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Growth defects in thick ion-plated coatings
Industrial ion plating conditions were selected to deposit metallic coatings such as copper, gold, and chromium 2 micrometer thick on metal and glass substrates. The surface finishes of 304 stainless steel, copper, and brass were utilized with mechanically and electrolytically polished surfaces. Nodular growth occurred in these coatings during ion plating as revealed by scanning electron microscopy. Surface irregularities such as scratches, steps, ledges, and so forth are responsible for outward growth, the typical cone type, whereas surface contaminants and loosely settled foreign particles are responsible for lateral growth; namely, the extreme localized surface outgrowths. These defect crystallographic features create porosity in the coatings when subjected to stresses and strains.
Fluorine-Free Ion-Selective Membrane with Enhanced Mg 2+ Transport for Mg-Organic Batteries
Magnesium batteries offer a safer alternative for next-generation battery technology due to their insusceptibility to dendrite deposition. Selective membranes tailored for magnesium-ion conduction will unlock further technological advancement. Herein, we demonstrate fluorine-free magnesiated sulfonated poly(ether ether ketone) (Mg-SPEEK) selective membranes capable of facilitating magnesium-ion conduction while effectively rejecting soluble organic species. These membranes demonstrate a reversible Mg plating and stripping Coulombic efficiency (CE) of 85.4% and an ionic conductivity of 3.3 × 10 –4 S cm –1 at room temperature, surpassing those for a Mg-Nafion selective membrane. Theoretical density functional theory (DFT) calculations reveal that SPEEK possesses more localized charge centers along its backbone compared with Nafion, potentially facilitating enhanced ion conduction. Finally, full cells assembled with Mg-SPEEK coupled with the organic cathode pyrene-4,5,9,10-tetraone (PTO) and Mg metal demonstrated significantly improved capacity retention as compared to those assembled with conventional nonselective separators.
Ohmic Versus Rectifying Contacts of Au to N-gaas by Ion Sputtering
Results of investigations of argon ion sputtering of heavily doped n-GaAs are compared with those obtained from studies of Au/low doping density n-GaAs contacts. The Au contact on Si-doped GaAs was nearly ohmic when the surface contamination (carbon and oxides) was reduced prior to deposition by chemical cleaning. However, when ion sputtering was used in situ to clean the surface, rectifying contact was produced whose barrier height varied with the energy of the sputtering ion. It was found that ion sputtering of GaAs doped to more than 3 x 10 to the 18th power/cu may be used to change ohmic contact to rectifying contacts. The barrier height may be changed by changing the ion energy. The behavior results from the sputter creation of deep level acceptor states at the GaAs surface. Annealing after sputtering can restore the contact to nearly an ohmic character.
Microbiological Characterization and Concerns of the International Space Station Internal Active Thermal Control System
Since January 1999, the chemical the International Space Station Thermal Control System (IATCS) and microbial state of (ISS) Internal Active fluid has been monitored by analysis of samples returned to Earth. Key chemical parameters have changed over time, including a drop in pH from the specified 9.5 +/- 0.5 ta = 58.4, an increase in the level of total inorganic carbon (TIC), total organic carbon (TOC) and dissolved nickel (Ni) in the fluid, and a decrease in the phosphate (PO,) level. In addition, silver (AS) ion levels in the fluid decreased rapidly as Ag deposited on internal metallic surfaces of the system. The lack of available Ag ions coupled with changes in the fluid chemistry has resulted in a favorable environment for microbial growth. Counts of heterotrophic bacteria have increased from less than 10 colony-forming units (CFUs)/l00 mL to l0(exp 6) to l0(exp 7) CFUs/100 mL. The increase of the microbial population is of concern because uncontrolled microbiological growth in the IATCS can contribute to deterioration in the performance of critical components within the system and potentially impact human health if opportunistic pathogens become established and escape into the cabin atmosphere. Micro-organisms can potentially degrade the coolant chemistry; attach to surfaces and form biofilms; lead to biofouling of filters, tubing, and pumps; decrease flow rates; reduce heat transfer; initiate and accelerate corrosion; and enhance mineral scale formation. The micro- biological data from the ISS IATCS fluid, and approaches to addressing the concerns, are summarized in this paper.
Electrochemical studies of thin films of conducting polymers and conducting polymer composites deposited on metal and semiconductor electrodes
Electrochemical studies indicate that poly(Isothianaphthene) or PITN, can be p-doped only. Electrochemical properties of PITN and Nafion-PITN in acetonitrile solutions containing tetra-phenyl Phosphonium chloride as supporting electrolyte are compared. In both cases, the electrochemical behavior of thin films are different from that of thick films. In addition, Nafion does not seem to alter the electrochemical properties of PITN. Cyclic voltammetric and chronocoulometric measurements were made to compute the diffusion coefficient of the counter ions. Electrochemical behavior of both PITN and Nafion-PITN in acetonitrile solution containing different counter ions are described. PITN, when electrochemically deposited, apparently neither passivates surface states present nor forms ohmic contacts with p-Si or p(+)Si single-crystal electrodes.
Ion irradiation and modification: The role of coupled electronic and nuclear energy dissipation and subsequent nonequilibrium processes in materials
Understanding material responses to energy deposition from energetic charged particles is important for defect engineering, ion-beam processing, ion-beam analysis and modification, geologic aging, space exploration, and nuclear applications. As an incident ion penetrates a solid, its energy is transferred to electrons and to atomic nuclei of the solid. Much of this electronic energy deposition is subsequently transferred to the atomic structure via electron–phonon (e–ph) coupling, leading to local inelastic thermal spikes in which energy dissipation is influenced by the local environment. In addition, intense ionization can lead to high densities of localized electronic excitations in wide-bandgap materials and ceramics that can affect defect dynamics and atomic mobility. Specifically, energy exchange between electrons and atomic nuclei, along with localized electronic excitations, can lead to substantial competitive (ionization-induced annealing), additive (both electronic and nuclear energy depositions contributing to damage production), and synergistic (more damage than the sums of separate damage processes) effects. Although nonmonotonic effects of the e–ph coupling strength and athermal processes are demonstrated for pre-existing defects and residual damage during ion–solid interactions, there is limited understanding of when such electronic effects must be considered in atomic-scale models of damage production and evolution in a broad variety of materials. Complex ceramics and chemically disordered solid solution alloys with different constituent elements allow a systematic evaluation of defect dynamics and irradiation performance with increasing complexity. Current knowledge regarding tuning of bonding characteristics and chemical disorder to control atomic-level dynamics is reviewed. Although a lack of fundamental understanding obstructs the advancement of reliable predictions for ion beam material modification, it highlights challenges and opens research opportunities. Insights into the complex electronic and atomic correlations with extreme energy deposition will strengthen our ability to design materials and predict ion-irradiation-induced damage in a radiation environment, and they may pave the way to better control fundamental processes and design new material functionalities for advanced technologies.
Solvent-Free Manufacturing of Lithium-Ion Battery Electrodes via Cold Plasma
Slurry casting has been used to fabricate lithium-ion battery electrodes for decades, which involves toxic and expensive organic solvents followed by high-cost vacuum drying and electrode calendering. This work presents a new manufacturing method using a nonthermal plasma to create inter-particle binding without using any polymeric binding materials, enabling solvent-free manufacturing electrodes with any electrochemistry of choice. The cold-plasma-coating technique enables fabricating electrodes with thickness (>200 μm), high mass loading (>30 mg cm -2 ), high peel strength, and the ability to print lithium-ion batteries in an arbitrary geometry. This crosscutting, chemistry agnostic, platform technology would increase energy density, eliminate the use of solvents, vacuum drying, and calendering processes during production, and reduce manufacturing cost for current and future cell designs. Here, lithium iron phosphate and lithium cobalt oxide were used as examples to demonstrate the efficacy of the cold-plasma-coating technique. It is found that the mechanical peel strength of cold-plasma-coating-manufactured lithium iron phosphate is over an order of magnitude higher than that of slurry-casted lithium iron phosphate electrodes. Full cells assembled with a graphite anode and the cold-plasma-coating-lithium iron phosphate cathode offer highly reversible cycling performance with a capacity retention of 81.6% over 500 cycles. For the highly conductive cathode material lithium cobalt oxide, an areal capacity of 4.2 mAh cm -2 at 0.2 C is attained. We anticipate that this new, highly scalable manufacturing technique will redefine global lithium-ion battery manufacturing providing significantly reduced plant footprints and material costs.
YBa2Cu3O(7-x)/Au/Nb device structures
Fabrication and testing of planar and edge geometry YBaCuO/Au/Nb superconductor/normal-metal/superconductor (SNS) device structures is described. Weak-link devices of this type serve as sensitive probes of the electrical quality of the YBaCuO/Au interface. The devices are fabricated using laser-ablated, in situ, c-axis-oriented YBaCuO thin films, with both annealed and unannealed YBaCuO/Au interfaces. The planar SNS structures are formed by sequential, in situ deposition of YBaCuO, Au, and Nb, followed by etching, planarization, and wiring electrode definition to produce junctions ranging from 5 to 20 micron on a side. Resulting RnA products are 1-10 x 10 to the -8th ohm-sq cm with critical current densities up to 5 kA/sq cm. For the edge geometry devices, the YBaCuO film edges are patterned using Ar ion milling, followed by a low energy ion cleaning step and in situ deposition of Au and Nb. Devices with areas in the 10 to the -7th to 10 to the -8th sq cm range have been fabricated with RnA products lower than 10 to the -8th ohm-sq cm and critical current densities up to 3kA/sq cm. Both types of devices show ac Josephson steps under microwave irradiation. The best results have been obtained with annealed YBaCuO/Au interfaces.
InP shallow-homojunction solar cells
Indium phosphide solar cells with very thin n-type emitters have been made by both ion implantation and metalorganic chemical vapor deposition. Air mass zero efficiencies as high as 18.8 percent (NASA measurement) have been achieved. Although calculations show that, as is the case with GaAs, a heterostructure is expected to be required for the highest efficiencies attainable, the material properties of InP give the shallow-homojunction structure a greater potential than in the case of GaAs. The best cells, which were those made by ion implantation, show open-circuit voltage (V sub oc) of 873 mV, short-circuit current of 357 A/sq m (35.7 mA/sq cm), and fill factor of 0.829. Improvements are anticipated in all three of these parameters. Internal quantum efficiency peaks at over 90 percent in the red end of the spectrum, but drops to 54 percent in the blue end. Other cells have achieved 74 percent in the blue end. Detailed modeling of the data indicates that a high front surface recombination velocity is responsible for the low blue response, that the carrier lifetime is high enough to allow good carrier collection from both the base and the emitter, and that the voltage is base-limited.
Atomic-scale constituting stable interface for improved LiNi 0.6 Mn 0.2 Co 0.2 O 2 cathodes of lithium-ion batteries
Ascribed to their higher capacity and lower cost compared to conventional LiCoO 2 , the Ni-rich layered LiNi 0.6 Mn 0.2 Co 0.2 O 2 (NMC622) is now considered as one promising cathode for lithium-ion batteries (LIBs). However, it still suffers from some evident performance degradation, especially under high cutoff voltages (i.e., >4.3 V versus Li/Li + ). The performance degradation typically is exhibited as capacity fading and voltage drop, mainly originating from an instable interface between the NMC622 and electrolyte as well as the evolution of the NMC structure. To improve the interfacial and structural stability of NMC cathodes, herein we deposited an ultrathin layer of Al 2 O 3 coatings (<5 nm) conformally over NMC622 composite electrodes directly using atomic layer deposition (ALD). It was found that, under different upper cutoff voltages (4.3, 4.5, and 4.7 V), the ALD Al 2 O 3 coatings enable enhanced performance of NMC622 cathodes with better cyclability and higher capacity. Particularly, the beneficial effects of the ALD Al 2 O 3 coatings are more remarkable at higher upper cutoff voltages (4.5 and 4.7 V). Furthermore, the ALD coatings can significantly improve the rate capability of NMC622. To this end, we utilized a suite of characterization tools and performed a series of electrochemical tests to clarify the effects of the ALD Al 2 O 3 coatings. This study revealed that the beneficial effects of the Al 2 O 3 ALD coatings are multiple: (i) serving as an artificial layer of solid electrolyte interphase to mitigate undesirable interfacial reactions; (ii) acting as a physical barrier to inhibit metal dissolution of NMC; and (iii) forming a reinforced networked overcoating to boost the mechanical integrity of NMC cathodes. This study is favorable for designing high-performance NMC cathodes.
Flare heating by energetic nonthermal electrons
A model has been developed which includes, in a self-consistent fashion, the energy degradation and attendant bremsstrahlung emission of a high-energy electron beam, heating of a flare plasma by the beam, and subsequent cooling by thermal conduction and radiation. To assist in the interpretation of experimental diagnostics, the model also characterizes the radiative behavior of iron ions present in the flare plasma. Electron deposition is described by the Fokker-Planck equation for an initial power-law particle distribution. Results are presented for the bremsstrahlung radiation emitted by the incident beam as it impinges on the disturbed atmosphere. A comparison is made between direct beam heating and thermal-conduction heating of the flare plasma. The radiation emitted by several selected spectral lines of Fe ions is determined as a function of time during and after deposition
Microfabrication Ion Acceleration Grid Design Issues: Electronic Breakdown Characteristics of Silicon Dioxide Insulator Material
Low-temperature (LTO) chemical vapor deposited (CVD) silicon dioxide was investigated for use as an insulator matierial in microfabriacted ion engine accelerator grids.
Assessing Metal Ion Assignment Accuracy in Protein Data Bank Models via Elemental Spectroscopy
Accurate representation of metal ions in macromolecular structures is critical for chemical interpretation, computational modeling, and machine-learning methods that rely on Protein Data Bank (PDB) entries. However, the elemental identity of metals modeled in crystallographic structures is often inferred indirectly and rarely validated experimentally. Here, we combine Particle Induced X-ray Emission (PIXE) and X-ray Fluorescence Spectroscopy (XRFS) to determine the elemental composition of protein samples used to generate 70 deposited metalloprotein crystal structures. By analyzing the original protein material employed for crystallization, but before the addition of crystallization buffer solutions, we assess whether the modeled metal ions in deposited structures are consistent with experimentally detectable elemental content. We find that in a majority of cases, the metals modeled in the corresponding PDB entries are inconsistent with the metals present in the protein samples before crystallization, or that additional metals are present but not represented in the structural models. Spectroscopic results were integrated with automated crystallographic validation metrics, including real-space Z-difference (RSZD) analysis and systematic rerefinement, to evaluate atomic-number mismatch at metal sites. PIXE and XRFS show strong agreement for dominant elemental signals and provide complementary, scalable approaches for identifying suspect metal assignments. This work does not address physiological or functional metalation but instead highlights a widespread data integrity issue in deposited macromolecular structures, PDB-wide. These results establish an experimentally corroborated link between elemental identity and crystallographic validation metrics, enabling the large-scale detection of chemically inconsistent annotations in structural databases used for computational modeling and machine learning.
Magnetohydrodynamic Control of Interfacial Degradation in Lithium-Ion Batteries for Fast Charging Applications
Interfacial anodic degradation in graphitic materials under fast charging conditions causes severe performance loss and safety hazard in lithium ion batteries. We present a novel method for minimizing the growth of these aging mechanism by application of an external magnetic field. Under magnetic field, paramagnetic lithium ions experience a magnetohydrodynamic force, which rotates the perpendicularly diffusing species and homogenizes the ionic transport. This phenomenon minimizes the overpotential hotspots at the anode/separator interface, consequently reducing SEI growth, lithium plating, and interfacial fracture. In situ electrochemical measurements indicate an improvement in capacity for lithium cobalt oxide/graphite pouch cell (20 mAh) charged from 1–5 C under an applied field of 1.8 kG, with a maximum capacity gain of 22% at 5C. Post-mortem FE-SEM and EDS mapping shows that samples charged with magnetic field have a reduced lithium deposition at 3C and a complete suppression of interfacial fracture at 5C. At 5C, a 24% reduction in the lithium content is observed by performing XPS on the anodic interfacial film. Finally, fast charging performance under variable magnetic field strengths indicate a saturation behavior in capacity at high fields (>2 kG), thereby limiting the field and consequent energy requirements to obtain maximum capacity gain under extreme conditions.
Nonlinear burn control in ITER using adaptive allocation of actuators with uncertain dynamics
Abstract ITER will be the first tokamak to sustain a fusion-producing, or burning, plasma. If the plasma temperature were to inadvertently rise in this burning regime, the positive correlation between temperature and the fusion reaction rate would establish a destabilizing positive feedback loop. Careful regulation of the plasma’s temperature and density, or burn control, is required to prevent these potentially reactor-damaging thermal excursions, neutralize disturbances and improve performance. In this work, a Lyapunov-based burn controller is designed using a full zero-dimensional nonlinear model. An adaptive estimator manages destabilizing uncertainties in the plasma confinement properties and the particle recycling conditions (caused by plasma–wall interactions). The controller regulates the plasma density with requests for deuterium and tritium particle injections. In ITER-like plasmas, the fusion-born alpha particles will primarily heat the plasma electrons, resulting in different electron and ion temperatures in the core. By considering separate response models for the electron and ion energies, the proposed controller can independently regulate the electron and ion temperatures by requesting that different amounts of auxiliary power be delivered to the electrons and ions. These two commands for a specific control effort (electron and ion heating) are sent to an actuator allocation module that optimally maps them to the heating actuators available to ITER: an electron cyclotron heating system (20 MW), an ion cyclotron heating system (20 MW), and two neutral beam injectors (16.5 MW each). Two different actuator allocators are presented in this work. The first actuator allocator finds the optimal mapping by solving a convex quadratic program that includes actuator saturation and rate limits. It is nonadaptive and assumes that the mapping between the commanded control efforts and the allocated actuators (i.e. the effector model) contains no uncertainties. The second actuator allocation module has an adaptive estimator to handle uncertainties in the effector model. This uncertainty includes actuator efficiencies, the fractions of neutral beam heating that are deposited into the plasma electrons and ions, and the tritium concentration of the fueling pellets. Furthermore, the adaptive allocator considers actuator dynamics (actuation lag) that contain uncertainty. This adaptive allocation algorithm is more computationally efficient than the aforementioned nonadaptive allocator because it is computed using dynamic update laws so that finding the solution to a static optimization problem is not required at every time step. A simulation study assesses the performance of the proposed adaptive burn controller augmented with each of the actuator allocation modules.
Ion beam microtexturing of surfaces
Some recent work in surface microtecturing by ion beam sputtering is described. The texturing is accomplished by deposition of an impurity onto a substrate while simultaneously bombarding it with an ion beam. A summary of the theory regarding surface diffusion of impurities and the initiation of cone formation is provided. A detailed experimental study of the time-development of individual sputter cones is described. A quasi-liquid coating was observed that apparently reduces the sputter rate of the body of a cone compared to the bulk material. Experimental measurements of surface diffusion activation energies are presented for a variety of substrate-seed combinations and range from about 0.3 eV to 1.2 eV. Observations of apparent crystal structure in sputter cones are discussed. Measurements of the critical temperature for cone formation are also given along with a correlation of critical temperature with substrate sputter rate.
Enabling 4C Fast Charging of Lithium–Ion Batteries by Coating Graphite with a Solid–State Electrolyte
Enabling fast-charging (≥4C) of lithium-ion batteries is an important challenge to accelerate the adoption of electric vehicles. However, the desire to maximize energy density has driven the use of increasingly thick electrodes, which hinders rate capability. Herein, atomic layer deposition is used to coat a single-ion conducting solid electrolyte (Li 3 BO 3 -Li 2 CO 3 ) onto postcalendered graphite electrodes, forming an artificial solid-electrolyte interphase (SEI). When compared to uncoated control electrodes, the solid electrolyte coating: 1) eliminates natural SEI formation during preconditioning; 2) decreases interphase impedance by >75% compared to the natural SEI; and 3) extends cycle life under 4C charging conditions, enabling retention of 80% capacity after 500 cycles (compared to 12 cycles in the uncoated control) in pouch cells with >3 mAh cm –2 loading. Furthermore, this work demonstrates that 4C charging without Li plating can be achieved through purely interfacial modification without sacrificing energy density and sheds new light on the role of the SEI in Li plating and fast-charge performance.