arXiv subjects

T. Schmitt

Publications and source records attributed to T. Schmitt.

At least 55 records · Page 3Linked to original sources

arXiv2016

Doping Evolution of Magnetic Order and Magnetic Excitations in (Sr$_{1-x}$La$_x$)$_3$Ir$_2$O$_7$

We use resonant elastic and inelastic X-ray scattering at the Ir-$L_3$ edge to study the doping-dependent magnetic order, magnetic excitations and spin-orbit excitons in the electron-doped bilayer iridate (Sr$_{1-x}$La$_{x}$)$_3$Ir$_2$O$_7$ ($0 \leq x \leq 0.065$). With increasing doping $x$, the three-dimensional long range antiferromagnetic order is gradually suppressed and evolves into a three-dimensional short range order from $x = 0$ to $0.05$, followed by a transition to two-dimensional short range order between $x = 0.05$ and $0.065$. Following the evolution of the antiferromagnetic order, the magnetic excitations undergo damping, anisotropic softening and gap collapse, accompanied by weakly doping-dependent spin-orbit excitons. Therefore, we conclude that electron doping suppresses the magnetic anisotropy and interlayer couplings and drives (Sr$_{1-x}$La$_x$)$_3$Ir$_2$O$_7$ into a correlated metallic state hosting two-dimensional short range antiferromagnetic order and strong antiferromagnetic fluctuations of $J_{\text{eff}} = \frac{1}{2}$ moments, with the magnon gap strongly suppressed.

cond-mat.str-el↗

arXiv2016

Direct observation of how the heavy fermion state develops in CeCoIn5

Heavy fermion materials gain high electronic masses and expand Fermi surfaces when the high-temperature localized f electrons become itinerant and hybridize with the conduction band at low temperatures. However, despite the common application of this model, direct microscopic verification remains lacking. Here we report high-resolution angle-resolved photoemission spectroscopy measurements on CeCoIn5, a prototypical heavy fermion compound, and reveal the long-sought band hybridization and Fermi surface expansion. Unexpectedly, the localized-to-itinerant transition occurs at surprisingly high temperatures, yet f electrons are still largely localized at the lowest temperature. Moreover, crystal field excitations likely play an important role in the anomalous temperature dependence. Our results paint an comprehensive unanticipated experimental picture of the heavy fermion formation in a periodic multi-level Anderson/Kondo lattice, and set the stage for understanding the emergent properties in related materials.

cond-mat.str-el↗

arXiv2016

Orbital engineering in nickelate heterostructures driven by anisotropic oxygen hybridization rather than orbital energy levels

Resonant inelastic x-ray scattering is used to investigate the electronic origin of orbital polarization in nickelate heterostructures taking $\mathrm{LaTiO_3-LaNiO_3-3x(LaAlO_3)}$, a system with exceptionally large polarization, as a model system. We find that heterostructuring generates only minor changes in the Ni $3d$ orbital energy levels, contradicting the often-invoked picture in which changes in orbital energy levels generate orbital polarization. Instead, O $K$-edge x-ray absorption spectroscopy demonstrates that orbital polarization is caused by an anisotropic reconstruction of the oxygen ligand hole states. This provides an explanation for the limited success of theoretical predictions based on tuning orbital energy levels and implies that future theories should focus on anisotropic hybridization as the most effective means to drive large changes in electronic structure and realize novel emergent phenomena.

cond-mat.str-el↗

arXiv2016

Quenched Magnon excitations by oxygen sublattice reconstruction in (SrCuO$_2$)$_n$/(SrTiO$_3$)$_2$ superlattices

The recently discovered structural reconstruction in the cuprate superlattice (SrCuO$_2$)$_n$/(SrTiO$_3$)$_2$ has been investigated across the critical value of $n=5$ using resonant inelastic x-ray scattering (RIXS). We find that at the critical value of $n$, the cuprate layer remains largely in the bulk-like two-dimensional structure with a minority of Cu plaquettes being reconstructed. The partial reconstruction leads to quenching of the magnons starting at the $Γ$-point due to the minority plaquettes acting as scattering points. Although comparable in relative abundance, the doped charge impurities in electron-doped cuprate superconductors do not show this quenching of magnetic excitations.

cond-mat.str-el↗

arXiv2016

Measurement of collective excitations in VO$_2$ by resonant inelastic X-ray scattering

Vanadium dioxide is of broad interest as a spin-1/2 electron system that realizes a metal-insulator transition near room temperature, due to a combination of strongly correlated and itinerant electron physics. Here, resonant inelastic X-ray scattering is used to measure the excitation spectrum of charge, spin, and lattice degrees of freedom at the vanadium L-edge under different polarization and temperature conditions. These spectra reveal the evolution of energetics across the metal-insulator transition, including the low temperature appearance of a strong candidate for the singlet-triplet excitation of a vanadium dimer.

cond-mat.str-el↗

arXiv2016

A resonant inelastic x-ray scattering study of the spin and charge excitations in the overdoped superconductor La1.77Sr0.23CuO4

We present a resonant inelastic x-ray scattering (RIXS) study of spin and charge excitations in overdoped La1.77Sr0.23CuO4 along two high-symmetry directions. The line shape of these excitations is analyzed and they are shown to be highly overdamped. Their spectral weight and damping are found to be strongly momentum dependent. Qualitative agreement between these observations and a calculated RPA susceptibility is obtained for this overdoped compound, implying that a significant contribution to the RIXS signal stems from a continuum of charge excitations. Furthermore, this suggests that the spin-excitations in the overdoped regime can be captured qualitatively by an itinerant picture. Our calculations also predict a new low-energy spin excitation branch to exist along the nodal direction near the zone center. With the energy resolution of the present experiment, this branch is not resolvable but we show that next generation of high-resolution spectrometers will be able to test this prediction.

cond-mat.supr-con↗

arXiv2015

Polaronic metal state at the LaAlO3/SrTiO3 interface

Interplay of spin, charge, orbital and lattice degrees of freedom in oxide heterostructures results in a plethora of fascinating properties, which can be exploited in new generations of electronic devices with enhanced functionalities. The paradigm example is the interface between the two band insulators LaAlO3 and SrTiO3 (LAO/STO) that hosts two-dimensional electron system (2DES). Apart from the mobile charge carriers, this system exhibits a range of intriguing properties such as field effect, superconductivity and ferromagnetism, whose fundamental origins are still debated. Here, we use soft-X-ray angle-resolved photoelectron spectroscopy to penetrate through the LAO overlayer and access charge carriers at the buried interface. The experimental spectral function directly identifies the interface charge carriers as large polarons, emerging from coupling of charge and lattice degrees of freedom, and involving two phonons of different energy and thermal activity. This phenomenon fundamentally limits the carrier mobility and explains its puzzling drop at high temperatures.

cond-mat.mtrl-sci↗

arXiv2015

Fermi surface of three-dimensional La1-xSrxMnO3 explored by soft-X-ray ARPES: Rhombohedral lattice distortion and its effect on magnetoresistance

Electronic structure of the three-dimensional colossal magnetoresistive perovskite La1-xSrxMnO3 has been established using soft-X-ray ARPES with its intrinsically sharp definition of three-dimensional electron momentum. The experimental results show much weaker polaronic coupling compared to the bilayer manganites and are consistent with the GGA+U band structure. The experimental Fermi surface unveils the canonical topology of alternating three-dimensional electron spheres and hole cubes, with their shadow contours manifesting the rhombohedral lattice distortion. This picture has been confirmed by one-step photoemission calculations including displacement of the apical oxygen atoms. The rhombohedral distortion is neutral to the Jahn-Teller effect and thus polaronic coupling, but affects the double-exchange electron hopping and thus the colossal magnetoresistance effect.

cond-mat.str-el↗

arXiv2015

Tailoring the electronic transitions of NdNiO_3 films through (111)_pc oriented interfaces

Bulk NdNiO_3 and thin films grown along the pseudocubic (001)_pc axis display a 1st order metal to insulator transition (MIT) together with a Néel transition at T=200K. Here, we show that for NdNiO3 films deposited on (111)_pc NdGaO_3 the MIT occurs at T=335K and the Néel transition at T=230 K. By comparing transport and magnetic properties of layers grown on substrates with different symmetries and lattice parameters, we demonstrate a particularly large tuning when the epitaxy is realized on (111)_pc surfaces. We attribute this effect to the specific lattice matching conditions imposed along this direction when using orthorhombic substrates.

cond-mat.str-el↗

arXiv2015

Electronic Transitions in Strained SmNiO_3 Thin Films

Nickelates are known for their metal to insulator transition (MIT) and an unusual magnetic ordering, occurring at T=T_Néel. Here, we investigate thin films of SmNiO_3 subjected to different levels of epitaxial strain. We find that the original bulk behavior (T_Néel<T_MI) is strongly affected by applying compressive strain to the films. For small compressive strains, a regime where T_Néel=T_MI is achieved, the paramagnetic insulating phase characteristic of the bulk compound is suppressed and the MIT becomes 1st order. Further increasing the in-plane compression of the SmNiO_3 lattice leads to the stabilization of a single metallic paramagnetic phase.

cond-mat.str-el↗

arXiv2015

Magnetic excitations and phonons simultaneously studied by resonant inelastic x-ray scattering in optimally doped Bi$_{1.5}$Pb$_{0.55}$Sr$_{1.6}$La$_{0.4}$CuO$_{6+δ}$

Magnetic excitations in the optimally doped high-$T_\mathrm{c}$ superconductor Bi$_{1.5}$Pb$_{0.55}$Sr$_{1.6}$La$_{0.4}$CuO$_{6+δ}$ (OP-Bi2201, $T_\mathrm{c}\simeq 34$ K) are investigated by Cu $L_3$ edge resonant inelastic x-ray scattering (RIXS), below and above the pseudogap opening temperature. At both temperatures the broad spectral distribution disperses along the (1,0) direction up to $\sim$350~meV at zone boundary, similarly to other hole-doped cuprates. However, above $\sim$0.22 reciprocal lattice units, we observe a concurrent intensity decrease for magnetic excitations and quasi-elastic signals with weak temperature dependence. This anomaly seems to indicate a coupling between magnetic, lattice and charge modes in this compound. We also compare the magnetic excitation spectra near the anti-nodal zone boundary in the single layer OP-Bi2201 and in the bi-layer optimally doped Bi$_{1.5}$Pb$_{0.6}$Sr$_{1.54}$CaCu$_2$O$_{8+δ}$ (OP-Bi2212, $T_\mathrm{c}\simeq96$ K). The strong similarities in the paramagnon dispersion and in their energy at zone boundary indicate that the strength of the super-exchange interaction and the short-range magnetic correlation cannot be directly related to $T_\mathrm{c}$, not even within the same family of cuprates.

cond-mat.supr-con↗

arXiv2015

Spin-Orbit-Induced Orbital Excitations in Sr2RuO4 and Ca2RuO4: A Resonant Inelastic X-ray Scattering Study

High-resolution resonant inelastic X-ray scattering (RIXS) at the oxygen K-edge has been used to study the orbital excitations of Ca2RuO4 and Sr2RuO4. In combination with linear dichroism X-ray absorption spectroscopy, the ruthenium 4d-orbital occupation and excitations were probed through their hybridization with the oxygen p-orbitals. These results are described within a minimal model, taking into account crystal field splitting and a spin-orbit coupling λ_{so}=200~meV. The effects of spin-orbit interaction on the electronic structure and implications for the Mott and superconducting ground states of (Ca,Sr)2RuO4 are discussed.

cond-mat.str-el↗

arXiv2015

Tuning electronic correlations in transition metal pnictides: chemistry beyond the valence count

The effects of electron-electron correlations on the low-energy electronic structure and their relationship with unconventional superconductivity are central aspects in the research on the iron-based pnictide superconductors. Here we use soft X-ray angle-resolved photoemission spectroscopy (SX-ARPES) to study how electronic correlations evolve in different chemically substituted iron pnictides. We find that correlations are intrinsically related to the effective filling of the correlated orbitals, rather than to the filling obtained by valence counting. Combined density functional theory (DFT) and dynamical mean-field theory (DMFT) calculations capture these effects, reproducing the experimentally observed trend in the correlation strength. The occupation-driven trend in the electronic correlation reported in our work supports the recently proposed connection between cuprate and pnictides phase diagrams.

cond-mat.supr-con↗

arXiv2015

Collective nature of spin excitations in superconducting cuprates probed by resonant inelastic x-ray scattering

We used resonant inelastic x-ray scattering (RIXS) with and without analysis of the scattered photon polarization, to study dispersive spin excitations in the high temperature superconductor YBa2Cu3O6+x over a wide range of doping levels (0.1 < x < 1). The excitation profiles were carefully monitored as the incident photon energy was detuned from the resonant condition, and the spin excitation energy was found to be independent of detuning for all x. These findings demonstrate that the largest fraction of the spin-flip RIXS profiles in doped cuprates arises from magnetic collective modes, rather than from incoherent particle-hole excitations as recently suggested theoretically [Benjamin et al. Phys. Rev. Lett. 112, 247002(2014)]. Implications for the theoretical description of the electron system in the cuprates are discussed.

cond-mat.supr-con↗

arXiv2014

Dimensionality-tuned electronic structure of nickelate superlattices explored by soft-x-ray angle resolved photoelectron spectroscopy

The electronic and magnetic properties of epitaxial LaNiO3/LaAlO3 superlattices can be tuned by layer thickness and substrate-induced strain. Here, we report on direct measurements of the k-space-resolved electronic structure of buried nickelate layers in superlattices under compressive strain by soft x-ray photoemission. After disentangling strong extrinsic contributions to the angle-dependent signal caused by photoelectron diffraction, we are able to extract Fermi surface information from our data. We find that with decreasing LaNiO3 thickness down to two unit cells (2 uc) quasiparticle coherence becomes strongly reduced, in accord with the dimension-induced metal-to-insulator transition seen in transport measurements. Nonetheless, on top of a strongly incoherent background a residual Fermi surface can be identified in the 2 uc superlattice whose nesting properties are consistent with the spin-density wave (SDW) instability recently reported. The overall behavior of the Ni 3d spectra and the absence of a complete gap opening indicate that the SDW phase is dominated by strong order parameter fluctuations.

cond-mat.str-el↗

arXiv2014

Itinerant effects and enhanced magnetic interactions in Bi-based multilayer cuprates

The cuprate high temperature superconductors exhibit a pronounced trend in which the superconducting transition temperature, $T_{\rm c}$, increases with the number of CuO$_2$ planes, $n$, in the crystal structure. We compare the magnetic excitation spectrum of Bi$_{2+x}$Sr$_{2-x}$CuO$_{6+δ}$ (Bi-2201) and Bi$_2$Sr$_2$Ca$_2$Cu$_3$O$_{10 + δ}$ (Bi-2223), with $n=1$ and $n=3$ respectively, using Cu $L_3$-edge resonant inelastic x-ray scattering (RIXS). Near the anti-nodal zone boundary we find the paramagnon energy in Bi-2223 is substantially higher than that in Bi-2201, indicating that multilayer cuprates host stronger effective magnetic exchange interactions, providing a possible explanation for the $T_{\rm c}$ vs.\ $n$ scaling. In contrast, the nodal direction exhibits very strongly damped, almost non-dispersive excitations. We argue that this implies that the magnetism in the doped cuprates is partially itinerant in nature.

cond-mat.supr-con↗

arXiv2014

Mixed Dimensionality of Confined Conducting Electrons in the Surface Region of SrTiO$_{3}$

Using angle-resolved photoemission spectroscopy, we show that the recently-discovered surface state on SrTiO$_{3}$ consists of non-degenerate $t_{2g}$ states with different dimensional characters. While the $d_{xy}$ bands have quasi-2D dispersions with weak $k_{z}$ dependence, the lifted $d_{xz}$/$d_{yz}$ bands show 3D dispersions that differ significantly from bulk expectations and signal that electrons associated with those orbitals permeate the near-surface region. Like their more 2D counterparts, the size and character of the $d_{xz}$/$d_{yz}$ Fermi surface components are essentially the same for different sample preparations. Irradiating SrTiO$_{3}$ in ultrahigh vacuum is one method observed so far to induce the "universal" surface metallic state. We reveal that during this process, changes in the oxygen valence band spectral weight that coincide with the emergence of surface conductivity are disproportionate to any change in the total intensity of the O $1s$ core level spectrum. This signifies that the formation of the metallic surface goes beyond a straightforward chemical doping scenario and occurs in conjunction with profound changes in the initial states and/or spatial distribution of near-$E_{F}$ electrons in the surface region.

cond-mat.mtrl-sci↗

arXiv2014

Inelastic X-ray scattering from valence electrons near absorption edges of FeTe and TiSe$_2$

We study resonant inelastic x-ray scattering (RIXS) peaks corresponding to low energy particle-hole excited states of metallic FeTe and semi-metallic TiSe$_2$ for photon incident energy tuned near the $L_{3}$ absorption edge of Fe and Ti respectively. We show that the cross section amplitudes are well described within a renormalization group theory where the effect of the core electrons is captured by effective dielectric functions expressed in terms of the the atomic scattering parameters $f_1$ of Fe and Ti. This method can be used to extract the dynamical structure factor from experimental RIXS spectra in metallic systems.

cond-mat.mtrl-sci↗