arXiv subjects

M. W. Haverkort

Publications and source records attributed to M. W. Haverkort.

At least 37 records · Page 2Linked to original sources

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↗

arXiv2016

Long-range interactions in the effective low energy Hamiltonian of Sr2IrO4: a core level resonant inelastic x-ray scattering study

We have investigated the electronic structure of Sr2IrO4 using core level resonant inelastic x-ray scattering. The experimental spectra can be well reproduced using ab initio density functional theory based multiplet ligand field theory calculations, thereby validating these calculations. We found that the low-energy, effective Ir t2g orbitals are practically degenerate in energy. We uncovered that covalency in Sr2IrO4, and generally in iridates, is very large with substantial oxygen ligand hole character in the Ir t2g Wannier orbitals. This has far reaching consequences, as not only the onsite crystal-field energies are determined by the long range crystal-structure, but, more significantly, magnetic exchange interactions will have long range distance dependent anisotropies in the spin direction. These findings set constraints and show pathways for the design of d^5 materials that can host compass-like magnetic interactions.

cond-mat.str-el↗

arXiv2016

The quartet ground state in CeB$_6$: an inelastic x-ray scattering study

We investigated the ground state symmetry of the cubic hidden order compound CeB$_6$ by means of core level non-resonant inelastic x-ray scattering (NIXS). The information is obtained from the directional dependence of the scattering function that arises from higher than dipole transitions. Our new method confirms that the ground state is well described using a localized crystal-field model assuming a $Γ_8$ quartet ground state.

cond-mat.str-el↗

arXiv2016

Quantitative determination of bond order and lattice distortions in nickel oxide heterostructures by resonant x-ray scattering

We present a combined study of Ni $K$-edge resonant x-ray scattering and density functional calculations to probe and distinguish electronically driven ordering and lattice distortions in nickelate heterostructures. We demonstrate that due to the low crystal symmetry, contributions from structural distortions can contribute significantly to the energy-dependent Bragg peak intensities of a bond-ordered NdNiO$_3$ reference film. For a LaNiO$_3$-LaAlO$_3$ superlattice that exhibits magnetic order, we establish a rigorous upper bound on the bond-order parameter. We thus conclusively confirm predictions of a dominant spin density wave order parameter in metallic nickelates with a quasi-two-dimensional electronic structure.

cond-mat.str-el↗

arXiv2016

Exploring small energy scales with x-ray absorption and dichroism

Soft x-ray linear and circular dichroism (XLD, XMCD) experiments at the Ce M$_{4,5}$ edges are being used to determine the energy scales characterizing the Ce $4f$ degrees of freedom in the ultrathin ordered surface intermetallic CeAg$_x$/Ag(111). We find that all relevant interactions, i. e. Kondo scattering, crystal field splitting and magnetic exchange coupling occur on small scales. Our study demonstrates the usefulness of combining x-ray absorption experiments probing linear and circular dichroism owing to their strong sensitivity for anisotropies in both charge distribution and paramagnetic response, respectively.

cond-mat.str-el↗

arXiv2015

CeRu$_4$Sn$_6$: a strongly correlated material with nontrivial topology

Topological insulators form a novel state of matter that provides new opportunities to create unique quantum phenomena. While the materials used so far are based on semiconductors, recent theoretical studies predict that also strongly correlated systems can show non-trivial topological properties, thereby allowing even the emergence of surface phenomena that are not possible with topological band insulators. From a practical point of view, it is also expected that strong correlations will reduce the disturbing impact of defects or impurities, and at the same increase the Fermi velocities of the topological surface states. The challenge is now to discover such correlated materials. Here, using advanced x-ray spectroscopies in combination with band structure calculations, we infer that CeRu$_4$Sn$_6$ is a strongly correlated material with non-trivial topology.

cond-mat.str-el↗

arXiv2015

Quantitative study of valence and configuration interaction parameters of the Kondo semiconductors CeM2Al10 (M = Ru, Os and Fe) by means of bulk-sensitive hard x-ray photoelectron spectroscopy

The occupancy of the 4f^n contributions in the Kondo semiconductors CeM2Al10(M = Ru, Os and Fe) has been quantitatively determined by means of bulk-sensitive hard x-ray photoelectron spectroscopy (HAXPES) on the Ce 3d core levels. Combining a configuration interaction scheme with full multiplet calculations allowed to accurately describe the HAXPES data despite the presence of strong plasmon excitations in the spectra. The configuration interaction parameters obtained from this analysis -- in particular the hybridization strength V_eff and the effective f binding energy Delta_f -- indicate a slightly stronger exchange interaction in CeOs2Al10 compared to CeRu2Al10, and a significant increase in CeFe2Al10. This verifies the coexistence of a substantial amount of Kondo screening with magnetic order and places the entire CeM2Al10 family in the region of strong exchange interactions.

cond-mat.str-el↗

arXiv2014

Bands, resonances, edge singularities and excitons in core level spectroscopy investigated within the dynamical mean field theory

Using a recently developed impurity solver we exemplify how dynamical mean field theory captures band excitations, resonances, edge singularities and excitons in core level x-ray absorption (XAS) and core level photo electron spectroscopy (cPES) on metals, correlated metals and Mott insulators. Comparing XAS at different values of the core-valence interaction shows how the quasiparticle peak in the absence of core-valence interactions evolves into a resonance of similar shape, but different origin. Whereas XAS is rather insensitive to the metal insulator transition, cPES can be used, due to nonlocal screening, to measure the amount of local charge fluctuation.

cond-mat.str-el↗

arXiv2014

Efficient real frequency solver for dynamical mean field theory

We here present how a self-consistent solution of the dynamical mean field theory equations can be obtained using exact diagonalization of an Anderson impurity model with accuracies comparable to those found using renormalization group or quantum Monte Carlo methods. We show how one can solve a correlated quantum impurity coupled to several hundred uncorrelated bath sites, using a restricted active basis set. The number of bath sites determines the resolution of the obtained spectral function, which consists of peaks roughly spaced by the band width divided by the number of bath sites. The self-consistency cycles are fully performed on the real frequency axis and expressed as numerical stable matrix operations. The same impurity solver has been used on Ligand Field and finite size cluster calculations and is capable of treating involved Hamiltonians including the full rotational invariant Coulomb interaction, spin-orbit coupling and low symmetry crystal-fields. The proposed method allows for the calculation of a variety of correlation functions at little extra cost.

cond-mat.str-el↗

arXiv2014

Photoelectron spin-polarization-control in the topological insulator Bi2Se3

We study the manipulation of the photoelectron spin-polarization in Bi$_2$Se$_3$ by spin- and angle-resolved photoemission spectroscopy. General rules are established that enable controlling the spin-polarization of photoemitted electrons via light polarization, sample orientation, and photon energy. We demonstrate the $\pm$100% reversal of a single component of the measured spin-polarization vector upon the rotation of light polarization, as well as a full three-dimensional manipulation by varying experimental configuration and photon energy. While a material-specific density-functional theory analysis is needed for the quantitative description, a minimal two-atomic-layer model qualitatively accounts for the spin response based on the interplay of optical selection rules, photoelectron interference, and topological surface-state complex structure. It follows that photoelectron spin-polarization control is generically achievable in systems with a layer-dependent, entangled spin-orbital texture.

cond-mat.mtrl-sci↗

arXiv2014

Breakdown of singlets and triplets in Sr2RuO4 revealed by spin-resolved ARPES

Spin-orbit coupling has been conjectured to play a key role in the low-energy electronic structure of Sr2RuO4. Using circularly polarized light combined with spin- and angle-resolved photoemission spectroscopy, we directly measure the value of the effective spin-orbit coupling to be 130 +/- 30 meV. This is even larger than theoretically predicted and comparable to the energy splitting of the dxy and dxz,yz orbitals around the Fermi surface, resulting in a strongly momentum-dependent entanglement of spin and orbital character. As demonstrated by the spin expectation value obtained for a pair of electrons with zero total momentum, the classification of the Cooper pairs in terms of pure singlets or triplets fundamentally breaks down, necessitating a description of the unconventional superconducting state of Sr2RuO4 in terms of these newly found spin-orbital entangled eigenstates.

cond-mat.supr-con↗

arXiv2013

Strain and composition dependence of the orbital polarization in nickelate superlattices

A combined analysis of x-ray absorption and resonant reflectivity data was used to obtain the orbital polarization profiles of superlattices composed of four-unit-cell-thick layers of metallic LaNiO3 and layers of insulating RXO3 (R=La, Gd, Dy and X=Al, Ga, Sc), grown on substrates that impose either compressive or tensile strain. This superlattice geometry allowed us to partly separate the influence of epitaxial strain from interfacial effects controlled by the chemical composition of the insulating blocking layers. Our quantitative analysis reveal orbital polarizations up to 25%. We further show that strain is the most effective control parameter, whereas the influence of the chemical composition of the blocking layers is comparatively small.

cond-mat.str-el↗

arXiv2013

Orbital superexchange and crystal field simultaneously at play in YVO3: resonant inelastic x-ray scattering at the V L edge and the O K edge

We report on the observation of orbital excitations in YVO3 by means of resonant inelastic x-ray scattering (RIXS) at energies across the vanadium L3 and oxygen K absorption edges. Due to the excellent experimental resolution we are able to resolve the intra-t2g excitations at 0.1-0.2 eV, 1.07 eV, and 1.28 eV, the lowest excitations from the t2g into the eg levels at 1.86 eV, and further excitations above 2.2 eV. For the intra-t2g excitations at 0.1-0.2 eV, the RIXS peaks show small shifts of the order of 10-40 meV as a function of temperature and of about 13-20 meV as a function of the transferred momentum q||a. We argue that the latter reflects a finite dispersion of the orbital excitations. For incident energies tuned to the oxygen K edge, RIXS is more sensitive to intersite excitations. We observe excitations across the Mott-Hubbard gap and find an additional feature at 0.4 eV which we attribute to two-orbiton scattering, i.e., an exchange of orbitals between adjacent sites. Altogether, these results indicate that both superexchange interactions and the coupling to the lattice are important for a quantitative understanding of the orbital excitations in YVO3.

cond-mat.str-el↗

arXiv2013

Layer-by-layer entangled spin-orbital texture of the topological surface state in Bi2Se3

We study Bi2Se3 by polarization-dependent angle-resolved photoemission spectroscopy (ARPES) and density-functional theory slab calculations. We find that the surface state Dirac fermions are characterized by a layer-dependent entangled spin-orbital texture, which becomes apparent through quantum interference effects. This explains the discrepancy between the spin polarization from spin-resovled ARPES - ranging from 20 to 85% - and the 100% value assumed in phenomenological models. It also suggests a way to probe the intrinsic spin texture of topological insulators, and to continuously manipulate the spin polarization of photoelectrons and photocurrents all the way from 0 to +/-100% by an appropriate choice of photon energy, linear polarization, and angle of incidence.

cond-mat.mtrl-sci↗

arXiv2013

Orbital control of noncollinear magnetic order in nickelate heterostructures

We have used resonant x-ray diffraction to develop a detailed description of antiferromagnetic ordering in epitaxial superlattices based on two-unit-cell thick layers of the strongly correlated metal LaNiO3. We also report reference experiments on thin films of PrNiO3 and NdNiO3. The resulting data indicate a spiral state whose polarization plane can be controlled by adjusting the Ni d-orbital occupation via two independent mechanisms: epitaxial strain and quantum confinement of the valence electrons. The data are discussed in the light of recent theoretical predictions.

cond-mat.str-el↗

arXiv2012

Crystal-field ground state of the orthorhombic Kondo insulator CeRu2Al10

We have succeeded in establishing the crystal-field ground state of CeRu2Al10, an orthorhombic intermetallic compound recently identified as a Kondo insulator. Using polarization dependent soft x-ray absorption spectroscopy at the Ce M4,5 edges, together with input from inelastic neutron and magnetic susceptibility experiments, we were able to determine unambiguously the orbital occupation of the 4f shell and to explain quantitatively both the measured magnetic moment along the easy a axis and the small ordered moment along the c-axis. The results provide not only a platform for a realistic modeling of the spin and charge gap of CeRu2Al10, but demonstrate also the potential of soft x-ray absorption spectroscopy to obtain information not easily accessible by neutron techniques for the study of Kondo insulators in general.

cond-mat.str-el↗

arXiv2012

Mott versus Slater-type metal-insulator transition in Mn-substituted Sr3Ru2O7

We present a temperature-dependent x-ray absorption (XAS) and resonant elastic x-ray scattering (REXS) study of the metal-insulator transition (MIT) in Sr3(Ru1-xMnx)2O7. The XAS results reveal that the MIT drives the onset of local antiferromagnetic correlations around the Mn impurities, a precursor of the long-range antiferromagnetism detected by REXS at T_order<T_MIT. This establishes that the MIT is of the Mott-type (electronic correlations) as opposed to Slater-type (magnetic order). While this behavior is induced by Mn impurities, the (1/4,1/4,0) order exists for a wide range of Mn concentrations, and points to an inherent instability of the parent compound.

cond-mat.str-el↗

arXiv2012

Spin-Orbital Separation in the quasi 1D Mott-insulator Sr2CuO3

As an elementary particle the electron carries spin \hbar/2 and charge e. When binding to the atomic nucleus it also acquires an angular momentum quantum number corresponding to the quantized atomic orbital it occupies (e.g., s, p or d). Even if electrons in solids form bands and delocalize from the nuclei, in Mott insulators they retain their three fundamental quantum numbers: spin, charge and orbital[1]. The hallmark of one-dimensional (1D) physics is a breaking up of the elementary electron into its separate degrees of freedom[2]. The separation of the electron into independent quasi-particles that carry either spin (spinons) or charge (holons) was first observed fifteen years ago[3]. Using Resonant Inelastic X-ray Scattering on the 1D Mott-insulator Sr2CuO3 we now observe also the orbital degree of freedom separating. We resolve an orbiton liberating itself from spinons and propagating through the lattice as a distinct quasi-particle with a substantial dispersion of ~0.2 eV.

cond-mat.str-el↗