Low to high spin-state transition induced by charge ordering in antiferromagnetic YBaCo2O5

The oxygen-deficient double perovskite YBaCo2O5, containing corner-linked CoO5 square pyramids as principal building units, undergoes a paramagnetic to antiferromagnetic spin ordering at 330 K. This is accompanied by a tetragonal to orthorhombic distortion. Below 220 K orbital ordering and long-range Co(2+)/Co(3+) charge ordering occur as well as a change in the Co2+ spin state from low to high spin. This transition is shown to be very sensitive to the oxygen content of the sample. To our knowledge this is the first observation of a spin-state transition induced by long-range orbital and charge ordering.     

Electric polarization, magnetoelectric effect, and orbital state of a layered iron oxide with frustrated geometry

A layered iron oxide RFe2O4 (R denotes rare-earth-metal elements) is an exotic dielectric material with charge-order (CO) driven electric polarization and magnetoelectric effect caused by spin-charge coupling. In this paper, a theory of electronic structure and dielectric property in RFe2O4 is presented. Charge frustration in paired-triangular lattices allows a charge imbalance without inversion symmetry. Spin frustration induces reinforcement of this polar CO by a magnetic ordering. We also analyze an orbital model for the Fe ion which does not show a conventional long-range order.     

Quantum J1-J2 antiferromagnet on a stacked square lattice: influence of the interlayer coupling on the ground-state magnetic ordering

Using the coupled-cluster method and the rotation-invariant Green's function method, we study the influence of the interlayer coupling Jperpendicular on the magnetic ordering in the ground state of the spin-1/2 J1-J2 frustrated Heisenberg antiferromagnet (J1-J2 model) on the stacked square lattice. In agreement with known results for the J1-J2 model on the strictly two-dimensional square lattice (Jperpendicular=0), we find that the phases with magnetic long-range order at small J2Jc2 are separated by a magnetically disordered (quantum paramagnetic) ground-state phase. Increasing the interlayer coupling Jperpendicular >0, the parameter region of this phase decreases, and, finally, the quantum paramagnetic phase disappears for quite small Jperpendicular approximately (0.2-0.3)J1.     

Orbital order and possible superconductivity in LaNiO3/LaMO3 superlattices

A hypothetical layered oxide La2NiMO6 where NiO2 and MO2 planes alternate along the c axis of ABO3 perovskite lattice is considered theoretically. Here, M denotes a trivalent cation Al, Ga,... such that MO2 planes are insulating and suppress the c-axis charge transfer. We predict that correlated eg electrons in the NiO2 planes develop a planar x2-y2 orbital order driven by the reduced dimensionality and further supported by epitaxial strain from the substrate. Low-energy electronic states can be mapped to a single-band t - t' - J model, suggesting favorable conditions for high-Tc superconductivity.     

Effect of Y-doping on the magnetic and charge orderings in Nd2/3Ca1/3MnO3

The shifts of the magnetic and charge ordering transition temperatures caused by Nd substitution for Y in Nd_2/3Ca_1/3MnO₃ CMR narrow-band perovskite manganite have been studied. At low temperatures, three different long-range magnetic orderings consistent with a phase separation scenario have been observed in the doped compound (Nd_0.9Y_0.1)_2/3Ca_1/3MnO₃ by neutron-diffraction study: the antiferromagnetic orderings of PCE and DE types existing below ∼110 and ∼60 K, respectively, and the ferromagnetic one of B type existing below ∼42. Magnetic phase transformations temperatures as well as those of charge ordering have been found to be structural-dependent. Y-doping leads to the decrease of the anisotropy of the orthorhombic Pnma crystal lattice b/√2c, which causes a decrease of the indirect exchange parameters in the system and thus a decrease in the magnetic transformation temperatures for 20-30 K in the doped compound. Doping leads as well to the higher level of the coherent Jahn-Teller distortions of the MnO₆ octahedra in the 200-300 K temperature region, which results in the increase of the charge ordering temperature for ∼80 K.     

Thickness dependence of antiferromagnetic phase transition in Heisenberg-type MnPS3

The behavior of 2-dimensional (2D) van der Waals (vdW) layered magnetic materials in the 2D limit of the few-layer thickness is an important fundamental issue for the understanding of the magnetic ordering in lower dimensions. The antiferromagnetic transition temperature T_N of the Heisenberg-type 2D magnetic vdW material MnPS₃ was estimated as a function of the number of layers. The antiferromagnetic transition was identified by temperature-dependent Raman spectroscopy, from the broadening of a phonon peak at 155 cm⁻¹, accompanied by an abrupt redshift and an increase of its spectral weight. T_N is found to decrease only slightly from ~78 K for bulk to ~66 K for 3L. The small reduction of T_N in thin MnPS₃ approaching the 2D limit implies that the interlayer vdW interaction is playing an important role in stabilizing magnetic ordering in layered magnetic materials.     

High-throughput computational material screening of the cycloalkane-based two-dimensional Dion—Jacobson halide perovskites for optoelectronics

Two-dimensional (2D) layered perovskites have emerged as potential alternates to traditional three-dimensional (3D) analogs to solve the stability issue of perovskite solar cells. In recent years, many efforts have been spent on manipulating the interlayer organic spacing cation to improve the photovoltaic properties of Dion—Jacobson (DJ) perovskites. In this work, a serious of cycloalkane (CA) molecules were selected as the organic spacing cation in 2D DJ perovskites, which can widely manipulate the optoelectronic properties of the DJ perovskites. The underlying relationship between the CA interlayer molecules and the crystal structures, thermodynamic stabilities, and electronic properties of 58 DJ perovskites has been investigated by using automatic high-throughput workflow cooperated with density-functional (DFT) calculations. We found that these CA-based DJ perovskites are all thermodynamic stable. The sizes of the cycloalkane molecules can influence the degree of inorganic framework distortion and further tune the bandgaps with a wide range of 0.9—2.1 eV. These findings indicate the cycloalkane molecules are suitable as spacing cation in 2D DJ perovskites and provide a useful guidance in designing novel 2D DJ perovskites for optoelectronic applications.     

Instability of the quantum-critical point of itinerant ferromagnets

We study the stability of the quantum-critical point for itinerant ferromagnets commonly described by the Hertz-Millis-Moriya (HMM) theory. We argue that in D相似文献   

Wigner crystallization in (DI-DCNQI)2Ag detected by synchrotron radiation X-Ray diffraction

The low-temperature electronic structure of the quarter-filled, quasi-one-dimensional (Q1D) system (DI-DCNQI)2Ag is revealed using synchrotron radiation x-ray diffraction. In spite of the interchain frustration in the twofold superstructure along the 1D chain, the body-centered tetragonal "charge ordering" structure, which consists of 4k_{F} charge ordering columns and 4k_{F} bond order wave columns, is realized. This is the first example of the Q1D system having plural kinds of columns as its ground state. This charge ordered structure is regarded as a Wigner crystal caused by intercolumn Coulomb repulsion.     

Disorder induced transitions in layered coulomb gases and superconductors

A 3D layered system of charges with logarithmic interaction parallel to the layers and random dipoles is studied via a novel variational method and an energy rationale which reproduces the known phase diagram for a single layer. Increasing interlayer coupling leads to successive transitions in which charge rods correlated in N>1 neighboring layers are nucleated by weaker disorder. For layered superconductors in the limit of only magnetic interlayer coupling, the method predicts and locates a disorder induced defect-unbinding transition in the flux lattice. While N = 1 charges dominate there, N>1 disorder induced defect rods are predicted for multilayer superconductors.     

Structure and Properties of Self-Organized 2D and 3D Antimony/Carbon Composites

The conditions of synthesis of antimony/carbon composites by interlayer self-assembly from colloidal solutions and melts are discussed. The morphology and the structure of these composites are examined. The potential to produce composites of 2D and 3D morphologies is demonstrated. The 2D composite has a multilayer graphene structure with submicron antimony inclusions, while the 3D composite has a spheroidal shell structure with a deformed film-shell with carbon nanoinclusions. The difference in properties of these composites is demonstrated: the 2D composite is conductive, while the 3D composite has a nonlinear current–voltage characteristic that indicates the emergence of novel functional properties of the spheroidal antimony/carbon composite. A model of exfoliation of the layered precursor with covalent interlayer coupling is proposed. This model provides an explanation for the experimentally observed nonlinear hydrodynamic processes in the colloidal antimony solution.     

Molecular Ordering of a Nematogen at Phase Transition Temperature - A Theoretical Study

Molecular ordering in 4-cyano-4'- n -propylbiphenyl ( CB3 ), a nematic liquid crystal, has been studied with the help of intermolecular interaction energy calculations. The CNDO / 2 method has been employed to compute the net atomic charge and atomic dipole moment at each atomic centre. Modified Rayleigh-Schrodinger perturbation theory along with multicentered-multipole expansion method has been employed to evaluate long-range intermolecular interactions, while a ' 6-exp ' potential function has been assumed for short-range interactions. The interaction energy values obtained through these computations were used to calculate the probability of each configuration at the phase transition temperature using Maxwell-Boltzmann formula. All possible geometrical arrangements between molecular pair have been considered during stacking, in-plane and terminal interactions. An attempt has been made to identify the most probable configuration at the phase transition temperature during stacking, in-plane and terminal interactions. Results obtained have been discussed in the light of experimental as well as other theoretical observations.     

AB合金有序化过程的动力学(Ⅰ)

由原子在点阵中扩散的反应率过程理论,在最近邻近似下,计算了AB合金的长程有序化动力学及长程序为零时的短程有序化动力学。所得结果与前人的实验结论及计算结果相比定性地符合,定量地接近。长程有序化动力学的计算表明,有序化过程存在有孕育期,有c-曲线形式的转变曲线,s近似与exp{-αt²}正比,算得的平衡有序度与前人计算结果相近。长程序为零时的短程有序化动力学的计算表明,σ近似与exp{-βt}正比,此时有序化速率甚快,以致在最快的淬火速率下,样品中也必然存在有一定的短程序,所得的平衡短程序值也符合前人的计算结果。本文是作为继续计算短程有序化动力学的准备及基础。     

Application of the cluster variation method to an interstitial solid solution: Calculation of the γ ′-Fe 4 N 1-x -ε-Fe 2 N 1-z equilibrium

The cluster variation method has been applied to establish effective interaction potentials that describe both n'-Fe 4 N 1 mx - k-Fe 2 N 1 mz miscibility gaps in the Fe-N phase diagram. The calculated nitrogen distributions show that long-range order occurs in the n:'-Fe 4 N 1 mx phase and that short-range ordering as well as long-range ordering occurs in the k-Fe 2 N 1 mz phase. The calculated nitrogen distributions for the k-Fe 2 N 1 mz , pertaining to temperatures and concentrations at the n'- k-phase boundaries, are compared with available data obtained by Mössbauer spectrometry. Preferential occupation of specific interstitial sites occurs from about 16 at.% N onwards; at the highest concentration considered, about 25 at.% N, the occupation is that of Fe 3 N as proposed in the literature on the basis of diffraction data.     

Independent freezing of charge and spin dynamics in La1.5Sr0.5CoO4

We present elastic and quasielastic neutron scattering measurements characterizing peculiar short-range charge-orbital and spin order in the layered perovskite material La1.5Sr0.5CoO4. We find that below T(c) approximately 750 K holes introduced by Sr doping lose mobility and enter a statically ordered charge glass phase with loosely correlated checkerboard arrangement of empty and occupied d(3z(2)-r(2)) orbitals ( Co3+ and Co2+). The dynamics of the resultant mixed spin system is governed by the anisotropic nature of the crystal-field Hamiltonian and the peculiar exchange pattern produced by the orbital order. It undergoes a spin freezing transition at a much lower temperature, T(s) less, similar30 K.     

Correlation-Driven Magnetic Frustration and Insulating Behavior of TiF3

The halide perovskite TiF₃, renowned for its intricate interplay between structure, electronic correlations, magnetism, and thermal expansion, is investigated. Despite its simple structure, understanding its low-temperature magnetic behavior has been a challenge. Previous theories propose antiferromagnetic ordering. In contrast, experimental signatures for an ordered magnetic state are absent down to 10 K. The current study has successfully reevaluated the theoretical modeling of TiF₃, unveiling the significance of strong electronic correlations as the key driver for its insulating behavior and magnetic frustration. In addition, frequency-dependent optical reflectivity measurements exhibit clear signs of an insulating state. The analysis of the calculated magnetic data gives an antiferromagnetic exchange coupling with a net Weiss temperature of order 25 K as well as a magnetic response consistent with a S = 1/2 local moment per Ti³⁺. Yet, the system shows no susceptibility peak at this temperature scale and appears free of long-range antiferromagnetic order down to 1 K. Extending ab initio modeling of the material to larger unit cells shows a tendency for relaxing into a noncollinear magnetic ordering, with a shallow energy landscape between several magnetic ground states, promoting the status of this simple, nearly cubic perovskite structured material as a candidate spin liquid.     

SO(4) Symmetry and Off-Diagonal Long-Range Order in the Hubbard Bilayer

Yang's η pairing operator is generalized to explore off-diagonal long-range order in the Hubbard bilayer with an arbitrary chemical potential. With this operator and a constraint condition on annihilation and creation operators, we construct explicitly eigenstates which possess simultaneously three kinds of off-diagonal long-range order, i.e., the intralayer one and the interlayer one for on-site pairing, and that for interlayer nearest-neighbor pairing. As in the simple Hubbard model there is also an SO(4) symmetry, with the generators properly defined. A sufficient condition leads to at least one of the above three kinds of off-diagonal long-range order. A constraint relation among different kinds of off-diagonal long-range order is also given. There exists a triplet of collective modes if the U(1) symmetry of a subgroup is spontaneously broken.     

Phase transitions and magnetic-transport phenomena in the system La2/3Ba1/3(Mn1−x Cox)O3

A study is performed of the crystalline structure, magnetization, and magnetotransport properties of the system La_2/3Ba_1/3(Mn_1−x Co_x)O₃ with perovskite structure. It is shown that cubic solid solutions exist over the entire range of cobalt concentrations 0⩽x⩽1. Compositions with x⩽0.2 are ferromagnets with maximum resistance near T _C . Compositions with 0.2<x<0.4 manifest properties of inhomogeneous ferromagnets. Measurements of magnetic properties indicate the absence of long-range magnetic order in compositions with 0.5⩽x⩽0.9, which are probably spin glasses. The spontaneous magnetization of cobaltate (2μ _B per formula unit) corresponds to ferromagnetic ordering of the moments of the Co³⁺ and Co⁴⁺ ions found in the intermediate spin state. It is conjectured that the magnetoresistance consists of an extrinsic and an intrinsic contribution. The first arises as a result of intergrain transport of spin-polarized charge carriers, and the second, as a result of magnetic ordering near T _C . The magnetoresistance is essentially independent of the spontaneous magnetization and decreases abruptly as the cobalt concentration is increased with a corresponding transition from long-range to short-range magnetic order. Zh. éksp. Teor. Fiz. 116, 604–610 (August 1999)     

Enhanced charge gap in the bilayer manganite La2-2xSr1+2xMn2O7 near x = 0.4

We have investigated the optical conductivity spectra of La2-2xSr1+2xMn2O7 (0.3相似文献   

Landau theory of charge and spin ordering in the nickelates

Guided by experiment and band structure, we introduce and study a phenomenological Landau theory for the unusual charge and spin ordering associated with the Mott transition in the perovskite nickelates, with chemical formula RNiO3, where R=Pr, Nd,Sm, Eu, Ho, Y, and Lu. While the Landau theory has general applicability, we show that for the most conducting materials, R=Pr, Nd, both types of order can be understood in terms of a nearly nested spin-density wave. Furthermore, we argue that in this regime, the charge ordering is reliant upon the orthorhombic symmetry of the sample, and therefore proportional to the magnitude of the orthorhombic distortion. The first order nature of the phase transitions is also explained. We briefly show by example how the theory is readily adapted to modified geometries such as nickelate films.