Cationic ordering transition in oxygen-redox layered oxide cathodes

Understanding the structural origin of the competition between oxygen 2p and transition-metal 3d orbitals in oxygen-redox(OR)layered oxides is eminently desirable for exploring reversible and high-energy-density Li/Na-ion cathodes.Here,we reveal the correlation between cationic ordering transition and OR degradation in ribbon-ordered P3-Na_(0.6)Li_(0.2)Mn_(0.8)O_(2) via in situ structural analysis.Comparing two different voltage windows,the OR capacity can be improved approximately twofold when suppressing the in-plane cationic ordering transition.We find that the intralayer cationic migration is promoted by electrochemical reduction from Mn^(4+)to Jahn–Teller Mn^(3+)and the concomitant NaO_(6) stacking transformation from triangular prisms to octahedra,resulting in the loss of ribbon ordering and electrochemical decay.First-principles calculations reveal that Mn^(4+)/Mn^(3+)charge ordering and alignment of the degenerate eg orbital induce lattice-level collective Jahn–Teller distortion,which favors intralayer Mn-ion migration and thereby accelerates OR degradation.These findings unravel the relationship between in-plane cationic ordering and OR reversibility and highlight the importance of superstructure protection for the rational design of reversible OR-active layered oxide cathodes.

Characterization of local chemical ordering and deformation behavior in high entropy alloys by transmission electron microscopy

Short-range ordering(SRO)is one of the most important structural features of high entropy alloys(HEAs).However,the chemical and structural analyses of SROs are very difficult due to their small size,complexed compositions,and varied locations.Transmission electron microscopy(TEM)as well as its aberration correction techniques are powerful for characterizing SROs in these compositionally complex alloys.In this short communication,we summarized recent progresses regarding characterization of SROs using TEM in the field of HEAs.By using advanced TEM techniques,not only the existence of SROs was confirmed,but also the effect of SROs on the deformation mechanism was clarified.Moreover,the perspective related to application of TEM techniques in HEAs are also discussed.

The chemical environment and structural ordering in liquid Mg-Y-Zn system:An ab-initio molecular dynamics investigation of melt for the formation mechanism of LPSO structure

In an effort to clarify the formation mechanism of LPSO structure in Mg-Y-Zn alloy,the chemical environment and structural ordering in liquid Mg-rich Mg-Y-Zn system are investigated with the aid of ab-initio molecular dynamics simulation.In liquid Mg-rich Mg-Y alloys,the strong Mg-Y interaction is determined,which promotes the formation of fivefold symmetric local structure.For Mg-Zn alloys,the weak Mg-Zn interaction results in the fivefold symmetry weakening in the liquid structure.Due to the coexistence of Y and Zn,the strong attractive interaction is introduced in liquid Mg-Y-Zn ternary alloy,and contributes to the clustering of Mg,Y,Zn launched from Zn.What is more,the distribution of local structures becomes closer to that in pure Mg compared with that in binary Mg-Y and Mg-Zn alloys.These results should relate to the origins of the Y/Zn segregation zone and close-packed stacking mode in LPSO structure,which provides a new insight into the formation mechanism of LPSO structure at atomic level.

Effect of Cd on matrix structure ordering and aging precipitation evolution in a Mg-Gd-Cd solid-solution alloy

The formation and evolution of Gd-rich precipitates companying with the matrix structure ordering in a Mg_(97)Gd_(2)Cd_(1)(at.%)solid-solution alloy aged at 200℃have been systemically investigated using high-angle annular dark-field scanning transmission electron microscopy(HAADF-STEM).The results show that Gd-rich precipitation dynamics during the aging treatment are noticeably affected by a continuous ordering transformation in the matrix.The ordering transformation process involving mainly re-distribution of Cd atoms was revealed to occur in the following way:random super-saturated solid solution(S.S.S.S.)→B19-type ordered domains→D019-type ordered domains.Four Gd(Cd)-rich precipitates,G.P.Ⅰ zone,G.P.Ⅱ zone,β′andβ_(1)phases,have been observed to be formed in sequence to coexist with the various ordered domains.Based on the HAADF-STEM characterization on the aging microstructures at different aging stages,it can be concluded that the Cd-addition and related matrix structure ordering can play significant roles in modifying the early-stage G.P.zone structure,altering the morphology ofβ′precipitates and promoting the forming ability of theβ_(1)precipitate.

New light fields based on integration theory within the Weyl ordering product of operators

The development of quantum optics theory based on the method of integration within an ordered product of operators(IWOP)has greatly stimulated the study of quantum states in the light field,especially non-Gaussian states with various non-classical properties.In this paper,the two-mode squeezing operator is derived with integral theory within the Weyl ordering product of operators using a combinatorial field in which one mode is a chaotic field and the other mode is a vacuum field.The density operator of the new light field,its entanglement property and photon number distribution are analyzed.We also note that tracing a three-mode pure state can yield this new light field.These methods represent a theoretical approach to investigating new density operators of light fields.

Magnetic ordering induced magnetodielectric effect in Ho_(2)Cu_(2)O_(5) and Yb_(2)Cu_(2)O_(5)

Materials with strongly coupled magnetic and electronic degrees of freedom provide new possibilities for practical applications.In this paper,we have investigated the structure,magnetic property,and magnetodielectric(MD) effect in Ho_(2)Cu_(2)O_(5) and Yb_(2)Cu_(2)O_(5) poly crystalline samples,which possess a non-centrosymmetric polar structure with space group Pna2_(1).In Ho_(2)Cu_(2)O_(5),Ho^(3+) and Cu^(2+) sublattices order simultaneously,exhibiting a typical paramagnetic to antiferromagnetic transition at 13.1 K.While for Yb_(2)Cu_(2)O_(5),two magnetic transitions which originate from the orderings of Yb^(3+)(7.8 K) and Cu^(2+)(13.5 K) sublattices are observed.A magnetic field induced metamagnetic transition is obtained in these two cuprates below Neel temperature(T_(N)).By means of dielectric measurement,distinct MD effect is demonstrated by the dielectric anomaly at T_(N.)Meanwhile,the MD effect is found to be directly related to the metamagnetic transition.Due to the specific spin configuration and different spin evolution in the magnetic field,a positive MD effect is formed in Ho_(2)Cu_(2)O_(5),and a negative one is observed in Yb_(2)Cu_(2)O_(5).The spontaneous dielectric anomaly at T_(N) is regarded as arising from the shifts in optical phonon frequencies,and the magnetoelectric coupling is used to interpret the magnetic field induced MD effect.Moreover,an H-T phase diagram is constructed for Ho_(2)Cu_(2)O_(5) and Yb_(2)Cu_(2)O_(5) based on the results of isothermal magnetic and dielectric hysteresis loops.

Normal ordering and antinormal ordering of the operator （fQ＋gP）n and some of their applications

In this paper by virtue of the technique of integration within an ordered product （IWOP） of operators and the intermediate coordinate-momentum representation in quantum optics, we derive the normal ordering and antinormal ordering products of the operator （fQ＋gP）n when n is an arbitrary integer. These products are very useful in calculating their matrix elements and expectation values and obtaining some useful mathematical formulae. Finally, the applications of some new identities are given.

Tuning charge and orbital ordering in DyNiO_(3) by biaxial strain

The first-principles calculations were used to explore the tunable electronic structure in DyNiO_(3)(DNO)under the effects of the biaxial compressive and tensile strains.We explored how the biaxial strain tunes the orbital hybridization and influences the charge and orbital ordering states.We found that breathing mode and Jahn–Teller distortion play a primary role in charge ordering state and orbital ordering state,respectively.Additionally,the calculated results revealed that the biaxial strain has the ability to manipulate the phase competition between the two states.A phase transition point has been found under tensile train.If the biaxial train is larger than the point,the system favors orbital ordering state.If the strain is smaller than the point,the system is in charge ordering state favorably.

Destruction of charge ordering phase in La_(0.4)Ca_(0.6)MnO_3 induced by low Cr doping

Polycrystalline samples of La0.4Cao.6Mn1-xCrxO3 （x = 0.00, 0.02, 0.04, 0.06） were prepared by the solid state reaction method. The influence of Cr3＋ substitution for Mn3＋ on the magnetic property and charge ordering phase of La0.4Ca0.6MnO3 was studied through the measurements of X-ray diffraction （XRD）, magnetization-temperature （M-T） curves and electron spin resonance （ESR） spectra. The experimental results indicate that the mother＇s body of La0.4Ca0.6MnO3 has very complicated magnetic structure, exhibits charge ordering phase at 258 K, and shows long-range strongly correlated charge ordering-antiferromagnetism （CO-AFM） phase from 175 to 50 K. Spin glass state appears when the temperature decreases to about 41 K. When the Cr substitution amount is x = 0.06, the charge ordering phase of the mother＇s body is de-stroyed, because the Cr3＋ substitution for Mn3＋ destroys the spin order of CE-type antiferromagnetism, and thus leads to the melting of charge ordering. It is verified experimentally that the strong coupling between charge order and spin order exists in the charge order system of CE-type antiferromagnetism.

Structure learning on Bayesian networks by finding the optimal ordering with and without priors

Ordering based search methods have advantages over graph based search methods for structure learning of Bayesian networks in terms on the efficiency. With the aim of further increasing the accuracy of ordering based search methods, we first propose to increase the search space, which can facilitate escaping from the local optima. We present our search operators with majorizations, which are easy to implement. Experiments show that the proposed algorithm can obtain significantly more accurate results. With regard to the problem of the decrease on efficiency due to the increase of the search space, we then propose to add path priors as constraints into the swap process. We analyze the coefficient which may influence the performance of the proposed algorithm, the experiments show that the constraints can enhance the efficiency greatly, while has little effect on the accuracy. The final experiments show that, compared to other competitive methods, the proposed algorithm can find better solutions while holding high efficiency at the same time on both synthetic and real data sets.

Regression model for stabilization energies associated with anion ordering in perovskite-type oxynitrides

Certain perovskite-type oxynitrides have bandgaps suitable for renewable hydrogen production via photocatalytic and photoelectrochemical water splitting under visible light.Understanding the ordering of oxide and nitride anions in these materials is important because this ordering affects their semiconductor properties.However, the numerous possible orderings complicate systematic analyses based on density functional theory(DFT) calculations using defined elemental arrangements.This work shows that anion ordering in large-scale supercells within perovskite-type oxynitrides can be rapidly predicted based on machine learning, using BaNbO2N(capable of oxidizing water under irradiation up to 740 nm) as an example.Machine learning allows the calculation of the total energy of BaNbO2N directly from randomly selected initial atomic placements without costly structural optimization, thus reducing the computational cost by more than 99.99%.Combined with the Metropolis Monte Carlo method, machine learning permits exploration of the stable anion orderings of large supercells without costly DFT calculations.This work therefore demonstrates a means of predicting the properties of functional materials having complex compositions based on the most realistic elemental arrangements in conjunction with reasonable computational loads.

Research on charge ordering and magnetic properties in La_(0.3)Ca_(0.7)Mn_(1-x)W_xO_3 system

The perovskite manganite sample La0.3Ca0.7Mn1-xWxO3 （x = 0.08, 0.12） was prepared by the solid-state reaction method. The effect of W doping on the Mn site to La0.3Ca0.7MnO3 charge ordering phase and the changing process of magnetic properties were studied through the measurement of the M-T curve, M-H curves, and ESR curves of the sample. The results showed that when x = 0.08, the charge ordering （CO） phase exists in the system, the transition temperature Tco= 275 K, and the system exhibits PM when T 〉 275 K. The system transforms from spin-disordering paramagnetism to spin-ordering antiferromagnetism in the charge ordering state with the temperature decreasing from 275 K to 230 K. The long-range antiferromagnetism forms and AFM/CO states coexist between 230 K and 5 K. There is a little ferromagnetic component in the AFM/CO background in a low temperature range. When x = 0.12, the CO phase in the system has almost melted completely. There is a little remnant of the CO phase below 150 K. The system exhibits paramagnetism when T 〉 150 K and transforms from paramagnetism to ferromagnetism when T〈 150 K.

Influence of the Jahn-Teller distortion on magnetic ordering in TbMn_(1-x)Fe_xO_3

The Jahn-Teller distortion plays an important role in determining the exchange interaction in rare-earth manganites.In this work we study the influence of the Jahn-Teller distortion on the magnetic structures of TbMn1-xFexO3（x = 0,0.02,0.05,0.10,and 0.20） single crystals in the basal MnO2 plane.The decrease in the quadruple splitting with the increasing Fe doping indicates the reduction of the Jahn-Teller distortion,which makes the nearest neighboring（NN） FM interaction dominant over the next nearest neighbor（NNN） AFM interaction.This alteration is favorable for the development of A-type AFM ordering instead of the spiral magnetic ordering,which collapses when x ≥ 0.05.The analysis of dielectric data indicates that the ferroelectricity is arising from the peculiar spiral magnetic ordering.

INFLUENCE OF GRAIN SIZE AND ORDERING OF PARENT PHASE ON M_s IN A CuZnAl ALLOY CONTAINING BORON

The effect of grain size and ordering of the parent phase on the critical points of thermoelastic martensitic transformation in Cu-25.62 Zn-3.97 Al-0.0018 B(wt-%)shape memory alloy has been investigated.Based on the thermodynamics of phase transformation,a linear rela- tionship between the starting temperature of martensitic transformation and the reciprocal of the square root of grain size is obtained,i.e.M_s temperature rises with increasing grain size. It shows a good agreement with the results of electric resistance measurement.Applying the Landau's theory,a quantitative relationship between M_s and the ordering parameter of the parent phase is set up,which is well confirmed by the results of X-ray diffraction and electric resistance measurement.The activation energy of the ordering process in the parent phase of the alloy is calculated to be 46 kJ/mol.

ORDERING CONTRACTION MAPPING PRINCIPLE AND APPLICATIONS

This paper establishes an ordering contraction mapping principle for increasing mapping in partial ordering metric spaces, and applies it to prove the existence and uniqueness of fixed point for some nonlinear operators controlled by a linear operator and phi-concave operator in a partial ordering Banach space. Therefore, this two results are unified.

On the ordering of the Kirchhoff indices of the complements of trees and unicyclic graphs

The Kirchhoff index Kf(G) of a graph G is defined to be the sum of the resistance distances between all pairs of vertices of G. In this paper, we develop a novel method for ordering the Kirchhoff indices of the complements of trees and unicyclic graphs. With this method, we determine the first five maximum values of Kf■ and the first four maximum values of Kf(ū),where ■ and ū are the complements of a tree T and unicyclic graph U, respectively.

EFFECT OF Si CONTENT ON ORDERING DEGREE AND ELECTROMAGNETIC CHARACTERISTICS IN FeSiAl ALLOYS

FeSiAl alloys ribbons synthesized by melt-quench were annealed in vacuum at 873 K for 60 rain. The flaky powders were prepared by milling the annealed ribbons for 70 h. After milling, the powders were heat treated at 573 K for 90 rain. The ordering degree of the powders lattice structure was analyzed by X-ray diffraction （XRD）. The measurement of specific saturation magnetization was carried out by vibrating samples magnetometer （VSM）. Complex permittivity and complex permeability in the frequency band of 0.5-18 GHz were measured with the vector network analyzer. The ordering degree of the superlattice structure increased from 0.2＇7 to 0.49. Complex permittivity and complex permeability decreased with increasing Si content. After ordering, the specific saturation magnetization decreased from 134.2 to 85.0 A.m2.kg-1. For use in anti-EMI material, the total contents of Si and Al in FeSiAl alloys should be controlled at a low level.

Joint optimization of inspection, maintenance, and spare ordering policy considering defective products loss

This paper proposes a joint inspection-based maintenance and spare ordering optimization policy that considers the problem of integrated inspection,preventive maintenance,spare ordering,and quality control for a four-state single-unit manufacturing system.When an inspection detects a minor defect,a second phase inspection is initiated and a regular order is placed.Product quality begins to deteriorate when the system undergoes a severe defect.To counter this,an advanced replacement of the minor defective system is carried out at the Jth second phase inspection.If a severe defect is recognized prior to the Jth inspection,or if system failure occurs,preventive or corrective replacement is executed.The timeliness of replacement depends on the availability of spare.We adopt two modes of ordering:a regular order and an emergency order.Meanwhile,a threshold level is introduced to determine whether an emergency order is preferred even when the regular order is already ordered but has not yet arrived.The optimal joint inspection-based maintenance and spare ordering policy is formulated by minimizing the expected cost per unit time.A simulation algorithm is proposed to obtain the optimal two-phase inspection interval,threshold level and advanced replacement interval.Results from several numerical examples demonstrate that,in terms of the expected cost per unit time,our proposed model is superior to some existing models.

ATOMIC ORDERING AND DISORDERING OF INTERMETALLIC PHASES

All intermetallic phases have a tendency to atomic long-range ordering, according to the ordering energy, they may be permanently ordered (up to the melting-point) or reversibly ordered (up to a critical temperature). The paper considers ways of disordering intermetallic phases, in relation to the ordering energy and diffusivities, and some properties of partially ordered intermetallic phases (including mechanical properties) The kinetics of re-ordering of disordered starting material will be examined,including sluggishly ordering phases (which can be aided by concurrent irradiation). The circumstances under which a partially disordered intermetallic phase may transform into an amorphous form will be outlined.

Joint optimization of inspection-based and age-based preventive maintenance and spare ordering policies for single-unit systems

This paper presents a joint optimization policy of preventive maintenance(PM)and spare ordering for single-unit systems,which deteriorate subject to the delay-time concept with three deterioration stages.PM activities that combine a non-periodic inspection scheme with age-replacement are implemented.When the system is detected to be in the minor defective stage by an inspection for the first time,place an order and shorten the inspection interval.If the system has deteriorated to a severe defective stage,it is either repaired imperfectly or replaced by a new spare.However,an immediate replacement is required once the system fails,the maximal number of imperfect maintenance(IPM)is satisfied or its age reaches to a pre-specified threshold.In consideration of the spare’s availability as needed,there are three types of decisions,i.e.,an immediate or a delayed replacement by a regular ordered spare,an immediate replacement by an expedited ordered spare with a relative higher cost.Then,some mutually independent and exclusive renewal events at the end of a renewal cycle are discussed,and the optimization model of such a joint policy is further developed by minimizing the long-run expected cost rate to find the optimal inspection and age-replacement intervals,and the maximum number of IPM.A Monte-Carlo based integration method is also designed to solve the proposed model.Finally,a numerical example is given to illustrate the proposed joint optimization policy and the performance of the Monte-Carlo based integration method.