arXiv subjects

Bernd Wolf

Publications and source records attributed to Bernd Wolf.

17 recordsLinked to original sources

arXiv2025

Single crystal growth and physical characterization to fine tune YbIn1-xTxCu4 (T = Au, Ag) towards the critical endpoint of the valence transition

Pure as well as Ag- and Au-substituted YbInCu$_4$ single crystals were structurally and chemically characterized and investigated by means of heat capacity, magnetization, resistivity and ultrasonic measurements. We studied the influence of different compositions of the initial melt as well as of Au and Ag substitutions on the valence change and investigated whether this change occurs via a first-order phase transition or via crossover. We constructed a phase diagram of YbInCu$_4$ as a function of various substitutions and show that the position of the critical endpoint of the valence transition depends on the substituent and on the conditions under which the samples were grown. Multiple thermal cycles through the first-order transition lead to a significant modification of the physical properties which clearly demonstrated the influence of defects in substituted YbInCu$_4$.

cond-mat.str-el↗

arXiv2023

Pressure study on the interplay between magnetic order and valence-change crossover in EuPd$_2$(Si$_{1-x}$Ge$_x$)$_2$

We present results of the magnetic susceptibility on high-quality single crystals of EuPd$_2$(Si$_{1-x}$Ge$_x$)$_2$ for Ge concentrations 0 $\leq x \leq$ 0.105 performed under varying hydrostatic (He-gas) pressure 0 $\leq p \leq$ 0.5 GPa. The work extends on recent studies at ambient pressure demonstrating the drastic change in the magnetic response from valence-change-crossover behavior for $x$ = 0 and 0.058, to long-range antiferromagnetic (afm) order below $T_{\text{N}}$ = 47 K for $x$ = 0.105. The valence-change-crossover temperature $T'_{\text{V}}$ shows an extraordinarily strong pressure dependence of d$T'_{\text{V}}$/d$p$ = +(80 $\pm$ 10) K/GPa. In contrast, a very small pressure dependence of d$T_{\text{N}}$/d$p \leq$ +(1 $\pm$ 0.5) K/GPa is found for the afm order upon pressurizing the $x$ = 0.105 crystal from $p$ = 0 to 0.05 GPa. Remarkably, by further increasing the pressure to 0.1 GPa, a drastic change in the ground state from afm order to valence-change-crossover behavior is observed. Estimates of the electronic entropy, derived from analyzing susceptibility data at varying pressures, indicate that the boundary between afm order and valence-change crossover represents a first-order phase transition. Our results suggest a particular type of second-order critical endpoint of the first-order transition for $x$ = 0.105 at $p_{\text{cr}} \approx$ 0.06 GPa and $T_{\text{cr}} \approx$ 45 K where intriguing strong-coupling effects between fluctuating charge-, spin- and lattice degrees of freedom can be expected.

cond-mat.str-el↗

arXiv2023

From valence fluctuations to long-range magnetic order in EuPd$_2$(Si$_{1-x}$Ge$_x$)$_2$ single crystals

EuPd$_2$Si$_2$ is a valence-fluctuating system undergoing a temperature-induced valence crossover at $T'_V\approx160\,$K. We present the successful single crystal growth using the Czochralski method for the substitution series EuPd$_2$(Si$_{1-x}$Ge$_x$)$_2$, with substitution levels $x\leq 0.15$. A careful determination of the germanium content revealed that only half of the nominal concentration is build into the crystal structure. From thermodynamic measurements it is established that $T'_V$ is strongly suppressed for small substitution levels and antiferromagnetic order from stable divalent europium emerges for $x\gtrsim 0.10$. The valence transition is accompanied by a pronounced change of the lattice parameter $a$ of order 1.8%. In the antiferromagnetically ordered state below $T_N = 47$ K, we find sizeable magnetic anisotropy with an easy plane perpendicular to the crystallographic c direction. An entropy analysis revealed that no valence fluctuations are present for the magnetically ordered materials. Combining the obtained thermodynamic and structural data, we construct a concentration-temperature phase diagram demonstrating a rather abrupt change from a valence-fluctuating to a magnetically-ordered state in EuPd$_2$(Si$_{1-x}$Ge$_x$)$_2$.

cond-mat.str-el↗

arXiv2023

Field-induced effects in the spin liquid candidate PbCuTe$_{2}$O$_{6}$

PbCuTe$_2$O$_6$ is considered as one of the rare candidate materials for a three-dimensional quantum spin liquid (QSL). This assessment was based on the results of various magnetic experiments, performed mainly on polycrystalline material. More recent measurements on single crystals revealed an even more exotic behavior, yielding ferroelectric order below $T_{\text{FE}}\approx 1\,\text{K}$, accompanied by distinct lattice distortions, and a somewhat modified magnetic response which is still consistent with a QSL. Here we report on low-temperature measurements of various thermodynamic, magnetic and dielectric properties of single crystalline PbCuTe$_2$O$_6$ in magnetic fields $B\leq 14.5\,\text{T}$. The combination of these various probes allows us to construct a detailed $B$-$T$ phase diagram including a ferroelectric phase for $B \leq$ $8\,\text{T}$ and a $B$-induced magnetic phase at $B \geq$ $11\,\text{T}$. These phases are preceded by or coincide with a structural transition from a cubic high-temperature phase into a distorted non-cubic low-temperature state. The phase diagram discloses two quantum critical points (QCPs) in the accessible field range, a ferroelectric QCP at $B_{c1}$ = $7.9\,\text{T}$ and a magnetic QCP at $B_{c2}$ = $11\,\text{T}$. Field-induced lattice distortions, observed in the state at $T>$ $1\,\text{K}$ and which are assigned to the effect of spin-orbit interaction of the Cu$^{2+}$-ions, are considered as the key mechanism by which the magnetic field couples to the dielectric degrees of freedom in this material.

cond-mat.str-el↗

arXiv2022

Advanced technique for measuring relative length changes under control of temperature and helium-gas pressure

We report the realization of an advanced technique for measuring relative length changes $ΔL/L$ of mm-sized samples under control of temperature ($T$) and helium-gas pressure ($P$). The system, which is an extension of the apparatus described in Manna et al., Rev. Sci. Instrum. 83, 085111 (2012), consists of two $^4$He-bath cryostats each of which houses a pressure cell and a capacitive dilatometer. The interconnection of the pressure cells, the temperature of which can be controlled individually, opens up various modes of operation to perform measurements of $ΔL/L$ under variation of temperature and pressure. Special features of this apparatus include the possibilities (1) to increase the pressure to values much in excess of the external pressure reservoir, (2) to substantially improve the pressure stability during temperature sweeps, (3) to enable continuous pressure sweeps both with decreasing and increasing pressure, and (4) to simultaneously measure the dielectric constant of the pressure-transmitting medium helium, $\varepsilon_{\mathrm{r}}^{\mathrm{He}}(T,P)$, along the same $T$-$P$ trajectory as used for taking the $ΔL(T,P)/L$ data. The performance of the setup is demonstrated by measurements of relative length changes $(ΔL/L)_T$ at $T=180\,\mathrm{K}$ of single crystalline NaCl upon continuously varying the pressure in the range $6\,\mathrm{MPa}\leq P \leq 40\,\mathrm{MPa}$.

physics.ins-det↗

arXiv2022

From magnetic order to valence-change crossover in EuPd$_2$(Si$_{1-x}$Ge$_x$)$_2$ using He-gas pressure

We present results of magnetic susceptibility and thermal expansion measurements performed on high-quality single crystals of EuPd$_2$(Si$_{1-x}$Ge$_x$)$_2$ for 0 $\leq$ x $\leq$ 0.2 and temperatures 2 K $\leq T \leq$ 300 K. Data were taken at ambient pressure and finite He-gas pressure $p$ $\leq$ 0.5 GPa. For x = 0 and ambient pressure we observe a pronounced valence-change crossover centred around $T'_V$ $\approx$ 160 K with a non-magnetic ground state. This valence-change crossover is characterized by an extraordinarily strong pressure dependence of d$T'_V$ /d$p$ = (80 $\pm 10)$ K/GPa. We observe a shift of $T'_V$ to lower temperatures with increasing Ge-concentration, reaching $T'_V$ $\approx$ 90 K for x = 0.1, while still showing a non-magnetic ground state. Remarkably, on further increasing x to 0.2 we find a stable Eu$^{(2+δ)+}$ valence with long-range antiferromagnetic order below $T_N$ = (47.5 $\pm$ 0.1) K, reflecting a close competition between two energy scales in this system. In fact, by the application of hydrostatic pressure as small as 0.1 GPa, the ground state of this system can be changed from long-range antiferromagnetic order for $p$ $<$ 0.1 GPa to an intermediate-valence state for $p$ $\geq$ 0.1 GPa.

cond-mat.str-el↗

arXiv2021

Spin liquid and ferroelectricity close to a quantum critical point in PbCuTe$_2$O$_6$

Geometrical frustration among interacting spins combined with strong quantum fluctuations destabilize long-range magnetic order in favour of more exotic states such as spin liquids. By following this guiding principle, a number of spin liquid candidate systems were identified in quasi-two-dimensional (quasi-2D) systems. For 3D, however, the situation is less favourable as quantum fluctuations are reduced and competing states become more relevant. Here we report a comprehensive study of thermodynamic, magnetic and dielectric properties on single crystalline and pressed-powder samples of PbCuTe$_2$O$_6$, a candidate material for a 3D frustrated quantum spin liquid featuring a hyperkagome lattice. Whereas the low-temperature properties of the powder samples are consistent with the recently proposed quantum spin liquid state, an even more exotic behaviour is revealed for the single crystals. These crystals show ferroelectric order at $T_{\text{FE}} \approx 1\,\text{K}$, accompanied by strong lattice distortions, and a modified magnetic response -- still consistent with a quantum spin liquid -- but with clear indications for quantum critical behaviour.

cond-mat.str-el↗

arXiv2018

Interplay between structure and magnetism in the low-dimensional spin system $K(C_8H_{16}O_4)_2CuCl_3{*}H_2O$

Materials based on a crown ether complex together with magnetic ions, especially Cu(II), can be used to synthesize new low dimesional quantum spin systems. We have prepared the new crown ether complex Di-μ-chloro-bis(12-crown-4)-aquqdichloro-copper(II)-potassium, $K(C_8H_{16}O_4)_2CuCl_3{*}H_2O$ (1), determined its structure, and analyzed its magnetic properties. Complex (1) has a monoclinic structure and crystallizes in space group $P2_1/n$ with the lattice parameters of $a=9.5976(5)Å$, $b=11.9814Å, c=21.8713Å$ and $β=100.945(4)°$. The magnetic properties of this compound have been investigated in the temperature range 1.8 K - 300 K. The magnetic susceptibility shows a maximum at 23 K, but no 3-D long range magnetic order down to 1.8 K. The S=1/2 Cu(II) ions form antiferromagnetically coupled dimers with Cu-Cl distances of $2.2554(8)Å$ and $4.683(6)Å$, and a Cu-Cl-Cu angle of $115.12(2)°$ with $2J_{dimer}=-2.96meV (-23.78 cm^{-1})$. The influence of $H_2O$ on the Cl-Cu-Cl exchange path is analyzed. Our results show that the values of the singlet-triplet splitting are increasing considering $H_2O$ molecules in the bridging interaction. This is supported by Density functional theory (DFT) calculations of coupling constants with Perdew and Wang (PWC), Perdew, Burke and Ernzenrhof (PBE) and strongly constrained and appropriately normed (SCAN) exchange-correlation function show excellent agreement for the studied compound.

cond-mat.mtrl-sci↗

arXiv2016

Stabilization of the tetragonal structure in (Ba$_{1-x}$Sr$_{x}$)CuSi$_{2}$O$_{6}$

We present a structural analysis of the substituted system (Ba$_{1-x}$Sr$_{x}$)CuSi$_{2}$O$_{6}$, which reveals a stable tetragonal crystal structure down to 1.5 K. We explore the structural details with lowtemperature neutron and synchrotron powder diffraction, room-temperature and cryogenic highresolution NMR, as well as magnetic- and specific-heat measurements and verify that a structural phase transition into the orthorhombic structure which occurs in the parent compound BaCuSi2O6, is absent for the x = 0.1 sample. Furthermore, synchrotron powder-diffraction patterns show a reduction of the unit cell for x = 0.1 and magnetic measurements prove that the Cu-dimers are preserved, yet with a slightly reduced intradimer coupling Jintra. Pulse-field magnetization measurements reveal the emergence of a field-induced ordered state, tantamount to Bose-Einsteincondensation (BEC) of triplons, within the tetragonal crystal structure of $I\,4_{1}/acd$. This material offers the opportunity to study the critical properties of triplon condensation in a simple crystal structure.

cond-mat.str-el↗

arXiv2016

Cooling through quantum criticality and many-body effects in condensed matter and cold gases

This article reviews some recent developments for new cooling technologies in the fields of condensed matter physics and cold gases, both from an experimental and theoretical point of view. The main idea is to make use of distinct many-body interactions of the system to be cooled which can be some cooling stage or the material of interest itself, as is the case in cold gases. For condensed matter systems, we discuss magnetic cooling schemes based on a large magnetocaloric effect as a result of a nearby quantum phase transition and consider effects of geometrical frustration. For ultracold gases, we review many-body cooling techniques, such as spin-gradient and Pomeranchuk cooling, which can be applied in the presence of an optical lattice. We compare the cooling performance of these new techniques with that of conventional approaches and discuss state-of-the-art applications.

cond-mat.str-el↗

arXiv2014

Barlowite as a canted antiferromagnet: theory and experiment

We investigate the structural, electronic and magnetic properties of the newly synthesized mineral barlowite Cu4(OH)6FBr which contains Cu2+ ions in a perfect kagome arrangement. In contrast to the spin-liquid candidate herbertsmithite ZnCu3(OH)6Cl2, kagome layers in barlowite are perfectly aligned due to the different bonding environments adopted by F- and Br- compared to Cl-. We perform density functional theory calculations to obtain the Heisenberg Hamiltonian parameters of Cu4(OH)6FBr which has a Cu2+ site coupling the kagome layers. The 3D network of exchange couplings together with a substantial Dzyaloshinskii-Moriya coupling lead to canted antiferromagnetic ordering of this compound at TN=15 K as observed by magnetic susceptibility measurements on single crystals.

cond-mat.str-el↗

arXiv2014

Low-temperature structural investigations of the frustrated quantum antiferromagnets Cs2CuCl(4-x)Br(x)

Powder X-ray diffraction (PXRD) and single-crystal neutron scattering were used to study in detail the structural properties of the Cs2CuCl(4-x)Br(x) series, good realizations of layered triangular antiferromagnets. Detailed temperature-dependent PXRD reveal a pronounced anisotropy of the thermal expansion for the three different crystal directions of the orthorhombic structure without any structural phase transition down to 20 K. Remarkably, the anisotropy of the thermal expansion varies for different $x$, leading to distinct changes of the geometry of the local Cu environment as a function of temperature and composition. The refinement of the atomic positions confirms that for x=1 and 2, the Br atoms occupy distinct halogen sites in the [CuX4]-tetrahedra (X = Cl, Br). The precise structure data are used to calculate the magnetic exchange couplings using density functional methods for x=0. We observe a pronounced temperature dependence of the calculated magnetic exchange couplings, reflected in the strong sensitivity of the magnetic exchange couplings on structural details. These calculations are in good agreement with the experimentally established values for Cs2CuCl4 if one takes the low-temperature structure data as a starting point.

cond-mat.str-el↗

arXiv2014

Magneto-elastic couplings in the distorted diamond-chain compound azurite

We present results of ultrasonic measurements on a single crystal of the distorted diamond-chain compound azurite Cu$_3$(CO$_3$)$_2$(OH)$_2$. Pronounced elastic anomalies are observed in the temperature dependence of the longitudinal elastic mode $c_{22}$ which can be assigned to the relevant magnetic interactions in the system and their couplings to the lattice degrees of freedom. From a quantitative analysis of the magnetic contribution to $c_{22}$ the magneto-elastic coupling $G$ = $\partial J_2$/$\partial ε_b$ can be determined, where $J_2$ is the intra-dimer coupling constant and $ε_b$ the strain along the intra-chain $b$ axis. We find an exceptionally large coupling constant of $|G| \sim ($3650 $\pm$ 150) K highlighting an extraordinarily strong sensitivity of $J_2$ against changes of the $b$-axis lattice parameter. These results are complemented by measurements of the hydrostatic pressure dependence of $J_2$ by means of thermal expansion and magnetic susceptibility measurements performed both at ambient and finite hydrostatic pressure. We propose that a structural peculiarity of this compound, in which Cu$_2$O$_6$ dimer units are incorporated in an unusually stretched manner, is responsible for the anomalously large magneto-elastic coupling.

cond-mat.str-el↗

arXiv2013

Structural variations and magnetic properties of the quantum antiferromagnets Cs2CuCl4-xBrx

Depending on the crystal growth conditions, an orthorhombic (O-type) or a tetragonal (T-type) structure can be found in the solid solution Cs2CuCl4-xBrx (0 < x < 4). Here we present measurements of the temperature-dependent magnetic susceptibility and isothermal magnetization on the T-type compounds x = 1.6 and 1.8 and compare these results with the magnetic properties recently derived for the O-type variant by Cong et al., Phys. Rev. B 83, 064425 (2011). The systems were found to exhibit quite dissimilar magnetic properties which can be assigned to differences in the Cu coordination in these two structural variants. Whereas the tetragonal compounds can be classified as quasi-2D ferromagnets, characterized by ferromagnetic layers with a weak antiferromagnetic inter-layer coupling, the orthorhombic materials, notably the border compounds x = 0 and 4, are model systems for frustrated 2D Heisenberg antiferromagnets

cond-mat.str-el↗

arXiv2011

Elastic constants and ultrasonic attenuation in the cone state of the frustrated antiferromagnet Cs_2CuCl_4

In an external magnetic field perpendicular to the plane of the layers, the quasi two-dimensional frustrated antiferromagnet Cs_2CuCl_4 exhibits a magnetically ordered "cone state" at low temperatures. In this state the component of the magnetic moments in field direction is finite, while their projection onto the plane of the layers forms a spiral. We present both theoretical and experimental results for the magnetic field dependence of the elastic constants and the ultrasonic attenuation rate in the cone state. Our theoretical analysis is based on the usual spin-wave expansion around the classical ground state of a Heisenberg model on an anisotropic triangular lattice with Dzyaloshinskii-Moriya interactions. Magnon-phonon interactions are modeled by expanding the exchange interactions up to second order in powers of the phonon coordinates. As long as the external magnetic field is not too close to the critical field where the cone state becomes unstable, we obtain reasonable agreement between theory and experiment, suggesting that at least in this regime magnons behave as well-defined quasiparticles. We also show that the assumption of well-defined magnons implies that at long wavelengths the ultrasonic attenuation rate in the cone state of Cs_2CuCl_4 is proportional to the fourth power of the phonon momentum.

cond-mat.str-el↗

arXiv2011

Multi-step approach to microscopic models for frustrated quantum magnets - the case of the natural mineral azurite

The natural mineral azurite Cu$_3$(CO$_3$)$_2$(OH)$_2$ is a frustrated magnet displaying unusual and controversially discussed magnetic behavior. Motivated by the lack of a unified description for this system, we perform a theoretical study based on density functional theory as well as state-of-the-art numerical many-body calculations. We propose an effective generalized spin-1/2 diamond chain model which provides a consistent description of experiments: low-temperature magnetization, inelastic neutron scattering, nuclear magnetic resonance measurements, magnetic susceptibility as well as new specific heat measurements. With this study we demonstrate that the balanced combination of first principles with powerful many-body methods successfully describes the behavior of this frustrated material.

cond-mat.str-el↗

arXiv2005

Magnetic properties of a metal-organic antiferromagnet on a distorted honeycomb lattice

For temperatures T well above the ordering temperature T*=3.0+-0.2K the magnetic properties of the metal-organic material Mn[C10H6(OH)(COO)]2x2H20 built from Mn^2+ ions and 3-hydroxy-2-naphthoic anions can be described by a S=5/2 quantum antiferromagnet on a distorted honeycomb lattice with two different nearest neighbor exchange couplings J2 \approx 2J1 \approx 1.8K. Measurements of the magnetization M(H,T) as a function of a uniform external field H and of the uniform zero field susceptibility χ(T) are explained within the framework of a modified spin-wave approach which takes into account the absence of a spontaneous staggered magnetization at finite temperatures.

cond-mat.str-el↗