Soot Particle Studies—Instrument Inter-Comparison—Project Overview

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 ( D _fm ), 2.0 ≤ D _fm ≤ 3.0), particle mobility size (30 ≤ d _m ≤ 300 nm), black carbon mass (0.07 ≤ m _BC ≤ 4.2 fg) and particle chemical composition. In selected runs, particles were coated with sulfuric acid or dioctyl sebacate (DOS) (0.5 ≤ Δ r _ve ≤ 201 nm) where Δ r _ve 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.     

An inter-comparison of black-carbon-related instruments in a laboratory study of biomass burning aerosol

Black carbon (BC)-containing particles are the most strongly light absorbing aerosols in the atmosphere. Measurements of BC are challenging because of its semi-empirical definition based on physical properties and not chemical structure, the complex and continuously changing morphology of the corresponding particles, and the effects of other particulate components on its absorption. In this study, we compare six available commercial continuous instruments measuring BC using biomass burning aerosol. The comparison involves a Soot Particle Aerosol Mass Spectrometer (SP-AMS), a Single-Particle Soot Photometer (SP2), an aethalometer, a Multiangle Absorption Photometer (MAAP), and a blue and a green photoacoustic extinctiometer (PAX). An SP-AMS collection efficiency equal to 0.35 was measured for this aerosol system. The corrected SP-AMS BC mass measurements agreed within 6% with the SP2 refractory BC mass values. Two regimes of behavior were identified for the optical instruments corresponding to high and low organic/BC ratio. The mass absorption cross-sections (MAC) measured varied from 26% to two times the instrument default values depending on the instrument and the regime. The presence of high organic aerosol concentration in this system can lead to overestimation of the BC mass by the optical instruments by as much as a factor of 2.7. In general, the discrepancy among the BC measurements increased as the organic carbon content of the BC-containing particles increased.

© 2018 American Association for Aerosol Research     

Effects of Mixing State on Black Carbon Measurements by Laser-Induced Incandescence

Laboratory experiments and theoretical calculations were made to characterize the performance of a Single Particle Soot Photometer (SP2) manufactured by Droplet Measurement Technologies (DMT), which was designed to measure the mass and the mixing state of individual black carbon (BC) or elemental carbon (EC) particles, based on the laser-induced incandescence (LII) technique. In this study, graphite was used as a surrogate of EC. Graphite particles with mass equivalent diameters of 110–200 nm were layered with organic liquids (glycerol and oleic acid) to produce coated graphite with diameters up to 650–800 nm. These were sampled by the SP2 to measure the waveforms (i.e., time development) of the LII and scattering signals. The peak temperature and the peak LII signal of graphite particles were independent of the coating thickness or the coating material to within experimental errors. These results indicate that the mass of EC can be measured by using peak LII signal without interference by the coating conditions. It was also shown that the difference between the times of the scattering and LII peaks can be used as an indicator of coating on EC with thicknesses larger than about 100–200 nm. LII and scattering waveforms were calculated using a newly developed theoretical model that takes into account the physical processes controlling the temperature and evaporation rate of the coated graphite particle in the laser beam. The calculations reproduced the general features of observed waveforms of LII and scattering signals, providing a firm theoretical basis for the interpretation of the SP2 data.     

Effects of volatile coatings and coating removal mechanisms on the morphology of graphitic soot

We have measured morphological changes of combustion-generated mature soot with various quantities of hydrocarbon coating and different coating-removal mechanisms. We made these measurements on soot extracted from a burner and then (1) coated with oleic acid, (2) coated with oleic acid and then denuded using a thermodenuder, (3) coated with oleic acid and then heated with a laser, and (4) coated with oleic acid, denuded with a thermodenuder, and then laser heated. We compared these results to results for untreated soot from the burner. The soot samples were size selected using a differential mobility analyzer prior to coating. Uncoated, coated, and denuded particles were characterized by electric-mobility size, particle and coating mass, and particle morphology. Our results show that the particles are restructured (become compact) when coated. Particles sent through the thermodenuder are irreversibly restructured. Laser desorption of coatings with thicknesses ⩾20% by mass, however, returns the soot particles to a less compact morphology with some fragmentation as the coating rapidly vaporizes. A majority of laser-heated heavily coated particles stay associated with unvaporized oleic acid droplets despite some fragment ejection from the droplet. Thermally denuded particles neither return to a less compact morphology nor fragment when laser heated.     

Coating Mass Dependence of Soot Aggregate Restructuring due to Coatings of Oleic Acid and Dioctyl Sebacate

Soot particles in the atmosphere can be coated with organic or nonorganic material, which may affect particle morphology and optical properties. The effect of the mass of coating on the morphology of soot particles was studied using oleic acid and dioctyl sebacate (DOS) coatings. A wide range of coatings were used, with up to 10 times as much coating as the mass of the soot. It is shown that as the coating mass increases the degree of collapsing increases until the coating is so large that the soot particle becomes completely contained within a spherical droplet of the coating material. Higher amounts of coating will not cause further collapse of the particle. The degree of collapse is also a function of the initial size of the soot particle but was independent of the coating materials tested, which have similar surface tensions. A model is presented to predict the change in mobility diameter as a function of coating mass ratio. The effect of coating mass on effective density, shape factor, and fractal dimension is also reported.

Copyright 2013 American Association for Aerosol Research     

The Detection Efficiency of the Single Particle Soot Photometer

A single particle soot photometer (SP2) uses an intense laser to heat individual aerosol particles of refractory black carbon (rBC) to vaporization, causing them to emit detectable amounts of thermal radiation that are used to quantify rBC mass. This approach is well suited for the detection of the majority of rBC mass loading in the ambient atmosphere, which occurs primarily in the accumulation mode (～ 1–300 fg-rBC/particle). In addition to operator choices about instrument parameters, SP2 detection of rBC number and/or mass can be limited by the physical process inherent in the SP2 detection technique — namely at small rBC mass or low laser intensities, particles fail to heat to vaporization, a requirement for proper detection. In this study, the SP2's ability to correctly detect and count individual flame-generated soot particles was measured at different laser intensities for different rBC particle masses. The flame-generated soot aerosol used for testing was optionally prepared with coatings of organic and non-organic material and/or thermally denuded. These data are used to identify a minimum laser intensity for accurate detection at sea level of total rBC mass in the accumulation mode (300 nW/(220-nm PSL)), a minimum rBC mass (～ 0.7-fg rBC-mass corresponding to 90 nm volume-equivalent diameter) for near-unity number detection efficiency with a typical operating laser intensity (450 nW/(220-nm PSL)), and a methodology using observed color temperature to recognize laser intensity insufficient for accurate rBC mass detection. Additionally, methods for measurement of laser intensity using either laboratory or ambient aerosol are presented.     

Evaluation of a Heated-Inlet for Calibration of the SP2

Black carbon (BC) calibration standards, such as fullerene soot, are routinely used to calibrate single-particle soot photometer (SP2) instruments. Impurities in BC standards create uncertainties in these calibrations, and thus it is desirable to remove non-BC compounds from the aerosol, though removal processes must not significantly alter BC microphysical properties. We present a series of experiments using mobility- and mass-selected fullerene soot particles to assess the performance of a high-temperature denuder system for treating BC prior to SP2 analysis. Particle mass, incandescence, and scattering properties were measured by tandem aerosol particle mass analyzers and an SP2, after thermal treatment at a range of temperatures and residence times (RT). For a longer RT (e.g., ～6 s at 300°C), monodisperse fullerene soot particles of initial mass 1.4 fg decreased in mass with increasing temperature, by 3% at 300°C to 15% at 600°C. Mass losses were similar for fullerene soot particles of initial mass 10.7 fg. The peak height of the particle laser-induced incandescence (LII) and scattering intensities of the 10.7 fg fullerene soot increased by 7% and 3%, respectively, at 300°C, and by over 15% and 10% at 400°C, possibly due to microphysical changes after heating. When sampling through a 300°C denuder with a particle RT of 2.5 s, the LII intensity of ambient BC particles of initial mass 1.1 fg increased by 8%. In light of these results, denuder temperatures of ～300°C with 0.4 s ≤ RT ≤ 2.5 s are recommended for SP2 calibration.

Copyright 2013 American Association for Aerosol Research     

Measurements of Morphology Changes of Fractal Soot Particles using Coating and Denuding Experiments: Implications for Optical Absorption and Atmospheric Lifetime

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.     

Quantification of online removal of refractory black carbon using laser-induced incandescence in the single particle soot photometer

Refractory black carbon (rBC) is an aerosol that has important impacts on climate and human health. rBC is often mixed with other species, making it difficult to isolate and quantify its important effects on physical and optical properties of ambient aerosol. To solve this measurement challenge, a new method to remove rBC was developed using laser-induced incandescence (LII) by Levin et al. in 2014. Application of the method with the Single Particle Soot Photometer (SP2) is used to determine the effects of rBC on ice nucleating particles (INP). Here, we quantify the efficacy of the method in the laboratory using the rBC surrogate Aquadag. Polydisperse and mobility-selected samples (100–500 nm diameter, 0.44–36.05 fg), are quantified by a second SP2. Removal rates are reported by mass and number. For the mobility-selected samples, the average percentages removed by mass and number of the original size are 88.9 ± 18.6% and 87.3 ± 21.9%, respectively. Removal of Aquadag is efficient for particles >100 nm mass-equivalent diameter (d_me), enabling application for microphysical studies. However, the removal of particles ≤100 nm d_me is less efficient. Absorption and scattering measurements are reported to assess its use to isolate brown carbon (BrC) absorption. Scattering removal rates for the mobility-selected samples are >90% on average, yet absorption rates are 53% on average across all wavelengths. Therefore, application to isolate effects of microphysical properties determined by larger sizes is promising, but will be challenging for optical properties. The results reported also have implications for other instruments employing internal LII, e.g., the Soot Particle Aerosol Mass Spectrometer (SP-AMS).

© 2016 American Association for Aerosol Research     

Direct Measurement of Aircraft Engine Soot Emissions Using a Cavity-Attenuated Phase Shift (CAPS)-Based Extinction Monitor

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 PM_ex) 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 (r ² > 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.     

An intercomparison of aerosol absorption measurements conducted during the SEAC4RS campaign

During the SEAC⁴RS campaign in 2013, inflight measurements of light-absorption by aerosol in biomass burning and agriculture fire plumes were collected along with concomitant measurements of aerosol extinction, scattering, and black carbon mass concentration. Here, we compare three measurements of aerosol absorption coefficients: from a photoacoustic spectrometer (PAS), a particle soot absorption photometer (PSAP), and a continuous light absorption photometer (CLAP). Each of these absorption measurements was collected in three visible spectral regions: red, green, and blue (although the precise wavelength and bandwidth vary with each instrument). The absorption measurements were compared during the plumes, in the boundary layer, and in the free troposphere. The slopes from the comparison ranged from 0.6 to 1.24. For biomass burning plumes, the uncertainty in the absorption measurements translates into a range in single scattering albedos of 0.93–0.94 at a wavelength of 660?nm, 0.94–0.95 at 532?nm and 0.92–0.95 at 405?nm. Overall, the aerosol absorption instruments agreed within their stated accuracies. Comparisons with simultaneous measurements of refractive black carbon mass concentration (collected by a single particle soot photometer), were used to derive the mass absorption coefficients (MAC). For all wavelengths, the MAC was high by greater than a factor of three compared to the expected MAC for black carbon.

© 2018 American Association for Aerosol Research     

Extrapolation of single particle soot photometer incandescent signal data

The Single Particle Soot Photometer (SP2) is an instrument for quantifying the refractory black carbon (rBC) mass of individual aerosol particles. It heats the particle’s rBC component to vaporization and quantifies the resulting visible thermal radiation to infer rBC mass. For purely technical reasons, SP2s are unable to quantify rBC mass beyond an easily adjustable limit due to eventual saturation of the electronics that record the visible light signals. Here, we evaluate an extrapolation algorithm to estimate rBC masses exceeding this upper limit in an SP2. The algorithm is based on identifying the crossing points of linear fits to unsaturated data, and using the duration of the saturated data to constrain potential errors. We find that extrapolation performance is quite insensitive to instrument parameters including laser intensity, rate of data acquisition, and particle speed through the laser. However, this approach increases uncertainty on the detection limit of the instrument, and is hence only useful in unknown aerosols for very limited extrapolation to approximately a factor of 1.5 increase in the upper mass range, corresponding to a 15% increase in the upper diameter limit. This increased range small enough that early identification of meaningful saturation during measurement campaigns remains the only tenable approach to robustly characterizing rBC mass size distributions and, in some cases, rBC mass concentrations.     

Soot Particle Aerosol Mass Spectrometer: Development,Validation, and Initial Application

The Soot Particle Aerosol Mass Spectrometer (SP-AMS) was developed to measure the chemical and physical properties of particles containing refractory black carbon (rBC). The SP-AMS is an Aerodyne Aerosol Mass Spectrometer (AMS) equipped with an intracavity laser vaporizer (1064 nm) based on the Single Particle Soot Photometer (SP2) design, in addition to the resistively heated, tungsten vaporizer used in a standard AMS. The SP-AMS can be operated with the laser vaporizer alone, with both the laser and tungsten vaporizers, or with the tungsten vaporizer alone. When operating with only the laser vaporizer, the SP-AMS is selectively sensitive to laser-light absorbing particles, such as ambient rBC-containing particles as well as metal nanoparticles, and measures both the refractory and nonrefractory components. When operated with both vaporizers and modulating the laser on and off, the instrument measures the refractory components of absorbing particles and the nonrefractory particulate matter of all sampled particles. The SP-AMS design, mass spectral interpretation, calibration, and sensitivity are described. Instrument calibrations yield a sensitivity of greater than 140 carbon ions detected per picogram of rBC mass sampled, a 3σ detection limit of less than 0.1 μg·m^?3 for 60 s averaging, and a mass-specific ionization efficiency relative to particulate nitrate of 0.2 ± 0.1. Sensitivities were found to vary depending upon laser-particle beam overlap. The utility of the instrument to characterize ambient rBC aerosol is demonstrated.

Copyright 2012 American Association for Aerosol Research     

Evidence in biomass burning smoke for a light-absorbing aerosol with properties intermediate between brown and black carbon

Biomass combustion produces black carbon (BC) and brown carbon (BrC) aerosols that contribute substantially to warming the Earth’s atmosphere. Accurate knowledge of their emissions and absorption per unit mass (mass absorption cross-section; MAC) can be used to quantify the radiative impact of these combustion products. We isolated particles generated from laboratory biomass burning fires by morphology and found that some particles from biomass burning do not correspond to either BC or BrC according to common operational definitions. Unlike BrC, these particles strongly absorb red light, with a MAC and spectral dependence of absorption between that of BrC and BC. They also have intermediate volatility: they survive thermodenuding at 250?°C but do not heat to incandescence in a single particle soot photometer (SP2) instrument. We also found evidence for intermediate properties in ambient wildfire smoke from the 2013 Rim Fire in California. More work is needed to understand how much this intermediate material contributes to atmospheric light absorption from typical combustion, whether or not it corresponds to “tar balls,” and how it may affect previous MAC measurements that were attributed to enhanced absorption by transparent coatings.

Copyright © 2019 American Association for Aerosol Research     

Examining the Relationship Between Black Carbon and Soot in Flames and Engine Exhaust

This article investigates the black carbon (BC) content of soot formed in premixed and diffusion flames and emitted by light duty gasoline and diesel vehicles. BC is measured photoacoustically and compared with particulate mass collected by filter and calculated from particle size distributions. The BC fraction of soot from rich premixed ethylene flames increases with height above the burner, but can remain well below unity in modestly sooting flames. The BC fraction produced by a propane diffusion flame soot generator (combustion aerosol standard, CAST) falls as the fuel is diluted with nitrogen, the principal means used to adjust the desired particle size. Thermally treating the soot to remove possible condensed semivolatile species does little to change these trends. Transmission electron microscopy (TEM) images show that despite low BC content, these particles display the characteristic fractal-like agglomerate morphology of soot. Particle mass spectra reveal polycyclic aromatic hydrocarbon (PAH) and fullerene fragments associated with low BC soot, which disappear as the BC fraction approaches unity. The results suggest that low BC content reflects immature solid soot that has not carbonized. Particulate matter (PM) measurements from current technology diesel and gasoline vehicles exhibit a high, >80% BC fraction. This is attributed to effective soot carbonization during the expansion and exhaust strokes of the engine, and to the substantial reductions of condensable hydrocarbons by catalytic aftertreatment. These results are discussed with respect to using light absorption-based instruments to monitor engine exhaust PM and using flame-generated soot for PM instrument calibration.     

Dependence of Laser-Induced Incandescence on Physical Properties of Black Carbon Aerosols: Measurements and Theoretical Interpretation

We used a single-particle soot photometer (SP2) to measure the mass of individual black carbon (BC) particles down to ～ 0.5 fg by means of laser-induced incandescence with an intra-cavity, continuous-wave laser. The incandescence of nine different types of BC samples was investigated to provide a physical basis for choosing appropriate BC materials for SP2 calibration. We estimated the vaporization temperatures of these BC samples from the spectral dependence of incandescence at the limit of the small size parameter x, for which spectral dependence of emissivity is known a priori. The vaporization temperatures differed by less than 2.2% among the samples. For the x < 1 regime of particle size, the peak amplitude of the incandescence signal measured by the SP2 was linearly proportional to the particle mass. The slopes of such linear proportionality were positively correlated with | (m ² -1)/(m ² +2)|, where the m is the complex refractive index of the BC particle. For particles in which x > 1, the rate of increase in the peak amplitude of the incandescence signal with increasing particle mass was negatively correlated with the compactness of particle shape, consistent with the theoretical prediction of emissivity, which accounts for particle shape. The incandescence–BC mass relationships were similar between fullerene soot and ambient soot sampled in Tokyo, thus suggesting that fullerene soot is a suitable calibration standard for SP2 measurements of ambient soot.     

Performance Comparison of Scanning Electrical Mobility Spectrometers

Scanning electrical mobility spectrometers (SEMS) are commonly used for near real-time ultrafine particle size distribution measurements. Analysis of SEMS measurements to calculate particle size distributions requires detailed understanding of instrument characteristics and operation. Varying instrument designs are used in the different commercial SEMS systems, and data analysis with these instruments requires accurate knowledge of their relative performance. In this study, an experimental approach to evaluate and reconcile differences between different SEMS instruments is established. This approach is used to characterize the relative performance of two SEMS systems—TSI's SMPS 3936-L22 and MSP's WPS XP1000—for particle sizes in the range of 20 to 300 nm. In these tests, the instruments were operated under a low flowrate condition with aerosol and sheath air flows of 0.3 and 3 LPM, respectively. Measurements show that the particle sizing characteristics of the instruments are very consistent with each other over the entire range of particle sizes studied. Particle number characteristics are dependent on the treatment of particle losses in the system and accounting of non-idealities of transfer function. The number concentrations reported by two instruments are generally consistent with each other and with an upstream reference counter for particle sizes larger than ～ 90 nm. For smaller particles, the low flowrate operation of the two systems results in significant penetration losses. A net particle detection efficiency (NPDE) factor for the two systems was determined from experiments with monodisperse aerosol. This factor is seen to be effective in characterizing and reconciling measurements made with these two SEMS instruments.     

A Potential Soot Mass Determination Method from Resistivity Measurement of Thermophoretically Deposited Soot

Miniaturized detection systems for nanometer-sized airborne particles are in demand, for example in applications for onboard diagnostics downstream particulate filters in modern diesel engines. A soot sensor based on resistivity measurements was developed and characterized. This involved generation of soot particles using a quenched co-flow diffusion flame; depositing the particles onto a sensor substrate using thermophoresis and particle detection using a finger electrode structure, patterned on thermally oxidized silicon substrate. The generated soot particles were characterized using techniques including Scanning Mobility Particle Sizer for mobility size distributions, Differential Mobility Analyzer—Aerosol Particle Mass analyzer for the mass–mobility relationship, and Transmission Electron Microscopy for morphology. The generated particles were similar to particles from diesel engines in concentration, mobility size distribution, and mass fractal dimension. The primary particle size, effective density and organic mass fraction were slightly lower than values reported for diesel engines. The response measured with the sensors was largely dependent on particle mass concentration, but increased with increasing soot aggregate mobility size. Detection down to cumulative mass as small as 20–30 μg has been demonstrated. The detection limit can be improved by using a more sensitive resistance meter, modified deposition cell, larger flow rates of soot aerosol and modifying the sensor surface.     

Mapping the Operation of the Miniature Combustion Aerosol Standard (Mini-CAST) Soot Generator

The Jing Ltd. miniature combustion aerosol standard (Mini-CAST) soot generator is a portable, commercially available burner that is widely used for laboratory measurements of soot processes. While many studies have used the Mini-CAST to generate soot with known size, concentration, and organic carbon fraction under a single or few conditions, there has been no systematic study of the burner operation over a wide range of operating conditions. Here, we present a comprehensive characterization of the microphysical, chemical, morphological, and hygroscopic properties of Mini-CAST soot over the full range of oxidation air and mixing N₂ flow rates. Very fuel-rich and fuel-lean flame conditions are found to produce organic-dominated soot with mode diameters of 10–60 nm, and the highest particle number concentrations are produced under fuel-rich conditions. The lowest organic fraction and largest diameter soot (70–130 nm) occur under slightly fuel-lean conditions. Moving from fuel-rich to fuel-lean conditions also increases the O:C ratio of the soot coatings from ～0.05 to ～0.25, which causes a small fraction of the particles to act as cloud condensation nuclei near the Kelvin limit (κ ～ 0–10^?3). Comparison of these property ranges to those reported in the literature for aircraft and diesel engine soots indicates that the Mini-CAST soot is similar to real-world primary soot particles, which lends itself to a variety of process-based soot studies. The trends in soot properties uncovered here will guide selection of burner operating conditions to achieve optimum soot properties that are most relevant to such studies.

Copyright 2014 American Association for Aerosol Research     

Absorption Enhancement of Coated Absorbing Aerosols: Validation of the Photo-Acoustic Technique for Measuring the Enhancement

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.