arXiv subjects

Reinhard K. Kremer

Publications and source records attributed to Reinhard K. Kremer.

At least 19 recordsLinked to original sources

arXiv2026

Chemical Perspectives on Cuprate Superconductivity: Hole-Protected Spin Dimers as d Wave Cooper Pairs

The observation that the coherence lengths in cuprate superconductors are extremely small motivated us to search for its real-space structure by examining the consequence of hole-doping in CuO4 units in cuprates. We analyzed aggregates of hole-doped CuO4 units that phase-separate from hole-doped CuO2 layers in terms of their segregation-pressure indices defined in this work. Our search suggests that each d-wave Cooper pair is an antiferromagnetically coupled spin dimer protected in an antiferromagnetic hole dimer (AHD), and that the antiferromagnetic chains of AHDs provide channels through which such spin dimers can move collectively without perturbation. Based on these suggestions and their implications, we examined the causes for several seemingly puzzling observations on cuprate superconductors to find that they are naturally explained by the suggestions.

cond-mat.supr-con↗

arXiv2026

Low-temperature structural instabilities of the halide double perovskite Cs$_2$AgBiBr$_6$ investigated via x-ray diffraction and infrared phonons

The halide double perovskite Cs$_2$AgBiBr$_6$ has been proposed as a potential replacement for organic halide perovskites for photovoltaic applications. Further investigation of its dielectric response, optical properties and structural stability is thus warranted. Cs$_2$AgBiBr$_6$ exhibits a well-documented structural phase transition at 120 K but indications for an additional lower temperature ($\sim$40 K) phase transition have also been reported. On the basis of measurements of the specific heat capacity, temperature dependent powder X-ray diffraction, low frequency capacitance, and infrared reflectivity we clarify the previously reported splitting of phonon modes in the Raman spectrum at $\sim$40 K as due to a subtle structural phase transition from the tetragonal I4/m structure to a monoclinic $P12_1$/$n1$ crystal structure. The infrared active vibrational modes are experimentally investigated in the three structural regimes. In the cubic structure at room temperature the four IR active modes are observed at 135,$\sim$95, 55, and $\sim$25 cm$^{-1}$, as the symmetry reduces to tetragonal a minute splitting of these modes is expected, however below 40 K an additional mode is observed indicating a further reduction in symmetry.

cond-mat.mtrl-sci↗

arXiv2026

Reduction of Ordered Spin Moments in Antiferromagnets of S = 5/2 Ions (Fe3+, Mn2+) Driven by Local Magnetic Excitation

For antiferromagnets composed of spin five-half ions, the moments of these ions in the ordered antiferromagnetic state can be significantly smaller than 5 BM (i.e., 1.56 - 4.48 BM) if these ions form quantum fluctuating entities (QFEs), for example, quasi one-dimensional uniform antiferromagnetic chains or quasi zero-spin antiferromagnetic spin dimers. It is reasonable to suppose that the stronger the quantum fluctuation in such an antiferromagnet, the greater the reduction in its ordered moment would become, but this supposition has not yet been confirmed because quantifying the strength of quantum fluctuation is not a straightforward matter. Here we show that the local magnetic excitations involving the QFEs can be used to quantify the strength of quantum fluctuation by analyzing six antiferromagnets showing significant reduction in their ordered spin moments.

cond-mat.str-el↗

arXiv2025

Nanoscale lattice heterostructure in high Tc superconductors

Low temperature superconductivity was known since 1957 to be described by BCS theory for an effective single band metals controlled by the density of states at the Fermi level, very far from band edges, the electron phonon coupling, and the energy of the boson in the pairing interaction w0, but BCS has failed to predict high temperature superconductivity in different materials above about 23 K. High temperature superconductivity above 35 K since 1986 has been a matter of materials science where manipulating the lattice complexity of high temperature superconducting ceramic oxides (HTSC) has driven material scientists to grow new HTSC quantum materials up to 138K in HgBa2Ca2Cu3O8 (Hg1223) at ambient pressure and near room temperature in pressurized hydrides. This perspective covers the major results of materials scientist in these last 39 years investigating the role of lattice inhomogeneity detected in these new quantum complex materials. We highlight the nanoscale heterogeneity in these complex materials and elucidate their special role played in the physics for HTSC. Especially, it is pointed out that the geometry of lattice and charge complex heterogeneity at nanoscale is essential and intrinsic in the mechanism of rising quantum coherence at high temperature

cond-mat.supr-con↗

arXiv2025

Elucidating the origin of long-range ferromagnetic order in Fe$_3$GeTe$_2$ by low-energy magnon excitation studies

We report a detailed high-field/high-frequency ferromagnetic resonance (HF-FMR) study of low-energy magnon excitations in the van der Waals ferromagnet Fe$_3$GeTe$_2$. At 2 K, the field dependence of the magnon branches is well described by a semiclassical domain-based model, from which we extract key microscopic parameters including the anisotropy gap $Δ= 170\pm 4$ GHz, the anisotropy field $B_{\rm A} = 5.85\pm 0.08$ T, and the effective $g$-factor $g_{\rm ab}\simeq g_{\rm c} = 2.07(4)$. Furthermore the uniaxial anisotropy constant was determined to be $K = (10.5\pm 0.23) \times 10^{-6}$ erg/cm$^3$. Anisotropic short-range magnetic order persists above $T_{\rm C}$ up to approximately 270 K, as evidenced by a finite anisotropy gap and anisotropic shifts in the FMR resonance fields. Both results clearly show the presence of anisotropic local magnetic fields well above $T_{\rm C}$. Our findings underscore the crucial role of magneto-crystalline anisotropy in driving long-range magnetic order in Fe$_3$GeTe$_2$.

cond-mat.str-el↗

arXiv2025

Exerting chemical pressure on the kagome lattice as frustration control in the kapellasite family $A$Cu$_3$(OH)$_{6+x}$(Cl,Br)$_{3-x}$

The kapellasite family $A$Cu$_3$(OH)$_{6+x}$(Cl,Br)$_{3-x}$ forms a series of compounds, wherein the chemical pressure realized by the $A-$site cation tunes the spin exchange in the frustrated distorted kagome lattice. Via hydrothermal synthesis we have grown single crystals of the whole series for $A=$ rare-earths and found a clear structural transition to a superstructure variant at a specific chemical pressure level exerted by $A$~=~Dy. Phases with crystal structures in the vicinity of this superstructure transition realize a distorted kagome lattice of the Cu$^{2+}$ cations with characteristic features of a spin liquid. Here, subtle structural disorder as well as controlled chemical pressure can stabilize the spin liquid phase. We study the crystal structure and the magnetic ground state of these phases via single crystal x-ray diffraction, magnetic susceptibility, specific heat and muon spin spectroscopy measurements.

cond-mat.str-el↗

arXiv2024

Chemo-Structural Disorder in the kagomé spin $S$ = 1/2 systems ZnCu$_3$(OH)$_6$Cl$_2$ and YCu$_3$(OH)$_{6}$Br$_{2}$[Br$_x$(OH)$_{1-x}$]

By single crystal diffraction we characterize the chemo-structural disorder introduced by Zn-Cu site mixing in the kagomé spin $S$-1/2 systems herbertsmithite ZnCu$_3$(OH)$_6$Cl$_2$ and YCu$_3$(OH)$_{6}$Br$_{2}$[Br$_x$(OH)$_{1-x}$]. For an untwinned single crystal of herbertsmithite of composition Zn$_{0.95(1)}$Cu$_{2.99(3)}$O$_{5.9(1)}$H$_{5.8(1)}$Cl$_2$ we find substitution by Cu of the Zn atoms in the layers separating the kagomé layers as well as substantial Zn substitution for Cu in the kagomé layers. In YCu$_3$(OH)$_{6}$Br$_{2}$[Br$_x$(OH)$_{1-x}$] site mixing disorder is present for intermediate $x$. Analogous to the Cl homologous system in crystals with $x = 1/3$ disorder is absent and a low-temperature structural transition emerges driven by strong magneto-phonon coupling as a release of frustration. Apart from this structural anomaly we find the physical properties of these crystals unchanged compared to intermediate $x$ and closely resembling the Cl homologue where long-range magnetic order was observed.

cond-mat.str-el↗

arXiv2024

Magnetization Plateaus by the Field-Induced Partitioning of Spin Lattices

To search for a conceptual picture describing the magnetization plateau phenomenon, we surveyed the crystal structures and the spin lattices of those magnets exhibiting plateaus in their magnetization vs. magnetic field curves by probing the three questions: (a) why only certain magnets exhibit magnetization plateaus, (b) why there occur several different types of magnetization plateaus, and (c) what controls the widths of magnetization plateaus. We show that the answers to these questions lie in how the magnets under field absorb Zeeman energy hence changing their magnetic structures. The magnetic structure of a magnet insulator is commonly described in terms of its spin lattice, which requires the determination of the spin exchanges nonnegligible strengths between the magnetic ions. Our work strongly suggests that a magnet under magnetic field partitions its spin lattice into antiferromagnetic (AFM) or ferrimagnetic fragments by breaking its weak magnetic bonds. Our supposition of the field-induced partitioning of spin lattice into magnetic fragments is supported by the anisotropic magnetization plateaus of Ising magnets and by the highly anisotropic width of the 1/3-magnetization plateau in azurite. The answers to the three questions (a) - (c) emerge naturally by analyzing how these fragments are formed under magnetic field.

cond-mat.mtrl-sci↗

arXiv2024

The incredible diversity of structural and magnetic instabilities in EuTiO3: from paramagnetic to spin glass, spin liquid and antiferromagnetic order

The perovskite oxide EuTiO3 (ETO) has attracted increased scientific interest due to its potential multiferroic properties and magnetic activity above and below its structural phase transition at TS=282K. Various experiments have indirectly evidenced that this transition is neither a cubic tetragonal nor the only one occurring in ETO. Here, we show new results demonstrating two further instabilities below TS based on lattice dynamics and spin-phonon interactions combined with a Landau free energy model with coupled order parameters. The new transition temperatures perfectly agree with available experimental data where further instabilities have been anticipated.

cond-mat.mtrl-sci↗

arXiv2024

Noncollinear electric dipoles in a polar, chiral phase of CsSnBr$_3$ perovskite

Polar and chiral crystal symmetries confer a variety of potentially useful functionalities upon solids by coupling otherwise noninteracting mechanical, electronic, optical, and magnetic degrees of freedom. We describe two unstudied phases of the 3D perovskite, CsSnBr$_3$, which emerge below 85 K due to the formation of Sn(II) lone pairs and their interaction with extant octahedral tilts. Phase II (77 K<$T$<85 K, space group $P2_1/m$) exhibits ferroaxial order driven by a noncollinear pattern of lone pair-driven distortions within the plane normal to the unique octahedral tilt axis, preserving the inversion symmetry observed at higher temperatures. Phase I ($T$<77 K, space group $P2_1$) additionally exhibits ferroelectric order due to distortions along the unique tilt axis, breaking both inversion and mirror symmetries. This polar and chiral phase exhibits second harmonic generation from the bulk and a large, intrinsic polarization$-$electrostriction coefficient along the polar axis ($Q_{22}\approx$1.1 m$^4$ C$^{-2}$), resulting in acute negative thermal expansion ($α_V=-9\times10^{-5}$ K$^{-1}$) through the onset of spontaneous polarization. The unprecedented structures of phases I and II were predicted by recursively following harmonic phonon instabilities to generate a tree of candidate structures and subsequently corroborated by synchrotron X-ray powder diffraction and polarized Raman and $^{81}$Br nuclear quadrupole resonance spectroscopies. Relativistic electronic structure scenarios compatible with reported photoluminescence measurements are discussed. Together, the polar symmetry, small bandgap, large spin-orbit splitting of Sn 5$p$ orbitals, and predicted strain sensitivity of the symmetry-breaking distortions suggest bulk samples and epitaxial films of CsSnBr$_3$ or its neighboring solid solutions as strong candidates for bulk Rashba effects.

cond-mat.mtrl-sci↗

arXiv2024

SrCu(OH)$_3$Cl, an ideal isolated equilateral triangle spin $S$ = 1/2 model system

We have investigated the magnetic ground state properties of the quantum spin trimer compound strontium hydroxy copper chloride SrCu(OH)$_3$Cl using bulk magnetization, specific heat measurements, nuclear magnetic resonance (NMR), and electron spin resonance (ESR) spectroscopy. SrCu(OH)$_3$Cl consists of layers with isolated Cu$^{2+}$ triangles and hence provides an opportunity to understand the magnetic ground state of an isolated system of \textit{S} = 1/2 arranged on an equilateral triangle. Although magnetization measurements do not exhibit a phase transition to a long-range ordered state down to \textit{T} = 2 K, they reveal the characteristic behavior of isolated trimers with an exchange of $J = 154$~K. The Curie-Weiss behavior changes around 50--80~K, as is also seen in the NMR spin-lattice relaxation rate. In zero magnetic field, our specific heat data establish a second-order phase transition to an antiferromagnetic ground state below \textit{T}= 1.2 K. We have drawn a magnetic field-temperature ($H$-$T$) phase diagram based on the specific heat measurements. The ESR data show divergence of the linewidth at lower temperatures, which precedes the phase transition to an antiferromagnetic long-range ordered state with unconventional critical exponents. The temperature variation of the $g$-factor further confirms the antiferromagnetic phase transition and reflects the underlying magneto-crystalline anisotropy of the compound.

cond-mat.str-el↗

arXiv2022

High-spin orbital interactions across van der Waals gaps controlling the interlayer ferromagnetism in van der Waals ferromagnets

We examined what interactions control the sign and strength of the interlayer coupling in van der Waals ferromagnets such as Fe3-xGeTe2, Cr2Ge2Te6, CrI3 and VI3, to find that high-spin orbital interaction across the van der Waals gaps are a key to understanding their ferromagnetism. Interlayer ferromagnetic coupling in Fe3-xGeTe2 Cr2Ge2Te6, and CrI3 is governed by the high-spin two-orbital two-electron destabilization, but that in VI3 by the high-spin four-orbital two-electron stabilization. These interactions explain a number of seemingly puzzling observations in van der Waals fer-romagnets.

cond-mat.str-el↗

arXiv2022

Absence of Spin Frustration in the Kagomé Layers of Cu2+ Ions in Volborthite Cu3V2O7(OH)2x2H2O and Observation of the Suppression and Re-entrance of Specific Heat Anomalies in Volborthite Under External Magnetic Field

We determined the spin exchanges between the Cu2+ ions in the kagome layers of volborthite, Cu3V2O7(OH)2x2H2O, by performing the energy-mapping analysis based on DFT+U calculations, to find that the kagomé layers of Cu2+ ions are hardly spin-frustrated, and the magnetic properties of volborthite below ~75 K should be described by very weakly interacting antiferromagnetic uniform chains made up of effective S=1/2 pseudospin units. This conclusion was verified by synthesizing single crystals of not only Cu3V2O7(OH)2x2H2O but also its deuterated analogue Cu3V2O7(OD)2x2D2O and then by investigating their magnetic susceptibilities and specific heats. Each kagome layer consists of intertwined two-leg spin ladders with rungs of linear spin trimers. With the latter acting as S=1/2 pseudospin units, each two-leg spin ladder behaves as a chain of S=1/2 pseudospins. Adjacent two-leg spin ladders in each kagome layer interact very weakly, so it is required that all nearest-neighbor spin exchange paths of every two-leg spin ladder remain antiferromagnetically coupled in all spin ladder arrangements of a kagome layer. This constraint imposes three sets of entropy spectra with which each kagome layer can exchange energy with the surrounding on lowering the temperature below ~1.5 K and on raising the external magnetic field B. We discovered that the specific heat anomalies of volborthite observed below ~1.5 K at B = 0 are suppressed by raising the magnetic field B to ~4.2 T, that a new specific heat anomaly occurs when B is increased above ~5.5 T, and that the imposed three sets of entropy spectra are responsible for the field-dependence of the specific heat anomalies.

cond-mat.str-el↗

arXiv2021

Discovery of Superconductivity in (Ba,K)SbO$_{3}$

Superconducting bismuthates (Ba,K)BiO$_{3}$ (BKBO) constitute an interesting class of superconductors in that superconductivity with a remarkably high $T_\mathrm{c}$ of 30 K arises in proximity to charge density wave (CDW) order. Prior understanding on the driving mechanism of the CDW and superconductivity emphasizes the role of either bismuth (negative $U$ model) or oxygen ions (ligand hole model). While holes in BKBO presumably reside on oxygen owing to their negative charge transfer energy, so far there has been no other comparative material studied. Here, we introduce (Ba,K)SbO$_{3}$ (BKSO) in which the Sb 5$s$ orbital energy is higher than that of the Bi 6$s$ orbitals enabling tuning of the charge transfer energy from negative to slightly positive. The parent compound BaSbO$_{3-δ}$ shows a larger CDW gap compared to the undoped bismuthate BaBiO$_{3}$. As the CDW order is suppressed via potassium substitution up to 65 %, superconductivity emerges, rising up to $T_\mathrm{c}$ = 15 K. This value is lower than the maximum $T_\mathrm{c}$ of BKBO, but higher by more than a factor of two at comparable potassium concentrations. The discovery of an enhanced CDW gap and superconductivity in BKSO indicates that the sign of the charge transfer energy may not be crucial, but instead strong metal-oxygen covalency plays the essential role in constituting a CDW and high-$T_\mathrm{c}$ superconductivity in the main-group perovskite oxides.

cond-mat.supr-con↗

arXiv2020

Low-Temperature Phase of the Cd$_2$Re$_2$O$_7$ Superconductor: Ab initio Phonon Calculations and Raman Scattering

Using an {\it ab initio} approach, we report a phonon soft mode in the tetragonal structure described by the space group $I4_{1}22$ of the $1$ K $5d$ superconductor Cd$_2$Re$_2$O$_7$. It induces an orthorhombic distortion to a crystal structure described by the space group $F222$ which hosts the superconducting state. This new phase has a lower total energy than the other known crystal structures of Cd$_2$Re$_2$O$_7$. Comprehensive temperature dependent Raman scattering experiments on isotope enriched samples, $^{116}$Cd$_2$Re$_2{^{18}}$O$_7$, not only confirm the already known structural phase transitions but also allow us to identify a new characteristic temperature regime around $\sim 80$ K, below which the Raman spectra undergo remarkable changes with the development of several sharp modes and mode splitting. Together with the results of the \textit{ab initio} phonon calculations we take these observations as strong evidence for another phase transition to a novel low-temperature crystal structure of Cd$_2$Re$_2$O$_7$.

cond-mat.supr-con↗

arXiv2019

Ordering of hidden multipoles in spin-orbital entangled 5$d^{1}$ Ta chlorides

Spin-orbit coupling of as large as a half eV for electrons in 5$d$ orbitals often gives rise to the formation of spin-orbital entangled objects, characterized by the effective total angular momentum $J_{eff}$. Of particular interest are the $J_{eff}$ = 3/2 states realized in 5$d^{1}$ transition metal ions surrounded by an anion octahedron. The pure $J_{eff}$ = 3/2 quartet does not have any magnetic dipolar moment (<$M$> = 0) but hosts hidden pseudo-dipolar moments accompanied by charge quadrupoles and magnetic octupoles. Cs$_2$TaCl$_6$ and Rb$_2$TaCl$_6$ are correlated insulators with 5$d^{1}$ Ta$^{4+}$ ions in a regular Cl octahedron. Here we demonstrate that these Ta chlorides have a substantially suppressed effective magnetic dipolar moment of ~ 0.2 $μ_B$. Two phase transitions are observed at low temperatures that are not pronounced in the magnetization but accompanied with large electronic entropy of $R$ln4. We ascribe the two transitions to the ordering of hidden multipoles.

cond-mat.str-el↗

arXiv2017

Linarite - a quasi-critical J$_1$-J$_2$ chain

The mineral linarite, PbCuSO$_4$(OH)$_2$, is a spin 1/2 chain with frustrating nearest neighbor ferromagnetic and next-nearest neighbor antiferromagnetic exchange interactions. Our inelastic neutron scattering experiments performed above the saturation field establish that the ratio between these exchanges is such that linarite is extremely close to the quantum critical point between spin-multipolar phases and the ferromagnetic state. However, the measured complex magnetic phase diagram depends strongly on the magnetic field direction. The field-dependent phase sequence is explained by our classical simulations of a nearly critical model with tiny orthorhombic exchange anisotropy. The simulations also capture qualitatively the measured variations of the wave vector as well as the staggered and the uniform magnetizations in an applied field.

cond-mat.str-el↗

arXiv2017

Tunable Weyl and Dirac states in the nonsymmorphic compound $\rm\mathbf{CeSbTe}$

Recent interest in topological semimetals has lead to the proposal of many new topological phases that can be realized in real materials. Next to Dirac and Weyl systems, these include more exotic phases based on manifold band degeneracies in the bulk electronic structure. The exotic states in topological semimetals are usually protected by some sort of crystal symmetry and the introduction of magnetic order can influence these states by breaking time reversal symmetry. Here we show that we can realize a rich variety of different topological semimetal states in a single material, $\rm CeSbTe$. This compound can exhibit different types of magnetic order that can be accessed easily by applying a small field. It allows, therefore, for tuning the electronic structure and can drive it through a manifold of topologically distinct phases, such as the first nonsymmorphic magnetic topological material with an eight-fold band crossing at a high symmetry point. Our experimental results are backed by a full magnetic group theory analysis and ab initio calculations. This discovery introduces a realistic and promising platform for studying the interplay of magnetism and topology.

cond-mat.mtrl-sci↗