Results for “Particle Mobility” — Page 3

DOE OSTI2016

Observations and Modeling of the Green Ocean Amazon 2014/15. Nanoparticle Size Distribution (NPSD) Field Campaign Report

Aerosol nucleation and initial growth were investigated during the Green Ocean Amazon (GoAmazon) 2014/15 campaign. Aerosol sampling occurred during the wet and dry seasons of 2014, and took place at the T3 measurement site, downwind of the city of Manaus, Brazil. Characterization of the aerosol size distribution from 10 to 500 nm was accomplished through the deployment of a conventional Scanning Mobility Particle Spectrometer (SMPS) and a fine condensation particle counter (> 10 nm). In order to directly measure aerosol nucleation and initial growth, a Nano SMPS (1.5-20 nm) was also deployed, consisting of a condensation particle counter-based electrical mobility spectrometer that was modified for the detection of sub-3 nm aerosol. Measurements of the aerosol size distribution from 1.5 nm to 10 nm were obtained during the first observational period, and from 3 nm to 15 nm during the second observational period. Routine, stable measurement in this size range was complicated due to persistent water condensation in the Nano SMPS and diffusional transport losses

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2026

Experimental Report: Multi-Instrument Comparison of AAF Size Distribution Instruments

Aerosols are particles suspended in the atmosphere, ranging in size from nanometers to micrometers. Their size distribution affects key atmospheric processes, including nucleation, coagulation, scavenging, activation, and radiative properties (Seinfeld and Pandis 2016). Aerosol size distribution is a critical parameter in atmospheric science, influencing processes such as cloud formation and radiative forcing. Accurate representation of aerosol size distributions is essential for understanding their impact on climate, air quality, and human health. However, aerosol size and composition vary significantly across time and space due to meteorological conditions and natural or anthropogenic sources. (Wu and Boor 2021). Various instruments are used to measure aerosol size distributions, each with distinct principles, advantages, and limitations. This report begins with an in-depth overview of aerosol size-distribution comparison studies, focusing on the passive cavity aerosol spectrometer probe (PCASP), portable optical particle spectrometer (POPS), ultra-high-sensitivity aerosol spectrometer (UHSAS), aerodynamic particle sizer (APS), and scanning mobility particle sizer (SMPS). All of these instruments are used by the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) Aerial Facility (AAF), which commissioned this comparison and report. The report evaluates the strengths and weaknesses of these instruments, highlights their applications, and discusses efforts to merge data from multiple instruments for comprehensive analysis.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Structure and dynamics of hydrodynamically interacting finite-size Brownian particles in a spherical cavity: Spheres and cylinders

The structure and dynamics of confined suspensions of particles of arbitrary shape are of interest in multiple disciplines from biology to engineering. Theoretical studies are often limited by the complexity of long-range particle-particle and particle-wall forces, including many-body fluctuating hydrodynamic interactions. Here, we report a computational study on the diffusion of spherical and cylindrical particles confined in a spherical cavity. We rely on an immersed-boundary general geometry Ewald-like method to capture lubrication and long-range hydrodynamics and include appropriate non-slip conditions at the confining walls. A Chebyshev polynomial approximation is used to satisfy the fluctuation-dissipation theorem for the Brownian suspension. We explore how lubrication, long-range hydrodynamics, particle volume fraction, and shape affect the equilibrium structure and the diffusion of the particles. It is found that once the particle volume fraction is greater than 10%, the particles start to form layered aggregates that greatly influence particle dynamics. Hydrodynamic interactions strongly influence the particle diffusion by inducing spatially dependent short-time diffusion coefficients, stronger wall effects on the particle diffusion toward the walls, and a sub-diffusive regime-caused by crowding-in the long-time particle mobility. The level of asymmetry of the cylindrical particles considered here is enough to induce an orientational order in the layered structure, decreasing the diffusion rate and facilitating a transition to the crowded mobility regime at low particle concentrations. Our results offer fundamental insights into the diffusion and distribution of globular and fibrillar proteins inside cells.

36 MATERIALS SCIENCE↗

DOE OSTI2016

Note: Evaluation of slurry particle size analyzers for chemical mechanical planarization process

In the chemical mechanical planarization (CMP) process, slurry particle size is important because large particles can cause defects. Hence, selection of an appropriate particle measuring system is necessary in the CMP process. In this study, a scanning mobility particle sizer (SMPS) and dynamic light scattering (DLS) were compared for particle size distribution (PSD) measurements. In addition, the actual particle size and shape were confirmed by transmission electron microscope (TEM) results. SMPS classifies the particle size according to the electrical mobility, and measures the particle concentration (single particle measurement). On the other hand, the DLS measures the particle size distribution by analyzing scattered light from multiple particles (multiple particle measurement). For the slurry particles selected for evaluation, it is observed that SMPS shows bi-modal particle sizes 30 nm and 80 nm, which closely matches with the TEM measurements, whereas DLS shows only single mode distribution in the range of 90 nm to 100 nm and showing incapability of measuring small particles. Hence, SMPS can be a better choice for the evaluation of CMP slurry particle size and concentration measurements.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2021

Characterizing the performance of a POPS miniaturized optical particle counter when operated on a quadcopter drone

We first validate the performance of the Portable Optical Particle Spectrometer (POPS), a small light-weight and high sensitivity optical particle counter, against a reference scanning mobility particle sizer (SMPS) for a month-long deployment in an environment dominated by biomass burning aerosols. Subsequently, we examine any biases introduced by operating the POPS on a quadcopter drone, a DJI Matrice 200 V2. We report the root mean square difference (RMSD) and mean absolute difference (MAD) in particle number concentrations (PNCs) when mounted on the UAV and operating on the ground and when hovering at 10 m. When wind speeds are low (less than 2.6 m s –1 ), we find only modest differences in the RMSDs and MADs of 5 % and 3 % when operating at 10 m altitude. When wind speeds are between 2.6 and 7.7 m s –1 the RMSDs and MADs increase to 26.2 % and 19.1 %, respectively, when operating at 10m altitude. No statistical difference in PNCs was detected when operating on the UAV in either ascent or descent. We also find size distributions of aerosols in the accumulation mode (defined by diameter, d, where 0.1 ≤ d ≤ 1 µm) are relatively consistent between measurements at the surface and measurements at 10 m altitude, while differences in the coarse mode (here defined by d > 1 µm) are universally larger. Our results suggest that the impact of the UAV rotors on the POPS PNCs are small at low wind speeds, but when operating under a higher wind speed of up to 7.6 m s –1 , larger discrepancies occur. In addition, it appears that the POPS measures sub-micron aerosol particles more accurately than super-micron aerosol particles when airborne on the UAV. These measurements lay the foundations for determining the magnitude of potential errors that might be introduced into measured aerosol particle size distributions and concentrations owing to the turbulence created by the rotors on the UAV.

47 OTHER INSTRUMENTATION↗

DOE OSTI2023

SMPS data from TAMU TRACER campaign in the Houston TX region from July to September 2022

During TRACER, the Texas A&M Rapid Onsite Atmospheric Measurements Van (ROAM-V) was deployed to capture airmasses behind (maritime) and ahead (continental) of the passage of the sea-breeze front through Houston. On select sampling days, ROAM-V sampled in the morning/mid-day on the coast and then transited to a second inland site for the afternoon/evening. The suite of instruments deployed on ROAM-V included a Condensation Particle Counter (CPC; GRIMM Model 5.403 CPC), Scanning Mobility Particle Sizer (SMPS; TSI 3750 detector, TSI 3082 classifier, TSI 3088 neutralizer, TSI 3081A Differential Mobility Analyzer), Cloud Condensation Nuclei counter (Droplet Measurement Technologies CCN Counter), micro pulse lidar (Droplet Measurement Technologies Micro Pulse LiDAR (miniMPL)), and a Davis Rotating Uniform size-cut Monitor (DRUM; DRUMAir 4-DRUM). Before sampling at each location, the latitude and longitude were recorded using the GPS on the phone application “My Altitude”. Onboard the ROAM-V, aerosol samples are drawn through a shared isokinetic inlet at a flow rate ranging from 3.5 to 7.0 LPM. A portion of this flow, 1.0 LPM, is directed through TSI's 0.071 cm impactor attached to the classifier of the SMPS setup. The SMPS’s DMA and CPC are connected through a 20.3 cm length of 0.48 cm diameter tubing. Measured SMPS size distributions were used to calculate size-dependent particle losses for each SMPS scan. Particle losses from diffusion (based on Kesten, 1991 and Gormley, 1949) and inertial impaction in 90-degree bends (based on Aerosol Measurement, 2011 and Crane, 1977) were included in the loss calculation. This data was collected for ARM Field Campaign AFC07055 and supported by DOE ASR grant DE-SC0021047. For any further questions, please feel free to contact the instrument PI, Sarah D. Brooks, sbrooks@tamu.edu. Kesten et. al. Calibration of a TSI Model 3025 Ultrafine Condensation Particle Counter. Aerosol Science and Technology, 15:2, 107-111, 1991. Gormley et. al. Diffusion from a Stream Flowing through a Cylindrical Tube. Proceedings of the Royal Irish Academy, Vol 52, 163-169, 1948. Aerosol Measurement: Principles, Techniques, and Applications, Third Edition. John Wiley & Sons, Inc, 2011. Crane et. al. Inertial Deposition of Particles in a Bent Pipe. Journal of Aerosol Science, Vol 8, 161-170, 1977.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

CCN data from TAMU TRACER campaign in the Houston TX region from July to September 2022

During TRACER, the Texas A&M Rapid Onsite Atmospheric Measurements Van (ROAM-V) was deployed to capture airmasses behind (maritime) and ahead (continental) of the passage of the sea-breeze front through Houston. On select sampling days, ROAM-V sampled in the morning/mid-day on the coast and then transited to a second inland site for the afternoon/evening. The suite of instruments deployed on ROAM-V included a Condensation Particle Counter (CPC; GRIMM Model 5.403 CPC), Scanning Mobility Particle Sizer (SMPS; TSI 3750 detector, TSI 3082 classifier, TSI 3088 neutralizer, TSI 3081A Differential Mobility Analyzer), Cloud Condensation Nuclei counter (Droplet Measurement Technologies CCN Counter), micro pulse lidar (Droplet Measurement Technologies Micro Pulse LiDAR (miniMPL)), and a Davis Rotating Uniform size-cut Monitor (DRUM; DRUMAir 4-DRUM). Before sampling at each location, the latitude and longitude were recorded using the GPS on the phone application “My Altitude”. Onboard the ROAM-V, aerosol samples are drawn through a shared isokinetic inlet at a flow rate ranging from 3.5 to 7.0 LPM. A portion of this flow is directed through a cyclone impactor (Brechtel, Inc. Model SCC 0.732) and 0.5 LPM is directed to the CCN. To calculate particle losses, we used a two-step method. First, the measured SMPS size distributions were used to calculate particle loss through the inlet during sampling. Second, the corrected SMPS data was used to calculate the average of the total losses per scan down the CCN line. Then, the correction was applied to the CCN data. This calculation was done separately for each deployment location due to changes in the measured size distributions between locations. Particle loss from diffusion (based on Kesten, 1991 and Gormley, 1949), inertial impaction in 90-degree bends (based on Aerosol Measurement, 2011 and Crane, 1977), and cyclone impactor efficiency (based on Dirgo, 1985) were included in the loss calculation. When the SMPS was not sampling at a location (in the case of an instrument malfunction or operator error), the reported CPC data was corrected with an average of the total losses for the entire campaign at the specified deployment location (e.g., if we needed to correct Galveston data, then the average of all calculated losses at Galveston was taken). These flatline corrections were used for all data on 22/07/13, 22/07/20, 22/07/22, and the data from Galveston on 22/08/09. The supersaturation uncertainty is estimated conservatively at +/- 0.03%, where variation in the inlet temperature, pressure, and calibration technique prevents a more accurate measurement. Confidence in the reported supersaturation measurements is based on a pre-campaign calibration (following the methods from our previous work and Deng, 2014 based on Rose, 2008) in addition to inter-comparisons with the DOE for two days (22/08/18 and 22/09/01) where TAMU was co-located with AMF1. The inter-comparisons show good agreement between our instrument and the DOEs instrument on both days at all supersaturations. After the last inter-comparison on 22/09/01, there was no indication of a malfunction by our instrument through the rest of the campaign. Unfortunately, the instrument was dropped during demobilization. A post-campaign calibration was conducted, which showed a substantial departure from the pre-campaign calibration. The drop may have damaged the instrument’s ability to produce the desired supersaturations. Therefore, we do consider the data after 22/09/01 to be correct, but it should be used with caution. The CCN counter sampled for 3 minutes at each supersaturation setpoint (0.2, 0.4, 0.6, 0.8, 1.0, and 1.2%). At the end of a cycle, the instrument was set to 0.01% supersaturation for 5 minutes. The data is comprised of the last 60 seconds of each supersaturation set point (0.2, 0.4, 0.6, 0.8, 1.0, and 1.2%) to ensure the instrument stabilized and was able to reach thermal equilibrium. We removed the data during the periods where there were operational difficulties, setup, or maintenance. This data was collected for ARM Field Campaign AFC07055 and supported by DOE ASR grant DE-SC0021047. For any further questions, please feel free to contact the instrument PI, Sarah D. Brooks, sbrooks@tamu.edu. Rose et. al. Calibration and Measurement Uncertainties of a Continuous-Flow Cloud Condensation Nuclei Counter (DMT-CCNC): CCN Activation of Ammonium Sulfate and Sodium Chloride Aerosol Particles in Theory and Experiment. Atmos. Chem. Phys., 8, 1153-1179, 2008. Deng et. al. Using Raman Microspectroscopy to Determine Chemical Composition and Mixing State of Airborne Marine Aerosols over the Pacific Ocean. Aerosol Science and Technology, Vol 48, Issue 2, 2014. Kesten et. al. Calibration of a TSI Model 3025 Ultrafine Condensation Particle Counter. Aerosol Science and Technology, 15:2, 107-111, 1991. Gormley et. al. Diffusion from a Stream Flowing through a Cylindrical Tube. Proceedings of the Royal Irish Academy, Vol 52, 163-169, 1948. Aerosol Measurement: Principles, Techniques, and Applications, Third Edition. John Wiley & Sons, Inc, 2011. Crane et. al. Inertial Deposition of Particles in a Bent Pipe. Journal of Aerosol Science, Vol 8, 161-170, 1977. Dirgo et. al. Cyclone Collection Efficiency: Comparison of Experimental Results with Theoretical Predictions. Aerosol Science and Technology, 4:4, 401-415, 1985.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

CPC data from TAMU TRACER campaign in the Houston, TX region from July to September 2022

During TRACER, the Texas A&M Rapid Onsite Atmospheric Measurements Van (ROAM-V) was deployed to capture airmasses behind (maritime) and ahead (continental) of the passage of the sea-breeze front through Houston. On select sampling days, ROAM-V sampled in the morning/mid-day on the coast and then transited to a second inland site for the afternoon/evening. The suite of instruments deployed on ROAM-V included a Condensation Particle Counter (CPC; GRIMM Model 5.403 CPC), Scanning Mobility Particle Sizer (SMPS; TSI 3750 detector, TSI 3082 classifier, TSI 3088 neutralizer, TSI 3081A Differential Mobility Analyzer), Cloud Condensation Nuclei counter (Droplet Measurement Technologies CCN Counter), micro pulse lidar (Droplet Measurement Technologies Micro Pulse LiDAR (miniMPL)), and a Davis Rotating Uniform size-cut Monitor (DRUM; DRUMAir 4-DRUM). Before sampling at each location, the latitude and longitude were recorded using the GPS on the phone application “My Altitude”. Onboard the ROAM-V, aerosol samples are drawn through a shared isokinetic inlet at a flow rate ranging from 3.5 to 7.0 LPM. A portion of this flow is directed through a cyclone impactor (Brechtel, Inc. Model SCC 0.732) and 0.3 LPM is directed to the CPC. To correct the data for particle losses, we used a two-step method. First, the measured SMPS size distributions were used to calculate total particle loss through the inlet for every SMPS scan at a single deployment location. Second, the CPC data was corrected for particle losses using the average of the total losses per scan. This calculation was done separately for each deployment location due to changes in the measured size distributions between locations. Particle loss from diffusion (based on Kesten, 1991 and Gormley, 1949), inertial impaction in 90-degree bends (based on Aerosol Measurement, 2011 and Crane, 1977), and cyclone impactor efficiency (based on Dirgo, 1985) were included in the loss calculation. When the SMPS was not sampling at a location (in the case of an instrument malfunction or operator error), the reported CPC data was corrected with an average of the total losses for the entire campaign at the specified deployment location (e.g., if we needed to correct Galveston data, then the average of all calculated losses at Galveston was taken). These flatline corrections were used for all data on 22/07/13, 22/07/20, 22/07/22, and the data from Galveston on 22/08/09. An additional flatline correction of 14% was applied to all CPC data based on laboratory calibration prior to and after the campaign. In laboratory calibrations, we identified that for the same sample of air the field CPC (GRIMM Model 5.403 CPC) undercounted the total concentration of particles by 14% compared to the ground truth laboratory CPC (TSI Model 3750). This data was collected for ARM Field Campaign AFC07055 and supported by DOE ASR grant DE-SC0021047. For any further questions, please feel free to contact the instrument PI, Sarah D. Brooks, sbrooks@tamu.edu. Kesten et. al. Calibration of a TSI Model 3025 Ultrafine Condensation Particle Counter. Aerosol Science and Technology, 15:2, 107-111, 1991. Gormley et. al. Diffusion from a Stream Flowing through a Cylindrical Tube. Proceedings of the Royal Irish Academy, Vol 52, 163-169, 1948. Aerosol Measurement: Principles, Techniques, and Applications, Third Edition. John Wiley & Sons, Inc, 2011. Crane et. al. Inertial Deposition of Particles in a Bent Pipe. Journal of Aerosol Science, Vol 8, 161-170, 1977. Dirgo et. al. Cyclone Collection Efficiency: Comparison of Experimental Results with Theoretical Predictions. Aerosol Science and Technology, 4:4, 401-415, 1985.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Optical Particle Measurements during EPCAPE Field Campaign Report

This campaign requested the deployment of the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) User Facility optical particle counter (OPC) at the first ARM Mobile Facility (AMF1) located at the Scripps Pier in La Jolla, California during the Eastern Pacific Cloud Aerosol Precipitation Experiment (EPCAPE). The addition of the OPC was requested for two reasons. (1) Close the gap between the scanning mobility particle sizer (SMPS) and aerodynamic particle sizer (APS) size distribution from the Aerosol Observing System (AOS) measurements. (2) Principal investigator Petters has been working with Tracking Aerosol Convection Interaction Experiment (TRACER) data to compute particle fluxes from Doppler lidar (Petters et al. 2024). Briefly, backscatter flux is obtained using the eddy covariance technique using the Doppler vertical velocity and attenuated backscatter. Building upon prior studies, we were able to relate backscatter to particle number concentration by calibrating the lidar retrievals against optical particle counter-measured ground-based aerosol size distribution and radiosonde-interpolated relative humidity at lidar sample height. Performing similar analysis was of interest to EPCAPE to better understand the emissions and vertical transport of large particles into the overlying stratus clouds. However, as stated above, this analysis requires an optical size distribution that covers the 0.3-30-μm-diameter size range. The OPC was deployed between 2023-04-14 and 2024-02-14. The deployment, data quality analysis, and data archiving was handled by the DOE ARM instrument mentor team without additional involvement by the principal investigator. Data quality was marked as “routine” for the majority of the campaign.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Ice nucleation measurements from DRUM impactors during TRACER campaign in the Houston TX region from July to September 2022

During TRACER, three Davis Rotating Uniform size-cut Monitors (DRUM; DRUMAir 4-DRUM) were used to collect aerosols for ice nucleation measurements in the Brooks laboratory at Texas A&M University. The three instruments were located at AMF1 in La Porte, Ancillary site in Guy (ANC), and onboard the Texas A&M Rapid Onsite Atmospheric Measurements Van (ROAM-V). ROAM-V was deployed to capture airmasses behind (maritime) and ahead (continental) of the passage of the sea-breeze front through Houston. On select sampling days, ROAM-V sampled in the morning/mid-day on the coast and then transited to a second inland site for the afternoon/evening. The suite of instruments deployed on ROAM-V included a Condensation Particle Counter (CPC; GRIMM Model 5.403 CPC), Scanning Mobility Particle Sizer (SMPS; TSI 3750 detector, TSI 3082 classifier, TSI 3088 neutralizer, TSI 3081A Differential Mobility Analyzer), Cloud Condensation Nuclei counter (Droplet Measurement Technologies CCN Counter), micro pulse lidar (Droplet Measurement Technologies Micro Pulse LiDAR (miniMPL)), and one of the Davis Rotating Uniform size-cut Monitors (DRUM; DRUMAir 4-DRUM). Before sampling at each location, the latitude and longitude were recorded using the GPS on the phone application “My Altitude”. Each DRUM sampler was operated at a flow rate of 23 LPM. Each DRUM has four stages where the aerodynamic diameter size cuts are as follows: stage 1 larger than 3 μm, stage 2 from 3 to 1.2 μm, stage 3 from 1.2 to 0.34 μm, and stage 4 from 0.34 to 0.15 μm. Pretreated aluminum foil was used as a substrate on all stages. At AMF1 and ANC sites, the DRUMs were operated on the shared aerosol inlet, with generous support of the DOE ARM site staff. These instruments rotated 24 mm per day and only contained aluminum foil substrates. Substrates were changed weekly and transported to Texas A&M for storage in -80C freezer until analysis. The DRUM onboard ROAM-V was operated at a faster rotation rate of 150 mm per day to clearly separate the multiple deployment locations for ROAM-V. For the ROAM-V DRUM, substrates were changed every deployment and transported to Texas A&M for storage in -80C freezer until analysis. At Texas A&M, ice nucleation experiments were conducted to measure the ice nucleation temperature of the ambient aerosol samples collected from the three DRUMs using our previously established procedures (Alsante et al., 2023; Fornea et al., 2009; Matthews et al., 2023). For ice nucleation, only samples collected on stage 3 were analyzed, given that these are the most relevant size (1.2 to 0.34 μm diameter) for potential ice nucleating particles. For the AMF1 and ANC sites, we cut and analyzed 2 mm (2-hour) samples. We analyzed the time periods of the AMF1 site instrument when the ROAM-V was deployed. A 72-hour period from July 11th at 23:49 through July 15th at 1:49 was analyzed from the ANC site instrument. For the ROAM-V instrument, we separated the daily samples by site location. Between 1- and 6-hour independent samples were analyzed at each location. We also cut the ROAM-V samples in half to allow for compositional analysis of the aerosol on the other half of the substrate. All viable samples from the ROAM-V were analyzed. Analysis was done using a custom-built ice nucleation apparatus, recently updated to include an array of 16 individual samples (Matthews et al., 2023). On our experimental setup, we used 100 μL of Ultra-High-Performance Liquid Chromatography (UHPLC) water (Sigma Aldrich, >99.9% purity) to wash off the aerosol from the DRUM substrate. Then, we micropipetted 2 μL droplet samples into each of the 16 wells of the array, using hydrophobically coated microscope slides. Experiments would cycle 28 times from 10 C to -40C over a 20-hour period. During analysis of the TRACER samples, nine experiments were conducted with UHPLC water process blanks that followed an identical preparation procedure. The average freezing temperature and standard deviation for these process blanks is -27.7±2.4 C. This data was collected for ARM Field Campaign AFC07023 and supported by DOE ASR grant DE-SC0021047. For any further questions, please feel free to contact the instrument PI, Sarah D. Brooks, sbrooks@tamu.edu. Alsante, A. N., Thornton, D. C., & Brooks, S. D. (2023). Ice nucleation catalyzed by the photosynthesis enzyme RuBisCO and other abundant biomolecules. Communications Earth & Environment, 4(1), 51. Fornea, A. P., Brooks, S. D., Dooley, J. B., & Saha, A. (2009). Heterogeneous freezing of ice on atmospheric aerosols containing ash, soot, and soil. Journal of Geophysical Research: Atmospheres, 114(D13). DOI:10.1029/2009JD011958 Matthews, B. H., Alsante, A. N., & Brooks, S. D. (2023). Pollen Emissions of Subpollen Particles and Ice Nucleating Particles. ACS Earth and Space Chemistry.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Mini-Micropulse Lidar data from TAMU TRACER campaign in the Houston TX region from July to September 2022

During TRACER, the Texas A&M Rapid Onsite Atmospheric Measurements Van (ROAM-V) was deployed to capture airmasses behind (maritime) and ahead (continental) of the passage of the sea-breeze front through Houston. On select sampling days, ROAM-V sampled in the morning/mid-day on the coast and then transited to a second inland site for the afternoon/evening. The suite of instruments deployed on ROAM-V included a Condensation Particle Counter (CPC; GRIMM Model 5.403 CPC), Scanning Mobility Particle Sizer (SMPS; TSI 3750 detector, TSI 3082 classifier, TSI 3088 neutralizer, TSI 3081A Differential Mobility Analyzer), Cloud Condensation Nuclei counter (Droplet Measurement Technologies CCN Counter), micro pulse lidar (Droplet Measurement Technologies Micro Pulse LiDAR (mini-MPL)), and a Davis Rotating Uniform size-cut Monitor (DRUM; DRUMAir 4-DRUM). Before sampling at each location, the latitude and longitude were recorded using the GPS on the phone application “My Altitude”. The mini-MPL deployed with ROAM-V is a 532 nm elastic and polarization lidar. The mini-MPL outputs normalized relative backscatter (NRB) derived from raw signal after after-pulse, overlap, and dead-time correction calibration. The depolarization ratio is calculated from the co-polarized and cross-polarized NRB (Flynna et al., 2007). The NRB and depolarization ratio data are resampled from the original data at 1-minute intervals. The vertical resolution of the mini-MPL data is 15 meters. The mini-MPL data can be used to determine the boundary layer, cloud top, and cloud bottom height and can be used to retrieve aerosol type and concentration profile. This data was collected for ARM Field Campaign AFC07055 and supported by DOE ASR grant DE-SC0021047. For any further questions, please feel free to contact the instrument PI, Sarah D. Brooks, sbrooks@tamu.edu . Flynna, C. J., Mendozaa, A., Zhengb, Y., & Mathurb, S. (2007). Novel polarization-sensitive micropulse lidar measurement technique. Optics express, 15(6), 2785-2790.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Ozone and aerosol size distribution measurements at the Oliktok Point, AK AMF3

Aerosol size distribution measurements at the Oliktok Point, AK AMF3 as measured by a TSI model 3082 scanning mobility particle sizer (SMPS), and ozone measurements at the Oliktok Point, AK AMF3 as measured by a 2B model 205 ozone monitor. 2B specifies a limit of detection (2σ) of 2 ppb and these data were calibrated using a 2B model 306 ozone calibration source. Users of the data are asked to contact PI Pratt prior to use for consultation, discussion of co-authorship, and to ensure that the most up-to-date information is provided.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2017

Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems (HI-SCALE) Field Campaign Report

Cumulus convection is an important component in the atmospheric radiation budget and hydrologic cycle over the southern Great Plains and over many regions of the world, particularly during the summertime growing season when intense turbulence induced by surface radiation couples the land surface to clouds. Current convective cloud parameterizations contain uncertainties resulting in part from insufficient coincident data that couples cloud macrophysical and microphysical properties to inhomogeneities in land surface, boundary layer, and aerosol properties. The Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems (HI-SCALE) campaign was designed to provide a detailed set of measurements that are needed to obtain a more complete understanding of the lifecycle of shallow clouds by coupling cloud macrophysical and microphysical properties to land surface properties, ecosystems, and aerosols. Some of the land-atmosphere-cloud interactions that can be studied using HI-SCALE data are shown in Figure 1. HI-SCALE consisted of two 4-week intensive operation periods (IOPs), one in the spring (April 24-May 21) and the other in the late summer (August 28-September 24) of 2016, to take advantage of different stages of the plant lifecycle, the distribution of “greenness” for various types of vegetation in the vicinity of the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Climate Research Facility Southern Great Plains (SGP) site, and aerosol properties that vary during the growing season. As expected, satellite measurements indicated that the Normalized Difference Vegetation Index (NDVI) was much “greener” in the vicinity of the SGP site during the spring IOP than the late summer IOP as a result of winter wheat maturing in the spring and being harvested in the early summer. As shown in Figure 2, temperatures were cooler than average and soil moisture was high during the spring IOP, while temperatures were warmer than average and soil moisture was low during the late summer IOP. These factors likely influence the occurrence and lifecycle of shallow clouds. Most of the instrumentation was deployed on the ARM Aerial Facility (AAF) Gulfstream 1 (G-1) aircraft, including those that measure atmospheric turbulence, cloud water content and drop size distributions, aerosol precursor gases, aerosol chemical composition and size distributions, and cloud condensation nuclei (CCN) concentrations. The specific instrumentation is listed in Table 1. The team of scientists participating in the G-1 flights were from Pacific Northwest National Laboratory (PNNL), Brookhaven National Laboratory (BNL), and the University of Washington. Routine ARM aerosol measurements made at the surface were supplemented with aerosol microphysical properties measurements, with support from the DOE Environmental Molecular Sciences Laboratory (EMSL) User Facility and the Atmospheric System Radiation (ASR) program. This included deploying a scanning mobility particle sizer (SMPS) to measure aerosol size distribution, a proton transfer reaction-mass spectrometer (PTR-MS) to measure volatile organic compounds, an aerosol mass spectrometer (AMS) to measure bulk aerosol composition, and the single-particle laser ablation time-of-flight mass spectrometer (SPLAT II) to measure single-particle aerosol composition at the SGP site Guest Instrumentation Facility. In this way, characterization of aerosol properties at the surface and on the G-1 were consistent. In addition, the HI-SCALE: Nanoparticle Composition and Precursors add-on campaign was conducted during the second IOP in which several state-of-the-science chemical ionization mass spectrometers were deployed to measure nanoparticle composition and precursors. Scientists participating in the surface measurements were from PNNL, BNL, University California–Irvine, Augsberg College, Colorado University, Aerodyne Inc., and Aerosol Dynamics Inc.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Engineering Anomalously Large Electron Transport in Topological Semimetals

Abstract Anomalous transport of topological semimetals has generated significant interest for applications in optoelectronics, nanoscale devices, and interconnects. Understanding the origin of novel transport is crucial to engineering the desired material properties, yet their orders of magnitude higher transport than single‐particle mobilities remain unexplained. This work demonstrates the dramatic mobility enhancements result from phonons primarily returning momentum to electrons due to phonon‐electron dominating over phonon–phonon scattering. Proving this idea, proposed by Peierls in 1932, requires tuning electron and phonon dispersions without changing symmetry, topology, or disorder. This is achieved by combining de Haas ‐ van Alphen (dHvA), electron transport, Raman scattering, and first‐principles calculations in the topological semimetals MX 2 (M = Nb, Ta and X = Ge, Si). Replacing Ge with Si brings the transport mobilities from an order magnitude larger than single particle ones to nearly balanced. This occurs without changing the crystal structure or topology and with small differences in disorder or Fermi surface. Simultaneously, Raman scattering and first‐principles calculations establish phonon–electron dominated scattering only in the MGe 2 compounds. Thus, this study proves that phonon‐drag is crucial to the transport properties of topological semimetals and provides insight to engineer these materials further.

36 MATERIALS SCIENCE↗

DOE OSTI2018

Effect of relative humidity on the composition of secondary organic aerosol from the oxidation of toluene

The effect of relative humidity (RH) on the chemical composition of secondary organic aerosol (SOA) formed from low-NO x toluene oxidation in the absence of seed particles was investigated. SOA samples were prepared in an aerosol smog chamber at < 2 % RH and 75 % RH, collected on Teflon filters, and analyzed with nanospray desorption electrospray ionization high-resolution mass spectrometry (nano-DESI–HRMS). Measurements revealed a significant reduction in the fraction of oligomers present in the SOA generated at 75 % RH compared to SOA generated under dry conditions. In a separate set of experiments, the particle mass concentrations were measured with a scanning mobility particle sizer (SMPS) at RHs ranging from < 2 to 90 %. It was found that the particle mass loading decreased by nearly an order of magnitude when RH increased from < 2 to 75–90 % for low-NO x toluene SOA. The volatility distributions of the SOA compounds, estimated from the distribution of molecular formulas using the “molecular corridor” approach, confirmed that low-NO x toluene SOA became more volatile on average under high-RH conditions. In contrast, the effect of RH on SOA mass loading was found to be much smaller for high-NO x toluene SOA. The observed increase in the oligomer fraction and particle mass loading under dry conditions were attributed to the enhancement of condensation reactions, which produce water and oligomers from smaller compounds in low-NO x toluene SOA. The reduction in the fraction of oligomeric compounds under humid conditions is predicted to partly counteract the previously observed enhancement in the toluene SOA yield driven by the aerosol liquid water chemistry in deliquesced inorganic seed particles.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

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 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 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↗