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1.
A light scattering module has been integrated into the current AMS instrument. This module provides the simultaneous measurement of vacuum aerodynamic diameter (d va) and scattered light intensity (RLS) for all particles sampled by the AMS above ~180 nm geometric diameter. Particle counting statistics and correlated chemical ion signal intensities are obtained for every particle that scatters light. A single calibration curve converts RLS to an optical diameter (d o). Using the relationship between d va and d o the LS-AMS provides a real-time, per particle measurement of the density of the sampled aerosol particles. The current article is focused on LS-AMS measurements of spherical, non-absorbing aerosol particles. The laboratory characterization of LS-AMS shows that a single calibration curve yields the material density of spherical particles with real refractive indices (n) over a range from 1.41 < n < 1.60 with an accuracy of about ±10%. The density resolution of the current LS-AMS system is also shown to be 10% indicating that externally mixed inorganic/organic aerosol distributions can be resolved. In addition to the single particle measurements of d va and RLS, correlated chemical ion signal intensities are obtained with the quadrupole mass spectrometer. A comparison of the particle mass derived from the physical (RLS and d va) and chemical measurements provides a consistency check on the performance of the LS-AMS. The ability of the LS-AMS instrument to measure the density of ambient aerosol particles is demonstrated with sample results obtained during the Northeast Air Quality Study (NEAQS) in the summer of 2004.  相似文献   

2.
Composition, shape factor, size, and fractal dimension of soot aerosol particles generated in a propane/O2, flame were determined as a function of the fuel equivalence ratio (φ). Soot particles were first size-selected by a differential mobility analyzer (DMA) and then analyzed by an Aerodyne aerosol mass spectrometer (AMS). The DMA provides particles of known mobility diameter (dm ). The AMS quantitatively measures the mass spectrum of the nonrefractory components of the particles and also provides the vacuum aerodynamic diam eter (dva ) corresponding to the particles of known mobility diameter. The measured dm, dva , and nonrefractory composition are used in a system of equations based on the formulation presented in the companion article to estimate the particle dynamic shape factor, total mass, and black carbon (BC) content. Fractal dimension was estimated based on the mass-mobility relationship. Two types of soot particles were observed depending on the fuel equivalence ratio. Type 1: for φ < 4 (lower propane/O2), dva ; was nearly constant and independent of dm . The value of dva increased with increasing φ. Analysis of the governing equations showed that these particles were highly irregular (likely fractal aggregates), with a dynamic shape factor that increased with dm and φ. The fractal dimension of these particles was approximately 1.7. These particles were composed mostly of BC, with the organic carbon content increasing as φ increased. At φ = 1.85, the particles were about 90% BC, 5% PAH, and 5% aliphatic hydrocarbon (particle density = 1.80 g/cm3). Type 2: for φ > 4 (high propane/O2), dva was linearly proportional to dm . Analysis of the governing equations showed that these particles were nearly spherical (likely compact aggregates), with a dynamic shape factor of 1.1 (versus 1 for a sphere) and a fr actal dimension of 2.95 (3 for a sphere). These particles were composed of about 50% PAH, 45% BC, and 5% aliphatic hydrocarbons (particle density = 1.50 g/cm3). These results help interpret some measurement s obtained in recent field studies.  相似文献   

3.
4.
The effective density and volatility of particulate emissions from five gasoline direct injection (GDI) passenger vehicles were measured using a tandem differential mobility analyzer (DMA) and centrifugal particle mass analyzer (CPMA) system. The measurements were conducted on a chassis dynamometer at three steady-state operating conditions. A thermodenuder was employed to find the volatility and mixing state of the particles as well as the effective density of nascent and non-volatile particles (defined as particle phase remaining after denuding at 200°C). The mass–mobility exponent ranged between 2.4 and 2.7 for nascent (or undenuded) particles and between 2.5 and 2.7 for non-volatile particles; higher than typical diesel soot. The effective density function was 4278dm?0.438 ± 76.3 kg/m3 (for mobility diameter, dm, in nm) for nascent particles and 3215dm?0.395 ± 37.9 kg/m3 for non-volatile particles. The effective density functions of the non-volatile particles were fairly similar for the conditions studied. The uncertainty in using the effective density and mixing state data to determine the mass concentration of the aerosol by integrating mobility size distributions was examined. The uncertainty in mass concentration is minimized when only the non-volatile component is measured. However, the uncertainty in the mass concentration increases substantially if nascent particles are measured due to uncertainties in the particle mixing state and their associated effective densities. Furthermore, transient vehicle operation (cold-starts, accelerations, and decelerations) would likely change the mixing state of the exhaust particles suggesting it is difficult to accurately measure the mass concentration of undenuded GDI exhaust particulate using integrated size distribution methods.

Copyright 2015 American Association for Aerosol Research  相似文献   

5.
Particle mass analyzers, such as the aerosol particle mass analyzer (APM) and the Couette centrifugal particle mass analyzer (CPMA), are frequently combined with a differential mobility analyzer (DMA) to measure particle mass mp and effective density ρeff distributions of particles with a specific electrical mobility diameter dm. Combinations of these instruments, which are referred to as the DMA–APM or DMA–CPMA system, are also used to quantify the mass-mobility exponent Dm of non-spherical particles as well as to eliminate multiple charged particles. This study investigates the transfer functions of these setups, focusing especially on the DMA–APM system. The transfer function of the DMA–APM system was derived by multiplying the transfer functions of DMA and APM. The APM transfer function can be calculated using either the uniform or parabolic flow models. The uniform flow model provides an analytical function, while the parabolic flow model is more accurate. The resulting DMA–APM transfer functions were plotted on log(mp)-log(dp) space. A theoretical analysis of the DMA–APM transfer function demonstrated that the resolution of the setup is maintained when the rotation speed ω of APM is scanned to measure distribution. In addition, an equation was derived to numerically calculate the minimum values of the APM resolution parameter λc for eliminating multiple charged particles.

Copyright 2015 American Association for Aerosol Research  相似文献   

6.
Particle density is an important and useful property that is difficult to measure because it usually requires two separate instruments to measure two particle attributes. As density measurements are often performed on size-classified particles, they are hampered by low particle numbers, and hence poor temporal resolution. We present here a new method for measuring particle densities using our single particle mass spectrometer, SPLAT. This method takes advantage of the fact that the detection efficiency in our single particle mass spectrometer drops off very rapidly as the particle size decreases below 100 nm creating a distinct sharp feature on the small particle side of the vacuum aerodynamic size distribution. Thus, the two quantities needed to determine particle density, the particle diameter and vacuum aerodynamic diameter, are known. We first test this method on particles of known compositions and densities to find that the densities it yields are accurate. We then apply the method to obtain the densities of particles that were characterized during instrument field deployments. We illustrate how the method can also be used to measure the density of chemically resolved particles. In addition, we present a new method to characterize the instrument detection efficiency as a function of particle size that relies on measuring the mobility and vacuum aerodynamic size distributions of polydisperse spherical particles of known density. We show that a new aerodynamic lens used in SPLAT II improves instrument performance, making it possible to detect 83 nm particles with 50% efficiency.  相似文献   

7.
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 (dm), 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 (χv) and transition (χt) flow regimes can be significantly different, and these differences vary with the size of the quartz particles. For quartz, χv of small (dm < 200 nm) particles is 1.25, while χv of larger particles (dm ~ 440 nm) is 1.6, with a continuously increasing trend with particle size. In contrast, χt 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  相似文献   


8.
The Differential Mobility Analyzer (DMA) is designed to measure particle mobility diameter, which for spherical particles is equal to particle volume equivalent diameter. In contrast, the mobility diameter of aspherical particles is a function of the particle shape and orientation. The magnitude of the DMA electric fields is such that it can cause aspherical particles to align preferentially in a specific orientation. The same electric field and the sheath flow rate ( q sh ) define the particle mobility diameter. But, the fact that particle orientation depends on the electric field makes the dynamic shape factor and hence the mobility diameter depend on q sh . Here, we describe an operating procedure that relies on a tandem DMA system, in which the second DMA is operated at a number of q sh , to obtain information about particle shape by measuring the effect of particle alignment on the particle mobility diameter. We show how the relationship between the mobility diameter and q sh can even be used to physically separate particles according to their shapes. In addition we explore the use of simultaneous measurements of particle alignment and particle vacuum aerodynamic diameters to gain further information on particle shape and account for particle alignment in the calculations of dynamic shape factor. We first test this approach on doublets and compact triplets of PSL spheres, for which the orientation dependent dynamic shape factors are known. We then investigate applications on a number of polydisperse particle systems of various shapes.  相似文献   

9.
Particle aerodynamic diameter measurement using an aerosizer (a time-of-flight (TOF) particle size measurement instrument) requires assuming the density of particle being measured. In this paper, a relationship between TOF of spherical particles with different densities through three laser beams, and the lumped parameter, Log[daeCD−1/2], is found. This allows the effect of density in particle aerodynamic diameter measurement to be minimized.  相似文献   

10.

The importance of atmospheric aerosols in regulating the Earth's climate and their potential detrimental impact on air quality and human health has stimulated the need for instrumentation which can provide real-time analysis of size resolved aerosol, mass, and chemical composition. We describe here an aerosol mass spectrometer (AMS) which has been developed in response to these aerosol sampling needs and present results which demonstrate quantitative mea surement capability for a laboratory-generated pure component NH4 NO3 aerosol. The instrument combines standard vacuum and mass spectrometric technologies with recently developed aerosol sampling techniques. A unique aerodynamic aerosol inlet (developed at the University of Minnesota) focuses particles into a narrow beam and efficiently transports them into vacuum where aerodynamic particle size is determined via a particle time-of-flight (TOF) measurement. Time-resolved particle mass detection is performed mass spectrometrically following particle flash vaporization on a resistively heated surface. Calibration data are presented for aerodynamic particle velocity and particle collection efficiency measurements. The capability to measure aerosol size and mass distributions is compared to simultaneous measurements using a differential mobility analyzer (DMA) and condensation particle counter (CPC). Quantitative size classification is demonstrated for pure component NH4 NO3 aerosols having mass concentrations 0.25mu g m -3. Results of fluid dynamics calculations illustrating the performance of the aerodynamic lens are also presented and compared to the measured performance. The utility of this AMS as both a laboratory and field portable instrument is discussed.  相似文献   

11.
A new instrument, namely the 1 × 3 tandem differential mobility analyzer (1 × 3-TDMA), has been developed. Its primary measurement is the irreversibility of the hygroscopic growth factor of aerosol particles. The instrument uses the hysteresis of phase transitions to infer the solid or aqueous state of the particles. A first DMA passes particles of a selected electric mobility at relative humidity RH0. Exiting this DMA, the particles are split into three separate flows. The first flow is exposed to RH 0  → (RH 0 δ ) → RH 0 in a deliquescence test before passing through a second DMA that is set to the same electric mobility as the first DMA. The second flow passes directly to a third DMA without change in RH, thereby serving as a reference arm. This DMA is also set to the same electric mobility as the first DMA. The transmission ratio of the 1 × 3-TDMA is defined as the particle concentration passing the deliquescence test divided by that passing through the reference arm. The transmission ratio is unity in the absence of deliquescence and zero when a phase transition occurs, at least for ideal instrument performance in application to a test aerosol of fully deliquesceable particles. For the third flow passing out of the first DMA, an efflorescence test is run by using the RH profile of RH 0  → (RH 0 ? δ ) → RH 0 before passing through a fourth DMA. A full data set for the 1 × 3-TDMA is obtained by scanning RH0, typically from 20 to 85%. In the present paper, the 1 × 3-TDMA instrument is described, and laboratory data are presented for the phase transitions of externally mixed aerosols of aqueous and solid sodium chloride particles, aqueous and solid ammonium sulfate particles, and their mixtures, as well as a mixture of aqueous and solid sea salt particles. The observed transmission ratio is compared to a model analysis. The intent behind the development of this instrument is to deploy it for field measurements and use observations of the irreversibility of the growth factors of atmospheric particles as markers of their physical state.  相似文献   

12.

The deliquescence and efflorescence relative humidity values of 6- to 60-nm NaCl particles were measured using a tandem nano-Differential Mobility Analyzer. The deliquescence relative humidity (DRH) increased when the dry particle mobility diameter decreased below approximately 40 nm. The efflorescence relative humidity (ERH) similarly increased. For example, the DRH and ERH of 6-nm particles were 87% and 53%, respectively, compared to 75% and 45% for particles larger than 40 nm. Power law fits describing the nanosize effect are: DRH(d m) = 213 d m ?1.6+ 76 and ERH(d m) = 213 d m ?1.65+ 44, which are calibrated for 6 < d m < 60 nm with less than 1% RH uncertainty and where d m is the dry particle mobility diameter (nm). Two independent methods were used to generate the aerosol particles, namely by vaporizing and condensing granular sodium chloride and by electrospraying a high-purity sodium chloride aqueous solution, to investigate possible effects of impurities on the results. The DRH and ERH values were the same within experimental uncertainty for the particles generated by the two methods. The physical explanation for the nanosize effect of increasing DRH and ERH for decreasing dry particle mobility diameter is that the free energy balance of NaCl increasingly favors smaller particles (i.e., those without water) because the surface areas and hence surface free energies per particle are less for small, anhydrous particles than for bloated, aqueous particles. [Supplementary materials are available for this article. Go to the publisher's online edition of Aerosol Science and Technology for the following free supplemental resources: Graphs and data of the size distribution measurements of the deliquescence- and the efflorescence-mode experiments of the 6-, 8-, 15-, 20-, 30-, and 60-nm dry mobility diameter particles.]  相似文献   

13.
The drag force on aggregate particles of uniform spheres was measured in a Millikan apparatus as a function of Knudsen number. Our experiment was designed to study the effect of particle orientation on the slip correction factor of nonspherical particles. The velocities of charged particles in a gravitational field with and without an applied electrical field were measured. An electrical field strength of 2000 V/cm was used to align doublet and triplet particles. Results showed that an aggregate particle moved in random orientation while in the gravitational field. The same particle moved with its polar axis parallel to the electric field (doublets) or with its plane of centers parallel to the electrical field (triangular triplets). Using a nonlinear regression method, both the dynamic shape factor and slip correction factor could be determined separately from the data. The dynamic shape factors at different orientations were in good agreement with those obtained previously in a sedimentation tank. The slip correction factor of singlet particles agreed with results previously obtained by Allen and Raabe for latex particles. Slip correction factors of doublets and triangular triplets can also be expressed in the Knudsen-Weber form: 1 + 2λ/d a [1.142 + 0.558 exp(?0.999 d a/2λ)]. The adjusted sphere diameter d a was 1.21 d 1 (primary diameter) for doublets moving parallel to the flow and 1.31 d 1 for doublets randomly oriented. These results show that the slip correction factor of a nonspherical particle depends on the orientation and confirm the theory proposed by Dahneke.  相似文献   

14.
Mobility-selected fractal and non-fractal soot particles (mobility diameters d m = 135 to 310 nm) were produced at three controlled fuel equivalence ratios (φ = 2.1, 3.5, and 4.5) by an ethylene/oxygen flame. Oleic acid (liquid) and anthracene (solid) coatings were alternately applied to the particles and removed. Simultaneous measurements with an Aerodyne aerosol mass spectrometer and a scanning mobility particle sizer yielded the particle mass, volume, density, composition, dynamic shape factor, fractal dimension, surface area, and the size and number of the primary spherules forming the fractal aggregate. For a given φ, the diameters of the primary spherules are approximately the same, independent of d m (15 nm, 35 nm, and 55 nm for φ = 2.1, 3.5, and 4.5, respectively). As the coating thickness on a particle increases, the dynamic shape factor decreases but d m remains constant until the particle reaches a spherical (for oleic acid) or non-fractal but irregular (for anthracene) shape. Under some conditions, liquid oleic acid coating causes the internal BC framework to rearrange into a more compact configuration. The surface area of fractal particles is up to 2.4 times greater than that of a sphere with the same d m . Using the surface area determinations, the time for a fractal particle to obtain a monolayer of coating material is compared to that of spheres. If it is assumed that the fractal particle is a sphere with the same d m as the fractal particle, the monolayer coating time is underestimated by a factor of up to 1.7.  相似文献   

15.
Soot particle (black carbon) morphology is of dual interest, both from a health perspective and due to the influence of soot on the global climate. In this study, the mass-mobility relationships, and thus effective densities, of soot agglomerates from three types of soot emitting sources were determined in situ by combining a differential mobility analyzer (DMA) and an aerosol particle mass analyzer (APM). High-resolution transmission electron microscopy was also used. The soot sources were diesel engines, diffusion flame soot generators, and tapered candles, operated under varying conditions. The soot microstructure was found to be similar for all sources and settings tested, with a distance between the graphene layers of 3.7–3.8 Å. The particle specific surface area was found to vary from 100 to 260 m2/g. The particle mass-mobility relationship could be described by a power law function with an average exponent of 2.3 (±0.1) for sources with a volatile mass fraction <10% and primary particle sizes of 11–29 nm. The diesel exhaust from a heavy duty engine at idling had a substantially higher volatile mass fraction and a higher mass-mobility exponent of 2.6. The mass-mobility exponent was essentially independent of the number of primary particles in the range covered (Npp = 10–1000). Despite the similar exponents, the effective density varied substantially from source to source. Two parameters were found to alter the effective density: primary particle size and coating mass fraction. A correlation was found between primary particle size and mass-mobility relationship/effective density and an empirical expression relating these parameters is presented. The effects on the DMA-APM results of doubly charged particles and DMA agglomerate alignment were investigated and quantified. Finally, the dataset was compared to three theoretical approaches describing agglomerate particles’ mass-mobility relationship.

Copyright 2013 American Association for Aerosol Research  相似文献   

16.
Cavity ring-down spectroscopy (CRDS) is a technique that is commonly used to measure the extinction of light by aerosol particles in situ. This extinction, when normalized to particle concentration, yields the extinction cross section, a measure of a single particle's ability to scatter and absorb light. The complex index of refraction can then be retrieved by comparison of the extinction cross sections at several particle diameters with those predicted by Mie theory. This approach requires accurate determination of particle diameter and concentration as well as the length of the extinction region in the cavity, but it is often difficult to quantify the systematic errors in the measurements of these quantities. Here, we introduce a calibration technique using particles of a reference compound to account for these systematic errors. The two calibration parameters are: Cf , which scales the measured extinction cross sections, and Δd, which shifts the particle diameters. It is found that Cf correlates strongly with the condensation particle counter (CPC) used to measure particle concentration and that Δd is associated with the differential mobility analyzer (DMA) used to select particle diameters. Calibration is shown to reduce errors of subsequently-measured extinction cross sections of a test aerosol from 11% to with a concomitant improvement in the accuracy of the retrieved complex index of refraction and corresponding atmospheric radiative forcing estimates.

Copyright 2013 American Association for Aerosol Research  相似文献   

17.
A test impactor with a 10-μm 50% cutoff diameter at a flow rate of 7 liters/min was designed to measure particle bounce by the observed penetration to an optical counter. The effects of surface loading and relative humidity on particle bounce were determined, and a set of test criteria was developed to avoid these effects. The particle bouncing experiments were performed for ten common aerosols: ammonium fluorescein, sodium chloride, ammonium sulfate, potassium biphthalate, polystyrene latex, lycopodium spores, paper mulberry pollen, short ragweed pollen, glass beads, and Pinole soil. The differences in the fraction of bounce for different particle materials are discussed. Systematic measurements for ammonium fluorescein revealed a correlation between the fraction of particles bouncing and the particle kinetic energy and aerodynamic diameter. The EPA bounce criterion for PM 10 samplers is criticized in terms of this correlation.  相似文献   

18.
The effective density ρeff of particles emitted from various types of automobile engines was measured using a differential mobility analyzer (DMA)–aerosol particle mass analyzer method, and their morphology was investigated via transmission electron microscopy analysis. The measured exhaust particles were particles emitted from diesel engines (DEs), gasoline direct injection spark ignition (DISI) engines, gasoline port fuel injection (PFI) engines, and liquefied petroleum gas (LPG) engines. ρeff and the morphology of the particles were measured after classification with the DMA, and six electrical mobility diameters Dm ranging from 30 to 300 nm were selected. ρeff was found to decrease as Dm increased for all particles. A morphological study showed that DE and DISI particles were mainly agglomerates and PFI and LPG particles were mainly nonagglomerates. Numbers and diameters of the primary particles in the agglomerates showed no systematic differences between DE and DISI particles at a given Dm. Rather, the primary particle diameter dp increased with increasing Dm of the agglomerates; the empirical relationship between the two diameters was found to be dp = 8.498ln(Dm) – 12.781 for DE and DISI particles. The core (elemental carbon) diameters in the primary particles of the DE particles increased as Dm increased and were estimated to range from 8.5 nm for Dm = 70 nm to 22.1 nm for Dm = 300 nm. Although the primary particle diameter and core diameter depend on Dm, the organic coating (shell) thickness, which ranged from 5.1 to 7.4 nm, was found to be independent of Dm.

Copyright © 2016 American Association for Aerosol Research  相似文献   


19.
An in vitro study was conducted in the Alberta idealized child mouth-throat, which mimics average deposition in a set of nine 6–14-year-old subjects, to examine the enhancement of deposition of monodisperse uniformly charged particles as a result of induced electrostatic forces. A purpose-based atomizer was designed and built for generating monodisperse, uniformly charged particles. The atomizer generates droplets by jet break up under the action of capillary waves and charges them via electrostatic induction. The experiments cover different particle aerodynamic diameters (d a = 3.6, 4.4, and 5.9 μm), at two flow rates (Q = 10 and 20 L/min), over a wide range of elementary charges per particle (0–10,000 e). The results show substantial increases in particle deposition in the present idealized pediatric mouth throat compared to neutral aerosols. Two empirical equations, as a function of Reynolds number, Stokes number, and induced charge number are introduced for the prediction of mouth-throat deposition in children, based on two different characteristic diameters of the airway.

Copyright 2014 American Association for Aerosol Research  相似文献   


20.
We have developed a new analyzer for the online measurement of aerosol composition: a particle trap laser desorption mass spectrometer (PT-LDMS). The main components of the instrument include an aerodynamic lens, a particle trap enclosed by a quartz cell, a quadrupole mass spectrometer (QMS), a vacuum chamber incorporating the above components, and a carbon dioxide (CO2) laser (wavelength 10.6 μm). The aerodynamic lens generates a beam of submicron particles, which is focused on a small area on the particle trap. The particle trap consists of custom-made mesh layers, the structure of which was newly designed using engineering techniques for micro electro mechanical systems (MEMS). A large number of mesh frames are well arranged in the trap, and particles can be efficiently captured after multiple impactions on the frames. The CO2 laser is used to vaporize aerosol compounds captured on the particle trap. The evolved gas confined within the quartz cell is analyzed using an electron impact ionization (EI) QMS to quantify the chemical composition of the particles. The concept of the PT-LDMS and first evaluation of its performance are presented, specifically focusing on the structure and performance of the particle trap.  相似文献   

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