arXiv subjects

H. -A. Krug von Nidda

Publications and source records attributed to H. -A. Krug von Nidda.

At least 19 recordsLinked to original sources

arXiv2026

Low temperature thermodynamics of $S_{\mathrm{eff}}=1/2$ triangular lattice quantum spin liquid candidate TlYbS$_2$

Geometrically frustrated triangular-lattice antiferromagnets exhibit a delicate competition between magnetic order and quantum spin liquid (QSL) behavior, with the Yb-based delafossite family $A$Yb$X_2$ providing a structurally clean platform for exploring this physics. Here, we report a comprehensive study of single-crystal TlYbS$_2$ using DC magnetization, AC susceptibility, electron spin resonance (ESR), and specific heat measurements extending from room temperature to the millikelvin regime. Single-crystal X-ray diffraction confirms a trigonal $R\bar{3}m$ structure comprising well-separated triangular layers of Yb$^{3+}$ ions with no detectable site disorder. At zero field, a weak thermodynamic anomaly is observed near $530$ mK, which may indicate the onset of a weakly ordered state similar to that reported in KYbSe$_2$. Below $300$ mK, the zero-field magnetic specific heat follows $C_{\rm m}\propto T^{1.8}$, close to a quadratic temperature dependence, in contrast to the linear temperature dependence reported for the sister compound TlYbSe$_2$, which has been described in terms of the interplay between spinons and thermally excited gauge-flux excitations. Magnetization and ESR measurements establish pronounced easy-plane magnetic anisotropy, with $g_\perp/g_\parallel \approx 6.9$. The anomaly near $530$ mK exhibits a strongly anisotropic response to magnetic field. For $H\perp c$, it remains visible up to approximately $2$ T and continuously evolves toward a field-induced ordered phase above approximately $2.5$ T, followed by a sequence of field-induced phases that includes a $1/3$ magnetization plateau between approximately $5$ and $8$ T and full polarization near $17$ T. In contrast, for $H\parallel c$, the anomaly weakens and is suppressed near $3$ T, consistent with the recently reported confinement--deconfinement transition from an ordered state to a field-induced QSL.

cond-mat.str-el↗

arXiv2026

Novel Quantum Spin Liquid States in the $S = {\frac{1}{2}}$ Three-Dimensional Compound Y$_{3}$Cu$_{2}$Sb$_{3}$O$_{14}$

The three-dimensional $S = {\frac{1}{2}}$ system Y$_{3}$Cu$_{2}$Sb$_{3}$O$_{14}$ consists of two inequivalent Cu$^{2+}$ sites, each forming an edge shared triangular lattice. Our magnetic susceptibility $χ(T)$, specific heat $C_p(T)$, $^{89}$Y nuclear magnetic resonance (NMR), muon spin relaxation ($\upmu\mathrm{SR}$), and electron spin resonance (ESR) measurements on this system confirm the absence of any long-range magnetic ordering and the persistence of spin dynamics down to 0.077 K. In $^{89}$Y NMR we find an anomaly at about 120 K which we suggest arises from a fraction of the spins condensing into a singlet (a valence bond solid VBS) state. A plateau in the muon relaxation rate is observed between 60 K and 10 K (signifying the VBS state from a fraction of the spins) followed by an increase and another plateau below about 1 K (presumably signifying the quantum spin liquid state from all the spins). Our density functional theory calculations find a dominant antiferromagnetic interaction along the body diagonal with inequivalent Cu(1) and Cu(2) ions alternately occupying the corners of the cube. All other near-neighbour interactions between the Cu ions are also found to be antiferromagnetic and are thought to drive the frustration.

cond-mat.str-el↗

arXiv2023

Magnetic resonance in the quasi-2D square lattice easy-plane antiferromagnet Ba$_2$MnGe$_2$O$_7$

We report results of a multi-frequency (0.8-60 GHz) electron spin resonance study of the spin dynamics in the quasi-2D square lattice antiferromagnet Ba$_2$MnGe$_2$O$_7$ both in antiferromagnetically ordered and paramagnetic phases. We directly observe two zero-field gaps in the excitation spectrum of the ordered phase, the larger one being due to easy-plane anisotropy, and the smaller one indicates the presence of fourth-order in-plane anisotropy probably related to the multiferroic properties of this compound. We observe effects of hyperfine interaction on the electron spin resonance spectra in the antiferromagnetically ordered state, which turns out to be comparable with in-plane anisotropy. The hyperfine field strength is found from the observed low-temperature electron spin resonance data. The spin dynamics of the paramagnetic phase is characterized by strong broadening of the ESR absorption line, which can be ascribed to the vortex dynamics of a 2D magnet.

cond-mat.str-el↗

arXiv2021

Magnetic correlations in infinite-layer nickelates: an experimental and theoretical multi-method study

We report a comprehensive study of magnetic correlations in LaNiO$_{2}$, a parent compound of the recently discovered family of infinite-layer (IL) nickelate superconductors, using multiple experimental and theoretical methods. Our specific heat, muon-spin rotation ($μ$SR), and magnetic susceptibility measurements on polycrystalline LaNiO$_{2}$ show that long-range magnetic order remains absent down to 2 K. Nevertheless, we detect residual entropy in the low-temperature specific heat, which is compatible with a model fit that includes paramagnon excitations. The $μ$SR and low-field static and dynamic magnetic susceptibility measurements indicate the presence of short-range magnetic correlations and glassy spin dynamics, which we attribute to local oxygen non-stoichiometry in the average infinite-layer crystal structure. This glassy behavior can be suppressed in strong external fields, allowing us to extract the intrinsic paramagnetic susceptibility. Remarkably, we find that the intrinsic susceptibility shows non-Curie-Weiss behavior at high temperatures, in analogy to doped cuprates that possess robust non-local spin fluctuations. The distinct temperature dependence of the intrinsic susceptibility of LaNiO$_{2}$ can be theoretically understood by a multi-method study of the single-band Hubbard model in which we apply complementary cutting-edge quantum many-body techniques (dynamical mean-field theory, cellular dynamical mean-field theory and the dynamical vertex approximation) to investigate the influence of both short- and long-ranged correlations. Our results suggest a profound analogy between the magnetic correlations in parent (undoped) IL nickelates and doped cuprates.

cond-mat.str-el↗

arXiv2021

On the complexity of spinels: Magnetic, electronic, and polar ground states

This review summarizes more than 100 years of research on spinel compounds, mainly focusing on the progress in understanding their magnetic, electronic, and polar properties during the last two decades. Many spinel compounds are magnetic insulators or semiconductors; however, a number of spinel-type metals exists including superconductors and some rare examples of d-derived heavy-fermion compounds. In the early days, they gained importance as ferrimagnetic or even ferromagnetic insulators with relatively high saturation magnetization and high ordering temperatures, with magnetite being the first magnetic mineral known to mankind. However, spinels played an outstanding role in the development of concepts of magnetism, in testing and verifying the fundamentals of magnetic exchange, in understanding orbital-ordering and charge-ordering phenomena. In addition, the A- site as well as the B-site cations in the spinel structure form lattices prone to strong frustration effects resulting in exotic ground-state properties. In case the A-site cation is Jahn-Teller active, additional entanglements of spin and orbital degrees of freedom appear, which can give rise to a spin-orbital liquid or an orbital glass state. The B-site cations form a pyrochlore lattice, one of the strongest contenders of frustration in three dimensions. In addition, in spinels with both cation lattices carrying magnetic moments, competing magnetic exchange interactions become important, yielding ground states like the time-honoured triangular Yafet-Kittel structure. Finally, yet importantly, there exists a long-standing dispute about the possibility of a polar ground state in spinels, despite their reported overall cubic symmetry. Indeed, over the years number of multiferroic spinels were identified.

cond-mat.str-el↗

arXiv2020

Vital role of anisotropy in cubic chiral skyrmion hosts

The impact of magnetic anisotropy on the skyrmion lattice (SkL) state in cubic chiral magnets has been overlooked for long, partly because a semi-quantitative description of the thermodynamically stable SkL phase pocket forming near the Curie temperature could be achieved without invoking anisotropy effects. However, there has been a range of phenomena reported recently in these materials, such as the formation of low-temperature tilted conical and SkL states as well as temperature-induced transformations of lattice geometry in metastable SkL states, where anisotropy was suspected to play a key role. To settle this issue on experimental basis, we quantified the cubic anisotropy in a series of CoZnMn-type cubic chiral magnets. We found that the strength of anisotropy is highly enhanced towards low temperatures in all the compounds, moreover, not only the magnitude but also the character of cubic anisotropy drastically varies upon changing the Co/Mn ratio. We correlate these changes with temperature- and composition-induced variations of the helical modulation vectors, the anharmonicity and structural rearrangements of the metastable SkLs and the spin relaxation rates. Similar systematic studies on magnetic anisotropy may not only pave the way for a quantitative and unified description of the stable and metastable modulated spin textures in cubic chiral magnets but would also help exploring further topological spin textures in this large class of skyrmion hosts.

cond-mat.str-el↗

arXiv2020

Topological magnetic order and superconductivity in EuRbFe$_4$As$_4$

We study single crystals of the magnetic superconductor EuRbFe$_4$As$_4$ by magnetization, electron spin resonance (ESR), angle-resolved photoemission spectroscopy (ARPES) and electrical resistance in pulsed magnetic fields up to 630 kOe. The superconducting state below 36.5 K is almost isotropic and only weakly affected by the development of Eu$^{2+}$ magnetic order at 15 K. On the other hand, for the external magnetic field applied along the c-axis the temperature dependence of the ESR linewidth reveals a Berezinskii-Kosterlitz-Thouless topological transition below 15 K. This indicates that Eu$^{2+}$-planes are a good realization of a two-dimensional XY-magnet, which reflects the decoupling of the Eu$^{2+}$ magnetic moments from superconducting FeAs-layers.

cond-mat.supr-con↗

arXiv2019

Spin-lattice coupling in a ferrimagnetic spinel: The exotic $H$-$T$ phase diagram of MnCr$_2$S$_4$ up to 110 T

In antiferromagnets, the interplay of spin frustration and spin-lattice coupling has been extensively studied as the source of complex spin patterns and exotic magnetism. Here, we demonstrate that, although neglected in the past, the spin-lattice coupling is essential to ferrimagnetic spinels as well. We performed ultrahigh-field magnetization measurements up to 110 T on a Yafet-Kittel ferrimagnetic spinel, MnCr$_2$S$_4$, which was complemented by measurements of magnetostriction and sound velocities up to 60 T. Classical Monte Carlo calculations were performed to identify the complex high-field spin structures. Our minimal model incorporating spin-lattice coupling accounts for the experimental results and corroborates the complete phase diagram, including two new high-field phase transitions at 75 and 85 T. Magnetoelastic coupling induces striking effects: An extremely robust magnetization plateau is embedded between two unconventional spin-asymmetric phases. Ferrimagnetic spinels provide a new platform to study asymmetric and multiferroic phases stabilized by spin-lattice coupling.

cond-mat.str-el↗

arXiv2019

Structure, superconductivity, and magnetism in Rb1-xFe1.6Se2-zSz

The single-crystal growth, stoichiometry, and structure of Rb1-xFe2-ySe2-zSz crystals with substitution of Se by S are reported. The variation of the magnetic and thermodynamic parameters of samples was studied by differential-scanning calorimetry, magnetic susceptibility, conductivity, and specific heat. The experimental results are discussed within a T-z phase diagram, which includes vacancy-ordered and vacancy-disordered antiferromagnetic (AFM), superconducting (SC), and non-superconducting phases. The structural study revealed change in the local environment of the Fe tetrahedrons depending on substitution: a reduction of the Fe-Fe and Fe-Ch(chalcogen) bond lengths and a tendency for the six out of eight bond angles to approach values for a regular tetrahedron suggesting a reduction of structural distortions with substitution. With increasing substitution, a lowering of the superconducting transition temperature Tc was observed; the percolation threshold for the SC state is located at the substitution z = 1.2. The SC state was found to coexist with the AFM state that persists in all samples independent of substitution. The temperature of the transition into the AFM state TN shows a monotonous decrease indicating a weakening of the AFM interactions with increasing substitution. The AFM phase exhibits an iron-vacancy-ordered structure below the structural transition at Ts. The temperature Ts shows a non-monotonous variation: a decrease with increasing z up to 1.3, followed by an increase for further increasing z. The suppression of the superconductivity with substitution is accompanied by a significant reduction of the density of states at the Fermi energy and a weakening of the electronic correlations in the studied system.

cond-mat.supr-con↗

arXiv2019

Spin relaxation in Cs$_2$CuCl$_{4-x}$Br$_x$

The quantum-spin S = 1=2 chain system Cs$_2$CuCl$_4$ is of high interest due to competing anti-ferromagnetic intra-chain J and inter-chain exchange J' interactions and represents a paramount example for Bose-Einstein condensation of magnons [R. Coldea et al., Phys. Rev. Lett. 88, 137202 (2002)]. Substitution of chlorine by bromine allows tuning the competing exchange interactions and corresponding magnetic frustration. Here we report on electron spin resonance (ESR) in single crystals of Cs$_2$CuCl$_{4-x}$Br$_x$ with the aim to analyze the evolution of anisotropic exchange contributions. The main source of the ESR linewidth is attributed to the uniform Dzyaloshinskii-Moriya interaction. The vector components of the Dzyaloshinskii-Moriya interaction are determined from the angular dependence of the ESR spectra using a high-temperature approximation. The obtained results support the site selectivity of the Br substitution suggested from the evolution of lattice parameters and magnetic susceptibility dependent on the Br concentration.

cond-mat.str-el↗

arXiv2018

Weak ferromagnetism and glassy state in kappa-(BEDT-TTF)2Hg(SCN)2Br

Since the first observation of weak ferromagnetism in the charge-transfer salt kappa-(BEDT-TTF)2-Cu[N(CN)2]Cl [U. Welp et al., Phys. Rev. Lett. 69, 840 (1992)], no further evidence of ferromagnetism in this class of organic materials has been reported. Here we present static and dynamic spin susceptibility measurements on kappa-(BEDT-TTF)2Hg(SCN)2Br revealing weak ferromagnetism below about TWF = 20 K. We suggest that frustrated spins in the molecular dimers suppress long-range order, forming a spin-glass ground state in the insulating phase.

cond-mat.str-el↗

arXiv2018

Sub-gap optical response across the structural phase transition in van der Waals layered α-RuCl$_3$

We report magnetic, thermodynamic, thermal expansion, and on detailed optical experiments on the layered compound $α$-RuCl$_3$ focusing on the THz and sub-gap optical response across the structural phase transition from the monoclinic high-temperature to the rhombohedral low-temperature structure, where the stacking sequence of the molecular layers is changed. This type of phase transition is characteristic for a variety of tri-halides crystallizing in a layered honeycomb-type structure and so far is unique, as the low-temperature phase exhibits the higher symmetry. One motivation is to unravel the microscopic nature of spin-orbital excitations via a study of temperature and symmetry-induced changes. We document a number of highly unusual findings: A characteristic two-step hysteresis of the structural phase transition, accompanied by a dramatic change of the reflectivity. An electronic excitation, which appears in a narrow temperature range just across the structural phase transition, and a complex dielectric loss spectrum in the THz regime, which could indicate remnants of Kitaev physics. Despite significant symmetry changes across the monoclinic to rhombohedral phase transition, phonon eigenfrequencies and the majority of spin-orbital excitations are not strongly influenced. Obviously, the symmetry of the single molecular layers determine the eigenfrequencies of most of these excitations. Finally, from this combined terahertz, far- and mid-infrared study we try to shed some light on the so far unsolved low energy (< 1eV) electronic structure of the ruthenium $4d^5$ electrons in $α$-RuCl$_3$.

cond-mat.str-el↗

arXiv2017

Complex nature of magnetic field-induced ferroelectricity in GdCrTiO5

This work shows an unconventional route for spin-driven ferroelectricity originating from a metastable magnetic field-induced canting of chromium sublattice in the presence of gadolinium moments in GdCrTiO5 at low temperatures. Compared to the isostructural neodymium compound, significant differences of magnetism and magnetoelectric effects are seen. We present the results of thorough investigations of temperature and magnetic field dependent magnetization as well as ac and dc magnetic susceptibility. These bulk measurements are complemented by local-probe spectroscopy utilizing electron-spin resonance and muon-spin rotation/relaxation for probing the chromium moments. Ferroelectric order is inferred from pyro- and magnetocurrent measurements. GdCrTiO5 shows a pyrocurrent signal around 10 K, only if the system is cooled in an applied magnetic field exceeding 10 kOe. A distinct spin-driven ferroelectric order is revealed in this state for temperatures below 10 K, which can be switched by changing magnetic-field direction and the polarity of the electric field. But, the magnetic measurements reveal no clear signature of long-range magnetic ordering. The presence of such meta-magnetoelectric-type behaviour in the absence of any meta-magnetic behavior is rare in the literature. Our microscopic spectroscopy results indicate significant changes of the magnetic properties around 10 K. Probably there is an exchange frustration between Gd and Cr moments, which prevents long-range magnetic ordering at further high temperature. Below 10 K, weak magnetic ordering occurs by minimizing frustration due to lattice distortion, which helps in magnetodielectric coupling. However, the non-polar distortion attains appreciable values after application of magnetic fields above 10 kOe to break the spatial inversion symmetry, which creates ferroelectricity.

cond-mat.str-el↗

arXiv2017

Structure, magnetic susceptibility and specific heat of the spin-orbital-liquid candidate FeSc2S4 : Influence of fe off-stoichiometry

We report structural, susceptibility and specific heat studies of stoichiometric and off-stoichiometric poly- and single crystals of the A-site spinel compound FeSc2S4. In stoichiometric samples no long-range magnetic order is found down to 1.8 K. The magnetic susceptibility of these samples is field independent in the temperature range 10 - 400 K and does not show irreversible effects at low temperatures. In contrast, the magnetic susceptibility of samples with iron excess shows substantial field dependence at high temperatures and manifests a pronounced magnetic irreversibility at low temperatures with a difference between ZFC and FC susceptibilities and a maximum at 10 K reminiscent of a magnetic transition. Single crystal x-ray diffraction of the stoichiometric samples revealed a single phase spinel structure without site inversion. In single crystalline samples with Fe excess besides the main spinel phase a second ordered single-crystal phase was detected with the diffraction pattern of a vacancy-ordered superstructure of iron sulfide, close to the 5C polytype Fe9S10. Specific heat studies reveal a broad anomaly, which evolves below 20 K in both stoichiometric and off-stoichiometric crystals. We show that the low-temperature specific heat can be well described by considering the low-lying spin-orbital electronic levels of Fe2+ ions. Our results demonstrate significant influence of excess Fe ions on intrinsic magnetic behavior of FeSc2S4 and provide support for the spin-orbital liquid scenario proposed in earlier studies for the stoichiometric compound.

cond-mat.mtrl-sci↗

arXiv2016

Structural, magnetic, electric, dielectric, and thermodynamic properties of multiferroic GeV4S8

The lacunar spinel GeV4S8 undergoes orbital and ferroelectric ordering at the Jahn-Teller transition around 30 K and exhibits antiferromagnetic order below about 14 K. In addition to this orbitally driven ferroelectricity, lacunar spinels are an interesting material class, as the vanadium ions form V4 clusters representing stable molecular entities with a common electron distribution and a well-defined level scheme of molecular states resulting in a unique spin state per V4 molecule. Here we report detailed x-ray, magnetic susceptibility, electrical resistivity, heat capacity, thermal expansion, and dielectric results to characterize the structural, electric, dielectric, magnetic, and thermodynamic properties of this interesting material, which also exhibits strong electronic correlations. From the magnetic susceptibility, we determine a negative Curie-Weiss temperature, indicative for antiferromagnetic exchange and a paramagnetic moment close to a spin S = 1 of the V4 molecular clusters. The low-temperature heat capacity provides experimental evidence for gapped magnon excitations. From the entropy release, we conclude about strong correlations between magnetic order and lattice distortions. In addition, the observed anomalies at the phase transitions also indicate strong coupling between structural and electronic degrees of freedom. Utilizing dielectric spectroscopy, we find the onset of significant dispersion effects at the polar Jahn-Teller transition. The dispersion becomes fully suppressed again with the onset of spin order. In addition, the temperature dependencies of dielectric constant and specific heat possibly indicate a sequential appearance of orbital and polar order.

cond-mat.str-el↗

arXiv2016

On the multiferroic skyrmion-host GaV4S8

The lacunar spinel GaV4S8 exhibits orbital ordering at 44 K and shows a complex magnetic phase diagram below 12.7 K, which includes ferromagnetic and cycloidal spin order. At low but finite external magnetic fields, Néel-type skyrmions are formed in this material. Skyrmions are whirl-like spin vortices that have received great theoretical interest because of their non-trivial spin topology and that are also considered as basic entities for new data-storage technologies. Interestingly, we found that the orbitally ordered phase shows sizable ferroelectric polarization and that excess spin-driven polarizations appear in all magnetic phases, including the skyrmion-lattice phase. Hence, GaV4S8 shows simultaneous magnetic and polar order and belongs to the class of multiferroics, materials that attracted enormous attention in recent years. Here, we summarize the existing experimental information on the magnetic, electronic, and dielectric properties of GaV4S8. By performing detailed magnetic susceptibility, resistivity, specific heat, and dielectric experiments, we complement the low-temperature phase diagram. Specifically, we show that the low-temperature and low-field ground state of GaV4S8 seems to have a more complex spin configuration than purely collinear ferromagnetic spin order. In addition, at the structural Jahn-Teller transition the magnetic exchange interaction changes from antiferromagnetic to ferromagnetic. We also provide experimental evidence that the vanadium V4 clusters in GaV4S8 can be regarded as molecular units with spin 1/2. However, at high temperatures deviations in the susceptibility show up, indicating that either the magnetic moments of the vanadium atoms fluctuate independently or excited states of the V4 molecule become relevant.

cond-mat.str-el↗

arXiv2016

Influence of the FFLO-like State on the Upper Critical Field of a S/F Bilayer: Angular and Temperature Dependence

We investigated the upper critical magnetic field, $H_{c}$, of a superconductor-ferromagnet (S/F) bilayer of Nb/Cu$_{41}$Ni$_{59}$ and a Nb film (as reference). We obtained the dependence of $H_{c\perp}$ and $H_{c\parallel}$ (perpendicular and parallel to the film plane, respectively) on the temperature, $T$, by measurements of the resistive transitions and the dependence on the inclination angle, $θ$, of the applied field to the film plane, by non-resonant microwave absorption. Over a wide range, $H_{c\perp}$ and $H_{c\parallel}$ show the temperature dependence predicted by the Ginzburg-Landau theory. At low temperatures and close to the critical temperature deviations are observed. While $H_{c}(θ)$ of the Nb film follows the Tinkham prediction for thin superconducting films, the Nb/Cu$_{41}$Ni$_{59}$-bilayer data exhibit deviations when $θ$ approaches zero. We attribute this finding to the additional anisotropy induced by the quasi-one-dimensional Fulde-Ferrell-Larkin-Ovchinnikov (FFLO)-like state and propose a new vortex structure in S/F bilayers, adopting the segmentation approach from high-temperature superconductors.

cond-mat.supr-con↗

arXiv2015

Quasi-two-dimensional $S=1/2$ magnetism of Cu[C$_6$H$_2$(COO)$_4$][C$_2$H$_5$NH$_3$]$_2$

We report structural and magnetic properties of the spin-$\frac12$ quantum antiferromagnet Cu[C$_6$H$_2$(COO)$_4$][C$_2$H$_5$NH$_3$]$_2$ by means of single-crystal x-ray diffraction, magnetization, heat capacity, and electron spin resonance (ESR) measurements on polycrystalline samples, as well as band-structure calculations. The triclinic crystal structure of this compound features CuO$_4$ plaquette units connected into a two-dimensional framework through anions of the pyromellitic acid [C$_6$H$_2$(COO)$_4$]$^{4-}$. The ethylamine cations [C$_2$H$_5$NH$_3]^+$ are located between the layers and act as spacers. Magnetic susceptibility and heat capacity measurements establish a quasi-two-dimensional, weakly anisotropic and non-frustrated spin-$\frac12$ square lattice with the ratio of the couplings $J_a/J_c\simeq 0.7$ along the $a$ and $c$ directions, respectively. No clear signatures of the long-range magnetic order are seen in thermodynamic measurements down to 1.8\,K. However, the gradual broadening of the ESR line suggests that magnetic ordering occurs at lower temperatures. Leading magnetic couplings are mediated by the organic anion of the pyromellitic acid and exhibit a non-trivial dependence on the Cu--Cu distance, with the stronger coupling between those Cu atoms that are further apart.

cond-mat.mtrl-sci↗