The semiconductor-insulator phase transition of the single-layer manganite La0.5Sr1.5MnO4 has been studied by means of high resolution synchrotron x-ray powder diffraction and resonant x-ray scattering at the Mn K edge. We conclude that a concomitant structural transition from tetragonal I4/mmm to orthorhombic Cmcm phases drives this electronic transition. A detailed symmetry-mode analysis reveals that condensation of three soft modes -Delta_2(B2u), X1+(B2u) and X1+(A)- acting on the oxygen atoms accounts for the structural transformation. The Delta_2 mode leads to a pseudo Jahn-Teller distortion (in the orthorhombic bc-plane only) on one Mn site (Mn1) whereas the two X1+ modes produce an overall contraction of the other Mn site (Mn2) and expansion of the Mn1 one. The X1+ modes are responsible for the tetragonal superlattice (1/2,1/2,0)-type reflections in agreement with a checkerboard ordering of two different Mn sites. A strong enhancement of the scattered intensity has been observed for these superlattice reflections close to the Mn K edge, which could be ascribed to some degree of charge disproportion between the two Mn sites of about 0.15 electrons. We also found that the local geometrical anisotropy of the Mn1 atoms and its ordering originated by the condensed Delta_2 mode alone perfectly explains the resonant scattering of forbidden (1/4,1/4,0)-type reflections without invoking any orbital ordering.
While double perovskites A2BB'O6, if ordered, usually form a rock-salt-type structure with a checkerboard B/B' ordering, it is surprising that Ca2FeMnO6 has alternate FeO2 and MnO2 layers in its perovskite structure. Here we demonstrate, using density functional calculations, that this unusual layered ordering facilitates, and is largely helped by, the Fe3+-Fe5+ charge disproportionation (CD) of the formal Fe4+ ions, which would otherwise be frustrated in the common rock salt structure. To further verify the important role of the CD for stabilization of this layered ordering, we carry out a co…
We have studied the sub-picosecond quasiparticle dynamics in the perovskite manganite La0.7Ca0.3MnO3 and the layered manganite La1.4Sr1.6Mn2O7 using ultrafast optical spectroscopy. We found that for T > TC, initial relaxation proceeds on the time scale of several hundred femtoseconds and corresponds to the redressing of a photoexcited electron to its polaronic ground state. The temperature and dimensionality dependence of this polaron redressing time provides insight into the relationship between polaronic motion and spin dynamics on a sub-picosecond time scale. We also observe a crossover to …
We investigated the electronic structures of the two-dimensional layered perovskite Sr$_{2}$\textit{M}O$_{4}$ (\textit{M}=4\textit{d} Ru, 4\textit{d} Rh, and 5\textit{d} Ir) using optical spectroscopy and polarization-dependent O 1\textit{s} x-ray absorption spectroscopy. While the ground states of the series of compounds are rather different, their optical conductivity spectra $σ(ω)$ exhibit similar interband transitions, indicative of the common electronic structures of the 4\textit{d} and 5\textit{d} layered oxides. The energy splittings between the two $e_{g}$ orbitals, $i.e.$, $d_{3z^{2}-…
Inelastic neutron-scattering measurements were performed on a single crystal of the layered colossal magnetoresistance (CMR) material La1.2Sr1.8Mn2O7 (Tc ~ 120K). We found that the spin wave dispersion is almost perfectly two-dimensional with the in-plane spin stiffness constant D ~ 151meVA. The value is similar to that of similarly doped La1-xSrxMnO3 though its Tc is three times higher, indicating a large renormalization due to low dimensionality. There exist two branches due to a coupling between layers within a double-layer. The out-of-plane coupling is about 30% of the in-plane coupling th…
We theoretically investigate magnetic properties of Sr$_2$TcO$_4$, a 4d transition-metal layered perovskite of the K$_2$NiF$_4$-type with half-filled t$_{2g}$ states. The effect of local Coulomb repulsion between the t$_{2g}$ orbitals is included within the density-functional theory (DFT)+U and DFT+dynamical mean-field theory (DMFT) methods. The DFT+DMFT predicts paramagnetic Sr$_2$TcO$_4$ to be close to the Mott insulator-to-metal transition, similarly to the cubic compound SrTcO$_3$. The inter-site exchange interactions computed within the DFT+DMFT framework point to a strong antiferromagnet…
Pressure effects on the charge and spin dynamics in the bilayer manganite compounds $La_{2-2x}Sr_{1+2x}Mn_2O_7$ are studied theoretically by taking into account the orbital degrees of freedom. The orbital degrees are active in the layered crystal structure, and applied hydrostatic pressure stabilizes the $3d_{x^2-y^2}$ orbital in comparison with $3d_{3z^2-r^2}$. The change of the orbital states weakens the interlayer charge and spin couplings, and suppresses the three dimensional ferromagnetic transition. Numerical results, based on an effective Hamiltonian which includes the energy level diff…
We present genuine bulk Ir 5d jeff states of layered perovskite iridates obtained by hard-x-ray photoemission spectroscopy (HAXPES) with s- and p-polarized lights. HAXPES spectra of Sr2IrO4 and Ba2IrO4 are well reproduced by the quasi-particle densities of states calculated by the local density approximation with dynamical mean-field theory (LDA+DMFT). It is demonstrated that the insulating nature of the iridates is triggered by antiferromagnetic correlation (Slater type) combined with electron correlation (Mott type). The extremely-low-energy bulk-sensitive photoemission spectroscopy reveals …
We report structural, magnetic and dielectric properties of layered perovskite materials LnBaCuFeO5 (Ln = La and Lu). LaBaCuFeO5 shows magnetic cluster glass behavior below 60 K owing to the competing ferromagnetic and antiferromagnetic exchange interactions. Glassy dynamics of electric dipoles has also been observed in the vicinity of the magnetic glass transition temperature. The presence of significant coupling between spin and polar degrees of freedom results in the multiglass feature in LaBaCuFeO5. The LuBaCuFeO5 compound undergoes YBaCuFeO5 like commensurate to incommensurate antiferroma…
In strongly correlated electronic systems, several novel physical properties are induced by the orbital degree of freedom. In particular, orbital degeneracy near the Fermi level leads to spontaneous symmetry breaking, such as the nematic state in FeSe and the orbital ordering in several perovskite systems. Here, the novel layered perovskite material CsVF$_4$, with a $3d^2$ electronic configuration, was systematically studied using density functional theory and a multiorbital Hubbard model within the Hatree-Fock approximation. Our results show that CsVF$_4$ should be magnetic, with a G-type ant…
We investigate the metal-insulator transition in the layered Ruddelsden Popper series of strontium iridates Srn+1IrnO3n+1. Tight-binding models of t2g orbitals for n = 1, 2, and infinity are constructed, and changes in band dispersion due to dimensionality and spin-orbit coupling are presented. Identifying the states near the Fermi level to be predominantly Jeff = 1/2, we use an effective Hubbard model to study the effect of correlations. Transitions from a metallic state to various magnetically ordered states at different critical interactions are obtained. A canted antiferromagnetic insulato…
We have investigated the peculiar structure of charge and spin ordering in the half-doped layered perovskite oxide La$_{1.5}$Sr$_{0.5}$CoO$_4$ by elastic neutron scattering. Two samples with different preparation histories were studied. We find that the generic features of the ordered states, such as their short-range, glassy nature and the spin incommensurability, are sample-independent. At the same time, some subtle features of the ordered phases, such as the correlation lengths, differ.
Monte Carlo simulations are performed on the three-dimensional (3D) Ising model with the 2-1-4 layered perovskite structure as a minimal model for checkerboard charge ordering phenomena in layered perovskite oxides. Due to the interlayer frustration, only 2D long-range order emerges with a finite correlation length along the c axis. Critical exponents of the transition change continuously as a function of the interlayer coupling constant. The interlayer long-range Coulomb interaction decays exponentially and is negligible even between the second-neighbor layers. Instead, monoclinic distortion …
Charge and orbital ordering behaviors in the half doped bi-layered compound LaSr2Mn2O7 have been studied by resonant and non-resonant X-ray scattering. Three different order parameters, which correspond to the A-type antiferromagnetic, a charge and an orbital ordered states, were observed by measuring the magnetostriction and the superlattice peaks characterized by wavevectors (1/2 1/2 0) and (1/4 1/4 0), respectively. The superlattice reflections indicating the charge and orbital ordered states were observed below 210 K. Both the intensities reach a maximum at 160 K on cooling and become very…
A series of layered perovskites Sr$_2$$M$O$_4$ ($M$=Ti, V, Cr, and Mn) is studied by $ab $ $initio$ calculations within generalized gradient approximation (GGA) and GGA+$U$ schemes. The total energies in different magnetic configurations, including the nonmagnetic, ferromagnetic, the layered antiferromagnetic with alternating ferromagnetic plane and the staggered in-plane antiferromagnetic (AFM-II) order, are calculated. It is found that Sr$_2$TiO$_4$ is always a nonmagnetic band insulator. For Sr$_2$MnO$_4$, both GGA and GGA+$U$ calculations show that the insulating AFM-II state has the lowes…
The effect of local structure on the magnetic and transport properties of the layered perovskites has been investigated. The samples PrBaCo$_{2}$O$_{5+δ}$, ($δ$ = 0.80 and 0.67) though crystallize in the same 112 type tetragonal structure have different magnetic ground states. Extended X-ray Absorption Fine Structure (EXAFS) spectroscopy has been employed to explain the changes in magnetic interactions based on the rotation and tilting of CoO polyhedra in these oxygen rich double perovskites.
We report on the magnetic properties of the layered perovskite PbVO(3). The results of magnetic susceptibility and specific heat measurements as well as band structure calculations consistently suggest that the S=1/2 square lattice of vanadium atoms in PbVO(3) is strongly frustrated due to next-nearest-neighbor antiferromagnetic interactions. The ratio of next-nearest-neighbor (J(2)) to nearest-neighbor (J(1)) exchange integrals is estimated to be J(2)/J(1)\approx 0.2-0.4. Thus, PbVO(3) is within or close to the critical region of the J(1)-J(2) frustrated square lattice. Supporting this, no si…
The ratio of orbital (L) and spin (S) contributions to the magnetically ordered moments of a 5d transition metal oxide, Sr2IrO4 was evaluated by non-resonant magnetic x-ray diffraction. We applied a new experimental setting to minimize the error in which we varied only the linear-polarization of incident x-ray at a fixed scattering angle. Strong polarization dependence of the intensity of magnetic diffraction was observed, from which we conclude that the ordered moments contain substantial contribution from the orbital degree of freedom with the ratio of <L>/<S> ~5.0, evidencing the pronounce …
The magnetic structure and spin-wave excitations in the quasi-square-lattice layered perovskite compound La$_5$Mo$_4$O$_{16}$ were studied by a combination of neutron diffraction and inelastic neutron scattering techniques using polycrystalline sample. Neutron powder diffraction refinement revealed that the magnetic structure is ferrimagnetic in the $ab$ plane with antiferromagnetic stacking along the $c$ axis where the magnetic propagation vector is $\mathbf{k}=\left(0,0,\frac{1}{2}\right)$. The ordered magnetic moments are estimated to be $0.54(2)μ_\text{B}$ for Mo$^{5+}$ ($4d^1$) ions and $…
The tri-layered perovskite Sr4Rh3O10 is reported for the first time. High-pressure and high-temperature heating (6 GPa and 1500 C) brought about successful preparation of a polycrystalline sample of the expected member at n=3 of Srn+1RhnO3n+1. Neutron-diffraction studies revealed the orthorhombic crystal structure (Pbam) at room temperature and 3.4 K. Local structure distortions rotationally tilt the RhO6 octahedra ~12 degrees in the perovskite-based blocks along the c-axis, and approximately a 20 % disorder was found in sequence of the alternating rotational tilt. The sample was also investig…
We have investigated cobaltite relatives of the layered perovskite cuprates and nickelates, Pr$_{2-x}$Ca$_x$CoO$_4$ ($0.39 \leq x \leq 0.73$) and La$_{2-x}$Sr$_x$CoO$_4$ ($x = 0.61$), using elastic neutron scattering. We have discovered doping-dependent incommensurate short-range ordering of charges and magnetic moments, which in cobaltites occur in the range of heavy doping, $ 0.5 \lesssim x \lesssim 0.75$. The charge order exists already at room temperature and shows no change on cooling. The incommensurability of its propagation vector, ${\bf Q}_c = (ε_c,0,l)$, roughly scales with the conce…
Charge-lattice fluctuations are observed in the layered perovskite manganite LaSr2Mn2O7 by Raman spectroscopy as high as 340 K and with decreasing temperature they become static and form a charge ordered (CO) phase below TCO=210 K. In the static regime, superlattice reflections are observed through neutron and x-ray diffraction with a propagation vector (h+1/4,k-1/4,l). Crystallographic analysis of the CO state demonstrates that the degree of charge and orbital ordering in this manganite is weaker than the charge ordering in three dimensional perovskite manganites. A TN=170K a type-A antiferro…
YBaCuFeO5 is one of the interesting multiferroic compounds, which exhibits magnetic ordering and dielectric anomaly above 200 K. Partial substitution of Fe with other magnetic and non-magnetic ion affects the magnetic and the structural properties of the system. We report detailed investigation of structural, magnetic and dielectric properties of YBaCuFe0.85M0.15O5 (M=Co, Ni and Ga). We observed that the partial replacement of Ni and Co in place of Fe, results in magnetic dilution and broadening of the magnetic transition and shifting towards lower temperature. The replacement of Fe with non-m…
We have measured the cyclotron masses in Sr2RuO4 through the observation of periodic-orbit-resonances - a magnetic resonance technique closely related to cyclotron resonance. We obtain values for the alpha, beta and gamma Fermi surfaces of (4.33+/-0.05)me, (5.81+/-0.03)me and (9.71+/-0.11)me respectively. The appreciable differences between these results and those obtained from de Haas- van Alphen measurements are attributable to strong electron-electron interactions in this system. Our findings appear to be consistent with predictions for a strongly interacting Fermi liquid; indeed, semi-quan…
The novel electronic state of the canted antiferromagnetic (AFM) insulator, strontium iridate (Sr2IrO4) has been well described by the spin-orbit-entangled isospin Jeff = 1/2, but the role of isospin in transport phenomena remains poorly understood. In this study, antiferromagnet-based spintronic functionality is demonstrated by combining unique characteristics of the isospin state in Sr2IrO4. Based on magnetic and transport measurements, large and highly anisotropic magnetoresistance (AMR) is obtained by manipulating the antiferromagnetic isospin domains. First-principles calculations suggest…
The magnetic properties of GdBaMn_{2}O_{5.0}, which exhibits charge ordering, are studied from 2 to 400 K using single crystals. In a small magnetic field applied along the easy axis, the magnetization M shows a temperature-induced reversal which is sometimes found in ferrimagnets. In a large magnetic field, on the other hand, a sharp change in the slope of M(T) coming from an unusual turnabout of the magnetization of the Mn sublattices is observed. Those observations are essentially explained by a molecular field theory which highlights the role of delicate magnetic interactions between Gd^{3…
The effect of oxygen content on the magnetic properties of the layered perovskites has been investigated. The samples, PrBaCo$_{2}$O$_{5+δ}$ (0.35 $\leq δ\leq$ 0.80) were prepared by sol-gel method and characterized by X-ray diffraction and DC magnetization. A detailed magnetic phase diagram for PrBaCo$_{2}$O$_{5+δ}$ is presented. It is found that unlike in the case of heavier rare-earths, ferromagnetic interactions are present at all temperatures below Tc and even in the antiferromagnetically ordered phase. Moreover, in compounds with lower oxygen content, short range ferromagnetic interactio…
Low-temperature spin dynamics of the double-layered perovskite La_2-2x_Sr_1+2x_Mn_2_O_7 (LSMO327) was systematically studied in a wide hole concentration range (0.3 <= x < 0.5). The spin-wave dispersion, which is almost perfectly 2D, has two branches due to a coupling between layers within a double-layer. Each branch exhibits a characteristic intensity oscillation along the out-of-plane direction. We found that the in-plane spin stiffness constant and the gap between the two branches strongly depend on x. By fitting to calculated dispersion relations and cross sections assuming Heisenberg mode…
The layered compound La2-2xSr1+2xMn2O7 (x=0.3) consists of bilayers of metallic MnO2 sheets separated by insulating material. The compound exhibits markedly anisotropic magnetoresistance at temperatures well below the three-dimensional magnetic ordering temperature TC=90 K in addition to colossal magnetoresistance around TC. We present neutron diffraction data which show that the magnetic structure of this material switches from antiferromagnetic stacking of the (ferromagnetically ordered) sheets in zero field to ferromagnetic stacking in a field of 1.5 Tesla. The data are the first to be coll…
Interplay of Fermi surface topology and electron correlation is the quintessential ingredient underlying spontaneous symmetry breaking in itinerant electronic systems. In one-dimensional (1D) systems at half-filling, the inherent Fermi surface nesting makes the translationally invariant metallic state unstable, which is known as Peierls instability. Extending the scope of Peierls instability to two (2D) or three dimensions (3D), however, is not straightforward, since the Fermi surface in higher dimensions is generally not nested. In this work, we show that a perfectly nested Fermi surface can …
In insulating materials with ordered magnetic spiral phases, ferroelectricity can emerge due to the breaking of inversion symmetry. This property is of both fundamental and practical interest, in particular with a view to exploiting it in low-power electronic devices. Advances towards technological applications have been hindered, however, by the relatively low ordering temperatures $T_\mathrm{spiral}$ of most magnetic spiral phases, which rarely exceed 100 K. We have recently established that the ordering temperature of a magnetic spiral can be increased up to 310 K by the introduction of che…
Two-dimensional magnetic materials have recently attracted great interest due to their unique functions as the electric field control of a magnetic phase and the anomalous spin Hall effect. For such remarkable functions, a spin-orbit coupling (SOC) serves as an essential ingredient. Here we report a giant positive magnetoresistance in a layered magnetic semiconductor AgCrSe2, which is a manifestation of the subtle combination of the SOC and Zeeman-type spin splitting. When the carrier concentration approaches the critical value of 2.5\times10^18 cm^-3, a sizable positive magnetoresistance of ~…
Compositionally tunable vanadium oxyhydrides Sr2VO4-xHx (x = 0 - 1) without considerable anion vacancy were synthesized by high-pressure solid state reaction. The crystal structures and their properties were characterized by powder neutron diffraction, synchrotron X-ray diffraction, thermal desorption spectroscopy, and first-principles density functional theory (DFT) calculations. The hydrogen anions selectively replaced equatorial oxygen sites in the VO6 layers via statistical substitution of hydrogen in the low x region (x < 0.2). A new orthorhombic phase (Immm) with an almost entirely hydro…
A new layered perovskite-type oxide Ba$_2$RhO$_4$ was synthesized by a high-pressure technique with the support of convex-hull calculations. The crystal and electronic structure were studied by both experimental and computational tools. Structural refinements for powder x-ray diffraction data showed that Ba$_2$RhO$_4$ crystallizes in a K$_2$NiF$_4$-type structure, isostructural to Sr$_2$RuO$_4$ and Ba$_2$IrO$_4$. Magnetic, resistivity, and specific heat measurements for polycrystalline samples of Ba$_2$RhO$_4$ indicate that the system can be characterized as a correlated metal. Despite the clo…
We report a detailed study of the magnetic-field-orientation dependence of the millimetre-wave magnetoconductivity of the superconductor Sr2RuO4 We find two harmonic series of cyclotron resonances. We assign the first, corresponding to a quasiparticle mass of $4.29 \pm 0.05 m_{\rm e}$, where $m_{\rm e}$ is the free-electron mass, to the $β$ Fermi-surface section. We assign the second series, which contains only odd harmonics, to cyclotron resonance of the $γ$ Fermi-surface section, yielding a quasiparticle mass of $12.35 \pm 0.20 m_{\rm e}$. A third, single cyclotron resonance, corresponding t…
We report the discovery of weak topological insulators by ab initio calculations in a honeycomb lattice. We propose a structure with an odd number of layers in the primitive unit-cell as a prerequisite for forming weak topological insulators. Here, the single-layered KHgSb is the most suitable candidate for its large bulk energy gap of 0.24 eV. Its side surface hosts metallic surface states, forming two anisotropic Dirac cones. Though the stacking of even-layered structures leads to trivial insulators, the structures can host a quantum spin Hall layer with a large bulk gap, if an additional si…
