Spin-orbital Mixing Research Articles

Single- and Multimagnon Dynamics in Antiferromagnetic α−Fe2O3 Thin Films

Understanding the spin dynamics in antiferromagnetic (AFM) thin films is fundamental for designing novel devices based on AFM magnon transport. Here, we study the magnon dynamics in thin films of AFM $S=5/2$ $\alpha$-Fe$_2$O$_3$ by combining resonant inelastic x-ray scattering, Anderson impurity model plus dynamical mean-field theory, and Heisenberg spin model. Below 100 meV, we observe the thickness-independent (down to 15 nm) acoustic single-magnon mode. At higher energies (100-500 meV), an unexpected sequence of equally spaced, optical modes is resolved and ascribed to $\Delta S_z = 1$, 2, 3, 4, and 5 magnetic excitations corresponding to multiple, noninteracting magnons. Our study unveils the energy, character, and momentum-dependence of single and multimagnons in $\alpha$-Fe$_2$O$_3$ thin films, with impact on AFM magnon transport and its related phenomena. From a broader perspective, we generalize the use of L-edge resonant inelastic x-ray scattering as a multispin-excitation probe up to $\Delta S_z = 2S$. Our analysis identifies the spin-orbital mixing in the valence shell as the key element for accessing excitations beyond $\Delta S_z = 1$, and up to, e.g., $\Delta S_z = 5$. At the same time, we elucidate the novel origin of the spin excitations beyond the $\Delta S_z = 2$, emphasizing the key role played by the crystal lattice as a reservoir of angular momentum that complements the quanta carried by the absorbed and emitted photons.

Hidden spin-orbital texture at the overline{{{Gamma }}}-located valence band maximum of a transition metal dichalcogenide semiconductor

Finding stimuli capable of driving an imbalance of spin-polarised electrons within a solid is the central challenge in the development of spintronic devices. However, without the aid of magnetism, routes towards this goal are highly constrained with only a few suitable pairings of compounds and driving mechanisms found to date. Here, through spin- and angle-resolved photoemission along with density functional theory, we establish how the p-derived bulk valence bands of semiconducting 1T-HfSe2 possess a local, ground-state spin texture spatially confined within each Se-sublayer due to strong sublayer-localised electric dipoles orientated along the c-axis. This hidden spin-polarisation manifests in a ‘coupled spin-orbital texture’ with in-equivalent contributions from the constituent p-orbitals. While the overall spin-orbital texture for each Se sublayer is in strict adherence to time-reversal symmetry (TRS), spin-orbital mixing terms with net polarisations at time-reversal invariant momenta are locally maintained. These apparent TRS-breaking contributions dominate, and can be selectively tuned between with a choice of linear light polarisation, facilitating the observation of pronounced spin-polarisations at the Brillouin zone centre for all kz. We discuss the implications for the generation of spin-polarised populations from 1T-structured transition metal dichalcogenides using a fixed energy, linearly polarised light source.

Room-Temperature Phosphorescence and Low-Energy Induced Direct Triplet Excitation of Alq3 Engineered Crystals.

Crystal engineering is a practical approach for tailoring material properties. This approach has been widely studied for modulating optical and electrical properties of semiconductors. However, the properties of organic molecular crystals are difficult to control following a similar engineering route. In this Letter, we demonstrate that engineered crystals of Alq3 and Ir(ppy)3 complexes, which are commonly used in organic light-emitting technologies, possess intriguing functional properties. Specifically, these structures not only process efficient low-energy induced triplet excitation directly from the ground state of Alq3 but also can show strong emission at the Alq3 triplet energy level at room temperatures. We associate these phenomena with local deformations of the host matrix around the guest molecules, which in turn lead to a stronger host-guest triplet-triplet coupling and spin-orbital mixing.

The role of spin-flip assisted or orbital mixing tunneling on transport through strongly correlated multilevel quantum dot

Using the slave boson Kotliar-Ruckenstein approach (SBMFA) for N level Anderson model, we compare fully symmetric SU(N) Kondo resonances occurring for spin and orbital conserving tunneling with many-body resonances for the dot with broken symmetry caused by spin, orbital or full spin-orbital mixing. As a result of interorbital or spin flip processes new interference paths emerge, which manifests in the occurrence of antibonding Dicke like and bonding Kondo like resonances. The analytical expressions for linear conductances and linear temperature thermopower coefficient for arbitrary N are found.

Avoided level crossing at the magnetic field induced topological phase transition due to spin-orbital mixing

A three-dimensional gapless Dirac state is expected to occur at the critical point between a topological and a trivial phase. By applying a strong magnetic field or increasing temperature, a transition from topological to trivial can be induced in the topological crystalline insulator Pb${}_{1\ensuremath{-}x}$Sn${}_{x}$Se ($x$>0.16). Using magneto-optical spectroscopy, the authors show that the critical gapless Dirac state is unstable in the case of Pb${}_{1\ensuremath{-}x}$Sn${}_{x}$Se ($x$=0.19). An avoided crossing of energy bands is observed when a topological phase transition is induced by a magnetic field or by increasing temperature. The avoided crossing is accompanied by a spin-orbital mixing of the band-edge parity. These results motivate research aimed at elucidating the mechanism behind this type of topological phase transition.

Role of Orbital Degeneracy in the Single Molecule Magnet Behavior of a Mononuclear High-Spin Fe(II) Complex

To explain the single-molecule magnet behavior of the mononuclear complex [(tpaMes)Fe](-) we have developed a model that takes into account the trigonal ligand field splitting of the atomic (5)D term of the Fe(II) ion, and the spin-orbital splitting and mixing of the ligand field terms. The ground ligand field term is shown to be the orbital doublet (5)E possessing an unquenched orbital angular momentum. We demonstrate that the splitting of this term cannot be described by the conventional zero-field splitting Hamiltonian proving thus the irrelevance of the spin-Hamiltonian formalism in the present case. The first-order orbital angular momentum is shown to lead to the strong magnetic anisotropy with the trigonal axis being the easy axis of the magnetization.

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.

Analysis of proton resonance scattering from non-zero spin targets

A practical description is given of the analysis of resonance excitation functions for proton elastic scattering from non-zero spin targets. The analysis utilizes a multilevel, multichannel formalism for unpolarized beams and targets. The effects of channel spin mixing and orbital angular momentum mixing are described in detail, as well as the determination of resonance J values. Two-level interference effects are considered for levels with the same spin and parity and with different spin or parity. Examples are provided.