Photo-induced switching between collective quantum states of matter is a fascinating rising field with exciting opportunities for novel technologies. Presently very intensively studied examples in this regard are nanometer-thick single crystals of the layered material 1T-TaS2, where picosecond laser pulses can trigger a fully reversible insulator-to-metal transition (IMT). This IMT is believed to be connected to the switching between metastable collective quantum states, but the microscopic nature of this so-called hidden quantum state remained largely elusive up to now. Here we determine the latter by means of state-of-the-art x-ray diffraction and show that the laser-driven IMT involves a marked rearrangement of the charge and orbital order in the direction perpendicular to the TaS2layers. More specifically, we identify the collapse of inter-layer molecular orbital dimers, which are a characteristic feature of the insulating phase, as a key mechanism for the non-thermal IMT in 1T-TaS2, which indeed involves a collective transition between two truly long-range ordered electronic crystals.The layered transition metal dichalcogenides (TMDs) form a vast class of materials hosting diverse non-trivial quantum phenomena such as spin-valley polarization [1], Ising-superconductivity [2] or intertwined electronic orders [3,4]. All these intriguing electronic effects along with the natural suitability of TMDs for the preparation of quasi two-dimensional (2D) nano-sheets render them highly appealing for next-generation technologies [5][6][7][8].1T-TaS 2 is a particularly interesting and extensively studied TMD in which external tuning parameters like temperature, pressure or chemical substitution span a particularly complex electronic phase diagram. Apart from several charge density waves (CDWs) this phase diagram also features pressure-induced superconductivity and a so-called Mott-phase, which stands out due to its semiconducting electronic transport properties [3,9].Remarkably, besides the aforementioned states that can be reached in thermal equilibrium, femto to picosecond optical or electrical pulses can launch a nonequilibrium IMT into a previously hidden and persistent metallic CDW-state [7,10,11]. The discovery of this so-called hidden CDW (HCDW) has sparked wide excitement as it might provide a new platform for memory device applications. Accordingly, in recent years, a significant number of experimental and theoretical studies aimed at pinning down the microscopic mechanism of this non-equilibrium IMT that is believed to be connected to a reorganization of the CDW-order. However, despite significant efforts to determine the microscopic processes underlying this novel IMT have been made [12][13][14][15][16][17], a clear picture remains elusive.In this article we address this open issue directly by means of high-resolution synchrotron x-ray diffraction (XRD) in combination with laser pumping. Our experiments enable examination of the laser-driven transition and in-particular the HCDW-order in 1T-TaS 2 nanosheets wi...
Magnetization and high-resolution x-ray diffraction measurements of the Kitaev-Heisenberg material α-RuCl 3 reveal a pressure-induced crystallographic and magnetic phase transition at a hydrostatic pressure of p ∼ 0.2 GPa. This structural transition into a triclinic phase is characterized by a very strong dimerization of the Ru-Ru bonds, accompanied by a collapse of the magnetic susceptibility. Ab initio quantum-chemistry calculations disclose a pressure-induced enhancement of the direct 4d-4d bonding on particular Ru-Ru links, causing a sharp increase of the antiferromagnetic exchange interactions. These combined experimental and computational data show that the Kitaev spin-liquid phase in α-RuCl 3 strongly competes with the crystallization of spin singlets into a valence bond solid. DOI: 10.1103/PhysRevB.97.241108 The Kitaev model on a honeycomb lattice has grown into a hot topic in the last decade due to its exact solubility and its quantum spin-liquid ground state, which would be relevant for, e.g., quantum computing [1,2]. It implies a bonddependent compass-type coupling K and strong intrinsic spin frustration [3]. A crucial ingredient for realizing the Kitaev model in real materials is a strong spin-orbit coupling together with a honeycomb structure. Recently, Kitaev interactions were identified in α-RuCl 3 , from its unusual magnetic excitation spectrum [4,5], its strong magnetic anisotropy [6], and electronic-structure calculations [7,8], which render this material an ideal platform for exploring Kitaev magnetism experimentally.α-RuCl 3 is a j eff = 1/2 Mott insulator with a twodimensional (2D) layered structure of edge-sharing RuCl 6 octahedra forming a honeycomb lattice. At ambient pressure, * g.bastien@ifw-dresden.de Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.the honeycomb layers are arranged in a monoclinic (C2/m) structure at room temperature with one of the three nearestneighbor (NN) Ru-Ru bonds slightly shorter than the other two [9]. A structural phase transition was reported at T S 60 K under cooling and T S 166 K upon warming, but the low-temperature crystal structure is still under debate and could be either rhombohedral (R3) [10,11] or monoclinic (C2/m) [12,13]. The onset of long-range magnetic order at T N 7 K [9] in α-RuCl 3 implies that other magnetic interactions have to be considered in addition to the Kitaev interaction K: a NN Heisenberg J , an off-diagonal coupling , as well as next-NN interactions J 2 and J 3 [7,8,14,15]. While electronic-structure calculations indicate that K is ferromagnetic in α-RuCl 3 and indeed defines the largest exchange energy scale [7,8,14,15], the debate on the minimal effective spin model and precise magnitude of the different couplings is not fully settled yet. By applying a magnetic field in the basal plane, the magnetic zigzag ground sta...
We present a combined experimental and theoretical study of the elementary magnetic excitations in Ba 2 YIrO 6 and Sr 2 YIrO 6-the two most intensively discussed candidates for a new type of magnetic instability caused by exciton condensation. For both materials, high-resolution resonant inelastic x-ray scattering (RIXS) at the Ir L 3 edge reveals sharp excitations around 370 and 650 meV energy loss, which we identify as triplet and quintet spin-orbit excitons. While the momentum-dependent RIXS spectra reveal that both the triplet and the quintet propagate coherently within the nonmagnetic background of the singlet sites, these modes remain fully gapped. The Ir-Ir exchange interactions in both double perovskites are therefore not strong enough to overcome the magnetic gap and, hence, our results exclude an intrinsic magnetic instability due to a condensation of magnetic excitations for both Ba 2 YIrO 6 and Sr 2 YIrO 6 .
The varied electronic localization of rare earth elements is essential to functional materials and a key to tailoring their properties. We establish with unprecedented spectral resolution the excitonic nature of the lanthanum 5p54f1 3D1 and 3D2 final states of resonant inelastic X-ray scattering (RIXS) at the La N4,5 edges. We extract the intrinsic lifetime, energy distance, and relative intensity ratio from single crystal LaAlO3 and construct an empirical model. With help of the model, we precisely determine the RIXS 3D1 final state position and identify La 5p as a descriptor of covalency with the host material. For metallic lanthanum, La3+ ions in mixed-covalent-ionic simple oxides and phosphates, and ionic salts alike, we find a sizable chemical shift, indicating band-like and free-ion-like La. The different electronic relaxation of the La 5p5 hole and the La 4f1 electron is discussed with local and nonlocal screening contributions. In addition, the energetics of the excitonic La 5p54f1 Coulomb attraction is quantified in its variation from lanthanum metal to mixed-covalent-ionic La2O3 and the ionic LaF3 salt. The power of the approach and analysis is applied to map the influence of geometric quantum confinement to La 5p sharing within quantum dots and quantum wires in comparison to bulk-like microrods of monoclinic LaPO4.
Doped IrTe2 is considered a platform for topological superconductivity and therefore receives currently a lot of interest. In addition, the superconductivity in these materials exists in close vicinity to electronic order and the formation of molecular orbital crystals, which we explore here by means of high-pressure single crystal x-ray diffraction in combination with density functional theory. Our crystallographic refinements provide detailed information about the structural evolution as a function of applied pressure up to 42 GPa. Using this structural information for density functional theory calculations, we show that the local multicenter bonding in IrTe2 is driven by changes in the Ir-Te-Ir bond angle. When the electronic order sets in, this bond angle decreases drastically, leading to a stabilization of a multicenter molecular orbital bond. This unusual local mechanism of bond formation in an itinerant material provides a natural explanation for the different electronic orders in IrTe2. It further illustrates the strong coupling of the electrons with the lattice and is most likely relevant for the superconductivity in this material.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.
hi@scite.ai
10624 S. Eastern Ave., Ste. A-614
Henderson, NV 89052, USA
Copyright © 2024 scite LLC. All rights reserved.
Made with 💙 for researchers
Part of the Research Solutions Family.