The interactions between charge and orbitally ordered $d$-electrons are important in many transition metal oxides. We propose an effective energy model for such interactions, parameterized with DFT+U calculations, so that energy contributions of both electronic and lattice origin can be simultaneously accounted for. The model is applied to the low-temperature phase of magnetite, for which we propose a new ground state structure. The effective interactions on the B-lattice of Fe$_3$O$_4$ can be interpreted in terms of electrostatics and short-range Kugel-Khomskii exchange coupling. The frustration between optimal charge and orbital orderings leads to a complex energy landscape whereby the supercell for the charge ordering, orbital ordering and ionic displacements can all be different.
The orbital shapes and charge disproportionations at nominal Mn$^{3+}$ and Mn$^{4+}$ sites for the charge- and orbital-ordered phases have been studied on half-doped manganites Pr(Sr$_{0.1}$Ca$_{0.9}$)$_2$Mn$_2$O$_7$ and Eu$_{0.5}$Ca$_{1.5}$MnO$_4$ with double-layer and single-layer Mn-O networks, respectively, by means of x-ray structural analyses, in comparison with Pr$_{0.5}$Ca$_{0.5}$MnO$_3$ with the pseudo cubic network. In a single-layer Eu$_{0.5}$Ca$_{1.5}$MnO$_4$ system, the ($y^2-z^2$)/($z^2-x^2$)-type orbital shape is observed, while the ($3y^2-r^2$)/($3x^2-r^2$)-type orbital shape i…
We report resonant x-ray scattering studies of charge and orbital order in Pr_{1-x}Ca_{x}MnO_3 with x=0.4 and 0.5. Below the ordering temperature, T_O=245 K, the charge and orbital order intensities follow the same temperature dependence, including an increase at the antiferromagnetic ordering temperature, T_N. High resolution measurements reveal, however, that long range orbital order is never achieved. Rather, an orbital domain state is formed. Above T_O, the charge order fluctuations are more highly correlated than the orbital fluctuations. Similar phenomenology is observed in a magnetic fi…
The role of lattice distortion in the charge, orbital and spin ordering in half doped manganites has been investigated. For fixed magnetic ordering, we show that the cooperative lattice distortion stabilize the experimentally observed ordering even when the strong on-site electronic correlation is taken into account. Furthermore, without invoking the magnetic interactions, the cooperative lattice distortion alone may lead to the correct charge and orbital ordering including the charge stacking effect, and the magnetic ordering can be the consequence of such a charge and orbital ordering. We pr…
Correlation-induced spin-charge and spin-orbital coupling effects on spin dynamics in ferromagnetic manganites are calculated with realistic parameters in order to provide a quantitative comparison with experimental results for spin stiffness, magnon dispersion, magnon damping, anomalous zone-boundary magnon softening, and Curie temperature. The role of orbital degeneracy, orbital ordering, and orbital correlations on spin dynamics in different doping regimes is highlighted.
We study effects of charge self-consistency within the combination of density functional theory (DFT; Wien2k) with dynamical mean field theory (DMFT; w2dynamics) in a basis of maximally localized Wannier orbitals. Using the example of two cuprates, we demonstrate that even if there is only a single Wannier orbital with fixed filling, a noteworthy charge redistribution can occur. This effect stems from a reoccupation of the Wannier orbital in k-space when going from the single, metallic DFT band to the split, insulating Hubbard bands of DMFT. We analyze another charge self-consistency effect be…
The two-orbital degenerate Hubbard model with distinct hopping integrals is studied by combining dynamical mean-field theory with quantum Monte Carlo simulations. The role of orbital fluctuations for the nature of the Mott transition is elucidated by examining the temperature dependence of spin, charge and orbital susceptibilities as well as the one-particle spectral function. We also consider the effect of the hybridization between the two orbitals, which is important particularly close to the Mott transition points. The introduction of the hybridization induces orbital fluctuations, resultin…
The competition of charge, orbital, and ferromagnetic interactions in layered manganites is investigated by magneto-Raman scattering spectroscopy. We find that the colossal magnetoresistance effect in the layered compounds results from the interplay of the orbital and ferromagnetic double-exchange correlations. Inelastic scattering by charge-order fluctuations dominates the quasiparticle dynamics in the ferromagnetic-metal state. The scattering is suppressed at low frequencies, consistent with the opening of a charge-density wave pseudogap.
Motivated by the recent ARPES measurements (Evtushinsky et. al., PRL {\bf 105}, 147201 (2010)) and evidence for the density-wave state for the charge and orbital ordering (García et al., PRL {\bf 109}, 107202 (2012)) in La$_{0.5}$Sr$_{1.5}$MnO$_4$, the issue of charge and orbital ordering in a two orbital tight-binding model for layered manganite near half doping is revisited. We find that the charge order with an ordering wavevector 2${\bf Q}$ = $(π, π)$ is induced by the orbital order of $B_{1g}$ representation with a different ordering wavevector ${\bf Q}$, where the primary order parameter…
We investigate the high temperature phase of layered manganites, and demonstrate that the charge-orbital phase transition without magnetic order in La$_{0.5}$Sr$_{1.5}$MnO$_4$ can be understood in terms of the density wave instability. The orbital ordering is found to be induced by the nesting between segments of Fermi surface with different orbital characters. The simultaneous charge and orbital orderings are elaborated with a mean field theory. The ordered orbitals are shown to be $d_{x^2-y^2} \pm d_{3z^2-r^2}$.
Temperature dependences of a magnetic and an orbital Bragg reflection at the Mn L2 and L3 edges of La0.5Sr1.5MnO4 have been collected. The temperature evolution of the orbital reflection depend strongly on the x-ray energy and reflects the different order parameteres for orbitals and Jahn-Teller distortions. The gradual increase of the orbital order parameter indicates that the orbital order and not the Jahn-Teller distortion drives the metal-insulator transition. Correspondingly, the orbital-orbital (super) exchange interaction dominates over the Jahn-Teller strain-field interaction.
We present the results of a systematic x-ray scattering study of the charge and orbital ordering in the manganite series Pr$_{1-x}$Ca$_x$MnO$_3$ with $x$=0.25, 0.4 and 0.5. The temperature dependence of the scattering at the charge and orbital wavevectors, and of the lattice constants, was characterized throughout the ordered phase of each sample. It was found that the charge and orbital order wavevectors are commensurate with the lattice, in striking contrast to the results of earlier electron diffraction studies of samples with $x$=0.5. High momentum-transfer resolution studies of the x=0.4 …
We investigate spin-charge-orbital ordering in a Mn$^{3+}$/Mn$^{4+}$ mixed valence state on a hollandite-type lattice using unrestricted Hartree-Fock calculation on a multi-band Mn 3$d$-O 2$p$ lattice model. The calculations show that the Mn$^{3+}$-Mn$^{4+}$ double exchange interaction, the Mn$^{3+}$-Mn$^{3+}$ and Mn$^{4+}$-Mn$^{4+}$ superexchange interactions are ferromagnetic and play important roles to stabilize the charge and orbital ordering pattern. The most stable charge and orbital ordering pattern is consistent with the $1\times1\times1$ orthorhombic or monoclinic structure of K$_{1.6…
The collective behavior of correlated electrons in the VO$_2-$interface layer of LaVO$_3$/SrTiO$_3$ heterostructure is studied within a quarter-filled $t_{2g}$-orbital Hubbard model on a square lattice. We argue that the ground state is ferromagnetic driven by the double exchange mechanism, and is orbitally and charge ordered due to a confined geometry and electron correlations. The orbital and charge density waves open gaps on the entire Fermi surfaces of all orbitals. The theory explains the observed insulating behavior of the $p$-type interface between LaVO$_3$ and SrTiO$_3$.
We study the real-time evolution of a charge-excited state in a one-dimensional $e_{\rm g}$-orbital degenerate Hubbard model, by a time-dependent density-matrix renormalization group method. Considering a chain along the $z$ direction, electrons hop between adjacent $3z^2-r^2$ orbitals, while $x^2-y^2$ orbitals are localized. For the charge-excited state, a holon-doublon pair is introduced into the ground state at quarter filling. At initial time, there is no electron in a holon site, while a pair of electrons occupies $3z^2-r^2$ orbital in a doublon site. As the time evolves, the holon motion…
We present a mean-field theory of charge, orbital, and spin ordering in manganites at 50% and 0% dopings by considering Jahn-Teller interaction, nearest-neighbor repulsion, and no single-site double occupancy. For spinless fermions, we show that Jahn-Teller distortion and charge-orbital ordering occur simultaneously. In our two-dimensional model at 50% doping, for small nearest-neighbor repulsion the system is orbitally polarized while for larger repulsion the system undergoes CE type ordering. As for the 0% doping case, the ground state is orbitally antiferromagnetic. Upon including spin degr…
Electronic structure of NdNiO3 and YNiO3 are calculated by using LSDA+U method with rotational invariance. No orbital order on Ni sites is observed in both systems but different charge orderings. In a small distorting system NdNiO3, all Ni ions are trivalent and oxygen sites have a particular ordering, both in charge and orbital. In a large distorting system YNiO3, the charge disproportionation occurs. The charge ordering stabilizes the asymmetry of the arrangement of the local magnetic moments around each nickel site without the Jahn-Teller distortion in both systems. The charge compensation …
We report coherent x-ray scattering studies of charge and orbital domains in manganite systems. The experiments were carried out on LaMnO_3 and Pr_{0.6}Ca_{0.4}MnO_3, with the incident photon energy tuned near the Mn K edge. At room temperature, the orbital speckle pattern of LaMnO_3 was observed to be constant over a timescale of at least minutes, which is indicative of static orbital domains on this timescale. For Pr_{0.6}Ca_{0.4}MnO_3, both charge and orbital speckle patterns were observed. The observation of the latter rules out the presence of fast orbital fluctuations, while long time se…
We propose the origin of the charge-ordered stripe structure with the orbital ordering observed experimentally in La_(1-x)Ca_(x)MnO_(3) (x=1/2, 2/3), in which the long-range Coulomb interaction plays an essential role. We study a Hubbard model with doubly-degenerate e_g orbitals, and treat the on-site Coulomb interaction (U) and the nearest-neighbor one (V) with the Hartree-Fock approximation. Both the charge and orbital ordering structures observed in experiments are reproduced in a wide region of the U-V phase diagram determined by the present study. The stability of the orbital ordering is …
Taking into account both Pauli and orbital effects of external magnetic field we compute the mean field phase diagram for charge density waves in quasi-one-dimensional electronic systems. The magnetic field can cause transitions to CDW states with two types of the shifts of wave vector from its zero-field value. It can also stabilize the field-induced charge density wave. Furthermore, the critical temperature shows peaks at a new kind of magic angles.
We have analyzed the experimental evidence of charge and orbital ordering in La0.5Sr1.5MnO4 using first principles band structure calculations. Our results suggest the presence of two types of Mn sites in the system. One of the Mn sites behaves like an Mn(3+) ion, favoring a Jahn-Teller distortion of the surrounding oxygen atoms, while the distortion around the other is not a simple breathing mode kind. Band structure effects are found to dominate the experimental spectrum for orbital and charge ordering, providing an alternate explanation for the experimentally observed results.
Theoretical and computational results are presented clarifying the role of long-ranged strain interactions in determining the charge and orbital ordering in colossal magnetoresistance manganites. The strain energy contribution is found to be of order 20-30 meV/Mn and in particular stabilizes the anomalous 'zig-zag chain' order observed in many half-doped manganites.
Using first principle band structure calculations, we critically examine results of resonant x-ray scattering experiments which is believed to directly probe charge and orbital ordering. Considering the specific case of La0.5Sr1.5MnO4, we show that this technique actually probes most directly and sensitively small structural distortions in the system. Such distortions, often difficult to detect with more conventional techniques, invariably accompany and usually cause the orbital and charge orderings. In this sense, this technique is only an indirect probe of such types of ordering. Our results…
In a recent published paper [Phys. Rev. B 64, 195133 (2001)], Zimmermann et al. present a systematic x-ray scattering study of charge and orbital ordering phenomena in the Pr1-xCaxMnO3 series with x= 0.25, 0.4 and 0.5. They propose that for Ca concentrations x=0.4 and 0.5, the appearance of (0, k+1/2, 0) reflections are originated by the orbital ordering of the eg electrons in the a-b plane while the (0, 2k+1, 0) reflections are due to the charge ordering among the Mn3+ and Mn4+ ions. Moreover, for small Ca concentrations (x<0.3), the orbital ordering is only considered and it occurs at (0, k,…
We investigate the ground-state properties of a t2g-orbital Hubbard model on a triangular lattice at electron density 5.5 by using numerical techniques. There appear several types of paramagnetic phases, but we observe in common that one or two orbitals among three orbitals become relevant due to the effect of orbital arrangement. It is found that charge stripes stabilized by the nearest-neighbor Coulomb interaction consist of antiferromagnetic/ferro-orbital chains for small Hund's coupling, while there occurs stripe charge ordering with ferromagnetic/antiferro-orbital chains for large Hund's …
Taking the orbital degeneracy of $e_g$ conduction bands and the Coulomb interaction into account in a double-exchange model, we investigate charge dynamics of perovskite Mn oxides by the Lancz$\ddot{\rm o}$s diagonalization method. In the metallic phase near the Mott insulator, it is found that the optical conductivity for a spin-polarized two-dimensional system exhibits a weight transfer to a broad and incoherent structure within the lower-Hubbard band together with a suppressed Drude weight. It reproduces qualitative feature of the experimental results. As an orbital effect, we find that an …
An explanation is given for the charge order, orbital order and insulating state observed in half-doped manganese oxides, such as Nd$_{1/2}$Sr$_{1/2}$MnO$_{3}$. The competition between the kinetic energy of the electrons and the magnetic exchange energy drives the formation of effectively one-dimensional ferromagnetic zig-zag chains. Due to a topological phase factor in the hopping, the chains are intrinsically insulating and orbital-ordered. Most surprisingly, the strong Coulomb interaction between electrons on the same Mn-ion leads to the experimentally observed charge ordering. For doping l…
The magnetic correlations in the charge- and orbital-ordered manganite La(0.5)Sr(1.5)MnO(4) have been studied by elastic and inelastic neutron scattering techniques. Out of the well-defined CE-type magnetic structure with the corresponding magnons a competition between CE-type and ferromagnetic fluctuations develops. Whereas ferromagnetic correlations are fully suppressed by the static CE-type order at low temperature, elastic and inelastic CE-type correlations disappear with the melting of the charge-orbital order at high temperature. In its charge-orbital disordered phase, La(0.5)Sr(1.5)MnO(…
The magnetic and electronic properties of Ba$_4$Ru$_3$O$_{10}$ were investigated by the ab-initio and model calculations. It is shown that nonmagnetic ground state of the one-third Ru$^{4+}$ ions is not due to the correlation effects. It is rather caused by the charge disproportionation between crystallographically different Ru and the molecular orbital formation in the Ru's trimer.
In the manganite Nd0.5Ca0.5MnO3, charge ordering occurs at much higher temperature than the antiferromagnetic order (TCO=250K,TN=160K). The magnetic behavior of the phase TN<T<TCO is puzzling: its magnetization and susceptibility are typical of an antiferromagnet while no magnetic order is detected by neutron diffraction.We have undertaken an extensive study of the cristallographic, electric and magnetic properties of Nd0.5Ca0.5MnO3 and established its phase diagram as a function of temperature and magnetic field. The charge disordered, paramagnetic phase above TCO present ferromagnetic correl…
The first-principles SIC-LSD theory is utilized to study electronic, magnetic and orbital phenomena in LaMnO$_{3}$. The correct ground state is found, which is antiferro orbitally ordered with the spin magnetic moments antiferromagnetically aligned. Jahn-Teller energies are found to be the largest energy scale. In addition it is the Jahn-Teller interaction which is the dominant effect in realising orbital order, and the electronic effects alone do not suffice.
We report on the in-plane anisotropy of the electronic response in the spin/charge/orbital ordered phase of a half-doped layered-structure manganite. The optical conductivity spectra for a single domain of Eu$_{1/2}$% Ca$_{3/2}$MnO$_{4}$ unambiguously show the anisotropic charge dynamics which well corresponds to the theoretical calculation: the optical conductivity with the polarization along the zigzag ferromagnetic chain direction exhibits a smaller gap and a larger intensity at lower energies than that of the perpendicular polarization mostly due to the charge/orbital ordering and the asso…
Combining macroscopic and diffraction methods we have studied the electric, magnetic and struc- tural properties of RE_(1-x)Ca_xTiO_3 (RE=Y, Er, Lu) focusing on the concentration range near the metal-insulator transition. The insulating phase, which is stabilized by a smaller rare-earth ionic ra- dius, exhibits charge order with a predominant occupation of the dxy orbital. The charge and orbital ordering explains the broad stability range of the insulating state in RE_(1-x)Ca_xTiO_3 with smaller rare-earth ions. The strong modulation of the Ti-O bond distances indicates sizeable modulation of …
We investigate the ground-state property of an e_g-orbital Hubbard model at quarter filling on a zigzag chain by exploiting the density matrix renormalization group method. When two orbitals are degenerate, the zigzag chain is decoupled to a doble-chain spin system to suppress the spin frustration due to the spatial anisotropy of the occupied orbital. On the other hand, when the level splitting is increased and the orbital anisotropy disappears, a characteristic change in the spin incommnsurability is observed due to the revival of the spin frustration.
The possibility of "orbitally selective Mott transitions" within a multiband Hubbard model, in which one orbital with large on-site electron-electron repulsion $U_1$ is insulating and another orbital, to which it is hybridized, with small $U_{-1}$, is metallic, is a problem of long-standing debate and investigation. In this paper we study an analogous phenomenon, the co-existence of metallic and insulating bands in a system of orbitals with different electron-phonon coupling (EPC). To this end, we examine two variants of the bilayer Holstein model: a uniform bilayer and a "Holstein-Metal inter…
Strongly anisotropic spin-orbit coupling (SOC) renormalization and strongly enhanced orbital magnetic moments are obtained in the fully self consistent approach including the orbital off-diagonal spin and charge condensates. For moderate tetragonal distortion as in $\rm Ca_2 RuO_4$, dominantly planar antiferromagnetic (AFM) order with small canting of moments in and about the crystal $c$ axis are obtained. For reduced tetragonal distortion, we find a tunable regime wherein the magnetic order can be tuned (AFM or FM) by the bare SOC strength and octahedral tilting magnitude. In this regime, wit…
A superposition of the Pauli and orbital coupling of a high magnetic field to charge carriers in a charge-density-wave (CDW) system is proposed to give rise to transitions between subphases with quantized values of the CDW wavevector. By contrast to the purely orbital field-induced density-wave effects which require a strongly imperfect nesting of the Fermi surface, the new transitions can occur even if the Fermi surface is well nested at zero field. We suggest that such transitions are observed in the organic metal $α$-(BEDT-TTF)$_2$KHg(SCN)$_4$ under a strongly tilted magnetic field.
We derive a realistic microscopic model for doped colossal magnetoresistance manganites, which includes the dynamics of charge, spin, orbital and lattice degrees of freedom on a quantum mechanical level. The model respects the SU(2) spin symmetry and the full multiplet structure of the manganese ions within the cubic lattice. Concentrating on the hole doped domain ($0\le x\le 0.5$) we study the influence of the electron-lattice interaction on spin and orbital correlations by means of exact diagonalisation techniques. We find that the lattice can cause a considerable suppression of the coupling…
Spin, charge, and orbital structures in models for doped manganites are studied by a combination of analytic mean-field and numerical relaxation techniques. At realistic values for the electron-phonon and antiferromagnetic $t_{2g}$ spin couplings, a competition between a ferromagnetic (FM) phase and a charge-orbital ordered (COO) insulating state is found for $x$=1/4, 3/8, and 1/2, as experimentally observed in Pr$_{1-x}$Ca$_{x}$MnO$_3$ for $x$=0.3$\sim$0.5. The theoretical predictions for the spin-charge-orbital ordering pattern are compared with experiments. The FM-COO energy difference is s…
The charge and orbital ordering in Pr_{0.5} Ca_{0.5} MnO_3 is studied for the first time by ^{17}O NMR. This local probe is sensitive to spin, charge and orbital correlations. Two transitions exist in this system: the charge and orbital ordering at T_{CO} = 225 K and the antiferromagnetic (AF) transition at T_N = 170 K. Both are clearly seen in the NMR spectra measured in a magnetic field of 7T. Above T_{CO} there exists only one NMR line with a large isotropic shift, whose temperature dependence is in accordance with the presence of ferromagnetic (FM) correlations. This line splits into two p…
We investigated the temperature ($T=$ 15 $\sim $ 290 K) and the magnetic field ($H=$ 0 $\sim $ 17 T) dependent optical conductivity spectra of a charge/orbital ordered manganite, Nd$_{1/2}$Sr$_{1/2}$MnO$_3$. With variation of $T$ and $H$, large spectral weight changes were observed up to 4.0 eV. These spectral weight changes could be explained using the polaron picture. Interestingly, our results suggested that some local ordered state might remain above the charge ordering temperature, and that the charge/orbital melted state at a high magnetic field (i.e. at $H=$ 17 T and $% T=$ 4.2 K) shoul…
The interlayer magnetoresistance of the low-dimensional organic metal α-(BEDT-TTF)2KHg(SCN)4 under pressure shows features which are likely associated with theoretically predicted field-induced charge-density-wave (FICDW) transitions. At ambient pressure, a magnetic field strongly tilted towards the conducting layers induces a series of hysteretic anomalies. We attribute these anomalies to a novel kind of FICDW originating from a superposition of the orbital quantization of the nesting vector and Pauli effect on the charge-density wave.
Based on the SO(2)-invariant slave-boson scheme, the static charge, orbital, and excitonic susceptibilities in the extended Falicov-Kimball model are calculated. Analyzing the phase without long-range order we find instabilities towards charge order, orbital order, and the excitonic insulator (EI) phase. The instability towards the EI is in agreement with the saddle-point phase diagram. We also evaluate the dynamic excitonic susceptibility, which allows the investigation of uncondensed excitons. We find qualitatively different features of the exciton dispersion at the semimetal-EI and at the s…
Mixed valence spinels provide a fertile playground for the interplay between charge, spin, and orbital degrees of freedom in strongly correlated electrons on a geometrically frustrated lattice. Among them, AlV$_2$O$_4$ and LiV$_2$O$_4$ exhibit contrasting and puzzling behavior: self-organization of seven-site clusters and heavy fermion behavior. We theoretically perform a comparative study of charge-spin-orbital fluctuations in these two compounds, on the basis of the multiband Hubbard models constructed by using the maximally-localized Wannier functions obtained from the ab initio band calcul…
Due to its unique structure, graphene provides a condensed-matter model of particle physics phenomena. One is the critical charge which is highly interested. The investigation of critical charge in gapped graphene is performed within single particle approach by means of Dirac equation integration. The screened Coulomb interaction between charged defect and graphene electron excitations is investigated. Two kinds of mass gap generation and various values of substrate dielectric permittivities are considered. It is shown that the critical charge phenomenon can be observed even with quite small c…
The metal-insulator transition of the Magneli phase Ti4O7 is studied by means of augmented spherical wave (ASW) electronic structure calculations as based on density functional theory and the local density approximation. The results show that the metal-insulator transition arises from a complex interplay of charge order, orbital order, and singlet formation of those Ti 3d states which mediate metal-metal bonding inside the four-atom chains characteristic of the material. Ti4O7 thus combines important aspects of Fe3O4 and VO2. While the charge ordering closely resembles that observed at the Ver…
We report a ground state with strongly coupled magnetic and charge density wave orders mediated via orbital ordering in the layered compound \tbt. In addition to the commensurate antiferromagnetic (AFM) and charge density wave (CDW) orders, new magnetic peaks are observed whose propagation vector equals the sum of the AFM and CDW propagation vectors, revealing an intricate and highly entwined relationship. This is especially interesting given that the magnetic and charge orders lie in different layers of the crystal structure where the highly localized magnetic moments of the Tb$^{3+}$ ions ar…
We present diffraction data on a single-layered manganite La(0.42)Sr(1.58)MnO4 with hole doping (x>0.5). Overdoped La(0.42)Sr(1.58)MnO4 exhibits a complex ordering of charges, orbitals and spins. Single crystal neutron diffraction experiments reveal three incommensurate and one commensurate order parameters to be tightly coupled. The position and the shape of the distinct superstructure scattering points to a stripe arrangement in which ferromagnetic zigzag chains are disrupted by additional Mn4+ stripes.
Single Crystals of Nd$_{1-x}$Ca$_{1+x}$MnO$_{4}$ have been prepared by the travelling floating-zone method, and possible evidence of a charge -orbital density wave in this material presented earlier [PRB68,092405 (2003)] using High Resolution Electron Microscopy [HRTEM] and Electron Diffraction [ED]. In the current note we present direct evidence of charge-orbital ordering in this material using heat capacity measurements. Our heat capacity measurements indicate a clear transition consistent with prior observation. We find two main transitions, one at temperature $T_{_H}=310-314$ K, and other …
In order to have a better understanding of ultrafast electrical control of exchange interactions in multi-orbital systems, we study a two-orbital Hubbard model at half filling under the action of a time-periodic electric field. Using suitable projection operators and a generalized time-dependent canonical transformation, we derive an effective Hamiltonian which describes two different regimes. First, for a wide range of non-resonant frequencies, we find a change of the bilinear Heisenberg exchange $J_{\textrm{ex}}$ that is analogous to the single-orbital case. Moreover we demonstrate that also…
We present the zero-temperature phase diagram of the one-dimensional t2g-orbital Hubbard model, obtained using the density-matrix renormalization group and Lanczos techniques. Emphasis is given to the case for the electron density n=5 corresponding to five electrons per site, of relevance for some Co-based compounds. However, several other cases for electron densities between n=3 and 6 are also studied. At n=5, our results indicate a first-order transition between a paramagnetic (PM) insulator phase and a fully-polarized ferromagnetic (FM) state by tuning the Hund's coupling. The results also …
We report an inelastic neutron scattering study of acoustic phonons in the charge and orbitally ordered bilayer manganite LaSr$_2$Mn$_2$O$_7$. For excitation energies less than $15\,\rm{meV}$, we observe an abrupt increase (decrease) of the phonon energies (linewidths) of a transverse acoustic phonon branch at $\mathbf{q} = (h, h, 0)$, $h\le0.3$, upon entering the low temperature charge and orbital ordered state ($T_{COO} = 225\,\rm{K}$). This indicates a reduced electron-phonon coupling due to a decrease of electronic states at the Fermi level leading to a partial removal of the Fermi surface…
We report a high-resolution neutron diffraction study on the orbitally-degenerate spin-1/2 hexagonal antiferromagnet AgNiO2. A structural transition to a tripled unit cell with expanded and contracted NiO6 octahedra indicates root(3) x root(3) charge order on the Ni triangular lattice. This suggests charge order as a possible mechanism of lifting the orbital degeneracy in the presence of charge fluctuations, as an alternative to Jahn-Teller distortions. A novel magnetic ground state is observed at base temperatures with the electron-rich S = 1 Ni sites arranged in alternating ferromagnetic row…
We present our theoretical results on the ground states in layered triangular-lattice compounds ANiO2 (A=Na, Li, Ag). To describe the interplay between charge, spin, orbital, and lattice degrees of freedom in these materials, we study a doubly-degenerate Hubbard model with electron-phonon couplings by the Hartree-Fock approximation combined with the adiabatic approximation. In a weakly-correlated region, we find a metallic state accompanied by \sqroot3x\sqroot3 charge ordering. On the other hand, we obtain an insulating phase with spin-ferro and orbital-ferro ordering in a wide range from inte…
Femtosecond reflection spectroscopy was performed on a perovskite-type manganite, Gd0.55Sr0.45MnO3, with the short-range charge and orbital order (CO/OO). Immediately after the photoirradiation, a large increase of the reflectivity was detected in the mid-infrared region. The optical conductivity spectrum under photoirradiation obtained from the Kramers-Kronig analyses of the reflectivity changes demonstrates a formation of a metallic state. This suggests that ferromagnetic spin arrangements occur within the time resolution (ca. 200 fs) through the double exchange interaction, resulting in an …
The temperature dependence of the electron-spin resonance linewidth in La0.95Sr0.05MnO3 has been determined and analyzed in the paramagnetic regime across the orbital ordering transition. From the temperature dependence and the anisotropy of linewidth and $g$-value the orbital order can be unambiguously determined via the mixing angle of the wave functions of the $e_{\rm g}$-doublet. The linewidth shows a similar evolution with temperature as resonant x-ray scattering results.
In a two orbital double exchange model we formulate Jahn-Teller coupled charge density wave in one electron per lattice site limit. Softening of Jahn-Teller phonons corresponding to distortion modes $Q_2$ or $Q_3$ associated with perfect nesting of Fermi surface leads to this instability at low temperature. The gap equation for charge density wave state and its dependences on electron-lattice coupling are calculated explicitly when any one of the Jahn-Teller modes is excited cooperatively. We find that the $Q_2$ distortion mode yields lowest free energy. The calculated heat capacity for each m…
The candidate magnetoelectric Pb3Mn7O15 has a structure consisting of 1/3 filled Kagome layers linked by ribbons of edge-sharing octahedra in the stacking direction. Previous reports have indicated a complex hexagonal-orthorhombic structural transition upon cooling to room temperature, although its origins are uncertain. Here both structures are revisited using a combination of neutron and synchrotron X-ray diffraction data. Large shifts of oxygen positions are detected which show that the interlayer sites and those which occupy voids in the kagome lattice are trivially charge ordered in both …
Phase diagram of half-doped perovskite manganites is studied within the extended double-exchange model. To demonstrate the role of orbital degrees of freedom both one- and two-orbital models are examined. A rich phase diagram is obtained in the mean-field theory at zero temperature as a function of J (antiferromagnetic (AFM) superexchange interaction) and V (intersite Coulomb repulsion). For the one-orbital model a charge-ordered (CO) state appears at any value of V with different types of magnetic order which changes with increasing J from ferromagnetic (F) to AFM ones of the types A, C and G…
We apply grazing-incidence femtosecond x-ray diffraction to investigate the details of the atomic motion connected with a displacively excited coherent optical phonon. We concentrate on the low frequency phonon associated with the charge and orbital order in the mixed valence manganite La0.25Pr0.375Ca0.375MnO3 for T < 210 K. We measure the response of three superlattice reflections that feature different sensitivities to the motion of the unit cell constituents. The results support the assignment to a translational mode of the Mn4+ atoms together with the oxygen atoms connecting adjacent Mn4+ …
Coupling between charge and spin, and magnetoelectric effects more generally, have been an area of great interest for several years, with the sought-after ability to control magnetic degrees of freedom via charge currents serving as an impetus. The orbital Edelstein effect (OEE) is a kinetic magnetoelectric effect consisting of a bulk orbital magnetization induced by a charge current. It is the orbital analogue of the spin Edelstein effect in spin-orbit coupled materials, in which a charge current drives nonzero electron spin magnetization. The OEE has recently been investigated in the context…
