arXiv subjects

H. -H. Klauss

Publications and source records attributed to H. -H. Klauss.

At least 19 recordsLinked to original sources

arXiv2025

Magnetic order and Li-diffusion in the 1/3-filled Kagome layers of antiperovskite Lithium-ion battery materials (Li$_2$Fe)SO and (Li$_2$Fe)SeO

The recently discovered lithium-rich antiperovskites (Li$_2$Fe)SeO and (Li$_2$Fe)SO host lithium and iron ions on the same atomic position which octahedrally coordinates to central oxygens. In a cubic antiperovskite these sites form Kagome planes stacked along the <111> directions which triangular motifs induce high geometric frustration in the diluted magnetic sublattice for antiferromagnetic interactions. Despite their compelling properties as high-capacity Li-ion battery cathode materials, very little is known about the electronic and magnetic properties of lithium-rich antiperovskites. We report static magnetization, Mössbauer, and NMR studies on both compounds. Our data reveal a Pauli paramagnetic-like behaviour, a long-range antiferromagnetically ordered ground state below 50 K and a regime of short-range magnetic correlations up to 100 K. Our results are consistent with a random Li-Fe distribution on the shared lattice position. In addition, Li-hopping is observed above 200 K with an activation energy of E$_a$ = 0.47 eV. Overall, our data elucidate static magnetism in a disordered magnetically frustrated and presumably semimetallic system with thermally induced ion diffusion dynamics.

cond-mat.mtrl-sci↗

arXiv2025

Quasi-two-dimensional magnetism and antiferromagnetic ground state in Li$_2$FeSiO$_4$

Our experimental (neutron diffraction, Mössbauer spectroscopy, magnetic susceptibility, specific heat) and numerical studies on the evolution of short- and long-range magnetic order in $γ_{\rm II}$-Li$_2$FeSiO$_4$ suggest a quasi-two-dimensional (2D) nature of magnetism. The experimental data obtained on single crystals imply long-range antiferromagnetic order below $T_{\rm N}= 17$~K. A broad maximum in magnetic susceptibility $χ$ at $T_{\rm m}\simeq 28$~K, observation of magnetic entropy changes up to 100~K and anisotropy in $χ$ are indicative of low-dimensional magnetism and suggest short-range magnetic correlations up to 200~K. Neutron diffraction shows that long-range antiferromagnetic order is characterised by the propagation vector k=(1/2,0,1/2). The ordered moment $μ= 2.50(2) μ_B$ /Fe, at $T = 1.5$~K, is along the crystallographic $a$-axis. This is consistent with the observed static hyperfine field of $B_{\rm hyp}=14.8(3)$\,T by Mössbauer spectroscopy which indicates significant orbital contributions. The temperature dependence of $B_{\rm hyp}$ yields the critical exponent $β=0.116(12)$ which is in the regime of the 2D Ising behaviour. LSDA+U studies exploiting the experimental spin structure suggest dominating magnetic exchange coupling within the $ac$-layers (i.e., $J_3\simeq -6$~K and $J_6\simeq-2$~K) while interlayer coupling is much smaller and partly frustrated. This confirms the 2D nature of magnetism and is in full agreement with the experimental findings.

cond-mat.str-el↗

arXiv2023

Magnetism in Kitaev Quantum Spin Liquid Candidate RuBr$_3$

The present studies show that long-range magnetic order takes place in RuBr$_3$ at $\approx$ 34 K. The observations of clear oscillations in the muon time spectra demonstrate the presence of well-defined internal fields at the muon sites. The magnetic ordering appears to be very robust and static suggesting a more conventional nature of magnetic ordering in the RuBr$_3$ system at zero field. Present investigations prove that in RuBr$_3$ the Kitaev interactions are likely to be weakened at zero field in comparison to the $α$-RuCl$_3$ system. This proves that it is possible to tune the Kitaev interactions by replacing Cl with heavier halogen elements such as Br.

cond-mat.str-el↗

arXiv2023

Designing the stripe-ordered cuprate phase diagram through uniaxial-stress

The ability to efficiently control charge and spin in the cuprate high-temperature superconductors is crucial for fundamental research and underpins technological development. Here, we explore the tunability of magnetism, superconductivity and crystal structure in the stripe phase of the cuprate La_2-xBa_xCuO_4, with x = 0.115 and 0.135, by employing temperature-dependent (down to 400 mK) muon-spin rotation and AC susceptibility, as well as X-ray scattering experiments under compressive uniaxial stress in the CuO_2 plane. A sixfold increase of the 3-dimensional (3D) superconducting critical temperature T_c and a full recovery of the 3D phase coherence is observed in both samples with the application of extremely low uniaxial stress of 0.1 GPa. This finding demonstrates the removal of the well-known 1/8-anomaly of cuprates by uniaxial stress. On the other hand, the spin-stripe order temperature as well as the magnetic fraction at 400 mK show only a modest decrease under stress. Moreover, the onset temperatures of 3D superconductivity and spin-stripe order are very similar in the large stress regime. However, a substantial decrease of the magnetic volume fraction and a full suppression of the low-temperature tetragonal structure is found at elevated temperatures, which is a necessary condition for the development of the 3D superconducting phase with optimal T_c. Our results evidence a remarkable cooperation between the long-range static spin-stripe order and the underlying crystalline order with the three-dimensional fully coherent superconductivity. Overall, these results suggest that the stripe- and the SC order may have a common physical mechanism.

cond-mat.supr-con↗

arXiv2023

Interplay of structure and magnetism in LuFe4Ge2 tuned by hydrostatic pressure

LuFe$_4$Ge$_2$ crystallizes in the ZrFe$_4$Si$_2$-type structure, hosting chains of Fe-tetrahedra giving rise to geometric frustration and low-dimensionality. The compound orders antiferromagnetically at around 36 K accompanied by a simultaneous structural transition from a tetragonal to an orthorhombic phase. The hydrostatic pressure dependence of the magnetic and structural transitions is investigated using electrical-transport, ac magnetic-susceptibility, ac calorimetry, M$\ddot{\rm o}$ssbauer, muon-spin relaxation ($μ$SR), and x-ray diffraction measurements. External pressure suppresses the first-order transition to the antiferromagnetic phase (AFM1) around 1.8 GPa. The structural transition is largely unaffected by pressure and remains between 30 to 35 K for pressures up to 2 GPa. A second antiferromagnetic phase (AFM2) is observed at higher pressures. The transition from the paramagnetic to the AFM2 phase is of second-order nature and appears to be connected to the structural transition. The magnetic volume fraction obtained from $μ$SR and M$\ddot{\rm o}$ssbauer measurements reveal that the entire sample undergoes magnetic ordering in both magnetic phases. In addition, similar low-temperature muon-precession frequencies in AFM1 and AFM2 phases point at similar ordered moments and magnetic structures in both phases. Our results further indicate enhanced magnetic fluctuations in the pressure induced AFM2 phase. The experimental observations together with density functional theory calculations suggest that the magnetic and structural order parameters in LuFe$_4$Ge$_2$ are linked by magnetic frustration, causing the simultaneous magneto-structural transition.

cond-mat.str-el↗

arXiv2020

Destruction of long-range magnetic order in an external magnetic field and the associated spin dynamics in Cu2GaBO5 and Cu2AlBO5 ludwigites

The quantum spin systems Cu$_2$M'BO$_5$ (M' = Al, Ga) with the ludwigite crystal structure consist of a structurally ordered Cu$^{2+}$ sublattice in the form of three-leg ladders, interpenetrated by a structurally disordered sublattice with a statistically random site occupation by magnetic Cu$^{2+}$ and nonmagnetic Ga$^{3+}$ or Al$^{3+}$ ions. A microscopic analysis based on density-functional-theory calculations for Cu$_2$GaBO$_5$ reveals a frustrated quasi-two-dimensional spin model featuring five inequivalent antiferromagnetic exchanges. A broad low-temperature $^{11}$B nuclear magnetic resonance points to a considerable spin disorder in the system. In zero magnetic field, antiferromagnetic order sets in below $T_\text{N}$ $\approx$ 4.1 K and ~2.4 K for the Ga and Al compounds, respectively. From neutron diffraction, we find that the magnetic propagation vector in Cu$_2$GaBO$_5$ is commensurate and lies on the Brillouin-zone boundary in the (H0L) plane, $\mathbf{q}_\text{m}$ = (0.45 0 -0.7), corresponding to a complex noncollinear long-range ordered structure with a large magnetic unit cell. Muon spin relaxation is monotonic, consisting of a fast static component typical for complex noncollinear spin systems and a slow dynamic component originating from the relaxation on low-energy spin fluctuations. Gapless spin dynamics in the form of a diffuse quasielastic peak is also evidenced by inelastic neutron scattering. Most remarkably, application of a magnetic field above 1 T destroys the static long-range order, which is manifested in the gradual broadening of the magnetic Bragg peaks. We argue that such a crossover from a magnetically long-range ordered state to a spin-glass regime may result from orphan spins on the structurally disordered magnetic sublattice, which are polarized in magnetic field and thus act as a tuning knob for field-controlled magnetic disorder.

cond-mat.str-el↗

arXiv2020

Using uniaxial stress to probe the relationship between competing superconducting states in a cuprate with spin-stripe order

We report muon spin rotation and magnetic susceptibility experiments on in-plane stress effects on the static spin-stripe order and superconductivity in the cuprate system La2-xBaxCuO4 with x = 0.115. An extremely low uniaxial stress of 0.1 GPa induces a substantial decrease in the magnetic volume fraction and a dramatic rise in the onset of 3D superconductivity, from 10 to 32 K; however, the onset of at-least-2D superconductivity is much less sensitive to stress. These results show not only that large-volume-fraction spin-stripe order is anti-correlated with 3D superconducting (SC) coherence, but also that these states are energetically very finely balanced. Moreover, the onset temperatures of 3D superconductivity and spin-stripe order are very similar in the large stress regime. These results strongly suggest a similar pairing mechanism for spin-stripe order, the spatially-modulated 2D and uniform 3D SC orders, imposing an important constraint on theoretical models.

cond-mat.supr-con↗

arXiv2020

Long-range magnetic order in the ${\tilde S}=1/2$ triangular lattice antiferromagnet KCeS$_2$

Recently, several putative quantum spin liquid (QSL) states were discovered in ${\tilde S} = 1/2$ rare-earth based triangular-lattice antiferromagnets (TLAF) with the delafossite structure. A way to clarify the origin of the QSL state in these systems is to identify ways to tune them from the putative QSL state towards long-range magnetic order. Here, we introduce the Ce-based TLAF KCeS$_2$ and show via low-temperature specific heat and $μ$SR investigations that it yields magnetic order below $T_{\mathrm N} = 0.38$ K despite the same delafossite structure. We identify a well separated ${\tilde S} = 1/2$ ground state for KCeS$_2$ from inelastic neutron scattering and embedded-cluster quantum chemical calculations. Magnetization and electron spin resonance measurements on single crystals indicate a strong easy-plane $g$~factor anisotropy, in agreement with the ab initio calculations. Finally, our specific-heat studies reveal an in-plane anisotropy of the magnetic field-temperature phase diagram which may indicate anisotropic magnetic interactions in KCeS$_2$.

cond-mat.str-el↗

arXiv2020

Anomalous Hall effect in Weyl semimetal half Heusler compounds RPtBi (R = Gd and Nd)

Topological materials ranging from topological insulators to Weyl and Dirac semimetals form one of the most exciting current fields in condensed-matter research. Many half-Heusler compounds, RPtBi (R= rare earth) have been theoretically predicted to be topological semimetals. Among various topological attributes envisaged in RPtBi, topological surface states, chiral anomaly and planar Hall effect have been observed experimentally. Here, we report on an unusual intrinsic anomalous Hall effect (AHE) in the antiferromagnetic Heusler Weyl semimetal compounds GdPtBi and NdPtBi that is observed over a wide temperature range. In particular, GdPtBi exhibits an anomalous Hall conductivity of up to 60 ohm-1cm-1 and an anomalous Hall angle as large as 23%. Muon spin resonance (mu-SR) studies of GdPtBi indicate a sharp antiferromagnetic transition (T_N) at 9 K without any noticeable magnetic correlations above T_N. Our studies indicate that Weyl points in these half-Heuslers are induced by a magnetic field via exchange-splitting of the electronic bands at or near to the Fermi energy which is the source of the chiral anomaly and the AHE.

cond-mat.mtrl-sci↗

arXiv2020

Nematic Fluctuations in Iron-Oxychalcogenide Mott Insulators

Nematic fluctuations occur in a wide range of physical systems from liquid crystals to biological molecules to solids such as exotic magnets, cuprates and iron-based high-$T_c$ superconductors. Nematic fluctuations are thought to be closely linked to the formation of Cooper-pairs in iron-based superconductors. It is unclear whether the anisotropy inherent in this nematicity arises from electronic spin or orbital degrees of freedom. We have studied the iron-based Mott insulators La$_{2}$O$_{2}$Fe$_{2}$O$M$$_{2}$ $M$ = (S, Se) which are structurally similar to the iron pnictide superconductors. They are also in close electronic phase diagram proximity to the iron pnictides. Nuclear magnetic resonance (NMR) revealed a critical slowing down of nematic fluctuations as observed by the spin-lattice relaxation rate ($1/T_1$). This is complemented by the observation of a change of electrical field gradient over a similar temperature range using Mössbauer spectroscopy. The neutron pair distribution function technique applied to the nuclear structure reveals the presence of local nematic $C_2$ fluctuations over a wide temperature range while neutron diffraction indicates that global $C_{4}$ symmetry is preserved. Theoretical modeling of a geometrically frustrated spin-$1$ Heisenberg model with biquadratic and single-ion anisotropic terms provides the interpretation of magnetic fluctuations in terms of hidden quadrupolar spin fluctuations. Nematicity is closely linked to geometrically frustrated magnetism, which emerges from orbital selectivity. The results highlight orbital order and spin fluctuations in the emergence of nematicity in Fe-based oxychalcogenides. The detection of nematic fluctuation within these Mott insulator expands the group of iron-based materials that show short-range symmetry-breaking.

cond-mat.str-el↗

arXiv2020

Impact of disorder on dynamics and ordering in the honeycomb lattice iridate Na$_2$IrO$_3$

Kitaev's honeycomb spin-liquid model and its proposed realization in materials such as $α$-RuCl$_3$, Li$_2$IrO$_3$ and Na$_2$IrO$_3$ continue to present open questions about how the dynamics of a spin-liquid are modified in the presence of non-Kitaev interactions as well as the presence of inhomogeneities. Here we use $^{23}$Na nuclear magnetic resonance to probe both static and dynamical magnetic properties in single crystal Na$_2$IrO$_3$. We find that the NMR shift follows the bulk susceptibility above 30 K but deviates from it below; moreover below $T_N$ the spectra show a broad distribution of internal magnetic fields. Both of these results provide evidence for inequivalent magnetic sites at low temperature, suggesting inhomogeneities are important for the magnetism. The spin-lattice relaxation rate is isotropic and diverges at $T_N$, suggesting that the Kitaev cubic axes may control the critical quantum spin fluctuations. In the ordered state, we observe gapless excitations, which may arise from site substitution, emergent defects from milder disorder, or possibly be associated with nearby quantum paramagnetic states distinct from the Kitaev spin liquid.

cond-mat.str-el↗

arXiv2020

Ground state and low-temperature magnetism of the quasi-two-dimensional honeycomb compound InCu$_{2/3}$V$_{1/3}$O$_3$

We report a combined $^{115}$In NQR, $^{51}$V NMR and $μ$SR spectroscopic study of the low-temperature magnetic properties of InCu$_{2/3}$V$_{1/3}$O$_3$, a quasi-two dimensional (2D) compound comprising in the spin sector a honeycomb lattice of antiferromagnetically coupled spins $S=1/2$ associated with Cu$^{2+}$ ions. Despite substantial experimental and theoretical efforts, the ground state of this material was has not been ultimately identified. In particular, two characteristic temperatures of about $\sim 40$ K and $\sim 20$ K manifesting themselves as anomalies in different magnetic measurements are discussed controversially. A combined analysis of the experimental data complemented with theoretical calculations of exchange constants enabled us to identify below 39 K an ``intermediate'' quasi-2D static spin state. This spin state is characterized by a staggered magnetization with a temperature evolution that agrees with the predictions for the 2D XY model. We observe that this state gradually transforms at 15 K into a fully developed 3D antiferromagnetic Néel state. We ascribe such an extended quasi-2D static regime to an effective magnetic decoupling of the honeycomb planes due to a strong frustration of the interlayer exchange interactions which inhibits long-range spin-spin correlations across the planes. Interestingly, we find indications of the topological Berezinsky-Kosterlitz-Thouless transition in the quasi-2D static state of the honeycomb spin-1/2 planes of InCu$_{2/3}$V$_{1/3}$O$_3$.

cond-mat.str-el↗

arXiv2019

Quantum spin liquid ground state in the disorder free triangular lattice NaYbS$_2$

Rare-earth delafossites were recently proposed as promising candidates for the realization of an effective $S$=1/2 quantum spin liquid (QSL) on the triangular lattice. In contrast to the most actively studied triangular-lattice antiferromagnet YbMgGaO$_4$, which is known for considerable structural disorder due to site intermixing, NaYbS$_2$ delafossite realizes structurally ideal triangular layers. We present detailed $μ$SR studies on this regular (undistorted) triangular Yb sublattice based system with effective spin $J_{\mathrm{eff}}=1/2$ in the temperature range 0.05 - 40 K. Zero-field (ZF) and longitudinal field (LF) $μ$SR studies confirm the absence of any long range magnetic order state down to 0.05K ($\sim J$/80). Current $μ$SR results together with the so far available bulk characterization data suggest that NaYbS$_2$ is an ideal candidate to identify QSL ground state.

cond-mat.str-el↗

arXiv2019

Muon spin rotation measurements on RbEuFe$_{4}$As$_{4}$ under pressure

We report muon spin rotation and magnetization measurements on the magnetic superconductor RbEuFe$_{4}$As$_{4}$ under hydrostatic pressures up to 3.8 GPa. At ambient pressure, RbEuFe$_{4}$As$_{4}$ exhibits a superconducting transition at $T_{c} \approx$ 36.5 K and a magnetic transition at $T_{m} \approx$ 15 K below which the magnetic and the superconducting order coexist. With increasing pressure, $T_{c}$ decreases while $T_{m}$ and the ordered Eu magnetic moment increase. In contrast to iron-based superconductors with ordering Fe moments, the size of the ordered Eu moment is not proportional to $T_{m}$. The muon spin rotation signal is dominated by the magnetic response impeding the determination of the superconducting properties.

cond-mat.supr-con↗

arXiv2019

Coupled Magnetic and Superconducting Transitions in Sr$_{2}$VO$_{3}$FeAs Under Pressure

We report muon spin rotation ($μ$SR) and magnetization measurements on superconducting Sr$_{2}$VO$_{3}$FeAs under pressure. At ambient pressure, Sr$_{2}$VO$_{3}$FeAs undergoes an antiferromagnetic transition of the V moments at $T_{N}$ and becomes superconducting at $T_{c}<T_{N}$. As a function of pressure, $T_{N}$ initially decreases while $T_{c}$ increases. Surprisingly, once $T_{N}\approx T_{c}$ at 0.6~GPa, $T_{N}$ reverses its trend and increases together with $T_{c}$ suggesting that the static V magnetism is a prerequisite for superconductivity. We explain this cooperative coupling by a possible localization of the V 3$d$ states below the magnetic transition which enables the nesting of the Fermi surface necessary for superconductivity.

cond-mat.supr-con↗

arXiv2019

Disordered magnetism in the double perovskite LaCaScIrO6 with a distorted fcc lattice of Ir4+

The synthesis and characterization of the previously unknown material LaCaScIrO$_6$ is reported. LaCaScIrO$_6$ presents a new example of the rare case of a double perovskite with the strongly spin-orbit coupled 5\textit{d}-ion Ir$^{4+}$ as its only magnetic species, forming a monoclinically distorted version of the frustrated fcc lattice. Magnetization measurements show a weak anomaly at 8~K. The Curie-Weiss temperature Θ$_{CW}$ and effective magnetic moment μ$_{eff}$ of LaCaScIrO$_6$ are in close proximity to the related compound La$_2$MgIrO$_6$ but differ from La$_2$ZnIrO$_6$. This suggests that the nature of the non-magnetic \textit{B}-ion, namely its \textit{d}-orbital filling has a strong influence on the magnetic properties. The \textit{d}$^{0}$-ions Sc$^{3+}$ and Mg$^{2+}$ allow a different kind of exchange interactions within the Ir-sublattice than the \textit{d}$^{10}$-ion Zn$^{2+}$. In addition, ac-susceptibility data does not show signs of a spin-glass ground state. The nature of the magnetism in LaCaScIrO$_6$ has been further elucidated using muon spin relaxation measurements. The zero-field measurements reveal the absence of well defined oscillations down to 1.6\,K, while temperature dependent $μ$SR studies show an anomaly at 8\,K. Overall, our results suggest the presence of two different magnetic environments or domains in LaCaScIrO$_6$, which is likely related to its structural features.

cond-mat.str-el↗

arXiv2019

Extended Magnetic Dome Induced by Low Pressures in Superconducting FeSe$_\mathrm{1\text{-}x}$S$_\mathrm{x}$

We report muon spin rotation ($μ$SR) and magnetization measurements under pressure on Fe$_{1+δ}$Se$_\mathrm{1\text{-}x}$S$_\mathrm{x}$ with x $\approx 0.11$.Above $p\approx0.6$ GPa we find microscopic coexistence of superconductivity with an extended dome of long range magnetic order that spans a pressure range between previously reported separated magnetic phases. The magnetism initially competes on an atomic scale with the coexisting superconductivity leading to a local maximum and minimum of the superconducting $T_\mathrm{c}(p)$. The maximum of $T_\mathrm{c}$ corresponds to the onset of magnetism while the minimum coincides with the pressure of strongest competition. A shift of the maximum of $T_\mathrm{c}(p)$ for a series of single crystals with x up to 0.14 roughly extrapolates to a putative magnetic and superconducting state at ambient pressure for x $\geq0.2$.

cond-mat.supr-con↗

arXiv2019

Magnetic Field tuning of low energy spin dynamics in the single-atomic magnet Li$_2$(Li$_{1-x}$Fe$_x$)N

We present a systematic 57Fe-Moessbauer study on highly diluted Fe centers in Li2(Li1-xFex)N single-crystals as a function of temperature and magnetic field applied transverse and longitudinal with respect to the single-ion anisotropy axis. Below 30 K the Fe centers exhibit a giant magnetic hyperfine field of E_A = 70.25(2)T parallel to the axis of strongest electric field gradient Vzz = -154.0(1) V/A2. Fluctuations of the magnetic hyperfine field are observed between 50K and 300K and described by the Blume two-level relaxation model. From the temperature dependence of the uctuation rate an Orbach spin-lattice relaxation process is deduced. An Arrhenius analysis yields a single thermal activation barrier of E_A = 570(6)K and an attempt frequency nu_0 = 309(10) GHz. Moessbauer spectroscopy studies with applied transverse magnetic fields up to 5T reveal a large increase of the uctuation rate by more than one order of magnitude. In longitudinal magnetic fields a splitting of the uctuation rate into two branches is observed consistent with a Zeeman induced modifcation of the energy levels. The experimental observations are qualitatively reproduced by a single-ion effective spin Hamiltonian analysis assuming a Fe1+ d7 charge state with unquenched orbital moment and a J = 7=2 ground state. It is demonstrated that a weak axial single-ion anisotropy D of the order of a few Kelvin can cause a two orders of magnitude larger energy barrier for longitudinal spin fluctuations.

cond-mat.str-el↗