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The Aerodyne Aerosol Mass Spectrometer (AMS) is a useful tool to study ambient particles. To be quantitative, the mass or (number) of particles detected by the AMS relative to the mass (or number) of particles sampled by the AMS, or the AMS collection efficiency (CE), must be known. Here we investigated the effect of particulate phase on AMS CE for ammonium nitrate, ammonium sulfate, mixed ammonium nitrate/ammonium sulfate, and ammonium sulfate particles coated with an organic liquid. Dry, solid ammonium sulfate particles were sampled with a CE of 24 ± 3%. Liquid droplets and solid particles that were thickly coated with a liquid organic were collected with a CE of 100%. Mixed phase particles, solid particles thinly coated with liquid organic, and metastable aqueous ammonium sulfate droplets had intermediate CEs. The higher CEs for liquid particles compared with solid particles were attributed to wet or coated particles tending to stick upon impact with the AMS vaporizer, while a significant fraction of solid particles bounced prior to vaporization/detection. The consistency of single particle signals indicated that the phase (and hence CE) of mixed component particles did not affect the AMS sensitivity to a particular chemical species once volatilization occurred. Particle phase might explain a significant fraction of the variable AMS CEs reported in the literature. For example, ambient particles that were liquid (e.g., composition dominated by ammonium nitrate or acidic sulfate) have been reported to be sampled with 100% CE. In contrast, most ambient particle measurements report CEs of < 100% (typically~ 50%).  相似文献   

3.

The Aerodyne Aerosol Mass Spectrometer (AMS) provides size-resolved chemical composition of non-refractory (vaporized at 600°C under vacuum) submicron aerosols with a time resolution of the order of minutes. Ambient measurements were performed in Tokyo between February 2003 and February 2004. We present intercomparisons of the AMS with a Particle-Into-Liquid Sampler combined with an Ion Chromatography analyzer (PILS-IC) and a Sunset Laboratory semi-continuous thermal-optical carbon analyzer. The temperature of the AMS inlet manifold was maintained at > 10 ? C above the ambient dew point to dry particles in the sample air (relative humidity (RH) in the inlet < 53%). Assuming a particle collection efficiency of 0.5 for the AMS, the mass concentrations of inorganic species (nitrate, sulfate, chloride, and ammonium) measured by the AMS agree with those measured by the PILS-IC to within 26%. The mass concentrations of organic compounds measured by the AMS correlate well with organic carbon (OC) mass measured by the Sunset Laboratory carbon analyzer (r 2 = 0.67–0.83). Assuming the same collection efficiency of 0.5 for the AMS organics, the linear regression slope is found to be 1.8 in summer and 1.6 in fall. These values are consistent with expected ratios of organic matter (OM) to OC in urban air.  相似文献   

4.
Incense burning is a common ritual in Asian communities both indoors in residential homes and outdoors in temple premises. Organic particles from burning of incense sticks, incense coils, and mosquito coils after extensive dilution (>1000×) were characterized by the Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). The obtained mass spectra in general resemble those reported for biomass burning aerosols. Ion peaks with m/z values higher than 100 accounted for 15%–25% of the organic signals in the unit-mass-resolution (UMR) mass spectra. In the high-resolution (HR) mass spectra, the ion peaks at m/z 60 and 73 are found to be related to the sugar anhydrides as in particles from other biomass burning processes. In addition, the ion peaks at m/z 107, 121, 137, 151, 167, and 181, some of which (e.g., m/z 137 and 167) have been observed in particles from biomass burning but not yet assigned, were assigned to lignin-related components. Elemental analysis from the HR data reveals that a large portion of particulate organics from incense burning are oxygenated (O/C between 0.3 and 0.5) and unsaturated (and/or cyclic) in nature. Results from this study also highlight that mass spectra from HR-ToF-AMS measurements concerning primary emissions such as incense burning contain very useful information in the high m/z (>100) region about the chemical characteristics of those primary organic particles.

Copyright 2012 American Association for Aerosol Research  相似文献   

5.
In recent years, Aerodyne aerosol mass spectrometers (AMS) have been used in many locations around the world to study the size-resolved, nonrefractory chemical composition of ambient particles. In order to obtain quantitative data, the mass or (number) of particles detected by the AMS relative to the mass (or number) of particles sampled by the AMS, i.e., the AMS collection efficiency (CE) must be known. Previous studies have proposed and used parameterizations of the AMS CE based on the aerosol composition and sampling line relative humidity. Here, we evaluate these parameterizations by comparing AMS mass concentrations with independent measurements of fine particle volume or particle-into-liquid sampler (PILS) ion chromatography measurements for 3 field campaigns with different dominant aerosol mixtures: (1) acidic sulfate particles, (2) aerosol containing a high mass fraction of ammonium nitrate, and (3) aerosol composed of primarily biomass burning emissions. The use of the default CE of 0.5 for all campaigns resulted in 81–90% of the AMS speciated and total mass concentrations comparing well with fine particle volume or PILS measurements within experimental uncertainties, with positive biases compared with a random error curve. By using composition-dependent CE values (sometimes as a function of size) which increased the CE for the above aerosol types, the fraction of data points within the measurement uncertainties increased to more than 92% and the mass concentrations decreased by ~5–15% on an average. The CE did not appear to be significantly dependent on changes in organic mass fraction although it was substantial in the 3 campaigns (47, 30, and 55%).

Copyright 2012 American Association for Aerosol Research  相似文献   

6.
The collection efficiency (CE) of the aerosol mass spectrometer (AMS) for chamber-generated secondary organic aerosol (SOA) at elevated mass concentrations (range: 19–207 μg m?3; average: 64 μg m?3) and under dry conditions was investigated by comparing AMS measurements to scanning mobility particle sizer (SMPS), Sunset semi-continuous carbon monitor (Sunset), and gravimetric filter measurements. While SMPS and Sunset measurements are consistent with gravimetric filter measurements throughout a series of reactions with varying parent hydrocarbon/oxidant combinations, AMS CE values were highly variable ranging from unity to <15%. The majority of mass discrepancy reflected by low CE values does not appear to be due to particle losses either in the aerodynamic lens system or in the vacuum chamber as the contributions of these mechanisms to CE are low and negligible, respectively. As a result, the largest contribution to CE in the case of chamber-generated SOA appears to be due to particle bounce at the vaporizer surface before volatilization, which is consistent with earlier studies that have investigated the CE of ambient and select laboratory-generated particles. CE values obtained throughout the series of reactions conducted here are also well correlated with the f 44/f 57 ratio, thereby indicating both that the composition of the organic fraction has an important impact on the CE of chamber-generated SOA and that this effect may be linked to the extent to which the organic fraction is oxidized.

Copyright 2013 American Association for Aerosol Research  相似文献   

7.

Aerodynamic lens inlets have revolutionized aerosol mass spectrometry by allowing the introduction of a very narrow particle beam into a vacuum chamber for subsequent analysis. The real-time measurement of particle beam width after an aerodynamic lens is of interest for two reasons: (1) it allows a correction to be made to the measured particle concentration if the beam is so broad, due to poor focusing by non-spherical particles, that some particles miss the detection system; and (2) under constant lens pressure it can provide a surrogate particle non-sphericity measurement. For these reasons, a beam width probe (BWP) has been designed and implemented for the Aerodyne Aerosol Mass Spectrometer (AMS), although this approach is also applicable to other instruments that use aerodynamic lens inlets. The probe implemented here consists of a thin vertical wire that can be precisely positioned to partially block the particle beam at fixed horizontal locations in order to map out the width of the particle beam. A computer model was developed to optimize the BWP and interpret its experimental data. Model assumptions were found to be reasonably accurate for all laboratory-generated particle types to which the model was compared. Comparisons of particle beam width data from a number of publications are also shown here. Particle losses due to beam broadening are found to be minor for the AMS for both laboratory and ambient particles. The model was then used to optimize the choice of the BWP dimensions, and to guide its use during continuous operation. A wire diameter approximately 1.55 times larger than the beam width to be measured provides near optimal sensitivity toward both collection efficiency and surrogate non-sphericity information. Wire diameters of 0.62 mm and 0.44 mm (for the AMS “long” and “short” chambers, respectively) provide reasonable sensitivity over the expected range of particle beam widths, for both spherical and non-spherical particles. Three other alternative BWP geometries were also modeled and discussed.  相似文献   

8.
By means of a newly designed portable aerosol mass spectrometer SPLAT (Single Particle Laser Ablation Time-of-flight mass spectrometer) for the analysis of single atmospheric aerosol particles we investigated the system performance in dependency on two different aerodynamic lenses (Liu and Schreiner type) capable of focusing particles with diameters ranging from 80 nm to 800 nm and 300 nm to 3000 nm, respectively. By using the pressure regulated Schreiner lens, the instrument is independent of variations in atmospheric pressure which would lead to changing dynamical properties of the aerosol particles. Active pressure control inside the inlet system facilitates airborne measurements without complicated corrections. With the Liu setup no pressure regulation was used. Here the overall efficiency of our instrument was 7% while with the Schreiner setup 2% was achieved. The Liu lens setup is optimal for measuring submicron particles at low particle concentrations. To detect supermicron particles the Schreiner lens setup is favored. Together with these experiments we present key details of the SPLAT setup and its characterization. Our instrument is able to measure simultaneously the size and the chemical composition of individual aerosol particles larger than 300 nm in diameter. It uses forward scattered light of single aerosol particles at two positions to determine their vacuum aerodynamic diameter from the flight time between the two lasers. Chemical analysis of the particles is done by laser ablation mass spectrometry utilizing a bipolar time-of-flight mass spectrometer.  相似文献   

9.
The Feldberg Aerosol Characterization Experiment (FACE-2004) took place from July 13–August 4, 2004 at the Taunus Observatory on the “Kleiner Feldberg” (825 m a.m.s.l.) in Central Germany. The experiment included (amongst others) size-resolved chemical characterization of non-refractory aerosol components. One of the experiment's objectives was to better understand and to characterize recently developed aerosol measurement instrumentation by intercomparison with other co-located instruments. One of these instruments was the Aerodyne Time-of-Flight Aerosol Mass Spectrometer (ToF-AMS).

Here we compare the datasets obtained by the ToF-AMS with those obtained by the well-characterized co-located Quadrupole Aerosol Mass Spectrometer (Q-AMS). A good agreement between the recently developed ToF-AMS with the established Q-AMS is reported here for all species measured with the two instruments for a time period where both instruments operated under well-calibrated conditions. During measurements with reduced detector gain after a pump failure changed species concentrations were measured with the ToF-AMS that did not agree with those measured with the Q-AMS. These changes were different for the individual species and could be attributed to the influence of the ion detection threshold as was shown by model calculations.

For efficient and user-friendly processing of ToF-AMS raw data a data processing software package was developed. Since this is the first time this software was used for field data, it is described in some detail here.  相似文献   

10.
Two pressure-controlled inlets (PCI) have been designed and integrated into the Aerodyne Aerosol Mass Spectrometer (AMS) inlet system containing an aerodynamic aerosol lens system for use in airborne measurements. Laboratory experiments show that size calibration and mass flow rate into the AMS are not affected by changes in upstream pressure (P 0 ) of the PCI as long as the pressure within the PCI chamber (P PCI ) is controlled to values lower than P 0 . Numerous experiments were conducted at different P PCI , P 0 , and AMS lens pressures (P Lens ) to determine particle transmission efficiency into the AMS. Based on the results, optimum operating conditions were selected which allow for constant pressure sampling with close to 100% transmission efficiency of particles in the size range of ~ 100–700 nm vacuum aerodynamic diameter (d va ) at altitudes up to ~ 6.5 km. Data from an airborne field study are presented for illustration.  相似文献   

11.
A large experimental study has been conducted to make definitive measurements of the aspiration efficiencies of idealized cylindrical thin-walled aerosol samplers in perfectly calm air, using a method that involved the direct visual observation of falling streams of particles of well-defined size for sampling under specific conditions of sampling flowrate and orientation (downwards facing and horizontal). These data augment an earlier set of experimental data for upwards-facing sampling, and those results are included again in this article for the sake of completeness. In addition to the experimental study, a numerical study was also carried out, first for the purpose of comparison with the experimental results in ranges where such results are available, and second for providing information in ranges where experiments could not be conducted satisfactorily. From this combined approach, a very comprehensive set of new data was generated. In general, the experimental and numerical results were seen to be in very good agreement for the ranges of conditions where data were obtained using both methods. For all cases it was shown in general that aspiration efficiency decreases with increasing Stokes' number (representing inertial forces) but increases with decreasing ratio of particle settling velocity to sampling inlet velocity (representing gravitational forces). From all the data it was seen that the detailed relationship between aspiration efficiency for the various sampler orientations is different for various particle inertia regimes. In the small Stc regime, aspiration efficiency is highest for upwards-facing sampling, with that for downwards-facing and horizontal sampling being about the same. In the intermediate Stc regime, aspiration efficiency for horizontal sampling is greater than for downwards facing, which in turn is greater than for upwards facing. In the large Stc regime, aspiration efficiency for upwards-facing sampling is greater than for horizontal, which in turn is greater than aspiration efficiency for downwards facing.  相似文献   

12.

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   

13.
A new mode of operation for the Aerodyne Quadrupole Aerosol Mass Spectrometer (Q-AMS) has been developed and used to improve the detection limits and time resolution of the instrument. The Jump Mass Spectrum (JMS) mode works by stepping through a small number of specific user defined positions within the mass spectrum, increasing the time spent scanning specific m/z's . The JMS mode is conceptually similar to the “Selected Ion Monitoring” mode of some commercial quadrupole-based instrumentation and can be used for direct quantification when the fragmentation pattern is known. The JMS mode can also be used to augment the standard Q-AMS operation in Mass Spectrum mode when the fragmentation pattern is not known, improving the effective signal-to-noise ratio (SNR) and in turn the detection limits and time resolution. A decrease in detection limits for the Q-AMS by factors of 4.6, 3.9, 1.3, and 3.5 for nitrate, sulphate, total organics, and m/z 43 mass loadings respectively was achieved for 1 minute sampling (20 s in each of the three Q-AMS modes, monitoring 10 m/z in JMS mode). Although the benefit to the SNR of the total organic mass concentration measured by the Q-AMS is smaller, sensitivity to organic fragments which can act as markers for various sources and processes (such as fresh primary anthropogenic emissions, aged secondary organics, and biomass burning aerosol), is greatly increased by the JMS mode. Example data from applications that benefit from this technique are presented, including an aircraft platform and in smog chamber experiments, alongside high time-resolution, ground-based data.  相似文献   

14.
Aerodyne Aerosol Mass Spectrometers (AMS) are routinely operated with a constant vaporizer temperature (Tvap) of 600°C in order to facilitate quantitative detection of non-refractory submicron (NR-PM1) species. By analogy with other thermal desorption instruments, systematically varying Tvap may provide additional information regarding NR-PM1 chemical composition and relative volatility, and was explored during two ambient studies. The performance of the AMS generally and the functional integrity of the vaporizer were not negatively impacted during vaporizer temperature cycling (VTC) periods. NR-PM1 species signals change substantially as Tvap decreases with that change being consistent with previous relative volatility measurements: large decreases in lower volatility components (e.g., sulfate, organic aerosol [OA]) with little, if any, decrease in higher volatility components (e.g., nitrate, ammonium) as Tvap decreases. At Tvap < 600°C, slower evaporation was observed as a shift in particle time-of-flight distributions and an increase in “particle beam blocked” (background) concentrations. Some chemically reduced (i.e., CxHy+) OA ions at higher m/z are enhanced at lower Tvap, indicating that this method may improve the analysis of some chemically reduced OA systems. The OA spectra changes dramatically with Tvap; however, the observed trends cannot easily be interpreted to derive volatility information. Reducing Tvap increases the relative O:C and CO2+, contrary to what is expected from measured volatility. This is interpreted as continuing decomposition of low volatility species that decreases more slowly (as Tvap decreases) than does the evaporation of reduced species. The reactive vaporizer surface and the inability to reach Tvap much below 200°C of the standard AMS limit the ability of this method to study the volatility of oxidized OA species.

Copyright 2015 American Association for Aerosol Research  相似文献   

15.
A combination of a differential mobility analyzer (DMA) and aerosol particle mass analyzer (APM) is used to measure the mass of NIST Standard Reference Materials (SRM®) PSL spheres with 60 and 100 nm nominal diameter, and NIST traceable 300 nm PSL spheres. The calibration PSL spheres were previously characterized by modal diameter and spread in particle size. We used the DMA to separate the particles with modal diameter in a narrow mobility diameter range. The mass of the separated particles is measured using the APM. The measured mass is converted to diameter using a specific density of 1.05. We found that there was good agreement between our measurements and calibration modal diameter. The measured average modal diameters are 59.23 and 101.2 nm for nominal diameters of 60 and 100 nm (calibration modal diameter: 60.39 and 100.7 nm) PSL spheres, respectively. The repeatability uncertainty of these measurements is reported. For 300 nm, the measured diameter was 305.5 nm, which is an agreement with calibration diameter within 1.8%.

The effect of spread in particle size on the APM transfer function is investigated. Two sources of the spread in “mono-dispersed” particle size distributions are discussed: (a) spread due to the triangular DMA transfer function, and (b) spread in the calibration particle size. The APM response function is calculated numerically with parabolic flow through the APM and diffusion broadening. As expected from theory, the calculated APM response function and measured data followed a similar trend with respect to APM voltage. However, the theoretical APM transfer function is narrower than the measured APM response.  相似文献   

16.
Aerodynamic particle sizer (APS) users typically calibrate the particle sizing capabilities, but not the counting efficiency upon which aerosol concentration results are based. Herein, comparisons were made between the counts provided by an ink jet aerosol generator (IJAG) with those measured by an APS. Near-monodisperse (geometric standard deviation of about 1.06) liquid or solid aerosols in the size range of 0.95 to 13.3 μm aerodynamic diameter (AD) generated with an IJAG were released into the inner inlet-tube of the APS in a manner that rendered APS wall and aspiration losses negligible. For most experiments, the IJAG generated 75 particles/s, which rate was maintained by the IJAG system through control of electrical pulses applied to its ink jet cartridge. For particles in the size range of 2–13.3 μm AD, the ratio of relative detection efficiency (ratio of the number of particles counted by the APS to the number reported as generated by the IJAG) was 99.3 ± 1.4%; however, for test particles between 0.95 and 2 μm AD, the relative detection efficiency was somewhat lower, but the drop off was less than about 2%. This slight drop off is likely associated with the light scattering detection approach and corresponding counting algorithm of the APS. Tests were conducted where the IJAG produced 7.0 μm AD particles at rates of 1 to 500 s-1 and the results showed essentially a 1:1 correspondence between IJAG and APS counts. The presence of smaller-sized background particles did not affect the measured APS counts of larger-sized challenge particles.

Copyright 2014 American Association for Aerosol Research  相似文献   


17.
The inlet of a commercial atmospheric pressure chemical ionization—mass spectrometer (APCI/MS/MS) has been modified to transform it into an aerosol mass spectrometer, named TD-API-AMS. The new inlet consists in a charcoal denuder (to trap gas phase VOCs and SVOCs) followed by the thermal-desorption unit of the APCI source. Thermal desorption and APCI were chosen because they avoid sample denaturizing while keeping good time resolution. The objectives of this paper are (1) to describe the simple and reversible modifications of the commercial APCI inlet allowing its use as an aerosol mass spectrometer and (2) to characterize the performances of this modified inlet. These performances are characterized in term of efficiency of (i) gas phase organic compounds removal, (ii) particle transmission, and (iii) particle volatilization in the thermal-desorption unit. The characterization was conduced with secondary organic aerosol (SOA) produced from the ozonolysis of α -pinene and 2-buten-1-ol in a continuous flow reactor. The results show a denuder gas phase trapping efficiency higher than 93 ± 3% while the particle transmission efficiency was nearly 100% in particle number, but decreased to as little as 85% in total particle volume. This result highlights a shift of the particle distribution towards the fine particles occurring through the denuder, due to a modification of the gas-particle equilibrium. The inlets' characterization has also shown a particle volatilization efficiency higher than 90% (in volume).  相似文献   

18.
The development of a thermal desorption chemical ionization ion trap mass spectrometer for the chemical characterization of ultrafine aerosol particles is reported and first experimental results are presented. Atmospheric particles are size-classified and collected using a unipolar charger, a radial differential mobility analyzer and an electrostatic precipitator, and analyzed after thermal desorption and chemical ionization using an ion trap mass spectrometer. Integration of an ion trap mass spectrometer allows for fast scans of the entire mass spectrum every 0.5 s and bears the potential to identify unknown particulate compounds by tandem mass spectrometry. Particle collection efficiencies range from 90–100% for 25 nm particles to about 50% for 40 nm particles. In the current configuration, the absolute sensitivity of the instrument with regard to ammonium is in the range of 10–100 pg NH + 4 . In ambient samples collected in the Colorado Front Range, NH + 4 was the major signal peak in the positive ion spectrum, and additional minor signals and peak patterns of organic compounds including methylamine were found.  相似文献   

19.
The creation of liquid-gas dispersions places very high demands on the process technology, which requires knowledge of bubble formation mechanisms. To extend the range of validity of the current calculation models to larger viscosity differences, the bubble formation mechanisms for the media combination oil/air are investigated. Compared to the media combination water/air, significant differences occur. The results obtained here will make it possible to design bubble columns in a more targeted manner in the future, which will lead to savings in resources and energy of industrial test stands.  相似文献   

20.
For nanoparticles with nonspherical morphologies, e.g., open agglomerates or fibrous particles, it is expected that the actual density of agglomerates may be significantly different from the bulk material density. It is further expected that using the material density may upset the relationship between surface area and mass when a method for estimating aerosol surface area from number and mass concentrations (referred to as “Maynard's estimation method”) is used. Therefore, it is necessary to quantitatively investigate how much the Maynard's estimation method depends on particle morphology and density. In this study, aerosol surface area estimated from number and mass concentration measurements was evaluated and compared with values from two reference methods: a method proposed by Lall and Friedlander for agglomerates and a mobility based method for compact nonspherical particles using well-defined polydisperse aerosols with known particle densities. Polydisperse silver aerosol particles were generated by an aerosol generation facility. Generated aerosols had a range of morphologies, count median diameters (CMD) between 25 and 50 nm, and geometric standard deviations (GSD) between 1.5 and 1.8. The surface area estimates from number and mass concentration measurements correlated well with the two reference values when gravimetric mass was used. The aerosol surface area estimates from the Maynard's estimation method were comparable to the reference method for all particle morphologies within the surface area ratios of 3.31 and 0.19 for assumed GSDs 1.5 and 1.8, respectively, when the bulk material density of silver was used. The difference between the Maynard's estimation method and surface area measured by the reference method for fractal-like agglomerates decreased from 79% to 23% when the measured effective particle density was used, while the difference for nearly spherical particles decreased from 30% to 24%. The results indicate that the use of particle density of agglomerates improves the accuracy of the Maynard's estimation method and that an effective density should be taken into account, when known, when estimating aerosol surface area of nonspherical aerosol such as open agglomerates and fibrous particles.  相似文献   

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