arXiv subjects

T. Schmitt

Publications and source records attributed to T. Schmitt.

At least 37 records · Page 2Linked to original sources

arXiv2019

Resolving the nature of electronic excitations in resonant inelastic x-ray scattering

The study of elementary bosonic excitations is essential toward a complete description of quantum electronic solids. In this context, resonant inelastic X-ray scattering (RIXS) has recently risen to becoming a versatile probe of electronic excitations in strongly correlated electron systems. The nature of the radiation-matter interaction endows RIXS with the ability to resolve the charge, spin and orbital nature of individual excitations. However, this capability has been only marginally explored to date. Here, we demonstrate a systematic method for the extraction of the character of excitations as imprinted in the azimuthal dependence of the RIXS signal. Using this novel approach, we resolve the charge, spin, and orbital nature of elastic scattering, (para-)magnon/bimagnon modes, and higher energy dd excitations in magnetically-ordered and superconducting copper-oxide perovskites (Nd2CuO4 and YBa2Cu3O6.75). Our method derives from a direct application of scattering theory, enabling us to deconstruct the complex scattering tensor as a function of energy loss. In particular, we use the characteristic tensorial nature of each excitation to precisely and reliably disentangle the charge and spin contributions to the low energy RIXS spectrum. This procedure enables to separately track the evolution of spin and charge spectral distributions in cuprates with doping. Our results demonstrate a new capability that can be integrated into the RIXS toolset, and that promises to be widely applicable to materials with intertwined spin, orbital, and charge excitations.

cond-mat.str-el↗

arXiv2018

Site selective spin and orbital excitations in Fe3O4

$Fe_3O_4$ is a mixed-valence strongly correlated transition metal oxide which displays the intriguing metal to insulator Verwey transition. Here we investigate the electronic and magnetic structure of $Fe_3O_4$ by a unique combination of high-resolution Fe 2p3d resonant inelastic scattering magnetic circular (RIXS-MCD) and magnetic linear (RIXS-MLD) dichroism. We show that by coupling the site selectivity of RIXS with the magnetic selectivity imposed by the incident polarization handedness, we can unambiguously identify spin-flip excitations and quantify the exchange interaction of the different sublattices. Furthermore, our RIXS-MLD measurements show spin-orbital excitations that exhibit strong polarization and magnetic field dependence. Guided by theoretical simulations, we reveal that the angular dependence arises from a strong interplay between trigonal crystal-field, magnetic exchange and spin-orbit interaction at the nominal $Fe^{2+}$ sites. Our results highlight the capabilities of RIXS magnetic dichroism studies to investigate the ground state of complex systems where in-equivalent sites and bonds are simultaneously present.

cond-mat.str-el↗

arXiv2018

Three-Dimensional Fermi Surface of Overdoped La-Based Cuprates

We present a soft x-ray angle-resolved photoemission spectroscopy study of the overdoped high-temperature superconductors La$_{2-x}$Sr$_x$CuO$_4$ and La$_{1.8-x}$Eu$_{0.2}$Sr$_x$CuO$_4$. In-plane and out-of-plane components of the Fermi surface are mapped by varying the photoemission angle and the incident photon energy. No $k_z$ dispersion is observed along the nodal direction, whereas a significant antinodal $k_z$ dispersion is identified. Based on a tight-binding parametrization, we discuss the implications for the density of states near the van-Hove singularity. Our results suggest that the large electronic specific heat found in overdoped La$_{2-x}$Sr$_x$CuO$_4$ can not be assigned to the van-Hove singularity alone. We therefore propose quantum criticality induced by a collapsing pseudogap phase as a plausible explanation for observed enhancement of electronic specific heat.

cond-mat.supr-con↗

arXiv2018

Three-dimensional Fermi surface of 2H-NbSe$_2$ - Implications for the mechanism of charge density waves

We investigate the three-dimensional electronic structure of the seminal charge-density-wave (CDW) material 2H-NbSe$_2$ by soft x-ray angle-resolved photoelectron spectroscopy and density-functional theory. Our results reveal the pronounced 3D character of the electronic structure formed in the quasi-two-dimensional layered crystal structure. In particular, we find a strong dispersion along $k_z$ excluding a nesting-driven CDW formation based on experimental data. The 3D-like band structure of 2H-NbSe$_2$ has strong implications for the intriguing phase competition of CDW order with superconductivity.

cond-mat.supr-con↗

arXiv2018

Comment on `Oxygen vacancy-induced magnetic moment in edge-sharing CuO$_{2}$ chains of Li$_{2}$CuO$_{2}$'

In a recent work devoted to the magnetism of Li$_{2}$CuO$_{2}$, Shu et al. [New J. Phys. 19 (2017) 023026] have proposed a "simplified" unfrustrated microscopic model that differs considerably from the models refined through decades of prior work. We show that the proposed model is at odds with known experimental data, including the reported magnetic susceptibility $χ(T)$ data up to 550~K. Using an 8$^{\rm th}$ order high-temperature expansion for $χ(T)$, we show that the experimental data for Li$_{2}$CuO$_{2}$ are consistent with the prior model derived from inelastic neutron scattering (INS) studies. We also establish the $T$-range of validity for a Curie-Weiss law for the real frustrated magnetic system. We argue that the knowledge of the long-range ordered magnetic structure for $T<T_N$ and of $χ(T)$ in a restricted $T$-range provides insufficient information to extract all of the relevant couplings in frustrated magnets; the saturation field and INS data must also be used to determine several exchange couplings, including the weak but decisive frustrating antiferromagnetic (AFM) interchain couplings.

cond-mat.str-el↗

arXiv2018

k-Space imaging of anisotropic 2D electron gas in GaN/GaAlN high-electron-mobility transistor heterostructures

Nanostructures based on buried interfaces and heterostructures are at the heart of modern semiconductor electronics as well as future devices utilizing spintronics, multiferroics, topological effects and other novel operational principles. Knowledge of electronic structure of these systems resolved in electron momentum k delivers unprecedented insights into their physics. Here, we explore 2D electron gas formed in GaN/AlGaN high-electron-mobility transistor (HEMT) heterostructures with an ultrathin barrier layer, key elements in current high-frequency and high-power electronics. Its electronic structure is accessed with angle-resolved photoelectron spectroscopy whose probing depth is pushed to a few nm using soft-X-ray synchrotron radiation. The experiment yields direct k-space images of the electronic structure fundamentals of this system: the Fermi surface, band dispersions and occupancy, and the Fourier composition of wavefunctions encoded in the k-dependent photoemission intensity. We discover significant planar anisotropy of the electron Fermi surface and effective mass connected with relaxation of the interfacial atomic positions, which translates into non-linear (high-field) transport properties of the GaN/AlGaN heterostructures as an anisotropy of the saturation drift velocity of the 2D electrons.

cond-mat.mtrl-sci↗

arXiv2018

RIXS studies of magnons and bimagnons in the lightly doped cuprate La2-xSrxCuO4

We investigated the doping dependence of magnetic excitations in the lightly doped cuprate La2-xSrxCuO4 via combined studies of resonant inelastic x-ray scattering (RIXS) at the Cu L3-edge and theoretical calculations. With increasing doping, the magnon dispersion is found to be essentially unchanged, but the spectral width broadens and the spectral weight varies differently at different momenta. Near the Brillouin zone center, we directly observe bimagnon excitations which possess the same energy scale and doping dependence as previously observed by Raman spectroscopy. They disperse weakly in energy-momentum space, and are consistent with a bimagnon dispersion that is renormalized by the magnon-magnon interaction at the zone center.

cond-mat.supr-con↗

arXiv2018

Direct observation of multi-spinon excitations outside of the two-spinon continuum in the antiferromagnetic spin chain cuprate Sr2CuO3

One-dimensional (1D) magnetic insulators have attracted significant interest as a platform for studying emergent phenomena such as quasiparticle fractionalization and quantum criticality. The antiferromagnetic Heisenberg chain of spins-1/2 is an important reference system; its elementary excitations are spin-1/2 quasiparticles called spinons that are always created in pairs. However, while inelastic neutron scattering (INS) experiments routinely observe the excitation continuum associated with two-spinon states, the presence of more complex dynamics associated with four-spinon states has only been inferred from comparison with theory. Here, we show that resonant inelastic x-ray scattering (RIXS) is capable of accessing the four-spinon excitations directly, in a spectroscopic region separated from the two-spinon continuum. Our results provide the first direct measurement of four-spinon excitations, which is made possible by the fundamentally different correlation functions probed by RIXS compared to INS. This advance holds great promise as a tool in the search for novel quantum states, in particular quantum spin liquids.

cond-mat.str-el↗

arXiv2018

Spin-Orbital Excitations in Ca$_{2}$RuO$_4$ Revealed by Resonant Inelastic X-ray Scattering

The strongly correlated insulator Ca$_{2}$RuO$_4$ is considered as a paradigmatic realization of both spin-orbital physics and a band-Mott insulating phase, characterized by orbitally selective coexistence of a band and a Mott gap. We present a high-resolution oxygen $K$-edge resonant inelastic X-ray scattering study of the antiferromagnetic Mott insulating state of Ca$_{2}$RuO$_4$. A set of low-energy ($\sim$80 and 400 meV) and high-energy ($\sim$1.3 and 2.2 eV) excitations are reported that show strong incident light polarization dependence. Our results strongly support a spin-orbit coupled band-Mott scenario and explore in detail the nature of its exotic excitations. Guided by theoretical modelling, we interpret the low-energy excitations as a result of composite spin-orbital excitations. Their nature unveil the intricate interplay of crystal-field splitting and spin-orbit coupling in the band-Mott scenario. The high-energy excitations correspond to intra-atomic singlet-triplet transitions at an energy scale set by the Hund's coupling. Our findings give a unifying picture of the spin and orbital excitations in the band-Mott insulator Ca$_{2}$RuO$_4$.

cond-mat.str-el↗

arXiv2017

Weakly-correlated nature of ferromagnetism in non symmorphic CrO$_2$ revealed by bulk-sensitive soft X ray ARPES

Chromium dioxide CrO$_2$ belongs to a class of materials called ferromagnetic half-metals, whose peculiar aspect is to act as a metal in one spin orientation and as semiconductor or insulator in the opposite one. Despite numerous experimental and theoretical studies motivated by technologically important applications of this material in spintronics, its fundamental properties such as momentum resolved electron dispersions and Fermi surface have so far remained experimentally inaccessible due to metastability of its surface that instantly reduces to amorphous Cr$_2$O$_3$. In this work, we demonstrate that direct access to the native electronic structure of CrO$_2$ can be achieved with soft-X-ray angle-resolved photoemission spectroscopy whose large probing depth penetrates through the Cr$_2$O$_3$ layer. For the first time the electronic dispersions and Fermi surface of CrO$_2$ are measured, which are fundamental prerequisites to solve the long debate on the nature of electronic correlations in this material. Since density functional theory augmented by a relatively weak local Coulomb repulsion gives an exhaustive description of our spectroscopic data, we rule out strong-coupling theories of CrO$_2$. Crucial for the correct interpretation of our experimental data in terms of the valence band dispersions is the understanding of a non-trivial spectral response of CrO$_2$ caused by interference effects in the photoemission process originating from the non-symmorphic space group of the rutile crystal structure of CrO$_2$.

cond-mat.mtrl-sci↗

arXiv2017

Electronic and magnetic excitations in the "half-stuffed" Cu--O planes of Ba$_2$Cu$_3$O$_4$Cl$_2$ measured by resonant inelastic x-ray scattering

We use resonant inelastic x-ray scattering (RIXS) at the Cu L$_3$ edge to measure the charge and spin excitations in the "half-stuffed" Cu--O planes of the cuprate antiferromagnet Ba$_2$Cu$_3$O$_4$Cl$_2$. The RIXS line shape reveals distinct contributions to the $dd$ excitations from the two structurally inequivalent Cu sites, which have different out-of-plane coordinations. The low-energy response exhibits magnetic excitations. We find a spin-wave branch whose dispersion follows the symmetry of a CuO$_2$ sublattice, similar to the case of the "fully-stuffed" planes of tetragonal CuO (T-CuO). Its bandwidth is closer to that of a typical cuprate material, such as Sr$_2$CuO$_2$Cl$_2$, than it is to that of T-CuO. We interpret this result as arising from the absence of the effective four-spin inter-sublattice interactions that act to reduce the bandwidth in T-CuO.

cond-mat.str-el↗

arXiv2017

Crossover from Collective to Incoherent Spin Excitations in Superconducting Cuprates Probed by Detuned Resonant Inelastic X-ray Scattering

Spin excitations in the overdoped high temperature superconductors Tl$_2$Ba$_2$CuO$_{6+δ}$ and (Bi,Pb)$_2$(Sr,La)$_{2}$CuO$_{6+δ}$ were investigated by resonant inelastic x-ray scattering (RIXS) as functions of doping and detuning of the incoming photon energy above the Cu-$L_3$ absorption peak. The RIXS spectra at optimal doping are dominated by a paramagnon feature with peak energy independent of photon energy, similar to prior results on underdoped cuprates. Beyond optimal doping, the RIXS data indicate a sharp crossover to a regime with a strong contribution from incoherent particle/hole excitations whose maximum shows a fluorescence-like shift upon detuning. The spectra of both compound families are closely similar, and their salient features are reproduced by exact-diagonalization calculations of the single-band Hubbard model on a finite cluster. The results are discussed in the light of recent transport experiments indicating a quantum phase transition near optimal doping.

cond-mat.supr-con↗

arXiv2017

Damped spin excitations in a doped cuprate superconductor with orbital hybridization

A resonant inelastic x-ray scattering (RIXS) study of overdamped spin-excitations in slightly underdoped La$_{2-x}$Sr$_{x}$CuO$_4$ (LSCO) with $x=0.12$ and $0.145$ is presented. Three high-symmetry directions have been investigated: (1) the antinodal $(0,0)\rightarrow (1/2,0)$, (2) the nodal $(0,0)\rightarrow (1/4,1/4)$ and (3) the zone boundary direction $(1/2,0)\rightarrow (1/4,1/4)$ connecting these two. The overdamped excitations exhibit strong dispersions along (1) and (3), whereas a much more modest dispersion is found along (2). This is in strong contrast to the undoped compound La$_{2}$CuO$_4$ (LCO) for which the strongest dispersions are found along (1) and (2). The $t-t^{\prime}-t^{\prime\prime}-U$ Hubbard model used to explain the excitation spectrum of LCO predicts $-$ for constant $U/t$ $-$ that the dispersion along (3) scales with $(t^{\prime}/t)^2$. However, the diagonal hopping $t^{\prime}$ extracted on LSCO using single-band models is low ($t^{\prime}/t\sim-0.16$) and decreasing with doping. We therefore invoked a two-orbital ($d_{x^2-y^2}$ and $d_{z^2}$) model which implies that $t^{\prime}$ is enhanced. This effect acts to enhance the zone-boundary dispersion within the Hubbard model. We thus conclude that hybridization of $d_{x^2-y^2}$ and $d_{z^2}$ states has a significant impact on the zone-boundary dispersion in LSCO.

cond-mat.supr-con↗

arXiv2017

Resonant inelastic X-ray scattering study of spin-wave excitations in the cuprate parent compound Ca$_{2}$CuO$_2$Cl$_2$

By means of resonant inelastic x-ray scattering at the Cu L$_3$ edge, we measured the spin wave dispersion along $\langle$100$\rangle$ and $\langle$110$\rangle$ in the undoped cuprate Ca$_2$CuO$_2$Cl$_2$. The data yields a reliable estimate of the superexchange parameter $J$ = 135 $\pm$ 4 meV using a classical spin-1/2 2D Heisenberg model with nearest-neighbor interactions and including quantum fluctuations. Including further exchange interactions increases the estimate to $J$ = 141 meV. The 40 meV dispersion between the magnetic Brillouin zone boundary points (1/2,\,0) and (1/4,\,1/4) indicates that next-nearest neighbor interactions in this compound are intermediate between the values found in La$_{2}$CuO$_4$ and Sr$_2$CuO$_2$Cl$_2$. Owing to the low-$Z$ elements composing Ca$_2$CuO$_2$Cl$_2$, the present results may enable a reliable comparison with the predictions of quantum many-body calculations, which would improve our understanding of the role of magnetic excitations and of electronic correlations in cuprates.

cond-mat.str-el↗

arXiv2017

Observation of a dispersive charge mode in hole-doped cuprates using resonant inelastic x-ray scattering at the oxygen K edge

We investigate electronic excitations in La2-x(Br,Sr)xCuO4 using resonant inelastic x-ray scattering (RIXS) at the oxygen K edge. RIXS spectra of the hole-doped cuprates show clear momentum dependence below 1 eV. The spectral weight exhibits positive dispersion and shifts to higher energy with increasing hole concentration. Theoretical calculation of the dynamical charge structure factor on oxygen orbitals in a three-band Hubbard model is consistent with the experimental observation of the momentum and doping dependence, and therefore the dispersive mode is ascribed to intraband charge excitations which have been observed in electron-doped cuprates.

cond-mat.str-el↗

arXiv2017

Doping Dependence of Collective Spin and Orbital Excitations in Spin 1 Quantum Antiferromagnet La$_{2-x}$Sr$_x$NiO$_4$ Observed by X-rays

We report the first empirical demonstration that resonant inelastic x-ray scattering (RIXS) is sensitive to \emph{collective} magnetic excitations in $S=1$ systems by probing the Ni $L_3$-edge of La$_{2-x}$Sr$_x$NiO$_4$ ($x = 0, 0.33, 0.45$). The magnetic excitation peak is asymmetric, indicating the presence of single and multi spin-flip excitations. As the hole doping level is increased, the zone boundary magnon energy is suppressed at a much larger rate than that in hole doped cuprates. Based on the analysis of the orbital and charge excitations observed by RIXS, we argue that this difference is related to the orbital character of the doped holes in these two families. This work establishes RIXS as a probe of fundamental magnetic interactions in nickelates opening the way towards studies of heterostructures and ultra-fast pump-probe experiments.

cond-mat.str-el↗

arXiv2017

Three-Dimensional Electronic Structure of type-II Weyl Semimetal WTe$_2$

By combining bulk sensitive soft-X-ray angular-resolved photoemission spectroscopy and accurate first-principles calculations we explored the bulk electronic properties of WTe$_2$, a candidate type-II Weyl semimetal featuring a large non-saturating magnetoresistance. Despite the layered geometry suggesting a two-dimensional electronic structure, we find a three-dimensional electronic dispersion. We report an evident band dispersion in the reciprocal direction perpendicular to the layers, implying that electrons can also travel coherently when crossing from one layer to the other. The measured Fermi surface is characterized by two well-separated electron and hole pockets at either side of the $Γ$ point, differently from previous more surface sensitive ARPES experiments that additionally found a significant quasiparticle weight at the zone center. Moreover, we observe a significant sensitivity of the bulk electronic structure of WTe$_2$ around the Fermi level to electronic correlations and renormalizations due to self-energy effects, previously neglected in first-principles descriptions.

cond-mat.mtrl-sci↗

arXiv2016

Doping dependence of the magnetic excitations in La$_{2-x}$Sr$_x$CuO$_4$

The magnetic correlations within the cuprates have undergone intense scrutiny as part of efforts to understand high temperature superconductivity. We explore the evolution of the magnetic correlations along the nodal direction of the Brillouin zone in La2-xSrxCuO4, spanning the doping phase diagram from the anti-ferromagnetic Mott insulator at x = 0 to the metallic phase at x = 0.26. Magnetic excitations along this direction are found to be systematically softened and broadened with doping, at a higher rate than the excitations along the anti-nodal direction. This phenomenology is discussed in terms of the nature of the magnetism in the doped cuprates. Survival of the high energy magnetic excitations, even in the overdoped regime, indicates that these excitations are marginal to pairing, while the influence of the low energy excitations remains ambiguous.

cond-mat.str-el↗