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All sourcesNASA NTRSDOE OSTI
NASA NTRS1989

Dissociative recombination in interstellar clouds

Molecular ions play a significant role in the chemistry and evolution of interstellar molecular clouds, even though these regions are overwhelmingly neutral. The dissociative recombination (DR) process governs the abundances of many of these ions and of related neutral species. The gas-phase ion-molecule chemistry of the simplest species is summarized, with emphasis on those problems which are most sensitive to uncertain rates or product branching ratios of DR processes. Examples of the kinds of information needed about DR processes are presented. The importance of the H3(+) ion and prospects for its direct observation are discussed.

Black, John H.↗
NASA NTRSDate not supplied

Aeroacoustic Analysis using Dynamic Mode Decomposition of Unsteady Pressure-Sensitive Paint Measurements

In this paper, we present a new method for the diagnosis and analysis of aeroacoustic phenomena. Taking advantage of the well-known property that the measurements of the Unsteady Pressure-Sensitive Paint (uPSP) have much higher spatial resolution compared to those of the conventional pressure transducers, the method is based on the visualization and analysis of the outputs of the Dynamic Mode Decomposition (DMD) of the uPSP measurements. The uPSP measurements were collected with four Phantom high-speed cameras in the Ascent Transient Aerodynamics Test (ATAT) of the Space Launch System (SLS) Block 1 cargo vehicle in the 11-by-11-foot transonic test section of the Unitary Plan Wind Tunnel (UPWT) at NASA Ames Research Center in September 2019. The method presented in this paper is demonstrated by investigating an interesting phenomenon observed in the SLS ATAT – the vortex shedding tone generated by the forward attachment of the Solid Rocket Booster (SRB). As examples, the DMD outputs of the uPSP measurements in a subsonic test in the SLS ATAT are presented. It is shown the information retrieved from the DMD outputs of the uPSP measurements can be effectively used in the identification and diagnosis of the aeroacoustic phenomena. The work described in this paper is a part of NASA’s development of a new state-of-the-art uPSP capability in production wind tunnels. Funding was provided by the NASA Aerosciences Evaluation and Test Capabilities Portfolio Office.

acoustics↗
DOE OSTI2023

Structure and Electronic Properties of Mesopores in Si PV Devices with PLEO Contacts

All current state-of-the-art silicon photovoltaic (PV) devices employ some flavor of passivating contact structure to minimize detrimental recombination while providing good conductivity. These properties are most often provided by a dielectric layer (SiNx, Al2O3, or SiOx) that is in contact with the crystalline silicon (c-Si) substrate. The effectiveness of these layers is heavily dependent on the nanoscale structure of both the dielectric layers and the crystalline silicon interface. As an example, the tunneling probability for charge carriers across thin SiOx layers, a process that is critical to maintain high conductivity, is extremely sensitive to the SiOx thickness. SiOx with a thickness below 2 nm readily allows charge carrier tunneling, whereas it is impeded for greater thicknesses. In the latter case it has been shown that modifications to the thermal processing schedule can induce disruptions, or pinholes, in thick SiOx layers that allow transport of charge carriers while maintaining excellent passivation. However, this requires higher temperatures processes that may inhibit widespread adoption by industry. Recently, another option has been presented that may circumvent the necessity for high temperature processing, namely metal assisted chemical etching (MACE). MACE relies on deposition of Ag nanoparticles onto the SiOx layers with subsequent electroless etching to form mesopores in the SiOx layers that are analogous to the pinholes created with high temperature processing. The size and density can be controlled based on the Ag nanoparticle deposition conditions. The resulting contact structure is known as polysilicon on locally etched oxide (PLEO) contacts. The nanoscale structure of the mesopores in PLEO contacts define the device level observables such as recombination current (Jo) and junction resistance. In this work we present atomic resolution transmission electron microscopy (TEM) analysis of mesopores in PLEO contacts formed with a different processing conditions to connect provide insight into how the nanoscale structure of the SiOx layer influences PV device properties. Additionally, we have previously used electron beam induced current (EBIC) to probe local transport properties in Si PV devices with a SiOx layer containing pinholes due to high temperature processing. Using EBIC we were able to directly show the enhance charge carrier transport through the pinholes. Here we also employ EBIC to study non-uniformities in charge carrier recombination and transport associated with mesopores in PLEO contacts and compare these results with our previous work on devices with pinholes in the SiOx formed through high temperature processes. The products of this work provide critical information that is required to both further optimize performance of Si PV devices with PLEO contact and to drive future adoption of this technology by industry.

ENGINEERING,SOLAR ENERGY↗
DOE OSTI2020

Rheological behavior of neat and carbon fiber-reinforced poly(ether ketone ketone) for extrusion deposition additive manufacturing

To develop new materials for extrusion additive manufacturing (AM) systems, a fundamental understanding of rheological properties is essential to correlate the effect of processing on material structure and its properties. In this work, the rheological properties of five different grades of neat and carbon fiber (CF)-reinforced poly(ether ketone ketone) are reported. Rheological properties are essential to understand the effect of reinforcing fibers and AM process parameters such as time, temperature, environment, and shear rate on flow behavior during processing. Small-amplitude oscillatory shear tests and steady shear tests indicated neat grades to exhibit less increase in viscosity over time when processed in air than the CF-filled grades. The filled grades showed greater shear thinning and lower sensitivity to temperature. Altogether, this rheological analysis provides a broad framework for determining appropriate processing conditions for extrusion deposition AM of such high-temperature polymer systems.

36 MATERIALS SCIENCE↗
NASA NTRS2013

PROcess Based Diagnostics PROBE

Many of the aspects of the climate system that are of the greatest interest (e.g., the sensitivity of the system to external forcings) are emergent properties that arise via the complex interplay between disparate processes. This is also true for climate models most diagnostics are not a function of an isolated portion of source code, but rather are affected by multiple components and procedures. Thus any model-observation mismatch is hard to attribute to any specific piece of code or imperfection in a specific model assumption. An alternative approach is to identify diagnostics that are more closely tied to specific processes -- implying that if a mismatch is found, it should be much easier to identify and address specific algorithmic choices that will improve the simulation. However, this approach requires looking at model output and observational data in a more sophisticated way than the more traditional production of monthly or annual mean quantities. The data must instead be filtered in time and space for examples of the specific process being targeted.We are developing a data analysis environment called PROcess-Based Explorer (PROBE) that seeks to enable efficient and systematic computation of process-based diagnostics on very large sets of data. In this environment, investigators can define arbitrarily complex filters and then seamlessly perform computations in parallel on the filtered output from their model. The same analysis can be performed on additional related data sets (e.g., reanalyses) thereby enabling routine comparisons between model and observational data. PROBE also incorporates workflow technology to automatically update computed diagnostics for subsequent executions of a model. In this presentation, we will discuss the design and current status of PROBE as well as share results from some preliminary use cases.

PROBE↗
NASA NTRS2006

Observing Ice in Clouds from Space

There are many satellite observations of cloud top properties and the liquid and rain content of clouds, however, we do not yet quantitatively understand the processes that control the water budget of the upper troposphere where ice is the predominant phase, and how these processes are linked to precipitation processes and the radiative energy budget. The ice in clouds in the upper troposphere either melts into rain or is detrained, and persists, as cirrus clouds affecting the hydrological and energy cycle, respectively. Fully modeling the Earth's climate and improving weather and climate forecasts requires accurate satellite measurements of various cloud properties at the temporal and spatial scales of cloud processes. These properties include cloud horizontal and vertical structure, cloud water content and some measure of particle sizes and shapes. The uncertainty in knowledge of these ice characteristics is reflected in the large discrepancies in model simulations of the upper tropospheric water budget. Model simulations are sensitive to the partition of ice between precipitation and outflow processes, i.e., to the parameterization of ice clouds and ice processes. One barrier to achieving accurate global ice cloud properties is the lack of adequate observations at millimeter and submillimeter wavelengths (183-874 GHz). Recent advances in instrumentation have allowed for the development and implementation of an airborne submillimeter-wave radiometer. The brightness temperatures at these frequencies are especially sensitive to cirrus ice particle sizes (because they are comparable to the wavelength). This allows for more accurate ice water path estimates when multiple channels are used to probe into the cloud layers. Further, submillimeter wavelengths offer simplicity in the retrieval algorithms because they do not probe into the liquid and near surface portions of clouds, thus requiring only one term of the radiative transfer equation (ice scattering) to relate brightness temperatures to ice. The next step is a satellite mission designed to acquire global Earth radiance measurements in the submillimeter-wave region, thus bridging the measurement gap between microwave sounders and shorter-wavelength infrared and visible sensors. This presentation provides scientific justification and an approach to measuring ice water path and particle size from a satellite platform that spans a range encompassing both the hydrologically active and radiatively active components of cloud systems.

Ackerman, S.↗
DOE OSTI2024

Portable fiber optic sensor for rare earth elements and other critical metals using photoluminescence methods

Rare earth elements and other metals are vital to a range of technologies that are used in the energy and defense sectors. However, monopolistic market conditions have caused significant concern over the stability of the critical metal supply chain, and this has spurred extensive efforts in many nations to produce these metals domestically, both from conventional sources such as mining and well as from unconventional sources such as coal and its utilization byproducts. Slow and expensive characterization methods pose a significant barrier for both metals prospecting and process monitoring. A promising solution to this challenge is the development of highly sensitive luminescent sensors for metals, which can offer low costs, portability, and sensitivity. Anionic zinc adeninate metal-organic frameworks (BioMOFs) are known to distinguishing and detect part-per-billion levels of terbium, europium, samarium, and dysprosium in water by sensitizing the narrow, element-specific emission bands from these lanthanides. Here, a BioMOF material is immobilized onto a large diameter, solarization-resistant fiber optic tip integrated with a portable, low-cost spectrometer for rare earth element sensing. Immobilizing the sensing material on fiber instead of dispersing the sensing material in solution offers several advantages: it facilitates solvent removal, which enhances luminescent signal from the sensitized lanthanides, and it also allows the BioMOF to be recycled for multiple uses. The sensing system was deployed on a simulated process stream and exhibited qualitative agreement with inductively-coupled plasma mass spectrometry for terbium and europium detection, highlighting the potential for the sensing system to be deployed for real-world applications. By using different sensing materials, the same portable sensor may be deployed to detect other energy relevant metals such as cobalt, providing a cost-effective and sensitive platform for critical metal characterization.

Crawford, Scott↗
NASA NTRS1995

Credible Computations: Standard and Uncertainty

The discipline of computational fluid dynamics (CFD) is at a crossroad. Most of the significant advances related to computational methods have taken place. The emphasis is now shifting from methods to results. Significant efforts are made in applying CFD to solve design problems. The value of CFD results in design depends on the credibility of computed results for the intended use. The process of establishing credibility requires a standard so that there is a consistency and uniformity in this process and in the interpretation of its outcome. The key element for establishing the credibility is the quantification of uncertainty. This paper presents salient features of a proposed standard and a procedure for determining the uncertainty. A customer of CFD products - computer codes and computed results - expects the following: A computer code in terms of its logic, numerics, and fluid dynamics and the results generated by this code are in compliance with specified requirements. This expectation is fulfilling by verification and validation of these requirements. The verification process assesses whether the problem is solved correctly and the validation process determines whether the right problem is solved. Standards for these processes are recommended. There is always some uncertainty, even if one uses validated models and verified computed results. The value of this uncertainty is important in the design process. This value is obtained by conducting a sensitivity-uncertainty analysis. Sensitivity analysis is generally defined as the procedure for determining the sensitivities of output parameters to input parameters. This analysis is a necessary step in the uncertainty analysis, and the results of this analysis highlight which computed quantities and integrated quantities in computations need to be determined accurately and which quantities do not require such attention. Uncertainty analysis is generally defined as the analysis of the effect of the uncertainties involved in all stages of a process on the final responses. There are two approaches for conducting the uncertainty analysis: experimental and computational. These analyses and approaches are briefly described.

Mehta, Unmeel B.↗
NASA NTRSDate not supplied

Joint Acceptance Attenuation Factor of Integrated Pressure with Unsteady Pressure-Sensitive Paint Measurements

The Unsteady Pressure-Sensitive Paint (uPSP) is widely used to measure the surface pressure of scaled models in wind tunnel tests. Compared to the conventional pressure transducers, uPSP has the advantage of high spatial resolution. With multiple high-speed Complementary Metal Oxide Superconductor (CMOS) cameras, the uPSP data collected with the camera pixels are mapped to the surface grid of the scaled model and converted to pressure. The shot noise is the dominant component of the noise in the uPSP measurement. The integrated pressure is usually computed on the grid nodes of a user-defined patch. The effect of shot noise is reduced in the integrated pressure on the patch; however, the measurement of the aerodynamic pressure may also be attenuated by the decorrelation of the flow pressure field being measured. This paper discusses the Joint Acceptance Attenuation Factor (JAAF) of the integrated pressure with uPSP measurements. The JAAF, a function of frequency, is defined as the ratio of the Power Spectral Density (PSD) of the integrated aerodynamic pressure on the patch to the average PSD of the aerodynamic pressure on the grid nodes of the patch. In this paper, the JAAF is investigated for the integrated pressure on rectangular patches, whose edges are defined in the direction along the streamline or across the streamline. Based on the assumption that the surface pressure field can be described by the Corcos model, the closed-form formulas to compute the JAAFs of the integrated pressure on the discrete grid nodes of a rectangular patch and over the continuous area of a rectangular patch are derived respectively. It is shown that the JAAF of the integrated pressure over the continuous area of a rectangular patch is the limit of that on discrete nodes of the rectangular patch when the number of nodes in each row or column goes to infinity. The closed-form formulas of the JAAF derived in this paper, with estimated parameters of the model, are verified with the measurements of the uPSP and the conventional pressure transducer collected in the Space Launch System Ascent Unsteady Aerodynamics Test at NASA Ames Research Center in November 2017. The closed-form formulas of the JAAF of the integrated pressure on the rectangular patches, based on the Corcos model, provide an efficient method to estimate the attenuation of integration by the decorrelation of the flow pressure field and set references for the comparison of the spectrum of the integrated uPSP measurements and the conventional pressure transducer measurements. The work described in this paper is a part of NASA’s development of a new state-of-the-art uPSP capability in production wind tunnels. Funding was provided by the NASA Aerosciences Evaluation and Test Capabilities Portfolio Office.

acoustics↗
NASA NTRSDate not supplied

Joint Acceptance Attenuation Factor of Integrated Pressure with Unsteady Pressure-Sensitive Paint Measurements

The Unsteady Pressure-Sensitive Paint (uPSP) is widely used to measure the surface pressure of scaled models in wind tunnel tests. Compared to the conventional pressure transducers, uPSP has the advantage of high spatial resolution. With multiple high-speed Complementary Metal Oxide Superconductor (CMOS) cameras, the uPSP data collected with the camera pixels are mapped to the surface grid of the scaled model and converted to pressure. The shot noise is the dominant component of the noise in the uPSP measurement. The integrated pressure is usually computed on the grid nodes of a user-defined patch. The effect of shot noise is reduced in the integrated pressure on the patch; however, the measurement of the aerodynamic pressure may also be attenuated by the decorrelation of the flow pressure field being measured. This paper discusses the Joint Acceptance Attenuation Factor (JAAF) of the integrated pressure with uPSP measurements. The JAAF, a function of frequency, is defined as the ratio of the Power Spectral Density (PSD) of the integrated aerodynamic pressure on the patch to the average PSD of the aerodynamic pressure on the grid nodes of the patch. In this paper, the JAAF is investigated for the integrated pressure on rectangular patches, whose edges are defined in the direction along the streamline or across the streamline. Based on the assumption that the surface pressure field can be described by the Corcos model, the closed-form formulas to compute the JAAFs of the integrated pressure on the discrete grid nodes of a rectangular patch and over the continuous area of a rectangular patch are derived respectively. It is shown that the JAAF of the integrated pressure over the continuous area of a rectangular patch is the limit of that on discrete nodes of the rectangular patch when the number of nodes in each row or column goes to infinity. The closed-form formulas of the JAAF derived in this paper, with estimated parameters of the model, are verified with the measurements of the uPSP and the conventional pressure transducer collected in the Space Launch System Ascent Unsteady Aerodynamics Test at NASA Ames Research Center in November 2017. The closed-form formulas of the JAAF of the integrated pressure on the rectangular patches, based on the Corcos model, provide an efficient method to estimate the attenuation of integration by the decorrelation of the flow pressure field and set references for the comparison of the spectrum of the integrated uPSP measurements and the conventional pressure transducer measurements. The work described in this paper is a part of NASA’s development of a new state-of-the-art uPSP capability in production wind tunnels. Funding was provided by the NASA Aerosciences Evaluation and Test Capabilities Portfolio Office.

acoustics↗
DOE OSTI2023

Search for Rare Processes: Mu2e and KOTO

The Standard Model (SM) of particle physics has been very successful in describing the fundamental forces, the properties of elementary particles, and predicting particles prior to their discovery, for example the top quark and the Higgs boson. Yet the SM does not explain all phenomena, and discoveries of physics processes beyond the SM will allow progress in our understanding of the fundamental nature of matter and forces. The search for rare processes is one of the paths to look for new physics. Two of these searches are for muon to electron conversion and the decay $\text{K}_\text{L}\rightarrow \pi^0 \nu \bar{\nu}$. Our main effort was in the Mu2e experiment under construction at Fermilab, which has the goal of searching for the neutrinoless conversion of a muon into an electron at a single event sensitivity of 2.87 x 10-17 and, in the process, provide evidence of physics processes beyond the Standard Model. We developed the firmware to be used in the Mu2e tracker readout, assisted in the construction and operation of the Mu2e Vertical Slice Test, and provided input to studies of cosmic event reconstructions in Mu2e using simulated data. Under this reward we also concluded our effort in two KOTO experiment in J-PARC, Japan and set a limit on the rate of the rare decay, $\text{K}_\text{L}\rightarrow \pi^0 \nu \bar{\nu}$ using the data collected in the 2016-2018 period. We also maintained and operated the DAQ system used for data collection thru 2021.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2026

Semi-Transparent Perovskite Solar Cells in a Stacked Tandem Module: Cooperative Research and Development Final Report, CRADA Number CRD-19-00810

This project seeks to develop device design, materials composition, and processing tools and parameters to fabricate semi-transparent perovskite solar cells and modules for application in stand-alone products or added to other solar cells in a mechanically stacked tandem configuration. This technology presents significant advanced manufacturing challenges and opportunities in getting to scale, including development of perovskite inks, scalable perovskite and heterojunction deposition and annealing processes, heterojunction composition, transparent electrode composition and deposition process, anti-reflection layer composition and deposition process, and cell to module integration processes. Modification 5: The proposed project seeks to develop device design, materials composition, and processing tools and parameters to fabricate semi-transparent perovskite solar cells and modules for application in stand-alone products or added to other solar cells in a mechanically-stacked tandem configuration. This technology presents significant advanced manufacturing challenges and opportunities in getting to scale, including development of perovskite inks, scalable perovskite and heterojunction deposition and annealing processes, heterojunction composition, transparent electrode composition and deposition process, passivation layers including in module scribes, anti-reflection layer composition and deposition process, and cell to module integration processes. Advanced metrology and characterization will be performed on perovskite films, cells and module. Furthermore, we will examine module or materials recycling for circular economy considerations. Modifcation 6: Gigahertz frequency microwave pump-probe spectroscopies are highly sensitive to thin film semiconductor photoconductivity of individual and stacks of layers that comprise perovskite solar cells. As such, these techniques will be used to qualify reproducibility and quality correlations during the manufacturing process. Modification 7: Mechanical adhesion of top contacts within perovskite modules significantly impacts the durability of the module when exposed to accelerated degradation testing. The adhesion between the perovskite/transport layer interface and the transport layer/top contact interface are both very sensitive small changes in processing. ALD processing conditions of the transport layer will be tuned to optimize the mechanical adhesion within the perovskite module stack.

14 SOLAR ENERGY↗
NASA NTRS2002

Method and Apparatus for Evaluating the Visual Quality of Processed Digital Video Sequences

A Digital Video Quality (DVQ) apparatus and method that incorporate a model of human visual sensitivity to predict the visibility of artifacts. The DVQ method and apparatus are used for the evaluation of the visual quality of processed digital video sequences and for adaptively controlling the bit rate of the processed digital video sequences without compromising the visual quality. The DVQ apparatus minimizes the required amount of memory and computation. The input to the DVQ apparatus is a pair of color image sequences: an original (R) non-compressed sequence, and a processed (T) sequence. Both sequences (R) and (T) are sampled, cropped, and subjected to color transformations. The sequences are then subjected to blocking and discrete cosine transformation, and the results are transformed to local contrast. The next step is a time filtering operation which implements the human sensitivity to different time frequencies. The results are converted to threshold units by dividing each discrete cosine transform coefficient by its respective visual threshold. At the next stage the two sequences are subtracted to produce an error sequence. The error sequence is subjected to a contrast masking operation, which also depends upon the reference sequence (R). The masked errors can be pooled in various ways to illustrate the perceptual error over various dimensions, and the pooled error can be converted to a visual quality measure.

Watson, Andrew B.↗
DOE OSTI2024

Characterization of latent image of electron beam resist via critical-dimension resonant soft X-ray scattering

Metrology plays a crucial role in semiconductor manufacturing by providing accurate and precise measurement and characterization of critical parameters. With the development of high-resolution extreme ultraviolet lithography (EUVL) processes, critical dimensions are shrinking to sub-10 nm. Resist materials encounter the challenge of providing heightened sensitivity and a handle on exacerbating stochastic variations. A comprehensive understanding of the chemical profile of the latent image is pivotal for mitigating stochastic effects and optimizing pattern quality. However, the subtle differences in chemistry between the exposed and unexposed regions of the resists make it extremely challenging to characterize the latent images with sub-nanometer precision. Here, we develop the metrology with critical-dimension resonant soft X-ray scattering (CD-RSoXS) to probe the chemical profiles of latent images stored in resist after exposure. The combination of absorption spectroscopy and enhanced scattering contrast makes it possible to characterize the subtle structural and chemical variations in the latent image. Moreover, the results of the measurements are compared with the simulations with a finite element method–based Maxwell solver to extract a detailed profile of the latent and developed images. We demonstrate that the CD-RSoXS technique can provide valuable insights into the high spatial resolution and local chemical sensitivity simultaneously, which is crucial to understanding the resolution limits and stochastic effects in EUVL processes.

36 MATERIALS SCIENCE↗
NASA NTRS2004

Sensitivity Equation Derivation for Transient Heat Transfer Problems

The focus of the paper is on the derivation of sensitivity equations for transient heat transfer problems modeled by different discretization processes. Two examples will be used in this study to facilitate the discussion. The first example is a coupled, transient heat transfer problem that simulates the press molding process in fabrication of composite laminates. These state equations are discretized into standard h-version finite elements and solved by a multiple step, predictor-corrector scheme. The sensitivity analysis results based upon the direct and adjoint variable approaches will be presented. The second example is a nonlinear transient heat transfer problem solved by a p-version time-discontinuous Galerkin's Method. The resulting matrix equation of the state equation is simply in the form of Ax = b, representing a single step, time marching scheme. A direct differentiation approach will be used to compute the thermal sensitivities of a sample 2D problem.

Hou, Gene↗
DOE OSTI2025

Surface Trap Dynamics and Gamma‐Ray Detection Enhancement in Passivated FAPbBr 3 Perovskite Crystals

Perovskite‐based direct radiation detectors offer a compelling platform for room‐temperature gamma spectroscopy due to their high sensitivity, tunable optoelectronic properties, and compatibility with solution processing. While prior studies on formamidinium lead tribromide (FAPbBr 3 ) have shown that surface passivation mitigates deep trap state impact on the charge collection efficiency (CCE), the influence of surface‐based shallow traps on time‐resolved detector response remains largely unexplored. In this article, a digital signal processing (DSP) method is applied to analyze waveform rising edge dynamics in FAPbBr 3 single‐crystal detectors, identifying prompt and delayed charge collection components. Using the second derivative of the collected charge signal, the onset of shallow trap reemission is isolated, occurring 1.1 µs after carrier generation. Surface passivation suppressed deep trap states, shifting carrier occupancy toward shallower traps and extending the temporal window of delayed charge collection. This delayed contribution correlates with measurable changes in the temporal and amplitude distributions of detector events. By leveraging time‐domain filtering informed by these dynamics, a selective enhancement in signal quality and gamma peak‐to‐Compton ratio (PCR) is achieved, while preserving over 90% of photoelectric events. An improvement in the PCR to 1.80, from the original 1.09, is enabled by focusing on high collection efficiency events corresponding to reemitted carriers in the 1.1 to 3 µs range after the generation event. These results demonstrate a pathway for leveraging shallow trap dynamics to enhance spectral fidelity in time‐resolved perovskite detectors.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Direct Visualization of Defect‐Controlled Diffusion in van der Waals Gaps

Abstract Diffusion processes govern fundamental phenomena such as phase transformations, doping, and intercalation in van der Waals (vdW) bonded materials. Here, the diffusion dynamics of W atoms by visualizing the motion of individual atoms at three different vdW interfaces: hexagonal boron nitride (BN)/vacuum, BN/BN, and BN/WSe 2 , by recording scanning transmission electron microscopy movies is quantified. Supported by density functional theory (DFT) calculations, it is inferred that in all cases diffusion is governed by intermittent trapping at electron beam‐generated defect sites. This leads to diffusion properties that depend strongly on the number of defects. These results suggest that diffusion and intercalation processes in vdW materials are highly tunable and sensitive to crystal quality. The demonstration of imaging, with high spatial and temporal resolution, of layers and individual atoms inside vdW heterostructures offers possibilities for direct visualization of diffusion and atomic interactions, as well as for experiments exploring atomic structures, their in situ modification, and electrical property measurements of active devices combined with atomic resolution imaging.

Chemistry↗
DOE OSTI2025

Preliminary Insights Into the Feasibility of Determining the Purification Date of Enriched Uranium by Direct Measurement of the 230 Th/ 234 U Ratio Using an All-Faraday Detector Configuration on the Neoma MC-ICP-MS

Rationale: Mass spectrometric measurement of the 230 Th/ 234 U ratio to calculate the purification age of enriched uranium is typically conducted via a combination of ion counters and faraday detectors, thus requiring an inter-detector calibration scheme. Here, our aim is to understand whether the pursuit of a simplified measurement scheme involving only faraday detectors is feasible. Methods: We investigate the possibility of determining U-Th model ages for two enriched uranium standards (NBL U630 and U850) by direct measurement of the 230 Th/ 234 U ratio (without chromatographic separation or isotope dilution) on a ThermoFisher Scientific Neoma MC-ICP-MS utilizing both solution and laser ablation (LA)-based sampling techniques and an all-faraday detector configuration. Results: For the solution mode analyses conducted on aliquots containing sub μg/mL total U, we produce composite average 230 Th/ 234 U model dates of May 19, 1988 (± 351 days), and March 26, 1961 (± 2.5 years) using the directly measured 230 Th/ 234 U ratios for the NBL U630 and U850 uranium standards, which have certified purification dates of June 6, 1988 (± 190 days), and December 31, 1957 (± 36.5 days), respectively. The ages produced by LA-based sampling of dried residues of the same standards deposited onto cotton TexWipes are less accurate and of poorer precision (June 23, 2004 ± 8.7 years for U630 and December 21, 1965 ± 7.9 years for U850) but still yield meaningful information in regards to the purification date. Conclusions: We believe that further refinement of the all faraday detector measurement approach to include development of a more robust Th/U relative sensitivity factor determination, signal cutoff selection, and data processing protocols will allow for this approach to be confidently applied to enriched uranium materials with unknown purification histories. Potential advantages of the method include the reduced sample handling and infrastructure requirements as well as the ability to simultaneously generate a broad picture of the uranium isotopic composition in tandem with the U-Th age determination.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗