First-principles study of orbital ordering in cubic fluoride KCrF_3

Comprehensive first-principles calculations are performed to provide insight into the intriguing physical properties of the ternary cubic fluoride KCrF3. The electronic structures exhibit a prominent dependence on the effective local Coulomb interaction parameter Ueff. The ground state of the cubic phase is a ferromagnetic （FM） half-metal with Ueff equal to 0, 2, and 4 eV, whereas the insulating A-type antiferromagnetic （A-AFM） state with concomitant homogeneous orbital ordering is more robust than the FM state for Ueff exceeding 4 eV. We propose that the origin of the orbital ordering is purely electronic when the cooperative Jahn-Teller distortions are absent in cubic KCrF3.

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.

Orbital Ordering Induced by Direct Coulomb Repulsion

We consider the covalence characters of the 3d electron with the eg orbital freedoms and put forward a new mechanism of the orbital ordering （00） based on the direct coulomb repulsion in this article. The results show that the orbital-orbital interaction （OO-I） between the adjacent ions in 180-degree configuration is dominated by the superexchange energy accompanied by a weak orbital-spin coupling, and the OO-I in 90-degree configuration is monitored by the oxygen on-site coulomb repulsion. The ferro-OO is the stable ground state for the one-dimensional chain in the case of the 90-degree configuration.

Magnetic order driven by orbital ordering in the semiconducting KFe1.5Se2

The two-orbital Hubbard model is studied numerically by using the Hartree-Fock approximation in both real space and momentum space, and the ground-state properties of the alkali metal iron selenide semiconducting KFel.5Se2 are investigated. A rhombus-type Fe vacancy order with stripe- type antiferromagnetic （AFM） order is found, as was observed in neutron scattering experiments [J. Zhao, et al., Phys. Rev. Lett. 109, 267003 （2012）]. Hopping parameters are obtained by fitting the experimentally observed stripe AFM phase in real space. These hopping parameters are then used to study the ground-state properties of the semiconductor in momentum space. It is found to be a strongly correlated system with a large on-site Coulomb repulsion U, similar to the AFM Mort insulator -- the parent compound of copper oxide superconductors. We also find that the electronic occupation numbers and magnetizations in the dxz and dyz orbitals become different simultaneously when U 〉 Uc （～3.4 eV）, indicating orbital ordering. These results imply that the rotational symmetry between the two orbitals is broken by orbital ordering and thus drives the strong anisotropy of the magnetic coupling that has been observed by experiments and that the stripe-type AFM order in this compound may be caused by orbital ordering together with the observed large anisotropy.

Effects of anharmonic lattice distortion on orbital and magnetic orderings in KCuF_3

Lattice, magnetic and orbital structures in KCuF3 are self-consistently determined by our cluster self-consistent field approach based on a spin-orbital-lattice Hamiltonian. Two stable structures are obtained and found to be degenerate, which confirms the presence of the coexistent phases observed experimentally. We clearly show that due to the inherent frustration, the ground state of the system only with the superexchange interaction is degenerate; while the Jahn-Teller distortion, especially the anharmonic effect, stabilizes the orbital ordered phase at about 23% in the x2-y2 orbit and at 77% in the 3z2-r2 orbit. Meanwhile the magnetic moment of Cu is considerably reduced to 0.56μB, and magnetic coupling strengths are highly anisotropic, Jx/Jxy ≈ 18. These results are in good agreement with the experiments, implying that the anharmonic Jahn-Teller effect plays an essential role in stabilising the orbital ordered ground state of KCuF3.

Roles of Electron Hopping on Orbital Ordering for Vanadium Spinels

We investigate the orbitM ordering quantitatively for the spinel systems RV204 （R=Mg, Zn, Cd） in the viewpoint of single-ion physics through the method of diagonalization. Through the quantitative calculation, it is found that the spin-orbit （SO）coupling and the Jahn-Teller （JT） effect enable the orbital ordering under the conditions of negligible electron hopping among different V3＋ sites. For the systems RV204, the electron hopping is implied to be observable from the energy gap in conductivity, so the orbital ordering of RV2 04 cannot be induced by the SO coupling and JT effect at definite temperature, which is on contrary to the conclusions in [Phys. Rev. Lett. 93 （2004） 157206].

Orbital ordering and fluctuations in a kagome superconductor CsV_(3)Sb_(5)

Recently,competing electronic instabilities,including superconductivity and density-wave-like order,have been discovered in vanadium-based kagome metals AV_(3)Sb_(5)(A=K,Rb,Cs)with a nontrivial band topology.This finding stimulates considerable interest to study the interplay of these competing electronic orders and possible exotic excitations in the superconducting state.Here,we performed51V and133Cs nuclear magnetic resonance(NMR)measurements on a CsV_(3)Sb_(5)single crystal to clarify the nature of density-wave-like transition in these kagome superconductors.A first-order structural transition is unambiguously revealed below T_(s)~94 K by observing the sudden splitting of Knight shift in^(51)V NMR spectrum.Moreover,combined with^(133)Cs NMR spectrum,the present result confirms a three-dimensional structural modulation.By further analyzing the anisotropy of Knight shift and 1/T_(1)T at^(51)V nuclei,we proposed that the orbital order is the primary electronic order induced by the firstorder structural transition,which is supported by further analysis on electric field gradient at^(51)V nuclei.In addition,the evidence for possible orbital fluctuations is also revealed above T_(s).The present work sheds light on a rich orbital physics in kagome superconductors AV_(3)Sb_(5).

Different effects of Ce-doping on orbital and spin ordering in perovskite vanadate Sm_(1-χ)Ce_χ VO_3

The effects of Ce-doping on the phase transition of the orbital/spin ordering （OO/SO） are studied through the structural, magnetic, and electrical transport measurements of perovskite vanadate Sm1 x Ce x VO 3 . The measurements of structure show that the cell volume decreases as x≤ 0.05, and then increases as Ce-doping level increases further. The OO state exists but is suppressed progressively in the sample with x≤0.2 and disappears as x0.2. The temperature at which the C-type SO transition is present increases monotonically with Ce-doping level increasing. The temperature dependence of resistivity for each of the samples shows a semiconducting transport behavior and the transport can be well described by the thermal activation model. The activation energy first decreases as x ≤0.2, and then increases for further doping. The obtained results are discussed in terms of the mixed-valent state of the doped-Ce ions.

On the Ground State of Spin Systems with Orbital Degeneracy

In order to understand the properties of the spin system with orbital degeneracy, we first study the ground state of the SU(4) spin-orbital model on a square lattice. The mean-field results suggest that for a small Hund's interaction, the flavor liquid state is stable against the solid state, but with sufficient deviation from the SU(4) limit the long-range order may be attained in 2D system. Furthermore, we employ a variational approach to calculate the phase diagram of the ground state and the temperature-dependent susceptibility by taking into account the Hund's interaction and the anisotropy in orbital wavefunctions. Finally, the implications for the experimental observations on the material, , are discussed.

Effect of anionic ordering on the electronic and optical properties of BaTaO2N：TB-mBJ density functional calculation

This report presents a first-principles investigation of the structural, electronic, and optical properties of perovskite oxynitrides BaTaO2 N by means of density functional theory（DFT） calculations using the full-potential linearized augmented plane wave（FP-LAPW） method. Three possible structures（P4mm, I4/mmm, and Pmma） are considered according to the TaO4N2 octahedral configurations. The calculated structural parameters are found to be in good agreement with the previous theoretical and experimental results. Moreover, the electronic band structure dispersion, total, and partial densities of electron states are investigated to explain the origin of bandgaps and the contribution of each orbital＇s species in the valence and the conduction bands. The calculated minimum bandgaps of the P4 mm, I4/mmm, and Pmma structures are 1.83 e V, 1.59 e V, and 1.49 e V, respectively. Furthermore, the optical properties represented by the dielectric functions calculated for BaTaO2 N show that the I4/mmm phase absorbs the light at a large window in both the visible and UV regions,whereas the other two structures（P4mm and Pmma） are more active in the UV region. Our investigations provide important information for the potential application of this material.

Physics picture from neutron scattering study on Fe-based superconductors

Neutron scattering, with its ability to measure the crystal structure, the magnetic order, and the structural and magnetic excitations, plays an active role in investigating various families of Fe-based high-Tc superconductors. Three different types of antiferromagnetic orders have been discovered in the Fe plane, but two of them cannot be explained by the spin-density-wave （SDW） mechanism of nesting Fermi surfaces. Noticing the close relation between antiferromagnetic order and lattice distortion in orbital ordering from previous studies on manganites and other oxides, we have advocated orbital ordering as the underlying common mechanism for the structural and antiferromagnetic transitions in the 1111, 122, and 11 parent compounds. We observe the coexistence of antiferromagnetic order and superconductivity in the （Ba,K）Fe2As2 system, when its phase separation is generally accepted. Optimal Tc is proposed to be controlled by the local FeAs4 tetrahedron from our investigation on the 1111 materials. The Bloch phase coherence of the Fermi liquid is found crucial to the occurrence of bulk superconductivity in iron chalcogenides of both the 11 and the 245 families. Iron chalcogenides carry a larger staggered magnetic moment （〉 2 tB/Fe） than that in iron pnictides （〈 1 .B/Fe） in the antiferromagnetic order. Normal state magnetic excitations in the 11 superconductor are of the itinerant nature while in the 245 superconductor the spin-waves of localized moments. The observation of superconducting resonance peak provides a crucial piece of information in current deliberation of the pairing symmetry in Fe-based superconductors.

R-site cation randomness effect in the A-site ordered Y_(0.5)La_(0.5)BaMn_2O_6 compound

The R/Ba-ordered and R-site mixed compound Y0.5La0.5BaMn2O6 is synthesized, in which （Y, La） and Ba are regularly arranged, while Y and La randomly occupy the R-site. Y0.5La0.5BaMn2O6 has a tetragonal unit cell with a space group of P4/mmm. A structural transition between tetragonal and orthorhombic is observed at about 325 K by X-ray powder diffraction （XRD）. Thermal magnetic measurement shows the occurrence of an antiferromagnetic transition at the temperature TN～190 K. Anomalies in magnetization, resistivity and lattice parameters observed around 340 K indicate a charge/orbital order transition accompanying the structural phase transition. The R-site randomness effect is discussed to interpret the different properties of Y0.5La0.5BaMn2O6 between NdBaMn2O6 and SmBaMn2O6.

Giant magneto field effect in up-conversion amplified spontaneous emission via spatially extended states in organic-inorganic hybrid perovskites

Up-conversion lasing actions are normally difficult to realize in light-emitting materials due to small multi-photon absorp-tion cross section and fast dephasing of excited states during multi-photon excitation.This paper reports an easily ac-cessible up-conversion amplified spontaneous emission(ASE)in organic-inorganic hybrid perovskites(MAPbBr3)films by optically exciting broad gap states with sub-bandgap laser excitation.The broad absorption was optimized by adjust-ing the grain sizes in the MAPbBr3 films.At low sub-bandgap pumping intensities,directly exciting the gap states leads to 2-photon,3-photon,and 4-photon up-conversion spontaneous emission,revealing a large optical cross section of multi-photon excitation occurring in such hybrid perovskite films.At moderate pumping intensity(1.19 mJ/cm2)of 700 nm laser excitation,a significant spectral narrowing phenomenon was observed with the full width at half maximum(FWHM)de-creasing from 18 nm to 4 nm at the peak wavelength of 550 nm,simultaneously with a nonlinear increase on spectral peak intensity,showing an up-conversion ASE realized at low threshold pumping fluence.More interestingly,the up-con-version ASE demonstrated a giant magnetic field effect,leading to a magneto-ASE reaching 120%.In contrast,the up-conversion photoluminescence(PL)showed a negligible magnetic field effect(<1%).This observation provides an evid-ence to indicate that the light-emitting states responsible for up-conversion ASE are essentially formed as spatially exten-ded states.The angular dependent spectrum results further verify the existence of spatially extended states which are polarized to develop coherent in-phase interaction.Clearly,using broad gap states with spatially extended light-emitting states presents a new approach to develop up-conversion ASE in organic-inorganic hybrid perovskites.

Phase separation in Sr doped BiMnO_3

Phase separation in Sr doped BiMnO3 （Bil_xSrxMnO3, x = 0.4-0.6） was studied by means of temperature-dependent high-resolution neutron powder diffraction （NPD）, high resolution X-ray powder diffraction （XRD）, and physical property measurements. All the experiments indicate that a phase separation occurs at the temperature coinciding with the reported charge ordering temperature （Tco） in the literature. Below the reported TCO, both the phases resulting from the phase separation crystallize in the orthorhombically distorted perovskite structure with space group Imma. At lower temperature, these two phases order in the CE-type antiferromagnetic structure and the A-type antiferromagnetic structure, respectively. However, a scrutiny of the high-resolution NPD and XRD data at different temperatures and the electron diffraction exper- iment at 300 K did not manifest any evidence of a long-range charge ordering （CO） in our investigated samples, suggesting that the anomalies of physical properties such as magnetization, electric transport, and lattice parameters at the TCO might be caused by the phase separation rather than by a CO transition.