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At least 415 records · Page 23

Compact, Highly Stable Ion Atomic Clock

A mercury-ion clock now at the breadboard stage of development (see figure) has a stability comparable to that of a hydrogen-maser clock: In tests, the clock exhibited an Allan deviation of between 2 x 10(exp -13) and 3 x 10(exp -13) at a measurement time of 1 second, averaging to about 10(exp -15) at 1 day. However, the clock occupies a volume of only about 2 liters . about a hundredth of the volume of a hydrogen-maser clock. The ion-handling parts of the apparatus are housed in a sealed vacuum tube, wherein only a getter pump is used to maintain the vacuum. Hence, this apparatus is a prototype of a generation of small, potentially portable high-precision clocks for diverse ground- and space-based navigation and radio science applications. Furthermore, this new ion-clock technology is about 100 times more stable and precise than the rubidium atomic clocks currently in use in the NAV STAR GPS Earth-orbiting satellites. In this clock, mercury ions are shuttled between a quadrupole and a 16-pole linear radio-frequency trap. In the quadrupole trap, the ions are tightly confined and optical state selection from a Hg-202 radio-frequency-discharge ultraviolet lamp is carried out. In the 16-pole trap, the ions are more loosely confined and atomic transitions resonant at frequency of about 40.507 GHz are interrogated by use of a microwave beam at that frequency. The trapping of ions effectively eliminates the frequency pulling caused by wall collisions inherent to gas-cell clocks. The shuttling of the ions between the two traps enables separation of the state-selection process from the clock microwave- resonance process, so that each of these processes can be optimized independently of the other. The basic ion-shuttling, two-trap scheme as described thus far is not new: it has been the basis of designs of prior larger clocks. The novelty of the present development lies in major redesigns of its physics package (the ion traps and the vacuum and optical subsystems) to effect the desired reduction of size to a volume of no more than a couple of liters. The redesign effort has included selection of materials for the vacuum tube, ion trap, and ultraviolet windows that withstand bakeout at a temperature of approx.450 C in preparation for sealing the tube to contain the vacuum. This part of the redesign effort follows the approach taken in the development of such other vacuum-tube electronic components as flight traveling- wave-tube amplifiers having operational and shelf lives as long as 15 years. The redesign effort has also included a thorough study of residual-gas-induced shifts of the ion-clock frequency and a study of alternative gases as candidates for use as a buffer gas within the sealed tube. It has been found that neon is more suitable than is helium, which has been traditionally used for this purpose, in that the pressure-induced frequency pulling by neon is between a third and a half of that of helium. In addition, because neon diffuses through solids much more slowly than does helium, the loss of neon by diffusion over the operational lifetime is expected to be negligible.

Prestage, John↗

Scalable Nano-Scaffold SOFC Anode Architecture Enabling Direct Hydrocarbon Utilization

This project is based on WVU’s pending patents, technology and aims to design and modify the internal surfaces of the Ni/YSZ anode from currently commercially viable Solid Oxide Fuel Cells (SOFCs) using the additive manufacturing process of Atomic Layer Deposition (ALD). The surface architecture/scaffold added onto the internal surface of the anode possesses an engineered nanostructure but it features only commonly-used oxide conductors and electro-catalyst materials. The surface layer possesses a minimum thickness of ~2-40 nm and is solely designed to control the surface reforming reactions and to increase catalytic activity. Three-dimensional (3D) nano scaffold architectures with the noble metal nano-catalyst, low-cost bimetallic catalytic alloys, and nano-scale ionic conducting oxide fully compatible with the state-of-the-art Ni/YSZ anode, were applied to the internal surface of the entire porous SOFC anode using ALD. In the present work, the surface scaffold architecture is essentially multi-functional at the nano-scale, facilitated by the multiple heterostructured interfaces. It will significantly enhance the power density and cell durability for direct hydrocarbon utilization by (1) increasing the number of electrochemical reaction sites to enhance the hydrogen/hydrocarbon oxidation reactions; (2) reducing carbon formation; (3) mitigating the coarsening of backbone Ni phase and the oxidation attack of Ni from oxidants (e.g., H2O, CO2); and (4) promoting the internal reforming capabilities, especially for natural gas applications. ALD is employed to generate stable anode surface architectures that are uniform, precisely controllable at the atomic scale, and accurately repeatable for processing. The engineered anode surface nano-scaffold architecture was cataloged and analyzed using High-resolution Transmission Electron Microscopy (TEM), and cell power/durability performance assessed via comprehensive electrochemical performance testing with commercial specimens and relevant environments using hydrocarbon fuels. To the best of our knowledge, this project is the First Report on ALD of Ni/YSZ. The actual achievement of this Project includes (1). Successful demonstration of 7 types of ALD layers on Ni/YSZ anode, including Co, Ni, Mn, Pt, Ru, ZrOx and multi-functional nano-composite. (1). Conformal coating and subsequently spontaneously pinning the discrete nano-catalyst, including the precious metal nano-catalyst and the Ni and Co catalysts, on the YSZ surface upon the electrochemical operation in the reduced atmosphere. Those nano-catalysts on the ionic-conducting YSZ provided excellent sites for promoting internal reforming; (2). Demonstrated ALD coating increased both catalytic activity and conductivity of Ni/YSZ. Conformal coating provided dopants and introduced additional electrical conducting pathways on the YSZ ionic conductor. The doped surface layer of YSZ with mixed conductivity thus further introduces the active triple phase boundaries adjacent to the ALD-coated nano-catalysts such as Pt, Co, and Ni that are pinned on the YSZ surface. The nano-composite ALD coating on Ni/YSZ anode has significantly increased cell durability; and (3). ALD coating of Ni/YSZ anode increased the power density of the entire cell by 300%. For a long time, the SOFC performance, such as the power density, was deemed hindered by the cathode. The sluggish oxygen reduction reaction (ORR) in the cathode was deemed as hindering the power density of the SOFCs. For the anode-supported commercial SOFCs, the cell performance is considered to be limited by the cathode's performance. For the first time in the field of SOFC, this project has demonstrated that (1). the performance of commercial SOFCs can be further increased by the ALD coating on Ni/YSZ anode backbone. (2). ALD coating on Ni/YSZ fuel electrodes results in the enhancement of power density, and increased reliability, robustness, and endurance of SOFCs, for their application using both hydrogen and hydrocarbon fuels over the entire operating temperature range of 650-800ºC for the inherently functional commercial cells. (3). ALD coating provides alternative approaches of exsolutions for introducing the stable catalyst onto the internal surface of the Ni/YSZ electrode. ALD coating could be much more versatile than exsolution in employing the catalysts with various chemistries onto the various backbones. (4). Due to the negligible amount of ALD materials coated onto the internal surface of the porous cathode of the as-fabricated cells, a peak power density increase up to 300 % induced by ALD coating was simultaneously achieved in terms of both power density and specific power. (5). The ALD coating developed through this project was applied to both the SOFC and Solid Oxide Electrolysis Cells (SOEC). SOEC’s face a similar but more demanding need to improve the fuel electrode's performance. It opens further research directions for electrocatalytic surface nanoionics with a wide range of chemistry. It will revolutionize our ability to render the formation of a nanostructured electrode that has been constantly pursued yet barely achieved for practical SOFC/SOEC applications. The research is also immediately transformative since both the preliminary data and the proposed work are on the direct implantation of nanoionics into the state-of-the-art inherently functional SOCs. It represents an immediate impact on the commercial sectors in SOC technology since the applied ALD processing is computer-controlled ALD coating using the commercial ALD systems, and it is scalable to both the single cells and SOC stacks.

36 MATERIALS SCIENCE↗

Epitaxial Design of Complex Nickelates as Electrocatalysts for the Oxygen Evolution Reaction

Abstract The oxygen evolution reaction (OER) is a crucial process in electrochemical water splitting, a promising technology to renewably yield hydrogen gas from water. Designing and developing earth‐abundant, efficient, and stable OER electrocatalysts to replace the most widely used but scarce RuO 2 and IrO 2 are thus of critical interest. Recently, ABO 3 ‐structured perovskite oxides, especially rare‐earth nickelates, are extensively studied for their potential use as OER electrocatalysts. In particular, the epitaxial synthesis of complex oxide thin films allows flexible and precise control over the materials so that their structure–stability–property relationships can be established. Using nickelate thin films as model systems, this review illustrates how epitaxial design allows researchers to test different hypotheses and proposed descriptors, as well as formulate new design principles. Following a brief introduction to the background of OER mechanisms, proposed activity descriptors, and synthesis methods, various epitaxial design strategies are surveyed including strain tuning, composition control, surface termination/orientation selection, defect engineering, and interface design. These have led to precise control over the atomic structures and electronic properties of nickelates which in turn determine their electrochemical performance. Finally, the remaining challenges and perspectives toward a deeper understanding and use of complex oxides as OER catalysts are discussed.

Choi, Min‐Ju↗

Photoinduced charge transfer in transition metal dichalcogenide heterojunctions – towards next generation energy technologies

Increasing interest in using two-dimensional transition metal dichalcogenides (2D TMDCs) in optical energy conversion technologies creates a demand for improving the yields and lifetimes of photogenerated charge carriers. Despite inherently fast photocarrier decay in neat 2D TMDCs, the unique photophysics in these quantum-confined systems motivates continued effort to control the evolution of photoexcited states and create functional devices. Here, an intriguing strategy to accomplish this goal is to employ TMDCs in heterojunctions with appropriate semiconductors, where energy level offsets drive photoinduced charge transfer (PCT) across material interfaces. PCT in TMDC-based systems can be optimized for many different applications, such as driving free carriers to photocatalytic sites for redox reactions like water splitting, extracting charge to perform work in photovoltaics or photodetectors, and manipulating the spin and momentum valley electronic degrees of freedom for quantum computing systems. Here, we review recent strides in optimizing PCT for such applications through greater fundamental understanding of the photophysics that occurs at TMDC/semiconductor interfaces. After giving an overview of isolated TMDC properties, synthetic methods, and the basics of PCT, we discuss TMDCs in heterojunctions with several classes of materials, including other TMDCs, small molecule semiconductors, polymers, single-walled carbon nanotubes, quantum dots, perovskites, and electrolytes. In addition to highlighting the unique benefits of each materials category, we also identify parallels across common themes, such as the roles of charge-transfer states, spin, electronic coupling, delocalization, interfacial atomic morphology, and the precise design of energy landscapes to direct charge and energy motion. We hope to capture a broad range of the valuable work in this fast-paced field to inspire new research directions for employing PCT in targeted TMDC-based systems.

30 DIRECT ENERGY CONVERSION↗

Synthesis of La 2–x Sr x CuO 4 films via atomic layer-by-layer molecular beam epitaxy

Atomic layer-by-layer molecular beam epitaxy (ALL-MBE) is a sophisticated technique to synthesize high-temperature superconductor (HTS) materials. ALL-MBE produces single-crystal HTS films with atomically smooth surfaces and interfaces, as well as precise multilayer heterostructures engineered down to a single atomic layer level. This enables the fabrication of tunnel junctions, nanowires, nanorings, and other HTS devices of interest. Our group has focused on ALL-MBE synthesis and materials science of La 2–x Sr x CuO 4 (LSCO), a representative HTS cuprate. In the past two decades, we have synthesized over three thousand LSCO thin films and characterized them by a range of analytical techniques. Here, we present in full detail a systematic process for the synthesis and engineering of atomically perfect LSCO films. The procedure includes the preparation of substrates, calibration of the elemental sources, the recipe for ALL growth of LSCO films without any secondary-phase precipitates, post-growth annealing of the films, and ex situ film characterization. This report should aid replication and dissemination of this technique of synthesizing single-crystal LSCO films for basic research as well as for HTS electronic applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Roadmap on methods and software for electronic structure based simulations in chemistry and materials

This Roadmap article provides a succinct, comprehensive overview of the state of electronic structure methods and software for molecular and materials simulations. Seventeen distinct sections collect insights by 51 leading scientists in the field. Each contribution addresses the status of a particular area, as well as current challenges and anticipated future advances, with a particular eye towards software related aspects and providing key references for further reading. Foundational sections cover density functional theory and its implementation in real-world simulation frameworks, Green's function based many-body perturbation theory, wave-function based and stochastic electronic structure approaches, relativistic effects and semiempirical electronic structure theory approaches. Subsequent sections cover nuclear quantum effects, real-time propagation of the electronic structure, challenges for computational spectroscopy simulations, and exploration of complex potential energy surfaces. The final sections summarize practical aspects, including computational workflows for complex simulation tasks, the impact of current and future high-performance computing architectures, software engineering practices, education and training to maintain and broaden the community, as well as the status of and needs for electronic structure based modeling from the vantage point of industry environments. Overall, the field of electronic structure software and method development continues to unlock immense opportunities for future scientific discovery, based on the growing ability of computations to reveal complex phenomena, processes and properties that are determined by the make-up of matter at the atomic scale, with high precision.

36 MATERIALS SCIENCE↗

Effect of localization on photoluminescence and zero-field splitting of silicon color centers

The study of defect centers in silicon has been recently reinvigorated by their potential applications in optical quantum information processing. A number of silicon defect centers emit single photons in the telecommunication O-band, making them promising building blocks for quantum networks between computing nodes. The two-carbon G-center, self-interstitial W-center, and spin-1/2 T-center are the most intensively studied silicon defect centers, yet despite this, there is no consensus on the precise configurations of defect atoms in these centers, and their electronic structures remain ambiguous. Here, in this work, we employ ab initio density functional theory to characterize these defect centers, providing insight into the relaxed structures, band structures, and photoluminescence spectra, which are compared to experimental results. Motivation is provided for how these properties are intimately related to the localization of electronic states in the defect centers. In particular, we present the calculation of the zero-field splitting for the excited triplet state of the G-center defect as the structure is linearly interpolated from the A-configuration to the B-configuration, showing a sudden increase in the magnitude of the D zz component of the zero-field-splitting tensor. By performing projections onto the local orbital states of the defect, we analyze this transition in terms of the symmetry and bonding character of the G-center defect, which sheds light on its potential application as a spin-photon interface.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

High-Power Clock Laser Spectrally Tailored for High-Fidelity Quantum State Engineering

Highly frequency-stable lasers are ubiquitous tools for optical-frequency metrology, precision interferometry, and quantum information science. While making a universally applicable laser is unrealistic, spectral noise can be tailored for specific applications. Here we report a high-power 698-nm clock laser with a maximum output of 4W and minimized frequency noise up to a few kHz Fourier frequency, together with long-term instability of 3.5 × 10 −17 at one to thousands of seconds. The laser-frequency noise is precisely characterized with atom-based spectral analysis that employs a pulse sequence designed to suppress sensitivity to intensity noise. This method provides universally applicable tunability of the spectral response and analysis of quantum sensors over a wide frequency range. With the optimized laser system characterized by this technique, we achieve an average single-qubit Clifford gate fidelity of up to 𝐹$^2_1$ = 0.999⁢64⁢(3) when simultaneously driving 3000 optical qubits with a homogeneous Rabi frequency ranging from 10 Hz to 1 kHz. This result represents the highest single optical-qubit-gate fidelity for a large number of atoms.

atomic gases↗

Ultralow 0.034 dB/m loss wafer-scale integrated photonics realizing 720 million Q and 380 μW threshold Brillouin lasing

We demonstrate 0.034 dB/m loss waveguides in a 200-mm wafer-scale, silicon nitride (Si 3 N 4 ) CMOS-foundry-compatible integration platform. We fabricate resonators that measure up to a 720 million intrinsic Q resonator at 1615 nm wavelength with a 258 kHz intrinsic linewidth. This resonator is used to realize a Brillouin laser with an energy-efficient 380 µW threshold power. The performance is achieved by reducing scattering losses through a combination of single-mode TM waveguide design and an etched blanket-layer low-pressure chemical vapor deposition (LPCVD) 80 nm Si 3 N 4 waveguide core combined with thermal oxide lower and tetraethoxysilane plasma-enhanced chemical vapor deposition (TEOS–PECVD) upper oxide cladding. This level of performance will enable photon preservation and energy-efficient generation of the spectrally pure light needed for photonic integration of a wide range of future precision scientific applications, including quantum, precision metrology, and optical atomic clocks.

Liu, Kaikai (ORCID:0000000213609646)↗

Crystal Engineering of Hydrogen Bonding for Direct Air Capture of CO2: A Quantum Crystallography Perspective

Rising atmospheric CO2 levels demand efficient and sustainable carbon capture solutions. Direct air capture (DAC) via crystallizing hydrogen-bonded frameworks such as carbonate salts has emerged as a promising approach. This review explores the potential of crystal engineering, in tandem with advanced quantum crystallography techniques and computational modeling, to unlock the full potential of DAC materials. We examine the critical role of hydrogen bonding and other noncovalent interactions within a family of bis-guanidines that governs the formation of carbonate salts with high CO2 capture capacity and low regeneration energies for utilization. Quantum crystallography and charge density analysis prove instrumental in elucidating these interactions. A case study of a highly insoluble carbonate salt of a 2,6-pyridine-bis-(iminoguanidine) exemplifies the effectiveness of these approaches. However, challenges remain in the systematic and precise determination of hydrogen atom positions and atomic displacement parameters within DAC materials using quantum crystallography, and limitations persist in the accuracy of current energy estimation models for hydrogen bonding interactions. Future directions lie in exploring diverse functional groups, designing advanced hydrogen-bonded frameworks, and seamlessly integrating experimental and computational modeling with machine learning. This synergistic approach promises to propel the design and optimization of DAC materials, paving the way for a more sustainable future.

36 MATERIALS SCIENCE↗

Design and chemical synthesis of iodine-containing molecules for application to solar-pumped I* lasers

This work is directed toward the design and chemical synthesis of new media for solar-pumped I* lasers. In view of the desirability of preparing a perfluoroalkyl iodide absorbing strongly at 300 nm, the relationship betwen perfluoroalkyl iodide structure and the corresponding absorption wavelength was reexamined. Analysis of existing data suggests that, in this family of compounds, the absorption maximum shifts to longer wavelength, as desired, as the C-I bond in the lasant is progressively weakened. Weakening of the C-I bond correlates, in turn, with increasing stability of the perfluoroalkyl radical formed upon photodissociation of the iodide. The extremely promising absorption characteristics of perfluoro-tert-butyl iodide can be accounted for on this basis. A new technique of diode laser probing to obtain precise yields of I* atoms in photodissociation was also developed.

Shiner, C. S.↗

Proportional counters as low energy photon detectors

We investigated the response of an argon-methane proportional counter to monochromatic X-rays in the range 99 to 277 eV. The apparent nonlinearities in mean pulse height as a function of photon energy and the detailed shape of the pulse height distribution for each energy can be predicted quite precisely using the extensive atomic data available for argon. Based on this understanding, we propose a semi-empirical system for using a limited amount of calibration data to predict the full response of counters employing less well-characterized gases. Such accurate models of proportional counters are required to maximize the spectral information that can be derived from observed pulse height distributions.

Jahoda, Keith↗

Hierarchical Approach to 'Atomistic' 3-D MOSFET Simulation

We present a hierarchical approach to the 'atomistic' simulation of aggressively scaled sub-0.1 micron MOSFET's. These devices are so small that their characteristics depend on the precise location of dopant atoms within them, not just on their average density. A full-scale three-dimensional drift-diffusion atomistic simulation approach is first described and used to verify more economical, but restricted, options. To reduce processor time and memory requirements at high drain voltage, we have developed a self-consistent option based on a solution of the current continuity equation restricted to a thin slab of the channel. This is coupled to the solution of the Poisson equation in the whole simulation domain in the Gummel iteration cycles. The accuracy of this approach is investigated in comparison to the full self-consistent solution. At low drain voltage, a single solution of the nonlinear Poisson equation is sufficient to extract the current with satisfactory accuracy. In this case, the current is calculated by solving the current continuity equation in a drift approximation only, also in a thin slab containing the MOSFET channel. The regions of applicability for the different components of this hierarchical approach are illustrated in example simulations covering the random dopant-induced threshold voltage fluctuations, threshold voltage lowering, threshold voltage asymmetry, and drain current fluctuations.

Asenov, Asen↗

Conveyor-belt magneto-optical trapping of molecules

Abstract Laser cooling is used to produce ultracold atoms and molecules for quantum science and precision measurement applications. Molecules are more challenging to cool than atoms due to their vibrational and rotational internal degrees of freedom. Molecular rotations lead to the use of type-II transitions ( F ⩾ F ′ ) for magneto-optical trapping (MOT). When typical red detuned light frequencies are applied to these transitions, sub-Doppler heating is induced, resulting in higher temperatures and larger molecular cloud sizes than realized with the type-I MOTs most often used with atoms. To improve type-II MOTs, Jarvis et al (2018 Phys. Rev. Lett. 120 083201) proposed a blue-detuned MOT to be applied after initial cooling and capture with a red-detuned MOT. This was successfully implemented (Burau et al 2023 Phys. Rev. Lett. 130 193401; Jorapur et al 2024 Phys. Rev. Lett. 132 163403; Li et al 2024 Phys. Rev. Lett. 132 233402), realizing colder and denser molecular samples. Very recently, Hallas et al (2024 arXiv:2404.03636) demonstrated a blue-detuned MOT with a ‘1+2’ configuration that resulted in even stronger compression of the molecular cloud. Here, we describe and characterize theoretically the conveyor-belt mechanism that underlies this observed enhanced compression. We perform numerical simulations of the conveyor-belt mechanism using both stochastic Schrödinger equation and optical Bloch equation approaches. We investigate the conveyor-belt MOT characteristics in relation to laser parameters, g -factors and the structure of the molecule, and find that conveyor-belt trapping should be applicable to a wide range of laser-coolable molecules.

Li, Grace K. (ORCID:0000000277223355)↗

Resonant X-ray excitation of the nuclear clock isomer 45 Sc

Resonant oscillators with stable frequencies and large quality factors help us to keep track of time with high precision. Examples range from quartz crystal oscillators in wristwatches to atomic oscillators in atomic clocks, which are, at present, our most precise time measurement devices. The search for more stable and convenient reference oscillators is continuing. Nuclear oscillators are better than atomic oscillators because of their naturally higher quality factors and higher resilience against external perturbations. One of the most promising cases is an ultra-narrow nuclear resonance transition in 45 Sc between the ground state and the 12.4-keV isomeric state with a long lifetime of 0.47 s (ref. 10 ). The scientific potential of 45 Sc was realized long ago, but applications require 45 Sc resonant excitation, which in turn requires accelerator-driven, high-brightness X-ray sources that have become available only recently. Here we report on resonant X-ray excitation of the 45 Sc isomeric state by irradiation of Sc-metal foil with 12.4-keV photon pulses from a state-of-the-art X-ray free-electron laser and subsequent detection of nuclear decay products. Simultaneously, the transition energy was determined as ${\mathrm{12,389.59}}_{+0.12\left({\rm{syst}}\right)}^{\pm 0.15\left({\rm{stat}}\right)}\,{\rm{eV}}$ with an uncertainty that is two orders of magnitude smaller than the previously known values. These advancements enable the application of this isomer in extreme metrology, nuclear clock technology, ultra-high-precision spectroscopy and similar applications.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Investigating the effects of precise mass measurements of Ru and Pd isotopes on machine learning mass modeling

Atomic masses are a foundational quantity in our understanding of nuclear structure, astrophysics, and fundamental symmetries. The longstanding goal of creating a predictive global model for the binding energy of a nucleus remains a significant challenge, however, and prompts the need for precise measurements of atomic masses to serve as anchor points for model developments. We present precise mass measurements of neutron-rich Ru and Pd isotopes performed at the Californium Rare Isotope Breeder Upgrade facility at Argonne National Laboratory using the Canadian Penning Trap mass spectrometer. The masses of 108 Ru, 110 Ru, and 116 Pd were measured to a relative mass precision $\delta$⁢$m/m$ ≈ 10 -8 via the phase-imaging ion-cyclotron-resonance technique, and represent an improvement of approximately an order of magnitude over previous measurements. Further, these mass data were used in conjunction with the physically interpretable machine learning (PIML) model, which uses a mixture density neural network to model mass excesses via a mixture of Gaussian distributions. The effects of our new mass data on a Bayesian-updating of a PIML model are presented.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗