Publications

14 Results

Search results

Jump to search filters

Laser-driven ionization mechanisms of aluminum for single particle aerosol mass spectrometry

Spectrochimica Acta - Part B Atomic Spectroscopy

Lietz, Amanda M.; Yee, Benjamin T.; Musk, Jeffrey H.; Moffat, Harry K.; Wiemann, Dora K.; Settecerri, Taylor S.; Fergenson, David; Omana, Michael A.; Hopkins, Matthew M.

Single particle aerosol mass spectrometry (SPAMS), an analytical technique for measuring the size and composition of individual micron-scale particles, is capable of analyzing atmospheric pollutants and bioaerosols much more efficiently and with more detail than conventional methods which require the collection of particles onto filters for analysis in the laboratory. Despite SPAMS’ demonstrated capabilities, the primary mechanisms of ionization are not fully understood, which creates challenges in optimizing and interpreting SPAMS signals. In this paper, we present a well-stirred reactor model for the reactions involved with the laser-induced vaporization and ionization of an individual particle. The SPAMS conditions modeled in this paper include a 248 nm laser which is pulsed for 8 ns to vaporize and ionize each particle in vacuum. The ionization of 1 μm, spherical Al particles was studied by approximating them with a 0-dimensional plasma chemistry model. The primary mechanism of absorption of the 248 nm photons was pressure-broadened direct photoexcitation to Al(y2D). Atoms in this highly excited state then undergo superelastic collisions with electrons, heating the electrons and populating the lower energy excited states. We found that the primary ionization mechanism is electron impact ionization of various excited state Al atoms, especially Al(y2D). Because the gas expands rapidly into vacuum, its temperature decreases rapidly. The rate of three-body recombination (e− + e− + Al+ → Al + e−) increases at low temperature, and most of the electrons and ions produced recombine within several μs of the laser pulse. The importance of the direct photoexcitation indicates that the relative peak heights of different elements in SPAMS mass spectra may be sensitive to the available photoexcitation transitions. The effects of laser intensity, particle diameter, and expansion dynamics are also discussed.

More Details

Airborne Release Fractions from Surrogate Nuclear Waste Fires Containing Lanthanide Nitrates and Depleted Uranium Nitrate in 30% Tributyl Phosphate in Kerosene

Nuclear Technology

Hubbard, Joshua A.; Boyle, Timothy J.; Zepper, Ethan T.; Brown, Alexander B.; Settecerri, Taylor S.; Kotula, Paul G.; McKenzie, Bonnie B.; Lemieux, Laura J.; Zigmond, Joseph Z.; Preston, Rose T.; Maes, Brenda M.; Wiemann, Dora K.; Guerrero, Fernando G.; Robinson, Xavier J.

Airborne contaminants from fires containing nuclear waste represent significant health hazards and shape the design and operation of nuclear facilities. Much of the data used to formulate DOE-HDBK-3010-94, “Airborne Release Fractions/Rates and Respirable Fractions for Nonreactor Nuclear Facilities,” from the U.S. Department of Energy, were taken over 40 years ago. The objectives of this study were to reproduce experiments from Pacific Northwest Laboratories conducted in June 1973 employing current aerosol measurement methods and instrumentation, develop an enhanced understanding of particulate formation and transport from fires containing nuclear waste, and provide modeling and experimental capabilities for updating current standards and practices in nuclear facilities. A special chamber was designed to conduct small fires containing 25 mL of flammable waste containing lutetium nitrate, ytterbium nitrate, or depleted uranium nitrate. Carbon soot aerosols showed aggregates of primary particles ranging from 20 to 60 nm in diameter. In scanning electron microscopy, ~200-nm spheroidal particles were also observed dispersed among the fractal aggregates. The 200-nm spherical particles were composed of metal phosphates. Airborne release fractions (ARFs) were characterized by leaching filter deposits and quantifying metal concentrations with mass spectrometry. The average mass-based ARF for 238U experiments was 1.0 × 10−3 with a standard deviation of 7.5 × 10−4. For the original experiments, DOE-HDBK-3010-94 states, “Uranium ARFs range from 2 × 10−4 to 3 × 10−3, an uncertainty of approximately an order of magnitude.” Thus, current measurements were consistent with DOE-HDBK-3010-94 values. ARF values for lutetium and ytterbium were approximately one to two orders of magnitude lower than 238U. Metal nitrate solubility may have varied with elemental composition and temperature, thereby affecting ARF values for uranium surrogates (Yb and Lu). In addition to ARF data, solution boiling temperatures and evaporation rates can also be deduced from experimental data.

More Details

CRISPR/Cas9 as an antiviral against Orthopoxviruses using an AAV vector

Scientific Reports

Mayes, Cathryn M.; Kinahan, Sean M.; Settecerri, Taylor S.; Greene, Adrienne C.; Santarpia, Joshua L.

A vaccine for smallpox is no longer administered to the general public, and there is no proven, safe treatment specific to poxvirus infections, leaving people susceptible to infections by smallpox and other zoonotic Orthopoxviruses such as monkeypox. Using vaccinia virus (VACV) as a model organism for other Orthopoxviruses, CRISPR–Cas9 technology was used to target three essential genes that are conserved across the genus, including A17L, E3L, and I2L. Three individual single guide RNAs (sgRNAs) were designed per gene to facilitate redundancy in rendering the genes inactive, thereby reducing the reproduction of the virus. The efficacy of the CRISPR targets was tested by transfecting human embryonic kidney (HEK293) cells with plasmids encoding both SaCas9 and an individual sgRNA. This resulted in a reduction of VACV titer by up to 93.19% per target. Following the verification of CRISPR targets, safe and targeted delivery of the VACV CRISPR antivirals was tested using adeno-associated virus (AAV) as a packaging vector for both SaCas9 and sgRNA. Similarly, AAV delivery of the CRISPR antivirals resulted in a reduction of viral titer by up to 92.97% for an individual target. Overall, we have identified highly specific CRISPR targets that significantly reduce VACV titer as well as an appropriate vector for delivering these CRISPR antiviral components to host cells in vitro.

More Details

A Parameterization Study of Sew-EZ Materials: Types #6 and #8

Omana, Michael A.; Dallman, Ann R.; Wiemann, Dora K.; Settecerri, Taylor S.

Two material types identified by Sew-EZ were tested in various configurations, and under various conditions, by Sandia National Laboratories (SNL). The primary focus of this study was to assess the filtration performance of these two materials and identify if they perform similarly to certified N95 respirators. Testing was conducted on two systems which use distinctly different techniques to characterize the aerosol penetration characteristics of materials: a) R&D Filtration System: A large-scale R&D filtration system was used with testing parameters that mimicked NIOSH guidelines, where possible. Efficiency data as a function of particle size was attained using NaC1 as the test aerosol and a Scanning Mobility Particle Sizer (SMPS) for measurements. A more detailed system description can be found in Omana et al. 2020. b) Automated Tester: A commercial, automated filter tester (100Xs, Air Techniques International) was used to provide penetration/efficiency data for Sew EZ materials. The 100Xs aerosolizes a polydisperse NaC1 aerosol with a consistent concentration and size profile. The 100Xs manual (Air Techniques International 2018) states, "The aerosol particle size and distribution are designed to meet all requirements as defined in the relevant sections of NIOSH 42 CFR, Part 84 (pg. 32)."

More Details

Filtration Performance Results: Sierra Peaks Material No. 4

Omana, Michael A.; Wiemann, Dora K.; Settecerri, Taylor S.; Dallman, Ann R.

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.

More Details
14 Results
14 Results