arXiv subjects

D. Kasinathan

Publications and source records attributed to D. Kasinathan.

At least 19 recordsLinked to original sources

arXiv2021

CaCu$_3$Ru$_4$O$_{12}$: a high Kondo-temperature transition metal oxide

We present a comprehensive study of CaCu$_3$Ru$_4$O$_{12}$ using bulk sensitive hard and soft x-ray spectroscopy combined with local-density approximation (LDA) + dynamical mean-field theory (DMFT) calculations. Correlation effects on both the Cu and Ru ions can be observed. From the Cu $2p$ core level spectra we deduce the presence of magnetic Cu$^{2+}$ ions hybridized with a reservoir of itinerant electrons. The strong photon energy dependence of the valence band allows us to disentangle the Ru, Cu, and O contributions and thus to optimize the DMFT calculations. The calculated spin and charge susceptibilities show that the transition metal oxide CaCu$_3$Ru$_4$O$_{12}$ must be classified as a Kondo system and that the Kondo temperature is in the range of 500-1000 K.

cond-mat.str-el↗

arXiv2020

Charge transfer energy in iridates: a hard x-ray photoelectron spectroscopy study

We have investigated the electronic structure of iridates in the double perovskite crystal structure containing either Ir$^{4+}$ or Ir$^{5+}$ using hard x-ray photoelectron spectroscopy. The experimental valence band spectra can be well reproduced using tight binding calculations including only the Ir $5d$, O $2p$ and O $2s$ orbitals with parameters based on the downfolding of the density-functional band structure results. We found that regardless of the A and B cations, the A$_2$BIrO$_6$ iridates have essentially zero O $2p$ to Ir $5d$ charge transfer energies. Hence, double perovskite iridates turn out to be extremely covalent systems with the consequence being that the magnetic exchange interactions become very long-ranged, thereby hampering the materialization of the long-sought Kitaev physics. Nevertheless, it still would be possible to realize a spin-liquid system using the iridates with a proper tuning of the various competing exchange interactions.

cond-mat.str-el↗

arXiv2019

Enhanced $T_c$ and multiband superconductivity in the fully-gapped ReBe$_{22}$ superconductor

In search of the origin of superconductivity in diluted rhenium superconductors and their significantly enhanced $T_c$ compared to pure Be (0.026 K), we investigated the intermetallic ReBe$_{22}$ compound, mostly by means of muon-spin rotation/relaxation ($μ$SR). At a macroscopic level, its bulk superconductivity (with $T_c=9.4$ K) was studied via electrical resistivity, magnetization, and heat-capacity measurements. The superfluid density, as determined from transverse-field $μ$SR and electronic specific-heat measurements, suggest that ReBe$_{22}$ is a fully-gapped superconductor with some multigap features. The larger gap value, $Δ_0^l=1.78$ k$_\mathrm{B}T_c$, with a weight of almost 90\%, is slightly higher than that expected from the BCS theory in the weak-coupling case. The multigap feature, rather unusal for an almost elemental superconductor, is further supported by the field-dependent specific-heat coefficient, the temperature dependence of the upper critical field, as well as by electronic band-structure calculations. The absence of spontaneous magnetic fields below $T_c$, as determined from zero-field $μ$SR measurements, indicates a preserved time-reversal symmetry in the superconducting state of ReBe$_{22}$. In general, we find that a dramatic increase in the density of states at the Fermi level and an increase in the electron-phonon coupling strength, both contribute to the highly enhanced $T_c$ value of ReBe$_{22}$.

cond-mat.supr-con↗

arXiv2018

Antiferromagnetic ground state in the MnGa$_4$ intermetallic compound

Magnetism of the binary intermetallic compound MnGa$_4$ is re-investigated. Band-structure calculations predict antiferromagnetic behavior in contrast to Pauli paramagnetism reported previously. Magnetic susceptibility measurements on single crystals indeed reveal an antiferromagnetic transition at $T_N=393$ K. Neutron powder diffraction and $^{69,71}$Ga nuclear quadrupole resonance spectroscopy show collinear antiferromagnetic order with magnetic moments alligned along the [111] direction of the cubic unit cell. The magnetic moment of 0.80(3)$μ_B$ at 1.5 K extracted from the neutron data is in good agreement with the band-structure results.

cond-mat.mtrl-sci↗

arXiv2017

Pressure-induced ferromagnetism due to an anisotropic electronic topological transition in Fe1.08Te

A rapid and anisotropic modification of the Fermi-surface shape can be associated with abrupt changes in crystalline lattice geometry or in the magnetic state of a material. In this study we show that such an electronic topological transition is at the basis of the formation of an unusual pressure-induced tetragonal ferromagnetic phase in Fe$_{1.08}$Te. Around 2 GPa, the orthorhombic and incommensurate antiferromagnetic ground-state of Fe$_{1.08}$Te is transformed upon increasing pressure into a tetragonal ferromagnetic state via a conventional first-order transition. On the other hand, an isostructural transition takes place from the paramagnetic high-temperature state into the ferromagnetic phase as a rare case of a `type 0' transformation with anisotropic properties. Electronic-structure calculations in combination with electrical resistivity, magnetization, and x-ray diffraction experiments show that the electronic system of Fe$_{1.08}$Te is instable with respect to profound topological transitions that can drive fundamental changes of the lattice anisotropy and the associated magnetic order.

cond-mat.supr-con↗

arXiv2017

Bulk and surface electronic properties of SmB6: a hard x-ray photoelectron spectroscopy study

We have carried out bulk-sensitive hard x-ray photoelectron spectroscopy (HAXPES) measurements on in-situ cleaved and ex-situ polished SmB6 single crystals. Using the multiplet-structure in the Sm 3d core level spectra, we determined reliably that the valence of Sm in bulk SmB6 is close to 2.55 at ~5 K. Temperature dependent measurements revealed that the Sm valence gradually increases to 2.64 at 300 K. From a detailed line shape analysis we can clearly observe that not only the J=0 but also the J=1 state of the Sm 4f 6 configuration becomes occupied at elevated temperatures. Making use of the polarization dependence, we were able to identify and extract the Sm 4f spectral weight of the bulk material. Finally, we revealed that the oxidized or chemically damaged surface region of the ex-situ polished SmB6 single crystal is surprisingly thin, about 1 nm only.

cond-mat.mtrl-sci↗

arXiv2017

Electronic signature of the vacancy ordering in NbO (Nb3O3)

We investigated the electronic structure of the vacancy-ordered 4d-transition metal monoxide NbO (Nb3O3) using angle-integrated soft- and hard-x-ray photoelectron spectroscopy as well as ultra-violet angle-resolved photoelectron spectroscopy. We found that density-functional-based band structure calculations can describe the spectral features accurately provided that self-interaction effects are taken into account. In the angle-resolved spectra we were able to identify the so-called vacancy band that characterizes the ordering of the vacancies. This together with the band structure results indicates the important role of the very large inter-Nb-4d hybridization for the formation of the ordered vacancies and the high thermal stability of the ordered structure of niobium monoxide.

cond-mat.mtrl-sci↗

arXiv2017

Maximal Rashba-like spin splitting via kinetic energy-driven inversion symmetry breaking

Engineering and enhancing inversion symmetry breaking in solids is a major goal in condensed matter physics and materials science, as a route to advancing new physics and applications ranging from improved ferroelectrics for memory devices to materials hosting Majorana zero modes for quantum computing. Here, we uncover a new mechanism for realising a much larger energy scale of inversion symmetry breaking at surfaces and interfaces than is typically achieved. The key ingredient is a pronounced asymmetry of surface hopping energies, i.e. a kinetic energy-driven inversion symmetry breaking, whose energy scale is pinned at a significant fraction of the bandwidth. We show, from spin- and angle-resolved photoemission, how this enables surface states of 3d and 4d-based transition-metal oxides to surprisingly develop some of the largest Rashba-like spin splittings that are known. Our findings open new possibilities to produce spin textured states in oxides which exploit the full potential of the bare atomic spin-orbit coupling, raising exciting prospects for oxide spintronics. More generally, the core structural building blocks which enable this are common to numerous materials, providing the prospect of enhanced inversion symmetry breaking at judiciously-chosen surfaces of a plethora of compounds, and suggesting routes to interfacial control of inversion symmetry breaking in designer heterostructures.

cond-mat.str-el↗

arXiv2017

Valence state of Sm in single crystalline EuO thin films

Samarium has two stable valence states, 2+ and 3+, which coexist in many compounds forming spatially homogeneous intermediate valence states. We study the valence state of samarium when incorporated in a single crystalline EuO thin film which crystallizes in a $fcc$-structure similar to that of the intermediate valence SmO, but with a larger lattice constant. Due to the increased lattice spacing, a stabilization of the larger Sm$^{2+}$ ion is expected. Surprisingly, the samarium incorporated in Sm$_{\mathrm{x}}$Eu$_{\mathrm{1-x}}$O thin films shows a predominantly trivalent character, as determined by x-ray photoelectron spectroscopy and magnetometry measurements. We infer that the O$^{2-}$ ions in the EuO lattice have enough room to move locally, so as to reduce the Sm-O distance and stabilize the Sm$^{3+}$ valence.

cond-mat.str-el↗

arXiv2017

Electronically highly cubic conditions for Ru in alpha-RuCl3

We studied the local Ru 4d electronic structure of alpha-RuCl3 by means of polarization dependent x-ray absorption spectroscopy at the Ru-L2,3 edges. We observed a vanishingly small linear dichroism indicating that electronically the Ru 4d local symmetry is highly cubic. Using full multiplet cluster calculations we were able to reproduce the spectra excellently and to extract that the trigonal splitting of the t2g orbitals is -12 $\pm10$ meV, i.e. negligible as compared to the Ru 4d spin-orbit coupling constant. Consistent with our magnetic circular dichroism measurements, we found that the ratio of the orbital and spin moments is 2.0, the value expected for a Jeff = 1/2 ground state. We have thus shown that as far as the Ru 4d local properties are concerned, alpha-RuCl3 is an ideal candidate for the realization of Kitaev physics.

cond-mat.str-el↗

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

Emergent Weyl fermion excitations in TaP explored by 181-Ta quadrupole resonance

The $^{181}$Ta quadrupole resonance (NQR) technique has been utilized to investigate the microscopic magnetic properties of the Weyl semi-metal TaP. We found three zero-field NQR signals associated with the transition between the quadrupole split levels for Ta with $I$=7/2 nuclear spin. A quadrupole coupling constant, $ν_{\mathrm{Q}}$ =19.250 MHz, and an asymmetric parameter of the electric field gradient, $η$ = 0.423 were extracted, in good agreement with band structure calculations. In order to examine the magnetic excitations, the temperature dependence of the spin lattice relaxation rate (1/$T_{\mathrm{1}}T$) has been measured for the $f_{\mathrm{2}}$-line ($\pm$5/2 $\leftrightarrow$ $\pm$3/2 transition). We found that there exists two regimes with quite different relaxation processes. Above $T\text{*}$ $\approx$ 30 K, a pronounced (1/$T_{\mathrm{1}}T$) $\propto$ $T^{2}$ behavior was found, which is attributed to the magnetic excitations at the Weyl nodes with temperature dependent orbital hyperfine coupling. Below $T\text{*}$, the relaxation is mainly governed by Korringa process with 1/$T_{\mathrm{1}}T$ = constant, accompanied by an additional $T^{-1/2}$ type dependence to fit our experimental data. We show that Ta-NQR is a novel probe for the bulk Weyl fermions and their excitations.

cond-mat.mtrl-sci↗

arXiv2016

Commensurate and incommensurate magnetic order in spin-1 chains stacked on the triangular lattice in Li$_2$NiW$_2$O$_8$

We report thermodynamic properties, magnetic ground state, and microscopic magnetic model of the spin-1 frustrated antiferromaget Li$_{2}$NiW$_{2}$O$_{8}$ showing successive transitions at $T_{\rm N1}\simeq 18$ K and $T_{\rm N2}\simeq 12.5$ K in zero field. Nuclear magnetic resonance and neutron diffraction reveal collinear and commensurate magnetic order with the propagation vector $\mathbf k=(\frac12,0,\frac12)$ below $T_{\rm N2}$. The ordered moment of 1.8 $μ_B$ at 1.5 K is directed along $[0.89(9),-0.10(5),-0.49(6)]$ and matches the magnetic easy axis of spin-1 Ni$^{2+}$ ions, which is determined by the scissor-like distortion of the NiO$_6$ octahedra. Incommensurate magnetic order, presumably of spin-density-wave type, is observed in the region between $T_{\rm N2}$ and $T_{\rm N1}$. Density-functional band-structure calculations put forward a three-dimensional spin lattice with spin-1 chains running along the $[01\bar 1]$ direction and stacked on a spatially anisotropic triangular lattice in the $ab$ plane. We show that the collinear magnetic order in Li$_2$NiW$_2$O$_8$ is incompatible with the triangular lattice geometry and thus driven by a pronounced easy-axis single-ion anisotropy of Ni$^{2+}$.

cond-mat.mtrl-sci↗

arXiv2016

TaIrTe4 a ternary Type-II Weyl semi-metal

In metallic condensed matter systems two different types of Weyl fermions can in principle emerge, with either a vanishing (type-I) or with a finite (type-II) density of states at the Weyl node energy. So far only WTe2 and MoTe2 were predicted to be type-II Weyl semi-metals. Here we identify TaIrTe4 as a third member of this family of topological semi-metals. TaIrTe4 has the attractive feature that it hosts only four well-separated Weyl points, the minimum imposed by symmetry. Moreover, the resulting topological surface states - Fermi arcs connecting Weyl nodes of opposite chirality - extend to about 1/3 of the surface Brillouin zone. This large momentum-space separation is very favorable for detecting the Fermi arcs spectroscopically and in transport experiments.

cond-mat.str-el↗

arXiv2016

Collinear order in a frustrated three-dimensional spin-$\frac12$ antiferromagnet Li$_2$CuW$_2$O$_8$

Magnetic frustration in three dimensions (3D) manifests itself in the spin-$\frac12$ insulator Li$_2$CuW$_2$O$_8$. Density-functional band-structure calculations reveal a peculiar spin lattice built of triangular planes with frustrated interplane couplings. The saturation field of 29 T contrasts with the susceptibility maximum at 8.5 K and a relatively low Néel temperature $T_N\simeq 3.9$ K. Magnetic order below $T_N$ is collinear with the propagation vector $(0,\frac12,0)$ and an ordered moment of 0.65(4) $μ_B$ according to neutron diffraction data. This reduced ordered moment together with the low maximum of the magnetic specific heat ($C^{\max}/R\simeq 0.35$) pinpoint strong magnetic frustration in 3D. Collinear magnetic order suggests that quantum fluctuations play crucial role in this system, where a non-collinear spiral state would be stabilized classically.

cond-mat.mtrl-sci↗

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↗

arXiv2012

Pressure-induced phase transitions and high-pressure tetragonal phase of Fe1.08Te

We report the effects of hydrostatic pressure on the temperature-induced phase transitions in Fe1.08Te in the pressure range 0-3 GPa using synchrotron powder x-ray diffraction (XRD). The results reveal a plethora of phase transitions. At ambient pressure, Fe1.08Te undergoes simultaneous first-order structural symmetry-breaking and magnetic phase transitions, namely from the paramagnetic tetragonal (P4/nmm) to the antiferromagnetic monoclinic (P2_1/m) phase. We show that, at a pressure of 1.33 GPa, the low temperature structure adopts an orthorhombic symmetry. More importantly, for pressures of 2.29 GPa and higher, a symmetry-conserving tetragonal-tetragonal phase transition has been identified from a change in the c/a ratio of the lattice parameters. The succession of different pressure and temperature-induced structural and magnetic phases indicates the presence of strong magneto-elastic coupling effects in this material.

cond-mat.supr-con↗

arXiv2009

Superconductivity induced by ruthenium substitution in an iron arsenide: investigation of SrFe2-xRuxAs2 (0 <= x <= 2)

The magnetism in SrFe2As2 can be suppressed by electron doping through a small substitution of Fe by Co or Ni, giving way to superconductivity. We demonstrate that a massive substitution of Fe by isovalent ruthenium similarly suppresses the magnetic ordering in SrFe2-xRuxAs2 and leads to bulk superconductivity for 0.6 <= x <= 0.8. Magnetization, electrical resistivity, and specific heat data show Tc up to approx 20K. Detailed structural investigations reveal a strong decrease of the lattice parameter ratio c/a with increasing x. DFT band structure calculations are in line with the observation that the magnetic order in SrFe2-xRuxAs2 is only destabilized for large x.

cond-mat.supr-con↗