arXiv subjects

E. Schierle

Publications and source records attributed to E. Schierle.

At least 19 recordsLinked to original sources

arXiv2026

From perovskite to infinite-layer nickelates: hole concentration from x-ray absorption

The difficulty of determining cation concentrations and oxygen stoichiometry in infinite-layer nickelate thin films has so far prevented clear experimental identification of the nickel electron configuration in the superconducting phase. We used soft x-ray absorption spectroscopy to study the successive changes in PrNiO$_x$ thin films at various intermediate stages of topotactic reduction with $x=2-3$. By comparing the Ni-$L$ edge spectra to single and double cluster ligand-field calculations, we find that none of our samples exhibit a pure $d^9$ configuration. Our quantitative analysis using the charge sum rule shows that even when films are maximally reduced, the averaged number of nickel $3d$ holes is 1.35. Superconducting samples have even higher values, calling into question the previously assumed limit of hole doping. Concomitant changes in the oxygen $K$-edge absorption spectra upon reduction indicate the presence of oxygen $2p$ holes, even in the most reduced films. Overall, our results suggest a complex interplay of hole doping mechanisms resulting from self-doping effects and oxygen non-stoichiometry.

cond-mat.supr-con↗

arXiv2025

Nodeless Hybridization as Proof of Trivial Topology in Samarium Hexaboride

Calculations unanimously predict samarium hexaboride to be a topological Kondo insulator, the first topological insulator driven by strong electron correlation. As of today it appears also experimentally established as the only representative of this material class. Here, we investigate the three-dimensional band structure of SmB$_6$ and show that it is incompatible with a topological Kondo insulator which must have hybridization nodes at high-symmetry points. In addition we clarify the remaining questions concerning the nature of the surface states with new data. We address consequences for the search for correlated topological insulators.

cond-mat.str-el↗

arXiv2025

Resonant x-ray scattering study of charge-density wave correlations in YBa$_{2}$Cu$_{3}$O$_{6+x}$ under uniaxial stress

We report a comprehensive study of the uniaxial stress response of charge-density-wave (CDW) correlations in detwinned single crystals of the high temperature superconductor YBa$_2$Cu$_3$O$_{6+x}$ (YBCO$_{6+x}$) with $0.40 \leq x \leq 0.93$ (hole-doping levels $0.072 \leq p \leq 0.168$) by means of Cu $L_3$-edge resonant energy-integrated x-ray scattering (REXS). We show that the influence of uniaxial stress is strongly doping dependent: the quasi-two-dimensional CDW is enhanced by in-plane uniaxial stress in a wide hole doping range ($0.45 \leq x \leq 0.80$), but only barely affected in the most underdoped and optimally doped samples ($x = 0.40$ and 0.93), where the CDW correlation length is minimal. A stress-induced three-dimensionally long-range ordered (3D) CDW was observed only in YBCO$_{6.50}$ and YBCO$_{6.67}$. The temperature dependence of the 3D CDW clearly indicates a strong competition with superconductivity. Based on the systematic strain-, doping-, and temperature-dependent REXS measurements reported here, we discuss the relationship between charge order and superconductivity in YBCO$_{6+x}$ and other cuprates.

cond-mat.supr-con↗

arXiv2025

Oxygen sublattice disorder and valence state modulation in infinite-layer nickelate superlattices

The family of infinite-layer nickelates promises important insights into the mechanism of unconventional superconductivity. Since superconductivity has so far only been observed in epitaxial thin films, heteroepitaxy with the substrate or a capping layer possibly plays an important role. Here, we use soft x-ray spectroscopy to investigate superlattices as a potential approach for a targeted material design of high-temperature superconductors. We observe modulations in valence state and oxygen coordination in topotactically reduced artificial superlattices with repeating interfaces between nickelate layers and layers of materials commonly used as substrates and capping layers. Our results show that depending on the interlayer material metallic conductivity akin to the parent infinite-layer compounds is achieved. Depth-resolved electronic structure measured by resonant x-ray reflectivity reveals a reconstructed ligand field and valence state at the interface, which is confined to one or two unit cells. The central layers show characteristics of monovalent nickel, but linear dichroism analysis reveals considerable disorder in the oxygen removal sites. We observe a quantitative correlation of this disorder with the interlayer material that is important for future modeling and design strategies.

cond-mat.supr-con↗

arXiv2023

Signature of quantum criticality in cuprates by charge density fluctuations

The universality of the strange metal phase in many quantum materials is often attributed to the presence of a quantum critical point (QCP), a zero-temperature phase transition ruled by quantum fluctuations. In cuprates, where superconductivity hinders direct QCP observation, indirect evidence comes from the identification of fluctuations compatible with the strange metal phase. Here we show that the recently discovered charge density fluctuations (CDF) possess the right properties to be associated to a quantum phase transition. Using resonant x-ray scattering, we studied the CDF in two families of cuprate superconductors across a wide doping range (up to $p$=0.22). At $p^*\approx$0.19, the putative QCP, the CDF intensity peaks, and the characteristic energy $Δ$ is minimum, marking a wedge-shaped region in the phase diagram indicative of a quantum critical behavior, albeit with anomalies. These findings strengthen the role of charge order in explaining strange metal phenomenology and provide insights into high-temperature superconductivity.

cond-mat.supr-con↗

arXiv2021

Search for enhanced magnetism at the interface between Bi$_2$Se$_3$ and EuSe

Enhanced magnetism has recently been reported for the topological-insulator/ferromagnet interface Bi$_2$Se$_3$/EuS with Curie temperatures claimed to be raised above room temperature from the bulk EuS value of 16 K. Here we investigate the analogous interface Bi$_2$Se$_3$/EuSe. EuSe is a low-temperature layered ferrimagnet that is particularly sensitive to external perturbations. We find that superconducting quantum interference device (SQUID) magnetometry of Bi$_2$Se$_3$/EuSe heterostructures reveals precisely the magnetic phase diagram known from EuSe, including the ferrimagnetic phase below 5 K, without any apparent changes from the bulk behavior. Choosing a temperature of 10 K to search for magnetic enhancement, we determine an upper limit for a possible magnetic coercive field of 3 mT. Using interface sensitive x-ray absorption spectroscopy we verify the magnetic divalent configuration of the Eu at the interface without contamination by Eu3+, and by x-ray magnetic circular dichroism (XMCD) we confirm at the interface the magnetic hysteresis obtained by SQUID. XMCD data obtained at 10 K in a magnetic field of 6 T indicate a magnetic spin moment of mz,spin = 7 $μ$B/Eu$^{2+}$, in good agreement with the SQUID data and the expected theoretical moment of Eu2+. Subsequent XMCD measurements in zero field show, however, that sizable remanent magnetization is absent at the interface for temperatures down to about 10 K.

cond-mat.str-el↗

arXiv2021

A superlattice approach to doping infinite-layer nickelates

The recent observation of superconductivity in infinite-layer Nd$_{1-x}$Sr$_x$NiO$_2$ thin films has attracted a lot of attention, since this compound is electronically and structurally analogous to the superconducting cuprates. Due to the challenges in the phase stabilization upon chemical doping with Sr, we synthesized artificial superlattices of LaNiO$_3$ embedded in insulating LaGaO$_3$, and used layer-selective topotactic reactions to reduce the nickelate layers to LaNiO$_{2}$. Hole doping is achieved via interfacial oxygen atoms and tuned via the layer thickness. We used electrical transport measurements, transmission electron microscopy, and x-ray spectroscopy together with ab initio calculations to track changes in the local nickel electronic configuration upon reduction and found that these changes are reversible. Our experimental and theoretical data indicate that the doped holes are trapped at the interfacial quadratic pyramidal Ni sites. Calculations for electron-doped cases predict a different behavior, with evenly distributed electrons among the layers, thus opening up interesting perspectives for interfacial doping of transition metal oxides.

cond-mat.supr-con↗

arXiv2021

Mn-rich MnSb2Te4: A topological insulator with magnetic gap closing at high Curie temperatures of 45-50 K

Ferromagnetic topological insulators exhibit the quantum anomalous Hall effect that might be used for high precision metrology and edge channel spintronics. In conjunction with superconductors, they could host chiral Majorana zero modes which are among the contenders for the realization of topological qubits. Recently, it was discovered that the stable 2+ state of Mn enables the formation of intrinsic magnetic topological insulators with A1B2C4 stoichiometry. However, the first representative, MnBi2Te4, is antiferromagnetic with 25 K Néel temperature and strongly n-doped. Here, we show that p-type MnSb2Te4, previously considered topologically trivial, is a ferromagnetic topological insulator in the case of a few percent of Mn excess. It shows (i) a ferromagnetic hysteresis with record high Curie temperature of 45-50 K, (ii) out-of-plane magnetic anisotropy and (iii) a two-dimensional Dirac cone with the Dirac point close to the Fermi level which features (iv) out-of-plane spin polarization as revealed by photoelectron spectroscopy and (v) a magnetically induced band gap that closes at the Curie temperature as demonstrated by scanning tunneling spectroscopy. Moreover, it displays (vi) a critical exponent of magnetization beta~1, indicating the vicinity of a quantum critical point. Ab initio band structure calculations reveal that the slight excess of Mn that substitutionally replaces Sb atoms provides the ferromagnetic interlayer coupling. Remaining deviations from the ferromagnetic order, likely related to this substitution, open the inverted bulk band gap and render MnSb2Te4 a robust topological insulator and new benchmark for magnetic topological insulators.

cond-mat.mtrl-sci↗

arXiv2021

Dynamic electron correlations with charge order wavelength along all directions in the copper oxide plane

In strongly correlated systems the strength of Coulomb interactions between electrons, relative to their kinetic energy, plays a central role in determining their emergent quantum mechanical phases. We perform resonant x-ray scattering on Bi$_2$Sr$_2$CaCu$_2$O$_{8+δ}$, a prototypical cuprate superconductor, to probe electronic correlations within the CuO$_2$ plane. We discover a dynamic quasi-circular pattern in the $x$-$y$ scattering plane with a radius that matches the wave vector magnitude of the well-known static charge order. Along with doping- and temperature-dependent measurements, our experiments reveal a picture of charge order competing with superconductivity where short-range domains along $x$ and $y$ can dynamically rotate into any other in-plane direction. This quasi-circular spectrum, a hallmark of Brazovskii-type fluctuations, has immediate consequences to our understanding of rotational and translational symmetry breaking in the cuprates. We discuss how the combination of short- and long-range Coulomb interactions results in an effective non-monotonic potential that may determine the quasi-circular pattern.

cond-mat.supr-con↗

arXiv2020

Large response of charge stripes to uniaxial stress in $\textrm{La}_{1.475}\textrm{Nd}_{0.4}\textrm{Sr}_{0.125}\textrm{Cu}\textrm{O}_{4}$

The La-based '214' cuprates host several symmetry breaking phases including superconductivity, charge and spin order in the form of stripes, and a structural othorhombic-to-tetragonal phase transition. Therefore, these materials are an ideal system to study the effects of uniaxial stress onto the various correlations that pervade the cuprate phase diagram. We report resonant x-ray scattering experiments on $\textrm{La}_{1.475}\textrm{Nd}_{0.4}\textrm{Sr}_{0.125}\textrm{Cu}\textrm{O}_{4}$ (LNSCO-125) that reveal a significant response of charge stripes to uniaxial tensile-stress of $\sim$ 0.1 GPa. These effects include a reduction of the onset temperature of stripes by $\sim$ 50 K, a 29 K reduction of the low-temperature orthorhombic-to-tetragonal transition, competition between charge order and superconductivity, and a preference for stripes to form along the direction of applied stress. Altogether, we observe a dramatic response of the electronic properties of LNSCO-125 to a modest amount of uniaxial stress.

cond-mat.str-el↗

arXiv2020

Strongly coupled charge, orbital and spin order in TbTe$_{3}$

We report a ground state with strongly coupled magnetic and charge density wave orders mediated via orbital ordering in the layered compound \tbt. In addition to the commensurate antiferromagnetic (AFM) and charge density wave (CDW) orders, new magnetic peaks are observed whose propagation vector equals the sum of the AFM and CDW propagation vectors, revealing an intricate and highly entwined relationship. This is especially interesting given that the magnetic and charge orders lie in different layers of the crystal structure where the highly localized magnetic moments of the Tb$^{3+}$ ions are netted in the Tb-Te stacks, while the charge order is formed by the conduction electrons of the adjacent Te-Te layers. Our results, based on neutron diffraction and resonant x-ray scattering reveal that the charge and magnetic subsystems mutually influence each other via the orbital ordering of Tb$^{3+}$ ions.

cond-mat.str-el↗

arXiv2020

Magnetization relaxation and search for the magnetic gap in bulk-insulating V-doped (Bi, Sb)$_2$Te$_3$

V-doped (Bi,Sb)$_2$Te$_3$ has a ten times higher magnetic coercivity than its Cr-doped counterpart and therefore is believed to be a superior system for the quantum anomalous Hall effect (QAHE). The QAHE requires the opening of a magnetic band gap at the Dirac point. We do not find this gap by angle-resolved photoelectron spectroscopy down to 1 K. By x-ray magnetic circular dichroism (XMCD) we directly probe the magnetism at the V site and in zerofield. Hysteresis curves of the XMCD signal show a strong dependence of the coercivity on the ramping velocity of the magnetic field. The XMCD signal decays on a time scale of minutes which we conclude contributes to the absence of a detectable magnetic gap at the Dirac point.

cond-mat.mtrl-sci↗

arXiv2019

Selective probing of magnetic order on Tb and Ir sites in stuffed Tb$_{2+x}$Ir$_{2-x}$O$_{7-y}$ using resonant X-ray scattering

We study the magnetic structure of the "stuffed" (Tb-rich) pyrochlore iridate Tb$_{2+x}$Ir$_{2-x}$O$_{7-y}$, using resonant elastic x-ray scattering (REXS). In order to disentangle contributions from Tb and Ir magnetic sublattices, experiments were performed at the Ir $L_3$ and Tb $M_5$ edges, which provide selective sensitivity to Ir $5d$ and Tb $4f$ magnetic moments, respectively. At the Ir $L_3$ edge, we found the onset of long-range ${\bf k}={\bf 0}$ magnetic order below $T_{N}^\text{Ir}\sim$ 71 K, consistent with the expected signal of all-in all-out (AIAO) magnetic order. Using a single-ion model to calculate REXS cross-sections, we estimate an ordered magnetic moment of $μ_{5d}^{\text{Ir}} \approx 0.34(3)\,μ_B$ at 5 K. At the Tb $M_5$ edge, long-range ${\bf k}={\bf 0}$ magnetic order appeared below $\sim40$ K, also consistent with an AIAO magnetic structure on the Tb site. Additional insight into the magnetism of the Tb sublattice is gleaned from measurements at the $M_5$ edge in applied magnetic fields up to 6 T, which is found to completely suppress the Tb AIAO magnetic order. In zero applied field, the observed gradual onset of the Tb sublattice magnetisation with temperature suggests that it is induced by the magnetic order on the Ir site. The persistence of AIAO magnetic order, despite the greatly reduced ordering temperature and moment size compared to stoichiometric Tb$_{2}$Ir$_{2}$O$_{7}$, for which $T_{N}^{\text{Ir}} =130$ K and $μ_{5d}^{\text{Ir}}=0.56\,μ_B$, indicates that stuffing could be a viable means of tuning the strength of electronic correlations, thereby potentially offering a new strategy to achieve topologically non-trivial band crossings in pyrochlore iridates.

cond-mat.str-el↗

arXiv2019

Adiabatic variation of the charge-density-wave phase diagram in the 123 cuprate (Ca$_x$La$_{1-x}$)(Ba$_{1.75-x}$La$_{0.25+x}$)Cu$_3$O$_y$

In order to explain the emergence of the anomalous pseudogap state and high-temperature superconductivity in the cuprates, intense research activity over three decades has focused on unravelling the connection between the various instabilities of the underdoped regime. In the high-temperature superconductor (Ca$_x$La$_{1-x}$)(Ba$_{1.75-x}$La$_{0.25+x}$)Cu$_3$O$_y$ (CLBLCO) isovalent chemical substitution produces smooth changes to the CuO$_2$ plane buckling and the Cu(II)-to-apical-oxygen distance, allowing us to study the interdependence of charge-density-wave (CDW) order, superconductivity and the pseudogap at constant hole doping in two adiabatically connected representations of the 123 cuprate structure. In this study, resonant soft x-ray scattering measurements reveal the first observation of incommensurate CDW correlations in CLBLCO and demonstrate a lack of correlation between $T_{\text{CDW}}$ and the pseudogap crossover temperature ($T^{\ast}$). This result disfavours a scenario in which the opening of the pseudogap at $T^{\ast}$ results from fluctuating CDW correlations.

cond-mat.supr-con↗

arXiv2019

Resonant inelastic x-ray scattering study of bond order and spin excitations in nickelate thin-film structures

We used high-resolution resonant inelastic x-ray scattering (RIXS) at the Ni $L_3$ edge to simultaneously investigate high-energy interband transitions characteristic of Ni-O bond ordering and low-energy collective excitations of the Ni spins in the rare-earth nickelates $R$NiO$_3$ ($R$ = Nd, Pr, La) with pseudocubic perovskite structure. With the support of calculations based on a double-cluster model we quantify bond order (BO) amplitudes for different thin films and heterostructures and discriminate short-range BO fluctuations from long-range static order. Moreover we investigate magnetic order and exchange interactions in spatially confined $R$NiO$_3$ slabs by probing dispersive magnon excitations. While our study of superlattices (SLs) grown in the (001) direction of the perovskite structure reveals a robust non-collinear spin spiral magnetic order with dispersive magnon excitations that are essentially unperturbed by BO modulations and spatial confinement, we find magnons with flat dispersions and strongly reduced energies in SLs grown in the $(111)_{\text{pc}}$ direction that exhibit collinear magnetic order. These results give insight into the interplay of different collective ordering phenomena in a prototypical 3$d$ transition metal oxide and establish RIXS as a powerful tool to quantitatively study several order parameters and the corresponding collective excitations within one experiment.

cond-mat.str-el↗

arXiv2018

Field-induced double spin spiral in a frustrated chiral magnet

We report the direct observation of a magnetic-feld induced long-wavelength spin spiral modulation in the chiral compound Ba3TaFe3Si2O14. This new spin texture emerges out of a chiral helical ground state, and is hallmarked by the onset of a unique contribution to the bulk electric polarization, the sign of which depends on the crystal chirality. The periodicity of the feld induced modulation, several hundreds of nm depending on the field value, is comparable to the length scales of mesoscopic topological defects such as skyrmions, merons and solitons. The phase transition and observed threshold behavior are consistent with a phenomenology based on the allowed Lifshitz invariants for the chiral symmetry of langasite, which intriguingly contain all the ingredients for the possible realization of topologically stable antiferromagnetic skyrmions.

cond-mat.str-el↗

arXiv2018

Spin-orbit effects surfacing on manganites

Spin-orbit coupling in magnetic systems lacking inversion symmetry can give rise to non trivial spin textures. Magnetic thin films and heterostructures are potential candidates for the formation of skyrmions and other non-collinear spin configurations as inversion symmetry is inherently lost at their surfaces and interfaces. However, manganites, in spite of their extraordinarily rich magnetic phase diagram, have not yet been considered of interest within this context as their spin-orbit coupling is assumed to be negligible. We demonstrate here, by means of angular dependent X-ray linear dichroism experiments and theoretical calculations, the existence of a noncollinear antiferromagnetic ordering at the surface of ferromagnetic La$_{2/3}$Sr$_{1/3}$MnO$_3$ thin films whose properties can only be explained by an unexpectedly large enhancement of the spin-orbit interaction. Our results reveal that spin-orbit coupling, usually assumed to be very small on manganites, can be significantly enhanced at surfaces and interfaces adding a new twist to the possible magnetic orders that can arise in electronically reconstructed systems.

cond-mat.str-el↗

arXiv2018

Magnetic and electronic structure of the layered rare-earth pnictide EuCd$_2$Sb$_2$

Resonant elastic X-ray scattering (REXS) at the Eu $M_5$ edge reveals an antiferromagnetic structure in layered EuCd$_2$Sb$_2$ at temperatures below $T_\textrm{N}$ = 7.4 K with a magnetic propagation vector of $(0,0,1/2)$ and spins in the basal plane. Magneto-transport and REXS measurements with an in-plane magnetic field show that features in the magnetoresistance are correlated with changes in the magnetic structure induced by the field. Ab initio electronic structure calculations predict that the observed spin structure gives rise to a gapped Dirac point close to the Fermi level with a gap of $ΔE \sim$0.01 eV. The results of this study indicate that the Eu spins are coupled to conduction electron states near the Dirac point.

cond-mat.str-el↗