Stability of concentration-related self-interstitial atoms in fusion material tungsten

Based on the density functional theory, we calculated the structures of the two main possible self-interstitial atoms（SIAs） as well as the migration energy of tungsten（W） atoms. It was found that the difference of the 110 and 111 formation energies is 0.05–0.3 e V. Further analysis indicated that the stability of SIAs is closely related to the concentration of the defect. When the concentration of the point defect is high, 110 SIAs are more likely to exist, 111 SIAs are the opposite. In addition, the vacancy migration probability and self-recovery zones for these SIAs were researched by making a detailed comparison. The calculation provided a new viewpoint about the stability of point defects for selfinterstitial configurations and would benefit the understanding of the control mechanism of defect behavior for this novel fusion material.

Superatomic-based chirality:Asymmetric structures constructed by superatoms

Chirality is one of the fundamental properties of molecules traditionally con-structed from atoms.Here,we report for thefirst time the successful construction of asymmetric chiral structures utilizing highly symmetric endohedral metallo-fullerene superatoms based on their own bonding properties.Specifically,stable mirror-symmetric sinister and rectus structures are obtained by selecting a super-atom capable of forming four chemical bonds as the chiral center.Further analysis shows that the chiral vibration frequency of superatomic assemblies can be as low as a few wavenumbers,which greatly expands the range of chiral spectra com-pared to atom-based molecules.We term this type of chirality based on superatoms as“superatomic-based chirality”.It is anticipated that this work will significantly expand the variety of chiral structures at the atomic level.

Efficient loading of cesium atoms in a magnetic levitated dimple trap

We report a detailed study of magnetically levitated loading of ultracold ^(133)Cs atoms in a dimple trap.The atomic sample was produced in a combined red-detuned optical dipole trap and dimple trap formed by two small waist beams crossing a horizontal plane.The magnetic levitation for the ^(133)Cs atoms forms an effective potential for a large number of atoms in a high spatial density.Dependence of the number of atoms loaded and trapped in the dimple trap on the magnetic field gradient and bias field is in good agreement with the theoretical analysis.This method has been widely used to obtain the Bose–Einstein condensation atoms for many atomic species.

Advances of Synergistic Electrocatalysis Between Single Atoms and Nanoparticles/Clusters

Combining single atoms with clusters or nanoparticles is an emerging tactic to design efficient electrocatalysts.Both synergy effect and high atomic utilization of active sites in the composite catalysts result in enhanced electrocatalytic performance,simultaneously provide a radical analysis of the interrelationship between structure and activity.In this review,the recent advances of single-atomic site catalysts coupled with clusters or nanoparticles are emphasized.Firstly,the synthetic strategies,characterization,dynamics and types of single atoms coupled with clusters/nanoparticles are introduced,and then the key factors controlling the structure of the composite catalysts are discussed.Next,several clean energy catalytic reactions performed over the synergistic composite catalysts are illustrated.Eventually,the encountering challenges and recommendations for the future advancement of synergistic structure in energy-transformation electrocatalysis are outlined.

Physics package based on intracavity laser cooling ^(87)Rb atoms for space cold atom microwave clock

This article proposes a new physics package to enhance the frequency stability of the space cold atom clock with the advantages of a microgravity environment. Clock working processes, including atom cooling, atomic state preparation,microwave interrogation, and transition probability detection, are integrated into the cylindrical microwave cavity to achieve a high-performance and compact physics package for the space cold atom clock. We present the detailed design and ground-test results of the cold atom clock physics package in this article, which demonstrates a frequency stability of 1.2×10^(-12) τ^(-1/2) with a Ramsey linewidth of 12.5 Hz, and a better performance is predicted with a 1 Hz or a narrower Ramsey linewidth in microgravity environment. The miniaturized cold atom clock based on intracavity cooling has great potential for achieving space high-precision time-frequency reference in the future.

Geometric properties of the first singlet S-wave excited state of two-electron atoms near the critical nuclear charge

The geometric structure parameters and radial density distribution of 1s2s1S excited state of the two-electron atomic system near the critical nuclear charge Z_(c)were calculated in detail under tripled Hylleraas basis set.Contrary to the localized behavior observed in the ground and the doubly excited 2p^(23)Pe states,for this state our results identify that while the behavior of the inner electron increasingly resembles that of a hydrogen-like atomic system,the outer electron in the excited state exhibits diffused hydrogen-like character and becomes perpendicular to the inner electron as nuclear charge Z approaches Z_(c).This study provides insights into the electronic structure and stability of the two-electron system in the vicinity of the critical nuclear charge.

Achieving Negatively Charged Pt Single Atoms on Amorphous Ni(OH)_(2)Nanosheets with Promoted Hydrogen Absorption in Hydrogen Evolution

Single-atom(SA)catalysts with nearly 100%atom utilization have been widely employed in electrolysis for decades,due to the outperforming catalytic activity and selectivity.However,most of the reported SA catalysts are fixed through the strong bonding between the dispersed single metallic atoms with nonmetallic atoms of the substrates,which greatly limits the controllable regulation of electrocatalytic activity of SA catalysts.In this work,Pt-Ni bonded Pt SA catalyst with adjustable electronic states was successfully constructed through a controllable electrochemical reduction on the coordination unsaturated amorphous Ni(OH)_(2)nanosheet arrays.Based on the X-ray absorption fine structure analysis and first-principles calculations,Pt SA was bonded with Ni sites of amorphous Ni(OH)_(2),rather than conventional O sites,resulting in negatively charged Pt^(δ-).In situ Raman spectroscopy revealed that the changed configuration and electronic states greatly enhanced absorbability for activated hydrogen atoms,which were the essential intermediate for alkaline hydrogen evolution reaction.The hydrogen spillover process was revealed from amorphous Ni(OH)_(2)that effectively cleave the H-O-H bond of H_(2)O and produce H atom to the Pt SA sites,leading to a low overpotential of 48 mV in alkaline electrolyte at-1000 mA cm^(-2)mg^(-1)_(Pt),evidently better than commercial Pt/C catalysts.This work provided new strategy for the control-lable modulation of the local structure of SA catalysts and the systematic regulation of the electronic states.

Microwave electrometry with Rydberg atoms in a vapor cell using microwave amplitude modulation

We have theoretically and experimentally studied the dispersive signal of the Rydberg atomic electromagneticallyinduced transparency(EIT)Autler–Townes(AT)splitting spectra obtained using amplitude modulation of the microwave(MW)electric field.In addition to the two zero-crossing points interval△f_(zeros),the dispersion signal has two positive maxima with an interval defined as the shoulder interval△f_(sho),which is theoretically expected to be used to measure a much weaker MW electric field.The relationship of the MW field strength E_(MW)and△f_(sho)is experimentally studied at the MW frequencies of 31.6 GHz and 9.2 GHz respectively.The results show that△f_(sho)can be used to characterize the much weaker E_(MW)than that of△f_(zeros)and the traditional EIT–AT splitting interval△f_(m);the minimum E_(MW)measured by△f_(sho)is about 30 times smaller than that by△f_(m).As an example,the minimum E_(MW)at 9.2 GHz that can be characterized by△f_(sho)is 0.056 mV/cm,which is the minimum value characterized by the frequency interval using a vapor cell without adding any auxiliary fields.The proposed method can improve the weak limit and sensitivity of E_(MW)measured by the spectral frequency interval,which is important in the direct measurement of weak E_(MW).

Optical PAM-4/PAM-8 generation via dual-Raman process in Rydberg atoms

A scheme of optical four-level pulse amplitude modulation(PAM-4) is proposed based on dual-Raman process in Rydberg atoms. A probe field counter-propagates with a dual-Raman field which drives the ground and the excited states transition, respectively, and the Rydberg transition is driven by a microwave(MW) field. A gain peak appears in the probe transmission and is sensitive to the MW field strength. Optical PAM-4 can be achieved by encoding an MW signal and decoding the magnitude of a probe signal. Simulation results show that the differential nonlinearity and the integral nonlinearity of the proposed scheme can be reduced by 5 times and 6 times, respectively, compared with the counterparts of previous scheme, and the ratio of level separation mismatch is close to the ideal value 1. Moreover, the scheme is extended to optical PAM-8 signal, which may further improve the spectral efficiency.

Lattice strain induced by trace Pt single atoms in nickel for accelerating industrial hydrogen evolution

Strategically designing the electrocatalytic system and cleverly inducing strain is an effective approach to balance the cost and activity of Pt-based electrocatalysts for industrial-scale hydrogen production.Herein,we present a unipolar pulsed electrodeposition(UPED) strategy to induce strain in the Ni lattice by introducing trace amounts of Pt single atoms(SAs)(0.22 wt%).The overpotential decreased by 183 mV at 10 mA cm^(-2) in 1.0 M KOH after introducing trace amounts of Pt_(SAs).The industrial electrolyzer,assembled with Pt_(SAs)Ni cathode and a commercial NiFeO_(x) anode,requires a cell voltage of 1.90 V to attain 1 A cm^(-2) of current density and remains stable for 280 h,demonstrating significant potential for practical applications.Spherical aberration corrected scanning transmission electron microscopy(AC-STEM),X-ray absorption(XAS),and geometric phase analysis(GPA) indicate that the introduction of trace amounts of Pt SAs induces tensile strain in the Ni lattice,thereby altering the local electronic structure and coordination environment around cubic Ni for enhancing the water decomposition kinetics and fundamentally changing the reaction pathway.The doping-strain strategy showcases conformational relationships that could offer new ideas to construct efficient hydrogen evolution reaction(HER) electrocatalysts for industrial hydrogen production in the future.

Simulation of space heavy-ion induced primary knock-on atoms in bipolar devices

Bipolar junction transistors(BJTs) are often used in spacecraft due to their excellent working characteristics. However,the complex space radiation environment induces primary knock-on atoms(PKAs) in BJTs through collisions, resulting in hard-to-recover displacement damage and affecting the performance of electronic components. In this paper, the properties of PKAs induced by typical space heavy ions(C, N, O, Fe) in BJTs are investigated using Monte Carlo simulations. The simulated results show that the energy spectrum of ion-induced PKAs is primarily concentrated in the low-energy range(17eV–100eV) and displays similar features across all tested ions. The PKAs induced by the collision of energetic ions have large forward scattering angles, mainly around 88°. Moreover, the distribution of PKAs within a transistor as a function of depth displays a peak characteristic, and the peak position is linearly proportional to the incident energy at a certain energy range. These simulation outcomes serve as crucial theoretical support for long-term semiconductor material defect evolution and ground testing of semiconductor devices.

Multifunctional Film Assembled from N‑Doped Carbon Nanofiber with Co–N_(4)–O Single Atoms for Highly Efficient Electromagnetic Energy Attenuation

Single-atom materials have demonstrated attractive physicochemical characteristics.However,understanding the relationships between the coordination environment of single atoms and their properties at the atomic level remains a considerable challenge.Herein,a facile waterassisted carbonization approach is developed to fabricate well-defined asymmetrically coordinated Co–N_(4)–O sites on biomass-derived carbon nanofiber(Co–N_(4)–O/NCF)for electromagnetic wave(EMW)absorption.In such nanofiber,one atomically dispersed Co site is coordinated with four N atoms in the graphene basal plane and one oxygen atom in the axial direction.In-depth experimental and theoretical studies reveal that the axial Co–O coordination breaks the charge distribution symmetry in the planar porphyrin-like Co–N_(4) structure,leading to significantly enhanced dielectric polarization loss relevant to the planar Co–N_(4) sites.Importantly,the film based on Co–N_(4)–O/NCF exhibits light weight,flexibility,excellent mechanical properties,great thermal insulating feature,and excellent EMW absorption with a reflection loss of−45.82 dB along with an effective absorption bandwidth of 4.8 GHz.The findings of this work offer insight into the relationships between the single-atom coordination environment and the dielectric performance,and the proposed strategy can be extended toward the engineering of asymmetrically coordinated single atoms for various applications.

Research of caged dynamics of clusters center atoms in Pd_(82)Si_(18) amorphous alloy

To date,there is still a lack of a comprehensive explanation for caged dynamics which is regarded as one of the intricate dynamic behaviors in amorphous alloys.This study focuses on Pd_(82)Si_(18)as the research object to further elucidate the underlying mechanism of caged dynamics from multiple perspectives,including the cage's lifetime,atomic local environment,and atomic potential energy.The results reveal that Si atoms exhibit a pronounced cage effect due to the hindrance of Pd atoms,resulting in an anomalous peak in the non-Gaussian parameters.An in-depth investigation was conducted on the caged dynamics differences between fast and slow Si atoms.In comparison to fast Si atoms,slow Si atoms were surrounded by more Pd atoms and occupied lower potential energy states,resulting in smaller diffusion displacements for the slow Si atoms.Concurrently,slow Si atoms tend to be in the centers of smaller clusters with coordination numbers of 9 and 10.During the isothermal relaxation process,clusters with coordination numbers 9 and 10 have longer lifetimes,suggesting that the escape of slow Si atoms from their cages is more challenging.The findings mentioned above hold significant implications for understanding the caged dynamics.

Bimetallic CoNi single atoms supported on three-dimensionally ordered mesoporous chromia:highly active catalysts for n-hexane combustion

Developing the alternative supported noble metal catalysts with low cost,high catalytic efficiency,and good resistance toward carbon dioxide and water vapor is critically demanded for the oxidative removal of volatile organic compounds(VOCs).In this work,we prepared the mesoporous chromia-supported bimetallic Co and Ni single-atom(Co_(1)Ni_(1)/meso-Cr_(2)O_(3))and bimetallic Co and Ni nanoparticle(Co_(NP)Ni_(NP)/mesoCr_(2)O_(3))catalysts adopting the one-pot polyvinyl pyrrolidone(PVP)-and polyvinyl alcohol(PVA)-protecting approaches,respectively.The results indicate that the Co_(1)Ni_(1)/meso-Cr_(2)O_(3)catalyst exhibited the best catalytic activity for n-hexane(C_(6)H_(14))combustion(T_(50%)and T_(90%)were 239 and 263℃ at a space velocity of 40,000 mL g^(-1)h^(-1);apparent activation energy and specific reaction rate at 260℃ were 54.7 kJ mol^(-1)and 4.3×10^(-7)mol g^(-1)_(cat)s^(-1),respectively),which was associated with its higher(Cr^(5+)+Cr^(6+))amount,large n-hexane adsorption capacity,and good lattice oxygen mobility that could enhance the deep oxidation of n-hexane,in which Ni_(1) was beneficial for the enhancements in surface lattice oxygen mobility and low-temperature reducibility,while Co_(1) preferred to generate higher contents of the high-valence states of chromium and surface oxygen species as well as adsorption and activation of n-hexane.n-Hexane combustion takes place via the Mars van Krevelen(MvK)mechanism,and its reaction pathways are as follows:n-hexane→olefins or 3-hexyl hydroperoxide→3-hexanone,2-hexanone or 2,5-dimethyltetrahydrofuran→2-methyloxirane or 2-ethyl-oxetane→acrylic acid→CO_x→CO_(2)and H_(2)O.

One-dimensional phenanthroline-based covalent organic framework bearing single cobalt atoms for efficient photocatalytic CO_(2) reduction

Metalated covalent organic frameworks(COFs)for 2D and 3D topologies are continuously being developed,whereas metalated COFs with 1D topologies are still in their infancy.Here,a novel 1D phenanthroline-based COF containing 4,4-(1,10-phenanthroline-2,9-diyl)bis[benzaldehyde](PBA)is reported(PAD-COF).Subsequently,a metalated 1D COF,Co SAS/PAD-COF,is constructed using the bidentate ligand properties of PBA and anchoring the single Co atoms in PAD-COF through a post-synthetic modification strategy.This complex significantly improved the photocatalytic performance of PAD-COF,and the CO yield of the optimized Co SAS/PAD-COF was stable at 3091µmol g^(-1) h^(-1) with a selectivity of 93%,which is approximately 43.7 times that of the original PAD-COF.Experimental and theoretical results demonstrate the excellent CO_(2) photoreduction activity of Co SAS/PAD-COF owing to the synergistic effect of single Co catalytic sites and PAD-COF.Among them,PAD-COF,as the host,adsorbs CO_(2) molecules and loads single Co atoms.Meanwhile,Co atoms function as catalytic sites and promote the adsorp-tion and activation of CO_(2),while reducing the reaction energy barrier formed by the*COOH intermediates.Therefore,this unique metalated 1D COF provides a fresh approach to photocatalytic CO_(2) reduction.

All-electron basis sets for H to Xe specific for ZORA calculations:Applications in atoms and molecules

A segmented basis set of quadruple zeta valence quality plus polarization functions(QZP)for H through Xe was developed to be used in conjunction with the ZORA Hamiltonian.This set was augmented with diffuse functions to describe electrons farther away from the nuclei adequately.Using the ZORA-CCSD(T)/QZP-ZORA theoretical model,atomic ionization energies and bond lengths,harmonic vibrational frequencies,and atomization energies of some molecules were calculated.The addition of core-valence corrections has been shown to improve the agreement between theoretical and experimental results for molecular properties.For atomization energies,a similar observation emerges when considering spin-orbit couplings.With the augmented QZP-ZORA set,static mean dipole polarizabilities of a set of atoms were calculated and compared with previously published recommended and experimental values.Performance evaluations of the ZORA and Douglas–Kroll–Hess Hamiltonians were made for each property studied.

Effects of surface chlorine atoms on charge distribution and reaction barriers for photocatalytic CO_(2)reduction

Photocatalytic CO_(2)reduction to produce high value-added carbon-based fuel has been proposed as a promising approach to mitigate global warming issues.However,the conversion efficiency and product selectivity are still low due to the sluggish dynamics of transfer processes involved in proton-assisted multi-electron reactions.Lowering the formation energy barriers of intermediate products is an effective method to enhance the selectivity and productivity of final products.In this study,we aim to regulate the surface electronic structure of Bi_(2)WO_(6)by doping surface chlorine atoms to achieve effective photocatalytic CO_(2)reduction.Surface Cl atoms can enhance the absorption ability of light,affect its energy band structure and promote charge separation.Combined with DFT calculations,it is revealed that surface Cl atoms can not only change the surface charge distribution which affects the competitive adsorption of H_(2)O and CO_(2),but also lower the formation energy barrier of intermediate products to generate more intermediate*COOH,thus facilitating CO production.Overall,this study demonstrates a promising surface halogenation strategy to enhance the photocatalytic CO_(2)reduction activity of a layered structure Bi-based catalyst.

Stability and diffusion properties of self-interstitial atoms in tungsten:a first-principles investigation

Employing a first-principles method based on the density function theory, we systematically investigate the structures, stability and diffusion of self-interstitial atoms （SIAs） in tungsten （W）. The （111 〉 dumbbell is shown to be the most stable SIA defect configuration with the formation energy of -9.43 eV. The on-site rotation modes can be described by a quite soft floating mechanism and a down-hill ＂drift＂ diffusion process from （110） dumbbell to 〈111〉 dumbbell and from （001） dumbbell to 〈110〉 dumbbell, respectively. Among different SIA configurations jumping to near neighboring site, the 〈111 〉 dumbbell is more preferable to migrate directly to first-nearest-neighboring site with a much lower energy barrier of 0.004 eV. These resuits provide a useful reference for W as a candidate plasma facing material in fusion Tokamak.

Anisotropic interaction between self-interstitial atoms and 1/2<111> dislocation loops in tungsten

We investigate the interaction between <111> self-interstitial atoms(SIAs) and 1/2<111> self-interstitial dislocation loops in tungsten(W) via atomistic simulations. We explore the variation of the anisotropic distribution of binding energies with the shapes and sizes of the 1/2[111] loop and the nonequivalent configurations of <111> SIAs. For an arbitrarily shaped loop, SIA can be more easily trapped in the concave region of the loop than the convex region, which forms a loop whose curvature is closer to that of a circular loop. The direction of SIAs can largely affect the interaction behaviors with the loop. The capture distance of an SIA by the edge of a circular-shaped 1/2[111] loop is clearly elongated along the direction of the SIA;however, it weakly depends on the size of the loop. Then, we analyze the slanted ring-like capture volume of <111> SIAs formed by the circular loop based on their generated anisotropic stress fields. Furthermore, the binding energies obtained from the elastic theory and atomistic simulations are compared. The results provide a reasonable interpretation of the growth mechanism of the loop and the anisotropic interaction that induces irregular-shaped capture volume, affording an insight into the numerical and Object Kinetic Monte Carlo simulations to evaluate the long-term and large-scale microstructural evolution and mechanical properties of W.

Size effect of He clusters on the interactions with self-interstitial tungsten atoms at different temperatures

The behaviors of helium clusters and self-interstitial tungsten atoms at different temperatures are investigated with the molecular dynamics method. The self-interstitial tungsten atoms prefer to form crowdions which can tightly bind the helium cluster at low temperature. The crowdion can change its position around the helium cluster by rotating and slipping at medium temperatures, which leads to formation of combined crowdions or dislocation loop locating at one side of a helium cluster. The combined crowdions or dislocation loop even separates from the helium cluster at high temperature. It is found that a big helium cluster is more stable and its interaction with crowdions or dislocation loop is stronger.