arXiv subjects

B. Delley

Publications and source records attributed to B. Delley.

At least 19 recordsLinked to original sources

arXiv2020

Observation of plaquette fluctuations in the spin-1/2 honeycomb lattice

Quantum spin liquids are materials that feature quantum entangled spin correlations and avoid magnetic long-range order at T = 0 K. Particularly interesting are two-dimensional honeycomb spin lattices where a plethora of exotic quantum spin liquids have been predicted. Here, we experimentally study an effective S=1/2 Heisenberg honeycomb lattice with competing nearest and next-nearest neighbor interactions. We demonstrate that YbBr$_3$ avoids order down to at least T=100 mK and features a dynamic spin-spin correlation function with broad continuum scattering typical of quantum spin liquids near a quantum critical point. The continuum in the spin spectrum is consistent with plaquette type fluctuations predicted by theory. Our study is the experimental demonstration that strong quantum fluctuations can exist on the honeycomb lattice even in the absence of Kitaev-type interactions, and opens a new perspective on quantum spin liquids.

cond-mat.str-el↗

arXiv2017

Absence of long range order in the frustrated magnet SrDy$_2$O$_4$ due to trapped defects from a dimensionality crossover

Magnetic frustration and low dimensionality can prevent long range magnetic order and lead to exotic correlated ground states. SrDy$_2$O$_4$ consists of magnetic Dy$^{3+}$ ions forming magnetically frustrated zig-zag chains along the c-axis and shows no long range order to temperatures as low as $T=60$ mK. We carried out neutron scattering and AC magnetic susceptibility measurements using powder and single crystals of SrDy$_2$O$_4$. Diffuse neutron scattering indicates strong one-dimensional (1D) magnetic correlations along the chain direction that can be qualitatively accounted for by the axial next-nearest neighbour Ising (ANNNI) model with nearest-neighbor and next-nearest-neighbor exchange $J_1=0.3$ meV and $J_2=0.2$ meV, respectively. Three-dimensional (3D) correlations become important below $T^*\approx0.7$ K. At $T=60$ mK, the short range correlations are characterized by a putative propagation vector $\textbf{k}_{1/2}=(0,\frac{1}{2},\frac{1}{2})$. We argue that the absence of long range order arises from the presence of slowly decaying 1D domain walls that are trapped due to 3D correlations. This stabilizes a low-temperature phase without long range magnetic order, but with well-ordered chain segments separated by slowly-moving domain walls.

cond-mat.str-el↗

arXiv2017

Doping-induced superconductivity of ZrB$_2$ and HfB$_2$

Unlike the widely studied $s$-type two-gap superconductor MgB$_2$, the chemically similar compounds ZrB$_2$ and HfB$_2$ do not superconduct above 1 K. Yet, it has been shown that small amounts of self- or extrinsic doping (in particular with vanadium), can induce superconductivity in these materials. Based on results of different macro- and microscopic measurements, including magnetometry, nuclear magnetic resonance (NMR), resistivity, and muon-spin rotation ($μ$SR), we present a comparative study of Zr$_{0.96}$V$_{0.04}$B$_2$ and Hf$_{0.97}$V$_{0.03}$B$_2$. Their key magnetic and superconducting features are determined and the results are considered within the theoretical framework of multiband superconductivity proposed for MgB$_2$. Detailed Fermi surface (FS) and electronic structure calculations reveal the difference between MgB$_2$ and transition-metal diborides.

cond-mat.supr-con↗

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↗

arXiv2015

Crystal structure and phonon softening in Ca3Ir4Sn13

We investigated the crystal structure and lattice excitations of the ternary intermetallic stannide Ca3Ir4Sn13 using neutron and x-ray scattering techniques. For T > T* ~ 38 K the x-ray diffraction data can be satisfactorily refined using the space group Pm-3n. Below T* the crystal structure is modulated with a propagation vector of q = (1/2, 1/2, 0). This may arise from a merohedral twinning in which three tetragonal domains overlap to mimic a higher symmetry, or from a doubling of the cubic unit cell. Neutron diffraction and neutron spectroscopy results show that the structural transition at T* is of a second-order, and that it is well described by mean-field theory. Inelastic neutron scattering data point towards a displacive structural transition at T* arising from the softening of a low-energy phonon mode with an energy gap of Delta(120 K) = 1.05 meV. Using density functional theory the soft phonon mode is identified as a 'breathing' mode of the Sn12 icosahedra and is consistent with the thermal ellipsoids of the Sn2 atoms found by single crystal diffraction data.

cond-mat.str-el↗

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↗

arXiv2012

Bulk electronic structure of superconducting LaRu2P2 single crystals measured by soft x-ray angle-resolved photoemission spectroscopy

We present a soft X-ray angle-resolved photoemission spectroscopy (SX-ARPES) study of the stoichiometric pnictide superconductor LaRu2P2. The observed electronic structure is in good agreement with density functional theory (DFT) calculations. However, it is significantly different from its counterpart in high-temperature superconducting Fe-pnictides. In particular the bandwidth renormalization present in the Fe-pnictides (~2 - 3) is negligible in LaRu2P2 even though the mass enhancement is similar in both systems. Our results suggest that the superconductivity in LaRu2P2 has a different origin with respect to the iron pnictides. Finally we demonstrate that the increased probing depth of SX-ARPES, compared to the widely used ultraviolet ARPES, is essential in determining the bulk electronic structure in the experiment.

cond-mat.supr-con↗

arXiv2012

Systematic computation of crystal field multiplets for X-ray core spectroscopies

We present a new approach to computing multiplets for core spectroscopies, whereby the crystal field is constructed explicitly from the positions and charges of surrounding atoms. The simplicity of the input allows the consideration of crystal fields of any symmetry, and in particular facilitates the study of spectroscopic effects arising from low symmetry environments. The interplay between polarization directions and crystal field can also be conveniently investigated. The determination of the multiplets proceeds from a Dirac density functional atomic calculation, followed by the exact diagonalization of the Coulomb, spin-orbit and crystal field interactions for the electrons in the open shells. The eigenstates are then used to simulate X-ray Absorption Spectroscopy and Resonant Inelastic X-ray Scattering spectra. In examples ranging from high symmetry down to low symmetry environment, comparisons with experiments are done with unadjusted model parameters as well as with semi-empirically optimized ones. Furthermore, predictions for the RIXS of low-temperature MnO and for Dy in a molecular complex are proposed.

cond-mat.other↗

arXiv2010

Evolution of the interfacial structure of LaAlO3 on SrTiO3

The evolution of the atomic structure of LaAlO3 grown on SrTiO3 was investigated using surface x-ray diffraction in conjunction with model-independent, phase-retrieval algorithms between two and five monolayers film thickness. A depolarizing buckling is observed between cation and oxygen positions in response to the electric field of polar LaAlO3, which decreases with increasing film thickness. We explain this in terms of competition between elastic strain energy, electrostatic energy, and electronic reconstructions. The findings are qualitatively reproduced by density-functional theory calculations. Significant cationic intermixing across the interface extends approximately three monolayers for all film thicknesses. The interfaces of films thinner than four monolayers therefore extend to the surface, which might affect conductivity.

cond-mat.mtrl-sci↗

arXiv2009

Evidence for weak electronic correlations in Fe-pnictides

Using x-ray absorption and resonant inelastic x-ray scattering, charge dynamics at and near the Fe $L$ edges is investigated in Fe pnictide materials, and contrasted to that measured in other Fe compounds. It is shown that the XAS and RIXS spectra for 122 and 1111 Fe pnictides are each qualitatively similar to Fe metal. Cluster diagonalization, multiplet, and density-functional calculations show that Coulomb correlations are much smaller than in the cuprates, highlighting the role of Fe metallicity and strong covalency in these materials. Best agreement with experiment is obtained using Hubbard parameters $U\lesssim 2$eV and $J\approx 0.8$eV.

cond-mat.supr-con↗

arXiv2009

Multiplets and Crystal Fields: Systematics for X-Ray Spectroscopies

An easily accessible method is presented that permits to calculate spectra involving atomic multiplets relevant to X-ray Absorption Spectroscopy (XAS) and Resonant Inelastic X-ray Scattering (RIXS) experiments. We present specific examples and compare the calculated spectra with available experimental data

cond-mat.str-el↗

arXiv2009

Collective spin excitations in a quantum spin ladder probed by high-resolution Resonant Inelastic X-ray Scattering

We investigate magnetic excitations in the spin-ladder compound Sr$_{14}$Cu$_{24}$O$_{41}$ using high-resolution Cu $L_3$-edge Resonant Inelastic X-ray Scattering (RIXS). Our findings demonstrate that RIXS couples to collective spin excitations from a quantum spin-liquid ground state. In contrast to Inelastic Neutron Scattering (INS), the RIXS cross section changes only moderately over the entire Brillouin Zone (BZ), revealing a high sensitivity also at small momentum transfers. The two-triplon energy gap is found to be $100\pm 30$ meV. Our results are supported by calculations within an effective Hubbard model for a finite-size cluster.

cond-mat.str-el↗

arXiv2008

Evidence for coupling between collective state and phonons in two-dimensional charge-density-wave systems

We report on a Raman scattering investigation of the charge-density-wave (CDW), quasi two-dimensional rare-earth tri-tellurides $R$Te$_3$ ($R$= La, Ce, Pr, Nd, Sm, Gd and Dy) at ambient pressure, and of LaTe$_3$ and CeTe$_3$ under externally applied pressure. The observed phonon peaks can be ascribed to the Raman active modes for both the undistorted as well as the distorted lattice in the CDW state by means of a first principles calculation. The latter also predicts the Kohn anomaly in the phonon dispersion, driving the CDW transition. The integrated intensity of the two most prominent modes scales as a characteristic power of the CDW-gap amplitude upon compressing the lattice, which provides clear evidence for the tight coupling between the CDW condensate and the vibrational modes.

cond-mat.str-el↗

arXiv2007

^{63,65}Cu NMR and NQR evidence for an unusual spin dynamics in PrCu_2 below 100 K

We report the results of a $^{63,65}$Cu NMR/NQR study probing the intermetallic compound PrCu$_2$. The previously claimed onset of magnetic order at 65 K, indicated in a $μ$SR study, is not confirmed. Based on our data we discuss different possible reasons for this apparent discrepancy, including a non negligible influence of the implanted muons on their environment. Competing dipolar and quadrupolar interactions lead to unusual features of the magnetic-ion/conduction-electron system, different from those of common intermetallics exhibiting structural or magnetic instabilities.

cond-mat.mtrl-sci↗

arXiv2007

Role of oxygen vacancies in Cr-doped SrTiO3 for resistance-change memory

Transition-metal oxides exhibiting a bistable resistance state are attractive for non-volatile memory applications. The relevance of oxygen vacancies (VO) for the resistance-change memory was investigated with x-ray fluorescence, infrared microscopy, and x-ray absorption spectroscopy using Cr-doped SrTiO3 as example. We propose that the microscopic origin of resistance switching in this class of materials is due to an oxygen-vacancy drift occurring in close proximity to one of the electrodes.

cond-mat.mtrl-sci↗

arXiv2007

Resistive Switching in Cr doped SrTiO3: An X-ray Absorption Spectroscopy study

X-ray absorption spectroscopy was used to study the microscopic origin of conductance and resistive switching in chromium doped strontium titanate (Cr:SrTiO3). Differences in the x-ray absorption near edge spectroscopy (XANES) at the Cr K-edge indicate that the valence of Cr changes from 3+ to 4+ underneath the anode of our sample device after the application of an electric field. Spatially resolved x-ray fluorescence microscopy ($μ$-XRF) maps show that the Cr4+ region retracts from the anode-Cr:SrTiO3 interface after a conducting state has been achieved. This interface region is studied with extended x-ray absorption fine structure (EXAFS) and the results are compared with structural parameters obtained from density functional theory (DFT) calculations. They confirm that oxygen vacancies which are localized at the octahedron with a Cr at its center are introduced at the interface. It is proposed that the switching state is not due to a valence change of chromium but caused by changes of oxygen vacancies at the interface.

cond-mat.mtrl-sci↗

arXiv2006

Questioning the existence of a unique ground state structure for Si clusters

Density functional and quantum Monte Carlo calculations challenge the existence of a unique ground state structure for certain Si clusters. For Si clusters with more than a dozen atoms the lowest ten isomers are close in energy and for some clusters entropic effects can change the energetic ordering of the configurations. Isotope pure configurations with rotational symmetry and symmetric configurations containing one additional isotope are disfavored by these effects. Comparisons with experiment are thus difficult since a mixture of configurations is to be expected at thermal equilibrium.

cond-mat.mtrl-sci↗

arXiv2004

Tunable Conductivity and Conduction Mechanism in a UV light activated electronic conductor

A tunable conductivity has been achieved by controllable substitution of a novel UV light activated electronic conductor. The transparent conducting oxide system H-doped Ca12-xMgxAl14O33 (x = 0; 0.1; 0.3; 0.5; 0.8; 1.0) presents a conductivity that is strongly dependent on the substitution level and temperature. Four-point dc-conductivity decreases with x from 0.26 S/cm (x = 0) to 0.106 S/cm (x = 1) at room temperature. At each composition the conductivity increases (reversibly with temperature) until a decomposition temperature is reached; above this value, the conductivity drops dramatically due to hydrogen recombination and loss. The observed conductivity behavior is consistent with the predictions of our first principles density functional calculations for the Mg-substituted system with x=0, 1 and 2. The Seebeck coefficient is essentially composition- and temperature-independent, the later suggesting the existence of an activated mobility associated with small polaron conduction. The optical gap measured remains constant near 2.6 eV while transparency increases with the substitution level, concomitant with a decrease in carrier content.

cond-mat.mtrl-sci↗