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Hans-Albrecht Krug von Nidda

Publications and source records attributed to Hans-Albrecht Krug von Nidda.

16 recordsLinked to original sources

Frustrated Gd3+ Double Perovskites as High-Performance Magnetocaloric Materials for Sub-100 mK Adiabatic Demagnetization Refrigeration

Achieving temperatures below 100 mK is essential for advancing quantum technologies and exploring fundamental quantum phenomena. While paramagnetic salts have traditionally enabled adiabatic demagnetization refrigeration (ADR), their limitations have driven the search for more effective alternatives. In this work, we present Gd3+-based double perovskites, Ba2GdSbO6 and Sr2GdSbO6, as high-performance magnetocaloric materials. Starting ADR from 2 K and 5 T, these compounds reach 67 mK and 68 mK in small finite magnetic fields, and 83 mK and 78 mK in zero field, respectively, which are the lowest reported ADR temperatures for Gd3+ magnets (S = 7/2) under these conditions. The frustrated geometry and the complex interplay of exchange and dipolar interactions suppress their antiferromagnetic ordering temperatures to 100 and 166 mK for Ba2GdSbO6 and 190 mK for Sr2GdSbO6, while maintaining an outstanding entropy density of 189 mJ K-1 cm-3 and 201 mJ K-1 cm-3, respectively. Notably, Ba2GdSbO6 sustains sub-100 mK cooling even at finite fields of 0.5 T, making it particularly promising for practical ADR applications.

cond-mat.mtrl-sci↗

Gapped magnetic ground state in the spin-liquid candidate $κ$-(BEDT-TTF)$_2$Ag$_2$(CN)$_3$ suggested by magnetic spectroscopy

The nature of the magnetic ground state of highly frustrated systems remained puzzling to this day. Here, we have performed multifrequency electron spin resonance (ESR) measurements on a putative quantum spin liquid compound $κ$-(BEDT-TTF)$_2$Ag$_2$(CN)$_3$, which is a rare example of $S = 1/2$ spins on a triangular lattice. At high temperatures, the spin susceptibility exhibits a weak temperature dependence which can be described by the Heisenberg model with an antiferromagnetic exchange interaction of strength $J/k_B \approx 175$ K. At low temperatures, however, the rapid drop of the static spin susceptibility, together with monotonic decrease of the ESR linewidth indicates that strong singlet correlations develop below a pairing energy scale $T^*$ accompanied by a spin gap. On the other hand, a weak Curie-like spin susceptibility and the angular dependence of the linewidth suggest additional contribution from impurity spins. We propose the gradual formation of spin singlets with an inhomogeneous spin gap at low temperatures.

cond-mat.str-el↗

Lattice-commensurate skyrmion texture in a centrosymmetric breathing kagome magnet

Skyrmion lattices (SkL) in centrosymmetric materials typically have a magnetic period on the nanometer-scale, so that the coupling between magnetic superstructures and the underlying crystal lattice cannot be neglected. Here, we reveal the commensurate locking of a SkL to the atomic lattice in Gd$_3$Ru$_4$Al$_{12}$ via high-resolution resonant elastic x-ray scattering (REXS). Weak easy-plane magnetic anisotropy, demonstrated here by a combination of ferromagnetic resonance and REXS, penalizes placing a skyrmion core on a site of the atomic lattice. Under these conditions, a commensurate SkL, locked to the crystal lattice, is stable at finite temperatures -- but gives way to a competing incommensurate ground state upon cooling. We discuss the role of Umklapp-terms in the Hamiltonian for the formation of this lattice-locked state, its magnetic space group, the role of slight discommensurations, or (line) defects in the magnetic texture, and contrast our findings with the case of SkLs in noncentrosymmetric material platforms.

cond-mat.str-el↗

Role of alkaline metal in the rare-earth triangular antiferromagnet KYbO$_2$

We report crystal structure and magnetic behavior of the triangular antiferromagnet KYbO$_2$, the A-site substituted version of the quantum spin liquid candidate NaYbO$_2$. The replacement of Na by K introduces an anisotropic tensile strain with 1.6% in-plane and 12.1% out-of-plane lattice expansion. Compared to NaYbO$_2$, both Curie-Weiss temperature and saturation field are reduced by about 20% as the result of the increased Yb--O--Yb angles, whereas the $g$-tensor of Yb$^{3+}$ becomes isotropic with $g=3.08(3)$. Field-dependent magnetization shows the plateau at 1/2 of the saturated value and suggests the formation of the up-up-up-down field-induced order in the triangular AYbO$_2$ oxides (A = alkali metal), in contrast to the isostructural selenides that exhibit the 1/3 plateau and the up-up-down field-induced order.

cond-mat.str-el↗

Frustration on a centred pyrochlore lattice in metal-organic frameworks

Geometric frustration inhibits magnetic systems from ordering, opening a window to unconventional phases of matter. The paradigmatic frustrated lattice in three dimensions to host a spin liquid is the pyrochlore, although there remain few experimental compounds thought to realize such a state. Here we go beyond the pyrochlore via molecular design in the metal-azolate framework [Mn(II)(ta)$_2$], which realizes a closely related centred pyrochlore lattice of Mn-spins with $S=5/2$. Despite a Curie-Weiss temperature of $-21$ K indicating the energy scale of magnetic interactions, [Mn(II)(ta)$_2$] orders at only 430 mK, putting it firmly in the category of highly frustrated magnets. Comparing magnetization and specific heat measurements to numerical results for a minimal Heisenberg model, we predict that this material displays distinct features of a classical spin liquid with a structure factor reflecting Coulomb physics in the presence of charges.

cond-mat.str-el↗

Doping control of magnetic anisotropy for stable antiskyrmion formation in schreibersite (Fe,Ni)$_3$P with $S_4$ symmetry

Magnetic skyrmions, vortex-like topological spin textures, have attracted much interest in a wide range of research fields from fundamental physics to spintronics applications. Recently, growing attention has also been paid to antiskyrmions emerging in opposite topological charge in non-centrosymmetric magnets with $D_{2\mathrm{d}}$ or $S_4$ symmetry. In these magnets, complex interplay among anisotropic Dzyaloshinskii-Moriya interaction, uniaxial magnetic anisotropy, and magnetic dipolar interactions generates a variety of magnetic structures. However, the relation between the stability of antiskyrmions and these magnetic interactions remains to be elucidated. In this work, we control the uniaxial magnetic anisotropy of schreibersite (Fe,Ni)$_3$P with $S_4$ symmetry by doping and investigate its impact on the stability of antiskyrmions. Our magnetometry study, supported by ferromagnetic resonance spectroscopy, shows that the variation of the Ni content and slight doping with 4$d$ transition metals considerably change the magnetic anisotropy. In particular, doping with Pd induces easy-axis anisotropy, giving rise to formation of antiskyrmions, while a temperature-induced spin reorientation is observed in a Rh-doped compound. In combination with Lorentz transmission electron microscopy and micromagnetic simulations, we quantitatively analyze the stability of antiskyrmion as functions of uniaxial anisotropy and demagnetization energy, and demonstrate that subtle balance between them is necessary to stabilize the antiskyrmions.

cond-mat.mtrl-sci↗

Chirality-driven ferroelectricity in LiCuVO$_4$

Chirality or the handedness of objects is of prime importance in life science, biology, chemistry and physics. It is also a major symmetry ingredient in frustrated magnets revealing spin-spiral ground states. Vector chiral phases, with the twist (either clock- or counter clock-wise) between neighbouring spins being ordered, but with disorder with respect to the angles between adjacent spins, have been predicted almost five decades ago. Experimental proofs, however, are rare and controversial. Here, we provide experimental evidence for such a phase in LiCuVO$_4$, a one-dimensional quantum magnet with competing ferromagnetic and antiferromagnetic interactions. The vector chiral state is identified via a finite ferroelectric polarization arising at temperatures well above the multiferroic phase exhibiting long-range three-dimensional spin-spiral and polar order. On increasing temperatures, spin order becomes suppressed at TN, while chiral long-range order still exist, leaving a temperature window with chirality-driven ferroelectricity in the presence of an external magnetic field.

cond-mat.str-el↗

Multiferroic spin-superfluid and spin-supersolid phases in MnCr2S4

Spin supersolids and spin superfluids reveal complex canted spin structures with independent order of longitudinal and transverse spin components. This work addresses the question whether these exotic phases can exhibit spin-driven ferroelectricity. Here we report the results of dielectric and pyrocurrent measurements of MnCr2S4 as function of temperature and magnetic field up to 60 T. This sulfide chromium spinel exhibits a Yafet-Kittel type canted spin structure at low temperatures. As function of external magnetic field, the manganese spins undergo a sequence of ordering patterns of the transverse and longitudinal spin components, which can be mapped onto phases as predicted by lattice-gas models including solid, liquid, super-fluid, and supersolid phases. By detailed dielectric and pyrocurrent measurements, we document a zoo of multiferroic phases with sizable ferroelectric polarization strongly varying from phase to phase. Using lattice-gas terminology, the title compound reveals multiferroic spin-superfluid and spin-supersolid phases, while the antiferromagnetic solid is paraelectric.

cond-mat.str-el↗

Evidence for electronically-driven ferroelectricity in the family of strongly correlated dimerized BEDT-TTF molecular conductors

By applying measurements of the dielectric constants and relative length changes to the dimerized molecular conductor $κ$-(BEDT-TTF)$_2$Hg(SCN)$_2$Cl, we provide evidence for order-disorder type electronic ferroelectricity which is driven by charge order within the (BEDT-TTF)$_2$ dimers and stabilized by a coupling to the anions. According to our density functional theory calculations, this material is characterized by a moderate strength of dimerization. This system thus bridges the gap between strongly dimerized materials, often approximated as dimer-Mott systems at 1/2 filling, and non- or weakly dimerized systems at 1/4 filling exhibiting charge order. Our results indicate that intra-dimer charge degrees of freedom are of particular importance in correlated $κ$-(BEDT-TTF)$_2$X salts and can create novel states, such as electronically-driven multiferroicity or charge-order-induced quasi-1D spin liquids.

cond-mat.str-el↗

Berezinskii-Kosterlitz-Thouless Type Scenario in Molecular Spin Liquid $A$Cr$_2$O$_4$

The spin relaxation in chromium spinel oxides $A$Cr$_{2}$O$_{4}$ ($A=$ Mg, Zn, Cd) is investigated in the paramagnetic regime by electron spin resonance (ESR). The temperature dependence of the ESR linewidth indicates an unconventional spin-relaxation behavior, similar to spin-spin relaxation in the two-dimensional (2D) chromium-oxide triangular lattice antiferromagnets. The data can be described in terms of a generalized Berezinskii-Kosterlitz-Thouless (BKT) type scenario for 2D systems with additional internal symmetries. Based on the characteristic exponents obtained from the evaluation of the ESR linewidth, short-range order with a hidden internal symmetry is suggested.

cond-mat.str-el↗

Anisotropic Exchange in ${\bf LiCu_2O_2}$

We investigate the magnetic properties of the multiferroic quantum-spin system LiCu$_2$O$_2$ by electron spin resonance (ESR) measurements at $X$- and $Q$-band frequencies in a wide temperature range $(T_{\rm N1} \leq T \leq 300$\,K). The observed anisotropies of the $g$ tensor and the ESR linewidth in untwinned single crystals result from the crystal-electric field and from local exchange geometries acting on the magnetic Cu$^{2+}$ ions in the zigzag-ladder like structure of LiCu$_2$O$_2$. Supported by a microscopic analysis of the exchange paths involved, we show that both the symmetric anisotropic exchange interaction and the antisymmetric Dzyaloshinskii-Moriya interaction provide the dominant spin-spin relaxation channels in this material.

cond-mat.str-el↗

Evidence for a Ru$^{4+}$ Kondo Lattice in LaCu$_3$Ru$_4$O$_{12}$

Rare $d$-electron derived heavy-fermion properties of the solid-solution series LaCu$_3$Ru$_x$Ti$_{4-x}$O$_{12}$ were studied for $1 \leq x \leq 4$ by resistivity, susceptibility, specific-heat measurements, and magnetic-resonance techniques. The pure ruthenate ($x = 4$) is a heavy-fermion metal characterized by a resistivity proportional to $T^2$ at low temperatures $T$. The coherent Kondo lattice formed by the localized Ru 4$d$ electrons is screened by the conduction electrons leading to strongly enhanced effective electron masses. By increasing titanium substitution the Kondo lattice becomes diluted resulting in single-ion Kondo properties like in the paradigm $4f$-based heavy-fermion compound Ce$_x$La$_{1-x}$Cu$_{2.05}$Si$_2$ [M. Ocko {\em et al.}, Phys. Rev. B \textbf{64}, 195106 (2001)]. In LaCu$_3$Ru$_x$Ti$_{4-x}$O$_{12}$ the heavy-fermion behavior finally breaks down on crossing the metal-to-insulator transition close to $x = 2$.

cond-mat.str-el↗

Magnetic Excitations in the Multiferroic Néel-type Skyrmion Host GaV$_4$S$_8$

Broadband microwave spectroscopy has been performed on single-crystalline GaV$_4$S$_8$, which exhibits a complex magnetic phase diagram including cycloidal, Néel-type skyrmion lattice, as well as field-polarized ferromagnetic phases below 13 K. At zero and small magnetic fields two collective modes are found at 5 and 15 GHz, which are characteristic of the cycloidal state in this easy-axis magnet. In finite fields, entering the skyrmion lattice phase, the spectrum transforms into a multi-mode pattern with absorption peaks near 4, 8, and 15 GHz. The spin excitation spectra in GaV$_4$S$_8$ and their field dependencies are found to be in close relation to those observed in materials with Bloch-type skyrmions. Distinct differences arise from the strong uniaxial magnetic anisotropy of GaV4S8 not present in so-far known skyrmion hosts.

cond-mat.str-el↗

Poly-MTO, {(CH_3)_{0.92} Re O_3}_\infty, a Conducting Two-Dimensional Organometallic Oxide

Polymeric methyltrioxorhenium, {(CH_{3})_{0.92}ReO_{3}}_{\infty} (poly-MTO), is the first member of a new class of organometallic hybrids which adopts the structural pattern and physical properties of classical perovskites in two dimensions (2D). We demonstrate how the electronic structure of poly-MTO can be tailored by intercalation of organic donor molecules, such as tetrathiafulvalene (TTF) or bis-(ethylendithio)-tetrathiafulvalene (BEDT-TTF), and by the inorganic acceptor SbF$_3$. Integration of donor molecules leads to a more insulating behavior of poly-MTO, whereas SbF$_3$ insertion does not cause any significant change in the resistivity. The resistivity data of pure poly-MTO is remarkably well described by a two-dimensional electron system. Below 38 K an unusual resistivity behavior, similar to that found in doped cuprates, is observed: The resistivity initially increases approximately as $ρ\sim$ ln$(1/T$) before it changes into a $\sqrt{T}$ dependence below 2 K. As an explanation we suggest a crossover from purely two-dimensional charge-carrier diffusion within the \{ReO$_2$\}$_{\infty}$ planes at high temperatures to three-dimensional diffusion at low temperatures in a disorder-enhanced electron-electron interaction scenario (Altshuler-Aronov correction). Furthermore, a linear positive magnetoresistance was found in the insulating regime, which is caused by spatial localization of itinerant electrons at some of the Re atoms, which formally adopt a $5d^1$ electronic configuration. X-ray diffraction, IR- and ESR-studies, temperature dependent magnetization and specific heat measurements in various magnetic fields suggest that the electronic structure of poly-MTO can safely be approximated by a purely 2D conductor.

cond-mat.mtrl-sci↗

Interplay of superexchange and orbital degeneracy in Cr-doped LaMnO3

We report on structural, magnetic and Electron Spin Resonance (ESR) investigations in the manganite system LaMn_{1-x}Cr_{x}O_{3} (x<=0.5). Upon Cr-doping we observe a reduction of the Jahn-Teller distortion yielding less distorted orthorhombic structures. A transition from the Jahn-Teller distorted O' to the pseudocubic O phase occurs between 0.3<x<0.4. A clear connection between this transition and the doping dependence of the magnetic and ESR properties has been observed. The effective moments determined by ESR seem reduced with respect to the spin-only value of both Mn^{3+} and Cr^{3+} ions.

cond-mat.str-el↗