Origin of the Magnetic Exciton in the van der Waals Antiferromagnet NiPS_{3}.

An ultrasharp photoluminescence line intimately related to antiferromagnetic order has been found in NiPS_{3}, a correlated van der Waals material, opening prospects for magneto-optical coupling schemes and spintronic applications. Here we unambiguously clarify the singlet origin of this excitation, confirming its roots in the spin structure. Based on a comprehensive investigation of the electronic structure using angle-resolved photoemission and q-dependent electron energy loss spectroscopy as experimental tools we develop, in a first step, an adequate theoretical understanding using density functional theory (DFT). In a second step the DFT is used as input for a dedicated multiplet theory by which we achieve excellent agreement with available multiplet spectroscopy. Our Letter connects the understanding of the electronic structure and of optical processes in NiPS_{3} and related materials as a prerequisite for further progress of the field.

Orbital Complexity in Intrinsic Magnetic Topological Insulators MnBi_{4}Te_{7} and MnBi_{6}Te_{10}.

Using angle-resolved photoelectron spectroscopy (ARPES), we investigate the surface electronic structure of the magnetic van der Waals compounds MnBi_{4}Te_{7} and MnBi_{6}Te_{10}, the n=1 and 2 members of a modular (Bi_{2}Te_{3})_{n}(MnBi_{2}Te_{4}) series, which have attracted recent interest as intrinsic magnetic topological insulators. Combining circular dichroic, spin-resolved and photon-energy-dependent ARPES measurements with calculations based on density functional theory, we unveil complex momentum-dependent orbital and spin textures in the surface electronic structure and disentangle topological from trivial surface bands. We find that the Dirac-cone dispersion of the topologial surface state is strongly perturbed by hybridization with valence-band states for Bi_{2}Te_{3}-terminated surfaces but remains preserved for MnBi_{2}Te_{4}-terminated surfaces. Our results firmly establish the topologically nontrivial nature of these magnetic van der Waals materials and indicate that the possibility of realizing a quantized anomalous Hall conductivity depends on surface termination.

Resonant inelastic x-ray incarnation of Young's double-slit experiment.

Young's archetypal double-slit experiment forms the basis for modern diffraction techniques: The elastic scattering of waves yields an interference pattern that captures the real-space structure. Here, we report on an inelastic incarnation of Young's experiment and demonstrate that resonant inelastic x-ray scattering (RIXS) measures interference patterns, which reveal the symmetry and character of electronic excited states in the same way as elastic scattering does for the ground state. A prototypical example is provided by the quasi-molecular electronic structure of insulating Ba3CeIr2O9 with structural Ir dimers and strong spin-orbit coupling. The double "slits" in this resonant experiment are the highly localized core levels of the two Ir atoms within a dimer. The clear double-slit-type sinusoidal interference patterns that we observe allow us to characterize the electronic excitations, demonstrating the power of RIXS interferometry to unravel the electronic structure of solids containing, e.g., dimers, trimers, ladders, or other superstructures.

Evolution of the Magnetic Excitations in NaOsO_{3} through its Metal-Insulator Transition.

The temperature dependence of the excitation spectrum in NaOsO_{3} through its metal-to-insulator transition (MIT) at 410 K has been investigated using resonant inelastic x-ray scattering at the Os L_{3} edge. High-resolution (ΔE∼56 meV) measurements show that the well-defined, low-energy magnons in the insulating state weaken and dampen upon approaching the metallic state. Concomitantly, a broad continuum of excitations develops which is well described by the magnetic fluctuations of a nearly antiferromagnetic Fermi liquid. By revealing the continuous evolution of the magnetic quasiparticle spectrum as it changes its character from itinerant to localized, our results provide unprecedented insight into the nature of the MIT in NaOsO_{3} [J. G. Vale, S. Calder, C. Donnerer, D. Pincini, Y. G. Shi, Y. Tsujimoto, K. Yamaura, M. M. Sala, J. van den Brink, A. D. Christianson, and D. F. McMorrow, Phys. Rev. B 97, 184429 (2018)PRBMDO2469-995010.1103/PhysRevB.97.184429].

Doping Dependence of Collective Spin and Orbital Excitations in the Spin-1 Quantum Antiferromagnet La_{2-x}Sr_{x}NiO_{4} Observed by X Rays.

We report the first empirical demonstration that resonant inelastic x-ray scattering (RIXS) is sensitive to collective magnetic excitations in S=1 systems by probing the Ni L_{3} edge of La_{2-x}Sr_{x}NiO_{4} (x=0, 0.33, 0.45). The magnetic excitation peak is asymmetric, indicating the presence of single and multi-spin-flip excitations. As the hole doping level is increased, the zone boundary magnon energy is suppressed at a much larger rate than that in hole doped cuprates. Based on the analysis of the orbital and charge excitations observed by RIXS, we argue that this difference is related to the orbital character of the doped holes in these two families. This work establishes RIXS as a probe of fundamental magnetic interactions in nickelates opening the way towards studies of heterostructures and ultrafast pump-probe experiments.

J_{eff} Description of the Honeycomb Mott Insulator α-RuCl_{3}.

Novel ground states might be realized in honeycomb lattices with strong spin-orbit coupling. Here we study the electronic structure of α-RuCl_{3}, in which the Ru ions are in a d^{5} configuration and form a honeycomb lattice, by angle-resolved photoemission, x-ray photoemission, and electron energy loss spectroscopy supported by density functional theory and multiplet calculations. We find that α-RuCl_{3} is a Mott insulator with significant spin-orbit coupling, whose low energy electronic structure is naturally mapped onto J_{eff} states. This makes α-RuCl_{3} a promising candidate for the realization of Kitaev physics. Relevant electronic parameters such as the Hubbard energy U, the crystal field splitting 10 Dq, and the charge transfer energy Δ are evaluated.

Spin-orbit-driven magnetic structure and excitation in the 5d pyrochlore Cd2Os2O7.

Much consideration has been given to the role of spin-orbit coupling (SOC) in 5d oxides, particularly on the formation of novel electronic states and manifested metal-insulator transitions (MITs). SOC plays a dominant role in 5d(5) iridates (Ir(4+)), undergoing MITs both concurrent (pyrochlores) and separated (perovskites) from the onset of magnetic order. However, the role of SOC for other 5d configurations is less clear. For example, 5d(3) (Os(5+)) systems are expected to have an orbital singlet with reduced effective SOC. The pyrochlore Cd2Os2O7 nonetheless exhibits a MIT entwined with magnetic order phenomenologically similar to pyrochlore iridates. Here, we resolve the magnetic structure in Cd2Os2O7 with neutron diffraction and then via resonant inelastic X-ray scattering determine the salient electronic and magnetic energy scales controlling the MIT. In particular, SOC plays a subtle role in creating the electronic ground state but drives the magnetic order and emergence of a multiple spin-flip magnetic excitation.

Anisotropic softening of magnetic excitations along the nodal direction in superconducting cuprates.

The high-Tc cuprate superconductors are close to antiferromagnetic order. Recent measurements of magnetic excitations have reported an intriguing similarity to the spin waves--magnons--of the antiferromagnetic insulating parent compounds, suggesting that magnons may survive in damped, broadened form throughout the phase diagram. Here we show by resonant inelastic X-ray scattering on Bi(2)Sr(2)CaCu(2)O(8+δ) (Bi-2212) that the analogy with spin waves is only partial. The magnon-like features collapse along the nodal direction in momentum space and exhibit a photon energy dependence markedly different from the Mott-insulating case. These observations can be naturally described by the continuum of charge and spin excitations of correlated electrons. The persistence of damped magnons could favour scenarios for superconductivity built from quasiparticles coupled to spin fluctuations. However, excitation spectra composed of particle-hole excitations suggest that superconductivity emerges from a coherent treatment of electronic spin and charge in the form of quasiparticles with very strong magnetic correlations.

Excitonic quasiparticles in a spin-orbit Mott insulator.

In condensed matter systems, out of a large number of interacting degrees of freedom emerge weakly coupled quasiparticles (QPs), in terms of which most physical properties are described. The lack of identification of such QPs is a major barrier for understanding myriad exotic properties of correlated electrons, such as unconventional superconductivity and non-Fermi liquid behaviours. Here we report the observation of a composite particle in a quasi-two-dimensional spin-1/2 antiferromagnet Sr2IrO4--an exciton dressed with magnons--that propagates with the canonical characteristics of a QP: a finite QP residue and a lifetime longer than the hopping time scale. The dynamics of this charge-neutral excitation mirrors the fundamental process of the analogous one-hole propagation in the background of spins-1/2, and reveals the same intrinsic dynamics that is obscured for a single, charged-hole doped into two-dimensional cuprates.

Quasi one dimensional Dirac electrons on the surface of Ru2Sn3.

We present an ARPES study of the surface states of Ru2Sn3, a new type of a strong 3D topological insulator (TI). In contrast to currently known 3D TIs, which display two-dimensional Dirac cones with linear isotropic dispersions crossing through one point in the surface Brillouin Zone (SBZ), the surface states on Ru2Sn3 are highly anisotropic, displaying an almost flat dispersion along certain high-symmetry directions. This results in quasi-one dimensional (1D) Dirac electronic states throughout the SBZ that we argue are inherited from features in the bulk electronic structure of Ru2Sn3 where the bulk conduction bands are highly anisotropic. Unlike previous experimentally characterized TIs, the topological surface states of Ru2Sn3 are the result of a d-p band inversion rather than an s-p band inversion. The observed surface states are the topological equivalent to a single 2D Dirac cone at the surface Brillouin zone.

Tuning magnetic coupling in Sr2IrO4 thin films with epitaxial strain.

We report x-ray resonant magnetic scattering and resonant inelastic x-ray scattering studies of epitaxially strained Sr2IrO4 thin films. The films were grown on SrTiO3 and (LaAlO3)0.3(Sr2AlTaO6)0.7 substrates, under slight tensile and compressive strains, respectively. Although the films develop a magnetic structure reminiscent of bulk Sr2IrO4, the magnetic correlations are extremely anisotropic, with in-plane correlation lengths significantly longer than the out-of-plane correlation lengths. In addition, the compressive (tensile) strain serves to suppress (enhance) the magnetic ordering temperature TN, while raising (lowering) the energy of the zone-boundary magnon. Quantum chemical calculations show that the tuning of magnetic energy scales can be understood in terms of strain-induced changes in bond lengths.

Role of lattice coupling in establishing electronic and magnetic properties in quasi-one-dimensional cuprates.

High resolution resonant inelastic x-ray scattering has been performed to reveal the role of lattice coupling in a family of quasi-1D insulating cuprates, Ca2+5xY2-5xCu5O10. Site-dependent low-energy excitations arising from progressive emissions of a 70 meV lattice vibrational mode are resolved for the first time, providing a direct measurement of electron-lattice coupling strength. We show that such electron-lattice coupling causes doping-dependent distortions of the Cu-O-Cu bond angle, which sets the intrachain spin exchange interactions. Our results indicate that the lattice degrees of freedom are fully integrated into the electronic behavior in low-dimensional systems.

Large spin-wave energy gap in the bilayer iridate Sr3Ir2O7: evidence for enhanced dipolar interactions near the mott metal-insulator transition.

Using resonant inelastic x-ray scattering, we observe in the bilayer iridate Sr3Ir2O7, a spin-orbit coupling driven magnetic insulator with a small charge gap, a magnon gap of ≈92 meV for both acoustic and optical branches. This exceptionally large magnon gap exceeds the total magnon bandwidth of ≈70 meV and implies a marked departure from the Heisenberg model, in stark contrast to the case of the single-layer iridate Sr2IrO4. Analyzing the origin of these observations, we find that the giant magnon gap results from bond-directional pseudodipolar interactions that are strongly enhanced near the metal-insulator transition boundary. This suggests that novel magnetism, such as that inspired by the Kitaev model built on the pseudodipolar interactions, may emerge in small charge-gap iridates.

Universal recovery of the energy-level degeneracy of bright excitons in InGaAs quantum dots without a structure symmetry.

The lack of structural symmetry which usually characterizes semiconductor quantum dots lifts the energetic degeneracy of the bright excitonic states and hampers severely their use as high-fidelity sources of entangled photons. We demonstrate experimentally and theoretically that it is always possible to restore the excitonic degeneracy by the simultaneous application of large strain and electric fields. This is achieved by using one external perturbation to align the polarization of the exciton emission along the axis of the second perturbation, which then erases completely the energy splitting of the states. This result, which holds for any quantum dot structure, highlights the potential of combining complementary external fields to create artificial atoms meeting the stringent requirements posed by scalable semiconductor-based quantum technology.

Spin excitations in a single La2CuO4 layer.

Cuprates and other high-temperature superconductors consist of two-dimensional layers that are crucial to their properties. The dynamics of the quantum spins in these layers lie at the heart of the mystery of the cuprates. In bulk cuprates such as La(2)CuO(4), the presence of a weak coupling between the two-dimensional layers stabilizes a three-dimensional magnetic order up to high temperatures. In a truly two-dimensional system however, thermal spin fluctuations melt long-range order at any finite temperature. Here, we measure the spin response of isolated layers of La(2)CuO(4) that are only one-unit-cell-thick. We show that coherent magnetic excitations, magnons, known from the bulk order, persist even in a single layer of La(2)CuO(4), with no evidence for more complex correlations such as resonating valence bond correlations. These magnons are, therefore, well described by spin-wave theory (SWT). On the other hand, we also observe a high-energy magnetic continuum in the isotropic magnetic response that is not well described by two-magnon SWT, or indeed any existing theories.

Dimensionality driven spin-flop transition in layered iridates.

Using resonant x-ray diffraction, we observe an easy c-axis collinear antiferromagnetic structure for the bilayer Sr3Ir2O7, a significant contrast to the single layer Sr2IrO4 with in-plane canted moments. Based on a microscopic model Hamiltonian, we show that the observed spin-flop transition as a function of number of IrO2 layers is due to strong competition among intra- and interlayer bond-directional pseudodipolar interactions of the spin-orbit entangled J(eff)=1/2 moments. With this we unravel the origin of anisotropic exchange interactions in a Mott insulator in the strong spin-orbit coupling regime, which holds the key to the various types of unconventional magnetism proposed in 5d transition metal oxides.

Magnetic excitation spectra of Sr2IrO4 probed by resonant inelastic x-ray scattering: establishing links to cuprate superconductors.

We used resonant inelastic x-ray scattering to reveal the nature of magnetic interactions in Sr2IrO4, a 5d transition-metal oxide with a spin-orbit entangled ground state and J(eff)=1/2 magnetic moments. The magnon dispersion in Sr2IrO4 is well-described by an antiferromagnetic Heisenberg model with an effective spin one-half on a square lattice, which renders the low-energy effective physics of Sr2IrO4 much akin to that in superconducting cuprates. This point is further supported by the observation of exciton modes in Sr2IrO4, whose dispersion is strongly renormalized by magnons, which can be understood by analogy to hole propagation in the background of antiferromagnetically ordered spins in the cuprates.

Spin-orbital separation in the quasi-one-dimensional Mott insulator Sr2CuO3.

When viewed as an elementary particle, the electron has spin and charge. When binding to the atomic nucleus, it also acquires an angular momentum quantum number corresponding to the quantized atomic orbital it occupies. Even if electrons in solids form bands and delocalize from the nuclei, in Mott insulators they retain their three fundamental quantum numbers: spin, charge and orbital. The hallmark of one-dimensional physics is a breaking up of the elementary electron into its separate degrees of freedom. The separation of the electron into independent quasi-particles that carry either spin (spinons) or charge (holons) was first observed fifteen years ago. Here we report observation of the separation of the orbital degree of freedom (orbiton) using resonant inelastic X-ray scattering on the one-dimensional Mott insulator Sr2CuO3. We resolve an orbiton separating itself from spinons and propagating through the lattice as a distinct quasi-particle with a substantial dispersion in energy over momentum, of about 0.2 electronvolts, over nearly one Brillouin zone.

Antidepressants reduce extinction-induced withdrawal and biting behaviors: a model for depressive-like behavior.

The withholding of expected rewards results in extinction of behavior and, hypothetically, to depression-like symptoms. In a test of this hypothesis, we examined the effects of extinction of food-reinforced lever-pressing on collateral behaviors that might be indices of depression. Operant extinction is known to be aversive to the organism and results in avoidance behavior. We hypothesized that avoidance of, or withdrawal from, the former source of reward may serve as a marker for "despair." Adult male Wistar rats (n=6-7 animals per group) were exposed to a Skinner box attached to a second compartment of the same size, providing opportunity for the animals to leave the operant chamber and to enter the "withdrawal" compartment. The animals spent a portion of the time during the extinction trials in this second chamber. To assess the predictive validity of this behavior as a potential marker of "despair," we tested the effects of chronic administration of two common antidepressant drugs on this measure. The tricyclic antidepressant imipramine (20 mg/kg) as well as the selective serotonin reuptake inhibitor citalopram (20 mg/kg) reduced the number of entries and time spent in the withdrawal compartment. We propose that entries into and time spent in the withdrawal compartment may operationalize "avoidance," a core symptom of major depression. Rearing as well as biting behaviors during the extinction trials were also attenuated by the antidepressant treatment. These results lend support to the hypothesis that extinction of positively reinforced operants evokes behaviors that reflect elements of "despair/depression" because these behaviors are modulated by antidepressant treatment. The avoidance of the operant chamber as a consequence of extinction, together with rearing and biting behaviors, may serve as useful measures for the testing of antidepressant treatments.

Delta doping of ferromagnetism in antiferromagnetic manganite superlattices.

We demonstrate that delta doping can be used to create a dimensionally confined region of metallic ferromagnetism in an antiferromagnetic (AFM) manganite host, without introducing any explicit disorder due to dopants or frustration of spins. Theoretical consideration of these additional carriers shows that they cause a local enhancement of ferromagnetic double exchange with respect to AFM superexchange, resulting in local canting of the AFM spins. This leads to a highly modulated magnetization, as measured by polarized neutron reflectometry. The spatial modulation of the canting is related to the spreading of charge from the doped layer and establishes a fundamental length scale for charge transfer, transformation of orbital occupancy, and magnetic order in these manganites. Furthermore, we confirm the existence of the canted, AFM state as was predicted by de Gennes [Phys. Rev. 118, 141 (1960)] but had remained elusive.