Urban organic aerosols measured by single particle mass spectrometry in the megacity of London

NASA Astrophysics Data System (ADS)

Dall'Osto, M.; Harrison, R. M.

2012-05-01

During the month of October 2006, as part of the REPARTEE-I experiment (Regent's Park and Tower Environmental Experiment) an Aerosol Time-Of-Flight Mass Spectrometer (ATOFMS) was deployed at an urban background location in the city of London, UK. Fifteen particle types were classified, some of which were already discussed (Dall'Osto et al., 2009a,b; Harrison et al., 2012). In this manuscript the origins and properties of four unreported particle types postulated to be due to locally generated aerosols, independent of the air mass type advected into London, are examined. One particle type, originating from lubricating oil (referred to as Ca-EC), was associated with morning rush hour traffic emissions. A second particle type, composed of both inorganic and organic species (called Na-EC-OC), was found enhanced in particle number concentration during evening time periods, and is likely to originate from a source operating at this time of day, or more probably from condensation of semi-volatile species. A third class, internally mixed with organic carbon and sulphate (called OC), was found to spike both in the morning and evenings although it could not unambiguously associated with a specific source or atmospheric process. The fourth class (Secondary Organic Aerosols - Polycyclic Aromatic Hydrocarbon; SOA-PAH) exhibited maximum frequency during the warmest part of the day, and a number of factors point towards secondary aerosol production from traffic-related volatile aromatic compounds. Single particle mass spectra of this particle type showed an oxidized polycyclic aromatic compound signature. A comparison of ATOFMS particle class data is then made with factors obtained by Positive Matrix Factorization and PAH signatures obtained from Aerosol Mass Spectrometer (AMS) data (Allan et al., 2010). Both the Ca-EC and OC particle types correlate with primary Hydrocarbon-like Organic Aerosol (HOA, R2 = 0.65 and 0.50 respectively), and Na-EC-OC correlates weakly with the AMS

Expanding Single Particle Mass Spectrometer Analyses for the Identification of Microbe Signatures in Sea Spray Aerosol.

PubMed

Sultana, Camille M; Al-Mashat, Hashim; Prather, Kimberly A

2017-10-03

Ocean-derived microbes in sea spray aersosol (SSA) have the potential to influence climate and weather by acting as ice nucleating particles in clouds. Single particle mass spectrometers (SPMSs), which generate in situ single particle composition data, are excellent tools for characterizing aerosols under changing environmental conditions as they can provide high temporal resolution and require no sample preparation. While SPMSs have proven capable of detecting microbes, these instruments have never been utilized to definitively identify aerosolized microbes in ambient sea spray aersosol. In this study, an aerosol time-of-flight mass spectrometer was used to analyze laboratory generated SSA produced from natural seawater in a marine aerosol reference tank. We present the first description of a population of biological SSA mass spectra (BioSS), which closely match the ion signatures observed in previous terrestrial microbe studies. The fraction of BioSS dramatically increased in the largest supermicron particles, consistent with field and laboratory measurements of microbes ejected by bubble bursting, further supporting the assignment of BioSS mass spectra as microbes. Finally, as supported by analysis of inorganic ion signals, we propose that dry BioSS particles have heterogeneous structures, with microbes adhered to sodium chloride nodules surrounded by magnesium-enriched coatings. Consistent with this structure, chlorine-containing ion markers were ubiquitous in BioSS spectra and identified as possible tracers for distinguishing recently aerosolized marine from terrestrial microbes.

Aerosol mass spectrometry: particle-vaporizer interactions and their consequences for the measurements

NASA Astrophysics Data System (ADS)

Drewnick, F.; Diesch, J.-M.; Faber, P.; Borrmann, S.

2015-09-01

The Aerodyne aerosol mass spectrometer (AMS) is a frequently used instrument for on-line measurement of the ambient sub-micron aerosol composition. With the help of calibrations and a number of assumptions on the flash vaporization and electron impact ionization processes, this instrument provides robust quantitative information on various non-refractory ambient aerosol components. However, when measuring close to certain anthropogenic or marine sources of semi-refractory aerosols, several of these assumptions may not be met and measurement results might easily be incorrectly interpreted if not carefully analyzed for unique ions, isotope patterns, and potential slow vaporization associated with semi-refractory species. Here we discuss various aspects of the interaction of aerosol particles with the AMS tungsten vaporizer and the consequences for the measurement results: semi-refractory components - i.e., components that vaporize but do not flash-vaporize at the vaporizer and ionizer temperatures, like metal halides (e.g., chlorides, bromides or iodides of Al, Ba, Cd, Cu, Fe, Hg, K, Na, Pb, Sr, Zn) - can be measured semi-quantitatively despite their relatively slow vaporization from the vaporizer. Even though non-refractory components (e.g., NH4NO3 or (NH4)2SO4) vaporize quickly, under certain conditions their differences in vaporization kinetics can result in undesired biases in ion collection efficiency in thresholded measurements. Chemical reactions with oxygen from the aerosol flow can have an influence on the mass spectra for certain components (e.g., organic species). Finally, chemical reactions of the aerosol with the vaporizer surface can result in additional signals in the mass spectra (e.g., WO2Cl2-related signals from particulate Cl) and in conditioning or contamination of the vaporizer, with potential memory effects influencing the mass spectra of subsequent measurements. Laboratory experiments that investigate these particle-vaporizer interactions are

Evaluation of Aerosol Mixing State Classes in the GISS Modele-matrix Climate Model Using Single-particle Mass Spectrometry Measurements

NASA Technical Reports Server (NTRS)

Bauer, Susanne E.; Ault, Andrew; Prather, Kimberly A.

2013-01-01

Aerosol particles in the atmosphere are composed of multiple chemical species. The aerosol mixing state, which describes how chemical species are mixed at the single-particle level, provides critical information on microphysical characteristics that determine the interaction of aerosols with the climate system. The evaluation of mixing state has become the next challenge. This study uses aerosol time-of-flight mass spectrometry (ATOFMS) data and compares the results to those of the Goddard Institute for Space Studies modelE-MATRIX (Multiconfiguration Aerosol TRacker of mIXing state) model, a global climate model that includes a detailed aerosol microphysical scheme. We use data from field campaigns that examine a variety of air mass regimens (urban, rural, and maritime). At all locations, polluted areas in California (Riverside, La Jolla, and Long Beach), a remote location in the Sierra Nevada Mountains (Sugar Pine) and observations from Jeju (South Korea), the majority of aerosol species are internally mixed. Coarse aerosol particles, those above 1 micron, are typically aged, such as coated dust or reacted sea-salt particles. Particles below 1 micron contain large fractions of organic material, internally-mixed with sulfate and black carbon, and few external mixtures. We conclude that observations taken over multiple weeks characterize typical air mass types at a given location well; however, due to the instrumentation, we could not evaluate mass budgets. These results represent the first detailed comparison of single-particle mixing states in a global climate model with real-time single-particle mass spectrometry data, an important step in improving the representation of mixing state in global climate models.

Source contributions to black carbon mass fractions in aerosol particles over the northwestern Pacific

NASA Astrophysics Data System (ADS)

Koga, Seizi; Maeda, Takahisa; Kaneyasu, Naoki

Aerosol particle number size distributions above 0.3 μm in diameter and black carbon mass concentrations in aerosols were observed on Chichi-jima of the Ogasawara Islands in the northwestern Pacific from January 2000 to December 2002. Chichi-jima is suitable to observe polluted air masses from East Asia in winter and clean air masses over the western North Pacific in summer. In winter, aerosols over Chichi-jima were strongly affected by anthropogenic emissions in East Asia. The form of energy consumption in East Asia varies in various regions. Hence, each source region is expected to be characterized by an individual black carbon mass fraction. A three-dimensional Eulerian transport model was used to estimate contribution rates to air pollutants from each source region in East Asia. Because the Miyake-jima eruption began at the end of June 2000, the influence of smokes from Miyake-jima was also considered in the model calculation. The results of model calculations represent what must be noticed about smokes from volcanoes including Miyake-jima to interpret temporal variations of sulfur compounds over the northwestern Pacific. To evaluate black carbon mass fractions in anthropogenic aerosols as a function of source region, the relationships between the volume concentration of aerosol particles and the black carbon mass concentration in the winter were classified under each source region in East Asia. Consequently, the black carbon mass fractions in aerosols from China, Japan and the Korean Peninsula, and other regions were estimated to be 9-13%, 5-7%, and 4-5%, respectively.

A Miniature System for Separating Aerosol Particles and Measuring Mass Concentrations

PubMed Central

Liang, Dao; Shih, Wen-Pin; Chen, Chuin-Shan; Dai, Chi-An

2010-01-01

We designed and fabricated a new sensing system which consists of two virtual impactors and two quartz-crystal microbalance (QCM) sensors for measuring particle mass concentration and size distribution. The virtual impactors utilized different inertial forces of particles in air flow to classify different particle sizes. They were designed to classify particle diameter, d, into three different ranges: d < 2.28 μm, 2.28 μm ≤ d ≤ 3.20 μm, d > 3.20 μm. The QCM sensors were coated with a hydrogel, which was found to be a reliable adhesive for capturing aerosol particles. The QCM sensor coated with hydrogel was used to measure the mass loading of particles by utilizing its characteristic of resonant frequency shift. An integrated system has been demonstrated. PMID:22319317

Mass spectra features of biomass burning boiler and coal burning boiler emitted particles by single particle aerosol mass spectrometer.

PubMed

Xu, Jiao; Li, Mei; Shi, Guoliang; Wang, Haiting; Ma, Xian; Wu, Jianhui; Shi, Xurong; Feng, Yinchang

2017-11-15

In this study, single particle mass spectra signatures of both coal burning boiler and biomass burning boiler emitted particles were studied. Particle samples were suspended in clean Resuspension Chamber, and analyzed by ELPI and SPAMS simultaneously. The size distribution of BBB (biomass burning boiler sample) and CBB (coal burning boiler sample) are different, as BBB peaks at smaller size, and CBB peaks at larger size. Mass spectra signatures of two samples were studied by analyzing the average mass spectrum of each particle cluster extracted by ART-2a in different size ranges. In conclusion, BBB sample mostly consists of OC and EC containing particles, and a small fraction of K-rich particles in the size range of 0.2-0.5μm. In 0.5-1.0μm, BBB sample consists of EC, OC, K-rich and Al_Silicate containing particles; CBB sample consists of EC, ECOC containing particles, while Al_Silicate (including Al_Ca_Ti_Silicate, Al_Ti_Silicate, Al_Silicate) containing particles got higher fractions as size increase. The similarity of single particle mass spectrum signatures between two samples were studied by analyzing the dot product, results indicated that part of the single particle mass spectra of two samples in the same size range are similar, which bring challenge to the future source apportionment activity by using single particle aerosol mass spectrometer. Results of this study will provide physicochemical information of important sources which contribute to particle pollution, and will support source apportionment activities. Copyright © 2017. Published by Elsevier B.V.

Characterization of urban aerosol in Cork city (Ireland) using aerosol mass spectrometry

NASA Astrophysics Data System (ADS)

Dall'Osto, M.; Ovadnevaite, J.; Ceburnis, D.; Martin, D.; Healy, R. M.; O'Connor, I. P.; Kourtchev, I.; Sodeau, J. R.; Wenger, J. C.; O'Dowd, C.

2013-05-01

Ambient wintertime background urban aerosol in Cork city, Ireland, was characterized using aerosol mass spectrometry. During the three-week measurement study in 2009, 93% of the ca. 1 350 000 single particles characterized by an Aerosol Time-of-Flight Mass Spectrometer (TSI ATOFMS) were classified into five organic-rich particle types, internally mixed to different proportions with elemental carbon (EC), sulphate and nitrate, while the remaining 7% was predominantly inorganic in nature. Non-refractory PM1 aerosol was characterized using a High Resolution Time-of-Flight Aerosol Mass Spectrometer (Aerodyne HR-ToF-AMS) and was also found to comprise organic aerosol as the most abundant species (62%), followed by nitrate (15%), sulphate (9%) and ammonium (9%), and chloride (5%). Positive matrix factorization (PMF) was applied to the HR-ToF-AMS organic matrix, and a five-factor solution was found to describe the variance in the data well. Specifically, "hydrocarbon-like" organic aerosol (HOA) comprised 20% of the mass, "low-volatility" oxygenated organic aerosol (LV-OOA) comprised 18%, "biomass burning" organic aerosol (BBOA) comprised 23%, non-wood solid-fuel combustion "peat and coal" organic aerosol (PCOA) comprised 21%, and finally a species type characterized by primary {m/z} peaks at 41 and 55, similar to previously reported "cooking" organic aerosol (COA), but possessing different diurnal variations to what would be expected for cooking activities, contributed 18%. Correlations between the different particle types obtained by the two aerosol mass spectrometers are also discussed. Despite wood, coal and peat being minor fuel types used for domestic space heating in urban areas, their relatively low combustion efficiencies result in a significant contribution to PM1 aerosol mass (44% and 28% of the total organic aerosol mass and non-refractory total PM1, respectively).

Mass-spectrometric identification of primary biological particle markers and application to pristine submicron aerosol measurements in Amazonia

NASA Astrophysics Data System (ADS)

Schneider, J.; Freutel, F.; Zorn, S. R.; Chen, Q.; Farmer, D. K.; Jimenez, J. L.; Martin, S. T.; Artaxo, P.; Wiedensohler, A.; Borrmann, S.

2011-11-01

The detection of primary biological material in submicron aerosol by means of thermal desorption/electron impact ionization aerosol mass spectrometry was investigated. Mass spectra of amino acids, carbohydrates, small peptides, and proteins, all of which are key building blocks of biological particles, were recorded in laboratory experiments. Several characteristic marker fragments were identified. The intensity of the marker signals relative to the total organic mass spectrum allows for an estimation of the content of primary biological material in ambient organic aerosol. The developed method was applied to mass spectra recorded during AMAZE-08, a field campaign conducted in the pristine rainforest of the central Amazon Basin, Brazil, during the wet season of February and March 2008. The low abundance of identified marker fragments places upper limits of 7.5% for amino acids and 5.6% for carbohydrates on the contribution of primary biological aerosol particles (PBAP) to the submicron organic aerosol mass concentration during this time period. Upper limits for the absolute submicron concentrations for both compound classes range from 0.01 to 0.1 μg m-3. Carbohydrates and proteins (composed of amino acids) make up for about two thirds of the dry mass of a biological cell. Thus, our findings suggest an upper limit for the PBAP mass fraction of about 20% to the submicron organic aerosol measured in Amazonia during AMAZE-08.

Criteria for significance of simultaneous presence of both condensible vapors and aerosol particles on mass transfer (deposition) rates

NASA Technical Reports Server (NTRS)

Gokoglu, S. A.

1987-01-01

The simultaneous presence of aerosol particles and condensible vapors in a saturated boundary layer which may affect deposition rates to subcooled surfaces because of vapor-particle interactions is discussed. Scavenging of condensible vapors by aerosol particles may lead to increased particle size and decreased vapor mass fraction, which alters both vapor and particle deposition rates. Particles, if sufficiently concentrated, may also coagulate. Criteria are provided to assess the significance of such phenomena when particles are already present in the mainstream and are not created inside the boundary layer via homogeneous nucleation. It is determined that there is direct proportionality with: (1) the mass concentration of both condensible vapors and aerosol particles; and (2) the square of the boundary layer thickness to particle diameter ratio (delta d sub p) square. Inverse proportionality was found for mainstream to surface temperature difference if thermophoresis dominates particle transport. It is concluded that the square of the boundary layer thickness to particle diameter ratio is the most critical factor to consider in deciding when to neglect vapor-particle interactions.

Criteria for significance of simultaneous presence of both condensible vapors and aerosol particles on mass transfer (deposition) rates

NASA Technical Reports Server (NTRS)

Gokoglu, S. A.

1986-01-01

The simultaneous presence of aerosol particles and condensible vapors in a saturated boundary layer which may affect deposition rates to subcooled surfaces because of vapor-particle interactions is discussed. Scavenging of condensible vapors by aerosol particles may lead to increased particle size and decreased vapor mass fraction, which alters both vapor and particle deposition rates. Particles, if sufficiently concentrated, may also coagulate. Criteria are provided to assess the significance of such phenomena when particles are already present in the mainstream and are not created inside the boundary layer via homogeneous nucleation. It is determined that there is direct proportionality with: (1) the mass concentration of both condensible vapors and aerosol particles; and (2) the square of the boundary layer thickness to particle diameter ratio (delta d sub p) square. Inverse proportionality was found for mainstream to surface temperature difference if thermophoresis dominates particle transport. It is concluded that the square of the boundary layer thickness to particle diameter ratio is the most critical factor to consider in deciding when to neglect vapor-particle interactions.

Microphysical processing of aerosol particles in orographic clouds

NASA Astrophysics Data System (ADS)

Pousse-Nottelmann, S.; Zubler, E. M.; Lohmann, U.

2015-01-01

An explicit and detailed treatment of cloud-borne particles allowing for the consideration of aerosol cycling in clouds has been implemented in the regional weather forecast and climate model COSMO. The effects of aerosol scavenging, cloud microphysical processing and regeneration upon cloud evaporation on the aerosol population and on subsequent cloud formation are investigated. For this, two-dimensional idealized simulations of moist flow over two bell-shaped mountains were carried out varying the treatment of aerosol scavenging and regeneration processes for a warm-phase and a mixed-phase orographic cloud. The results allowed to identify different aerosol cycling mechanisms. In the simulated non-precipitating warm-phase cloud, aerosol mass is incorporated into cloud droplets by activation scavenging and released back to the atmosphere upon cloud droplet evaporation. In the mixed-phase cloud, a first cycle comprises cloud droplet activation and evaporation via the Wegener-Bergeron-Findeisen process. A second cycle includes below-cloud scavenging by precipitating snow particles and snow sublimation and is connected to the first cycle via the riming process which transfers aerosol mass from cloud droplets to snow flakes. In the simulated mixed-phase cloud, only a negligible part of the total aerosol mass is incorporated into ice crystals. Sedimenting snow flakes reaching the surface remove aerosol mass from the atmosphere. The results show that aerosol processing and regeneration lead to a vertical redistribution of aerosol mass and number. However, the processes not only impact the total aerosol number and mass, but also the shape of the aerosol size distributions by enhancing the internally mixed/soluble accumulation mode and generating coarse mode particles. Concerning subsequent cloud formation at the second mountain, accounting for aerosol processing and regeneration increases the cloud droplet number concentration with possible implications for the ice

Microphysical processing of aerosol particles in orographic clouds

NASA Astrophysics Data System (ADS)

Pousse-Nottelmann, S.; Zubler, E. M.; Lohmann, U.

2015-08-01

An explicit and detailed treatment of cloud-borne particles allowing for the consideration of aerosol cycling in clouds has been implemented into COSMO-Model, the regional weather forecast and climate model of the Consortium for Small-scale Modeling (COSMO). The effects of aerosol scavenging, cloud microphysical processing and regeneration upon cloud evaporation on the aerosol population and on subsequent cloud formation are investigated. For this, two-dimensional idealized simulations of moist flow over two bell-shaped mountains were carried out varying the treatment of aerosol scavenging and regeneration processes for a warm-phase and a mixed-phase orographic cloud. The results allowed us to identify different aerosol cycling mechanisms. In the simulated non-precipitating warm-phase cloud, aerosol mass is incorporated into cloud droplets by activation scavenging and released back to the atmosphere upon cloud droplet evaporation. In the mixed-phase cloud, a first cycle comprises cloud droplet activation and evaporation via the Wegener-Bergeron-Findeisen (WBF) process. A second cycle includes below-cloud scavenging by precipitating snow particles and snow sublimation and is connected to the first cycle via the riming process which transfers aerosol mass from cloud droplets to snowflakes. In the simulated mixed-phase cloud, only a negligible part of the total aerosol mass is incorporated into ice crystals. Sedimenting snowflakes reaching the surface remove aerosol mass from the atmosphere. The results show that aerosol processing and regeneration lead to a vertical redistribution of aerosol mass and number. Thereby, the processes impact the total aerosol number and mass and additionally alter the shape of the aerosol size distributions by enhancing the internally mixed/soluble Aitken and accumulation mode and generating coarse-mode particles. Concerning subsequent cloud formation at the second mountain, accounting for aerosol processing and regeneration increases

Mixing state of particles with secondary species by single particle aerosol mass spectrometer in an atmospheric pollution event

NASA Astrophysics Data System (ADS)

Xu, Lingling; Chen, Jinsheng

2016-04-01

Single particle aerosol mass spectrometer (SPAMS) was used to characterize size distribution, chemical composition, and mixing state of particles in an atmospheric pollution event during 20 Oct. - 5 Nov., 2015 in Xiamen, Southeast China. A total of 533,012 particle mass spectra were obtained and clustered into six groups, comprising of industry metal (4.5%), dust particles (2.6%), carbonaceous species (70.7%), K-Rich particles (20.7%), seasalt (0.6%) and other particles (0.9%). Carbonaceous species were further divided into EC (70.6%), OC (28.5%), and mixed ECOC (0.9%). There were 61.7%, 58.3%, 4.0%, and 14.6% of particles internally mixed with sulfate, nitrate, ammonium and C2H3O, respectively, indicating that these particles had undergone significant aging processing. Sulfate was preferentially mixed with carbonaceous particles, while nitrate tended to mix with metal-containing and dust particles. Compared to clear days, the fractions of EC-, metal- and dust particles remarkably increased, while the fraction of OC-containing particles decreased in pollution days. The mixing state of particles, excepted for OC-containing particles with secondary species was much stronger in pollution days than that in clear days, which revealed the significant influence of secondary particles in atmospheric pollution. The different activity of OC-containing particles might be related to their much smaller aerodynamic diameter. These results could improve our understanding of aerosol characteristics and could be helpful to further investigate the atmospheric process of particles.

New approaches for the chemical and physical characterization of aerosols using a single particle mass spectrometry based technique

NASA Astrophysics Data System (ADS)

Spencer, Matthew Todd

Aerosols affect the lives of people every day. They can decrease visibility, alter cloud formation and cloud lifetimes, change the energy balance of the earth and are implicated in causing numerous health problems. Measuring the physical and chemical properties of aerosols is essential to understand and mitigate any negative impacts that aerosols might have on climate and human health. Aerosol time-of-flight mass spectrometry (ATOFMS) is a technique that measures the size and chemical composition of individual particles in real time. The goal of this dissertation is to develop new and useful approaches for measuring the physical and/or chemical properties of particles using ATOFMS. This has been accomplished using laboratory experiments, ambient field measurements and sometimes comparisons between them. A comparison of mass spectra generated from petrochemical particles was made to light duty vehicle (LDV) and heavy duty diesel vehicle (HDDV) particle mass spectra. This comparison has given us new insight into how to differentiate between particles from these two sources. A method for coating elemental carbon (EC) particles with organic carbon (OC) was used to generate a calibration curve for quantifying the fraction of organic carbon and elemental carbon on particles using ATOFMS. This work demonstrates that it is possible to obtain quantitative chemical information with regards to EC and OC using ATOFMS. The relationship between electrical mobility diameter and aerodynamic diameter is used to develop a tandem differential mobility analyzer-ATOFMS technique to measure the effective density, size and chemical composition of particles. The method is applied in the field and gives new insight into the physical/chemical properties of particles. The size resolved chemical composition of aerosols was measured in the Indian Ocean during the monsoonal transition period. This field work shows that a significant fraction of aerosol transported from India was from biomass

Characterization of urban aerosol in Cork City (Ireland) using aerosol mass spectrometry

NASA Astrophysics Data System (ADS)

Dall'Osto, M.; Ovadnevaite, J.; Ceburnis, D.; Martin, D.; Healy, R. M.; O'Connor, I. P.; Sodeau, J. R.; Wenger, J. C.; O'Dowd, C.

2012-11-01

Ambient wintertime background urban aerosol in Cork City, Ireland, was characterized using aerosol mass spectrometry. During the three-week measurement study in 2009, 93% of the 1 200 000 single particles characterized by an Aerosol Time-Of-Flight Mass Spectrometer (TSI ATOFMS) were classified into five organic-rich particle types, internally-mixed to different proportions with Elemental Carbon (EC), sulphate and nitrate while the remaining 7% was predominantly inorganic in nature. Non-refractory PM1 aerosol was also characterized using a High Resolution Time-Of-Flight Aerodyne Aerosol Mass Spectrometer (HR-ToF-AMS) and was also found to comprise organic matter as the most abundant species (62%), followed by nitrate (15%), sulphate (9%) and ammonium (9%), and then chloride (5%). Positive matrix factorization (PMF) was applied to the HR-ToF-AMS organic matrix and a five-factor solution was found to describe the variance in the data well. Specifically, "Hydrocarbon-like" Organic Aerosol (HOA) comprised 19% of the mass, "Oxygenated low volatility" Organic Aerosols (LV-OOA) comprised 19%, "Biomass wood Burning" Organic Aerosol (BBOA) comprised 23%, non-wood solid-fuel combustion "Peat and Coal" Organic Aerosol (PCOA) comprised 21%, and finally, a species type characterized by primary m/z peaks at 41 and 55, similar to previously-reported "Cooking" Organic Aerosol (COA) but possessing different diurnal variations to what would be expected for cooking activities, contributed 18%. Despite wood, cool and peat being minor fuel types used for domestic space heating in urban areas, their relatively low combustion efficiencies result in a significant contribution to PM1 aerosol mass (44% and 28% of the total organic aerosols mass and non refractory PM1, respectively).

Characterization of vertical aerosol flows by single particle mass spectrometry for micrometeorological analysis

NASA Astrophysics Data System (ADS)

Gelhausen, Elmar; Hinz, Klaus-Peter; Schmidt, Andres; Spengler, Bernhard

2011-10-01

A single particle mass spectrometer LAMPAS 2 (Laser Mass Analyzer for Particles in the Airborne State) was combined with an ultrasonic anemometer to provide a measurement system for monitoring environmental substance exchange as caused by emission/deposition of aerosol particles. For this study, 681 mass spectra of detected particles were sorted into groups of similarity by a clustering algorithm leading to five classes of different particle types. Each single mass spectrum was correlated to corresponding anemometer data (vertical wind vector and wind speed) in a time-resolved analysis. Due to sampling constraints time-resolution was limited to 36 s, as a result of transition time distributions through the sampling tube. Vertical particle flow (emission/deposition) was determined for all particles based on these data as acquired during a measuring campaign in Giessen, Germany. For a selected particle class a detailed up- and downwards flow consideration was performed to prove the developed approach. Particle flow of that class was dominated by an emission trend as expected. The presented combination of single-particle mass spectrometry and ultrasonic anemometry provides for the possibility to correlate chemical particle data and wind data in a distinct assignment for the description of turbulent particle behavior near earth surface. Results demonstrate the ability to apply the method to real micrometeorological systems, if sampling issues are properly considered for an intended time resolution.

Single particle mass spectral signatures from vehicle exhaust particles and the source apportionment of on-line PM2.5 by single particle aerosol mass spectrometry.

PubMed

Yang, Jian; Ma, Shexia; Gao, Bo; Li, Xiaoying; Zhang, Yanjun; Cai, Jing; Li, Mei; Yao, Ling'ai; Huang, Bo; Zheng, Mei

2017-09-01

In order to accurately apportion the many distinct types of individual particles observed, it is necessary to characterize fingerprints of individual particles emitted directly from known sources. In this study, single particle mass spectral signatures from vehicle exhaust particles in a tunnel were performed. These data were used to evaluate particle signatures in a real-world PM 2.5 apportionment study. The dominant chemical type originating from average positive and negative mass spectra for vehicle exhaust particles are EC species. Four distinct particle types describe the majority of particles emitted by vehicle exhaust particles in this tunnel. Each particle class is labeled according to the most significant chemical features in both average positive and negative mass spectral signatures, including ECOC, NaK, Metal and PAHs species. A single particle aerosol mass spectrometry (SPAMS) was also employed during the winter of 2013 in Guangzhou to determine both the size and chemical composition of individual atmospheric particles, with vacuum aerodynamic diameter (d va ) in the size range of 0.2-2μm. A total of 487,570 particles were chemically analyzed with positive and negative ion mass spectra and a large set of single particle mass spectra was collected and analyzed in order to identify the speciation. According to the typical tracer ions from different source types and classification by the ART-2a algorithm which uses source fingerprints for apportioning ambient particles, the major sources of single particles were simulated. Coal combustion, vehicle exhaust, and secondary ion were the most abundant particle sources, contributing 28.5%, 17.8%, and 18.2%, respectively. The fraction with vehicle exhaust species particles decreased slightly with particle size in the condensation mode particles. Copyright © 2017 Elsevier B.V. All rights reserved.

Biological particle analysis by mass spectrometry

NASA Technical Reports Server (NTRS)

Vilker, V. L.; Platz, R. M.

1983-01-01

An instrument that analyzes the chemical composition of biological particles in aerosol or hydrosol form was developed. Efforts were directed toward the acquisition of mass spectra from aerosols of biomolecules and bacteria. The filament ion source was installed on the particle analysis by mass spectrometry system. Modifications of the vacuum system improved the sensitivity of the mass spectrometer. After the modifications were incorporated, detailed mass spectra of simple compounds from the three major classes of biomolecules, proteins, nucleic acids, and carbohydrates were obtained. A method of generating bacterial aerosols was developed. The aerosols generated were collected and examined in the scanning electron microscope to insure that the bacteria delivered to the mass spectrometer were intact and free from debris.

The performance and the characterization of laser ablation aerosol particle time-of-flight mass spectrometry (LAAP-ToF-MS)

NASA Astrophysics Data System (ADS)

Gemayel, Rachel; Hellebust, Stig; Temime-Roussel, Brice; Hayeck, Nathalie; Van Elteren, Johannes T.; Wortham, Henri; Gligorovski, Sasho

2016-05-01

Hyphenated laser ablation-mass spectrometry instruments have been recognized as useful analytical tools for the detection and chemical characterization of aerosol particles. Here we describe the performances of a laser ablation aerosol particle time-of-flight mass spectrometer (LAAP-ToF-MS) which was designed for aerodynamic particle sizing using two 405 nm scattering lasers and characterization of the chemical composition of single aerosol particle via ablation/ionization by a 193 nm excimer laser and detection in a bipolar time-of-flight mass spectrometer with a mass resolving power of m/Δm > 600.

We describe a laboratory based optimization strategy for the development of an analytical methodology for characterization of atmospheric particles using the LAAP-ToF-MS instrument in combination with a particle generator, a differential mobility analyzer and an optical particle counter. We investigated the influence of particle number concentration, particle size and particle composition on the detection efficiency. The detection efficiency is a product of the scattering efficiency of the laser diodes and the ionization efficiency or hit rate of the excimer laser. The scattering efficiency was found to vary between 0.6 and 1.9 % with an average of 1.1 %; the relative standard deviation (RSD) was 17.0 %. The hit rate exhibited good repeatability with an average value of 63 % and an RSD of 18 %. In addition to laboratory tests, the LAAP-ToF-MS was used to sample ambient air during a period of 6 days at the campus of Aix-Marseille University, situated in the city center of Marseille, France. The optimized LAAP-ToF-MS methodology enables high temporal resolution measurements of the chemical composition of ambient particles, provides new insights into environmental science, and a new investigative tool for atmospheric chemistry and physics, aerosol science and health impact studies.

Real-time detection method and system for identifying individual aerosol particles

DOEpatents

Gard, Eric E [San Francisco, CA; Coffee, Keith R [Patterson, CA; Frank, Matthias [Oakland, CA; Tobias, Herbert J [Kensington, CA; Fergenson, David P [Alamo, CA; Madden, Norm [Livermore, CA; Riot, Vincent J [Berkeley, CA; Steele, Paul T [Livermore, CA; Woods, Bruce W [Livermore, CA

2007-08-21

An improved method and system of identifying individual aerosol particles in real time. Sample aerosol particles are collimated, tracked, and screened to determine which ones qualify for mass spectrometric analysis based on predetermined qualification or selection criteria. Screening techniques include one or more of determining particle size, shape, symmetry, and fluorescence. Only qualifying particles passing all screening criteria are subject to desorption/ionization and single particle mass spectrometry to produce corresponding test spectra, which is used to determine the identities of each of the qualifying aerosol particles by comparing the test spectra against predetermined spectra for known particle types. In this manner, activation cycling of a particle ablation laser of a single particle mass spectrometer is reduced.

Laser ablation aerosol particle time-of-flight mass spectrometer (LAAPTOF): performance, reference spectra and classification of atmospheric samples

NASA Astrophysics Data System (ADS)

Shen, Xiaoli; Ramisetty, Ramakrishna; Mohr, Claudia; Huang, Wei; Leisner, Thomas; Saathoff, Harald

2018-04-01

The laser ablation aerosol particle time-of-flight mass spectrometer (LAAPTOF, AeroMegt GmbH) is able to identify the chemical composition and mixing state of individual aerosol particles, and thus is a tool for elucidating their impacts on human health, visibility, ecosystem, and climate. The overall detection efficiency (ODE) of the instrument we use was determined to range from ˜ (0.01 ± 0.01) to ˜ (4.23 ± 2.36) % for polystyrene latex (PSL) in the size range of 200 to 2000 nm, ˜ (0.44 ± 0.19) to ˜ (6.57 ± 2.38) % for ammonium nitrate (NH4NO3), and ˜ (0.14 ± 0.02) to ˜ (1.46 ± 0.08) % for sodium chloride (NaCl) particles in the size range of 300 to 1000 nm. Reference mass spectra of 32 different particle types relevant for atmospheric aerosol (e.g. pure compounds NH4NO3, K2SO4, NaCl, oxalic acid, pinic acid, and pinonic acid; internal mixtures of e.g. salts, secondary organic aerosol, and metallic core-organic shell particles; more complex particles such as soot and dust particles) were determined. Our results show that internally mixed aerosol particles can result in spectra with new clusters of ions, rather than simply a combination of the spectra from the single components. An exemplary 1-day ambient data set was analysed by both classical fuzzy clustering and a reference-spectra-based classification method. Resulting identified particle types were generally well correlated. We show how a combination of both methods can greatly improve the interpretation of single-particle data in field measurements.

Single particle characterization using a light scattering module coupled to a time-of-flight aerosol mass spectrometer

NASA Astrophysics Data System (ADS)

Cross, E. S.; Onasch, T. B.; Canagaratna, M.; Jayne, J. T.; Kimmel, J.; Yu, X.-Y.; Alexander, M. L.; Worsnop, D. R.; Davidovits, P.

2008-12-01

We present the first single particle results obtained using an Aerodyne time-of-flight aerosol mass spectrometer coupled with a light scattering module (LS-ToF-AMS). The instrument was deployed at the T1 ground site approximately 40 km northeast of the Mexico City Metropolitan Area (MCMA) as part of the MILAGRO field study in March of 2006. The instrument was operated as a standard AMS from 12-30 March, acquiring average chemical composition and size distributions for the ambient aerosol, and in single particle mode from 27-30 March. Over a 75-h sampling period, 12 853 single particle mass spectra were optically triggered, saved, and analyzed. The correlated optical and chemical detection allowed detailed examination of single particle collection and quantification within the LS-ToF-AMS. The single particle data enabled the mixing states of the ambient aerosol to be characterized within the context of the size-resolved ensemble chemical information. The particulate mixing states were examined as a function of sampling time and most of the particles were found to be internal mixtures containing many of the organic and inorganic species identified in the ensemble analysis. The single particle mass spectra were deconvolved, using techniques developed for ensemble AMS data analysis, into HOA, OOA, NH4NO3, (NH4)2SO4, and NH4Cl fractions. Average single particle mass and chemistry measurements are shown to be in agreement with ensemble MS and PTOF measurements. While a significant fraction of ambient particles were internal mixtures of varying degrees, single particle measurements of chemical composition allowed the identification of time periods during which the ambient ensemble was externally mixed. In some cases the chemical composition of the particles suggested a likely source. Throughout the full sampling period, the ambient ensemble was an external mixture of combustion-generated HOA particles from local sources (e.g. traffic), with number concentrations peaking

Fractal morphology, imaging and mass spectrometry of single aerosol particles in flight.

PubMed

Loh, N D; Hampton, C Y; Martin, A V; Starodub, D; Sierra, R G; Barty, A; Aquila, A; Schulz, J; Lomb, L; Steinbrener, J; Shoeman, R L; Kassemeyer, S; Bostedt, C; Bozek, J; Epp, S W; Erk, B; Hartmann, R; Rolles, D; Rudenko, A; Rudek, B; Foucar, L; Kimmel, N; Weidenspointner, G; Hauser, G; Holl, P; Pedersoli, E; Liang, M; Hunter, M S; Hunter, M M; Gumprecht, L; Coppola, N; Wunderer, C; Graafsma, H; Maia, F R N C; Ekeberg, T; Hantke, M; Fleckenstein, H; Hirsemann, H; Nass, K; White, T A; Tobias, H J; Farquar, G R; Benner, W H; Hau-Riege, S P; Reich, C; Hartmann, A; Soltau, H; Marchesini, S; Bajt, S; Barthelmess, M; Bucksbaum, P; Hodgson, K O; Strüder, L; Ullrich, J; Frank, M; Schlichting, I; Chapman, H N; Bogan, M J

2012-06-27

The morphology of micrometre-size particulate matter is of critical importance in fields ranging from toxicology to climate science, yet these properties are surprisingly difficult to measure in the particles' native environment. Electron microscopy requires collection of particles on a substrate; visible light scattering provides insufficient resolution; and X-ray synchrotron studies have been limited to ensembles of particles. Here we demonstrate an in situ method for imaging individual sub-micrometre particles to nanometre resolution in their native environment, using intense, coherent X-ray pulses from the Linac Coherent Light Source free-electron laser. We introduced individual aerosol particles into the pulsed X-ray beam, which is sufficiently intense that diffraction from individual particles can be measured for morphological analysis. At the same time, ion fragments ejected from the beam were analysed using mass spectrometry, to determine the composition of single aerosol particles. Our results show the extent of internal dilation symmetry of individual soot particles subject to non-equilibrium aggregation, and the surprisingly large variability in their fractal dimensions. More broadly, our methods can be extended to resolve both static and dynamic morphology of general ensembles of disordered particles. Such general morphology has implications in topics such as solvent accessibilities in proteins, vibrational energy transfer by the hydrodynamic interaction of amino acids, and large-scale production of nanoscale structures by flame synthesis.

Single-particle aerosol mass spectrometry for the detection and identification of chemical warfare agent simulants.

PubMed

Martin, Audrey N; Farquar, George R; Frank, Matthias; Gard, Eric E; Fergenson, David P

2007-08-15

Single-particle aerosol mass spectrometry (SPAMS) was used for the real-time detection of liquid nerve agent simulants. A total of 1000 dual-polarity time-of-flight mass spectra were obtained for micrometer-sized single particles each of dimethyl methyl phosphonate, diethyl ethyl phosphonate, diethyl phosphoramidate, and diethyl phthalate using laser fluences between 0.58 and 7.83 nJ/microm2, and mass spectral variation with laser fluence was studied. The mass spectra obtained allowed identification of single particles of the chemical warfare agent (CWA) simulants at each laser fluence used although lower laser fluences allowed more facile identification. SPAMS is presented as a promising real-time detection system for the presence of CWAs.

Preliminary observations of organic gas-particle partitioning from biomass combustion smoke using an aerosol mass spectrometer

Treesearch

T. Lee; S. M. Kreidenweis; J. L. Collett; A. P. Sullivan; C. M. Carrico; J. L. Jimenez; M. Cubison; S. Saarikoski; D. R. Worsnop; T. B. Onasch; E. Fortner; W. C. Malm; E. Lincoln; Cyle Wold; WeiMin Hao

2010-01-01

Aerosols play important roles in adverse health effects, indirect and direct forcing of Earth’s climate, and visibility degradation. Biomass burning emissions from wild and prescribed fires can make a significant contribution to ambient aerosol mass in many locations and seasons. In order to better understand the chemical properties of particles produced by combustion...

Aerosol detection efficiency in inductively coupled plasma mass spectrometry

NASA Astrophysics Data System (ADS)

Hubbard, Joshua A.; Zigmond, Joseph A.

2016-05-01

An electrostatic size classification technique was used to segregate particles of known composition prior to being injected into an inductively coupled plasma mass spectrometer (ICP-MS). Size-segregated particles were counted with a condensation nuclei counter as well as sampled with an ICP-MS. By injecting particles of known size, composition, and aerosol concentration into the ICP-MS, efficiencies of the order of magnitude aerosol detection were calculated, and the particle size dependencies for volatile and refractory species were quantified. Similar to laser ablation ICP-MS, aerosol detection efficiency was defined as the rate at which atoms were detected in the ICP-MS normalized by the rate at which atoms were injected in the form of particles. This method adds valuable insight into the development of technologies like laser ablation ICP-MS where aerosol particles (of relatively unknown size and gas concentration) are generated during ablation and then transported into the plasma of an ICP-MS. In this study, we characterized aerosol detection efficiencies of volatile species gold and silver along with refractory species aluminum oxide, cerium oxide, and yttrium oxide. Aerosols were generated with electrical mobility diameters ranging from 100 to 1000 nm. In general, it was observed that refractory species had lower aerosol detection efficiencies than volatile species, and there were strong dependencies on particle size and plasma torch residence time. Volatile species showed a distinct transition point at which aerosol detection efficiency began decreasing with increasing particle size. This critical diameter indicated the largest particle size for which complete particle detection should be expected and agreed with theories published in other works. Aerosol detection efficiencies also displayed power law dependencies on particle size. Aerosol detection efficiencies ranged from 10- 5 to 10- 11. Free molecular heat and mass transfer theory was applied, but

Aerosol detection efficiency in inductively coupled plasma mass spectrometry

DOE PAGES

Hubbard, Joshua A.; Zigmond, Joseph A.

2016-03-02

We used an electrostatic size classification technique to segregate particles of known composition prior to being injected into an inductively coupled plasma mass spectrometer (ICP-MS). Moreover, we counted size-segregated particles with a condensation nuclei counter as well as sampled with an ICP-MS. By injecting particles of known size, composition, and aerosol concentration into the ICP-MS, efficiencies of the order of magnitude aerosol detection were calculated, and the particle size dependencies for volatile and refractory species were quantified. Similar to laser ablation ICP-MS, aerosol detection efficiency was defined as the rate at which atoms were detected in the ICP-MS normalized bymore » the rate at which atoms were injected in the form of particles. This method adds valuable insight into the development of technologies like laser ablation ICP-MS where aerosol particles (of relatively unknown size and gas concentration) are generated during ablation and then transported into the plasma of an ICP-MS. In this study, we characterized aerosol detection efficiencies of volatile species gold and silver along with refractory species aluminum oxide, cerium oxide, and yttrium oxide. Aerosols were generated with electrical mobility diameters ranging from 100 to 1000 nm. In general, it was observed that refractory species had lower aerosol detection efficiencies than volatile species, and there were strong dependencies on particle size and plasma torch residence time. Volatile species showed a distinct transition point at which aerosol detection efficiency began decreasing with increasing particle size. This critical diameter indicated the largest particle size for which complete particle detection should be expected and agreed with theories published in other works. Aerosol detection efficiencies also displayed power law dependencies on particle size. Aerosol detection efficiencies ranged from 10 -5 to 10 -11. Free molecular heat and mass transfer theory was

Single-particle characterization of the High Arctic summertime aerosol

NASA Astrophysics Data System (ADS)

Sierau, B.; Chang, R. Y.-W.; Leck, C.; Paatero, J.; Lohmann, U.

2014-01-01

Single-particle mass spectrometric measurements were carried out in the High Arctic north of 80° during summer 2008. The campaign took place onboard the icebreaker Oden and was part of the Arctic Summer Cloud Ocean Study (ASCOS). The instrument deployed was an Aerosol Time-of-Flight Mass Spectrometer (ATOFMS) that provides information on the chemical composition of individual particles and their mixing state in real-time. Aerosols were sampled in the marine boundary layer at stations in the open ocean, in the marginal ice zone, and in the pack ice region. The largest fraction of particles detected for subsequent analysis in the size range of the ATOFMS between approximately 200 nm to 3000 nm in diameter showed mass spectrometric patterns indicating an internal mixing state and a biomass burning and/or biofuel source. The majority of these particles were connected to an air mass layer of elevated particle concentration mixed into the surface mixed layer from the upper part of the marine boundary layer. The second largest fraction was represented by sea salt particles. The chemical analysis of the over-ice sea salt aerosol revealed tracer compounds that reflect chemical aging of the particles during their long-range advection from the marginal ice zone, or open waters south thereof prior to detection at the ship. From our findings we conclude that long-range transport of particles is one source of aerosols in the High Arctic. To assess the importance of long-range particle sources for aerosol-cloud interactions over the inner Arctic in comparison to local and regional biogenic primary aerosol sources, the chemical composition of the detected particles was analyzed for indicators of marine biological origin. Only a~minor fraction showed chemical signatures of potentially ocean-derived primary particles of that kind. However, a chemical bias in the ATOFMS's detection capabilities observed during ASCOS might suggest a presence of a particle type of unknown composition

Single-particle characterization of the high-Arctic summertime aerosol

NASA Astrophysics Data System (ADS)

Sierau, B.; Chang, R. Y.-W.; Leck, C.; Paatero, J.; Lohmann, U.

2014-07-01

Single-particle mass-spectrometric measurements were carried out in the high Arctic north of 80° during summer 2008. The campaign took place onboard the icebreaker Oden and was part of the Arctic Summer Cloud Ocean Study (ASCOS). The instrument deployed was an aerosol time-of-flight mass spectrometer (ATOFMS) that provides information on the chemical composition of individual particles and their mixing state in real time. Aerosols were sampled in the marine boundary layer at stations in the open ocean, in the marginal ice zone, and in the pack ice region. The largest fraction of particles detected for subsequent analysis in the size range of the ATOFMS between approximately 200 and 3000 nm in diameter showed mass-spectrometric patterns, indicating an internal mixing state and a biomass burning and/or biofuel source. The majority of these particles were connected to an air mass layer of elevated particle concentration mixed into the surface mixed layer from the upper part of the marine boundary layer. The second largest fraction was represented by sea salt particles. The chemical analysis of the over-ice sea salt aerosol revealed tracer compounds that reflect chemical aging of the particles during their long-range advection from the marginal ice zone, or open waters south thereof prior to detection at the ship. From our findings we conclude that long-range transport of particles is one source of aerosols in the high Arctic. To assess the importance of long-range particle sources for aerosol-cloud interactions over the inner Arctic in comparison to local and regional biogenic primary aerosol sources, the chemical composition of the detected particles was analyzed for indicators of marine biological origin. Only a minor fraction showed chemical signatures of potentially ocean-derived primary particles of that kind. However, a chemical bias in the ATOFMS's detection capabilities observed during ASCOS might suggest the presence of a particle type of unknown composition

Toward Quantifying the Mass-Based Hygroscopicity of Individual Submicron Atmospheric Aerosol Particles with STXM/NEXAFS and SEM/EDX

NASA Astrophysics Data System (ADS)

Yancey Piens, D.; Kelly, S. T.; OBrien, R. E.; Wang, B.; Petters, M. D.; Laskin, A.; Gilles, M. K.

2014-12-01

The hygroscopic behavior of atmospheric aerosols influences their optical and cloud-nucleation properties, and therefore affects climate. Although changes in particle size as a function of relative humidity have often been used to quantify the hygroscopic behavior of submicron aerosol particles, it has been noted that calculations of hygroscopicity based on size contain error due to particle porosity, non-ideal volume additivity and changes in surface tension. We will present a method to quantify the hygroscopic behavior of submicron aerosol particles based on changes in mass, rather than size, as a function of relative humidity. This method results from a novel experimental approach combining scanning transmission x-ray microscopy with near-edge x-ray absorption fine spectroscopy (STXM/NEXAFS), as well as scanning electron microscopy with energy dispersive x-ray spectroscopy (SEM/EDX) on the same individual particles. First, using STXM/NEXAFS, our methods are applied to aerosol particles of known composition ‒ for instance ammonium sulfate, sodium bromide and levoglucosan ‒ and validated by theory. Then, using STXM/NEXAFS and SEM/EDX, these methods are extended to mixed atmospheric aerosol particles collected in the field at the DOE Atmospheric Radiation Measurement (ARM) Climate Research Facility at the Southern Great Planes sampling site in Oklahoma, USA. We have observed and quantified a range of hygroscopic behaviors which are correlated to the composition and morphology of individual aerosol particles. These methods will have implications for parameterizing aerosol mixing state and cloud-nucleation activity in atmospheric models.

Reduction in biomass burning aerosol light absorption upon humidification: roles of inorganically-induced hygroscopicity, particle collapse, and photoacoustic heat and mass transfer

NASA Astrophysics Data System (ADS)

Lewis, K. A.; Arnott, W. P.; Moosmüller, H.; Chakrabarty, R. K.; Carrico, C. M.; Kreidenweis, S. M.; Day, D. E.; Malm, W. C.; Laskin, A.; Jimenez, J. L.; Ulbrich, I. M.; Huffman, J. A.; Onasch, T. B.; Trimborn, A.; Liu, L.; Mishchenko, M. I.

2009-11-01

Smoke particle emissions from the combustion of biomass fuels typical for the western and southeastern United States were studied and compared under high humidity and ambient conditions in the laboratory. The fuels used were Montana ponderosa pine (Pinus ponderosa), southern California chamise (Adenostoma fasciculatum), and Florida saw palmetto (Serenoa repens). Information on the non-refractory chemical composition of biomass burning aerosol from each fuel was obtained with an aerosol mass spectrometer and through estimation of the black carbon concentration from light absorption measurements at 870 nm. Changes in the optical and physical particle properties under high humidity conditions were observed for hygroscopic smoke particles containing substantial inorganic mass fractions that were emitted from combustion of chamise and palmetto fuels. Light scattering cross sections increased under high humidity for these particles, consistent with the hygroscopic growth measured for 100 nm particles in HTDMA measurements. Photoacoustic measurements of aerosol light absorption coefficients revealed a 20% reduction with increasing relative humidity, contrary to the expectation of light absorption enhancement by the liquid coating taken up by hygroscopic particles. This reduction is hypothesized to arise from two mechanisms: (1) shielding of inner monomers after particle consolidation or collapse with water uptake; (2) the lower case contribution of mass transfer through evaporation and condensation at high relative humidity (RH) to the usual heat transfer pathway for energy release by laser-heated particles in the photoacoustic measurement of aerosol light absorption. The mass transfer contribution is used to evaluate the fraction of aerosol surface covered with liquid water solution as a function of RH.

Reduction in biomass burning aerosol light absorption upon humidification: roles of inorganically-induced hygroscopicity, particle collapse, and photoacoustic heat and mass transfer

NASA Astrophysics Data System (ADS)

Lewis, K. A.; Arnott, W. P.; Moosmüller, H.; Chakrabarty, R. K.; Carrico, C. M.; Kreidenweis, S. M.; Day, D. E.; Malm, W. C.; Laskin, A.; Jimenez, J. L.; Ulbrich, I. M.; Huffman, J. A.; Onasch, T. B.; Trimborn, A.; Liu, L.; Mishchenko, M. I.

2009-07-01

Smoke particle emissions from the combustion of biomass fuels typical for the western and southeastern United States were studied and compared under high humidity and ambient conditions in the laboratory. The fuels used are Montana ponderosa pine (Pinus ponderosa), southern California chamise (Adenostoma fasciculatum), and Florida saw palmetto (Serenoa repens). Information on the non-refractory chemical composition of biomass burning aerosol from each fuel was obtained with an aerosol mass spectrometer and through estimation of the black carbon concentration from light absorption measurements at 870 nm. Changes in the optical and physical particle properties under high humidity conditions were observed for hygroscopic smoke particles containing substantial inorganic mass fractions that were emitted from combustion of chamise and palmetto fuels. Light scattering cross sections increased under high humidity for these particles, consistent with the hygroscopic growth measured for 100 nm particles in HTDMA measurements. Photoacoustic measurements of aerosol light absorption coefficients reveal a 20% reduction with increasing relative humidity, contrary to the expectation of light absorption enhancement by the liquid coating taken up by hygroscopic particles. This reduction is hypothesized to arise from two mechanisms: 1. Shielding of inner monomers after particle consolidation or collapse with water uptake; 2. The contribution of mass transfer through evaporation and condensation at high relative humidity to the usual heat transfer pathway for energy release by laser-heated particles in the photoacoustic measurement of aerosol light absorption. The mass transfer contribution is used to evaluate the fraction of aerosol surface covered with liquid water solution as a function of RH.

Detecting trace pesticides in real time using single particle aerosol mass spectrometry.

PubMed

Barker, Zachary; Venkatchalam, Veena; Martin, Audrey N; Farquar, George R; Frank, Matthias

2010-02-28

Pesticides are toxic substances and may cause unintentional harm if improperly used. The ubiquitous nature of pesticides, with frequent use in agriculture and the household, and the potential for harm that pesticides pose to non-target organisms such as wildlife, humans, and pets, demonstrate the need for rapid and effective detection and identification of these compounds. In this study, single particle aerosol mass spectrometry (SPAMS) was used to rapidly detect compounds from four classes of pesticides commonly used in agricultural and household applications. These include permethrin (pyrethroid class), malathion and dichlorvos (organophosphate class), imidacloprid (chloronicotinyl class), and carbaryl (carbamate class). Analytical standards of each compound were diluted and aerosolized using a nebulizer to create particles for analysis in the SPAMS instrument. The resultant dual-polarity time-of-flight mass spectra were then analyzed to identify the characteristic peaks of the compound in each sample. In addition, samples of commercial products containing pesticides, a commercial insecticide spray, containing permethrin, and a canine flea collar, containing carbaryl, were analyzed in their original form using SPAMS without any significant sample preparation. The characteristic mass spectral peaks of the active pesticides in these samples were identified using the mass spectra obtained earlier from the pesticide analytical standards. By successfully identifying pesticides in analytical standards and in commercial products, it is demonstrated herein that the SPAMS system may be capable of pesticide detection in numerous environmental and agricultural situations. Copyright 2010 Elsevier B.V. All rights reserved.

Background aerosol over the Himalayas and Tibetan Plateau: observed characteristics of aerosol mass loading

NASA Astrophysics Data System (ADS)

Liu, B.; Cong, Z.; Wang, Y.; Xin, J.; Wan, X.; Pan, Y.; Liu, Z.; Wang, Y.; Zhang, G.; Kang, S.

2016-12-01

To investigate the atmospheric aerosols of the Himalayas and Tibetan Plateau (HTP), an observation network was established within the region's various ecosystems, including at Ngari, Qomolangma (QOMS), Nam Co, and SouthEastern Tibetan (SET) stations. In this paper we illustrate aerosol mass loadings by integrating in situ measurements with satellite and ground-based remote sensing datasets for the 2011-2013 period, on both local and large scales. Mass concentrations of these surface atmospheric aerosols were relatively low and varied with land cover, showing a general tendency of Ngari and QOMS (barren sites) > Nam Co (grassland site) > SET (forest site). Bimodal mass distributions of size-segregated particles were found at all sites, with a relatively small peak in accumulation mode and a more notable peak in coarse mode. Diurnal variations in fine aerosol masses generally displayed a bi-peak pattern at the QOMS, Nam Co and SET stations and a single-peak pattern at the Ngari station, controlled by the effects of local geomorphology, mountain-valley breeze circulation and aerosol emissions. Combining surface aerosols data and atmospheric-column aerosol optical properties, the TSP mass and aerosol optical depth (AOD) of the Multi-angle Imaging Spectroradiometer (MISR) generally decreased as land cover changed from barren to forest, in inverse relation to the PM2.5 ratios. The seasonality of aerosol mass parameters was land-cover dependent. Over forest and grassland areas, TSP mass, PM2.5 mass, MISR-AOD and fine-mode AOD were higher in spring and summer, followed by relatively lower values in autumn and winter. At the barren site (the QOMS station), there were inconsistent seasonal variations between surface TSP mass (PM2.5 mass) and atmospheric column AOD (fine-mode AOD). Our findings implicate that, HTP aerosol masses (especially their reginal characteristics and fine particle emissions) need to be treated sensitively in relation to assessments of their climatic

Structural analysis of aerosol particles by microscopic observation using a time-of-flight secondary ion mass spectrometer

NASA Astrophysics Data System (ADS)

Takami, Akinori; Mayama, Norihito; Sakamoto, Tetsuo; Ohishi, Kenji; Irei, Satoshi; Yoshino, Ayako; Hatakeyama, Shiro; Murano, Kentaro; Sadanaga, Yasuhiro; Bandow, Hiroshi; Misawa, Kentaro; Fujii, Masaaki

2013-06-01

The chemical composition and structure of fine aerosol particles with diameters of less than 1 µm were analyzed in the spring of 2011 at Fukue Island, Japan, using an aerosol quadrupole mass spectrometer (Q-AMS, Aerodyne Research, Inc.) and a time-of-flight secondary ion mass spectrometer (TOF-SIMS). The Q-AMS results were similar to those of previous studies conducted at the same location, suggesting that the composition we observed is typical of this site. Based on the TOF-SIMS results, we classified the fine aerosol particles into three types: Type A, in which sulfate was covered with organic matter (OM); Type B, in which soil-containing particles with a diameter of 0.5 µm were associated with sulfate and OM; and Type C, in which black carbon (BC) and sulfate aggregates were associated with OM. During the observation period, the relative abundances of Type A, B, and C particles were 55%, 20%, and 25%, respectively. The structure, chemical composition, and the proportion of each type of particles provide information for a more representative particle model in radiative models. The relative abundance of Type C, i.e., BC-containing particles, is quite different to that in Tokyo, suggesting that Type C could be an indicator of transboundary air pollution, in this case from mainland China.

Mass-spectrometric identification of primary biological particle markers: indication for low abundance of primary biological material in the pristine submicron aerosol of Amazonia

NASA Astrophysics Data System (ADS)

Schneider, J.; Freutel, F.; Zorn, S. R.; Chen, Q.; Farmer, D. K.; Jimenez, J. L.; Martin, S. T.; Artaxo, P.; Wiedensohler, A.; Borrmann, S.

2011-07-01

The abundance of marker compounds for primary biological particles in submicron aerosol was investigated by means of aerosol mass spectrometry. Mass spectra of amino acids, carbohydrates, small peptides, and proteins, all of which are key building blocks of biological particles, were recorded in laboratory experiments. Several characteristic marker peaks were identified. The identified marker peaks were compared with mass spectra recorded during AMAZE-08, a field campaign conducted in the pristine rainforest of the Central Amazon Basin, Brazil, during the wet season of February and March 2008. The low abundance of identified marker peaks places upper limits of 7.5 % for amino acids and 5.6 % for carbohydrates on the contribution of primary biological aerosol particles (PBAPs) to the submicron organic aerosol mass concentration during this time period. Upper limits for the absolute submicron concentrations for both compound classes range from 0.01 to 0.1 μg m-3. Carbohydrates and protein amino acids make up for about two thirds of the dry mass of a biological cell. Thus, our findings suggest an upper limit for the PBAPs mass fraction of about 20 % to the submicron organic aerosol.

Can Condensing Organic Aerosols Lead to Less Cloud Particles?

NASA Astrophysics Data System (ADS)

Gao, C. Y.; Tsigaridis, K.; Bauer, S.

2017-12-01

We examined the impact of condensing organic aerosols on activated cloud number concentration in a new aerosol microphysics box model, MATRIX-VBS. The model includes the volatility-basis set (VBS) framework in an aerosol microphysical scheme MATRIX (Multiconfiguration Aerosol TRacker of mIXing state) that resolves aerosol mass and number concentrations and aerosol mixing state. Preliminary results show that by including the condensation of organic aerosols, the new model (MATRIX-VBS) has less activated particles compared to the original model (MATRIX), which treats organic aerosols as non-volatile. Parameters such as aerosol chemical composition, mass and number concentrations, and particle sizes which affect activated cloud number concentration are thoroughly evaluated via a suite of Monte-Carlo simulations. The Monte-Carlo simulations also provide information on which climate-relevant parameters play a critical role in the aerosol evolution in the atmosphere. This study also helps simplifying the newly developed box model which will soon be implemented in the global model GISS ModelE as a module.

Desert Dust Aerosol Air Mass Mapping in the Western Sahara, Using Particle Properties Derived from Space-Based Multi-Angle Imaging

NASA Technical Reports Server (NTRS)

Kahn, Ralph; Petzold, Andreas; Wendisch, Manfred; Bierwirth, Eike; Dinter, Tilman; Esselborn, Michael; Fiebig, Marcus; Heese, Birgit; Knippertz, Peter; Mueller, Detlef;

Background aerosol over the Himalayas and Tibetan Plateau: observed characteristics of aerosol mass loading

NASA Astrophysics Data System (ADS)

Liu, Bin; Cong, Zhiyuan; Wang, Yuesi; Xin, Jinyuan; Wan, Xin; Pan, Yuepeng; Liu, Zirui; Wang, Yonghong; Zhang, Guoshuai; Wang, Zhongyan; Wang, Yongjie; Kang, Shichang

2017-01-01

To investigate the atmospheric aerosols of the Himalayas and Tibetan Plateau (HTP), an observation network was established within the region's various ecosystems, including at the Ngari, Qomolangma (QOMS), Nam Co, and Southeastern Tibetan (SET) stations. In this paper we illustrate aerosol mass loadings by integrating in situ measurements with satellite and ground-based remote sensing datasets for the 2011-2013 period, on both local and large scales. Mass concentrations of these surface atmospheric aerosols were relatively low and varied with land cover, showing a general tendency of Ngari and QOMS (barren sites) > Nam Co (grassland site) > SET (forest site). Daily averages of online PM2.5 (particulates with aerodynamic diameters below 2.5 µm) at these sites were sequentially 18.2 ± 8.9, 14.5 ± 7.4, 11.9 ± 4.9 and 11.7 ± 4.7 µg m-3. Correspondingly, the ratios of PM2.5 to total suspended particles (TSP) were 27.4 ± 6.65, 22.3 ± 10.9, 37.3 ± 11.1 and 54.4 ± 6.72 %. Bimodal mass distributions of size-segregated particles were found at all sites, with a relatively small peak in accumulation mode and a more notable peak in coarse mode. Diurnal variations in fine-aerosol masses generally displayed a bi-peak pattern at the QOMS, Nam Co and SET stations and a single-peak pattern at the Ngari station, controlled by the effects of local geomorphology, mountain-valley breeze circulation and aerosol emissions. Dust aerosol content in PM2.1 samples gave fractions of 26 % at the Ngari station and 29 % at the QOMS station, or ˜ 2-3 times that of reported results at human-influenced sites. Furthermore, observed evidence confirmed the existence of the aerodynamic conditions necessary for the uplift of fine particles from a barren land surface. Combining surface aerosol data and atmospheric-column aerosol optical properties, the TSP mass and aerosol optical depth (AOD) of the Multi-angle Imaging Spectroradiometer (MISR) generally decreased as land cover changed from

Chemical compositions of black carbon particle cores and coatings via soot particle aerosol mass spectrometry with photoionization and electron ionization.

PubMed

Canagaratna, Manjula R; Massoli, Paola; Browne, Eleanor C; Franklin, Jonathan P; Wilson, Kevin R; Onasch, Timothy B; Kirchstetter, Thomas W; Fortner, Edward C; Kolb, Charles E; Jayne, John T; Kroll, Jesse H; Worsnop, Douglas R

2015-05-14

Black carbon is an important constituent of atmospheric aerosol particle matter (PM) with significant effects on the global radiation budget and on human health. The soot particle aerosol mass spectrometer (SP-AMS) has been developed and deployed for real-time ambient measurements of refractory carbon particles. In the SP-AMS, black carbon or metallic particles are vaporized through absorption of 1064 nm light from a CW Nd:YAG laser. This scheme allows for continuous "soft" vaporization of both core and coating materials. The main focus of this work is to characterize the extent to which this vaporization scheme provides enhanced chemical composition information about aerosol particles. This information is difficult to extract from standard SP-AMS mass spectra because they are complicated by extensive fragmentation from the harsh 70 eV EI ionization scheme that is typically used in these instruments. Thus, in this work synchotron-generated vacuum ultraviolet (VUV) light in the 8-14 eV range is used to measure VUV-SP-AMS spectra with minimal fragmentation. VUV-SP-AMS spectra of commercially available carbon black, fullerene black, and laboratory generated flame soots were obtained. Small carbon cluster cations (C(+)-C5(+)) were found to dominate the VUV-SP-AMS spectra of all the samples, indicating that the corresponding neutral clusters are key products of the SP vaporization process. Intercomparisons of carbon cluster ratios observed in VUV-SP-AMS and SP-AMS spectra are used to confirm spectral features that could be used to distinguish between different types of refractory carbon particles. VUV-SP-AMS spectra of oxidized organic species adsorbed on absorbing cores are also examined and found to display less thermally induced decomposition and fragmentation than spectra obtained with thermal vaporization at 200 °C (the minimum temperature needed to quantitatively vaporize ambient oxidized organic aerosol with a continuously heated surface). The particle cores

Pollutants identification of ambient aerosols by two types of aerosol mass spectrometers over southeast coastal area, China.

PubMed

Yan, Jinpei; Chen, Liqi; Lin, Qi; Zhao, Shuhui; Li, Lei

2018-02-01

Two different aerosol mass spectrometers, Aerodyne Aerosol Mass Spectrometer (AMS) and Single Particle Aerosol Mass Spectrometer (SPAMS) were deployed to identify the aerosol pollutants over Xiamen, representing the coastal urban area. Five obvious processes were classified during the whole observation period. Organics and sulfate were the dominant components in ambient aerosols over Xiamen. Most of the particles were in the size range of 0.2-1.0μm, accounting for over 97% of the total particles measured by both instruments. Organics, as well as sulfate, measured by AMS were in good correlation with measured by SPAMS. However, high concentration of NH 4 + was obtained by AMS, while extremely low value of NH 4 + was detected by SPAMS. Contrarily, high particle number counts of NO 3 - and Cl - were given by SPAMS while low concentrations of NO 3 - and Cl - were measured by AMS. The variations of POA and SOA obtained from SPAMS during event 1 and event 2 were in accordance with the analysis of HOA and OOA given by AMS, suggesting that both of AMS and SPAMS can well identify the organic clusters of aerosol particles. Overestimate or underestimate of the aerosol sources and acidity would be present in some circumstances when the measurement results were used to analyze the aerosol properties, because of the detection loss of some species for both instruments. Copyright © 2017. Published by Elsevier B.V.

Aerosol chemical composition in cloud events by high resolution time-of-flight aerosol mass spectrometry.

PubMed

Hao, Liqing; Romakkaniemi, Sami; Kortelainen, Aki; Jaatinen, Antti; Portin, Harri; Miettinen, Pasi; Komppula, Mika; Leskinen, Ari; Virtanen, Annele; Smith, James N; Sueper, Donna; Worsnop, Douglas R; Lehtinen, Kari E J; Laaksonen, Ari

2013-03-19

This study presents results of direct observations of aerosol chemical composition in clouds. A high-resolution time-of-flight aerosol mass spectrometer was used to make measurements of cloud interstitial particles (INT) and mixed cloud interstitial and droplet residual particles (TOT). The differences between these two are the cloud droplet residuals (RES). Positive matrix factorization analysis of high-resolution mass spectral data sets and theoretical calculations were performed to yield distributions of chemical composition of the INT and RES particles. We observed that less oxidized hydrocarbon-like organic aerosols (HOA) were mainly distributed into the INT particles, whereas more oxidized low-volatile oxygenated OA (LVOOA) mainly in the RES particles. Nitrates existed as organic nitrate and in chemical form of NH(4)NO(3). Organic nitrates accounted for 45% of total nitrates in the INT particles, in clear contrast to 26% in the RES particles. Meanwhile, sulfates coexist in forms of acidic NH(4)HSO(4) and neutralized (NH(4))(2)SO(4). Acidic sulfate made up 64.8% of total sulfates in the INT particles, much higher than 10.7% in the RES particles. The results indicate a possible joint effect of activation ability of aerosol particles, cloud processing, and particle size effects on cloud formation.

Complementary online aerosol mass spectrometry and offline FT-IR spectroscopy measurements: Prospects and challenges for the analysis of anthropogenic aerosol particle emissions

NASA Astrophysics Data System (ADS)

Faber, Peter; Drewnick, Frank; Bierl, Reinhard; Borrmann, Stephan

2017-10-01

The aerosol mass spectrometer (AMS) is well established in investigating highly time-resolved dynamics of submicron aerosol chemical composition including organic aerosol (OA). However, interpretation of mass spectra on molecular level is limited due to strong fragmentation of organic substances and potential reactions inside the AMS ion chamber. Results from complementary filter-based FT-IR absorption measurements were used to explain features in high-resolution AMS mass spectra of different types of OA (e.g. cooking OA, cigarette smoking OA, wood burning OA). Using this approach some AMS fragment ions were validated in this study as appropriate and rather specific markers for a certain class of organic compounds for all particle types under investigation. These markers can therefore be used to get deeper insights in the chemical composition of OA based on AMS mass spectra in upcoming studies. However, the specificity of other fragment ions such as C2H4O2+ (m/z 60.02114) remains ambiguous. In such cases, complementary FT-IR measurements allow the interpretation of highly time-resolved AMS mass spectra at the level of molecular functional groups. Furthermore, this study discusses the challenges in reducing inorganic interferences (e.g. from water and ammonium salts) in FT-IR spectra of atmospheric aerosols to decrease spectral uncertainties for better comparisons and, thus, to get more robust results.

Characterization of ambient aerosols at the San Francisco International Airport using BioAerosol Mass Spectrometry

DOE Office of Scientific and Technical Information (OSTI.GOV)

Steele, P T; McJimpsey, E L; Coffee, K R

2006-03-16

The BioAerosol Mass Spectrometry (BAMS) system is a rapidly fieldable, fully autonomous instrument that can perform correlated measurements of multiple orthogonal properties of individual aerosol particles. The BAMS front end uses optical techniques to nondestructively measure a particle's aerodynamic diameter and fluorescence properties. Fluorescence can be excited at 266nm or 355nm and is detected in two broad wavelength bands. Individual particles with appropriate size and fluorescence properties can then be analyzed more thoroughly in a dual-polarity time-of-flight mass spectrometer. Over the course of two deployments to the San Francisco International Airport, more than 6.5 million individual aerosol particles were fullymore » analyzed by the system. Analysis of the resulting data has provided a number of important insights relevant to rapid bioaerosol detection, which are described here.« less

Characterization of aerosol particles from grass mowing by joint deployment of ToF-AMS and ATOFMS instruments

NASA Astrophysics Data System (ADS)

Drewnick, Frank; Dall'Osto, Manuel; Harrison, Roy

During a measurement campaign at a semi-urban/industrial site a grass-cutting event was observed, when the lawn in the immediate surrounding of the measurement site was mowed. Using a wide variety of state-of-the-art aerosol measurement technology allowed a broad characterization of the aerosol generated by the lawn mowing. The instrumentation included two on-line aerosol mass spectrometers: an Aerodyne Time-of-Flight Aerosol Mass Spectrometer (ToF-AMS) and a TSI Aerosol Time-of-Flight Mass Spectrometer (ATOFMS); in addition, a selection of on-line aerosol concentration and size distribution instruments (OPC, APS, SMPS, CPC, FDMS-TEOM, MAAP) was deployed. From comparison of background aerosol measurements during most of the day with the aerosol measured during the lawn mowing, the grass cutting was found to generate mainly two different types of aerosol particles: an intense ultrafine particle mode (1 h average: 4 μg m -3) of almost pure hydrocarbon-like organics and a distinct particle mode in the upper sub-micrometer size range containing particles with potassium and nitrogen-organic compounds. The ultrafine particles are probably lubricating oil particles from the lawn mower exhaust; the larger particles are swirled-up plant debris particles from the mowing process. While these particle types were identified in the data from the two mass spectrometers, the on-line aerosol concentration and size distribution data support these findings. The results presented here show that the combination of quantitative aerosol particle ensemble mass spectrometry (ToF-AMS) and single particle mass spectrometry (ATOFMS) provides much deeper insights into the nature of the aerosol properties than each of the instruments could do alone. Therefore a combined deployment of both types of instruments is strongly recommended.

Physicochemical characterization of Capstone depleted uranium aerosols I: uranium concentration in aerosols as a function of time and particle size.

PubMed

Parkhurst, Mary Ann; Cheng, Yung Sung; Kenoyer, Judson L; Traub, Richard J

2009-03-01

During the Capstone Depleted Uranium (DU) Aerosol Study, aerosols containing DU were produced inside unventilated armored vehicles (i.e., Abrams tanks and Bradley Fighting Vehicles) by perforation with large-caliber DU penetrators. These aerosols were collected and characterized, and the data were subsequently used to assess human health risks to personnel exposed to DU aerosols. The DU content of each aerosol sample was first quantified by radioanalytical methods, and selected samples, primarily those from the cyclone separator grit chambers, were analyzed radiochemically. Deposition occurred inside the vehicles as particles settled on interior surfaces. Settling rates of uranium from the aerosols were evaluated using filter cassette samples that collected aerosol as total mass over eight sequential time intervals. A moving filter was used to collect aerosol samples over time, particularly within the first minute after a shot. The results demonstrate that the peak uranium concentration in the aerosol occurred in the first 10 s after perforation, and the concentration decreased in the Abrams tank shots to about 50% within 1 min and to less than 2% after 30 min. The initial and maximum uranium concentrations were lower in the Bradley vehicle than those observed in the Abrams tank, and the concentration levels decreased more slowly. Uranium mass concentrations in the aerosols as a function of particle size were evaluated using samples collected in a cyclone sampler, which collected aerosol continuously for 2 h after perforation. The percentages of uranium mass in the cyclone separator stages ranged from 38 to 72% for the Abrams tank with conventional armor. In most cases, it varied with particle size, typically with less uranium associated with the smaller particle sizes. Neither the Abrams tank with DU armor nor the Bradley vehicle results were specifically correlated with particle size and can best be represented by their average uranium mass concentrations of 65

Assessment of aerosol's mass concentrations from measured linear particle depolarization ratio (vertically resolved) and simulations

NASA Astrophysics Data System (ADS)

Nemuc, A.; Vasilescu, J.; Talianu, C.; Belegante, L.; Nicolae, D.

2013-11-01

Multi-wavelength depolarization Raman lidar measurements from Magurele, Romania are used in this study along with simulated mass-extinction efficiencies to calculate the mass concentration profiles of different atmospheric components, due to their different depolarization contribution to the 532 nm backscatter coefficient. Linear particle depolarization ratio (δpart) was computed using the relative amplification factor and the system-dependent molecular depolarization. The low depolarizing component was considered as urban/smoke, with a mean δpart of 3%, while for the high depolarizing component (mineral dust) a mean δpart of 35% was assumed. For this study 11 months of lidar measurements were analysed. Two study cases are presented in details: one for a typical Saharan dust aerosol intrusion, 10 June 2012 and one for 12 July 2012 when a lofted layer consisting of biomass burning smoke extended from 3 to 4.5 km height. Optical Properties of Aerosols and Clouds software package (OPAC) classification and conversion factors were used to calculate mass concentrations. We found that calibrated depolarization measurements are critical in distinguishing between smoke-reach aerosol during the winter and dust-reach aerosol during the summer, as well as between elevated aerosol layers having different origins. Good agreement was found between lidar retrievals and DREAM- Dust REgional Atmospheric Model forecasts in cases of Saharan dust. Our method was also compared against LIRIC (The Lidar/Radiometer Inversion Code) and very small differences were observed.

Assessment of aerosol's mass concentrations from measured linear particle depolarization ratio (vertically resolved) and simulations

NASA Astrophysics Data System (ADS)

Nemuc, A.; Vasilescu, J.; Talianu, C.; Belegante, L.; Nicolae, D.

2013-06-01

Multiwavelength depolarization Raman lidar measurements from Magurele, Romania are used in this study along with simulated mass-extinction efficiencies to calculate the mass concentrations profiles of different atmospheric components, due to their different depolarization contribution to the 532 nm backscatter coefficient. Linear particle depolarization ratio (δpart) was computed using the relative amplification factor and the system-dependent molecular depolarization. The low depolarizing component was considered as urban/smoke, with a mean δpart of 3%, while for the high depolarizing component (mineral dust) a mean δpart of 35% was assumed. For this study 11 months of lidar measurements were analyzed. Two study cases are presented in details: one for a typical Saharan dust aerosol intrusion, 10 June 2012 and one for 12 July 2012 when a lofted layer consisting of biomass burning smoke extended from 3 to 4.5 km height. Optical Properties of Aerosols and Clouds software package (OPAC) classification and conversion factors were used to calculate mass concentrations. We found that calibrated depolarization measurements are critical to distinguish between smoke-reach aerosol during the winter and dust-reach aerosol during the summer, as well as between elevated aerosol layers having different origins. Good agreement was found between lidar retrievals and DREAM- Dust REgional Atmospheric Model forecasts in cases of Saharan dust. Our method was also compared against LIRIC (The Lidar/Radiometer Inversion Code) and very small differences were observed.

BioAerosol Mass Spectrometry: Reagentless Detection of Individual Airborne Spores and Other Bioagent Particles Based on Laser Desorption/Ionization Mass Spectrometry

DOE Office of Scientific and Technical Information (OSTI.GOV)

Steele, Paul Thomas

2004-09-01

Better devices are needed for the detection of aerosolized biological warfare agents. Advances in the ongoing development of one such device, the BioAerosol Mass Spectrometry (BAMS) system, are described here in detail. The system samples individual, micrometer-sized particles directly from the air and analyzes them in real-time without sample preparation or use of reagents. At the core of the BAMS system is a dual-polarity, single-particle mass spectrometer with a laser based desorption and ionization (DI) system. The mass spectra produced by early proof-of-concept instruments were highly variable and contained limited information to differentiate certain types of similar biological particles. Themore » investigation of this variability and subsequent changes to the DI laser system are described. The modifications have reduced the observed variability and thereby increased the usable information content in the spectra. These improvements would have little value without software to analyze and identify the mass spectra. Important improvements have been made to the algorithms that initially processed and analyzed the data. Single particles can be identified with an impressive level of accuracy, but to obtain significant reductions in the overall false alarm rate of the BAMS instrument, alarm decisions must be made dynamically on the basis of multiple analyzed particles. A statistical model has been developed to make these decisions and the resulting performance of a hypothetical BAMS system is quantitatively predicted. The predictions indicate that a BAMS system, with reasonably attainable characteristics, can operate with a very low false alarm rate (orders of magnitude lower than some currently fielded biodetectors) while still being sensitive to small concentrations of biological particles in a large range of environments. Proof-of-concept instruments, incorporating some of the modifications described here, have already performed well in independent testing.« less

Real-Time Detection Method And System For Identifying Individual Aerosol Particles

DOEpatents

Gard, Eric Evan; Fergenson, David Philip

2005-10-25

A method and system of identifying individual aerosol particles in real time. Sample aerosol particles are compared against and identified with substantially matching known particle types by producing positive and negative test spectra of an individual aerosol particle using a bipolar single particle mass spectrometer. Each test spectrum is compared to spectra of the same respective polarity in a database of predetermined positive and negative spectra for known particle types and a set of substantially matching spectra is obtained. Finally the identity of the individual aerosol particle is determined from the set of substantially matching spectra by determining a best matching one of the known particle types having both a substantially matching positive spectrum and a substantially matching negative spectrum associated with the best matching known particle type.

Aerosol properties, source identification, and cloud processing in orographic clouds measured by single particle mass spectrometry on a central European mountain site during HCCT-2010

NASA Astrophysics Data System (ADS)

Roth, A.; Schneider, J.; Klimach, T.; Mertes, S.; van Pinxteren, D.; Herrmann, H.; Borrmann, S.

2016-01-01

Cloud residues and out-of-cloud aerosol particles with diameters between 150 and 900 nm were analysed by online single particle aerosol mass spectrometry during the 6-week study Hill Cap Cloud Thuringia (HCCT)-2010 in September-October 2010. The measurement location was the mountain Schmücke (937 m a.s.l.) in central Germany. More than 160 000 bipolar mass spectra from out-of-cloud aerosol particles and more than 13 000 bipolar mass spectra from cloud residual particles were obtained and were classified using a fuzzy c-means clustering algorithm. Analysis of the uncertainty of the sorting algorithm was conducted on a subset of the data by comparing the clustering output with particle-by-particle inspection and classification by the operator. This analysis yielded a false classification probability between 13 and 48 %. Additionally, particle types were identified by specific marker ions. The results from the ambient aerosol analysis show that 63 % of the analysed particles belong to clusters having a diurnal variation, suggesting that local or regional sources dominate the aerosol, especially for particles containing soot and biomass burning particles. In the cloud residues, the relative percentage of large soot-containing particles and particles containing amines was found to be increased compared to the out-of-cloud aerosol, while, in general, organic particles were less abundant in the cloud residues. In the case of amines, this can be explained by the high solubility of the amines, while the large soot-containing particles were found to be internally mixed with inorganics, which explains their activation as cloud condensation nuclei. Furthermore, the results show that during cloud processing, both sulfate and nitrate are added to the residual particles, thereby changing the mixing state and increasing the fraction of particles with nitrate and/or sulfate. This is expected to lead to higher hygroscopicity after cloud evaporation, and therefore to an increase of

Characterization of aerosol particles at the forested site in Lithuania

NASA Astrophysics Data System (ADS)

Rimselyte, I.; Garbaras, A.; Kvietkus, K.; Remeikis, V.

2009-04-01

Atmospheric particulate matter (PM), especially fine particles (particles with aerodynamic diameter less than 1 m, PM1), has been found to play an important role in global climate change, air quality, and human health. The continuous study of aerosol parameters is therefore imperative for better understanding the environmental effects of the atmospheric particles, as well as their sources, formation and transformation processes. The particle size distribution is particularly important, since this physical parameter determines the mass and number density, lifetime and atmospheric transport, or optical scattering behavior of the particles in the atmosphere (Jaenicke, 1998). Over the years several efforts have been made to improve the knowledge about the chemical composition of atmospheric particles as a function of size (Samara and Voutsa, 2005) and to characterize the relative contribution of different components to the fine particulate matter. It is well established that organic materials constitute a highly variable fraction of the atmospheric aerosol. This fraction is predominantly found in the fine size mode in concentrations ranging from 10 to 70% of the total dry fine particle mass (Middlebrook et al., 1998). Although organic compounds are major components of the fine particles, the composition, formation mechanism of organic aerosols are not well understood. This is because particulate organic matter is part of a complex atmospheric system with hundreds of different compounds, both natural and anthropogenic, covering a wide range of chemical properties. The aim of this study was to characterize the forest PM1, and investigate effects of air mass transport on the aerosol size distribution and chemical composition, estimate and provide insights into the sources and characteristics of carbonaceous aerosols through analysis ^13C/12C isotopic ratio as a function of the aerosol particles size. The measurements were performed at the Rugšteliškis integrated

Mass spectrometry of atmospheric aerosols--recent developments and applications. Part II: On-line mass spectrometry techniques.

PubMed

Pratt, Kerri A; Prather, Kimberly A

2012-01-01

Many of the significant advances in our understanding of atmospheric particles can be attributed to the application of mass spectrometry. Mass spectrometry provides high sensitivity with fast response time to probe chemically complex particles. This review focuses on recent developments and applications in the field of mass spectrometry of atmospheric aerosols. In Part II of this two-part review, we concentrate on real-time mass spectrometry techniques, which provide high time resolution for insight into brief events and diurnal changes while eliminating the potential artifacts acquired during long-term filter sampling. In particular, real-time mass spectrometry has been shown recently to provide the ability to probe the chemical composition of ambient individual particles <30 nm in diameter to further our understanding of how particles are formed through nucleation in the atmosphere. Further, transportable real-time mass spectrometry techniques are now used frequently on ground-, ship-, and aircraft-based studies around the globe to further our understanding of the spatial distribution of atmospheric aerosols. In addition, coupling aerosol mass spectrometry techniques with other measurements in series has allowed the in situ determination of chemically resolved particle effective density, refractive index, volatility, and cloud activation properties. Copyright © 2011 Wiley Periodicals, Inc.

Laboratory Experiments and Instrument Intercomparison Studies of Carbonaceous Aerosol Particles

DOE Office of Scientific and Technical Information (OSTI.GOV)

Davidovits, Paul

particles: (a) two well-characterized source of soot particles and (b) a flow reactor for controlled OH and/or O3 oxidation of relevant gas phase species to produce well-characterized SOA particles. After formation, the aerosol particles are subjected to physical and chemical processes that simulate aerosol growth and aging. A suite of instruments in our laboratory is used to characterize the physical and chemical properties of aerosol particles before and after processing. The Time of Flight Aerosol Mass Spectrometer (ToF-AMS) together with a Scanning Mobility Particle Sizer (SMPS) measures particle mass, volume, density, composition (including black carbon content), dynamic shape factor, and fractal dimension. The–ToF-AMS was developed at ARI with Boston College participation. About 120 AMS instruments are now in service (including 5 built for DOE laboratories) performing field and laboratory studies world-wide. Other major instruments include a thermal denuder, two Differential Mobility Analyzers (DMA), a Cloud Condensation Nuclei Counter (CCN), a Thermal desorption Aerosol GC/MS (TAG) and the new Soot Particle Aerosol Mass Spectrometer (SP-AMS). Optical instrumentation required for the studies have been brought to our laboratory as part of ongoing and planned collaborative projects with colleagues from DOE, NOAA and university laboratories. Optical instruments that will be utilized include a Photoacoustic Spectrometer (PAS), a Cavity Ring Down Aerosol Extinction Spectrometer (CRD-AES), a Photo Thermal Interferometer (PTI), a new 7-wavelength Aethalometer and a Cavity Attenuated Phase Shift Extinction Monitor (CAPS). These instruments are providing aerosol absorption, extinction and scattering coefficients at a range of atmospherically relevant wavelengths. During the past two years our work has continued along the lines of our original proposal. We report on 12 completed and/or continuing projects conducted during the period 08/14 to 0814/2015. These projects are

Size distribution dynamics reveal particle-phase chemistry in organic aerosol formation

PubMed Central

Shiraiwa, Manabu; Yee, Lindsay D.; Schilling, Katherine A.; Loza, Christine L.; Craven, Jill S.; Zuend, Andreas; Ziemann, Paul J.; Seinfeld, John H.

2013-01-01

Organic aerosols are ubiquitous in the atmosphere and play a central role in climate, air quality, and public health. The aerosol size distribution is key in determining its optical properties and cloud condensation nucleus activity. The dominant portion of organic aerosol is formed through gas-phase oxidation of volatile organic compounds, so-called secondary organic aerosols (SOAs). Typical experimental measurements of SOA formation include total SOA mass and atomic oxygen-to-carbon ratio. These measurements, alone, are generally insufficient to reveal the extent to which condensed-phase reactions occur in conjunction with the multigeneration gas-phase photooxidation. Combining laboratory chamber experiments and kinetic gas-particle modeling for the dodecane SOA system, here we show that the presence of particle-phase chemistry is reflected in the evolution of the SOA size distribution as well as its mass concentration. Particle-phase reactions are predicted to occur mainly at the particle surface, and the reaction products contribute more than half of the SOA mass. Chamber photooxidation with a midexperiment aldehyde injection confirms that heterogeneous reaction of aldehydes with organic hydroperoxides forming peroxyhemiacetals can lead to a large increase in SOA mass. Although experiments need to be conducted with other SOA precursor hydrocarbons, current results demonstrate coupling between particle-phase chemistry and size distribution dynamics in the formation of SOAs, thereby opening up an avenue for analysis of the SOA formation process. PMID:23818634

Size distribution dynamics reveal particle-phase chemistry in organic aerosol formation.

PubMed

Shiraiwa, Manabu; Yee, Lindsay D; Schilling, Katherine A; Loza, Christine L; Craven, Jill S; Zuend, Andreas; Ziemann, Paul J; Seinfeld, John H

2013-07-16

Organic aerosols are ubiquitous in the atmosphere and play a central role in climate, air quality, and public health. The aerosol size distribution is key in determining its optical properties and cloud condensation nucleus activity. The dominant portion of organic aerosol is formed through gas-phase oxidation of volatile organic compounds, so-called secondary organic aerosols (SOAs). Typical experimental measurements of SOA formation include total SOA mass and atomic oxygen-to-carbon ratio. These measurements, alone, are generally insufficient to reveal the extent to which condensed-phase reactions occur in conjunction with the multigeneration gas-phase photooxidation. Combining laboratory chamber experiments and kinetic gas-particle modeling for the dodecane SOA system, here we show that the presence of particle-phase chemistry is reflected in the evolution of the SOA size distribution as well as its mass concentration. Particle-phase reactions are predicted to occur mainly at the particle surface, and the reaction products contribute more than half of the SOA mass. Chamber photooxidation with a midexperiment aldehyde injection confirms that heterogeneous reaction of aldehydes with organic hydroperoxides forming peroxyhemiacetals can lead to a large increase in SOA mass. Although experiments need to be conducted with other SOA precursor hydrocarbons, current results demonstrate coupling between particle-phase chemistry and size distribution dynamics in the formation of SOAs, thereby opening up an avenue for analysis of the SOA formation process.

Physicochemical Characterization of Capstone Depleted Uranium Aerosols I: Uranium Concentration in Aerosols as a Function of Time and Particle Size

DOE Office of Scientific and Technical Information (OSTI.GOV)

Parkhurst, MaryAnn; Cheng, Yung-Sung; Kenoyer, Judson L.

2009-03-01

During the Capstone Depleted Uranium (DU) Aerosol Study, aerosols containing depleted uranium were produced inside unventilated armored vehicles (i.e., Abrams tanks and Bradley Fighting Vehicles) by perforation with large-caliber DU penetrators. These aerosols were collected and characterized, and the data were subsequently used to assess human health risks to personnel exposed to DU aerosols. The DU content of each aerosol sample was first quantified by radioanalytical methods, and selected samples, primarily those from the cyclone separator grit chambers, were analyzed radiochemically. Deposition occurred inside the vehicles as particles settled on interior surfaces. Settling rates of uranium from the aerosols weremore » evaluated using filter cassette samples that collected aerosol as total mass over eight sequential time intervals. A moving filter was used to collect aerosol samples over time particularly within the first minute after the shot. The results demonstrate that the peak uranium concentration in the aerosol occurred in the first 10 s, and the concentration decreased in the Abrams tank shots to about 50% within 1 min and to less than 2% 30 min after perforation. In the Bradley vehicle, the initial (and maximum) uranium concentration was lower than those observed in the Abrams tank and decreased more slowly. Uranium mass concentrations in the aerosols as a function of particle size were evaluated using samples collected in the cyclone samplers, which collected aerosol continuously for 2 h post perforation. The percentages of uranium mass in the cyclone separator stages from the Abrams tank tests ranged from 38% to 72% and, in most cases, varied with particle size, typically with less uranium associated with the smaller particle sizes. Results with the Bradley vehicle ranged from 18% to 29% and were not specifically correlated with particle size.« less

Contributions of Organic Sources to Atmospheric Aerosol Particle Concentrations and Growth

NASA Astrophysics Data System (ADS)

Russell, L. M.

2017-12-01

Organic molecules are important contributors to aerosol particle mass and number concentrations through primary emissions as well as secondary growth in the atmosphere. New techniques for measuring organic aerosol components in atmospheric particles have improved measurements of this contribution in the last 20 years, including Scanning Transmission X-ray Microscopy Near Edge X-ray Absorption Fine Structure (STXM-NEXAFS), Fourier Transform Infrared spectroscopy (FTIR), and High-Resolution Aerosol Mass Spectrometry (AMS). STXM-NEXAFS individual aerosol particle composition illustrated the variety of morphology of organic components in marine aerosols, the inherent relationships between organic composition and shape, and the links between atmospheric aerosol composition and particles produced in smog chambers. This type of single particle microscopy has also added to size distribution measurements by providing evidence of how surface-controlled and bulk-controlled processes contribute to the growth of particles in the atmosphere. FTIR analysis of organic functional groups are sufficient to distinguish combustion, marine, and terrestrial organic particle sources and to show that each of those types of sources has a surprisingly similar organic functional group composition over four different oceans and four different continents. Augmenting the limited sampling of these off-line techniques with side-by-side inter-comparisons to online AMS provides complementary composition information and consistent quantitative attribution to sources (despite some clear method differences). Single-particle AMS techniques using light scattering and event trigger modes have now also characterized the types of particles found in urban, marine, and ship emission aerosols. Most recently, by combining with off-line techniques, single particle composition measurements have separated and quantified the contributions of organic, sulfate and salt components from ocean biogenic and sea spray

Mass spectrometric analysis and aerodynamic properties of various types of combustion-related aerosol particles

NASA Astrophysics Data System (ADS)

Schneider, J.; Weimer, S.; Drewnick, F.; Borrmann, S.; Helas, G.; Gwaze, P.; Schmid, O.; Andreae, M. O.; Kirchner, U.

2006-12-01

Various types of combustion-related particles in the size range between 100 and 850 nm were analyzed with an aerosol mass spectrometer and a differential mobility analyzer. The measurements were performed with particles originating from biomass burning, diesel engine exhaust, laboratory combustion of diesel fuel and gasoline, as well as from spark soot generation. Physical and morphological parameters like fractal dimension, effective density, bulk density and dynamic shape factor were derived or at least approximated from the measurements of electrical mobility diameter and vacuum aerodynamic diameter. The relative intensities of the mass peaks in the mass spectra obtained from particles generated by a commercial diesel passenger car, by diesel combustion in a laboratory burner, and by evaporating and re-condensing lubrication oil were found to be very similar. The mass spectra from biomass burning particles show signatures identified as organic compounds like levoglucosan but also others which are yet unidentified. The aerodynamic behavior yielded a fractal dimension (Df) of 2.09 +/- 0.06 for biomass burning particles from the combustion of dry beech sticks, but showed values around three, and hence more compact particle morphologies, for particles from combustion of more natural oak. Scanning electron microscope images confirmed the finding that the beech combustion particles were fractal-like aggregates, while the oak combustion particles displayed a much more compact shape. For particles from laboratory combusted diesel fuel, a Df value of 2.35 was found, for spark soot particles, Df [approximate] 2.10. The aerodynamic properties of fractal-like particles from dry beech wood combustion indicate an aerodynamic shape factor [chi] that increases with electrical mobility diameter, and a bulk density of 1.92 g cm-3. An upper limit of [chi] [approximate] 1.2 was inferred for the shape factor of the more compact particles from oak combustion.

Mass-Mobility Characterization of Flame-made ZrO2 Aerosols: Primary Particle Diameter & Extent of Aggregation

PubMed Central

Eggersdorfer, M.L.; Gröhn, A.J.; Sorensen, C.M.; McMurry, P.H.; Pratsinis, S.E.

2013-01-01

Gas-borne nanoparticles undergoing coagulation and sintering form irregular or fractal-like structures affecting their transport, light scattering, effective surface area and density. Here, zirconia (ZrO2) nanoparticles are generated by scalable spray combustion, and their mobility diameter and mass are obtained nearly in-situ by differential mobility analyzer (DMA) and aerosol particle mass (APM) measurements. Using these data, the density of ZrO2 and a power law between mobility and primary particle diameters, the structure of fractal-like particles is determined (mass-mobility exponent, prefactor and average number and surface area mean diameter of primary particles, dva). The dva determined by DMA-APM measurements and this power law is in good agreement with the dva obtained by ex-situ nitrogen adsorption and microscopic analysis. Using this combination of measurements and above power law, the effect of flame spray process parameters (e.g. precursor solution and oxygen flow rate as well as zirconium concentration) on fractal-like particle structure characteristics is investigated in detail. This reveals that predominantly agglomerates (physically-bonded particles) and aggregates (chemically- or sinter-bonded particles) of nanoparticles are formed at low and high particle concentrations, respectively. PMID:22959835

Global distribution of secondary organic aerosol particle phase state

NASA Astrophysics Data System (ADS)

Shiraiwa, M.; Li, Y., Sr.; Tsimpidi, A.; Karydis, V.; Berkemeier, T.; Pandis, S. N.; Lelieveld, J.; Koop, T.; Poeschl, U.

2016-12-01

Secondary organic aerosols (SOA) account for a large fraction of submicron particles in the atmosphere and play a key role in aerosol effects on climate, air quality and public health. The formation and aging of SOA proceed through multiple steps of chemical reaction and mass transport in the gas and particle phases, which is challenging for the interpretation of field measurements and laboratory experiments as well as accurate representation of SOA evolution in atmospheric aerosol models. SOA particles can adopt liquid, semi-solid and amorphous solid (glassy) phase states depending on chemical composition, relative humidity and temperature. The particle phase state is crucial for various atmospheric gas-particle interactions, including SOA formation, heterogeneous and multiphase reactions and ice nucleation. We found that organic compounds with a wide variety of functional groups fall into molecular corridors, characterized by a tight inverse correlation between molar mass and volatility. Based on the concept of molecular corridors, we develop a method to estimate glass transition temperatures based on the molar mass and molecular O:C ratio of SOA components, which is a key property for determination of particle phase state. We use the global chemistry climate model EMAC with the organic aerosol module ORACLE to predict the atmospheric SOA phase state. For the planetary boundary layer, global simulations indicate that SOA is mostly liquid in tropical and polar air with high relative humidity, semi-solid in the mid-latitudes, and solid over dry lands. We find that in the middle and upper troposphere (>500 hPa) SOA should be mostly in a glassy solid phase state. Thus, slow diffusion of water, oxidants, and organic molecules could kinetically limit gas-particle interactions of SOA in the free and upper troposphere, promote ice nucleation and facilitate long-range transport of reactive and toxic organic pollutants embedded within SOA.

Highly time-resolved chemical characterization of atmospheric submicron particles during 2008 Beijing Olympic Games using an Aerodyne High-Resolution Aerosol Mass Spectrometer

NASA Astrophysics Data System (ADS)

Huang, X.-F.; He, L.-Y.; Hu, M.; Canagaratna, M. R.; Sun, Y.; Zhang, Q.; Zhu, T.; Xue, L.; Zeng, L.-W.; Liu, X.-G.; Zhang, Y.-H.; Jayne, J. T.; Ng, N. L.; Worsnop, D. R.

2010-09-01

As part of Campaigns of Air Quality Research in Beijing and Surrounding Region-2008 (CAREBeijing-2008), an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed in urban Beijing to characterize submicron aerosol particles during the time of 2008 Beijing Olympic Games and Paralympic Games (24 July to 20 September 2008). The campaign mean PM1 mass concentration was 63.1 ± 39.8 μg m-3; the mean composition consisted of organics (37.9%), sulfate (26.7%), ammonium (15.9%), nitrate (15.8%), black carbon (3.1%), and chloride (0.87%). The average size distributions of the species (except BC) were all dominated by an accumulation mode peaking at about 600 nm in vacuum aerodynamic diameter, and organics was characterized by an additional smaller mode extending below 100 nm. Positive Matrix Factorization (PMF) analysis of the high resolution organic mass spectral dataset differentiated the organic aerosol into four components, i.e., hydrocarbon-like (HOA), cooking-related (COA), and two oxygenated organic aerosols (OOA-1 and OOA-2), which on average accounted for 18.1, 24.4, 33.7 and 23.7% of the total organic mass, respectively. The HOA was identified to be closely associated with primary combustion sources, while the COA mass spectrum and diurnal pattern showed similar characteristics to that measured for cooking emissions. The OOA components correspond to aged secondary organic aerosol. Although the two OOA components have similar elemental (O/C, H/C) compositions, they display differences in mass spectra and time series which appear to correlate with the different source regions sampled during the campaign. Back trajectory clustering analysis indicated that the southerly air flows were associated with the highest PM1 pollution during the campaign. Aerosol particles in southern airmasses were especially rich in inorganic and oxidized organic species. Aerosol particles in northern airmasses contained a large fraction of primary HOA

FTIR Analysis of Functional Groups in Aerosol Particles

NASA Astrophysics Data System (ADS)

Shokri, S. M.; McKenzie, G.; Dransfield, T. J.

2012-12-01

Secondary organic aerosols (SOA) are suspensions of particulate matter composed of compounds formed from chemical reactions of organic species in the atmosphere. Atmospheric particulate matter can have impacts on climate, the environment and human health. Standardized techniques to analyze the characteristics and composition of complex secondary organic aerosols are necessary to further investigate the formation of SOA and provide a better understanding of the reaction pathways of organic species in the atmosphere. While Aerosol Mass Spectrometry (AMS) can provide detailed information about the elemental composition of a sample, it reveals little about the chemical moieties which make up the particles. This work probes aerosol particles deposited on Teflon filters using FTIR, based on the protocols of Russell, et al. (Journal of Geophysical Research - Atmospheres, 114, 2009) and the spectral fitting algorithm of Takahama, et al (submitted, 2012). To validate the necessary calibration curves for the analysis of complex samples, primary aerosols of key compounds (e.g., citric acid, ammonium sulfate, sodium benzoate) were generated, and the accumulated masses of the aerosol samples were related to their IR absorption intensity. These validated calibration curves were then used to classify and quantify functional groups in SOA samples generated in chamber studies by MIT's Kroll group. The fitting algorithm currently quantifies the following functionalities: alcohols, alkanes, alkenes, amines, aromatics, carbonyls and carboxylic acids.

Single particles measured by a light scattering module coupled to a time-of-flight aerosol mass spectrometer onboard the NOAA P-3 aircraft during SENEX

NASA Astrophysics Data System (ADS)

Liao, J.; Middlebrook, A. M.; Welti, A.; Sueper, D.; Murphy, D. M.

2014-12-01

Single particles in the eastern US were characterized by a light scattering module coupled to a time-of-flight aerosol mass spectrometer (LS-ToF-AMS) onboard the NOAA P-3 aircraft during the Southeastern Nexus (SENEX) campaign. Single particle data were collected for 30 seconds every 5 minutes. Aerosols larger than 200-300 nm in vacuum aerodynamic diameter can be optically detected by the 405 nm crystal laser and trigger the saving of single particle mass spectra. The measured single particles are internally-mixed as expected. The single particles were classified as prompt, delayed, and null based on the chemical ion signal arrival time difference between prediction from the light scattering signal and measurement by mass spectrometer and the presence or absence of a mass spectrum. On average the number fraction of particles detected as prompt, delayed, and null (no spectrum) is about 30%, 10%, and 60%. The number fraction of these three particle types varied with aerosol size, chemical composition and the investigation region and will be discussed in detail. For example, the number fraction of prompt particles was significantly higher for the flight to the Pennsylvania natural gas shale region on July 6, 2013, which is probably related to the chemical composition (more acidic) and phase of the ambient particles. These particle types and detection efficiency are related to the bouncing effect on the vaporizer and may provide insight into the non-unit AMS collection efficiency. Moreover, most of the particles larger than 800 nm in vacuum aerodynamic diameter sized with the traditional AMS PToF mode are delayed particles and their mass spectral signals appear to be affected by this process.

Single particle aerosol mass spectrometry of coal combustion particles associated with high lung cancer rates in Xuanwei and Fuyuan, China.

PubMed

Lu, Senlin; Tan, Zhengying; Liu, Pinwei; Zhao, Hui; Liu, Dingyu; Yu, Shang; Cheng, Ping; Win, Myat Sandar; Hu, Jiwen; Tian, Linwei; Wu, Minghong; Yonemochi, Shinich; Wang, Qingyue

2017-11-01

Coal combustion particles (CCPs) are linked to the high incidence of lung cancer in Xuanwei and in Fuyuan, China, but studies on the chemical composition of the CCPs are still limited. Single particle aerosol mass spectrometry (SPAMS) was recently developed to measure the chemical composition and size of single particles in real-time. In this study, SPAMS was used to measure individual combustion particles emitted from Xuanwei and Fuyuan coal samples and the results were compared with those by ICP-MS and transmission electron microscopy (TEM). The total of 38,372 particles mass-analyzed by SPAMS can be divided into 9 groups based on their chemical composition and their number percentages: carbonaceous, Na-rich, K-rich, Al-rich, Fe-rich, Si-rich, Ca-rich, heavy metal-bearing, and PAH-bearing particles. The carbonaceous and PAH-bearing particles are enriched in the size range below 0.56 μm, Fe-bearing particles range from 0.56 to 1.0 μm in size, and heavy metals such as Ti, V, Cr, Cu, Zn, and Pb have diameters below 1 μm. The TEM results show that the particles from Xuanwei and Fuyuan coal combustion can be classified into soot aggregates, Fe-rich particles, heavy metal containing particles, and mineral particles. Non-volatile particles detected by SPAMS could also be observed with TEM. The number percentages by SPAMS also correlate with the mass concentrations measured by ICP-MS. Our results could provide valuable insight for understanding high lung cancer incidence in the area. Copyright © 2017 Elsevier Ltd. All rights reserved.

Supercritical Fluid Extraction and Analysis of Tropospheric Aerosol Particles

NASA Astrophysics Data System (ADS)

Hansen, Kristen J.

An integrated sampling and supercritical fluid extraction (SFE) cell has been designed for whole-sample analysis of organic compounds on tropospheric aerosol particles. The low-volume extraction cell has been interfaced with a sampling manifold for aerosol particle collection in the field. After sample collection, the entire SFE cell was coupled to a gas chromatograph; after on-line extraction, the cryogenically -focused sample was separated and the volatile compounds detected with either a mass spectrometer or a flame ionization detector. A 20-minute extraction at 450 atm and 90 ^circC with pure supercritical CO _2 is sufficient for quantitative extraction of most volatile compounds in aerosol particle samples. A comparison between SFE and thermal desorption, the traditional whole-sample technique for analyses of this type, was performed using ambient aerosol particle samples, as well as samples containing known amounts of standard analytes. The results of these studies indicate that SFE of atmospheric aerosol particles provides quantitative measurement of several classes of organic compounds. SFE provides information that is complementary to that gained by the thermal desorption analysis. The results also indicate that SFE with CO _2 can be validated as an alternative to thermal desorption for quantitative recovery of several organic compounds. In 1989, the organic constituents of atmospheric aerosol particles collected at Niwot Ridge, Colorado, along with various physical and meteorological data, were measured during a collaborative field study. Temporal changes in the composition of samples collected during summertime at the rural site were studied. Thermal desorption-GC/FID was used to quantify selected compounds in samples collected during the field study. The statistical analysis of the 1989 Niwot Ridge data set is presented in this work. Principal component analysis was performed on thirty-one variables selected from the data set in order to ascertain

Development and characterization of an aircraft aerosol time-of-flight mass spectrometer.

PubMed

Pratt, Kerri A; Mayer, Joseph E; Holecek, John C; Moffet, Ryan C; Sanchez, Rene O; Rebotier, Thomas P; Furutani, Hiroshi; Gonin, Marc; Fuhrer, Katrin; Su, Yongxuan; Guazzotti, Sergio; Prather, Kimberly A

2009-03-01

Vertical and horizontal profiles of atmospheric aerosols are necessary for understanding the impact of air pollution on regional and global climate. To gain further insight into the size-resolved chemistry of individual atmospheric particles, a smaller aerosol time-of-flight mass spectrometer (ATOFMS) with increased data acquisition capabilities was developed for aircraft-based studies. Compared to previous ATOFMS systems, the new instrument has a faster data acquisition rate with improved ion transmission and mass resolution, as well as reduced physical size and power consumption, all required advances for use in aircraft studies. In addition, real-time source apportionment software allows the immediate identification and classification of individual particles to guide sampling decisions while in the field. The aircraft (A)-ATOFMS was field-tested on the ground during the Study of Organic Aerosols in Riverside, CA (SOAR) and aboard an aircraft during the Ice in Clouds Experiment-Layer Clouds (ICE-L). Initial results from ICE-L represent the first reported aircraft-based single-particle dual-polarity mass spectrometry measurements and provide an increased understanding of particle mixing state as a function of altitude. Improved ion transmission allows for the first single-particle detection of species out to approximately m/z 2000, an important mass range for the detection of biological aerosols and oligomeric species. In addition, high time resolution measurements of single-particle mixing state are demonstrated and shown to be important for airborne studies where particle concentrations and chemistry vary rapidly.

Sources and composition of submicron organic mass in marine aerosol particles

NASA Astrophysics Data System (ADS)

Frossard, Amanda A.; Russell, Lynn M.; Burrows, Susannah M.; Elliott, Scott M.; Bates, Timothy S.; Quinn, Patricia K.

2014-11-01

The sources and composition of atmospheric marine aerosol particles (aMA) have been investigated with a range of physical and chemical measurements from open-ocean research cruises. This study uses the characteristic functional group composition (from Fourier transform infrared spectroscopy) of aMA from five ocean regions to show the following: (i) The organic functional group composition of aMA that can be identified as mainly atmospheric primary marine (ocean derived) aerosol particles (aPMA) is 65 ± 12% hydroxyl, 21 ± 9% alkane, 6 ± 6% amine, and 7 ± 8% carboxylic acid functional groups. Contributions from photochemical reactions add carboxylic acid groups (15%-25%), shipping effluent in seawater and ship emissions add additional alkane groups (up to 70%), and coastal or continental emissions mix in alkane and carboxylic acid groups. (ii) The organic composition of aPMA is nearly identical to model-generated primary marine aerosol particles from bubbled seawater (gPMA, which has 55 ± 14% hydroxyl, 32 ± 14% alkane, and 13 ± 3% amine functional groups), indicating that its overall functional group composition is the direct consequence of the organic constituents of the seawater source. (iii) While the seawater organic functional group composition was nearly invariant across all three ocean regions studied and the ratio of organic carbon to sodium (OC/Na+) in the gPMA remained nearly constant over a broad range of chlorophyll a concentrations, the gPMA alkane group fraction appeared to increase with chlorophyll a concentrations (r = 0.66). gPMA from productive seawater had a larger fraction of alkane functional groups (42 ± 9%) compared to gPMA from nonproductive seawater (22 ± 10%), perhaps due to the presence of surfactants in productive seawater that stabilize the bubble film and lead to preferential drainage of the more soluble (lower alkane group fraction) organic components. gPMA has a hydroxyl group absorption peak location characteristic of

Fullerene Soot in Eastern China Air: Results from Soot Particle-Aerosol Mass Spectrometer

NASA Astrophysics Data System (ADS)

Wang, J.; Ge, X.; Chen, M.; Zhang, Q.; Yu, H.; Sun, Y.; Worsnop, D. R.; Collier, S.

2015-12-01

In this work, we present for the first time, the observation and quantification of fullerenes in ambient airborne particulate using an Aerodyne Soot Particle - Aerosol Mass Spectrometer (SP-AMS) deployed during 2015 winter in suburban Nanjing, a megacity in eastern China. The laser desorption and electron impact ionization techniques employed by the SP-AMS allow us to differentiate various fullerenes from other aerosol components. Mass spectrum of the identified fullerene soot is consisted by a series of high molecular weight carbon clusters (up to m/z of 2000 in this study), almost identical to the spectral features of commercially available fullerene soot, both with C70 and C60 clusters as the first and second most abundant species. This type of soot was observed throughout the entire study period, with an average mass loading of 0.18 μg/m3, accounting for 6.4% of the black carbon mass, 1.2% of the total organic mass. Temporal variation and diurnal pattern of fullerene soot are overall similar to those of black carbon, but are clearly different in some periods. Combining the positive matrix factorization, back-trajectory and analyses of the meteorological parameters, we identified the petrochemical industrial plants situating upwind from the sampling site, as the major source of fullerene soot. In this regard, our findings imply the ubiquitous presence of fullerene soot in ambient air of industry-influenced area, especially the oil and gas production regions. This study also offers new insights into the characterization of fullerenes from other environmental samples via the advanced SP-AMS technique.

Experimental demonstration that a free-falling aerosol particle obeys a fluctuation theorem

NASA Astrophysics Data System (ADS)

Wong, Chun-Shang; Goree, J.; Gopalakrishnan, Ranganathan

2018-05-01

We investigate the fluctuating motion of an aerosol particle falling in air. Using a Millikan-like setup, we tracked a 1-μ m sphere falling at its terminal velocity. We observe occurrences of particles undergoing upward displacements against the force of gravity, so that negative work is done briefly. These negative-work events have a probability that is shown to obey the work fluctuation theorem. This experimental confirmation of the theorem's applicability to aerosols leads us to develop and demonstrate an application: an in situ measurement of an aerosol particle's mass.

Wintertime water-soluble aerosol composition and particle water content in Fresno, California

NASA Astrophysics Data System (ADS)

Parworth, Caroline L.; Young, Dominique E.; Kim, Hwajin; Zhang, Xiaolu; Cappa, Christopher D.; Collier, Sonya; Zhang, Qi

2017-03-01

The composition and concentrations of water-soluble gases and ionic aerosol components were measured from January to February 2013 in Fresno, CA, with a particle-into-liquid sampler with ion chromatography and annular denuders. The average (±1σ) ionic aerosol mass concentration was 15.0 (±9.4) µg m-3, and dominated by nitrate (61%), followed by ammonium, sulfate, chloride, potassium, nitrite, and sodium. Aerosol-phase organic acids, including formate and glycolate, and amines including methylaminium, triethanolaminium, ethanolaminium, dimethylaminium, and ethylaminium were also detected. Although the dominant species all came from secondary aerosol formation, there were primary sources of ionic aerosols as well, including biomass burning for potassium and glycolate, sea spray for sodium, chloride, and dimethylamine, and vehicles for formate. Particulate methanesulfonic acid was also detected and mainly associated with terrestrial sources. On average, the molar concentration of ammonia was 49 times greater than nitric acid, indicating that ammonium nitrate formation was limited by nitric acid availability. Particle water was calculated based on the Extended Aerosol Inorganics Model (E-AIM) thermodynamic prediction of inorganic particle water and κ-Köhler theory approximation of organic particle water. The average (±1σ) particle water concentration was 19.2 (±18.6) µg m-3, of which 90% was attributed to inorganic species. The fractional contribution of particle water to total fine particle mass averaged at 36% during this study and was greatest during early morning and night and least during the day. Based on aqueous-phase concentrations of ions calculated by using E-AIM, the average (±1σ) pH of particles in Fresno during the winter was estimated to be 4.2 (±0.2).

Mixed-phase aerosol particles

NASA Astrophysics Data System (ADS)

Corti, T.; Krieger, U. K.; Koop, T.; Peter, T.

2003-04-01

Within a liquid aerosol particle a solid phase may coexist with the liquid over a wide range of ambient conditions. The optical properties of such particles are of interest for a number of reasons. They will affect the scattering albedo of atmospheric aerosols, may cause depolarisation in lidar measurements, and potentially open a window for studying the internal morphology and physical properties (e.g. wetting properties, diffusion constants) of composite particles in laboratory experiments. In this contribution, we will present results of experimental and theoretical work on mixed-phase aerosol particles. The optical properties of mixed-phase particles depend on the location of the inclusion in the liquid phase, which is determined by the surface tensions of the involved interfaces. In the case of complete wetting, the energetically favoured position of the inclusion is in the volume of the liquid phase. For partial wetting, a position at the surface of the liquid phase is favoured, with the contact angle between the solid, liquid and air being described by Young's equation. For systems with small contact angles, the difference in energy between an inclusion situated at the droplets surface and in its volume may be so small that the thermal energy kT is sufficient to displace the inclusion from the droplet surface into its volume. The critical contact angle depends on the size of the inclusion and the droplet and ranges from 0.1 to 10 degrees. Examples of mixed-phase aerosol particles are aged soot particles and sea salt particles at low relative humidity. For aged soot, contact angles on sulphuric acid clearly above 10 degrees have been reported, so that soot inclusions are expected to be located at the surface of aerosol particles. For mixed-phase sea salt particles, consisting of a solid NaCl inclusion and an aqueous solution of mainly NaCl and MgCl2, our measurements on macroscopic NaCl crystals show a contact angle clearly below 10 degrees and possibly as

Modeling Gas-Particle Partitioning of SOA: Effects of Aerosol Physical State and RH

NASA Astrophysics Data System (ADS)

Zuend, A.; Seinfeld, J.

2011-12-01

Aged tropospheric aerosol particles contain mixtures of inorganic salts, acids, water, and a large variety of organic compounds. In liquid aerosol particles non-ideal mixing of all species determines whether the condensed phase undergoes liquid-liquid phase separation or whether it is stable in a single mixed phase, and whether it contains solid salts in equilibrium with their saturated solution. The extended thermodynamic model AIOMFAC is able to predict such phase states by representing the variety of organic components using functional groups within a group-contribution concept. The number and composition of different condensed phases impacts the diversity of reaction media for multiphase chemistry and the gas-particle partitioning of semivolatile species. Recent studies show that under certain conditions biogenic and other organic-rich particles can be present in a highly viscous, semisolid or amorphous solid physical state, with consequences regarding reaction kinetics and mass transfer limitations. We present results of new gas-particle partitioning computations for aerosol chamber data using a model based on AIOMFAC activity coefficients and state-of-the-art vapor pressure estimation methods. Different environmental conditions in terms of temperature, relative humidity (RH), salt content, amount of precursor VOCs, and physical state of the particles are considered. We show how modifications of absorptive and adsorptive gas-particle mass transfer affects the total aerosol mass in the calculations and how the results of these modeling approaches compare to data of aerosol chamber experiments, such as alpha-pinene oxidation SOA. For a condensed phase in a mixed liquid state containing ammonium sulfate, the model predicts liquid-liquid phase separation up to high RH in case of, on average, moderately hydrophilic organic compounds, such as first generation oxidation products of alpha-pinene. The computations also reveal that treating liquid phases as ideal

LASER DESORPTION IONIZATION OF ULTRAFINE AEROSOL PARTICLES. (R823980)

EPA Science Inventory

On-line analysis of ultrafine aerosol particle in the 12 to 150 nm size range is performed by
laser desorption/ionization. Particles are size selected with a differential mobility analyzer and then
sent into a linear time-of-flight mass spectrometer where they are ablated w...

Ambient measurement of fluorescent aerosol particles with a WIBS in the Yangtze River Delta of China: potential impacts of combustion-related aerosol particles

NASA Astrophysics Data System (ADS)

Yu, Xiawei; Wang, Zhibin; Zhang, Minghui; Kuhn, Uwe; Xie, Zhouqing; Cheng, Yafang; Pöschl, Ulrich; Su, Hang

2016-09-01

Fluorescence characteristics of aerosol particles in a polluted atmosphere were studied using a wideband integrated bioaerosol spectrometer (WIBS-4A) in Nanjing, Yangtze River Delta area of China. We observed strong diurnal and day-to-day variations of fluorescent aerosol particles (FAPs). The average number concentrations of FAPs (1-15 µm) detected in the three WIBS measurement channels (FL1: 0.6 cm-3, FL2: 3.4 cm-3, FL3: 2.1 cm-3) were much higher than those observed in forests and rural areas, suggesting that FAPs other than bioaerosols were detected. We found that the number fractions of FAPs were positively correlated with the black carbon mass fraction, especially for the FL1 channel, indicating a large contribution of combustion-related aerosols. To distinguish bioaerosols from combustion-related FAPs, we investigated two classification schemes for use with WIBS data. Our analysis suggests a strong size dependence for the fractional contributions of different types of FAPs. In the FL3 channel, combustion-related particles seem to dominate the 1-2 µm size range while bioaerosols dominate the 2-5 µm range. The number fractions of combustion-related particles and non-combustion-related particles to total aerosol particles were ˜ 11 and ˜ 5 %, respectively.

Aerosol Vacuum-Assisted Plasma Ionization (Aero-VaPI) Coupled to Ion Mobility-Mass Spectrometry

NASA Astrophysics Data System (ADS)

Blair, Sandra L.; Ng, Nga L.; Zambrzycki, Stephen C.; Li, Anyin; Fernández, Facundo M.

2018-02-01

In this communication, we report on the real-time analysis of organic aerosol particles by Vacuum-assisted Plasma Ionization-Mass Spectrometry (Aero-VaPI-MS) using a home-built VaPI ion source coupled to a Synapt G2-S HDMS ion mobility-mass spectrometry (IM-MS) system. Standards of organic molecules of interest in prebiotic chemistry were used to generate aerosols. Monocaprin and decanoic acid aerosol particles were successfully detected in both the positive and negative ion modes, respectively. A complex aerosol mixture of different sizes of polymers of L-malic acid was also examined through ion mobility (IM) separations, resulting in the detection of polymers of up to eight monomeric units. This noncommercial plasma ion source is proposed as a low cost alternative to other plasma ionization platforms used for aerosol analysis, and a higher-performance alternative to more traditional aerosol mass spectrometers. VaPI provides robust online ionization of organics in aerosols without extensive ion activation, with the coupling to IM-MS providing higher peak capacity and excellent mass accuracy. [Figure not available: see fulltext.

Chemical Characterization of Particulate Matter at the La Porte site Using an Aerosol Mass Spectrometer

NASA Astrophysics Data System (ADS)

Silva, P. J.; Worsnop, D.; Canagaratna, M.; Jimenez, J. L.; Delia, A.; Purvis, K.; Davidovits, P.

2001-12-01

During the summer of 2000, a large atmospheric chemistry field campaign took place in the Greater Houston area in conjunction with an EPA supersite. As part of the campaign, we operated an aerosol mass spectrometer from 20 August, 2000 until 15 September, 2000. The aerosol mass spectrometer (AMS) obtained chemical composition data and particle size distributions continuously with 10 minute averaging times. The measured aerosol mass concentration ranged from approximately 2 μ g m-3 to a high of 30 μ g m-3. Ammonium and sulfate were the two dominant chemical species present during most of the study. The mass concentration of particulate nitrate was typically less than a few μ g m-3, with one major nitrate event on 23 August, 2000. Very small amounts of non-sea salt chloride were detected in the particles, typically less than one μ g m-3, again with the largest value detected on 23 August 2000. In addition to the inorganic species, several different organic aerosol types were identified based on simple evaluation of mass spectral and size distribution data. Three organic particle types appear to be from discrete primary sources of organic aerosol. A combustion particle type displays mass spectra similar to those observed from diesel exhaust emissions. The temporal variation of this type shows sharp spikes, consistent with primary sources and sharp plumes that drift pass. A second organic particle type is responsible for the largest particle mass concentrations observed during the entire study, occurring during a fire episode on 5-6 September, 2000. The mass spectra exhibit characteristic peaks representative of markers for compounds from biomass burning, including levoglucosan and dehydroabietic acid. A third organic particle type observed during the study exhibits peaks in the mass spectra that are characteristic of fluorinated hydrocarbons and are similar to mass spectra of pump oil. This particle type contributes several μ g m-3 to the ambient particle mass

Novel Measurements of Aerosol Particle Interfaces Using Biphasic Microfluidics

NASA Astrophysics Data System (ADS)

Metcalf, A. R.; Dutcher, C. S.

2014-12-01

Secondary organic aerosol (SOA) particles are nearly ubiquitous in the atmosphere and yet there remains large uncertainties in their formation processes and ambient properties. These particles are complex microenvironments, which can contain multiple interfaces due to internal aqueous-organic phase partitioning and to the external liquid-vapor surface. These aerosol interfaces can profoundly affect the fate of condensable organic compounds emitted into the atmosphere by altering the way in which organic vapors interact with the ambient aerosol. Aerosol interfaces affect particle internal structure, species uptake, equilibrium partitioning, activation to cloud condensation or ice nuclei, and optical properties. For example, organic thin films can shield the core of the aerosol from the ambient environment, which may disrupt equilibrium partitioning and mass transfer. To improve our ability to accurately predict the fate of SOA in the atmosphere, we must improve our knowledge of aerosol interfaces and their interactions with the ambient environment. Few technologies exist to accurately probe aerosol interfaces at atmospherically-relevant conditions. In this talk, a novel method using biphasic microscale flows will be introduced for generating, trapping, and perturbing complex interfaces at atmospherically relevant conditions. These microfluidic experiments utilize high-speed imaging to monitor interfacial phenomena at the microscale and are performed with phase contrast and fluorescence microscopy on a temperature-controlled inverted microscope stage. From these experiments, interfacial thermodynamic properties such as surface tension, rheological properties such as interfacial moduli, and kinetic properties such as mass transfer coefficients can be measured or inferred. Chemical compositions of the liquid phases studied here span a range of viscosities and include electrolyte and water soluble organic acid species often observed in the atmosphere, such as mixtures

Microphysical processes affecting stratospheric aerosol particles

NASA Technical Reports Server (NTRS)

Hamill, P.; Toon, O. B.; Kiang, C. S.

1977-01-01

Physical processes which affect stratospheric aerosol particles include nucleation, condensation, evaporation, coagulation and sedimentation. Quantitative studies of these mechanisms to determine if they can account for some of the observed properties of the aerosol are carried out. It is shown that the altitude range in which nucleation of sulfuric acid-water solution droplets can take place corresponds to that region of the stratosphere where the aerosol is generally found. Since heterogeneous nucleation is the dominant nucleation mechanism, the stratospheric solution droplets are mainly formed on particles which have been mixed up from the troposphere or injected into the stratosphere by volcanoes or meteorites. Particle growth by heteromolecular condensation can account for the observed increase in mixing ratio of large particles in the stratosphere. Coagulation is important in reducing the number of particles smaller than 0.05 micron radius. Growth by condensation, applied to the mixed nature of the particles, shows that available information is consistent with ammonium sulfate being formed by liquid phase chemical reactions in the aerosol particles. The upper altitude limit of the aerosol layer is probably due to the evaporation of sulfuric acid aerosol particles, while the lower limit is due to mixing across the tropopause.

A numerical determination of the evolution of cloud drop spectra due to condensation on natural aerosol particles

NASA Technical Reports Server (NTRS)

Lee, I. Y.; Haenel, G.; Pruppacher, H. R.

1980-01-01

The time variation in size of aerosol particles growing by condensation is studied numerically by means of an air parcel model which allows entrainment of air and aerosol particles. Particles of four types of aerosols typically occurring in atmospheric air masses were considered. The present model circumvents any assumption about the size distribution and chemical composition of the aerosol particles by basing the aerosol particle growth on actually observed size distributions and on observed amounts of water taken up under equilibrium by a deposit of the aerosol particles. Characteristic differences in the drop size distribution, liquid water content and supersaturation were found for the clouds which evolved from the four aerosol types considered.

Characterization of key aerosol, trace gas and meteorological properties and particle formation and growth processes dependent on air mass origins in coastal Southern Spain

NASA Astrophysics Data System (ADS)

Diesch, J.; Drewnick, F.; Sinha, V.; Williams, J.; Borrmann, S.

2011-12-01

The chemical composition and concentration of aerosols at a certain site can vary depending on season, the air mass source region and distance from sources. Regardless of the environment, new particle formation (NPF) events are one of the major sources for ultrafine particles which are potentially hazardous to human health. Grown particles are optically active and efficient CCN resulting in important implications for visibility and climate (Zhang et al., 2004). The study presented here is intended to provide information about various aspects of continental, urban and marine air masses reflected by wind patterns of the air arriving at the measurement site. Additionally we will be focusing on NPF events associated with different types of air masses affecting their emergence and temporal evolution. Measurements of the ambient aerosol, various trace gases and meteorological parameters were performed within the framework of the DOMINO (Diel Oxidant Mechanisms In relation to Nitrogen Oxides) project. The field campaign took place from mid-November to mid-December 2008 at the atmospheric research station "El Arenosillo" located at the interface between a natural park, industrial cities (Huelva, Seville) and the Atlantic Ocean. Number and mass as well as PAH and black carbon concentrations were measured in PM1 and size distribution instruments covered the size range 6 nm up to 32 μm. The chemical composition of the non-refractory submicron aerosol was measured by means of an Aerosol Mass Spectrometer (AMS). In order to evaluate the characteristics of different air masses linking local and regional sources as well as NPF processes, characteristic air mass types were classified dependent on backwards trajectory pathways and local meteorology. Large nuclei mode concentrations in the number size distribution were found within continental and urban influenced air mass types due to frequently occurring NPF events. Exploring individual production and sink variables, sulfuric

Online differentiation of mineral phase in aerosol particles by ion formation mechanism using a LAAP-TOF single-particle mass spectrometer

NASA Astrophysics Data System (ADS)

Marsden, Nicholas A.; Flynn, Michael J.; Allan, James D.; Coe, Hugh

2018-01-01

Mineralogy of silicate mineral dust has a strong influence on climate and ecosystems due to variation in physiochemical properties that result from differences in composition and crystal structure (mineral phase). Traditional offline methods of analysing mineral phase are labour intensive and the temporal resolution of the data is much longer than many atmospheric processes. Single-particle mass spectrometry (SPMS) is an established technique for the online size-resolved measurement of particle composition by laser desorption ionisation (LDI) followed by time-of-flight mass spectrometry (TOF-MS). Although non-quantitative, the technique is able to identify the presence of silicate minerals in airborne dust particles from markers of alkali metals and silicate molecular ions in the mass spectra. However, the differentiation of mineral phase in silicate particles by traditional mass spectral peak area measurements is not possible. This is because instrument function and matrix effects in the ionisation process result in variations in instrument response that are greater than the differences in composition between common mineral phases.In this study, we introduce a novel technique that enables the differentiation of mineral phase in silicate mineral particles by ion formation mechanism measured from subtle changes in ion arrival times at the TOF-MS detector. Using a combination of peak area and peak centroid measurements, we show that the arrangement of the interstitial alkali metals in the crystal structure, an important property in silicate mineralogy, influences the ion arrival times of elemental and molecular ion species in the negative ion mass spectra. A classification scheme is presented that allowed for the differentiation of illite-smectite, kaolinite and feldspar minerals on a single-particle basis. Online analysis of mineral dust aerosol generated from clay mineral standards produced mineral fractions that are in agreement with bulk measurements reported by

Cloud droplet activation through oxidation of organic aerosol influenced by temperature and particle phase state: CLOUD ACTIVATION BY AGED ORGANIC AEROSOL

DOE PAGES

Slade, Jonathan H.; Shiraiwa, Manabu; Arangio, Andrea; ...

2017-02-04

Chemical aging of organic aerosol (OA) through multiphase oxidation reactions can alter their cloud condensation nuclei (CCN) activity and hygroscopicity. However, the oxidation kinetics and OA reactivity depend strongly on the particle phase state, potentially influencing the hydrophobic-to-hydrophilic conversion rate of carbonaceous aerosol. Here, amorphous Suwannee River fulvic acid (SRFA) aerosol particles, a surrogate humic-like substance (HULIS) that contributes substantially to global OA mass, are oxidized by OH radicals at different temperatures and phase states. When oxidized at low temperature in a glassy solid state, the hygroscopicity of SRFA particles increased by almost a factor of two, whereas oxidation ofmore » liquid-like SRFA particles at higher temperatures did not affect CCN activity. Low-temperature oxidation appears to promote the formation of highly-oxygenated particle-bound fragmentation products with lower molar mass and greater CCN activity, underscoring the importance of chemical aging in the free troposphere and its influence on the CCN activity of OA.« less

Effect of secondary organic aerosol coating thickness on the real-time detection and characterization of biomass-burning soot by two particle mass spectrometers

DOE PAGES

Ahern, Adam T.; Subramanian, Ramachandran; Saliba, Georges; ...

2016-12-22

Biomass burning is a large source of light-absorbing refractory black carbon (rBC) particles with a wide range of morphologies and sizes. The net radiative forcing from these particles is strongly dependent on the amount and composition of non-light-absorbing material internally mixed with the rBC and on the morphology of the mixed particles. Understanding how the mixing state and morphology of biomass-burning aerosol evolves in the atmosphere is critical for constraining the influence of these particles on radiative forcing and climate. We investigated the response of two commercial laser-based particle mass spectrometers, the vacuum ultraviolet (VUV) ablation LAAPTOF and the IRmore » vaporization SP-AMS, to monodisperse biomass-burning particles as we sequentially coated the particles with secondary organic aerosol (SOA) from α-pinene ozonolysis. We studied three mobility-selected soot core sizes, each with a number of successively thicker coatings of SOA applied. Using IR laser vaporization, the SP-AMS had different changes in sensitivity to rBC compared to potassium as a function of applied SOA coatings. We show that this is due to different effective beam widths for the IR laser vaporization region of potassium versus black carbon. The SP-AMS's sensitivity to black carbon (BC) mass was not observed to plateau following successive SOA coatings, despite achieving high OA : BC mass ratios greater than 9. We also measured the ion fragmentation pattern of biomass-burning rBC and found it changed only slightly with increasing SOA mass. The average organic matter ion signal measured by the LAAPTOF demonstrated a positive correlation with the condensed SOA mass on individual particles, despite the inhomogeneity of the particle core compositions. This demonstrates that the LAAPTOF can obtain quantitative mass measurements of aged soot-particle composition from realistic biomass-burning particles with complex morphologies and composition.« less

Effect of secondary organic aerosol coating thickness on the real-time detection and characterization of biomass-burning soot by two particle mass spectrometers

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ahern, Adam T.; Subramanian, Ramachandran; Saliba, Georges

Biomass burning is a large source of light-absorbing refractory black carbon (rBC) particles with a wide range of morphologies and sizes. The net radiative forcing from these particles is strongly dependent on the amount and composition of non-light-absorbing material internally mixed with the rBC and on the morphology of the mixed particles. Understanding how the mixing state and morphology of biomass-burning aerosol evolves in the atmosphere is critical for constraining the influence of these particles on radiative forcing and climate. We investigated the response of two commercial laser-based particle mass spectrometers, the vacuum ultraviolet (VUV) ablation LAAPTOF and the IRmore » vaporization SP-AMS, to monodisperse biomass-burning particles as we sequentially coated the particles with secondary organic aerosol (SOA) from α-pinene ozonolysis. We studied three mobility-selected soot core sizes, each with a number of successively thicker coatings of SOA applied. Using IR laser vaporization, the SP-AMS had different changes in sensitivity to rBC compared to potassium as a function of applied SOA coatings. We show that this is due to different effective beam widths for the IR laser vaporization region of potassium versus black carbon. The SP-AMS's sensitivity to black carbon (BC) mass was not observed to plateau following successive SOA coatings, despite achieving high OA : BC mass ratios greater than 9. We also measured the ion fragmentation pattern of biomass-burning rBC and found it changed only slightly with increasing SOA mass. The average organic matter ion signal measured by the LAAPTOF demonstrated a positive correlation with the condensed SOA mass on individual particles, despite the inhomogeneity of the particle core compositions. This demonstrates that the LAAPTOF can obtain quantitative mass measurements of aged soot-particle composition from realistic biomass-burning particles with complex morphologies and composition.« less

A CLOSURE STUDY OF AEROSOL MASS CONCENTRATION MEASUREMENTS: COMPARISON OF VALUES OBTAINED WITH FILTERS AND BY DIRECT MEASUREMENTS OF MASS DISTRIBUTIONS. (R826372)

EPA Science Inventory

We compare measurements of aerosol mass concentrations obtained gravimetrically using Teflon coated glass fiber filters and by integrating mass distributions measured with the differential mobility analyzer–aerosol particle mass analyzer (DMA–APM) technique (Aero...

Thermophoretic separation of aerosol particles from a sampled gas stream

DOEpatents

Postma, A.K.

1984-09-07

This disclosure relates to separation of aerosol particles from gas samples withdrawn from within a contained atmosphere, such as containment vessels for nuclear reactors or other process equipment where remote gaseous sampling is required. It is specifically directed to separation of dense aerosols including particles of any size and at high mass loadings and high corrosivity. The United States Government has rights in this invention pursuant to Contract DE-AC06-76FF02170 between the US Department of Energy and Westinghouse Electric Corporation.

Mass spectrometric airborne measurements of submicron aerosol and cloud residual composition in tropic deep convection during ACRIDICON-CHUVA

NASA Astrophysics Data System (ADS)

Schulz, Christiane; Schneider, Johannes; Mertes, Stephan; Kästner, Udo; Weinzierl, Bernadett; Sauer, Daniel; Fütterer, Daniel; Walser, Adrian; Borrmann, Stephan

2015-04-01

Airborne measurements of submicron aerosol and cloud particles were conducted in the region of Manaus (Amazonas, Brazil) during the ACRIDICON-CHUVA campaign in September 2014. ACRIDICON-CHUVA aimed at the investigation of convective cloud systems in order to get a better understanding and quantification of aerosol-cloud-interactions and radiative effects of convective clouds. For that, data from airborne measurements within convective cloud systems are combined with satellite and ground-based data. We used a C-ToF-AMS (Compact-Time-of-Flight-Aerosol-Mass-Spectrometer) to obtain information on aerosol composition and vertical profiles of different aerosol species, like organics, sulphate, nitrate, ammonium and chloride. The instrument was operated behind two different inlets: The HASI (HALO Aerosol Submicrometer Inlet) samples aerosol particles, whereas the CVI (Counterflow Virtual Impactor) samples cloud droplets and ice particles during in-cloud measurements, such that cloud residual particles can be analyzed. Differences in aerosol composition inside and outside of clouds and cloud properties over forested or deforested region were investigated. Additionally, the in- and outflow of convective clouds was sampled on dedicated cloud missions in order to study the evolution of the clouds and the processing of aerosol particles. First results show high organic aerosol mass concentrations (typically 15 μg/m3 and during one flight up to 25 μg/m3). Although high amounts of organic aerosol in tropic air over rainforest regions were expected, such high mass concentrations were not anticipated. Next to that, high sulphate aerosol mass concentrations (about 4 μg/m3) were measured at low altitudes (up to 5 km). During some flights organic and nitrate aerosol was observed with higher mass concentrations at high altitudes (10-12 km) than at lower altitudes, indicating redistribution of boundary layer particles by convection. The cloud residuals measured during in

Elucidating determinants of aerosol composition through particle-type-based receptor modeling

NASA Astrophysics Data System (ADS)

McGuire, M. L.; Jeong, C.-H.; Slowik, J. G.; Chang, R. Y.-W.; Corbin, J. C.; Lu, G.; Mihele, C.; Rehbein, P. J. G.; Sills, D. M. L.; Abbatt, J. P. D.; Brook, J. R.; Evans, G. J.

2011-03-01

An aerosol time-of-flight mass spectrometer (ATOFMS) was deployed at a semi-rural site in Southern Ontario to characterize the size and chemical composition of individual particles. Particle-type-based receptor modelling of these data was used to investigate the determinants of aerosol chemical composition in this region. Individual particles were classified into particle-types and positive matrix factorization (PMF) was applied to their temporal trends to separate and cross-apportion particle-types to factors. The extent of chemical processing for each factor was assessed by evaluating the internal and external mixing state of the characteristic particle-types. The nine factors identified helped to elucidate the coupled interactions of these determinants. Nitrate-laden dust was found to be the dominant type of locally emitted particles measured by ATOFMS. Several factors associated with aerosol transported to the site from intermediate local-to-regional distances were identified: the Organic factor was associated with a combustion source to the north-west; the ECOC Day factor was characterized by nearby local-to-regional carbonaceous emissions transported from the south-west during the daytime; and the Fireworks factor consisted of pyrotechnic particles from the Detroit region following holiday fireworks displays. Regional aerosol from farther emissions sources were reflected through three factors: two biomass burning factors and a highly chemically processed long range transport factor. The biomass burning factors were separated by PMF due to differences in chemical processing which were caused in part by the passage of two thunderstorm gust fronts with different air mass histories. The remaining two factors, ECOC Night and Nitrate Background, represented the night-time partitioning of nitrate to pre-existing particles of different origins. The distinct meteorological conditions observed during this month-long study in the summer of 2007 provided a unique range

Elucidating determinants of aerosol composition through particle-type-based receptor modeling

NASA Astrophysics Data System (ADS)

McGuire, M. L.; Jeong, C.-H.; Slowik, J. G.; Chang, R. Y.-W.; Corbin, J. C.; Lu, G.; Mihele, C.; Rehbein, P. J. G.; Sills, D. M. L.; Abbatt, J. P. D.; Brook, J. R.; Evans, G. J.

2011-08-01

An aerosol time-of-flight mass spectrometer (ATOFMS) was deployed at a semi-rural site in southern Ontario to characterize the size and chemical composition of individual particles. Particle-type-based receptor modelling of these data was used to investigate the determinants of aerosol chemical composition in this region. Individual particles were classified into particle-types and positive matrix factorization (PMF) was applied to their temporal trends to separate and cross-apportion particle-types to factors. The extent of chemical processing for each factor was assessed by evaluating the internal and external mixing state of the characteristic particle-types. The nine factors identified helped to elucidate the coupled interactions of these determinants. Nitrate-laden dust was found to be the dominant type of locally emitted particles measured by ATOFMS. Several factors associated with aerosol transported to the site from intermediate local-to-regional distances were identified: the Organic factor was associated with a combustion source to the north-west; the ECOC Day factor was characterized by nearby local-to-regional carbonaceous emissions transported from the south-west during the daytime; and the Fireworks factor consisted of pyrotechnic particles from the Detroit region following holiday fireworks displays. Regional aerosol from farther emissions sources was reflected through three factors: two Biomass Burning factors and a highly chemically processed Long Range Transport factor. The Biomass Burning factors were separated by PMF due to differences in chemical processing which were in part elucidated by the passage of two thunderstorm gust fronts with different air mass histories. The remaining two factors, ECOC Night and Nitrate Background, represented the night-time partitioning of nitrate to pre-existing particles of different origins. The distinct meteorological conditions observed during this month-long study in the summer of 2007 provided a unique

Composition and formation of organic aerosol particles in the Amazon

NASA Astrophysics Data System (ADS)

Pöhlker, C.; Wiedemann, K.; Sinha, B.; Shiraiwa, M.; Gunthe, S. S.; Artaxo, P.; Gilles, M. K.; Kilcoyne, A. L. D.; Moffet, R. C.; Smith, M.; Weigand, M.; Martin, S. T.; Pöschl, U.; Andreae, M. O.

2012-04-01

We applied scanning transmission X-ray microscopy with near edge X-ray absorption fine structure (STXM-NEXAFS) analysis to investigate the morphology and chemical composition of aerosol samples from a pristine tropical environment, the Amazon Basin. The samples were collected in the Amazonian rainforest during the rainy season and can be regarded as a natural background aerosol. The samples were found to be dominated by secondary organic aerosol (SOA) particles in the fine and primary biological aerosol particles (PBAP) in the coarse mode. Lab-generated SOA-samples from isoprene and terpene oxidation as well as pure organic compounds from spray-drying of aqueous solution were measured as reference samples. The aim of this study was to investigate the microphysical and chemical properties of a tropical background aerosol in the submicron size range and its internal mixing state. The lab-generated SOA and pure organic compounds occurred as spherical and mostly homogenous droplet-like particles, whereas the Amazonian SOA particles comprised a mixture of homogeneous droplets and droplets having internal structures due to atmospheric aging. In spite of the similar morphological appearance, the Amazon samples showed considerable differences in elemental and functional group composition. According to their NEXAFS spectra, three chemically distinct types of organic material were found and could be assigned to the following three categories: (1) particles with a pronounced carboxylic acid (COOH) peak similar to those of laboratory-generated SOA particles from terpene oxidation; (2) particles with a strong hydroxy (COH) signal similar to pure carbohydrate particles; and (3) particles with spectra resembling a mixture of the first two classes. In addition to the dominant organic component, the NEXAFS spectra revealed clearly resolved potassium (K) signals for all analyzed particles. During the rainy season and in the absence of anthropogenic influence, active biota is

THE MASS ACCOMMODATION COEFFICIENT OF AMMONIUM NITRATE AEROSOL. (R823514)

EPA Science Inventory

The mass transfer rate of pure ammonium nitrate between the aerosol and gas phases was
quantified experimentally by the use of the tandem differential mobility analyzer/scanning mobility
particle sizer (TDMA/SMPS) technique. Ammonium nitrate particles 80-220 nm in diameter<...

Single particle characterization, source apportionment, and aging effects of ambient aerosols in Southern California

NASA Astrophysics Data System (ADS)

Shields, Laura Grace

Composed of a mixture of chemical species and phases and existing in a variety of shapes and sizes, atmospheric aerosols are complex and can have serious influence on human health, the environment, and climate. In order to better understand the impact of aerosols on local to global scales, detailed measurements on the physical and chemical properties of ambient particles are essential. In addition, knowing the origin or the source of the aerosols is important for policymakers to implement targeted regulations and effective control strategies to reduce air pollution in their region. One of the most ground breaking techniques in aerosol instrumentation is single particle mass spectrometry (SPMS), which can provide online chemical composition and size information on the individual particle level. The primary focus of this work is to further improve the ability of one specific SPMS technique, aerosol time-of-flight mass spectrometry (ATOFMS), for the use of identifying the specific origin of ambient aerosols, which is known as source apportionment. The ATOFMS source apportionment method utilizes a library of distinct source mass spectral signatures to match the chemical information of the single ambient particles. The unique signatures are obtained in controlled source characterization studies, such as with the exhaust emissions of heavy duty diesel vehicles (HDDV) operating on a dynamometer. The apportionment of ambient aerosols is complicated by the chemical and physical processes an individual particle can undergo as it spends time in the atmosphere, which is referred to as "aging" of the aerosol. Therefore, the performance of the source signature library technique was investigated on the ambient dataset of the highly aged environment of Riverside, California. Additionally, two specific subsets of the Riverside dataset (ultrafine particles and particles containing trace metals), which are known to cause adverse health effects, were probed in greater detail. Finally

Formation of secondary organic aerosol coating on black carbon particles near vehicular emissions

NASA Astrophysics Data System (ADS)

Lee, Alex K. Y.; Chen, Chia-Li; Liu, Jun; Price, Derek J.; Betha, Raghu; Russell, Lynn M.; Zhang, Xiaolu; Cappa, Christopher D.

2017-12-01

Black carbon (BC) emitted from incomplete combustion can result in significant impacts on air quality and climate. Understanding the mixing state of ambient BC and the chemical characteristics of its associated coatings is particularly important to evaluate BC fate and environmental impacts. In this study, we investigate the formation of organic coatings on BC particles in an urban environment (Fontana, California) under hot and dry conditions using a soot-particle aerosol mass spectrometer (SP-AMS). The SP-AMS was operated in a configuration that can exclusively detect refractory BC (rBC) particles and their coatings. Using the -log(NOx / NOy) ratio as a proxy for photochemical age of air masses, substantial formation of secondary organic aerosol (SOA) coatings on rBC particles was observed due to active photochemistry in the afternoon, whereas primary organic aerosol (POA) components were strongly associated with rBC from fresh vehicular emissions in the morning rush hours. There is also evidence that cooking-related organic aerosols were externally mixed from rBC. Positive matrix factorization and elemental analysis illustrate that most of the observed SOA coatings were freshly formed, providing an opportunity to examine SOA coating formation on rBCs near vehicular emissions. Approximately 7-20 wt % of secondary organic and inorganic species were estimated to be internally mixed with rBC on average, implying that rBC is unlikely the major condensation sink of SOA in this study. Comparison of our results to a co-located standard high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) measurement suggests that at least a portion of SOA materials condensed on rBC surfaces were chemically different from oxygenated organic aerosol (OOA) particles that were externally mixed with rBC, although they could both be generated from local photochemistry.

Characterization of urban aerosol using aerosol mass spectrometry and proton nuclear magnetic resonance spectroscopy

NASA Astrophysics Data System (ADS)

Cleveland, M. J.; Ziemba, L. D.; Griffin, R. J.; Dibb, J. E.; Anderson, C. H.; Lefer, B.; Rappenglück, B.

2012-07-01

Particulate matter was measured during August and September of 2006 in Houston as part of the Texas Air Quality Study II Radical and Aerosol Measurement Project. Aerosol size and composition were determined using an Aerodyne quadrupole aerosol mass spectrometer. Aerosol was dominated by sulfate (4.1 ± 2.6 μg m-3) and organic material (5.5 ± 4.0 μg m-3), with contributions of organic material from both primary (˜32%) and secondary (˜68%) sources. Secondary organic aerosol appears to be formed locally. In addition, 29 aerosol filter samples were analyzed using proton nuclear magnetic resonance (1H NMR) spectroscopy to determine relative concentrations of organic functional groups. Houston aerosols are less oxidized than those observed elsewhere, with smaller relative contributions of carbon-oxygen double bonds. These particles do not fit 1H NMR source apportionment fingerprints for identification of secondary, marine, and biomass burning organic aerosol, suggesting that a new fingerprint for highly urbanized and industrially influenced locations be established.

Constraining Aerosol Optical Models Using Ground-Based, Collocated Particle Size and Mass Measurements in Variable Air Mass Regimes During the 7-SEAS/Dongsha Experiment

NASA Technical Reports Server (NTRS)

Bell, Shaun W.; Hansell, Richard A.; Chow, Judith C.; Tsay, Si-Chee; Wang, Sheng-Hsiang; Ji, Qiang; Li, Can; Watson, John G.; Khlystov, Andrey

2012-01-01

During the spring of 2010, NASA Goddard's COMMIT ground-based mobile laboratory was stationed on Dongsha Island off the southwest coast of Taiwan, in preparation for the upcoming 2012 7-SEAS field campaign. The measurement period offered a unique opportunity for conducting detailed investigations of the optical properties of aerosols associated with different air mass regimes including background maritime and those contaminated by anthropogenic air pollution and mineral dust. What appears to be the first time for this region, a shortwave optical closure experiment for both scattering and absorption was attempted over a 12-day period during which aerosols exhibited the most change. Constraints to the optical model included combined SMPS and APS number concentration data for a continuum of fine and coarse-mode particle sizes up to PM2.5. We also take advantage of an IMPROVE chemical sampler to help constrain aerosol composition and mass partitioning of key elemental species including sea-salt, particulate organic matter, soil, non sea-salt sulphate, nitrate, and elemental carbon. Our results demonstrate that the observed aerosol scattering and absorption for these diverse air masses are reasonably captured by the model, where peak aerosol events and transitions between key aerosols types are evident. Signatures of heavy polluted aerosol composed mostly of ammonium and non sea-salt sulphate mixed with some dust with transitions to background sea-salt conditions are apparent in the absorption data, which is particularly reassuring owing to the large variability in the imaginary component of the refractive indices. Extinctive features at significantly smaller time scales than the one-day sample period of IMPROVE are more difficult to reproduce, as this requires further knowledge concerning the source apportionment of major chemical components in the model. Consistency between the measured and modeled optical parameters serves as an important link for advancing remote

Aerosol Particle Shape and Radiative Coupling in a Three Dimensional Titan GCM

NASA Astrophysics Data System (ADS)

Larson, Erik J.; Toon, O. B.; Friedson, A. J.; West, R. A.

2010-10-01

Understanding the aerosols on Titan is imperative for understanding the atmosphere as a whole. The aerosols affect the albedo, optical depth, as well as heating and cooling rates which in turn affect the circulation on Titan leading to feedback with the aerosol distribution. Correctly representing the aerosols in atmospheric models is crucial to understanding this atmosphere. Friedson et al. (2009, A global climate model of Titan's atmosphere and surface. Planet. SpaceSci. 57, 1931-1949.) produced a three-dimensional model for Titan using the NCAR CAM3 model, to which we coupled the aerosol microphysics model CARMA. We have also made the aerosols produced by CARMA interactive with the radiation code in CAM. We compare simulations with radiatively interactive aerosols with those using a prescribed aerosol radiative effect. Preliminary results show that this model is capable of reproducing the seasonal changes in aerosols on Titan and many of the associated phenomena. For instance, the radiatively interactive aerosols are lofted by winds more in the summer hemisphere than the non-radiatively interactive aerosols, which is necessary to reproduce the observed seasonal cycle of the albedo. We compare simulations using spherical particles to simulations using fractal aggregate particles, which are expected from laboratory and observational data. Fractal particles have higher absorption in the UV, slower fall velocities and faster coagulation rates than equivalent mass spherical particles. We compare model simulations with observational data from the Cassini and Huygens missions.

The physico-chemical evolution of atmospheric aerosols and the gas-particle partitioning of inorganic aerosol during KORUS-AQ

NASA Astrophysics Data System (ADS)

Lee, T.; Park, T.; Lee, J. B.; Lim, Y. J.; Ahn, J.; Park, J. S.; Soo, C. J.; Desyaterik, Y.; Collett, J. L., Jr.

2017-12-01

Aerosols influence climate change directly by scattering and absorption and indirectly by acting as cloud condensation nuclei and some of the effects of aerosols are reduction in visibility, deterioration of human health, and deposition of pollutants to ecosystems. Urban area is large source of aerosols and aerosol precursors. Aerosol sources are both local and from long-range transport. Long-range transport processed aerosol are often dominant sources of aerosol pollution in Korea. To improve our knowledge of aerosol chemistry, Korea and U.S-Air Quality (KORUS-AQ) of Aircraft-based aerosol measurement took place in and around Seoul, Korea during May and June 2016. KORUS-AQ campaigns were conducted to study the chemical characterization and processes of pollutants in the Seoul Metropolitan area to regional scales of Korean peninsula. Aerodyne High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed on aircraft platforms on-board DC-8 (NASA) aircraft. We characterized aerosol chemical properties and mass concentrations of sulfate, nitrate, ammonium and organics in polluted air plumes and investigate the spatial and vertical distribution of the species. The results of studies show that organics is predominant in Aerosol and a significant fraction of the organics is oxygenated organic aerosol (OOA) at the high altitude. Both Nitrate and sulfate can partition between the gas and particle phases. The ratios for HNO3/(N(V) (=gaseous HNO3 + particulate Nitrate) and SO2/(SO2+Sulfate) were found to exhibit quite different distributions between the particles and gas phase for the locations during KORUS-AQ campaign, representing potential for formation of additional particulate nitrate and sulfate. The results of those studies can provide highly resolved temporal and spatial air pollutant, which are valuable for air quality model input parameters for aerosol behaviour.

A novel inversion method to calculate the mass fraction of coated refractory black carbon using a centrifugal particle mass analyzer and single particle soot photometer

NASA Astrophysics Data System (ADS)

Irwin, M.; Broda, K.; Olfert, J. S.; Schill, G. P.; McMeeking, G. R.; Schnitzler, E.; Jäger, W.

2016-12-01

Refractory black carbon (rBC) has important atmospheric impacts due to its ability to absorb light, and its interactions with light are partly governed by the acquisition of coatings or other mixing processes. Here, a novel inversion method is presented which derives the mass fraction of coated rBC using a coupled centrifugal particle mass analyzer (CPMA) and single particle soot photometer (SP2). The CPMA selects particles of a known mass-­to-­charge ratio, and the SP2 detects the mass of rBC in each individual particle. The results of the inversion are the simultaneous number distributions of both rBC mass and total particle mass. Practically, the distribution can be integrated to find properties of the total aerosol population, for example, i) mass fraction of coating and ii) mass of coating on a particle of known total mass. This was demonstrated via smog chamber experiments. Initially, particles in the chamber were pure rBC, produced from a methane burner and passed through a diffusion dryer and thermal denuder. An organic (non-rBC) coating was then grown onto the aerosol over several hours via photooxidation with p-xylene. The CPMA-SP2 coupled system sampled the aerosol over the reaction period as the coating grew. The CPMA was sequentially stepped over a mass range from 0.3 to 28 fg and the SP2 measured the mass of rBC in each individual CPMA-classified particle. The number and mass distributions were constructed using the inversion. As expected, the mass and number distributions of rBC and total mass were equivalent for uncoated particles. As the non-rBC coating thickness increased over time, a shift in the number distribution towards higher total mass was observed. At the end of the experiment, fresh rBC (i.e. uncoated, bare particles) was injected into the chamber, creating an external mixture of coated and uncoated particles. This external mixture was clearly resolved in the number distribution of rBC and total particle mass. It is expected that the

Analysis of individual biological particles by mass spectrometry

NASA Technical Reports Server (NTRS)

Sinha, M. P.; Platz, R. M.; Vilker, V. L.; Friedlander, S. K.

1984-01-01

A method is developed for the detection and identification of biological particles introduced in aerosol form into a quadrupole mass spectrometer. The bacterial aerosol is generated by nebulizing an ethanol suspension. The particles are introduced into the ion source of the mass spectrometer in the form of a beam, where they are individually volatilized on a V-type rhenium filament and ionized by electron impaction. It is shown that the average intensity of a mass peak is obtained from the pulse height distribution of about a thousand ion pulses from different particles. Pseudomonas putida, Bacillus subtilis, and Bacillus cereus are used in the studies. Differences between the relative intensities of mass peaks in the spectra from P. putida and B. subtilis are found and may provide a method for differentiation of microorganisms. The results for the two species agree reasonably well with those reported by Kistemaker et al. (1975) and Schulten et al. (1973). However, there exist some differences between the two spectra in the high mass range due to the difference in the pyrolysis conditions.

The Impact of Aerosol Particle Mixing State on the Hygroscopicity of Sea Spray Aerosol.

PubMed

Schill, Steven R; Collins, Douglas B; Lee, Christopher; Morris, Holly S; Novak, Gordon A; Prather, Kimberly A; Quinn, Patricia K; Sultana, Camille M; Tivanski, Alexei V; Zimmermann, Kathryn; Cappa, Christopher D; Bertram, Timothy H

2015-06-24

Aerosol particles influence global climate by determining cloud droplet number concentrations, brightness, and lifetime. Primary aerosol particles, such as those produced from breaking waves in the ocean, display large particle-particle variability in chemical composition, morphology, and physical phase state, all of which affect the ability of individual particles to accommodate water and grow into cloud droplets. Despite such diversity in molecular composition, there is a paucity of methods available to assess how particle-particle variability in chemistry translates to corresponding differences in aerosol hygroscopicity. Here, an approach has been developed that allows for characterization of the distribution of aerosol hygroscopicity within a chemically complex population of atmospheric particles. This methodology, when applied to the interpretation of nascent sea spray aerosol, provides a quantitative framework for connecting results obtained using molecular mimics generated in the laboratory with chemically complex ambient aerosol. We show that nascent sea spray aerosol, generated in situ in the Atlantic Ocean, displays a broad distribution of particle hygroscopicities, indicative of a correspondingly broad distribution of particle chemical compositions. Molecular mimics of sea spray aerosol organic material were used in the laboratory to assess the volume fractions and molecular functionality required to suppress sea spray aerosol hygroscopicity to the extent indicated by field observations. We show that proper accounting for the distribution and diversity in particle hygroscopicity and composition are important to the assessment of particle impacts on clouds and global climate.

In Situ Single Particle Measurement of Atmospheric Aging of Carbonaceous Aerosols During CARES

NASA Astrophysics Data System (ADS)

Cahill, J. F.; Suski, K.; Hubbe, J.; Shilling, J.; Zaveri, R. A.; Springston, S. R.; Prather, K. A.

2011-12-01

Atmospheric aging of aerosols through photochemistry, heterogeneous reactions and aqueous processing can change their physical and chemical properties, impacting their gas uptake, radiative forcing, and activation of cloud nuclei. Understanding the timescale and magnitude of this aging process is essential for accurate aerosol-climate modeling and predictions. An aircraft aerosol time-of-flight mass spectrometer (A-ATOFMS) measured single particle mixing state during the Carbonaceous Aerosols and Radiative Effects Study (CARES) in the summer of 2010 over Sacramento, CA. On 6/23/10, flights in the morning and afternoon performed pseudo-Lagrangian sampling of the Sacramento urban plume. Carbonaceous particles from these flights were classified into 'aged' and 'fresh' classes based on their mixing state, with aged particles having more secondary species, such as nitrate and sulfate. In the morning flight, a clear decreasing trend in the ratio of fresh/aged particle types was seen as the flight progressed, whereas in the afternoon flight, the ratio was essentially constant. These data show that in the morning carbonaceous aerosols can become heavily oxidized in a few hours. Further analysis of particle mixing state and the timescale of carbonaceous aerosol aging will be presented

Properties of Arctic Aerosol Particles and Residuals of Warm Clouds: Cloud Activation Efficiency and the Aerosol Indirect Effect

NASA Astrophysics Data System (ADS)

Zelenyuk, A.; Imre, D. G.; Leaitch, R.; Ovchinnikov, M.; Liu, P.; Macdonald, A.; Strapp, W.; Ghan, S. J.; Earle, M. E.

2012-12-01

Single particle mass spectrometer, SPLAT II, was used to characterize the size, composition, number concentration, density, and shape of individual Arctic spring aerosol. Background particles, particles above and below the cloud, cloud droplet residuals, and interstitial particles were characterized with goal to identify the properties that separate cloud condensation nuclei (CCN) from background aerosol particles. The analysis offers a comparison between warm clouds formed on clean and polluted days, with clean days having maximum particle concentrations (Na) lower than ~250 cm-3, as compared with polluted days, in which maximum concentration was tenfold higher. On clean days, particles were composed of organics, organics mixed with sulfates, biomass burning (BB), sea salt (SS), and few soot and dust particles. On polluted days, BB, organics associated with BB, and their mixtures with sulfate dominated particle compositions. Based on the measured compositions and size distributions of cloud droplet residuals, background aerosols, and interstitial particles, we conclude that these three particle types had virtually the same compositions, which means that cloud activation probabilities were surprisingly nearly composition independent. Moreover, these conclusions hold in cases in which less than 20% or more than 90% of background particles got activated. We concluded that for the warm clouds interrogated in this study particle size played a more important factor on aerosol CCN activity. Comparative analysis of all studied clouds reveals that aerosol activation efficiency strongly depends on the aerosol concentrations, such that at Na <200 cm-3, nearly all particles activate, and at higher concentrations the activation efficiency is lower. For example, when Na was greater than 1500 cm-3, less than ~30% of particles activated. The data suggest that as the number of nucleated droplets increases, condensation on existing droplets effectively competes with particle

Chemical characteristics of submicron particles at the central Tibetan Plateau: insights from aerosol mass spectrometry

NASA Astrophysics Data System (ADS)

Xu, Jianzhong; Zhang, Qi; Shi, Jinsen; Ge, Xinlei; Xie, Conghui; Wang, Junfeng; Kang, Shichang; Zhang, Ruixiong; Wang, Yuhang

2018-01-01

Recent studies have revealed a significant influx of anthropogenic aerosol from South Asia to the Himalayas and Tibetan Plateau (TP) during pre-monsoon period. In order to characterize the chemical composition, sources, and transport processes of aerosol in this area, we carried out a field study during June 2015 by deploying a suite of online instruments including an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) and a multi-angle absorption photometer (MAAP) at Nam Co station (90°57' E, 30°46' N; 4730 m a.s.l.) at the central of the TP. The measurements were made at a period when the transition from pre-monsoon to monsoon occurred. The average ambient mass concentration of submicron particulate matter (PM1) over the whole campaign was ˜ 2.0 µg m-3, with organics accounting for 68 %, followed by sulfate (15 %), black carbon (8 %), ammonium (7 %), and nitrate (2 %). Relatively higher aerosol mass concentration episodes were observed during the pre-monsoon period, whereas persistently low aerosol concentrations were observed during the monsoon period. However, the chemical composition of aerosol during the higher aerosol concentration episodes in the pre-monsoon season was on a case-by-case basis, depending on the prevailing meteorological conditions and air mass transport routes. Most of the chemical species exhibited significant diurnal variations with higher values occurring during afternoon and lower values during early morning, whereas nitrate peaked during early morning in association with higher relative humidity and lower air temperature. Organic aerosol (OA), with an oxygen-to-carbon ratio (O / C) of 0.94, was more oxidized during the pre-monsoon period than during monsoon (average O / C ratio of 0.72), and an average O / C was 0.88 over the entire campaign period, suggesting overall highly oxygenated aerosol in the central TP. Positive matrix factorization of the high-resolution mass spectra of OA identified two oxygenated

[Seasonal Variation Characteristics and Potential Source Contribution of Sulfate, Nitrate and Ammonium in Beijing by Using Single Particle Aerosol Mass Spectrometry].

PubMed

Liu, Lang; Zhang, Wen-jie; Du, Shi-yong; Hou, Lu-jian; Han, Bin; Yang, Wen; Chen, Min-dong; Bai, Zhi-peng

2016-05-15

Single particle aerosol mass spectrometry (SPAMS) was deployed to continuously observe the aerosol particles of Beijing urban area from 2013-12 to 2014-11, and the hourly average data of sulfate, nitrate and ammonium (SNA) were obtained using the characteristic ion tracer method. The mixing state and size distribution of SNA were analyzed. In addition, based on Hysplit 48 h back air mass trajectory results in combination with Concentration Weighted Trajectory method (CWT), we obtained the seasonal potential source contribution area of SNA. The results showed that the mixture of sulfate, nitrate and ammonium in spring and summer was more stable than that in autumn and winter. The size distribution of sulfate and nitrate was very similar. The size distribution characteristics of SNA followed the order of autumn > summer > spring > winter. The potential source region of SNA had similar spatial distribution characteristics, and the potential source region of SNA was mainly located in Beijing and south areas, especially at Tianjin, Langfang, Hengshui, Baoding and Shijiazhuang.

Observation of Asian Mineral Dust Particles in Japan by a Single-Particle Mass Spectrometer

NASA Astrophysics Data System (ADS)

Matsumoto, J.; Takahashi, K.; Matsumi, Y.; Sugimoto, N.; Matsui, I.; Shimizu, A.

2005-12-01

The Asian mineral dust (Kosa) particles, emitted from the desert area of inland China, are characteristic of East Asian aerosols. The Kosa particles are important as regional carriers of various materials, especially in spring when the stormy dusts are transported to Japan and Pacific Ocean. In this study, the chemical mixing state of each atmospheric aerosol was measured individually by a laser-based time-of-flight mass spectrometer (TOFMS) to discuss chemical changes of Kosa particles during the transport. Observation was conducted at Tsukuba (36.05°N, 140.12°E) in April and May 2004. The LIDAR measurement was also carried out to determine the Kosa events. To classify the source of the air mass, the NOAA-HYSPLIT backward trajectory was applied. For the TOFMS instrument, particles with μm and sub-μm diameters were detected. The polarity of ion detection was altered every minute. During 30 days, the numbers of logged mass spectra (MS) were 5993 and 4382 for positive and negative ions, respectively. When the MS of ambient aerosols were compared with that of the standard Kosa sample, sulfate- and nitrate-mixed Kosa particles were found. To explore the mixing state of particles further, classification of the particles by the ART-2a algorithm was adopted. NO2-, NO3-, HSO4-, SiO2-, SiO3-, Cl- and NaCl2- were focused. Finally, particles were classified to 4 categories as A: sulfate and sulfate-rich mineral; B: sulfate-poor mineral; C: sea salt; D: unidentified. The relative fractions of A were 30 % and 1 % for a Kosa event and a maritime air mass, respectively. Note that the air mass for Kosa event case passed over the coast region of China, where SOx emission was intensive. It was reasonable that sulfate was internally mixed with Kosa particles and transported to Japan. Consequently, it was confirmed experimentally that Kosa particles are important as carriers of pollutants in the rim region of Pacific Ocean. Comparison with the observation in 2005 is also shown.

Contribution of bacteria-like particles to PM2.5 aerosol in urban and rural environments

NASA Astrophysics Data System (ADS)

Wolf, R.; El-Haddad, I.; Slowik, J. G.; Dällenbach, K.; Bruns, E.; Vasilescu, J.; Baltensperger, U.; Prévôt, A. S. H.

2017-07-01

We report highly time-resolved estimates of airborne bacteria-like particle concentrations in ambient aerosol using an Aerodyne aerosol mass spectrometer (AMS). AMS measurements with a newly developed PM2.5 and the standard (PM1) aerodynamic lens were performed at an urban background site (Zurich) and at a rural site (Payerne) in Switzerland. Positive matrix factorization using the multilinear engine (ME-2) implementation was used to estimate the contribution of bacteria-like particles to non-refractory organic aerosol. The success of the method was evaluated by a size-resolved analysis of the organic mass and the analysis of single particle mass spectra, which were detected with a light scattering system integrated into the AMS. Use of the PM2.5 aerodynamic lens increased measured bacteria-like concentrations, supporting the analysis method. However, at all sites, the low concentrations of this component suggest that airborne bacteria constitute a minor fraction of non-refractory PM2.5 organic aerosol mass. Estimated average mass concentrations were below 0.1 μg/m3 and relative contributions were lower than 2% at both sites. During rainfall periods, concentrations of the bacteria-like component increased considerably reaching a short-time maximum of approximately 2 μg/m3 at the Payerne site in summer.

High-Resolution Electrospray Ionization Mass Spectrometry Analysis of Water- Soluble Organic Aerosols Collected with a Particle into Liquid Sampler

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bateman, Adam P.; Nizkorodov, Serguei; Laskin, Julia

2010-10-01

This work demonstrates the utility of a particle-into-liquid sampler (PILS) a technique traditionally used for identification of inorganic ions present in ambient or laboratory aerosols for the analysis of water soluble organic aerosol (OA) using high resolution electrospray ionization mass spectrometry (HR ESI-MS). Secondary organic aerosol (SOA) was produced from 0.5 ppm mixing ratios of limonene and ozone in a 5 m3 Teflon chamber. SOA was collected simultaneously using a traditional filter sampler and a PILS. The filter samples were later extracted with either water or acetonitrile, while the aqueous PILS samples were analyzed directly. In terms of peak intensities,more » types of detectable compounds, average O:C ratios, and organic mass to organic carbon ratios, the resulting high resolution mass spectra were essentially identical for the PILS and filter based samples. SOA compounds extracted from both filter/acetonitrile extraction and PILS/water extraction accounted for >95% of the total ion current in ESI mass spectra. This similarity was attributed to high solubility of limonene SOA in water. In contrast, significant differences in detected ions and peak abundances were observed for pine needle biomass burning organic aerosol (BBOA) collected with PILS and filter sampling. The water soluble fraction of BBOA is considerably smaller than for SOA, and a number of unique peaks were detectable only by the filter/acetonitrile method. The combination of PILS collection with HR-ESI-MS analysis offers a new approach for molecular analysis of the water-soluble organic fraction in biogenic SOA, aged photochemical smog, and BBOA.« less

Source characterization of urban particles from meat smoking activities in Chongqing, China using single particle aerosol mass spectrometry.

PubMed

Chen, Yang; Wenger, John C; Yang, Fumo; Cao, Junji; Huang, Rujin; Shi, Guangming; Zhang, Shumin; Tian, Mi; Wang, Huanbo

2017-09-01

A Single Particle Aerosol Mass Spectrometer (SPAMS) was deployed in the urban area of Chongqing to characterize the particles present during a severe particulate pollution event that occurred in winter 2014-2015. The measurements were made at a time when residents engaged in traditional outdoor meat smoking activities to preserve meat before the Chinese Spring Festival. The measurement period was predominantly characterized by stagnant weather conditions, highly elevated levels of PM 2.5 , and low visibility. Eleven major single particle types were identified, with over 92.5% of the particles attributed to biomass burning emissions. Most of the particle types showed appreciable signs of aging in the stagnant air conditions. To simulate the meat smoking activities, a series of controlled smoldering experiments was conducted using freshly cut pine and cypress branches, both with and without wood logs. SPAMS data obtained from these experiments revealed a number of biomass burning particle types, including an elemental and organic carbon (ECOC) type that proved to be the most suitable marker for meat smoking activities. The traditional activity of making preserved meat in southwestern China is shown here to be a major source of particulate pollution. Improved measures to reduce emissions from the smoking of meat should be introduced to improve air quality in regions where smoking meat activity prevails. Copyright © 2017 Elsevier Ltd. All rights reserved.

Sub 2 nm Particle Characterization in Systems with Aerosol Formation and Growth

NASA Astrophysics Data System (ADS)

Wang, Yang

size distributions were discrete, suggesting the formation of stable clusters that may be intermediate phases between initial chemical reactions and downstream particle growth. The evolution of incipient cluster size distributions further provided information on the gaseous precursor reaction kinetics, which matched well with the data obtained through other techniques. Part 2. The size distributions and their evolution measured by the DMAs help explain the physical pathways of aerosol formation. The chemical analysis of the incipient particles is an important counterpart to the existing characterization method. The chemical compositions of charged species were measured online with an atmospheric pressure interface time-of-flight mass spectrometer (APi-TOF). The tandem arrangement of the high-resolution DMA and the APi-TOF realized the simultaneous measurement of the mobility and the mass of combustion-generated natively charged particles, which enabled their chemical and physical formation pathways to be derived. The results showed that the initial stages of particle formation were strongly influenced by chemically ionized species during combustion, and that incipient particles composed of pure oxides did not exist. The effective densities of the incipient particles were much lower than those of bulk materials, due to their amorphous structures and different chemical compositions. Measuring incipient particles with high-resolution DMAs is limited because a DMA classifies charged particles only, while the charging characteristics of sub 2 nm particles are not well understood. The charge fraction of combustion-generated incipient particles was measured by coupling a charged particle remover and a condensation particle counter. A high charge fraction was observed, confirming the strong interaction among chemically ionized species and formed particles. The combustion system was modeled by using a unimodal aerosol dynamics model combined with Fuchs' charging theory, and

Evaluation of species-dependent detection efficiencies in the aerosol mass spectrometer

USDA-ARS?s Scientific Manuscript database

Mass concentrations of chemical species calculated from the aerosol mass spectrometer (AMS) depend on two factors: particle collection efficiency (CE) and relative ionization efficiency (RIE, relative to the primary calibrant ammonium nitrate). While previous studies have characterized CE, RIE is re...

Unique DNA-barcoded aerosol test particles for studying aerosol transport

DOE Office of Scientific and Technical Information (OSTI.GOV)

Harding, Ruth N.; Hara, Christine A.; Hall, Sara B.

Data are presented for the first use of novel DNA-barcoded aerosol test particles that have been developed to track the fate of airborne contaminants in populated environments. Until DNATrax (DNA Tagged Reagents for Aerosol eXperiments) particles were developed, there was no way to rapidly validate air transport models with realistic particles in the respirable range of 1–10 μm in diameter. The DNATrax particles, developed at Lawrence Livermore National Laboratory (LLNL) and tested with the assistance of the Pentagon Force Protection Agency, are the first safe and effective materials for aerosol transport studies that are identified by DNA molecules. The usemore » of unique synthetic DNA barcodes overcomes the challenges of discerning the test material from pre-existing environmental or background contaminants (either naturally occurring or previously released). The DNATrax particle properties are demonstrated to have appropriate size range (approximately 1–4.5 μm in diameter) to accurately simulate bacterial spore transport. As a result, we describe details of the first field test of the DNATrax aerosol test particles in a large indoor facility.« less

Unique DNA-barcoded aerosol test particles for studying aerosol transport

DOE PAGES

Harding, Ruth N.; Hara, Christine A.; Hall, Sara B.; ...

2016-03-22

Data are presented for the first use of novel DNA-barcoded aerosol test particles that have been developed to track the fate of airborne contaminants in populated environments. Until DNATrax (DNA Tagged Reagents for Aerosol eXperiments) particles were developed, there was no way to rapidly validate air transport models with realistic particles in the respirable range of 1–10 μm in diameter. The DNATrax particles, developed at Lawrence Livermore National Laboratory (LLNL) and tested with the assistance of the Pentagon Force Protection Agency, are the first safe and effective materials for aerosol transport studies that are identified by DNA molecules. The usemore » of unique synthetic DNA barcodes overcomes the challenges of discerning the test material from pre-existing environmental or background contaminants (either naturally occurring or previously released). The DNATrax particle properties are demonstrated to have appropriate size range (approximately 1–4.5 μm in diameter) to accurately simulate bacterial spore transport. As a result, we describe details of the first field test of the DNATrax aerosol test particles in a large indoor facility.« less

A COMPARISON OF PARTICLE MASS SPECTROMETERS DURING THE 1999 ATLANTA SUPERSITES EXPERIMENT

EPA Science Inventory

During the Atlanta SuperSite Experiment, four particle mass spectrometers were operated together for the first time: NOAA's PALMS (Particle Analysis by Laser Mass Spectrometry), U. C. Riverside's ATOFMS (Aerosol Time-of-Flight Mass Spectrometry), U. Delaware's RSMS-II (Rapid Si...

Aerosolization, Chemical Characterization, Hygroscopicity and Ice Formation of Marine Biogenic Particles

NASA Astrophysics Data System (ADS)

Alpert, P. A.; Radway, J.; Kilthau, W.; Bothe, D.; Knopf, D. A.; Aller, J. Y.

2013-12-01

The oceans cover the majority of the earth's surface, host nearly half the total global primary productivity and are a major source of atmospheric aerosol particles. However, effects of biological activity on sea spray generation and composition, and subsequent cloud formation are not well understood. Our goal is to elucidate these effects which will be particularly important over nutrient rich seas, where microorganisms can reach concentrations of 10^9 per mL and along with transparent exopolymer particles (TEP) can become aerosolized. Here we report the results of mesocosm experiments in which bubbles were generated by two methods, either recirculating impinging water jets or glass frits, in natural or artificial seawater containing bacteria and unialgal cultures of three representative phytoplankton species, Thalassiosira pseudonana, Emiliania huxleyi, and Nannochloris atomus. Over time we followed the size distribution of aerosolized particles as well as their hygroscopicity, heterogeneous ice nucleation potential, and individual physical-chemical characteristics. Numbers of cells and the mass of dissolved and particulate organic carbon (DOC, POC), TEP (which includes polysaccharide-containing microgels and nanogels >0.4 μm in diameter) were determined in the bulk water, the surface microlayer, and aerosolized material. Aerosolized particles were also impacted onto substrates for ice nucleation and water uptake experiments, elemental analysis using computer controlled scanning electron microscopy and energy dispersive analysis of X-rays (CCSEM/EDX), and determination of carbon bonding with scanning transmission X-ray microscopy and near-edge X-ray absorption fine structure spectroscopy (STXM/NEXAFS). Regardless of bubble generation method, the overall concentration of aerosol particles, TEP, POC and DOC increased as concentrations of bacterial and phytoplankton cells increased, stabilized, and subsequently declined. Particles <100 nm generated by means of jets

A study on the relationship between mass concentrations, chemistry and number size distribution of urban fine aerosols in Milan, Barcelona and London

NASA Astrophysics Data System (ADS)

Rodríguez, S.; van Dingenen, R.; Putaud, J.-P.; Dell'Acqua, A.; Pey, J.; Querol, X.; Alastuey, A.; Chenery, S.; Ho, K.-F.; Harrison, R.; Tardivo, R.; Scarnato, B.; Gemelli, V.

2007-05-01

A physicochemical characterization, including aerosol number size distribution, chemical composition and mass concentrations, of the urban fine aerosol captured in MILAN, BARCELONA and LONDON is presented in this article. The objective is to obtain a comprehensive picture of the microphysical processes involved in aerosol dynamics during the: 1) regular evolution of the urban aerosol (daily, weekly and seasonal basis) and in the day-to-day variations (from clean-air to pollution-events), and 2) the link between "aerosol chemistry and mass concentrations" with the "number size distribution". The mass concentrations of the fine PM2.5 aerosol exhibit a high correlation with the number concentration of >100 nm particles N>100 (nm) ("accumulation mode particles") which only account for <20% of the total number concentration N of fine aerosols; but do not correlate with the number of <100 nm particles ("ultrafine particles"), which accounts for >80% of fine particles number concentration. Organic matter and black-carbon are the only aerosol components showing a significant correlation with the ultrafine particles, attributed to vehicles exhausts emissions; whereas ammonium-nitrate, ammonium-sulphate and also organic matter and black-carbon correlate with N>100 (nm) and attributed to condensation mechanisms, other particle growth processes and some primary emissions. Time series of the aerosol DpN diameter (dN/dlogD mode), mass PM2.5 concentrations and number N>100 (nm) concentrations exhibit correlated day-to-day variations, which point to a significant involvement of condensation of semi-volatile compounds during urban pollution events. This agrees with the observation that ammonium-nitrate is the component exhibiting the highest increases from mid-to-high pollution episodes, when the highest DpN increases are observed. The results indicates that "fine PM2.5 particles urban pollution events" tend to occur when condensation processes have made particles grow large enough

Single-particle characterization of atmospheric aerosols collected at Gosan, Korea, during the Asian Pacific Regional Aerosol Characterization Experiment field campaign using low-Z (atomic number) particle electron probe X-ray microanalysis.

PubMed

Geng, Hong; Cheng, Fangqin; Ro, Chul-Un

2011-11-01

A quantitative energy-dispersive electron probe X-ray microanalysis (ED-EPMA), namely low-Z (atomic number) particle EPMA, was used to characterize the chemical compositions of the individual aerosol particles collected at the Gosan supersite, Jeju Island, Korea, as a part of the Asian Pacific Regional Aerosol Characterization Experiment (ACE-Asia). On 4-10 April 2001 just before a severe dust storm arrived, seven sets of aerosol samples were obtained by a seven-stage May cascade impactor with a flow rate of 20 L/min. Overall 11,200 particles on stages 1-6 with cutoff diameters of 16, 8, 4, 2, 1, and 0.5 microm, respectively, were examined and classified based on their secondary electron images and X-ray spectra. In general, sea salt particles were the most frequently encountered, followed by mineral dust, organic carbon (OC)-like, (NH4)2SO4/NH4HSO4-containing, elemental carbon (EC)-like, Fe-rich, and K-rich particles. Sea salt and mineral dust particles had a higher relative abundance on stages 1-5, whereas OC-like, (NH4)2SO4/NH4HSO4-containing, Fe-rich, and K-rich particles were relatively abundant on stage 6. The analysis on relative number abundances of various particle types combined with 72-hr backward air mass trajectories indicated that a lot of reacted sea salt and reacted mineral dust (with airborne NOx and SO2 or their acidic products) and OC-like particles were carried by the air masses passing over the Yellow Sea (for sample "10 April") and many NH4HSO4/ (NH4)2SO4-containing particles were carried by the air masses passing over the Sea of Japan and Korea Strait (for samples "4-9 April"). It was concluded that the atmosphere over Jeju Island was influenced by anthropogenic SO2 and NOx, organic compounds, and secondary aerosols when Asian dust was absent.

Effective density and mixing state of aerosol particles in a near-traffic urban environment.

PubMed

Rissler, Jenny; Nordin, Erik Z; Eriksson, Axel C; Nilsson, Patrik T; Frosch, Mia; Sporre, Moa K; Wierzbicka, Aneta; Svenningsson, Birgitta; Löndahl, Jakob; Messing, Maria E; Sjogren, Staffan; Hemmingsen, Jette G; Loft, Steffen; Pagels, Joakim H; Swietlicki, Erik

2014-06-03

In urban environments, airborne particles are continuously emitted, followed by atmospheric aging. Also, particles emitted elsewhere, transported by winds, contribute to the urban aerosol. We studied the effective density (mass-mobility relationship) and mixing state with respect to the density of particles in central Copenhagen, in wintertime. The results are related to particle origin, morphology, and aging. Using a differential mobility analyzer-aerosol particle mass analyzer (DMA-APM), we determined that particles in the diameter range of 50-400 nm were of two groups: porous soot aggregates and more dense particles. Both groups were present at each size in varying proportions. Two types of temporal variability in the relative number fraction of the two groups were found: soot correlated with intense traffic in a diel pattern and dense particles increased during episodes with long-range transport from polluted continental areas. The effective density of each group was relatively stable over time, especially of the soot aggregates, which had effective densities similar to those observed in laboratory studies of fresh diesel exhaust emissions. When heated to 300 °C, the soot aggregate volatile mass fraction was ∼10%. For the dense particles, the volatile mass fraction varied from ∼80% to nearly 100%.

Submicron particles influenced by mixed biogenic and anthropogenic emissions: high-resolution aerosol mass spectrometry results from the Carbonaceous Aerosols and Radiative Effects Study (CARES)

NASA Astrophysics Data System (ADS)

Setyan, A.; Zhang, Q.; Merkel, M.; Knighton, W. B.; Sun, Y.; Song, C.; Shilling, J. E.; Onasch, T. B.; Herndon, S. C.; Worsnop, D. R.; Fast, J. D.; Zaveri, R. A.; Berg, L. K.; Wiedensohler, A.; Flowers, B. A.; Dubey, M. K.; Subramanian, R.

2012-02-01

The Carbonaceous Aerosols and Radiative Effects Study (CARES) took place in the Sacramento Valley of California in summer 2010. We present results obtained at Cool, CA, the T1 site of the project (~40 km downwind of urban emissions from Sacramento), where we deployed an Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) in parallel with complementary instrumentation to characterize the sources and processes of submicron particles (PM1). Cool is located at the foothill of the Sierra Nevada Mountains, where intense biogenic emissions are periodically mixed with urban outflow transported by daytime southwesterly winds from the Sacramento metropolitan area. The particle mass loading was low (3.0 μg m-3 on average) and dominated by organics (80 % of the PM1 mass) followed by sulfate (9.9 %). Organics and sulfate appeared to be externally mixed, as suggested by their different time series (r2 = 0.13) and size distributions. Sulfate showed a bimodal distribution with a droplet mode peaking at ˜400 nm in vacuum aerodynamic diameter (Dva), and a condensation mode at ~150 nm, while organics generally displayed a broad distribution in 60-600 nm (Dva). New particle formation and growth events were observed almost every day, emphasizing the roles of organics and sulfate in new particle growth, especially that of organics. The organic aerosol (OA) had a~nominal formula of C1H1.38N0.004O0.44, thus an average organic mass-to-carbon (OM/OC) ratio of 1.70. Two different oxygenated OA (OOA, 90 % of total OA mass) and a hydrocarbon-like OA (HOA, 10 %) were identified by Positive matrix factorization (PMF) of the high-resolution mass spectra. The more oxidized MO-OOA (O/C = 0.54) corresponded to secondary OA (SOA) primarily influenced by biogenic emissions, while the less oxidized LO-OOA (O/C = 0.42) corresponded to SOA associated with urban transport. The HOA factor corresponded to primary emissions mainly due to local traffic. Twenty three periods of

Control of particle size by coagulation of novel condensation aerosols in reservoir chambers.

PubMed

Hong, John N; Hindle, Michael; Byron, Peter R

2002-01-01

The coagulation growth behavior of capillary aerosol generator (CAG) condensation aerosols was investigated in a series of reservoir chambers. Aerosols consisted of a condensed system of 0.7% w/w benzil (model drug) in propylene glycol (vehicle). These were generated into 250-, 500-, 1,000-, and 2,000-mL reservoirs in both flowing air-stream and static air experiments. Changes in drug and total aerosol particle size were measured by a MOUDI cascade impactor. In both series of experiments the CAG aerosols grew in size. Growth in flowing air-stream experiments was attributed to the amount of accumulation aerosols experienced in reservoirs during sampling and increased with increasing reservoir volume. Mean (SD) MMAD's for the total mass distribution measured for the 250- and 2,000-mL reservoirs were 0.70 (0.02) and 0.87 (0.03) microm, respectively. For the benzil mass distribution, they were 0.64 (0.02) and 0.87 (0.06) microm, respectively. Growth in static air experiments was dependent on the volume aerosol boluses were restricted to and increased with decreasing reservoir volume. Mean (SD) initial MMAD's for the benzil mass distribution for the 250- and 2,000-mL reservoirs were 1.44 (0.03) and 1.24 (0.08) microm, respectively. Holding aerosols for up to 60 sec further increased their size. Mean (SD) MMAD's for benzil after holding for 60 sec in these reservoirs were 2.28 (0.04) and 1.67 (0.09) microm, respectively. The coagulation behavior and therefore particle size of CAG aerosols may be modified and controlled by reservoir chambers for drug targeting within the respiratory tract.

Chemistry and Composition of Atmospheric Aerosol Particles

NASA Astrophysics Data System (ADS)

Kolb, Charles E.; Worsnop, Douglas R.

2012-05-01

For more than two decades a cadre of physical chemists has focused on understanding the formation processes, chemical composition, and chemical kinetics of atmospheric aerosol particles and droplets with diameters ranging from a few nanometers to ˜10,000 nm. They have adapted or invented a range of fundamental experimental and theoretical tools to investigate the thermochemistry, mass transport, and chemical kinetics of processes occurring at nanoscale gas-liquid and gas-solid interfaces for a wide range of nonideal, real-world substances. State-of-the-art laboratory methods devised to study molecular spectroscopy, chemical kinetics, and molecular dynamics also have been incorporated into field measurement instruments that are deployed routinely on research aircraft, ships, and mobile laboratories as well as at field sites from megacities to the most remote jungle, desert, and polar locations. These instruments can now provide real-time, size-resolved aerosol particle physical property and chemical composition data anywhere in Earth's troposphere and lower stratosphere.

Crystallization pathways of sulfate-nitrate-ammonium aerosol particles.

PubMed

Schlenker, Julie C; Martin, Scot T

2005-11-10

Crystallization experiments are conducted for aerosol particles composed of aqueous mixtures of (NH(4))(2)SO(4)(aq) and NH(4)NO(3)(aq), (NH(4))(2)SO(4)(aq) and NH(4)HSO(4)(aq), and NH(4)NO(3)(aq) and NH(4)HSO(4)(aq). Depending on the aqueous composition, crystals of (NH(4))(2)SO(4)(s), (NH(4))(3)H(SO(4))(2)(s), NH(4)HSO(4)(s), NH(4)NO(3)(s), 2NH(4)NO(3) x (NH(4))(2)SO(4)(s), and 3NH(4)NO(3) x (NH(4))(2)SO(4)(s) are formed. Although particles of NH(4)NO(3)(aq) and NH(4)HSO(4)(aq) do not crystallize even at 1% relative humidity, additions of 0.05 mol fraction SO(4)(2-)(aq) or NO(3)(-)(aq) ions promote crystallization, respectively. 2NH(4)NO(3) x (NH(4))(2)SO(4)(s) and (NH(4))(3)H(SO(4))(2)(s) appear to serve as good heterogeneous nuclei for NH(4)NO(3)(s) and NH(4)HSO(4)(s), respectively. 2NH(4)NO(3) x (NH(4))(2)SO(4)(s) crystallizes over a greater range of aqueous compositions than 3NH(4)NO(3) x (NH(4))(2)SO(4)(s). An infrared aerosol spectrum is provided for each solid based upon a linear decomposition analysis of the recorded spectra. Small nonzero residuals occur in the analysis because aerosol spectra depend on particle morphology, which changes slightly across the range of compositions studied. In addition, several of the mixed compositions crystallize with residual aqueous water of up to 5% particle mass. We attribute this water content to enclosed water pockets. The results provide further insights into the nonlinear crystallization pathways of sulfate-nitrate-ammonium aerosol particles.

Gas-particle partitioning of atmospheric aerosols: interplay of physical state, non-ideal mixing and morphology.

PubMed

Shiraiwa, Manabu; Zuend, Andreas; Bertram, Allan K; Seinfeld, John H

2013-07-21

Atmospheric aerosols, comprising organic compounds and inorganic salts, play a key role in air quality and climate. Mounting evidence exists that these particles frequently exhibit phase separation into predominantly organic and aqueous electrolyte-rich phases. As well, the presence of amorphous semi-solid or glassy particle phases has been established. Using the canonical system of ammonium sulfate mixed with organics from the ozone oxidation of α-pinene, we illustrate theoretically the interplay of physical state, non-ideality, and particle morphology affecting aerosol mass concentration and the characteristic timescale of gas-particle mass transfer. Phase separation can significantly affect overall particle mass and chemical composition. Semi-solid or glassy phases can kinetically inhibit the partitioning of semivolatile components and hygroscopic growth, in contrast to the traditional assumption that organic compounds exist in quasi-instantaneous gas-particle equilibrium. These effects have significant implications for the interpretation of laboratory data and the development of improved atmospheric air quality and climate models.

Identifying Metals as Marker for Waste Burning Aerosol Particles in New Delhi

NASA Astrophysics Data System (ADS)

Kumar, Sudhanshu

2012-07-01

{Identifying Metals as Marker for Waste Burning Aerosol Particles in New Delhi } Tracing of aerosol sources is an important task helpful for making control strategy, and for climate change study. However, it is a difficult job as aerosols have several sources, involve in complex atmospheric processing, degradation and removal processes. Several approaches have been used for this task, e.g., models, which are based on the input of chemical species; stable- and radio-isotope compositions of certain species; chemical markers in which trace metals are the better options because they persist in atmosphere until the life of a particle. For example, K and Hg are used for biomass and coal burning tracings, respectively. Open waste burning has recently been believed to be a considerable source of aerosols in several mega cities in India and China. To better understand this source contribution in New Delhi aerosols, we have conducted aerosol sampling at a landfill site (Okhla), and in proximity (within 1 km distance) of this site. Aerosol filter samples were acid digested in microwave digestion system and analyzed using inductively coupled plasma -- high resolution mass spectrometry (ICP-HRMS) for getting metal signatures in particles. The metals, e.g., Sn, Sb and As those are found almost negligible in remote aerosols, are maximized in these waste burning aerosols. Sample collected in other location of New Delhi also shows the considerable presence of these metals in particles. Preliminary studies of isotopic ratios of these metals suggested that these metals, especially Sn can be used as marker for tracing the open waste burning sources of aerosols in New Delhi.

Particle deposition in human respiratory system: deposition of concentrated hygroscopic aerosols.

PubMed

Varghese, Suresh K; Gangamma, S

2009-06-01

In the nearly saturated human respiratory tract, the presence of water-soluble substances in the inhaled aerosols can cause change in the size distribution of the particles. This consequently alters the lung deposition profiles of the inhaled airborne particles. Similarly, the presence of high concentration of hygroscopic aerosols also affects the water vapor and temperature profiles in the respiratory tract. A model is presented to analyze these effects in human respiratory system. The model solves simultaneously the heat and mass transfer equations to determine the size evolution of respirable particles and gas-phase properties within human respiratory tract. First, the model predictions for nonhygroscopic aerosols are compared with experimental results. The model results are compared with experimental results of sodium chloride particles. The model reproduces the major features of the experimental data. The water vapor profile is significantly modified only when a high concentration of particles is present. The model is used to study the effect of equilibrium assumptions on particle deposition. Simulations show that an infinite dilution solution assumption to calculate the saturation equilibrium over droplet could induce errors in estimating particle growth. This error is significant in the case of particles of size greater than 1 mum and at number concentrations higher than 10(5)/cm(3).

Physicochemical characteristics of aerosol particles generated during the milling of beryllium silicate ores: implications for risk assessment.

PubMed

Stefaniak, Aleksandr B; Chipera, Steve J; Day, Gregory A; Sabey, Phil; Dickerson, Robert M; Sbarra, Deborah C; Duling, Mathew G; Lawrence, Robert B; Stanton, Marcia L; Scripsick, Ronald C

2008-01-01

Inhalation of beryllium dusts generated during milling of ores and cutting of beryl-containing gemstones is associated with development of beryllium sensitization and low prevalence of chronic beryllium disease (CBD). Inhalation of beryllium aerosols generated during primary beryllium production and machining of the metal, alloys, and ceramics are associated with sensitization and high rates of CBD, despite similar airborne beryllium mass concentrations among these industries. Understanding the physicochemical properties of exposure aerosols may help to understand the differential immunopathologic mechanisms of sensitization and CBD and lead to more biologically relevant exposure standards. Properties of aerosols generated during the industrial milling of bertrandite and beryl ores were evaluated. Airborne beryllium mass concentrations among work areas ranged from 0.001 microg/m(3) (beryl ore grinding) to 2.1 microg/m(3) (beryl ore crushing). Respirable mass fractions of airborne beryllium-containing particles were < 20% in low-energy input operation areas (ore crushing, hydroxide product drumming) and > 80% in high-energy input areas (beryl melting, beryl grinding). Particle specific surface area decreased with processing from feedstock ores to drumming final product beryllium hydroxide. Among work areas, beryllium was identified in three crystalline forms: beryl, poorly crystalline beryllium oxide, and beryllium hydroxide. In comparison to aerosols generated by high-CBD risk primary production processes, aerosol particles encountered during milling had similar mass concentrations, generally lower number concentrations and surface area, and contained no identifiable highly crystalline beryllium oxide. One possible explanation for the apparent low prevalence of CBD among workers exposed to beryllium mineral dusts may be that characteristics of the exposure material do not contribute to the development of lung burdens sufficient for progression from sensitization to

Measurement of the atmospheric aerosol particle size distribution in a highly polluted mega-city in Southeast Asia (Dhaka-Bangladesh)

NASA Astrophysics Data System (ADS)

Salam, Abdus; Mamoon, Hassan Al; Ullah, Md. Basir; Ullah, Shah M.

2012-11-01

Aerosol particle size distribution was measured with an aerodynamic particle sizer (APS) spectrometer continuously from January 21 to April 24, 2006 in Dhaka, Bangladesh. Particles number, surface and mass distributions data were stored automatically with Aerosol Instrument Manager (AIM) software on average every half an hour in a computer attached to the APS. The grand total average of number, surface and mass concentrations were 8.2 × 103 ± 7.8 × 103 particles cm-3, 13.3 × 103 ± 11.8 × 103 μm2 cm-3 and 3.04 ± 2.10 mg m-3, respectively. Fine particles with diameter smaller than 1.0 μm aerodynamic diameter (AD) dominated the number concentration, accounted for 91.7% of the total particles indicating vehicular emissions were dominating in Dhaka air either from fossil fuel burning or compressed natural gas (CNGs). The surface and mass concentrations between 0.5 and 1.0 μm AD were about 56.0% and 26.4% of the total particles, respectively. Remarkable seasonal differences were observed between winter and pre-monsoon seasons with the highest monthly average in January and the lowest in April. Aerosol particles in winter were 3.79 times higher for number, 3.15 times for surface and 2.18 times for mass distributions than during the pre-monsoon season. Weekends had lower concentrations than weekdays due to less vehicular traffic in the streets. Aerosol particles concentrations were about 15.0% (ranging from 9.4% to 17.3%) higher during traffic peak hours (6:00am-8:00pm) than off hours (8:00pm-6:00am). These are the first aerosol size distribution measurements with respect to number, surface and mass concentrations in real time at Dhaka, Bangladesh.

Modelling non-equilibrium secondary organic aerosol formation and evaporation with the aerosol dynamics, gas- and particle-phase chemistry kinetic multilayer model ADCHAM

DOE Office of Scientific and Technical Information (OSTI.GOV)

Roldin, P.; Eriksson, A. C.; Nordin, E. Z.

2014-08-11

We have developed the novel Aerosol Dynamics, gas- and particle- phase chemistry model for laboratory CHAMber studies (ADCHAM). The model combines the detailed gas phase Master Chemical Mechanism version 3.2, an aerosol dynamics and particle phase chemistry module (which considers acid catalysed oligomerization, heterogeneous oxidation reactions in the particle phase and non-ideal interactions between organic compounds, water and inorganic ions) and a kinetic multilayer module for diffusion limited transport of compounds between the gas phase, particle surface and particle bulk phase. In this article we describe and use ADCHAM to study: 1) the mass transfer limited uptake of ammonia (NH3)more » and formation of organic salts between ammonium (NH4+) and carboxylic acids (RCOOH), 2) the slow and almost particle size independent evaporation of α-pinene secondary organic aerosol (SOA) particles, and 3) the influence of chamber wall effects on the observed SOA formation in smog chambers.« less

Aerosol concentration measurements and correlations with air mass trajectories at the Pierre Auger Observatory

NASA Astrophysics Data System (ADS)

Micheletti, M. I.; Louedec, K.; Freire, M.; Vitale, P.; Piacentini, R. D.

2017-06-01

Aerosols play an important role in radiative transfer processes involved in different fields of study. In particular, their influence is crucial in the attenuation of light at astronomical and astrophysical observatories, and has to be taken into account in light transfer models employed to reconstruct the signals. The Andean Argentinean region is increasingly being considered as a good candidate to host such facilities, as well as the ones for solar-energy resources, and an adequate knowledge of aerosols characteristics there is needed, but it is not always possible due to the vast area involved and the scarce atmospheric data at ground. The aim of this work is to find correlations between aerosol data and particle trajectories that can give an insight into the origin and behaviour of aerosols in this zone and can be employed in situations in which one does not have local aerosol measurements. For this purpose, an aerosol spectrometer and dust monitor (Grimm 1.109) was installed at the Pierre Auger Observatory of ultra-high-energy cosmic rays, to record aerosol concentrations in different size intervals, at surface level. These measurements are analysed and correlated with air mass trajectories obtained from HYSPLIT (NOAA) model calculations. High aerosol concentrations are registered predominantly when air masses have travelled mostly over continental areas, mainly from the NE direction, while low aerosol concentrations are found in correspondence with air masses coming from the Pacific Ocean, from the NW direction. Different size distribution patterns were found for the aerosols depending on their origin: marine or continental. This work shows for the first time the size distribution of aerosols registered at the Pierre Auger Observatory. The correlations found between mass and particle concentrations (total and for different size ranges) and HYSPLIT air mass trajectories, confirm that the latter can be employed as a useful tool to infer the sources, evolution

A new method for assessing the contribution of Primary Biological Atmospheric Particles to the mass concentration of the atmospheric aerosol.

PubMed

Perrino, Cinzia; Marcovecchio, Francesca

2016-02-01

Primary Biologic Atmospheric Particles (PBAPs) constitute an interesting and poorly investigated component of the atmospheric aerosol. We have developed and validated a method for evaluating the contribution of overall PBAPs to the mass concentration of atmospheric particulate matter (PM). The method is based on PM sampling on polycarbonate filters, staining of the collected particles with propidium iodide, observation at epifluorescence microscope and calculation of the bioaerosol mass using a digital image analysis software. The method has been also adapted to the observation and quantification of size-segregated aerosol samples collected by multi-stage impactors. Each step of the procedure has been individually validated. The relative repeatability of the method, calculated on 10 pairs of atmospheric PM samples collected side-by-side, was 16%. The method has been applied to real atmospheric samples collected in the vicinity of Rome, Italy. Size distribution measurements revealed that PBAPs was mainly in the coarse fraction of PM, with maxima in the range 5.6-10 μm. 24-h samples collected during different period of the year have shown that the concentration of bioaerosol was in the range 0.18-5.3 μg m(-3) (N=20), with a contribution to the organic matter in PM10 in the range 0.5-31% and to the total mass concentration of PM10 in the range 0.3-18%. The possibility to determine the concentration of total PBAPs in PM opens up interesting perspectives in terms of studying the health effects of these components and of increasing our knowledge about the composition of the organic fraction of the atmospheric aerosol. Copyright © 2015 Elsevier Ltd. All rights reserved.

Black carbon aerosol mixing state, organic aerosols and aerosol optical properties over the UK

NASA Astrophysics Data System (ADS)

McMeeking, G. R.; Morgan, W. T.; Flynn, M.; Highwood, E. J.; Turnbull, K.; Haywood, J.; Coe, H.

2011-05-01

Black carbon (BC) aerosols absorb sunlight thereby leading to a positive radiative forcing and a warming of climate and can also impact human health through their impact on the respiratory system. The state of mixing of BC with other aerosol species, particularly the degree of internal/external mixing, has been highlighted as a major uncertainty in assessing its radiative forcing and hence its climate impact, but few in situ observations of mixing state exist. We present airborne single particle soot photometer (SP2) measurements of refractory BC (rBC) mass concentrations and mixing state coupled with aerosol composition and optical properties measured in urban plumes and regional pollution over the UK. All data were obtained using instrumentation flown on the UK's BAe-146-301 large Atmospheric Research Aircraft (ARA) operated by the Facility for Airborne Atmospheric Measurements (FAAM). We measured sub-micron aerosol composition using an aerosol mass spectrometer (AMS) and used positive matrix factorization to separate hydrocarbon-like (HOA) and oxygenated organic aerosols (OOA). We found a higher number fraction of thickly coated rBC particles in air masses with large OOA relative to HOA, higher ozone-to-nitrogen oxides (NOx) ratios and large concentrations of total sub-micron aerosol mass relative to rBC mass concentrations. The more ozone- and OOA-rich air masses were associated with transport from continental Europe, while plumes from UK cities had higher HOA and NOx and fewer thickly coated rBC particles. We did not observe any significant change in the rBC mass absorption efficiency calculated from rBC mass and light absorption coefficients measured by a particle soot absorption photometer despite observing significant changes in aerosol composition and rBC mixing state. The contributions of light scattering and absorption to total extinction (quantified by the single scattering albedo; SSA) did change for different air masses, with lower SSA observed in

A study on the relationship between mass concentrations, chemistry and number size distribution of urban fine aerosols in Milan, Barcelona and London

NASA Astrophysics Data System (ADS)

Rodríguez, S.; van Dingenen, R.; Putaud, J.-P.; Dell'Acqua, A.; Pey, J.; Querol, X.; Alastuey, A.; Chenery, S.; Ho, K.-F.; Harrison, R. M.; Tardivo, R.; Scarnato, B.; Gianelle, V.

2007-01-01

A physicochemical characterization of the urban fine aerosol (aerosol number size distribution, chemical composition and mass concentrations) in Milan, Barcelona and London is presented in this article. The objective is to obtain a comprehensive picture on the involvement of the microphysical processes of the aerosol dynamic in the: 1) regular evolution of the urban aerosol (daily, weekly and seasonal basis) and in the day-to-day variations (from clean-air to pollution-events), and 2) link between "aerosol chemistry and mass concentrations" with the "number size distribution". The mass concentrations of the fine PM2.5 aerosol exhibit a high correlation with the number concentration of particles >100 nm (which only accounts for <20% of the total number concentration N of fine aerosols) and do not correlate with the number of particles <100 nm ("ultrafine particles", which accounts for >80% of fine particles). Organic matter (OM) and black-carbon (BC) are the only aerosol components showing a significant correlation with ultrafine particles (attributed to vehicles emissions), whereas ammonium-nitrate, ammonium-sulphate and also OM and BC correlate with N>100(nm) (attributed to gas-to-particle transformation mechanisms and some primary emissions). Time series of the aerosol DpN diameter (dN/dlogD mode), mass PM2.5 concentrations and number N>100(nm) concentrations, exhibit correlated day-to-day variations which point to a significant involvement of condensation of semi-volatile compounds during urban pollution events. This agrees with the fact that ammonium-nitrate is the component exhibiting the highest increases from mid-to-high pollution episodes, when the highest DpN increases are observed. The results indicates that "fine PM2.5 particles urban pollution events" tend to occur when condensation processes have made particles grow enough to produce significant concentrations of N>100(nm). In contrast, because the low contribution of ultrafine particles to the fine

Aerosol Particle Interfacial Thermodynamics and Phase Partitioning Measurements Using Biphasic Microfluidics

NASA Astrophysics Data System (ADS)

Dutcher, Cari; Metcalf, Andrew

2015-03-01

Secondary organic aerosol particles are nearly ubiquitous in the atmosphere and yet there remain large uncertainties in their formation processes and ambient properties. These particles are complex microenvironments, which can contain multiple interfaces due to internal aqueous-organic phase partitioning and to the external liquid-vapor surface. Interfacial properties affect the ambient aerosol morphology, or internal structure of the particle, which in turn can affect the way a particle interacts with an environment of condensable clusters and organic vapors. To improve our ability to accurately predict ambient aerosol morphology, we must improve our knowledge of aerosol interfaces and their interactions with the ambient environment. Unfortunately, many techniques employed to measure interfacial properties do so in bulk solutions or in the presence of a ternary (e.g. solid) phase. In this talk, a novel method using biphasic microscale flows will be introduced for generating, trapping, and perturbing complex interfaces at atmospherically relevant conditions. These microfluidic experiments utilize high-speed imaging to monitor interfacial phenomena at the microscale and are performed with phase contrast and fluorescence microscopy on a temperature-controlled inverted microscope stage. From these experiments, interfacial thermodynamic properties such as surface or interfacial tension, rheological properties such as interfacial moduli, and kinetic properties such as mass transfer coefficients can be measured or inferred.

Black carbon aerosol mixing state, organic aerosols and aerosol optical properties over the United Kingdom

NASA Astrophysics Data System (ADS)

McMeeking, G. R.; Morgan, W. T.; Flynn, M.; Highwood, E. J.; Turnbull, K.; Haywood, J.; Coe, H.

2011-09-01

Black carbon (BC) aerosols absorb sunlight thereby leading to a positive radiative forcing and a warming of climate and can also impact human health through their impact on the respiratory system. The state of mixing of BC with other aerosol species, particularly the degree of internal/external mixing, has been highlighted as a major uncertainty in assessing its radiative forcing and hence its climate impact, but few in situ observations of mixing state exist. We present airborne single particle soot photometer (SP2) measurements of refractory BC (rBC) mass concentrations and mixing state coupled with aerosol composition and optical properties measured in urban plumes and regional pollution over the United Kingdom. All data were obtained using instrumentation flown on the UK's BAe-146-301 large Atmospheric Research Aircraft (ARA) operated by the Facility for Airborne Atmospheric Measurements (FAAM). We measured sub-micron aerosol composition using an aerosol mass spectrometer (AMS) and used positive matrix factorization to separate hydrocarbon-like (HOA) and oxygenated organic aerosols (OOA). We found a higher number fraction of thickly coated rBC particles in air masses with large OOA relative to HOA, higher ozone-to-nitrogen oxides (NOx) ratios and large concentrations of total sub-micron aerosol mass relative to rBC mass concentrations. The more ozone- and OOA-rich air masses were associated with transport from continental Europe, while plumes from UK cities had higher HOA and NOx and fewer thickly coated rBC particles. We did not observe any significant change in the rBC mass absorption efficiency calculated from rBC mass and light absorption coefficients measured by a particle soot absorption photometer despite observing significant changes in aerosol composition and rBC mixing state. The contributions of light scattering and absorption to total extinction (quantified by the single scattering albedo; SSA) did change for different air masses, with lower SSA

Single particle analysis of eastern Mediterranean aerosol particles: Influence of the source region on the chemical composition

NASA Astrophysics Data System (ADS)

Clemen, Hans-Christian; Schneider, Johannes; Köllner, Franziska; Klimach, Thomas; Pikridas, Michael; Stavroulas, Iasonas; Sciare, Jean; Borrmann, Stephan

2017-04-01

The Mediterranean region is one of the most climatically sensitive areas and is influenced by air masses of different origin. Aerosol particles are one important factor contributing to the Earth's radiative forcing, but knowledge about their composition and sources is still limited. Here, we report on results from the INUIT-BACCHUS-ACTRIS campaign, which was conducted at the Cyprus Atmospheric Observatory (CAO, Agia Marina Xyliatou) in Cyprus in April 2016. Our results show that the chemical composition of the aerosol particles in the eastern Mediterranean is strongly dependent on their source region. The composition of particles in a size range between 150 nm and 3 μm was measured using the Aircraft-based Laser ABlation Aerosol MAss spectrometer (ALABAMA), which is a single particle laser ablation instrument using a bipolar time-of-flight mass spectrometer. The mass spectral information on cations and anions allow for the analysis of different molecular fragments. The information about the source regions results from backward trajectories using HYSPLIT Trajectory Model (Trajectory Ensemble) on hourly basis. To assess the influence of certain source regions on the air masses arriving at CAO, we consider the number of trajectories that crossed the respective source region within defined time steps. For a more detailed picture also the height and the velocity of the air masses during their overpass above the source regions will be considered. During the campaign at CAO in April 2016 three main air mass source regions were observed: 1) Northern Central Europe, likely with an enhanced anthropogenic influence (e.g. sulfate and black carbon from combustion processes, fly ash particles from power plants, characterized by Sr and Ba), 2) Southwest Europe, with a higher influence of the Mediterranean Sea including sea salt particles (characterized by, e.g., NaxCly, NaClxNOy), 3) Northern Africa/Sahara, with air masses that are expected to have a higher load of mineral dust

Uptake of Semivolatile Secondary Organic Aerosol Formed from α-Pinene into Nonvolatile Polyethylene Glycol Probe Particles.

PubMed

Ye, Penglin; Ding, Xiang; Ye, Qing; Robinson, Ellis S; Donahue, Neil M

2016-03-10

Semivolatile organic compounds (SVOCs) play an essential role in secondary organic aerosol (SOA) formation, chemical aging, and mixing of organic aerosol (OA) from different sources. Polyethylene glycol (PEG400) particles are liquid, polar, and nearly nonvolatile; they provide a new vehicle to study the interaction between SVOCs with OA. With a unique fragment ion C4H9O2(+) (m/z 89), PEG400 can be easily separated from α-pinene SOA in aerosol mass spectra. By injecting separately prepared PEG probe particles into a chamber containing SOA coated on ammonium sulfate seeds, we show that a substantial pool of SVOCs exists in equilibrium with the original SOA particles. Quantitative findings are based on bulk mass spectra, size-dependent composition, and the evolution of individual particle mass spectra, which we use to separate the two particle populations. We observed a larger fraction of SVOC vapors with increased amounts of reacted α-pinene. For the same amount of reacted α-pinene, the SOA formed from α-pinene oxidized by OH radicals had a higher fraction of SOA vapors than SOA formed by α-pinene ozonolysis. Compared to the PEG400 probe particles, we observed a lower mass fraction of SVOCs in poly(ethylene glycol) dimethyl ether (MePEG500) probe particles under otherwise identical conditions; this may be due to the lower polarity of the MePEG500 or caused by esterification reactions between the PEG400 and organic acids in the SOA.

Aerosol characteristics and particle production in the upper troposphere over the Amazon Basin

NASA Astrophysics Data System (ADS)

Andreae, Meinrat O.; Afchine, Armin; Albrecht, Rachel; Amorim Holanda, Bruna; Artaxo, Paulo; Barbosa, Henrique M. J.; Borrmann, Stephan; Cecchini, Micael A.; Costa, Anja; Dollner, Maximilian; Fütterer, Daniel; Järvinen, Emma; Jurkat, Tina; Klimach, Thomas; Konemann, Tobias; Knote, Christoph; Krämer, Martina; Krisna, Trismono; Machado, Luiz A. T.; Mertes, Stephan; Minikin, Andreas; Pöhlker, Christopher; Pöhlker, Mira L.; Pöschl, Ulrich; Rosenfeld, Daniel; Sauer, Daniel; Schlager, Hans; Schnaiter, Martin; Schneider, Johannes; Schulz, Christiane; Spanu, Antonio; Sperling, Vinicius B.; Voigt, Christiane; Walser, Adrian; Wang, Jian; Weinzierl, Bernadett; Wendisch, Manfred; Ziereis, Helmut

2018-01-01

Airborne observations over the Amazon Basin showed high aerosol particle concentrations in the upper troposphere (UT) between 8 and 15 km altitude, with number densities (normalized to standard temperature and pressure) often exceeding those in the planetary boundary layer (PBL) by 1 or 2 orders of magnitude. The measurements were made during the German-Brazilian cooperative aircraft campaign ACRIDICON-CHUVA, where ACRIDICON stands for Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems and CHUVA is the acronym for Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM (global precipitation measurement), on the German High Altitude and Long Range Research Aircraft (HALO). The campaign took place in September-October 2014, with the objective of studying tropical deep convective clouds over the Amazon rainforest and their interactions with atmospheric trace gases, aerosol particles, and atmospheric radiation. Aerosol enhancements were observed consistently on all flights during which the UT was probed, using several aerosol metrics, including condensation nuclei (CN) and cloud condensation nuclei (CCN) number concentrations and chemical species mass concentrations. The UT particles differed sharply in their chemical composition and size distribution from those in the PBL, ruling out convective transport of combustion-derived particles from the boundary layer (BL) as a source. The air in the immediate outflow of deep convective clouds was depleted of aerosol particles, whereas strongly enhanced number concentrations of small particles (< 90 nm diameter) were found in UT regions that had experienced outflow from deep convection in the preceding 5-72 h. We also found elevated concentrations of larger (> 90 nm) particles in the UT, which consisted mostly of organic matter and nitrate and were very effective CCN. Our findings suggest a

Aerosol characteristics and particle production in the upper troposphere over the Amazon Basin

DOE PAGES

Andreae, Meinrat O.; Afchine, Armin; Albrecht, Rachel; ...

2018-01-25

Airborne observations over the Amazon Basin showed high aerosol particle concentrations in the upper troposphere (UT) between 8 and 15 km altitude, with number densities (normalized to standard temperature and pressure) often exceeding those in the planetary boundary layer (PBL) by 1 or 2 orders of magnitude. The measurements were made during the German–Brazilian cooperative aircraft campaign ACRIDICON–CHUVA, where ACRIDICON stands for Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems and CHUVA is the acronym for Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM (globalmore » precipitation measurement), on the German High Altitude and Long Range Research Aircraft (HALO). The campaign took place in September–October 2014, with the objective of studying tropical deep convective clouds over the Amazon rainforest and their interactions with atmospheric trace gases, aerosol particles, and atmospheric radiation. Aerosol enhancements were observed consistently on all flights during which the UT was probed, using several aerosol metrics, including condensation nuclei (CN) and cloud condensation nuclei (CCN) number concentrations and chemical species mass concentrations. The UT particles differed sharply in their chemical composition and size distribution from those in the PBL, ruling out convective transport of combustion-derived particles from the boundary layer (BL) as a source. The air in the immediate outflow of deep convective clouds was depleted of aerosol particles, whereas strongly enhanced number concentrations of small particles (< 90 nm diameter) were found in UT regions that had experienced outflow from deep convection in the preceding 5–72 h. We also found elevated concentrations of larger (> 90 nm) particles in the UT, which consisted mostly of organic matter and nitrate and were very effective CCN. Our findings suggest a conceptual

Aerosol characteristics and particle production in the upper troposphere over the Amazon Basin

DOE Office of Scientific and Technical Information (OSTI.GOV)

Andreae, Meinrat O.; Afchine, Armin; Albrecht, Rachel

Airborne observations over the Amazon Basin showed high aerosol particle concentrations in the upper troposphere (UT) between 8 and 15 km altitude, with number densities (normalized to standard temperature and pressure) often exceeding those in the planetary boundary layer (PBL) by 1 or 2 orders of magnitude. The measurements were made during the German–Brazilian cooperative aircraft campaign ACRIDICON–CHUVA, where ACRIDICON stands for Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems and CHUVA is the acronym for Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM (globalmore » precipitation measurement), on the German High Altitude and Long Range Research Aircraft (HALO). The campaign took place in September–October 2014, with the objective of studying tropical deep convective clouds over the Amazon rainforest and their interactions with atmospheric trace gases, aerosol particles, and atmospheric radiation. Aerosol enhancements were observed consistently on all flights during which the UT was probed, using several aerosol metrics, including condensation nuclei (CN) and cloud condensation nuclei (CCN) number concentrations and chemical species mass concentrations. The UT particles differed sharply in their chemical composition and size distribution from those in the PBL, ruling out convective transport of combustion-derived particles from the boundary layer (BL) as a source. The air in the immediate outflow of deep convective clouds was depleted of aerosol particles, whereas strongly enhanced number concentrations of small particles (< 90 nm diameter) were found in UT regions that had experienced outflow from deep convection in the preceding 5–72 h. We also found elevated concentrations of larger (> 90 nm) particles in the UT, which consisted mostly of organic matter and nitrate and were very effective CCN. Our findings suggest a conceptual

Single Aerosol Particle Studies Using Optical Trapping Raman And Cavity Ringdown Spectroscopy

NASA Astrophysics Data System (ADS)

Gong, Z.; Wang, C.; Pan, Y. L.; Videen, G.

2017-12-01

Due to the physical and chemical complexity of aerosol particles and the interdisciplinary nature of aerosol science that involves physics, chemistry, and biology, our knowledge of aerosol particles is rather incomplete; our current understanding of aerosol particles is limited by averaged (over size, composition, shape, and orientation) and/or ensemble (over time, size, and multi-particles) measurements. Physically, single aerosol particles are the fundamental units of any large aerosol ensembles. Chemically, single aerosol particles carry individual chemical components (properties and constituents) in particle ensemble processes. Therefore, the study of single aerosol particles can bridge the gap between aerosol ensembles and bulk/surface properties and provide a hierarchical progression from a simple benchmark single-component system to a mixed-phase multicomponent system. A single aerosol particle can be an effective reactor to study heterogeneous surface chemistry in multiple phases. Latest technological advances provide exciting new opportunities to study single aerosol particles and to further develop single aerosol particle instrumentation. We present updates on our recent studies of single aerosol particles optically trapped in air using the optical-trapping Raman and cavity ringdown spectroscopy.

A Miniature Aerosol Sensor for Detecting Polydisperse Airborne Ultrafine Particles.

PubMed

Zhang, Chao; Wang, Dingqu; Zhu, Rong; Yang, Wenming; Jiang, Peng

2017-04-22

Counting and sizing of polydisperse airborne nanoparticles have attracted most attentions owing to increasing widespread presence of airborne engineered nanoparticles or ultrafine particles. Here we report a miniature aerosol sensor to detect particle size distribution of polydisperse ultrafine particles based on ion diffusion charging and electrical detection. The aerosol sensor comprises a couple of planar electrodes printed on two circuit boards assembled in parallel, where charging, precipitation and measurement sections are integrated into one chip, which can detect aerosol particle size in of 30-500 nm, number concentration in range of 5 × 10²-10⁷ /cm³. The average relative errors of the measured aerosol number concentration and the particle size are estimated to be 12.2% and 13.5% respectively. A novel measurement scheme is proposed to actualize a real-time detection of polydisperse particles by successively modulating the measurement voltage and deducing the particle size distribution through a smart data fusion algorithm. The effectiveness of the aerosol sensor is experimentally demonstrated via measurements of polystyrene latex (PSL) aerosol and nucleic acid aerosol, as well as sodium chloride aerosol particles.

Towards depth profiling of organic aerosols in real time using aerosol flowing atmospheric-pressure afterglow mass spectrometry (AeroFAPA-MS)

NASA Astrophysics Data System (ADS)

Brüggemann, Martin; Hoffmann, Thorsten

2014-05-01

Organic aerosol accounts for a substantial fraction of tropospheric aerosol and has implications on the earth's climate and human health. However, the characterization of its chemical composition and transformations remain a major challenge and is still connected to large uncertainties (IPCC, 2013). Recent measurements revealed that organic aerosol particles may reside in an amorphous or semi-solid phase state which impedes the diffusion within the particles (Virtanen et al., 2010; Shiraiwa et al., 2011). This means that reaction products which are formed on the surface of a particle, e.g. by OH, NO3 or ozone chemistry, cannot diffuse into the particle's core and remain at the surface. Eventually, this leads to particles with a core/shell structure. In the particles' cores the initial compounds are preserved whereas the shells contain mainly the oxidation products. By analyzing the particles' cores and shells separately, thus, it is possible to obtain valuable information on the formation and evolution of the aerosols' particle and gas phase. Here we present the development of the aerosol flowing atmospheric-pressure afterglow (AeroFAPA) technique which allows the mass spectrometric analysis of organic aerosols in real time. The AeroFAPA is an ion source based on a helium glow discharge at atmospheric pressure. The plasma produces excited helium species and primary reagent ions which are transferred into the afterglow region where the ionization of the analytes takes place. Due to temperatures of only 80 ° C to 150 ° C and ambient pressure in the afterglow region, the ionization is very soft and almost no fragmentation of organic molecules is observed. Thus, the obtained mass spectra are easy to interpret and no extensive data analysis procedure is necessary. Additionally, first results of a combination of the AeroFAPA-MS with a scanning mobility particle sizer (SMPS) suggest that it is not only possible to analyze the entire particle phase but rather that a

Sources and composition of submicron organic mass in marine aerosol particles

DOE PAGES

Frossard, Amanda A.; Russell, Lynn M.; Burrows, Susannah M.; ...

2014-11-27

Recent studies have proposed a variety of interpretations of the sources and composition of atmospheric marine aerosol particles (aMA) based on a range of physical and chemical measurements collected during open-ocean research cruises. To investigate the processes that affect marine organic particles, this study uses the characteristic functional group composition (from Fourier transform infrared (FTIR) spectroscopy) of aMAP from five ocean regions to show that: (i) The organic functional group composition of aMAP that can be identified as atmospheric primary marine (ocean-derived) aerosol (aPMA) is 65±12% hydroxyl, 21±9% alkane, 6±6% amine, and 7±8% carboxylic acid functional groups. Contributions from photochemicalmore » reactions add carboxylic acid groups (15%-25%), shipping effluent in seawater and ship emissions add additional alkane groups (up to 70%), and coastal emissions mix in alkane and carboxylic acid groups from coastal pollution sources. (ii) The organic composition of aPMA is nearly identical to model generated primary marine aerosol particles (gPMA) from bubbled seawater (55% hydroxyl, 32% alkane, and 13% amine functional groups), indicating that its overall functional group composition is the direct consequence of the organic constituents of the seawater source. (iii) While the seawater organic functional group composition was nearly invariant across all three ocean regions studied, the gPMA alkane group fraction increased with chlorophyll-a concentrations (r = 0.79). gPMA from productive seawater had a larger fraction of alkane functional groups (35%) compared to gPMA from non-productive seawater (16%), likely due to the presence of surfactants in productive seawater that stabilize the bubble film and lead to preferential drainage of the more soluble (lower alkane group fraction) organic components. gPMA has a hydroxyl group absorption peak location characteristic of monosaccharides and disaccharides, where the seawater OM hydroxyl group

Sources and composition of submicron organic mass in marine aerosol particles

DOE Office of Scientific and Technical Information (OSTI.GOV)

Frossard, Amanda A.; Russell, Lynn M.; Burrows, Susannah M.

Recent studies have proposed a variety of interpretations of the sources and composition of atmospheric marine aerosol particles (aMA) based on a range of physical and chemical measurements collected during open-ocean research cruises. To investigate the processes that affect marine organic particles, this study uses the characteristic functional group composition (from Fourier transform infrared (FTIR) spectroscopy) of aMAP from five ocean regions to show that: (i) The organic functional group composition of aMAP that can be identified as atmospheric primary marine (ocean-derived) aerosol (aPMA) is 65±12% hydroxyl, 21±9% alkane, 6±6% amine, and 7±8% carboxylic acid functional groups. Contributions from photochemicalmore » reactions add carboxylic acid groups (15%-25%), shipping effluent in seawater and ship emissions add additional alkane groups (up to 70%), and coastal emissions mix in alkane and carboxylic acid groups from coastal pollution sources. (ii) The organic composition of aPMA is nearly identical to model generated primary marine aerosol particles (gPMA) from bubbled seawater (55% hydroxyl, 32% alkane, and 13% amine functional groups), indicating that its overall functional group composition is the direct consequence of the organic constituents of the seawater source. (iii) While the seawater organic functional group composition was nearly invariant across all three ocean regions studied, the gPMA alkane group fraction increased with chlorophyll-a concentrations (r = 0.79). gPMA from productive seawater had a larger fraction of alkane functional groups (35%) compared to gPMA from non-productive seawater (16%), likely due to the presence of surfactants in productive seawater that stabilize the bubble film and lead to preferential drainage of the more soluble (lower alkane group fraction) organic components. gPMA has a hydroxyl group absorption peak location characteristic of monosaccharides and disaccharides, where the seawater OM hydroxyl group

Collection efficiency of the soot-particle aerosol mass spectrometer (SP-AMS) for internally mixed particulate black carbon

DOE Office of Scientific and Technical Information (OSTI.GOV)

Willis, M. D.; Lee, A. K. Y.; Onasch, T. B.

The soot-particle aerosol mass spectrometer (SP-AMS) uses an intra-cavity infrared laser to vaporize refractory black carbon (rBC) containing particles, making the particle beam–laser beam overlap critical in determining the collection efficiency (CE) for rBC and associated non-refractory particulate matter (NR-PM). This work evaluates the ability of the SP-AMS to quantify rBC and NR-PM mass in internally mixed particles with different thicknesses of organic coating. Using apparent relative ionization efficiencies for uncoated and thickly coated rBC particles, we report measurements of SP-AMS sensitivity to NR-PM and rBC, for Regal Black, the recommended particulate calibration material. Beam width probe (BWP) measurements aremore » used to illustrate an increase in sensitivity for highly coated particles due to narrowing of the particle beam, which enhances the CE of the SP-AMS by increasing the laser beam–particle beam overlap. Assuming complete overlap for thick coatings, we estimate CE for bare Regal Black particles of 0.6 ± 0.1, which suggests that previously measured SP-AMS sensitivities to Regal Black were underestimated by up to a factor of 2. The efficacy of the BWP measurements is highlighted by studies at a busy road in downtown Toronto and at a non-roadside location, which show particle beam widths similar to, but greater than that of bare Regal Black and coated Regal Black, respectively. Further BWP measurements at field locations will help to constrain the range of CE for fresh and aged rBC-containing particles. The ability of the SP-AMS to quantitatively assess the composition of internally mixed particles is validated through measurements of laboratory-generated organic coated particles, which demonstrate that the SP-AMS can quantify rBC and NR-PM over a wide range of particle compositions and rBC core sizes.« less

Collection efficiency of the soot-particle aerosol mass spectrometer (SP-AMS) for internally mixed particulate black carbon

DOE PAGES

Willis, M. D.; Lee, A. K. Y.; Onasch, T. B.; ...

2014-12-18

The soot-particle aerosol mass spectrometer (SP-AMS) uses an intra-cavity infrared laser to vaporize refractory black carbon (rBC) containing particles, making the particle beam–laser beam overlap critical in determining the collection efficiency (CE) for rBC and associated non-refractory particulate matter (NR-PM). This work evaluates the ability of the SP-AMS to quantify rBC and NR-PM mass in internally mixed particles with different thicknesses of organic coating. Using apparent relative ionization efficiencies for uncoated and thickly coated rBC particles, we report measurements of SP-AMS sensitivity to NR-PM and rBC, for Regal Black, the recommended particulate calibration material. Beam width probe (BWP) measurements aremore » used to illustrate an increase in sensitivity for highly coated particles due to narrowing of the particle beam, which enhances the CE of the SP-AMS by increasing the laser beam–particle beam overlap. Assuming complete overlap for thick coatings, we estimate CE for bare Regal Black particles of 0.6 ± 0.1, which suggests that previously measured SP-AMS sensitivities to Regal Black were underestimated by up to a factor of 2. The efficacy of the BWP measurements is highlighted by studies at a busy road in downtown Toronto and at a non-roadside location, which show particle beam widths similar to, but greater than that of bare Regal Black and coated Regal Black, respectively. Further BWP measurements at field locations will help to constrain the range of CE for fresh and aged rBC-containing particles. The ability of the SP-AMS to quantitatively assess the composition of internally mixed particles is validated through measurements of laboratory-generated organic coated particles, which demonstrate that the SP-AMS can quantify rBC and NR-PM over a wide range of particle compositions and rBC core sizes.« less

Chemical evolution of multicomponent aerosol particles during evaporation

NASA Astrophysics Data System (ADS)

Zardini, Alessandro; Riipinen, Ilona; Pagels, Joakim; Eriksson, Axel; Worsnop, Douglas; Switieckli, Erik; Kulmala, Markku; Bilde, Merete

2010-05-01

Atmospheric aerosol particles have an important but not well quantified effect on climate and human health. Despite the efforts made in the last decades, the formation and evolution of aerosol particles in the atmosphere is still not fully understood. The uncertainty is partly due to the complex chemical composition of the particles which comprise inorganic and organic compounds. Many organics (like dicarboxylic acids) can be present both in the gas and in the condensed phase due to their low vapor pressure. Clearly, an understanding of this partition is crucial to address any other issue in atmospheric physics and chemistry. Moreover, many organics are water soluble, and their influence on the properties of aqueous solution droplets is still poorly characterized. The solid and sub-cooled liquid state vapor pressures of some organic compounds have been previously determined by measuring the evaporation rate of single-compound crystals [1-3] or binary aqueous droplets [4-6]. In this work, we deploy the HTDMA technique (Hygroscopicity Tandem Differential Mobility Analyzer) coupled with a 3.5m laminar flow-tube and an Aerosol Mass Spectrometer (AMS) for determining the chemical evolution during evaporation of ternary droplets made of one dicarboxylic acid (succinic acid, commonly found in atmospheric samples) and one inorganic compound (sodium chloride or ammonium sulfate) in different mixing ratios, in equilibrium with water vapor at a fixed relative humidity. In addition, we investigate the evaporation of multicomponent droplets and crystals made of three organic species (dicarboxylic acids and sugars), of which one or two are semi-volatile. 1. Bilde M. and Pandis, S.N.: Evaporation Rates and Vapor Pressures of Individual Aerosol Species Formed in the Atmospheric Oxidation of alpha- and beta-Pinene. Environmental Science and Technology, 35, 2001. 2. Bilde M., et al.: Even-Odd Alternation of Evaporation Rates and Vapor Pressures of C3-C9 Dicarboxylic Acid Aerosols

In-Situ Characterization of Cloud Condensation Nuclei, Interstitial, and background Particles using Single Particle Mass Spectrometer, SPLAT II

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zelenyuk, Alla; Imre, D.; Earle, Michael

2010-10-01

Aerosol indirect effect remains the most uncertain aspect of climate change modeling because proper test requires knowledge of individual particles sizes and compositions with high spatial and temporal resolution. We present the first deployment of a single particle mass spectrometer (SPLAT II) that is operated in a dual data acquisition mode to measure all the required individual particle properties with sufficient temporal resolution to definitively resolve the aerosol-cloud interaction in this exemplary case. We measured particle number concentrations, asphericity, and individual particle size, composition, and density with better than 60 seconds resolution. SPLAT II measured particle number concentrations between 70more » particles cm-3and 300 particles cm-3, an average particle density of 1.4 g cm-3. Found that most particles are composed of oxygenated organics, many of which are mixed with sulfates. Biomass burn particles some with sulfates were prevalent, particularly at higher altitudes, and processed sea-salt was observed over the ocean. Analysis of cloud residuals shows that with time cloud droplets acquire sulfate by the reaction of peroxide with SO2. Based on the particle mass spectra and densities we find that the compositions of cloud condensation nuclei are similar to those of background aerosol but, contain on average ~7% more sulfate, and do not include dust and metallic particles. A comparison between the size distributions of background, activated, and interstitial particles shows that while nearly none of the activated particles is smaller than 115 nm, more than 80% of interstitial particles are smaller than 115 nm. We conclude that for this cloud the most important difference between CCN and background aerosol is particle size although having more sulfate also helps.« less

Measurements of Size Resolved Organic Particulate Mass Using An On-line Aerosol Mass Spectrometer (ams) Laboratory Validation; Analysis Tool Development; and Interpretation of Field Data

NASA Astrophysics Data System (ADS)

Alfarra, M. R.; Coe, H.; Allan, J. D.; Bower, K. N.; Garforth, A. A.; Canagaratna, M.; Worsnop, D.

The aerosol mass spectrometer (AMS) is a quantitative instrument designed to deliver real-time size resolved chemical composition of the volatile and semi volatile aerosol fractions. The AMS response to a wide range of organic compounds has been exper- imentally characterized, and has been shown to compare well with standard libraries of 70 eV electron impact ionization mass spectra. These results will be presented. Due to the scanning nature of the quadrupole mass spectrometer, the AMS provides averaged composition of ensemble of particles rather than single particle composi- tion. However, the mass spectra measured by AMS are reproducible and similar to those of standard libraries so analysis tools can be developed on large mass spectral libraries that can provide chemical composition information about the type of organic compounds in the aerosol. One such tool is presented and compared with laboratory measurements of single species and mixed component organic particles by the AMS. We will then discuss the applicability of these tools to interpreting field AMS data ob- tained in a range of experiments at different sites in the UK and Canada. The data will be combined with other measurements to show the behaviour of the organic aerosol fraction in urban and sub-urban environments.

High-efficiency particulate air filter test stand and aerosol generator for particle loading studies

NASA Astrophysics Data System (ADS)

Arunkumar, R.; Hogancamp, Kristina U.; Parsons, Michael S.; Rogers, Donna M.; Norton, Olin P.; Nagel, Brian A.; Alderman, Steven L.; Waggoner, Charles A.

2007-08-01

This manuscript describes the design, characterization, and operational range of a test stand and high-output aerosol generator developed to evaluate the performance of 30×30×29cm3 nuclear grade high-efficiency particulate air (HEPA) filters under variable, highly controlled conditions. The test stand system is operable at volumetric flow rates ranging from 1.5to12standardm3/min. Relative humidity levels are controllable from 5%-90% and the temperature of the aerosol stream is variable from ambient to 150°C. Test aerosols are produced through spray drying source material solutions that are introduced into a heated stainless steel evaporation chamber through an air-atomizing nozzle. Regulation of the particle size distribution of the aerosol challenge is achieved by varying source solution concentrations and through the use of a postgeneration cyclone. The aerosol generation system is unique in that it facilitates the testing of standard HEPA filters at and beyond rated media velocities by consistently providing, into a nominal flow of 7standardm3/min, high mass concentrations (˜25mg/m3) of dry aerosol streams having count mean diameters centered near the most penetrating particle size for HEPA filters (120-160nm). Aerosol streams that have been generated and characterized include those derived from various concentrations of KCl, NaCl, and sucrose solutions. Additionally, a water insoluble aerosol stream in which the solid component is predominantly iron (III) has been produced. Multiple ports are available on the test stand for making simultaneous aerosol measurements upstream and downstream of the test filter. Types of filter performance related studies that can be performed using this test stand system include filter lifetime studies, filtering efficiency testing, media velocity testing, evaluations under high mass loading and high humidity conditions, and determination of the downstream particle size distributions.

High-efficiency particulate air filter test stand and aerosol generator for particle loading studies.

PubMed

Arunkumar, R; Hogancamp, Kristina U; Parsons, Michael S; Rogers, Donna M; Norton, Olin P; Nagel, Brian A; Alderman, Steven L; Waggoner, Charles A

2007-08-01

This manuscript describes the design, characterization, and operational range of a test stand and high-output aerosol generator developed to evaluate the performance of 30 x 30 x 29 cm(3) nuclear grade high-efficiency particulate air (HEPA) filters under variable, highly controlled conditions. The test stand system is operable at volumetric flow rates ranging from 1.5 to 12 standard m(3)/min. Relative humidity levels are controllable from 5%-90% and the temperature of the aerosol stream is variable from ambient to 150 degrees C. Test aerosols are produced through spray drying source material solutions that are introduced into a heated stainless steel evaporation chamber through an air-atomizing nozzle. Regulation of the particle size distribution of the aerosol challenge is achieved by varying source solution concentrations and through the use of a postgeneration cyclone. The aerosol generation system is unique in that it facilitates the testing of standard HEPA filters at and beyond rated media velocities by consistently providing, into a nominal flow of 7 standard m(3)/min, high mass concentrations (approximately 25 mg/m(3)) of dry aerosol streams having count mean diameters centered near the most penetrating particle size for HEPA filters (120-160 nm). Aerosol streams that have been generated and characterized include those derived from various concentrations of KCl, NaCl, and sucrose solutions. Additionally, a water insoluble aerosol stream in which the solid component is predominantly iron (III) has been produced. Multiple ports are available on the test stand for making simultaneous aerosol measurements upstream and downstream of the test filter. Types of filter performance related studies that can be performed using this test stand system include filter lifetime studies, filtering efficiency testing, media velocity testing, evaluations under high mass loading and high humidity conditions, and determination of the downstream particle size distributions.

Vertical profiles of fine and coarse aerosol particles over Cyprus: Comparison between in-situ drone measurements and remote sensing observations

NASA Astrophysics Data System (ADS)

Mamali, Dimitra; Marinou, Eleni; Pikridas, Michael; Kottas, Michael; Binietoglou, Ioannis; Kokkalis, Panagiotis; Tsekeri, Aleksandra; Amiridis, Vasilis; Sciare, Jean; Keleshis, Christos; Engelmann, Ronny; Ansmann, Albert; Russchenberg, Herman W. J.; Biskos, George

2017-04-01

Vertical profiles of the aerosol mass concentration derived from light detection and ranging (lidar) measurements were compared to airborne dried optical particle counter (OPC MetOne; Model 212) measurements during the INUIT-BACCHUS-ACTRIS campaign. The campaign took place in April 2016 and its main focus was the study of aerosol dust particles. During the campaign the NOA Polly-XT Raman lidar located at Nicosia (35.08° N, 33.22° E) was providing round-the-clock vertical profiles of aerosol optical properties. In addition, an unmanned aerial vehicle (UAV) carrying an OPC flew on 7 days during the first morning hours. The flights were performed at Orounda (35.1018° N, 33.0944° E) reaching altitudes of 2.5 km a.s.l, which allows comparison with a good fraction of the recorded lidar data. The polarization lidar photometer networking method (POLIPHON) was used for the estimation of the fine (non-dust) and coarse (dust) mode aerosol mass concentration profiles. This method uses as input the particle backscatter coefficient and the particle depolarization profiles of the lidar at 532 nm wavelength and derives the aerosol mass concentration. The first step in this approach makes use of the lidar observations to separate the backscatter and extinction contributions of the weakly depolarizing non-dust aerosol components from the contributions of the strongly depolarizing dust particles, under the assumption of an externally mixed two-component aerosol. In the second step, sun photometer retrievals of the fine and the coarse modes aerosol optical thickness (AOT) and volume concentration are used to calculate the associated concentrations from the extinction coefficients retrieved from the lidar. The estimated aerosol volume concentrations were converted into mass concentration with an assumption for the bulk aerosol density, and compared with the OPC measurements. The first results show agreement within the experimental uncertainty. This project received funding from the

Wind reduction by aerosol particles

NASA Astrophysics Data System (ADS)

Jacobson, Mark Z.; Kaufman, Yoram J.

2006-12-01

Aerosol particles are known to affect radiation, temperatures, stability, clouds, and precipitation, but their effects on spatially-distributed wind speed have not been examined to date. Here, it is found that aerosol particles, directly and through their enhancement of clouds, may reduce near-surface wind speeds below them by up to 8% locally. This reduction may explain a portion of observed ``disappearing winds'' in China, and it decreases the energy available for wind-turbine electricity. In California, slower winds reduce emissions of wind-driven soil dust and sea spray. Slower winds and cooler surface temperatures also reduce moisture advection and evaporation. These factors, along with the second indirect aerosol effect, may reduce California precipitation by 2-5%, contributing to a strain on water supply.

Organic Functional Group Composition of Submicron Aerosol Particles at Alert, Nunavut, during 2012-2014

NASA Astrophysics Data System (ADS)

Russell, L. M.; Leaitch, W. R.; Liu, J.; Desiree, T. S.; Huang, L.; Sharma, S.; Chivulescu, A.; Veber, D.; Zhang, W.

2016-12-01

Long-term measurements of submicron aerosol particle chemical composition and size distributions are essential for evaluating whether global climate models correctly transport particles from lower latitudes to polar regions, especially in the winter months when satellite retrieval of aerosol properties is limited. In collaboration with ongoing measurements by the Dr. Neil Trivett Global Atmospheric Watch observatory at Alert, Nunavut (82.5°N; elevation 185 m-ASL), we measured the organic functional group composition of submicron aerosol particles sampled from the 10-m inlet from April 2012 to October 2014. The sampling site is approximately 10 km from the Alert station, and vehicle traffic is restricted except when filter sampling is stopped, making the impact of local emissions on submicron particle mass concentrations small. The organic functional group (OFG) composition is measured by Fourier Transform Infrared spectroscopy of samples collected on pre-loaded Teflon filters and stored and shipped frozen to La Jolla, California, for analysis. Samples were collected weekly to complement the twice hourly online measurements of non-refractory organic and inorganic composition by an Aerodyne ACSM. Organic components are shown to contribute a substantial fraction of the measured aerosol submicron mass year round. These measurements illustrate the seasonal contributions to the aerosol size distribution from OFG and illustrate the potential sources of the OFG at this remote site. The three largest OFG sources are transported fossil fuel combustion emissions from lower latitudes, sea spray and other marine particles, and episodic contributions from wildfires, volcanoes, and other high-latitude events. These sources are similar to those identified from earlier OFG measurements at Barrow, Alaska, and during the ICEALOT cruise in the Arctic Ocean.

A Miniature Aerosol Sensor for Detecting Polydisperse Airborne Ultrafine Particles

PubMed Central

Zhang, Chao; Wang, Dingqu; Zhu, Rong; Yang, Wenming; Jiang, Peng

2017-01-01

Counting and sizing of polydisperse airborne nanoparticles have attracted most attentions owing to increasing widespread presence of airborne engineered nanoparticles or ultrafine particles. Here we report a miniature aerosol sensor to detect particle size distribution of polydisperse ultrafine particles based on ion diffusion charging and electrical detection. The aerosol sensor comprises a couple of planar electrodes printed on two circuit boards assembled in parallel, where charging, precipitation and measurement sections are integrated into one chip, which can detect aerosol particle size in of 30–500 nm, number concentration in range of 5 × 102–5 × 107 /cm3. The average relative errors of the measured aerosol number concentration and the particle size are estimated to be 12.2% and 13.5% respectively. A novel measurement scheme is proposed to actualize a real-time detection of polydisperse particles by successively modulating the measurement voltage and deducing the particle size distribution through a smart data fusion algorithm. The effectiveness of the aerosol sensor is experimentally demonstrated via measurements of polystyrene latex (PSL) aerosol and nucleic acid aerosol, as well as sodium chloride aerosol particles. PMID:28441740

Volatility-resolved Measurements of the Chemical Composition of Arctic Aerosol Particles

NASA Astrophysics Data System (ADS)

Ehn, M.; Kroll, J.; Coffman, D.; Quinn, P.; Bates, T.; Williams, E.; Kulmala, M.; Worsnop, D.

2008-12-01

Here we describe measurements of the chemical composition of submicron particles in the Arctic marine boundary layer, taken on board the R/V Knorr during the IPY-ICEALOT mission (March-April 2008). Measurements were made with an Aerodyne high-resolution aerosol mass spectrometer (HR-AMS) for the measurement of the non-refractory fraction of the aerosol, in particular allowing for the determination of the oxygen/carbon (O/C) ratio of the particulate organics and the unambiguous identification of trace inorganic species. Sampling alternated between ambient air and air sent through a thermodenuder (TD), continually scanned between 50 and 250C in order to remove aerosol components by volatility. The mass spectra of particulate matter in the Arctic (including Arctic haze) were dominated by sulfur-containing peaks and the CO2+ ion (at m/z 44), indicating the main non-refractory components of the aerosol are acidic sulfate and highly oxygenated organics. Thermodenuder measurements allow for the clear speciation of sulfate compounds by volatility, as well as the comparison of the degree of atmospheric aging of the organics to measurements taken elsewhere (including at terrestrial sites). AMS measurements will be compared to results from a hygroscopicity tandem differential mobility analyzer (HTDMA), also downstream of the thermodenuder, as well as from semicontinuous (PILS) and offline (filter) measurements of particle composition.

ANALYSIS OF RESPIRATORY DEPOSITION OF INHALED PARTICLES FOR DIFFERENT DOSE METRICS: COMPARISON OF NUMBER, SURFACE AREA AND MASS DOSE OF TYPICAL AMBIENT BI-MODAL AEROSOLS

EPA Science Inventory

ANALYSIS OF RESPIRATORY DEPOSITION OF INHALED PARTICLES FOR DIFFERENT DOSE METRICS: COMPARISON OF NUMBER, SURFACE AREA AND MASS DOSE OF TYPICAL AMBIENT BI-MODAL AEROSOLS.
Chong S. Kim, SC. Hu*, PA Jaques*, US EPA, National Health and Environmental Effects Research Laboratory, ...

Reactive uptake of HOCl to laboratory generated sea salt particles and nascent sea-spray aerosol

NASA Astrophysics Data System (ADS)

Campbell, N. R.; Ryder, O. S.; Bertram, T. H.

2013-12-01

Field observations suggest that the reactive uptake of HOCl on marine aerosol particles is an important source of chlorine radicals, particularly under low NOx conditions. However to date, laboratory measurements disagree on the magnitude of the reactive uptake coefficient for HOCl by a factor of 5 (γ(HOCl) ranges between 0.0004 and 0.0018), and there are no measurements of γ(HOCl) on nascent sea-spray aerosol. Here, we present measurements of the reactive uptake of HOCl to laboratory generated sodium chloride and sea-spray aerosol particles generated in a novel Marine Aerosol Reference Tank (MART), coupled to an entrained aerosol flow reactor and Chemical Ionization Mass Spectrometer (CIMS). Measurements of γ(HOCl) retrieved here are compared against those in the literature, and the role of organic coatings on nascent sea-spray aerosol is explored.

Single-Particle Measurements of Midlatitude Black Carbon and Light-Scattering Aerosols from the Boundary Layer to the Lower Stratosphere

NASA Technical Reports Server (NTRS)

Schwartz, J. P.; Gao, R. S.; Fahey, D. W.; Thomson, D. S.; Watts, L. A.; Wilson, J. C.; Reeves, J. M.; Darbeheshti, M.; Baumgardner, D. G.; Kok, G. L.;

Selection of quasi-monodisperse super-micron aerosol particles

NASA Astrophysics Data System (ADS)

Rösch, Michael; Pfeifer, Sascha; Wiedensohler, Alfred; Stratmann, Frank

2014-05-01

Size-segregated quasi monodisperse particles are essential for e.g. fundamental research concerning cloud microphysical processes. Commonly a DMA (Differential Mobility Analyzer) is used to produce quasi-monodisperse submicron particles. Thereto first, polydisperse aerosol particles are bipolarly charged by a neutralizer, and then selected according to their electrical mobility with the DMA [Knutson et al. 1975]. Selecting a certain electrical mobility with a DMA results in a particle size distribution, which contains singly charged particles as well as undesired multiply charged larger particles. Often these larger particles need to either be removed from the generated aerosol or their signals have to be corrected for in the data inversion and interpretation process. This problem becomes even more serious when considering super-micron particles. Here we will present two different techniques for generating quasi-monodisperse super-micron aerosol particles with no or only an insignificant number of larger sized particles being present. First, we use a combination of a cyclone with adjustable aerodynamic cut-off diameter and our custom-built Maxi-DMA [Raddatz et al. 2013]. The cyclone removes particles larger than the desired ones prior to mobility selection with the DMA. This results in a reduction of the number of multiply charged particles of up to 99.8%. Second, we utilize a new combination of cyclone and PCVI (Pumped Counterflow Virtual Impactor), which is based on purely inertial separation and avoids particle charging. The PCVI instrument was previously described by Boulter et al. (2006) and Kulkarni et al. (2011). With our two setups we are able to produce quasi-monodisperse aerosol particles in the diameter range from 0.5 to 4.4 µm without a significant number of larger undesired particles being present. Acknowledgements: This work was done within the framework of the DFG funded Ice Nucleation research UnIT (INUIT, FOR 1525) under WE 4722/1-1. References

Accelerated simulation of stochastic particle removal processes in particle-resolved aerosol models

DOE Office of Scientific and Technical Information (OSTI.GOV)

Curtis, J.H.; Michelotti, M.D.; Riemer, N.

2016-10-01

Stochastic particle-resolved methods have proven useful for simulating multi-dimensional systems such as composition-resolved aerosol size distributions. While particle-resolved methods have substantial benefits for highly detailed simulations, these techniques suffer from high computational cost, motivating efforts to improve their algorithmic efficiency. Here we formulate an algorithm for accelerating particle removal processes by aggregating particles of similar size into bins. We present the Binned Algorithm for particle removal processes and analyze its performance with application to the atmospherically relevant process of aerosol dry deposition. We show that the Binned Algorithm can dramatically improve the efficiency of particle removals, particularly for low removalmore » rates, and that computational cost is reduced without introducing additional error. In simulations of aerosol particle removal by dry deposition in atmospherically relevant conditions, we demonstrate about 50-times increase in algorithm efficiency.« less

Direct Measurements of Gas/Particle Partitioning and Mass Accommodation Coefficients in Environmental Chambers.

PubMed

Krechmer, Jordan E; Day, Douglas A; Ziemann, Paul J; Jimenez, Jose L

2017-10-17

Secondary organic aerosols (SOA) are a major contributor to fine particulate mass and wield substantial influences on the Earth's climate and human health. Despite extensive research in recent years, many of the fundamental processes of SOA formation and evolution remain poorly understood. Most atmospheric aerosol models use gas/particle equilibrium partitioning theory as a default treatment of gas-aerosol transfer, despite questions about potentially large kinetic effects. We have conducted fundamental SOA formation experiments in a Teflon environmental chamber using a novel method. A simple chemical system produces a very fast burst of low-volatility gas-phase products, which are competitively taken up by liquid organic seed particles and Teflon chamber walls. Clear changes in the species time evolution with differing amounts of seed allow us to quantify the particle uptake processes. We reproduce gas- and aerosol-phase observations using a kinetic box model, from which we quantify the aerosol mass accommodation coefficient (α) as 0.7 on average, with values near unity especially for low volatility species. α appears to decrease as volatility increases. α has historically been a very difficult parameter to measure with reported values varying over 3 orders of magnitude. We use the experimentally constrained model to evaluate the correction factor (Φ) needed for chamber SOA mass yields due to losses of vapors to walls as a function of species volatility and particle condensational sink. Φ ranges from 1-4.

Single-particle speciation of alkylamines in ambient aerosol at five European sites.

PubMed

Healy, Robert M; Evans, Greg J; Murphy, Michael; Sierau, Berko; Arndt, Jovanna; McGillicuddy, Eoin; O'Connor, Ian P; Sodeau, John R; Wenger, John C

2015-08-01

Alkylamines are associated with both natural and anthropogenic sources and have been detected in ambient aerosol in a variety of environments. However, little is known about the ubiquity or relative abundance of these species in Europe. In this work, ambient single-particle mass spectra collected at five sampling sites across Europe have been analysed for their alkylamine content. The aerosol time-of-flight mass spectrometer (ATOFMS) data used were collected in Ireland (Cork), France (Paris, Dunkirk and Corsica) and Switzerland (Zurich) between 2008 and 2013. Each dataset was queried for mass spectral marker ions associated with the following ambient alkylamines: dimethylamine (DMA), trimethylamine (TMA), diethylamine (DEA), triethylamine (TEA), dipropylamine (DPA) and tripropylamine (TPA). The fraction of ambient particles that contained detectable alkylamines ranged from 1 to 17 % depending on location, with the highest fractions observed in Paris and Zurich in the winter months. The lowest fractions were observed at coastal sites, where the influence of animal husbandry-related alkylamine emissions is also expected to be lowest. TMA was the most ubiquitous particle phase alkylamine detected and was observed at all locations. Alkylamines were found to be internally mixed with both sulphate and nitrate for each dataset, suggesting that aminium salt formation may be important at all sites investigated. Interestingly, in Corsica, all alkylamine particles detected were also found to be internally mixed with methanesulphonic acid (MSA), indicating that aminium methanesulphonate salts may represent a component of marine ambient aerosol in the summer months. Internal mixing of alkylamines with sea salt was not observed, however. Alkylamine-containing particle composition was found to be reasonably homogeneous at each location, with the exception of the Corsica and Dunkirk sites, where two and four distinct mixing states were observed, respectively.

Dispersion of aerosol particles undergoing Brownian motion

NASA Astrophysics Data System (ADS)

Alonso, Manuel; Endo, Yoshiyuki

2001-12-01

The variance of the position distribution for a Brownian particle is derived in the general case where the particle is suspended in a flowing medium and, at the same time, is acted upon by an external field of force. It is shown that, for uniform force and flow fields, the variance is equal to that for a free particle. When the force field is not uniform but depends on spatial location, the variance can be larger or smaller than that for a free particle depending on whether the average motion of the particles takes place toward, respectively, increasing or decreasing absolute values of the field strength. A few examples concerning aerosol particles are discussed, with especial attention paid to the mobility classification of charged aerosols by a non-uniform electric field. As a practical application of these ideas, a new design of particle-size electrostatic classifier differential mobility analyser (DMA) is proposed in which the aerosol particles migrate between the electrodes in a direction opposite to that for a conventional DMA, thereby improving the resolution power of the instrument.

Wintertime hygroscopicity and volatility of ambient urban aerosol particles

NASA Astrophysics Data System (ADS)

Enroth, Joonas; Mikkilä, Jyri; Németh, Zoltán; Kulmala, Markku; Salma, Imre

2018-04-01

Hygroscopic and volatile properties of atmospheric aerosol particles with dry diameters of (20), 50, 75, 110 and 145 nm were determined in situ by using a volatility-hygroscopicity tandem differential mobility analyser (VH-TDMA) system with a relative humidity of 90 % and denuding temperature of 270 °C in central Budapest during 2 months in winter 2014-2015. The probability density function of the hygroscopic growth factor (HGF) showed a distinct bimodal distribution. One of the modes was characterised by an overall mean HGF of approximately 1.07 (this corresponds to a hygroscopicity parameter κ of 0.033) independently of the particle size and was assigned to nearly hydrophobic (NH) particles. Its mean particle number fraction was large, and it decreased monotonically from 69 to 41 % with particle diameter. The other mode showed a mean HGF increasing slightly from 1.31 to 1.38 (κ values from 0.186 to 0.196) with particle diameter, and it was attributed to less hygroscopic (LH) particles. The mode with more hygroscopic particles was not identified. The probability density function of the volatility GF (VGF) also exhibited a distinct bimodal distribution with an overall mean VGF of approximately 0.96 independently of the particle size, and with another mean VGF increasing from 0.49 to 0.55 with particle diameter. The two modes were associated with less volatile (LV) and volatile (V) particles. The mean particle number fraction for the LV mode decreased from 34 to 21 % with particle diameter. The bimodal distributions indicated that the urban atmospheric aerosol contained an external mixture of particles with a diverse chemical composition. Particles corresponding to the NH and LV modes were assigned mainly to freshly emitted combustion particles, more specifically to vehicle emissions consisting of large mass fractions of soot likely coated with or containing some water-insoluble organic compounds such as non-hygroscopic hydrocarbon-like organics. The hygroscopic

Humidity influence on gas-particle phase partitioning of α-pinene + O3 secondary organic aerosol

NASA Astrophysics Data System (ADS)

Prisle, N. L.; Engelhart, G. J.; Bilde, M.; Donahue, N. M.

2010-01-01

Water vapor uptake to particles could potentially affect organic-aerosol mass in three ways: first, water in the organic phase could reduce organic (equilibrium) partial pressures according to Raoult's law; second, an aqueous phase could attract water soluble organics according to Henry's law; finally, deliquescence of inorganic particle cores could mix the organic and inorganic particle phases, significantly diluting the organics and again reducing organic partial pressures according to Raoult's law. We present experiments using initially dry α-pinene + ozone secondary organic aerosol (SOA) on ammonium sulfate (AS) seeds at atmospheric concentrations in a smog chamber. After SOA formation, the chamber relative humidity is increased steadily by addition of steam to near 100%. Little subsequent SOA mass growth is observed, suggesting that none of these potential effects play a strong role in this system.

Influence of air mass origin on aerosol properties at a remote Michigan forest site

NASA Astrophysics Data System (ADS)

VanReken, T. M.; Mwaniki, G. R.; Wallace, H. W.; Pressley, S. N.; Erickson, M. H.; Jobson, B. T.; Lamb, B. K.

2015-04-01

The northern Great Lakes region of North America is a large, relatively pristine area. To date, there has only been limited study of the atmospheric aerosol in this region. During summer 2009, a detailed characterization of the atmospheric aerosol was conducted at the University of Michigan Biological Station (UMBS) as part of the Community Atmosphere-Biosphere Interactions Experiment (CABINEX). Measurements included particle size distribution, water-soluble composition, and CCN activity. Aerosol properties were strongly dependent on the origin of the air masses reaching the site. For ∼60% of the study period, air was transported from sparsely populated regions to the northwest. During these times aerosol loadings were low, with mean number and volume concentrations of 1630 cm-3 and 1.91 μm3 cm-3, respectively. The aerosol during clean periods was dominated by organics, and exhibited low hygroscopicities (mean κ = 0.18 at s = 0.3%). When air was from more populated regions to the east and south (∼29% of the time), aerosol properties reflected a stronger anthropogenic influence, with 85% greater particle number concentrations, 2.5 times greater aerosol volume, six times more sulfate mass, and increased hygroscopicity (mean к = 0.24 at s = 0.3%). These trends are have the potential to influence forest-atmosphere interactions and should be targeted for future study.

Influence of air mass origin on aerosol properties at a remote Michigan forest site

DOE PAGES

VanReken, T. M.; Mwaniki, G. R.; Wallace, H. W.; ...

2015-02-10

The northern Great Lakes region of North America is a large, relatively pristine area. To date, there has only been limited study of the atmospheric aerosol in this region. During summer 2009, a detailed characterization of the atmospheric aerosol was conducted at the University of Michigan Biological Station (UMBS) as part of the Community Atmosphere–Biosphere Interactions Experiment (CABINEX). Measurements included particle size distribution, water-soluble composition, and CCN activity. Aerosol properties were strongly dependent on the origin of the air masses reaching the site. For ~60% of the study period, air was transported from sparsely populated regions to the northwest. Duringmore » these times aerosol loadings were low, with mean number and volume concentrations of 1630 cm -3 and 1.91 μm 3 cm -3, respectively. The aerosol during clean periods was dominated by organics, and exhibited low hygroscopicities (mean κ = 0.18 at s = 0.3%). When air was from more populated regions to the east and south (~29% of the time), aerosol properties reflected a stronger anthropogenic influence, with 85% greater particle number concentrations, 2.5 times greater aerosol volume, six times more sulfate mass, and increased hygroscopicity (mean к = 0.24 at s = 0.3%). Furthermore, these trends are have the potential to influence forest–atmosphere interactions and should be targeted for future study.« less

Fluorescence lifetime imaging of optically levitated aerosol: a technique to quantitatively map the viscosity of suspended aerosol particles.

PubMed

Fitzgerald, C; Hosny, N A; Tong, H; Seville, P C; Gallimore, P J; Davidson, N M; Athanasiadis, A; Botchway, S W; Ward, A D; Kalberer, M; Kuimova, M K; Pope, F D

2016-08-21

We describe a technique to measure the viscosity of stably levitated single micron-sized aerosol particles. Particle levitation allows the aerosol phase to be probed in the absence of potentially artefact-causing surfaces. To achieve this feat, we combined two laser based techniques: optical trapping for aerosol particle levitation, using a counter-propagating laser beam configuration, and fluorescent lifetime imaging microscopy (FLIM) of molecular rotors for the measurement of viscosity within the particle. Unlike other techniques used to measure aerosol particle viscosity, this allows for the non-destructive probing of viscosity of aerosol particles without interference from surfaces. The well-described viscosity of sucrose aerosol, under a range of relative humidity conditions, is used to validate the technique. Furthermore we investigate a pharmaceutically-relevant mixture of sodium chloride and salbutamol sulphate under humidities representative of in vivo drug inhalation. Finally, we provide a methodology for incorporating molecular rotors into already levitated particles, thereby making the FLIM/optical trapping technique applicable to real world aerosol systems, such as atmospheric aerosols and those generated by pharmaceutical inhalers.

The Life Cycle of Stratospheric Aerosol Particles

NASA Technical Reports Server (NTRS)

Hamill, Patrick; Jensen, Eric J.; Russell, P. B.; Bauman, Jill J.

1997-01-01

This paper describes the life cycle of the background (nonvolcanic) stratospheric sulfate aerosol. The authors assume the particles are formed by homogeneous nucleation near the tropical tropopause and are carried aloft into the stratosphere. The particles remain in the Tropics for most of their life, and during this period of time a size distribution is developed by a combination of coagulation, growth by heteromolecular condensation, and mixing with air parcels containing preexisting sulfate particles. The aerosol eventually migrates to higher latitudes and descends across isentropic surfaces to the lower stratosphere. The aerosol is removed from the stratosphere primarily at mid- and high latitudes through various processes, mainly by isentropic transport across the tropopause from the stratosphere into the troposphere.

Aerosol and CCN properties at Princess Elisabeth station, East Antarctica: seasonality, new particle formation events and properties around precipitation events

NASA Astrophysics Data System (ADS)

Mangold, Alexander; Laffineur, Quentin; De Backer, Hugo; Herenz, Paul; Wex, Heike; Gossart, Alexandra; Souverijns, Niels; Gorodetskaya, Irina; Van Lipzig, Nicole

2016-04-01

Since 2010, several complementary ground-based instruments for measuring the aerosol composition of the Antarctic atmosphere have been operated at the Belgian Antarctic research station Princess Elisabeth, in Dronning Maud Land, East Antarctica (71.95° S, 23.35° E, 1390 m asl.). In addition, three ground-based remote sensing instruments for cloud and precipitation observations have been installed for continuous operation, including a ceilometer (cloud base height, type, vertical extent), a 24 Ghz micro-rain radar (vertical profiles of radar effective reflectivity and Doppler velocity), and a pyrometer (cloud base temperature). The station is inhabited from November to end of February and operates under remote control during the other months. In this contribution, the general aerosol and cloud condensation nuclei (CCN) properties will be described with a special focus on new particle formation events and around precipitation events. New particle formation events are important for the atmospheric aerosol budget and they also show that aerosols are not only transported to Antarctica but are also produced there, also inland. Aerosols are essential for cloud formation and therefore also for precipitation, which is the only source for mass gain of the Antarctic ice sheet. Measured aerosol properties comprise size distribution, total number, total mass concentration, mass concentration of light-absorbing aerosol and absorption coefficient and total scattering coefficient. In addition, a CCN counter has been operated during austral summers 2013/14, 2014/15 and 2015/16. The baseline total number concentration N-total was around some hundreds of particles/cm3. During new particle formation events N-total increased to some thousands of particles/cm3. Simultaneous measurements of N-total, size distribution and CCN number revealed that mostly the number of particles smaller than 100 nm increased and that the concentration of cloud condensation nuclei increased only very

Comparison of the DiSCmini aerosol monitor to a handheld condensation particle counter and a scanning mobility particle sizer for submicrometer sodium chloride and metal aerosols

PubMed Central

Mills, Jessica B.; Park, Jae Hong; Peters, Thomas M.

2016-01-01

We evaluated the robust, lightweight DiSCmini (DM) aerosol monitor for its ability to measure the concentration and mean diameter of submicrometer aerosols. Tests were conducted with monodispersed and polydispersed aerosols composed of two particle types (sodium chloride, NaCl, and spark generated metal particles, which simulate particles found in welding fume) at three different steady-state concentration ranges (Low, <103; Medium, 103–104; and High, >104 particles/cm3). Particle number concentration, lung deposited surface area (LDSA) concentration, and mean size measured with the DM were compared to those measured with reference instruments, a scanning mobility particle sizer (SMPS) and a handheld condensation particle counter (CPC). Particle number concentrations measured with the DM were within 21% of those measured by reference instruments for polydisperse aerosols. Poorer agreement was observed for monodispersed aerosols (±35% for most tests and +130% for 300-nm NaCl). LDSA concentrations measured by the DM were 96% to 155% of those estimated with the SMPS. The geometric mean diameters measured with the DM were within 30% of those measured with the SMPS for monodispersed aerosols and within 25% for polydispersed aerosols (except for the case when the aerosol contained a substantial number of particles larger than 300 nm). The accuracy of the DM is reasonable for particles smaller than 300 nm but caution should be exercised when particles larger than 300 nm are present. PMID:23473056

Deposition of biomass combustion aerosol particles in the human respiratory tract.

PubMed

Löndahl, Jakob; Pagels, Joakim; Boman, Christoffer; Swietlicki, Erik; Massling, Andreas; Rissler, Jenny; Blomberg, Anders; Bohgard, Mats; Sandström, Thomas

2008-08-01

Smoke from biomass combustion has been identified as a major environmental risk factor associated with adverse health effects globally. Deposition of the smoke particles in the lungs is a crucial factor for toxicological effects, but has not previously been studied experimentally. We investigated the size-dependent respiratory-tract deposition of aerosol particles from wood combustion in humans. Two combustion conditions were studied in a wood pellet burner: efficient ("complete") combustion and low-temperature (incomplete) combustion simulating "wood smoke." The size-dependent deposition fraction of 15-to 680-nm particles was measured for 10 healthy subjects with a novel setup. Both aerosols were extensively characterized with regard to chemical and physical particle properties. The deposition was additionally estimated with the ICRP model, modified for the determined aerosol properties, in order to validate the experiments and allow a generalization of the results. The measured total deposited fraction of particles from both efficient combustion and low-temperature combustion was 0.21-0.24 by number, surface, and mass. The deposition behavior can be explained by the size distributions of the particles and by their ability to grow by water uptake in the lungs, where the relative humidity is close to saturation. The experiments were in basic agreement with the model calculations. Our findings illustrate: (1) that particles from biomass combustion obtain a size in the respiratory tract at which the deposition probability is close to its minimum, (2) that particle water absorption has substantial impact on deposition, and (3) that deposition is markedly influenced by individual factors.

Aerosol particle properties in a South American megacity

NASA Astrophysics Data System (ADS)

Ulke, Ana; Torres-Brizuela, Marcela; Raga, Graciela; Baumgardner, Darrel; Cancelada, Marcela

2015-04-01

The subtropical city of Buenos Aires is located on the western shore of Río de la Plata, on the southeastern coast of Argentina. It is the second largest metropolitan area in South America, with a population density of around 14 thousand people per km2. When all 24 counties of the Great Buenos Aires Metropolitan Area are included it is the third-largest conurbation in Latin America, with a population of around fifteen million inhabitants. The generalized worldwide trend to concentrate human activities in urban regions that continue to expand in area, threatens the local and regional environment. Air pollution in the Buenos Aires airshed is due to local sources (mainly the mobile sources, followed by the electric power plants and some industries) and to distant sources (like biomass burning, dust, marine aerosols and occasionally volcanic ash) whose products arrive in the city area due to the regional transport patterns. Previous research suggests that ambient aerosol particle concentrations should be considered an air quality problem. A field campaign was conducted in Buenos Aires in 2011 in order to characterize some aerosol particles properties measured for the first time in the city. Measurements began in mid- April and continued until December. The field observations were done in a collaborative effort between the Universities of Mexico (UNAM) and Buenos Aires (UBA). A suite of instruments was installed on the roof of an UBA laboratory and classroom buildings (34.54° S, 58.44° W) at an altitude of approximately 30 m above sea level. The measurements included the number concentration of condensation nuclei (CN) larger than approximately 50 nm, the mass concentration of particle-bound polycyclic aromatic hydrocarbons (PPAH), the scattering (Bscat) and absorption (Babs) coefficients at 550 nm and the vertical profiles of backscattered light from aerosols at a wavelength of 910 nm using a ceilometer. In addition, a weather station recorded the meteorological

Enhancing non-refractory aerosol apportionment from an urban industrial site through receptor modeling of complete high time-resolution aerosol mass spectra

NASA Astrophysics Data System (ADS)

McGuire, M. L.; Chang, R. Y.-W.; Slowik, J. G.; Jeong, C.-H.; Healy, R. M.; Lu, G.; Mihele, C.; Abbatt, J. P. D.; Brook, J. R.; Evans, G. J.

2014-08-01

Receptor modeling was performed on quadrupole unit mass resolution aerosol mass spectrometer (Q-AMS) sub-micron particulate matter (PM) chemical speciation measurements from Windsor, Ontario, an industrial city situated across the Detroit River from Detroit, Michigan. Aerosol and trace gas measurements were collected on board Environment Canada's Canadian Regional and Urban Investigation System for Environmental Research (CRUISER) mobile laboratory. Positive matrix factorization (PMF) was performed on the AMS full particle-phase mass spectrum (PMFFull MS) encompassing both organic and inorganic components. This approach compared to the more common method of analyzing only the organic mass spectra (PMFOrg MS). PMF of the full mass spectrum revealed that variability in the non-refractory sub-micron aerosol concentration and composition was best explained by six factors: an amine-containing factor (Amine); an ammonium sulfate- and oxygenated organic aerosol-containing factor (Sulfate-OA); an ammonium nitrate- and oxygenated organic aerosol-containing factor (Nitrate-OA); an ammonium chloride-containing factor (Chloride); a hydrocarbon-like organic aerosol (HOA) factor; and a moderately oxygenated organic aerosol factor (OOA). PMF of the organic mass spectrum revealed three factors of similar composition to some of those revealed through PMFFull MS: Amine, HOA and OOA. Including both the inorganic and organic mass proved to be a beneficial approach to analyzing the unit mass resolution AMS data for several reasons. First, it provided a method for potentially calculating more accurate sub-micron PM mass concentrations, particularly when unusual factors are present, in this case the Amine factor. As this method does not rely on a priori knowledge of chemical species, it circumvents the need for any adjustments to the traditional AMS species fragmentation patterns to account for atypical species, and can thus lead to more complete factor profiles. It is expected that this

Enhancing non-refractory aerosol apportionment from an urban industrial site through receptor modelling of complete high time-resolution aerosol mass spectra

NASA Astrophysics Data System (ADS)

McGuire, M. L.; Chang, R. Y.-W.; Slowik, J. G.; Jeong, C.-H.; Healy, R. M.; Lu, G.; Mihele, C.; Abbatt, J. P. D.; Brook, J. R.; Evans, G. J.

2014-02-01

Receptor modelling was performed on quadrupole unit mass resolution aerosol mass spectrometer (Q-AMS) sub-micron particulate matter (PM) chemical speciation measurements from Windsor, Ontario, an industrial city situated across the Detroit River from Detroit, Michigan. Aerosol and trace gas measurements were collected on board Environment Canada's CRUISER mobile laboratory. Positive matrix factorization (PMF) was performed on the AMS full particle-phase mass spectrum (PMFFull MS) encompassing both organic and inorganic components. This approach was compared to the more common method of analysing only the organic mass spectra (PMFOrg MS). PMF of the full mass spectrum revealed that variability in the non-refractory sub-micron aerosol concentration and composition was best explained by six factors: an amine-containing factor (Amine); an ammonium sulphate and oxygenated organic aerosol containing factor (Sulphate-OA); an ammonium nitrate and oxygenated organic aerosol containing factor (Nitrate-OA); an ammonium chloride containing factor (Chloride); a hydrocarbon-like organic aerosol (HOA) factor; and a moderately oxygenated organic aerosol factor (OOA). PMF of the organic mass spectrum revealed three factors of similar composition to some of those revealed through PMFFull MS: Amine, HOA and OOA. Including both the inorganic and organic mass proved to be a beneficial approach to analysing the unit mass resolution AMS data for several reasons. First, it provided a method for potentially calculating more accurate sub-micron PM mass concentrations, particularly when unusual factors are present, in this case, an Amine factor. As this method does not rely on a priori knowledge of chemical species, it circumvents the need for any adjustments to the traditional AMS species fragmentation patterns to account for atypical species, and can thus lead to more complete factor profiles. It is expected that this method would be even more useful for HR-ToF-AMS data, due to the ability

Aerosol particle mixing state, refractory particle number size distributions and emission factors in a polluted urban environment: Case study of Metro Manila, Philippines

NASA Astrophysics Data System (ADS)

Kecorius, Simonas; Madueño, Leizel; Vallar, Edgar; Alas, Honey; Betito, Grace; Birmili, Wolfram; Cambaliza, Maria Obiminda; Catipay, Grethyl; Gonzaga-Cayetano, Mylene; Galvez, Maria Cecilia; Lorenzo, Genie; Müller, Thomas; Simpas, James B.; Tamayo, Everlyn Gayle; Wiedensohler, Alfred

2017-12-01

Ultrafine soot particles (black carbon, BC) in urban environments are related to adverse respiratory and cardiovascular effects, increased cases of asthma and premature deaths. These problems are especially pronounced in developing megacities in South-East Asia, Latin America, and Africa, where unsustainable urbanization ant outdated environmental protection legislation resulted in severe degradation of urban air quality in terms of black carbon emission. Since ultrafine soot particles do often not lead to enhanced PM10 and PM2.5 mass concentration, the risks related to ultrafine particle pollution may therefore be significantly underestimated compared to the contribution of secondary aerosol constituents. To increase the awareness of the potential toxicological relevant problems of ultrafine black carbon particles, we conducted a case study in Metro Manila, the capital of the Philippines. Here, we present a part of the results from a detailed field campaign, called Manila Aerosol Characterization Experiment (MACE, 2015). Measurements took place from May to June 2015 with the focus on the state of mixing of aerosol particles. The results were alarming, showing the abundance of externally mixed refractory particles (soot proxy) at street site with a maximum daily number concentration of approximately 15000 #/cm3. That is up to 10 times higher than in cities of Western countries. We also found that the soot particle mass contributed from 55 to 75% of total street site PM2.5. The retrieved refractory particle number size distribution appeared to be a superposition of 2 ultrafine modes at 20 and 80 nm with a corresponding contribution to the total refractory particle number of 45 and 55%, respectively. The particles in the 20 nm mode were most likely ash from metallic additives in lubricating oil, tiny carbonaceous particles and/or nucleated and oxidized organic polymers, while bigger ones (80 nm) were soot agglomerates. To the best of the authors' knowledge, no other

The generation of diesel exhaust particle aerosols from a bulk source in an aerodynamic size range similar to atmospheric particles

PubMed Central

Cooney, Daniel J; Hickey, Anthony J

2008-01-01

The influence of diesel exhaust particles (DEP) on the lungs and heart is currently a topic of great interest in inhalation toxicology. Epidemiological data and animal studies have implicated airborne particulate matter and DEP in increased morbidity and mortality due to a number of cardiopulmonary diseases including asthma, chronic obstructive pulmonary disorder, and lung cancer. The pathogeneses of these diseases are being studied using animal models and cell culture techniques. Real-time exposures to freshly combusted diesel fuel are complex and require significant infrastructure including engine operations, dilution air, and monitoring and control of gases. A method of generating DEP aerosols from a bulk source in an aerodynamic size range similar to atmospheric DEP would be a desirable and useful alternative. Metered dose inhaler technology was adopted to generate aerosols from suspensions of DEP in the propellant hydrofluoroalkane 134a. Inertial impaction data indicated that the particle size distributions of the generated aerosols were trimodal, with count median aerodynamic diameters less than 100 nm. Scanning electron microscopy of deposited particles showed tightly aggregated particles, as would be expected from an evaporative process. Chemical analysis indicated that there were no major changes in the mass proportion of 2 specific aromatic hydrocarbons (benzo[a]pyrene and benzo[k]fluoranthene) in the particles resulting from the aerosolization process. PMID:19337412

Polarization resolved angular optical scattering of aerosol particles

NASA Astrophysics Data System (ADS)

Redding, B.; Pan, Y.; Wang, C.; Videen, G.; Cao, Hui

2014-05-01

Real-time detection and identification of bio-aerosol particles are crucial for the protection against chemical and biological agents. The strong elastic light scattering properties of airborne particles provides a natural means for rapid, non-invasive aerosol characterization. Recent theoretical predictions suggested that variations in the polarization dependent angular scattering cross section could provide an efficient means of classifying different airborne particles. In particular, the polarization dependent scattering cross section of aggregate particles is expected to depend on the shape of the primary particles. In order to experimentally validate this prediction, we built a high throughput, sampling system, capable of measuring the polarization resolved angular scattering cross section of individual aerosol particles flowing through an interrogating volume with a single shot of laser pulse. We calibrated the system by comparing the polarization dependent scattering cross section of individual polystyrene spheres with that predicted by Mie theory. We then used the system to study different particles types: Polystyrene aggregates composed 500 nm spheres and Bacillus subtilis (BG, Anthrax simulant) spores composed of elongated 500 nm × 1000 nm cylinder-line particles. We found that the polarization resolved scattering cross section depends on the shape of the constituent elements of the aggregates. This work indicates that the polarization resolved scattering cross section could be used for rapid discrimination between different bio-aerosol particles.

Coupling a versatile aerosol apparatus to a synchrotron: Vacuum ultraviolet light scattering, photoelectron imaging, and fragment free mass spectrometry

NASA Astrophysics Data System (ADS)

Shu, Jinian; Wilson, Kevin R.; Ahmed, Musahid; Leone, Stephen R.

2006-04-01

An aerosol apparatus has been coupled to the Chemical Dynamics Beamline of the Advanced Light Source at Lawrence Berkeley National Laboratory. This apparatus has multiple capabilities for aerosol studies, including vacuum ultraviolet (VUV) light scattering, photoelectron imaging, and mass spectroscopy of aerosols. By utilizing an inlet system consisting of a 200μm orifice nozzle and aerodynamic lenses, aerosol particles of ˜50nm-˜1μm in diameter can be sampled directly from atmospheric pressure. The machine is versatile and can probe carbonaceous aerosols generated by a laboratory flame, nebulized solutions of biological molecules, hydrocarbon aerosol reaction products, and synthesized inorganic nanoparticles. The sensitivity of this apparatus is demonstrated by the detection of nanoparticles with VUV light scattering, photoelectron imaging, and charged particle detection. In addition to the detection of nanoparticles, the thermal vaporization of aerosols on a heater tip leads to the generation of intact gas phase molecules. This phenomenon coupled to threshold single photon ionization, accessible with tunable VUV light, allows for fragment-free mass spectrometry of complex molecules. The initial experiments with light scattering, photoelectron imaging, and aerosol mass spectrometry reported here serve as a demonstration of the design philosophy and multiple capabilities of the apparatus.

Individual aerosol particles in and below clouds along a Mt. Fuji slope: Modification of sea-salt-containing particles by in-cloud processing

NASA Astrophysics Data System (ADS)

Ueda, S.; Hirose, Y.; Miura, K.; Okochi, H.

2014-02-01

Sizes and compositions of atmospheric aerosol particles can be altered by in-cloud processing by absorption/adsorption of gaseous and particulate materials and drying of aerosol particles that were formerly activated as cloud condensation nuclei. To elucidate differences of aerosol particles before and after in-cloud processing, aerosols were observed along a slope of Mt. Fuji, Japan (3776 m a.s.l.) during the summer in 2011 and 2012 using a portable laser particle counter (LPC) and an aerosol sampler. Aerosol samples for analyses of elemental compositions were obtained using a cascade impactor at top-of-cloud, in-cloud, and below-cloud altitudes. To investigate composition changes via in-cloud processing, individual particles (0.5-2 μm diameter) of samples from five cases (days) collected at different altitudes under similar backward air mass trajectory conditions were analyzed using a transmission electron microscope (TEM) equipped with an energy dispersive X-ray analyzer. For most cases (four cases), most particles at all altitudes mainly comprised sea salts: mainly Na with some S and/or Cl. Of those, in two cases, sea-salt-containing particles with Cl were found in below-cloud samples, although sea-salt-containing particles in top-of-cloud samples did not contain Cl. This result suggests that Cl in the sea salt was displaced by other cloud components. In the other two cases, sea-salt-containing particles on samples at all altitudes were without Cl. However, molar ratios of S to Na (S/Na) of the sea-salt-containing particles of top-of-cloud samples were higher than those of below-cloud samples, suggesting that sulfuric acid or sulfate was added to sea-salt-containing particles after complete displacement of Cl by absorption of SO2 or coagulation with sulfate. The additional volume of sulfuric acid in clouds for the two cases was estimated using the observed S/Na values of sea-salt-containing particles. The estimation revealed that size changes by in

Characterization of aerosol composition, concentrations, and sources at Baengnyeong Island, Korea using an aerosol mass spectrometer

NASA Astrophysics Data System (ADS)

Lee, Taehyoung; Choi, Jinsoo; Lee, Gangwoong; Ahn, Junyoung; Park, Jin Soo; Atwood, Samuel A.; Schurman, Misha; Choi, Yongjoo; Chung, Yoomi; Collett, Jeffrey L.

2015-11-01

To improve understanding of the sources and chemical properties of particulate pollutants on the western side of the Korean Peninsula, an Aerodyne High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS) measured non-refractory fine (PM1) particles from May to November, 2011 at Baengnyeong Island, South Korea. Organic matter and sulfate were generally the most abundant species and exhibited maximum concentrations of 36 μg/m3 and 39 μg/m3, respectively. Nitrate concentrations peaked at 32 μg/m3 but were typically much lower than sulfate and organic matter concentrations. May, September, October, and November featured the highest monthly average concentrations, with lower concentrations typically observed from June through August. Potential source contribution function (PSCF) analysis and individual case studies revealed that transport from eastern China, an area with high SO2 emissions, was associated with high particulate sulfate concentrations at the measurement site. Observed sulfate aerosol sometimes was fully neutralized by ammonium but often was acidic; the average ammonium to sulfate molar ratio was 1.49. Measured species size distributions revealed a range of sulfate particle size distributions with modes between 100 and 600 nm. Organic aerosol source regions were widespread, including contributions from eastern China and South Korea. Positive matrix factorization (PMF) analysis indicated three "factors," or types of organic aerosol, comprising one primary, hydrocarbon-like organic aerosol (HOA) and two oxidized organic aerosol (OOA) components, including a more oxidized (MO-OOA) and a less oxidized (LO-OOA) oxidized organic aerosol. On average, HOA and OOA contributed 21% and 79% of the organic mass (OM), respectively, with the MO-OOA fraction nearly three times as abundant as the LO-OOA fraction. Biomass burning contributions to observed OM were low during the late spring/early summer agricultural burning season in eastern China, since

Hygroscopic growth of size-resolved, emission-source classified, aerosol particles sampled across the United States

NASA Astrophysics Data System (ADS)

Shingler, T.; Crosbie, E. C.; Ziemba, L. D.; Anderson, B. E.; Campuzano Jost, P.; Jimenez, J. L.; Mikoviny, T.; Wisthaler, A.; Sorooshian, A.

2014-12-01

The hygroscopic growth of atmospheric aerosol particles is a key air quality parameter, impacting the radiation budget, visibility, and cloud formation. During the DC3 and SEAC4RS field campaigns (>300 total flight hours), measurements were made over 32 US states, Canada, the Pacific Ocean, and the Gulf of Mexico, between the surface and 41,000 feet ASL. The aircraft research payloads included a suite of in-situ aerosol and gas phase instruments. The Differential Aerosol Sizing and Hygroscopicity Spectrometer Probe (DASH-SP) and the Langley Aerosol Research Group Experiment (LARGE) humidified nephelometer instrument applied different techniques to measure water uptake by aerosol particles at prescribed relative humidity values. Size-resolved growth factor (GF ≡ Dp,wet/Dp,dry) measurements by the DASH-SP are compared to bulk scattering measurements (f(RH) ≡ σscat,wet/σscat,dry) by the LARGE instrument. Spatial location and volatile organic compound tracers such as isoprene and acetonitrile are used to classify the origin of distinct air masses, including: forest fires, biogenic-emitting forests, agricultural use lands, marine boundary layer, urban, and rural background. Analyses of GF results by air mass origin are reported and results are compared with f(RH) measurements. A parameterization between the f(RH) and GF measurements and its potential uses are discussed.

Microphysical and optical properties of aerosol particles in urban zone during ESCOMPTE

NASA Astrophysics Data System (ADS)

Mallet, M.; Roger, J. C.; Despiau, S.; Dubovik, O.; Putaud, J. P.

2003-10-01

Microphysical and optical properties of the main aerosol species on a peri-urban site have been investigated during the ESCOMPTE experiment. Ammonium sulfate (AS), nitrate (N), black carbon (BC), particulate organic matter (POM), sea salt (SS) and mineral aerosol (D) size distributions have been used, associated with their refractive index, to compute, from the Mie theory, the key radiative aerosol properties as the extinction coefficient Kext, the mass extinction efficiencies σext, the single scattering albedo ω0 and the asymmetry parameter g at the wavelength of 550 nm. Optical computations show that 90% of the light extinction is due to anthropogenic aerosol and only 10% is due to natural aerosol (SS and D). 44±6% of the extinction is due to (AS) and 40±6% to carbonaceous particles (20±4% to BC and 21±4% to POM). Nitrate aerosol has a weak contribution of 5±2%. Computations of the mass extinction efficiencies σext, single scattering albedo ω0 and asymmetry parameter g indicate that the optical properties of the anthropogenic aerosol are often quite different from those yet published and generally used in global models. For example, the (AS) mean specific mass extinction presents a large difference with the value classically adopted at low relative humidity ( h<60%) (2.6±0.5 instead of 6 m 2 g -1 at 550 nm). The optical properties of the total aerosol layer, including all the aerosol species, indicate a mean observed single-scattering albedo ω0=0.85±0.05, leading to an important absorption of the solar radiation and an asymmetry parameter g=0.59±0.05 which are in a reasonably good agreements with the AERONET retrieval of ω0 (=0.86±0.05) and g (=0.64±0.05) at this wavelength.

Single-particle characterization of biomass burning organic aerosol (BBOA): evidence for non-uniform mixing of high molecular weight organics and potassium

NASA Astrophysics Data System (ADS)

Lee, Alex K. Y.; Willis, Megan D.; Healy, Robert M.; Wang, Jon M.; Jeong, Cheol-Heon; Wenger, John C.; Evans, Greg J.; Abbatt, Jonathan P. D.

2016-05-01

Biomass burning organic aerosol (BBOA) can be emitted from natural forest fires and human activities such as agricultural burning and domestic energy generation. BBOA is strongly associated with atmospheric brown carbon (BrC) that absorbs near-ultraviolet and visible light, resulting in significant impacts on regional visibility degradation and radiative forcing. The mixing state of BBOA can play a critical role in the prediction of aerosol optical properties. In this work, single-particle measurements from a Soot-Particle Aerosol Mass Spectrometer coupled with a light scattering module (LS-SP-AMS) were performed to examine the mixing state of BBOA, refractory black carbon (rBC), and potassium (K, a tracer for biomass burning aerosol) in an air mass influenced by wildfire emissions transported from northern Québec to Toronto, representing aged biomass burning plumes. Cluster analysis of single-particle measurements identified five BBOA-related particle types. rBC accounted for 3-14 wt % of these particle types on average. Only one particle type exhibited a strong ion signal for K+, with mass spectra characterized by low molecular weight organic species. The remaining four particle types were classified based on the apparent molecular weight of the BBOA constituents. Two particle types were associated with low potassium content and significant amounts of high molecular weight (HMW) organic compounds. Our observations indicate non-uniform mixing of particles within a biomass burning plume in terms of molecular weight and illustrate that HMW BBOA can be a key contributor to low-volatility BrC observed in BBOA particles. The average mass absorption efficiency of low-volatility BBOA is about 0.8-1.1 m2 g-1 based on a theoretical closure calculation. Our estimates indicate that low-volatility BBOA contributes ˜ 33-44 % of thermo-processed particle absorption at 405 nm; and almost all of the BBOA absorption was associated with low-volatility organics.

An aerosol particle containing enriched uranium encountered during routine sampling

NASA Astrophysics Data System (ADS)

Murphy, Daniel; Froyd, Karl; Evangeliou, NIkolaos; Stohl, Andreas

2017-04-01

The composition of single aerosol particles has been measured using a laser ionization mass spectrometer during the global Atmospheric Tomography mission. The measurements were targeting the background atmosphere, not radiochemical emissions. One sub-micron particle sampled at about 7 km altitude near the Aleutian Islands contained uranium with approximately 3% 235U. It is the only particle with enriched uranium out of millions of particles sampled over several decades of measurements with this instrument. The particle also contained vanadium, alkali metals, and organic material similar to that present in emissions from combustion of heavy oil. No zirconium or other metals that might be characteristic of nuclear reactors were present, probably suggesting a source other than Fukushima or Chernobyl. Back trajectories suggest several areas in Asia that might be sources for the particle.

Impact of aerosol size representation on modeling aerosol-cloud interactions

DOE PAGES

Zhang, Y.; Easter, R. C.; Ghan, S. J.; ...

2002-11-07

In this study, we use a 1-D version of a climate-aerosol-chemistry model with both modal and sectional aerosol size representations to evaluate the impact of aerosol size representation on modeling aerosol-cloud interactions in shallow stratiform clouds observed during the 2nd Aerosol Characterization Experiment. Both the modal (with prognostic aerosol number and mass or prognostic aerosol number, surface area and mass, referred to as the Modal-NM and Modal-NSM) and the sectional approaches (with 12 and 36 sections) predict total number and mass for interstitial and activated particles that are generally within several percent of references from a high resolution 108-section approach.more » The modal approach with prognostic aerosol mass but diagnostic number (referred to as the Modal-M) cannot accurately predict the total particle number and surface areas, with deviations from the references ranging from 7-161%. The particle size distributions are sensitive to size representations, with normalized absolute differences of up to 12% and 37% for the 36- and 12-section approaches, and 30%, 39%, and 179% for the Modal-NSM, Modal-NM, and Modal-M, respectively. For the Modal-NSM and Modal-NM, differences from the references are primarily due to the inherent assumptions and limitations of the modal approach. In particular, they cannot resolve the abrupt size transition between the interstitial and activated aerosol fractions. For the 12- and 36-section approaches, differences are largely due to limitations of the parameterized activation for non-log-normal size distributions, plus the coarse resolution for the 12-section case. Differences are larger both with higher aerosol (i.e., less complete activation) and higher SO2 concentrations (i.e., greater modification of the initial aerosol distribution).« less

Aerosol volatility in a boreal forest environment

NASA Astrophysics Data System (ADS)

Häkkinen, S. A. K.; ńijälä, M.; Lehtipalo, K.; Junninen, H.; Virkkula, A.; Worsnop, D. R.; Kulmala, M.; Petäjä, T.; Riipinen, I.

2012-04-01

Climate and health effects of atmospheric aerosols are determined by their properties such as their chemical composition. Aerosol chemical composition can be studied indirectly by measuring volatility of aerosol particles. The volatility of submicron aerosol particles (20-500 nm) was studied in a boreal forest site at SMEAR II (Station for Measuring Ecosystem-Atmosphere Relations II) station (Vesala et al., 1998) in Hyytiälä, Finland, during 01/2008-05/2010. The instrument used for the measurements was VDMPS (Volatility Differential Mobility Particle Sizer), which consists of two separate instruments: DMPS (Differential Mobility Particle Sizer, Aalto et al., 2001) and TD (Thermodenuder, Wehner et al., 2002). Aerosol evaporation was examined by heating the aerosol and comparing the total aerosol mass before and after heating. In the VDMPS system ambient aerosol sample was heated up to temperatures ranging from 80 °C to 280 °C. The higher the heating temperature was the more aerosol material was evaporated. There was a non-volatile residual present in aerosol particles when heated up to 280 °C. This residual explained (20±8)% of the total aerosol mass. Aerosol non-volatile mass fraction was highest during winter and smallest during summer months. The role of black carbon in the observed non-volatile residual was determined. Black carbon explained 40 to 90% of the non-volatile mass. Especially during colder seasons noticeable amount of non-volatile material, something else than black carbon, was observed. According to Kalberer et al. (2004) some atmospheric organic species can form polymers that have high evaporation temperatures. Also low-volatile organic salts may contribute to the non-volatile aerosol (Smith et al., 2010). Aerosol mass composition measured directly with AMS (Aerosol Mass Spectrometer, Jayne et al., 2000) was analyzed in order to examine the properties of the non-volatile material (other than black carbon). The AMS measurements were performed

SAM-CAAM: A Concept for Acquiring Systematic Aircraft Measurements to Characterize Aerosol Air Masses.

PubMed

Kahn, Ralph A; Berkoff, Tim A; Brock, Charles; Chen, Gao; Ferrare, Richard A; Ghan, Steven; Hansico, Thomas F; Hegg, Dean A; Martins, J Vanderlei; McNaughton, Cameron S; Murphy, Daniel M; Ogren, John A; Penner, Joyce E; Pilewskie, Peter; Seinfeld, John H; Worsnop, Douglas R

2017-10-01

A modest operational program of systematic aircraft measurements can resolve key satellite-aerosol-data-record limitations. Satellite observations provide frequent, global aerosol-amount maps, but offer only loose aerosol property constraints needed for climate and air quality applications. We define and illustrate the feasibility of flying an aircraft payload to measure key aerosol optical, microphysical, and chemical properties in situ . The flight program could characterize major aerosol air-mass types statistically, at a level-of-detail unobtainable from space. It would: (1) enhance satellite aerosol retrieval products with better climatology assumptions, and (2) improve translation between satellite-retrieved optical properties and species-specific aerosol mass and size simulated in climate models to assess aerosol forcing, its anthropogenic components, and other environmental impacts. As such, Systematic Aircraft Measurements to Characterize Aerosol Air Masses (SAM-CAAM) could add value to data records representing several decades of aerosol observations from space, improve aerosol constraints on climate modeling , help interrelate remote-sensing, in situ, and modeling aerosol-type definitions , and contribute to future satellite aerosol missions. Fifteen Required Variables are identified, and four Payload Options of increasing ambition are defined, to constrain these quantities. "Option C" could meet all the SAM-CAAM objectives with about 20 instruments, most of which have flown before, but never routinely several times per week, and never as a group. Aircraft integration, and approaches to data handling, payload support, and logistical considerations for a long-term, operational mission are discussed. SAM-CAAM is feasible because, for most aerosol sources and specified seasons, particle properties tend to be repeatable , even if aerosol loading varies.

A size-composition resolved aerosol model for simulating the dynamics of externally mixed particles: SCRAM (v 1.0)

NASA Astrophysics Data System (ADS)

Zhu, S.; Sartelet, K. N.; Seigneur, C.

2015-06-01

The Size-Composition Resolved Aerosol Model (SCRAM) for simulating the dynamics of externally mixed atmospheric particles is presented. This new model classifies aerosols by both composition and size, based on a comprehensive combination of all chemical species and their mass-fraction sections. All three main processes involved in aerosol dynamics (coagulation, condensation/evaporation and nucleation) are included. The model is first validated by comparison with a reference solution and with results of simulations using internally mixed particles. The degree of mixing of particles is investigated in a box model simulation using data representative of air pollution in Greater Paris. The relative influence on the mixing state of the different aerosol processes (condensation/evaporation, coagulation) and of the algorithm used to model condensation/evaporation (bulk equilibrium, dynamic) is studied.

Condensation Kinetics of Water on Amorphous Aerosol Particles.

PubMed

Rothfuss, Nicholas E; Marsh, Aleksandra; Rovelli, Grazia; Petters, Markus D; Reid, Jonathan P

2018-06-25

Responding to changes in the surrounding environment, aerosol particles can grow by water condensation changing rapidly in composition and changing dramatically in viscosity. The timescale for growth is important to establish for particles undergoing hydration processes in the atmosphere or during inhalation. Using an electrodynamic balance, we report direct measurements at -7.5, 0, and 20 °C of timescales for hygroscopic condensational growth on a range of model hygroscopic aerosol systems. These extend from viscous aerosol particles containing a single saccharide solute (sucrose, glucose, raffinose, or trehalose) and a starting viscosity equivalent to a glass of ∼10 12 Pa·s, to nonviscous (∼10 -2 Pa·s) tetraethylene glycol particles. The condensation timescales observed in this work indicate that water condensation occurs rapidly at all temperatures examined (<10 s) and for particles of all initial viscosities spanning 10 -2 to 10 12 Pa·s. Only a marginal delay (<1 order of magnitude) is observed for particles starting as a glass.

α-Pinene secondary organic aerosol at low temperature: chemical composition and implications for particle viscosity

NASA Astrophysics Data System (ADS)

Huang, Wei; Saathoff, Harald; Pajunoja, Aki; Shen, Xiaoli; Naumann, Karl-Heinz; Wagner, Robert; Virtanen, Annele; Leisner, Thomas; Mohr, Claudia

2018-02-01

Chemical composition, size distributions, and degree of oligomerization of secondary organic aerosol (SOA) from α-pinene (C10H16) ozonolysis were investigated for low-temperature conditions (223 K). Two types of experiments were performed using two simulation chambers at the Karlsruhe Institute of Technology: the Aerosol Preparation and Characterization (APC) chamber, and the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) chamber. Experiment type 1 simulated SOA formation at upper tropospheric conditions: SOA was generated in the AIDA chamber directly at 223 K at 61 % relative humidity (RH; experiment termed cold humid, CH) and for comparison at 6 % RH (experiment termed cold dry, CD) conditions. Experiment type 2 simulated SOA uplifting: SOA was formed in the APC chamber at room temperature (296 K) and < 1 % RH (experiment termed warm dry, WD) or 21 % RH (experiment termed warm humid, WH) conditions, and then partially transferred to the AIDA chamber kept at 223 K, and 61 % RH (WDtoCH) or 30 % RH (WHtoCH), respectively. Precursor concentrations varied between 0.7 and 2.2 ppm α-pinene, and between 2.3 and 1.8 ppm ozone for type 1 and type 2 experiments, respectively. Among other instrumentation, a chemical ionization mass spectrometer (CIMS) coupled to a filter inlet for gases and aerosols (FIGAERO), deploying I- as reagent ion, was used for SOA chemical composition analysis. For type 1 experiments with lower α-pinene concentrations and cold SOA formation temperature (223 K), smaller particles of 100-300 nm vacuum aerodynamic diameter (dva) and higher mass fractions (> 40 %) of adducts (molecules with more than 10 carbon atoms) of α-pinene oxidation products were observed. For type 2 experiments with higher α-pinene concentrations and warm SOA formation temperature (296 K), larger particles ( ˜ 500 nm dva) with smaller mass fractions of adducts (< 35 %) were produced. We also observed differences (up to 20 °C) in

Application of FIGAERO (Filter Inlet for Gases and AEROsol) coupled to a high resolution time of flight chemical ionization mass spectrometer to field and chamber organic aerosol: Implications for carboxylic acid formation and gas-particle partitioning from monoterpene oxidation

NASA Astrophysics Data System (ADS)

Lopez-Hilfiker, F.; Mohr, C.; Ehn, M.; Rubach, F.; Mentel, T. F.; Kleist, E.; Wildt, J.; Thornton, J. A.

2013-12-01

We present measurements of a large suite of gas and particle phase carboxylic acid containing compounds made with a Filter Inlet for Gas and AEROsol (FIGAERO) coupled to a high resolution time of flight chemical ionization mass spectrometer (HR-ToF-CIMS) developed at the University of Washington. A prototype operated with acetate negative ion proton transfer chemistry was deployed on the Julich Plant Atmosphere Chamber to study a-pinene oxidation, and a modified version was deployed at the SMEAR II forest station in Hyytiälä, Finland and SOAS, in Brent Alabama. We focus here on results from JPAC and Hyytiälä, where we utilized the same ionization method most selective towards carboxylic acids. In all locations, 100's of organic acid compounds were observed in the gas and particles and many of the same composition acids detected in the gas-phase were detected in the particles upon temperature programmed thermal desorption. Particulate organics detected by FIGAERO are highly correlated with organic aerosol mass measured by an AMS, providing additional volatility and molecular level information about collected aerosol. The fraction of a given compound measured in the particle phase follows expected trends with elemental composition, but many compounds would not be well described by an absorptive partitioning model assuming unity activity coefficients. Moreover the detailed structure in the thermal desorption signals reveals a contribution from thermal decomposition of large molecular weight organics and or oligomers with implications for partitioning measurements and model validation

New aerosol particles formation in the Sao Paulo Metropolitan Area

NASA Astrophysics Data System (ADS)

Vela, Angel; Andrade, Maria de Fatima; Ynoue, Rita

2016-04-01

The Sao Paulo Metropolitan Area (SPMA), in the southeast region of Brazil, is considered a megalopolis comprised of Sao Paulo city and more 38 municipalities. The air pollutant emissions in the SPMA are related to the burning of the fuels: etanol, gasohol (gasoline with 25% ethanol) and diesel. According to CETESB (2013), the road vehicles contributed up to about 97, 87, and 80% of CO, VOCs and NOx emissions in 2012, respectively, being most of NOx associated to diesel combustion and most of CO and VOCs from gasohol and ethanol combustion. Studies conducted on ambient air pollution in the SPMA have shown that black carbon (BC) explains 21% of mass concentration of PM2.5 compared with 40% of organic carbon (OC), 20% of sulfates, and 12% of soil dust (Andrade et al., 2012). Most of the observed ambient PM2.5 mass concentration usually originates from precursors gases such as sulphur dioxide (SO2), ammonia (NH3), nitrogen oxides (NOx) and VOCs as well as through the physico-chemical processes such as the oxidation of low volatile hydrocarbons transferring to the condensed phase (McMurry et al., 2004). The Weather Research and Forecasting with Chemistry model (WRF-Chem; Grell et al. 2005), configured with three nested grid cells: 75, 15, and 3 km, is used as photochemical modeling to describe the physico-chemical processes leading to evolution of particles number and mass size distribution from a vehicular emission model developed by the IAG-USP laboratory of Atmospheric Processes and based on statistical information of vehicular activity. The spatial and temporal distributions of emissions in the finest grid cell are based on road density products compiled by the OpenStreetMap project and measurements performed inside tunnels in the SPMA, respectively. WRF-Chem simulation with coupled primary aerosol (dust and sea-salt) and biogenic emission modules and aerosol radiative effects turned on is conducted as the baseline simulation (Case_0) to evaluate the model

Rapid Measurements of Aerosol Ionic Composition and 3-10 nm Particle Size Distributions On The NASA P3 To Better Quantify Processes Affecting Aerosols Advected From East Asia

NASA Technical Reports Server (NTRS)

Weber, Rodney J.

2004-01-01

The Particle Into Liquid Sample (PILS) was deployed on the NASA P3 for airborne measurements of fine particle ionic chemical composition. The data have been quality assured and reside in the NASA data archive. We have analyzed our data to characterize the sources and atmospheric processing of fine aerosol particles advected from the region during the experiments. Fine particle water-soluble potassium was found to serve as a useful aerosol tracer for biomass smoke. Ratios of PILS potassium to sulfate are used as a means of estimating the percent contribution of biomass burning to fine particle mass in mixed plumes advecting from Asia. The high correlations between K+ and NO3(sup -) and NH4(sup +)' indicated that biomass burning was a significant source of these aerosol compounds in the region. It is noteworthy that the air mass containing the highest concentrations of fine particles recorded in all of ACE-Asia and TRACE-P appeared to be advecting from the Bejing/Tientsin urban region and also had the highest K(+), NO3(sup -) and NH4(sup +) concentrations of both studies. Based on K+/SO4(sup 2-) ratio's, we estimated that the plume was composed of approx. 60% biomass burning emissions, possibly from the use of bio-fuels in the urban regions.

Solid versus Liquid Particle Sampling Efficiency of Three Personal Aerosol Samplers when Facing the Wind

PubMed Central

Koehler, Kirsten A.; Anthony, T. Renee; Van Dyke, Michael

2016-01-01

The objective of this study was to examine the facing-the-wind sampling efficiency of three personal aerosol samplers as a function of particle phase (solid versus liquid). Samplers examined were the IOM, Button, and a prototype personal high-flow inhalable sampler head (PHISH). The prototype PHISH was designed to interface with the 37-mm closed-face cassette and provide an inhalable sample at 10 l min−1 of flow. Increased flow rate increases the amount of mass collected during a typical work shift and helps to ensure that limits of detection are met, particularly for well-controlled but highly toxic species. Two PHISH prototypes were tested: one with a screened inlet and one with a single-pore open-face inlet. Personal aerosol samplers were tested on a bluff-body disc that was rotated along the facing-the-wind axis to reduce spatiotemporal variability associated with sampling supermicron aerosol in low-velocity wind tunnels. When compared to published data for facing-wind aspiration efficiency for a mouth-breathing mannequin, the IOM oversampled relative to mannequin facing-the-wind aspiration efficiency for all sizes and particle types (solid and liquid). The sampling efficiency of the Button sampler was closer to the mannequin facing-the-wind aspiration efficiency than the IOM for solid particles, but the screened inlet removed most liquid particles, resulting in a large underestimation compared to the mannequin facing-the-wind aspiration efficiency. The open-face PHISH results showed overestimation for solid particles and underestimation for liquid particles when compared to the mannequin facing-the-wind aspiration efficiency. Substantial (and statistically significant) differences in sampling efficiency were observed between liquid and solid particles, particularly for the Button and screened-PHISH, with a majority of aerosol mass depositing on the screened inlets of these samplers. Our results suggest that large droplets have low penetration efficiencies

Single-particle Analyses of Compositions, Morphology, and Viscosity of Aerosol Particles Collected During GoAmazon2014

NASA Astrophysics Data System (ADS)

Adachi, K.; Gong, Z.; Bateman, A. P.; Martin, S. T.; Cirino, G. G.; Artaxo, P.; Sedlacek, A. J., III; Buseck, P. R.

2014-12-01

Single-particle analysis using transmission electron microscopy (TEM) shows composition and morphology of individual aerosol particles collected during the GoAmazon2014 campaign. These TEM results indicate aerosol types and mixing states, both of which are important for evaluating particle optical properties and cloud condensation nuclei activity. The samples were collected at the T3 site, which is located in the Amazon forest with influences from the urban pollution plume from Manaus. Samples were also collected from the T0 site, which is in the middle of the jungle with minimal to no influences of anthropogenic sources. The aerosol particles mainly originated from 1) anthropogenic pollution (e.g., nanosphere soot, sulfate), 2) biogenic emissions (e.g., primary biogenic particles, organic aerosols), and 3) long-range transport (e.g., sea salts). We found that the biogenic organic aerosol particles contain homogeneously distributed potassium. Particle viscosity is important for evaluating gas-particle interactions and atmospheric chemistry for the particles. Viscosity can be estimated from the rebounding behavior at controlled relative humidities, i.e., highly viscous particles display less rebound on a plate than low-viscosity particles. We collected 1) aerosol particles from a plate (non-rebounded), 2) those that had rebounded from the plate and were then captured onto an adjacent sampling plate, and 3) particles from ambient air using a separate impactor sampler. Preliminary results show that more than 90% of non-rebounded particles consisted of nanosphere soot with or without coatings. The coatings mostly consisted of organic matter. Although rebounded particles also contain nanosphere soot (number fraction 64-69%), they were mostly internally mixed with sulfate, organic matter, or their mixtures. TEM tilted images suggested that the rebounded particles were less deformed on the substrate, whereas the non-rebounded particles were more deformed, which could

Distinct high molecular weight organic compound (HMW-OC) types in aerosol particles collected at a coastal urban site

NASA Astrophysics Data System (ADS)

Dall'Osto, M.; Healy, R. M.; Wenger, J. C.; O'Dowd, C.; Ovadnevaite, J.; Ceburnis, D.; Harrison, Roy M.; Beddows, D. C. S.

2017-12-01

Organic oligomers were discovered in laboratory-generated atmospheric aerosol over a decade ago. However, evidence for the presence of oligomers in ambient aerosols is scarce and mechanisms for their formation have yet to be fully elucidated. In this work, three unique aerosol particle types internally mixed with High molecular weight organic compounds (HMW-OC) species - likely oligomers - were detected in ambient air using single particle Aerosol Time-Of-Flight Mass Spectrometry (ATOFMS) in Cork (Ireland) during winter 2009. These particle types can be described as follows: (1) HMW-OCs rich in organic nitrogen - possibly containing nitrocatechols and nitroguaiacols - originating from primary emissions of biomass burning particles during evening times; (2) HMW-OCs internally mixed with nitric acid, occurring in stagnant conditions during night time; and (3) HMW-OCs internally mixed with sea salt, likely formed via photochemical reactions during day time. The study exemplifies the power of methodologies capable of monitoring the simultaneous formation of organic and inorganic particle-phase reaction products. Primary emissions and atmospheric aging of different types of HMW-OC contributes to aerosol with a range of acidity, hygroscopic and optical properties, which can have different impacts on climate and health.

Laser Ablation-Aerosol Mass Spectrometry-Chemical Ionization Mass Spectrometry for Ambient Surface Imaging

DOE PAGES

Berry, Jennifer L.; Day, Douglas A.; Elseberg, Tim; ...

2018-02-20

Mass spectrometry imaging is becoming an increasingly common analytical technique due to its ability to provide spatially resolved chemical information. In this paper, we report a novel imaging approach combining laser ablation with two mass spectrometric techniques, aerosol mass spectrometry and chemical ionization mass spectrometry, separately and in parallel. Both mass spectrometric methods provide the fast response, rapid data acquisition, low detection limits, and high-resolution peak separation desirable for imaging complex samples. Additionally, the two techniques provide complementary information with aerosol mass spectrometry providing near universal detection of all aerosol molecules and chemical ionization mass spectrometry with a heated inletmore » providing molecular-level detail of both gases and aerosols. The two techniques operate with atmospheric pressure interfaces and require no matrix addition for ionization, allowing for samples to be investigated in their native state under ambient pressure conditions. We demonstrate the ability of laser ablation-aerosol mass spectrometry-chemical ionization mass spectrometry (LA-AMS-CIMS) to create 2D images of both standard compounds and complex mixtures. Finally, the results suggest that LA-AMS-CIMS, particularly when combined with advanced data analysis methods, could have broad applications in mass spectrometry imaging applications.« less

Laser Ablation-Aerosol Mass Spectrometry-Chemical Ionization Mass Spectrometry for Ambient Surface Imaging

DOE Office of Scientific and Technical Information (OSTI.GOV)

Berry, Jennifer L.; Day, Douglas A.; Elseberg, Tim

Mass spectrometry imaging is becoming an increasingly common analytical technique due to its ability to provide spatially resolved chemical information. In this paper, we report a novel imaging approach combining laser ablation with two mass spectrometric techniques, aerosol mass spectrometry and chemical ionization mass spectrometry, separately and in parallel. Both mass spectrometric methods provide the fast response, rapid data acquisition, low detection limits, and high-resolution peak separation desirable for imaging complex samples. Additionally, the two techniques provide complementary information with aerosol mass spectrometry providing near universal detection of all aerosol molecules and chemical ionization mass spectrometry with a heated inletmore » providing molecular-level detail of both gases and aerosols. The two techniques operate with atmospheric pressure interfaces and require no matrix addition for ionization, allowing for samples to be investigated in their native state under ambient pressure conditions. We demonstrate the ability of laser ablation-aerosol mass spectrometry-chemical ionization mass spectrometry (LA-AMS-CIMS) to create 2D images of both standard compounds and complex mixtures. Finally, the results suggest that LA-AMS-CIMS, particularly when combined with advanced data analysis methods, could have broad applications in mass spectrometry imaging applications.« less

Isotope source apportionment of carbonaceous aerosol as a function of particle size and thermal refractiveness

NASA Astrophysics Data System (ADS)

Masalaite, Agne; Holzinger, Rupert; Remeikis, Vidmantas; Röckmann, Thomas; Dusek, Ulrike

2016-04-01

The stable carbon isotopes can be used to get information about sources and processing of carbonaceous aerosol. We will present results from source apportionment of carbonaceous aerosol as a function of particle size thermal refractiveness. Separate source apportionment for particles smaller than 200 nm and for different carbon volatility classes are rarely reported and give new insights into aerosol sources in the urban environment. Stable carbon isotope ratios were measured for the organic carbon (OC) fraction and total carbon (TC) of MOUDI impactor samples that were collected on a coastal site (Lithuania) during the winter 2012 and in the city of Vilnius (Lithuania) during the winter of 2009. The 11 impactor stages spanned a size range from 0.056 to 18 μm, but only the 6 stages in the submicron range were analysed. The δ13C values of bulk total carbon (δ13CTC) were determined with an elemental analyser (Flash EA 1112) coupled with an isotope ratio mass spectrometer (Thermo Finnigan Delta Plus Advantage) (EA - IRMS). Meanwhile δ13COC was measured using thermal-desorption isotope ratio mass spectrometry (IRMS) system. This allows a rough separation of the more volatile OC fraction (desorbed in the oven of IRMS up to 250 0C) from the more refractory fraction (desorbed up to 400 0C). In this study we investigated the composition of organic aerosol desorbed from filter samples at different temperatures using the thermal-desorption proton-transfer-reaction mass spectrometry (TD-PTR-MS) technique. During winter-time in Lithuania we expect photochemistry and biogenic emissions to be of minor importance. The main sources of aerosol carbon should be fossil fuel and biomass combustion. In both sites, the coastal and the urban site, δ13C measurements give a clear indication that the source contributions differ for small and large particles. Small particles < 200 nm are depleted in 13C with respect to larger particles by 1 - 2 ‰Ṫhis shows that OC in small particle

Physical characterization of aerosol particles during the Chinese New Year’s firework events

NASA Astrophysics Data System (ADS)

Zhang, Min; Wang, Xuemei; Chen, Jianmin; Cheng, Tiantao; Wang, Tao; Yang, Xin; Gong, Youguo; Geng, Fuhai; Chen, Changhong

2010-12-01

Measurements for particles 10 nm to 10 μm were taken using a Wide-range Particle Spectrometer during the Chinese New Year (CNY) celebrations in 2009 in Shanghai, China. These celebrations provided an opportunity to study the number concentration and size distribution of particles in an especial atmospheric pollution situation due to firework displays. The firework activities had a clear contribution to the number concentration of small accumulation mode particles (100-500 nm) and PM 1 mass concentration, with a maximum total number concentration of 3.8 × 10 4 cm -3. A clear shift of particles from nucleation and Aitken mode to small accumulation mode was observed at the peak of the CNY firework event, which can be explained by reduced atmospheric lifetimes of smaller particles via the concept of the coagulation sink. High particle density (2.7 g cm -3) was identified as being particularly characteristic of the firework aerosols. Recalculated fine particles PM 1 exhibited on average above 150 μg m -3 for more than 12 hours, which was a health risk to susceptible individuals. Integral physical parameters of firework aerosols were calculated for understanding their physical properties and further model simulation.

On remote sensing of small aerosol particles with polarized light

NASA Astrophysics Data System (ADS)

Sun, W.

2012-12-01

The CALIPSO satellite mission consistently measures volume (including molecule and particulate) light depolarization ratio of ~2% for smoke, compared to ~1% for marine aerosols and ~15% for dust. The observed ~2% smoke depolarization ratio comes primarily from the nonspherical habits of particles in the smoke at certain particle sizes. The depolarization of linearly polarized light by small sphere aggregates and irregular Gaussian-shaped particles is studied, to reveal the physics between the depolarization of linearly polarized light and aerosol shape and size. It is found that randomly oriented nonspherical particles have some common depolarization properties as functions of scattering angle and size parameter. This may be very useful information for active remote sensing of small nonspherical aerosols using polarized light. We also show that the depolarization ratio from the CALIPSO measurements could be used to derive smoke aerosol particle size. The mean particle size of South-African smoke is estimated to be about half of the 532 nm wavelength of the CALIPSO lidar.

The application of single particle aerosol mass spectrometry for the detection and identification of high explosives and chemical warfare agents

DOE Office of Scientific and Technical Information (OSTI.GOV)

Martin, Audrey Noreen

2006-01-01

Single Particle Aerosol Mass Spectrometry (SPAMS) was evaluated as a real-time detection technique for single particles of high explosives. Dual-polarity time-of-flight mass spectra were obtained for samples of 2,4,6-trinitrotoluene (TNT), 1,3,5-trinitro-1,3,5-triazinane (RDX), and pentaerythritol tetranitrate (PETN); peaks indicative of each compound were identified. Composite explosives, Comp B, Semtex 1A, and Semtex 1H were also analyzed, and peaks due to the explosive components of each sample were present in each spectrum. Mass spectral variability with laser fluence is discussed. The ability of the SPAMS system to identify explosive components in a single complex explosive particle (~1 pg) without the need formore » consumables is demonstrated. SPAMS was also applied to the detection of Chemical Warfare Agent (CWA) simulants in the liquid and vapor phases. Liquid simulants for sarin, cyclosarin, tabun, and VX were analyzed; peaks indicative of each simulant were identified. Vapor phase CWA simulants were adsorbed onto alumina, silica, Zeolite, activated carbon, and metal powders which were directly analyzed using SPAMS. The use of metal powders as adsorbent materials was especially useful in the analysis of triethyl phosphate (TEP), a VX stimulant, which was undetectable using SPAMS in the liquid phase. The capability of SPAMS to detect high explosives and CWA simulants using one set of operational conditions is established.« less

Ubiquitous influence of wildfire emissions and secondary organic aerosol on summertime atmospheric aerosol in the forested Great Lakes region

NASA Astrophysics Data System (ADS)

Gunsch, Matthew J.; May, Nathaniel W.; Wen, Miao; Bottenus, Courtney L. H.; Gardner, Daniel J.; VanReken, Timothy M.; Bertman, Steven B.; Hopke, Philip K.; Ault, Andrew P.; Pratt, Kerri A.

2018-03-01

Long-range aerosol transport affects locations hundreds of kilometers from the point of emission, leading to distant particle sources influencing rural environments that have few major local sources. Source apportionment was conducted using real-time aerosol chemistry measurements made in July 2014 at the forested University of Michigan Biological Station near Pellston, Michigan, a site representative of the remote forested Great Lakes region. Size-resolved chemical composition of individual 0.5-2.0 µm particles was measured using an aerosol time-of-flight mass spectrometer (ATOFMS), and non-refractory aerosol mass less than 1 µm (PM1) was measured with a high-resolution aerosol mass spectrometer (HR-AMS). The field site was influenced by air masses transporting Canadian wildfire emissions and urban pollution from Milwaukee and Chicago. During wildfire-influenced periods, 0.5-2.0 µm particles were primarily aged biomass burning particles (88 % by number). These particles were heavily coated with secondary organic aerosol (SOA) formed during transport, with organics (average O/C ratio of 0.8) contributing 89 % of the PM1 mass. During urban-influenced periods, organic carbon, elemental carbon-organic carbon, and aged biomass burning particles were identified, with inorganic secondary species (ammonium, sulfate, and nitrate) contributing 41 % of the PM1 mass, indicative of atmospheric processing. With current models underpredicting organic carbon in this region and biomass burning being the largest combustion contributor to SOA by mass, these results highlight the importance for regional chemical transport models to accurately predict the impact of long-range transported particles on air quality in the upper Midwest, United States, particularly considering increasing intensity and frequency of Canadian wildfires.

Increased absorption by coarse aerosol particles over the Gangetic–Himalayan region

DOE PAGES

Manoharan, Vani Starry; Kotamarthi, R.; Feng, Yan; ...

2014-02-03

Each atmospheric aerosol type has distinctive light-absorption characteristics related to its physical/chemical properties. Climate models treat black carbon as the main light-absorbing component of carbonaceous atmospheric aerosols, while absorption by some organic aerosols is also considered, particularly at ultraviolet wavelengths. Most absorbing aerosols are assumed to be < 1 μm in diameter (sub-micron). Here we present results from a recent field study in India, primarily during the post-monsoon season (October–November), suggesting the presence of absorbing aerosols sized 1–10 μm. Absorption due to super-micron-sized particles was nearly 30% greater than that due to smaller particles. Periods of increased absorption by largermore » particles ranged from a week to a month. Radiative forcing calculations under clear-sky conditions show that super-micron particles account for nearly 44% of the total aerosol forcing. The origin of the large aerosols is unknown, but meteorological conditions indicate that they are of local origin. Such economic and habitation conditions exist throughout much of the developing world. Furthermore, large absorbing particles could be an important component of the regional-scale atmospheric energy balance.« less

Chemical Imaging of Ambient Aerosol Particles: Observational Constraints on Mixing State Parameterization

DOE Office of Scientific and Technical Information (OSTI.GOV)

O'Brien, Rachel; Wang, Bingbing; Laskin, Alexander

2015-09-28

A new parameterization for quantifying the mixing state of aerosol populations has been applied for the first time to samples of ambient particles analyzed using spectro-microscopy techniques. Scanning transmission x-ray microscopy/near edge x-ray absorption fine structure (STXM/NEXAFS) and computer controlled scanning electron microscopy/energy dispersive x-ray spectroscopy (CCSEM/EDX) were used to probe the composition of the organic and inorganic fraction of individual particles collected on June 27th and 28th during the 2010 Carbonaceous Aerosols and Radiative Effects (CARES) study in the Central Valley, California. The first field site, T0, was located in downtown Sacramento, while T1 was located near the Sierramore » Nevada Mountains. Mass estimates of the aerosol particle components were used to calculate mixing state metrics, such as the particle-specific diversity, bulk population diversity, and mixing state index, for each sample. Both microscopy imaging techniques showed more changes over these two days in the mixing state at the T0 site than at the T1 site. The STXM data showed evidence of changes in the mixing state associated with a build-up of organic matter confirmed by collocated measurements and the largest impact on the mixing state was due to an increase in soot dominant particles during this build-up. The CCSEM/EDX analysis showed the presence of two types of particle populations; the first was dominated by aged sea salt particles and had a higher mixing state index (indicating a more homogeneous population), the second was dominated by carbonaceous particles and had a lower mixing state index.« less

Chemical imaging of ambient aerosol particles: Observational constraints on mixing state parameterization

DOE PAGES

O'Brien, Rachel E.; Wang, Bingbing; Laskin, Alexander; ...

2015-08-26

In this study, a new parameterization for quantifying the mixing state of aerosol populations has been applied for the first time to samples of ambient particles analyzed using spectro-microscopy techniques. Scanning transmission X-ray microscopy/near edge X-ray absorption fine structure (STXM/NEXAFS) and computer-controlled scanning electron microscopy/energy dispersive X-ray spectroscopy (CCSEM/EDX) were used to probe the composition of the organic and inorganic fraction of individual particles collected on 27 and 28 June during the 2010 Carbonaceous Aerosols and Radiative Effects study in the Central Valley, California. The first field site, T0, was located in downtown Sacramento, while T1 was located near themore » Sierra Nevada Mountains. Mass estimates of the aerosol particle components were used to calculate mixing state metrics, such as the particle-specific diversity, bulk population diversity, and mixing state index, for each sample. The STXM data showed evidence of changes in the mixing state associated with a buildup of organic matter confirmed by collocated measurements, and the largest impact on the mixing state was due to an increase in soot dominant particles during this buildup. The mixing state from STXM was similar between T0 and T1, indicating that the increased organic fraction at T1 had a small effect on the mixing state of the population. The CCSEM/EDX analysis showed the presence of two types of particle populations: the first was dominated by aged sea-salt particles and had a higher mixing state index (indicating a more homogeneous population); the second was dominated by carbonaceous particles and had a lower mixing state index.« less

Improved Tandem Measurement Techniques for Aerosol Particle Analysis

NASA Astrophysics Data System (ADS)

Rawat, Vivek Kumar

Non-spherical, chemically inhomogeneous (complex) nanoparticles are encountered in a number of natural and engineered environments, including combustion systems (which produces highly non-spherical aggregates), reactors used in gas-phase materials synthesis of doped or multicomponent materials, and in ambient air. These nanoparticles are often highly diverse in size, composition and shape, and hence require determination of property distribution functions for accurate characterization. This thesis focuses on development of tandem mobility-mass measurement techniques coupled with appropriate data inversion routines to facilitate measurement of two dimensional size-mass distribution functions while correcting for the non-idealities of the instruments. Chapter 1 provides the detailed background and motivation for the studies performed in this thesis. In chapter 2, the development of an inversion routine is described which is employed to determine two dimensional size-mass distribution functions from Differential Mobility Analyzer-Aerosol Particle Mass analyzer tandem measurements. Chapter 3 demonstrates the application of the two dimensional distribution function to compute cumulative mass distribution function and also evaluates the validity of this technique by comparing the calculated total mass concentrations to measured values for a variety of aerosols. In Chapter 4, this tandem measurement technique with the inversion routine is employed to analyze colloidal suspensions. Chapter 5 focuses on application of a transverse modulation ion mobility spectrometer coupled with a mass spectrometer to study the effect of vapor dopants on the mobility shifts of sub 2 nm peptide ion clusters. These mobility shifts are then compared to models based on vapor uptake theories. Finally, in Chapter 6, a conclusion of all the studies performed in this thesis is provided and future avenues of research are discussed.

A recirculation aerosol wind tunnel for evaluating aerosol samplers and measuring particle penetration through protective clothing materials.

PubMed

Jaques, Peter A; Hsiao, Ta-Chih; Gao, Pengfei

2011-08-01

A recirculation aerosol wind tunnel was designed to maintain a uniform airflow and stable aerosol size distribution for evaluating aerosol sampler performance and determining particle penetration through protective clothing materials. The oval-shaped wind tunnel was designed to be small enough to fit onto a lab bench, have optimized dimensions for uniformity in wind speed and particle size distributions, sufficient mixing for even distribution of particles, and minimum particle losses. Performance evaluation demonstrates a relatively high level of spatial uniformity, with a coefficient of variation of 1.5-6.2% for wind velocities between 0.4 and 2.8 m s(-1) and, in this range, 0.8-8.5% for particles between 50 and 450 nm. Aerosol concentration stabilized within the first 5-20 min with, approximately, a count median diameter of 135 nm and geometric standard deviation of 2.20. Negligible agglomerate growth and particle loss are suggested. The recirculation design appears to result in unique features as needed for our research.

Online investigations on ozonation products of pyrene and benz[ a]anthracene particles with a vacuum ultraviolet photoionization aerosol time-of-flight mass spectrometer

NASA Astrophysics Data System (ADS)

Gao, Shaokai; Zhang, Yang; Meng, Junwang; Shu, Jinian

The reaction products of ozone with pyrene and benz[ a]anthracene absorbed on azelaic acid particles under the pseudo-first-order reaction conditions have been investigated with a vacuum ultraviolet photoionization aerosol time-of-flight mass spectrometer (VUV-ATOFMS). The pyrene and benz[ a]anthracene particles with the initial concentrations of ˜1 mg m -3 are respectively exposed to ˜22 ppm ozone in a reaction chamber with a volume of ˜180 L. The time-of-flight mass spectra of the particulate ozonides are obtained. The assignments of the mass spectra reveal that 4-carboxy-5-phenanthrene-carboxyaldehyde (71%) and hydroxypyrene (23%) are the main solid state ozonides of pyrene, while 2-(2-formyl)phenyl-3-naphthoic acid (35%), hydroxybenz[ a]anthrone (30%), and benz[ a]anthracene-7,12-dione (18%) are the main solid state ozonides of benz[ a]anthracene. The pathways of the ozonations are proposed in the paper.

Fractal morphology, imaging and mass spectrometry of single aerosol particles in flight (CXIDB ID 16)

DOE Data Explorer

Loh, N. Duane

2012-06-20

This deposition includes the aerosol diffraction images used for phasing, fractal morphology, and time-of-flight mass spectrometry. Files in this deposition are ordered in subdirectories that reflect the specifics.

Introduction of the new concept: Potential Aerosol Mass (PAM) for Inorganic and Organic Secondary Aerosol

NASA Astrophysics Data System (ADS)

Kang, E.; Root, M. J.; Brune, W. H.

2006-12-01

A new concept, the Potential Aerosol Mass (PAM), is being developed and tested in the laboratory with the goal of deploying instruments to measure PAM in the atmosphere. PAM can be defined as the maximum aerosol mass that precursor gases can be oxidized to form. In the PAM concept, all precursor gases are oxidized to low volatile compounds with excessive amount of oxidants in a small continuous-flow Teflon cylinder, resulting in aerosol formation. Excessive amounts of OH and O3 are produced by a UV light that shines into the Teflon chamber. For our studies, the aerosol mass is then detected with a real-time aerosol mass measurement instrument, the Rupprecht and Patashnick Tapered Element Oscillating Microbalance (TEOM) and Filter Dynamic Measurement System (FDMS). As a test of the system, SO2 was oxidized to sulfate; the measured and calculated conversion ratios of sulfate aerosol mass to SO2 mass agree to within 10%. We will discuss the results of a series of laboratory tests that have been conducted with α-pinene to determine the variables that most affect its Secondary Organic Aerosol (SOA) yield. We will also discuss the results of some atmospheric measurement tests made at a site on the Penn State University campus.

Numerical investigation of the coagulation mixing between dust and hygroscopic aerosol particles and its impacts

NASA Astrophysics Data System (ADS)

Tsai, I.-Chun; Chen, Jen-Ping; Lin, Yi-Chiu; Chung-Kuang Chou, Charles; Chen, Wei-Nai

2015-05-01

A statistical-numerical aerosol parameterization was incorporated into the Community Multiscale Air Quality modeling system to study the coagulation mixing process focusing on a dust storm event that occurred over East Asia. Simulation results show that the coagulation mixing process tends to decrease aerosol mass, surface area, and number concentrations over the dust source areas. Over the downwind oceanic areas, aerosol concentrations generally increased due to enhanced sedimentation as particles became larger upon coagulation. The mixture process can reduce the overall single-scattering albedo by up to 10% as a result of enhanced core with shell absorption by dust and reduction in the number of scattering particles. The enhanced dry deposition speed also altered the vertical distribution. In addition, the ability of aerosol particles to serve as cloud condensation nuclei (CCN) increased from around 107 m-3 to above 109 m-3 over downwind areas because a large amount of mineral dust particles became effective CCN with solute coating, except over the highly polluted areas where multiple collections of hygroscopic particles by dust in effect reduced CCN number. This CCN effect is much stronger for coagulation mixing than by the uptake of sulfuric acid gas on dust, although the nitric acid gas uptake was not investigated. The ability of dust particles to serve as ice nuclei may decrease or increase at low or high subzero temperatures, respectively, due to the switching from deposition nucleation to immersion freezing or haze freezing.

Light Absorption of Biogenic Aerosol Particles in Amazonia

NASA Astrophysics Data System (ADS)

Holanda, B. A.; Artaxo, P.; Ferreira De Brito, J.; Barbosa, H. M.; Andreae, M. O.; Saturno, J.; Pöhlker, C.; Holben, B. N.; Schafer, J.

2014-12-01

Aerosol absorption is a key issue in proper calculation of aerosol radiative forcing. Especially in the tropics with the dominance of natural biogenic aerosol and brown carbon, the so called anomalous absorption is of particular interest. A special experiment was designed to study the wavelength dependence of aerosol absorption for PM2.5 as well as for PM10 particles in the wet season in Central Amazonia. Aerosol analysis occurred from May to August 2014, in the ZF2 ecological reservation, situated at about 55 km North of Manaus in very pristine conditions Two 7 wavelengths AE33 Aethalometers were deployed measuring in parallel, but with a PM2.5 and PM10 inlets. Two MAAP (Multiangle Aerosol Absorption Photometer) were operated in parallel with the AE33 exactly at the same PM2.5 and PM10 inlets. Organic and elemental carbon was analyzed using collection with quartz filters and analysis using a Sunset OC/EC analyzer. Aerosol light scattering for 3 wavelengths was measured using Air Photon and TSI Nephelometers. Aerosol size distribution was measured with one TSI SMPS and a GRIMM OPC to have the size range from 10 nm to 10 micrometers. Particles were measured under dry conditions using diffusion dryers. Aerosol optical depth and absorption was also measured with an AERONET sunphotometer operated close to the site. As the experiment was run in the wet season, very low equivalent black carbon (EBC) were measured, with average concentrations around 50 ng/m³ during May, increasing to 130 ng/m³ in June and July. The measurements adjusted for similar wavelengths shows excellent agreement between the MAAP and AE33 for both inlets (PM2.5 and PM10). It was not possible statistically infer absorption from the coarse mode biogenic particles, since the absorption was completely dominated by fine mode particles. AERONET measurements shows very low values of AOD, at 0.17 at 500 nm and 0.13 at 870 nm, with very low absorption AOD values at 0.00086 at 676 nm and 0.0068 at 872 nm

Hygroscopic properties of potassium chloride and its internal mixtures with organic compounds relevant to biomass burning aerosol particles

PubMed Central

Jing, Bo; Peng, Chao; Wang, Yidan; Liu, Qifan; Tong, Shengrui; Zhang, Yunhong; Ge, Maofa

2017-01-01

While water uptake of aerosols exerts considerable impacts on climate, the effects of aerosol composition and potential interactions between species on hygroscopicity of atmospheric particles have not been fully characterized. The water uptake behaviors of potassium chloride and its internal mixtures with water soluble organic compounds (WSOCs) related to biomass burning aerosols including oxalic acid, levoglucosan and humic acid at different mass ratios were investigated using a hygroscopicity tandem differential mobility analyzer (HTDMA). Deliquescence points of KCl/organic mixtures were observed to occur at lower RH values and over a broader RH range eventually disappearing at high organic mass fractions. This leads to substantial under-prediction of water uptake at intermediate RH. Large discrepancies for water content between model predictions and measurements were observed for KCl aerosols with 75 wt% oxalic acid content, which is likely due to the formation of less hygroscopic potassium oxalate from interactions between KCl and oxalic acid without taken into account in the model methods. Our results also indicate strong influence of levoglucosan on hygroscopic behaviors of multicomponent mixed particles. These findings are important in further understanding the role of interactions between WSOCs and inorganic salt on hygroscopic behaviors and environmental effects of atmospheric particles. PMID:28240258

Hygroscopic properties of potassium chloride and its internal mixtures with organic compounds relevant to biomass burning aerosol particles.

PubMed

Jing, Bo; Peng, Chao; Wang, Yidan; Liu, Qifan; Tong, Shengrui; Zhang, Yunhong; Ge, Maofa

2017-02-27

While water uptake of aerosols exerts considerable impacts on climate, the effects of aerosol composition and potential interactions between species on hygroscopicity of atmospheric particles have not been fully characterized. The water uptake behaviors of potassium chloride and its internal mixtures with water soluble organic compounds (WSOCs) related to biomass burning aerosols including oxalic acid, levoglucosan and humic acid at different mass ratios were investigated using a hygroscopicity tandem differential mobility analyzer (HTDMA). Deliquescence points of KCl/organic mixtures were observed to occur at lower RH values and over a broader RH range eventually disappearing at high organic mass fractions. This leads to substantial under-prediction of water uptake at intermediate RH. Large discrepancies for water content between model predictions and measurements were observed for KCl aerosols with 75 wt% oxalic acid content, which is likely due to the formation of less hygroscopic potassium oxalate from interactions between KCl and oxalic acid without taken into account in the model methods. Our results also indicate strong influence of levoglucosan on hygroscopic behaviors of multicomponent mixed particles. These findings are important in further understanding the role of interactions between WSOCs and inorganic salt on hygroscopic behaviors and environmental effects of atmospheric particles.

Hygroscopic properties of potassium chloride and its internal mixtures with organic compounds relevant to biomass burning aerosol particles

NASA Astrophysics Data System (ADS)

Jing, Bo; Peng, Chao; Wang, Yidan; Liu, Qifan; Tong, Shengrui; Zhang, Yunhong; Ge, Maofa

2017-02-01

While water uptake of aerosols exerts considerable impacts on climate, the effects of aerosol composition and potential interactions between species on hygroscopicity of atmospheric particles have not been fully characterized. The water uptake behaviors of potassium chloride and its internal mixtures with water soluble organic compounds (WSOCs) related to biomass burning aerosols including oxalic acid, levoglucosan and humic acid at different mass ratios were investigated using a hygroscopicity tandem differential mobility analyzer (HTDMA). Deliquescence points of KCl/organic mixtures were observed to occur at lower RH values and over a broader RH range eventually disappearing at high organic mass fractions. This leads to substantial under-prediction of water uptake at intermediate RH. Large discrepancies for water content between model predictions and measurements were observed for KCl aerosols with 75 wt% oxalic acid content, which is likely due to the formation of less hygroscopic potassium oxalate from interactions between KCl and oxalic acid without taken into account in the model methods. Our results also indicate strong influence of levoglucosan on hygroscopic behaviors of multicomponent mixed particles. These findings are important in further understanding the role of interactions between WSOCs and inorganic salt on hygroscopic behaviors and environmental effects of atmospheric particles.

Stable Carbon Fractionation In Size Segregated Aerosol Particles Produced By Controlled Biomass Burning

NASA Astrophysics Data System (ADS)

Masalaite, Agne; Garbaras, Andrius; Garbariene, Inga; Ceburnis, Darius; Martuzevicius, Dainius; Puida, Egidijus; Kvietkus, Kestutis; Remeikis, Vidmantas

2014-05-01

Biomass burning is the largest source of primary fine fraction carbonaceous particles and the second largest source of trace gases in the global atmosphere with a strong effect not only on the regional scale but also in areas distant from the source . Many studies have often assumed no significant carbon isotope fractionation occurring between black carbon and the original vegetation during combustion. However, other studies suggested that stable carbon isotope ratios of char or BC may not reliably reflect carbon isotopic signatures of the source vegetation. Overall, the apparently conflicting results throughout the literature regarding the observed fractionation suggest that combustion conditions may be responsible for the observed effects. The purpose of the present study was to gather more quantitative information on carbonaceous aerosols produced in controlled biomass burning, thereby having a potential impact on interpreting ambient atmospheric observations. Seven different biomass fuel types were burned under controlled conditions to determine the effect of the biomass type on the emitted particulate matter mass and stable carbon isotope composition of bulk and size segregated particles. Size segregated aerosol particles were collected using the total suspended particle (TSP) sampler and a micro-orifice uniform deposit impactor (MOUDI). The results demonstrated that particle emissions were dominated by the submicron particles in all biomass types. However, significant differences in emissions of submicron particles and their dominant sizes were found between different biomass fuels. The largest negative fractionation was obtained for the wood pellet fuel type while the largest positive isotopic fractionation was observed during the buckwheat shells combustion. The carbon isotope composition of MOUDI samples compared very well with isotope composition of TSP samples indicating consistency of the results. The measurements of the stable carbon isotope ratio in

Computation of liquid-liquid equilibria and phase stabilities: implications for RH-dependent gas/particle partitioning of organic-inorganic aerosols

NASA Astrophysics Data System (ADS)

Zuend, A.; Marcolli, C.; Peter, T.; Seinfeld, J. H.

2010-08-01

Semivolatile organic and inorganic aerosol species partition between the gas and aerosol particle phases to maintain thermodynamic equilibrium. Liquid-liquid phase separation into an organic-rich and an aqueous electrolyte phase can occur in the aerosol as a result of the salting-out effect. Such liquid-liquid equilibria (LLE) affect the gas/particle partitioning of the different semivolatile compounds and might significantly alter both particle mass and composition as compared to a one-phase particle. We present a new liquid-liquid equilibrium and gas/particle partitioning model, using as a basis the group-contribution model AIOMFAC (Zuend et al., 2008). This model allows the reliable computation of the liquid-liquid coexistence curve (binodal), corresponding tie-lines, the limit of stability/metastability (spinodal), and further thermodynamic properties of multicomponent systems. Calculations for ternary and multicomponent alcohol/polyol-water-salt mixtures suggest that LLE are a prevalent feature of organic-inorganic aerosol systems. A six-component polyol-water-ammonium sulphate system is used to simulate effects of relative humidity (RH) and the presence of liquid-liquid phase separation on the gas/particle partitioning. RH, salt concentration, and hydrophilicity (water-solubility) are identified as key features in defining the region of a miscibility gap and govern the extent to which compound partitioning is affected by changes in RH. The model predicts that liquid-liquid phase separation can lead to either an increase or decrease in total particulate mass, depending on the overall composition of a system and the particle water content, which is related to the hydrophilicity of the different organic and inorganic compounds. Neglecting non-ideality and liquid-liquid phase separations by assuming an ideal mixture leads to an overestimation of the total particulate mass by up to 30% for the composition and RH range considered in the six-component system

Computation of liquid-liquid equilibria and phase stabilities: implications for RH-dependent gas/particle partitioning of organic-inorganic aerosols

NASA Astrophysics Data System (ADS)

Zuend, A.; Marcolli, C.; Peter, T.; Seinfeld, J. H.

2010-05-01

Semivolatile organic and inorganic aerosol species partition between the gas and aerosol particle phases to maintain thermodynamic equilibrium. Liquid-liquid phase separation into an organic-rich and an aqueous electrolyte phase can occur in the aerosol as a result of the salting-out effect. Such liquid-liquid equilibria (LLE) affect the gas/particle partitioning of the different semivolatile compounds and might significantly alter both particle mass and composition as compared to a one-phase particle. We present a new liquid-liquid equilibrium and gas/particle partitioning model, using as a basis the group-contribution model AIOMFAC (Zuend et al., 2008). This model allows the reliable computation of the liquid-liquid coexistence curve (binodal), corresponding tie-lines, the limit of stability/metastability (spinodal), and further thermodynamic properties of the phase diagram. Calculations for ternary and multicomponent alcohol/polyol-water-salt mixtures suggest that LLE are a prevalent feature of organic-inorganic aerosol systems. A six-component polyol-water-ammonium sulphate system is used to simulate effects of relative humidity (RH) and the presence of liquid-liquid phase separation on the gas/particle partitioning. RH, salt concentration, and hydrophilicity (water-solubility) are identified as key features in defining the region of a miscibility gap and govern the extent to which compound partitioning is affected by changes in RH. The model predicts that liquid-liquid phase separation can lead to either an increase or decrease in total particulate mass, depending on the overall composition of a system and the particle water content, which is related to the hydrophilicity of the different organic and inorganic compounds. Neglecting non-ideality and liquid-liquid phase separations by assuming an ideal mixture leads to an overestimation of the total particulate mass by up to 30% for the composition and RH range considered in the six-component system simulation

Effect of aerosol particles generated by ultrasonic humidifiers on the lung in mouse.

PubMed

Umezawa, Masakazu; Sekita, Keisuke; Suzuki, Ken-Ichiro; Kubo-Irie, Miyoko; Niki, Rikio; Ihara, Tomomi; Sugamata, Masao; Takeda, Ken

2013-12-21

Ultrasonic humidifiers silently generate water droplets as a cool fog and produce most of the dissolved minerals in the fog in the form of an aerosolized "white dust." However, the health effect of these airborne particles is largely unknown. This study aimed to characterize the aerosol particles generated by ultrasonic humidifiers and to investigate their effect on the lung tissue of mice. An ultrasonic humidifier was operated with tap water, high-silica water, ultrapure water, or other water types. In a chamber (0.765 m3, ventilation ratio 11.5 m3/hr), male ICR mice (10-week-old) were exposed by inhalation to an aerosol-containing vapor generated by the humidifier. After exposure for 7 or 14 days, lung tissues and bronchoalveolar lavage fluid (BALF) were collected from each mouse and examined by microarray, quantitative reverse transcription-polymerase chain reaction, and light and electron microscopy. Particles generated from the humidifier operated with tap water had a mass concentration of 0.46 ± 0.03 mg/m3, number concentration of (5.0 ± 1.1) × 10(4)/cm3, and peak size distribution of 183 nm. The particles were phagocytosed by alveolar macrophages in the lung of mice. Inhalation of particles caused dysregulation of genes related to mitosis, cell adhesion molecules, MHC molecules and endocytosis, but did not induce any signs of inflammation or tissue injury in the lung. These results indicate that aerosol particles released from ultrasonic humidifiers operated with tap water initiated a cellular response but did not cause severe acute inflammation in pulmonary tissue. Additionally, high mineral content tap water is not recommended and de-mineralized water should be recommended in order to exclude any adverse effects.

Seasonal variabilities in chemical compounds and acidity of aerosol particles at urban site in the west Pacific.

PubMed

Pan, Xiaole; Uno, Itsushi; Wang, Zhe; Yamamoto, Shigekazu; Hara, Yukari; Wang, Zifa

2018-06-01

Mass concentrations of chemical compounds in both PM 2.5 (particle aerodynamic diameter, Dp < 2.5 μm) and PM 2.5-10 (2.5 < Dp < 10 μm), and acidity of aerosol particles were measured at an urban site in western Japan using a continuous dichotomous Aerosol Chemical Speciation Analyzer (ACSA-12) throughout 2014. Mass concentrations of both PM 2.5 and sulfate had distinct seasonal variabilities with maxima in spring and winter, mostly due to long-range transport with the prevailing westerly wind. Mass concentration of nitrate in PM 2.5 (fNO 3 ) showed an obvious warm-season-low and cold-season-high pattern as a result of both gas-aerosol phase equilibrium processes under high temperature conditions as well as transport. Nitrate in PM 2.5-10 (cNO 3 ) increased during long-range transport of dust, implying the great importance of heterogeneous processes at the surface of coarse mode particles. In this study, Δ[H + ] (derived from the difference in pH of extract liquid with/without sampling) was used to indicate the acidity of particles. We found that acidity of particles in PM 2.5 (fΔH) was mostly positive with a maximum in August because of the large fraction of nitrate and sulfate. Acidity of particles in PM 2.5-10 (cΔH) was negative in winter and spring due to presence of alkaline matter from crustal sources. This study highlights the great importance of anthropogenic pollutants on the acidity of particles in the western Pacific Ocean and further impact on the marine environment and climate. Copyright © 2017 The Authors. Published by Elsevier Ltd.. All rights reserved.

Dispersion of aerosol particles in the atmosphere: Fukushima

NASA Astrophysics Data System (ADS)

Haszpra, Tímea; Lagzi, István; Tél, Tamás

2013-04-01

Investigation of dispersion and deposition of aerosol particles in the atmosphere is an essential issue, because they have an effect on the biosphere and atmosphere. Moreover, aerosol particles have different transport properties and chemical and physical transformations in the atmosphere compared to gas phase air pollutants. The motion of a particle is described by a set of ordinary differential equations. The large-scale dynamics in the horizontal direction can be described by the equations of passive scalar advection, but in the vertical direction a well-defined terminal velocity should be taken into account as a term added to the vertical wind component. In the planetary boundary layer turbulent diffusion has an important role in the particle dispersion, which is taken into account by adding stochastic terms to the deterministic equations above. Wet deposition is also an essential process in the lower levels of the atmosphere, however, its precise parameterization is a challenge. For the simulations the wind field and other necessary data were taken from the ECMWF ERA-Interim database. In the case of the Fukushima Daiichi nuclear disaster (March-April 2011) radioactive aerosol particles were also released in the planetary boundary layer. Simulations (included the continuous and varying emission from the nuclear power plant) will be presented for the period of 14-23 March. Results show that wet deposition also has to be taken into consideration in the lower levels of the atmosphere. Furthermore, dynamical system characteristics are evaluated for the aerosol particle dynamics. The escape rate of particles was estimated both with and without turbulent diffusion, and in both cases when there was no wet deposition and also when wet deposition was taken into consideration.

Single-particle characterization of indoor aerosol particles collected at an underground shopping area in Seoul, Korea.

PubMed

Maskey, Shila; Kang, TaeHee; Jung, Hae-Jin; Ro, Chul-Un

2011-02-01

In this study, single-particle characterization of aerosol particles collected at an underground shopping area was performed for the first time. A quantitative single-particle analytical technique, low-Z particle electron probe X-ray microanalysis, was used to characterize a total of 7900 individual particles for eight sets of aerosol samples collected at an underground shopping area in Seoul, Korea. Based on secondary electron images and X-ray spectral data of individual particles, fourteen particle types were identified, in which primary soil-derived particles were the most abundant, followed by carbonaceous, Fe-containing, secondary soil-derived, and secondary sea-salt particles. Carbonaceous particles exist in three types: organic carbon, carbon-rich, and CNO-rich. A significant number of textile particles with chemical composition C, N, and O were encountered in some of the aerosol samples, which were from the textile shops and/or from clothes of passersby. Primary soil-derived particles showed seasonal variation, with peak values in spring samples, reflecting higher air exchange between indoor and outdoor environments in the spring. Secondary soil-derived, secondary sea-salt, and ammonium sulfate particles were frequently encountered in winter samples. Fe-containing particles, contributed from a nearby subway station, were in the range of about 19% relative abundances for all samples. In underground shopping areas, particulate matters can be a considerable health hazard to the workers, shoppers, passersby, and shop-keepers as they spend their considerable time in this closed microenvironment. However, no study on the characteristics of indoor aerosols in an underground shopping area has been reported to our knowledge. This work provides detailed information on characteristics of underground shopping area aerosols on a single particle level. © 2010 John Wiley & Sons A/S.

The relationship between aerosol particles chemical composition and optical properties to identify the biomass burning contribution to fine particles concentration: a case study for São Paulo city, Brazil.

PubMed

de Miranda, Regina Maura; Lopes, Fabio; do Rosário, Nilton Évora; Yamasoe, Marcia Akemi; Landulfo, Eduardo; de Fatima Andrade, Maria

2016-12-01

The air quality in the Metropolitan Area of São Paulo (MASP) is primarily determined by the local pollution source contribution, mainly the vehicular fleet, but there is a concern about the role of remote sources to the fine mode particles (PM 2.5 ) concentration and composition. One of the most important remote sources of atmospheric aerosol is the biomass burning emissions from São Paulo state's inland and from the central and north portions of Brazil. This study presents a synergy of different measurements of atmospheric aerosol chemistry and optical properties in the MASP in order to show how they can be used as a tool to identify particles from local and remote sources. For the clear identification of the local and remote source contribution, aerosol properties measurements at surface level were combined with vertical profiles information. Over 15 days in the austral winter of 2012, particulate matter (PM) was collected using a cascade impactor and a Partisol sampler in São Paulo City. Mass concentrations were determined by gravimetry, black carbon concentrations by reflectance, and trace element concentrations by X-ray fluorescence. Aerosol optical properties were studied using a multifilter rotating shadowband radiometer (MFRSR), a Lidar system and satellite data. Optical properties, concentrations, size distributions, and elemental composition of atmospheric particles were strongly related and varied according to meteorological conditions. During the sampling period, PM mean mass concentrations were 17.4 ± 10.1 and 15.3 ± 6.9 μg/m 3 for the fine and coarse fractions, respectively. The mean aerosol optical depths at 415 nm and Ångström exponent (AE) over the whole period were 0.29 ± 0.14 and 1.35 ± 0.11, respectively. Lidar ratios reached values of 75 sr. The analyses of the impacts of an event of biomass burning smoke transport to the São Paulo city revealed significant changing on local aerosol concentrations and optical parameters

SAM-CAAM: A Concept for Acquiring Systematic Aircraft Measurements to Characterize Aerosol Air Masses

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kahn, Ralph A.; Berkoff, Tim A.; Brock, Charles

A modest operational program of systematic aircraft measurements can resolve key satellite aerosol data record limitations. Satellite observations provide frequent global aerosol amount maps but offer only loose aerosol property constraints needed for climate and air quality applications. In this paper, we define and illustrate the feasibility of flying an aircraft payload to measure key aerosol optical, microphysical, and chemical properties in situ. The flight program could characterize major aerosol airmass types statistically, at a level of detail unobtainable from space. It would 1) enhance satellite aerosol retrieval products with better climatology assumptions and 2) improve translation between satellite-retrieved opticalmore » properties and species-specific aerosol mass and size simulated in climate models to assess aerosol forcing, its anthropogenic components, and other environmental impacts. As such, Systematic Aircraft Measurements to Characterize Aerosol Air Masses (SAM-CAAM) could add value to data records representing several decades of aerosol observations from space; improve aerosol constraints on climate modeling; help interrelate remote sensing, in situ, and modeling aerosol-type definitions; and contribute to future satellite aerosol missions. Fifteen required variables are identified and four payload options of increasing ambition are defined to constrain these quantities. “Option C” could meet all the SAM-CAAM objectives with about 20 instruments, most of which have flown before, but never routinely several times per week, and never as a group. Aircraft integration and approaches to data handling, payload support, and logistical considerations for a long-term, operational mission are discussed. Finally, SAM-CAAM is feasible because, for most aerosol sources and specified seasons, particle properties tend to be repeatable, even if aerosol loading varies.« less

SAM-CAAM: A Concept for Acquiring Systematic Aircraft Measurements to Characterize Aerosol Air Masses

DOE PAGES

Kahn, Ralph A.; Berkoff, Tim A.; Brock, Charles; ...

2017-10-30

A modest operational program of systematic aircraft measurements can resolve key satellite aerosol data record limitations. Satellite observations provide frequent global aerosol amount maps but offer only loose aerosol property constraints needed for climate and air quality applications. In this paper, we define and illustrate the feasibility of flying an aircraft payload to measure key aerosol optical, microphysical, and chemical properties in situ. The flight program could characterize major aerosol airmass types statistically, at a level of detail unobtainable from space. It would 1) enhance satellite aerosol retrieval products with better climatology assumptions and 2) improve translation between satellite-retrieved opticalmore » properties and species-specific aerosol mass and size simulated in climate models to assess aerosol forcing, its anthropogenic components, and other environmental impacts. As such, Systematic Aircraft Measurements to Characterize Aerosol Air Masses (SAM-CAAM) could add value to data records representing several decades of aerosol observations from space; improve aerosol constraints on climate modeling; help interrelate remote sensing, in situ, and modeling aerosol-type definitions; and contribute to future satellite aerosol missions. Fifteen required variables are identified and four payload options of increasing ambition are defined to constrain these quantities. “Option C” could meet all the SAM-CAAM objectives with about 20 instruments, most of which have flown before, but never routinely several times per week, and never as a group. Aircraft integration and approaches to data handling, payload support, and logistical considerations for a long-term, operational mission are discussed. Finally, SAM-CAAM is feasible because, for most aerosol sources and specified seasons, particle properties tend to be repeatable, even if aerosol loading varies.« less

Characterization of aerosol particle episodes in Finland caused by wildfires in Eastern Europe

NASA Astrophysics Data System (ADS)

Niemi, J. V.; Tervahattu, H.; Vehkamäki, H.; Martikainen, J.; Laakso, L.; Kulmala, M.; Aarnio, P.; Koskentalo, T.; Sillanpää, M.; Makkonen, U.

2005-04-01

We studied the sources, compositions and size distributions of aerosol particles during long-range transport (LRT) PM2.5 episodes occurred on 12-15 August, 26-28 August and 5-6 September 2002 in Finland. Backward air mass trajectories, satellite detections of fire areas, and dispersion modelling results indicate that emissions from wildfires in Russia and other Eastern European countries arrived to Finland during the episodes. Individual particle analyses using scanning electron microscopy (SEM) coupled with energy dispersive X-ray analyses (EDX) showed that the proportion of S-rich particles increased during the episodes and they contained elevated fractions of K, which indicates emissions from biomass burning. These aerosols were mixed with S-rich emissions from fossil fuel burning during the transport, since air masses came through polluted areas of Europe. Minor amounts of coarse Ca-rich particles were also brought by LRT during the episodes, and they probably originated from wildfires and/or from Estonian and Russian oil-shale burning industrial areas. The ion chromatography analysis showed that concentrations of sulphate (SO42-), total nitrate (NO3-+HNO3(g)) and total ammonium (NH4++NH3(g)) increased during the episodes, but the ratio of total amount of these ions to PM10 concentration decreased indicating unusually high fractions of other chemical components. The particle number size distribution measurements with differential mobility particle sizer (DMPS) showed that the concentrations of 90-500 nm particles increased during the episodes, but the concentrations of particles smaller than 90nm decreased. The reduction of the smallest particles was caused by suppressed new particle formation due to the vapour and molecular cluster uptake of LRT particles. Our results show that the emissions from wildfires in Russian and other Eastern European deteriorated air quality on very large areas, even at the distance of over 1000 km from the fire areas.

Aerosol Enhancements in the Upper Troposphere Over The Amazon Forest: Do Amazonian Clouds Produce Aerosols?

NASA Astrophysics Data System (ADS)

Andreae, M. O.; Afchine, A.; Albrecht, R. I.; Artaxo, P.; Borrmann, S.; Cecchini, M. A.; Costa, A.; Dollner, M.; Fütterer, D.; Järvinen, E.; Klimach, T.; Konemann, T.; Kraemer, M.; Krüger, M. L.; Machado, L.; Mertes, S.; Pöhlker, C.; Poeschl, U.; Sauer, D. N.; Schnaiter, M.; Schneider, J.; Schulz, C.; Spanu, A.; Walser, A.; Weinzierl, B.; Wendisch, M.

2015-12-01

The German-Brazilian cooperative aircraft campaign ACRIDICON-CHUVA (Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems) on the German research aircraft HALO took place over the Amazon Basin in September/October 2014, with the objective of studying tropical deep convective clouds over the Amazon rainforest and their interactions with trace gases, aerosol particles, and atmospheric radiation. The aircraft was equipped with about 30 remote sensing and in-situ instruments for meteorological, trace gas, aerosol, cloud, precipitation, and solar radiation measurements. Fourteen research flights were conducted during this campaign. Observations during ACRIDICON-CHUVA showed high aerosol concentrations in the upper troposphere (UT) over the Amazon Basin, with concentrations after normalization to standard conditions often exceeding those in the boundary layer (BL). This behavior was consistent between several aerosol metrics, including condensation nuclei (CN), cloud condensation nuclei (CCN), and chemical species mass concentrations. These UT aerosols were different in their composition and size distribution from the aerosol in the BL, making convective transport of particles unlikely as a source. The regions in the immediate outflow of deep convective clouds were found to be depleted in aerosol particles, whereas enhanced aerosol number and mass concentrations were found in UT regions that had experienced outflow from deep convection in the preceding 24-48 hours. This suggests that aerosol production takes place in the UT based on volatile and condensable material brought up by deep convection. Subsequently, downward mixing and transport of upper tropospheric aerosol may be a source of particles to the BL, where they increase in size by the condensation of biogenic volatile organic carbon (BVOC) oxidation products. This may be an important source of aerosol particles in the Amazonian BL, where aerosol nucleation and new

On the Nature of Aerosol Particles in the Atmosphere of Irkutsk

NASA Astrophysics Data System (ADS)

Yermakov, A. N.; Golobokova, L. P.; Netsvetaeva, O. G.; Aloyan, A. E.; Arutyunyan, V. O.; Khodzher, T. V.

2018-03-01

Monitoring data on the ion composition of precipitation and the water-soluble fraction of aerosol have been used to identify two types of aerosol particles in the surface atmosphere of Irkutsk ("metal" and "ammonia" groups). The aerosol acidity is basically governed by the acidity of ammonia particles, and the ion composition depends on air relative humidity (RH). Preliminary estimates are given for the distribution of major cations and anions by aerosol groups.

Aerosol composition and source apportionment in Santiago de Chile

NASA Astrophysics Data System (ADS)

Artaxo, Paulo; Oyola, Pedro; Martinez, Roberto

1999-04-01

Santiago de Chile, São Paulo and Mexico City are Latin American urban areas that suffer from heavy air pollution. In order to study air pollution in Santiago area, an aerosol source apportionment study was designed to measure ambient aerosol composition and size distribution for two downtown sampling sites in Santiago. The aerosol monitoring stations were operated in Gotuzo and Las Condes during July and August 1996. The study employed stacked filter units (SFU) for aerosol sampling, collecting fine mode aerosol (dp<2 μm) and coarse mode aerosol (2Aerosol mass (PM 10 mass of particles smaller than 10 μm) and black carbon concentration were also measured. Particle-Induced X-ray Emission (PIXE) was used to measure the concentration of 22 trace elements at levels below 0.5 ng m -3. Quantitative aerosol source apportionment was performed using Absolute Principal Factor Analysis (APFA). Very high aerosol concentrations were observed (up to 400 μg/m 3 PM 10). The main aerosol particle sources in Santiago are resuspended soil dust and traffic emissions. Coarse particles account for 63% of PM 10 aerosol in Gotuzo and 53% in Las Condes. A major part of this component is resuspended soil dust. In the fine fraction, resuspended soil dust accounts for 15% of fine mass, and the aerosols associated with transportation activities account for a high 64% of the fine particle mass. Sulfate particle is an important component of the aerosol in Santiago, mainly originating from gas-to-particle conversion from SO 2. In the Gotuzo site, sulfates are the highest aerosol component, accounting for 64.5% of fine mass. Direct traffic emissions are generally mixed with resuspended soil dust. It is difficult to separate the two components, because the soil dust in downtown Santiago is contaminated with Pb, Br, Cl, and other heavy metals that are also tracers for traffic emissions. Residual oil combustion is observed, with the presence of V, S and Ni. An

Brown Carbon Production in Ammonium- or Amine-Containing Aerosol Particles by Reactive Uptake of Methylglyoxal and Photolytic Cloud Cycling.

PubMed

De Haan, David O; Hawkins, Lelia N; Welsh, Hannah G; Pednekar, Raunak; Casar, Jason R; Pennington, Elyse A; de Loera, Alexia; Jimenez, Natalie G; Symons, Michael A; Zauscher, Melanie; Pajunoja, Aki; Caponi, Lorenzo; Cazaunau, Mathieu; Formenti, Paola; Gratien, Aline; Pangui, Edouard; Doussin, Jean-François

2017-07-05

The effects of methylglyoxal uptake on the physical and optical properties of aerosol containing amines or ammonium sulfate were determined before and after cloud processing in a temperature- and RH-controlled chamber. The formation of brown carbon was observed upon methylglyoxal addition, detected as an increase in water-soluble organic carbon mass absorption coefficients below 370 nm and as a drop in single-scattering albedo at 450 nm. The imaginary refractive index component k 450 reached a maximum value of 0.03 ± 0.009 with aqueous glycine aerosol particles. Browning of solid particles occurred at rates limited by chamber mixing (<1 min), and in liquid particles occurred more gradually, but in all cases occurred much more rapidly than in bulk aqueous studies. Further browning in AS and methylammonium sulfate seeds was triggered by cloud events with chamber lights on, suggesting photosensitized brown carbon formation. Despite these changes in optical aerosol characteristics, increases in dried aerosol mass were rarely observed (<1 μg/m 3 in all cases), consistent with previous experiments on methylglyoxal. Under dry, particle-free conditions, methylglyoxal reacted (presumably on chamber walls) with methylamine with a rate constant k = (9 ± 2) × 10 -17 cm 3 molecule -1 s -1 at 294 K and activation energy E a = 64 ± 37 kJ/mol.

Tar balls are processed, weakly absorbing, primary aerosol particles formed downwind of boreal forest fires

NASA Astrophysics Data System (ADS)

Sedlacek, A. J., III; Buseck, P. R.; Adachi, K.; Kleinman, L. I.; Onasch, T. B.; Springston, S. R.

2017-12-01

Biomass burning is a major source of light-absorbing black and brown carbonaceous aerosols Brown carbon is a poorly characterized mixture that includes tar balls (TBs), a type of carbonaceous particle unique to biomass burning. Here we describe the first atmospheric observations of the formation and evolution of TBs Aerosol particles were collected on TEM grids during individual aircraft transects at varying downwind distances from the Colockum Tarp wildland fire. The TEM images show primary particles transforming from viscous, impact-deformed particles to spherical TBs. The number fraction of TBs in the wildfire smoke plume increased from less than 5% in samples collected close to the emission source to greater than 40% after 3 hours of aging, with little change in downwind TB diameters. The TB mass fraction increased from 2% near the fire to 23±9% downwind. Single-scatter albedo determined from scattering and absorption measurements increased slightly with downwind distance. Mie calculations show this observation is consistent with weak light absorbance by TBs (m=1.56 - 0.02i) but not consistent with order-of-magnitude stronger absorption observed in different settings. The field-derived TB mass fractions reported here indicate that this particle type should be accounted for in biomass-burn emission inventories.

Use of stable carbon and nitrogen isotope ratios in size segregated aerosol particles for the O/I penetration evaluation

NASA Astrophysics Data System (ADS)

Garbaras, Andrius; Garbariene, Inga; Masalaite, Agne; Ceburnis, Darius; Krugly, Edvinas; Kvietkus, Kestutis; Remeikis, Vidmantas; Martuzevicius, Dainius

2015-04-01

Stable carbon and nitrogen isotope ratio are successfully used in the atmospheric aerosol particle source identification [1, 2], transformation, pollution [3] research. The main purpose of this study was to evaluate the penetration of atmospheric aerosol particles from outdoor to indoor using stable carbon and nitrogen isotope ratios. Six houses in Kaunas (Lithuania) were investigated during February and March 2013. Electrical low pressure impactor was used to measure in real time concentration and size distribution of outdoor aerosol particles. ELPI+ includes 15 channels covering the size range from 0.017 to 10.0 µm. The 25 mm diameter aluminium foils were used to collect aerosol particles. Gravimetric analysis of samples was made using microbalance. In parallel, indoor aerosol samples were collected with a micro-orifice uniform deposition impactor (MOUDI model 110), where the aerosol particles were separated with the nominal D50 cut-off sizes of 0.056, 0.1, 0.18,0.32,0.56, 1.0, 1.8, 3.2, 5.6, 10, 18 μm for impactor stages 1-11, respectively. The impactor was run at a flow rate of 30 L/min. Air quality meters were used to record meteorological conditions (temperature, relative humidity) during the investigated period. All aerosol samples were analyzed for total carbon (TC) and total nitrogen (TN) contents and their isotopic compositions using elemental analyzer (EA) connected to the stable isotope ratio mass spectrometer (IRMS). TC concentration in indoors ranged from 1.5 to 247.5 µg/m3. During the sampling period outdoors TN levels ranged from 0.1 to 10.9 µg/m3. The obtained outdoor δ13C(PM2.5) values varied from -24.21 to -26.3‰, while the δ15N values varied from 2.4 to 11.1 ‰ (average 7.2±2.5 ‰). Indoors carbonaceous aerosol particles were depleted in 13C compared to outdoors in all sampling sites. This depletion in δ13C varied from 0.1 to 3.2 ‰. We think that this depletion occurs due ongoing chemical reactions (oxidation) when aerosol

Characterization of new particle and secondary aerosol formation during summertime in Beijing, China

NASA Astrophysics Data System (ADS)

Zhang, Y. M.; Zhang, X. Y.; Sun, J. Y.; Lin, W. L.; Gong, S. L.; Shen, X. J.; Yang, S.

2011-07-01

Size-resolved aerosol number and mass concentrations and the mixing ratios of O3 and various trace gases were continuously measured at an urban station before and during the Beijing Olympic and Paralympic Games (5 June to 22 September, 2008). 23 new particle formation (NPF) events were identified; these usually were associated with changes in wind direction and/or rising concentrations of gas-phase precursors or after precipitation events. Most of the NPF events started in the morning and continued to noon as particles in the nucleation mode grew into the Aitken mode. From noon to midnight, the aerosols grew into the accumulation mode through condensation and coagulation. Ozone showed a gradual rise starting around 10:00 local time, reached its peak around 15:00 and then declined as the organics increased. The dominant new particle species were organics (40-75% of PM1) and sulphate; nitrate and ammonium were more minor contributors.

Relation between aerosol sources and meteorological parameters for inhalable atmospheric particles in Sao Paulo City, Brazil

NASA Astrophysics Data System (ADS)

Andrade, Fatima; Orsini, Celso; Maenhaut, Willy

Stacked filter units were used to collect atmospheric particles in separate coarse and fine fractions at the Sao Paulo University Campus during the winter of 1989. The samples were analysed by particle-induced X-ray emission (PIXE) and the data were subjected to an absolute principal component analysis (APCA). Five sources were identified for the fine particles: industrial emissions, which accounted for 13% of the fine mass; emissions from residual oil and diesel, explaining 41%; resuspended soil dust, with 28%; and emissions of Cu and of Mg, together with 18%. For the coarse particles, four sources were identified: soil dust, accounting for 59% of the coarse mass; industrial emissions, with 19%; oil burning, with 8%; and sea salt aerosol, with 14% of the coarse mass. A data set with various meteorological parameters was also subjected to APCA, and a correlation analysis was performed between the meteorological "absolute principal component scores" (APCS) and the APCS from the fine and coarse particle data sets. The soil dust sources for the fine and coarse aerosol were highly correlated with each other and were anticorrelated with the sea breeze component. The industrial components in the fine and coarse size fractions were also highly positively correlated. Furthermore, the industrial component was related with the northeasterly wind direction and, to a lesser extent, with the sea breeze component.

Thermal behavior of aerosol particles from biomass burning during the BBOP campaign using transmission electron microscopy

NASA Astrophysics Data System (ADS)

Adachi, K.; Ishimoto, H.; Sedlacek, A. J., III; Kleinman, L. I.; Chand, D.; Hubbe, J. M.; Buseck, P. R.

2017-12-01

Aerosol samples were collected from wildland and agricultural biomass fires in North America during the 2013 Biomass Burning Observation Project (BBOP). We show in-situ shape and size changes and variations in the compositions of individual particles before and after heating using a transmission electron microscope (TEM). The responses of aerosol particles to heating are important for measurements of their chemical, physical, and optical properties, classification, and determination of origin. However, the thermal behavior of organic aerosol particles is largely unknown. We provide a method to analyze such thermal behavior through heating from room temperature to >600°C by using a heating holder within TEM. The results indicate that individual tar balls (TB; spherical organic material) from biomass burning retained, on average, up to 30% of their volume when heated to 600°C. Chemical analysis reveals that K and Na remained in the residues, whereas S and O were lost. In contrast to bulk sample measurements of carbonaceous particles using thermal/optical carbon analyzers, our single-particle results imply that many individual organic particles consist of multiple types of organic matter having different thermal stabilities. Our results also suggest that because of their thermal stability, some organic particles may not be detectable by using aerosol mass spectrometry or thermal/optical carbon analyzers. This result can lead to an underestimate of the abundance of TBs and other organic particles, and therefore biomass burning may have a greater influence than is currently recognized in regional and global climate models.

Measurements of Primary Biogenic Aerosol Particles with an Ultraviolet Aerodynamic Particle Sizer (UVAPS) During AMAZE-08

NASA Astrophysics Data System (ADS)

Wollny, A. G.; Garland, R.; Pöschl, U.

2008-12-01

Biogenic aerosols are ubiquitous in the Earth's atmosphere and they influence atmospheric chemistry and physics, the biosphere, climate, and public health. They play an important role in the spread of biological organisms and reproductive materials, and they can cause or enhance human, animal, and plant diseases. Moreover, they influence the Earth's energy budget by scattering and absorbing radiation, and they can initiate the formation of clouds and precipitation as cloud condensation and ice nuclei. The composition, abundance, and origin of biogenic aerosol particles and components are, however, still not well understood and poorly quantified. Prominent examples of primary biogenic aerosol particles, which are directly emitted from the biosphere to the atmosphere, are pollen, bacteria, fungal spores, viruses, and fragments of animals and plants. During the AMazonian Aerosol CharacteriZation Experiment (AMAZE-08) a large number of aerosol and gas-phase measurements were taken on a remote site close to Manaus, Brazil, during a period of five weeks in February and March 2008. The presented study is focused on data from an ultraviolet aerodynamic particle sizer (UVAPS, TSI inc.) that has been deployed for the first time in Amazonia. In this instrument, particle counting and aerodynamic sizing over the range of 0.5-20 μm are complemented by the measurement of UV fluorescence at 355 nm (excitation) and 420-575 nm (emission), respectively. Fluorescence at these wavelengths is characteristic for reduced pyridine nucleotides (e.g., NAD(P)H) and for riboflavin, which are specific for living cells. Thus particles exhibiting fluorescence signals can be regarded as 'viable aerosols' or 'fluorescent bioparticles' (FBAP), and their concentration can be considered as lower limit for the actual abundance of primary biogenic aerosol particles. First data analyses show a pronounced peak of FBAP at diameters around 2-3 μm. In this size range the biogenic particle fraction was

Physical and Chemical Characterization of Particles in the Upper Troposphere and Lower Stratosphere: Microanalysis of Aerosol Impactor Samples

NASA Technical Reports Server (NTRS)

Sheridan, Patrick J.

1999-01-01

Herein is reported activities to support the characterization of the aerosol in the upper troposphere (UT) and lower stratosphere (LS) collected during the Airborne Southern Hemisphere Ozone Experiment/Measurements for Assessing the Effects of Stratospheric Aircraft (ASHOE/MAESA) missions in 1994. Through a companion proposal, another group was to measure the size distribution of aerosols in the 0.008 to 2 micrometer diameter range and to collect for us impactor samples of particles larger than about 0.02 gm. In the first year, we conducted laboratory studies related to particulate deposition patterns on our collection substrates, and have performed the analysis of many ASHOE/MAESA aerosol samples from 1994 using analytical electron microscopy (AEM). We have been building an "aerosol climatology" with these data that documents the types and relative abundances of particles observed at different latitudes and altitudes. The second year (and non-funded extension periods) saw continued analyses of impactor aerosol samples, including more ASHOE/MAESA samples, some northern hemisphere samples from the NASA Stratospheric Photochemistry Aerosols and Dynamics Expedition (SPADE) program for comparison, and a few aerosol samples from the NASA Stratospheric TRacers of Atmospheric Transport (STRAT) program. A high-resolution field emission microscope was used for the analysis and re-analysis of a number of samples to determine if this instrument was superior in performance to our conventional electron microscope. In addition, some basic laboratory studies were conducted to determine the minimum detectable and analyzable particle size for different types of aerosols. In all, 61 aerosol samples were analyzed, with a total of over 30,000 individual particle analyses. In all analyzed samples, sulfate particles comprised the major aerosol number fraction. It must be stressed that particles composed of more than one species, for example sulfate and organic carbon, were classified

Real-Time Characterization of Aerosol Particle Composition above the Urban Canopy in Beijing: Insights into the Interactions between the Atmospheric Boundary Layer and Aerosol Chemistry.

PubMed

Sun, Yele; Du, Wei; Wang, Qingqing; Zhang, Qi; Chen, Chen; Chen, Yong; Chen, Zhenyi; Fu, Pingqing; Wang, Zifa; Gao, Zhiqiu; Worsnop, Douglas R

2015-10-06

Despite extensive efforts into the characterization of air pollution during the past decade, real-time characterization of aerosol particle composition above the urban canopy in the megacity Beijing has never been performed to date. Here we conducted the first simultaneous real-time measurements of aerosol composition at two different heights at the same location in urban Beijing from December 19, 2013 to January 2, 2014. The nonrefractory submicron aerosol (NR-PM1) species were measured in situ by a high-resolution aerosol mass spectrometer at near-ground level and an aerosol chemical speciation monitor at 260 m on a 325 m meteorological tower in Beijing. Secondary aerosol showed similar temporal variations between ground level and 260 m, whereas much weaker correlations were found for the primary aerosol. The diurnal evolution of the ratios and correlations of aerosol species between 260 m and the ground level further illustrated a complex interaction between vertical mixing processes and local source emissions on aerosol chemistry in the atmospheric boundary layer. As a result, the aerosol compositions at the two heights were substantially different. Organic aerosol (OA), mainly composed of primary OA (62%), at the ground level showed a higher contribution to NR-PM1 (65%) than at 260 m (54%), whereas a higher concentration and contribution (15%) of nitrate was observed at 260 m, probably due to the favorable gas-particle partitioning under lower temperature conditions. In addition, two different boundary layer structures were observed, each interacting differently with the evolution processes of aerosol chemistry.

Quantification of black carbon mixing state from traffic: Implications for aerosol optical properties

DOE PAGES

Willis, Megan D.; Healy, Robert M.; Riemer, Nicole; ...

2016-04-14

The climatic impacts of black carbon (BC) aerosol, an important absorber of solar radiation in the atmosphere, remain poorly constrained and are intimately related to its particle-scale physical and chemical properties. Using particle-resolved modelling informed by quantitative measurements from a soot-particle aerosol mass spectrometer, we confirm that the mixing state (the distribution of co-emitted aerosol amongst fresh BC-containing particles) at the time of emission significantly affects BC-aerosol optical properties even after a day of atmospheric processing. Both single particle and ensemble aerosol mass spectrometry observations indicate that BC near the point of emission co-exists with hydrocarbon-like organic aerosol (HOA) inmore » two distinct particle types: HOA-rich and BC-rich particles. The average mass fraction of black carbon in HOA-rich and BC-rich particle classes was < 0.1 and 0.8, respectively. Notably, approximately 90 % of BC mass resides in BC-rich particles. This new measurement capability provides quantitative insight into the physical and chemical nature of BC-containing particles and is used to drive a particle-resolved aerosol box model. Lastly, significant differences in calculated single scattering albedo (an increase of 0.1) arise from accurate treatment of initial particle mixing state as compared to the assumption of uniform aerosol composition at the point of BC injection into the atmosphere.« less

Nicotine, aerosol particles, carbonyls and volatile organic compounds in tobacco- and menthol-flavored e-cigarettes.

PubMed

Lee, Mi-Sun; LeBouf, Ryan F; Son, Youn-Suk; Koutrakis, Petros; Christiani, David C

2017-04-27

We aimed to assess the content of electronic cigarette (EC) emissions for five groups of potentially toxic compounds that are known to be present in tobacco smoke: nicotine, particles, carbonyls, volatile organic compounds (VOCs), and trace elements by flavor and puffing time. We used ECs containing a common nicotine strength (1.8%) and the most popular flavors, tobacco and menthol. An automatic multiple smoking machine was used to generate EC aerosols under controlled conditions. Using a dilution chamber, we targeted nicotine concentrations similar to that of exposure in a general indoor environment. The selected toxic compounds were extracted from EC aerosols into a solid or liquid phase and analyzed with chromatographic and spectroscopic methods. We found that EC aerosols contained toxic compounds including nicotine, fine and nanoparticles, carbonyls, and some toxic VOCs such as benzene and toluene. Higher mass and number concentrations of aerosol particles were generated from tobacco-flavored ECs than from menthol-flavored ECs. We found that diluted machine-generated EC aerosols contain some pollutants. These findings are limited by the small number of ECs tested and the conditions of testing. More comprehensive research on EC exposure extending to more brands and flavor compounds is warranted.

Substantial convection and precipitation enhancements by ultrafine aerosol particles

NASA Astrophysics Data System (ADS)

Fan, Jiwen; Rosenfeld, Daniel; Zhang, Yuwei; Giangrande, Scott E.; Li, Zhanqing; Machado, Luiz A. T.; Martin, Scot T.; Yang, Yan; Wang, Jian; Artaxo, Paulo; Barbosa, Henrique M. J.; Braga, Ramon C.; Comstock, Jennifer M.; Feng, Zhe; Gao, Wenhua; Gomes, Helber B.; Mei, Fan; Pöhlker, Christopher; Pöhlker, Mira L.; Pöschl, Ulrich; de Souza, Rodrigo A. F.

2018-01-01

Ultrafine aerosol particles (smaller than 50 nanometers in diameter) have been thought to be too small to affect cloud formation. Fan et al. show that this is not the case. They studied the effect of urban pollution transported into the otherwise nearly pristine atmosphere of the Amazon. Condensational growth of water droplets around the tiny particles releases latent heat, thereby intensifying atmospheric convection. Thus, anthropogenic ultrafine aerosol particles may exert a more important influence on cloud formation processes than previously believed.

Characterization of aerosol particle episodes in Finland caused by wildfires in Eastern Europe

NASA Astrophysics Data System (ADS)

Niemi, J. V.; Tervahattu, H.; Vehkamäki, H.; Martikainen, J.; Laakso, L.; Kulmala, M.; Aarnio, P.; Koskentalo, T.; Sillanpää, M.; Makkonen, U.

2005-08-01

We studied the sources, compositions and size distributions of aerosol particles during long-range transport (LRT) PM2.5 episodes which occurred on 12-15 August, 26-28 August and 5-6 September 2002 in Finland. Backward air mass trajectories, satellite detections of fire areas and dispersion modelling results indicate that emissions from wildfires in Russia and other Eastern European countries arrived in Finland during these episodes. Elemental analyses using scanning electron microscopy (SEM) coupled with energy dispersive X-ray microanalyses (EDX) showed that the proportions of S-rich particles and agglomerates (agglomeration was caused partly by the sampling method used) increased during the episodes, and they contained elevated fractions of K, indicating emissions from biomass burning. These aerosols were mixed with S-rich emissions from fossil fuel burning during transport since air masses came through polluted areas of Europe. Minor amounts of coarse Ca-rich particles were also brought by LRT during the episodes, and they probably originated from wildfires and/or from Estonian and Russian oil-shale-burning industrial areas. Ion chromatography analysis showed that concentrations of sulphate (SO42-), total nitrate (NO3-+HNO3(g)) and total ammonium (NH4++NH3(g)) increased during the episodes, but the ratio of the total amount of these ions to PM10 concentration decreased, indicating unusually high fractions of other chemical components. Particle number size distribution measurements with differential mobility particle sizer (DMPS) revealed that concentrations of particles 90-500 nm increased during the episodes, while concentrations of particles smaller than 90 nm decreased. The reduction of the smallest particles was caused by suppressed new particle formation due to vapour and molecular cluster uptake of LRT particles. Our results show that emissions from wildfires in Russian and other Eastern European countries deteriorated air quality of very large areas

Whole-body nanoparticle aerosol inhalation exposures.

PubMed

Yi, Jinghai; Chen, Bean T; Schwegler-Berry, Diane; Frazer, Dave; Castranova, Vince; McBride, Carroll; Knuckles, Travis L; Stapleton, Phoebe A; Minarchick, Valerie C; Nurkiewicz, Timothy R

2013-05-07

Inhalation is the most likely exposure route for individuals working with aerosolizable engineered nano-materials (ENM). To properly perform nanoparticle inhalation toxicology studies, the aerosols in a chamber housing the experimental animals must have: 1) a steady concentration maintained at a desired level for the entire exposure period; 2) a homogenous composition free of contaminants; and 3) a stable size distribution with a geometric mean diameter < 200 nm and a geometric standard deviation σg < 2.5 (5). The generation of aerosols containing nanoparticles is quite challenging because nanoparticles easily agglomerate. This is largely due to very strong inter-particle forces and the formation of large fractal structures in tens or hundreds of microns in size (6), which are difficult to be broken up. Several common aerosol generators, including nebulizers, fluidized beds, Venturi aspirators and the Wright dust feed, were tested; however, none were able to produce nanoparticle aerosols which satisfy all criteria (5). A whole-body nanoparticle aerosol inhalation exposure system was fabricated, validated and utilized for nano-TiO2 inhalation toxicology studies. Critical components: 1) novel nano-TiO2 aerosol generator; 2) 0.5 m(3) whole-body inhalation exposure chamber; and 3) monitor and control system. Nano-TiO2 aerosols generated from bulk dry nano-TiO2 powders (primary diameter of 21 nm, bulk density of 3.8 g/cm(3)) were delivered into the exposure chamber at a flow rate of 90 LPM (10.8 air changes/hr). Particle size distribution and mass concentration profiles were measured continuously with a scanning mobility particle sizer (SMPS), and an electric low pressure impactor (ELPI). The aerosol mass concentration (C) was verified gravimetrically (mg/m(3)). The mass (M) of the collected particles was determined as M = (Mpost-Mpre), where Mpre and Mpost are masses of the filter before and after sampling (mg). The mass concentration was calculated as C = M

Whole-Body Nanoparticle Aerosol Inhalation Exposures

PubMed Central

Yi, Jinghai; Chen, Bean T.; Schwegler-Berry, Diane; Frazer, Dave; Castranova, Vince; McBride, Carroll; Knuckles, Travis L.; Stapleton, Phoebe A.; Minarchick, Valerie C.; Nurkiewicz, Timothy R.

2013-01-01

Inhalation is the most likely exposure route for individuals working with aerosolizable engineered nano-materials (ENM). To properly perform nanoparticle inhalation toxicology studies, the aerosols in a chamber housing the experimental animals must have: 1) a steady concentration maintained at a desired level for the entire exposure period; 2) a homogenous composition free of contaminants; and 3) a stable size distribution with a geometric mean diameter < 200 nm and a geometric standard deviation σg < 2.5 5. The generation of aerosols containing nanoparticles is quite challenging because nanoparticles easily agglomerate. This is largely due to very strong inter-particle forces and the formation of large fractal structures in tens or hundreds of microns in size 6, which are difficult to be broken up. Several common aerosol generators, including nebulizers, fluidized beds, Venturi aspirators and the Wright dust feed, were tested; however, none were able to produce nanoparticle aerosols which satisfy all criteria 5. A whole-body nanoparticle aerosol inhalation exposure system was fabricated, validated and utilized for nano-TiO2 inhalation toxicology studies. Critical components: 1) novel nano-TiO2 aerosol generator; 2) 0.5 m3 whole-body inhalation exposure chamber; and 3) monitor and control system. Nano-TiO2 aerosols generated from bulk dry nano-TiO2 powders (primary diameter of 21 nm, bulk density of 3.8 g/cm3) were delivered into the exposure chamber at a flow rate of 90 LPM (10.8 air changes/hr). Particle size distribution and mass concentration profiles were measured continuously with a scanning mobility particle sizer (SMPS), and an electric low pressure impactor (ELPI). The aerosol mass concentration (C) was verified gravimetrically (mg/m3). The mass (M) of the collected particles was determined as M = (Mpost-Mpre), where Mpreand Mpost are masses of the filter before and after sampling (mg). The mass concentration was calculated as C = M/(Q*t), where Q is

Evolution of wavelength-dependent mass absorption cross sections of carbonaceous aerosols during the 2010 DOE CARES campaign

NASA Astrophysics Data System (ADS)

Flowers, B. A.; Dubey, M. K.; Subramanian, R.; Sedlacek, A. J.; Kelley, P.; Luke, W. T.; Jobson, B. T.; Zaveri, R. A.

2011-12-01

Predictions of aerosol radiative forcing require process level optical property models that are built on precise and accurate field observations. Evolution of aerosol optical properties for urban influenced carbonaceous aerosol undergoing transport and mixing with rural air masses was a focal point of the DOE Carbonaceous Aerosol and Radiative Effects (CARES) campaign near Sacramento, CA in summer 2010. Urban aerosol was transported from Sacramento, CA (T0) to the foothills of the Sierra Nevada Mountains to a rural site located near Cool, CA (T1). Aerosol absorption and scattering coefficients were measured at the T0 and T1 sites using integrated photoacoustic acoustic/nephelometer instruments (PASS-3 and PASS-UV) at 781, 532, 405, and 375 nm. Single particle soot photometry (SP2) instrumentation was used to monitor black carbon (BC) mass at both sites. Combining data from these sensors allows estimate of the wavelength-dependent mass absorption coefficient (MAC(λ)) and partitioning of MAC(λ) into contributions from the BC core and from enhancements from coating of BC cores. MAC(λ) measured in this way is free of artifacts associated with filter-based aerosol absorption measurements and takes advantage of the single particle sensitivity of the SP2 instrument, allowing observation of MAC(λ) on 10 minute and faster time scales. Coating was observed to enhance MAC(λ) by 20 - 30 % and different wavelength dependence for MAC(λ) was observed for urban and biomass burning aerosol. Further, T0 - T1 evolution of MAC(λ) was correlated with separately measured NO/NOy ratios and CO/CO2 ratios to understand the effects of aging & transport on MAC(λ) and the implications of aerosol processing that links air quality to radiative forcing on a regional scale. Aircraft observations made from the Gulfstream-1 during CARES are also analyzed to enhance process level understanding of the optical properties of fresh and aged carbonaceous aerosol in the urban-rural interface.

Measurements of Organic Composition of Aerosol and Rainwater Samples Using Offline Aerosol Mass Spectrometry

NASA Astrophysics Data System (ADS)

OBrien, R. E.; Ridley, K. J.; Canagaratna, M. R.; Croteau, P.; Budisulistiorini, S. H.; Cui, T.; Green, H. S.; Surratt, J. D.; Jayne, J. T.; Kroll, J. H.

2016-12-01

A thorough understanding of the sources, evolution, and budgets of atmospheric organic aerosol requires widespread measurements of the amount and chemical composition of atmospheric organic carbon in the condensed phase (within particles and water droplets). Collecting such datasets requires substantial spatial and temporal (long term) coverage, which can be challenging when relying on online measurements by state-of-the-art research-grade instrumentation (such as those used in atmospheric chemistry field studies). Instead, samples are routinely collected using relatively low-cost techniques, such as aerosol filters, for offline analysis of their chemical composition. However, measurements made by online and offline instruments can be fundamentally different, leading to disparities between data from field studies and those from more routine monitoring. To better connect these two approaches, and take advantage of the benefits of each, we have developed a method to introduce collected samples into online aerosol instruments using nebulization. Because nebulizers typically require tens to hundreds of milliliters of solution, limiting this technique to large samples, we developed a new, ultrasonic micro-nebulizer that requires only small volumes (tens of microliters) of sample for chemical analysis. The nebulized (resuspended) sample is then sent into a high-resolution Aerosol Mass Spectrometer (AMS), a widely-used instrument that provides key information on the chemical composition of aerosol particulate matter (elemental ratios, carbon oxidation state, etc.), measurements that are not typically made for collected atmospheric samples. Here, we compare AMS data collected using standard on-line techniques with our offline analysis, demonstrating the utility of this new technique to aerosol filter samples. We then apply this approach to organic aerosol filter samples collected in remote regions, as well as rainwater samples from across the US. This data provides

Time Resolved Measurements of Primary Biogenic Aerosol Particles in Amazonia

NASA Astrophysics Data System (ADS)

Wollny, A. G.; Garland, R.; Pöschl, U.

2009-04-01

Biogenic aerosols are ubiquitous in the Earth's atmosphere and they influence atmospheric chemistry and physics, the biosphere, climate, and public health. They play an important role in the spread of biological organisms and reproductive materials, and they can cause or enhance human, animal, and plant diseases. Moreover, they influence the Earth's energy budget by scattering and absorbing radiation, and they can initiate the formation of clouds and precipitation as cloud condensation and ice nuclei. The composition, abundance, and origin of biogenic aerosol particles and components are, however, still not well understood and poorly quantified. Prominent examples of primary biogenic aerosol particles, which are directly emitted from the biosphere to the atmosphere, are pollen, bacteria, fungal spores, viruses, and fragments of animals and plants. During the Amazonian Aerosol Characterization Experiment (AMAZE-08) a large number of aerosol and gas-phase measurements were taken on a remote site close to Manaus, Brazil, during a period of five weeks in February and March 2008. This presented study is focused on data from an ultraviolet aerodynamic particle sizer (UVAPS, TSI inc.) that has been deployed for the first time in Amazonia. In this instrument, particle counting and aerodynamic sizing over the range of 0.5-20 µm are complemented by the measurement of UV fluorescence at 355 nm (excitation) and 420-575 nm (emission), respectively. Fluorescence at these wavelengths is characteristic for reduced pyridine nucleotides (e.g., NAD(P)H) and for riboflavin, which are specific for living cells. Thus particles exhibiting fluorescence signals can be regarded as "viable aerosols" or "fluorescent bioparticles" (FBAP), and their concentration can be considered as lower limit for the actual abundance of primary biogenic aerosol particles. Data from the UVAPS were averaged over 5 minute time intervals. The presence of bioparticles in the observed size range has been

Volume changes upon heating of aerosol particles from biomass burning using transmission electron microscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Adachi, Kouji; Sedlacek, Arthur J.; Kleinman, Lawrence

The responses of aerosol particles to heating are important for measurements of their chemical, physical, and optical properties, classification, and determination of origin. However, the thermal behavior of organic aerosol particles is largely unknown. We provide a method to analyze such thermal behavior through heating from room temperature to >600°C by using a heating holder within a transmission electron microscope (TEM). Here we describe in-situ shape and size changes and variations in the compositions of individual particles before and after heating. We use ambient samples from wildland and agricultural biomass fires in North America collected during the 2013 Biomass Burnmore » Observation Project (BBOP). The results indicate that individual tar balls (TB; spherical organic material) from biomass burning retained, on average, up to 30% of their volume when heated to 600°C. Chemical analysis reveals that K and Na remain in the residues, whereas S and O were lost. In contrast to bulk sample measurements of carbonaceous particles using thermal/optical carbon analyzers, our single-particle results imply that many individual organic particles consist of multiple types of organic matter having different thermal stabilities. Beyond TBs, our results suggest that because of their thermal stability some organic particles may not be detectable by using aerosol mass spectrometry or thermal/optical carbon analyzers. This result can lead to an underestimate of the abundance of TBs and other organic particles, and therefore biomass burning may have more influence than currently recognized in regional and global climate models.« less

Volume changes upon heating of aerosol particles from biomass burning using transmission electron microscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Adachi, Kouji; Sedlacek, Arthur J.; Kleinman, Lawrence

Here, the responses of aerosol particles to heating are important for measurements of their chemical, physical, and optical properties, classification, and determination of origin. However, the thermal behavior of organic aerosol particles is largely unknown. We provide a method to analyze such thermal behavior through heating from room temperature to >600°C by using a heating holder within a transmission electron microscope (TEM). Here we describe in-situ shape and size changes and variations in the compositions of individual particles before and after heating. We use ambient samples from wildland and agricultural biomass fires in North America collected during the 2013 Biomassmore » Burn Observation Project (BBOP). The results indicate that individual tar balls (TB; spherical organic material) from biomass burning retained, on average, up to 30% of their volume when heated to 600°C. Chemical analysis reveals that K and Na remain in the residues, whereas S and O were lost. In contrast to bulk sample measurements of carbonaceous particles using thermal/optical carbon analyzers, our single-particle results imply that many individual organic particles consist of multiple types of organic matter having different thermal stabilities. Beyond TBs, our results suggest that because of their thermal stability some organic particles may not be detectable by using aerosol mass spectrometry or thermal/optical carbon analyzers. This result can lead to an underestimate of the abundance of TBs and other organic particles, and therefore biomass burning may have more influence than currently recognized in regional and global climate models.« less

Volume changes upon heating of aerosol particles from biomass burning using transmission electron microscopy

DOE PAGES

Adachi, Kouji; Sedlacek, Arthur J.; Kleinman, Lawrence; ...

2017-09-26

Here, the responses of aerosol particles to heating are important for measurements of their chemical, physical, and optical properties, classification, and determination of origin. However, the thermal behavior of organic aerosol particles is largely unknown. We provide a method to analyze such thermal behavior through heating from room temperature to >600°C by using a heating holder within a transmission electron microscope (TEM). Here we describe in-situ shape and size changes and variations in the compositions of individual particles before and after heating. We use ambient samples from wildland and agricultural biomass fires in North America collected during the 2013 Biomassmore » Burn Observation Project (BBOP). The results indicate that individual tar balls (TB; spherical organic material) from biomass burning retained, on average, up to 30% of their volume when heated to 600°C. Chemical analysis reveals that K and Na remain in the residues, whereas S and O were lost. In contrast to bulk sample measurements of carbonaceous particles using thermal/optical carbon analyzers, our single-particle results imply that many individual organic particles consist of multiple types of organic matter having different thermal stabilities. Beyond TBs, our results suggest that because of their thermal stability some organic particles may not be detectable by using aerosol mass spectrometry or thermal/optical carbon analyzers. This result can lead to an underestimate of the abundance of TBs and other organic particles, and therefore biomass burning may have more influence than currently recognized in regional and global climate models.« less

Aerosol transport over the western Mediterranean basin: Evidence of the contribution of fine particles to desert dust plumes over Alborán Island

NASA Astrophysics Data System (ADS)

Valenzuela, A.; Olmo, F. J.; Lyamani, H.; Granados-Muñoz, M. J.; Antón, M.; Guerrero-Rascado, J. L.; Quirantes, A.; Toledano, C.; Perez-Ramírez, D.; Alados-Arboledas, L.

2014-12-01

Eight months (June 2011 to January 2012) of aerosol property data were obtained at the remote site of Alborán Island (35.95°N, 3.03°W) in the western Mediterranean basin. The aim of this work is to assess the aerosol properties according to air mass origin and transport over this remote station with a special focus on air mass transport from North Africa. For air masses coming from North Africa, different aerosol properties showed strong contributions from mineral dust lifted from desert areas. Nevertheless, during these desert dust intrusions, some atmospheric aerosol properties are clearly different from pure mineral dust particles. Thus, Angström exponent α(440-870) presents larger values than those reported for pure desert dust measured close to dust source regions. These results combine with α(440, 670) - α(670, 870) ≥ 0.1 and low single scattering albedo (ω(λ)) values, especially at the largest wavelengths. Most of the desert dust intrusions over Alborán can be described as a mixture of dust and anthropogenic particles. The analyses support that our results apply to North Africa desert dust air masses transported from different source areas. Therefore, our results indicate a significant contribution of fine absorbing particles during desert dust intrusions over Alborán arriving from different source regions. The aerosol optical depth data retrieved from Sun photometer measurements have been used to check Moderate Resolution Imaging Spectroradiometer retrievals, and they show reasonable agreement, especially for North African air masses.

New apparatus of single particle trap system for aerosol visualization

NASA Astrophysics Data System (ADS)

Higashi, Hidenori; Fujioka, Tomomi; Endo, Tetsuo; Kitayama, Chiho; Seto, Takafumi; Otani, Yoshio

2014-08-01

Control of transport and deposition of charged aerosol particles is important in various manufacturing processes. Aerosol visualization is an effective method to directly observe light scattering signal from laser-irradiated single aerosol particle trapped in a visualization cell. New single particle trap system triggered by light scattering pulse signal was developed in this study. The performance of the device was evaluated experimentally. Experimental setup consisted of an aerosol generator, a differential mobility analyzer (DMA), an optical particle counter (OPC) and the single particle trap system. Polystylene latex standard (PSL) particles (0.5, 1.0 and 2.0 μm) were generated and classified according to the charge by the DMA. Singly charged 0.5 and 1.0 μm particles and doubly charged 2.0 μm particles were used as test particles. The single particle trap system was composed of a light scattering signal detector and a visualization cell. When the particle passed through the detector, trigger signal with a given delay time sent to the solenoid valves upstream and downstream of the visualization cell for trapping the particle in the visualization cell. The motion of particle in the visualization cell was monitored by CCD camera and the gravitational settling velocity and the electrostatic migration velocity were measured from the video image. The aerodynamic diameter obtained from the settling velocity was in good agreement with Stokes diameter calculated from the electrostatic migration velocity for individual particles. It was also found that the aerodynamic diameter obtained from the settling velocity was a one-to-one function of the scattered light intensity of individual particles. The applicability of this system will be discussed.

Interactions between meteoric smoke particles and the stratospheric aerosol layer

NASA Astrophysics Data System (ADS)

Mann, G. W.; Marshall, L.; Brooke, J. S. A.; Dhomse, S.; Plane, J. M. C.; Feng, W.; Neely, R.; Bardeen, C.; Bellouin, N.; Dalvi, M.; Johnson, C.; Abraham, N. L.; Schmidt, A.; Carslaw, K. S.; Chipperfield, M.; Deshler, T.; Thomason, L. W.

2017-12-01

In-situ measurements in the Arctic, Antarctic and at mid-latitudes suggest a widespread presence of meteoric smoke particles (MSPs), as an inclusion within a distinct class of stratospheric aerosol particles. We apply the UM-UKCA stratosphere-troposphere composition-climate model, with interactive aerosol microphysics, to map the global distribution of these "meteoric-sulphuric particles" and explore the implications of their presence. Comparing to balloon-borne stratospheric aerosol measurements, we indirectly constrain the uncertain MSP flux into the upper mesosphere, and assess whether meteoric inclusion can explain observed refractory/non-volatile particle concentrations. Our experiments suggest meteoric-sulphuric particles are present at all latitudes, the Junge layer transitioning from mostly homogeneously nucleated particles at the bottom, to mostly meteoric-sulphuric particles at the top. We find MSPs exert a major influence on the quiescent Junge layer, with meteoric-sulphuric particles generally bigger than homogeneously nucleated particles, and therefore more rapidly removed into the upper troposphere. Resolving the smoke interactions weakens homogeneous nucleation in polar spring, reduces the quiescent sulphur burden, and improves comparisons to a range of different stratospheric aerosol measurements. The refractory nature of meteoric-sulphuric particles also means they "survive" ascent through the uppermost Junge layer, whereas homogeneously nucleated particles evaporate completely. Simulations through the Pinatubo-perturbed period are more realistic, with greater volcanic enhancement of effective radius, causing faster decay towards quiescent conditions, both effects matching better with observations. Overall, our experiments suggest meteoric-sulphuric particles are an important component of the Junge layer, strongly influential in both quiescent and volcanically perturbed conditions.

Physical and Optical/Radiative Characteristics of Aerosol and Cloud Particles in Tropical Cirrus: Importance in Radiation Balance

NASA Technical Reports Server (NTRS)

Pueschel, R. F.; Howard, S. D.; Foster, T. C.; Hallett, J.; Arnott, W. P.; Condon, Estelle P. (Technical Monitor)

1996-01-01

Whether cirrus clouds heat or cool the Earth-atmosphere system depends on the relative importance of the cloud shortwave albedo effect and the cloud thermal greenhouse effect. Both are determined by the distribution of ice condensate with cloud particle size. The microphysics instrument package flown aboard the NASA DC-8 in TOGA/COARE included an ice crystal replicator, a 2D Greyscale Cloud Particle Probe and a Forward Scattering Spectrometer Aerosol Probe. In combination, the electro-optical instruments permitted particle size measurements between 0.5 micrometer and 2.6 millimeter diameter. Ice crystal replicas were used to validate signals from the electrooptical instruments. Both optical and scanning electron microscopy were utilized to analyze aerosol and ice particle replicas between 0.1 micrometer and several 100 micrometer diameter. In first approximation, the combined aerosol-cloud particle spectrum in several clouds followed a power law N alpha D(sup -2.5). Thus, large cloud particles carried most of the condensate mass, while small cloud and aerosol particles determined the surface area. The mechanism of formation of small particles is growth of (hygroscopic, possibly ocean-derived) aerosol particles along the Kohler curves. The concentration of small particles is higher and less variable in space and time, and their tropospheric residence time is longer, than those of large cloud particles because of lower sedimentation velocities. Small particles shift effective cloud particle radii to sizes much smaller than the mean diameter of the cloud particles. This causes an increase in shortwave reflectivity and IR emissivity, and a decrease in transmissivity. Occasionally, the cloud reflectivity increased with altitude (decreasing temperature) stronger than did cloud emissivity, yielding enhanced radiative cooling at higher altitudes. Thus, cirrus produced by deep convection in the tropics may be critical in controlling processes whereby energy from warm

Measuring Sodium Chloride Contents of Aerosols

NASA Technical Reports Server (NTRS)

Sinha, M. P.; Friedlander, S. K.

1986-01-01

Amount of sodium chloride in individual aerosol particles measured in real time by analyzer that includes mass spectrometer. Analyzer used to determine mass distributions of active agents in therapeutic or diagnostic aerosols derived from saline solutions and in analyzing ocean spray. Aerosol particles composed of sodium chloride introduced into oven, where individually vaporized on hot wall. Vapor molecules thermally dissociated, and some of resulting sodium atoms ionized on wall. Ions leave oven in burst and analyzed by spectrometer, which is set to monitor sodium-ion intensity.

Synchronised Aerosol Mass Spectrometer Measurements across Europe

NASA Astrophysics Data System (ADS)

Nemitz, Eiko

2010-05-01

Up to twelve Aerodyne Aerosol Mass Spectrometers (AMSs) were operated simultaneously at rural and background stations (EMEP and EUSAAR sites) across Europe. Measurements took place during three intensive periods, in collaboration between the European EUCAARI IP and the EMEP monitoring activities under the UNECE Convention for Long-Range Transboundary Air Pollution (CLRTAP) during three contrasting months (May 2008, Sep/Oct 2008, Feb/Mar 2009). These measurements were conducted, analysed and quality controlled carefully using a unified protocol, providing the largest spatial database of aerosol chemical composition measured with a unified online technique to date, and a unique snapshots of the European non-refractory submicron aerosol climatology. As campaign averages over all active monitoring sites, organics represent 28 to 43%, sulphate 18 to 25%, ammonium 13 to 15% and nitrate 15 to 36% of the resolved aerosol mass, with the highest relative nitrate contribution during the Feb/Mar campaign. The measurements demonstrate that in NW Europe (e.g. Ireland, UK, The Netherlands, Germany, Switzerland) the regional submicron aerosol tends to be neutralised and here nitrates make a major contribution to the aerosol mass. By contrast, periods with low nitrate and acidic aerosol were observed at sites in S and E Europe (e.g. Greece, Finland), presumably due to a combination of larger SO2 point sources in Easter Europe, smaller local NH3 sources and, in the case of Greece, higher temperatures. While at the more marine and remote sites (Ireland, Scotland, Finland) nitrate concentrations were dominated by episodic transport phenomena, at continental sites (Switzerland, Germany, Hungary) nitrate followed a clear diurnal cycle, reflecting the thermodynamic behaviour of ammonium nitrate. The datasets clearly shows spatially co-ordinated, large-scale pollution episodes of organics, sulphate and nitrate, the latter being most pronounced during the Feb/Mar campaign. At selected

Inhomogeneities in particle composition of single, levitated aerosol particles observed by Mie resonance spectroscopy

NASA Astrophysics Data System (ADS)

Krieger, Ulrich; Lienhard, Daniel; Bastelberger, Sandra; Steimer, Sarah

2014-05-01

Recent observations have indicated that organic aerosol particles in the atmosphere may exist in an amorphous semi-solid or even solid (i.e. glassy) state, e.g. [1]. The influence of highly viscous and glassy states on the timescale of aerosol particle equilibration with respect to water vapor have been investigated for some model systems of atmospheric aerosol, e.g. [2,3]. In particular, it has been shown that the kinetics of the water absorption/desorption process is controlled entirely by liquid-phase diffusion of water molecules for a highly viscous aerosol particle. A liquid phase diffusion model based on numerically solving the non-linear diffusion equation predicts strong internal gradients in water concentration when condensed phase diffusion impedes the water uptake from the gas phase [2]. Here we observe and quantify the internal concentration gradients in single, levitated, micron size aerosol particles of aqueous shikimic acid using elastic Mie resonance spectroscopy. A single, aqueous particle is levitated in an electro-dynamic balance (for details see [2]), dried for several days at room temperature, cooled to the target temperature and exposed to a rapid change in relative humidity. In addition to measuring the elastically backscattered light of a "white light" LED source and recording the full spectrum with a spectrograph as in [2], we use a tunable diode laser (TDL) to scan high resolution TE- and TM spectra. This combination allows observing various Mie resonance mode orders simultaneously. Since we perform the experiment at low temperatures and low humidities the changes in the Mie-spectra due to water uptake are sufficiently slow to resolve the kinetics. Experimental Mie resonance spectra are inverted to concentration profiles of water within the particle by applying the numerical diffusion model [2] in conjunction with Mie calculations of multilayered spheres [4]. [1] A. Virtanen et al. (2010): An amorphous solid state of biogenic secondary

Relationships among particle number, surface area, and respirable mass concentrations in automotive engine manufacturing.

PubMed

Heitbrink, William A; Evans, Douglas E; Ku, Bon Ki; Maynard, Andrew D; Slavin, Thomas J; Peters, Thomas M

2009-01-01

This study investigated the relationships between particle number, surface area, and respirable mass concentration measured simultaneously in a foundry and an automotive engine machining and assembly center. Aerosol concentrations were measured throughout each plant with a condensation particle counter for number concentration, a diffusion charger for active surface area concentration, and an optical particle counter for respirable mass concentration. At selected locations, particle size distributions were characterized with the optical particle counter and an electrical low pressure impactor. Statistical analyses showed that active surface area concentration was correlated with ultrafine particle number concentration and weakly correlated with respirable mass concentration. Correlation between number and active surface area concentration was stronger during winter (R2 = 0.6 for both plants) than in the summer (R2 = 0.38 and 0.36 for the foundry and engine plant respectively). The stronger correlation in winter was attributed to use of direct-fire gas fired heaters that produced substantial numbers of ultrafine particles with a modal diameter between 0.007 and 0.023 mu m. These correlations support findings obtained through theoretical analysis. Such analysis predicts that active surface area increasingly underestimates geometric surface area with increasing particle size, particularly for particles larger than 100 nm. Thus, a stronger correlation between particle number concentration and active surface area concentration is expected in the presence of high concentrations of ultrafine particles. In general, active surface area concentration may be a concentration metric that is distinct from particle number concentration and respirable mass concentration. For future health effects or toxicological studies involving nano-materials or ultrafine aerosols, this finding needs to be considered, as exposure metrics may influence data interpretation.

Design of Aerosol Particle Coating: Thickness, Texture and Efficiency

PubMed Central

Buesser, B.; Pratsinis, S.E.

2013-01-01

Core-shell particles preserve the performance (e.g. magnetic, plasmonic or opacifying) of a core material while modifying its surface with a shell that facilitates (e.g. by blocking its reactivity) their incorporation into a host liquid or polymer matrix. Here coating of titania (core) aerosol particles with thin silica shells (films or layers) is investigated at non-isothermal conditions by a trimodal aerosol dynamics model, accounting for SiO2 generation by gas phase and surface oxidation of hexamethyldisiloxane (HMDSO) vapor, coagulation and sintering. After TiO2 particles have reached their final primary particle size (e.g. upon completion of sintering during their flame synthesis), coating starts by uniformly mixing them with HMDSO vapor that is oxidized either in the gas phase or on the particles’ surface resulting in SiO2 aerosols or deposits, respectively. Sintering of SiO2 deposited onto the core TiO2 particles takes place transforming rough into smooth coating shells depending on process conditions. The core-shell characteristics (thickness, texture and efficiency) are calculated for two limiting cases of coating shells: perfectly smooth (e.g. hermetic) and fractal-like. At constant TiO2 core particle production rate, the influence of coating weight fraction, surface oxidation and core particle size on coating shell characteristics is investigated and compared to pertinent experimental data through coating diagrams. With an optimal temperature profile for complete precursor conversion, the TiO2 aerosol and SiO2-precursor (HMDSO) vapor concentrations have the strongest influence on product coating shell characteristics. PMID:23729833

Growth rates of fine aerosol particles at a site near Beijing in June 2013

NASA Astrophysics Data System (ADS)

Zhao, Chuanfeng; Li, Yanan; Zhang, Fang; Sun, Yele; Wang, Pucai

2018-02-01

Growth of fine aerosol particles is investigated during the Aerosol-CCN-Cloud Closure Experiment campaign in June 2013 at an urban site near Beijing. Analyses show a high frequency (˜ 50%) of fine aerosol particle growth events, and show that the growth rates range from 2.1 to 6.5 nm h-1 with a mean value of ˜ 5.1 nm h-1. A review of previous studies indicates that at least four mechanisms can affect the growth of fine aerosol particles: vapor condensation, intramodal coagulation, extramodal coagulation, and multi-phase chemical reaction. At the initial stage of fine aerosol particle growth, condensational growth usually plays a major role and coagulation efficiency generally increases with particle sizes. An overview of previous studies shows higher growth rates over megacity, urban and boreal forest regions than over rural and oceanic regions. This is most likely due to the higher condensational vapor, which can cause strong condensational growth of fine aerosol particles. Associated with these multiple factors of influence, there are large uncertainties for the aerosol particle growth rates, even at the same location.

Linking variations in sea spray aerosol particle hygroscopicity to composition during two microcosm experiments

NASA Astrophysics Data System (ADS)

Forestieri, Sara D.; Cornwell, Gavin C.; Helgestad, Taylor M.; Moore, Kathryn A.; Lee, Christopher; Novak, Gordon A.; Sultana, Camille M.; Wang, Xiaofei; Bertram, Timothy H.; Prather, Kimberly A.; Cappa, Christopher D.

2016-07-01

The extent to which water uptake influences the light scattering ability of marine sea spray aerosol (SSA) particles depends critically on SSA chemical composition. The organic fraction of SSA can increase during phytoplankton blooms, decreasing the salt content and therefore the hygroscopicity of the particles. In this study, subsaturated hygroscopic growth factors at 85 % relative humidity (GF(85 %)) of predominately submicron SSA particles were quantified during two induced phytoplankton blooms in marine aerosol reference tanks (MARTs). One MART was illuminated with fluorescent lights and the other was illuminated with sunlight, referred to as the "indoor" and "outdoor" MARTs, respectively. Optically weighted GF(85 %) values for SSA particles were derived from measurements of light scattering and particle size distributions. The mean optically weighted SSA diameters were 530 and 570 nm for the indoor and outdoor MARTs, respectively. The GF(85 %) measurements were made concurrently with online particle composition measurements, including bulk composition (using an Aerodyne high-resolution aerosol mass spectrometer) and single particle (using an aerosol time-of-flight mass spectrometer) measurement, and a variety of water-composition measurements. During both microcosm experiments, the observed optically weighted GF(85 %) values were depressed substantially relative to pure inorganic sea salt by 5 to 15 %. There was also a time lag between GF(85 %) depression and the peak chlorophyll a (Chl a) concentrations by either 1 (indoor MART) or 3-to-6 (outdoor MART) days. The fraction of organic matter in the SSA particles generally increased after the Chl a peaked, also with a time lag, and ranged from about 0.25 to 0.5 by volume. The observed depression in the GF(85 %) values (relative to pure sea salt) is consistent with the large observed volume fractions of non-refractory organic matter (NR-OM) comprising the SSA. The GF(85 %) values exhibited a reasonable negative

Evaluations of tropospheric aerosol properties simulated by the community earth system model with a sectional aerosol microphysics scheme

PubMed Central

Toon, Owen B.; Bardeen, Charles G.; Mills, Michael J.; Fan, Tianyi; English, Jason M.; Neely, Ryan R.

2015-01-01

Abstract A sectional aerosol model (CARMA) has been developed and coupled with the Community Earth System Model (CESM1). Aerosol microphysics, radiative properties, and interactions with clouds are simulated in the size‐resolving model. The model described here uses 20 particle size bins for each aerosol component including freshly nucleated sulfate particles, as well as mixed particles containing sulfate, primary organics, black carbon, dust, and sea salt. The model also includes five types of bulk secondary organic aerosols with four volatility bins. The overall cost of CESM1‐CARMA is approximately ∼2.6 times as much computer time as the standard three‐mode aerosol model in CESM1 (CESM1‐MAM3) and twice as much computer time as the seven‐mode aerosol model in CESM1 (CESM1‐MAM7) using similar gas phase chemistry codes. Aerosol spatial‐temporal distributions are simulated and compared with a large set of observations from satellites, ground‐based measurements, and airborne field campaigns. Simulated annual average aerosol optical depths are lower than MODIS/MISR satellite observations and AERONET observations by ∼32%. This difference is within the uncertainty of the satellite observations. CESM1/CARMA reproduces sulfate aerosol mass within 8%, organic aerosol mass within 20%, and black carbon aerosol mass within 50% compared with a multiyear average of the IMPROVE/EPA data over United States, but differences vary considerably at individual locations. Other data sets show similar levels of comparison with model simulations. The model suggests that in addition to sulfate, organic aerosols also significantly contribute to aerosol mass in the tropical UTLS, which is consistent with limited data. PMID:27668039

Ice nucleation properties of atmospheric aerosol particles collected during a field campaign in Cyprus

NASA Astrophysics Data System (ADS)

Yordanova, Petya; Maier, Stefanie; Lang-Yona, Naama; Tamm, Alexandra; Meusel, Hannah; Pöschl, Ulrich; Weber, Bettina; Fröhlich-Nowoisky, Janine

2017-04-01

Atmospheric aerosol particles, including desert and soil dust as well as marine aerosols, are well known to act as ice nuclei (IN) and thus have been investigated in numerous ice nucleation studies. Based on their cloud condensation nuclei potential and their impacts on radiative properties of clouds (via scattering and absorption of solar radiation), aerosol particles may significantly affect the cloud and precipitation development. Atmospheric aerosols of the Eastern Mediterranean have been described to be dominated by desert dust, but only little is known on their composition and ice nucleating properties. In this study we investigated the ice nucleating ability of total suspended particles (TSP), collected at the remote site Agia Marina Xyliatou on Cyprus during a field campaign in April 2016. Airborne TSP samples containing air masses of various types such as African (Saharan) and Arabian dust and European and Middle Eastern pollution were collected on glass fiber filters at 24 h intervals. Sampling was performed ˜5 m above ground level and ˜521 m above sea level. During the sampling period, two major dust storms (PM 10max 118 μg/m3 and 66 μg/m3) and a rain event (rainfall amount: 3.4 mm) were documented. Chemical and physical characterizations of the particles were analyzed experimentally through filtration, thermal, chemical and enzyme treatments. Immersion freezing experiments were performed at relatively high subzero temperatures (-1 to -15˚ C) using the mono ice nucleation array. Preliminary results indicate that highest IN particle numbers (INPs) occurred during the second dust storm event with lower particle concentrations. Treatments at 60˚ C lead to a gradual IN deactivation, indicating the presence of biological INPs, which were observed to be larger than 300 kDa. Additional results originating from this study will be shown. Acknowledgement: This work was funded by the DFG Ice Nuclei Research Unit (INUIT).

Satellite measurement of aerosol mass over land

NASA Technical Reports Server (NTRS)

Fraser, R. S.; Kaufman, Y. J.; Mahoney, R. L.

1984-01-01

The estimation of aerosol optical thickness and mass from satellite observations over land is demonstrated using data from the GOES Visible/IR Spin-Scan Radiometer for the eastern U.S. The post-launch calibration technique is described; the algorithm used to derive optical thickness from the radiance of scattered sunlight (by means of a radiative-transfer model in which the optical characteristics of the aerosol are assumed) is presented; and data on aerosol S for July 31, 1980 are analyzed. The results are presented in a series of graphs and maps and compared with ground-based data. The errors in the optical thickness and columnar mass are estimated as 15 and 40 percent, respectively, and the need for independent-data-set validation of satellite-based mass, transport, and divergence values is indicated.

Thermophoretic separation of aerosol particles from a sampled gas stream

DOEpatents

Postma, Arlin K.

1986-01-01

A method for separating gaseous samples from a contained atmosphere that includes aerosol particles uses the step of repelling particles from a gas permeable surface or membrane by heating the surface to a temperature greater than that of the surrounding atmosphere. The resulting thermophoretic forces maintain the gas permeable surface clear of aerosol particles. The disclosed apparatus utilizes a downwardly facing heated plate of gas permeable material to combine thermophoretic repulsion and gravity forces to prevent particles of any size from contacting the separating plate surfaces.

Is the gas-particle partitioning in alpha-pinene secondary organic aerosol reversible?

NASA Astrophysics Data System (ADS)

Grieshop, Andrew P.; Donahue, Neil M.; Robinson, Allen L.

2007-07-01