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At least 343 records · Page 19

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DOE OSTI2025

Bidirectional Suzuki Catalyst Transfer Polymerization of Poly( p -phenylene)

Suzuki catalyst transfer polymerization (SCTP) has emerged as an effective method for accessing length-controlled π-conjugated poly(p-phenylene). Regio-controlled functional group sequencing along the backbone and the chain ends of synthetic polymers remains a challenge for the successful integration of organic semiconductors in sensors and electronic devices. Here, we report a bidirectional SCTP system based on dinuclear palladium(II) initiators. Functional groups transferred during the initiation and termination steps unlock independently addressable synthetic handles at the polymer core and respective chain ends. These functional groups open opportunities for late-stage regio-controlled and chemoselective derivatizations. Control over key polymer parameters, including molecular weight (M n ), dispersity ( Đ = M w /M n ), degree of polymerization ( DP ), termination efficiency, and functional group interconversion, is corroborated by size exclusion chromatography (SEC) and NMR spectroscopy. The modular design of SCTP initiators, in combination with commercially available terminating groups, represents a highly flexible toolbox for late-stage polymer conjugation, e.g., chemoselective anchoring groups for integration with functional electronics or bioorthogonal conjugation for molecular sensing.

Aldehydes↗

DOE OSTI2024

ZIF-8 Vibrational Spectra: Peak Assignments and Defect Signals

In this study, Zeolitic Imidazolate Framework-8 (ZIF-8) is a promising material for gas separation applications. It also serves as a prototype for numerous ZIFs, including amorphous ones, with a broader range of possible applications, including sensors, catalysis, and lithography. It consists of zinc coordinated with 2-methylimidazolate (2mIm) and has been synthesized with methods ranging from liquid-phase to solvent-free synthesis, which aim to control its crystal size and shape, film thickness and microstructure, and incorporation into nanocomposites. Depending on the synthesis method and post-synthesis treatments, ZIF-8 materials may deviate from the nominal defect-free ZIF-8 crystal structure due to defects like missing 2mIm, missing zinc, and physically adsorbed 2mIm trapped in the ZIF-8 pores, which may alter its performance and stability. Infra-red (IR) spectroscopy has been used to assess the presence of defects in ZIF-8 and related materials. However, conflicting interpretations by various authors persist in the literature. Here, we systematically investigate ZIF-8 vibrational spectra by combining experimental IR spectroscopy and first-principles molecular dynamics simulations, focusing on assigning peaks and elucidating the spectroscopic signals of putative defects present in ZIF-8 material. We attempt to resolve conflicting assignments from the literature and to provide a comprehensive understanding of the vibrational spectra of ZIF-8 and its defect-induced variations, aiming towards more precise quality control and design of ZIF-8-based materials for emerging applications.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Excitonic density wave and spin-valley superfluid in bilayer transition metal dichalcogenide

Artificial moiré superlattices in 2 d van der Waals heterostructures are a new venue for realizing and controlling correlated electronic phenomena. Recently, twisted bilayer WSe 2 emerged as a new robust moiré system hosting a correlated insulator at moiré half-filling over a range of twist angle. In this work, we present a theory of this insulating state as an excitonic density wave due to intervalley electron–hole pairing. We show that exciton condensation is strongly enhanced by a van Hove singularity near the Fermi level. Our theory explains the remarkable sensitivity of the insulating gap to the vertical electric field. In contrast, the gap is weakly reduced by a perpendicular magnetic field, with quadratic dependence at low field. The different responses to electric and magnetic field can be understood in terms of pair-breaking versus non-pair-breaking effects in a BCS analog of the system. We further predict superfluid spin transport in this electrical insulator, which can be detected by optical spin injection and spatial-temporal imaging.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2023

High-fidelity parallel entangling gates on a neutral-atom quantum computer

The ability to perform entangling quantum operations with low error rates in a scalable fashion is a central element of useful quantum information processing. Neutral-atom arrays have recently emerged as a promising quantum computing platform, featuring coherent control over hundreds of qubits and any-to-any gate connectivity in a flexible, dynamically reconfigurable architecture. The main outstanding challenge has been to reduce errors in entangling operations mediated through Rydberg interactions. Here we report the realization of two-qubit entangling gates with 99.5% fidelity on up to 60 atoms in parallel, surpassing the surface-code threshold for error correction. Our method uses fast, single-pulse gates based on optimal control, atomic dark states to reduce scattering and improvements to Rydberg excitation and atom cooling. We benchmark fidelity using several methods based on repeated gate applications, characterize the physical error sources and outline future improvements. Finally, we generalize our method to design entangling gates involving a higher number of qubits, which we demonstrate by realizing low-error three-qubit gates. By enabling high-fidelity operation in a scalable, highly connected system, these advances lay the groundwork for large-scale implementation of quantum algorithms, error-corrected circuits and digital simulations.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2021

Design nanoporous metal thin films via solid state interfacial dealloying

Thin-film solid-state interfacial dealloying (thin-film SSID) is an emerging technique to design nanoarchitecture thin films. The resulting controllable 3D bicontinuous nanostructure is promising for a range of applications including catalysis, sensing, and energy storage. Using a multiscale microscopy approach, we combine X-ray and electron nano-tomography to demonstrate that besides dense bicontinuous nanocomposites, thin-film SSID can create a very fine (5–15 nm) nanoporous structure. Not only is such a fine feature among one of the finest fabrications by metal-agent dealloying, but a multilayer thin-film design enables creating nanoporous films on a wider range of substrates for functional applications. Through multimodal synchrotron diffraction and spectroscopy analysis with which the materials’ chemical and structural evolution in this novel approach is characterized in details, we further deduce that the contribution of change in entropy should be considered to explain the phase evolution in metal-agent dealloying, in addition to the commonly used enthalpy term in prior studies. Here, the discussion is an important step leading towards better explaining the underlying design principles for controllable 3D nanoarchitecture, as well as exploring a wider range of elemental and substrate selections for new applications.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Effect of Gamma Radiation on TaOₓ ECRAM

Electrochemical random access memory (ECRAM) is an emerging three-terminal nonvolatile memory (NVM) with highly controllable channel conductance which is promising for use as an analog memory (or synapse) in analog in-memory computing (IMC) systems. Energy-efficient analog IMC computing is particularly desirable for power-constrained, high-radiation environments such as satellites. However, little is known about the suitability of ECRAM for use in a total ionizing dose (TID) environment. Here, this work investigates the effect of Co-60 gamma radiation on the channel conductance and noise—two properties critical for analog IMC systems—of a TaO x -based ECRAM up to 17.3 Mrad(SiO 2 ) for both low- and high-channel-conductance state devices. A transient increase in conductance is observed in response to radiation which consists of two elements: an immediate increase in conductivity due to photocurrent and a secondary increase in conductivity, which has a slower rise and saturation and can persist for hours after exposure. This secondary, persistent photoconductivity is attributed to charging caused by hole trapping. These transient effects would not likely occur in a space environment due to the low dose rate compared with this experiment. No permanent change is found in the low conductance state (LCS) following exposure and the minor shift in the high conductance change would be less significant than the regular retention decay in this state. A permanent increase in the random telegraph noise is observed, possibly due to increased traps created in the channel. This work demonstrates that TaO x -based ECRAM is suitable for use in spaceborne analog IMC systems that are subject to significant TID.

ECRAM↗

DOE OSTI2022

Results From Invoking Artificial Neural Networks to Measure Insider Threat Detection & Mitigation

Advances on differentiating between malicious intent and natural “organizational evolution” to explain observed anomalies in operational workplace patterns suggest benefit from evaluating collective behaviors observed in the facilities to improve insider threat detection and mitigation (ITDM). Advances in artificial neural networks (ANN) provide more robust pathways for capturing, analyzing, and collating disparate data signals into quantitative descriptions of operational workplace patterns. In response, a joint study by Sandia National Laboratories and the University of Texas at Austin explored the effectiveness of commercial artificial neural network (ANN) software to improve ITDM. Overall, this research demonstrates the benefit of learning patterns of organizational behaviors, detecting off-normal (or anomalous) deviations from these patterns, and alerting when certain types, frequencies, or quantities of deviations emerge for improving ITDM. Evaluating nearly 33,000 access control data points and over 1,600 intrusion sensor data points collected over a nearly twelve-month period, this study's results demonstrated the ANN could recognize operational patterns at the Nuclear Engineering Teaching Laboratory (NETL) and detect off-normal behaviors—suggesting that ANNs can be used to support a data-analytic approach to ITDM. Several representative experiments were conducted to further evaluate these conclusions, with the resultant insights supporting collective behavior-based analytical approaches to quantitatively describe insider threat detection and mitigation.

45 MILITARY TECHNOLOGY, WEAPONRY, AND NATIONAL DEF↗

DOE OSTI2021

Microcontroller-based aerosol jet printer control software

This software is used with a microcontroller to control an aerosol jet printing system. It was written for a 32-bit ARM microcontroller, providing greater processing speed and complexity relative to more conventional low-cost printer controllers. The microcontroller software was written using a real-time operating system (FreeRTOS), which simplifies parallel operation of multiple functions and further customization. It supports simultaneous motion planning, pulse generation for stepper motors, reading encoder feedback, communicating with multiple mass flow controllers, controlling solid state relays, handling a software-based emergency stop, and sending data to the client PC. The program is written in C and communicates with the client PC via USB connection. Sandia National Laboratories is a multi-mission laboratory managed and operated by National Technology & Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International Inc., for the U.S. Department of Energy’s National Nuclear Security Administration under contract DE-NA0003525. SAND2021-0436 O

Secor, EthanBenjamin↗

DOE OSTI2023

Sociodemographic effects on pandemic fatigue are multifaceted and context-specific: A longitudinal analysis of physical distancing adherence

Pandemic fatigue emerged early during the COVID-19 pandemic and remains a concern as new variants emerge and ongoing public health measures are needed to control them. A wide range of factors can affect pandemic fatigue, but empiric research indicating which may be most important to adherence in specific populations is lacking. We conducted a longitudinal study of changes in physical distancing in two cohorts: adults living with children <18 years and adults ≥50 years old. Six types of non-work, non-household contacts were ascertained at six times from April to October 2020. We used generalized estimating equations Poisson regression to estimate the one-week change in contact rate and how this differed based on sociodemographic characteristics. The rate of all contact types increased during the middle of the study period and decreased toward the end. Changes in contact rates over time differed according to several sociodemographic characteristics, including age, gender, race/ethnicity, education, household composition, and access to transportation. Furthermore, the factors influencing the rate of change in contact rates differed by the type or setting of the contact, for example contacts as a result of visiting another person’s home versus during a retail outing. These results provide evidence for potential mechanisms by which pandemic fatigue has resulted in lower physical distancing adherence.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2022

Start-up and Emergency Shutdown Modeling for a Coal-fired 10MWe sCO₂ Power Plant

As part of a Phase II Front End Engineering Design (FEED) study for the DOE Fossil Fuel Large Scale Pilots program, investigations of novel start-up and emergency shutdown methods for a stoker-fed, coal-fired, 10MWe sCO₂ power plant proposal were performed. These investigations were performed using 1D transient system models of the plant created within the GT-SUITE system modeling platform. The system model components were created using vendor quotation data (heat exchangers), performance maps (turbomachines), or FMU models (fired heater). Previously, Echogen Power Systems (Echogen) has used a sCO₂ power cycle start-up method that fills the system with liquid CO₂ to facilitate easy use of an electrically-driven start pump to transition the system from initial CO₂ fill to turbo-compressor initialization. The novel start-up method presented attempts this transition with a minimal filling of the system with liquid CO₂, to reduce the total CO₂ inventory required. This method leaves the start pump vulnerable to a two phase inlet condition as system pressure is below the CO₂ saturation pressure for the condenser cooling water temperature (Tcw). System model cases at Tcw of 18°C, 26°C, and 32°C, corresponding to cold, design, and hot ambient days, were analyzed to determine if the SP inlet condition could be kept as a subcooled liquid and estimate the CO₂ inventory reduction amount./p> Stoker-fed, coal-fired heaters continue to emit heat for some time even after emergency shutdown from events such as a power failure. This heat emission would lead to a failure of the fired heater, as the metal overheats, if the CO₂ flow is shut off. The emergency shutdown method presented utilizes CO₂ vented by a controllable vent valve (CRV) to provide CO₂ cooling flow to the fired heater. To determine the effectiveness of this method at keeping the fired heater peak tubing metal temperature below the ASME material temperature limit, for pressures below 5 MPa, of 816 °C, system model cases with CRV diameters ranging from 4” to 10”, and an alternative CO₂ vent routing with CRV size of 6”, were investigated./p>

01 COAL, LIGNITE, AND PEAT↗

DOE OSTI2025

Idaho National Laboratory’s Mobile Hot Cell Transportation: Engineering Solutions for Global Disused Sealed Radioactive Sources.

Title: Idaho National Laboratory’s Mobile Hot Cell Transportation: Engineering Solutions for Global Disused Sealed Radioactive Sources. Abstract: The Mobile Hot Cell (MHC), currently under development by Idaho National Laboratory (INL) for the Off-Site Source Recovery Project (OSRP), is designed to help international partners meet the unique challenges of end-of-life radioactive material management. The MHC will provide a critical resource for countries that require assistance securing and disposing of Disused Sealed Radioactive Sources (DSRS) and orphaned sources in challenging environments, allowing these sources to be secured against misuse and nefarious activities. The MHC is a rapidly deployable system for conditioning and preparing end-of-life radioactive sources for transportation or storage. It is designed to handle sources of up to 1,000 Ci Co-60 equivalent while maintaining full radiological and biological containment. It will be deployable within 48 hours of an alert, making it ideal for emergency situations. The MHC features an operational suite for control, support racks for electronics, pneumatics, and welding systems, and a modular robust steel structure providing radiological shielding and internal robotic support. This design allows configurations for multiple device types to be conditioned and the ability to safely manage routine issues such as leaking or damaged sources. The MHC has been designed with the transportation challenges of rapid deployment to difficult environments in mind. The system weighs approximately 150,000 pounds, with individual systems breaking down into pieces not exceeding 20,000 pounds. Components are to be transportable on standard 20ft ISO containers, with shielding shells on 20ft flat racks. It is estimated that a total of eight containers and flat racks will be required. The use of 20ft containers, as opposed to 40ft containers, minimizes the impact on less developed road infrastructures, enabling the MHC to be positioned in constrained environments such as hospital parking lots. The system’s modularity also allows for deployment using smaller equipment, such as a 10-ton boom truck or forklift, which is crucial given the potential logistical challenges in different countries. This transportation strategy, evaluated in collaboration with Utah State University, ensures the MHC can be deployed via ground, rail, sea, or air, addressing the primary concern of international transport logistics.

99 - GENERAL AND MISCELLANEOUS↗

DOE OSTI2023

Impact of Control on Availability and Cycling of Residential HVAC in a Real-World Experiment

Demand response is an important emerging part of smart grids and there is a large stream of research from theoretical and modeling perspectives. However, there is relatively little experimental evidence that could help researchers and building operators make informed decisions on best practices for modeling, developing, and deployment of control mechanisms. We contribute to the body of experimental research by providing numerical insights into the role and availability of residential HVAC systems for control. We share the findings on the duration of the cooling cycle, off cycle, and temperature settling time of HVAC systems from data collected from a smart neighborhood located in Atlanta, GA.

cycling↗

DOE OSTI2023

Adaptive changes in sexual behavior in the high–risk population in response to human monkeypox transmission in Canada can help control the outbreak: Insights from a two–group, two–route epidemic model

Monkeypox, a zoonotic disease, is emerging as a potential sexually transmitted infection/disease, with underlying transmission mechanisms still unclear. We devised a risk-structured, compartmental model, incorporating sexual behavior dynamics. We compared different strategies targeting the high-risk population: a scenario of control policies geared toward the use of condoms and/or sexual abstinence (robust control strategy) with risk compensation behavior change, and a scenario of control strategies with behavior change in response to the doubling rate (adaptive control strategy). Monkeypox's basic reproduction number is 1.464, 0.0066, and 1.461 in the high-risk, low-risk, and total populations, respectively, with the high-risk group being the major driver of monkeypox spread. Policies imposing condom use or sexual abstinence need to achieve a 35% minimum compliance rate to stop further transmission, while a combination of both can curb the spread with 10% compliance to abstinence and 25% to condom use. With risk compensation, the only option is to impose sexual abstinence by at least 35%. Adaptive control is more effective than robust control where the daily sexual contact number is reduced proportionally and remains constant thereafter, shortening the time to epidemic peak, lowering its size, facilitating disease attenuation, and playing a key role in controlling the current outbreak.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2024

Arbitrary electro-optic bandwidth and frequency control in lithium niobate optical resonators

In situ tunable photonic filters and memories are important for emerging quantum and classical optics technologies. However, most photonic devices have fixed resonances and bandwidths determined at the time of fabrication. Here we present an in situ tunable optical resonator on thin-film lithium niobate. By leveraging the linear electro-optic effect, we demonstrate widely tunable control over resonator frequency and bandwidth on two different devices. We observe up to ∼50 × tuning in the bandwidth over ∼50 V with linear frequency control of ∼230 MHz/V. We also develop a closed-form model predicting the tuning behavior of the device. This paves the way for rapid phase and amplitude control over light transmitted through our device.

42 ENGINEERING↗

DOE OSTI2021

Enhanced Interface-Driven Perpendicular Magnetic Anisotropy by Symmetry Control in Oxide Superlattices

Perpendicular magnetic anisotropy (PMA) has recently been shown to emerge at interfaces of 3d and 5d transition-metal oxides (TMOs). However, strategies to systematically stabilize such interface-driven PMA still remains elusive, hindering further applications of this design approach. Here, tuning crystal symmetry is shown to be an effective means to engineer this interfacial phenomenon. The evolution of PMA strength as a function of ferromagnetic oxide thickness quantitatively reveals the competition between volume- and interface-specific contributions that determine the magnetic anisotropy. By applying different degrees of epitaxial strain, the relative contributions to PMA are modulated, clearly revealing their correlations with crystal symmetries. To be more specific, the volume anisotropy energy is found to be correlated with the tetragonal distortion of the ferromagnetic layer, while the interface anisotropy energy is mainly modulated by the octahedral tilting at the interface. With these insights, superlattices with enhanced interface-driven PMA and higher Curie temperature are realized. These findings reveal a route to engineering interface-driven PMA and associated magnetic phenomena in TMO heterostructures for future spintronic applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2020

Ligand-Mediated Phase Control in Colloidal AgInSe 2 Nanocrystals

Synthetic studies of colloidal nanoparticles that crystallize in metastable structures represent an emerging area of interest in the development of novel functional materials, as metastable nanomaterials may exhibit unique properties when compared to their counterparts that crystallize in thermodynamically preferred structures. Herein, we demonstrate how phase control of colloidal AgInSe 2 nanocrystals can be achieved by performing reactions in the presence, or absence, of coordinating ligands that can act as cation exchange mediators (i.e., oleylamine or 1-dodecanethiol). These coordinating ligands play a crucial role in formation of metastable AgInSe 2 nanocrystals, as they mediate in-situ topotactic conversion of an orthorhombic Ag2Se intermediate to a metastable orthorhombic phase of AgInSe 2 . We pro-vide a detailed mechanistic crystal chemistry description of this process to structurally elucidate how the orthorhombic phase of AgInSe 2 forms. Density functional theory calculations suggest that the metastable orthorhombic phase of AgInSe 2 is metastable by a small margin, at 10 meV/atom above the thermodynamic ground state. In the absence of oleylamine or 1-dodecanethiol, Ag 2 Se nanocrystal intermediates convert through kinetically slow, non-topotactic conversion processes to yield the thermodynamically preferred chalcopyrite structure of AgInSe 2 . Furthermore, on the basis of these discoveries, we offer new insight into the prediction of novel metastable multinary nanocrystal phases that do not exist on bulk phase diagrams.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Combustion, criteria pollutant and soot property assessment of mixing-controlled high-load engine operation with gasoline and diesel

Gasoline compression ignition (GCI) is an emerging technology that can achieve high fuel efficiency and low criteria emissions in diesel engine platforms using gasoline and gasoline-like fuels. While low- and mid-range loads are enabled with low temperature combustion (LTC) approaches, high-loads are more efficient with high temperature combustion (HTC) requiring mixing-controlled combustion (MCC). Lower soot emissions are achieved with gasoline even in high-load MCC than with diesel, but detailed soot properties from gasoline and diesel have been rarely discussed. In order to better understand how high-load operations affect soot properties, in this study gasoline and diesel were tested in a six-cylinder heavy duty engine at 14 bar brake mean effective pressure (BMEP) at similar combustion phasing. Effects of pilot mass ratio and EGR on heat release rates, cylinder temperatures, ignition delay (ID) and combustion duration (CD) were examined, relating with emissions variations with applications of the two fuels. Soot mass and particle number emissions were slightly lower with gasoline than with diesel, resulting in a more favorable NOx-soot trade-off with gasoline like other reports. Contrary to other findings in the literature, gasoline and diesel soot samples presented similar particle distribution shapes, carbon crystalline structures and primary particle sizes, regardless of fuel type and EGR rate. Consequently, the current result proposes that soot particles have undergone similar soot formation and oxidation processes despite reactivity difference and oxygen availability under the examined high-load MCC with similar combustion phases.

02 PETROLEUM↗

DOE OSTI2024

Customer enrollment and participation in building demand management programs: A review of key factors

Increasing the efficiency and flexibility of electricity demand is necessary for ensuring a cost-effective and reliable transition to zero-carbon electricity systems. Such demand-side management (DSM) resources have been procured by utilities for decades via energy efficiency and demand response programs; however, the key drivers of program enrollment and customer participation levels remain poorly understood — even as governments and grid planners seek to scale up the deployment of DSM assets to meet climate targets. Here we systematically review the evidence on multiple factors that may influence customer enrollment and participation in building DSM programs, focusing primarily on residential and commercial buildings. We examine the contexts in which relationships between DSM factors and outcomes are most often explored and with which methods; we also score the strength, direction, and internal consistency of each factor's reported impact on the enrollment and participation outcomes. We find that studies most commonly assess the effects of economic incentives for load flexibility on program participation levels, often using simulation-based methods in lieu of measured data. Few studies focus on program enrollment outcomes or regulatory drivers of either enrollment or participation, and gaps are also evident in the coverage of emerging DSM opportunities like load electrification. Removal of structural barriers (e.g., the lack of controls infrastructure) and the use of third party services (e.g., load aggregators) are the factors with the largest positive impacts on DSM outcomes, but no single factor emerges as clearly most impactful. For a given factor, the range of reported impacts typically varies widely across the relevant studies reviewed. Our findings provide a snapshot of the state of knowledge about building DSM and customer decision-making, and they expose key gaps in understanding that must be filled if building DSM is to expand as a critical resource for operating clean power grids.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗