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The soot particle aerosol mass spectrometer (SP-AMS) instrument combines continuous wave laser vaporization with electron ionization aerosol mass spectrometry to characterize airborne, refractory black carbon (rBC) particles. The laser selectively vaporizes absorbing rBC-containing particles, allowing the SP-AMS to provide direct chemical information on the refractory and non-refractory chemical components, providing the potential to fingerprint various rBC particle types. In this study, SP-AMS mass spectra were measured for 12 types of rBC particles produced by industrial and combustion processes to explore differences in the carbon cluster (Cn+) mass spectra. TheCn+mass spectra were classified into three categories based on their ion distributions, which varied with rBC particle type. The carbon ion distributions were investigated as a function of laser power, electron ionization (on/off), and ion charge (positive or negative). Results indicate that the dominant positive ion-formation mechanism is likely the vaporization of small, neutral carbon clusters followed by electron ionization (C1+to C5+). Significant ion signal from larger carbon cluster ions (and their fragment ions in the small carbon cluster range), including mid carbon (C6+to C29+) and fullerene (greater than C30+) ions, were observed in soot produced under incomplete combustion conditions, including biomass burning, as well as in fullerene-enriched materials. Fullerene ions were also observed at high laser power with electron ionization turned off, formed via an additional ionization mechanism. We expect this SP-AMS technique to find application in the identification of the source and atmospheric history of airborne ambient rBC particles. Copyright 2015 American Association for Aerosol Research [ABSTRACT FROM AUTHOR]

We describe a robust, compact, field deployable instrument (the CAPS PMssa) that simultaneously measures airborne particle light extinction and scattering coefficients and thus the single scattering albedo (SSA) on the same sample volume. With an appropriate change in mirrors and light source, measurements have been made at wavelengths ranging from 450 to 780 nm. The extinction measurement is based on cavity attenuated phase shift (CAPS) techniques as employed in the CAPS PMexparticle extinction monitor; scattering is measured using integrating nephelometry by incorporating a Lambertian integrating sphere within the sample cell. The scattering measurement is calibrated using the extinction measurement. Measurements using ammonium sulfate particles of various sizes indicate that the response of the scattering channel with respect to measured extinction is linear to within 1% up to 1000 Mm−1and can be extended further (4000 Mm−1) with additional corrections. The precision in both measurement channels is less than 1 Mm−1(1s, 1σ). The truncation effect in the scattering channel, caused by light lost at extreme forward/backward scattering angles, was measured as a function of particle size using monodisperse polystyrene latex particles (n= 1.59). The results were successfully fit using a simple geometric model allowing for reasonable extrapolation to a given wavelength, particle index of refraction, and particle size distribution, assuming spherical particles. For sub-micron sized particles, the truncation corrections are comparable to those reported for commercial nephelometers. Measurements of the optical properties of ambient aerosol indicate that the values of the SSA of these particles measured with this instrument (0.91 ± 0.03) using scattering and extinction agreed within experimental uncertainty with those determined using extinction measured by this instrument and absorption measured using a multi-angle absorption photometer (0.89 ± 0.03) where the uncertainties are derived from best estimates of the accuracy of the two approaches. Copyright 2015 American Association for Aerosol Research [ABSTRACT FROM AUTHOR]

An inter-comparison study of instruments designed to measure the microphysical and optical properties of soot particles was completed. The following mass-based instruments were tested: Couette Centrifugal Particle Mass Analyzer (CPMA), Time-of-Flight Aerosol Mass Spectrometer—Scanning Mobility Particle Sizer (AMS-SMPS), Single Particle Soot Photometer (SP2), Soot Particle-Aerosol Mass Spectrometer (SP-AMS) and Photoelectric Aerosol Sensor (PAS2000CE). Optical instruments measured absorption (photoacoustic, interferometric, and filter-based), scattering (in situ), and extinction (light attenuation within an optical cavity). The study covered an experimental matrix consisting of 318 runs that systematically tested the performance of instruments across a range of parameters including: fuel equivalence ratio (1.8 ≤ φ ≤ 5), particle shape (mass-mobility exponent (Dfm), 2.0 ≤ Dfm ≤ 3.0), particle mobility size (30 ≤ dm≤ 300 nm), black carbon mass (0.07 ≤ mBC ≤ 4.2 fg) and particle chemical composition. In selected runs, particles were coated with sulfuric acid or dioctyl sebacate (DOS) (0.5 ≤ Δrve≤ 201 nm) where Δrve is the change in the volume equivalent radius due to the coating material. The effect of non-absorbing coatings on instrument response was determined. Changes in the morphology of fractal soot particles were monitored during coating and denuding processes and the effect of particle shape on instrument response was determined. The combination of optical and mass based measurements was used to determine the mass specific absorption coefficient for denuded soot particles. The single scattering albedo of the particles was also measured. An overview of the experiments and sample results are presented. [ABSTRACT FROM AUTHOR]

Particulate emission indices (per kg fuel) have been determined by sampling the advected plumes of in-use commercial aircraft at two different airports using a novel approach. Differences are observed in the number, magnitude, and composition of the particle emissions between idle and take-off. At the first airport, Electrical Low Pressure Impactor (ELPI) data indicate that number based emission indices (EI n ) vary by an order of magnitude for take-off plumes from different aircraft. Additionally, EI n values for idle plumes are greater than take-off. At the second airport, EI n values derived from condensation particle counter (CPC) measurements span ∼⃒ an order of magnitude (3–50 × 10 15 particles per kg fuel). The median values of the idle and take-off plumes were 1.8 × 10 16 and 7.6 × 10 15 particles per kg fuel, respectively. For take-off plumes, the magnitude of the particulate emission index is not correlated with NO x at either airport. The surface properties of the particulate emissions in take-off and idle plumes differ significantly as measured by diffusion charging (DC) and photoelectric aerosol sensor (PAS) instruments. Results indicate that take-off plumes are characterized by particles with photoelectric-active surfaces, presumably elemental carbon, whereas idle plumes are composed of non-photoelectric-active constituents and coated soot particles. Measurements of the particulate size distribution (ELPI) show evidence for two modes, one at ∼⃒ 90 nm aerodynamic diameter and a second mode at or below the instrument cutoff ( [ABSTRACT FROM AUTHOR]

This article presents a validation study of the stochastic particle-resolved aerosol model PartMC with experimental data from an aerosol chamber experiment. For the experiment, a scanning mobility particle sizer and a single-particle soot photometer were used to monitor the aerosol mixing state evolution of two initially externally mixed aerosol populations of ammonium sulfate and black carbon particles undergoing agglomeration. We applied an efficient optimization algorithm (ProSRS) to determine several unconstrained simulation parameters and were able to successfully reproduce number concentrations and size distributions of mixed particles that formed by agglomeration. The PartMC modeling approach in conjunction with the optimization procedure provides a tool for detailed comparisons of chamber experiments and modeling, where aerosol mixing state is the focus of investigation. Copyright © 2019 American Association for Aerosol Research [ABSTRACT FROM AUTHOR]

An important source of uncertainty in radiative forcing by absorbing aerosol particles is the uncertainty in their morphologies (i.e., the location of the absorbing substance on/in the particles). To examine the effects of particle morphology on the response of an individual black carbon-containing particle in a Single-Particle Soot Photometer (SP2), a series of experiments was conducted to investigate black carbon-containing particles of known morphology using Regal black (RB), a proxy for collapsed soot, as the light-absorbing substance. Particles were formed by coagulation of RB with either a solid substance (sodium chloride or ammonium sulfate) or a liquid substance (dioctyl sebacate), and by condensation with dioctyl sebacate, the latter experiment forming particles in a core-shell configuration. Each particle type experienced fragmentation (observed as negative lagtimes), and each yielded similar lagtime responses in some instances, confounding attempts to differentiate particle morphology using current SP2 lagtime analysis. SP2 operating conditions, specifically laser power and sample flow rate, which in turn affect the particle heating and dissipation rates, play an important role in the behavior of particles in the SP2, including probability of fragmentation. This behavior also depended on the morphology of the particles and on the thermochemical properties of the non-RB substance. Although these influences cannot currently be unambiguously separated, the SP2 analysis may still provide useful information on particle mixing states and black carbon particle sources. Copyright 2015 American Association for Aerosol Research [ABSTRACT FROM PUBLISHER]

We report a positive matrix factorization (PMF) analysis of organic particulate material (PM) emissions of aircraft engine exhaust that includes data from five different aircraft engines and two different fuels (petroleum jet fuel and a Fischer-Tropsch fuel) collected over three field missions. PMF of aerosol mass spectrometer (AMS) data was used to identify six distinct factors: two lubrication oil factors, two aliphatic factors, an aromatic factor, and a siloxane factor. Of these, the lubrication oil factors and the siloxane factor were noncombustion sources. The siloxane factor was attributed to silicone tubing used in the sampling system deployed in one of the three missions included in this study, but not the other two. The two lubrication oil factors correlate with the two different lubrication oils used by the aircraft engines evaluated in this study (Mobil II and Air BP) as well as minor differences presumably due to variation in the blend stocks, temperature history, and analytical factors. Overall, the sum of the aliphatic and aromatic factors decreased with increasing power, as expected based on known trends in VOC emissions. The aliphatic #1 factor correlated with soot emissions, especially at power conditions where EIm-soot was greater than 30 mg kg?1. The aliphatic factor #2 mass spectrum shared some similarities with ambient aerosol organic PM present during the tests and correlated most strongly with dilution levels, two observations that suggest that aliphatic #2 contains components found in ambient aerosol. The aromatic factor correlated with benzene emissions, especially at low power conditions were EIm-benzene was greater than 0.03 mg kg?1. Our results improve the current understanding of aircraft PM composition. Copyright 2014 American Association for Aerosol Research [ABSTRACT FROM PUBLISHER]

The optical properties of soot particles in plumes emanating from a high bypass turbofan aircraft engine (V2527) were measured at distances of 40-80 m behind the engine with a cavity-enhanced phase shift (CAPS)-based extinction monitor (known as the CAPS PMex) and a multi-angle absorption photometer, both operating at wavelength ∼630 nm. Integrated plume measurements from the two instruments were highly correlated with each other (r2 > 0.99, N = 12) and with measured carbon dioxide emission concentrations. Ancillary measurements indicated that the soot particle volume-weighted mobility diameter distribution peaked at 60 nm with a full width at half maximum of ∼60 nm. The soot single scattering albedo determined using the absorption and extinction measurements under engine idle conditions was 0.05 ± 0.02 (where the uncertainty represents 2σ precision), in agreement with previous measurements of aircraft exhaust. The engine soot emission index (mass soot per mass fuel burned) for this particular engine, derived from these measurements and a wavelength-specific mass absorption coefficient and the measured in-plume carbon dioxide concentrations, was 225 ± 35 mg kg-1 at engine idle conditions. These results plus more limited data collected from in-use aircraft on the runway indicate that the CAPS extinction monitor can provide (with an appropriate albedo correction) a credible measurement of the engine soot emission index in situations where the time response and sensitivity of particle absorption monitors are not otherwise sufficient. [ABSTRACT FROM AUTHOR]

We present laboratory and field measurements of aerosol light extinction (σep) using an instrument that employs Cavity Attenuated Phase Shift (CAPS) spectroscopy. The CAPS extinction monitor comprises a light emitting diode (LED), an optical cavity that acts as the sample cell, and a vacuum photodiode for light detection. The particle σep is determined from changes in the phase shift of the distorted waveform of the square-wave modulated LED light that is transmitted through the optical cell. The 3-σ detection limit of the CAPS monitor under dry particle-free air is 3 Mm-1 for 1s integration time. Laboratory measurements of absolute particle extinction cross section (σext) using non-absorbing, monodisperse polystyrene latex (PSL) spheres are made with an average precision of ± 3% (2-σ) at both 445 and 632 nm. A comparison with Mie theory scattering calculations indicates that these results are accurate within the 10% uncertainty stated for the particle number density measurements. The CAPS extinction monitor was deployed twice in 2009 to test its robustness and performance outside of the laboratory environment. During these field campaigns, a co-located Multi Angle Absorption Photometer (MAAP) provided particle light absorption coefficient (σap) at 635 nm: the single scattering albedo (ω) of the ambient aerosol particles was estimated by combining the CAPS σep measured at 632 nm with the MAAP σap data. Our initial results show the high potential of the CAPS as lightweight, compact instrument to perform precise and accurate σep measurements of atmospheric aerosol particles in both laboratory and field conditions. [ABSTRACT FROM AUTHOR]

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%). [ABSTRACT FROM AUTHOR]

A fluidized bed aerosol generator has been designed and built for the purpose of generating a constant output of dry, submicrometer particles with a large number density. The output of the fluidized bed for generating aerosol particles from dry soot powder has been characterized using a differential mobility analyzer and a condensation particle counter. The particle size distribution is bimodal, with a mode in the submicrometer diameter size range and a mode in the supermicrometer diameter size range. The larger diameter mode is fully separated from the smaller mode and can thus be easily removed from the aerosol flow using impaction techniques. The distribution in the submicrometer size range is nearly log-normal, with a count median diameter falling between 0.1 and 0.3 micrometers. A number density of greater than 10[sup 5] particles cm[sup -3] of soot particles in the submicrometer range can be produced, constant to within 25% (1 standard deviation) over a 4 h time period. The number density of particles produced in the submicrometer range was found to vary with the ratio of soot to bronze beads in the bed mixture, whether or not a feed system was used, and nitrogen flow rate through the fluidized bed and feed system. [ABSTRACT FROM AUTHOR]

We report the development and validation of a new humidified aerosol single-scattering albedometer to quantify the effects of water uptake on submicrometer particle optical properties. The instrument simultaneously measures in situ aerosol light extinction (σep) and scattering (σsp) using a cavity-attenuated phase shift-single scattering albedo particulate matter (PM) monitor (CAPS-PMSSA, Aerodyne Research, Inc., Billerica, MA, USA). It retrieves by difference aerosol light absorption (σap) and directly quantifies aerosol single-scattering albedo (SSA), the aerosol "brightness." We custom built a relative humidity (RH) control system using a water vapor-permeable membrane humidifier and coupled it to the CAPS-PMSSA to enable humidified aerosol observations. Our humidified instrument (H-CAPS-PMSSA) overcomes problems with noise caused by mirror purge-flow humidification, heating, and characterizing cell RH. Careful angular truncation corrections in scattering, particularly for larger particles, were combined with empirical observations. Results show that the optimal operational size to be Dp < 400 nm. The H-CAPS-PMSSA was evaluated with several pure single-component aerosols including ammonium sulfate ((NH4)2SO4), absorbing nigrosin, and levoglucosan, an organic biomass smoke tracer. The measured σep, σsp, and the derived optical hygroscopicity parameter (κ) for size-selected ammonium sulfate are in good agreement with literature values. For dry size-selected nigrosin in the 100 < Dp < 400 nm range, SSA values increased from ∼0.3 to 0.65 with increasing Dp. The enhancement in nigrosin σap at RH = 80% was a factor of 1.05–1.20 relative to dry conditions, with the larger particles showing greater enhancement. SSA increased with RH with the largest fractional enhancement measured for the smallest particles. For polydisperse levoglucosan, we measured an optical κ of 0.26 for both light extinction and scattering and negligible absorption. Our new instrument enables reliable observations of the effects of ambient humidity on mixed aerosol optical properties, particularly for light-absorbing aerosols whose climate forcing is uncertain due to measurement gaps. Copyright © 2021 American Association for Aerosol Research [ABSTRACT FROM AUTHOR]

The Aerodyne Soot Particle Aerosol Mass Spectrometer (SP-AMS) can operate with one or both of two particle vaporizers: (1) the standard resistively heated tungsten vaporizer (TV) for detection of non-refractory particulate matter (NR-PM), and (2) an intracavity laser vaporizer (LV) for detection of absorbing, refractory materials, including refractory black carbon (rBC), metal nanoparticles, and associated coatings. In addition to using these vaporizers individually, both can be used simultaneously (dual vaporizer, DV, mode), commonly implemented by sequentially turning the laser vaporizer on (DV-Lon) and off (DV-Loff). Recent results in DV mode have shown an apparent enhancement in measured NR-PM signal during DV-Lon compared with DV-Loff, even for inorganic species unlikely to be strongly associated with rBC. The use of dual vaporizers is complicated by different collection efficiencies (CE) of the two vaporizers, potential differences in the relative ionization efficiencies (RIE) for the same species vaporized from the two vaporizers, and potential interference between the two vaporizers due to laser heating of AMS internal components. Here, we investigated the effect of the laser-heating interference on NR-PM signal. We tested a variety of laser baffles to minimize laser-heating interferences and to constrain the alignment of the laser vaporizer and we identified a baffle that meets these criteria and can be incorporated into SP-AMS systems. For well aligned standard and laser vaporizers, laser heating was found to have only a minor effect on the NR-PM ion signals. Most of the observed increases in NR-PM signals during DV-Lon are attributed to vaporizer-specific differences in the CE and RIE values of NR-PM associated with the rBC-containing particles. Copyright © 2020 American Association for Aerosol Research [ABSTRACT FROM AUTHOR]

Mass concentrations calculated from Aerodyne's aerosol mass spectrometers depend on particle collection efficiency (CE) and relative ionization efficiency (RIE, relative to the primary calibrant ammonium nitrate). We present new laboratory RIE measurements for a wide range of organic aerosol species (RIEOA). An improved laboratory RIE calibration protocol with size and mass selection of calibrant particles and a light scattering-based detection of CE is used. Simpler calibrations of alcohol RIEs using binary mixtures with NH4NO3 are demonstrated. Models that account for only thermal velocity and electron ionization of vaporized molecules do not reproduce RIEOA measurements, confirming that other processes are significant. The relationship between RIEOA and average carbon oxidation state (), a metric used to describe atmospheric OA, is investigated. An average RIEOA of 1.6 ± 0.5 (2σ) is found for −1.0 < < 0.5, a range consistent with most ambient OA except hydrocarbon-like organic aerosol (HOA) and cooking organic aerosol (COA). RIEOA from 2 to 7 are found for below and above this range. The RIEOA typically used for ambient OA (1.4 ± 0.3) is within the laboratory RIEOA measurement uncertainty of oxidized organic species, but is a factor of 2 to 5 lower than that of reduced species. Such biases in OA mass concentrations have not been observed in published field analyses. Chemically reduced ambient OA may have composition, phase states, or compensating CE effects that are not mimicked well in the laboratory. This work highlights the need for further ambient OA studies to better constrain the composition dependence of ambient RIEOA, and the need to always calibrate with the OA under study for laboratory experiments. Copyright © 2018 American Association for Aerosol Research [ABSTRACT FROM AUTHOR]

An evaluation of the operation and performance of a Cavity Attenuated Phase-Shift Particle Extinction Monitor (CAPS PMex) was performed for use on board commercial aircraft as part of the research infrastructure IAGOS (In-service Aircraft for a Global Observing System,www.iagos.org). After extensive laboratory testing, a new flow system, using mass flow controllers, was installed to maintain constant purge and sample flows under low and varying pressure conditions. The instrument was then tested for pressures as low as 200 hPa and evaluated against particle-free compressed air and CO2. Extinction coefficients for the studied gases were in close agreement with literature values with differences between 2.2% and 8%, proving that the CAPS technology works at low pressures. The instrument's limit of detection, with respect to 3 times the variability of the background signal for the full pressure range, was 0.2 Mm−1for 60s integration time. During its first research aircraft operations, the IAGOS instrument prototype, composed of one CAPS PMex and one OPC, showed excellent results regarding the stability of the instruments and the potential for characterizing different aerosol types and for estimating the contribution of sub- and super-μm sized particles to aerosol light extinction. Copyright © 2017 American Association for Aerosol Research [ABSTRACT FROM AUTHOR]

The Aerodyne Aerosol Chemical Speciation Monitor (ACSM) is well suited for measuring non-refractory particulate matter up to approximately 1.0 µm in aerodynamic diameter (NR-sub-PM1). However, for larger particles the detection efficiency is limited by losses in the sampling inlet system and through the standard aerodynamic focusing lens. In addition, larger particles have reduced collection efficiency due to particle bounce at the vaporizer. These factors have limited the NR-sub-PM1ACSM from meeting PM2.5(particulate matter with aerodynamic diameter smaller than 2.5 µm) monitoring standards. To overcome these limitations, we have redesigned the sampling inlet, the aerodynamic lens, and particle vaporizer. Both the new lens and vaporizer are tested in the lab using a quadruple aerosol mass spectrometer (QAMS) system equipped with light scattering module. Our results show that the capture vaporizer introduces additional thermal decomposition of both inorganic and organic compounds, requiring modifications to the standard AMS fragmentation table, which is used to partition ion fragments to chemical classes. Experiments with mixed NH4NO3and (NH4)2SO4particles demonstrated linearity in the NH4+ion balance, suggesting that there is no apparent matrix effect in the thermal vaporization-electron impact ionization detection scheme for mixed inorganic particles. Considering a typical ambient PM2.5size distribution, we found that 89% of the non-refractory mass is detected with the new system, while only 65% with the old system. The NR-PM2.5system described here can be adapted to existing Aerodyne Aerosol Mass Spectrometer (AMS) and ACSM systems. Copyright © 2017 American Association for Aerosol Research [ABSTRACT FROM PUBLISHER]

We present measurements of traffic-related pollutants made near the Long Island Expressway (LIE, I-495), in Queens, New York. The Aerodyne Research Inc. (ARI) mobile laboratory (AML) was deployed to map spatial and temporal gradients of gas-phase species and particulate matter (PM) associated with vehicular exhaust in the residential areas near the LIE. We observe that pollutant levels build up during the early morning hours under stable boundary layer conditions yet fall off quickly within 150 m downwind of the highway. An ARI soot particle aerosol mass spectrometer (SP-AMS) provided measurements of the size-resolved chemical composition of refractory black carbon (rBC) and the associated coating species. The average size distribution of the traffic related PM is characterized by a rBC mode centered at ∼100 nm in vacuum aerodynamic diameter, D va (rBC mass fraction ∼50%). A second rBC mode (rBC mass fraction ∼5%) more heavily coated with organic material is also observed at D va ∼500 nm. Positive matrix factorization (PMF) analyses of the traffic-related PM indicates that rBC is mostly associated with hydrocarbon-like organic (HOA) PM. These results are discussed in the context of chemically resolved size distributions and PMF analysis results performed on the SP-AMS stationary data collected at the Queens College site. Finally, we report emission indices (EI) for both fleet-average conditions and single vehicles, including several New York City Metropolitan Transit Authority (MTA) buses, sampled by the AML in “chase” mode during the study. Copyright 2012 American Association for Aerosol Research [ABSTRACT FROM PUBLISHER]

A photo-acoustic absorption spectrometer (PAS) and a cavity ring down aerosol extinction spectrometer (CRD-AES) were used, in conjunction with Mie Theory, to measure the refractive index (RI) of absorbing polystyrene spheres (APSS). The PAS and CRD-AES were also used to measure the absorption and extinction enhancement after these APSS were coated in oleic acid. The experimental enhancements were then compared to predictions from coated-sphere Mie Theory. The measured absorption and extinction enhancements both agreed with modeled enhancements to within an average of 5%. A filter-based absorption technique (particle soot absorption photometer, PSAP) was also used to measure the absorption by the APSS and showed a significant size-dependent bias, as evidenced by the filter-based method measuring significantly lower absorption for both uncoated and coated APSS compared to the PAS. These results suggest the validity of applying photo-acoustics to measure the absorption enhancement created by semi-volatile atmospheric species coating absorbing particles. [ABSTRACT FROM AUTHOR]

We report evidence that carbon impregnated conductive silicone tubing used in aerosol sampling systems can introduce two types of experimental artifacts: (1) silicon tubing dynamically absorbs carbon dioxide gas, requiring greater than 5 minutes to reach equilibrium and (2) silicone tubing emits organic contaminants containing siloxane that are adsorbed onto particles traveling through it and onto downstream quartz fiber filters. The consequence can be substantial for engine exhaust measurements as both artifacts directly impact calculations of particulate mass-based emission indices. The emission of contaminants from the silicone tubing can result in overestimation of organic particle mass concentrations based on real-time aerosol mass spectrometry and the off-line thermal analysis of quartz filters. The adsorption of siloxane contaminants can affect the surface properties of aerosol particles; we observed a marked reduction in the water-affinity of soot particles passed through conductive silicone tubing. These combined observations suggest that the silicone tubing artifacts may have wide consequence for the aerosol community and the tubing should, therefore, be used with caution. Contamination associated with the use of silicone tubing was observed at ambient temperature and, in some cases, was enhanced by mild heating (<70°C) or pre-exposure to a solvent (methanol). Further evaluation is warranted to quantify systematically how the contamination responds to variations in system temperature, physicochemical particle properties, exposure to solvent, sample contact time, tubing age, and sample flow rates. [ABSTRACT FROM AUTHOR]

Mobility-selected fractal and non-fractal soot particles (mobility diameters dm = 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 dm (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 dm 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 dm. 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 dm as the fractal particle, the monolayer coating time is underestimated by a factor of up to 1.7. [ABSTRACT FROM AUTHOR]

The size-dependent particle transmission efficiency of the aerodynamic lens system used in the Aerodyne Aerosol Mass Spectrometer (AMS) was investigated with computational fluid dynamics (CFD) calculations and experimental measurements. The CFD calculations revealed that the entire lens system, including the aerodynamic lens itself, the critical orifice which defines the operating lens pressure, and a valve assembly, needs to be considered. Previous calculations considered only the aerodynamic lens. The calculations also investigated the effect of operating the lens system at two different sampling pressures, 7.8 × 104 Pa (585 torr) and 1.0 × 105 Pa (760 torr). Experimental measurements of transmission efficiency were performed with size-selected diethyl hexyl sebacate (DEHS), NH4NO3, and NaNO3 particles on three different AMS instruments at two different ambient sampling pressures (7.8 × 104 Pa, 585 torr and 1.0 × 105 Pa, 760 torr). Comparisons of the measurements and the calculations show qualitative agreement, but there are significant deviations which are as yet unexplained. On the small size end (30 nm to 150 nm vacuum aerodynamic diameter), the measured transmission efficiency is lower than predicted. On the large size end (> 350 nm vacuum aerodynamic diameter) the measured transmission efficiency is greater than predicted at 7.8 × 104 Pa (585 torr) and in good agreement with the prediction at 1.0 × 105 Pa (760 torr). [ABSTRACT FROM AUTHOR]

A light scattering module has been integrated into the current AMS instrument. This module provides the simultaneous measurement of vacuum aerodynamic diameter (dva) 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 (do). Using the relationship between dva and do 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 dva 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 dva) 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. [ABSTRACT FROM AUTHOR]

Inter-comparison studies of well-characterized fractal soot particles were conducted using the following four instruments: Aerosol Mass Spectrometer-Scanning Mobility Particle Sizer (AMS-SMPS), Single Particle Soot Photometer (SP2), Multi-Angle Absorption Photometer (MAAP), and Photoacoustic Spectrometer (PAS). These instruments provided measurements of the refractory mass (AMS-SMPS), incandescent mass (SP2) and optically absorbing mass (MAAP and PAS). The particles studied were in the mobility diameter range from 150 nm to 460 nm and were generated by controlled flames with fuel equivalence ratios ranging between 2.3 and 3.5. The effect of organic coatings (oleic acid and anthracene) on the instrument measurements was determined. For uncoated soot particles, the mass measurements by the AMS-SMPS, SP2, and PAS instruments were in agreement to within 15%, while the MAAP measurement of optically-absorbing mass was higher by ~50%. Thin organic coatings (~10 nm) did not affect the instrument readings. A thicker (~50 nm) oleic acid coating likewise did not affect the instrument readings. The thicker (~60 nm) anthracene coating did not affect the readings provided by the AMS-SMPS or SP2 instruments but increased the reading of the MAAP instrument by ~20% and the reading of the PAS by ~65%. The response of each instrument to the different particle types is discussed in terms of particle morphology and coating material. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]