arXiv subjects

Reinhard K. Kremer

Publications and source records attributed to Reinhard K. Kremer.

32 records · Page 2Linked to original sources

arXiv2016

Structure and Composition of the 200 K-Superconducting Phase of H2S under Ultrahigh Pressure: The Perovskite (SH-)(H3S+)

H2S is converted under ultrahigh pressure (> 110 GPa) to a metallic phase that becomes superconducting with a record Tc of 200 K. It has been proposed that the superconducting phase is body-centered cubic H3S ( Im3m , a = 3.089 Å) resulting from a decomposition reaction 3H2S --> 2H3S + S. The analogy of H2S and H2O leads us to a very different conclusion. The well-known dissociation of water into H3O+ and OH- increases by orders of magnitude under pressure. An equivalent behavior of H2S is anticipated under pressure with the dissociation, 2H2S --> H3S+ + SH- forming a perovskite structure (SH-)(H3S+), which consists of corner-sharing SH6 octahedra with SH- at each A-site (i.e., the center of each S8 cube). Our DFT calculations show that the perovskite (SH-)(H3S+) is thermodynamically more stable than the Im3m structure of H3S, and suggest that the A-site H atoms are most likely fluxional even at Tc.

cond-mat.supr-con↗

arXiv2014

Most spin-1/2 transition-metal ions do have single ion anisotropy

The cause for the preferred spin orientation in magnetic systems containing spin-1/2 transition-metal ions was explored by studying the origin of the easy-plane anisotropy of the spin-1/2 Cu2+ ions in CuCl2.2H2O, LiCuVO4, CuCl2 and CuBr2 on the basis of density functional theory and magnetic dipole-dipole energy calculations as well as a perturbation theory treatment of the spin-orbit coupling. We find that the spin orientation observed for these spin-1/2 ions is not caused by their anisotropic spin exchange interactions, nor by their magnetic dipole-dipole interactions, but by the spin-orbit coupling associated with their crystal-field split d-states. Our study also predicts in-plane anisotropy for the Cu2+ ions of Bi2CuO4 and Li2CuO2. The results of our investigations dispel the mistaken belief that magnetic systems with spin-1/2 ions have no magnetic anisotropy induced by spin-orbit coupling.

cond-mat.str-el↗

arXiv2014

Vibrational states of a water molecule in a nano-cavity of beryl crystal lattice

Low-energy excitations of a single water molecule are studied when confined within a nano-size cage formed by the ionic crystal lattice. Optical spectra are measured of manganese doped beryl single crystal Mn:Be3Al2Si6O18, that contains water molecules individually isolated in 0.51 nm diameter voids within the crystal lattice. Two types of orientation are distinguished: water-I molecules have their dipole moments aligned perpendicular to the c axis, and dipole moments of water-II molecules are parallel to the c-axis. The optical conductivity and permittivity spectra are recorded in terahertz and infrared ranges, at frequencies from several wavenumbers up to 7000cm-1, at temperatures from 5K to 300K and for two polarizations, when the electric vector E of the radiation is parallel and perpendicular to the c-axis. Comparative experiments on as-grown and on dehydrated samples allow to identify the conductivity and permittivity spectra caused exclusively by water molecules. In the infrared range well-known internal modes nu1, nu2 and nu3 of the H2O molecule are observed for both polarizations, indicating the presence of water-I and water-II molecules in the crystal. Spectra recorded below 1000cm-1 reveal a rich set of highly anisotropic features in the low-energy response of H2O molecule in a crystalline nanocage. While for E parallel to c only two absorption peaks are detected, at 90cm-1 and 160cm-1, several absorption bands are discovered for E perpendicular to c, each consisting of narrower resonances. The bands are assigned to librational and translational vibrations of water-I molecule that is weakly, via hydrogen bonds, coupled to the nanocage walls. A model is presented that explains the fine structure of the bands by splitting of the energy levels due to quantum tunneling between the minima in a six-well potential relief felt by a molecule within the cage.

cond-mat.mes-hall↗

arXiv2013

Lattice and orbital fluctuations in TiPO4

In the s = 1/2 antiferromagnetic spin chain material TiPO4 the formation of a spin gap takes place in a two step process with two characteristic temperatures, T*=111 K and TSP=74 K. We observe an unusual lattice dynamics over a large temperature regime as well as evidence for an orbital instability preceding the spin-Peierls transition. We relate different intrachain exchange interactions of the high temperature compared to the spin-Peierls phase to a modification of the orbital ordering pattern. In particular, our observation of a high energy excitation of mixed electronic and lattice origin suggests an exotic dimerization process different from other spin-Peierls materials.

cond-mat.str-el↗

arXiv2013

Quantum Behavior of Water Molecules Confined to Nanocavities in Gemstone

When water is confined to nanocavities, its quantum-mechanical behavior can be revealed by terahertz spectroscopy. We place H2O molecules in the nanopores of a beryl crystal-lattice and observe a rich and highly anisotropic set of absorption lines in the terahertz spectral range. Two bands can be identified, which originate from translational and librational motions of the water molecule isolated within the cage; they correspond to the analogous broad bands in liquid water and ice. In the present case of well-defined and highly symmetric nanocavities, the observed fine structure can be explained by macroscopic tunneling of the H2O molecules within a six-fold potential caused by the interaction of the molecule with the cavity walls.

cond-mat.mes-hall↗

arXiv2012

Spin reorientation in the square-lattice antiferromagnets RMnAsO (R = Ce, Nd): Density functional analysis of the spin exchange interactions between the rare-earth and transition-metal ions

The spin reorientation (SR) phenomenon of the square-lattice antiferromagnets RMnAsO (R = Ce, Nd) was investigated by analyzing the spin exchange interactions between the rare-earth and transition-metal ions (R3+ and Mn2+, respectively) on the basis of density functional calculations. It is found that the symmetry and strength of the Dzyaloshinskii-Moriya (DM) interaction are determined primarily by the partially filled 4f states of the R3+ ions, and that the DM and biquadratic (BQ) exchanges between the R3+ and Mn2+ ions are unusually strong and control the observed spin reorientation phenomenon. Below their SR temperature, the Mn2+ and Ce3+ moments are orthogonal in CeMnAsO but are collinear in NdMnAsO, because the DM interaction dominates over the BQ interaction for CeMnAsO while the opposite is the case for NdMnAsO. Experiments designed to test the implications of our findings are proposed.

cond-mat.str-el↗

arXiv2011

On the nature of the spin frustration in the CuO2 ribbon chains of LiCuVO4: Crystal structure determination at 1.6 K, magnetic susceptibility analysis and density functional evaluation of the spin exchange constants

The spin-1/2 Cu2+ ions of LiCuVO4 form one-dimensional chains along the b-direction, and the spin frustration in LiCuVO4 is described in terms of the nearest-neighbor ferromagnetic exchange J1 and the next-nearest-neighbor antiferromagnetic exchange J2 in these chains. Recently, it has become controversial whether or not J1 is stronger in magnitude than J2. To resolve this controversy, we determined the crystal structure of LiCuVO4 at 1.6 K by neutron diffraction, analyzed the magnetic susceptibility of LiCuVO4 to deduce the Curie-Weiss temperature θand the J2/J1 ratio, and finally extracted the spin exchange constants of LiCuVO4 on the basis of density functional calculations. Our work shows unambiguously that the Curie-Weiss temperature θof LiCuVO4 is negative in the range of -20 K, so that J2 is substantially stronger in magnitude than J1.

cond-mat.str-el↗

arXiv2009

On the Two-Dimensional Character of the Magnetic Properties of Azurite Cu3(CO3)2(OH)2

The spin lattice appropriate for Azurite Cu3(CO3)2(OH)2 was determined by evaluating its spin exchange interactions on the basis of first principles density functional calculations. It is found that Azurite is not described by an isolated diamond chain with no spin frustration, but by a two-dimensional spin lattice in which diamond chains with spin frustration interact through the interchain spin exchange in the ab-plane. Our analysis indicates that the magnetic properties of Azurite at low temperatures can be approximated by two independent contributions, i.e., an isolated dimer and an effective uniform chain contributions. This prediction was verified by analyzing the magnetic susceptibility and specific heat data of Azurite.

cond-mat.mtrl-sci↗

arXiv2007

Carbon Based Superconductors

We review the characteristics of some carbon based novel superconductors which emerged in the past two decades since the discovery of superconductivity in the high-T_c oxocuprates. In particular, we summarize the properties of ternary layered carbide halides of the rare rarth metals with composition RE2C2X2 (RE = Y, La; X=Cl, Br, I) and of the rare earth di- and sesquicarbides, YC2, LaC2 and La2C3. Finally, we briefly discuss the properties of the recently discovered Ca and Yb intercalated graphite superconductors, CaC6 and YbC6.

cond-mat.supr-con↗

arXiv2006

Investigation of the oxohalogenide Cu4Te5O12Cl4 with weakly coupled Cu(II) tetrahedra

The crystal structure of the copper(II) tellurium(IV) oxochloride Cu$_{4}$Te$_{5}$O$_{12}$Cl$_{4}$ (Cu-45124) is composed of weakly coupled tetrahedral Cu clusters and shows crystallographic similarities with the intensively investigated compound Cu$_{2}$Te$_{2}$O$_{5}$X$_{2}$, with X~=~Cl, Br (Cu-2252). It differs from the latter by a larger separation of the tetrahedra within the crystallographic ab plane, that allows a more direct assignment of important inter-tetrahedra exchange paths and the existence of an inversion center. Magnetic susceptibility and specific heat evidence antiferromagnetic, frustrated correlations of the Cu spin moments and long range ordering with $T_{c}$=13.6 K. The entropy related to the transition is reduced due to quantum fluctuations. In Raman scattering a well structured low energy magnetic excitation is observed at energies of $\approx$50K (35cm$^{-1})$. This energy scale is reduced as compared to Cu-2252.

cond-mat.str-el↗

arXiv2005

Thermodynamics of Two - Band Superconductors: The Case of MgB$_{2}$

Thermodynamic properties of the multiband superconductor MgB$_{2}$ have often been described using a simple sum of the standard BCS expressions corresponding to $σ$- and $π$-bands. Although, it is \textit{a priori} not clear if this approach is working always adequately, in particular in cases of strong interband scattering. Here we compare the often used approach of a sum of two independent bands using BCS-like $α$-model expressions for the specific heat, entropy and free energy to the solution of the full Eliashberg equations. The superconducting energy gaps, the free energy, the entropy and the heat capacity for varying interband scattering rates are calculated within the framework of two-band Eliashberg theory. We obtain good agreement between the phenomenological two-band $α$-model with the Eliashberg results, which delivers for the first time the theoretical verification to use the $α$-model as a useful tool for a reliable analysis of heat capacity data. For the thermodynamic potential and the entropy we demonstrate that only the sum over the contributions of the two bands has physical meaning.

cond-mat.supr-con↗

arXiv2004

Influence of Pressure on the Structure and Electronic Properties of the Layered Superconductor Y2C2I2

The structural properties under hydrostatic pressure up to 3 GPa of the layered rare earth carbide halide superconductor Y2C2I2 are studied by neutron powder diffraction at room temperature. The compressibilities are anisotropic, such that the compressibility perpendicular to the layers being approximately twice as large as within the layers. The atomic positional parameters determined from the powder diffraction patterns as a function of pressure were used as the basis for highly resolved electronic structure calculations. These reveal the electronic density of states at E_F to increase with pressure. As is shown quantitatively, this effect outweighs the pressure induced lattice stiffening effects and is responsible for the pressure induced increase and saturation of Tc towards 2 GPa.

cond-mat.supr-con↗

arXiv2004

Band filling and interband scattering effects in MgB$_2$: C vs Al doping

We argue, based on band structure calculations and Eliashberg theory, that the observed decrease of $T_c$ of Al and C doped MgB$_2$ samples can be understood mainly in terms of a band filling effect due to the electron doping by Al and C. A simple scaling of the electron-phonon coupling constant $λ$ by the variation of the density of states as function of electron doping is sufficient to capture the experimentally observed behavior. Further, we also explain the long standing open question of the experimental observation of a nearly constant $π$ gap as function of doping by a compensation of the effect of band filling and interband scattering. Both effects together generate a nearly constant $π$ gap and shift the merging point of both gaps to higher doping concentrations, resolving the discrepancy between experiment and theoretical predictions based on interband scattering only.

cond-mat.supr-con↗

arXiv2001

Orthorhombic versus monoclinic symmetry of the charge-ordered state of NaV2O5

High-resolution X-ray diffraction data show that the low-temperature superstructure of alpha-NaV2O5 has an F-centered orthorhombic 2a x 2b x 4c superlattice. A structure model is proposed, that is characterized by layers with zigzag charge order on all ladders and stacking disorder, such that the averaged structure has space group Fmm2. This model is in accordance with both X-ray scattering and NMR data. Variations in the stacking order and disorder offer an explanation for the recently observed devils staircase of the superlattice period along c.

cond-mat.mtrl-sci↗