arXiv subjects

Thorsten Schmitt

Publications and source records attributed to Thorsten Schmitt.

At least 73 records · Page 4Linked to original sources

arXiv2016

A Mott insulator continuously connected to iron pnictide superconductors

Iron-based superconductivity develops near an antiferromagnetic order and out of a bad metal normal state, which has been interpreted as originating from a proximate Mott transition. Whether an actual Mott insulator can be realized in the phase diagram of the iron pnictides remains an open question. Here we use transport, transmission electron microscopy, X-ray absorption spectroscopy, and neutron scattering to demonstrate that NaFe$_{1-x}$Cu$_x$As near $x\approx 0.5$ exhibits real space Fe and Cu ordering, and are antiferromagnetic insulators with the insulating behavior persisting above the Néel temperature, indicative of a Mott insulator. Upon decreasing $x$ from $0.5$, the antiferromagnetic ordered moment continuously decreases, yielding to superconductivity around $x=0.05$. Our discovery of a Mott insulating state in NaFe$_{1-x}$Cu$_x$As thus makes it the only known Fe-based material in which superconductivity can be smoothly connected to the Mott insulating state, highlighting the important role of electron correlations in the high-$T_{\rm c}$ superconductivity.

cond-mat.supr-con↗

arXiv2016

Presence of magnetic excitations in SmFeAsO

We measured dispersive spin excitations in $\mathrm{SmFeAsO}$, parent compound of $\mathrm{SmFeAsO_{\text{1-x}}F_{\text{x}}}$ one of the highest temperature superconductors of Fe pnictides (T$_{\text{C}}\approx$55~K). We determine the magnetic excitations to disperse with a bandwidth energy of ca 170 meV at (0.47, 0) and (0.34, 0.34), which merges into the elastic line approaching the $Γ$ point. Comparing our results with other parent Fe pnictides, we show the importance of structural parameters for the magnetic excitation spectrum, with small modifications of the tetrahedron angles and As height strongly affecting the magnetism.

cond-mat.supr-con↗

arXiv2016

Orbital breathing effects in the computation of x-ray d-ion spectra in solids by ab initio wave-function-based methods

In existing theoretical approaches to core-level excitations of transition-metal ions in solids relaxation and polarization effects due to the inner core hole are often ignored or described phenomenologically. Here we set up an ab initio computational scheme that explicitly accounts for such physics in the calculation of x-ray absorption and resonant inelastic x-ray scattering spectra. Good agreement is found with experimental transition-metal $L$-edge data for the strongly correlated $d^9$ cuprate Li$_2$CuO$_2$, for which we determine the absolute scattering intensities. The newly developed methodology opens the way for the investigation of even more complex $d^n$ electronic structures of group VI B to VIII B correlated oxide compounds.

cond-mat.str-el↗

arXiv2016

Intra-layer doping effects on the high-energy magnetic correlations in NaFeAs

We have used Resonant Inelastic X-ray Scattering (RIXS) and dynamical susceptibility calculations to study the magnetic excitations in NaFe$_{1-x}$Co$_x$As (x = 0, 0.03, and 0.08). Despite a relatively low ordered magnetic moment, collective magnetic modes are observed in parent compounds (x = 0) and persist in optimally (x = 0.03) and overdoped (x = 0.08) samples. Their magnetic bandwidths are unaffected by doping within the range investigated. High energy magnetic excitations in iron pnictides are robust against doping, and present irrespectively of the ordered magnetic moment. Nevertheless, Co doping slightly reduces the overall magnetic spectral weight, differently from previous studies on hole-doped BaFe$_{2}$As$_{2}$, where it was observed constant. Finally, we demonstrate that the doping evolution of magnetic modes is different for the dopants being inside or outside the Fe-As layer.

cond-mat.supr-con↗

arXiv2016

Probing inter- and intrachain Zhang-Rice excitons in Li$_2$CuO$_2$ and determining their binding energy

Cuprate materials, like those hosting high temperature superconductivity, represent a famous class of materials where the correlations between the strongly entangled charges and spins produce complex phase diagrams. Several years ago the Zhang-Rice singlet was proposed as a natural quasiparticle in hole-doped cuprates. The occurance and binding energy of this quasiparticle, consisting of a pair of bound holes with antiparallel spins on the same CuO$_4$ plaquette, depends on the local electronic interactions, which are fundamental quantities for understanding the physics of the cuprates. Here, we employ state-of-the-art Resonant Inelastic X-ray Scattering (RIXS) to probe the correlated physics of the CuO$_4$ plaquettes in the quasi-one dimensional chain cuprate Li$_2$CuO$_2$. By tuning the incoming photon energy to the O $K$-edge, we populate bound states related to the Zhang-Rice quasiparticles in the RIXS process. Both intra- and interchain Zhang-Rice singlets are observed and their occurrence is shown to depend on the nearest-neighbor spin-spin correlations, which are readily probed in this experiment. We also extract the binding energy of the Zhang-Rice singlet and identify the Zhang-Rice triplet excitation in the RIXS spectra.

cond-mat.str-el↗

arXiv2016

Alternative interpretation of the recent experimental results of angle-resolved photoemission spectroscopy on GaMnAs [Sci. Rep. 6, 27266 (2016)]

Clarification of the position of the Fermi level ($E_\mathrm{F}$) is important in understanding the origin of ferromagnetism in the prototypical ferromagnetic semiconductor Ga$_{1-x}$Mn$_x$As (GaMnAs). In a recent publication, Souma $et$ $al$. [Sci. Rep. $\mathbf{6}$, 27266 (2016)], have investigated the band structure and the $E_\mathrm{F}$ position of GaMnAs using angle-resolved photoemission spectroscopy (ARPES), and concluded that $E_\mathrm{F}$ is located in the valence band (VB). However, this conclusion contradicts a number of recent experimental results for GaMnAs, which showed that $E_\mathrm{F}$ is located above the VB maximum in the impurity band (IB). Here, we show an alternative interpretation of their ARPES experiments, which is consistent with those recent experiments and supports the picture that $E_\mathrm{F}$ is located above the VB maximum in the IB.

cond-mat.mtrl-sci↗

arXiv2016

Ground state oxygen holes and the metal-insulator transition in the negative charge transfer rare-earth nickelates

The metal-insulator transitions and the intriguing physical properties of rare-earth perovskite nickelates have attracted considerable attention in recent years. Nonetheless, a complete understanding of these materials remains elusive. Here, taking a NdNiO3 thin film as a representative example, we utilize a combination of x-ray absorption and resonant inelastic x-ray scattering (RIXS) spectroscopies to resolve important aspects of the complex electronic structure of the rare-earth nickelates. The unusual coexistence of bound and continuum excitations observed in the RIXS spectra provides strong evidence for the abundance of oxygen 2p holes in the ground state of these materials. Using cluster calculations and Anderson impurity model interpretation, we show that these distinct spectral signatures arise from a Ni 3d8 configuration along with holes in the oxygen 2p valence band, confirming suggestions that these materials do not obey a conventional positive charge-transfer picture, but instead exhibit a negative charge-transfer energy, in line with recent models interpreting the metal to insulator transition in terms of bond disproportionation.

cond-mat.str-el↗

arXiv2016

Magnetic moment evolution and spin freezing in doped BaFe$_{2}$As$_{2}$

Fe-K$_β$ X-ray emission spectroscopy measurements reveal an asymmetric doping dependence of the magnetic moments $μ_\text{bare}$ in electron- and hole-doped BaFe$_{2}$As$_{2}$. At low temperature, $μ_\text{bare}$ is nearly constant in hole-doped samples, whereas it decreases upon electron doping. Increasing temperature substantially enhances $μ_\text{bare}$ in the hole-doped region, which is naturally explained by the theoretically predicted crossover into a spin-frozen state. Our measurements demonstrate the importance of Hund's coupling and electronic correlations, especially for hole-doped BaFe$_{2}$As$_{2}$, and the inadequacy of a fully localized or fully itinerant description of the 122 family of Fe pnictides.

cond-mat.supr-con↗

arXiv2015

Electron-lattice interactions strongly renormalize the charge transfer energy in the spin-chain cuprate Li$_2$CuO$_2$

Strongly correlated insulators are broadly divided into two classes: Mott-Hubbard insulators, where the insulating gap is driven by the Coulomb repulsion $U$ on the transition-metal cation, and charge-transfer insulators, where the gap is driven by the charge transfer energy $Δ$ between the cation and the ligand anions. The relative magnitudes of $U$ and $Δ$ determine which class a material belongs to, and subsequently the nature of its low-energy excitations. These energy scales are typically understood through the local chemistry of the active ions. Here we show that the situation is more complex in the low-dimensional charge transfer insulator Li$_\mathrm{2}$CuO$_\mathrm{2}$, where $Δ$ has a large non-electronic component. Combining resonant inelastic x-ray scattering with detailed modeling, we determine how the elementary lattice, charge, spin, and orbital excitations are entangled in this material. This results in a large lattice-driven renormalization of $Δ$, which significantly reshapes the fundamental electronic properties of Li$_\mathrm{2}$CuO$_\mathrm{2}$.

cond-mat.str-el↗

arXiv2015

Sputtering induced re-emergence of the topological surface state in Bi$_2$Se$_3$

We study the fate of the surface states of Bi$_2$Se$_3$ under disorder with strength larger than the bulk gap, caused by neon sputtering and nonmagnetic adsorbates. We find that neon sputtering introduces strong but dilute defects, which can be modeled by a unitary impurity distribution, whereas adsorbates, such as water vapor or carbon monoxide, are best described by Gaussian disorder. Remarkably, these two disorder types have a dramatically different effect on the surface states. Our soft x-ray ARPES measurements combined with numerical simulations show that unitary surface disorder pushes the Dirac state to inward quintuplet layers, burying it below an insulating surface layer. As a consequence, the surface spectral function becomes weaker, but retains its quasiparticle peak. This is in contrast to Gaussian disorder, which smears out the quasiparticle peak completely. At the surface of Bi$_2$Se$_3$, the effects of Gaussian disorder can be reduced by removing surface adsorbates using neon sputtering, which, however, introduces unitary scatterers. Since unitary disorder has a weaker effect than Gaussian disorder, the ARPES signal of the Dirac surface state becomes sharper upon sputtering.

cond-mat.mes-hall↗

arXiv2015

Correlation of the Superconducting Critical Temperature with Spin and Orbital Excitation Energies In (Ca{x}La{1-x})(Ba{1.75-x}La{0.25+x})Cu{3}O{y} as Measured by Resonant Inelastic X-ray Scattering

Electronic spin and orbital (dd) excitation spectra of (Ca{x}La{1-x})(Ba{1.75-x}La{0.25+x})Cu{3}O{y} samples are measured by resonant inelastic x-ray scattering (RIXS). In this compound, Tc of samples with identical hole dopings is strongly affected by the Ca/Ba substitution x due to subtle variations in the lattice constants, while crystal symmetry and disorder as measured by line-widths are x independent. We examine two extreme values of x and two extreme values of hole-doping content y corresponding to antiferromagnetic and superconducting states. The x dependence of the spin mode energies is approximately the same for both the antiferromagnetic and superconducting samples. This clearly demonstrates that RIXS is sensitive to J even in doped samples. A positive correlation between the superexchange J and the maximum of Tc at optimal doping Tc^{max} is observed. We also measured the x dependence of the d_{xy} -> d_{x^2-y^2} and d_{xz/yz} -> d_{x^2-y^2} orbital splittings. We infer that the effect of the unresolved d_{3z^2-r^2} -> d_{x^2-y^2} excitation on Tc^{max} is much smaller than the effect of J. There appears to be dispersion in the d_{xy} -> d_{x^2-y^2} peak of up to 0.05 eV. Our fitting of the peaks furthermore indicates an asymmetric dispersion for the d_{xz/yz} -> d_{x^2-y^2} excitation. A peak at ~0.8 eV is also observed, and attributed to a dd excitation in the chain layer.

cond-mat.supr-con↗

arXiv2015

Orbital control of effective dimensionality: from spin-orbital fractionalization to confinement in the anisotropic ladder system CaCu2O3

Fractionalization of an electronic quasiparticle into spin, charge and orbital parts is a fundamental and characteristic property of interacting electrons in one dimension. However, real materials are never strictly one-dimensional and the fractionalization phenomena are hard to observe. Here we studied the spin and orbital excitations of the anisotropic ladder material CaCu2O3, whose electronic structure is not one-dimensional. Combining high-resolution resonant inelastic x-ray scattering experiments with theoretical model calculations we show that: (i) spin-orbital fractionalization occurs in CaCu2O3 along the leg direction x through the xz orbital channel as in a 1D system; and (ii) no fractionalization is observed for the xy orbital, which extends in both leg and rung direction, contrary to a 1D system. We conclude that the directional character of the orbital hopping can select different degrees of dimensionality. Using additional model calculations, we show that spin-orbital separation is generally far more robust than the spin-charge separation. This is not only due to the already mentioned selection realized by the orbital hopping, but also due to the fact that spinons are faster than the orbitons.

cond-mat.str-el↗

arXiv2013

Femtosecond dynamics of magnetic excitations from resonant inelastic x-ray scattering in CaCu2O3

Taking spinon excitations in the quantum antiferromagnet CaCu2O3 as an example, we demonstrate that femtosecond dynamics of magnetic excitations can be probed by direct resonant inelastic x-ray scattering (RIXS). To this end, we isolate the contributions of single and double spin-flip excitations in experimental RIXS spectra, identify the physical mechanisms that cause them and determine their respective timescales. By comparing theory and experiment, we find that double spin flips need a finite amount of time to be generated, rendering them sensitive to the core-hole lifetime, whereas single spin flips are to a very good approximation independent of it. This shows that RIXS can grant access to time-domain dynamics of excitations and illustrates how RIXS experiments can distinguish between excitations in correlated electron systems based on their different time dependence.

cond-mat.str-el↗

arXiv2013

Unveiling the impurity band inducing ferromagnetism in magnetic semiconductor (Ga,Mn)As

(Ga,Mn)As is a paradigm diluted magnetic semiconductor which shows ferromagnetism induced by doped hole carriers. With a few controversial models emerged from numerous experimental and theoretical studies, the mechanism of the ferromagnetism in (Ga,Mn)As still remains a puzzling enigma. In this Letter, we use soft x-ray angle-resolved photoemission spectroscopy to positively identify the ferromagnetic Mn 3d-derived impurity band in (Ga,Mn)As. The band appears hybridized with the light-hole band of the host GaAs. These findings conclude the picture of the valence band structure of (Ga,Mn)As disputed for more than a decade. The non-dispersive character of the IB and its location in vicinity of the valence-band maximum indicate that the Mn 3d-derived impurity band is formed as a split-off Mn-impurity state predicted by the Anderson impurity model. Responsible for the ferromagnetism in (Ga,Mn)As is the transport of hole carriers in the impurity band.

cond-mat.mtrl-sci↗

arXiv2012

Determining the Short-Range Spin Correlations in Cuprate Chain Materials with Resonant Inelastic X-ray Scattering

We report a high-resolution resonant inelastic soft x-ray scattering study of the quantum magnetic spin-chain materials Li2CuO2 and CuGeO3. By tuning the incoming photon energy to the oxygen K-edge, a strong excitation around 3.5 eV energy loss is clearly resolved for both materials. Comparing the experimental data to many-body calculations, we identify this excitation as a Zhang-Rice singlet exciton on neighboring CuO4-plaquettes. We demonstrate that the strong temperature dependence of the inelastic scattering related to this high-energy exciton enables to probe short-range spin correlations on the 1 meV scale with outstanding sensitivity.

cond-mat.str-el↗

arXiv2012

Digging up bulk band dispersion buried under a passivation layer

Atomically controlled crystal growth of thin films has established foundations of nanotechnology aimed at the development of advanced functional devices. Crystallization under non-equilibrium conditions allows engineering of new materials with their atomically-flat interfaces in the heterostructures exhibiting novel physical properties. From a fundamental point of view, knowledge of the electronic structures of thin films and their interfaces is indispensable to understand the origins of their functionality which further evolves into realistic device application. In view of extreme surface sensitivity of the conventional vacuum-ultraviolet (VUV) angle-resolved photoemission spectroscopy (ARPES), with a probing depth of several angstroms, experiments on thin films have to use sophisticated in-situ sample transfer systems to avoid surface contamination. In this Letter, we put forward a method to circumvent these difficulties using soft X-ray (SX) ARPES. A GaAs:Be thin film in our samples was protected by an amorphous As layer with an thickness of $\sim 1$ nm exceeding the probing depth of the VUV photoemission with photon energy $hν$ around 100 eV. The increase of the probing depth with increasing $hν$ towards the SX region has clearly exposed the bulk band dispersion without any surface treatment. Any contributions from potential interface states between the thin film and the amorphous capping layer has been below the detection limit. Our results demonstrate that SX-ARPES enables the observation of coherent three-dimensional band dispersion of buried heterostructure layers through an amorphous capping layer, breaking through the necessity of surface cleaning of thin film samples. Thereby, this opens new frontiers in diagnostics of authentic momentum-resolved electronic structure of protected thin-film heterostructures.

cond-mat.mtrl-sci↗

arXiv2012

Three-Dimensional Fermiology by Soft-X-Ray ARPES: Origin of Charge Density Waves in VSe2

Electronic structure of crystalline materials is their fundamental characteristic which is the basis of almost all their physical and chemical properties. Angle-resolved photoemission spectroscopy (ARPES) is the main experimental tool to study all electronic structure aspects with resolution in k-space. However, its application to three-dimensional (3D) materials suffers from a fundamental problem of ill-defined surface-perpendicular wavevector kz. Here, we achieve sharp definition of kz to enable precise navigation in 3D k space by pushing ARPES into the soft-X-ray photon energy range. Essential to break through the notorious problem of small photoexcitation cross-section was an advanced photon flux performance of our instrumentation. We explore the electronic structure of a transition metal dichalcogenide VSe2 which develops charge density waves (CDWs) possessing exotic 3D character. We experimentally identify nesting of its 3D Fermi surface (FS) as the precursor for these CDWs. Our study demonstrates an immense potential of soft-X-ray ARPES (SX-ARPES) to resolve various aspects of 3D electronic structure.

cond-mat.str-el↗

arXiv2012

Surface and bulk Fermiology and band dispersion in non-centrosymmetric BiTeI

BiTeI has a layered and non-centrosymmetric structure where strong spin-orbit interaction leads to a giant spin splitting in the bulk bands. Here we present high-resolution angle-resolved photoemission (ARPES) data in the UV and soft x-ray regime that clearly disentangle the surface from the bulk electronic structure. Spin-resolved UV-ARPES measurements on opposite, non-equivalent surfaces show identical spin structures, thus clarifying the surface state character. Soft x-ray ARPES data clearly reveal the spindle-torus shape of the bulk Fermi surface, induced by the spin-orbit interaction.

cond-mat.mtrl-sci↗