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At least 73 records · Page 4

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DOE OSTI2020

Current status and future directions of multivalent metal-ion batteries

Batteries based on multivalent metals have the potential to meet the future needs of large-scale energy storage, due to the relatively high abundance of elements such as magnesium, calcium, aluminium and zinc in the Earth’s crust. However, the com- plexity of multivalent metal-ion chemistries has led to rampant confusions, technical challenges, and eventually doubts and uncertainties about the future of these technologies. In this Review, we clarify the key strengths as well as common misconceptions of multivalent metal-based batteries. We then examine the growth behaviour of metal anodes, which is crucial for their safety promises but hitherto unestablished. We further discuss scrutiny of anode efficiency and cathode storage mechanism pertaining to complications arising from electrolyte solutions. Lastly, we critically review existing cathode materials and discuss design strategies to enable genuine multivalent metal-ion-based energy storage materials with competitive performance.

25 ENERGY STORAGE↗

DOE OSTI2022

Understanding What Limits the Voltage of Polycrystalline CdSeTe Solar Cells

The origin of voltage deficits in polycrystalline cadmium selenide telluride (CdSeTe) solar cells is unclear. Here, we present a comprehensive voltage loss analysis performed on state-of-the-art CdSeTe devices - fabricated at Colorado State University and First Solar - using photoluminescence techniques, including external radiative efficiency (ERE) measurements. More specifically, we report the thermodynamic voltage limit Voc,ideal, internal voltage iVoc and external voltage Voc of partially and fully finished cells fabricated with different dopant species, dopant concentrations and back contacts. Arsenic-doped aluminium-oxide-passivated cells made at Colorado State University present remarkably high ERE (>1%) - translating into iVoc above 970 mV - but suffer from poor back-contact selectivity. On the other hand, arsenic-doped devices from First Solar present almost perfect carrier selectivity (Voc=iVoc), leading to Voc above 840 mV, and are limited by recombination in various parts of the device. Thus, development of contact structures that are both passivating and selective in combination with highly luminescent absorbers is key to reducing voltage losses.

CdSeTe devices↗

DOE OSTI2025

Mineralogical evidence for hydrothermal alteration of Bennu samples

Samples of asteroid (101955) Bennu delivered by the OSIRIS-REx mission offer the opportunity to study pristine planetary materials unchanged by exposure to the terrestrial environment. Here we use a combination of X-ray diffraction and various electron microscopy techniques to explore the detailed mineralogy of Bennu samples and determine the alteration history of the planetesimal protolith from which they originated. The samples consist largely of hydrated sheet-silicate minerals, namely nanoscale serpentine and saponite of varied grain size, which are decorated with micro- to nanoscale Fe-sulfides, magnetite and carbonates. We observe sheet silicates parallel and normal to sulfide surfaces and as inclusions in sulfides; sulfur-rich veins transecting the sheet-silicate matrix; zoned carbonates and phosphates and sulfide and magnetite grains exhibiting embayment. The mineralogical evidence indicates alteration of accreted minerals by a fluid that evolved with time, leading to etching, dissolution and reprecipitation. Sulfide compositions indicate alteration at ~25 °C, similar to conditions inferred for asteroid (162173) Ryugu and Ivuna-type (CI) chondrite meteorites. The fluid probably evolved from neutral to alkaline, culminating with the precipitation of highly soluble salts. We conclude that Bennu’s protolith comprised mainly nanometre to micrometre silicates, with fewer chondrules and calcium–aluminium-rich inclusions than those of most chondrite groups.

Zega, T J↗

DOE OSTI2021

High-speed programmable photonic circuits in a cryogenically compatible, visible–near-infrared 200 mm CMOS architecture

Abstract Recent advances in photonic integrated circuits have enabled a new generation of programmable Mach–Zehnder meshes (MZMs) realized by using cascaded Mach–Zehnder interferometers capable of universal linear-optical transformations on N input/output optical modes. MZMs serve critical functions in photonic quantum information processing, quantum-enhanced sensor networks, machine learning and other applications. However, MZM implementations reported to date rely on thermo-optic phase shifters, which limit applications due to slow response times and high power consumption. Here we introduce a large-scale MZM platform made in a 200 mm complementary metal–oxide–semiconductor foundry, which uses aluminium nitride piezo-optomechanical actuators coupled to silicon nitride waveguides, enabling low-loss propagation with phase modulation at greater than 100 MHz in the visible–near-infrared wavelengths. Moreover, the vanishingly low hold-power consumption of the piezo-actuators enables these photonic integrated circuits to operate at cryogenic temperatures, paving the way for a fully integrated device architecture for a range of quantum applications.

47 OTHER INSTRUMENTATION↗

DOE OSTI2025

Spatio-spectral optical fission in time-varying subwavelength layers

Transparent conducting oxides are highly doped semiconductors that exhibit favourable optical features compared with metals, including reduced material losses, tuneable electronic and optical properties, and enhanced damage thresholds. Recently, the photonic community has renewed its attention towards these materials, recognizing their remarkable nonlinear optical properties in the near-infrared spectrum. The exceptionally large and ultrafast change in the refractive index, which can be optically induced in these compounds, extends beyond the boundaries of conventional perturbative analysis and makes this class of materials the closest approximation to a time-varying system. Here we report the spatio-spectral fission of an ultrafast pulse trespassing a thin film of aluminium zinc oxide with a non-stationary refractive index. By applying phase conservation to this time-varying layer, our model can account for both space and time refraction and explain, in quantitative terms, the spatial separation of both spectrum and energy. Our findings represent an example of extreme nonlinear phenomena on subwavelength propagation distances, which provides new insights into transparent conducting oxides’ transient optical properties. This can be critical for the ongoing research on photonic time crystals, on-chip generation of non-classical states of light, integrated optical neural networks, ultrafast beam steering and frequency-division multiplexing.

integrated optics↗

DOE OSTI2026

A 1-km photonic link connecting superconducting circuits in two dilution refrigerators

Superconducting quantum processors are a leading platform for implementing practical quantum computation algorithms. Although superconducting quantum processors with hundreds of qubits have been demonstrated, their further scale-up is constrained by the physical size and cooling power of dilution refrigerators. This constraint can be overcome by constructing a quantum network to interconnect qubits hosted in different refrigerators, which requires microwave-to-optical transducers to enable low-loss signal transmission over long distances. Although various designs and demonstrations have achieved high-efficiency and low-added-noise transducers, a coherent photonic link between separate refrigerators has not yet been realized. Here, in this work, we experimentally demonstrate coherent signal transfer between two superconducting circuits housed in separate dilution refrigerators, enabled by a pair of frequency-matched aluminium nitride electro-optic transducers connected via a 1-km telecom optical fibre. The optical frequency matching between two transducers is realized by an asymmetric photonic molecule design, and an overall 80 dB improvement in transduction efficiency over commercial electro-optic modulators is achieved, paving the way towards a fully quantum-enabled link. This work provides critical design guidelines for scalable superconducting quantum networks interconnected by photonic links.

nonlinear optics↗

DOE OSTI2020

Iron-based binary ferromagnets for transverse thermoelectric conversion

Thermoelectric generation using the anomalous Nernst effect (ANE) has great potential for application in energy harvesting technology because the transverse geometry of the Nernst effect should enable efficient, large-area and flexible coverage of a heat source. For such applications to be viable, substantial improvements will be necessary not only for their performance but also for the associated material costs, safety and stability. In terms of the electronic structure, the anomalous Nernst effect (ANE) originates from the Berry curvature of the conduction electrons near the Fermi energy. To design a large Berry curvature, several approaches have been considered using nodal points and lines in momentum space. Here we perform a high-throughput computational search and find that 25 percent doping of aluminium and gallium in alpha iron, a naturally abundant and low-cost element, dramatically enhances the ANE by a factor of more than ten, reaching about 4 and 6 microvolts per kelvin at room temperature, respectively, close to the highest value reported so far. The comparison between experiment and theory indicates that the Fermi energy tuning to the nodal web—a flat band structure made of interconnected nodal lines—is the key for the strong enhancement in the transverse thermoelectric coefficient, reaching a value of about 5 amperes per kelvin per metre with a logarithmic temperature dependence. We have also succeeded in fabricating thin films that exhibit a large ANE at zero field, which could be suitable for designing low-cost, flexible microelectronic thermoelectric generators.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2020

Large-scale integration of artificial atoms in hybrid photonic circuits

A central challenge in developing quantum computers and long-range quantum networks is the distribution of entanglement across many individually controllable qubits. Colour centres in diamond have emerged as leading solid-state ‘artificial atom’ qubits because they enable on-demand remote entanglement, coherent control of over ten ancillae qubits with minute-long coherence times and memory-enhanced quantum communication. A critical next step is to integrate large numbers of artificial atoms with photonic architectures to enable large-scale quantum information processing systems. So far, these efforts have been stymied by qubit inhomogeneities, low device yield and complex device requirements. Here we introduce a process for the high-yield heterogeneous integration of ‘quantum microchiplets’—diamond waveguide arrays containing highly coherent colour centres—on a photonic integrated circuit (PIC). We use this process to realize a 128-channel, defect-free array of germanium-vacancy and silicon-vacancy colour centres in an aluminium nitride PIC. Photoluminescence spectroscopy reveals long-term, stable and narrow average optical linewidths of 54 megahertz (146 megahertz) for germanium-vacancy (silicon-vacancy) emitters, close to the lifetime-limited linewidth of 32 megahertz (93 megahertz). We show that inhomogeneities of individual colour centre optical transitions can be compensated in situ by integrated tuning over 50 gigahertz without linewidth degradation. The ability to assemble large numbers of nearly indistinguishable and tunable artificial atoms into phase-stable PICs marks a key step towards multiplexed quantum repeaters and general-purpose quantum processors

36 MATERIALS SCIENCE↗

DOE OSTI2025

Spotlight: efficient automated global optimization in rietveld analysis of diffraction data

Performing reliable Rietveld analysis on tens or hundreds of powder diffraction datasets from parametric or time-resolved experiments often poses a bottleneck in extracting meaningful results from the data. While automated analysis of data has recently been demonstrated, high temperature annealing studies, during which phase transformations occur and lattice parameters may change due to repartitioning of elements, are prime examples where automation by a simple phase identification from a database of room temperature structures or automation by sequential refinements is likely to fail. To enable reliable, efficient, automated Rietveld analysis, we present a Python package named Spotlight , building on established Rietveld packages such as MAUD, GSAS , or GSAS-II , which extends the refinement of best fit parameters to a global optimization using an ensemble of optimizers leveraging hierarchical parallel execution on high-performance computing clusters. Spotlight further enables the efficient design of refinement plans through the iterative automated machine-learning of a surrogate for the refinement on which the global optimizations are performed until results from the surrogate converge to the response surface data. We demonstrate Spotlight with the analysis of uranium molybdenum and Ti–6Al–4V datasets, as well as in two open-source tutorials analyzing aluminium oxide and lead sulphate.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Facile synthesis of epoxide-co-propylene sulphide polymers with compositional and architectural control

Here, we present a facile method to produce propylene sulphide (PS) homopolymers up to 100 kg mol -1 and PS-epoxide statistical, block, and ABA copolymers using inexpensive and versatile thio-aluminium (SAl) based initiators. Homopolymerizations of PS with SAl initiators are living and controlled, with number averaged molecular weights ($\bar M$ n ) up to 100 kg mol -1 while maintaining narrow polydispersity (Ð < 1.4). Statistical and block copolymers of PS and epichlorohydrin (ECH) or propylene oxide (PO) are synthesized and characterized by size-exclusion chromatography (SEC), differential scanning calorimetry (DSC), 1 H and 13 C NMR spectroscopy, diffusion ordered spectroscopy (DOSY), and small-angle X-ray scattering (SAXS). This work represents the first statistical copolymerization of PS and epoxides with similar reactivity ratios, allowing fine control over composition. Block-copolymers of PS and epoxides are synthesized by sequential addition, without intermediate preparative steps. Polymer architecture is controlled through modification of the initiator; we synthesized a di-functional (d-H) SAl initiator to produce ABA tri-block-copolymers. Finally, poly(ethylene glycol) (PEG) was used as a macroinitiator to create PEG-b-PPS block copolymers and characterized by 1 H, 13 C NMR spectroscopy, DOSY, DSC, and SEC.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

UO 2 target preparation with spin coating assisted solution combustion synthesis

A simple and efficient target preparation method is developed combining spin coating and solution combustion synthesis. Multiple smooth and uniform UO 2 targets have been prepared using this method on a variety of backings (aluminium, carbon, silicon) used in nuclear physics experiments. The thicknesses of the targets can be precisely tuned by changing the number of coatings within the range of ~50-1000 µm/cm 2 . These targets are highly uniform (<5% deviation), robust, and remain strongly adherent to their backings even after being irradiated by high doses (10 17 ions/ cm 2 ) of 1.7 MeV Ar 2+ ions.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2023

Contribution of carbon pricing to meeting a mid-century net zero target

A mid-century net zero target creates a challenge for reducing the emissions of emissions-intensive, trade-exposed sectors with high cost mitigation options. These sectors include aluminium, cement, chemicals, iron and steel, lime, pulp and paper and petroleum refining. Available studies agree that decarbonization of these sectors is possible by mid-century if more ambitious policies are implemented soon. Existing carbon pricing policies have had limited impact on the emissions of these sectors because their marginal abatement costs almost always exceed the tax rate or allowance price. But emissions trading systems with free allowance allocations to emissions-intensive, trade-exposed sectors have minimized the adverse economic impacts and associated leakage. Internationally coordinated policies are unlikely, so implementing more ambitious policies creates a risk of leakage. This paper presents policy packages a country can implement to accelerate emission reduction by these sectors with minimal risk of leakage. To comply with international trade law the policy packages differ for producers whose goods compete with imports in the domestic market and producers whose goods are exported. Carbon pricing is a critical component of each package due its ability to minimize the risk of adverse economic impacts on domestic industry, support innovation and generate revenue. The revenue can be used to assist groups adversely impacted by the domestic price and production changes due to carbon pricing and to build public support for the policies.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Revealing the loss mechanisms of a 3D superconducting microwave cavity for use in a dark matter search

Superconducting microwave cavities have found applications in many areas including quantum computing, particle accelerators, and dark matter searches. Their extremely high quality factors translate to very narrow bandwidth, which makes them key components of sensitive detectors. In this study, we aim to understand the loss mechanisms of an aluminium cavity, with a fundamental mode frequency of about 2.5123 GHz, and how they change as the cavity material transitions from the superconducting to normal state. We found that at temperatures not much lower than the transition temperature $T_c$, losses are dominated by quasiparticle excitations and are well described by the Bardeen–Cooper–Schrieffer theory. The exponential decrease of the quasiparticle density below $T_c$ results in a 1000-fold increase of the quality factor, as well as a shift of the resonance frequency due to the change of the kinetic inductance of the superconductor. At very low temperatures, losses due to two-level systems begin to dominate giving a peak in the quality factor of about 2.76 x 10 7 at 130 mK. Understanding the loss mechanisms is invaluable, as the working temperature of the cavity may vary during operation regardless of its application.

Physics - Physics of elementary particles and fiel↗

DOE OSTI2021

Magnetic triggering — time-resolved characterisation of silicon strip modules in the presence of switching DC-DC converters

Modules for the ATLAS Inner Tracker (ITk) strip tracker include a DC-DC converter circuit glued directly to the silicon sensor which converts the 11 V supplied to the module to the 1.5 V required for the operation of the readout chips. The DC-DC converter unit, consisting of a copper solenoid and custom ASIC, is located directly above the silicon strip sensor and therefore needs to be shielded to protect the sensor from EMI noise created during the operation of the circuit. Despite dedicated shielding, consisting of an aluminium shield box with continuous solder seams encompassing the surface components and a copper layer in the PCB beneath it, module channels connected to sensor strips located beneath the converter circuit were found to show a noise increase. While the DC-DC converter unit causing the underlying EMI noise operates at a frequency of 2 MHz, module characterisation measurements for ITk strip tracker modules are typically performed asynchronously to the DC-DC switching and are therefore averaged over the full range of time bins with respect to the converter frequency. In order to investigate the time dependence of the noise injection relative to the DC-DC switching frequency, a dedicated setup to understand the time-resolved performance change in modules was developed. By using a magnetic field probe to measure the field leaking through the shield box and triggering on its rising edge, data taking could be synchronised with the DC-DC switching. This paper illustrates the concept and setup of such time-resolved performance measurements using magnetic triggering and presents results for the observed effects on signal and noise for ATLAS ITk strip modules from both laboratory and beam tests.

47 OTHER INSTRUMENTATION↗

DOE OSTI2026

Development of thermal joints for conduction-cooling applications

Abstract In support of the development of conduction-cooled superconducting radiofrequency (SRF) niobium cavities for use in continuous-wave linear accelerators, an experimental study of thermal contact resistance was performed on bolted joints using high-purity niobium, aluminium, and copper along with Apiezon N grease and indium foil as interfacial materials. The geometry of each joint investigated aims at replicating the design adopted in conduction-cooled SRF cavities currently under development at Jefferson Lab. The materials’ thermal conductivity and the joints’ thermal resistance were measured in the temperature range of 3.5 - 10 K. The results showed that the low thermal contact resistance of 2-4 K·cm 2 /W at 4.3 K achieved with Al-In-Nb and Al-Apiezon N-Cu joints should allow the operation of conduction-cooled SRF cavities at a targeted accelerating gradient of ∼10 MV/m.

Lewis, J. [Old Dominion University]↗

DOE OSTI2020

Permanent magnets for the return loop of the Cornell-Brookhaven energy recovery linac test accelerator

214 neodymium permanent magnets have been manufactured for the return loop of the CBETA multi-turn ERL at Cornell University. There are 5 types of quadrupole and combined-function gradient magnets using a variant of the circular Halbach design. These are made out of NdFeB material and glued into an aluminium housing with water channels for temperature stabilisation. The NdFeB wedges and magnet construction were done by outside companies, while the final “tuning” using inserts containing 64 iron rods per magnet was done at BNL over a period of about 6 months. Average relative field errors of 2.2×10 -4 were achieved on the beam region. The magnet strengths vary by type but are of order 10 T/m for quadrupole component and up to 0.3 T for the dipole. This paper reports on the field quality and timeline achieved in this production process

43 PARTICLE ACCELERATORS↗

DOE OSTI2025

Group Conductivity and Nonadiabatic Born Effective Charges of Disordered Metals, Warm Dense Matter, and Hot Dense Plasma

The average ionization state is a critical parameter in plasma models for charged particle transport, equations of state, and optical response. The dynamical or nonadiabatic Born effective charge (NBEC), calculated via first principles time-dependent density-functional theory, provides exact ionic partitioning of bulk electron response for both metallic and insulating materials. The NBEC can be transformed into a “group conductivity,” i.e., the electron conductivity ascribed to a subset of ions. We show that for disordered metallic systems, such as warm dense matter (WDM) and hot dense plasma, the static limit of the NBEC is different from the average ionization states, but that the ionization state can be extracted from the group conductivity even in mixed systems. Here we demonstrate this approach using a set of archetypical examples, including cold and warm aluminium, low- and high-density WDM carbon, and a WDM carbon-beryllium-hydrogen mixture.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2022

Pressure cells for in situ neutron total scattering: time and real-space resolution during deuterium absorption

In situ gas-loading sample holders for two-dimensionally arranged detectors in time-of-flight neutron total scattering experiments have been developed to investigate atomic arrangements during deuterium absorption using time and real-space resolution. A single-crystal sapphire container was developed that allows conditions of 473 K and 10 MPa hydrogen gas pressure. High-resolution transient measurements detected deuterium absorption by palladium that proceeded within a few seconds. A double-layered container with thick- and thin-walled vanadium allowed conditions of 423 K and 10 MPa hydrogen gas pressure. The deuterium occupation sites of a lanthanum–nickel–aluminium alloy are discussed in detail on the basis of real-space high-resolution data obtained from in situ neutron scattering measurements and reverse Monte Carlo structural modeling.

08 HYDROGEN↗