arXiv subjects

Thorsten Schmitt

Publications and source records attributed to Thorsten Schmitt.

At least 37 records · Page 2Linked to original sources

arXiv2023

Nature of the metallic and in-gap states in Ni-doped SrTiO$_3$

Epitaxial thin films of SrTiO$_3$(100) doped with 6% and 12% Ni are studied with resonant angle-resolved photoelectron spectroscopy (ARPES) at the Ti and Ni L2,3-edges. We find that the Ni doping shifts the valence band (VB) of pristine SrTiO$_3$ towards the Fermi level (p-doping) and reduces its band gap. This is accompanied by an upward energy shift of the Ti t2g-derived mobile electron system (MES). Thereby, the in-plane dxy-derived bands reduce the embedded electron density, as evidenced by progressive reduction of their Fermi momentum with the Ni concentration, and the out-of-plane dxz/yz-derived bands depopulate, making the MES purely two-dimensional. Furthermore, the Ti and Ni L2,3-edge resonant photoemission is used to identify the Ni 3d impurity state in the vicinity of the valence-band maximum, and decipher the full spectrum of the VO-induced in-gap states originating from the Ni atoms, Ti atoms, and from their hybridized orbitals. Our experimental information about the dependence of the valence bands, MES and in-gap states in Ni-doped SrTiO$_3$ may help development of this material towards its device applications associated with the reduced optical band gap.

cond-mat.mtrl-sci↗

arXiv2023

k-dependent proximity-induced modulation of spin-orbit interaction in MoSe2 interfaced with amorphous Pb

The ability to modulate the spin-orbit (SO) interaction is crucial for engineering a wide range of spintronics-based quantum devices, extending from state-of-the-art data storage to materials for quantum computing. The use of proximity-induced effects for this purpose may become the mainstream approach, whereas their experimental verification using angle-resolved photoelectron spectroscopy (ARPES) has so far been elusive. Here, using the advantages of soft-X-ray ARPES on its probing depth and intrinsic resolution in three-dimensional momentum k, we identify a distinct modulation of the SO interaction in a van der Waals semiconductor (MoSe2) proximitized to a high-Z metal (Pb), and measure its variation through the k-space. The strong SO field from Pb boosts the SO splitting by up to 30% at the H-point of the bulk Brillouin zone, the spin-orbit hotspot of MoSe2. Tunability of the splitting via the Pb thickness allows its tailoring to particular applications in emerging quantum devices.

cond-mat.mtrl-sci↗

arXiv2023

Nematic spin correlations pervading the phase diagram of FeSe$_{1-x}$S$_{x}$

We use resonant inelastic X-ray scattering (RIXS) at the Fe-L$_3$ edge to study the spin excitations of uniaxial-strained and unstrained FeSe$_{1-x}$S$_{x}$ ($0\leq x\leq0.21$) samples. The measurements on unstrained samples reveal dispersive spin excitations in all doping levels, which show only minor doping dependence in energy dispersion, lifetime, and intensity, indicating that high-energy spin excitations are only marginally affected by sulfur doping. RIXS measurements on uniaxial-strained samples reveal that the high-energy spin-excitation anisotropy observed previously in FeSe is also present in the doping range $0< x\leq0.21$ of FeSe$_{1-x}$S$_{x}$. The spin-excitation anisotropy persists to a high temperature up to $T>200$ K in $x=0.18$ and reaches a maximum around the nematic quantum critical doping ($x_c\approx0.17$). Since the spin-excitation anisotropy directly reflects the existence of nematic spin correlations, our results indicate that high-energy nematic spin correlations pervade the regime of nematicity in the phase diagram and are enhanced by the nematic quantum criticality. These results emphasize the essential role of spin fluctuations in driving electronic nematicity and open the door for uniaxial strain tuning of spin excitations in quantum materials hosting strong magnetoelastic coupling and electronic nematicity.

cond-mat.str-el↗

arXiv2023

Unravelling the Nature of Spin Excitations Disentangled from Charge Contributions in a Doped Cuprate Superconductor

The nature of the spin excitations in superconducting cuprates is a key question toward a unified understanding of the cuprate physics from long-range antiferromagnetism to superconductivity. The intense spin excitations up to the over-doped regime revealed by resonant inelastic X-ray scattering bring new insights as well as questions like how to understand their persistence or their relation to the collective excitations in ordered magnets (magnons). Here, we study the evolution of the spin excitations upon hole-doping the superconducting cuprate Bi$_2$Sr$_2$CaCu$_2$O$_{8+δ}$ by disentangling the spin from the charge excitations in the experimental cross section. We compare our experimental results against density matrix renormalization group calculations for a $t$-$J$-like model on a square lattice. Our results unambiguously confirm the persistence of the spin excitations, which are closely connected to the persistence of short-range magnetic correlations up to high doping. This suggests that the spin excitations in hole-doped cuprates are related to magnons -- albeit short-ranged.

cond-mat.supr-con↗

arXiv2022

Probing magnetic orbitals and Berry curvature with circular dichroism in resonant inelastic X-ray scattering

Resonant inelastic X-ray scattering (RIXS) can probe localized excitations at selected atoms in materials, including particle-hole transitions between the valence and conduction bands. These transitions are governed by fundamental properties of the corresponding Bloch wave-functions, including orbital and magnetic degrees of freedom, and quantum geometric properties such as the Berry curvature. In particular, orbital angular momentum (OAM), which is closely linked to the Berry curvature, can exhibit a nontrivial momentum dependence. We demonstrate how information on such OAM textures can be extracted from the circular dichroism in RIXS. Based on accurate modeling with first-principles treatment of the key ingredient -- the light-matter interaction -- we simulate dichroic RIXS spectra for the prototypical transition metal dichalcogenide MoSe$_2$ and the two-dimensional topological insulator 1T$^\prime$-MoS$_2$. Guided by an intuitive picture for the optical selection rules, we discuss how the momentum-dependent OAM manifests itself in the dichroic RIXS signal if one controls the momentum transfer. Our calculations are performed for typical experimental geometries and parameter regimes, and demonstrate the possibility of observing the predicted circular dichroism in forthcoming experiments. Thus, our work establishes a new avenue to observing Berry curvature and topological states in quantum materials.

cond-mat.mtrl-sci↗

arXiv2022

Hydrogen-impurity induced unconventional magnetism in semiconducting molybdenum ditelluride

Layered transition-metal dichalcogenides are proposed as building blocks for van der Waals (vdW) heterostructures due to their graphene-like two dimensional structure. For this purpose, a magnetic semiconductor could represent an invaluable component for various spintronics and topotronics devices. Here, we combine different local magnetic probe spectroscopies with angle-resolved photoemission and density-functional theory calculations to show that 2H-MoTe2 is on the verge of becoming magnetic. Our results present clear evidence that the magnetism can be "switched on" by a hydrogen-like impurity. We also show that this magnetic state survives up to the free surface region, demonstrating the material's potential applicability as a magnetic component for thin-film heterostructures.

cond-mat.mtrl-sci↗

arXiv2021

Spin-excitation anisotropy in the nematic state of detwinned FeSe

The origin of the electronic nematicity in FeSe is one of the most important unresolved puzzles in the study of iron-based superconductors. In both spin- and orbital-nematic models, the intrinsic magnetic excitations at $\mathbf{Q}_1=(1, 0)$ and $\mathbf{Q}_2=(0, 1)$ of twin-free FeSe are expected to provide decisive criteria for clarifying this issue. Although a spin-fluctuation anisotropy below 10 meV between $\mathbf{Q}_1$ and $\mathbf{Q}_2$ has been observed by inelastic neutron scattering around $T_c\sim 9$ K ($<<T_s\sim 90$ K), it remains unclear whether such an anisotropy also persists at higher energies and associates with the nematic transition $T_{\rm s}$. Here we use resonant inelastic x-ray scattering (RIXS) to probe the high-energy magnetic excitations of uniaxial-strain detwinned FeSe and {\BFA}. A prominent anisotropy between the magnetic excitations along the $H$ and $K$ directions is found to persist to $\sim200$ meV in FeSe, which is even more pronounced than the anisotropy of spin waves in {\BFA}. This anisotropy decreases gradually with increasing temperature and finally vanishes at a temperature around the nematic transition temperature $T_{\rm s}$. Our results reveal an unprecedented strong spin-excitation anisotropy with a large energy scale well above the $d_{xz}/d_{yz}$ orbital splitting, suggesting that the nematic phase transition is primarily spin-driven. Moreover, the measured high-energy spin excitations are dispersive and underdamped, which can be understood from a local-moment perspective. Our findings provide the much-needed understanding of the mechanism for the nematicity of FeSe and points to a unified description of the correlation physics across seemingly distinct classes of Fe-based superconductors.

cond-mat.supr-con↗

arXiv2021

Dispersionless orbital excitations in (Li,Fe)OHFeSe superconductors

The superconducting critical temperature $T_{\mathrm{c}}$ of intercalated iron-selenide superconductor (Li,Fe)OHFeSe (FeSe11111) can be increased to 42 K from 8 K of bulk FeSe. It shows remarkably similar electronic properties as the high-$T_{\mathrm{c}}$ monolayer FeSe and provides a bulk counterpart to investigate the origin of enhanced superconductivity. Unraveling the nature of excitations is crucial for understanding the pairing mechanism in high-$T_{\mathrm{c}}$ iron selenides. Here we use resonant inelastic x-ray scattering (RIXS) to investigate the excitations in FeSe11111. Our high-quality data exhibit several Raman-like excitations, which are dispersionless and isotropic in momentum transfer and robust against varying $T_{\mathrm{c}}$. Using atomic multiplet calculations, we assign the low-energy $\sim 0.3$ and 0.7 eV Raman peaks as local $e_g-e_g$ and $e_g-t_{2g}$ orbital excitations. The intensity of these two features decreases with increasing temperature, suggesting a primary contribution of the orbital fluctuations. Our results highlight the importance of orbital degree of freedom for high-$T_{\mathrm{c}}$ iron selenides.

cond-mat.supr-con↗

arXiv2021

Unraveling higher-order corrections in the spin dynamics of RIXS spectra

Resonant inelastic x-ray scattering (RIXS) is an evolving tool for investigating spin dynamics of strongly correlated materials, which complements inelastic neutron scattering. Both techniques have found that non-spin-conserving (NSC) excitations in quasi-1D isotropic quantum antiferromagnets are confined to the two-spinon phase space. Outside this phase space, only spin-conserving (SC) four-spinon excitations have been detected using O $K$-edge RIXS. Here, we investigate SrCuO$_2$ and find four-spinon excitations outside the two-spinon phase space at both O $K$- and Cu $L_3$-edges. Using the Kramers-Heisenberg formalism, we demonstrate that the four-spinon excitations arise from both SC and NSC processes at Cu $L_3$-edge. We show that these new excitations only appear in the second-order terms of the ultra-fast core-hole lifetime expansion and arise from long-range spin fluctuations. These results thus open a new window to the spin dynamics of quantum magnets.

cond-mat.str-el↗

arXiv2021

Isostructural Metal-Insulator Transition Driven by Dimensional-Crossover in SrIrO3 Heterostructures

Dimensionality reduction induced metal-insulator transitions in oxide heterostructures are usually coupled with structural and magnetic phase transitions, which complicate the interpretation of the underlying physics. Therefore, achieving isostructural MIT is of great importance for fundamental physics and even more for applications. Here, we report an isostructural metal-insulator transition driven by dimensional-crossover in spin-orbital coupled SrIrO3 films. By using in-situ pulsed laser deposition and angle-resolved photoemission spectroscopy, we synthesized and investigated the electronic structure of SrIrO3 ultrathin films with atomic-layer precision. Through inserting orthorhombic CaTiO3 buffer layers, we demonstrate that the crystal structure of SrIrO3 films remains bulk-like with similar oxygen octahedra rotation and tilting when approaching the ultrathin limit. We observe that a dimensional-crossover metal-insulator transition occurs in isostructural SrIrO3 films. Intriguingly, we find the bandwidth of Jeff=3/2 states reduces with lowering the dimensionality and drives the metal-insulator transition. Our results establish a bandwidth controlled metal-insulator transition in the isostructural SrIrO3 thin films.

cond-mat.str-el↗

arXiv2021

Band-Order Anomaly at the γ-Al2O3/SrTiO3 Interface Drives the Electron-Mobility Boost

Rich functionalities of transition-metal oxides and their interfaces bear an enormous technological potential. Its realization in practical devices requires, however, a significant improvement of yet relatively low electron mobility in oxide materials. Recently, a mobility boost of about two orders of magnitude has been demonstrated at the spinel/perovskite γ-Al2O3/SrTiO3 interface compared to the paradigm perovskite/perovskite LaAlO3/SrTiO3. We explore the fundamental physics behind this phenomenon from direct measurements of the momentum-resolved electronic structure of this interface using resonant soft-X-ray angle-resolved photoemission. We find an anomaly in orbital ordering of the mobile electrons in γ-Al2O3/SrTiO3 which depopulates electron states in the top STO layer. This rearrangement of the mobile electron system pushes the electron density away from the interface that reduces its overlap with the interfacial defects and weakens the electron-phonon interaction, both effects contributing to the mobility boost. A crystal-field analysis shows that the band order alters owing to the symmetry breaking between the spinel γ-Al2O3 and perovskite SrTiO3. The band-order engineering exploiting the fundamental symmetry properties emerges as another route to boost the performance of oxide devices.

cond-mat.mtrl-sci↗

arXiv2021

Fluctuating magnetism of Co- and Cu-doped NaFeAs

We report an x-ray emission spectroscopy (XES) study of the local fluctuating magnetic moment ($μ_{bare}$) in $\mathrm{NaFe_{1-x}Co_{x}As}$ and $\mathrm{NaFe_{1-x}Cu_{x}As}$. In NaFeAs, the reduced height of the As ions induces a local magnetic moment higher than $\mathrm{Ba_2As_2}$, despite lower T$_N$ and ordered magnetic moment. As NaFeAs is doped with Co $μ_{bare}$ is slightly reduced, whereas Cu doping leaves it unaffected, indicating a different doping mechanism: based on electron counting for Co whereas impurity scattering dominates in the case of Cu. Finally, we observe an increase of $μ_{bare}$ with temperature in all samples as observed in electron- and hole-doped $\mathrm{BaFe_2As_2}$. Since both Co and Cu doping display superconductivity, our findings demonstrate that the formation of Cooper pairs is not connected with the complete loss of fluctuating paramagnetic moments.

cond-mat.supr-con↗

arXiv2021

Momentum-resolved electronic band structure and offsets in an epitaxial NbN/GaN superconductor/semiconductor heterojunction

The electronic structure of heterointerfaces play a pivotal role in their device functionality. Recently, highly crystalline ultrathin films of superconducting NbN have been integrated by molecular beam epitaxy with the semiconducting GaN. We use soft X-ray angle-resolved photoelectron spectroscopy to directly measure the momentum-resolved electronic band structures for both NbN and GaN constituents of this Schottky heterointerface, and determine their momentum-dependent interfacial band offset as well as the band-bending profile into GaN. We find, in particular, that the Fermi states in NbN are aligned against the band gap in GaN, which excludes any significant electronic cross-talk of the superconducting states in NbN through the interface to GaN. We support the experimental findings with first-principles calculations for bulk NbN and GaN. The Schottky barrier height obtained from photoemission is corroborated by electronic transport and optical measurements. The momentum-resolved understanding of electronic properties elucidated by the combined materials advances and experimental methods in our work opens up new possibilities in systems where interfacial states play a defining role.

cond-mat.mtrl-sci↗

arXiv2021

Charge ordering in Ir dimers in the ground state of Ba$_5$AlIr$_2$O$_{11}$

It has been well established experimentally that the interplay of electronic correlations and spin-orbit interactions in Ir$^{4+}$ and Ir$^{5+}$ oxides results in insulating J$_{\rm eff}$=1/2 and J$_{\rm eff}$=0 ground states, respectively. However, in compounds where the structural dimerization of iridum ions is favourable, the direct Ir $d$--$d$ hybridisation can be significant and takes a key role. Here, we investigate the effects of direct Ir $d$--$d$ hybridisation in comparison with electronic correlations and spin-orbit coupling in Ba$_5$AlIr$_2$O$_{11}$, a compound with Ir dimers. Using a combination of $ab$ $initio$ many-body wave function quantum chemistry calculations and resonant inelastic X-ray scattering (RIXS) experiments, we elucidate the electronic structure of Ba$_5$AlIr$_2$O$_{11}$. We find excellent agreement between the calculated and the measured spin-orbit excitations. Contrary to the expectations, the analysis of the many-body wave function shows that the two Ir (Ir$^{4+}$ and Ir$^{5+}$) ions in the Ir$_2$O$_9$ dimer unit in this compound preserve their local J$_{\rm eff}$ character close to 1/2 and 0, respectively. The local point group symmetry at each of the Ir sites assumes an important role, significantly limiting the direct $d$--$d$ hybridisation. Our results emphasize that minute details in the local crystal field (CF) environment can lead to dramatic differences in electronic states in iridates and 5$d$ oxides in general.

cond-mat.str-el↗

arXiv2021

Spin dynamics in NaFeAs and NaFe$_{0.53}$Cu$_{0.47}$As probed by resonant inelastic X-ray scattering

The parent compounds of iron-based superconductors are magnetically-ordered bad metals, with superconductivity appearing near a putative magnetic quantum critical point. The presence of both Hubbard repulsion and Hund's coupling leads to rich physics in these multiorbital systems, and motivated descriptions of magnetism in terms of itinerant electrons or localized spins. The NaFe$_{1-x}$Cu$_x$As series consists of magnetically-ordered bad metal ($x=0$), superconducting ($x\approx0.02$) and magnetically-ordered semiconducing/insulating ($x\approx0.5$) phases, providing a platform to investigate the connection between superconductivity, magnetism and electronic correlations. Here we use X-ray absorption spectroscopy and resonant inelastic X-ray scattering to study the valence state of Fe and spin dynamics in two NaFe$_{1-x}$Cu$_x$As compounds ($x=0$ and 0.47). We find that magnetism in both compounds arises from Fe$^{2+}$ atoms, and exhibits underdamped dispersive spin waves in their respective ordered states. The dispersion of spin excitations in NaFe$_{0.53}$Cu$_{0.47}$As is consistent with being quasi-one-dimensional. Compared to NaFeAs, the band top of spin waves in NaFe$_{0.53}$Cu$_{0.47}$As is slightly softened with significantly more spectral weight of the spin excitations. Our results indicate the spin dynamics in NaFe$_{0.53}$Cu$_{0.47}$As arise from localized magnetic moments and suggest the iron-based superconductors are proximate to a correlated insulating state with localized iron moments.

cond-mat.str-el↗

arXiv2020

Description of resonant inelastic x-ray scattering in correlated metals

To fully capitalize on the potential and versatility of resonant inelastic x-ray scattering (RIXS), it is essential to develop the capability to interpret different RIXS contributions through calculations, including the dependence on momentum transfer, from first-principles for correlated materials. Toward that objective, we present new methodology for calculating the full RIXS response of a correlated metal in an unbiased fashion. Through comparison of measurements and calculations that tune the incident photon energy over a wide portion of the Fe L$_3$ absorption resonance of the example material BaFe$_2$As$_2$, we show that the RIXS response in BaFe$_2$As$_2$ is dominated by the direct channel contribution, including the Raman-like response below threshold, which we explain as a consequence of the finite core-hole lifetime broadening. Calculations are initially performed within the first-principles Bethe-Salpeter framework, which we then significantly improve by convolution with an effective spectral function for the intermediate-state excitation. We construct this spectral function, also from first-principles, by employing the cumulant expansion of the Green's function and performing a real-time time dependent density functional theory calculation of the response of the electronic system to the perturbation of the intermediate-state excitation. Importantly, this allows us to evaluate the indirect RIXS response from first-principles, accounting for the full periodicity of the crystal structure and with dependence on the momentum transfer.

cond-mat.str-el↗

arXiv2020

Strain-engineering of the charge and spin-orbital interactions in Sr2IrO4

In the high spin-orbit coupled Sr2IrO4, the high sensitivity of the ground state to the details of the local lattice structure shows a large potential for the manipulation of the functional properties by inducing local lattice distortions. We use epitaxial strain to modify the Ir-O bond geometry in Sr2IrO4 and perform momentum-dependent Resonant Inelastic X-ray Scattering (RIXS) at the metal and at the ligand sites to unveil the response of the low energy elementary excitations. We observe that the pseudospin-wave dispersion for tensile-strained Sr2IrO4 films displays large softening along the [h,0] direction, while along the [h,h] direction it shows hardening. This evolution reveals a renormalization of the magnetic interactions caused by a strain-driven crossover from anisotropic to isotropic interactions between the magnetic moments. Moreover, we detect dispersive electron-hole pair excitations which shift to lower (higher) energies upon compressive (tensile) strain, manifesting a reduction (increase) in the size of the charge gap. This behavior shows an intimate coupling between charge excitations and lattice distortions in Sr2IrO4, originating from the modified hopping elements between the t2g orbitals. Our work highlights the central role played by the lattice degrees of freedom in determining both the pseudospin and charge excitations of Sr2IrO4 and provides valuable information towards the control of the ground state of complex oxides in the presence of high spin-orbit coupling.

cond-mat.str-el↗

arXiv2020

Minority-Spin Impurity Band in n-Type (In,Fe)As: A Materials Perspective for Ferromagnetic Semiconductors

Fully understanding the properties of n-type ferromagnetic semiconductors (FMSs), complementary to the mainstream p-type ones, is a challenging goal in semiconductor spintronics because ferromagnetism in n-type FMSs is theoretically non-trivial. Soft-x-ray angle-resolved photoemission spectroscopy (SX-ARPES) is a powerful approach to examine the mechanism of carrier-induced ferromagnetism in FMSs. Here our SX-ARPES study on the prototypical n-type FMS (In,Fe)As reveals the entire band structure including the Fe-3d impurity bands (IBs) and the host InAs ones, and provides direct evidence for electron occupation of the InAs-derived conduction band (CB). A minority-spin Fe-3d IB is found to be located just below the conduction-band minimum (CBM). The IB is formed by the hybridization of the unoccupied Fe-3d states with the occupied CBM of InAs in a spin-dependent way, resulting in the large spin polarization of CB. The band structure with the IB is varied with band filling, which cannot be explained by the rigid-band picture, suggesting a unified picture for realization of carrier-induced ferromagnetism in FMS materials.

cond-mat.mtrl-sci↗