LiMnO[subscript 2] cathode stabilized by interfacial orbital ordering for sustainable lithium-ion ba
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Multi-electron polyanion cathodes offer the potential for achieving both high voltage and high capacity in rechargeable alkali-ion batteries. Among the few materials known to exhibit multi-electron cycling, the polymorphs of VOPO 4 , which operate on the V 3+ –V 4+ –V 5+ redox couples, are particularly promising due to the high gravimetric capacities that have been achieved and the high voltage of the V 4+/5+ couple. In this work, we performed a systematic first principles investigation, supported by careful electrochemical characterization and published experimental data, of the relative thermodynamic stability, voltage, band gap, and diffusion kinetics for alkali intercalation into the β, ε and αI polymorphs of VOPO 4 . We find that all VOPO4 polymorphs remain reasonably stable with the insertion of one alkali ion per V, but are significantly destabilized with the insertion of two alkali ions per V. The voltages for Na insertion are ~0.33–0.69 V lower than those for Li insertion. We find that the αI polymorph is predicted to have higher Li + migration barriers and larger band gaps than the β and ε polymorphs, which account for the relatively worse electrochemical cycling performance observed. On the other hand, only the αI polymorph exhibits reasonably low barriers for Na + migration compared to the β and ε polymorphs, which are consistent with observed electrochemical performances reported thus far in the literature. We also show that differences in the voltage, kinetics and rate capability of these different polymorphs for Li and Na insertion can be traced back to their fundamentally different VO 6 /VO 5 -PO 4 frameworks.
We present results of combined experimental photoelectron spectroscopy and theoretical modeling studies of solvated dicarboxylate species ( − O 2 C(CH 2 ) 2 CO 2 − ) in complex with Na + and K + metal cations.
Uniform size of Si nanowires (NWs) is highly desirable to enhance the performance of Si NW-based lithium-ion batteries.
Fully non-linear kinetic simulations of electron plasma and ion acoustic waves (IAWs) have been carried out with a new multi-species, parallelized Vlasov code. The numerical implementation of the Vlasov model and the methods used to compute the wave frequency are described in detail. For the first time, the nonlinear frequency of IAWs, combining the contributions from electron and ion kinetic effects and from harmonic generation, has been calculated and compared to Vlasov results. Excellent agreement of theory with simulation results is shown at all amplitudes, harmonic generation being an essential component at large amplitudes. For IAWs, the positive frequency shift from trapped electrons is confirmed and is dominant for the effective electron-to-ion temperature ratio, Z T{sub e}/T{sub i} Greater-Than-Or-Equivalent-To 10 with Z as the charge state. Furthermore, numerical results demonstrate unambiguously the dependence [R. L. Dewar, Phys. Fluids 15, 712 (1972)] of the kinetic shifts on details of the distribution of the trapped particles, which depends in turn on the conditions under which the waves were generated. The trapped particle fractions and energy distributions are derived and, upon inclusion of harmonic effects, shown to agree with the simulation results, completing a consistent picture. Fluid models of the wave evolution are considered but prove unable to capture essential details of the kinetic simulations. Detrapping by collisions and sideloss is also discussed.
Extraction of negative ions from a saddle antenna radio-frequency surface plasma source is considered. Several versions of new plasma generators with different antennas and magnetic field configurations were tested in the smal Oak Ridge National Laboratory Spallation Neutron Source Test Stand. The efficiency of positive ion generation in plasma has been improved to 200 mA/cm{sup 2} kW from 2.5 mA/cm{sup 2} kW. A small oven was developed for cesiation by cesium compounds and alloy decomposition. After cesiation, a current of negative ions to the collector was increased from 1 mA to 10 mA with 1.5 kW RF power in the plasma and longitudinal magnetic field B{sub l} ∼ 250 G. The specific efficiency of H{sup −} production was increased to 20 mA/cm{sup 2} kW from 2.5 mA/cm{sup 2} kW.
Dust-ion-acoustic (DIA) rogue waves are investigated in a three-dimensional magnetized plasma containing nonthermal electrons featuring Tsallis distribution, both positive and negative ions, and immobile dust grains having both positive and negative charges. Via the reductive perturbation method, a (3 + 1)-dimensional nonlinear Schrödinger (NLS) equation is derived to govern the dynamics of the DIA wave packets. The modulation instability of DIA waves described by the (3 + 1)-dimensional NLS equation is investigated. By means of the similarity transformation and symbolic computation, both the first- and second-order rogue wave solutions of the (3 + 1)-dimensional NLS equation are constructed in terms of rational functions. Moreover, the dynamics properties and the effects of plasma parameters on the nonlinear structures of rogue waves are discussed in detail. The results could be useful for understanding the physical mechanism of rogue waves in laboratory experiments where pair-ion plasmas with electrons and dust grains can be found.
Upgrades to electronic hardware and detector design have been made to the JET thin-foil Faraday cup fast ion loss detector in anticipation of the upcoming deuterium–tritium (DT) campaign. An improved foil stack design has been implemented, which greatly reduces the number of foil-to-foil shorts, and triaxial cabling has mitigated ambient noise pickup. Initial tests of 200 kHz digitizers, as opposed to the original 5 kHz digitizers, have provided enhanced analysis techniques and direct coherence measurements of fast ion losses with magnetohydrodynamic activity. Here, we present recent loss measurements in JET deuterium plasmas correlated with kink modes, fishbone modes, edge-localized modes, and sawteeth. Sources of systematic noise are discussed with emphasis on capacitive plasma pickup. Overall, the system upgrades have established a diagnostic capable of recording alpha particle losses due to a wide variety of resonant fast ion transport mechanisms to be used in future DT-experiments and modeling efforts.
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We compare the suitability of various magnesium-based liquid metal alloy ion sources (LMAISs) for scalable focused-ion-beam (FIB) implantation doping of GaN. We consider GaMg, MgSO 4 $\bullet$7H 2 O, MgZn, AlMg, and AuMgSi alloys. Although issues of oxidation (GaMg), decomposition (MgSO 4 $\bullet$7H 2 O), and excessive vapor pressure (MgZn and AlMg) were encountered, the AuMgSi alloy LMAIS operating in a Wien-filtered FIB column emits all Mg isotopes in singly and doubly charged ionization states. We discuss the operating conditions to achieve <20 nm spot size Mg FIB implantation and present Mg depth profile data from time-of-flight secondary ion mass spectrometry. We also provide insight into implantation damage and recovery based on cathodoluminescence spectroscopy before and after rapid thermal processing. Prospects for incorporating the Mg LMAIS into high-power electronic device fabrication are also discussed.
An electron beam ion source serves as a charge breeder for the Californium Rare Isotope Breeder Upgrade (CARIBU) at the Argonne Tandem Linac Accelerator System (ATLAS). The source accepts radioactive beams of 1+ or 2+ ions and raises their charge state for post-acceleration by ATLAS. The efficiency of this process impacts the length of each experiment and, hence, the type and number of experiments that can be run in each program cycle. Recent efforts to improve the charge breeding efficiency for the 80 < A < 160 species typical of CARIBU have focused on utilizing the closed shell breeding technique. Here, with this technique, the electron beam energy is manipulated to take advantage of the large gap in ionization energies at shell closures and selectively populate a single charge state. Charge breeding studies with stable cesium ions have demonstrated an absolute efficiency of 72% for Cs 27+ and a total efficiency of 93%. The Cs 27+ efficiency result represents a factor of 3 improvement over the previous best charge breeding result of 23% for Cs 27+ .
Linear plasma devices are cost-effective alternatives for testing materials under reactor-relevant divertor plasma conditions. In this work, we describe how an intense radio-frequency (RF) plasma source concept for the Material Plasma Exposure eXperiment (MPEX) is under development at Oak Ridge National Laboratory. The source concept, Proto-MPEX, aims to produce high-density background deuterium helicon plasmas ( n e > 3 × 10 19 m - 3 ) that are subsequently heated with additional RF and microwave systems to deliver reactor-relevant conditions for studies on plasma-material interaction. In this work, we focus on the plasma-producing stage and its effectiveness in converting input neutral gas into plasma, namely, the neutral gas ionization efficiency. We provide a direct quantitative measurement of the ionization efficiency by measuring the total ion flux arriving at the target region relative to the neutral gas injected at the source. Using 80 kW at 13.56 MHz and a source magnetic field of 0.05 T, the helicon plasma source delivers ion fluxes up to 1 × 10 24 m - 2 s - 1 and heat fluxes greater than 1 M W m - 2 to a target plate located 2 m away from the source. Under these conditions, we observe that the plasma source converts ~89% of the input neutral gas into plasma that arrives at the target as ion flux at a rate of 5 × 10 20 s - 1 . We demonstrate that because of the large pumping capacity of the plasma, neutral gas pumping systems are required only in the target region to maintain optimal plasma operation.
There is considerable interest in improving plant productivity by altering the dynamic responses of photosynthesis in tune with natural conditions. This is exemplified by the 'energy-dependent' form of non-photochemical quenching (q E ), the formation and decay of which can be considerably slower than natural light fluctuations, limiting photochemical yield. In addition, we recently reported that rapidly fluctuating light can produce field recombination-induced photodamage (FRIP), where large spikes in electric field across the thylakoid membrane (Δψ) induce photosystem II recombination reactions that produce damaging singlet oxygen ( 1 O 2 ). Both q E and FRIP are directly linked to the thylakoid proton motive force (pmf), and in particular, the slow kinetics of partitioning pmf into its ΔpH and Δψ components. In this work, using a series of computational simulations, we explored the possibility of 'hacking' pmf partitioning as a target for improving photosynthesis. Under a range of illumination conditions, increasing the rate of counter-ion fluxes across the thylakoid membrane should lead to more rapid dissipation of Δψ and formation of ΔpH. This would result in increased rates for the formation and decay of qE while resulting in a more rapid decline in the amplitudes of Δψ-spikes and decreasing 1 O 2 production. These results suggest that ion fluxes may be a viable target for plant breeding or engineering. However, these changes also induce transient, but substantial mismatches in the ATP : NADPH output ratio as well as in the osmotic balance between the lumen and stroma, either of which may explain why evolution has not already accelerated thylakoid ion fluxes. Overall, though the model is simplified, it recapitulates many of the responses seen in vivo, while spotlighting critical aspects of the complex interactions between pmf components and photosynthetic processes. By making the programme available, we hope to enable the community of photosynthesis researchers to further explore and test specific hypotheses. This article is part of the themed issue 'Enhancing photosynthesis in crop plants: targets for improvement'.
The electron-ion collider (EIC), to be constructed at Brookhaven National Laboratory, will collide polarized high-energy electron beams with hadron beams, achieving luminosities of up to 1.0 × 10 34 cm −2 s −1 in the center-of-mass energy range of 20–140 GeV. To reach such high luminosity, the EIC will employ small, flat beams at the interaction point. According to the design of the EIC hadron storage ring (HSR), hadron beams with a large transverse emittance ratio of 11:1 will be generated at the injection energy using an electron cooling technique and then accelerated to high energies for collisions. Accelerating hadron beams with such a large emittance ratio had never been demonstrated elsewhere—until our recent beam experiment at the relativistic heavy ion collider (RHIC). In this experiment, we successfully generated a large transverse emittance ratio of 13:1 with a gold-ion beam at 31 GeV/nucleon using stochastic cooling. We then accelerated this beam, with a transverse emittance ratio of 11:1, from 31 to 100 GeV/nucleon. Thanks to RHIC’s high-performance orbit, tune, and decoupling feedback systems, the large emittance ratio was well maintained throughout the 5-min-long acceleration process. This experiment fully validated the EIC/HSR design assumptions—namely, that large-emittance-ratio hadron beams can be generated at injection energy and then accelerated to high energies for collisions.
Electron correlation plays a crucial role in quantum many-body physics ranging from molecular bonding, strong-field–induced multi-electron ionization, to superconducting in materials. Understanding the dynamic electron correlation in the photoionization of relatively simple quantum three-body systems, such as He and He-like ions, is an important step toward manipulating complex systems through photo-induced processes. Here we have performed ab initio investigations of two-photon double ionization (TPDI) of He and He-like ions [Li + , Be 2+ , and C 4+ ] exposed to intense attosecond x-ray pulses. Results from such fully correlated quantum calculations show weaker and weaker electron correlation effects in TPDI spectra as the ionic charge increases, which is counterintuitive to the belief that the strongly correlated ground state and the strong Coulomb field of He-like ions should lead to more equal-energy sharing in photoionization. Lastly, these findings indicate that the final-state electron–electron correlation ultimately determines their energy sharing in TPDI.
Within five different approaches to parton propagation and energy loss in dense matter, a phenomenological study of experimental data on suppression of large- p T single inclusive hadrons in heavy-ion collisions at both the BNL Relativistic Heavy Ion Collider (RHIC) and the CERN Large Hadron Collider (LHC) was carried out. The evolution of bulk medium used in the study for parton propagation was given by 2 + 1 dimensional or 3 + 1 dimensional hydrodynamic models which are also constrained by experimental data on bulk hadron spectra. Values for the jet transport parameter $\hat{q}$ at the center of the most central heavy-ion collisions are extracted or calculated within each model, with parameters for the medium properties that are constrained by experimental data on the hadron suppression factor R AA . For a quark with initial energy of 10 GeV we find that $\hat{q}$ ≈ 1.2 ± 0.3 GeV 2 /fm at an initial time τ 0 = 0.6 fm/ c in Au + Au collisions at √s = 200 GeV/n and $\hat{q}$ ≈ 1.9 ± 0.7 GeV 2 /fm in Pb + Pb collisions at √s = 2.76 TeV/n. Compared to earlier studies, these represent significant convergence on values of the extracted jet transport parameter due to new constraints provided by recent experiment data from the LHC.
Here, the strong ion-ion correlation peak characteristic of warm dense matter (WDM) is observed for the first time using simultaneous angularly, temporally, and spectrally resolved x-ray scattering measurements in laser-driven shock-compressed aluminum. Laser-produced molybdenum x-ray line emission at an energy of 17.9 keV is employed to probe aluminum compressed to a density of ρ > 8 g/cm 3 . We observe a well pronounced peak in the static structure factor at a wave number of $\textit{k}$ = 4:0 Å -1 . The measurements of the magnitude and position of this correlation peak are precise enough to test different theoretical models for the ion structure and show that only models taking the complex interaction in WDM into account agree with the data. As a result, this also demonstrates a new highly accurate diagnostic to directly measure the state of compression of warm dense matter.