Distinct effects of homogeneous weak disorder and dilute strong scatterers on phase competition in manganites

We study the two orbital double-exchange model in two dimensions including antiferromagnetic (AFM) superexchange, Jahn-Teller coupling, and substitutional disorder. At hole doping x = 0.5 we focus on phase competition between the ferromagnetic metal (FMM) and the charge-ordered (CO) and orbital-ordered (OO) CE state and compare the impact of weak homogeneous disorder to that of a low density of strong scatterers. Even moderate homogeneous disorder suppresses the CE-CO-OO phase and leads to a glass with nanoscale correlations, while dilute strong scatterers of comparable strength convert the CE-CO-OO phase to a phase separated state with ferromagnetic metal and AFM-CO-OO clusters.     

Transition from antiferromagnetic to ferromagnetic state of systems LaMnO3+λ and La1−x Srx(Mn1−x/2Nb x/2)O3

The crystal structure and magnetic and elastic properties of the system LaMnO_3+λ are investigated for various concentrations of oxygen. Upon an increase in the oxygen concentration, the orbital-ordered phase is transformed into an orbital-disordered phase via a two-phase crystal-structure state in the interval 0.04<λ<0.06. The transition is accompanied by a jumplike increase in the Curie temperature and spontaneous magnetization. An analysis of the magnetic properties in weak fields and of the temperature dependence of the Young modulus reveals the properties typical of the orbital-ordered antiferromagnetic phase up to λ=0.08. It is proposed that the two-phase state is associated with the martensite type of the orbital order-disorder phase transformation. The system La_1?x Sr_x(Mn_{1 ?x/2}Nb _x/2)O₃ in which all manganese ions are in the trivalent state exhibits a sequence of antiferromagnetic-ferromagnetic (x>0.2) and ferromagnetic-spin glass (x>0.4) transitions. In both systems, the orbital-disordered phases are ferromagnetic, indicating the crucial role of orbital ordering in the formation of magnetic properties.     

Effect of orbital rotation and mixing on the optical properties of orthorhombic RMnO3 (R=La, Pr, Nd, Gd, and Tb)

We investigated the ab-plane absorption spectra of RMnO3 (R=La, Pr, Nd, Gd, and Tb) thin films. As the ionic radius of the R ion decreases, we observed a drastic suppression of the 2 eV peak, i.e., the intersite optical transition between spin- and orbital-aligned states across the Mott gap. We found that, in addition to orbital rotation, orbital mixing in the orbital-ordered state should play an important role in the suppression of 2 eV peak. We also found that the spectral weight of 2 eV peak is proportional to the A-type antiferromagnetic ordering temperature, which suggests that the magnetic interaction should be sensitively coupled to the orbital degree of freedom.     

轨道序对半掺杂锰氧化物光学性质的影响

在两轨道双交换模型基础上，讨论了电子关联作用对半掺杂锰氧化物轨道序的影响，推导出能计算各个相的光电导公式.结果显示，光吸收与轨道序之间存在关联现象.对于铁磁相，当格点库仑相互作用(U)从无到有逐渐增加时，铁磁相会从无轨道序过渡到有轨道序，相变前 后非相干光吸收有一个从无能隙到有能隙的明显变化.对于层状反铁磁的A相，U的增加会使 轨道序更明显，非相干光吸收部分的能隙随之也增大. 关键词： 轨道序 光电导 锰氧化物 库仑相互作用     

Orbital-order-induced metal-insulator transition in La(1-x)Ca(x)MnO3

We present evidence that the insulator-to-metal transition in La(1-x)Ca(x)MnO3 near x approximately 0.2 is driven by the suppression of coherent Jahn-Teller distortions, originating from d-type orbital ordering. The orbital-ordered state is characterized by large long-range Q2 distortions below T(O'- O*). Above T(O'- O*) we find evidence for coexistence between an orbital-ordered and an orbital-disordered state. This behavior is discussed in terms of electronic phase separation in an orbital-ordered insulating and an orbital-disordered metallic state.     

Field-induced orbital and magnetic phases in Ca3Ru2O7

Magnetic-field- and temperature-dependent Raman scattering studies of Ca3Ru2O7 reveal dramatic field-dependent properties arising from transitions between various complex orbital and magnetic phases, including a field-induced orbital-ordered to orbital-disordered transition (H(o) // hard axis), and a reentrant orbital-ordered to orbital-disordered to orbital-ordered transition (H(o) // easy axis). We find that the dramatic magnetic-field properties are most prevalent in a "mixed"-magnetic and -orbital phase regime, providing evidence for a strong connection between orbital phase inhomogeneity and "colossal" field effects in the ruthenates.     

Emergent phenomena in perovskite-type manganites

Perovskite-type manganites exhibit various interesting phenomena arising from complex interplay among spin, charge, orbital, and lattice degrees of freedom. One such example is the keen competition between phases with different spin/charge/orbital orders. Keen competition between antiferromagnetic metal and orbital-ordered insulator is found in the slightly electron-doped regime near Mn⁴⁺ state which is stabilized by the high oxygen-pressure condition. Another one is the emergence of ferroelectricity either induced by the magnetic ordering or independently of the magnetic ordering. As the respective examples, perovskite-type YMnO₃ and Sr_1−xBa_xMnO₃ are discussed. In the YMnO₃, the ferroelectric lattice distortion associated with the E-type spin order is observed for the first time. Displacement-type ferroelectricity with off-center magnetic ions is discovered for Sr_0.5Ba_0.5MnO₃, which shows both large polarization value and strong coupling between ferroelectricity and magnetism.     

Ground state of BaCoS2 as a set of energy-degenerate orbital-ordered configurations of Co2+ ions

The linear muffin-tin orbital method in the local density approximation (LDA + U) explicitly considering Coulomb correlations has been applied to calculate the electronic structure, magnetic moments, and parameters of the Heisenberg exchange interaction for cobalt ions in BaCoS₂. Five solutions close in total energy with various orbital ordering of Co²⁺ ions and almost identical spin magnetic moments μ = 2.32μ_B of the Co²⁺ ion 3d-shell have been found. The BaCoS₂ ground state can be considered as a set of energy-degenerate orbital-ordered configurations of Co²⁺ ions in the high-spin state.     

The first principle study on the electronic structure and spin ordering of the rare earth palladium sulfide, EuPd3S4

We have performed relativistic first-principles full-potential linearized augmented plane wave (FLAPW) calculation for rare earth palladium sulfide EuPd₃S₄ in the ferromagnetic and antiferromagnetic states. The density of 4f electrons of Eu is taken from a local-spin-density approximation self-interaction correction (LSDA-SIC) atomic calculation. EuPd₃S₄ is found to exhibit antiferromagnetic ordering in its ground state. The charge, orbital, magnetic moment and spin ordering are explained with the electronic structure, the orbital-projected density of states and the total energy study. EuPd₃S₄ is found to be stable in the body-centered Type-I antiferromagnetic state, in agreement with experimental results. Different Eu states are found in antiferromagnetic ordering. The magnetic moments of different states obtained through spin-polarized calculation are also in good agreement with experimental results. The phenomena observed are explained by the orbital hybridization of Eu and Pd ions as compared with the free ions.     

Parameter dependence of optical conductivity in antiferromagnetic phase of iron pnictides

We investigate the optical conductivity of iron pnictides in antiferromagnetic state by mean-field calculation in a five-band Hubbard model, focusing on its anisotropic behavior by examining several states calculated with different Hund coupling J, such as the states with a low or high magnetization and with or without a strong orbital ordering. In addition, we investigate the J dependence of the Dirac cone structure, which is crucial for the low energy excitation. In our calculations, a weakly ordered state with no orbital ordering shows the anisotropy of optical conductivity in accord with experiments. We conclude that the low energy part of the optical conductivity is relevant to the Dirac electron structure rather than the orbital ordering.     

一维自旋轨道模型中自旋-轨道能隙产生机理分析

讨论考虑洪特耦合的两带赫伯德模型得到的一维自旋轨道模型中自旋-轨道能隙的产生.运用SU(4)赝费米子表象下的平均场理论,计算求得价键序参数、准粒子激发谱能隙和自旋、轨道密度-密度关联函数随系统耦合参数变化的结果.随洪特耦合相互作用由零开始增强,系统激发谱能隙逐渐打开,并且系统在参数取值为J₁/J₂=1/3处由具有阻错的无序状态相变到自旋铁磁有序和轨道反铁磁有序的状态.     

一维自旋-轨道模型中的畴状轨道液体态

研究了一个一维可解自旋-轨道模型.在大自旋极限下，自旋自由度可以近似用经典自旋来描 述.在没有外磁场情形，系统的基态是伊辛自旋反铁磁背景下的轨道液体态.其低能元激发是 类似于spinon的轨道量子.而在有外磁场情形，系统会出现磁通点阵相.同时，磁通将系统分 割成不连通的轨道液体. 关键词： 自旋轨道系统 畴状轨道液体     

Orbital ordering transition in Ca2RuO4 observed with resonant X-ray diffraction

Resonant x-ray diffraction performed at the L(II) and L(III) absorption edges of Ru has been used to investigate the magnetic and orbital ordering in Ca2RuO4 single crystals. A large resonant enhancement due to electric dipole 2p-->4d transitions is observed at the wave-vector characteristic of antiferromagnetic ordering. Besides the previously known antiferromagnetic phase transition at T(N)=110 K, an additional phase transition, between two paramagnetic phases, is observed around 260 K. Based on the polarization and azimuthal angle dependence of the diffraction signal, this transition can be attributed to orbital ordering of the Ru t(2g) electrons. The propagation vector of the orbital order is inconsistent with some theoretical predictions for the orbital state of Ca2RuO4.     

Ordered valence-bond states in symmetric two-dimensional spin-orbital systems

We consider a superexchange Hamiltonian, H = -SUM ()(2S(i) . S(j)-(1/2)) (2T(i) . T(j)-(1/2)), which describes systems with orbital degeneracy and strong electron-phonon coupling in the limit of large on-site repulsion. In an SU(4) Schwinger boson representation, a reduced spin-orbital interaction is derived exactly, and a mean field theory has been developed. In one dimension, a spin-orbital liquid state with a finite gap is obtained. On a two-dimensional square lattice a novel type of spin-orbital ferromagnetically ordered state appears, while spin and orbital are antiferromagnetic. An important relation has been found, relating the spin and orbital correlation functions to the combined spin-orbital ones.     

Dimerization versus orbital-moment ordering in a Mott insulator YVO3

We use exact diagonalization combined with mean-field theory to investigate the phase diagram of the spin-orbital model for cubic vanadates. The spin-orbit coupling competes with Hund's exchange and triggers a novel phase, with the ordering of t(2g) orbital magnetic moments stabilized by the tilting of VO6 octahedra. It explains qualitatively spin canting and reduction of magnetization observed in YVO3. At finite temperature, an orbital instability in the C-type antiferromagnetic phase induces modulation of magnetic exchange constants even in the absence of lattice distortions. The calculated spin structure factor shows a magnon splitting at q-->=(0,0,pi / 2) due to the orbital dimerization.     

阳离子空位磁矩起因探讨

运用群论和分子轨道理论的方法, 系统地研究了非掺杂磁性半导体中阳离子空位产生磁矩的原因, 并用海森堡模型阐明了磁矩之间的交换耦合机理. 研究发现: 阳离子空位磁矩的大小与占据缺陷能级轨道的未配对电子数有关, 而缺陷能级的分布与空位的晶场对称性密切相关; 通过体系的反铁磁状态和铁磁状态下的能量差估算交换耦合系数J₀, 交换耦合系数J₀的正负可以用来预测磁矩之间的耦合是否为铁磁耦合:J₀>0, 则表明磁矩之间的耦合为铁磁耦合, 反之为反铁磁耦合. 最后指出空位的几何构型发生畸变(John-Teller效应)的原因: 缺陷能级轨道简并度的降低与占据缺陷能级轨道的电子的数目有直接的关系.     

Fragile magnetic ground state in half-doped LaSr2Mn2O7

We investigated the orbital and antiferromagnetic ordering behaviors of the half-doped bilayer manganite La(2-2x)Sr(1+2x)Mn2O7 (x ? 0.5) by using Mn L(2,3)-edge resonant soft x-ray scattering. Resonant soft x-ray scattering reveals the CE-type orbital order below T(oo) ? 220 K, which shows partial melting behavior below T(m) ? 165 K. We also found coexistence CE- and A-type antiferromagnetic orders. Both orders involve the CE-type orbital order with nearly the same orbital character and are coupled with each other. These results manifest that the ground state with the CE-type antiferromagnetic order is easily susceptible to destabilization into the A-type one even with a small fluctuation of the doping level, as suggested by the extremely narrow magnetic phase boundaries at x ? 0.5±0.005.     

Optical spectra of nearest neighbour nickel pairs in KMgF3 and KZnF3 crystals

The absorption, MCD, and emission spectra associated with the nearest neighbour Ni²⁺ pairs in KMgF₃ and KZnF₃ have been studied and analysed on the basis of the theory which includes spin dependent excitation transfer as well as spin independent transfer. It is shown that excitation transfers are important in determining the pair energy levels for the case where the singleion states involve orbital degeneracy. The antiferromagnetic J value of the ground state is determined to be 68 cm^-1.     

Competition between crystal field splitting and Hund’s rule coupling in two-orbital magnetic metal-insulator transitions

Competition between crystal field splitting and Hund’s rule coupling in magnetic metal-insulator transitions of half-filled two-orbital Hubbard model is investigated by multi-orbital slave-boson mean field theory. We show that with the increase of Coulomb interaction, the system firstly transits from a paramagnetic (PM) metal to a Néel antiferromagnetic (AFM) Mott insulator, or to a nonmagnetic orbital insulator, depending on the competition of crystal field splitting and the Hund’s rule coupling. The AFM Mott insulating, PM metallic and orbital insulating phases are not, partially and fully orbital polarized, respectively. For a small J _H and a finite crystal field, the orbital insulator is robust. These results demonstrate that large crystal field splitting favors the formation of the orbital insulating phase, while large Hund’s rule coupling tends to destroy it, driving the low-spin to high-spin transition.     

Magnetism of Co overlayers and nanostructures on W(0 0 1): A first-principles study

The magnetic properties of Co nanostructures and a Co monolayer on W(0 0 1) have been studied in the framework of density functional theory. Different geometries such as planar and three-dimensional clusters have been considered, with cluster sizes varying between 2 and 13 atoms. The calculations were performed using the real-space linear muffin-tin orbital method (RS-LMTO-ASA). With respect to the stability of the magnetic state, we predict an antiferromagnetic (AFM) structure for the ground state of the planar Co clusters and a ferromagnetic (FM) state for the three-dimensional clusters. For the three-dimensional clusters, one of the AFM arrangements leads to frustration due to the competing FM and AFM exchange interactions between different atoms in the cluster, and gives rise to a non-collinear state with energy close to that of the FM ground state. The relative role of the Co–Co and Co–W exchange interactions is also investigated.