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DOE OSTI2013

Ion generation and CPC detection efficiency studies in sub 3-nm size range

We studied the chemical composition of commonly used condensation particle counter calibration ions with a mass spectrometer and found that in our calibration setup the negatively charged ammonium sulphate, sodium chloride and tungsten oxide are the least contaminated whereas silver on both positive and negative and the three mentioned earlier in positive mode are contaminated with organics. We report cut-off diameters for Airmodus Particle Size Magnifier (PSM) 1.1, 1.3, 1.4, 1.6 and 1.6-1.8 nm for negative sodium chloride, ammonium sulphate, tungsten oxide, silver and positive organics, respectively. To study the effect of sample relative humidity on detection efficiency of the PSM we used different humidities in the differential mobility analyzer sheath flow and found that with increasing relative humidity also the detection efficiency of the PSM increases.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2017

A fast integrated mobility spectrometer for rapid measurement of sub-micrometer aerosol size distribution, Part II: Experimental characterization

A Fast Integrated Mobility Spectrometer (FIMS) with a wide dynamic size range has been developed for rapid aerosol size distribution measurements. The design and model evaluation of the FIMS are presented in the preceding paper (Paper I), and this paper focuses on the experimental characterization of the FIMS. Monodisperse aerosol with diameter ranging from 8 to 600 nm was generated using Differential Mobility Analyzer (DMA), and was measured by the FIMS in parallel with a Condensation Particle Counter (CPC). The mean particle diameter measured by the FIMS is in good agreement with the DMA centroid diameter. Comparison of the particle concentrations measured by the FIMS and CPC indicates the FIMS detection efficiency is essentially 100% for particles with diameters of 8 nm or larger. For particles smaller than 20 nm or larger than 200 nm, FIMS transfer function and resolution can be well represented by the calculated ones based on simulated particle trajectories in the FIMS. For particles between 20 and 200 nm, the FIMS transfer function is boarder than the calculated, likely due to non-ideality of the electric field, including edge effects near the end of the electrode, which are not represented by the 2-D electric field used to simulate particle trajectories.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2018

Rapid measurement of sub-micrometer aerosol size distribution using a fast integrated mobility spectrometer

We present rapid measurement of submicron particle size distributions enables the characterization of aerosols with fast changing properties, and is often necessary for measurements onboard mobile platforms (e.g., research aircraft). Aerosol mobility size distribution is commonly measured by a scanning mobility particle sizer (SMPS), which relies on voltage scanning or stepping to classify particles of different sizes, and may take up to several minutes to obtain a complete size spectrum of aerosol particles. The recently developed fast integrated mobility spectrometer (FIMS) with enhanced dynamic size range classifies and detects particles from 10 to ~600 nm simultaneously, allowing submicron aerosol mobility size distributions to be captured at a time resolution of 1 second. In this study, we present a detailed data inversion routine for deriving aerosol size distribution from FIMS measurements. The inversion routine takes into consideration the FIMS transfer function, particle penetration efficiency in the FIMS, and multiple charging of aerosols. The accuracy of the FIMS measurement is demonstrated by comparing parallel FIMS and SMPS measurements of stable aerosols with a wide range of size spectrum shapes, including ambient aerosols and aerosols classified by a differential mobility analyzer (DMA). The FIMS and SMPS-derived size distributions show excellent agreements for all aerosols tested. In addition, total number concentrations of ambient aerosols were integrated from 1 Hz FIMS size distributions, and compared with those directly measured by a condensation particle counter (CPC) operated in parallel. Finally, the integrated and measured total particle concentrations agree well within 5%.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Turbulent Flux Measurements of the Near‐Surface and Residual‐Layer Small Particle Events

Abstract According to recent field studies, almost half of the New Particle Formation (NPF) events occur aloft, in a residual layer, near the top of the boundary layer. Therefore, measurements of the meteorological parameters, precursor gas concentrations, and aerosol loadings conducted at the ground level are often not representative of the conditions where the NPFs take place. This paper presents new measurements obtained during the Turbulent Flux Measurements of the Residual Layer Nucleation Particles, conducted at the Southern Great Plains research site. Vertical turbulent fluxes of 3–10 nm‐sized particles were measured using a sonic anemometer and two condensation particle counters with nominal cutoff diameters of 3 nm and 10 nm mounted at the top of the 10‐m telescoping tower. Aerosol number size distribution (5–300 nm) was determined through the ground‐based Scanning Mobility Particle Sizers. The size selected (15–50 nm) particle hygroscopicity was derived with the Humidified Tandem Differential Mobility Analyzer. The ground level observations were supplemented by vertically‐resolved measurements of horizontal and vertical wind speeds and aerosol backscatter. The data analysis suggests that (a) turbulent flux measurements of 3–10 nm particles can distinguish between near‐surface and residual‐layer small particle events; (b) sub‐50 nm particles had a hygroscopicity value of 0.2, suggesting that organic compounds dominate atmospheric nanoparticle chemical composition at the site; and (c) current methodologies are inadequate for estimating the dry deposition velocity of sub‐10 nm particles because it is not feasible to measure particle concentration very near the surface, in the diffusion sublayer.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2026

High Time Resolution Modelled and Measured New Particle Formation Rates During the 2023 Pittsburgh, PA Campaign

Particle size distributions are used to calculate nucleation rates during new particle formation (NPF). However, the low time resolution and poor sensitivity of instruments deployed to observe particle size distributions can lead to inaccurate estimates of nucleation rates. We calculated nucleation rates in Pittsburgh, PA from particle size distributions measured with the new high time resolution Condensation Particle Counters For Atmospheric Rapid Measurements (CPC FARM) and from gas precursor concentrations measured with a chemical ionization mass spectrometer. The CPC FARM nucleation rates were calculated by examining the appearance rate of particles in the smallest size bin at 1.6 nm. The nucleation rate of 1.6 nm determined every second resulted in positive and negative rates, indicating the influence of inhomogeneous mixing and advection of precursor gases and clusters. These effects are not currently considered when estimating nucleation rates from measurements. The nucleation rates from the CPC FARM were compared to the nucleation rates determined from a transient acid‐base reaction model using measured sulfuric acid concentration, strong base concentrations, and CPC detection efficiencies. The transient form of the model allowed the advection of heterogeneously mixed precursors to influence the nucleation rate. Good agreement between particle and gas‐based nucleation rates is observed during sulfuric acid‐driven NPF events. This study demonstrates that high time resolution measurements of short‐lived and rapidly formed particles are needed to accurately capture nucleation rates, which are likely influenced by advection of nucleation precursors and clusters in heterogeneous environments such as urban areas.

Cheng, D. [Carnegie Mellon Univ., Pittsburgh, PA (↗

DOE OSTI2017

Temperature Dependence in Heterogeneous Nucleation with Application to the Direct Determination of Cluster Energy on Nearly Molecular Scale

A re-examination of measurements of heterogeneous nucleation of water vapor on silver nanoparticles is presented here using a model-free framework that derives the energy of critical cluster formation directly from measurements of nucleation probability. Temperature dependence is correlated with cluster stabilization by the nanoparticle seed and previously found cases of unusual increasing nucleation onset saturation ratio with increasing temperature are explained. A necessary condition for the unusual positive temperature dependence is identified, namely that the critical cluster be more stable, on a per molecule basis, than the bulk liquid to exhibit the effect. Temperature dependence is next examined in the classical Fletcher model, modified here to make the energy of cluster formation explicit in the model. The contact angle used in the Fletcher model is identified as the microscopic contact angle, which can be directly obtained from heterogeneous nucleation experimental data by a recently developed analysis method. Here an equivalent condition, increasing contact angle with temperature, is found necessary for occurrence of unusual temperature dependence. Our findings have immediate applications to atmospheric particle formation and nanoparticle detection in condensation particle counters (CPCs).

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2012

Kinetics of heterogeneous nucleation in supersaturated vapor: Fundamental limits to neutral particle detection revisited

We examine the nucleated (with barrier) activation of perfectly wetting (zero contact angle) particles ranging from essentially bulk size down to approximately 1-nm mass diameter. While similar studies trace back to the pioneering work of Fletcher, we present here a novel approach to the analysis based on general area constructions that enable key thermodynamic properties, including surface and bulk contributions to nucleation work, to be interpreted geometrically with reference to the Kelvin curve. The kinetics of activation are described in more detail in terms of the mean first passage time (MFPT) for barrier crossing. MFPT theory and benchmark calculations are used to develop and test a new approximate-but-simpler-to-use analytic expression for the barrier crossing rate. The present study is motivated by recent condensation particle counter (CPC) studies that appear to finally establish the long-predicted detection of 'sub-Kelvin' particles in the nano-size regime. Corresponding states thermodynamic and kinetic scaling approaches are used to facilitate the correlation and selection of optimal CPC working fluids and operating conditions based on a new metric for heterogeneous nucleation, the signal-to-noise ratio, and physical and chemical properties.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2017

A water-based fast integrated mobility spectrometer (WFIMS) with enhanced dynamic size range

We developed a water-based fast integrated mobility spectrometer (WFIMS) with enhanced dynamic size range. The WFIMS builds on two established technologies: the fast integrated mobility spectrometer and laminar flow water-based condensation methodology. Inside WFIMS, particles of differing electrical mobility are separated in a drift tube and subsequently enlarged through water condensation. Particle size and concentration are measured via digital imaging at a frame rate of 10 Hz. When we measure particles of different mobilities simultaneously, the WFIMS resolves particle diameters ranging from 8 to 580 nm within 1 s or less. The performance of WFIMS was characterized with differential mobility analyzer (DMA) classified (NH 4 ) 2 SO 2 particles with diameters ranging from 8 to 265 nm. The mean particle diameters measured by WFIMS were found to be in excellent agreement with DMA centroid diameters. Furthermore, detection efficiency of WFIMS was characterized using a condensation particle counter as a reference and is nearly 100% for particles with diameter greater than 8 nm. In general, measured and simulated WFIMS mobility resolutions are in good agreement. But, some deviations are observed at low particle mobilities, likely due to the non-idealities of the WFIMS electric field.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Particle charge distributions in the effluent of a flow-through atmospheric pressure low temperature plasma

Atmospheric pressure low-temperature plasmas are often utilized to perform particle synthesis, treatment, and removal. It is well-known that dust particles are highly negatively charged in these plasmas; however, little is known about dust particle charging behavior as particles leave the plasma volume and pass through the spatial afterglow region. In this work, monodisperse particles of various sizes and work functions were introduced into an atmospheric pressure radiofrequency capacitively coupled flow-through plasma. Dust particle electrical mobility distributions downstream of the flow-through plasma were measured utilizing a differential mobility analyzer in conjunction with a condensation particle counter at various gas flow velocities. Charge distributions were determined from the measured electrical mobility distributions. Experiments confirm that particles become less negatively charged, and even net-positively charged after leaving the plasma volume, with a distribution that follows a shifted Boltzmann charge distribution. Additionally, particle charge in the effluent of the flow-through plasma is negligibly dependent on work function but highly size and flow velocity dependent. Larger particles were shown to have a higher magnitude of charge under all studied conditions; however, particle polarity was switchable by varying gas flow velocity. The charging dynamics were simulated utilizing a constant number Monte Carlo model that accounts for electron temperature decay and the transition from ambipolar to free diffusion of electrons and ions in the spatial afterglow. Simulation results also suggest that, at the same flow velocity, larger particles obtain a greater magnitude of charge, negative or positive. Furthermore, the decrease in electron mobility and the difference between ion and electron convective loss rates create an ion-rich region in the plasma effluent that promotes ion–particle collisions and drives particle charge removal and even reversal of polarity. Larger particles more favorably collide with energetic species in these environments, which results in higher charge states.

atmospheric pressure low temperature plasma↗

DOE OSTI2019

Effects of reformed fuel on dual-fuel combustion particulate morphology

Advancements in catalytic reforming have demonstrated the ability to generate syngas (a mixture of CO and hydrogen) from a single hydrocarbon stream. This syngas mixture can then be used to replace diesel fuel and enable dual-fuel combustion strategies. The role of port-fuel injected syngas, composed of equal parts hydrogen and carbon monoxide by volume, was explored experimentally for soot reduction benefits under diesel pilot ignition and reactivity controlled compression ignition strategies. Particle size distribution measurements were made with a scanning mobility particle sizer and condensation particle counter for different levels of syngas substitution. To explain the experimental findings, computational fluid dynamics simulations utilizing a detailed stochastic soot model were used to validate and initialize additional simulations that isolate mixing and chemistry effects. Based on these simulations, the influence of adding syngas on soot particle size and quantity is discussed.

42 ENGINEERING↗

DOE OSTI2024

Scanning Mobility Particle Sizer (SMPS) Instrument Handbook

The Model 3936 Scanning Mobility Particle Spectrometer (SMPS) measures the size distribution of aerosols ranging from 10 nm up to 1000 nm. The SMPS uses a bipolar aerosol charger to keep particles within a known charge distribution. Charged particles are classified according to their electrical mobility, using a long-column differential mobility analyzer (DMA). Particle concentration is measured with a condensation particle counter (CPC). The SMPS is well-suited for applications including: nanoparticle research, atmospheric aerosol studies, pollution studies, smog chamber evaluations, engine exhaust and combustion studies, materials synthesis, filter efficiency testing, nucleation/condensation studies, and rapidly changing aerosol systems.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2024

3002 Humidified Tandem Differential Mobility Analyzer (HTDMA) Instrument Handbook

The Brechtel Manufacturing Inc. (BMI) Humidified Tandem Differential Mobility Analyzer (HT-DMA Model 3002) (Brechtel and Kreidenweis 2000a,b, Henning et al. 2005, Xerxes et al. 2014) measures how aerosol particles of different initial dry sizes grow or shrink when exposed to changing relative humidity (RH) conditions. It uses two different mobility analyzers (DMA) and a humidification system to make the measurements. One DMA selects a narrow size range of dry aerosol particles, which are exposed to varying RH conditions in the humidification system. The second (humidified) DMA scans the particle size distribution output from the humidification system. Scanning a wide range of particle sizes enables the second DMA to measure changes in size or growth factor (growth factor = humidified size/dry size), due to water uptake by the particles. A Condensation Particle Counter (CPC) downstream of the second DMA counts particles as a function of selected size in order to obtain the number size distribution of particles exposed to different RH conditions.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Filtration Performance Results: Sierra Peaks Material No. 4

Sandia National Laboratories (SNL) assessed the filtration performance of materials from Sierra Peaks to identify alternatives which may perform similarly to materials used in FDA-approved N95 respirators. This work is meant to characterize the aerosol performance of materials to give Sierra Peaks information for them to determine if they elect to submit masks made using these materials for follow-on N95 certification testing at an accredited facility. The R&D testbed used is a large-scale filtration system designed to test commercial filter boxes. System modifications were performed to simulate, where possible, parameters defined by the National Institute for Occupational Safety and Health (NIOSH) for certification of filter materials for N95 respirators (NIOSH 2019). The system is a pull-through design. Air enters through a Laminar Flow Element (LFE) and the volumetric flow is measured based on the pressure drop across the LFE. Pressure is measured via a Pressure Transducer (PT). The air then passes through a High Efficiency Particulate Air (HEPA) filter to purge the air of ambient airborne particulates. Test aerosol is injected into the flow shortly after and mixing is induced via a coarse mesh. The airflow is allowed to fully develop prior to arriving at the test section. The aerosol then passes through the test material mounted in a box in the test section. Pressure drop across the test article is measured and aerosol sampling probes measure the aerosol concentrations upstream and downstream of the sample. The air passes through a second HEPA filter prior to being exhausted to ambient by a blower. A Topas aerosol generator is used to produce the test aerosol from Sodium Chloride (NaC1) dissolved in deionized (DI) water. Generated aerosol passes through a heated mixing chamber and a desiccant dryer to produce nanosized solid-state particulates. A dilution loop allows for the aerosol concentration to be regulated. The aerosol sampling probes upstream and downstream of the test section are aligned with the flow path. These are ducted directly to the aerosol sizing and counting instruments. A Laser Aerosol Spectrometer (LAS) was used for data collection in the original configuration of the system and was also used for initial testing in this project. Because the lower measurement range for the LAS is 90 nanometers (nm), the LAS was switched out for a more complicated Scanning Mobility Particle Sizer (SMPS) spectrometer system. The SMPS is comprised of an Electrostatic Classifier (EC), Differential Mobility Analyzer (DMA), and a Condensation Particle Counter (CPC). This enabled data collection at 75 nm, the particle size called out in the NIOSH guidelines.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Time-Resolved Aerosol Filter Sampler Instrument Handbook

The U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility’s aerosol counting, composition, extinction, and sizing system (ACCESS) includes a base module (9400), a filter sampler (9401), an advanced mixing condensation particle counter (MCPC, 9403), a miniaturized optical particle counter (MOPC, 9405), and a single-channel tricolor absorption photometer (STAP, 9406). This handbook describes the principles and operations of the filter sampler.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Single-Channel Tricolor Absorption Photometer (STAP) Instrument Handbook

47 OTHER INSTRUMENTATION↗

DOE OSTI2023

Particle Flux Measurements during TRACER (TRACER PFM) (Field Campaign Report)

The purpose of this campaign was to deploy an instrument payload collocated with a suite of in situ and remote-sensing aerosol instruments at the urban site at the La Porte, Texas Municipal Airport during the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Tracking Aerosol Convection Interactions Experiment (TRACER) in Houston, Texas. The payload was designed to characterize the physicochemical properties, mixing state, and size-resolved vertical fluxes of aerosols. Deployed aerosol instruments associated with the flux measurements included three condensation particle counters (CPCs) with different lower cutoff diameters ( D > 2.5 nm, D > 10 nm, and D > 40 nm), a single-particle soot photometer (SP2) measuring refractory black carbon, and a portable optical particle spectrometer (POPS) measuring the optical size distribution (~180 nm < D < ~5000 nm). A 10-m flux tower hosted a sonic anemometer (SONIC) for vertical velocity measurements. In addition, a humidified tandem differential mobility analyzer (HTDMA) was deployed to measure the growth factors and hygroscopicity parameter of 15-50 nm-sized particles in order to constrain the composition of compounds responsible for modal aerosol growth during new particle formation/growth events. Finally, a radial differential mobility analyzer (RDMA) was deployed to extend the size distribution measurement to 5 nm.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Second ARM Aerosol Chemical Speciation Monitor Users’ Meeting Report

The aerosol chemical speciation monitor (ACSM) was developed to adapt the technology of the aerosol mass spectrometer (AMS) to routine, long-term, standalone monitoring. The calculation of particulate mass concentration from ACSM data requires the measurement of the response of the instrument to aerosol of specific size and composition as well as assumptions about the instrument response based on laboratory measurements and field experience acquired over more than two decades of operation of AMS and a decade of operation of the ACSM. Three parameters in the concentration calculations that are particularly important are the NO3 response factor (RFNO3), relative ionization efficiency (RIE), and the collection efficiency (CE). The values of RFNO3 and RIEs are determined from calibration, however the jump calibration method previously used in calibration can result in errors in the RIE for sulfate. This has been corrected by implementing a continuous calibration method. The default collection efficiency is 0.5. This has been shown to result in mass loadings that do not agree with mass determinations from other instruments because of effects of composition on the vaporization of the particles. The previous work of investigators addressing this issue is discussed. After preliminary work on ACSM and scanning mobility particle sizer (SMPS) data from the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) user facility Southern Great Plains (SGP) observatory collected in late 2016 and 2017 produced a parameterization of composition dependent collection efficiency very different from the results of previous studies, SMPS data were examined and we determined that there was significant mass that the instrument did not capture because the particles with diameters larger than 465 nm are not counted by this instrument. Data for the ultra-high-sensitivity aerosol spectrometer (UHSAS), SMPS, and ACSM are available for nearly all of 2019. The data from UHSAS and SMPS collected in 2019 were compared. We found that the UHSAS data has particle counts and total volumes significantly less than measured by the condensation particle counter (CPC) and SMPS. The SMPS data were extended by fitting the average volume distribution with a log normal curve and using this relationship to estimate a mass value for the SMPS over extended diameter range. The extended SMPS mass values result in a CDCE parameterization that is in better agreement with the results of other investigators, but is still different from other formulations. The working group recommends that the ACSM data be processed with a collective efficiency (CE)=1, that this be documented clearly in the metadata, and the use of the default CE of 0.5 or a formulation of composition-dependent collection efficiencies (CDCE) chosen by the user should be implemented based on the ammonium nitrate mass fraction. This is clearly necessary for the wintertime SGP ACSM data because of the high nitrate concentrations.

47 OTHER INSTRUMENTATION↗

DOE OSTI2018

Vertically resolved concentration and liquid water content of atmospheric nanoparticles at the US DOE Southern Great Plains site

Abstract. Most prior field studies of new particle formation (NPF) have been performed at or near ground level, leaving many unanswered questions regarding the vertical extent of NPF. To address this, we measured concentrations of 11–16 nm diameter particles from ground level to 1000 m during the 2013 New Particle Formation Study at the Atmospheric Radiation Measurement Southern Great Plains site in Lamont, Oklahoma. The measurements were performed using a tethered balloon carrying two condensation particle counters that were configured for two different particle cut-off diameters. These observations were compared to data from three scanning mobility particle sizers at the ground level. We observed that 11–16 nm diameter particles were generated at the top region of the boundary layer, and were then rapidly mixed throughout the boundary layer. We also estimate liquid water content of nanoparticles using ground-based measurements of particle hygroscopicity obtained with a Humidified Tandem Differential Mobility Analyzer and vertically resolved relative humidity (RH) and temperature measured with a Raman lidar. Our analyses of these observations lead to the following conclusions regarding nanoparticles formed during NPF events at this site: (1) ground-based observations may not always accurately represent the timing, distribution, and meteorological conditions associated with the onset of NPF; (2) nanoparticles are highly hygroscopic and typically contain up to 50 % water by volume, and during conditions of high RH combined with high particle hygroscopicity, particles can be up to 95 % water by volume; (3) increased liquid water content of nanoparticles at high RH greatly enhances the partitioning of water-soluble species like organic acids into ambient nanoparticles.

54 ENVIRONMENTAL SCIENCES↗