DFT Studies of Electronic Properties and Effect of He and Xe Incorporation in Selected Ceramics

The electronic properties of several prospective nuclear fuels are not yet well known. We used Quantum Espresso and EPW codes to evaluate the electron density of states, the electronic heat capacity coefficient, the electron-phonon coupling strength, the number of mobility electrons, and the electronic heat conductivity. The electronic properties for ThN, ThC and UN using a slightly different approach that were previously evaluated are discussed and the results are compared. We confirmed that while the electronic heat capacity coefficient is linearly dependent on the electron density of states at Fermi energy, such a simple relation could not be used to determine the difference in the electronic heat conductivity of investigated materials. The highest heat conductivity was registered in ThN. These metallic fuels also have high U/Th density, therefore are more economical since enrichment is expensive. Furthermore, it is important to examine swelling in these high-density fuels. We evaluated that UN had 42% more U atoms per unit volume than UO2 and a 55% higher volume increase when accommodating one Xe atom in one interstitial of a (2 × 2 × 2) supercell. However, for He, the volume increase was 27% lower in UN. Interestingly, even though the Th atom’s density in ThN and ThC was lower than that of U atoms in the UN compound, a similar trend of volume changes was found. We concluded, therefore, that when we consider swelling, the local structural symmetry (tetrahedral versus octahedral sites) is more important than the density of atoms. The 37 % greater of absolute value of the total energy increase due to incorporation of Xe in ThC versus ThN cannot be explained by the crystal structure since a ThC-Xe supercell has a higher lattice constant than a ThN-Xe corresponding supercell. Such results can only be explained by investigating electronic structure.

Interface engineering in two-dimensional heterostructures towards novel emitters

Two-dimensional(2D) semiconductors have captured broad interest as light emitters, due to their unique excitonic effects. These layer-blocks can be integrated through van der Waals assembly, i.e., fabricating homo-or heterojunctions, which show novel emission properties caused by interface engineering. In this review, we will first give an overview of the basic strategies that have been employed in interface engineering, including changing components, adjusting interlayer gap, and tuning twist angle. By modifying the interfacial factors, novel emission properties of emerging excitons are unveiled and discussed. Generally, well-tailored interfacial energy transfer and charge transfer within a 2D heterostructure cause static modulation of the brightness of intralayer excitons. As a special case, dynamically correlated dual-color emission in weakly-coupled bilayers will be introduced, which originates from intermittent interlayer charge transfer. For homobilayers and type Ⅱ heterobilayers, interlayer excitons with electrons and holes residing in neighboring layers are another important topic in this review. Moreover, the overlap of two crystal lattices forms moiré patterns with a relatively large period, taking effect on intralayer and interlayer excitons. Particularly, theoretical and experimental progresses on spatially modulated moiré excitons with ultra-sharp linewidth and quantum emission properties will be highlighted. Moiré quantum emitter provides uniform and integratable arrays of single photon emitters that are previously inaccessible, which is essential in quantum many-body simulation and quantum information processing. Benefiting from the optically addressable spin and valley indices, 2D heterostructures have become an indispensable platform for investigating exciton physics, designing and integrating novel concept emitters.

Effects of vacuum magnetic field region on the compact torus trajectory in a tokamak plasma

The trajectory of the compact torus(CT)within a tokamak discharge is crucial to fueling.In this study,we developed a penetration model with a vacuum magnetic field region to accurately determine CT trajectories in tokamak discharges.This model was used to calculate the trajectory and penetration parameters of CT injections by applying both perpendicular and tangential injection schemes in both HL-2A and ITER tokamaks.For perpendicular injection along the tokamak's major radius direction from the outboard,CTs with the same injection parameters exhibited a 0.08 reduction in relative penetration depth when injected into HL-2A and a 0.13reduction when injected into ITER geometry when considering the vacuum magnetic field region compared with cases where this region was not considered.In addition,we proposed an optimization method for determining the CT's initial injection velocity to accurately calculate the initial injection velocity of CTs for central fueling in tokamaks.Furthermore,this paper discusses schemes for the tangential injection of CT into tokamak discharges.The optimal injection angle and CT magnetic moment direction for injection into both HL-2A and ITER were determined through numerical simulations.Finally,the kinetic energy loss occurring when the CT penetrated the vacuum magnetic field region in ITER was reduced byΔEk=975.08 J by optimizing the injection angle for the CT injected into ITER.These results provide valuable insights for optimizing injection angles in fusion experiments.Our model closely represents actual experimental scenarios and can assist the design of CT parameters.

Identifying the Zn-Co binary as a robust bifunctional electrocatalyst in oxygen reduction and evolution reactions via shifting the apexes of the volcano plot

The performance of an electrocatalyst is closely correlated with the binding strength of key oxygencontaining intermediates,i.e.,*OOH,*O and*OH,in the oxygen reduction reaction(ORR)and oxygen evolution reaction(OER).Facile strategies to achieve favorable binding strength of these oxygen-containing species are urgently demanded,yet it still remains great challenges.Herein,the Zn-Co bimetallic isolation,which serves as an ideal model,is studied systematically by the density functional theory(DFT).Reaction activity volcano plots are built from 48 models,among them the ZnCoN6-gra(I)configuration is confirmed to be the most stable,featured of the strongest interaction with the oxygen-containing species.Optimal △G*O(free energy change of an atomic oxygen containing intermediate)is facilitated,which effectively drifts the volcano peaks of ORR and OER closer to each other,enabling promising bifunctional catalyst.Moreover,the small overpotential in the simulation of protonation and oxidation by hydroxy groups rationalizes the durability of the catalyst in both acid and alkaline media.

Mean-field description of heavy-ion scattering at low energies and fusion

The nuclear mean-field potential built up during the ^(12)C+^(12)C and ^(16)O+^(16)O collisions at low energies relevant for the carbon-and oxygen-burning processes is constructed within the double-folding model(DFM) using the realistic ground-state densities of^(12)C and^(16)O, and CDM3Yn density-dependent nucleon–nucleon(NN) interaction. The rearrangement term, indicated by the Hugenholtz–van Hove theorem for the single-particle energy in nuclear matter, is properly considered in the DFM calculation. To validate the use of the density-dependent NN interaction at low energies, an adiabatic approximation was suggested for the dinuclear overlap density. The reliability of the nucleus–nucleus potential predicted through this low-energy version of the DFM was tested in the optical model(OM) analysis of the elastic^(12)C+^(12)C and ^(16)O+^(16)O scattering data at energies below 10 MeV/nucleon.These OM results provide a consistently good description of the elastic angular distributions and 90 excitation function. The dinuclear mean-field potential predicted by the DFM is further used to determine the astrophysical S factor of the ^(12)C+^(12)C and ^(16)O+^(16)O fusions in the barrier penetration model. Without any adjustment of the potential strength, our results reproduce the non-resonant behavior of the S factor of the ^(12)C+^(12)C and ^(16)O+^(16)O fusions very well over a wide range of energies.

First-Principles Methods in the Investigation of the Chemical and Transport Properties of Materials under Extreme Conditions

Earth is a dynamic system. The thermodynamics conditions of Earth vary drastically depending on the depth, ranging from ambient temperature and pressure at the surface to 360 GPa and 6600 K at the core. Consequently, the physical and chemical properties of Earth’s constituents (e.g., silicate and carbonate minerals) are strongly affected by their immediate environment. In the past 30 years, there has been a tremendous amount of progress in both experimental techniques and theoretical modeling methods for material characterization under extreme conditions. These advancements have elevated our understanding of the properties of minerals, which is essential in order to achieve full comprehension of the formation of this planet and the origin of life on it. This article reviews recent computational techniques for predicting the behavior of materials under extreme conditions. This survey is limited to the application of the first-principles molecular dynamics (FPMD) method to the investigation of chemical and thermodynamic transport processes relevant to Earth Science.

Inelastic Cotunneling Current and Shot Noise of an Interacting Quantum Dot with Ferromagnetic Correlations

We explore inelastic cotunneling through a strongly Coulomb-blockaded quantum dot attached to twoferromagnetic leads in the weak coupling limit using a generic quantum Langevin equation approach.We first developa B1och-type equation microscopically to describe the cotunneling-induced spin relaxation dynamics,and then developexplicit analytical expressions for the local magnetization,current,and its fluctuations.On this basis,we predict a novelzero-bias anomaly of the differential conductance in the absence of a magnetic field for the anti-parallel configuration,and asymmetric peak splitting in a magnetic field.Also,for the same system with large polarization,we find a negativezero-frequency differential shot noise in the low positive bias-voltage region. All these effects are ascribed to rapidspin-reversal due to underlying spin-flip cotunneling.

Effect of Cleaving Temperature on the Surface and Bulk Fermi Surface of Sr2RuO4 Investigated by High Resolution Angle-Resolved Photoemission

High resolution angle-resolved photoemission measurements are carried out to systematically investigate the effect of cleaving temperature on the electronic structures and Fermi surfaces of Sr2RuO4.Unlike previous reports,which found that a high cleaving temperature can suppress the surface Fermi surface,we find that the surface Fermi surface remains obvious and strong in Sr2RuO4 cleaved at high temperature,even at room temperature.This indicates that cleaving temperature is not a key effective factor in suppressing surface bands.On the other hand,the bulk bands can be enhanced in an aged surface of Sr2RuO4 that has been cleaved and held for a long time.We have also carried out laser ARPES measurements on Sr_(2)RuO_(4) by using a vacuum ultra-violet laser (photon energy at 6.994eV) and found an obvious enhancement of bulk bands even for samples cleaved at low temperature.This information is important for realizing an effective approach to manipulating and detecting the surface and bulk electronic structure of Sr2RuO4.In particular,the enhancement of bulk sensitivity,along with the super-high instrumental resolution of VUV laser ARPES,will be advantageous in investigating fine electronic structure and superconducting properties of Sr_(2)RuO_(4) in the future.

A Novel Outage Capacity Objective Function for Optimal Performance Monitoring and Predictive Fault Detection in Hybrid Free-Space Optical and RF Wireless Networks

This study develops an optimal performance monitoring metric for a hybrid free space optical and radio wireless network, the Outage Capacity Objective Function. The objective function—the dependence of hybrid channel outage capacity upon the error rate, jointly quantifies the effects of atmospheric optical impairments on the performance of the free space optical segment as well as the effect of RF channel impairments on the radio frequency segment. The objective function is developed from the basic information-theoretic capacity of the optical and radio channels using the gamma-gamma model for optical fading and Ricean statistics for the radio channel fading. A simulation is performed by using the hybrid network. The objective function is shown to provide significantly improved sensitivity to degrading performance trends and supports of proactive link failure prediction and mitigation when compared to current thresholding techniques for signal quality metrics.

Structural Domain Imaging and Direct Determination of Crystallographic Orientation in Noncentrosymmetric Ca3 Ru2O7 Using Polarized Light Reflectance

The noncentrosymmetricity of a prototypical correlated electron system Ca3Ru2O7 renders extensive interest in the possible polar metallic state,along with multiple other closely competing interactions.However,the structural domain formation in this material often complicates the study of intrinsic material properties.It is crucial to fully characterize the structural domains for unrevealing underlying physics.Here,we report the domain imaging on Ca3Ru2O7 crystal using the reflection of polarized light at normal incidence.The reflection anisotropy measurement utilizes the relative orientation between electric field component of the incident polarized light and the principal axis of the crystal,and gives rise to a peculiar contrast.The domain walls are found to be the interfaces between 90° rotated twin crystals by complementary magnetization measurements.A distinct contrast in reflectance is also found in the opposite cleavage surfaces,owing to the polar mode of the RuO6 octahedra.More importantly,the analysis of the contrast between all inequivalent cleavage surfaces enables a direct determination of the crystallographic orientation of each domain.Such an approach provides an efficient yet feasible method for structural domain characterization,which can also find applications in noncentrosymmetric crystals in general.

Synthesis and Characterization of Metal Organic Chemical Vapour Deposited Chromium Doped Zinc Oxide Thin Film for Gas Sensing Applications

Chromium (Cr) doped Zinc oxide ZnO thin films were deposited onto glass substrates by Metal Organic Chemical Vapour Deposition (MOCVD) technique with varying dopant concentration at a temperature of 420°C. The effect of the chromium concentration on morphological, structural, optical, electrical and gas sensing properties of the films were investigated. The scanning electron microscopy results revealed that the Cr concentration has great influence on the crystallinity, surface smoothness and grain size. X-ray diffraction (XRD) studies shows that films were polycrystalline in nature and grown as a hexagonal wurtzite structure. A direct optical band energy gap of 3.32 to 3.10 eV was obtained from the optical measurements. The transmission was found to decrease with increasing Cr doping concentration. Rutherford Backscattering Spectroscopy (RBS) analysis also demonstrates that Cr ions are substitutionally incorporated into ZnO. I-V characteristic of the film shows a resistivity ranges from 1.134 × 10-2 · cm to 1.24 × 10-2 · cm at room temperature. The gas sensing response of the films were enhanced with incorporation of Cr as a dopant with optimum operating temperature around 200°C.

Preparation and Some Properties of Metal Organic Chemical Vapour Deposited Al-Doped ZnO Thin Films Using Single Solid Precursors

Zinc Oxide (ZnO) and Aluminium doped ZnO (AZO) thin films were deposited on soda lime glass by Metal Organic Chemical Vapour deposition technique (MOCVD), using prepared compound mixtures of Zinc Acetate di-hydrate (Zn(CH3COO)2⋅2H2O;ZAD) and Aluminium Acetyl-Acetonate (Al(C5H702)3;AAA) precursors at a temperature of 420°C. Effects of the varying mole percent concentrations of AAA precursor additives on the Al dopant concentrations in ZnO were systematically studied. The observations were made via investigations carried out on the morphological, optical, electrical and compositional properties of the deposited thin films. The thin films morphology was found to be strongly dependent on the varying concentration of AAA in the precursor mixtures. The average optical transmittance of the thin films in the uv-visible region was over 85% except 5 mol.% Al. While the energy band gaps were found to be in range of 3.27 - 3.36 eV. There is a blue-shift of the energy band edge observed between 0 and 5 mol.% AAA, which may be due to Burstein-Moss’ band gap widening effect and an opposing band gap renormalization effect at 10 mol.% AAA along with an extra band gap stabilization effect (Roth’s effect) at 15 mol.% AAA in rather quasi-sinusoidal or anomalous behaviour. The optical transmittance and electrical conductivity of ZnO were enhanced with addition of Al dopants. The RBS confirm the presence of Al, Zn and O, and evidence that Al dopants were successfully incorporated into the ZnO.

Positron Annihilation in Perfect and Defective TiO₂Rutile Crystal with Single Particle Wave Function: Slater Type Orbital and Modified Jastrow Functions

Positron annihilation in TiO2 rutile crystal is studied by an assumption that a positron binds with valance electrons of a titanium dioxide to form a pseudo TiO2-positron molecule before it annihilates with these electrons. The orbital modification consisting of explicit electron-positron and electron-electron correlation in each electronic orbital is used for the electrons and positron wave functions. By these wave functions, the calculation results of the positron lifetimes in unmitigated and defective TiO2 crystals are about 170 ps, 266 ps and 243 ps, respectively. These results are in good agreement with experimental data of the positron lifetimes in vacancies of TiO2 from 180 ps to 300 ps.

Synthesis and Characterization of Graphene Oxide and Reduced Graphene Oxide Thin Films Deposited by Spray Pyrolysis Method

Graphene Oxide (GO) was chemically synthesized from Natural Flake Graphite (NFG). The GO was chemically reduced to Reduced Graphene Oxide (RGO) using hydrazine monohydrate. Thin films of GO and RGO were also deposited on sodalime glass substrate using spray pyrolysis technique (SPT). The samples were characterized using Fourier Transform Infrared (FTIR) spectroscopy, Scanning Electron Microscopy (SEM) with Energy Dispersive X-Ray (EDS) facility attached to it, UV-Visible Spectrometry and Four-Point probe. The FTIR spectra showed the addition of oxygen functionality groups in GO while such groups was drastically reduced in RGO. SEM micrograph of GO thin film showed a porous sponge-like structure while the micrograph of RGO thin film showed evenly distributed and well connected graphene structure. The EDX spectrum of RGO showed that there was decrease in oxygen content and increase in carbon content of RGO when compared to GO. The optical analysis of the GO and RGO thin films gave a direct energy bandgap of 2.7 eV and 2.2 eV respectively. The value of sheet resistance of GO and RGO films was determined to be 22.9 × 106Ω/sq and 4.95 × 106Ω/sq respectively.

Single photon emitters originating from donor-acceptor pairs

Starting from the groundbreaking work in graphene[1],the active research in two-dimensional(2D)layered materials has unveiled a number of exotic phenomena that are unique in the 2D limit.In addition to the semimetal graphene,the semiconducting transition metal dichalcogenides(TMDs)and the insulating hexagonal boron nitride(hBN)are also the main driving forces of the field.

一种超硬新材料BeP2N4的电子结构和力学性质及本征硬度

基于密度泛函理论,采用局域密度近似(LDA)和广义梯度近似(GGA)泛函研究了硅铍石、尖晶石结构的BeP_2N_4材料的晶格参数、能带结构、态密度、分态密度、Mulliken布居值和弹性性质,计算结果与已有的实验值和理论值符合很好.能带结构和态密度表明两种结构的BeP_2N_4材料是宽的直接带隙的绝缘体材料.尖晶石结构BeP_2N_4的体弹性模量、剪切模量和弹性模量比硅铍石结构的相应的力学量大得多.利用Sung等提出的硬度经验划据和Gao等提出的基于Muilliken轨道重叠布居数的共价同体本征硬度计算方法,预测了两种结构的本征硬度值.计算结果表明硅铍石结构BeP_2N_4虽然体弹模量小,但是它并不是一种软的材料,而是一种易脆的硬度较硬的材料,随着压力增加硅铍石结构BeP_2N_4的脆性逐渐过渡到延性.尖晶石结构BeP_2N_4是一种易脆的超硬材料.采用GGA计算得到的硅铍石BeP_2N_4向尖晶石相转变压力为14 GPa,与理论预测值(24 GPa)相比偏小.

Co-MOF as an electron donor for promoting visible-light photoactivities of g-C3N4 nanosheets for CO2 reduction

A possible mechanism for boosting the visible-light photoactivities of graphitic carbon nitride(g-C3N4)nanosheets for CO2 reduction via coupling with the electron donor Co-metal-organic framework(MOF)is proposed in this study.Specifically,Co-MOF as an electron donor is capable of transferring the photogenerated electrons in the lowest unoccupied molecular orbital(LUMO)to the conduction band of g-C3N4 to facilitate charge separation.As expected,the prepared Co-MOF/g-C3N4 nanocomposites display excellent visible-light-driven photocatalytic CO2 reduction activities.The CO production rate of 6.75μmol g–1 h–1 and CH4 evolution rate of 5.47μmol g–1 h–1 are obtained,which are approximately 2 times those obtained with the original g-C3N4 under the same conditions.Based on a series of analyses,it is shown that the introduction of Co-MOF not only broadens the range of visible-light absorption but also enhances the charge separation,which improves the photocatalytic activity of g-C3N4 to a higher level.In particular,the hydroxyl radical(·OH)experiment was operated under 590 nm(single-wavelength)irradiation,which further proved that the photogenerated electrons in the LUMO of Co-MOF can successfully migrate to g-C3N4.This work may provide an important strategy for the design of highly efficient g-C3N4-based photocatalysts for CO2 reduction.

Interface electron collaborative migration of Co–Co3O4/carbon dots:Boosting the hydrolytic dehydrogenation of ammonia borane

Ammonia borane(AB)is an excellent candidate for the chemical storage of hydrogen.However,its practical utilization for hydrogen production is hindered by the need for expensive noble-metal-based catalysts.Herein,we report Co-Co3O4 nanoparticles(NPs)facilely deposited on carbon dots(CDs)as a highly efficient,robust,and noble-metal-free catalyst for the hydrolysis of AB.The incorporation of the multiinterfaces between Co,Co3O4 NPs,and CDs endows this hybrid material with excellent catalytic activity(rB=6816 mLH2 min^-1 gCo^-1)exceeding that of previous non-noble-metal NP systems and even that of some noble-metal NP systems.A further mechanistic study suggests that these interfacial interactions can affect the electronic structures of interfacial atoms and provide abundant adsorption sites for AB and water molecules,resulting in a low energy barrier for the activation of reactive molecules and thus substantial improvement of the catalytic rate.

Development of a compact torus injection system for the Keda Torus eXperiment

A compact torus injection system,KTX-CTI,has been developed for the planned injection experiments on the Keda Torus e Xperiment(KTX)reversed field pinch(RFP)device to investigate the physics and engineering issues associated with interaction between a compact torus(CT)and RFP.The key interests include fueling directly into the reactor center,confinement improvement,and the injection of momentum and helicity into the RFP discharges.The CT velocity and mass have been measured using a multichannel optical fiber interferometer,and for the first time the time evolution of the CT density profile during CT propagation is obtained.The effects of discharge parameters on the number of injected particles,CT velocity and CT density have been characterized:the maximum hydrogen CT plasma mass,m,CTis 50μg,corresponding to 30%of the mass in a typical KTX plasma;the CT velocity exceeds 120 km s-1.It is observed for the first time that multiple CTs can be produced and emitted during a very short period(<100μs)in one discharge,which is significant for the future study of repetitive CT injection,even with an ultra-high frequency.