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At least 487 records · Page 27

Architecting a Stable High-Energy Aqueous Al-Ion Battery

Aqueous Al-ion batteries (AAIBs) are the subject of great interest due to the inherent safety and high theoretical capacity of aluminum. The high abundancy and easy accessibility of aluminum raw materials further make AAIBs appealing for grid-scale energy storage. However, the passivating oxide film formation and hydrogen side reactions at the aluminum anode as well as limited availability of the cathode lead to low discharge voltage and poor cycling stability. Here, we proposed a new AAIB system consisting of an Al x MnO 2 cathode, a zinc substrate-supported Zn-Al alloy anode, and an Al(OTF) 3 aqueous electrolyte. Through the in situ electrochemical activation of MnO, the cathode was synthesized to incorporate a two-electron reaction, thus enabling its high theoretical capacity. The anode was realized by a simple deposition process of Al 3+ onto Zn foil substrate. The featured alloy interface layer can effectively alleviate the passivation and suppress the dendrite growth, ensuring ultralong-term stable aluminum stripping/plating. The architected cell delivers a record-high discharge voltage plateau near 1.6 V and specific capacity of 460 mAh g -1 for over 80 cycles. Finally, this work provides new opportunities for the development of high-performance and low-cost AAIBs for practical applications.

25 ENERGY STORAGE↗

Fluoride-Rich, Organic–Inorganic Gradient Interphase Enabled by Sacrificial Solvation Shells for Reversible Zinc Metal Batteries

Zinc metal batteries are strongly hindered by water corrosion, as solvated zinc ions would bring the active water molecules to the electrode/electrolyte interface constantly. Herein, we report a sacrificial solvation shell to repel active water molecules from the electrode/electrolyte interface and assist in forming a fluoride-rich, organic-inorganic gradient solid electrolyte interface (SEI) layer. Additionally, the simultaneous sacrificial process of methanol and Zn(CF 3 SO 3 ) 2 results in the gradient SEI layer with an organic-rich surface (CH 2 OC- and C 5 product) and an inorganic-rich (ZnF 2 ) bottom, which combines the merits of fast ion diffusion and high flexibility. As a result, the methanol additive enables corrosion-free zinc stripping/plating on copper foils for 300 cycles with an average coulombic efficiency of 99.5%, a record high cumulative plating capacity of 10 A h/cm 2 at 40 mA/cm 2 in Zn/Zn symmetrical batteries. More importantly, at an ultralow N/P ratio of 2, the practical VO 2 //20 mu m thick Zn plate full batteries with a high areal capacity of 4.7 mAh/cm 2 stably operate for over 250 cycles, establishing their promising application for grid-scale energy storage devices. Furthermore, directly utilizing the 20 μm thick Zn for the commercial-level areal capacity (4.7 mAh/cm 2 ) full zinc battery in our work would simplify the manufacturing process and boost the development of the commercial zinc battery for stationary storage.

25 ENERGY STORAGE↗

Decoherence of $V^{–}_{B}$ spin defects in monoisotopic hexagonal boron nitride

Spin defects in hexagonal boron nitride (hBN) are promising quantum systems for the design of flexible two-dimensional quantum sensing platforms. Here we rely on hBN crystals isotopically enriched with either 10 B or 11 B to investigate the isotope-dependent properties of a spin defect featuring a broadband photoluminescence signal in the near infrared. By analyzing the hyperfine structure of the spin defect while changing the boron isotope, we first confirm that it corresponds to the negatively charged boron-vacancy center ($V^{–}_{B}$). We then show that its spin coherence properties are slightly improved in 10B-enriched samples. This is supported by numerical simulations employing cluster correlation expansion methods, which reveal the importance of the hyperfine Fermi contact term for calculating the coherence time of point defects in hBN. Using cross-relaxation spectroscopy, we finally identify dark electron spin impurities as an additional source of decoherence. This work provides new insights into the properties of $V^{–}_{B}$ spin defects, which are valuable for the future development of hBN-based quantum sensing foils.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Spatiotemporal dynamics of fast electron heating in solid-density matter via XFEL

Abstract High-intensity, short-pulse lasers are crucial for generating energetic electrons that produce high-energy-density (HED) states in matter, offering potential applications in igniting dense fusion fuels for fast ignition laser fusion. High-density targets heated by these electrons exhibit spatially non-uniform and highly transient conditions, which have been challenging to characterize due to limitations in diagnostics that provide simultaneous high spatial and temporal resolution. Here, we employ an X-ray Free Electron Laser (XFEL) to achieve spatiotemporally resolved measurements at sub-micron and femtosecond scales on a solid-density copper foil heated by laser-driven fast electrons. Our X-ray transmission imaging reveals the formation of a solid-density hot plasma localized to the laser spot size, surrounded by Fermi degenerate, warm dense matter within a picosecond, and the energy relaxation occurring within the hot plasma over tens of picoseconds. These results validate 2D particle-in-cell simulations incorporating atomic processes and provide insights into the energy transfer mechanisms beyond current simulation capabilities. This work significantly advances our understanding of rapid fast electron heating and energy relaxation in solid-density matter, serving as a key stepping stone towards efficient high-density plasma heating and furthering the fields of HED science and inertial fusion energy research using intense, short-pulse lasers.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Low-symmetry vacancy-related spin qubit in hexagonal boron nitride

Abstract Point defect qubits in semiconductors have demonstrated their outstanding capabilities for high spatial resolution sensing generating broad multidisciplinary interest. Hexagonal boron nitride (hBN) hosting point defect qubits have recently opened up new horizons for quantum sensing by implementing sensing foils. The sensitivity of point defect sensors in hBN is currently limited by the linewidth of the magnetic resonance signal, which is broadened due to strong hyperfine couplings. Here, we report on a vacancy-related spin qubit with an inherently low symmetry configuration, the VB2 center, giving rise to a reduced magnetic resonance linewidth at zero magnetic fields. The VB2 center is also equipped with a classical memory that can be utilized for storing population information. Using scanning transmission electron microscopy imaging, we confirm the existence of the VB2 configuration in free-standing monolayer hBN.

Chemistry↗

Impact of nitrogen on lithium-induced corrosion and cracking of RAFM steel

The emergence of private fusion enterprises, combined with advancements in U.S. and EU ITER-TBM as well as EU DEMO liquid breeder blanket concepts, has renewed focus on the materials challenges. This study examines the compatibility of reduced activation ferritic/martensitic (RAFM) steel in liquid Lithium (Li) containing various Nitrogen (N) concentrations, tested at 600 and 700 °C for 500 and 1000 h under static conditions. Microstructural characterization revealed the corrosion-induced dissolution and precipitation in Li containing 0.082 and 0.17 wt.% N at 600 °C, while limited dissolution and precipitation were observed in N-gettered Li using zirconium (Zr) and titanium (Ti) foils at 600 °C. Tensile testing at room temperature after Li exposure revealed a decrease in strength and ductility of the RAFM steel as a function of N content in Li. Severe embrittlement was observed after 500 h in Li containing 0.17 wt.% N at 600 °C and after 500 h in hot-gettered Li at 700 °C. Chromium (Cr) depletion from the steel matrix was observed, leading to the formation of M6C-type carbides on the surface identified by electron microscopy (SEM), X-ray diffraction (XRD), in agreement with thermodynamic calculations. These findings highlight the critical materials challenges posed by liquid Li breeder blanket concepts, emphasizing the need for improved strategies to address Li-induced dissolution, precipitation, and steel embrittlement due to N contamination of the coolant.

Romedenne, Marie [ORNL] (ORCID:0000000317936561)↗

Revealing the three-dimensional structure of microbunched plasma-wakefield-accelerated electron beams

Abstract Plasma wakefield accelerators use tabletop equipment to produce relativistic femtosecond electron bunches. Optical and X-ray diagnostics have established that their charge concentrates within a micrometre-sized volume, but its sub-micrometre internal distribution, which critically influences gain in free-electron lasers or particle yield in colliders, has proven elusive to characterize. Here, by simultaneously imaging different wavelengths of coherent optical transition radiation that a laser-wakefield-accelerated electron bunch generates when exiting a metal foil, we reveal the structure of the coherently radiating component of bunch charge. The key features of the images are shown to uniquely correlate with how plasma electrons injected into the wake: by a plasma-density discontinuity, by ionizing high- Z gas-target dopants or by uncontrolled laser–plasma dynamics. With additional input from the electron spectra, spatially averaged coherent optical transition radiation spectra and particle-in-cell simulations, we reconstruct coherent three-dimensional charge structures. The results demonstrate an essential metrology for next-generation compact X-ray free-electron lasers driven by plasma-based accelerators.

43 PARTICLE ACCELERATORS↗

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↗

The X-Ray Emission Effectiveness of Plasma Mirrors: Reexamining Power-Law Scaling for Relativistic High-Order Harmonic Generation

Ultrashort pulsed lasers provide uniquely detailed access to the ultrafast dynamics of physical, chemical, and biological systems, but only a handful of wavelengths are directly produced by solid-state lasers, necessitating efficient high-power frequency conversion. Relativistic plasma mirrors generate broadband power-law spectra, that may span the gap between petawatt-class infrared laser facilities and x-ray free-electron lasers; despite substantial theoretical work the ultimate efficiency of this relativistic high-order-harmonic generation remains unclear. We show that the coherent radiation emitted by plasma mirrors follows a power-law distribution of energy over frequency with an exponent that, even in the ultrarelativistic limit, strongly depends on the ratio of laser intensity to plasma density and exceeds the frequently quoted value of -8/3 over a wide range of parameters. The coherent synchrotron emission model, when adequately corrected for the finite width of emitting electron bunches, is not just valid for p-polarized light and thin foil targets, but generally describes relativistic harmonic generation, including at normal incidence and with finite-gradient plasmas. Our numerical results support the ω-4/3 scaling of the synchrotron emission model as a limiting efficiency of the process under most conditions. The highest frequencies that can be generated with this scaling are usually restricted by the width of the emitting electron bunch rather than the Lorentz factor of the fastest electrons. The theoretical scaling relations developed here suggest, for example, that with a 20-PW 800-nm driving laser, 1 TW/harmonic can be produced for 1-keV photons.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Focussing Protons from a Kilojoule Laser for Intense Beam Heating using Proximal Target Structures

Proton beams driven by chirped pulse amplified lasers have multi-picosecond duration and can isochorically and volumetrically heat material samples, potentially providing an approach for creating samples of warm dense matter with conditions not present on Earth. Envisioned on a larger scale, they could heat fusion fuel to achieve ignition. We have shown in an experiment that a kilojoule-class, multi-picosecond short pulse laser is particularly effective for heating materials. The proton beam can be focussed via target design to achieve exceptionally high flux, important for the applications mentioned. The laser irradiated spherically curved diamond-like-carbon targets with intensity 4 × 10 18 W/cm 2 , producing proton beams with 3 MeV slope temperature. A Cu witness foil was positioned behind the curved target, and the gap between was either empty or spanned with a structure. With a structured target, the total emission of Cu Kα fluorescence was increased 18 fold and the emission profile was consistent with a tightly focussed beam. Transverse proton radiography probed the target with ps order temporal and 10 μm spatial resolution, revealing the fast-acting focussing electric field. Complementary particle-in-cell simulations show how the structures funnel protons to the tight focus. Here, the beam of protons and neutralizing electrons induce the bright Kα emission observed and heat the Cu to 100 eV.

47 OTHER INSTRUMENTATION↗

First on-line detection of radioactive fission isotopes produced by laser-accelerated protons

Abstract The on-going developments in laser acceleration of protons and light ions, as well as the production of strong bursts of neutrons and multi- $$\hbox {MeV}$$ MeV photons by secondary processes now provide a basis for novel high-flux nuclear physics experiments. While the maximum energy of protons resulting from Target Normal Sheath Acceleration is presently still limited to around $$100 \, \hbox {MeV}$$ 100 MeV , the generated proton peak flux within the short laser-accelerated bunches can already today exceed the values achievable at the most advanced conventional accelerators by orders of magnitude. This paper consists of two parts covering the scientific motivation and relevance of such experiments and a first proof-of-principle demonstration. In the presented experiment pulses of $$200 \, \hbox {J}$$ 200 J at $$\approx \, 500 \, \hbox {fs}$$ ≈ 500 fs duration from the PHELIX laser produced more than $$10^{12}$$ 10 12 protons with energies above $$15 \, \hbox {MeV}$$ 15 MeV in a bunch of sub-nanosecond duration. They were used to induce fission in foil targets made of natural uranium. To make use of the nonpareil flux, these targets have to be very close to the laser acceleration source, since the particle density within the bunch is strongly affected by Coulomb explosion and the velocity differences between ions of different energy. The main challenge for nuclear detection with high-purity germanium detectors is given by the strong electromagnetic pulse caused by the laser-matter interaction close to the laser acceleration source. This was mitigated by utilizing fast transport of the fission products by a gas flow to a carbon filter, where the $$\upgamma$$ γ -rays were registered. The identified nuclides include those that have half-lives down to $$39 \, \hbox {s}$$ 39 s . These results demonstrate the capability to produce, extract, and detect short-lived reaction products under the demanding experimental condition imposed by the high-power laser interaction. The approach promotes research towards relevant nuclear astrophysical studies at conditions currently only accessible at nuclear high energy density laser facilities.

07 ISOTOPE AND RADIATION SOURCES↗

Quantized electronic transitions in electrodeposited copper indium selenide nanocrystalline homojunctions

Pairing semiconductors with electrochemical processing offers an untapped opportunity to create novel nanostructures for practical devices. Here we report the results of one such pairing: the in-situ formation of highly-doped, interface-matched, sharp nanocrystalline homojunctions (NHJs) with single step electrodeposition of two copper-indium-selenide (CISe) compounds on flexible foil. It produces a homogenous film, comprising inherently ordered, 3-dimensional interconnected network of pn -CISe NHJs. These CISe NHJs exhibit surprising non-linear emissions, quantized transitions, large carrier mobility, low trap-state-density, long carrier lifetime and possible up-conversion. They facilitate efficient separation of minority carriers, reduce recombination and essentially function like quantum materials. This approach mitigates the material issues and complex fabrication of incumbent nanoscale heterojunctions; it also overcomes the flexibility and scale-up challenges of conventional planar pn junctions. The self-stabilized CISe NHJ film can be roll-to-roll processed in ambient atmosphere, thus providing a promising platform for a range of optoelectronic technologies. This concept exemplified by CISe compounds can be adapted to create nano-scale pn junctions with other inorganic semiconductors.

36 MATERIALS SCIENCE↗

Super-strong magnetic field-dominated ion beam dynamics in focusing plasma devices

High energy density physics is the field of physics dedicated to the study of matter and plasmas in extreme conditions of temperature, densities and pressures. It encompasses multiple disciplines such as material science, planetary science, laboratory and astrophysical plasma science. For the latter, high energy density states can be accompanied by extreme radiation environments and super-strong magnetic fields. The creation of high energy density states in the laboratory consists in concentrating/depositing large amounts of energy in a reduced mass, typically solid material sample or dense plasma, over a time shorter than the typical timescales of heat conduction and hydrodynamic expansion. Laser-generated, high current–density ion beams constitute an important tool for the creation of high energy density states in the laboratory. Focusing plasma devices, such as cone-targets are necessary in order to focus and direct these intense beams towards the heating sample or dense plasma, while protecting the proton generation foil from the harsh environments typical of an integrated high-power laser experiment. A full understanding of the ion beam dynamics in focusing devices is therefore necessary in order to properly design and interpret the numerous experiments in the field. In this work, we report a detailed investigation of large-scale, kilojoule-class laser-generated ion beam dynamics in focusing devices and we demonstrate that high-brilliance ion beams compress magnetic fields to amplitudes exceeding tens of kilo-Tesla, which in turn play a dominant role in the focusing process, resulting either in a worsening or enhancement of focusing capabilities depending on the target geometry.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Demonstration of an intense lithium beam for forward-directed pulsed neutron generation

Abstract As an alternative to research nuclear reactors, a compact accelerator-driven neutron generator that uses a lithium beam driver could be a promising candidate since it produces almost no undesired radiation. However, providing an intense lithium-ion beam has been difficult, and it has been thought that the practical application of such a device would be impossible. The most critical problem of insufficient ion fluxes has been solved by applying a direct plasma injection scheme. In this scheme, a pulsed high-density plasma from a metallic lithium foil generated by laser ablation is efficiently injected and accelerated by a radio-frequency quadrupole linear accelerator (RFQ linac). We have obtained a peak beam current of 35 mA accelerated to 1.43 MeV, which is two orders of magnitude higher than a conventional injector and accelerator system can deliver.

43 PARTICLE ACCELERATORS↗

Natural and enriched Cr target development for production of Manganese-52

52 Mn is a promising PET radiometal with a half-life of 5.6 days and an average positron energy of 242 keV. Typically, chromium of natural isotope abundance is used as a target material to produce this isotope through the nat/52 Cr(p,n) 52 Mn reaction. While natural Cr is a suitable target material, higher purity 52 Mn could be produced by transitioning to enriched 52 Cr targets to prevent the co-production of long-lived 54 Mn (t 1/2 = 312 day). Unfortunately, 52 Cr targets are not cost-effective without recycling processes in place, therefore, this work aims to explore routes to prepare Cr targets that could be recycled. Natural Cr foils, metal powder pellets, enriched chromium-52 oxide and Cr(III) electroplated targets were investigated in this work. Each of these cyclotron targets were irradiated, and the produced 52 Mn was purified, when possible, using a semi-automated system. An improved purification by solid-phase anion exchange from ethanol-HCl mixtures resulted in recoveries of 94.5 ± 2.2% of 52 Mn. The most promising target configuration to produce a recyclable target was electroplated Cr(III). This work presents several pathways to optimize enriched Cr targets for the production of high purity 52 Mn.

62 RADIOLOGY AND NUCLEAR MEDICINE↗

Fabrication of THz corrugated wakefield structure and its high power test

We present overall process for developing terahertz (THz) corrugated structure and its beam-based measurement results. 0.2-THz corrugated structures were fabricated by die stamping method as the first step demonstration towards GW THz radiation source and GV/m THz wakefield accelerator. 150-μm thick disks were produced from an OFHC (C10100) foil by stamping. Two types of disks were stacked alternately to form 46 mm structure with ~ 170 corrugations. Custom assembly was designed to provide diffusion bonding with a high precision alignment of disks. The compliance of the fabricated structure have been verified through beam-based wakefield measurement at Argonne Wakefield Accelerator Facility. Both measured longitudinal and transverse wakefield showed good agreement with simulated wakefields. Measured peak gradients, 9.4 MV/m/nC for a long single bunch and 35.4 MV/m/nC for a four bunch trains, showed good agreement with the simulation.

43 PARTICLE ACCELERATORS↗

Production and performance of a 172 Hf/ 172 Lu generator

A 172 Hf/ 172 Lu radionuclide generator system to produce 172 Lu for laboratory scale applications in lutetium-based radiochemistry development was established and evaluated. The parent 172 Hf radionuclide was produced through 35.2 MeV proton irradiation of natural lutetium metal foil at the Brookhaven Linac Isotope Producer. Four resins were investigated for 172 Hf separation from bulk Lu target material: LN resin, ZR resin, in-house synthesized hydroxamate, and methyl-substituted hydroxamate resins, all with comparable performance. Separated 172 Hf was consolidated and used to create a ZR resin-based 4.9(3) MBq 172 Hf/ 172 Lu generator which was eluted 49 times over two years with no observed breakthrough of 172 Hf, and an average elution efficiency of 98(1)%. The eluted 172 Lu was used to radiolabel the macrocyclic chelator DOTA with an apparent molar activity of 8(2)x10 2 kBq/nmol.

172Hf/172Lu radionuclide generator↗