Facile Method for Determining the Aspect Ratios of Mineral Dust Aerosol by Electron Microscopy

Mineral dust is the second largest atmospheric emission by mass and one of the least understood sources. The shape of the particles depends on their composition and has implications for particle optical properties and reactive surface area. Mineral dust particles are often approximated as spheroids to model their optical properties. In this study, scanning electron microscopy (SEM) is used to measure the aspect ratios of calcite, quartz, NX-illite, kaolinite (KGa-1b and KGa-2), and montmorillonite (STx-1b and SWy-2). In addition to traditional SEM images of the top of the particles, the SEM substrates are oriented approximately normal to the electron beam in order to image the side of the particles. In this manner, aspect ratios for the top and side orientation of the particles are determined. Calcite particles have an aspect ratio of approximately 1.3 in both orientations, while quartz particles have an aspect ratio of 1.38 in the top orientation and 1.64 in the side orientation. The clay minerals studied all exhibited plate-like structures with aspect ratios of 1.35 to 1.44 for the top orientation and 4.80 to 9.14 for the side orientation. These values are used to estimate the specific surface areas (SSAs) of the minerals, which are compared to Brunauer-Emmett-Teller (BET) surface area measurements. Through this study, we present a simple method for determining the aspect ratios of aerosolized samples, rather than relying on literature values of model systems. As a result, this technique should provide a better method for determining the optical properties of mineral dust particles.

Copyright 2014 American Association for Aerosol Research     

An artifact-minimizing method for total dust sampling and chemical characterization of industrial high-temperature aerosols

Conventional methods for total dust sampling from industrial high-temperature aerosols containing condensable species, e.g., in boilers of municipal solid waste incinerators (MSWI), are always influenced by condensation artifacts. Therefore, we extended the scope of a previously developed probe intended for size-fractionated aerosol sampling with reduced artifacts and employed it for total dust measurements. The dust is collected on quartz fiber filters, which are gravimetrically evaluated and chemically analyzed by energy dispersive X-ray spectroscopy and wet-chemical methods. First measurements in the boiler of an MSWI confirm that the probe is also suitable for artifact-minimized total dust sampling. The data are consistent with results from measurements with the size-fractionating method conducted in parallel. By combining the results of both sampling methods, we reveal the average chemical composition of the submicron particles in the aerosol, which is not accessible by one of the two methods alone.

© 2017 American Association for Aerosol Research     

Single Particle Measurements of the Optical Properties of Small Ice Crystals and Heterogeneous Ice Nuclei

Dust aerosol and ice crystals are two major types of nonspherical particles in the atmosphere which have significant roles in cloud-aerosol interactions and the radiative budget. The presence of dust and ice often coincide in the atmosphere because dust particles are efficient ice nuclei. The size and composition dependence of the scattering properties of dust and ice are needed to assess their individual contributions to the optical scattering of sunlight. Here we present a new measurement technique used to determine the single particle forward scattering, backscattering, and depolarization ratio (at a wavelength of 680 nm) for representative nonspherical atmospheric particles. The Texas A&M University Continuous Flow Diffusion Chamber (CFDC) was used as an ice crystal generator to produce ice crystals via both homogenous and heterogeneous nucleation mechanisms under well-controlled laboratory conditions. Optical scattering properties of mineral dusts and small ice crystals (0.6 μm to 50 μm optical diameter) were measured by the Droplet Measurement Technologies, Inc. (DMT) Cloud Aerosol Spectrometer with Polarization (CASPOL). Significant differences between the optical properties of single dusts and ice particles of the same size were observed. Differences between the optical signatures of homogeneously and heterogeneously nucleated ice crystals were not statistically significant. Our results suggest that atmospheric ice crystals can be identified and quantified independently from the dust particles on which they form based on analysis of their backscatter and depolarization signals.

Copyright 2014 American Association for Aerosol Research     

Sensitivity of Aerosol Refractive Index Retrievals Using Optical Spectroscopy

Accurate refractive index values are required to determine the effects of aerosol particles on direct radiative forcing. Theoretical retrievals using extinction data alone or extinction plus absorption data have been simulated to determine the sensitivity of each retrieval. A range of aerosol types with a range of different refractive indices were considered. The simulations showed that the extinction-only retrieval was not able to accurately or precisely retrieve refractive index values, even for purely scattering compounds, but the addition of a simulated absorption measurement greatly improved the retrieval.

Copyright 2014 American Association for Aerosol Research     

Detachment of adhered particles from a cloth surface subjected to a rod strike

A mechanical impulse can cause adhered particles to detach from a surface. For various purposes, particle detachment may need to be enhanced or restricted. Unlike rigid solids, cloth material can be deformed or bent by a mechanical impulse. However, neither the cloth deformation nor the induced turbulent airflow has been well studied. This investigation experimentally measured the detachment of Arizona test dust (ATD) from cloth segments. The vertical margins of each cloth segment were fastened to a frame, and the cloth surface with the ATD adhered to the reverse side was struck with a rod. The cloth motion, induced airflow, and particle detachment were recorded by a high-speed camera. In addition, the displacement and acceleration of the cloth were monitored with a laser distance sensor. The mass percentages of detached particles from the cloth and the particle residual were weighed. Several factors that affected particle detachment were compared. The results revealed that the particle detachment was caused by a combination of the vibrating motion of the cloth surface, the hydrodynamic action of the induced turbulent airflows, and the particle agglomeration when the cloth was bent. A strike could even leave fewer residual particles when a much higher surface dust load had initially adhered to the cloth.

Copyright © 2019 American Association for Aerosol Research     

Assessing the accuracy of complex refractive index retrievals from single aerosol particle cavity ring-down spectroscopy

Cavity ring-down spectroscopy (CRDS) of single, optically manipulated aerosol particles affords quantitative retrieval of refractive indices for particles of fixed or evolving composition with high precision. Here, we quantify the accuracy with which refractive index determinations can be made by CRDS for single particles confined within the core of a Bessel laser beam and how that accuracy is degraded as the particle size is progressively reduced from the coarse mode (>1 μm radius) to the accumulation mode (<500 nm radius) regime. We apply generalized Lorenz–Mie theory to the intra-cavity standing wave to explore the effect of particle absorption on the distribution of extinction cross section determinations resulting from stochastic particle motion in the Bessel beam trap. The analysis provides an assessment of the accuracy with which the real, n, and imaginary, κ, components of the refractive index can be determined for a single aerosol particle.

Published with license by American Association for Aerosol Research     

Characteristics of traffic-induced fugitive dust from unpaved roads

The characteristics of fugitive dust emitted from vehicles traveling on unpaved dirt roads were measured using a suite of instruments including a real-time fugitive dust sampler. The fugitive dust sampler is formed from a combination of a large particle inlet and an optical particle spectrometer that reports particle sizes from 6 to 75 µm. The large particle inlet permits the sampling of particles up to 75 µm with only a moderate dependence of sampling efficiency on wind-speed. Measurements made with the sampler showed that particles as large as ～50 µm were suspended from vehicular movement on the dirt roads, with the mode of the fugitive dust particle number size distribution ～2 µm, while the mass distribution mode was ～7 µm. A comparison of the fugitive dust sampler measurements with those made using standard PM instruments showed that the conventional instruments have a wind-direction bias that can result in under-sampling of large particles. The current measurements suggest that particles suspended from dirt roadways are of importance for local air quality within the near-road environment.

Copyright © 2017 American Association for Aerosol Research     

Measurement of size-dependent dynamic shape factors of quartz particles in two flow regimes

Understanding and modeling the behavior of quartz dust particles, commonly found in the atmosphere, requires knowledge of many relevant particle properties, including particle shape. This study uses a single particle mass spectrometer, a differential mobility analyzer, and an aerosol particle mass analyzer to measure quartz aerosol particles mobility (d_m), vacuum aerodynamic, and volume equivalent diameters, mass, composition, effective density, and dynamic shape factor as a function of particle size, in both the free molecular and transition flow regimes. The results clearly demonstrate that dynamic shape factors can vary significantly as a function of particle size. For the quartz samples studied here, the dynamic shape factors increase with size, indicating that larger particles are significantly more aspherical than smaller particles. In addition, dynamic shape factors measured in the free-molecular (χ_v) and transition (χ_t) flow regimes can be significantly different, and these differences vary with the size of the quartz particles. For quartz, χ_v of small (d_m < 200 nm) particles is 1.25, while χ_v of larger particles (d_m ～ 440 nm) is 1.6, with a continuously increasing trend with particle size. In contrast, χ_t of small particles starts at 1.1 increasing slowly to 1.34 for 550 nm diameter particles. The multidimensional particle characterization approach used here goes beyond determination of average properties for each size, to provide additional information about how the particle dynamic shape factor may vary even for particles with the same mass and volume equivalent diameter.

© 2016 American Association for Aerosol Research     

Observations of a Correlation Between Primary Particle and Aggregate Size for Soot Particles

For decades, soot has been modeled as fractal-like aggregates of nearly equiaxed spherules. Cluster–cluster aggregation simulations, starting from a population of primary particles, give rise to structures that closely match real aerosols of solid particles produced in flames. In such simulations, primary particle size is uncorrelated with aggregate size, as all aggregates contain primary particles drawn from the same population. Aerosol measurements have been interpreted with this geometric model. Examination of transmission electron micrographs of soot samples from various sources shows that primary particle sizes are not well mixed within an aerosol population. Larger aggregates tend to contain larger primary particles and the variation in size is much larger between aggregates than within aggregates. The soot sources considered here are all substantially not well-mixed (aircraft jet engine, inverted diffusion flame, gasoline direct injection engine, heavy-duty compression ignition engine). The observed variations in primary particle size can be explained if soot aggregates are formed and grew by coagulation in small zones of the combustion chamber, prior to dilution and transport (with minimal coagulation) to the sampling system.

Copyright 2014 American Association for Aerosol Research     

Differential diffusion analyzer

In this article, a proof of concept of a new measurement instrument, differential diffusion analyzer (DDA), is established. The DDA enables the measurement of the size distribution of sub-10 nm aerosol particles, and it can also be used as a size classifier to separate a certain particle size from a size distribution for subsequent analysis. The developed technique is based on the diffusion separation of different size particles. Thus, the main advantage of the DDA compared to other methods is that particle charging is not required. Simulated and experimentally measured transmission efficiencies show that the diffusion-based differential size classification is a feasible concept, and moreover, shows that particle size is inversely proportional to the square root of the total flow rate.

Copyright © 2017 American Association for Aerosol Research     

Simulating aerosol chamber experiments with the particle-resolved aerosol model PartMC

This article presents a verification and validation study of the stochastic particle-resolved aerosol model PartMC. Model verification was performed against self-preserving analytical solutions, while for validation three experiments were performed where the size distribution evolution of coagulating ammonium sulfate particles was measured in a cylindrical stainless steel chamber. To compare with the chamber measurements, PartMC was extended to include the representation of fractal particle structure and wall loss. This introduced five unknown parameters to the governing equation, which were determined by a combination of scanning electron microscopy (SEM) analysis and an objective optimization procedure. Excellent agreement between modeled and measured size distributions was achieved using the same set of parameters for all three experiments. Assuming spherical particles led to model results that were inconsistent with the measurements. The best agreement between model and measurement was obtained for the fractal dimension of 2.3, indicating that the non-spherical structure of the particle agglomerates in the chamber needed to be taken into account.

© 2017 American Association for Aerosol Research     

Dominant environmental parameters for dust deposition and resuspension in desert climates

Field studies of dry deposition usually measure dust accumulation over periods of days or weeks. However, long measurement periods obscure the effects of meteorological conditions on the deposition rate. Previously we developed an “outdoor soiling microscope” (OSM) in order to measure dust deposition and detachment every 10 min in the field. In this study a greased/ungreased pair of OSMs was deployed for 51 days in the desert climate of Doha, Qatar. Stepwise regression analysis was performed to quantify the explanatory power of meteorological parameters on dust deposition and detachment rates. It was found that wind speed dominated deposition and rebound of dust particles, and produced a distinctive “threshold” response in deposition. The dry deposition results were highly consistent with a model by Kim et al. (2000) derived from outdoor experiments. By comparison, relative humidity and particulate matter concentration had less influence on dust flux rates.

Copyright © 2018 American Association for Aerosol Research     

Adhesion of Dust Particles to Common Indoor Surfaces in an Air-Conditioned Environment

Adhesion between dust particles and indoor surfaces can lead to negative effects on human health by triggering allergic and asthmatic reactions. In this study, adhesion forces of indoor office dust and activated carbon (AC, as model soot) particles to four common indoor materials (Al, Cu, PVC, and glass) were measured by colloidal probe atomic force microscopy. Chemical analysis of office dust shows it is largely made up of oxygenated hydrophilic organic carbon material. Both metal surfaces experienced weaker dust and AC adhesion than PVC or glass by up to 2–12 times lower primarily due to the presence of attractive electrostatic forces in the latter two (non-conducting) surfaces. Dust and AC adhesion were also highly sensitive to surface roughness, with an inverse relationship between adhesion force and roughness due to the reduction in contact area between the particle and a rougher material surface. Capillary forces play only a minor or negligible role in dust and AC surface adhesion. Adhesion models utilizing a purely van der Waals approach such as the simple Hamaker model and modified Rumpf's model are insufficient to determine the actual particle-surface contact radii and requires the accounting of non-van der Waals forces to adhesion.

Copyright 2014 American Association for Aerosol Research     

Molecular-resolution simulations of new particle formation: Evaluation of common assumptions made in describing nucleation in aerosol dynamics models

Aerosol dynamics models that describe the evolution of a particle distribution incorporate nucleation as a particle formation rate at a small size around a few nanometers in diameter. This rate is commonly obtained from molecular models that cover the distribution below the given formation size – although in reality the distribution of nanometer-sized particles cannot be unambiguously divided into separate sections of particle formation and growth. When incorporating nucleation, the distribution below the formation size is omitted, and the formation rate is assumed to be in a steady state. In addition, to reduce the modeled size range, the formation rate is often scaled to a larger size based on estimated growth and scavenging rates and the assumption that also the larger size is in a steady state. This work evaluates these assumptions by simulating sub-10 nm particle distributions in typical atmospheric conditions with an explicit molecular-resolution model. Particle formation is included either (1) dynamically, that is, the whole size range starting from single vapor molecules is modeled explicitly or (2) implicitly by using an input formation rate as is done in aerosol models. The results suggest that while each assumption can affect the outcome of new particle formation modeling, the most significant source of uncertainty affecting the formation rates and resulting nanoparticle concentrations is the steady-state assumption, which may lead to an overprediction of the concentrations by factors of approximately from two to even orders of magnitude. This can have implications for modeling and predicting atmospheric particle formation.

Copyright © 2017 American Association for Aerosol Research     

An integrative model for the filtration efficiencies in realistic tests with consideration of the filtration velocity profile and challenging particle size distribution

Many well-established models can be applied to calculate the filtration efficiencies. In these models the filtration velocity and challenging particle size are assumed to be known accurately. However, in realistic filtration tests, the filtration velocity has profiles dependent on the filter holder geometry and experimental conditions; the challenging particles have size distributions dependent on the instruments and operation conditions. These factors can potentially affect the measured filtration efficiency and lead to discrepancies with the models.

This study aims to develop an integrative model to predict the filtration efficiencies in realistic tests by incorporating the effects of the filtration velocity profile and challenging particle size distribution classified by a differential mobility analyzer (DMA) into the existing filtration models. Face velocity profile is modeled with fluid mechanics simulations; the initial generated particle size distribution, the particle charging status and the DMA transfer function are modeled to obtain the challenging particle size distribution. These results are then fed into the filtration models. Simulated results are compared with experimental ones to verify the model accuracy. This model can be used to reduce filtration test artifacts and to improve the experimental procedure.

The results reveal that the face velocity upstream the filter exhibits high degree of homogeneity not affecting the filtration efficiency if the filter pressure drop is not very low. The generated particle size distribution and the DMA selection size window could influence the challenging particle size distribution and therefore the measured filtration efficiency.

Copyright © 2017 American Association for Aerosol Research     

Infrared Optical Constants of Organic Aerosols: Organic Acids and Model Humic-Like Substances (HULIS)

Aerosols are important atmospheric constituents as they impact the Earth's energy balance and climate. An analysis of the impact of aerosols depends on the detailed knowledge of aerosol optical properties. However, there is a lack of refractive index data for atmospherically relevant organic compounds in the infrared (IR) region which complicates the quantitative estimation of the aerosol influence on the radiative balance. In this study, we investigate the optical properties of atmospherically relevant carboxylic acids and HUmic-LIke Substances (HULIS) proxies. Aerosol size distributions are measured simultaneously with Fourier transform infrared (FTIR) extinction spectra to calculate the complex refractive index. Scanning electron microscopy (SEM) images are also collected to investigate particle shape. Analysis of SEM images shows evidence for agglomeration in some cases. The experimentally measured IR resonances do not appear to be highly sensitive to agglomeration effects. However, there is an increase in the scattering efficiency at shorter wavelengths as the result of larger overall particle size of the agglomerates. Refractive indices are retrieved from the IR extinction spectra of organic acids and HULIS proxies. Mie simulation results confirm the quality of the retrieved optical constants. Interestingly, the optical constants determined for the acids are in agreement with the published data for fire smoke plumes.

Copyright 2014 American Association for Aerosol Research     

Comparison of the relative performance efficiencies of melt-blown and glass fiber filter media for managing fine particles

The purpose of this study was to compare the performance efficiency of melt-blown and currently used glass fiber filter media under the same environmental conditions. To evaluate filter efficiency, filter class was determined according to ISO and European standards (EN 1822-1:2009) using an automated filter tester (0.3 μm size), taking into account particle filtration, fractional efficiency for negative pressure devices, and consumption of electrical power. The average fractional efficiency, quality factor (QF), fractional efficiency by dust loading amount, pressure by dust loading amount, and QF by dust loading amount were higher in the case of melt-blown media than in the case of glass fiber filters. The fractional efficiency of hydrocharged melt-blown filters was higher than that of uncharged media. Based on performance efficiency, melt-blown filters are more effective high efficiency particulate air filters than glass fiber media.

Copyright © 2018 American Association for Aerosol Research     

Development of an aerosol mass spectrometer lens system for PM2.5

The aerodynamic lens system of the Aerodyne Aerosol Mass Spectrometer (AMS) was analyzed using the Aerodynamic Lens Calculator. Using this tool, key loss mechanisms were identified, and a new lens design that can extend the transmission of particulate matter up to 2.5 μm in diameter (PM2.5) was proposed. The new lens was fabricated and experimentally characterized. Test results indicate that this modification to the AMS lens can significantly improve the transmission of large sized particles, successfully achieving a high transmission efficiency up to PM2.5 range.

© 2016 American Association for Aerosol Research     

Direct radiative impacts of desert dust on atmospheric water content

The direct and indirect radiative impact of naturally produced dust particles influences climate from regional to global scale, introducing one of the largest uncertainties in future climate projections. By absorbing and scattering solar radiation, aerosols reduce the amount of energy reaching the earth's surface, while at the same time they enhance the greenhouse effect by absorbing and emitting longwave radiation (direct dust effect). In this study an attempt is made to quantify the feedback of this energy redistribution in the atmospheric water content in the Arabian Peninsula (one of the main sources of atmospheric mineral dust globally). To this end the SKIRON/dust modeling system was used for 2 years (2014–2015) and two sets of simulations were performed: in the first one the dust particles exert no feedback on the radiative transfer due to dust particles (control run), while in the second set dust interacts with radiation (direct radiative effect). Both simulations have been evaluated in their ability to describe the impacts on surface humidity, with the simulations including the dust feedback showing improved results. These direct feedbacks lead to an increase in the mass of water in the atmospheric column that can reach a maximum daily average of 0.5 g per kg of dry air. Water vapor is the most important greenhouse gas and through this process dust enhances its own greenhouse effect, further increasing the surface temperature and humidity, making life difficult for people living in an already harsh desert climate.

© 2018 American Association for Aerosol Research