Momentum dependence of orbital excitations in Mott-insulating titanates

High-resolution resonant inelastic x-ray scattering has been used to determine the momentum dependence of orbital excitations in Mott-insulating LaTiO$_3$ and YTiO$_3$ over a wide range of the Brillouin zone. The data are compared to calculations in the framework of lattice-driven and superexchange-driven orbital ordering models. A superexchange model in which the experimentally observed modes are attributed to two-orbiton excitations yields the best description of the data.Comment: to appear in PR

Spin-orbital excitation continuum and anomalous electron-phonon interaction in the Mott insulator LaTiO3_3

Raman scattering experiments on stoichiometric, Mott-insulating LaTiO$_3$ over a wide range of excitation energies reveal a broad electronic continuum which is featureless in the paramagnetic state, but develops a gap of $\sim 800$ cm$^{-1}$ upon cooling below the N\'eel temperature $T_N = 146$ K. In the antiferromagnetic state, the spectral weight below the gap is transferred to well-defined spectral features due to spin and orbital excitations. Low-energy phonons exhibit pronounced Fano anomalies indicative of strong interaction with the electron system for $T > T_N$, but become sharp and symmetric for $T < T_N$. The electronic continuum and the marked renormalization of the phonon lifetime by the onset of magnetic order are highly unusual for Mott insulators and indicate liquid-like correlations between spins and orbitals.Comment: to appear in Phys. Rev. Let

Orbital order and fluctuations in Mott insulators

Basic mechanisms controlling orbital order and orbital fluctuations in transition metal oxides are discussed. The lattice driven classical orbital picture, e.g. like in manganites LaMnO$_3$, is contrasted to the quantum behavior of orbitals in frustrated superexchange models as realised in pseudocubic titanites ATiO$_3$ and vanadates AVO$_3$. In YVO$_3$, the lattice and superexchange effects strongly compete -- this explains the extreme sensitivity of magnetic states to temperature and doping. Lifting the $t_{2g}$ orbital degeneracy by a relativistic spin-orbital coupling is considered on example of the layered cobaltates. We find that the spin-orbital mixing of low-energy states leads to unusual magnetic correlations in a triangular lattice of the CoO$_2$ parent compound. Finally, the magnetism of sodium-rich compounds Na$_{1-x}$CoO$_2$ is discussed in terms of a spin/orbital polaronic liquid.Comment: 48 pages, 5 figures; typos corrected, journal reference adde

Dynamics of photo-induced ferromagnetism in oxides with orbital degeneracy

By using intense coherent electromagnetic radiation, it may be possible to manipulate the properties of quantum materials very quickly, or even induce new and potentially useful phases that are absent in equilibrium. For instance, ultrafast control of magnetic dynamics is crucial for a number of proposed spintronic devices and can also shed light on the possible dynamics of correlated phases out of equilibrium. Inspired by recent experiments on spin-orbital ferromagnet YTiO3 we consider the nonequilibrium dynamics of Heisenberg ferromagnetic insulator with low-lying orbital excitations. We model the dynamics of the magnon excitations in this system following an optical pulse which resonantly excites infrared-active phonon modes. As the phonons ring down they can dynamically couple the orbitals with the low-lying magnons, leading to a dramatically modified effective bath for the magnons. We show this transient coupling can lead to a dynamical acceleration of the magnetization dynamics, which is otherwise bottlenecked by small anisotropy. Exploring the parameter space more we find that the magnon dynamics can also even completely reverse, leading to a negative relaxation rate when the pump is blue-detuned with respect to the orbital bath resonance. We therefore show that by using specially targeted optical pulses, one can exert a much greater degree of control over the magnetization dynamics, allowing one to optically steer magnetic order in this system. We conclude by discussing interesting parallels between the magnetization dynamics we find here and recent experiments on photo-induced superconductivity, where it is similarly observed that depending on the initial pump frequency, an apparent metastable superconducting phase emerges

Dynamics of photo-induced ferromagnetism in oxides with orbital degeneracy

By using intense coherent electromagnetic radiation, it may be possible to manipulate the properties of quantum materials very quickly, or even induce new and potentially useful phases that are absent in equilibrium. For instance, ultrafast control of magnetic dynamics is crucial for a number of proposed spintronic devices and can also shed light on the possible dynamics of correlated phases out of equilibrium. Inspired by recent experiments on spin-orbital ferromagnet YTiO$_3$ we consider the nonequilibrium dynamics of Heisenberg ferromagnetic insulator with low-lying orbital excitations. We model the dynamics of the magnon excitations in this system following an optical pulse which resonantly excites infrared-active phonon modes. As the phonons ring down they can dynamically couple the orbitals with the low-lying magnons, leading to a dramatically modified effective bath for the magnons. We show this transient coupling can lead to a dynamical acceleration of the magnetization dynamics, which is otherwise bottlenecked by small anisotropy. Exploring the parameter space more we find that the magnon dynamics can also even completely reverse, leading to a negative relaxation rate when the pump is blue-detuned with respect to the orbital bath resonance. We therefore show that by using specially targeted optical pulses, one can exert a much greater degree of control over the magnetization dynamics, allowing one to optically steer magnetic order in this system. We conclude by discussing interesting parallels between the magnetization dynamics we find here and recent experiments on photo-induced superconductivity, where it is similarly observed that depending on the initial pump frequency, an apparent metastable superconducting phase emerges.Comment: 16 pages, 11 figures + 5 pages, no figure

Optical Stabilization of Fluctuating High Temperature Ferromagnetism in YTiO₃

In quantum materials, degeneracies and frustrated interactions can have a profound impact on the emergence of long-range order, often driving strong fluctuations that suppress functionally relevant electronic or magnetic phases. Engineering the atomic structure in the bulk or at heterointerfaces has been an important research strategy to lift these degeneracies, but these equilibrium methods are limited by thermodynamic, elastic, and chemical constraints. Here, we show that all-optical, mode-selective manipulation of the crystal lattice can be used to enhance and stabilize high-temperature ferromagnetism in YTiO3, a material that exhibits only partial orbital polarization, an unsaturated low-temperature magnetic moment, and a suppressed Curie temperature, Tc = 27 K. The enhancement is largest when exciting a 9 THz oxygen rotation mode, for which complete magnetic saturation is achieved at low temperatures and transient ferromagnetism is realized up to Tneq> 80 K, nearly three times the thermodynamic transition temperature. First-principles and model calculations of the nonlinear phonon-orbital-spin coupling reveal that these effects originate from dynamical changes to the orbital polarization and the makeup of the lowest quasi-degenerate Ti t2g levels. Notably, light-induced high temperature ferromagnetism in YTiO3 is found to be metastable over many nanoseconds, underscoring the ability to dynamically engineer practically useful non-equilibrium functionalities

Optical Stabilization of Fluctuating High Temperature Ferromagnetism in YTiO3_3

In quantum materials, degeneracies and frustrated interactions can have a profound impact on the emergence of long-range order, often driving strong fluctuations that suppress functionally relevant electronic or magnetic phases. Engineering the atomic structure in the bulk or at heterointerfaces has been an important research strategy to lift these degeneracies, but these equilibrium methods are limited by thermodynamic, elastic, and chemical constraints. Here, we show that all-optical, mode-selective manipulation of the crystal lattice can be used to enhance and stabilize high-temperature ferromagnetism in YTiO$_3$, a material that exhibits only partial orbital polarization, an unsaturated low-temperature magnetic moment, and a suppressed Curie temperature, $T_c$ = 27 K. The enhancement is largest when exciting a 9 THz oxygen rotation mode, for which complete magnetic saturation is achieved at low temperatures and transient ferromagnetism is realized up to $T_{neq} >$ 80 K, nearly three times the thermodynamic transition temperature. First-principles and model calculations of the nonlinear phonon-orbital-spin coupling reveal that these effects originate from dynamical changes to the orbital polarization and the makeup of the lowest quasi-degenerate Ti $t_{2g}$ levels. Notably, light-induced high temperature ferromagnetism in YTiO$_3$ is found to be metastable over many nanoseconds, underscoring the ability to dynamically engineer practically useful non-equilibrium functionalities.Comment: 14 pages, 4 figure

Electronic reconstruction in correlated electron heterostructures

Electronic phase behavior in correlated-electron systems is a fundamental problem of condensed matter physics. We argue here that the change in the phase behavior near the surface and interface, i.e., {\em electronic reconstruction}, is the fundamental issue of the correlated-electron surface or interface science. Beyond its importance to basic science, understanding of this behavior is crucial for potential devices exploiting the novel properties of the correlated systems. % We present a general overview of the field, and then illustrate the general concepts by theoretical studies of the model heterostructures comprised of a Mott-insulator and a band-insulator, which show that spin (and orbital) orderings in thin heterostructures are generically different from the bulk and that the interface region, about three-unit-cell wide, is always metallic, demonstrating that {\em electronic reconstruction} generally occurs. % Predictions for photoemission experiments are made to show how the electronic properties change as a function of position, and the magnetic phase diagram is determined as a function of temperature, number of layers, and interaction strength. Future directions for research are also discussed.Comment: Proceedings of SPIE conference on Strongly Correlated Electron Materials: Physics and Nanoengineering, San Diego, CA, 31 July - 4 August, 200

Strongly correlated electrons in solids

In this review, phenomena and ideas connected with strongly interacting electrons in condensed matter systems will be outlined. A simple picture which regards electrons as basically a free gas of quantum particles is the basis of our understanding of all electronic behaviour of metals and insulators. In the last few decades, families of systems have been explored in which the interaction energy is much larger than the energy of free motion, or kinetic energy. These include transition metal oxides with unfilled d electron shells, rare earth intermetallics with f electrons, etc. Their behaviour is rich and not well understood in terms of existing paradigms. I point out some experimental features common to these, e.g. that they are ‘bad’ metals with unusually low quantum coherence temperatures. I also briefly give illustrative examples such as cuprates (which are high temperature superconductors), man-ganites (exhibiting colossal magnetoresistance) and heavy fermions (rare earth intermetallics). Some of the ideas, theories and methods available for describing these sysytems are outlined. It is suggested that a new general approach may be needed for this qualitatively different regime of many electron behaviour