Characterizing and Understanding Aerosol Optical Properties: CARES - Final Report

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

Cappa, Christopher D; Atkinson, Dean B

The scientific focus of this study was to use ambient measurements to develop new insights into the understanding of the direct radiative forcing by atmospheric aerosol particles. The study used data collected by the PI’s and others as part of both the 2010 U.S. Department of Energy (DOE) sponsored Carbonaceous Aerosols and Radiative Effects Study (CARES), which took place in and around Sacramento, CA, and the 2012 Clean Air for London (ClearfLo) study. We focus on measurements that were made of aerosol particle optical properties, namely the wavelength-dependent light absorption, scattering and extinction. Interpretation of these optical property measurements ismore » facilitated through consideration of complementary measurements of the aerosol particle chemical composition and size distributions. With these measurements, we addressed the following general scientific questions: 1. How does light scattering and extinction by atmospheric aerosol particles depend on particle composition, water uptake, and size? 2. To what extent is light absorption by aerosol particles enhanced through the mixing of black carbon with other particulate components? 3. What relationships exist between intensive aerosol particle optical properties, and how do these depend on particle source and photochemical aging? 4. How well do spectral deconvolution methods, which are commonly used in remote sensing, retrieve information about particle size distributions?« less

Column-integrated aerosol optical properties of coarse- and fine-mode particles over the Pearl River Delta region in China.

PubMed

Mai, B; Deng, X; Xia, X; Che, H; Guo, J; Liu, X; Zhu, J; Ling, C

2018-05-01

The sun-photometer data from 2011 to 2013 at Panyu site (Panyu) and from 2007 to 2013 at Dongguan site (Dg) in the Pearl River Delta region, were used for the retrieving of the aerosol optical depth (AOD), single scattering albedo (SSA), Ångström exponent (AE) and volume size distribution of coarse- and fine-mode particles. The coarse-mode particles presented low AOD (ranging from 0.05±0.03 to 0.08±0.05) but a strong absorption property (SSA ranged from 0.70±0.03 to 0.90±0.02) for the wavelengths between 440 and 1020nm. However, these coarse particles accounted for <10% of the total particles. The AOD of fine particles (AODf) was over 3 times as large as that of coarse particles (AODc). The fine particles SSA (SSAf) generally decreased as a function of wavelength, and the relatively lower SSAf value in summer was likely to be due to the stronger solar radiation and higher temperature. More than 70% of the aerosols at Panyu site were dominated by fine-mode absorbing particles, whereas about 70% of the particles at Dg site were attributed to fine-mode scattering particles. The differences of the aerosol optical properties between the two sites are likely associated with local emissions of the light-absorbing carbonaceous aerosols and the scattering aerosols (e.g., sulfate and nitrate particles) caused by the gas-phase oxidation of gaseous precursors (e.g., SO 2 and NO 2 ). The size distribution exhibited bimodal structures in which the accumulation mode was predominant. The fine-mode volume showed positive dependence on AOD (500nm), and the growth of peak value of the fine-mode volume was higher than that of the coarse volume. Both the AOD and SSA increased with increasing relative humidity (RH), while the AE decreased with increasing RH. These correlations imply that the aerosol properties are greatly modified by condensation growth. Copyright © 2017 Elsevier B.V. All rights reserved.

Aircraft observations of the physical and radiative properties of biomass aerosol particles during SAFARI-2000.

NASA Astrophysics Data System (ADS)

Osborne, S. R.; Haywood, J. M.

2001-12-01

An initial analysis will be shown from the ~80 h of data collected between 2--18 September 2000 by the UK Met Office C-130 aircraft during the dry season campaign of the Southern African Regional Science Initiative (SAFARI-2000). The talk will concentrate on the physical and optical properties of the biomass aerosol. The evolution of the particle size spectrum and its optical properties at emission and after ageing will be shown. The vertical distribution of the biomass plume over the land and sea will be compared in view of the local meteorology. A generalised three log-normal model is shown to represent aged biomass aerosol over the sea areas, both in terms of the number and mass particle size spectra, but also derived optical properties (e.g. asymmetry factor, single scatter albedo (ω 0) and extinction coefficient) as calculated using Mie theory and appropriate refractive indices. ω 0 was determined independently using a particle soot absorption photometer (giving the absorption coefficient at a wavelength of 0.567 μ m) and a nephelometer (giving the scattering coefficients at 0.45, 0.55 and 0.65 μ m). Good agreement was found between the measurements and those obtained from the Mie calculations and observed size distributions. A typical value of ω 0 at 0.55 μ m for aged biomass aerosol was 0.90. The radiative properties of the biomass aerosol over both land and sea will be summarised. Stratocumulus cloud was present on some of the days over the sea and the surprising lack of interaction between the elevated biomass plume (containing significant levels of cloud condensation nuclei) and the cloud capping the marine boundary layer will be illustrated. Using the cloud-free and cloudy case studies we can begin to elucidate the levels of direct and indirect forcing of the biomass aerosol on a regional scale. >http://www.mrfnet.demon.co.uk/africa/SAFARI2000.htm

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

Modeling the Relationships Between Aerosol Properties and the Direct and Indirect Effects of Aerosols on Climate

NASA Technical Reports Server (NTRS)

Toon, Owen B.

1994-01-01

Aerosols may affect climate directly by scattering and absorbing visible and infrared energy, They may also affect climate indirectly by modifying the properties of clouds through microphysical processes, and by altering abundances of radiatively important gases through heterogeneous chemistry. Researchers understand which aerosol properties control the direct effect of aerosols on the radiation budget. Unfortunately, despite an abundance of data on certain types of aerosols, much work remains to be done to determine the values of these properties. For instance we have little idea about the global distribution, seasonal variation, or interannual variability of the aerosol optical depth. Also we do not know the visible light absorption properties of tropical aerosols which may contain much debris from slash and burn agriculture. A positive correlation between aerosol concentrations and albedos of marine stratus clouds is observed, and the causative microphysics is understood. However, models suggest that it is difficult to produce new particles in the marine boundary layer. Some modelers have suggested that the particles in the marine boundary layer may originate in the free troposphere and be transported into the boundary layer. Others argue that the aerosols are created in the marine boundary layer. There are no data linking aerosol concentration and cirrus cloud albedo, and models suggest cirrus properties may not be very sensitive to aerosol abundance. There is clear evidence of a radiatively significant change in the global lower stratospheric ozone abundance during the past few decades. These changes are caused by heterogeneous chemical reactions occurring on the surfaces of particles. The rates of these reactions depend upon the chemical composition of the particles. Although rapid advances in understanding heterogeneous chemistry have been made, much remains to be done.

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.

Laboratory Experiments and Instrument Intercomparison Studies of Carbonaceous Aerosol Particles

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

Davidovits, Paul

Aerosols containing black carbon (and some specific types of organic particulate matter) directly absorb incoming light, heating the atmosphere. In addition, all aerosol particles backscatter solar light, leading to a net-cooling effect. Indirect effects involve hydrophilic aerosols, which serve as cloud condensation nuclei (CCN) that affect cloud cover and cloud stability, impacting both atmospheric radiation balance and precipitation patterns. At night, all clouds produce local warming, but overall clouds exert a net-cooling effect on the Earth. The effect of aerosol radiative forcing on climate may be as large as that of the greenhouse gases, but predominantly opposite in sign andmore » much more uncertain. The uncertainties in the representation of aerosol interactions in climate models makes it problematic to use model projections to guide energy policy. The objective of our program is to reduce the uncertainties in the aerosol radiative forcing in the two areas highlighted in the ASR Science and Program Plan. That is, (1) addressing the direct effect by correlating particle chemistry and morphology with particle optical properties (i.e. absorption, scattering, extinction), and (2) addressing the indirect effect by correlating particle hygroscopicity and CCN activity with particle size, chemistry, and morphology. In this connection we are systematically studying particle formation, oxidation, and the effects of particle coating. The work is specifically focused on carbonaceous particles where the uncertainties in the climate relevant properties are the highest. The ongoing work consists of laboratory experiments and related instrument inter-comparison studies both coordinated with field and modeling studies, with the aim of providing reliable data to represent aerosol processes in climate models. The work is performed in the aerosol laboratory at Boston College. At the center of our laboratory setup are two main sources for the production of aerosol

Global Analysis of Aerosol Properties Above Clouds

NASA Technical Reports Server (NTRS)

Waquet, F.; Peers, F.; Ducos, F.; Goloub, P.; Platnick, S. E.; Riedi, J.; Tanre, D.; Thieuleux, F.

2013-01-01

The seasonal and spatial varability of Aerosol Above Cloud (AAC) properties are derived from passive satellite data for the year 2008. A significant amount of aerosols are transported above liquid water clouds on the global scale. For particles in the fine mode (i.e., radius smaller than 0.3 m), including both clear sky and AAC retrievals increases the global mean aerosol optical thickness by 25(+/- 6%). The two main regions with man-made AAC are the tropical Southeast Atlantic, for biomass burning aerosols, and the North Pacific, mainly for pollutants. Man-made AAC are also detected over the Arctic during the spring. Mineral dust particles are detected above clouds within the so-called dust belt region (5-40 N). AAC may cause a warming effect and bias the retrieval of the cloud properties. This study will then help to better quantify the impacts of aerosols on clouds and climate.

Simulation of the influence of aerosol particles on Stokes parameters of polarized skylight

NASA Astrophysics Data System (ADS)

Li, L.; Li, Z. Q.; Wendisch, M.

2014-03-01

Microphysical properties and chemical compositions of aerosol particles determine polarized radiance distribution in the atmosphere. In this paper, the influences of different aerosol properties (particle size, shape, real and imaginary parts of refractive index) on Stokes parameters of polarized skylight in the solar principal and almucantar planes are studied by using vector radiative transfer simulations. The results show high sensitivity of the normalized Stokes parameters due to fine particle size, shape and real part of refractive index of aerosols. It is possible to utilize the strength variations at the peak positions of the normalized Stokes parameters in the principal and almucantar planes to identify aerosol types.

Decadal-scale trends in regional aerosol particle properties and their linkage to emission changes

NASA Astrophysics Data System (ADS)

Zhao, Bin; Jiang, Jonathan H.; Gu, Yu; Diner, David; Worden, John; Liou, Kuo-Nan; Su, Hui; Xing, Jia; Garay, Michael; Huang, Lei

2017-05-01

Understanding long-term trends in aerosol loading and properties is essential for evaluating the health and climatic effects of these airborne particulates as well as the effectiveness of pollution control policies. While many studies have used satellite data to examine the trends in aerosol optical depth (AOD), very few have investigated the trends in aerosol properties associated with particle size, morphology, and light absorption. In this study, we investigate decadal-scale (13-15 year) trends in aerosol loading and properties during 2001-2015 over three populous regions: the Eastern United States (EUS), Western Europe (WEU), and Eastern and Central China (ECC). We use observations from MISR (Multi-angle Imaging SpectroRadiometer) and MODIS (Moderate resolution Imaging Spectroradiometer). Relationships between aerosol property trends and air pollutant emission changes are examined. We find that annual mean AOD shows pronounced decreasing trends over EUS and WEU regions, as a result of considerable emission reductions in all major pollutants except for mineral dust and ammonia (NH3). Over the ECC region, AOD increases before 2006 due to emission increases induced by rapid economic development, fluctuates between 2006 and 2011, and subsequently decreases after 2011 in conjunction with effective emission reduction in anthropogenic primary aerosols, sulfur dioxide (SO2), and nitrogen oxides (NOx). The fraction of small-size AOD (<0.7 μm diameter), Ångstrom exponent and single-scattering albedo have generally decreased, while the fractions of large-size (>1.4 μm diameter), nonspherical and absorbing AOD have generally shown increasing trends over EUS and WEU regions, indicating that fine and light-scattering aerosol constituents have been more effectively reduced than coarse and light-absorbing constituents. These trends are consistent with the larger reduction ratios in SO2 and NOx emissions than in primary aerosols, including mineral dust and black carbon (BC

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.

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.

Organic Aerosols from SÃO Paulo and its Relationship with Aerosol Absorption and Scattering Properties

NASA Astrophysics Data System (ADS)

Artaxo, P.; Brito, J. F.; Rizzo, L. V.

2012-12-01

The megacity of São Paulo with its 19 million people and 7 million cars is a challenge from the point of view of air pollution. High levels of organic aerosols, PM10, black carbon and ozone and the peculiar situation of the large scale use of ethanol fuel makes it a special case. Little is known about the impact of ethanol on air quality and human health and the increase of ethanol as vehicle fuel is rising worldwide An experiment was designed to physico-chemical properties of aerosols in São Paulo, as well as their optical properties. Aerosol size distribution in the size range of 1nm to 10 micrometers is being measured with a Helsinki University SMPS (Scanning Mobility Particle Sizer), an NAIS (Neutral ion Spectrometer) and a GRIMM OPC (Optical Particle Counter). Optical properties are being measured with a TSI Nephelometer and a Thermo MAAP (Multi Angle Absorption Photometer). A CIMEL sunphotometer from the AERONET network measure the aerosol optical depth. Furthermore, a Proton-Transfer-Reaction Mass Spectrometer (PTR-MS) and an Aerosol Chemical Speciation Monitor (ACSM) are used to real-time VOC analysis and aerosol composition, respectively. The ACSM was operated for 3 months continuosly during teh wintertime of 2012. The measured total particle concentration typically varies between 10,000 and 30,000 cm-3 being the lowest late in the night and highest around noon and frequently exceeding 50,000 cm-3. Clear diurnal patterns in aerosol optical properties were observed. Scattering and absorption coefficients typically range between 20 and 100 Mm-1 at 450 nm, and between 10 to 40 Mm-1 at 637 nm, respectively, both of them peaking at 7:00 local time, the morning rush hour. The corresponding single scattering albedo varies between 0.50 and 0.85, indicating a significant contribution of primary absorbing particles to the aerosol population. During the first month a total of seven new particle formation events were observed with growth rates ranging from 9 to 25

Scattering of aerosol particles by a Hermite-Gaussian beam in marine atmosphere.

PubMed

Huang, Qingqing; Cheng, Mingjian; Guo, Lixin; Li, Jiangting; Yan, Xu; Liu, Songhua

2017-07-01

Based on the complex-source-point method and the generalized Lorenz-Mie theory, the scattering properties and polarization of aerosol particles by a Hermite-Gaussian (HG) beam in marine atmosphere is investigated. The influences of beam mode, beam width, and humidity on the scattered field are analyzed numerically. Results indicate that when the number of HG beam modes u (v) increase, the radar cross section of aerosol particles alternating appears at maximum and minimum values in the forward and backward scattering, respectively, because of the special petal-shaped distribution of the HG beam. The forward and backward scattering of aerosol particles decreases with the increase in beam waist. When beam waist is less than the radius of the aerosol particle, a minimum value is observed in the forward direction. The scattering properties of aerosol particles by the HG beam are more sensitive to the change in relative humidity compared with those by the plane wave and the Gaussian beam (GB). The HG beam shows superiority over the plane wave and the GB in detecting changes in the relative humidity of marine atmosphere aerosol. The effects of relative humidity on the polarization of the HG beam have been numerically analyzed in detail.

Microphysical Properties of Single Secondary Organic Aerosol (SOA) Particles

NASA Astrophysics Data System (ADS)

Rovelli, Grazia; Song, Young-Chul; Pereira, Kelly; Hamilton, Jacqueline; Topping, David; Reid, Jonathan

2017-04-01

Secondary Organic Aerosols (SOA) deriving from the oxidation of volatile organic compounds (VOCs) can account for a substantial fraction of the overall atmospheric aerosol mass.[1] Therefore, the investigation of SOA microphysical properties is crucial to better comprehend their role in the atmospheric processes they are involved in. This works describes a single particle approach to accurately characterise the hygroscopic response, the optical properties and the gas-particle partitioning kinetics of water and semivolatile components for laboratory generated SOA. SOA was generated from the oxidation of different VOCs precursors (e.g. α-pinene, toluene) in a photo-chemical flow reactor, which consists of a temperature and relative humidity controlled 300 L polyvinyl fluoride bag. Known VOC, NOx and ozone concentrations are introduced in the chamber and UV irradiation is performed by means of a Hg pen-ray. SOA samples were collected with an electrical low pressure impactor, wrapped in aluminium foil and kept refrigerated at -20°C. SOA samples were extracted in a 1:1 water/methanol mixture. Single charged SOA particles were generated from the obtained solution using a microdispenser and confined within an electrodynamic balance (EDB), where they sit in a T (250-320 K) and RH (0-95%) controlled nitrogen flow. Suspended droplets are irradiated with a 532 nm laser and the evolving angularly resolved scattered light is used to keep track of changes in droplet size. One of the key features of this experimental approach is that very little SOA solution is required because of the small volumes needed to load the dispensers (<20 μL). A number of diverse experiments were performed in order to characterise different microphysical properties of SOA. The equilibrium hygroscopic response of SOA was determined with comparative evaporation kinetics experiments (CK-EDB) of suspended probe and sample droplets.[2] The variation of the refractive index of SOA droplets following to

Estimating particle speciation concentrations using MISR retrieved aerosol properties in southern California

NASA Astrophysics Data System (ADS)

Meng, X.; Liu, Y.; Diner, D. J.; Garay, M. J.

2016-12-01

Ambient fine particle (PM2.5) has been positively associated with increased mortality and morbidity worldwide. Recent studies highlight the characteristics and differential toxicity of PM2.5 chemical components, which are important for identifying sources, developing targeted particulate matter (PM) control strategies, and protecting public health. Modelling with satellite retrieved data has been proved as the most cost-effective way to estimate ground PM2.5 levels; however, limited studies have predict PM2.5 chemical components with this method. In this study, the experimental MISR 4.4 km aerosol retrievals were used to predict ground-level particle sulfate, nitrite, organic carbon and element carbon concentrations in 16 counties of southern California. The PM2.5 chemical components concentrations were obtained from the National Chemical Speciation Network (CSN) and the Interagency Monitoring of Protected Visual Environments (IMPROVE) network. A generalized additive model (GAM) was developed based on 16-years data (2000-2015) by combining the MISR aerosol retrievals, meteorological variables and geographical indicators together. Model performance was assessed by model fitted R2 and root-mean-square error (RMSE) and 10-fold cross validation. Spatial patterns of sulfate, nitrate, OC and EC concentrations were also examined with 2-D prediction surfaces. This is the first attempt to develop high-resolution spatial models to predict PM2.5 chemical component concentrations with MISR retrieved aerosol properties, which will provide valuable population exposure estimates for future studies on the characteristics and differential toxicity of PM2.5 speciation.

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

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

Retrieval of Aerosol Properties

NASA Astrophysics Data System (ADS)

de Leeuw, Gerrit; Kinne, Stefan; Léon, Jean-Francois; Pelon, Jacques; Rosenfeld, Daniel; Schaap, Martijn; Veefkind, Pepijn J.; Veihelmann, Ben; Winker, David M.; von Hoyningen-Huene, Wolfgang

Atmospheric aerosol is a suspension of liquid and solid particles in air, i.e. the aerosol includes both particles and its surrounding medium; in practice aerosol is usually referred to as the suspended matter, i.e. the particles or the droplets, depending on their aggregation state.

Relation between aerosol particles and their optical properties: a case study for São Paulo-Brazil

NASA Astrophysics Data System (ADS)

Miranda, Regina; Andrade, Maria de Fatima

2013-04-01

Brazil has a territory of 8.5 million km2 and a population of more than 160 million inhabitants, distributed throughout 26 states. Brazillian capital-cities with millions inhabitants and vehicles have several problems concerning air pollution. São Paulo, capital of São Paulo State, with more than 19 million inhabitants, 7 million vehicles, as well as the major industrial and technological park of the country, has high concentrations of air pollutants, especially in the winter. Air pollution, high building density, and a lack of green areas, combined with the proliferation of asphalt and concrete surfaces, have resulted in a greater number of urban heat island effects, fewer drizzle events, and rainfall events of greater intensity. São Paulo has an extensive air quality monitoring network, which has shown that ozone levels often exceed the NAAQS limit during spring and summer, and that concentrations of inhalable particles exceed the NAAQS limit mainly during the winter, from June to August. Aerosols are produced by a variety of processes, creating differences in their physicochemical properties and hence in their ability to scatter and absorb solar radiation. For most urban areas in Brazil, vehicles are considered the principal source of particles emitted to the atmosphere. Particles have been monitored in the winter of 2012 in São Paulo using a MOUDI (Micro Orifice Uniform Deposit Impactor), in order to have the mass distribution of the aerosol. The concentrations of coarse particles can still be larger than those of fine particles, although the difference between both has become smaller than in the past. The samples collected were analyzed by gravimetry for mass concentration, optical reflectance for Black Carbon concentration and X-ray Fluorescence for elementar characterization. Optical properties were obtained from Aeronet (Aerosol Robotic Network, http://aeronet.gsfc.nasa.gov/) for São Paulo city. It was found that a high fraction of elements was derived

The statistical distribution of aerosol properties in sourthern West Africa

NASA Astrophysics Data System (ADS)

Haslett, Sophie; Taylor, Jonathan; Flynn, Michael; Bower, Keith; Dorsey, James; Crawford, Ian; Brito, Joel; Denjean, Cyrielle; Bourrianne, Thierry; Burnet, Frederic; Batenburg, Anneke; Schulz, Christiane; Schneider, Johannes; Borrmann, Stephan; Sauer, Daniel; Duplissy, Jonathan; Lee, James; Vaughan, Adam; Coe, Hugh

2017-04-01

The population and economy in southern West Africa have been growing at an exceptional rate in recent years and this trend is expected to continue, with the population projected to more than double to 800 million by 2050. This will result in a dramatic increase in anthropogenic pollutants, already estimated to have tripled between 1950 and 2000 (Lamarque et al., 2010). It is known that aerosols can modify the radiative properties of clouds. As such, the entrainment of anthropogenic aerosol into the large banks of clouds forming during the onset of the West African Monsoon could have a substantial impact on the region's response to climate change. Such projections, however, are greatly limited by the scarcity of observations in this part of the world. As part of the Dynamics-Aerosol-Chemistry-Cloud Interactions in West Africa (DACCIWA) project, three research aircraft were deployed, each carrying equipment capable of measuring aerosol properties in-situ. Instrumentation included Aerosol Mass Spectrometers (AMS), Single Particle Soot Photometers (SP2), Condensation Particle Counters (CPC) and Scanning Mobility Particle Sizers (SMPS). Throughout the intensive aircraft campaign, 155 hours of scientific flights covered an area including large parts of Benin, Togo, Ghana and parts of Côte D'Ivoire. Approximately 70 hours were dedicated to the measurement of cloud-aerosol interactions, with many other flights producing data contributing towards this objective. Using datasets collected during this campaign period, it is possible to build a robust statistical understanding of aerosol properties in this region for the first time, including size distributions and optical and chemical properties. Here, we describe preliminary results from aerosol measurements on board the three aircraft. These have been used to describe aerosol properties throughout the region and time period encompassed by the DACCIWA aircraft campaign. Such statistics will be invaluable for improving future

Size distribution and scattering phase function of aerosol particles retrieved from sky brightness measurements

NASA Technical Reports Server (NTRS)

Kaufman, Y. J.; Gitelson, A.; Karnieli, A.; Ganor, E. (Editor); Fraser, R. S.; Nakajima, T.; Mattoo, S.; Holben, B. N.

1994-01-01

Ground-based measurements of the solar transmission and sky radiance in a horizontal plane through the Sun are taken in several geographical regions and aerosol types: dust in a desert transition zone in Israel, sulfate particles in Eastern and Western Europe, tropical aerosol in Brazil, and mixed continental/maritime aerosol in California. Stratospheric aerosol was introduced after the eruption of Mount Pinatubo in June 1991. Therefore measurements taken before the eruption are used to analyze the properties of tropospheric aerosol; measurements from 1992 are also used to detect the particle size and concentration of stratospheric aerosol. The measurements are used to retrieve the size distribution and the scattering phase function at large scattering angles of the undisturbed aerosol particles. The retrieved properties represent an average on the entire atmospheric column. A comparison between the retrieved phase function for a scattering angle of 120 deg, with phase function predicted from the retrieved size distribution, is used to test the assumption of particle homogeneity and sphericity in radiative transfer models (Mie theory). The effect was found to be small (20% +/- 15%). For the stratospheric aerosol (sulfates), as expected, the phase function was very well predicted using the Mie theory. A model with a power law distribution, based on the spectral dependence of the optical thickness, alpha, cannot estimate accurately the phase function (up to 50% error for lambda = 0.87 microns). Before the Pinatubo eruption the ratio between the volumes of sulfate and coarse particles was very well correlated with alpha. The Pinatubo stratospheric aerosol destroyed this correlation. The aerosol optical properties are compared with analysis of the size, shape, and composition of the individual particles by electron microscopy of in situ samples. The measured volume size distribution before the injection of stratospheric aerosol consistently show two modes, sulfate

Chemical Composition and Oxidation State of Iron-Containing Aerosol Particles Over West Antarctic Peninsula

NASA Astrophysics Data System (ADS)

Fan, S.; Yu, S.; Lai, B.; Gao, Y.

2017-12-01

Iron is a limiting micronutrient element critical for the marine ecosystem. In the extensive high-nutrient low-chlorophyll (HNLC) regions of the Southern Ocean, the activities of phytoplankton are partly controlled by iron (Fe) from different sources, including atmospheric deposition. Among important properties of atmospheric Fe are the elemental composition and Fe oxidation state of Fe-containing aerosol particles, as these properties affect aerosol Fe solubility. To explore these issues, aerosol samples were collected at Palmer Station in West Antarctic Peninsula. Samples were analyzed by submicron synchrotron-based X-ray fluorescence (XRF) and X-ray absorption near edge structure (XANES) spectroscopy for the Fe oxidation state and elemental composition of aerosol particles. The morphological information of aerosol particles was also observed by the high-resolution fluorescence microscopy, revealing possible sources and formation processes of iron-containing particles. More detailed results will be discussed in this presentation.

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

Quantifying the risks of solid aerosol geoengineering: the role of fundamental material properties

NASA Astrophysics Data System (ADS)

Dykema, J. A.; Keutsch, F. N.; Keith, D.

2017-12-01

Solid aerosols have been considered as an alternative to sulfate aerosols for solar geoengineering due to their optical and chemical properties, which lead to different and possibly more attractive risk profiles. Solid aerosols can achieve higher solar scattering efficiency due to their higher refractive index, and in some cases may also be less effective absorbers of thermal infrared radiation. The optical properties of solid aerosols are however sensitive functions of the detailed physical properties of solid materials in question. The relevant details include the exact crystalline structure of the aerosols, the physical size of the particles, and interactions with background stratospheric molecular and particulate constituents. In this work, we examine the impact of these detailed physical properties on the radiative properties of calcite (CaCO3) solid aerosols. We examine how crystal morphology, size, chemical reactions, and interaction with background stratospheric aerosol may alter the scattering and absorption properties of calcite aerosols for solar and thermal infrared radiation. For example, in small particles, crystal lattice vibrations associated with the particle surface may lead to substantially different infrared absorption properties than bulk materials. We examine the wavelength dependence of absorption by the particles, which may lead to altered patterns of stratospheric radiative heating and equilibrium temperatures. Such temperature changes can lead to dynamical changes, with consequences for both stratospheric composition and tropospheric climate. We identify important uncertainties in the current state of understanding, investigate risks associated with these uncertainties, and survey potential approaches to quantitatively improving our knowledge of the relevant material properties.

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

Measurements of Semi-volatile Aerosol and Its Effect on Aerosol Optical Properties During Southern Oxidant and Aerosol Study

NASA Astrophysics Data System (ADS)

Khlystov, A.; Grieshop, A. P.; Saha, P.; Subramanian, R.

2013-12-01

Semi-volatile compounds, including particle-bound water, comprise a large part of aerosol mass and have a significant influence on aerosol lifecycle and its optical properties. Understanding the properties of semi-volatile compounds, especially those pertaining to gas/aerosol partitioning, is of critical importance for our ability to predict concentrations and properties of ambient aerosol. A set of state-of-the-art instruments was deployed at the SEARCH site near Centerville, AL during the Southern Oxidant and Aerosol Study (SOAS) campaign in summer 2013 to measure the effect of temperature and relative humidity on aerosol size distribution, composition and optical properties. Light scattering and absorption by temperature- and humidity-conditioned aerosols was measured using three photo-acoustic extinctiometers (PAX) at three wavelengths (405 nm, 532 nm, and 870 nm). In parallel to these measurements, a long residence time temperature-stepping thermodenuder and a variable residence time constant temperature thermodenuder in combination with three SMPS systems and an Aerosol Chemical Speciation Monitor (ACSM) were used to assess aerosol volatility and kinetics of aerosol evaporation. It was found that both temperature and relative humidity have a strong effect on aerosol optical properties. The variable residence time thermodenuder data suggest that aerosol equilibrated fairly quickly, within 2 s, in contrast to other ambient observations. Preliminary analysis show that approximately 50% and 90% of total aerosol mass evaporated at temperatures of 100 C and 180C, respectively. Evaporation varied substantially with ambient aerosol loading and composition and meteorology. During course of this study, T50 (temperatures at which 50% aerosol mass evaporates) varied from 60 C to more than 120 C.

Theophylline cocrystals prepared by spray drying: physicochemical properties and aerosolization performance.

PubMed

Alhalaweh, Amjad; Kaialy, Waseem; Buckton, Graham; Gill, Hardyal; Nokhodchi, Ali; Velaga, Sitaram P

2013-03-01

The purpose of this work was to characterize theophylline (THF) cocrystals prepared by spray drying in terms of the physicochemical properties and inhalation performance when aerosolized from a dry powder inhaler. Cocrystals of theophylline with urea (THF-URE), saccharin (THF-SAC) and nicotinamide (THF-NIC) were prepared by spray drying. Milled THF and THF-SAC cocrystals were also used for comparison. The physical purity, particle size, particle morphology and surface energy of the materials were determined. The in vitro aerosol performance of the spray-dried cocrystals, drug-alone and a drug-carrier aerosol, was assessed. The spray-dried particles had different size distributions, morphologies and surface energies. The milled samples had higher surface energy than those prepared by spray drying. Good agreement was observed between multi-stage liquid impinger and next-generation impactor in terms of assessing spray-dried THF particles. The fine particle fractions of both formulations were similar for THF, but drug-alone formulations outperformed drug-carrier formulations for the THF cocrystals. The aerosolization performance of different THF cocrystals was within the following rank order as obtained from both drug-alone and drug-carrier formulations: THF-NIC>THF-URE>THF-SAC. It was proposed that micromeritic properties dominate over particle surface energy in terms of determining the aerosol performance of THF cocrystals. Spray drying could be a potential technique for preparing cocrystals with modified physical properties.

Understanding hygroscopic growth and phase transformation of aerosols using single particle Raman spectroscopy in an electrodynamic balance.

PubMed

Lee, Alex K Y; Ling, T Y; Chan, Chak K

2008-01-01

Hygroscopic growth is one of the most fundamental properties of atmospheric aerosols. By absorbing or evaporating water, an aerosol particle changes its size, morphology, phase, chemical composition and reactivity and other parameters such as its refractive index. These changes affect the fate and the environmental impacts of atmospheric aerosols, including global climate change. The ElectroDynamic Balance (EDB) has been widely accepted as a unique tool for measuring hygroscopic properties and for investigating phase transformation of aerosols via single particle levitation. Coupled with Raman spectroscopy, an EDB/Raman system is a powerful tool that can be used to investigate both physical and chemical changes associated with the hygroscopic properties of individually levitated particles under controlled environments. In this paper, we report the use of an EDB/Raman system to investigate (1) contact ion pairs formation in supersaturated magnesium sulfate solutions; (2) phase transformation in ammonium nitrate/ammonium sulfate mixed particles; (3) hygroscopicity of organically coated inorganic aerosols; and (4) heterogeneous reactions altering the hygroscopicity of organic aerosols.

Study of the hygroscopic properties of selected pharmaceutical aerosols using single particle levitation.

PubMed

Peng, C; Chow, A H; Chan, C K

2000-09-01

To use a single particle levitation technique to investigate the equilibrium water sorption characteristics in both the evaporation and growth of four respiratory drugs at 37 degrees C: atropine sulfate (AS), isoproterenol hydrochloride (IPHC) and isoproterenol hemisulfate (IPHS) and disodium cromoglycate (DSCG). The equilibrium water content was measured as a function of relative humidity (RH) by a single particle levitation technique using an electrodynamic balance (EDB). The change of water content was determined by the voltage required to balance the weight of the levitated particle electrostatically. The water activities of bulk samples were also measured. Growth ratios were determined and compared with values in the literature. Crystallization or deliquescence was not observed for AS, IPHC and IPHS. The hysteresis in the water cycle was not observed for any of the drugs. At RH approximately 0%, AS particles still contain about 5% water but IPHC and IPHS particles do not contain any residual water. The aerodynamic growth ratio from RH 0% to 99.5% is 2.60, 2.86, 2.42 and 1.26 for AS, IPHC, IPHS and DSCG, respectively. Supersaturated droplets of IPHC and IPHS are expected to exist in the ambient conditions. DSCG is in a solid state in the RH range of 10-90%. It is expected that some aerosolized drugs of low solubility may experience supersaturation before they enter the human body and this could exert a significant influence both on particle loss before inhalation and on the deposition of the drugs in the lungs. The EDB is a convenient and reliable tool for studying the hygroscopic properties of pharmaceutical aerosols, especially for supersaturated solutions.

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

Measurements of Intensive Aerosol Optical Properties During TexAQS II

NASA Astrophysics Data System (ADS)

Atkinson, D. B.; Radney, J. G.; Wright, M. E.

2007-12-01

Time-resolved measurements of the bulk extensive aerosol optical properties - particle extinction coefficient (bext) and particle scattering coefficient (bscat) - and particle number concentrations were made as part of the six-week TRAMP experiment during the TexAQS II (2006) study. These measurements were done at a nominal surface site (the roof of an 18 story building) on the University of Houston campus near downtown Houston, Texas. Our ground-based tandem cavity ring-down transmissometer/nephelometer instrument (CRDT/N) provided the aerosol optical property measurements. A commercial Condensation Particle Counter (TSI 3007) was used to measure the number concentrations during part of the study period. The optical data was used to construct the intensive aerosol optical properties single scattering albedo ω0 at 532 nm and the Angstrom exponent for extinction between 532 nm and 1064 nm. Recent validation studies of size- selected laboratory generated aerosols are presented to illustrate the soundness of this approach using our instrument. The Angstrom exponent is compared to values from other instruments operating in the area and is found to be a characteristic of the regional air mass under some conditions. Size distributions measured during the study were used to create a new empirical adjustment to scattering measured by the Radiance Research nephelometer, resulting in improved results for particle absorption coefficient and single scattering albedo. The study average value of ω0(532 nm) = 0.78 is lower than expected from comparable field studies and even lower values are experienced during the study. Possible causes of this discrepancy are examined and the utility of using the current version of the CRDT/N instrument to measure the key radiative property ω0 is assessed. Observed episodes of rapid increases in particle number concentration with little corresponding growth in the optical properties can presumably be used to signal the occurrence of particle

Investigation of Atmospheric Aerosol properties by Atomic Force Microscopy

NASA Astrophysics Data System (ADS)

Sevalia, Barry; Joseph, Kelli; Gasseller, Morewell

The effects of aerosols on the atmosphere, climate, and public health are among the central topics in current environmental research. Aerosol particles scatter and absorb solar and terrestrial radiation, they are involved in the formation of clouds and precipitation as cloud condensation and ice nuclei, and they affect the abundance and distribution of atmospheric trace gases by chemical reactions and other multiphase processes. Moreover, airborne particles play an important role in the spreading of biological organisms, reproductive materials, and pathogens and they can cause or enhance respiratory, cardiovascular, infectious, and allergic diseases. In this study we use two distinct methods to characterize atmospheric aerosol particles. With the AFM, we use analytical and interpretative techniques to deduce fundamental physical properties of the aerosol particles such as particle sizes and morphology. The microscopy techniques are then compared and complemented with optical techniques that employ hand held sun photometers to measure aerosol optical thickness (AOT) of the atmosphere. The chemical nature of the aerosols is investigated by exposing the samples to a stream of ozone gas and then reimage them. Using this approach, we are only able to classify particles as organic, gr Maryam Foroozesh, Ph.D. Chair, Division of Mathematical and Physical Sciences Head, Department of Chemistry.

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.

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.

Optical properties of mineral dust aerosol including analysis of particle size, composition, and shape effects, and the impact of physical and chemical processing

NASA Astrophysics Data System (ADS)

Alexander, Jennifer Mary

Atmospheric mineral dust has a large impact on the earth's radiation balance and climate. The radiative effects of mineral dust depend on factors including, particle size, shape, and composition which can all be extremely complex. Mineral dust particles are typically irregular in shape and can include sharp edges, voids, and fine scale surface roughness. Particle shape can also depend on the type of mineral and can vary as a function of particle size. In addition, atmospheric mineral dust is a complex mixture of different minerals as well as other, possibly organic, components that have been mixed in while these particles are suspended in the atmosphere. Aerosol optical properties are investigated in this work, including studies of the effect of particle size, shape, and composition on the infrared (IR) extinction and visible scattering properties in order to achieve more accurate modeling methods. Studies of particle shape effects on dust optical properties for single component mineral samples of silicate clay and diatomaceous earth are carried out here first. Experimental measurements are modeled using T-matrix theory in a uniform spheroid approximation. Previous efforts to simulate the measured optical properties of silicate clay, using models that assumed particle shape was independent of particle size, have achieved only limited success. However, a model which accounts for a correlation between particle size and shape for the silicate clays offers a large improvement over earlier modeling approaches. Diatomaceous earth is also studied as an example of a single component mineral dust aerosol with extreme particle shapes. A particle shape distribution, determined by fitting the experimental IR extinction data, used as a basis for modeling the visible light scattering properties. While the visible simulations show only modestly good agreement with the scattering data, the fits are generally better than those obtained using more commonly invoked particle shape

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

Aerosol Properties Observed in the Subtropical North Pacific Boundary Layer

NASA Astrophysics Data System (ADS)

Royalty, T. M.; Phillips, B. N.; Dawson, K. W.; Reed, R.; Meskhidze, N.; Petters, M. D.

2017-09-01

The impact of anthropogenic aerosol on climate forcing remains uncertain largely due to inadequate representation of natural aerosols in climate models. The marine boundary layer (MBL) might serve as a model location to study natural aerosol processes. Yet source and sink mechanisms controlling the MBL aerosol number, size distribution, chemical composition, and hygroscopic properties remain poorly constrained. Here aerosol size distribution and water uptake measurements were made aboard the R/V Hi'ialakai from 27 June to 3 July 2016 in the subtropical North Pacific Ocean. Size distributions were predominantly bimodal with an average integrated number concentration of 197 ± 98 cm-3. Hygroscopic growth factors were measured using the tandem differential mobility analyzer technique for dry 48, 96, and 144 nm particles. Mode kappa values for these were 0.57 ± 0.12, 0.51 ± 0.09, and 0.52 ± 0.08, respectively. To better understand remote MBL aerosol sources, a new algorithm was developed which decomposes hygroscopicity distributions into three classes: carbon-containing particles, sulfate-like particles, and sodium-containing particles. Results from this algorithm showed low and steady sodium-containing particle concentrations while the sulfate-like and carbon-containing particle concentrations varied during the cruise. According to the classification scheme, carbon-containing particles contributed at least 3-7%, sulfate-like particles contributed at most 77-88% and sodium-containing particles at least contributed 9-16% to the total aerosol number concentration. Size distribution and hygroscopicity data, in conjunction with air mass back trajectory analysis, suggested that the aerosol budget in the subtropical North Pacific MBL may be controlled by aerosol entrainment from the free troposphere.

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

Climatology of Aerosol Optical Properties in Southern Africa

NASA Technical Reports Server (NTRS)

Queface, Antonio J.; Piketh, Stuart J.; Eck, Thomas F.; Tsay, Si-Chee

2011-01-01

A thorough regionally dependent understanding of optical properties of aerosols and their spatial and temporal distribution is required before we can accurately evaluate aerosol effects in the climate system. Long term measurements of aerosol optical depth, Angstrom exponent and retrieved single scattering albedo and size distribution, were analyzed and compiled into an aerosol optical properties climatology for southern Africa. Monitoring of aerosol parameters have been made by the AERONET program since the middle of the last decade in southern Africa. This valuable information provided an opportunity for understanding how aerosols of different types influence the regional radiation budget. Two long term sites, Mongu in Zambia and Skukuza in South Africa formed the core sources of data in this study. Results show that seasonal variation of aerosol optical thicknesses at 500 nm in southern Africa are characterized by low seasonal multi-month mean values (0.11 to 0.17) from December to May, medium values (0.20 to 0.27) between June and August, and high to very high values (0.30 to 0.46) during September to November. The spatial distribution of aerosol loadings shows that the north has high magnitudes than the south in the biomass burning season and the opposite in none biomass burning season. From the present aerosol data, no long term discernable trends are observable in aerosol concentrations in this region. This study also reveals that biomass burning aerosols contribute the bulk of the aerosol loading in August-October. Therefore if biomass burning could be controlled, southern Africa will experience a significant reduction in total atmospheric aerosol loading. In addition to that, aerosol volume size distribution is characterized by low concentrations in the non biomass burning period and well balanced particle size contributions of both coarse and fine modes. In contrast high concentrations are characteristic of biomass burning period, combined with

International Workshop on Stratospheric Aerosols: Measurements, Properties, and Effects

NASA Technical Reports Server (NTRS)

Pueschel, Rudolf F. (Editor)

1991-01-01

Following a mandate by the International Aerosol Climatology Program under the auspices of International Association of Meteorology and Atmospheric Physics International Radiation Commission, 45 scientists from five nations convened to discuss relevant issues associated with the measurement, properties, and effects of stratospheric aerosols. A summary is presented of the discussions on formation and evolution, transport and fate, effects on climate, role in heterogeneous chemistry, and validation of lidar and satellite remote sensing of stratospheric aerosols. Measurements are recommended of the natural (background) and the volcanically enhanced aerosol (sulfuric acid and silica particles), the exhaust of shuttle, civil aviation and supersonic aircraft operations (alumina, soot, and ice particles), and polar stratospheric clouds (ice, condensed nitric and hydrochloric acids).

Aerosol Properties of the Atmospheres of Extrasolar Giant Planets

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

Lavvas, P.; Koskinen, T., E-mail: panayotis.lavvas@univ-reims.fr

2017-09-20

We use a model of aerosol microphysics to investigate the impact of high-altitude photochemical aerosols on the transmission spectra and atmospheric properties of close-in exoplanets, such as HD 209458 b and HD 189733 b. The results depend strongly on the temperature profiles in the middle and upper atmospheres, which are poorly understood. Nevertheless, our model of HD 189733 b, based on the most recently inferred temperature profiles, produces an aerosol distribution that matches the observed transmission spectrum. We argue that the hotter temperature of HD 209458 b inhibits the production of high-altitude aerosols and leads to the appearance of amore » clearer atmosphere than on HD 189733 b. The aerosol distribution also depends on the particle composition, photochemical production, and atmospheric mixing. Due to degeneracies among these inputs, current data cannot constrain the aerosol properties in detail. Instead, our work highlights the role of different factors in controlling the aerosol distribution that will prove useful in understanding different observations, including those from future missions. For the atmospheric mixing efficiency suggested by general circulation models, we find that the aerosol particles are small (∼nm) and probably spherical. We further conclude that a composition based on complex hydrocarbons (soots) is the most likely candidate to survive the high temperatures in hot-Jupiter atmospheres. Such particles would have a significant impact on the energy balance of HD 189733 b’s atmosphere and should be incorporated in future studies of atmospheric structure. We also evaluate the contribution of external sources to photochemical aerosol formation and find that their spectral signature is not consistent with observations.« less

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

Aerosol Optical Properties of Smoke from the Las Conchas Wildfire, Los Alamos, NM

NASA Astrophysics Data System (ADS)

Gorkowski, K.; Dubey, M. K.; Flowers, B. A.; Aiken, A. C.; Klein, B. Z.; Mazzoleni, C.; Sharma, N.; China`, S.

2011-12-01

The Las Conchas wildfire in Northern New Mexico started on June, 26 2011 and spread rapidly, eventually burning an area of 634 km2 (245 mi2). Due to the close proximity to the fire, the Los Alamos National Laboratory (LANL) was shut down and the town evacuated for several days. Immediately after LANL reopened (7/6/2011) the Earth and Environmental Sciences Division (EES-14) attained unique measurements of the smoke by sampling the ambient air. Three Integrated Photoacoustic/Nephelometer Spectrometers (DMT Inc.) were set up to measure aerosol light absorption and scattering coefficients. A University of Northwest Switzerland thermodenuder was used to remove compounds that are volatile at temperatures up to 200C. The aerosol's optical properties were measured before and after denuding the sample at 405nm (blue), 532nm (green), 781nm (red), and for non-denuded particles also at 375nm (ultraviolet). The aerosol size distributions were measured after the denuder with a Laser Aerosol Spectrometer (LAS, TSI Inc.) and black carbon was measured with a Single Particle Soot Photometer (SP2, DMT Inc.). Additionally, ambient measurements of Total Particulate Matter (PM2.5 and PM10) were collected continuously at the LANL air monitoring stations. These measurements are used in conjunction with numerical simulations to determine the bulk optical properties of the aerosol. Aerosols in wildfire smoke are composed of organic and black carbon (soot) particles that are formed during wood combustion and pyrolysis. The optical properties of the smoke particles are complex and lead to large uncertainties in assessing the global climate. During the measurement period, the Las Conchas fire provided very high particle concentrations (up to 200 μg/m3) that were exploited to investigate their optical properties. By heating the particles to temperatures ranging from 75 to 200C in the denuder, volatile organics were removed and the optical properties of the remaining particles were measured

Processing of aerosol particles within the Habshan pollution plume

NASA Astrophysics Data System (ADS)

Semeniuk, T. A.; Bruintjes, R.; Salazar, V.; Breed, D.; Jensen, T.; Buseck, P. R.

2015-03-01

The Habshan industrial site in the United Arab Emirates produces a regional-scale pollution plume associated with oil and gas processing, discharging high loadings of sulfates and chlorides into the atmosphere, which interact with the ambient aerosol population. Aerosol particles and trace gas chemistry at this site were studied on two flights in the summer of 2002. Measurements were collected along vertical plume profiles to show changes associated with atmospheric processing of particle and gas components. Close to the outlet stack, particle concentrations were over 10,000 cm-3, dropping to <2000 cm-3 in more dilute plume around 1500 m above the stack. Particles collected close to the stack and within the dilute plume were individually measured for size, morphology, composition, and mixing state using transmission electron microscopy coupled with energy-dispersive X-ray spectroscopy. Close to the stack, most coarse particles consisted of mineral dust and NaCl crystals from burning oil brines, while sulfate droplets dominated the fine mode. In more dilute plume, at least 1500 m above the stack, the particle spectrum was more diverse, with a significant increase in internally mixed particle types. Dilute plume samples consisted of coarse NaCl/silicate aggregates or NaCl-rich droplets, often with a sulfate component, while fine-fraction particles were of mixed cation sulfates, also internally mixed with nanospherical soot or silicates. Thus, both chloride and sulfate components of the pollution plume rapidly reacted with ambient mineral dust to form coated and aggregate particles, enhancing particle size, hygroscopicity, and reactivity of the coarse mode. The fine-fraction sulfate-bearing particles formed in the plume contribute to regional transport of sulfates, while coarse sulfate-bearing fractions locally reduced the SO2 loading through sedimentation. The chloride- and sulfate-bearing internally mixed particles formed in the plume markedly changed the

Aerosols, light, and water: Measurements of aerosol optical properties at different relative humidities

NASA Astrophysics Data System (ADS)

Orozco, Daniel

The Earth's atmosphere is composed of a large number of different gases as well as tiny suspended particles, both in solid and liquid state. These tiny particles, called atmospheric aerosols, have an immense impact on our health and on our global climate. Atmospheric aerosols influence the Earth's radiation budget both directly and indirectly. In the direct effect, aerosols scatter and absorb sunlight changing the radiative balance of the Earth-atmosphere system. Aerosols indirectly influence the Earth's radiation budget by modifying the microphysical and radiative properties of clouds as well as their water content and lifetime. In ambient conditions, aerosol particles experience hygroscopic growth due to the influence of relative humidity (RH), scattering more light than when the particles are dry. The quantitative knowledge of the RH effect and its influence on the light scattering coefficient and, in particular, on the phase function and polarization of aerosol particles is of substantial importance when comparing ground based observations with other optical aerosol measurements techniques such satellite and sunphotometric retrievals of aerosol optical depth and their inversions. This dissertation presents the aerosol hygroscopicity experiment investigated using a novel dryer-humidifier system, coupled to a TSI-3563 nephelometer, to obtain the light scattering coefficient (sp) as a function of relative humidity (RH) in hydration and dehydration modes. The measurements were performed in Porterville, CA (Jan 10-Feb 6, 2013), Baltimore, MD (Jul 3-30, 2013), and Golden, CO (Jul 12-Aug 10, 2014). Observations in Porterville and Golden were part of the NASA-sponsored DISCOVER-AQ project. The measured sp under varying RH in the three sites was combined with ground aerosol extinction, PM2:5mass concentrations, particle composition measurements, and compared with airborne observations performed during campaigns. The enhancement factor, f(RH), defined as the ratio of sp

Modelling the optical properties of aerosols in a chemical transport model

NASA Astrophysics Data System (ADS)

Andersson, E.; Kahnert, M.

2015-12-01

According to the IPCC fifth assessment report (2013), clouds and aerosols still contribute to the largest uncertainty when estimating and interpreting changes to the Earth's energy budget. Therefore, understanding the interaction between radiation and aerosols is both crucial for remote sensing observations and modelling the climate forcing arising from aerosols. Carbon particles are the largest contributor to the aerosol absorption of solar radiation, thereby enhancing the warming of the planet. Modelling the radiative properties of carbon particles is a hard task and involves many uncertainties arising from the difficulties of accounting for the morphologies and heterogeneous chemical composition of the particles. This study aims to compare two ways of modelling the optical properties of aerosols simulated by a chemical transport model. The first method models particle optical properties as homogeneous spheres and are externally mixed. This is a simple model that is particularly easy to use in data assimilation methods, since the optics model is linear. The second method involves a core-shell internal mixture of soot, where sulphate, nitrate, ammonia, organic carbon, sea salt, and water are contained in the shell. However, by contrast to previously used core-shell models, only part of the carbon is concentrated in the core, while the remaining part is homogeneously mixed with the shell. The chemical transport model (CTM) simulations are done regionally over Europe with the Multiple-scale Atmospheric Transport and CHemistry (MATCH) model, developed by the Swedish Meteorological and Hydrological Institute (SMHI). The MATCH model was run with both an aerosol dynamics module, called SALSA, and with a regular "bulk" approach, i.e., a mass transport model without aerosol dynamics. Two events from 2007 are used in the analysis, one with high (22/12-2007) and one with low (22/6-2007) levels of elemental carbon (EC) over Europe. The results of the study help to assess the

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

NASA Astrophysics Data System (ADS)

Wang, Yang

Aerosol science and technology enable continual advances in material synthesis and atmospheric pollutant control. Among these advances, one important frontier is characterizing the initial stages of particle formation by real time measurement of particles below 2 nm in size. Sub 2 nm particles play important roles by acting as seeds for particle growth, ultimately determining the final properties of the generated particles. Tailoring nanoparticle properties requires a thorough understanding and precise control of the particle formation processes, which in turn requires characterizing nanoparticle formation from the initial stages. The knowledge on particle formation in early stages can also be applied in quantum dot synthesis and material doping. This dissertation pursued two approaches in investigating incipient particle characterization in systems with aerosol formation and growth: (1) using a high-resolution differential mobility analyzer (DMA) to measure the size distributions of sub 2 nm particles generated from high-temperature aerosol reactors, and (2) analyzing the physical and chemical pathways of aerosol formation during combustion. Part. 1. Particle size distributions reveal important information about particle formation dynamics. DMAs are widely utilized to measure particle size distributions. However, our knowledge of the initial stages of particle formation is incomplete, due to the Brownian broadening effects in conventional DMAs. The first part of this dissertation studied the applicability of high-resolution DMAs in characterizing sub 2 nm particles generated from high-temperature aerosol reactors, including a flame aerosol reactor (FLAR) and a furnace aerosol reactor (FUAR). Comparison against a conventional DMA (Nano DMA, Model 3085, TSI Inc.) demonstrated that the increased sheath flow rates and shortened residence time indeed greatly suppressed the diffusion broadening effect in a high-resolution DMA (half mini type). The incipient particle

Formation of highly porous aerosol particles by atmospheric freeze-drying in ice clouds

PubMed Central

Adler, Gabriela; Koop, Thomas; Haspel, Carynelisa; Taraniuk, Ilya; Moise, Tamar; Koren, Ilan; Heiblum, Reuven H.; Rudich, Yinon

2013-01-01

The cycling of atmospheric aerosols through clouds can change their chemical and physical properties and thus modify how aerosols affect cloud microphysics and, subsequently, precipitation and climate. Current knowledge about aerosol processing by clouds is rather limited to chemical reactions within water droplets in warm low-altitude clouds. However, in cold high-altitude cirrus clouds and anvils of high convective clouds in the tropics and midlatitudes, humidified aerosols freeze to form ice, which upon exposure to subsaturation conditions with respect to ice can sublimate, leaving behind residual modified aerosols. This freeze-drying process can occur in various types of clouds. Here we simulate an atmospheric freeze-drying cycle of aerosols in laboratory experiments using proxies for atmospheric aerosols. We find that aerosols that contain organic material that undergo such a process can form highly porous aerosol particles with a larger diameter and a lower density than the initial homogeneous aerosol. We attribute this morphology change to phase separation upon freezing followed by a glass transition of the organic material that can preserve a porous structure after ice sublimation. A porous structure may explain the previously observed enhancement in ice nucleation efficiency of glassy organic particles. We find that highly porous aerosol particles scatter solar light less efficiently than nonporous aerosol particles. Using a combination of satellite and radiosonde data, we show that highly porous aerosol formation can readily occur in highly convective clouds, which are widespread in the tropics and midlatitudes. These observations may have implications for subsequent cloud formation cycles and aerosol albedo near cloud edges. PMID:24297908

Formation of highly porous aerosol particles by atmospheric freeze-drying in ice clouds.

PubMed

Adler, Gabriela; Koop, Thomas; Haspel, Carynelisa; Taraniuk, Ilya; Moise, Tamar; Koren, Ilan; Heiblum, Reuven H; Rudich, Yinon

2013-12-17

The cycling of atmospheric aerosols through clouds can change their chemical and physical properties and thus modify how aerosols affect cloud microphysics and, subsequently, precipitation and climate. Current knowledge about aerosol processing by clouds is rather limited to chemical reactions within water droplets in warm low-altitude clouds. However, in cold high-altitude cirrus clouds and anvils of high convective clouds in the tropics and midlatitudes, humidified aerosols freeze to form ice, which upon exposure to subsaturation conditions with respect to ice can sublimate, leaving behind residual modified aerosols. This freeze-drying process can occur in various types of clouds. Here we simulate an atmospheric freeze-drying cycle of aerosols in laboratory experiments using proxies for atmospheric aerosols. We find that aerosols that contain organic material that undergo such a process can form highly porous aerosol particles with a larger diameter and a lower density than the initial homogeneous aerosol. We attribute this morphology change to phase separation upon freezing followed by a glass transition of the organic material that can preserve a porous structure after ice sublimation. A porous structure may explain the previously observed enhancement in ice nucleation efficiency of glassy organic particles. We find that highly porous aerosol particles scatter solar light less efficiently than nonporous aerosol particles. Using a combination of satellite and radiosonde data, we show that highly porous aerosol formation can readily occur in highly convective clouds, which are widespread in the tropics and midlatitudes. These observations may have implications for subsequent cloud formation cycles and aerosol albedo near cloud edges.

Aerosol Activation Properties within and above Mixing Layer in the North China Plain

NASA Astrophysics Data System (ADS)

Deng, Z.; Ran, L.

2013-12-01

Aerosol particles, serving as cloud condensation nuclei (CCN), may modify the properties of clouds and have an impact on climate. The vertical distribution of aerosols and their activation properties is critical to quantify the effect of aerosols on clouds. An intensive field campaign, Vertical Observations of trace Gases and Aerosols in the North China Plain (VOGA-NCP 2013), was conducted in the North China Plain during the late July and early August 2013 to measure the vertical profiles of atmospheric components in this polluted region and estimate their effects on atmospheric environment and climate. Aerosols were measured with in-situ instruments and Lidar. Particularly, the aerosols were collected at 1000 m height with a 1 m3 bag sampler attached to a tethered balloon, and subsequently measured with combined scanning mobility particle sizer (SMPS) and CCN counter. Comparisons of size-resolved activation ratios at ground level and 1000 m height showed that aerosols in upper atmosphere were not only less concentrated, but also less CCN-active than those at the surface. The difference in aerosol properties between upper atmosphere and the ground indicates that the analysis of impacts of aerosols on cloud might be misleading in heavily polluted region based on the relationship of cloud properties and surface aerosols or column without considering the vertical distribution of aerosol activation abilities.

Deep Blue Retrievals of Asian Aerosol Properties During ACE-Asia

NASA Technical Reports Server (NTRS)

Hsu, N. Christina; Tsay, Si-Cee; King, Michael D.; Herman, Jay R.

2006-01-01

During the ACE-Asia field campaign, unprecedented amounts of aerosol property data in East Asia during springtime were collected from an array of aircraft, shipboard, and surface instruments. However, most of the observations were obtained in areas downwind of the source regions. In this paper, the newly developed satellite aerosol algorithm called "Deep Blue" was employed to characterize the properties of aerosols over source regions using radiance measurements from the Sea-viewing Wide Field-of-view Sensor (SeaWiFS) and Moderate Resolution Imaging Spectroradiometer (MODIS). Based upon the ngstr m exponent derived from the Deep Blue algorithm, it was demonstrated that this new algorithm is able to distinguish dust plumes from fine-mode pollution particles even in complex aerosol environments such as the one over Beijing. Furthermore, these results were validated by comparing them with observations from AERONET sites in China and Mongolia during spring 2001. These comparisons show that the values of satellite-retrieved aerosol optical thickness from Deep Blue are generally within 20%-30% of those measured by sunphotometers. The analyses also indicate that the roles of mineral dust and anthropogenic particles are comparable in contributing to the overall aerosol distributions during spring in northern China, while fine-mode particles are dominant over southern China. The spring season in East Asia consists of one of the most complex environments in terms of frequent cloudiness and wide ranges of aerosol loadings and types. This paper will discuss how the factors contributing to this complexity influence the resulting aerosol monthly averages from various satellite sensors and, thus, the synergy among satellite aerosol products.

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.

Properties of arctic haze aerosol from lidar observations during iarea 2015 campaign on spitsbergen

NASA Astrophysics Data System (ADS)

Stachlewska, Iwona S.; Ritter, Christoph; Böckmann, Christine; Engelmann, Ronny

2018-04-01

Arctic Haze event was observed on 5-8 April 2015 using simultaneously Near-range Aerosol Raman Lidar of IGFUW and Koldewey Aerosol Raman Lidar of AWI, both based at AWIPEV German-French station in Ny-Ålesund, Spitsbergen. The alterations in particle abundance and altitude of the aerosol load observed on following days of the event is analyzed. The daytime profiles of particle optical properties were obtained for both lidars, and then served as input for microphysical parameters inversion. The results indicate aerosol composition typical for the Arctic Haze. However, in some layers, a likely abundance of aqueous aerosol or black carbon originating in biomass burning over Siberia, changes measurably the Arctic Haze properties.

The necessity of microscopy to characterize the optical properties of size-selected, nonspherical aerosol particles.

PubMed

Veghte, Daniel P; Freedman, Miriam A

2012-11-06

It is currently unknown whether mineral dust causes a net warming or cooling effect on the climate system. This uncertainty stems from the varied and evolving shape and composition of mineral dust, which leads to diverse interactions of dust with solar and terrestrial radiation. To investigate these interactions, we have used a cavity ring-down spectrometer to study the optical properties of size-selected calcium carbonate particles, a reactive component of mineral dust. The size selection of nonspherical particles like mineral dust can differ from spherical particles in the polydispersity of the population selected. To calculate the expected extinction cross sections, we use Mie scattering theory for monodisperse spherical particles and for spherical particles with the polydispersity observed in transmission electron microscopy images. Our results for calcium carbonate are compared to the well-studied system of ammonium sulfate. While ammonium sulfate extinction cross sections agree with Mie scattering theory for monodisperse spherical particles, the results for calcium carbonate deviate at large and small particle sizes. We find good agreement for both systems, however, between the calculations performed using the particle images and the cavity ring-down data, indicating that both ammonium sulfate and calcium carbonate can be treated as polydisperse spherical particles. Our results indicate that having an independent measure of polydispersity is essential for understanding the optical properties of nonspherical particles measured with cavity ring-down spectroscopy. Our combined spectroscopy and microscopy techniques demonstrate a novel method by which cavity ring-down spectroscopy can be extended for the study of more complex aerosol particles.

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.

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.

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.

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).

The properties and behavior of α-pinene secondary organic aerosol particles exposed to ammonia under dry conditions

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

Bell, David M.; Imre, Dan; T. Martin, Scot

Chemical transformations and aging of secondary organic aerosol (SOA) particles can alter their physical and chemical properties, including particle morphology. Ammonia, one of the common atmospheric reactive constituents, can react with SOA particles, changing their properties and behavior. At low relative humidity NH3 uptake by α-pinene SOA particles appears to be limited to the particle surface, which suggests that the reacted particles might not be homogeneous and have complex morphology. Here, we present a study aimed at detailed characterization of the effect of ammonia on the composition, density, morphology, shape, and evaporation kinetics of α-pinene SOA particles. We find thatmore » a small amount of NH3 diffuses and reacts throughout the particles bulk, while most of the ammoniated products result from the reaction of NH3 with carboxylic acids on the particle surface, leading to a slight increase in particle size. We show that the reaction products form a solid semi-volatile coating that is a few nanometers thick. This solid coating prevents coagulating particles from coalescing for over two days. However, when the gas phase is diluted this semi-volatile coating evaporates in minutes, which is ensued by rapid coalescence. The ammoniated products in the particle bulk affect particles evaporation kinetics, more so for the smaller particles that contain higher fraction of ammoniated products.« less

Southeast Asian Summer Burning: A Micro Pulse Lidar Network Study of Aerosol Particle Physical Properties near Fires in Borneo and Sumatra

NASA Astrophysics Data System (ADS)

Lolli, S.; Welton, E. J.; Holben, B. N.; Campbell, J. R.

2013-12-01

In August and September 2012, as part of the continuing Seven South East Asian Studies (7-SEAS) project, three autonomous elastic-scattering 355 nm lidars were deployed by the NASA Micro Pulse Lidar Network (MPLNET) to Sumatra and Borneo, measuring the vertical profile of aerosol particle scattering during peak burning season. In coordination with the Aerosol Robotic Network (AERONET), a regional characterization of aerosol particle physical properties and distribution was performed. In addition to a permanent regional network site at Singapore, the three temporary sites established for this research include Jambi (Sumatra, Indonesia), Kuching (northwest Borneo, Malaysia) and Palangkaraya (south-central Borneo, Indonesia). In this paper, we discuss the mission and instruments, and introduce data products available to the community through the MPLNET online website. We further describe initial results of the study, including a contrast of mean vertical scattering profiles versus those observed near active fire sources at Jambi and Palangkaraya, and resolve longer-range particle evolution at receptor sites, like Kuching, that are most commonly 1-2 days downwind of larger fire complexes.

Gas-particle partitioning of alcohol vapors on organic aerosols.

PubMed

Chan, Lap P; Lee, Alex K Y; Chan, Chak K

2010-01-01

Single particle levitation using an electrodynamic balance (EDB) has been found to give accurate and direct hygroscopic measurements (gas-particle partitioning of water) for a number of inorganic and organic aerosol systems. In this paper, we extend the use of an EDB to examine the gas-particle partitioning of volatile to semivolatile alcohols, including methanol, n-butanol, n-octanol, and n-decanol, on levitated oleic acid particles. The measured K(p) agreed with Pankow's absorptive partitioning model. At high n-butanol vapor concentrations (10(3) ppm), the uptake of n-butanol reduced the average molecular-weight of the oleic acid particle appreciably and hence increased the K(p) according to Pankow's equation. Moreover, the hygroscopicity of mixed oleic acid/n-butanol particles was higher than the predictions given by the UNIFAC model (molecular group contribution method) and the ZSR equation (additive rule), presumably due to molecular interactions between the chemical species in the mixed particles. Despite the high vapor concentrations used, these findings warrant further research on the partitioning of atmospheric organic vapors (K(p)) near sources and how collectively they affect the hygroscopic properties of organic aerosols.

Aerosol-Cloud Interactions and Cloud Microphysical Properties in the Asir Region of Saudi Arabia

NASA Astrophysics Data System (ADS)

Kucera, P. A.; Axisa, D.; Burger, R. P.; Li, R.; Collins, D. R.; Freney, E. J.; Buseck, P. R.

2009-12-01

In recent advertent and inadvertent weather modification studies, a considerable effort has been made to understand the impact of varying aerosol properties and concentration on cloud properties. Significant uncertainties exist with aerosol-cloud interactions for which complex microphysical processes link the aerosol and cloud properties. Under almost all environmental conditions, increased aerosol concentrations within polluted air masses will enhance cloud droplet concentration relative to that in unperturbed regions. The interaction between dust particles and clouds are significant, yet the conditions in which dust particles become cloud condensation nuclei (CCN) are uncertain. In order to quantify this aerosol effect on clouds and precipitation, a field campaign was launched in the Asir region, located adjacent to the Red Sea in the southwest region of Saudi Arabia. Ground measurements of aerosol size distributions, hygroscopic growth factors, CCN concentrations as well as aircraft measurements of cloud hydrometeor size distributions were observed in the Asir region in August 2009. The presentation will include a summary of the analysis and results with a focus on aerosol-cloud interactions and cloud microphysical properties observed during the convective season in the Asir region.

Case study of modeled aerosol optical properties during the SAFARI 2000 campaign

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

Kuzmanoski, Maja; Box, Michael A.; Schmid, Beat

2007-08-01

We present modeled aerosol optical properties (single scattering albedo, asymmetry parameter, and lidar ratio) in two layers with different aerosol loadings and particle sizes, observed during the Southern African Regional Science Initiative 2000 (SAFARI 2000) campaign. The optical properties were calculated from aerosol size distributions retrieved from aerosol layer optical thickness spectra, measured using the NASA Ames airborne tracking 14-channel sunphotometer (AATS-14) and the refractive index based on the available information on aerosol chemical composition. The study focuses on sensitivity of modeled optical properties in the 0.3–1.5 μm wavelength range to assumptions regarding the mixing scenario. We considered two modelsmore » for the mixture of absorbing and nonabsorbing aerosol components commonly used to model optical properties of biomass burning aerosol: a layered sphere with absorbing core and nonabsorbing shell and the Maxwell–Garnett effective medium model. In addition, comparisons of modeled optical properties with the measurements are discussed. We also estimated the radiative effect of the difference in aerosol absorption implied by the large difference between the single scattering albedo values (~0.1 at midvisible wavelengths) obtained from different measurement methods for the case with a high amount of biomass burning particles. For that purpose, the volume fraction of black carbon was varied to obtain a range of single scattering albedo values (0.81–0.91 at λ=0.50 μm). Finally, the difference in absorption resulted in a significant difference in the instantaneous radiative forcing at the surface and the top of the atmosphere (TOA) and can result in a change of the sign of the aerosol forcing at TOA from negative to positive.« less

Particle size distribution of the stratospheric aerosol from SCIAMACHY limb measurements

NASA Astrophysics Data System (ADS)

Rozanov, Alexei; Malinina, Elizaveta; Bovensmann, Heinrich; Burrows, John

2017-04-01

A crucial role of the stratospheric aerosols for the radiative budget of the Earth's atmosphere and the consequences for the climate change are widely recognized. A reliable knowledge on physical and optical properties of the stratospheric aerosols as well as on their vertical and spatial distributing is a key issue to assure a proper initialization and running conditions for climate models. On a global scale this information can only be gained from space borne measurements. While a series of past, present and future instruments provide extensive date sets of such aerosol characteristics as extinction coefficient or backscattering ratio, information on a size distribution of the stratospheric aerosols is sparse. One of the important sources on vertically and spatially resolved information on the particle size distribution of stratospheric aerosols is provided by space borne measurements of the scattered solar light in limb viewing geometry performed in visible, near-infrared and short-wave infrared spectral ranges. SCIAMACHY (SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY) instrument operated on the European satellite Envisat from 2002 to 2102 was capable of providing spectral information needed to retrieve parameters of aerosol particle size distributions. In this presentation we discuss the retrieval method, present first validation results with SAGE II data and analyze first data sets of stratospheric aerosol particle size distribution parameters obtained from SCIAMACHY limb measurements. The research work was performed in the framework of ROMIC (Role of the middle atmosphere in climate) project.

Raman Lidar Measurements of Aerosol Optical Properties Performed at CNR- IMAA

NASA Astrophysics Data System (ADS)

Mona, L.; Amodeo, A.; Cornacchia, C.; D'Amico, G.; Madonna, F.; Pandolfi, M.; Pappalardo, G.

2005-12-01

The lidar system for tropospheric aerosol study, located at CNR-IMAA in Tito Scalo, Potenza (40 °36'N, 15°44' E, 760 m above sea level), is a Raman/elastic lidar system operational since May 2000 in the framework of EARLINET (European Aerosol Research LIdar NETwork), the first lidar network for tropospheric aerosol study on continental scale. It provides independent measurements of aerosol extinction and backscatter coefficient profiles at 355 nm and aerosol backscatter profiles at 532 nm. Both the IMAA aerosol lidar system and the used algorithms for the retrieval of aerosol optical parameters have been successfully tested with different intercomparison exercises in the frame of the EARLINET quality assurance program. In the frame of EARLINET, regular measurements are performed three times per week, allowing to study the aerosol content typically present in the planetary boundary layer over Potenza. Particular attention is devoted to Saharan dust intrusions in Europe, and Saharan dust forecasts are distributed to all EARLINET stations. The large dataset of Saharan dust optical properties profiles collected at IMAA allowed to study the contribution of dust particles to the aerosol load typically present in our area as well as to investigate transformations of aerosol optical properties during the transport. Several intensive measurement campaigns have been performed at IMAA with this system to study optical properties of different types of aerosol, and how the transport and modification mechanisms and the water content affect these optical properties. In particular, direct transport of volcanic aerosol emitted in 2002 during the Etna eruptions was observed, and in summer 2004, aerosol layers related to forest fires smoke or pollution plume transported from Alaska, Canada and North America were observed at IMAA during the International Consortium for Atmospheric Research on Transport and Transformation (ICARTT) field campaign. Moreover, this system has been used

Individual Aerosol Particles from Biomass Burning in Southern Africa Compositions and Aging of Inorganic Particles. 2; Compositions and Aging of Inorganic Particles

NASA Technical Reports Server (NTRS)

Li, Jia; Posfai, Mihaly; Hobbs, Peter V.; Buseck, Peter R.

2003-01-01

Individual aerosol particles collected over southern Africa during the SAFARI 2000 field study were studied using transmission electron microscopy and field-emission scanning electron microscopy. The sizes, shapes, compositions, mixing states, surface coatings, and relative abundances of aerosol particles from biomass burning, in boundary layer hazes, and in the free troposphere were compared, with emphasis on aging and reactions of inorganic smoke particles. Potassium salts and organic particles were the predominant species in the smoke, and most were internally mixed. More KCl particles occur in young smoke, whereas more K2SO4 and KNO3 particles were present in aged smoke. This change indicates that with the aging of the smoke, KCl particles from the fires were converted to K2SO4 and KNO3 through reactions with sulfur- and nitrogen- bearing species from biomass burning as well as other sources. More soot was present in smoke from flaming grass fires than bush and wood fires, probably due to the predominance of flaming combustion in grass fires. The high abundance of organic particles and soluble salts can affect the hygroscopic properties of biomass-burning aerosols and therefore influence their role as cloud condensation nuclei. Particles from biomass burning were important constituents of the regional hazes.

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.

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

Aerosol optical properties in the Marine Environment during the TCAP-I campaign

NASA Astrophysics Data System (ADS)

Chand, D.; Berg, L. K.; Barnard, J.; Berkowitz, C. M.; Burton, S. P.; Chapman, E. G.; Comstock, J. M.; Fast, J. D.; Ferrare, R. A.; Connor, F. J.; Hair, J. W.; Hostetler, C. A.; Hubbe, J.; Kluzek, C.; Mei, F.; Pekour, M. S.; Sedlacek, A. J.; Schmid, B.; Shilling, J. E.; Shinozuka, Y.; Tomlinson, J. M.; Wilson, J. M.; Zelenyuk-Imre, A.

2013-12-01

The role of direct radiative forcing by atmospheric aerosol is one of the largest sources of uncertainty in predicting climate change. Much of this uncertainty comes from the limited knowledge of observed aerosol optical properties. In this presentation we discuss derived aerosol optical properties based on measurements made during the summer 2012 Two-Column Aerosol Project-I (TCAP) campaign and relate these properties to the corresponding chemical and physical properties of the aerosol. TCAP was designed to provide simultaneous, in-situ observations of the size distribution, chemical properties, and optical properties of aerosol within and between two atmospheric columns over the Atlantic Ocean near the eastern seaboard of the United States. These columns are separated by 200-300 km and were sampled in July 2012 during a summer intensive operation period (IOP) using the U.S. Department of Energy's Gulfstream-1 (G-1) and NASA's B200 aircraft, winter IOP using G-1 aircraft in February 2013, and the surface-based DOE Atmospheric Radiation Measurement (ARM) Mobile Facility (AMF) located on Cape Cod. In this presentation we examine the spectral dependence of the aerosol optical properties measured from the aircraft over the TCAP-I domain, with an emphasis on in-situ derived intensive properties measured by a 3-λ Nephelometer, a Particle Soot Absorption Photometer (PSAP), a humidograph (f(RH)), and a Single Particle Soot Photometer (SP2). Preliminary results indicate that the aerosol are more light-absorbing as well as more hygroscopic at higher altitudes (2-4 km) compared to the corresponding values made within residual layers near the surface (0-2 km altitude). The average column (0-4 km) single scattering albedo (ω) and hygroscopic scattering factor (F) are found to be ~0.96 and 1.25, respectively. Additional results on key aerosol intensive properties such as the angstrom exponent (å), asymmetry parameter (g), backscattering fraction (b), and gamma parameter (�

The optical properties, physical properties and direct radiative forcing of urban columnar aerosols in the Yangtze River Delta, China

NASA Astrophysics Data System (ADS)

Zhuang, Bingliang; Wang, Tijian; Liu, Jane; Che, Huizheng; Han, Yong; Fu, Yu; Li, Shu; Xie, Min; Li, Mengmeng; Chen, Pulong; Chen, Huimin; Yang, Xiu-qun; Sun, Jianning

2018-02-01

The optical and physical properties as well as the direct radiative forcings (DRFs) of fractionated aerosols in the urban area of the western Yangtze River Delta (YRD) are investigated with measurements from a Cimel sun photometer combined with a radiation transfer model. Ground-based observations of aerosols have much higher temporal resolutions than satellite retrievals. An initial analysis reveals the characteristics of the optical properties of different types of fractionated aerosols in the western YRD. The total aerosols, mostly composed of scattering components (93.8 %), have mean optical depths of 0.65 at 550 nm and refractive index of 1.44 + 0.0084i at 440 nm. The fine aerosols are approximately four times more abundant and have very different compositions from coarse aerosols. The absorbing components account for only ˜ 4.6 % of fine aerosols and 15.5 % of coarse aerosols and have smaller sizes than the scattering aerosols within the same mode. Therefore, fine particles have stronger scattering than coarse ones, simultaneously reflecting the different size distributions between the absorbing and scattering aerosols. The relationships among the optical properties quantify the aerosol mixing and imply that approximately 15 and 27.5 % of the total occurrences result in dust- and black-carbon-dominating mixing aerosols, respectively, in the western YRD. Unlike the optical properties, the size distributions of aerosols in the western YRD are similar to those found at other sites over eastern China on a climatological scale, peaking at radii of 0.148 and 2.94 µm. However, further analysis reveals that the coarse-dominated particles can also lead to severe haze pollution over the YRD. Observation-based estimations indicate that both fine and coarse aerosols in the western YRD exert negative DRFs, and this is especially true for fine aerosols (-11.17 W m-2 at the top of atmosphere, TOA). A higher absorption fraction leads directly to the negative DRF being

Physicochemical properties of fine aerosols at Plan d'Aups during ESCOMPTE

NASA Astrophysics Data System (ADS)

Marinoni, Angela; Laj, Paolo; Deveau, Pierre Alexandre; Marino, Federica; Ghermandi, Grazia; Aulagnier, Fabien; Cachier, Hélène

2005-03-01

The physical and chemical properties of aerosol particles were investigated at Plan d'Aups, one of the ESCOMPTE sites located in the St. Baume mountain area (700 m a.s.l.), 50 km east of Marseilles (France). The site is ideally located for assessing the vertical and horizontal extent of the pollution plume from the Marseilles-Berre area. Our study showed that polluted air masses from the Marseilles-Berre area are advected to Plan d'Aups in the early afternoon. Average daily concentration of particles reaches up to 40 μg m -3 while 1-h average particle number concentration is greater than 30,000 cm -3. Most of the particle mass is composed of SO 42- and organic carbon (OC). The chemical properties of the particles revealed that an additional source, possibly from the industrial area of Gardanne, contributes to the aerosol mass. This last source is characterised by significant emissions of elements, such as Zn, V, Al and Si. In addition to transport, we found that gas-to-particle conversion takes place at the interface between the free troposphere and the boundary layer. We estimated that on average, 30% of the particle number is accounted for by direct nucleation. This is potentially a major aerosol source to the free troposphere.

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.

The Influence of Chemical Composition and Relative Humidity on the Optical Properties of Aerosols During the Southern Oxidant and Aerosol Study (SOAS)

NASA Astrophysics Data System (ADS)

Attwood, A. R.; Washenfelder, R. A.; Brock, C. A.; Brown, S. S.; Hu, W.; Campuzano Jost, P.; Day, D. A.; Palm, B. B.; Simoes de Sa, S.; Jimenez, J. L.

2013-12-01

Atmospheric particles are produced from a wide variety of both anthropogenic and natural sources and play an important role in the Earth's radiative budget by direct scattering and absorption of radiation. To address this impact, in situ measurements of aerosol optical, chemical and hygroscopic properties were performed during the Southern Oxidant and Aerosol Study (SOAS), which took place in the summer of 2013. Ground based measurements of sub-micron aerosol in the southeastern United States were made to investigate the influence of chemical composition and hygroscopicity on aerosol optical properties. We report the wavelength dependence of aerosol extinction cross sections measured with a novel broadband cavity enhanced spectrometer covering a wavelength range of 360-420 nm using two light emitting diodes (LED) and a separate cavity ring down (CRDS) channel. The sensitivity of the relative humidity dependence of extinction based on the type of aerosol present is examined and we show that the optical properties and hygroscopicity of aerosols are greatly influenced by the fraction of sulfate and organics within the particles. Additional data analysis from the SOAS campaign will be presented. The results, thus far, illustrate that the variability in aerosol chemical composition can impact visibility and climate forcing in this region.

Individual Aerosol Particle Types Produced by Savanna Burning

NASA Astrophysics Data System (ADS)

Posfai, M.; Simonics, R.; Li, J.; Hobbs, P. V.; Buseck, P. R.; Buseck, P. R.

2001-12-01

We used analytical transmission electron microscopy (TEM) to study individual aerosol particles that were collected on the University of Washington Convair-580 research aircraft over southern Africa during the Safari2000 Dry Season Experiment. Our goals were to study the compositions, morphologies, and mixing states of carbonaceous particles, in order to better understand the physical and chemical properties of biomass smoke on the individual-particle level. The compositions of single particles were determined using energy-dispersive x-ray spectrometry (EDS) and electron energy-loss spectroscopy (EELS). Energy-loss maps obtained with the TEM are useful for studying the spatial distribution of light elements such as carbon within the particles; thus, they provide a detailed picture of complex particles. Carbonaceous particles were assigned into three main groups on the basis of morphology and composition: "organic particles with inorganic inclusions," "tar balls," and "soot." Soot is recognized by its characteristic morphology and microstructure. The distinction between "organic particles with inorganic inclusions" and "tar balls" is somewhat arbitrary, since the two criteria that are used for their distinction (composition and aspect ratio) change continually. The relative concentrations of the three major particle types vary with the type of fire and distance from fire. In the plume of a smoldering fire west of Beria (August 31) the relative concentration of tar balls increased with aging of the plume. Tar balls have a fairly narrow size distribution with a maximum between 100 and 200 nm (diameter). The inorganic K-salt inclusions (KCl, K2SO4, KNO3) within "organic particles" should make these particles hygroscopic, regardless of the properties of the organic compounds. Aging causes the conversion of KCl into K2SO4, KNO3. Aerosol production from flaming and smoldering fires was compared over Kruger National Park on August 17; more soot and more Cl-rich inclusions

Microspectroscopic Analysis of Anthropogenic- and Biogenic-Influenced Aerosol Particles during the SOAS Field Campaign

NASA Astrophysics Data System (ADS)

Ault, A. P.; Bondy, A. L.; Nhliziyo, M. V.; Bertman, S. B.; Pratt, K.; Shepson, P. B.

2013-12-01

During the summer, the southeastern United States experiences a cooling haze due to the interaction of anthropogenic and biogenic aerosol sources. An objective of the summer 2013 Southern Oxidant and Aerosol Study (SOAS) was to improve our understanding of how trace gases and aerosols are contributing to this relative cooling through light scattering and absorption. To improve understanding of biogenic-anthropogenic interactions through secondary organic aerosol (SOA) formation on primary aerosol cores requires detailed physicochemical characterization of the particles after uptake and processing. Our measurements focus on single particle analysis of aerosols in the accumulation mode (300-1000 nm) collected using a multi orifice uniform deposition impactor (MOUDI) at the Centreville, Alabama SEARCH site. Particles were characterized using an array of microscopic and spectroscopic techniques, including: scanning electron microscopy (SEM), transmission electron microscopy (TEM), energy dispersive X-ray analysis (EDX), and Raman microspectroscopy. These analyses provide detailed information on particle size, morphology, elemental composition, and functional groups. This information is combined with mapping capabilities to explore individual particle spatial patterns and how that impacts structural characteristics. The improved understanding will be used to explore how sources and processing (such as SOA coating of soot) change particle structure (i.e. core shell) and how the altered optical properties impact air quality/climate effects on a regional scale.

Internally mixed soot, sulfates, and organic matter in aerosol particles from Mexico City

NASA Astrophysics Data System (ADS)

Adachi, K.; Buseck, P. R.

2008-05-01

Soot particles are major aerosol constituents that result from emissions of burning of fossil fuel and biomass. Because they both absorb sunlight and contribute to cloud formation, they are an influence on climate on local, regional, and global scales. It is therefore important to evaluate their optical and hygroscopic properties and those effects on the radiation budget. Those properties commonly change through reaction with other particles or gases, resulting in complex internal mixtures. Using transmission electron microscopy, we measured ~8000 particles (25 samples) with aerodynamic diameters from 0.05 to 0.3 μm that were collected in March 2006 from aircraft over Mexico City (MC) and adjacent areas. More than 50% of the particles consist of internally mixed soot, organic matter, and sulfate. Imaging combined with chemical analysis of individual particles show that many are coated, consist of aggregates, or both. Coatings on soot particles can amplify their light absorption, and coagulation with sulfates changes their hygroscopic properties, resulting in shorter lifetime. Our results suggest that a mixture of materials from multiple sources such as vehicles, power plants, and biomass burning occurs in individual particles, thereby increasing their complexity. Through changes in their optical and hygroscopic properties, internally mixed soot particles have a greater effect on the regional climate than uncoated soot particles. Moreover, soot occurs in more than 60% of all particles in the MC plumes, suggesting its important role in the formation of secondary aerosol particles.

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

an aerosol climatology optical properties and its associated direct radiative forcing

NASA Astrophysics Data System (ADS)

Kinne, Stefan

2010-05-01

Aerosol particles are quite complex in nature. Aerosol impacts on the distribution of radiative energy and on cloud microphysics have been debated climate impact issues. Here, a new aerosol-climatology is presented, combining the consistency and completeness of global modelling with quality data by ground-monitoring. It provides global monthly maps for spectral aerosol optical properties and for concentrations of CCN and IN. Based on the optical properties the aerosol direct forcing is determined. And with environmental data for clouds and estimates on the anthropogenic fraction from emission experiments with global modelling even the climate relevant aerosol direct forcing at the top of the atmosphere (ToA) is determined. This value is rather small near -0.2W/m2 with limited uncertainty estimated at (+/-0.3) due to uncertainties in aerosol absorption and underlying surface conditions or clouds.

Spatial Variability of CCN Sized Aerosol Particles

NASA Astrophysics Data System (ADS)

Asmi, A.; Väänänen, R.

2014-12-01

The computational limitations restrict the grid size used in GCM models, and for many cloud types they are too large when compared to the scale of the cloud formation processes. Several parameterizations for e.g. convective cloud formation exist, but information on spatial subgrid variation of the cloud condensation nuclei (CCNs) sized aerosol concentration is not known. We quantify this variation as a function of the spatial scale by using datasets from airborne aerosol measurement campaigns around the world including EUCAARI LONGREX, ATAR, INCA, INDOEX, CLAIRE, PEGASOS and several regional airborne campaigns in Finland. The typical shapes of the distributions are analyzed. When possible, we use information obtained by CCN counters. In some other cases, we use particle size distribution measured by for example SMPS to get approximated CCN concentration. Other instruments used include optical particle counters or condensational particle counters. When using the GCM models, the CCN concentration used for each the grid-box is often considered to be either flat, or as an arithmetic mean of the concentration inside the grid-box. However, the aircraft data shows that the concentration values are often lognormal distributed. This, combined with the subgrid variations in the land use and atmospheric properties, might cause that the aerosol-cloud interactions calculated by using mean values to vary significantly from the true effects both temporary and spatially. This, in turn, can cause non-linear bias into the GCMs. We calculate the CCN aerosol concentration distribution as a function of different spatial scales. The measurements allow us to study the variation of these distributions within from hundreds of meters up to hundreds of kilometers. This is used to quantify the potential error when mean values are used in GCMs.

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

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.

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

Chemical properties and outflow patterns of anthropogenic and dust particles on Rishiri Island during the Asian Pacific Regional Aerosol Characterization Experiment (ACE-Asia)

NASA Astrophysics Data System (ADS)

Matsumoto, Kiyoshi; Uyama, Yukiko; Hayano, Teruaki; Tanimoto, Hiroshi; Uno, Itsushi; Uematsu, Mitsuo

2003-12-01

Investigations of chemical properties and transport mechanisms of continental aerosols are necessary for estimating their influences on global radiative budget and on the global material cycle. Intensive measurements of atmospheric aerosols and the associated species on Rishiri Island, near the northern tip of Japan, were conducted from March to May 2001, in order to understand the chemical properties, source regions, transport pathways, and transport patterns of anthropogenic and mineral aerosols over the east Asian Pacific Rim region during the spring. Mean concentrations of nss-SO42-, NO3-, NH4+, nss-Ca2+ in aerosols were 2.48, 0.64, 0.72, and 0.17 μg m-3, respectively. Elemental carbon and organic carbon in fine particles (d < 2.5 μm) yielded mean concentrations of 0.25 and 0.80 μg m-3, respectively. The concentrations of these species frequently increased to higher values because of outbreaks of continental polluted air masses, whereas under background conditions, they decreased to lower values similar to those observed over the remote ocean. Our results demonstrate that nss-SO42- and NH4+ coexist in fine particles, that NO3- and nss-Ca2+ coexist in coarse particles, and that each set is transported in an alternate manner. Continentally derived NO3- is transported as coarse particle to the east Asian Pacific Rim region. Anthropogenic pollutants and dust particles are not necessarily transported together. It was often found that anthropogenic fine particles containing abundant nss-SO42- appeared first and were then followed by large mineral particles that had absorbed NO3-. Short-term intrusion of the air masses containing abundant particulate carbonaceous compounds, probably due to the influence of biomass burning, also often occurred during the outflow events of continental air masses. Atmospheric behaviors of sulfate, nitrate, and carbonaceous species are different from one another, although they are all derived mainly from combustion processes.

Hygroscopic Measurements of Aerosol Particles in Colorado during the Discover AQ Campaign 2014

NASA Astrophysics Data System (ADS)

Orozco, D.; Delgado, R.; Espinosa, R.; Martins, J. V.; Hoff, R. M.

2014-12-01

In ambient conditions, aerosol particles experience hygroscopic growth due to the influence of relative humidity (RH), scattering more light than when the particles are dry. The quantitative knowledge of the RH effect and its influence on the light scattering and, in particular, on the phase function and polarization of aerosol particles is of substantial importance when comparing ground observations with other optical aerosol measurements such satellite and sunphotometric retrievals of aerosol optical depth and their inversions. In the summer of 2014, the DISCOVER-AQ campaign was held in Colorado, where systematic and concurrent observations of column- integrated surface, and vertically-resolved distributions of aerosols and trace gases relevant to air quality and their evolution during the day were observed. Aerosol optical properties were measured in the UMBC trailer at the city of Golden using a TSI-3563 nephelometer and an in-situ Polarized Imaging Nephelometer (PI-NEPH) designed and built by the LACO group at UMBC. The PI-NEPH measures aerosol phase matrix components in high angular range between 2 and 178 degrees scattering angle at three wavelengths (λ=473, 532 and 671nm). The two measured elements of the phase matrix, intensity (P11) and linear polarization (P12) provide extensive characterization of the scattering properties of the studied aerosol. The scattering coefficient, P11 and P12 were measured under different humidity conditions to obtain the enhancement factor f(RH) and the dependence of P11 and P12 to RH using a humidifier dryer system covering a RH range from 20 to 90%. The ratio between scattering coefficients at high and low humidity in Golden Colorado showed relatively low hygroscopic growth in the aerosol particles f(RH=80%) was 1.27±0.19 for the first three weeks of sampling. According to speciated measurements performed at the UMBC trailer, the predominance of dust and organic aerosols over more hygroscopic nitrate and sulfate in the

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.

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.

Atmospheric Condensational Properties of Ultrafine Chain and Fractal Aerosol Particles

NASA Technical Reports Server (NTRS)

Marlow, William H.

1997-01-01

The purpose for the research sponsored by this grant was to lay the foundations for qualitative understanding and quantitative description of the equilibrium vapor pressure of water vapor over the irregularly shaped, carbonaceous particles that are present in the atmosphere. This work apparently was the first systematic treatment of the subject. Research was conducted in two complementary components: 1. Calculations were performed of the equilibrium vapor pressure of water over particles comprised of aggregates of spheres in the 50-200 nm radius range. The purposes of this work were two-fold. First, since no systematic treatment of this subject had previously been conducted, its availability would be directly useful for quantitative treatment for a limited range of atmospheric aerosols. Second, it would provide qualitative indications of the effects of highly irregular particle shape on equilibrium vapor pressure of aggregates comprised of smaller spheres.

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

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.

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.

Ice nucleating particle concentration during a combustion aerosol event

NASA Astrophysics Data System (ADS)

Adams, Mike; O'Sullivan, Daniel; Porter, Grace; Sanchez-Marroquin, Alberto; Tarn, Mark; Harrison, Alex; McQuaid, Jim; Murray, Benjamin

2017-04-01

The formation of ice in supercooled clouds is important for cloud radiative properties, their lifetime and the formation of precipitation. Cloud water droplets can supercool to below -33oC, but in the presence of Ice Nucleating Particles (INPs) freezing can be initiated at much higher temperatures. The concentration of atmospheric aerosols that are active as INPs depends on a number of factors, such as temperature and aerosol composition and concentration. However, our knowledge of which aerosol types serve as INPs is limited. For example, there has been much discussion over whether aerosol from combustion processes are important as INP. This is significant because combustion aerosol have increased in concentration dramatically since pre-industrial times and therefore have the potential to exert a significant anthropogenic impact on clouds and climate. In this study we made measurements of INP concentrations in Leeds over a specific combustion aerosol event in order to test if there was a correlation between INP concentrations and combustion aerosol. The combustion aerosol event was on the 5th November which is a major bonfire and firework event celebrated throughout the UK. During the event we observed a factor of five increase in aerosol and a factor of 10 increase in black carbon, but observed no significant increase in INP concentration. This implies that black carbon and combustion aerosol did not compete with the background INP during this event.

Classifying aerosol type using in situ surface spectral aerosol optical properties

NASA Astrophysics Data System (ADS)

Schmeisser, Lauren; Andrews, Elisabeth; Ogren, John A.; Sheridan, Patrick; Jefferson, Anne; Sharma, Sangeeta; Kim, Jeong Eun; Sherman, James P.; Sorribas, Mar; Kalapov, Ivo; Arsov, Todor; Angelov, Christo; Mayol-Bracero, Olga L.; Labuschagne, Casper; Kim, Sang-Woo; Hoffer, András; Lin, Neng-Huei; Chia, Hao-Ping; Bergin, Michael; Sun, Junying; Liu, Peng; Wu, Hao

2017-10-01

Knowledge of aerosol size and composition is important for determining radiative forcing effects of aerosols, identifying aerosol sources and improving aerosol satellite retrieval algorithms. The ability to extrapolate aerosol size and composition, or type, from intensive aerosol optical properties can help expand the current knowledge of spatiotemporal variability in aerosol type globally, particularly where chemical composition measurements do not exist concurrently with optical property measurements. This study uses medians of the scattering Ångström exponent (SAE), absorption Ångström exponent (AAE) and single scattering albedo (SSA) from 24 stations within the NOAA/ESRL Federated Aerosol Monitoring Network to infer aerosol type using previously published aerosol classification schemes.Three methods are implemented to obtain a best estimate of dominant aerosol type at each station using aerosol optical properties. The first method plots station medians into an AAE vs. SAE plot space, so that a unique combination of intensive properties corresponds with an aerosol type. The second typing method expands on the first by introducing a multivariate cluster analysis, which aims to group stations with similar optical characteristics and thus similar dominant aerosol type. The third and final classification method pairs 3-day backward air mass trajectories with median aerosol optical properties to explore the relationship between trajectory origin (proxy for likely aerosol type) and aerosol intensive parameters, while allowing for multiple dominant aerosol types at each station.The three aerosol classification methods have some common, and thus robust, results. In general, estimating dominant aerosol type using optical properties is best suited for site locations with a stable and homogenous aerosol population, particularly continental polluted (carbonaceous aerosol), marine polluted (carbonaceous aerosol mixed with sea salt) and continental dust/biomass sites

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

Effects of mixing states on the multiple-scattering properties of soot aerosols.

PubMed

Cheng, Tianhai; Wu, Yu; Gu, Xingfa; Chen, Hao

2015-04-20

The radiative properties of soot aerosols are highly sensitive to the mixing states of black carbon particles and other aerosol components. Light absorption properties are enhanced by the mixing state of soot aerosols. Quantification of the effects of mixing states on the scattering properties of soot aerosol are still not completely resolved, especially for multiple-scattering properties. This study focuses on the effects of the mixing state on the multiple scattering of soot aerosols using the vector radiative transfer model. Two types of soot aerosols with different mixing states such as external mixture soot aerosols and internal mixture soot aerosols are studied. Upward radiance/polarization and hemispheric flux are studied with variable soot aerosol loadings for clear and haze scenarios. Our study showed dramatic changes in upward radiance/polarization due to the effects of the mixing state on the multiple scattering of soot aerosols. The relative difference in upward radiance due to the different mixing states can reach 16%, whereas the relative difference of upward polarization can reach 200%. The effects of the mixing state on the multiple-scattering properties of soot aerosols increase with increasing soot aerosol loading. The effects of the soot aerosol mixing state on upwelling hemispheric flux are much smaller than in upward radiance/polarization, which increase with increasing solar zenith angle. The relative difference in upwelling hemispheric flux due to the different soot aerosol mixing states can reach 18% when the solar zenith angle is 75°. The findings should improve our understanding of the effects of mixing states on the optical properties of soot aerosols and their effects on climate. The mixing mechanism of soot aerosols is of critical importance in evaluating the climate effects of soot aerosols, which should be explicitly included in radiative forcing models and aerosol remote sensing.

Optical properties of aerosol contaminated cloud derived from MODIS instrument

NASA Astrophysics Data System (ADS)

Mei, Linlu; Rozanov, Vladimir; Lelli, Luca; Vountas, Marco; Burrows, John P.

2016-04-01

The presence of absorbing aerosols above/within cloud can reduce the amount of up-welling radiation in visible (VIS) and short-wave infrared and darken the spectral reflectance when compared with a spectrum of a clean cloud observed by satellite instruments (Jethva et al., 2013). Cloud properties retrieval for aerosol contaminated cases is a great challenge. Even small additional injection of aerosol particles into clouds in the cleanest regions of Earth's atmosphere will cause significant effect on those clouds and on climate forcing (Koren et al., 2014; Rosenfeld et al., 2014) because the micro-physical cloud process are non-linear with respect to the aerosol loading. The current cloud products like Moderate Resolution Imaging Spectroradiometer (MODIS) ignoring the aerosol effect for the retrieval, which may cause significant error in the satellite-derived cloud properties. In this paper, a new cloud properties retrieval method, considering aerosol effect, based on the weighting-function (WF) method, is presented. The retrieval results shows that the WF retrieved cloud properties (e.g COT) agrees quite well with MODIS COT product for relative clear atmosphere (AOT ≤ 0.4) while there is a large difference for large aerosol loading. The MODIS COT product is underestimated for at least 2 - 3 times for AOT>0.4, and this underestimation increases with the increase of AOT.

Thermo-optical properties of residential coals and combustion aerosols

NASA Astrophysics Data System (ADS)

Pintér, Máté; Ajtai, Tibor; Kiss-Albert, Gergely; Kiss, Diána; Utry, Noémi; Janovszky, Patrik; Palásti, Dávid; Smausz, Tomi; Kohut, Attila; Hopp, Béla; Galbács, Gábor; Kukovecz, Ákos; Kónya, Zoltán; Szabó, Gábor; Bozóki, Zoltán

2018-04-01

In this study, we present the inherent optical properties of carbonaceous aerosols generated from various coals (hard through bituminous to lignite) and their correlation with the thermochemical and energetic properties of the bulk coal samples. The nanoablation method provided a unique opportunity for the comprehensive investigation of the generated particles under well controlled laboratory circumstances. First, the wavelength dependent radiative features (optical absorption and scattering) and the size distribution (SD) of the generated particulate matter were measured in-situ in aerosol phase using in-house developed and customised state-of-the-art instrumentation. We also investigated the morphology and microstructure of the generated particles using Transmission Electron Microscopy (TEM) and Electron Diffraction (ED). The absorption spectra of the measured samples (quantified by Absorption Angström Exponent (AAE)) were observed to be distinctive. The correlation between the thermochemical features of bulk coal samples (fixed carbon (FC) to volatile matter (VM) ratio and calorific value (CV)) and the AAE of aerosol assembly were found to be (r2 = 0.97 and r2 = 0.97) respectively. Lignite was off the fitted curves in both cases most probably due to its high optically inactive volatile material content. Although more samples are necessary to be investigated to draw statistically relevant conclusion, the revealed correlation between CV and Single Scattering Albedo (SSA) implies that climatic impact of coal combusted aerosol could depend on the thermal and energetic properties of the bulk material.

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

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

Effect of sea breeze circulation on aerosol mixing state and radiative properties in a desert setting

NASA Astrophysics Data System (ADS)

Derimian, Yevgeny; Choël, Marie; Rudich, Yinon; Deboudt, Karine; Dubovik, Oleg; Laskin, Alexander; Legrand, Michel; Damiri, Bahaiddin; Koren, Ilan; Unga, Florin; Moreau, Myriam; Andreae, Meinrat O.; Karnieli, Arnon

2017-09-01

Chemical composition, microphysical, and optical properties of atmospheric aerosol deep inland in the Negev Desert of Israel are found to be influenced by daily occurrences of sea breeze flow from the Mediterranean Sea. Abrupt increases in aerosol volume concentration and shifts of size distributions towards larger sizes, which are associated with increase in wind speed and atmospheric water content, were systematically recorded during the summertime at a distance of at least 80 km from the coast. Chemical imaging of aerosol samples showed an increased contribution of highly hygroscopic particles during the intrusion of the sea breeze. Besides a significant fraction of marine aerosols, the amount of internally mixed marine and mineral dust particles was also increased during the sea breeze period. The number fraction of marine and internally mixed particles during the sea breeze reached up to 88 % in the PM1-2. 5 and up to 62 % in the PM2. 5-10 size range. Additionally, numerous particles with residuals of liquid coating were observed by SEM/EDX analysis. Ca-rich dust particles that had reacted with anthropogenic nitrates were evidenced by Raman microspectroscopy. The resulting hygroscopic particles can deliquesce at very low relative humidity. Our observations suggest that aerosol hygroscopic growth in the Negev Desert is induced by the daily sea breeze arrival. The varying aerosol microphysical and optical characteristics perturb the solar and thermal infrared radiations. The changes in aerosol properties induced by the sea breeze, relative to the background situation, doubled the shortwave radiative cooling at the surface (from -10 to -20.5 W m-2) and increased by almost 3 times the warming of the atmosphere (from 5 to 14 W m-2), as evaluated for a case study. Given the important value of observed liquid coating of particles, we also examined the possible influence of the particle homogeneity assumption on the retrieval of aerosol microphysical characteristics

Monthly and seasonal variations of aerosol optical properties and direct radiative forcing over Zanjan, Iran

NASA Astrophysics Data System (ADS)

Gharibzadeh, Maryam; Alam, Khan; Abedini, Yousefali; Bidokhti, Abbasali Aliakbari; Masoumi, Amir

2017-11-01

Aerosol optical properties and radiative forcing over Zanjan in northwest of Iran has been analyzed during 2010-2013. The aerosol optical and radiative properties are less studied over Zanjan, and therefore, require a careful and in depth analysis. The optical properties like Aerosol Optical Depth (AOD), Ångström Exponent (AE), ASYmmetry parameter (ASY), Single Scattering Albedo (SSA), and Aerosol Volume Size Distribution (AVSD) have been evaluated using the ground-based AErosol RObotic NETwork (AERONET) data. Higher AOD while relatively lower AE were observed in the spring and summer, which showed the presence of coarse mode particles in these seasons. An obvious increase of coarse mode particles in AVSD distribution, as well as a higher value of SSA represented considerable addition of coarse mode particles like dust into the atmosphere of Zanjan in these two seasons. Increase in AE, while a decrease in AOD was detected in the winter and fall. The presence of fine particles indicates the dominance of particles like urban-industrial aerosols from local sources especially in the winter. The Santa Barbara DISORT Atmospheric Radiative Transfer (SBDART) model was utilized to calculate the Aerosol Radiative Forcing (ARF) at the Top of the Atmosphere (TOA), earth's surface and within the atmosphere. The annual averaged ARF values were -13.47 W m-2 and -36.1 W m-2 at the TOA and earth's surface, respectively, which indicate a significant cooling effect. Likewise, the ARF efficiencies at the TOA and earth's surface were -65.08 W m-2 and -158.43 W m-2, respectively. The annual mean atmospheric ARF and heating rate within the atmosphere were 22.63 W m-2 and 0.27 Kday-1 respectively, represented the warming effect within the atmosphere. Finally, a good agreement was found between AERONET retrieved ARF and SBDART simulated ARF.

The Unique Properties of Agricultural Aerosols Measured at a Cattle Feeding Operation

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

Hiranuma, Naruki; Brooks, S. D.; Gramann, J.

2011-05-11

Housing roughly 10 million head of cattle in the United States alone, open air cattle feedlots represent a significant but poorly constrained source of atmospheric particles. Here we present a comprehensive characterization of physical and chemical properties of particles emitted from a large representative cattle feedlot in the Southwest United States. In the summer of 2008, measurements and samplings were conducted at the nominally upwind and downwind edges of the facility. A series of far-field measurements and samplings was also conducted 3.5 km north of the facility. Two instruments, a GRIMM Sequential Mobility Particle Sizer (SMPS) and a GRIMM Portablemore » Aerosol Spectrometer (PAS), were used to measure particle size distributions over the range of 0.01 to 25 μm diameter. Raman microspectroscopy (RM) was used to determine the chemical composition of particles on a single particle basis. Volume size distributions of fugitive dust were dominated by coarse mode particles. Twenty-four hour averaged concentrations of PM10 (particulate matter with a diameter of 10 µm or less) were as high as 1200 μg/m3 during the campaign. The primary constituents of the particulate matter were carbonaceous materials, such as humic acid, water soluble organics, and less soluble fatty acids, including stearic acid and tristearin. A significant fraction of the organic particles was composed of internally mixed with salts. Basic characteristics such as size distribution and composition of agricultural aerosols were found to be different than the properties of those found in urban and semi-urban aerosols. Failing to account for such differences will lead to serious errors in estimates of aerosol effects on climate, visibility, and public health.« less

The unique properties of agricultural aerosols measured at a cattle feeding operation

NASA Astrophysics Data System (ADS)

Hiranuma, N.; Brooks, S. D.; Gramann, J.; Auvermann, B. W.

2011-05-01

Housing roughly 10 million head of cattle in the United States alone, open air cattle feedlots represent a significant but poorly constrained source of atmospheric particles. Here we present a comprehensive characterization of physical and chemical properties of particles emitted from a large representative cattle feedlot in the Southwest United States. In the summer of 2008, measurements and samplings were conducted at the nominally upwind and downwind edges of the facility. A series of far-field measurements and samplings was also conducted 3.5 km north of the facility. Two instruments, a GRIMM Sequential Mobility Particle Sizer (SMPS) and a GRIMM Portable Aerosol Spectrometer (PAS), were used to measure particle size distributions over the range of 0.01 to 25 μm diameter. Raman microspectroscopy (RM) was used to determine the chemical composition of particles on a single particle basis. Volume size distributions of fugitive dust were dominated by coarse mode particles. Twenty-four hour averaged concentrations of PM10 (particulate matter with a diameter of 10 μm or less) were as high as 1200 μg m-3 during the campaign. The primary constituents of the particulate matter were carbonaceous materials, such as humic acid, water soluble organics, and less soluble fatty acids, including stearic acid and tristearin. A significant percentage of the organic particles, up to 28 %, were composed of internally mixed with salts. Basic characteristics such as size distribution and composition of agricultural aerosols were found to be different than the properties of those found in urban and semi-urban aerosols. Failing to account for such differences will lead to serious errors in estimates of aerosol effects on climate, visibility, and public health.

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

Aerosol and Cloud Microphysical Properties in the Asir region of Saudi Arabia

NASA Astrophysics Data System (ADS)

Axisa, Duncan; Kucera, Paul; Burger, Roelof; Li, Runjun; Collins, Don; Freney, Evelyn; Posada, Rafael; Buseck, Peter

2010-05-01

In recent advertent and inadvertent weather modification studies, a considerable effort has been made to understand the impact of varying aerosol properties and concentration on cloud properties. Significant uncertainties exist with aerosol-cloud interactions for which complex microphysical processes link the aerosol and cloud properties. Under almost all environmental conditions, increased aerosol concentrations within polluted air masses will enhance cloud droplet concentration relative to that in unperturbed regions. The interaction between dust particles and clouds are significant, yet the conditions in which dust particles become cloud condensation nuclei (CCN) are uncertain. In order to quantify this aerosol effect on clouds and precipitation, a field campaign was launched in the Asir region of Saudi Arabia as part of a Precipitation Enhancement Feasibility Study. Ground measurements of aerosol size distributions, hygroscopic growth factor, CCN concentrations as well as aircraft measurements of cloud hydrometeor size distributions were done in the Asir region of Saudi Arabia in August 2009. Research aircraft operations focused primarily on conducting measurements in clouds that are targeted for cloud top-seeding, on their microphysical characterization, especially the preconditions necessary for precipitation; understanding the evolution of droplet coalescence, supercooled liquid water, cloud ice and precipitation hydrometeors is necessary if advances are to be made in the study of cloud modification by cloud seeding. Non-precipitating mixed-phase clouds less than 3km in diameter that developed on top of the stable inversion were characterized by flying at the convective cloud top just above the inversion. Aerosol measurements were also done during the climb to cloud base height. The presentation will include a summary of the analysis and results with a focus on the unique features of the Asir region in producing convective clouds, characterization of the

Electrospray ionizer for mass spectrometry of aerosol particles

DOEpatents

He, Siqin; Hogan, Chris; Li, Lin; Liu, Benjamin Y. H.; Naqwi, Amir; Romay, Francisco

2017-09-19

A device and method are disclosed to apply ESI-based mass spectroscopy to submicrometer and nanometer scale aerosol particles. Unipolar ionization is utilized to charge the particles in order to collect them electrostatically on the tip of a tungsten rod. Subsequently, the species composing the collected particles are dissolved by making a liquid flow over the tungsten rod. This liquid with dissolved aerosol contents is formed into highly charged droplets, which release unfragmented ions for mass spectroscopy, such as time-of-flight mass spectroscopy. The device is configured to operate in a switching mode, wherein aerosol deposition occurs while solvent delivery is turned off and vice versa.

A perspective on SOA generated in aerosol water from glyoxal and methylglyoxal and its impacts on climate-relevant aerosol properties

NASA Astrophysics Data System (ADS)

Sareen, N.; McNeill, V. F.

2011-12-01

In recent years, glyoxal and methylglyoxal have emerged to be potentially important SOA precursors with significant implications for climate-related aerosol properties. Here we will discuss how the chemistry of these and similar organic compounds in aerosol water can affect the aerosol optical and cloud formation properties. Aqueous-phase SOA production from glyoxal and methylglyoxal is a potential source of strongly light-absorbing organics, or "brown carbon". We characterized the kinetics of brown carbon formation from these precursors in mixtures of ammonium sulfate and water using UV-Vis spectrophotometry. This mechanism has been incorporated into a photochemical box model with coupled gas phase-aqueous aerosol chemistry. Methylglyoxal and related compounds also may impact an aerosol's ability to act as a cloud condensation nucleus. We recently showed via pendant drop tensiometry and aerosol chamber studies that uptake of methylglyoxal from the gas phase driven by aqueous-phase oligomerization chemistry is a potentially significant, previously unidentified source of surface-active organic material in aerosols. Results from pendant drop tensiometry showed significantly depressed surface tension in methylglyoxal-ammonium sulfate solutions. We further found that ammonium sulfate particles exposed to gas-phase methylglyoxal in a 3.5 m3 aerosol reaction chamber activate into cloud droplets at sizes up to 15% lower at a given supersaturation than do pure ammonium sulfate particles. The observed enhancement exceeds that predicted based on Henry's Law and our measurements of surface tension depression in bulk solutions, suggesting that surface adsorption of methylglyoxal plays a role in determining CCN activity. Methylglyoxal and similar gas-phase surfactants may be an important and overlooked source of enhanced CCN activity in the atmosphere. To characterize the SOA products formed in these solutions, an Aerosol Chemical Ionization Mass Spectrometer (CIMS) was used

Variability in morphology, hygroscopicity, and optical properties of soot aerosols during atmospheric processing

PubMed Central

Zhang, Renyi; Khalizov, Alexei F.; Pagels, Joakim; Zhang, Dan; Xue, Huaxin; McMurry, Peter H.

2008-01-01

The atmospheric effects of soot aerosols include interference with radiative transfer, visibility impairment, and alteration of cloud formation and are highly sensitive to the manner by which soot is internally mixed with other aerosol constituents. We present experimental studies to show that soot particles acquire a large mass fraction of sulfuric acid during atmospheric aging, considerably altering their properties. Soot particles exposed to subsaturated sulfuric acid vapor exhibit a marked change in morphology, characterized by a decreased mobility-based diameter but an increased fractal dimension and effective density. These particles experience large hygroscopic size and mass growth at subsaturated conditions (<90% relative humidity) and act efficiently as cloud-condensation nuclei. Coating with sulfuric acid and subsequent hygroscopic growth enhance the optical properties of soot aerosols, increasing scattering by ≈10-fold and absorption by nearly 2-fold at 80% relative humidity relative to fresh particles. In addition, condensation of sulfuric acid is shown to occur at a similar rate on ambient aerosols of various types of a given mobility size, regardless of their chemical compositions and microphysical structures. Representing an important mechanism of atmospheric aging, internal mixing of soot with sulfuric acid has profound implications on visibility, human health, and direct and indirect climate forcing. PMID:18645179

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.

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.

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

Black carbon mixing state impacts on cloud microphysical properties: effects of aerosol plume and environmental conditions

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

Ching, Ping Pui; Riemer, Nicole; West, Matthew

2016-05-27

Black carbon (BC) is usually mixed with other aerosol species within individual aerosol particles. This mixture, along with the particles' size and morphology, determines the particles' optical and cloud condensation nuclei properties, and hence black carbon's climate impacts. In this study the particle-resolved aerosol model PartMC-MOSAIC was used to quantify the importance of black carbon mixing state for predicting cloud microphysical quantities. Based on a set of about 100 cloud parcel simulations a process level analysis framework was developed to attribute the response in cloud microphysical properties to changes in the underlying aerosol population ("plume effect") and the cloud parcelmore » cooling rate ("parcel effect"). It shows that the response of cloud droplet number concentration to changes in BC emissions depends on the BC mixing state. When the aerosol population contains mainly aged BC particles an increase in BC emission results in increasing cloud droplet number concentrations ("additive effect"). In contrast, when the aerosol population contains mainly fresh BC particles they act as sinks for condensable gaseous species, resulting in a decrease in cloud droplet number concentration as BC emissions are increased ("competition effect"). Additionally, we quantified the error in cloud microphysical quantities when neglecting the information on BC mixing state, which is often done in aerosol models. The errors ranged from -12% to +45% for the cloud droplet number fraction, from 0% to +1022% for the nucleation-scavenged black carbon (BC) mass fraction, from -12% to +4% for the effective radius, and from -30% to +60% for the relative dispersion.« less

Atmospheric Optical Properties and Spectral Analysis of Desert Aerosols

NASA Astrophysics Data System (ADS)

Yvgeni, D.; Karnieli, A.; Kaufman, Y. J.; Andreae, M. O.; Holben, B. N.; Maenhaut, W.

2002-05-01

Scientific background Aerosols can interact directly with solar and terrestrial radiation by scattering as well as absorption. In addition, they can indirectly alter the planetary albedo by modifying the properties of clouds. Objectives Investigations have been devoted to two main areas: (1) Aerosol climatology situation in the Negev desert, investigations of physical and chemical characteristics of aerosols, and study of the local and long-range transport trajectory of polluted air masses over the Negev desert; and (2) An estimation of the optical properties throughout the atmospheric column by surface measurements via performance of spectral and statistical analysis of the data received from two measurement systems. Results and conclusions Analyzed data from the Sede Boker site, in the Negev Desert of Israel, shows an increase in aerosol optical depth during the summer seasons and a decrease during winter. One of the possible reasons for this characteristic is an increase of the precipitable water (reaches 3.0-3.5 cm) due to a constant wind stream from the Mediterranean Sea in same time. The highest probability distribution of the aerosol optical depth is in the range of 0.15-0.20; and of the Angstrom parameter is in range of 0.83 - 1.07. During dust storm events, the scattering coefficient range at 670 nm and 440 nm wavelengths were inverted. It was discovered that the dust particles in this case had non-spherical character. Comparison between optical depth, measured through all atmospheric column, and scattering coefficient from surface measurements provides correlation coefficient (r) equal to 0.64. The Angstrom parameter, calculated via optical depth and via scattering coefficient, provides a correlation coefficient of 0.66. Thus we can obtain an estimate of the influence of the surface aerosol situation on column optical properties. The combined analysis of dust cloud altitude and optical depth as a function of the time indicates long-term transport and

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.

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.

CCN activity of thermodenuded aerosol particles downwind of the Sacramento area urban plume

NASA Astrophysics Data System (ADS)

Hiranuma, N.; Cziczo, D. J.; Nelson, D.; Zhang, Q.; Setyan, A.; Song, C.; Shrivastava, M.; Shilling, J. E.

2010-12-01

This study focuses on the characterization of cloud condensation nuclei (CCN) properties of aerosol particles measured during the Carbonaceous Aerosols and Radiative Effects Study (CARES) near Sacramento, CA in June 2010. Supersaturation-dependant CCN activity (0.07 - 0.5% supersaturation) was measured with DMT CCN counters at two locations; one near the city center (T0) and the other in Cool, CA, a small town located ~40 kilometers downwind of the urban plume in the Sierra Nevada foothills (T1). The T1 CCN counter was operated behind a thermodenuder to study volatility-dependant CCN activity of the urban aerosol plume as it was transported into the biogenically influenced foothills. Preliminary analysis indicated that activated fraction was inversely proportional to the thermodenuder temperature, suggesting that the more-volatile fraction of the aerosol might have played an important role in the CCN activity of the aerosol. The relationship between the chemical composition and CCN activity of the aerosol will be discussed. The physical and chemical transformations of particles aged in the foothills as well as the diurnal profiles of CCN both at T0 and T1 will also be discussed for the transport event of 15 June 2010.

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

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

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.

2011-02-01

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 accompanied by Aerosol Mass Spectrometer (AMS) quantitative aerosol mass loading measurements (Dall'Osto et al., 2009a, b). In this manuscript the origins and properties of four particle types associated with 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, and contains both primary and secondary components. A third class, internally mixed with organic carbon and sulphate (called OC), was found to spike both in the morning and evenings. The fourth class (SOA-PAH) exhibited maximum frequency during the warmest part of the day, and a number of factors point towards secondary production from traffic-related volatile aromatic compounds. Single particle mass spectra of this particle type showed an oxidized polycyclic aromatic compound signature. Finally, a comparison of ATOFMS particle class data is made with factors obtained by Positive Matrix Factorization from AMS data.. Both the Ca-EC and OC particle types correlate with the AMS HOA primary organic fraction (R2 = 0.65 and 0.50 respectively), and Na-EC-OC, but not SOA-PAH, which correlates weakly with the AMS OOA secondary organic aerosol factor (R2 = 0.35). A detailed analysis was conducted to identify ATOFMS particle type(s) representative

Investigation of the seasonal variations of aerosol physicochemical properties and their impact on cloud condensation nuclei number concentration

NASA Astrophysics Data System (ADS)

Logan, Timothy S.

selected four Asian sites. A strongly absorbing mineral dust influence is seen at the Xianghe, Taihu, and SACOL sites during the spring months (MAM) as given by coarse mode dominance. There is a shift towards weakly absorbing pollution (sulfate) and biomass (OC) aerosol dominance in the summer (JJA) and autumn (SON) months as given by a strong fine mode influence. A winter season (DJF) shift toward strongly fine mode, absorbing particles (BC and OC) is observed at Xianghe and Taihu. At Mukdahan, a strong fine mode influence is evident year round with weakly and strongly absorbing biomass particles dominant in the autumn and winter months, respectively, while particles exhibit variable absorption during the spring season. To address SQ2, four cases are selected in Asia to investigate how the optical properties of Asian aerosol plumes change during transport across the remote Pacific Ocean. In addition, six strong smoke events are selected to investigate how the physical and chemical properties of biomass smoke aerosols change during transport in North America. From four selected Asian cases, it was shown by DC-8 aircraft in situ measurements that the Asian plumes contained varying amounts of mineral dust and pollution aerosols during transport. In addition, backward trajectory analysis identified two main dust source regions (Gobi and Taklamakan deserts) and urban/industrial pollution regions in central and eastern China. During the anomalously active wildfire season of 2012 in North America, strong smoke events were observed over the Northern Great Plains region by the Grand Forks, North Dakota, AERONET site and selected as cases. The spectral dependences of absorption aerosol optical depth (AAOD) and o oabs illustrated the varying absorption of the smoke plumes due to carbonaceous particle influences. The AAOD parameter was found to be primarily influenced by aerosol particle size while ooabs was more sensitive to the carbonaceous content. The aerosols likely contain

Investigating the Spectral Dependence of Biomass Burning Aerosol Optical Properties

NASA Astrophysics Data System (ADS)

Odwuor, A.; Corr, C.; Pusede, S.

2016-12-01

Aerosol optical properties, such as light absorption and scattering, are important for understanding how aerosols affect the global radiation budget and for comparison with data gathered from remote sensing. It has been established that the optical properties of aerosols are wavelength dependent, although some remote sensing measurements do not consider this. Airborne measurements of these optical properties were used to calculate the absorption Angstrom exponent, a parameter that characterizes the wavelength dependence of light absorption by aerosols, and single scattering albedo, which measures the relative magnitude of light scattering to total extinction (scattering and absorption combined). Aerosols produced by biomass burning in Saskatchewan, Canada in July 2008 and a forest fire in Southern California, U.S. in June 2016 were included in this analysis. These wildfires were sampled by the NASA DC-8 aircraft during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) and NASA Student Airborne Research Program (SARP) missions, respectively. Aerosol absorption was measured using a particle soot photometer (PSAP) at 470, 532 and 660 nm. Scattering was measured using a 3-wavelength (450, 550 and 700 nm) nephelometer. Absorption Angstrom exponents were calculated at 470 and 660 nm and single scattering albedos were calculated at 450 and 550 nm. Results of this study indicate that disregarding the wavelength dependence of organic aerosol can understate the positive radiative forcing (warming) associated with aerosol absorption.

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

Physical properties of the stratospheric aerosols

NASA Technical Reports Server (NTRS)

Toon, O. B.; Pollack, J. B.

1973-01-01

A comparison of the equilibrium vapor pressure over nitric acid solutions with observed water and nitric acid partial pressures in the stratosphere implies that nitric acid cannot be present as an aerosol particle in the lower stratosphere. A similar comparison for sulfuric acid solutions indicates that sulfuric acid aerosol particles are 75% H2SO4 by weight in water, in good agreement with direct observations. The freezing curve of H2SO4 solutions requires that the H2SO4 aerosol particles be solid or supercooled. The equilibrium vapor pressure of H2SO4 in the stratosphere is of the order of 20 picotorr. At stratospheric temperatures, ammonium sulfate is in a ferroelectric phase. As a result, polar molecules may form a surface coating on these aerosols, which may be a fertile ground for further chemical reaction.

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.

Investigating hygroscopic behavior and phase separation of organic/inorganic mixed phase aerosol particles with FTIR spectroscopy

NASA Astrophysics Data System (ADS)

Zawadowicz, M. A.; Cziczo, D. J.

2013-12-01

Atmospheric aerosol particles can be composed of inorganic salts, such as ammonium sulfate and sodium chloride, and therefore exhibit hygroscopic properties. Many inorganic salts have very well-defined deliquescence and efflorescence points at which they take up and lose water, respectively. For example, the deliquescence relative humidity of pure ammonium sulfate is about 80% and its efflorescence point is about 35%. This behavior of ammonium sulfate is important to atmospheric chemistry because some reactions, such as the hydrolysis of nitrogen pentoxide, occur on aqueous but not crystalline surfaces. Deliquescence and efflorescence of simple inorganic salt particles have been investigated by a variety of methods, such as IR spectroscopy, tandem mobility analysis and electrodynamic balance. Field measurements have shown that atmospheric aerosol are not typically a single inorganic salt, instead they often contain organic as well as inorganic species. Mixed inorganic/organic aerosol particles, while abundant in the atmosphere, have not been studied as extensively. Many recent studies have focused on microscopy techniques that require deposition of the aerosol on a glass slide, possibly changing its surface properties. This project investigates the deliquescence and efflorescence points, phase separation and ability to exchange gas-phase components of mixed organic and inorganic aerosol using a flow tube coupled with FTIR spectroscopy. Ammonium sulfate aerosol mixed with organic polyols with different O:C ratios, including glycerol, 1,2,6-hexanetriol, 1,4-butanediol and 1,5-pentanediol have been investigated. This project aims to study gas-phase exchange in these aerosol systems to determine if exchange is impacted when phase separation occurs.

Evidence for Natural Variability in Marine Stratocumulus Cloud Properties Due to Cloud-Aerosol

NASA Technical Reports Server (NTRS)

Albrecht, Bruce; Sharon, Tarah; Jonsson, Haf; Minnis, Patrick; Minnis, Patrick; Ayers, J. Kirk; Khaiyer, Mandana M.

2004-01-01

In this study, aircraft observations from the Interdisciplinary Remotely-Piloted Aircraft Studies (CIRPAS) Twin Otter are used to characterize the variability in drizzle, cloud, and aerosol properties associated with cloud rifts and the surrounding solid clouds observed off the coast of California. A flight made on 16 July 1999 provided measurements directly across an interface between solid and rift cloud conditions. Aircraft instrumentation allowed for measurements of aerosol, cloud droplet, and drizzle spectra. CCN concentrations were measured in addition to standard thermodynamic variables and the winds. A Forward Scatter Spectrometer Probe (FSSP) measured size distribution of cloud-sized droplets. A Cloud Imaging Probe (CIP) was used to measure distributions of drizzle-sized droplets. Aerosol distributions were obtained from a Cloud Aerosol Scatterprobe (CAS). The CAS probe measured aerosols, cloud droplets and drizzle-sized drops; for this study. The CAS probe was used to measure aerosols in the size range of 0.5 micron - 1 micron. Smaller aerosols were characterized using an Ultrafine Condensation Particle Counter (CPC) sensor. The CPC was used to measure particles with diameters greater than 0.003 micron. By subtracting different count concentrations measured with the CPC, this probe was capable of identifying ultrafine particles those falling in the size range of 3 nanometers - 7 nanometers that are believed to be associated with new particle production.

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

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

Method and apparatus for aerosol particle absorption spectroscopy

DOEpatents

Campillo, Anthony J.; Lin, Horn-Bond

1983-11-15

A method and apparatus for determining the absorption spectra, and other properties, of aerosol particles. A heating beam source provides a beam of electromagnetic energy which is scanned through the region of the spectrum which is of interest. Particles exposed to the heating beam which have absorption bands within the band width of the heating beam absorb energy from the beam. The particles are also illuminated by light of a wave length such that the light is scattered by the particles. The absorption spectra of the particles can thus be determined from an analysis of the scattered light since the absorption of energy by the particles will affect the way the light is scattered. Preferably the heating beam is modulated to simplify the analysis of the scattered light. In one embodiment the heating beam is intensity modulated so that the scattered light will also be intensity modulated when the particles absorb energy. In another embodiment the heating beam passes through an interferometer and the scattered light reflects the Fourier Transform of the absorption spectra.

Optical Properties of Aerosol Types from Satellite and Ground-based Observations

NASA Astrophysics Data System (ADS)

Lin, Tang-Huang; Liu, Gin-Rong; Liu, Chian-Yi

2014-05-01

In this study, the properties of aerosol types are characterized from the aspects of remote sensing and in situ measurements. Particles of dust, smoke and anthropogenic pollutant are selected as the principal types in the study. The measurements of AERONET sites and MODIS data, during the dust storm and biomass burning events in the period from 2002 to 2008, suggest that the aerosol species can be discriminated sufficiently based on the dissimilarity of AE (Ångström exponent) and SSA (single scattering albedo) properties. However, the physicochemical characteristics of source aerosols can be altered after the external/internal combination along the pathway of transportation, thus induce error to the satellite retrievals. In order to eliminate from this kind of errors, the optical properties of mixed aerosols (external) are also simulated with the database of dust and soot aggregates in this study. The preliminary results show that SSA value (at 470 nm) of mineral dust may decay 5-11 % when external mixed with 15-30 % soot aggregates, then result in 11-22 % variation of reflectance observed from satellite which could lead to sufficiently large uncertainty on the retrieval of aerosol optical thickness. As a result, the effect of heterogeneous mixture should be taken into account for more accurate retrieval of aerosol properties, especially after the long-range transport. Keywords: Aerosol type, Ångström exponent, Single scattering albedo, AERONET, MODIS, External mixture

Optical properties of mineral dust aerosol in the thermal infrared

NASA Astrophysics Data System (ADS)

Köhler, Claas H.

2017-02-01

The optical properties of mineral dust and biomass burning aerosol in the thermal infrared (TIR) are examined by means of Fourier Transform Infrared Spectrometer (FTIR) measurements and radiative transfer (RT) simulations. The measurements were conducted within the scope of the Saharan Mineral Dust Experiment 2 (SAMUM-2) at Praia (Cape Verde) in January and February 2008. The aerosol radiative effect in the TIR atmospheric window region 800-1200 cm-1 (8-12 µm) is discussed in two case studies. The first case study employs a combination of IASI measurements and RT simulations to investigate a lofted optically thin biomass burning layer with emphasis on its potential influence on sea surface temperature (SST) retrieval. The second case study uses ground based measurements to establish the importance of particle shape and refractive index for benchmark RT simulations of dust optical properties in the TIR domain. Our research confirms earlier studies suggesting that spheroidal model particles lead to a significantly improved agreement between RT simulations and measurements compared to spheres. However, room for improvement remains, as the uncertainty originating from the refractive index data for many aerosol constituents prohibits more conclusive results.

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.

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.

Global Atmospheric Aerosol Modeling

NASA Technical Reports Server (NTRS)

Hendricks, Johannes; Aquila, Valentina; Righi, Mattia

2012-01-01

Global aerosol models are used to study the distribution and properties of atmospheric aerosol particles as well as their effects on clouds, atmospheric chemistry, radiation, and climate. The present article provides an overview of the basic concepts of global atmospheric aerosol modeling and shows some examples from a global aerosol simulation. Particular emphasis is placed on the simulation of aerosol particles and their effects within global climate models.

AEROSOL CHEMICAL CHARACTERISTION ON BOARD THE DOE G1 AIRCRAFT USING A PARTICLE INTO LIQUID SAMPLER DURING THE TEXAQS 2000 EXPERIMENT.

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

LEE,Y.N.; SONG,Z.; LIU,Y.

2001-01-13

Knowledge of aerosol chemical composition is key to understanding a number of properties of ambient aerosol particles including sources, size/number distribution, chemical evolution, optical properties and human health effects. Although filter based techniques have been widely used to determine aerosol chemical constituents, they generally cannot provide sufficiently fast time resolution needed to investigate sources and chemical evolution that effect aerosol chemical, size and number changes. In order to gain an ability to describe and predict the life cycles of ambient aerosols as a basis for ambient air quality control, fast and sensitive determination of the aerosol chemical composition must bemore » made available. To help to achieve this goal, we deployed a newly developed technique, referred to as PILS (particle-into-liquid-sampler), on the DOE G1 aircraft during the 2000 Texas Air Quality Study (TexAQS 2000) to characterize the major ionic species of aerosol particles with aerodynamic size smaller than 2.5 {micro}m (PM 2.5). The results obtained are examined in the context of other simultaneously collected data for insights into the measurement capability of the PILS system.« less

Comprehensive Airborne in Situ Characterization of Atmospheric Aerosols: From Angular Light Scattering to Particle Microphysics

NASA Astrophysics Data System (ADS)

Espinosa, W. Reed

A comprehensive understanding of atmospheric aerosols is necessary both to understand Earth's climate as well as produce skillful air quality forecasts. In order to advance our understanding of aerosols, the Laboratory for Aerosols, Clouds and Optics (LACO) has recently developed the Imaging Polar Nephelometer instrument concept for the in situ measurement of aerosol scattering properties. Imaging Nephelometers provide measurements of absolute phase function and polarized phase function over a wide angular range, typically 3 degrees to 177 degrees, with an angular resolution smaller than one degree. The first of these instruments, the Polarized Imaging Nephelometer (PI-Neph), has taken part in five airborne field experiments and is the only modern aerosol polar nephelometer to have flown aboard an aircraft. A method for the retrieval of aerosol optical and microphysical properties from I-Neph measurements is presented and the results are compared with existing measurement techniques. The resulting retrieved particle size distributions agree to within experimental error with measurements made by commercial optical particle counters. Additionally, the retrieved real part of the refractive index is generally found to be within the predicted error of 0.02 from the expected values for three species of humidified salt particles, whose refractive index is well established. A synopsis is then presented of aerosol scattering measurements made by the PI-Neph during the Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) and the Deep Convection Clouds and Chemistry (DC3) field campaigns. To better summarize these extensive datasets a novel aerosol classification scheme is developed, making use of ancillary data that includes gas tracers, chemical composition, aerodynamic particle size and geographic location, all independent of PI-Neph measurements. Principal component analysis (PCA) is then used to reduce the

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

Climatology and Characteristics of Aerosol Optical Properties in the Arctic

NASA Astrophysics Data System (ADS)

Schmeisser, Lauren; Ogren, John; Backman, John; Asmi, Eija; Andrews, Elisabeth; Jefferson, Anne; Bergin, Michael; Tunved, Peter; Sharma, Sangeeta; Starkweather, Sandra

2016-04-01

Within the Arctic, climate forcers like atmospheric aerosols are important contributors to the observed warming and environmental changes in the region. Quantifying the forcing by aerosols in the Arctic is especially difficult, given short aerosol lifetimes, annual variability in illumination and surface albedo, stratified atmospheric conditions, complex feedbacks, and long-range aerosol transport. However, in-situ surface measurements of Arctic aerosol optical properties can be used to constrain variability of light scattering and absorption, identify potential particle sources, and help evaluate the resulting forcing. Data from six WMO Global Atmosphere Watch stations are presented: Alert, Canada (ALT); Barrow, Alaska (BRW); Pallas, Finland (PAL); Summit, Greenland (SUM); Tiksi, Russia (TIK); and Zeppelin Mountain, Norway (ZEP). These sites contribute to the International Arctic System for Observing the Atmosphere (IASOA), which facilitates Arctic-wide data collection and analysis. Climatologies of aerosol optical properties from each station show differences in magnitude and variability of observed parameters. For example, most stations (ALT, BRW, SUM, TIK, ZEP) experience maximum scattering in winter/spring, while PAL exhibits maximum scattering in the summer. The observed range in scattering across these sites is large (almost an order of magnitude) - SUM has the lowest annual median scattering at 0.82 Mm-1 while BRW has the highest at 6.9 Mm-1. A closer look at systematic variability between optical properties at each station, as well as site back trajectories, suggest differences in aerosol processes, sources and transport. The development of consistent climatologies and additional analyses like the ones presented here can help provide a better understanding of trans-Arctic aerosol variability, which can be an asset for improving aerosol models in this unique and remote region.

Aeronet-based Microphysical and Optical Properties of Smoke-dominated Aerosol near Source Regions and Transported over Oceans, and Implications for Satellite Retrievals of Aerosol Optical Depth

NASA Technical Reports Server (NTRS)

Sayer, A. M.; Hsu, N. C.; Eck, T. F.; Smirnov, A.; Holben, B. N.

2013-01-01

Smoke aerosols from biomass burning are an important component of the global aerosol cycle. Analysis of Aerosol Robotic Network (AERONET) retrievals of size distribution and refractive index reveals variety between biomass burning aerosols in different global source regions, in terms of aerosol particle size and single scatter albedo (SSA). Case studies of smoke transported to coastal/island AERONET sites also mostly lie within the range of variability at near-source sites. Two broad families of aerosol properties are found, corresponding to sites dominated by boreal forest burning (larger, broader fine mode, with midvisible SSA 0.95), and those influenced by grass, shrub, or crop burning with additional forest contributions (smaller, narrower particles with SSA 0.88-0.9 in the midvisible). The strongest absorption is seen in southern African savanna at Mongu (Zambia), with average SSA 0.85 in the midvisible. These can serve as candidate sets of aerosol microphysicaloptical properties for use in satellite aerosol optical depth (AOD) retrieval algorithms. The models presently adopted by these algorithms over ocean are often insufficiently absorbing to represent these biomass burning aerosols. A corollary of this is an underestimate of AOD in smoke outflow regions, which has important consequences for applications of these satellite datasets.

Satellite remote sensing of aerosol and cloud properties over Eurasia

NASA Astrophysics Data System (ADS)

Sogacheva, Larisa; Kolmonen, Pekka; Saponaro, Giulia; Virtanen, Timo; Rodriguez, Edith; Sundström, Anu-Maija; Atlaskina, Ksenia; de Leeuw, Gerrit

2015-04-01

surface properties, the surface reflectance can be independently retrieved using the AOD for atmospheric correction. For the retrieval of cloud properties, the SACURA algorithm has been implemented in the ADV/ASV aerosol retrieval suite. Cloud properties retrieved from AATSR data are cloud fraction, cloud optical thickness, cloud top height, cloud droplet effective radius, liquid water path. Aerosol and cloud properties are applied for different studies over the Eurasia area. Using the simultaneous retrieval of aerosol and cloud properties allows for study of the transition from the aerosol regime to the cloud regime, such as changes in effective radius or AOD (aerosol optical depth) to COT (cloud optical thickness). The column- integrated aerosol extinction, aerosol optical depth or AOD, which is primarily reported from satellite observations, can be used as a proxy for cloud condensation nuclei (CCN) and hence contains information on the ability of aerosol particles to form clouds. Hence, connecting this information with direct observations of cloud properties provides information on aerosol-cloud interactions.

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;

Sensitivity of Multiangle Imaging to the Optical and Microphysical Properties of Biomass Burning Aerosols

NASA Technical Reports Server (NTRS)

Chen, Wei-Ting; Kahn, Ralph A.; Nelson, David; Yau, Kevin; Seinfeld, John H.

2008-01-01

The treatment of biomass burning (BB) carbonaceous particles in the Multiangle Imaging SpectroRadiometer (MISR) Standard Aerosol Retrieval Algorithm is assessed, and algorithm refinements are suggested, based on a theoretical sensitivity analysis and comparisons with near-coincident AERONET measurements at representative BB sites. Over the natural ranges of BB aerosol microphysical and optical properties observed in past field campaigns, patterns of retrieved Aerosol Optical Depth (AOD), particle size, and single scattering albedo (SSA) are evaluated. On the basis of the theoretical analysis, assuming total column AOD of 0.2, over a dark, uniform surface, MISR can distinguish two to three groups in each of size and SSA, except when the assumed atmospheric particles are significantly absorbing (mid-visible SSA approx.0.84), or of medium sizes (mean radius approx.0.13 pin); sensitivity to absorbing, medium-large size particles increases considerably when the assumed column AOD is raised to 0.5. MISR Research Aerosol Retrievals confirm the theoretical results, based on coincident AERONET inversions under BB-dominated conditions. When BB is externally mixed with dust in the atmosphere, dust optical model and surface reflection uncertainties, along with spatial variability, contribute to differences between the Research Retrievals and AERONET. These results suggest specific refinements to the MISR Standard Aerosol Algorithm complement of component particles and mixtures. They also highlight the importance for satellite aerosol retrievals of surface reflectance characterization, with accuracies that can be difficult to achieve with coupled surface-aerosol algorithms in some higher AOD situations.

Optical, physical, and chemical properties of springtime aerosol over Barrow Alaska in 2008

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

Shantz, Nicole C.; Gultepe, Ismail; Andrews, Elisabeth

2014-03-06

Airborne observations from four flights during the 2008 Indirect and Semi-Direct Aerosol Campaign (ISDAC) are used to examine some cloud-free optical, physical, and chemical properties of aerosol particles in the springtime Arctic troposphere. The number concentrations of particles larger than 0.12 μm (Na>120), important for light extinction and cloud droplet formation, ranged from 15 to 2260 cm -3, with the higher Na>120 cases dominated by measurements from two flights of long-range transported biomass burning (BB) aerosols. The two other flights examined here document a relatively clean aerosol and an Arctic Haze aerosol impacted by larger particles largely composed of dust.more » For observations from the cleaner case and the BB cases, the particle light scattering coefficients at low relative humidity (RH<20%) increased nonlinearly with increasing Na>120, driven mostly by an increase in mean sizes of particles with increasing Na>120 (BB cases). For those three cases, particle light absorption coefficients also increased nonlinearly with increasing Na>120 and linearly with increasing submicron particle volume concentration. In addition to black carbon, brown carbon was estimated to have increased light absorption coefficients by 27% (450 nm wavelength) and 14% (550 nm) in the BB cases. For the case with strong dust influence, the absorption relative to submicron particle volume was small compared with the other cases. There was a slight gradient of Passive Cavity Aerosol Spectrometer Probe (PCASP) mean volume diameter (MVD) towards smaller sizes with increasing height, which suggests more scavenging of the more elevated particles, consistent with a typically longer lifetime of particles higher in the atmosphere. However, in approximately 10% of the cases, the MVD increased (>0.4 μm) with increasing altitude, suggesting transport of larger fine particle mass (possibly coarse particle mass) at high levels over the Arctic. This may be because of transport of

Hygroscopic properties of large aerosol particles using the example of aged Saharan mineral dust - a semi-automated electron microscopy approach

NASA Astrophysics Data System (ADS)

Hartmann, Markus; Heim, Lars-Oliver; Ebert, Martin; Weinbruch, Stephan; Kandler, Konrad

2015-04-01

Hygroscopic properties of large aerosol particles using the example of aged Saharan mineral dust - a semi-automated electron microscopy approach Markus Hartmann(1), Lars-Oliver Heim(2), Martin Ebert(1), Stephan Weinbruch(1), Konrad Kandler(1) The Saharan Aerosol Long-range Transport and Aerosol-Cloud-Interaction Experiment (SALTRACE) took place at Barbados from June 10 to July 15 2013. During this period, dust was frequently transported from Africa across the Atlantic Ocean toward the Caribbean. In this study, we investigate the atmospheric aging of the dust aerosol based on its hygroscopicity. Aerosol samples were collected ground-based at Ragged Point (13°9'54.4"N, 59°25'55.7"W) with a single round jet cascade impactor on nickel-substrates. The particles from the stage with a 50% efficiency cutoff size of 1 µm were analyzed with an Environmental Scanning Electron Microscope (ESEM) equipped with an energy-dispersive X-ray detector (EDX) and a cooling stage. In an initial automated run, information on particle size and chemical composition for elements heavier than carbon were gathered. Afterwards, electron microscope images of the same sample areas as before were taken during a stepwise increase of relative humidities (between 50 % and 92%), so that the hygroscopic growth of the droplets could be directly observed. The observed hygroscopic growth can be correlated to the chemical composition of the respective particles. For the automated analysis of several hundred images of droplets an image processing algorithm in Python was developed. The algorithm is based on histogram equalization and watershed segmentation. Since SEM images can only deliver two-dimensional information, but the hygroscopic growth factor usually refers to the volume of a drop, Atomic Force Microscopy (AFM) was used to derive an empirical function for the drop volume depending on the apparent drop diameter in the electron images. Aside from the mineral dust, composed of mostly silicates and

Optical and microphysical properties of atmospheric aerosols in Moldova

NASA Astrophysics Data System (ADS)

Aculinin, Alexandr; Smicov, Vladimir

2010-05-01

Measurements of aerosol properties in Kishinev, Moldova are being carried out within the framework of the international AERONET program managed by NASA/GSFC since 1999. Direct solar and sky diffuse radiances are measured by using of sunphotometer Cimel-318. Aerosol optical properties are retrieved from measured radiances by using of smart computational procedures developed by the AERONET's team. The instrument is situated at the ground-based solar radiation monitoring station giving the opportunity to make simultaneous spectral (win sunphotometer) and broadband (with the set of sensors from radiometric complex) solar radiation. Detailed description of the station and investigations in progress can be found at the http://arg.phys.asm.md. Ground station is placed in an urban environment of Kishinev city (47.00N; 28.56E; 205 m a.s.l). Summary of aerosol optical and microphysical properties retrieved from direct solar and diffuse sky radiance observations at Moldova site from September 1999 to June 2009 are presented below. Number of measurements (total): 1695 Number of measurements (for ?o, n, k): 223 Range of aerosol optical depth (AOD) @440 nm: 0.03 < ?(440) < 2.30, < ?(440)>=0.25 Range of Ångström parameter < α440_870 >: 0.14 < α < 2.28 Asymmetry factor (440/670/870/1020): 0.70/0.63/0.59/0.58 ±0.04 Refraction (n) and absorption (k) indices@440 nm: 1.41 ± 0.06; 0.009 ± 0.005 Single scattering albedo < ?o >(440/670/870/1020): 0.93/0.92/0.90/0.89 ±0.04 Parameters of volume particle size distribution function: (fine mode) volume median radius r v,f , μm: 0.17 ± 0.06 particle volume concentration Cv,f, μm3/μm2: 0.04 ± 0.03 (coarse mode) volume median radius rv,c , μm: 3.08 ± 0.64 particle volume concentration Cv,c, μm3/μm2: 0.03 ± 0.03 Climatic norms of AOD@500 nm and Ångström parameter < α440_870 > at the site of observation are equal to 0.21 ± 0.06 and 1.45 ± 0.14, respectively. The aerosol type in Moldova may be considered as 'urban

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...

Beyond the Alphabet Soup: Molecular Properties of Aerosol Components Influence Optics. (Invited)

NASA Astrophysics Data System (ADS)

Thompson, J. E.

2013-12-01

Components within atmospheric aerosols exhibit almost every imaginable model of chemical bonding and physical diversity. The materials run the spectrum from crystalline to amorphous, covalent to ionic, and have varying viscosities, phase, and hygroscopicity. This seminar will focus on the molecular properties of materials that influence the optical behavior of aerosols. Special focus will be placed on the polarizability of materials, hygroscopic growth, and particle phase.

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.

North Atlantic Aerosol Radiative Impacts Based on Satellite Measurements and Aerosol Intensive Properties from TARFOX and ACE-2

NASA Technical Reports Server (NTRS)

Russell, P. B.; Bergstrom, Robert W.; Schmid, B.; Livingston, J. M.

2000-01-01

We estimate the impact of North Atlantic aerosols on the net short-wave flux at the tropopause by combining satellite-derived aerosol optical depth (AOD) maps with model aerosol properties determined via closure analyses in TARFOX and ACE 2. We exclude African dust, primarily by restricting latitudes to 25-60 N. The analyses use in situ aerosol composition measurements and air- and ship-borne sun-photometer measurements of AOD spectra. The aerosol model yields computed flux sensitivities (dFlux/dAOD) that agree with measurements by airborne flux radiometers in TARFOX. Its midvisible single-scattering albedo is 0.9. which is in the range obtained from in situ measurements of scattering and absorption in both TARFOX and ACE 2. Combining satellite-derived AOD maps with the aerosol model yields maps of 24-hour average net radiative flux changes. For simultaneous AVHRR, radiance measurements exceeded the sunphotometer AODs by about 0.04. However. shipboard sunphotometer and AVHRR AODs agreed Within 0.02 for data acquired during satellite overflights on two other days. We discuss attempts to demonstrate column closure within the MBL by comparing shipboard sunphotometer AODs and values calculated from simultaneous shipboard in-situ aerosol size distribution measurements. These comparisons were mostly unsuccessful, but they illustrate the difficulties inherent in this type of closure analysis. Specifically, AODs derived from near-surface in-situ size distribution measurements are extremely sensitive to the assumed hygroscopic growth model that itself requires an assumption of particle composition as a function of height and size, to the radiosonde-measured relative humidity, and to the vertical profile of particle number. We investigate further the effects of hygroscopic particle growth within the MBL by using shipboard lidar aerosol backscatter profiles together with the sunphotometer AOD.

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

Physico-chemical properties of aerosols in Sao Paulo, Brazil and mechanisms of secondary organic aerosol formation.

NASA Astrophysics Data System (ADS)

Artaxo, Paulo; Ferreira de Brito, Joel; Varanda Rizzo, Luciana; Luiza Godoy, Maria; Godoy, Jose Marcus

2013-04-01

Megacities emissions are increasingly becoming a global issue, where emissions from the transportation sector play an increasingly important role. Sao Paulo is a megacity with a population of about 18 million people, 7 million cars and large-scale industrial emissions. As a result of the vehicular and industrial emissions, the air quality in Sao Paulo is bellow WMO standards for aerosol particles and ozone. Many uncertainties are found on gas- and particulate matter vehicular emission factors and their following atmospheric processes, e.g. secondary organic aerosol formation. Due to the uniqueness of the vehicular fuel in Brazil, largely based on ethanol use, such characterization currently holds further uncertainties. To improve the understanding of the role of this unique emission characteristics, we are running a source apportionment study in Sao Paulo focused on the mechanisms of organic aerosol formation. One of the goals of this study is a quantitative aerosol source apportionment focused on vehicular emissions, including ethanol and gasohol (both fuels used by light-duty vehicles). This study comprises four sampling sites with continuous measurements for one year, where trace elements and organic aerosol are being measured for PM2.5 and PM10 along with real-time NOx, O3, PM10 and CO measurements. Aerosol optical properties and size distribution are being measured on a rotation basis between sampling stations. Furthermore, a Proton-Transfer-Reaction Mass Spectrometer (PTR-MS) and an Aerosol Chemical Speciation Monitor (ACSM) are used to measure in real time VOCs and aerosol composition, respectively. Trace elements were measured using XRF and OC/EC analysis was determined with a Sunset OC/EC instrument. A TSI Nephelometer with 3 wavelengths measure light scattering and a MAAP measure black carbon. Results show aerosol number concentrations ranging between 10,000 and 35,000 cm-3, mostly concentrated in the nucleation and Aitken modes, with a peak in size at 80

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.

Optical properties of aerosols at Grand Canyon National Park

NASA Astrophysics Data System (ADS)

Malm, William C.; Day, Derek E.

Visibility in the United States is expected to improve over the next few decades because of reduced emissions, especially sulfur dioxide. In the eastern United States, sulfates make up about 60-70% of aerosol extinction, while in the inner mountain west that fraction is only about 30%. In the inner mountain west, carbon aerosols make up about 35% of extinction, while coarse mass contributes between 15 and 25% depending on how absorption is estimated. Although sulfur dioxide emissions are projected to decrease, carbon emissions due to prescribed fire activity will increase by factors of 5-10, and while optical properties of sulfates have been extensively studied, similar properties of carbon and coarse particles are less well understood. The inability to conclusively apportion about 50% of the extinction budget motivated a study to examine aerosol physio-chemical-optical properties at Grand Canyon, Arizona during the months of July and August. Coarse particle mass has usually been assumed to consist primarily of wind-blown dust, with a mass-scattering efficiency between about 0.4 and 0.6 m 2 g -1. Although there were episodes where crustal material made up most of the coarse mass, on the average, organics and crustal material mass were about equal. Furthermore, about one-half of the sampling periods had coarse-mass-scattering efficiencies greater than 0.6 m 2 g -1 and at times coarse-mass-scattering efficiencies were near 1.0 m 2 g -1. It was shown that absorption by coarse- and fine-particle absorption were about equal and that both fine organic and sulfate mass-scattering efficiencies were substantially less than the nominal values of 4.0 and 3.0 m 2 g -1 that have typically been used.

Perspective: Aerosol microphysics: From molecules to the chemical physics of aerosols

NASA Astrophysics Data System (ADS)

Bzdek, Bryan R.; Reid, Jonathan P.

2017-12-01

Aerosols are found in a wide diversity of contexts and applications, including the atmosphere, pharmaceutics, and industry. Aerosols are dispersions of particles in a gas, and the coupling of the two phases results in highly dynamic systems where chemical and physical properties like size, composition, phase, and refractive index change rapidly in response to environmental perturbations. Aerosol particles span a wide range of sizes from 1 nm to tens of micrometres or from small molecular clusters that may more closely resemble gas phase molecules to large particles that can have similar qualities to bulk materials. However, even large particles with finite volumes exhibit distinct properties from the bulk condensed phase, due in part to their higher surface-to-volume ratio and their ability to easily access supersaturated solute states inaccessible in the bulk. Aerosols represent a major challenge for study because of the facile coupling between the particle and gas, the small amounts of sample available for analysis, and the sheer breadth of operative processes. Time scales of aerosol processes can be as short as nanoseconds or as long as years. Despite their very different impacts and applications, fundamental chemical physics processes serve as a common theme that underpins our understanding of aerosols. This perspective article discusses challenges in the study of aerosols and highlights recent chemical physics advancements that have enabled improved understanding of these complex systems.

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

Measurement of aerosol optical properties by integrating cavity ring-down spectroscopy and nephelometery

NASA Astrophysics Data System (ADS)

Tedela, Getachew; Singh, Sujeeta; Fiddler, Marc; Bililign, Solomon

2013-03-01

Accurate measurement of optical properties of aerosols is crucial for quantifying the influence of aerosols on climate. Aerosols that scatter and absorb radiation can have a cooling or warming effect depending on the magnitude of the respective scattering and absorption terms. One example is black carbon known for its strong absorption. The reported refractive indices for black carbon particles range from 1.2 +0i to 2.75 +1.44i. Our work attempts to measure extinction coefficient, and scattering coefficient of black carbon particles at different incident beam wavelengths using a cavity ring-down spectrometer and a Nephelometer and compare to Mie theory predictions. We report calibration results using polystyrene latex spheres and preliminary results on using commercial black carbon particles. The work is supported by the Department of Defense grant W911NF-11-1-0188.

On-the-fly cross flow laser guided separation of aerosol particles

NASA Astrophysics Data System (ADS)

Lall, A. A.; Terray, A.; Hart, S. J.

2010-08-01

Laser separation of particles is achieved using forces resulting from the momentum exchange between particles and photons constituting the laser radiation. Particles can experience different optical forces depending on their size and/or optical properties, such as refractive index. Thus, particles can move at different speeds in the presence of an optical force, leading to spatial separations. Several studies for aqueous suspension of particles have been reported in the past. In this paper, we present extensive analysis for optical forces on non-absorbing aerosol particles. We used a loosely focused Gaussian 1064 nm laser to simultaneously hold and deflect particles entrained in flow perpendicular to their direction of travel. The gradient force is used to hold the particles against the viscous drag for a short period of time. The scattering force simultaneously pushes the particles during this period. Theoretical calculations are used to simulate particle trajectories and to determine the net deflection: a measure of the ability to separate. We invented a novel method for aerosol generation and delivery to the flow cell. Particle motion was imaged using a high speed camera working at 3000+ frames per second with a viewing area up to a few millimeters. An 8W near-infrared 1064 nm laser was used to provide the optical force to the particles. Theoretical predictions were corroborated with measurements using polystyrene latex particles of 20 micron diameter. We measured particle deflections up to about 1500 microns. Such large deflections represent a new milestone for optical chromatography in the gas phase.

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.

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.

SAGE II Measurements of Stratospheric Aerosol Properties at Non-Volcanic Levels

NASA Technical Reports Server (NTRS)

Thomason, Larry W.; Burton, Sharon P.; Luo, Bei-Ping; Peter, Thomas

2008-01-01

Since 2000, stratospheric aerosol levels have been relatively stable and at the lowest levels observed in the historical record. Given the challenges of making satellite measurements of aerosol properties at these levels, we have performed a study of the sensitivity of the product to the major components of the processing algorithm used in the production of SAGE II aerosol extinction measurements and the retrieval process that produces the operational surface area density (SAD) product. We find that the aerosol extinction measurements, particularly at 1020 nm, remain robust and reliable at the observed aerosol levels. On the other hand, during background periods, the SAD operational product has an uncertainty of at least a factor of 2 during due to the lack of sensitivity to particles with radii less than 100 nm.

Individual Aerosol Particles from Biomass Burning in Southern Africa. 1; Compositions and Size Distributions of Carbonaceous Particles

NASA Technical Reports Server (NTRS)

Posfai, Mihaly; Simonics, Renata; Li, Jia; Hobbs, Peter V.; Buseck, Peter R.

2003-01-01

Individual aerosol particles in smoke plumes from biomass fires and in regional hazes in southern Africa were studied using analytical transmission electron microscopy (TEM), which allowed detailed characterization of carbonaceous particle types in smoke and determination of changes in particle properties and concentrations during smoke aging. Based on composition, morphology, and microstructure, three distinct types of carbonaceous particles were present in the smoke: organic particles with inorganic (K-salt) inclusions, tar ball particles, and soot. The relative number concentrations of organic particles were largest in young smoke, whereas tar balls were dominant in a slightly aged (1 hour) smoke from a smoldering fire. Flaming fires emitted relatively more soot particles than smoldering fires, but soot was a minor constituent of all studied plumes. Further aging caused the accumulation of sulfate on organic and soot particles, as indicated by the large number of internally mixed organic/sulfate and soot/sulfate particles in the regional haze. Externally mixed ammonium sulfate particles dominated in the boundary layer hazes, whereas organic/sulfate particles were the most abundant type in the upper hazes. Apparently, elevated haze layers were more strongly affected by biomass smoke than those within the boundary layer. Based on size distributions and the observed patterns of internal mixing, we hypothesize that organic and soot particles are the cloud-nucleating constituents of biomass smoke aerosols. Sea-salt particles dominated in the samples taken in stratus clouds over the Atlantic Ocean, off the coast of Namibia, whereas a distinct haze layer above the clouds consisted of aged biomass smoke particles.

[Aerosol optical properties during different air-pollution episodes over Beijing].

PubMed

Shi, Chan-Zhen; Yu, Xing-Na; Zhou, Bin; Xiang, Lei; Nie, Hao-Hao

2013-11-01

Based on the 2005-2011 data from Aerosol Robotic Network (AERONET), this study conducted analysis on aerosol optical properties over Beijing during different air-pollution episodes (biomass burning, CNY firework, dust storm). The aerosol optical depth (AOD) showed notable increases in the air-pollution episodes while the AOD (at 440 nm) during dust storm was 4. 91, 4. 07 and 2.65 times higher as background, biomass burning and firework aerosols. AOD along with Angstrom exponent (alpha) can be used to determine the aerosol types. The dust aerosol had the highest AOD and the lowest alpha. The alpha value of firework (1.09) was smaller than biomass burning (1.21) and background (1.27), indicating that coarse particles were dominant in the former type. Higher AOD of burnings (than background) can be attributed to the optical extinction capability of black carbon aerosol. The single scattering albedo (SSA) was insensitive to wavelength. The SSA value of dust (0.934) was higher than background (0.878), biomass burning (0.921) and firework (0.905). Additionally, the extremely large SSA of burnings here maybe was caused by the aging smoke, hygroscopic growth and so on. The peak radius of aerosol volume size distributions were 0.1-0.2 microm and 2.24 -3.85 microm in clear and polluted conditions. The value of volume concentration ratio between coarse and fine particles was in the order of clear background (1.04), biomass burning (1.10), CNY firework (1.91) and dust storm (4.96) episode.

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.

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

A study of remotely sensed aerosol properties from ground-based sun and sky scanning radiometers

NASA Astrophysics Data System (ADS)

Giles, David M.

Aerosol particles impact human health by degrading air quality and affect climate by heating or cooling the atmosphere. The Indo-Gangetic Plain (IGP) of Northern India, one of the most populous regions in the world, produces and is impacted by a variety of aerosols including pollution, smoke, dust, and mixtures of them. The NASA Aerosol Robotic Network (AERONET) mesoscale distribution of Sun and sky-pointing instruments in India was established to measure aerosol characteristics at sites across the IGP and around Kanpur, India, a large urban and industrial center in the IGP, during the 2008 pre-monsoon (April-June). This study focused on detecting spatial and temporal variability of aerosols, validating satellite retrievals, and classifying the dominant aerosol mixing states and origins. The Kanpur region typically experiences high aerosol loading due to pollution and smoke during the winter and high aerosol loading due to the addition of dust to the pollution and smoke mixture during the pre-monsoon. Aerosol emissions in Kanpur likely contribute up to 20% of the aerosol loading during the pre-monsoon over the IGP. Aerosol absorption also increases significantly downwind of Kanpur indicating the possibility of the black carbon emissions from aerosol sources such as coal-fired power plants and brick kilns. Aerosol retrievals from satellite show a high bias when compared to the mesoscale distributed instruments around Kanpur during the pre-monsoon with few high quality retrievals due to imperfect aerosol type and land surface characteristic assumptions. Aerosol type classification using the aerosol absorption, size, and shape properties can identify dominant aerosol mixing states of absorbing dust and black carbon particles. Using 19 long-term AERONET sites near various aerosol source regions (Dust, Mixed, Urban/Industrial, and Biomass Burning), aerosol absorption property statistics are expanded upon and show significant differences when compared to previous work

Column and Near-surface Aerosol Properties during TCAP: Temporal Changes in a Coastal Region

NASA Astrophysics Data System (ADS)

Kassianov, E.; Barnard, J.; Pekour, M. S.; Berg, L. K.; Shilling, J. E.; Fast, J. D.; Michalsky, J. J.; Lantz, K. O.; Hodges, G.

2013-12-01

An important problem facing climate-related studies is to separate the impacts of naturally occurring and anthropogenic aerosol. This problem is even more challenging in coastal regions located downwind of large metropolitan areas. Cape Cod situated on the easternmost portion of Massachusetts (along the east coast of the United States) is an example of one of these regions. The Two-Column Aerosol Project (TCAP; http://campaign.arm.gov/tcap/) was designed to study the evolution of optical, microphysical and chemical properties of both marine aerosol and aerosol transported from North America to the Atlantic as well as their impact on the radiation energy budget. The TCAP has been recently conducted (2012-2013) on Cape Cod with support from the U.S. Department of Energy's (DOE's) Atmospheric Radiation Measurement (ARM) Program (http://www.arm.gov/). During the TCAP, the ground-based ARM Mobile Facility (AMF) was deployed on Cape Cod. The AMF site (at 41.87°N; 70.28°W) was equipped with numerous instruments for sampling aerosol, cloud and radiative properties, including a Multi-Filter Rotating Shadowband Radiometer (MFRSR), a Scanning Mobility Particle Sizer (SMPS), an Aerodynamic Particle Sizer (APS), a three-wavelength nephelometer, and suite of instruments to measure the aerosol chemical composition. In this study we present an analysis of diurnal and day-to-day variability of the column and near-surface aerosol properties obtained from remote sensing (MFRSR data) and in situ measurements (SMPS, APS, nephelometer, chemical composition), respectively. The importance of this variability to direct aerosol radiative forcing at different time scales and its relation to the long-range transport will be discussed. Some regional model results will also be presented.

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.

Chemical apportionment of aerosol optical properties during the Asia-Pacific Economic Cooperation summit in Beijing, China

NASA Astrophysics Data System (ADS)

Han, Tingting; Xu, Weiqi; Chen, Chen; Liu, Xingang; Wang, Qingqing; Li, Jie; Zhao, Xiujuan; Du, Wei; Wang, Zifa; Sun, Yele

2015-12-01

We have investigated the chemical and optical properties of aerosol particles during the 2014 Asia-Pacific Economic Cooperation (APEC) summit in Beijing, China, using the highly time-resolved measurements by a high-resolution aerosol mass spectrometer and a cavity attenuated phase shift extinction monitor. The average (±σ) extinction coefficient (bext) and absorption coefficient (bap) were 186.5 (±184.5) M m-1 and 23.3 (±21.9) M m-1 during APEC, which were decreased by 63% and 56%, respectively, compared to those before APEC primarily due to strict emission controls. The aerosol composition and size distributions showed substantial changes during APEC; as a response, the mass scattering efficiency (MSE) of PM1 was decreased from 4.7 m2 g-1 to 3.5 m2 g-1. Comparatively, the average single-scattering albedo (SSA) remained relatively unchanged, illustrating the synchronous reductions of bext and bap during APEC. MSE and SSA were found to increase as function of the oxidation degree of organic aerosol (OA), indicating a change of aerosol optical properties during the aging processes. The empirical relationships between chemical composition and particle extinction were established using a multiple linear regression model. Our results showed the largest contribution of ammonium nitrate to particle extinction, accounting for 35.1% and 29.3% before and during APEC, respectively. This result highlights the important role of ammonium nitrate in the formation of severe haze pollution during this study period. We also observed very different optical properties of primary and secondary aerosol. Owing to emission controls in Beijing and surrounding regions and also partly the influences of meteorological changes, the average bext of secondary aerosol during APEC was decreased by 71% from 372.3 M m-1 to 108.5 M m-1, whereas that of primary aerosol mainly from cooking, traffic, and biomass burning emissions showed a smaller reduction from 136.7 M m-1 to 71.3 M m-1. As a result

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

An Accurate Analytic Approximation for Light Scattering by Non-absorbing Spherical Aerosol Particles

NASA Astrophysics Data System (ADS)

Lewis, E. R.

2017-12-01

The scattering of light by particles in the atmosphere is a ubiquitous and important phenomenon, with applications to numerous fields of science and technology. The problem of scattering of electromagnetic radiation by a uniform spherical particle can be solved by the method of Mie and Debye as a series of terms depending on the size parameter, x=2πr/λ, and the complex index of refraction, m. However, this solution does not provide insight into the dependence of the scattering on the radius of the particle, the wavelength, or the index of refraction, or how the scattering varies with relative humidity. Van de Hulst demonstrated that the scattering efficiency (the scattering cross section divided by the geometric cross section) of a non-absorbing sphere, over a wide range of particle sizes of atmospheric importance, depends not on x and m separately, but on the quantity 2x(m-1); this is the basis for the anomalous diffraction approximation. Here an analytic approximation for the scattering efficiency of a non-absorbing spherical particle is presented in terms of this new quantity that is accurate over a wide range of particle sizes of atmospheric importance and which readily displays the dependences of the scattering efficiency on particle radius, index of refraction, and wavelength. For an aerosol for which the particle size distribution is parameterized as a gamma function, this approximation also yields analytical results for the scattering coefficient and for the Ångström exponent, with the dependences of scattering properties on wavelength and index of refraction clearly displayed. This approximation provides insight into the dependence of light scattering properties on factors such as relative humidity, readily enables conversion of scattering from one index of refraction to another, and demonstrates the conditions under which the aerosol index (the product of the aerosol optical depth and the Ångström exponent) is a useful proxy for the number of cloud

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.

The study of thin films on solid aerosol particles using optical trapping and Mie scattering from a broadband white LED

NASA Astrophysics Data System (ADS)

Jones, Stephanie H.; King, Martin D.; Ward, Andrew D.

2014-09-01

A counter-propagating optical trap has been used to study thin organic films on the surface of solid particles levitated in air. Micron sized silica spheres have been trapped in air between opposed 1064 nm laser beams, and illuminated with a broadband white LED. Backscattered light from the trapped particle was collected to obtain a Mie spectrum over the 495-670 nm wavelength range and this was used to determine particle radius and wavelength dependent refractive index (Jones et al., 2013). The trapped particle was coated using a flow of organic vapour and the resultant thin film analysed using a coated sphere model. Resonance positions in the Mie spectrum were monitored with time in order to determine film formation, thickness and refractive index. Whilst thin films are believed to form naturally on atmospheric aerosols (Tervahattu et al., 2002), a debate remains as to whether the organic component completely coats the aerosol surface or partially engulfs it. Such films are readily oxidised in the atmosphere causing a change in aerosol properties and knowledge of aerosol properties is required to understand their effect on the climate. The use of optical trapping combined with Mie spectra acquisition to study and characterise coated solid particles is therefore an important step in atmospheric science.

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.;

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.

Near-Cloud Aerosol Properties from the 1 Km Resolution MODIS Ocean Product

NASA Technical Reports Server (NTRS)

Varnai, Tamas; Marshak, Alexander

2014-01-01

This study examines aerosol properties in the vicinity of clouds by analyzing high-resolution atmospheric correction parameters provided in the MODIS (Moderate Resolution Imaging Spectroradiometer) ocean color product. The study analyzes data from a 2 week long period of September in 10 years, covering a large area in the northeast Atlantic Ocean. The results indicate that on the one hand, the Quality Assessment (QA) flags of the ocean color product successfully eliminate cloud-related uncertainties in ocean parameters such as chlorophyll content, but on the other hand, using the flags introduces a sampling bias in atmospheric products such as aerosol optical thickness (AOT) and Angstrom exponent. Therefore, researchers need to select QA flags by balancing the risks of increased retrieval uncertainties and sampling biases. Using an optimal set of QA flags, the results reveal substantial increases in optical thickness near clouds-on average the increase is 50% for the roughly half of pixels within 5 km from clouds and is accompanied by a roughly matching increase in particle size. Theoretical simulations show that the 50% increase in 550nm AOT changes instantaneous direct aerosol radiative forcing by up to 8W/m2 and that the radiative impact is significantly larger if observed near-cloud changes are attributed to aerosol particles as opposed to undetected cloud particles. These results underline that accounting for near-cloud areas and understanding the causes of near-cloud particle changes are critical for accurate calculations of direct aerosol radiative forcing.

MASS SPECTROMETRY OF INDIVIDUAL AEROSOL PARTICLES. (R823980)

EPA Science Inventory

Typically, in real-time aerosol mass spectrometry (RTAMS), individual airborne particles
are ablated and ionized with a single focused laser pulse. This technique yields information that
permits bulk characterization of the particle, but information about the particle's sur...

Importance of the mixing state for ice nucleating capabilities of individual aerosol particles

NASA Astrophysics Data System (ADS)

Ebert, Martin; Worringen, Annette; Benker, Nathalie; Weinbruch, Stephan

2010-05-01

The effects of aerosol particles on heterogeneous ice formation are currently insufficiently understood. Modelling studies have shown that the type and quantity of atmospheric aerosol particles acting as ice nuclei (IN) can influence ice cloud microphysical and radiative properties as well as their precipitation efficiency. Therefore, the physicochemical identification of IN and a quantitative description of the ice nucleation processes are crucial for a better understanding of formation, life cycles, and the optical properties of clouds as well as for numerical precipitation forecast. During the CLACE 5 campaign in 2006 at the high alpine research station Jungfraujoch (3580 m asl), Switzerland, the physicochemical parameters of IN within mixed-phase clouds were studied. By the use of special Ice-Counterflow Virtual Impactor, residual particles of small ice nuclei (IN) and the interstitial aerosol fraction were sampled seperately within mixed-phase clouds. The size, morphology, elemental composition and mixing state of more than 7000 particles of selected IN- and interstitial-samples were analyzed by scanning electron microscopy (SEM) combined with energy-dispersive X-ray analysis (EDX). For selected particles, the mineralogical phase composition was determined by transmission electron microscopy. In order to receive detailed information about the mixing state (coatings, agglomerates, heterogeneous inclusions) of the IN- and interstitial-samples, the complete individual particle analysis was performed operator controlled. Four different particle types were identified to act as IN. 1) Carbonaceous particles, which were identified to be a complex mixture of soot (main component), sulfate and nitrate. 2) Complex mixtures of two or more diverse particle groups. In almost 75% of these particles silicates or metal oxides are the main-component. 3) Aluminium oxide particles, which were internally mixed with calcium and sulphate rich material and 4) Pb bearing particles

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

Reactions and mass spectra of complex particles using Aerosol CIMS

NASA Astrophysics Data System (ADS)

Hearn, John D.; Smith, Geoffrey D.

2006-12-01

Aerosol chemical ionization mass spectrometry (CIMS) is used both on- and off-line for the analysis of complex laboratory-generated and ambient particles. One of the primary advantages of Aerosol CIMS is the low degree of ion fragmentation, making this technique well suited for investigating the reactivity of complex particles. To demonstrate the usefulness of this "soft" ionization, particles generated from meat cooking were reacted with ozone and the composition was monitored as a function of reaction time. Two distinct kinetic regimes were observed with most of the oleic acid in these particles reacting quickly but with 30% appearing to be trapped in the complex mixture. Additionally, detection limits are measured to be sufficiently low (100-200 ng/m3) to detect some of the more abundant constituents in ambient particles, including sulfate, which is measured in real-time at 1.2 [mu]g/m3. To better characterize complex aerosols from a variety of sources, a novel off-line collection method was also developed in which non-volatile and semi-volatile organics are desorbed from particles and concentrated in a cold U-tube. Desorption from the U-tube followed by analysis with Aerosol CIMS revealed significant amounts of nicotine in cigarette smoke and levoglucosan in oak and pine smoke, suggesting that this may be a useful technique for monitoring particle tracer species. Additionally, secondary organic aerosol formed from the reaction of ozone with R-limonene and volatile organics from orange peel were analyzed off-line showing large molecular weight products (m/z > 300 amu) that may indicate the formation of oligomers. Finally, mass spectra of ambient aerosol collected offline reveal a complex mixture of what appears to be highly processed organics, some of which may contain nitrogen.

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.

Properties of jet engine combustion particles during the PartEmis experiment: Microphysics and Chemistry

NASA Astrophysics Data System (ADS)

Petzold, A.; Stein, C.; Nyeki, S.; Gysel, M.; Weingartner, E.; Baltensperger, U.; Giebl, H.; Hitzenberger, R.; Döpelheuer, A.; Vrchoticky, S.; Puxbaum, H.; Johnson, M.; Hurley, C. D.; Marsh, R.; Wilson, C. W.

2003-07-01

The particles emitted from an aircraft engine combustor were investigated in the European project PartEmis. Measured aerosol properties were mass and number concentration, size distribution, mixing state, thermal stability of internally mixed particles, hygroscopicity, and cloud condensation nuclei (CCN) activation potential. The combustor operation conditions corresponded to modern and older engine gas path temperatures at cruise altitude, with fuel sulphur contents (FSC) of 50, 410, and 1270 μg g-1. Operation conditions and FSC showed only a weak influence on the microphysical aerosol properties, except for hygroscopic and CCN properties. Particles of size D >= 30 nm were almost entirely internally mixed. Particles of sizes D < 20 nm showed a considerable volume fraction of compounds that volatilise at 390 K (10-15%) and 573 K (4-10%), while respective fractions decreased to <5% for particles of size D >= 50 nm.

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.

Aerosol Optical Properties over Northwestern European Seas

NASA Astrophysics Data System (ADS)

Avgousta Floutsi, Athina; Korras Carraca, Marios Bruno; Matsoukas, Christos; Riva, Riccardo; Biskos, George

2017-04-01

Atmospheric aerosols, both natural and anthropogenic, can affect the regional and global climate through their direct, indirect, and semi-direct effects on the radiative energy budget of the Earth-atmosphere system. In order to quantify these effects it is necessary to determine the aerosol load. An effective way to do this is by measuring the aerosol optical depth (AOD). Besides AOD, the Fine mode Fraction (AOD of particles smaller than 1 μm / total AOD, FF) is a useful parameter for the characterization of the aerosol and provides a good proxy for particle size. In this study, we investigate the spatial and temporal variability of the AOD and FF over the Western and Northwestern European Seas (43° N - 67° N, 10° W - 31° E), where significant sources of both natural and anthropogenic particles are located. Anthropogenic particles (mostly fine mode) originate from ship activity, or from urban-industrial and biomass-burning processes in the European countries. The natural, coarse mode particles are primarily sea salt. The study is performed using Collection 006 Level-3 mean daily aerosol data from the Moderate Resolution Imaging Spectroradiometer (MODIS) instrument on board Aqua satellite, available in 1° × 1° resolution (ca. 100 km × 100 km) over the period 2002- 2014. Our results indicate significant spatial variability of the aerosol load over the study region. The highest AOD values (up to 0.32 on annual level) are observed over the English Channel and the coasts of the Netherlands and Germany. In these regions the highest FF values are also observed (up to 0.77), indicating a relatively large contribution of anthropogenic particles to the aerosol load. Offshore, both AOD and FF are lower compared to coastal regions, indicating the predominance of maritime aerosols (sea salt). The data also show a clear seasonal cycle, with larger aerosol load during spring and summer (AOD up to 0.60), and lower during autumn and winter (AOD up to 0.30). A similar

An aerosol climatology for a rapidly growing arid region (southern Arizona): Major aerosol species and remotely sensed aerosol properties

NASA Astrophysics Data System (ADS)

Sorooshian, Armin; Wonaschütz, Anna; Jarjour, Elias G.; Hashimoto, Bryce I.; Schichtel, Bret A.; Betterton, Eric A.

2011-10-01

This study reports a comprehensive characterization of atmospheric aerosol particle properties in relation to meteorological and back trajectory data in the southern Arizona region, which includes two of the fastest growing metropolitan areas in the United States (Phoenix and Tucson). Multiple data sets (MODIS, AERONET, OMI/TOMS, MISR, GOCART, ground-based aerosol measurements) are used to examine monthly trends in aerosol composition, aerosol optical depth (AOD), and aerosol size. Fine soil, sulfate, and organics dominate PM2.5 mass in the region. Dust strongly influences the region between March and July owing to the dry and hot meteorological conditions and back trajectory patterns. Because monsoon precipitation begins typically in July, dust levels decrease, while AOD, sulfate, and organic aerosol reach their maximum levels because of summertime photochemistry and monsoon moisture. Evidence points to biogenic volatile organic compounds being a significant source of secondary organic aerosol in this region. Biomass burning also is shown to be a major contributor to the carbonaceous aerosol budget in the region, leading to enhanced organic and elemental carbon levels aloft at a sky-island site north of Tucson (Mt. Lemmon). Phoenix exhibits different monthly trends for aerosol components in comparison with the other sites owing to the strong influence of fossil carbon and anthropogenic dust. Trend analyses between 1988 and 2009 indicate that the strongest statistically significant trends are reductions in sulfate, elemental carbon, and organic carbon, and increases in fine soil during the spring (March-May) at select sites. These results can be explained by population growth, land-use changes, and improved source controls.

A Comparison of Aerosol Optical Property Measurements Made During the DOE Aerosol Intensive Operating Period and Their Effects on Regional Climate

NASA Technical Reports Server (NTRS)

Strawa, Anthony W.; Hallar, A. G.; Arnott, W. P.; Covert, D.; Elleman, R.; Ogren, J.; Schmid, B.; Luu, A.

2004-01-01

The amount of radiant energy an aerosol absorbs has profound effects on climate and air quality. It is ironic that aerosol absorption coefficient is one of the most difficult to measure aerosol properties. One of the main purposes of the DOE Aerosol Intensive Operating Period (IOP) flown in May, 2003 was to assess our ability to measure absorption coefficient in situ. This paper compares measurements of aerosol optical properties made during the IOP. Measurements of aerosol absorption coefficient were made by Particle Soot Absorption Photometer (PSAP) aboard the CIRPAS Twin-Otter (U. Washington) and on the DOE Cessna 172 (NOAA-C,MDL). Aerosol absorption coefficient was also measured by a photoacoustic instrument (DRI) that was operated on an aircraft for the first time during the IOP. A new cavity ring-down (CRD) instrument, called Cadenza (NASA-AkC), measures the aerosol extinction coefficient for 675 nm and 1550 nm light, and simultaneously measures the scattering coefficient at 675 nm. Absorption coefficient is obtained from the difference of measured extinction and scattering within the instrument. Measurements of absorption coefficient from all of these instruments during appropriate periods are compared. During the IOP, several significant aerosol layers were sampled aloft. These layers are identified in the remote (AATS-14) as well as in situ measurements. Extinction profiles measured by Cadenza are compared to those derived from the Ames Airborne Tracking Sunphotometer (AATS-14, NASA-ARC). The regional radiative impact of these layers is assessed by using the measured aerosol optical properties in a radiative transfer model.

Aerosol optical properties and direct radiative forcing based on measurements from the China Aerosol Remote Sensing Network (CARSNET) in eastern China

NASA Astrophysics Data System (ADS)

Che, Huizheng; Qi, Bing; Zhao, Hujia; Xia, Xiangao; Eck, Thomas F.; Goloub, Philippe; Dubovik, Oleg; Estelles, Victor; Cuevas-Agulló, Emilio; Blarel, Luc; Wu, Yunfei; Zhu, Jun; Du, Rongguang; Wang, Yaqiang; Wang, Hong; Gui, Ke; Yu, Jie; Zheng, Yu; Sun, Tianze; Chen, Quanliang; Shi, Guangyu; Zhang, Xiaoye

2018-01-01

Aerosol pollution in eastern China is an unfortunate consequence of the region's rapid economic and industrial growth. Here, sun photometer measurements from seven sites in the Yangtze River Delta (YRD) from 2011 to 2015 were used to characterize the climatology of aerosol microphysical and optical properties, calculate direct aerosol radiative forcing (DARF) and classify the aerosols based on size and absorption. Bimodal size distributions were found throughout the year, but larger volumes and effective radii of fine-mode particles occurred in June and September due to hygroscopic growth and/or cloud processing. Increases in the fine-mode particles in June and September caused AOD440 nm > 1.00 at most sites, and annual mean AOD440 nm values of 0.71-0.76 were found at the urban sites and 0.68 at the rural site. Unlike northern China, the AOD440 nm was lower in July and August (˜ 0.40-0.60) than in January and February (0.71-0.89) due to particle dispersion associated with subtropical anticyclones in summer. Low volumes and large bandwidths of both fine-mode and coarse-mode aerosol size distributions occurred in July and August because of biomass burning. Single-scattering albedos at 440 nm (SSA440 nm) from 0.91 to 0.94 indicated particles with relatively strong to moderate absorption. Strongly absorbing particles from biomass burning with a significant SSA wavelength dependence were found in July and August at most sites, while coarse particles in March to May were mineral dust. Absorbing aerosols were distributed more or less homogeneously throughout the region with absorption aerosol optical depths at 440 nm ˜ 0.04-0.06, but inter-site differences in the absorption Angström exponent indicate a degree of spatial heterogeneity in particle composition. The annual mean DARF was -93 ± 44 to -79 ± 39 W m-2 at the Earth's surface and ˜ -40 W m-2 at the top of the atmosphere (for the solar zenith angle range of 50 to 80°) under cloud-free conditions. The fine mode

Effect of pH and leucine concentration on aerosolization properties of carrier-free formulations of levofloxacin.

PubMed

Barazesh, Ahmadreza; Gilani, Kambiz; Rouini, Mohammadreza; Barghi, Mohammad Ali

2018-06-15

The aim of this study was to evaluate the effect of leucine at different pH values preferred for inhalation on particle characteristics and aerosolization performance of spray dried carrier-free formulations of levofloxacin. A full factorial design was applied to optimize the formulation containing levofloxacin with or without leucine in different pH values and the optimum condition was determined. Particle size and morphology, crystallinity state, electrostatic charge and surface composition of the particles were determined. Aerodynamic properties of the powders were also assessed by an Andersen cascade impactor after aerosolization through an Aerolizer® at an air flow rate of 60 L/min. The pH of initial solution affected various physical properties of the drug containing particles and hence their in vitro deposition. The profound effect of pH was on water content, electrostatic charge and surface composition of the particles. The negative effect of water content on in vitro deposition of the drug was covered by preferred surface accumulation of leucine at pH 6. Optimum formulation which obtained by co-spray drying of the drug with 21.79% leucine at pH 5.98 presented a fine particle fraction equal to 54.38. In conclusion, changing pH of the initial solution influenced the effect of leucine on aerosolization of levofloxacine spray dried particles by modification of their physical properties. Copyright © 2018 Elsevier B.V. All rights reserved.

Imaginary refractive index and other microphysical properties of volcanic ash, Sarahan dust, and other mineral aerosols

NASA Astrophysics Data System (ADS)

Rocha Lima, A.; Martins, J.; Krotkov, N. A.; Artaxo, P.; Todd, M.; Ben Ami, Y.; Dolgos, G.; Espinosa, R.

2013-12-01

Aerosol properties are essential to support remote sensing measurements, atmospheric circulation and climate models. This research aims to improve the understanding of the optical and microphysical properties of different types of aerosols particles. Samples of volcanic ash, Saharan dust and other mineral aerosols particles were analyzed by different techniques. Ground samples were sieved down to 45um, de-agglomerated and resuspended in the laboratory using a Fluidized Bed Aerosol Generator (FBAG). Particles were collected on Nuclepore filters into PM10, PM2.5, or PM1.0. and analyzed by different techniques, such as Scanning Electron Microscopy (SEM) for determination of size distribution and shape, spectral reflectance for determination of the optical absorption properties as a function of the wavelength, material density, and X-Ray fluorescence for the elemental composition. The spectral imaginary part of refractive index from the UV to the short wave infrared (SWIR) wavelength was derived empirically from the measurements of the spectral mass absorption coefficient, size distribution and density of the material. Some selected samples were also analyzed with the Polarized Imaging Nephelometer (PI-Neph) instrument for the characterization of the aerosol polarized phase function. This work compares results of the spectral refractive index of different materials obtained by our methodology with those available in the literature. In some cases there are significant differences both in magnitude and spectral dependence of the imaginary refractive index. These differences are evaluated and discussed in this work.

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

Chemical composition, microstructure, and hygroscopic properties of aerosol particles at the Zotino Tall Tower Observatory (ZOTTO), Siberia, during a summer campaign

DOE PAGES

Mikhailov, E. F.; Mironov, G. N.; Pöhlker, C.; ...

2015-03-16

In this study we describe the hygroscopic properties of accumulation- and coarse-mode aerosol particles sampled at the Zotino Tall Tower Observatory (ZOTTO) in Central Siberia (61° N; 89° E) from 16 to 21 June 2013. The hygroscopic growth measurements were supplemented with chemical analyses of the samples, including inorganic ions and organic/elemental carbon. In addition, the microstructure and chemical composition of aerosol particles were analyzed by X-ray micro-spectroscopy (STXM-NEXAFS) and transmission electron microscopy (TEM). A mass closure analysis indicates that organic carbon accounted for 61 and 38% of PM in the accumulation mode and coarse mode, respectively. The water solublemore » fraction of organic matter was estimated to be 52 and 8% of PM in these modes. Sulfate, predominantly in the form of ammoniated sulfate, was the dominant inorganic component in both size modes: ~ 34% in the accumulation vs. ~ 47% in the coarse mode. The hygroscopic growth measurements were conducted with a filter-based differential hygroscopicity analyzer (FDHA) over the range of 5–99.4% RH in the hydration and dehydration operation modes. The FDHA study indicates that both accumulation and coarse modes exhibit pronounced water uptake approximately at the same RH, starting at ~ 70%, while efflorescence occurred at different humidities, i.e., at ~ 35% RH for submicron particles vs. ~ 50% RH for supermicron particles. This ~ 15% RH difference was attributed to higher content of organic material in the submicron particles, which suppresses water release in the dehydration experiments. The kappa mass interaction model (KIM) was applied to characterize and parameterize non-ideal solution behavior and concentration-dependent water uptake by atmospheric aerosol samples in the 5–99.4% RH range. Based on KIM, the volume-based hygroscopicity parameter, κ v, was calculated. The κ v, ws value related to the water soluble (ws) fraction was estimated to be ~ 0.15 for the

Chemical composition, microstructure, and hygroscopic properties of aerosol particles at the Zotino Tall Tower Observatory (ZOTTO), Siberia, during a summer campaign

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

Mikhailov, E. F.; Mironov, G. N.; Pöhlker, C.

In this study we describe the hygroscopic properties of accumulation- and coarse-mode aerosol particles sampled at the Zotino Tall Tower Observatory (ZOTTO) in Central Siberia (61° N; 89° E) from 16 to 21 June 2013. The hygroscopic growth measurements were supplemented with chemical analyses of the samples, including inorganic ions and organic/elemental carbon. In addition, the microstructure and chemical composition of aerosol particles were analyzed by X-ray micro-spectroscopy (STXM-NEXAFS) and transmission electron microscopy (TEM). A mass closure analysis indicates that organic carbon accounted for 61 and 38% of PM in the accumulation mode and coarse mode, respectively. The water solublemore » fraction of organic matter was estimated to be 52 and 8% of PM in these modes. Sulfate, predominantly in the form of ammoniated sulfate, was the dominant inorganic component in both size modes: ~ 34% in the accumulation vs. ~ 47% in the coarse mode. The hygroscopic growth measurements were conducted with a filter-based differential hygroscopicity analyzer (FDHA) over the range of 5–99.4% RH in the hydration and dehydration operation modes. The FDHA study indicates that both accumulation and coarse modes exhibit pronounced water uptake approximately at the same RH, starting at ~ 70%, while efflorescence occurred at different humidities, i.e., at ~ 35% RH for submicron particles vs. ~ 50% RH for supermicron particles. This ~ 15% RH difference was attributed to higher content of organic material in the submicron particles, which suppresses water release in the dehydration experiments. The kappa mass interaction model (KIM) was applied to characterize and parameterize non-ideal solution behavior and concentration-dependent water uptake by atmospheric aerosol samples in the 5–99.4% RH range. Based on KIM, the volume-based hygroscopicity parameter, κ v, was calculated. The κ v, ws value related to the water soluble (ws) fraction was estimated to be ~ 0.15 for the

Chemical composition, microstructure, and hygroscopic properties of aerosol particles at the Zotino Tall Tower Observatory (ZOTTO), Siberia, during a summer campaign

NASA Astrophysics Data System (ADS)

Mikhailov, E. F.; Mironov, G. N.; Pöhlker, C.; Chi, X.; Krüger, M. L.; Shiraiwa, M.; Förster, J.-D.; Pöschl, U.; Vlasenko, S. S.; Ryshkevich, T. I.; Weigand, M.; Kilcoyne, A. L. D.; Andreae, M. O.

2015-03-01

In this study we describe the hygroscopic properties of accumulation- and coarse-mode aerosol particles sampled at the Zotino Tall Tower Observatory (ZOTTO) in Central Siberia (61° N; 89° E) from 16 to 21 June 2013. The hygroscopic growth measurements were supplemented with chemical analyses of the samples, including inorganic ions and organic/elemental carbon. In addition, the microstructure and chemical composition of aerosol particles were analyzed by X-ray micro-spectroscopy (STXM-NEXAFS) and transmission electron microscopy (TEM). A mass closure analysis indicates that organic carbon accounted for 61 and 38% of PM in the accumulation mode and coarse mode, respectively. The water soluble fraction of organic matter was estimated to be 52 and 8% of PM in these modes. Sulfate, predominantly in the form of ammoniated sulfate, was the dominant inorganic component in both size modes: ∼34% in the accumulation vs. ∼47% in the coarse mode. The hygroscopic growth measurements were conducted with a filter-based differential hygroscopicity analyzer (FDHA) over the range of 5-99.4% RH in the hydration and dehydration operation modes. The FDHA study indicates that both accumulation and coarse modes exhibit pronounced water uptake approximately at the same RH, starting at ∼70%, while efflorescence occurred at different humidities, i.e., at ∼35% RH for submicron particles vs. ∼50% RH for supermicron particles. This ∼15% RH difference was attributed to higher content of organic material in the submicron particles, which suppresses water release in the dehydration experiments. The kappa mass interaction model (KIM) was applied to characterize and parameterize non-ideal solution behavior and concentration-dependent water uptake by atmospheric aerosol samples in the 5-99.4% RH range. Based on KIM, the volume-based hygroscopicity parameter, κv, was calculated. The κv, ws value related to the water soluble (ws) fraction was estimated to be ∼0.15 for

Chemical composition, microstructure, and hygroscopic properties of aerosol particles at the Zotino Tall Tower Observatory (ZOTTO), Siberia, during a summer campaign

NASA Astrophysics Data System (ADS)

Mikhailov, E. F.; Mironov, G. N.; Pöhlker, C.; Chi, X.; Krüger, M. L.; Shiraiwa, M.; Förster, J.-D.; Pöschl, U.; Vlasenko, S. S.; Ryshkevich, T. I.; Weigand, M.; Kilcoyne, A. L. D.; Andreae, M. O.

2015-08-01

In this study we describe the hygroscopic properties of accumulation- and coarse-mode aerosol particles sampled at the Zotino Tall Tower Observatory (ZOTTO) in central Siberia (61° N, 89° E) from 16 to 21 June 2013. The hygroscopic growth measurements were supplemented with chemical analyses of the samples, including inorganic ions and organic/elemental carbon. In addition, the microstructure and chemical compositions of aerosol particles were analyzed by x-ray micro-spectroscopy (STXM-NEXAFS) and transmission electron microscopy (TEM). A mass closure analysis indicates that organic carbon accounted for 61 and 38 % of particulate matter (PM) in the accumulation mode and coarse mode, respectively. The water-soluble fraction of organic matter was estimated to be 52 and 8 % of PM in these modes. Sulfate, predominantly in the form of ammoniated sulfate, was the dominant inorganic component in both size modes: ~ 34 % in the accumulation mode vs. ~ 47 % in the coarse mode. The hygroscopic growth measurements were conducted with a filter-based differential hygroscopicity analyzer (FDHA) over the range of 5-99.4 % RH in the hydration and dehydration operation modes. The FDHA study indicates that both accumulation and coarse modes exhibit pronounced water uptake approximately at the same relative humidity (RH), starting at ~ 70 %, while efflorescence occurred at different humidities, i.e., at ~ 35 % RH for submicron particles vs. ~ 50 % RH for supermicron particles. This ~ 15 % RH difference was attributed to higher content of organic material in the submicron particles, which suppresses water release in the dehydration experiments. The kappa mass interaction model (KIM) was applied to characterize and parameterize non-ideal solution behavior and concentration-dependent water uptake by atmospheric aerosol samples in the 5-99.4 % RH range. Based on KIM, the volume-based hygroscopicity parameter, κv, was calculated. The κv,ws value related to the water-soluble (ws

Vertical distribution of aerosol optical properties based on aircraft measurements over the Loess Plateau in China.

PubMed

Li, Junxia; Liu, Xingang; Yuan, Liang; Yin, Yan; Li, Zhanqing; Li, Peiren; Ren, Gang; Jin, Lijun; Li, Runjun; Dong, Zipeng; Li, Yiyu; Yang, Junmei

2015-08-01

Vertical distributions of aerosol optical properties based on aircraft measurements over the Loess Plateau were measured for the first time during a summertime aircraft campaign, 2013 in Shanxi, China. Data from four flights were analyzed. The vertical distributions of aerosol optical properties including aerosol scattering coefficients (σsc), absorption coefficients (σab), Angström exponent (α), single scattering albedo (ω), backscattering ratio (βsc), aerosol mass scattering proficiency (Qsc) and aerosol surface scattering proficiency (Qsc(')) were obtained. The mean statistical values of σsc were 77.45 Mm(-1) (at 450 nm), 50.72 Mm(-1) (at 550n m), and 32.02 Mm(-1) (at 700 nm). The mean value of σab was 7.62 Mm(-1) (at 550 nm). The mean values of α, βsc and ω were 1.93, 0.15, and 0.91, respectively. Aerosol concentration decreased with altitude. Most effective diameters (ED) of aerosols were less than 0.8 μm. The vertical profiles of σsc,, α, βsc, Qsc and Qsc(') showed that the aerosol scattering properties at lower levels contributed the most to the total aerosol radiative forcing. Both α and βsc had relatively large values, suggesting that most aerosols in the observational region were small particles. The mean values of σsc, α, βsc, Qsc, Qsc('), σab and ω at different height ranges showed that most of the parameters decreased with altitude. The forty-eight hour backward trajectories of air masses during the observation days indicated that the majority of aerosols in the lower level contributed the most to the total aerosol loading, and most of these particles originated from local or regional pollution emissions. Copyright © 2015. Published by Elsevier B.V.

An instrument for the simultaneous acquisition of size, shape, and spectral fluorescence data from single aerosol particles

NASA Astrophysics Data System (ADS)

Hirst, Edwin; Kaye, Paul H.; Foot, Virginia E.; Clark, James M.; Withers, Philip B.

2004-12-01

We describe the construction of a bio-aerosol monitor designed to capture and record intrinsic fluorescence spectra from individual aerosol particles carried in a sample airflow and to simultaneously capture data relating to the spatial distribution of elastically scattered light from each particle. The spectral fluorescence data recorded by this PFAS (Particle Fluorescence and Shape) monitor contains information relating to the particle material content and specifically to possible biological fluorophores. The spatial scattering data from PFAS yields information relating to particle size and shape. The combination of these data can provide a means of aiding the discrimination of bio-aerosols from background or interferent aerosol particles which may have similar fluorescence properties but exhibit shapes and/or sizes not normally associated with biological particles. The radiation used both to excite particle fluorescence and generate the necessary spatially scattered light flux is provided by a novel compact UV fiber laser operating at 266nm wavelength. Particles drawn from the ambient environment traverse the laser beam in single file. Intrinsic particle fluorescence in the range 300-570nm is collected via an ellipsoidal concentrator into a concave grating spectrometer, the spectral data being recorded using a 16-anode linear array photomultiplier detector. Simultaneously, the spatial radiation pattern scattered by the particle over 5°-30° scattering angle and 360° of azimuth is recorded using a custom designed 31-pixel radial hybrid photodiode array. Data from up to ~5,000 particles per second may be acquired for analysis, usually performed by artificial neural network classification.

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.

Ground-based observation of aerosol optical properties in Lanzhou, China.

PubMed

Yu, Xingna; Zhu, Bin; Fan, Shuxian; Yin, Yan; Bu, Xiaoli

2009-01-01

Aerosol optical properties from August 2006 to July 2007 were obtained from ground-based and sky radiance measurements in Semi-Arid Climate and Environment Observatory of Lanzhou University (SACOL), China. High aerosol optical thickness (AOT) associated with low Angström exponent (alpha) was mainly observed in spring, which was consistent with the seasonal dust production from Hexi Corridor. The maximum monthly average value of AOT 0.56 occurred in March of 2007, which was two times larger than the minimum value of 0.28 in October of 2006. Approximately 60% of the AOT ranged between 0.3 and 0.5, and nearly 93% of alpha value varied from 0.1 to 0.8, which occurred in spring. The significant correlation between aerosol properties and water vapor content was not observed. The aerosol volume size distribution can be characterized by the bimodal logarithm normal structure: fine mode (r < 0.6 microm) and coarse mode (r > 0.6 microm). Aerosols in spring of SACOL were dominated by large particles with the volume concentration ratio of coarse to fine modes being 7.85. The average values of asymmetry factor (g) in the wavelength range 440-1020 nm were found to be 0.71, 0.67, 0.67 and 0.69 in spring, summer, autumn and winter, respectively.

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.

Estimating Marine Aerosol Particle Volume and Number from Maritime Aerosol Network Data

NASA Technical Reports Server (NTRS)

Sayer, A. M.; Smirnov, A.; Hsu, N. C.; Munchak, L. A.; Holben, B. N.

2012-01-01

As well as spectral aerosol optical depth (AOD), aerosol composition and concentration (number, volume, or mass) are of interest for a variety of applications. However, remote sensing of these quantities is more difficult than for AOD, as it is more sensitive to assumptions relating to aerosol composition. This study uses spectral AOD measured on Maritime Aerosol Network (MAN) cruises, with the additional constraint of a microphysical model for unpolluted maritime aerosol based on analysis of Aerosol Robotic Network (AERONET) inversions, to estimate these quantities over open ocean. When the MAN data are subset to those likely to be comprised of maritime aerosol, number and volume concentrations obtained are physically reasonable. Attempts to estimate surface concentration from columnar abundance, however, are shown to be limited by uncertainties in vertical distribution. Columnar AOD at 550 nm and aerosol number for unpolluted maritime cases are also compared with Moderate Resolution Imaging Spectroradiometer (MODIS) data, for both the present Collection 5.1 and forthcoming Collection 6. MODIS provides a best-fitting retrieval solution, as well as the average for several different solutions, with different aerosol microphysical models. The average solution MODIS dataset agrees more closely with MAN than the best solution dataset. Terra tends to retrieve lower aerosol number than MAN, and Aqua higher, linked with differences in the aerosol models commonly chosen. Collection 6 AOD is likely to agree more closely with MAN over open ocean than Collection 5.1. In situations where spectral AOD is measured accurately, and aerosol microphysical properties are reasonably well-constrained, estimates of aerosol number and volume using MAN or similar data would provide for a greater variety of potential comparisons with aerosol properties derived from satellite or chemistry transport model data.

Properties of transported African mineral dust aerosols in the Mediterranean region

NASA Astrophysics Data System (ADS)

Denjean, Cyrielle; Chevaillier, Servanne; Gaimoz, Cécile; Grand, Noel; Triquet, Sylvain; Zapf, Pascal; Loisil, Rodrigue; Bourrianne, Thierry; Freney, Evelyn; Dupuy, Regis; Sellegri, Karine; Schwarzenbock, Alfons; Torres, Benjamin; Mallet, Marc; Cassola, Federico; Prati, Paolo; Formenti, Paola

2015-04-01

The transport of mineral dust aerosols is a global phenomenon with strong climate implications. Depending on the travel distance over source regions, the atmospheric conditions and the residence time in the atmosphere, various transformation processes (size-selective sedimentation, mixing, condensation of gaseous species, and weathering) can modify the physical and chemical properties of mineral dust, which, in turn, can change the dust's optical properties. The model predictions of the radiative effect by mineral dust still suffer of the lack of certainty of these properties, and their temporal evolution with transport time. Within the frame of the ChArMex project (Chemistry-Aerosol Mediterranean experiment, http://charmex.lsce.ipsl.fr/), one intensive airborne campaign (ADRIMED, Aerosol Direct Radiative Impact in the regional climate in the MEDiterranean region, 06 June - 08 July 2013) has been performed over the Central and Western Mediterranean, one of the two major transport pathways of African mineral dust. In this study we have set up a systematic strategy to determine the optical, physical and optical properties of mineral dust to be compared to an equivalent dataset for dust close to source regions in Africa. This study is based on airborne observations onboard the SAFIRE ATR-42 aircraft, equipped with state of the art in situ instrumentation to measure the particle scattering and backscattering coefficients (nephelometer at 450, 550, and 700 nm), the absorption coefficient (PSAP at 467, 530, and 660 nm), the extinction coefficient (CAPS at 530 nm), the aerosol optical depth (PLASMA at 340 to 1640 nm), the size distribution in the extended range 40 nm - 30 µm by the combination of different particle counters (SMPS, USHAS, FSSP, GRIMM) and the chemical composition obtained by filter sampling. The chemistry and transport model CHIMERE-Dust have been used to classify the air masses according to the dust origin and transport. Case studies of dust transport

Baseline Maritime Aerosol: Methodology to Derive the Optical Thickness and Scattering Properties

NASA Technical Reports Server (NTRS)

Kaufman, Yoram J.; Smirnov, Alexander; Holben, Brent N.; Dubovik, Oleg; Einaudi, Franco (Technical Monitor)

2001-01-01

Satellite Measurements of the global distribution of aerosol and their effect on climate should be viewed in respect to a baseline aerosol. In this concept, concentration of fine mode aerosol particles is elevated above the baseline by man-made activities (smoke or urban pollution), while coarse mode by natural processes (e.g. dust or sea-spray). Using 1-3 years of measurements in 10 stations of the Aerosol Robotic network (ACRONET we develop a methodology and derive the optical thickness and properties of this baseline aerosol for the Pacific and Atlantic Oceans. Defined as the median for periods of stable optical thickness (standard deviation < 0.02) during 2-6 days, the median baseline aerosol optical thickness over the Pacific Ocean is 0.052 at 500 am with Angstrom exponent of 0.77, and 0.071 and 1.1 respectively, over the Atlantic Ocean.

Evolution of biomass burning aerosol over the Amazon: airborne measurements of aerosol chemical composition, microphysical properties, mixing state and optical properties during SAMBBA

NASA Astrophysics Data System (ADS)

Morgan, W.; Allan, J. D.; Flynn, M.; Darbyshire, E.; Hodgson, A.; Liu, D.; O'Shea, S.; Bauguitte, S.; Szpek, K.; Johnson, B.; Haywood, J.; Longo, K.; Artaxo, P.; Coe, H.

2013-12-01

Biomass burning represents one of the largest sources of particulate matter to the atmosphere, resulting in a significant perturbation to the Earth's radiative balance coupled with serious impacts on public health. On regional scales, the impacts are substantial, particularly in areas such as the Amazon Basin where large, intense and frequent burning occurs on an annual basis for several months. Absorption by atmospheric aerosols is underestimated by models over South America, which points to significant uncertainties relating to Black Carbon (BC) aerosol properties. Initial results from the South American Biomass Burning Analysis (SAMBBA) field experiment, which took place during September and October 2012 over Brazil on-board the UK Facility for Airborne Atmospheric Measurement (FAAM) BAe-146 research aircraft, are presented here. Aerosol chemical composition was measured by an Aerodyne Aerosol Mass Spectrometer (AMS) and a DMT Single Particle Soot Photometer (SP2). The physical, chemical and optical properties of the aerosols across the region will be characterized in order to establish the impact of biomass burning on regional air quality, weather and climate. The aircraft sampled a range of conditions including sampling of pristine Rainforest, fresh biomass burning plumes, regional haze and elevated biomass burning layers within the free troposphere. The aircraft sampled biomass burning aerosol across the southern Amazon in the states of Rondonia and Mato Grosso, as well as in a Cerrado (Savannah-like) region in Tocantins state. This presented a range of fire conditions, in terms of their number, intensity, vegetation-type and their combustion efficiencies. Near-source sampling of fires in Rainforest environments suggested that smouldering combustion dominated, while flaming combustion dominated in the Cerrado. This led to significant differences in aerosol chemical composition, particularly in terms of the BC content, with BC being enhanced in the Cerrado

Dynamic viscosity mapping of the oxidation of squalene aerosol particles.

PubMed

Athanasiadis, Athanasios; Fitzgerald, Clare; Davidson, Nicholas M; Giorio, Chiara; Botchway, Stanley W; Ward, Andrew D; Kalberer, Markus; Pope, Francis D; Kuimova, Marina K

2016-11-09

Organic aerosols (OAs) play important roles in multiple atmospheric processes, including climate change, and can impact human health. The physico-chemical properties of OAs are important for all these processes and can evolve through reactions with various atmospheric components, including oxidants. The dynamic nature of these reactions makes it challenging to obtain a true representation of their composition and surface chemistry. Here we investigate the microscopic viscosity of the model OA composed of squalene, undergoing chemical aging. We employ Fluorescent Lifetime Imaging Microscopy (FLIM) in conjunction with viscosity sensitive probes termed molecular rotors, in order to image the changes in microviscosity in real time during oxidation with ozone and hydroxyl radicals, which are two key oxidising species in the troposphere. We also recorded the Raman spectra of the levitated particles to follow the reactivity during particle ozonolysis. The levitation of droplets was achieved via optical trapping that enabled simultaneous levitation and measurement via FLIM or Raman spectroscopy and allowed the true aerosol phase to be probed. Our data revealed a very significant increase in viscosity of the levitated squalene droplets upon ozonolysis, following their transformation from the liquid to solid phase that was not observable when the oxidation was carried out on coverslip mounted droplets. FLIM imaging with sub-micron spatial resolution also revealed spatial heterogeneity in the viscosity distribution of oxidised droplets. Overall, a combination of molecular rotors, FLIM and optical trapping is able to provide powerful insights into OA chemistry and the microscopic structure that enables the dynamic monitoring of microscopic viscosity in aerosol particles in their true phase.

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.

A thermal desorption mass spectrometer for freshly nucleated secondary aerosol particles

NASA Astrophysics Data System (ADS)

Held, A.; Gonser, S. G.

2012-04-01

Secondary aerosol formation in the atmosphere is observed in a large variety of locations worldwide, introducing new particles to the atmosphere which can grow to sizes relevant for health and climate effects of aerosols. The chemical reactions leading to atmospheric secondary aerosol formation are not yet fully understood. At the same time, analyzing the chemical composition of freshly nucleated particles is still a challenging task. We are currently finishing the development of a field portable aerosol mass spectrometer for nucleation particles with diameters smaller than 30 nm. This instrument consists of a custom-built aerosol sizing and collection unit coupled to a time-of-flight mass spectrometer (TOF-MS). The aerosol sizing and collection unit is composed of three major parts: (1) a unipolar corona aerosol charger, (2) a radial differential mobility analyzer (rDMA) for aerosol size separation, and (3) an electrostatic precipitator for aerosol collection. After collection, the aerosol sample is thermally desorbed, and the resulting gas sample is transferred to the TOF-MS for chemical analysis. The unipolar charger is based on corona discharge from carbon fibres (e.g. Han et al., 2008). This design allows efficient charging at voltages below 2 kV, thus eliminating the potential for ozone production which would interfere with the collected aerosol. With the current configuration the extrinsic charging efficiency for 20 nm particles is 32 %. The compact radial DMA similar to the design of Zhang et al. (1995) is optimized for a diameter range from 1 nm to 100 nm. Preliminary tests show that monodisperse aerosol samples (geometric standard deviation of 1.09) at 10 nm, 20 nm, and 30 nm can easily be separated from the ambient polydisperse aerosol population. Finally, the size-segregated aerosol sample is collected on a high-voltage biased metal filament. The collected sample is protected from contamination using a He sheath counterflow. Resistive heating of the

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.

Aerosol-halogen interaction: Change of physico-chemical properties of SOA by naturally released halogen species

NASA Astrophysics Data System (ADS)

Ofner, J.; Balzer, N.; Buxmann, J.; Grothe, H.; Krüger, H.; Platt, U.; Schmitt-Kopplin, P.; Zetzsch, C.

2011-12-01

Reactive halogen species are released by various sources like photo-activated sea-salt aerosol or salt pans and salt lakes. These heterogeneous release mechanisms have been overlooked so far, although their potential of interaction with organic aerosols like Secondary Organic Aerosol (SOA), Biomass Burning Organic Aerosol (BBOA) or Atmospheric Humic LIke Substances (HULIS) is completely unknown. Such reactions can constitute sources of gaseous organo-halogen compounds or halogenated organic particles in the atmospheric boundary layer. To study the interaction of organic aerosols with reactive halogen species (RHS), SOA was produced from α-pinene, catechol and guaiacol using an aerosol smog-chamber. The model SOAs were characterized in detail using a variety of physico-chemical methods (Ofner et al., 2011). Those aerosols were exposed to molecular halogens in the presence of UV/VIS irradiation and to halogens, released from simulated natural halogen sources like salt pans, in order to study the complex aerosol-halogen interaction. The heterogeneous reaction of RHS with those model aerosols leads to different gaseous species like CO2, CO and small reactive/toxic molecules like phosgene (COCl2). Hydrogen containing groups on the aerosol particles are destroyed to form HCl or HBr, and a significant formation of C-Br bonds could be verified in the particle phase. Carbonyl containing functional groups of the aerosol are strongly affected by the halogenation process. While changes of functional groups and gaseous species were visible using FTIR spectroscopy, optical properties were studied using Diffuse Reflectance UV/VIS spectroscopy. Overall, the optical properties of the processed organic aerosols are significantly changed. While chlorine causes a "bleaching" of the aerosol particles, bromine shifts the maximum of UV/VIS absorption to the red end of the UV/VIS spectrum. Further physico-chemical changes were recognized according to the aerosol size-distributions or the

Apparatus having reduced background for measuring radiation activity in aerosol particles

DOEpatents

Rodgers, John C.; McFarland, Andrew R.; Oritz, Carlos A.; Marlow, William H.

1992-01-01

Apparatus having reduced background for measuring radiation activity in aerosol particles. A continuous air monitoring sampler is described for use in detecting the presence of alpha-emitting aerosol particles. An inlet fractionating screen has been demonstrated to remove about 95% of freshly formed radon progeny from the aerosol sample, and approximately 33% of partially aged progeny. Addition of an electrical condenser and a modified dichotomous virtual impactor are expected to produce considerable improvement in these numbers, the goal being to enrich the transuranic (TRU) fraction of the aerosols. This offers the possibility of improving the signal-to-noise ratio for the detected alpha-particle energy spectrum in the region of interest for detecting TRU materials associated with aerosols, thereby enhancing the performance of background-compensation algorithms for improving the quality of alarm signals intended to warn personnel of potentially harmful quantities of TRU materials in the ambient air.

Ice Nucleation Activity of Various Agricultural Soil Dust Aerosol Particles

NASA Astrophysics Data System (ADS)

Schiebel, Thea; Höhler, Kristina; Funk, Roger; Hill, Thomas C. J.; Levin, Ezra J. T.; Nadolny, Jens; Steinke, Isabelle; Suski, Kaitlyn J.; Ullrich, Romy; Wagner, Robert; Weber, Ines; DeMott, Paul J.; Möhler, Ottmar

2016-04-01

Recent investigations at the cloud simulation chamber AIDA (Aerosol Interactions and Dynamics in the Atmosphere) suggest that agricultural soil dust has an ice nucleation ability that is enhanced up to a factor of 10 compared to desert dust, especially at temperatures above -26 °C (Steinke et al., in preparation for submission). This enhancement might be caused by the contribution of very ice-active biological particles. In addition, soil dust aerosol particles often contain a considerably higher amount of organic matter compared to desert dust particles. To test agricultural soil dust as a source of ice nucleating particles, especially for ice formation in warm clouds, we conducted a series of laboratory measurements with different soil dust samples to extend the existing AIDA dataset. The AIDA has a volume of 84 m3 and operates under atmospherically relevant conditions over wide ranges of temperature, pressure and humidity. By controlled adiabatic expansions, the ascent of an air parcel in the troposphere can be simulated. As a supplement to the AIDA facility, we use the INKA (Ice Nucleation Instrument of the KArlsruhe Institute of Technology) continuous flow diffusion chamber based on the design by Rogers (1988) to expose the sampled aerosol particles to a continuously increasing saturation ratio by keeping the aerosol temperature constant. For our experiments, soil dust was dry dispersed into the AIDA vessel. First, fast saturation ratio scans at different temperatures were performed with INKA, sampling soil dust aerosol particles directly from the AIDA vessel. Then, we conducted the AIDA expansion experiment starting at a preset temperature. The combination of these two different methods provides a robust data set on the temperature-dependent ice activity of various agriculture soil dust aerosol particles with a special focus on relatively high temperatures. In addition, to extend the data set, we investigated the role of biological and organic matter in more

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

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

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

Composition of individual aerosol particles above the Israelian Mediterranean coast during the summer time

NASA Astrophysics Data System (ADS)

Ganor, E.; Levin, Z.; Van Grieken, R.

Aerosol particles were collected aboard a ship in Haifa Bay and Tel Aviv, Israel, during the summer time. The aerosol particles (6170) were analyzed as individual particles and classified according to their chemical composition, size, number concentration per cubic centimeter and morphology. Most of the aerosol particles could be classified into four groups. The first contains gypsum from the sea and from industrial sources brought in by land breezes. A second group is characterized by continental aluminosilicate and quartz. A third group consists of sea salt mixed with sulfate particles. The fourth group is characterized by an abundance of sulfate particles, some of which are ammonium sulfate brought by the land breezes. The particles were identified as marine and mineral aerosols which originated in Eastern Europe and the Mediterranean sea, while local aerosols brought by land breeze characterized by phosphate, fly ash and soil particles originated in the Haifa industrial zone. In addition, the aerosols were analyzed for sulfates and nitrates. Aerosols of sea and land breezes differed as follows: (1) Sulfate and nitrate concentrations in the aerosols were 5-10 times higher during land breeze than during sea breeze, and the total content of suspended particles was, respectively, 6-12 times higher. (2) Particle size spectra during land breeze were broader than during sea breeze and their concentrations were about 20 times greater. Analyses of individual particles by electron microscopy revealed that during the sea breeze the aerosols contained calcium sulfate, sodium sulfate and sulfuric acid. The sulfuric acid, of pH 2.5, is due to the long-range transport as previously reported ( Ganor et al., 1993) while the other sulfates are from the sea. This explains the high concentration of sulfates in the atmospheric sea breeze above the Israelian Mediterranean coast during the summertime.

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

Hygroscopic and Chemical Properties of Aerosols collected near a Copper Smelter: Implications for Public and Environmental Health

PubMed Central

Sorooshian, Armin; Csavina, Janae; Shingler, Taylor; Dey, Stephen; Brechtel, Fred J.; Sáez, A. Eduardo; Betterton, Eric A.

2012-01-01

Particulate matter emissions near active copper smelters and mine tailings in the southwestern United States pose a potential threat to nearby environments owing to toxic species that can be inhaled and deposited in various regions of the body depending on the composition and size of the particles, which are linked by particle hygroscopic properties. This study reports the first simultaneous measurements of size-resolved chemical and hygroscopic properties of particles next to an active copper smelter and mine tailings by the towns of Hayden and Winkelman in southern Arizona. Size-resolved particulate matter samples collected near an active copper smelter were examined with inductively coupled plasma mass spectrometry, ion chromatography, and a humidified tandem differential mobility analyzer. Aerosol particles collected at the measurement site are enriched in metals and metalloids (e.g. arsenic, lead, and cadmium) and water-uptake measurements of aqueous extracts of collected samples indicate that the particle diameter range of particles most enriched with these species (0.18–0.55 µm) overlaps with the most hygroscopic mode at a relative humidity of 90% (0.10–0.32 µm). These measurements have implications for public health, microphysical effects of aerosols, and regional impacts owing to the transport and deposition of contaminated aerosol particles. PMID:22852879

Characterization of Individual Aerosol Particles Associated with Clouds (CRYSTAL-FACE)

NASA Technical Reports Server (NTRS)

Buseck, Peter R.

2004-01-01

The aim of our research was to obtain data on the chemical and physical properties of individual aerosol particles from near the bottoms and tops of the deep convective systems that lead to the generation of tropical cirrus clouds and to provide insights into the particles that serve as CCN or IN. We used analytical transmission electron microscopy (ATEM), including energy-dispersive X-ray spectrometry (EDS) and electron energy-loss spectroscopy (EELS), and field-emission electron microscopy (FESEM) to compare the compositions, concentrations, size distributions, shapes, surface coatings, and degrees of aggregation of individual particles from cloud bases and the anvils near the tropopause. Aggregates of sea salt and mineral dust, ammonium sulfate, and soot particles are abundant in in-cloud samples. Cirrus samples contain many H2SO4 droplets, but acidic sulfate particles are rare at the cloud bases. H2SO4 probably formed at higher altitudes through oxidation of SO2 in cloud droplets. The relatively high extent of ammoniation in the upper troposphere in-cloud samples appears to have resulted from vertical transport by strong convection. The morphology of H2SO4 droplets indicates that they had been at least yartiy ammoniated at the time of collection. They are internally mixed with organic materials, metal sulfates, and solid particles of various compositions. Ammoniation and internal mixing of result in freezing at higher temperature than in pure H2SO4 aerosols. K- and S-bearing organic particles and Si-Al-rich particles are common throughout. Sea salt and mineral dust were incorporated into the convective systems from the cloud bases and worked as ice nuclei while being vertically transported. The nonsulfate particles originated from the lower troposphere and were transported to the upper troposphere and lower stratosphere.

Virtual Impactor for Sub-micron Aerosol Particles

NASA Astrophysics Data System (ADS)

Bolshakov, A. A.; Strawa, A. W.; Hallar, A. G.

2005-12-01

The objective of a virtual impactor is to separate out the larger particles in a flow from the smaller particles in such a way that both sizes of particles are available for sampling. A jet of particle-laden air is accelerated toward a collection probe so that a small gap exists between the acceleration nozzle and the probe. A vacuum is applied to deflect a major portion of the airstream away form the collection probe. Particles larger than a certain size have sufficient momentum so that they cross the deflected streamlines and enter the collection probe, whereas smaller particles follow the deflected streamlines. The result is that the collection probe will contain a higher concentration of larger particles than is in the initial airstream. Typically, virtual impactors are high-flow devices used to separate out particles greater than several microns in diameter. We have developed a special virtual impactor to concentrate aerosol particles of diameters between 0.5 to 1 micron for the purpose of calibrating the optical cavity ring-down instrument [1]. No similar virtual impactors are commercially available. In our design, we have exploited considerations described earlier [2-4]. Performance of our virtual impactor was evaluated in an experimental set-up using TSI 3076 nebulizer and TSI 3936 scanning mobility particle size spectrometer. Under experimental conditions optimized for the best performance of the virtual impactor, we were able to concentrate the 700-nm polystyrene particles no less than 15-fold. However, under experimental conditions optimized for calibrating our cavity ring-down instrument, a concentration factor attainable was from 4 to 5. During calibration experiments, maximum realized particle number densities were 190, 300 and 1600 cm-3 for the 900-nm, 700-nm and 500-nm spheres, respectively. This paper discusses the design of the impactor and laboratory studies verifying its performance. References: 1. A.W. Strawa, R. Castaneda, T. Owano, D.S. Baer

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

Optimal estimation retrieval of aerosol microphysical properties from SAGE~II satellite observations in the volcanically unperturbed lower stratosphere

NASA Astrophysics Data System (ADS)

Wurl, D.; Grainger, R. G.; McDonald, A. J.; Deshler, T.

2010-05-01

Stratospheric aerosol particles under non-volcanic conditions are typically smaller than 0.1 μm. Due to fundamental limitations of the scattering theory in the Rayleigh limit, these tiny particles are hard to measure by satellite instruments. As a consequence, current estimates of global aerosol properties retrieved from spectral aerosol extinction measurements tend to be strongly biased. Aerosol surface area densities, for instance, are observed to be about 40% smaller than those derived from correlative in situ measurements (Deshler et al., 2003). An accurate knowledge of the global distribution of aerosol properties is, however, essential to better understand and quantify the role they play in atmospheric chemistry, dynamics, radiation and climate. To address this need a new retrieval algorithm was developed, which employs a nonlinear Optimal Estimation (OE) method to iteratively solve for the monomodal size distribution parameters which are statistically most consistent with both the satellite-measured multi-wavelength aerosol extinction data and a priori information. By thus combining spectral extinction measurements (at visible to near infrared wavelengths) with prior knowledge of aerosol properties at background level, even the smallest particles are taken into account which are practically invisible to optical remote sensing instruments. The performance of the OE retrieval algorithm was assessed based on synthetic spectral extinction data generated from both monomodal and small-mode-dominant bimodal sulphuric acid aerosol size distributions. For monomodal background aerosol, the new algorithm was shown to fairly accurately retrieve the particle sizes and associated integrated properties (surface area and volume densities), even in the presence of large extinction uncertainty. The associated retrieved uncertainties are a good estimate of the true errors. In the case of bimodal background aerosol, where the retrieved (monomodal) size distributions naturally

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.

Deposition flux of aerosol particles and 15 polycyclic aromatic hydrocarbons in the North China Plain.

PubMed

Wang, Xilong; Liu, Shuzhen; Zhao, Jingyu; Zuo, Qian; Liu, Wenxin; Li, Bengang; Tao, Shu

2014-04-01

The present study examined deposition fluxes of aerosol particles and 15 polycyclic aromatic hydrocarbons (PAHs) associated with the particles in the North China Plain. The annual mean deposition fluxes of aerosol particles and 15 PAHs were 0.69 ± 0.46 g/(m(2) ×d) and 8.5 ± 6.2 μg/(m(2) ×d), respectively. Phenanthrene, fluoranthene, pyrene, chrysene, benzo[b]fluoranthene, and benzo[k]fluoranthene were the dominant PAHs bound to deposited aerosol particles throughout the year. The total concentration of 15 PAHs in the deposited aerosol particles was the highest in winter but lowest in spring. The highest PAH concentration in the deposited aerosol particles in winter was because the heating processes highly increased the concentration in atmospheric aerosol particles. Low temperature and weak sunshine in winter reduced the degradation rate of deposited aerosol particle-bound PAHs, especially for those with low molecular weight. The lowest PAH concentration in deposited aerosol particles in spring resulted from the frequently occurring dust storms, which diluted PAH concentrations. The mean deposition flux of PAHs with aerosol particles in winter (16 μg/[m(2) ×d]) reached 3 times to 5 times that in other seasons (3.5-5.0 μg/[m(2) ×d]). The spatial variation of the deposition flux of PAHs with high molecular weight (e.g., benzo[a]pyrene) was consistent with their concentrations in the atmospheric aerosol particles, whereas such a phenomenon was not observed for those with low molecular weight (e.g., phenanthrene) because of their distinct hydrophobicity, Henry's law constant, and the spatially heterogeneous meteorological conditions. © 2013 SETAC.

Intercomparison and closure calculations using measurements of aerosol species and optical properties during the Yosemite Aerosol Characterization Study

NASA Astrophysics Data System (ADS)

Malm, William C.; Day, Derek E.; Carrico, Christian; Kreidenweis, Sonia M.; Collett, Jeffrey L.; McMeeking, Gavin; Lee, Taehyoung; Carrillo, Jacqueline; Schichtel, Bret

2005-07-01

Physical and optical properties of inorganic aerosols have been extensively studied, but less is known about carbonaceous aerosols, especially as they relate to the non-urban settings such as our nation's national parks and wilderness areas. Therefore an aerosol characterization study was conceived and implemented at one national park that is highly impacted by carbonaceous aerosols, Yosemite. The primary objective of the study was to characterize the physical, chemical, and optical properties of a carbon-dominated aerosol, including the ratio of total organic matter weight to organic carbon, organic mass scattering efficiencies, and the hygroscopic characteristics of a carbon-laden ambient aerosol, while a secondary objective was to evaluate a variety of semi-continuous monitoring systems. Inorganic ions were characterized using 24-hour samples that were collected using the URG and Interagency Monitoring of Protected Visual Environments (IMPROVE) monitoring systems, the micro-orifice uniform deposit impactor (MOUDI) cascade impactor, as well as the semi-continuous particle-into-liquid sampler (PILS) technology. Likewise, carbonaceous material was collected over 24-hour periods using IMPROVE technology along with the thermal optical reflectance (TOR) analysis, while semi-continuous total carbon concentrations were measured using the Rupprecht and Patashnick (R&P) instrument. Dry aerosol number size distributions were measured using a differential mobility analyzer (DMA) and optical particle counter, scattering coefficients at near-ambient conditions were measured with nephelometers fitted with PM10 and PM2.5 inlets, and "dry" PM2.5 scattering was measured after passing ambient air through Perma Pure Nafion® dryers. In general, the 24-hour "bulk" measurements of various aerosol species compared more favorably with each other than with the semi-continuous data. Semi-continuous sulfate measurements correlated well with the 24-hour measurements, but were biased low by

Soot Aerosol Particles as Cloud Condensation Nuclei: from Ice Nucleation Activity to Ice Crystal Morphology

NASA Astrophysics Data System (ADS)

Pirim, Claire; Ikhenazene, Raouf; Ortega, Isamel Kenneth; Carpentier, Yvain; Focsa, Cristian; Chazallon, Bertrand; Ouf, François-Xavier

2016-04-01

Emissions of solid-state particles (soot) from engine exhausts due to incomplete fuel combustion is considered to influence ice and liquid water cloud droplet activation [1]. The activity of these aerosols would originate from their ability to be important centers of ice-particle nucleation, as they would promote ice formation above water homogeneous freezing point. Soot particles are reported to be generally worse ice nuclei than mineral dust because they activate nucleation at higher ice-supersaturations for deposition nucleation and at lower temperatures for immersion freezing than ratios usually expected for homogeneous nucleation [2]. In fact, there are still numerous opened questions as to whether and how soot's physico-chemical properties (structure, morphology and chemical composition) can influence their nucleation ability. Therefore, systematic investigations of soot aerosol nucleation activity via one specific nucleation mode, here deposition nucleation, combined with thorough structural and compositional analyzes are needed in order to establish any association between the particles' activity and their physico-chemical properties. In addition, since the morphology of the ice crystals can influence their radiative properties [3], we investigated their morphology as they grow over both soot and pristine substrates at different temperatures and humidity ratios. In the present work, Combustion Aerosol STandart soot samples were produced from propane using various experimental conditions. Their nucleation activity was studied in deposition mode (from water vapor), and monitored using a temperature-controlled reactor in which the sample's relative humidity is precisely measured with a cryo-hygrometer. Formation of water/ice onto the particles is followed both optically and spectroscopically, using a microscope coupled to a Raman spectrometer. Vibrational signatures of hydroxyls (O-H) emerge when the particle becomes hydrated and are used to characterize ice

Influence of biomass burning on mixing state of sub-micron aerosol particles in the North China Plain

NASA Astrophysics Data System (ADS)

Kecorius, Simonas; Ma, Nan; Teich, Monique; van Pinxteren, Dominik; Zhang, Shenglan; Gröβ, Johannes; Spindler, Gerald; Müller, Konrad; Iinuma, Yoshiteru; Hu, Min; Herrmann, Hartmut; Wiedensohler, Alfred

2017-09-01

Particulate emissions from crop residue burning decrease the air quality as well as influence aerosol radiative properties on a regional scale. The North China Plain (NCP) is known for the large scale biomass burning (BB) of field residues, which often results in heavy haze pollution episodes across the region. We have been able to capture a unique BB episode during the international CAREBeijing-NCP intensive field campaign in Wangdu in the NCP (38.6°N, 115.2°E) from June to July 2014. It was found that aerosol particles originating from this BB event showed a significantly different mixing state compared with clean and non-BB pollution episodes. BB originated particles showed a narrower probability density function (PDF) of shrink factor (SF). And the maximum was found at shrink factor of 0.6, which is higher than in other episodes. The non-volatile particle number fraction during the BB episode decreased to 3% and was the lowest measured value compared to all other predefined episodes. To evaluate the influence of particle mixing state on aerosol single scattering albedo (SSA), SSA at different RHs was simulated using the measured aerosol physical-chemical properties. The differences between the calculated SSA for biomass burning, clean and pollution episodes are significant, meaning that the variation of SSA in different pollution conditions needs to be considered in the evaluation of aerosol direct radiative effects in the NCP. And the calculated SSA was found to be quite sensitive on the mixing state of BC, especially at low-RH condition. The simulated SSA was also compared with the measured values. For all the three predefined episodes, the measured SSA are very close to the calculated ones with assumed mixing states of homogeneously internal and core-shell internal mixing, indicating that both of the conception models are appropriate for the calculation of ambient SSA in the NCP.

A Micro Aerosol Sensor for the Measurement of Airborne Ultrafine Particles.

PubMed

Zhang, Chao; Zhu, Rong; Yang, Wenming

2016-03-18

Particle number concentration and particle size are the two key parameters used to characterize exposure to airborne nanoparticles or ultrafine particles that have attracted the most attention. This paper proposes a simple micro aerosol sensor for detecting the number concentration and particle size of ultrafine particles with diameters from 50 to 253 nm based on electrical diffusion charging. The sensor is composed of a micro channel and a couple of planar electrodes printed on two circuit boards assembled in parallel, which thus integrate charging, precipitating and measurement elements into one chip, the overall size of which is 98 × 38 × 25 mm³. The experiment results demonstrate that the sensor is useful for measuring monodisperse aerosol particles with number concentrations from 300 to 2.5 × 10⁴ /cm³ and particle sizes from 50 to 253 nm. The aerosol sensor has a simple structure and small size, which is favorable for use in handheld devices.

A Micro Aerosol Sensor for the Measurement of Airborne Ultrafine Particles

PubMed Central

Zhang, Chao; Zhu, Rong; Yang, Wenming

2016-01-01

Particle number concentration and particle size are the two key parameters used to characterize exposure to airborne nanoparticles or ultrafine particles that have attracted the most attention. This paper proposes a simple micro aerosol sensor for detecting the number concentration and particle size of ultrafine particles with diameters from 50 to 253 nm based on electrical diffusion charging. The sensor is composed of a micro channel and a couple of planar electrodes printed on two circuit boards assembled in parallel, which thus integrate charging, precipitating and measurement elements into one chip, the overall size of which is 98 × 38 × 25 mm3. The experiment results demonstrate that the sensor is useful for measuring monodisperse aerosol particles with number concentrations from 300 to 2.5 × 104 /cm3 and particle sizes from 50 to 253 nm. The aerosol sensor has a simple structure and small size, which is favorable for use in handheld devices. PMID:26999156

Sensitivity metric approach for retrieval of aerosol properties from multiangular and multispectral polarized radiances

NASA Astrophysics Data System (ADS)

Miecznik, Grzegorz; Illing, Rainer; Petroy, Shelley; Sokolik, Irina N.

2005-07-01

Linearly polarized radiation is sensitive to the microphysical properties of aerosols, namely, to the particle- size distribution and refractive index. The discriminating power of polarized radiation increases strongly with the increasing range of scattering angles and the addition of multiple wavelengths. The polarization and directionality of the Earth's reflectances (POLDER) missions demonstrate that some aerosol properties can be successfully derived from spaceborne polarimetric, multiangular measurements at two visible wavelengths. We extend the concept to analyze the retrieval capabilities of a spaceborne instrument with six polarimetric channels at 412, 445, 555, 865, 1250, and 2250 nm, measuring approximately 100 scattering angles covering a range between 50 and 150 deg. Our focus is development of an analysis methodology that can help quantify the benefits of such multiangular and multispectral polarimetric measurements. To that goal we employ a sensitivity metric approach in a framework of the principal-component analysis. The radiances and noise used to construct the sensitivity metric are calculated with the realistic solar flux for representative orbital viewing geometries, accounting for surface reflection from the ground, and statistical and calibration errors of a notional instrument. Spherical aerosol particles covering a range of representative microphysical properties (effective radius, effective variance, real and imaginary parts of the refractive index, single-scattering albedo) are considered in the calculations. We find that there is a limiting threshold for the effective size (approximately 0.7 μm), below which the weak scattering intensity results in a decreased signal-to-noise ratio and minimal polarization sensitivity, precluding reliable aerosol retrievals. For such small particles, close to the Rayleigh scattering limit, the total intensity provides a much stronger aerosol signature than the linear polarization, inspiring retrieval

Polyhexamethylene guanidine phosphate aerosol particles induce pulmonary inflammatory and fibrotic responses.

PubMed

Kim, Ha Ryong; Lee, Kyuhong; Park, Chang We; Song, Jeong Ah; Shin, Da Young; Park, Yong Joo; Chung, Kyu Hyuck

2016-03-01

Polyhexamethylene guanidine (PHMG) phosphate was used as a disinfectant for the prevention of microorganism growth in humidifiers, without recognizing that a change of exposure route might cause significant health effects. Epidemiological studies reported that the use of humidifier disinfectant containing PHMG-phosphate can provoke pulmonary fibrosis. However, the pulmonary toxicity of PHMG-phosphate aerosol particles is unknown yet. This study aimed to elucidate the toxicological relationship between PHMG-phosphate aerosol particles and pulmonary fibrosis. An in vivo nose-only exposure system and an in vitro air-liquid interface (ALI) co-culture model were applied to confirm whether PHMG-phosphate induces inflammatory and fibrotic responses in the respiratory tract. Seven-week-old male Sprague-Dawley rats were exposed to PHMG-phosphate aerosol particles for 3 weeks and recovered for 3 weeks in a nose-only exposure chamber. In addition, three human lung cells (Calu-3, differentiated THP-1 and HMC-1 cells) were cultured at ALI condition for 12 days and were treated with PHMG-phosphate at set concentrations and times. The reactive oxygen species (ROS) generation, airway barrier injuries and inflammatory and fibrotic responses were evaluated in vivo and in vitro. The rats exposed to PHMG-phosphate aerosol particles in nanometer size showed pulmonary inflammation and fibrosis including inflammatory cytokines and fibronectin mRNA increase, as well as histopathological changes. In addition, PHMG-phosphate triggered the ROS generation, airway barrier injuries and inflammatory responses in a bronchial ALI co-culture model. Those results demonstrated that PHMG-phosphate aerosol particles cause pulmonary inflammatory and fibrotic responses. All features of fibrogenesis by PHMG-phosphate aerosol particles closely resembled the pathology of fibrosis that was reported in epidemiological studies. Finally, we expected that PHMG-phosphate infiltrated into the lungs in the form of

Morphologies of aerosol particles consisting of two liquid phases

NASA Astrophysics Data System (ADS)

Song, Mijung; Marcolli, Claudia; Krieger, Ulrich; Peter, Thomas

2013-04-01

Recent studies have shown that liquid-liquid phase separation (LLPS) might be a common feature in mixed organic/ammonium sulfate (AS)/H2O particles. Song et al. (2012) observed that in atmospheric relevant organic/AS/H2O mixtures LLPS always occurred for organic aerosol compositions with O:C < 0.56, depended on the specific functional groups of organics in the range of 0.56 < O:C < 0.80 and never appeared for O:C > 0.80. The composition of the organic fraction and the mixing state of aerosol particles may influence deliquescence relative humidity (DRH) and efflorescence relative humidity (ERH) of inorganic salts during RH cycles and also aerosol morphology. In order to determine how the deliquescence and efflorescence of AS in mixed organic/AS/H2O particles is influenced by LLPS and to identify the corresponding morphologies of the particles, we subjected organic/AS/H2O particles deposited on a hydrophobically coated substrate to RH cycles and observed the phase transitions using optical microscopy and Raman spectroscopy. In this study, we report results from 21 organic/AS/H2O systems with O:C ranging from 0.55 - 0.85 covering aliphatic and aromatic oxidized compounds. Eight systems did not show LLPS for all investigated organic-to-inorganic ratios, nine showed core-shell morphology when present in a two-liquid-phases state and four showed both, core-shell or partially engulfed configurations depending on the organic-to-inorganic ratio. While AS in aerosol particles with complete LLPS showed almost constant values of ERH = 44 ± 4 % and DRH = 77 ± 2 %, a strong reduction or complete inhibition of efflorescence occurred for mixtures that did not exhibit LLPS. To confirm these findings, we performed supplementary experiments on levitated particles in an electrodynamic balance and compared surface and interfacial tensions of the investigated mixtures. Reference Song, M., C. Marcolli, U. K. Krieger, A. Zuend, and T. Peter (2012), Liquid-liquid phase separation in

Columnar and ground-level aerosol optical properties: sensitivity to the transboundary pollution, daily and weekly patterns, and relationships.

PubMed

Perrone, M R; Romano, S; Orza, J A G

2015-11-01

Columnar and ground-level aerosol optical properties co-located in space and time and retrieved from sun/sky photometer and nephelometer measurements, respectively, have been analyzed to investigate the impact of local and transboundary pollution, to analyze their relationships, and hence to contribute to the aerosol load characterization over the Central Mediterranean. The aerosol optical depth (AOD) at 440 nm, the Ångström exponent (Å) calculated from the AOD at 440 and 675 nm, and the asymmetry parameter (g col ) at 440 nm represent the investigated columnar aerosol parameters. The scattering coefficient (σ p) at 450 nm, the scattering Ångström exponent (å) calculated from σ p at 450 and 635 nm, and the asymmetry parameter (g) at 450 nm are the corresponding ground-level parameters. It is shown that the columnar and ground-level aerosol properties were significantly and similarly affected by the main airflows identified with backtrajectory cluster analysis. The yearly averaged daily evolution of σ p, å, and g was fairly correlated to the one of the AOD, Å, and g col , respectively. These results indicate that the aerosol particles were on average characterized by similar yearly averaged optical properties up to the ground level. In particular, the yearly means of columnar and ground-level Ångström exponents, 1.3 ± 0.4 and 1.1 ± 0.4, respectively, which are close to one, reveal a coarse-mode aerosol contribution in addition to the fine-mode particle contribution up to the ground level. Hourly means, day-by-day, and seasonal daily patterns of ground-level parameters were, however, very weakly correlated with the corresponding columnar parameters. The large impact of the local meteorology on the daily evolution of the ground-level aerosol properties, which makes the impact of long-range transported particles less apparent, was mainly responsible for these last results. It has also been found that columnar Ångström exponents much smaller

Effect of typhoon on atmospheric aerosol particle pollutants accumulation over Xiamen, China.

PubMed

Yan, Jinpei; Chen, Liqi; Lin, Qi; Zhao, Shuhui; Zhang, Miming

2016-09-01

Great influence of typhoon on air quality has been confirmed, however, rare data especially high time resolved aerosol particle data could be used to establish the behavior of typhoon on air pollution. A single particle aerosol spectrometer (SPAMS) was employed to characterize the particles with particle number count in high time resolution for two typhoons of Soulik (2013) and Soudelor (2015) with similar tracks. Three periods with five events were classified during the whole observation time, including pre - typhoon (event 1 and event 2), typhoon (event 3 and event 4) and post - typhoon (event 5) based on the meteorological parameters and particle pollutant properties. First pollutant group appeared during pre-typhoon (event 2) with high relative contributions of V - Ni rich particles. Pollution from the ship emissions and accumulated by local processes with stagnant meteorological atmosphere dominated the formation of the pollutant group before typhoon. The second pollutant group was present during typhoon (event 3), while typhoon began to change the local wind direction and increase wind speed. Particle number count reached up to the maximum value. High relative contributions of V - Ni rich and dust particles with low value of NO3(-)/SO4(2-) was observed during this period, indicating that the pollutant group was governed by the combined effect of local pollutant emissions and long-term transports. The analysis of this study sheds a deep insight into understand the relationship between the air pollution and typhoon. Copyright © 2016 Elsevier Ltd. All rights reserved.

Chemical and Physical Properties of Individual Aerosol Particles Characterized in Sacramento, CA during CARES Field Campaign

NASA Astrophysics Data System (ADS)

Zelenyuk, A.; Beranek, J.; Vaden, T.; Imre, D. G.; Zaveri, R. A.

2011-12-01

We present results of measurements conducted by our Single Particle Mass Spectrometer, SPLAT II, in Sacramento, CA over the month of June 2010. SPLAT II measured the size of 195 million particles, and compositions of 10 million particles. In addition to size and composition, SPLAT II simultaneously measured size, density and composition of 121,000 individual particles. These measurements were conducted 2 - 3 times per day, depending on conditions. The data show that throughout the day particles were relatively small (<200 nm), and the vast majority were composed of oxygenated organics mixed with various amounts of sulfate. In addition, we characterized fresh and processed soot, biomass burning aerosol, organic amines, fresh and processed sea salt, and few dust particles. The data show a reproducible diurnal pattern in aerosol size distributions, number concentrations, and compositions. Early in the day, number concentrations were low, particles were very small, and the size distributions peaked at ~70 nm. At this time of the day, 80 nm particles had a density of 1.3 g cm-3; while the density of 200 nm particles was 1.6 g cm-3, consistent with our mass spectra showing that smaller particles were composed of organics mixed with ~10% sulfates, while larger particles were composed mostly of sulfate mixed with a small amount of organics. Later in the day, secondary organic aerosols (SOA) formation led to a number of nucleation events that significantly increased the number concentrations of very small particles. By mid-afternoon, as more SOA formed and condensed, particles increased in size the number concentrations of particles larger than 70 nm increased and the densities of particles 80 to 200 nm particles was ~1.3 g cm-3. The vast majority of these particles were composed of oxygenated organics mixed with a ~10% sulfate. In other words they were SOA particles mixed with a small amount of sulfate. The mass spectra of these particles shows that there were two types of

Photon Counting Techniques Applied to Single Aerosol Particle Spectroscopy.

NASA Astrophysics Data System (ADS)

Joynson, Steven

Available from UMI in association with The British Library. Optical effects on single airborne particles were examined for their potential use in aerosol characterisation. All phenomena arising from the elastic or quasi-elastic scattering, or the absorption of light were considered. A survey of published research identified the effects that have so far been proposed and investigated by other researchers. The feasibility of using these effects is then discussed and appropriate calculations and measurements made. After reviewing the classical theory of the interaction of light with small particles it was apparent that there was a number of other effects that had not yet been considered or examined by other researchers. Calculations and measurements of these effects were then made and are also presented here. The effects were examined optically using photon counting equipment to count and store the dynamic light scattering signals from a single particles in an aerosol flow. The measurement thus entailed using a low intensity probe beam to measure the effects of higher intensity pump radiation on the motion, shape and scattering properties of a test particle. The amount of information in the probe signal was increased by using a velocimetry arrangement. In the absence of suitable commercially available photon counting equipment a new system had to be designed and developed at RMCS. Although requiring much time and effort to develop, the equipment allowed a new approach to light scattering research. The successful operation of the equipment was confirmed by the good agreement found when comparing measured photon count series statistics with those of the simulated signals presented by other researchers. Experiments that were done to measure some of the optical effects are described and the results presented. They demonstrate the successful diffusion sizing of individual aerosol particles and their motion under radiation pressure. Further experimental results demonstrate

Resolving the Aerosol Piece of the Global Climate Picture

NASA Astrophysics Data System (ADS)

Kahn, R. A.

2017-12-01

Factors affecting our ability to calculate climate forcing and estimate model predictive skill include direct radiative effects of aerosols and their indirect effects on clouds. Several decades of Earth-observing satellite observations have produced a global aerosol column-amount (AOD) record, but an aerosol microphysical property record required for climate and many air quality applications is lacking. Surface-based photometers offer qualitative aerosol-type classification, and several space-based instruments map aerosol air-mass types under favorable conditions. However, aerosol hygroscopicity, mass extinction efficiency (MEE), and quantitative light absorption, must be obtained from in situ measurements. Completing the aerosol piece of the climate picture requires three elements: (1) continuing global AOD and qualitative type mapping from space-based, multi-angle imagers and aerosol vertical distribution from near-source stereo imaging and downwind lidar, (2) systematic, quantitative in situ observations of particle properties unobtainable from space, and (3) continuing transport modeling to connect observations to sources, and extrapolate limited sampling in space and time. At present, the biggest challenges to producing the needed aerosol data record are: filling gaps in particle property observations, maintaining global observing capabilities, and putting the pieces together. Obtaining the PDFs of key particle properties, adequately sampled, is now the leading observational deficiency. One simplifying factor is that, for a given aerosol source and season, aerosol amounts often vary, but particle properties tend to be repeatable. SAM-CAAM (Systematic Aircraft Measurements to Characterize Aerosol Air Masses), a modest aircraft payload deployed frequently could fill this gap, adding value to the entire satellite data record, improving aerosol property assumptions in retrieval algorithms, and providing MEEs to translate between remote-sensing optical constraints

Source apportionment of lead-containing aerosol particles in Shanghai using single particle mass spectrometry.

PubMed

Zhang, Yaping; Wang, Xiaofei; Chen, Hong; Yang, Xin; Chen, Jianmin; Allen, Jonathan O

2009-01-01

Lead (Pb) in individual aerosol particles was measured using single particle aerosol mass spectrometer (ATOFMS) in the summer of 2007 in Shanghai, China. Pb was found in 3% of particles with diameters in the range 0.1-2.0 microm. Single particle data were analyzed focusing on the particles with high Pb content which were mostly submicron. Using the ART-2a neural network algorithm, these fine Pb-rich particles were classified into eight main classes by their mass spectral patterns. Based on the size distribution, temporal variation of number density, chemical composition and the correlation between different chemical species for each class, three major emission sources were identified. About 45% of the Pb-rich particles contained organic or elemental carbon and were attributed to the emission from coal combustion; particles with good correlation between Cl and Pb content were mostly attributed to waste incineration. One unique class of particles was identified by strong phosphate and Pb signals, which were assigned to emissions from phosphate industry. Other Pb-rich particles included aged sea salt and particles from metallurgical processes.

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.

Spectral Absorption Properties of Aerosol Particles from 350-2500nm

NASA Technical Reports Server (NTRS)

Martins, J. Vanderlei; Artaxo, Paulo; Kaufman, Yoram J.; Castanho, Andrea D.; Remer, Lorraine A.

2009-01-01

The aerosol spectral absorption efficiency (alpha (sub a) in square meters per gram) is measured over an extended wavelength range (350 2500 nm) using an improved calibrated and validated reflectance technique and applied to urban aerosol samples from Sao Paulo, Brazil and from a site in Virginia, Eastern US, that experiences transported urban/industrial aerosol. The average alpha (sub a) values (approximately 3 square meters per gram at 550 nm) for Sao Paulo samples are 10 times larger than alpha (sub a) values obtained for aerosols in Virginia. Sao Paulo aerosols also show evidence of enhanced UV absorption in selected samples, probably associated with organic aerosol components. This extra UV absorption can double the absorption efficiency observed from black carbon alone, therefore reducing by up to 50% the surface UV fluxes, with important implications for climate, UV photolysis rates, and remote sensing from space.

Some Technical Aspects of a CALIOP and MODIS Data Analysis that Examines Near-Cloud Aerosol Properties as a Function of Cloud Fraction

NASA Technical Reports Server (NTRS)

Varnai, Tamas; Yang, Weidong; Marshak, Alexander

2016-01-01

CALIOP shows stronger near-cloud changes in aerosol properties at higher cloud fractions. Cloud fraction variations explain a third of near-cloud changes in overall aerosol statistics. Cloud fraction and aerosol particle size distribution have a complex relationship.

Aerosol physicochemical properties in relation to meteorology: Case studies in urban, marine, and arid settings

NASA Astrophysics Data System (ADS)

Wonaschuetz, Anna

Atmospheric aerosols are a highly relevant component of the climate system affecting atmospheric radiative transfer and the hydrological cycle. As opposed to other key atmospheric constituents with climatic relevance, atmospheric aerosol particles are highly heterogeneous in time and space with respect to their size, concentration, chemical composition and physical properties. Many aspects of their life cycle are not understood, making them difficult to represent in climate models and hard to control as a pollutant. Aerosol-cloud interactions in particular are infamous as a major source of uncertainty in future climate predictions. Field measurements are an important source of information for the modeling community and can lead to a better understanding of chemical and microphysical processes. In this study, field data from urban, marine, and arid settings are analyzed and the impact of meteorological conditions on the evolution of aerosol particles while in the atmosphere is investigated. Particular attention is given to organic aerosols, which are a poorly understood component of atmospheric aerosols. Local wind characteristics, solar radiation, relative humidity and the presence or absence of clouds and fog are found to be crucial factors in the transport and chemical evolution of aerosol particles. Organic aerosols in particular are found to be heavily impacted by processes in the liquid phase (cloud droplets and aerosol water). The reported measurements serve to improve the process-level understanding of aerosol evolution in different environments and to inform the modeling community by providing realistic values for input parameters and validation of model calculations.

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

Total particle, sulfate, and acidic aerosol emissions from kerosene space heaters

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

Leaderer, B.P.; Boone, P.M.; Hammond, S.K.

1990-06-01

Chamber studies were conducted on four unvented kerosene space heaters to assess emissions of total particle, sulfate, and acidic aerosol. The heaters tested represented four burner designs currently in use by the public. Kerosene space heaters are a potential source of fine particles ({<=} 2.5-{mu}m diameter), sulfate, and acidic aerosol indoors. Fine particle concentrations in homes in which the heaters are used may be increased in excess of 20 {mu}g/m{sup 3} over background levels. Sulfate and acidic aerosol levels in such homes could exceed average and peak outdoor concentrations. Maltuned heaters could produce exceptionally high levels of all air contaminantsmore » measured.« less

Total particle, sulfate, and acidic aerosol emissions from kerosene space heaters

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

Leaderer, B.P.; Boone, P.M.; Hammond, S.K.

1990-01-01

The article discusses chamber studies of four unvented kerosene space heaters to assess emissions of total particle, sulfate, and acidic aerosol. The heaters tested represented four burner designs currently in use by the public. Kerosene space heaters are a potential source of fine particles (= or < 2.5 micrometer diameter), sulfate, and acidic aerosol indoors. Fine particle concentrations in houses in which the heaters are used may be increased in excess of 20 micrograms/m3 over background levels. Sulfate and acidic aerosol levels in such houses could exceed average and peak outdoor concentrations. Maltuned heaters could produce exceptionally high levels ofmore » all air contaminants measured.« less

Constraints on Martian Aerosol Particles Using MGS/TES and HST Data: Shapes

NASA Astrophysics Data System (ADS)

Wolff, M. J.; Clancy, R. T.; Pitman, K. M.; Bell, J. F.; James, P. B.

2001-12-01

In order to constrain the shape of water ice and dust aerosols, we have combined a numerical approach for axisymmetric particle shapes, i.e., cylinders, disks, spheroids (Waterman's T-Matrix approach as improved by Mishchenko and collaborators; cf., Mishchenko et al. 1997, JGR, 102, D14, 16,831), with a multiple-scattering radiative transfer algorithm. We utilize a two-stage iterative process. First, we empirically derive a scattering phase function for each aerosol component from radiative transfer models of Mars Global Surveyor Thermal Emission Spectrometer Emission Phase Function (EPF) sequences. Next, we perform a series of scattering calculations, adjusting our parameters to arrive at a ``best-fit'' theoretical phase function. It is important to note that in addition to randomly-oriented particles, we explicitly consider the possibility of (partially) aligned aerosol particles as well. Thus far, we have been analyzing the three empirically-derived presented by Clancy et al. (this meeting): dust, Type I ice particles (effective radii ~ 1-2 microns), and Type II ice particles (effective radii ~ 3-4 microns). We find that the ``dust'' phase function is best fit by randomly-oriented cylinders with an axial ratio (D/L = diameter-to-length) of either 2.3 or 0.6. Similarly, the shape of the Type II ice curve is reasonably reproduced by randomly-oriented spheroids with an axial ratio of either 0.7 or 1.4. However, neither of the two shapes (nor that of spheres or randomly-oriented hexagonal prisms) can reproduce the phase function derived for the Type I ice. This led to the direct consideration of oriented or aligned particles. which, at least qualitatively, have the ability to account for the phase function shapes for both Type I and II ice particles. The difference between these two phase functions may represent the degree of alignment, with the Type II particles being much less-aligned. The calculations for partially aligned particles is quite numerically intensive

Single-particle characterization of urban aerosol particles collected in three Korean cites using low-Z electron probe X-ray microanalysis.

PubMed

Ro, Chul-Un; Kim, HyeKyeong; Oh, Keun-Young; Yea, Sun Kyung; Lee, Chong Bum; Jang, Meongdo; Van Grieken, René

2002-11-15

A recently developed single-particle analytical technique, called low-Z electron probe X-ray microanalysis (low-Z EPMA), was applied to characterize urban aerosol particles collected in three cities of Korea (Seoul, CheongJu, and ChunCheon) on single days in the winter of 1999. In this study, it is clearly demonstrated that the low-Z EPMA technique can provide detailed and quantitative information on the chemical composition of particles in the urban atmosphere. The collected aerosol particles were analyzed and classified on the basis of their chemical species. Various types of particles were identified, such as soil-derived, carbonaceous, marine-originated, and anthropogenic particles. In the sample collected in Seoul, carbonaceous, aluminosilicates, silicon dioxide, and calcium carbonate aerosol particles were abundantly encountered. In the CheongJu and ChunCheon samples, carbonaceous, aluminosilicates, reacted sea salts, and ammonium sulfate aerosol particles were often seen. However, in the CheongJu sample, ammonium sulfate particles were the most abundant in the fine fraction. Also, calcium sulfate and nitrate particles were significantly observed. In the ChunCheon sample, organic particles were the most abundant in the fine fraction. Also, sodium nitrate particles were seen at high levels. The ChunCheon sample seemed to be strongly influenced by sea-salt aerosols originating from the Yellow Sea, which is located about 115 km away from the city.

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).

Physico-Chemical Properties, Aerosolization and Dissolution of Co-Spray Dried Azithromycin Particles with L-Leucine for Inhalation.

PubMed

Mangal, Sharad; Nie, Haichen; Xu, Rongkun; Guo, Rui; Cavallaro, Alex; Zemlyanov, Dmitry; Zhou, Qi Tony

2018-01-08

Inhalation therapy is popular to treat lower respiratory tract infections. Azithromycin is effective against some bacteria that cause respiratory tract infections; but it has poor water solubility that may limit its efficacy when administrated as inhalation therapy. In this study, dry powder inhaler formulations were developed by co-spray drying azithromycin with L-leucine with a purpose to improve dissolution. The produced powder formulations were characterized regarding particle size, morphology, surface composition and in-vitro aerosolization performance. Effects of L-leucine on the solubility and in-vitro dissolution of azithromycin were also evaluated. The spray dried azithromycin alone formulation exhibited a satisfactory aerosol performance with a fine particle fraction (FPF) of 62.5 ± 4.1%. Addition of L-leucine in the formulation resulted in no significant change in particle morphology and FPF, which can be attributed to enrichment of azithromycin on the surfaces of composite particles. Importantly, compared with the spray-dried amorphous azithromycin alone powder, the co-spray dried powder formulations of azithromycin and L-leucine demonstrated a substantially enhanced in-vitro dissolution rate. Such enhanced dissolution of azithromycin could be attributed to the formation of composite system and the acidic microenvironment around azithromycin molecules created by the dissolution of acidic L-leucine in the co-spray dried powder. Fourier transform infrared spectroscopic data showed intermolecular interactions between azithromycin and L-leucine in the co-spray dried formulations. We developed the dry powder formulations with satisfactory aerosol performance and enhanced dissolution for a poorly water soluble weak base, azithromycin, by co-spray drying with an amino acid, L-leucine.

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.

Aerosol particle size distribution in the stratosphere retrieved from SCIAMACHY limb measurements

NASA Astrophysics Data System (ADS)

Malinina, Elizaveta; Rozanov, Alexei; Rozanov, Vladimir; Liebing, Patricia; Bovensmann, Heinrich; Burrows, John P.

2018-04-01

aerosols in the Earth's atmosphere is of a great importance in the scientific community. While tropospheric aerosol influences the radiative balance of the troposphere and affects human health, stratospheric aerosol plays an important role in atmospheric chemistry and climate change. In particular, information about the amount and distribution of stratospheric aerosols is required to initialize climate models, as well as validate aerosol microphysics models and investigate geoengineering. In addition, good knowledge of stratospheric aerosol loading is needed to increase the retrieval accuracy of key trace gases (e.g. ozone or water vapour) when interpreting remote sensing measurements of the scattered solar light. The most commonly used characteristics to describe stratospheric aerosols are the aerosol extinction coefficient and Ångström coefficient. However, the use of particle size distribution parameters along with the aerosol number density is a more optimal approach. In this paper we present a new retrieval algorithm to obtain the particle size distribution of stratospheric aerosol from space-borne observations of the scattered solar light in the limb-viewing geometry. While the mode radius and width of the aerosol particle size distribution are retrieved, the aerosol particle number density profile remains unchanged. The latter is justified by a lower sensitivity of the limb-scattering measurements to changes in this parameter. To our knowledge this is the first data set providing two parameters of the particle size distribution of stratospheric aerosol from space-borne measurements of scattered solar light. Typically, the mode radius and w can be retrieved with an uncertainty of less than 20 %. The algorithm was successfully applied to the tropical region (20° N-20° S) for 10 years (2002-2012) of SCIAMACHY observations in limb-viewing geometry, establishing a unique data set. Analysis of this new climatology for the particle size

Shapes of soot aerosol particles and implications for their effects on climate

NASA Astrophysics Data System (ADS)

Adachi, Kouji; Chung, Serena H.; Buseck, Peter R.

2010-08-01

Soot aerosol particles (also called light-absorbing, black, or elemental carbon) are major contributors to global warming through their absorption of solar radiation. When embedded in organic matter or sulfate, as is common in polluted areas such as over Mexico City (MC) and other megacities, their optical properties are affected by their shapes and positions within their host particles. However, large uncertainties remain regarding those variables and how they affect warming by soot. Using electron tomography with a transmission electron microscope, three-dimensional (3-D) images of individual soot particles embedded within host particles collected from MC and its surroundings were obtained. From those 3-D images, we calculated the optical properties using a discrete dipole approximation. Many soot particles have open, chainlike shapes even after being surrounded by organic matter and are located in off-center positions within their host materials. Such embedded soot absorbs sunlight less efficiently than if compact and located near the center of its host particle. In the case of our MC samples, their contribution to direct radiative forcing is ˜20% less than if they had a simple core-shell shape, which is the shape assumed in many climate models. This study shows that the shapes and positions of soot within its host particles have an important effect on particle optical properties and should be recognized as potentially important variables when evaluating global climate change.

¹¹¹Indium-labeled ultrafine carbon particles; a novel aerosol for pulmonary deposition and retention studies.

PubMed

Sanchez-Crespo, Alejandro; Klepczynska-Nyström, Anna; Lundin, Anders; Larsson, Britt Marie; Svartengren, Magnus

2011-02-01

Continuous environmental or occupational exposure to airborne particulate pollution is believed to be a major hazard for human health. A technique to characterize their deposition and clearance from the lungs is fundamental to understand the underlying mechanisms behind their negative health effects. In this work, we describe a method for production and follow up of ultrafine carbon particles labeled with radioactive ¹¹¹Indium (¹¹¹In). The physicochemical and biological properties of the aerosol are described in terms of particle size and concentration, agglomeration rate, chemical bonding stability, and human lung deposition and retention. Preliminary in vivo data from a healthy human pilot exposure and 1-week follow up of the aerosol is presented. More than 98% of the generated aerosol was labeled with Indium and with particle sizes log normally distributed around 79  nm count median diameter. The aerosol showed good generation reproducibility and chemical stability, about 5% leaching 7 days after generation. During human inhalation, the particles were deposited in the alveolar space, with no central airways involvement. Seven days after exposure, the cumulative activity retention was 95.3%. Activity leaching tests from blood and urine samples confirmed that the observed clearance was explained by unbound activity, suggesting that there was no significant elimination of ultrafine particles. Compared to previously presented methods based on Technegas, ¹¹¹In-labelled ultrafine carbon particles allow for extended follow-up assessments of particulate pollution retention in healthy and diseased lungs.

Columnar aerosol optical properties at AERONET sites in northern, central and southern Mexico

NASA Astrophysics Data System (ADS)

Carabali, Giovanni; Estévez, Hector; Florean-Cruz, Claudia; Navarro-Medina, Abigail; Valdés-Barrón, Mauro; Bonifaz-Alfonzo, Roberto; Riveros-Rosas, David; Velasco-Herrera, Víctor; Vázquez-Gálvez, Felipe

2017-04-01

The column-integrated optical properties of aerosol in the north, central and southern Mexico were investigated based on Sun/sky radiometer measurements made at Aerosol Robotic Network (AERONET) sites. Characterization of aerosol properties in these Mexico regions is important due to natural and anthropogenic significant events that occurred: dust storms from Sonora desert, biomass burning from south forest areas and urban/industrial from Mexico City due to the increases in fossil fuel combustion. Some cities in northern Mexico located near desert areas are affected by the dust from Sonora and Chihuahua deserts. These particles are suspended in the atmosphere due to strong wind activity that creates dust storms. In the central part of the Mexican territory, urban air pollution is one of the biggest problems. Mexico City is the most important urban area that face seriously environmental problem generated by daily anthropogenic emissions from activities of some 21 million people and the vast amount of industry. On the other hand, biomass burning in the Yucatan Peninsula, Southern Mexico, and Guatemala is an important source of anthropogenic aerosol in the troposphere (Crutzen and Andrade, 1990). The pollution from these fires affects air quality locally and is transported over the Gulf of Mexico to the United States (Wang et al., 2006). The aim of this work is to study the optical properties of different types of aerosols by analyzing a 5-year (2005-2010) data set from AErosol RObotic NETwork (AERONET). Time series of Angstrom exponent (α) and aerosol optical depth (τ) in 7 wavelengths from 340 to 1020 nm are shown. Additionally, a graphical framework to classify aerosol properties using direct sun-photometer observations in the different regions of Mexico is presented. That aerosol classification was made by applying the method described by Gobbi et al (2007), which relies on the combined analysis of α and its spectral curvature δα.

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.

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.

Endotoxin in Size-Separated Metal Working Fluid Aerosol Particles.

PubMed

Dahlman-Höglund, Anna; Lindgren, Åsa; Mattsby-Baltzer, Inger

2016-08-01

Patients with airway symptoms working in metal working industries are increasing, despite efforts to improve the environmental air surrounding the machines. Our aim was to analyse the amount of endotoxin in size-separated airborne particles of metal working fluid (MWF) aerosol, by using the personal sampler Sioutas cascade impactor, to compare filter types, and to compare the concentration of airborne endotoxin to that of the corresponding MWFs. In a pilot field study, aerosols were collected in two separate machine halls on totally 10 occasions, using glass fibre and polytetrafluoroethylene (PTFE) filters in parallel at each station. Airborne endotoxin was distributed over all size fractions. While a major part was found in the largest size fraction (72%, 2.5-10 µm), up to 8% of the airborne endotoxin was detected in the smallest size fraction (<0.25 µm). Comparing the efficiency of the filter types, a significantly higher median endotoxin level was found with glass fibres filters collecting the largest particle-size fraction (1.2-fold) and with PTFE filters collecting the smallest ones (5-fold). The levels of endotoxin in the size-separated airborne particle fractions correlated to those of the MWFs supporting the aerosol-generating machines. Our study indicates that a significant part of inhalable aerosols of MWFs consists of endotoxin-containing particles below the size of intact bacteria, and thus small enough to readily reach the deepest part of the lung. Combined with other chemical irritants of the MWF, exposure to MWF aerosols containing endotoxin pose a risk to respiratory health problems. © The Author 2016. Published by Oxford University Press on behalf of the British Occupational Hygiene Society.

Developing and diagnosing climate change indictors of regional aerosol optical properties

NASA Astrophysics Data System (ADS)

Sullivan, Ryan C.; Levy, Robert C.; da Silva, Arlindo M.; Pryor, Sara C.

2017-04-01

The US Global Change Research Program has developed climate indicators (CIs) to track changes in the physical, chemical, biological, and societal components of the climate system. Given the importance of atmospheric aerosol particles to clouds and radiative forcing, human mortality and morbidity, and biogeochemical cycles, we propose new aerosol particle CIs applicable to the US National Climate Assessment (NCA). Here we define these aerosol CIs and use them to quantify temporal trends in each NCA region. Furthermore, we use a synoptic classification (e.g., meteorological variables), and gas and particle emissions inventories to diagnose and attribute causes of observed changes. Our CIs are derived using output from the satellite-constrained Modern-Era Retrospective Analysis for Research and Application, Version 2 (MERRA-2) reanalysis. MERRA-2 provides estimates of column-integrated aerosol optical properties at 0.625° by 0.5° resolution, including aerosol optical depth (AOD), Ångström exponent (AE), and single scattering albedo (SSA), which are related to aerosol loading, relative particle size, and chemical composition, respectively. For each NCA region, and for each aerosol variable, we derive statistics that describe mean and extreme values, as well as two metrics (spatial autocorrelation and coherence) that describe the spatial scales of aerosol variability. Consistent with previous analyses of aerosol precursor emissions and near-surface fine aerosol mass concentrations in the US, analyses of our aerosol CIs show that since 2000, both mean and extreme AOD have decreased over most NCA regions. There are significant (α = 0.05, using the non-parametric Kendall's tau) decreases in AOD for the Northeast (NE), Southeast (SE), Midwest (MW), and lower Great Plains (GPl) regions, and notable but not significant decreases in the Southwest (SW). AOD has increased for the Northwest (NW; significant) and upper Great Plains (GPu; not significant). Over all regions

In situ airborne measurements of aerosol optical properties during photochemical pollution events

NASA Astrophysics Data System (ADS)

Mallet, M.; van Dingenen, R.; Roger, J. C.; Despiau, S.; Cachier, H.

2005-02-01

Dry aerosol optical properties (scattering, absorbing coefficients, and single scattering albedo) were derived from in situ airborne measurements during two photochemical pollution events (25 and 26 June) observed during the Experience sur Site pour Contraindre les Modeles de Pollution atmospherique et de Transport d'Emissions (ESCOMPTE) experiment. Two flights were carried out during daytime (one during the morning and one at noon) over a domain, allowing the investigation of how an air pollution event affects the particle optical properties. Both horizontal distribution and vertical profiles are presented. Results from the horizontal mapping show that plumes of enhanced scattering and absorption are formed in the planetary boundary layer (PBL) during the day in the sea breeze-driven outflow of the coastal urban-industrial area of Marseille-Fos de Berre. The domain-averaged scattering coefficient (at 550 nm) over land σs changes from 35 (28) Mm-1 during land breeze to 63 (43) Mm-1 during sea breeze on 25 June (26 June), with local maxima reaching > 100 Mm-1. The increase in the scattering coefficient is associated with new particle formation, indicative of secondary aerosol formation. Simultaneously, the domain-averaged absorption coefficient increases from 5.6 (3.4) Mm-1 to 9.3 (8.0) Mm-1. The pollution plume leads to strong gradients in the single scattering albedo ωo over the domain studied, with local values as low as 0.73 observed inside the pollution plume. The role of photochemistry and secondary aerosol formation during the 25 June case is shown to increase ωo and to make the aerosol more `reflecting' while the plume moves away from the sources. The lower photochemical activity, observed in the 26 June case, induces a relatively higher contribution of black carbon, making the aerosol more absorbing. Results from vertical profiles at a single near-urban location in the domain indicate that the changes in optical properties happen almost entirely within

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

First Quantification of Imidazoles in Ambient Aerosol Particles: Potential Photosensitizers, Brown Carbon Constituents, and Hazardous Components.

PubMed

Teich, Monique; van Pinxteren, Dominik; Kecorius, Simonas; Wang, Zhibin; Herrmann, Hartmut

2016-02-02

Imidazoles are widely discussed in recent literature. They have been studied as a secondary product of the reaction of dicarbonyls with nitrogen containing compounds in a number of laboratory studies, potentially acting as photosensitizers triggering secondary organic aerosol growth and are forming constituents of light absorbing brown carbon. Despite the knowledge from laboratory studies, no quantitative information about imidazoles in ambient aerosol particles is available. Within the present study, five imidazoles (1-butylimidazole, 1-ethylimidazole, 2-ethylimidazole, imidazol-2-carboxaldehyde, and 4(5)-methylimidazole) were successfully identified and quantified for the first time in ambient aerosol samples from different environments in Europe and China. Their concentrations range between 0.2 and 14 ng/m(3). 4(5)-Methylimidazole was found to be the most abundant imidazole. The occurrence of imidazoles seems to be favored at sites with strong biomass burning influence or connected to more polluted air masses. No connection was found between aerosol particle pH and imidazole concentration. Our work corroborates the laboratory studies by showing that imidazoles are present in ambient aerosol samples in measurable amounts. Moreover, it further motivates to explore the potential photosensitizing properties of small alkyl-substituted imidazoles.

A three-dimensional sectional representation of aerosol mixing state for simulating optical properties and cloud condensation nuclei

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

Ching, Ping Pui; Zaveri, Rahul A.; Easter, Richard C.

2016-05-27

Light absorption by black carbon (BC) particles emitted from fossil fuel combustion depends on the how thickly they are coated with non-refractory species such as ammonium, sulfate, nitrate, organics, and water. The cloud condensation nuclei (CCN) activation property of a particle depends on its dry size and the hygroscopicities of all the individual species mixed together. It is therefore necessary to represent both size and mixing state of aerosols to reliably predict their climate-relevant properties in atmospheric models. Here we describe and evaluate a novel sectional framework in the Model for Simulating Aerosol Interactions and Chemistry, referred to as MOSAIC-mix,more » that represents the mixing state by resolving aerosol dry size (Ddry), BC dry mass fraction (wBC), and hygroscopicity (κ). Using ten idealized urban plume scenarios in which different types of aerosols evolve over 24 hours under a range of atmospherically relevant environmental conditions, we examine errors in CCN concentrations and optical properties with respect to a more explicit aerosol mixing state representation. We find that only a small number of wBC and κ bins are needed to achieve significant reductions in the errors, and propose a configuration consisting of 24 Ddry bins, 2 wBC bins, and 2 κ bins that gives 24-hour average errors of about 5% or less in CCN concentrations and optical properties, 3-4 times lower than those from size-only-resolved simulations. These results show that MOSAIC-mix is suitable for use in regional and global models to examine the effects of evolving aerosol mixing states on aerosol-radiation-cloud feedbacks.« less

Relations Between Cloud Condensation Nuclei And Aerosol Optical Properties Relevant to Remote Sensing: Airborne Measurements in Biomass Burning, Pollution and Dust Aerosol Over North America

NASA Astrophysics Data System (ADS)

Shinozuka, Y.; Clarke, A.; Howell, S.; Kapustin, V.; McNaughton, C.; Zhou, J.; Decarlo, P.; Jimenez, J.; Roberts, G.; Tomlinson, J.; Collins, D.

2008-12-01

Remote sensing of the concentration of cloud condensation nuclei (CCN) would help investigate the indirect effect of tropospheric aerosols on clouds and climate. In order to assess its feasibility, this paper evaluates the spectral-based retrieval technique for aerosol number and seeks one for aerosol solubility, using in-situ aircraft measurements of aerosol size distribution, chemical composition, hygroscopicity, CCN activity and optical properties. Our statistical analysis reveals that the CCN concentration over Mexico can be optically determined to a relative error of <20%, smaller than that for the mainland US and the surrounding oceans (~a factor of 2). Mexico's advantage is four-fold. Firstly, many particles originating from the lightly regulated industrial combustion and biomass burning are large enough to significantly affect light extinction, elevating the correlation between extinction and CCN number in absence of substantial dust. Secondly, the generally low ambient humidity near the major aerosol sources limits the error in the estimated response of particle extinction to humidity changes. Thirdly, because many CCN contain black carbon, light absorption also provides a measure of the CCN concentration. Fourthly, the organic fraction of volatile mass of submicron particles (OMF) is anti-correlated with the wavelength dependence of extinction due to preferential anion uptake by coarse dust, which provides a potential tool for remote-sensing OMF and the particle solubility.

Radiative Importance of Aerosol-Cloud Interaction

NASA Technical Reports Server (NTRS)

Tsay, Si-Chee

1999-01-01

Aerosol particles are input into the troposphere by biomass burning, among other sources. These aerosol palls cover large expanses of the earth's surface. Aerosols may directly scatter solar radiation back to space, thus increasing the earth's albedo and act to cool the earth's surface and atmosphere. Aerosols also contribute to the earth's energy balance indirectly. Hygroscopic aerosol act as cloud condensation nuclei (CCN) and thus affects cloud properties. In 1977, Twomey theorized that additional available CCN would create smaller but more numerous cloud droplets in a cloud with a given amount of liquid water. This in turn would increase the cloud albedo which would scatter additional radiation back to space and create a similar cooling pattern as the direct aerosol effect. Estimates of the magnitude of the aerosol indirect effect on a global scale range from 0.0 to -4.8 W/sq m. Thus the indirect effect can be of comparable magnitude and opposite in sign to the estimates of global greenhouse gas forcing Aerosol-cloud interaction is not a one-way process. Just as aerosols have an influence on clouds through the cloud microphysics, clouds have an influence on aerosols. Cloud droplets are solutions of liquid water and CCN, now dissolved. When the cloud droplet evaporates it leaves behind an aerosol particle. This new particle does not have to have the same properties as the original CCN. In fact, studies show that aerosol particles that result from cloud processing are larger in size than the original CCN. Optical properties of aerosol particles are dependent on the size of the particles. Larger particles have a smaller backscattering fraction, and thus less incoming solar radiation will be backscattered to space if the aerosol particles are larger. Therefore, we see that aerosols and clouds modify each other to influence the radiative balance of the earth. Understanding and quantifying the spatial and seasonal patterns of the aerosol indirect forcing may have

Aqueous aerosol SOA formation: impact on aerosol physical properties.

PubMed

Woo, Joseph L; Kim, Derek D; Schwier, Allison N; Li, Ruizhi; McNeill, V Faye

2013-01-01

Organic chemistry in aerosol water has recently been recognized as a potentially important source of secondary organic aerosol (SOA) material. This SOA material may be surface-active, therefore potentially affecting aerosol heterogeneous activity, ice nucleation, and CCN activity. Aqueous aerosol chemistry has also been shown to be a potential source of light-absorbing products ("brown carbon"). We present results on the formation of secondary organic aerosol material in aerosol water and the associated changes in aerosol physical properties from GAMMA (Gas-Aerosol Model for Mechanism Analysis), a photochemical box model with coupled gas and detailed aqueous aerosol chemistry. The detailed aerosol composition output from GAMMA was coupled with two recently developed modules for predicting a) aerosol surface tension and b) the UV-Vis absorption spectrum of the aerosol, based on our previous laboratory observations. The simulation results suggest that the formation of oligomers and organic acids in bulk aerosol water is unlikely to perturb aerosol surface tension significantly. Isoprene-derived organosulfates are formed in high concentrations in acidic aerosols under low-NO(x) conditions, but more experimental data are needed before the potential impact of these species on aerosol surface tension may be evaluated. Adsorption of surfactants from the gas phase may further suppress aerosol surface tension. Light absorption by aqueous aerosol SOA material is driven by dark glyoxal chemistry and is highest under high-NO(x) conditions, at high relative humidity, in the early morning hours. The wavelength dependence of the predicted absorption spectra is comparable to field observations and the predicted mass absorption efficiencies suggest that aqueous aerosol chemistry can be a significant source of aerosol brown carbon under urban conditions.

Gas uptake and chemical aging of semisolid organic aerosol particles

PubMed Central

Shiraiwa, Manabu; Ammann, Markus; Koop, Thomas; Pöschl, Ulrich

2011-01-01

Organic substances can adopt an amorphous solid or semisolid state, influencing the rate of heterogeneous reactions and multiphase processes in atmospheric aerosols. Here we demonstrate how molecular diffusion in the condensed phase affects the gas uptake and chemical transformation of semisolid organic particles. Flow tube experiments show that the ozone uptake and oxidative aging of amorphous protein is kinetically limited by bulk diffusion. The reactive gas uptake exhibits a pronounced increase with relative humidity, which can be explained by a decrease of viscosity and increase of diffusivity due to hygroscopic water uptake transforming the amorphous organic matrix from a glassy to a semisolid state (moisture-induced phase transition). The reaction rate depends on the condensed phase diffusion coefficients of both the oxidant and the organic reactant molecules, which can be described by a kinetic multilayer flux model but not by the traditional resistor model approach of multiphase chemistry. The chemical lifetime of reactive compounds in atmospheric particles can increase from seconds to days as the rate of diffusion in semisolid phases can decrease by multiple orders of magnitude in response to low temperature or low relative humidity. The findings demonstrate that the occurrence and properties of amorphous semisolid phases challenge traditional views and require advanced formalisms for the description of organic particle formation and transformation in atmospheric models of aerosol effects on air quality, public health, and climate. PMID:21690350

The Effect of Aerosol Hygroscopicity and Volatility on Aerosol Optical Properties During Southern Oxidant and Aerosol Study

NASA Astrophysics Data System (ADS)

Khlystov, A.; Grieshop, A. P.; Saha, P.; Subramanian, R.

2014-12-01

Secondary organic aerosol (SOA) from biogenic sources can influence optical properties of ambient aerosol by altering its hygroscopicity and contributing to light absorption directly via formation of brown carbon and indirectly by enhancing light absorption by black carbon ("lensing effect"). The magnitude of these effects remains highly uncertain. A set of state-of-the-art instruments was deployed at the SEARCH site near Centerville, AL during the Southern Oxidant and Aerosol Study (SOAS) campaign in summer 2013 to measure the effect of relative humidity and temperature on aerosol size distribution, composition and optical properties. Light scattering and absorption by temperature- and humidity-conditioned aerosols was measured using three photo-acoustic extinctiometers (PAX) at three wavelengths (405 nm, 532 nm, and 870 nm). The sample-conditioning system provided measurements at ambient RH, 10%RH ("dry"), 85%RH ("wet"), and 200 C ("TD"). In parallel to these measurements, a long residence time temperature-stepping thermodenuder (TD) and a variable residence time constant temperature TD in combination with three SMPS systems and an Aerosol Chemical Speciation Monitor (ACSM) were used to assess aerosol volatility and kinetics of aerosol evaporation. We will present results of the on-going analysis of the collected data set. We will show that both temperature and relative humidity have a strong effect on aerosol optical properties. SOA appears to increase aerosol light absorption by about 10%. TD measurements suggest that aerosol equilibrated fairly quickly, within 2 s. Evaporation varied substantially with ambient aerosol loading and composition and meteorology.

Influences of aerosol physiochemical properties and new particle formation on CCN activity from observation at a suburban site of China

NASA Astrophysics Data System (ADS)

Li, Yanan; Zhang, Fang; Li, Zhanqing; Sun, Li; Wang, Zhenzhu; Li, Ping; Sun, Yele; Ren, Jingye; Wang, Yuying; Cribb, Maureen; Yuan, Cheng

2017-05-01

With the aim of understanding the impact of aerosol particle size and chemical composition on CCN activity, the size-resolved cloud condensation nuclei (CCN) number concentration (NCCN), particle number size distribution (PSD) (10-600 nm), and bulk chemical composition of particles with a diameter < 1.0 μm (PM1) were measured simultaneously at Xinzhou, a suburban site in northern China, from 22 July to 26 August 2014. The NCCN was measured at five different supersaturations (SS) ranging from 0.075%-0.76%. Diurnal variations in the aerosol number concentration (NCN), NCCN, the bulk aerosol activation ratio (AR), the hygroscopicity parameter (κchem), and the ratio of 44 mass to charge ration (m/z 44) to total organic signal in the component spectrum (f44), and the PSD were examined integrally to study the influence of particle size and chemical composition on CCN activation. We found that particle size was more related to the CCN activation ratios in the morning, whereas in the afternoon ( 1400 LST), κchem and f44 were more closely associated with the bulk AR. Assuming the internal mixing of aerosol particles, NCCN was estimated using the bulk chemical composition and real-time PSD. We found that the predicted CCN number concentrations were underestimated by 20-30% at SS < 0.2% probably due to the measurement uncertainties. Estimates were more accurate at higher SS levels, suggesting that the hygroscopicity parameter based on bulk chemical composition information can provide a good estimate of CCN number concentrations. We studied the impacts of new particle formation (NPF) events on size-resolved CCN activity at the ;growth; stage and ;leveling-off; stage during a typical NPF event by comparing with the case during non-NPF event. It has been found that CCN activation was restrained at the ;growth; stage during which larger particle diameters were needed to reach an activation diameter(Da), and the bulk AR decreased as well. However, during the ;leveling

Characterization of a Quadrotor Unmanned Aircraft System for Aerosol-Particle-Concentration Measurements.

PubMed

Brady, James M; Stokes, M Dale; Bonnardel, Jim; Bertram, Timothy H

2016-02-02

High-spatial-resolution, near-surface vertical profiling of atmospheric chemical composition is currently limited by the availability of experimental platforms that can sample in constrained environments. As a result, measurements of near-surface gradients in trace gas and aerosol particle concentrations have been limited to studies conducted from fixed location towers or tethered balloons. Here, we explore the utility of a quadrotor unmanned aircraft system (UAS) as a sampling platform to measure vertical and horizontal concentration gradients of trace gases and aerosol particles at high spatial resolution (1 m) within the mixed layer (0-100 m). A 3D Robotics Iris+ autonomous quadrotor UAS was outfitted with a sensor package consisting of a two-channel aerosol optical particle counter and a CO2 sensor. The UAS demonstrated high precision in both vertical (±0.5 m) and horizontal positions (±1 m), highlighting the potential utility of quadrotor UAS drones for aerosol- and trace-gas measurements within complex terrain, such as the urban environment, forest canopies, and above difficult-to-access areas such as breaking surf. Vertical profiles of aerosol particle number concentrations, acquired from flights conducted along the California coastline, were used to constrain sea-spray aerosol-emission rates from coastal wave breaking.

Volatility Properties of Internally- and Externally-Mixed Ambient Aerosols at an Anthropogenically-influenced Forest Site in Southeastern USA

NASA Astrophysics Data System (ADS)

Khlystov, A.; Subramanian, R.

2015-12-01

Secondary organic aerosol (SOA) from biogenic sources has a significant contribution to ambient aerosol loadings in Southeastern USA and thus contributes to adverse health effects of air pollution and influences regional and global climate. Volatility properties of biogenic SOA determine its concentration, reactivity, and lifetime, but are still largely unknown. As part of a larger study to assess the effect of biogenic SOA on aerosol optical properties, a set of instruments, including scanning mobility sizers (SMPS), single particle soot photometer (SP2), and a thermodenuder, was deployed during June 2015 at a Duke Forest site near Chapel Hill, NC. The site is characterized by a significant contribution of both biogenic and urban (mostly traffic) sources. Measurements of changes in aerosol volume and optical size upon heating in the thermodenuder at different temperatures are used to derive volatility properties of the ambient aerosol. A limited set of experiments was carried out using the tandem differential mobility analysis (TDMA) approach to investigate whether the ambient aerosol at the Duke Forest site is internally mixed with respect to its volatility properties. In this presentation we will discuss equilibrium and kinetic aspects of aerosol volatility observed during this study and implications of external vs. internal mixing for derivation of bulk volatility properties of ambient aerosol.