Electronically highly cubic conditions for Ru in alpha-RuCl3

We studied the local Ru 4d electronic structure of alpha-RuCl3 by means of polarization dependent x-ray absorption spectroscopy at the Ru-L2,3 edges. We observed a vanishingly small linear dichroism indicating that electronically the Ru 4d local symmetry is highly cubic. Using full multiplet cluster calculations we were able to reproduce the spectra excellently and to extract that the trigonal splitting of the t2g orbitals is -12 $\pm10$ meV, i.e. negligible as compared to the Ru 4d spin-orbit coupling constant. Consistent with our magnetic circular dichroism measurements, we found that the ratio of the orbital and spin moments is 2.0, the value expected for a Jeff = 1/2 ground state. We have thus shown that as far as the Ru 4d local properties are concerned, alpha-RuCl3 is an ideal candidate for the realization of Kitaev physics

Whole-nanoparticle atomistic modelling of the schwertmannite structure from total scattering data

Schwertmannite is a poorly crystalline nanometric iron sulfate oxyhydroxide. This mineral shows a structural variability under different environments. Because of that, the determination of its structure and, consequently, of its physical–chemical properties is quite challenging. This article presents a detailed structural investigation of the structure of schwertmannite conducted under different approaches: X-ray absorption spectroscopy, Rietveld refinement, and a combined reverse Monte Carlo and Debye function analysis of the whole nanoparticle structure. The schwertmannite model presented here is, to the auhors' knowledge, the most complete model so far reported.This work has been supported by a grant from Labex OSUG@2020 (Investissements d'avenir - ANR10 LABX56). SC was partially funded by a 'Nano Espagne' fellowship (Campus France)

Van der Waals epitaxy growth of 2D ferromagnetic Cr_(1+δ)Te₂ nanolayers with concentration-tunable magnetic anisotropy

Cr(1+δ)Te2 are pseudo-layered compounds consisting of CrTe2 transition metal dichalcogenide (TMD) layers with additional (δ) self-intercalated Cr atoms. The recent search for ferromagnetic 2D materials revived the interest into chromium tellurides. Here, Cr(1+δ)Te2 nanolayers are epitaxially grown on MoS2 (0001), forming prototypical van der Waals heterostructures. Under optimized growth conditions, ultrathin films of only two TMD layers with a single intercalated Cr-layer are achieved, forming a 2D sheet with van der Waals surfaces. Detailed compositional and structural characterization by scanning tunneling microscopy, grazing incidence x-ray diffraction, and high-resolution Rutherford backscattering indicate the layer-by-layer growth and that the δ can be tuned by post-growth annealing in a range between ∼0.5 and 1. X-ray magnetic circular dichroism and magnetometry measurements demonstrate that all self-intercalated Cr(1+δ)Te2 nanolayers exhibit strong ferromagnetism with magnetic moments larger than 3μB per Cr-atom. The magnetic properties are maintained in the ultrathin limit of a material with a single intercalation layer. Interestingly, the magnetic anisotropy can be tuned from close to isotropic (δ = 1) to a desirable perpendicular anisotropy for low δ values. Thus, the bottom-up growth of these 2D Cr(1+δ)Te2 sheets is a promising approach for designing magnetic van der Waals heterostructures

Absence of magnetic-proximity effect at the interface of Bi2_2Se3_3 and (Bi,Sb)2_2Te3_3 with EuS

We performed x-ray magnetic circular dichroism (XMCD) measurements on heterostructures comprising topological insulators (TIs) of the (Bi,Sb)$_2$(Se,Te)$_3$ family and the magnetic insulator EuS. XMCD measurements allow us to investigate element-selective magnetic proximity effects at the very TI/EuS interface. A systematic analysis reveals that there is neither significant induced magnetism within the TI nor an enhancement of the Eu magnetic moment at such interface. The induced magnetic moments in Bi, Sb, Te, and Se sites are lower than the estimated detection limit of the XMCD measurements of $\sim\!10^{-3}$ $\mu_\mathrm{B}$/at.Comment: 7 pages, 3 figures, published in Physical Review Letter

Systematics of electronic and magnetic properties in the transition metal doped Sb2_2Te3_3 quantum anomalous Hall platform

The quantum anomalous Hall effect (QAHE) has recently been reported to emerge in magnetically-doped topological insulators. Although its general phenomenology is well established, the microscopic origin is far from being properly understood and controlled. Here we report on a detailed and systematic investigation of transition-metal (TM)-doped Sb$_2$Te$_3$. By combining density functional theory (DFT) calculations with complementary experimental techniques, i.e., scanning tunneling microscopy (STM), resonant photoemission (resPES), and x-ray magnetic circular dichroism (XMCD), we provide a complete spectroscopic characterization of both electronic and magnetic properties. Our results reveal that the TM dopants not only affect the magnetic state of the host material, but also significantly alter the electronic structure by generating impurity-derived energy bands. Our findings demonstrate the existence of a delicate interplay between electronic and magnetic properties in TM-doped TIs. In particular, we find that the fate of the topological surface states critically depends on the specific character of the TM impurity: while V- and Fe-doped Sb$_2$Te$_3$ display resonant impurity states in the vicinity of the Dirac point, Cr and Mn impurities leave the energy gap unaffected. The single-ion magnetic anisotropy energy and easy axis, which control the magnetic gap opening and its stability, are also found to be strongly TM impurity-dependent and can vary from in-plane to out-of-plane depending on the impurity and its distance from the surface. Overall, our results provide general guidelines for the realization of a robust QAHE in TM-doped Sb$_2$Te$_3$ in the ferromagnetic state.Comment: 40 pages, 13 figure

Reversal of anomalous Hall effect and octahedral tilting in SrRuO₃ thin films via hydrogen spillover

The perovskite SrRuO3 (SRO) is a strongly correlated oxide whose physical and structural properties are strongly intertwined. Notably, SRO is an itinerant ferromagnet that exhibits a large anomalous Hall effect (AHE) whose sign can be readily modified. Here, a hydrogen spillover method is used to tailor the properties of SRO thin films via hydrogen incorporation. It is found that the magnetization and Curie temperature of the films are strongly reduced and, at the same time, the structure evolves from an orthorhombic to a tetragonal phase as the hydrogen content is increased up to ≈0.9 H per SRO formula unit. The structural phase transition is shown, via in situ crystal truncation rod measurements, to be related to tilting of the RuO6 octahedral units. The significant changes observed in magnetization are shown, via density functional theory (DFT), to be a consequence of shifts in the Fermi level. The reported findings provide new insights into the physical properties of SRO via tailoring its lattice symmetry and emergent physical phenomena via the hydrogen spillover technique

Control of oxygen vacancy ordering in brownmillerite thin films via ionic liquid gating

Oxygen defects and their atomic arrangements play a significant role in the physical properties of many transition metal oxides. The exemplary perovskite SrCoO3-δ (P-SCO) is metallic and ferromagnetic. However, its daughter phase, the brownmillerite SrCoO2.5 (BM-SCO), is insulating and an antiferromagnet. Moreover, BM-SCO exhibits oxygen vacancy channels (OVCs) that in thin films can be oriented either horizontally (H-SCO) or vertically (V-SCO) to the film’s surface. To date, the orientation of these OVCs has been manipulated by control of the thin film deposition parameters or by using a substrate-induced strain. Here, we present a method to electrically control the OVC ordering in thin layers via ionic liquid gating (ILG). We show that H-SCO (antiferromagnetic insulator, AFI) can be converted to P-SCO (ferromagnetic metal, FM) and subsequently to V-SCO (AFI) by the insertion and subtraction of oxygen throughout thick films via ILG. Moreover, these processes are independent of substrate-induced strain which favors formation of H-SCO in the as-deposited film. The electric-field control of the OVC channels is a path toward the creation of oxitronic devices