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DOE OSTI2020

Room‐Temperature Phosphorescent Platinum(II) Alkynyls with Microsecond Lifetimes Bearing a Strong‐Field Pincer Ligand

Abstract The use of organometallic triplet emitters in organic light emitting diodes (OLEDs) is motivated by the premise of efficient intersystem crossing leading to unit internal quantum efficiencies. However, since most devices are based on solid‐state components, an inherent limitation to square‐planar platinum(II) phosphors is their tendency toward aggregation‐based quenching. Here, a new class of emissive, four‐coordinate Pt II species based on the bisimidazolyl carbazolide (BIMCA) ligand is introduced, which displays highly efficient, long‐lived solid‐state phosphorescence at room temperature. A set of four BIMCAPt phenyl acetylides were synthesized that emit in the green ( λ max =507–540 nm) with >60 % quantum yield and millisecond lifetimes. The structures of the resulting species reveal a non‐planar structure imposed by steric clashes between BIMCA and the iodo or alkynyl co‐ligand. Ground‐state and photophysical characterization are presented. Density functional theory calculations indicate that the BIMCA ligand dominates the frontier orbitals along with the first Franck–Condon singlet and triplet excited states.

Liska, Tadeas↗

DOE OSTI2026

Optimized Photoemission from Organic Molecules in 2D Layered Halide Perovskites

In recent years, hybrid organic−inorganic metal halides have been at the forefront of materials research. Typically, the functional (e.g., optoelectronic) properties of hybrid halides are derived from the inorganic structural part, whereas the organic structural units can add extra advantages in terms of stability, rigidity, and processability. Here, we report the design, synthesis, and characterization of two new hybrid materials in which the outstanding photophysical properties originate from the organic structural part. The new compounds, (C 15 H 16 N) 2 CdCl 4 and ((Br)C 15 H 15 N) 2 CdCl 4 , have 2D layered Ruddlesden−Poppertype perovskite structures. These hybrids are blue-white light emitters just like their corresponding pure organic salts, but with much improved emission efficiencies. Optical spectroscopy and density functional theory (DFT) studies confirm that photoemission comes from the trans-stilbene organic cations. The photoluminescence quantum yield (PLQY) values of these new materials are among the highest known, 50.83% and 26.60% for (C 15 H 16 N) 2 CdCl 4 and ((Br)C 15 H 15 N) 2 CdCl 4 , respectively. This is up to a 5-fold increase as compared to the light emission efficiency of the precursor salt C 15 H 16 NCl (PLQY of 10.33%). Alongside their outstanding optical properties, their environmental and thermal stability allow their consideration for potential practical applications such as radiation detection. This work shows that hybrid metal halides can be compositionally and structurally engineered to have highly efficient photoemission originating from the organic components for fast scintillation applications.

Halogens↗

DOE OSTI2020

GaN‐based split phase transformer‐less PV inverter with auxiliary ZVT circuit

This paper explores performance enhancement of the common ground dynamic dc‐link (CGDL) inverter for single phase photovoltaic (PV) applications by a combination of gallium nitride (GaN) devices, split phase topology, coupled inductors, and zero voltage transition (ZVT) scheme. The CGDL inverter has the inherent advantage of minimised dc‐link capacitance and negligible leakage current due to the common ground configuration, but its reported efficiency was usually lower because of the higher dc‐link voltage used for the reduction of decoupling capacitance to a great extent. To solve the efficiency problem, in this study, a soft switching circuit is proposed for the first stage, while a coupled inductor integrated magnetics is incorporated in the second stage to reduce inductor loss, volume, and cost. Both of these topological improvements combined with the use of GaN devices facilitate in achieving high efficiency without compromising converter power density. Extensive experimental results are provided from a GaN based 1 kVA hardware prototype to demonstrate the superior performance of the CGDL inverter attaining a peak efficiency of 98.7% and a California Energy Commission efficiency of 98.5% at 75/50 kHz switching frequency.

Xia, Yinglai↗

DOE OSTI2025

Wafer-Free Crystalline Silicon Solar Cells (CRADA Final Report)

This CRADA project, based on the DOE Solar Energy Technologies Office (SETO) Solar Prize Voucher program, helped Leap Photovoltaics to develop methodologies to immobilize Si particles by permanently attaching them to an Al-coated substrate and thereby forming carrier-selective electrical contacts to the Si particles. The bigger goal was to help Leap Photovoltaics develop these immobilized and contacted particle arrays into relatively efficient, inexpensive, and industrially relevant solar cells. By using Si particles instead of wafers in a solar cell absorber layer, one can avoid costs associated with growing monocrystalline Si ingots, then diamond-sawing them into wafers, then processing wafers into cells – a mainstream practice in today's high-efficiency Si cell and module technology. Monocrystalline or polycrystalline Si particles can be obtained in various ways: for example, Si kerf from wafer sawing is monocrystalline; recycled Si cell wafers can be ball-milled into particles; particles can be grown using various gas-phase techniques (mostly from SiH4). These Si particles can be assembled onto a substrate and serve as an absorber layer for the solar cell, absorbing photons to generate photocarriers. The challenge with this technique is to collect photocarriers from individual Si particles, with separation of photogenerated electrons to the negative cell’s electrode and positive photogenerated holes to the positive electrode. Therefore, each particle must have two isolated, carrier-selective contacts: one for electrons and one for holes. Plus, particles need to be immobilized onto a solid substrate. The goal of this work was focused on the immobilization of Si particles and creating hole-selective contact to them at the same time, using industrially relevant Si photovoltaic (PV) cell technology: screen printing of Al back-surface field electrodes. This is used in the mainstream Propane Education and Research Council (PERC) technology for hole-collecting contacts at the back of the cell. The work performed at NREL consisted of screen printing of Al metal paste on substrates, spreading Si particles onto it, and thermally processing the structures to form hole-collecting contacts. The final structures were investigated by scanning electron microscopy (SEM) after focused ion beam (FIB) cross-sectioning and polishing. The work was done jointly by NREL staff and Leap Photovoltaics (Leap PV) employees stationed at NREL. The samples were then taken to Leap PV for further processing. Training the Leap PV employee on various NREL techniques (laser cutting, screen printing, thermal processing, characterization) was part of the scope.

14 SOLAR ENERGY↗

DOE OSTI2026

Enhancing Value-Added CO Production from CO 2 Hydrogenation by Tailoring the Ru-CeO 2 Interface on MgO

Catalytic CO 2 hydrogenation presents a promising route for converting CO 2 into valuable products, contributing to the mitigation of net CO 2 emissions. Supported Ru catalysts have recently gained considerable attention due to their tunability for 100% CO selectivity via the reverse water-gas shift pathway, effectively suppressing the competing methanation route. However, despite achieving full CO selectivity, the overall CO yield remains limited by low CO 2 conversion, necessitating further improvement. In this work, CeO 2 was introduced to modify a Ru/MgO single-atom catalyst for CO 2 hydrogenation. The resulting Ru-CeO 2 /MgO catalyst, featuring abundant Ru-CeO 2 interfacial sites, exhibited a favorable balance of CO 2 conversion and CO selectivity, delivering the highest CO yield (32.5% at 500 °C), which is 9.0 and 1.8 times higher than that on Ru/MgO (3.6%) and Ru/CeO 2 (18.4%), respectively. Although the CO selectivity was slightly compromised due to enhanced CO binding at Ru-CeO 2 interfacial sites, H 2 was more efficiently activated at these interfaces and readily reacted with CO 2 adsorbed on CeO 2 -MgO surfaces, thereby boosting the CO 2 hydrogenation activity and CO yield. This study underscores the critical role of Ru-metal oxide interface engineering in improving CO yield and advancing the rational design of highly efficient Ru catalysts for CO production from CO 2 hydrogenation.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Probing the surface oxidation process in hexagonal boron nitride epilayers

Thermal neutron detectors based on hexagonal boron nitride ( h -BN) epilayers have demonstrated a record high efficiency among solid-state detectors at 58%. It was found that the performance of h -BN detectors is profoundly influenced by charge recombination at the surfaces. The dynamic process of surface oxidation in h -BN epilayers has been probed by x-ray photoelectron spectroscopy. The spectra of high-resolution (0.1 eV) scans indicated that the linewidth of the B 1s peak at 190.6 eV increased and the peak intensity decreased with an increase in exposure time in-air (t air ). The main B 1s peak at 190.6 eV evolved into multiple peaks at a higher binding energy position due to oxygen impurities tending to occupy nitrogen sites and form the B–O bond. Time constants of the oxidation process have been determined, revealing that the formation process of the B–O bond is very fast and within minutes in h -BN. The results suggest that reducing nitrogen vacancy generation during growth and employing surface treatment techniques would further improve the performance of h -BN devices.

2D materials↗

DOE OSTI2024

Development of electro-optical quantum transducers based on three-dimensional superconducting cavities

Quantum transducers enable the conversion of quantum information and signals between different physical platforms. Based on the pioneering works in three-dimensional superconducting cavity technology developed at Fermilab, we are advancing the development of three-dimensional microwave-optical transducers and exploring their applications in quantum information processing and sensing. We present our progress in the design, fabrication, and characterization of three-dimensional microwave cavities integrated with bulk lithium niobate resonators. The material characterization using three-dimensional cavities based on a resonant-type method allows for understanding of complex permittivity and loss mechanism of electro-optic materials at cryogenic temperatures. We also evaluate the potential of the high-efficiency quantum transducers in enhancing the performance of quantum sensors for applications such as dark matter detection, compared to conventional homodyne detection approaches. This manuscript has been authored by Fermi Research Alliance, LLC under Contract No. DE-AC0207CH11359 with the U.S. Department of Energy, Office of Science, Office of High Energy Physics. This work is funded by the DOE's Early Career Research Program. This research used resources of the U.S. Department of Energy, Office of Science, National Quantum Information Science Research Centers, Superconducting Quantum Materials and Systems Center (SQMS) under Contract No. DE-AC02-07CH11359.

Zorzetti, Silvia↗

DOE OSTI2020

Update on ASME AG-1 and Revision of the DOE Nuclear Air Cleaning Handbook - 20536

The American Society of Mechanical Engineers AG-1 Code on Nuclear Air and Gas Treatment is updated every two years. This paper provides an overview of issues being discussed within AG-1 committee meetings and revisions that will be included in the next version of the code. Additional information is provided on issues being discussed ranging from media velocity limits, control of airflow using actual versus and standard cubic feet per minute. Navigation and identification of applicable high-efficiency particulate air (HEPA) filter code sections can be confusing for those unfamiliar with AG-1. A general reorganization of filtration code sections clarifies geometry, flow, and performance envelopes for nuclear grade HEPA filters. The initial step consists of establishment of Section FN covering qualification of conventional, ceramic, metal, and high strength fibrous glass media. Future filter sections are currently expected to be characterized by geometry and flow direction (axial vs. radial). The Department of Energy's (DOE) Nuclear Air Cleaning Handbook (NACH) is also undergoing revision. An update on the status of that effort, along with issues and changes being considered. The original charter of the AG-1 Code was specific to commercial nuclear power plants, and to safety-related air cleaning systems. This has evolved over the years to include normal non-safety ventilation systems and process gas systems. Corollary guidance for DOE facilities has been available in several editions of the Nuclear Air Cleaning Handbook, starting with ORNL-NSIC 65. The latest edition of the Handbook, 2003, is undergoing revision and modifications. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2023

Search for e → τ charged lepton flavor violation at the EIC with the ECCE detector

The recently approved Electron-Ion Collider (EIC) will provide a unique new opportunity for searches of charged lepton flavor violation (CLFV) and other new physics scenarios. In contrast to the e ↔ μ CLFV transition for which very stringent limits exist, there is still a relatively large discovery space for the e → τ CLFV transition, potentially to be explored by the EIC. Here, with the latest detector design of ECCE (EIC Comprehensive Chromodynamics Experiment) and projected integral luminosity of the EIC, we find the τ-leptons created in the DIS process ep → τX are expected to be identified with high efficiency. A first ECCE simulation study, restricted to the 3-prong τ-decay mode and with limited statistics for the Standard Model backgrounds, estimates that the EIC will be able to improve the current exclusion limit on e → τ CLFV by an order of magnitude. As a result, the very high vertex resolution of the ECCE detector configuration plays a critical role in τ identification.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2025

Integrating catalytic fractionation and microbial funneling to produce 2-pyrone-4,6-dicarboxylic acid and ethanol

Replacing biorefinery designs that use stepwise fractionation, depolymerization, and conversion processes with designed tandem process steps can greatly reduce a biorefinery's operating costs and environmental impact. Reductive Catalytic Fractionation (RCF) is a highly efficient lignin-first approach that combines biomass fractionation and lignin depolymerization to generate a hydrogenolysis oil and pulp. The oil is composed of a complex mixture of phenolic monomers, dimers, and oligomers. Intergrating this chemical deconstruction process with microbial funneling of phenolics can simplify the product mixture and make high-value products. We applied RCF to poplar biomass in a biomass-to-bioproduct processing chain in which the phenolics were funneled to 2-pyrone-4,6-dicarboxylic acid (PDC) by an engineered strain of Novosphingobium aromaticivorans DSM12444. The pulp was enzymatically digested and the glucose and xylose was funneled to ethanol by an engineered strain of Saccharomyces cerevisiae GLBRCY945. By combining biomass fractionation and lignin depolymerization we removed a costly processing step that directly translated into a 29% reduction in the minimum selling price of PDC. This work combines experimentation with process modeling of an integrated biorefinery design to show how utilizing tandem process steps can significantly reduce operating expenses and environmental impact of upgrading lignocellulosic biomass to a portfolio of high value products.

Sener, Canan [Great Lakes Bioenergy Research Cente↗

DOE OSTI2020

Sr 1-x Ca x Fe 1-y Co y O 3-δ as facile and tunable oxygen sorbents for chemical looping air separation

Abstract Chemical looping air separation (CLAS) is a promising technology for oxygen generation with high efficiency. The key challenge for CLAS is to design robust oxygen sorbents with suitable redox properties and fast redox kinetics. In this work, perovskite-structured Sr 1-x Ca x Fe 1-y Co y O 3 oxygen sorbents were investigated and demonstrated for oxygen production with tunable redox properties, high redox rate, and excellent thermal/steam stability. Cobalt doping at B site was found to be highly effective, 33% improvement in oxygen productivity was observed at 500 °C. Moreover, it stabilizes the perovskite structure and prevents phase segregation under pressure swing conditions in the presence of steam. Scalable synthesis of Sr 0.8 Ca 0.2 Fe 0.4 Co 0.6 O 3 oxygen sorbents was carried out through solid state reaction, co-precipitation, and sol-gel methods. Both co-precipitation and sol-gel methods are capable of producing Sr 0.8 Ca 0.2 Fe 0.4 Co 0.6 O 3 sorbents with satisfactory phase purity, high oxygen capacity, and fast redox kinetics. Large scale evaluation of Sr 0.8 Ca 0.2 Fe 0.4 Co 0.6 O 3 , using an automated CLAS testbed with over 300 g sorbent loading, further demonstrated the effectiveness of the oxygen sorbent to produce 95% pure O 2 with a satisfactory productivity of 0.04 g O2 g sorbent −1 h −1 at 600 °C.

25 ENERGY STORAGE↗

DOE OSTI2021

Assessment of Turbulent Combustion Models for Simulating Prechamber Ignition in a Natural Gas Engine

Lean combustion is a promising strategy to increase thermal efficiency in an internal combustion engine, by exploiting a favorable specific heat ratio of the fresh mixture while simultaneously suppressing the heat losses to the cylinder wall. However, unstable ignition and slow flame propagation at fuel-lean conditions lead to large cycle-to-cycle variability and limit the high-efficiency engine operating range. Prechamber ignition is considered an effective concept to extend the lean operating limit, by providing spatially distributed ignition with multiple turbulent flame-jets and enabling a faster combustion rate compared to the conventional spark ignition approach. From a numerical modeling standpoint to date science base and available simulation tools are inadequate to properly understand and predict the combustion processes in prechamber ignited engines. In this paper, conceptually different Reynolds-averaged Navier–Stokes (RANS) combustion models widely adopted in the engine modeling community are used to simulate the ignition and combustion processes in a medium-duty natural gas engine with a prechamber spark-ignition system. Here, a flamelet-based turbulent combustion model, i.e., G-equation, and a multizone well-stirred reactor model are employed for this modeling study. Simulation results are compared with experimental data in terms of in-cylinder pressure and heat release rate. Finally, the analysis of the performance of the two models is carried out to highlight the strengths and limitations of the two evaluated approaches.

42 ENGINEERING↗

DOE OSTI2022

Short-Lived Modules Need to be Efficient, Lightweight, and Circular for the Energy Transition

Deployment projections for decarbonizing the grid predict 1.75 TW of PV is needed in the United States by 2050. This entails a cumulative demand of 97 million metric tonnes of virgin materials for c-Si modules. These material needs are extraction and energy intensive, making them a key target for improving PV sustainability. Emerging PV technologies, such as perovskites, are targeting 15-year modules, high efficiencies, and circular designs. Previous analysis found that by just modifying the life expectancy to 15 years (keeping target c-Si efficiencies and BOM), an additional 1.4 TW of replacement modules are required to maintain capacity, increasing virgin material demand by 1.75x unless >95% closed-loop recycling is maintained. This study examines the effect of achieving higher efficiencies with thin-film designs and a 15-year expectancy. Higher efficiencies and thin film designs can decrease deployment and material demands, making the level of circularity more attainable. If BOM mass is reduced by 50%, closed-loop recycling rates need to be >80% to reduce virgin material demands compared to a 35-yr c-Si module. If module efficiencies are 30%, closed-loop recycling rates can be reduced to 65%. This efficiency increase also reflects that 1500 million fewer modules can be deployed, however, this is still 2000 million more modules than a 35-year module needs to deploy to achieve energy transition targets, and no PV technology is closed-loop recycled for all component materials.

circular economy↗

DOE OSTI2024

Efficient laser-driven proton acceleration from a petawatt contrast-enhanced second harmonic mixed-glass laser system

Efficient laser-driven plasma acceleration of ion beams requires precision control of the target–plasma profile, which is crucial to optimize the laser energy transfer. Along the laser propagation direction, this can be achieved by tailoring the temporal structure of the laser pulse. We show for the first time that frequency-doubling of a short pulse (hundreds-femtosecond range) petawatt-class mixed-glass laser system, which results in temporal intensity contrast enhancement, enables surface and volumetric laser–energy coupling, and the acceleration of proton beams from few-nanometer-thick foil targets. Experimentally, maximum ion energies and laser-to-proton energy conversion efficiencies were found to be both maximized at optimum laser and target conditions manifested when the normalized target density nearly equalizes the normalized laser vector potential, which is in agreement with theory and simulations. These signatures are recognized as a unique indication of the interaction between ultra-intense laser pulses with high temporal intensity contrast and ultra-thin nanometer-scale targets. Transverse modulations of accelerated proton beams in the form of bubble- and ring-like structures measured in the thinnest targets provide additional evidence of volumetric laser-driven particle acceleration regimes and transitional features in ultra-thin foil targets specific to laser–plasma interactions characterized by a high temporal intensity contrast. These results open avenues in the generation of high contrast laser pulses from short-pulse-femtosecond petawatt mixed-glass laser systems and demonstrate the feasibility of this technique for applications requiring high laser intensity contrast with high efficiency.

Physics↗

DOE OSTI2022

TEAMER: Sandia and CalWave Torque Spring Assessment

Power-take-off (PTO) systems for wave energy converters (WEC) require restoring forces for efficient hydrodynamic as well as mechanical to electric power transfer. Implementation of an effective spring mechanism that can provide a restoring torque on e.g. a rotational, winch type PTO shaft is challenging. SNL in collaboration with CalWave, will use numerical finite element simulations to study application of mechanical torsion springs as a highly efficient restoring force element for CalWave's rotational PTO. Material studies will include common steel as a baseline and potentially advanced materials such as fiber composite materials with different cross-sectional profiles. Test report including description and results of FEA (finite element analysis) models. Excel sheet summarizes which scripts were used for which tables and figures in the report. Part of TEAMER request for technical support (RFTS 1) award to CalWave and Sandia National Lab (SNL).

16 TIDAL AND WAVE POWER↗

DOE OSTI2021

A two-phase three-field modeling framework for heat pipe application in nuclear reactors

Heat pipes and two-phase thermosyphons are highly efficient heat transfer devices utilizing continuous evaporation and condensation of working fluid for two-phase heat transport in closed systems. Because of the nearly isothermal and fully passive phase-change heat transfer mechanism, heat pipes and thermosyphons have found many applications in nuclear engineering, space technologies, and other energy systems. High-temperature heat pipes are used in nuclear microreactors to remove fission power from the primary system and are coupled with power conversion systems or process heat applications. Modeling of the two-phase flow phenomena inside a heat pipe is essential to its design and safety analysis. In this study, a comprehensive one-dimensional two-phase three-field flow model has been developed for the analysis of heat pipes in normal operation conditions and transients. The conservation or field equations of mass, momentum, and energy were developed for the liquid film, vapor, and droplet. In addition, constitutive models or correlations were reviewed thoroughly and provided for the closure of the three-field equations. Specific constitutive equations regarding interfacial mass and heat transfer at two interfaces, namely film-gas interface and gas-droplet interface, were reviewed for droplet entrainment and deposition rates as well as film and droplet evaporation rates. Furthermore, mechanistic correlations of annular flow film thickness were recommended for the modeling of the thermosyphons without a wick as a critical constitutive correlation. Furthermore, experimental data needs from new experiments using a prototype working fluid or surrogate fluids for the model validation of high-temperature heat pipes in microreactors were recommended for future research.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2022

Optimizing molecular light absorption in the strong coupling regime for solar energy harvesting

The strong coupling of optical absorbers (e.g., molecules or semiconductors) to confined photonic modes fundamentally alters the physical properties of the coupled system via the formation of hybrid light-matter states. One potential application of strong light-matter coupling relies on exploiting it to localize light-induced charge excitation processes to small volumes of material. Applications that would benefit from this localization include thin-film photovoltaics, photodetection, photocatalysis, and others, where the overall performance depends on the ability of a material to amplify light absorption (i.e., the formation of electron-hole pairs) within specific locations in space. This contribution investigates how strong light-matter coupling affects light absorption rates in molecular absorbers coupled to photonic nanostructures. Here, our results show that the molecular light absorption efficiencies are highest in configurations where the strongly coupled molecules interact directly with the incoming photon flux. We also identify a nonlinear dependence in the molecular absorption as a function of concentration, unique to the strongly coupled systems. Based on these results, we propose design principles for engineering nanostructured systems that allow for high efficiencies of charge carrier localization into strongly coupled absorbers.

14 SOLAR ENERGY↗

DOE OSTI2023

Reliable bi-functional nickel-phosphate /TiO2 integration enables stable n-GaAs photoanode for water oxidation under alkaline condition

Abstract Hydrogen is one of the most widely used essential chemicals worldwide, and it is also employed in the production of many other chemicals, especially carbon-free energy fuels produced via photoelectrochemical (PEC) water splitting. At present, gallium arsenide represents the most efficient photoanode material for PEC water oxidation, but it is known to either be anodically photocorroded or photopassivated by native metal oxides in the competitive reaction, limiting efficiency and stability. Here, we report chemically etched GaAs that is decorated with thin titanium dioxide (~30 nm-thick, crystalline) surface passivation layer along with nickel-phosphate (Ni-Pi) cocatalyst as a surface hole-sink layer. The integration of Ni-Pi bifunctional co-catalyst results in a highly efficient GaAs electrode with a ~ 100 mV cathodic shift of the onset potential. In this work, the electrode also has enhanced photostability under 110 h testing for PEC water oxidation at a steady current density J ph > 25 mA·cm −2 . The Et-GaAs/TiO 2 /Ni-Pi║Ni-Pi tandem configuration results in the best unassisted bias-free water splitting device with the highest J ph (~7.6 mA·cm −2 ) and a stable solar-to-hydrogen conversion efficiency of 9.5%.

08 HYDROGEN↗