol properties, CCN concentrations (N CCN ) at supersaturation (SS = 0.1%–1.0%), and hygroscopicity at the Department of Energy's Southern Great Plains (SGP) site to illustrate the dependence of N CCN on aerosol properties and transport pathways. Cluster analysis was applied to the back trajectories of air masses to investigate their respective source regions. The results showed that aged biomass burning aerosols from Central America were characterized by higher accumulation mode particles (N accu ; median value 805 cm -3 ) and relatively high aerosol hygroscopicity (κ; median value ~0.25) values that result in the higher CCN activation and relatively high N CCN (median value 258–1578 cm -3 at a SS of 0.1%–1.0%). Aerosols from the Gulf of Mexico were characterized by higher N accu (~35%), and N CCN (230–1721 cm -3 at a SS of 0.1%–1.0%) with the lowest κ (~0.17). In contrast, relatively high nucleation mode particles (N nucl ; ~20%) and low N CCN (128–1553 cm -3 at a SS of 0.1%–1.0%) with higher κ (~0.30) values were observed on the aerosols associated with a westerly wind. The results indicate particle size as the most critical factor influencing the ability of aerosols to activate, whereas the effect of chemical composition was secondary. Our CCN closure analysis suggests that chemical composition and mixing state information are more crucial at lower SS, whereas at higher SS, most particles become activated regardless of their chemical composition and size. This study affirms that soluble organic fraction information is required at higher SS for better N CCN prediction, but both the soluble organics fraction and mixing state are vital to reduce the N CCN prediction uncertainty at lower SS.
54 ENVIRONMENTAL SCIENCES↗
An Empirical Characterization of the Aerosol Angstrom Exponent Interpolation Bias using SAGE III/ISS Data
This work uses multispectral measurements of vertically resolved aerosol extinction coefficients from the Stratospheric Aerosol and Gas Experiment (SAGE) III on the International Space Station (ISS) to demonstrate how the use of the Ångström exponent for interpolation of aerosol data between two different wavelengths creates a bias. An empirical relationship is derived between the magnitude of this bias and the Ångström exponent at several different SAGE wavelengths. This relationship can thus be used as a correction factor for other studies, such as multi-instrument intercomparisons or merging, that wish to convert aerosol data from one wavelength to another using the Ångström exponent and is applicable to all stratospheric non-cloud aerosol except highly aged particles that are evaporating at altitudes above the Junge layer.
Aerosol↗
Probing Atmospheric Aerosols by Multimodal Mass Spectrometry Techniques: Revealing Aging Characteristics of Its Individual Molecular Components
Explore the source record for details and available documents.
54 ENVIRONMENTAL SCIENCES↗