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H. -H. Klauss

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

At least 37 records · Page 2Linked to original sources

Tuning interactions in the spin-ice materials Dy$_2$Ge$_{2-x}$Si$_x$O$_7$ by silicon substitution

We report that the lattice constant of Dy$_2$Ge$_{2-x}$Si$_x$O$_7$ ($x=0, 0.02, 0.08, 0.125$) can be systematically reduced by substituting the non-magnetic germanium ion in the cubic pyrochlore oxide with silicon. A multi-anvil high-pressure synthesis was performed up to 16 GPa and 1100 $^\circ$C to obtain polycrystalline samples in a solid-state reaction. Measurements of magnetization, ac susceptibility, and heat capacity reveal the typical signatures of a spin-ice phase. From the temperature shift of the peaks, observed in the temperature-dependent heat capacity, we deduce an increase of the strength of the exchange interaction. In conclusion, the reduced lattice constant leads to a changed ratio of the competing exchange and dipolar interaction. This puts the new spin-ice compounds closer towards the phase boundary of short-range spin-ice arrangement and antiferromagnetic long-range order consistent with an observed reduction of the monopole energy scale.

cond-mat.str-el↗

Magnetic interactions and spin dynamics in the bond-disordered pyrochlore fluoride NaCaCo$_2$F$_7$

We report high-frequency/high-field electron spin resonance (ESR) and high-field magnetization studies on single crystals of the bond-disordered pyrochlore NaCaCo$_2$F$_7$. Frequency- and temperature-dependent ESR investigations above the freezing temperature $T_f \sim 2.4$ K reveal the coexistence of two distinct magnetic phases. A cooperative paramagnetic phase, evidenced by a gapless excitation mode, is found as well as a spin-glass phase developing below 20 K which is associated with a gapped low-energy excitation. Effective $g$-factors close to 2 are obtained for both modes in line with pulsed high-field magnetization measurements which show an unsaturated isotropic behavior up to 58 T at 2 K. In order to describe the field-dependent magnetization in high magnetic fields, we propose an empirical model accounting for highly anisotropic ionic $g$-tensors expected for this material and taking into account the strongly competing interactions between the spins which lead to a frustrated ground state. As a detailed quantitative relation between effective $g$-factors as determined from ESR and the local $g$-tensors obtained by neutron scattering [Ross et al., Phys. Rev. B 93, 014433 (2016)] is still sought after, our work motivates further theoretical investigations of the low-energy excitations in bond-disordered pyrochlores.

cond-mat.str-el↗

Anomalous Knight shift and low-energy spin dynamics in the nematic state of FeSe$_{\rm 1-x}$S$_{\rm x}$

The interplay between the nematic order and magnetism in FeSe is not yet well understood. There is a controversy concerning the relationship between orbital and spin degrees of freedom in FeSe and their relevance for superconductivity. Here we investigate the effect of S substitution on the nematic transition temperature ($T_{\rm n}$) and the low-energy spin fluctuations (SF) in FeSe single crystals. We show that the low-energy SF emerge below the nematic transition. The difference between the onset temperature for the critical SF ($T_{\rm SF}$) and $T_{\rm n}$ is small for FeSe but significantly increases with S substitution. Below $T_{\rm SF}$ the Korringa relation is violated and the effective muon hyperfine coupling constant changes a sign. Our results exclude a direct coupling of the low-energy SF to the electronic nematic order indicating a presence of multiple spin degrees of freedom in FeSe$_{\rm 1-x}$S$_{\rm x}$.

cond-mat.str-el↗

Magnetism and the phase diagram of MnSb$_2$O$_6$

Static and dynamic magnetic properties of P\={3}1$m$-phase MnSb$_2$O$_6$ have been studied by means of muon spin relaxation ($μ$SR), high-frequency electron spin resonance (HF-ESR), specific heat, and magnetisation studies in magnetic fields up to 25\,T. The data imply onset of long-range antiferromagnetic order at $T_N$ =~8~K and a spin-flop-like transition at $B_{SF}\approx 0.7 - 1$~T. Below $T_N$, muon asymmetry exhibits well-defined oscillations indicating a narrow distribution of the local fields. A competing antiferromagnetic phase appearing below $T_2$ =~5.3~K is evidenced by a step in the magnetisation and a slight kink of the relaxation rate. Above $T_N$ , both $μ$SR and HF-ESR data suggest short-range spin order. HF-ESR data show that local magnetic fields persist up to at least $12\cdot T_{\rm N}\approx 100$\,K. Analysis of the antiferromagnetic resonance modes and the thermodynamic spin-flop field suggest zero-field splitting of $Δ\approx 18$\,GHz which implies small but finite magnetic anisotropy.

cond-mat.str-el↗

Close proximity of FeSe to a magnetic quantum critical point as revealed by high-resolution $μ$SR measurements

A nematic transition preceding a long-range spin density wave antiferromagnetic phase is a common feature of many Fe based superconductors. However, in the FeSe system with a nematic transition at $T_{\rm s} \approx$ 90 K no evidence for long-range static magnetism down to very low temperature was found. The lack of magnetism is a challenge for the theoretical description of FeSe. Here, we investigated high-quality single crystals of FeSe using high-field (up to 9.5 Tesla) muon spin rotation ($μ$SR) measurements. The $μ$SR Knight shift and the bulk susceptibility linearly scale at high temperatures but deviate from this behavior around $T^{*} \sim 10$ K, where the Knight shift exhibits a kink. This behavior hints to an essential change of the electronic and/or magnetic properties crossing the region near $T^{*}$. In the temperature range $T_{\rm s} \gtrsim T \gtrsim T^{*}$ the muon spin depolarization rate follows a critical behavior $Λ\propto T^{-0.4}$. The observed non-Fermi liquid behavior with a cutoff at $T^{*}$ indicates that FeSe is in the vicinity to a antiferromagnetic quantum critical point. Our analysis is suggestive for $T^{*}$ triggered by the Lifshitz transition.

cond-mat.supr-con↗

Ferromagnetism or slow paramagnetic relaxation in Fe-doped Li$_3$N?

We report on isothermal magnetization, Mössbauer spectroscopy, and magnetostriction as well as temperature-dependent alternating-current (ac) susceptibility, specific heat, and thermal expansion of single crystalline and polycrstalline Li$_2$(Li$_{1-x}$Fe$_x$)N with $x = 0$ and $x \approx 0.30$. Magnetic hysteresis emerges at temperatures below $T \approx 50\,$K with coercivity fields of up to $μ_0H = 11.6\,$T at $T = 2\,$K and magnetic anisotropy energies of $310\,$K ($27\,$meV). The ac susceptibility is strongly frequency dependent ($f\,=\,10$--$10,000\,$Hz) and reveals an effective energy barrier for spin reversal of $ΔE \approx 1100\,$K. The relaxation times follow Arrhenius behavior for $T > 25\,$K. For $T < 10\,$K, however, the relaxation times of $τ\approx 10^{10}\,$s are only weakly temperature-dependent indicating the relevance of a quantum tunneling process instead of thermal excitations. The magnetic entropy amounts to more than $25\,$J mol$^{-1}_{\rm Fe}\,$K$^{-1}$ which significantly exceeds $R$ln2, the value expected for the entropy of a ground state doublet. Thermal expansion and magnetostriction indicate a weak magneto-elastic coupling in accordance with slow relaxation of the magnetization. The classification of Li$_2$(Li$_{1-x}$Fe$_x$)N as ferromagnet is stressed and contrasted with highly anisotropic and slowly relaxing paramagnetic behavior.

cond-mat.str-el↗

Spin-order-induced multiferroicity in LiCuFe2(VO4)3 and disorder effects in NaCuFe2(VO4)3

Mixed spin chain compounds, ACuFe2(VO4)3 (A= Li,Na), reach magnetically ordered state at TN ~ 11 K (Li) or ~ 9 K (Na) and experience further transformation of magnetic order at T* ~ 7 K (Li) or ~ 5 K (Na), evidenced in magnetic susceptibility chi and specific heat Cp measurements. While no anomaly has been detected in dielectric property of NaCuFe2(VO4)3, the step-like feature precedes a sharp peak in permittivity epsilon at TN in LiCuFe2(VO4)3. These data suggest the spin-order-induced ferroelectricity in Li compound and no such thing in Na compound. On the contrary, the Moessbauer spectroscopy study suggests similarly wide distribution of hyperfine field in between T* and TN for both the compounds. The first principles calculations also provide similar values for magnetic exchange interaction parameters in both compounds. These observations lead us to conclude on the crucial role of alkali metals mobility within the channels of the crystal structure needed to be considered in explaining the improper multiferroicity in one compound and its absence in other.

cond-mat.mtrl-sci↗

Diluted paramagnetic impurities in nonmagnetic Ba$_2$YIrO$_6$

The cubic double perovskite Ba$_2$YIrO$_6$ has been investigated by the local probe techniques nuclear magnetic resonance ($^{89}$Y NMR) and muon spin rotation (muSR). Both methods confirm the absence of magnetic long-range order in this compound but find evidence for diluted localized paramagnetic moments. NMR spin-lattice relaxation rate 1/T1 measurements suggest a slowing down of localized spin moments at low temperatures. An increase of the muSR spin-lattice relaxation rate lambda confirms the presence of weak magnetism in Ba$_2$YIrO$_6$ . However, these findings cannot be explained by the recently suggested excitonic type of magnetism. Instead, they point towards tiny amounts of localized paramagnetic spin centers leading to this magnetic response on the background of a simple nonmagnetic ground state of the 5d$^4$ ($J=0)$ electronic configuration of Ir$^{5+}$.

cond-mat.str-el↗

Spin freezing in the disordered pyrochlore magnet NaCaCo$_2$F$_7$: NMR studies and Monte-Carlo simulations

We present results of $^{23}$Na and $^{19}$F nuclear magnetic resonance (NMR) measurements on NaCaCo$_2$F$_7$, a frustrated pyrochlore magnet with a Curie-Weiss temperature, $T_{cw}$ ~-140 K, and intrinsic bond disorder. Below 3.6 K both the $^{23}$Na and $^{19}$F spectra broaden substantially in comparison to higher temperatures accompanied by a considerable reduction (80 \%) of the NMR signal intensity: This proves a broad quasi-static field distribution. The $^{19}$F spin-lattice relaxation rate $^{19}(1/T_1$) exhibits a peak at 2.9 K already starting to develop below 10 K. We attribute the spin freezing to the presence of bond disorder. This is corroborated by large-scale Monte-Carlo simulations of a classical bond-disordered XY model on the pyrochlore lattice. The low freezing temperature, together with the very short magnetic correlation length not captured by the simulations, suggesting that quantum effects play a decisive role in NaCaCo$_2$F$_7$.

cond-mat.str-el↗

Magnetic properties of the spin-1 chain compound NiCl$_3$C$_6$H$_5$CH$_2$CH$_2$NH$_3$

We report experimental results of the static magnetization, ESR and NMR spectroscopic measurements of the Ni-hybrid compound NiCl$_3$C$_6$H$_5$CH$_2$CH$_2$NH$_3$. In this material NiCl$_3$ octahedra are structurally arranged in chains along the crystallographic $a$-axis. According to the static susceptibility and ESR data Ni$^{2+}$ spins $S = 1$ are isotropic and are coupled antiferromagnetically (AFM) along the chain with the exchange constant $J = 25.5$ K. These are important prerequisites for the realization of the so-called Haldane spin-1 chain with the spin-singlet ground state and a quantum spin gap. However, experimental results evidence AFM order at $T_{\rm N} \approx 10$ K presumably due to small interchain couplings. Interestingly, frequency-, magnetic field-, and temperature-dependent ESR measurements, as well as the NMR data, reveal signatures which could presumably indicate an inhomogeneous ground state of co-existent mesoscopically spatially separated AFM ordered and spin-singlet state regions similar to the situation observed before in some spin-diluted Haldane magnets.

cond-mat.str-el↗

Macroscopic phase separation of superconductivity and ferromagnetism in Sr0.5Ce0.5FBiS2-xSex revealed by muSR

The compound Sr$_{0.5}$Ce$_{0.5}$FBiS$_{2}$ belongs to the intensively studied family of layered BiS$_2$ superconductors. It attracts special attention because superconductivity at $T_{sc} = 2.8$ K was found to coexist with local-moment ferromagnetic order with a Curie temperature $T_C = 7.5$ K. Recently it was reported that upon replacing S by Se $T_C$ drops and ferromagnetism becomes of an itinerant nature (Thakur et al., Sci. Reports 6, 37527 (2016)). At the same time $T_{sc}$ increases and it was argued superconductivity coexists with itinerant ferromagnetism. Here we report a muon spin rotation and relaxation study ($μ$SR) conducted to investigate the coexistence of superconductivity and ferromagnetic order in Sr$_{0.5}$Ce$_{0.5}$FBiS$_{2-x}$Se$_x$ with $x=0.5$ and $1.0$. By inspecting the muon asymmetry function we find that both phases do not coexist on the microscopic scale, but occupy different sample volumes. For $x=0.5$ and $x=1.0$ we find a ferromagnetic volume fraction of $\sim \, 8 \%$ and $\sim \, 30 \%$ at $T=0.25$ K, well below $T_{C} = 3.4$ K and $T_C = 3.3$ K, respectively. For $x=1.0$ ($T_{sc} = 2.9$ K) the superconducting phase occupies the remaining sample volume ($\sim \, 70 \%$), as shown by transverse field experiments that probe the Gaussian damping due to the vortex lattice. We conclude ferromagnetism and superconductivity are macroscopically phase separated.

cond-mat.supr-con↗

Magnetic order and spin dynamics in the helical magnetic system Fe$_3$PO$_4$O$_3$

The 3$d$-electronic spin dynamics and the magnetic order in Fe$_3$PO$_4$O$_3$ were investigated by muon spin rotation and relaxation ($μ$SR) and $^{57}$Fe Mössbauer spectroscopy. Zero-field (ZF)-$μ$SR and $^{57}$Fe Mössbauer studies confirm static long range magnetic ordering below $T_{\mathrm{N}}$ $\approx$ 164\,K. Both transverse-field (TF) and ZF-$μ$SR results evidence 100\% magnetic volume fraction in the ordered state. The ZF-$μ$SR time spectra can be best described by a Bessel function, which is consistent with the helical magnetic structure proposed by neutron scattering experiments. The Mössbauer spectra are described in detail by considering the specific angular distribution of the local hyperfine field $B_{\mathrm{hyp}}$ with respect to the local electric field gradient. The $μ$SR spin-lattice relaxation rate exhibits two peaks: One at the magnetic ordering temperature related to critical magnetic fluctuations and another peak at 35\,K signaling the presence of a secondary low energy scale in Fe$_3$PO$_4$O$_3$.

cond-mat.str-el↗

Superconductivity with broken time reversal symmetry in ion irradiated Ba$_{0.27}$K$_{0.73}$Fe$_2$As$_2$ single crystals

Over the last years a lot of theoretical and experimental efforts have been made to find states with broken time reversal symmetry (BTRS) in multi-band superconductors. In particular, it was theoretically proposed that in the Ba$_{1-x}$K$_{x}$Fe$_2$As$_2$ system either an $s+is$ or an $s+id$ BTRS state may exist at high doping levels in a narrow region of the phase diagram. Here we report the observation of an enhanced zero field muon spin relaxation rate below the superconducting transition temperature for a high quality crystalline sample with $x \approx$ 0.73. This indicates that indeed the time reversal symmetry is broken in superconducting Ba$_{1-x}$K$_{x}$Fe$_2$As$_2$ at this doping level.

cond-mat.supr-con↗

Fast recovery of the stripe magnetic order by Mn/Fe substitution in F-doped LaFeAsO superconductors

$^{75}$As Nuclear Magnetic (NMR) and Quadrupolar (NQR) Resonance were used, together with Mössbauer spectroscopy, to investigate the magnetic state induced by Mn for Fe substitutions in F-doped LaFe$_{1-x}$Mn$_{x}$AsO superconductors. The results show that $0.5$% of Mn doping is enough to suppress the superconducting transition temperature $T_c$ from 27 K to zero and to recover the magnetic structure observed in the parent undoped LaFeAsO. Also the tetragonal to orthorhombic transition of the parent compound is recovered by introducing Mn, as evidenced by a sharp drop of the NQR frequency. The NQR spectra also show that a charge localization process is at play in the system. Theoretical calculations using a realistic five-band model show that correlation-enhanced RKKY exchange interactions between nearby Mn ions stabilize the observed magnetic order, dominated by $Q_1=(π,0)$ and $Q_2=(0,π)$ ordering vectors. These results give compelling evidence that F-doped LaFeAsO is a strongly correlated electron system at the verge of an electronic instability.

cond-mat.supr-con↗

Magnetic order and spin dynamics across a ferromagnetic quantum critical point: $μ$SR investigations of YbNi$_4$(P$_{1-x}$As$_x$)$_2$

In the quasi-1D heavy-fermion system YbNi$_4$(P$_{1-x}$As$_x$)$_2$ the presence of a ferromagnetic (FM) quantum critical point (QCP) at $x_c$ $\approx 0.1$ with unconventional quantum critical exponents in the thermodynamic properties has been recently reported. Here, we present muon-spin relaxation ($μ$SR) experiments on polycrystals of this series to study the magnetic order and the low energy 4$f$-electronic spin dynamics across the FM QCP. The zero field $μ$SR measurements on pure YbNi$_4$(P$_{2}$ proved static long range magnetic order and suggested a strongly reduced ordered Yb moment of about 0.04$μ_B$. With increasing As substitution the ordered moment is reduced by half at $x = 0.04$ and to less than 0.005 $μ_B$ at $x=0.08$. The dynamic behavior in the $μ$SR response show that magnetism remains homogeneous upon As substitution, without evidence for disorder effect. In the paramagnetic state across the FM QCP the dynamic muon-spin relaxation rate follows 1/$T_{1}T\propto T^{-n}$ with $1.01 \pm 0.04 \leq n \leq 1.13 \pm 0.06$. The critical fluctuations are very slow and are even becoming slower when approaching the QCP.

cond-mat.str-el↗

Non-collinear antiferromagnetism of coupled spins and pseudospins in the double perovskite La2CuIrO6

We report the structural, magnetic and thermodynamic properties of the double perovskite compound La2CuIrO6 from X-ray, neutron diffraction, neutron depolarization, dc magnetization, ac susceptibility, specific heat, muon-spin-relaxation (uSR), electron-spin-resonance (ESR) and nuclear magnetic resonance (NMR) measurements. Below ~113 K, short-range spin-spin correlations occur within the Cu2+ sublattice. With decreasing temperature, the Ir4+ sublattice progressively involves in the correlation process. Below T = 74 K, the magnetic sublattices of Cu (spin s = 1/2) and Ir (pseudospin j = 1/2) in La2CuIrO6 are strongly coupled and exhibit an antiferromagnetic phase transition into a non-collinear magnetic structure accompanied by a small uncompensated transverse moment. A weak anomaly in ac-susceptibility as well as in the NMR and μSR spin lattice relaxation rates at 54 K is interpreted as a cooperative ordering of the transverse moments which is influenced by the strong spin-orbit coupled 5d ion Ir4+. We argue that the rich magnetic behaviour observed in La2CuIrO6 is related to complex magnetic interactions between the strongly correlated spin-only 3d ions with the strongly spin-orbit coupled 5d transition ions where a combination of the spin-orbit coupling and the low-symmetry of the crystal lattice plays a special role for the spin structure in the magnetically ordered state.

cond-mat.str-el↗

Coexistence of low moment magnetism and superconductivity in tetragonal FeS and suppression of $T_\mathrm{c}$ under pressure

We report local probe ($μ$SR) measurements on the recently discovered tetragonal FeS superconductor which has been predicted to be electronically very similar to superconducting FeSe. Most remarkably, we find that low moment ($10^{-2}-10^{-3}μ_\mathrm{B})$ disordered magnetism with a transition temperature of $T_\mathrm{N}\approx 20$ K microscopically coexists with bulk superconductivity below $T_\mathrm{c}=4.3(1)$ K. From transverse field $μ$SR we obtain an in-plane penetration depth $λ_\mathrm{ab}(0)=223(2)$ nm for FeS. The temperature dependence of the corresponding superfluid density $λ_\mathrm{ab}^{-2}(T)$ indicates a fully gapped superconducting state and is consistent with a two gap s-wave model. Additionally, we find that the superconducting $T_\mathrm{c}$ of FeS continuously decreases for hydrostatic pressures up to 2.2 GPa.

cond-mat.supr-con↗

Superconducting properties and pseudogap from preformed Cooper pairs in the triclinic (CaFe$_{1-x}$Pt$_x$As)$_{10}$Pt$_3$As$_8$

Using a combination of muon-spin relaxation ($μ$SR), inelastic neutron scattering (INS) and nuclear magnetic resonance (NMR), we investigated the novel iron-based superconductor with a triclinic crystal structure (CaFe$_{1-x}$Pt$_x$As)$_{10}$Pt$_3$As$_8$ (T$_{\rm c}$ = 13 K), containing platinum-arsenide intermediary layers. The temperature dependence of the superfluid density obtained from the $μ$SR relaxation-rate measurements indicates the presence of two superconducting gaps, $Δ_\text{1}\ggΔ_\text{2}$. According to our INS measurements, commensurate spin fluctuations are centered at the ($π$, 0) wave vector, like in most other iron arsenides. Their intensity remains unchanged across T$_\text{c}$, indicating the absence of a spin resonance typical for many Fe-based superconductors. Instead, we observed a peak in the spin-excitation spectrum around $\hslashω_0=\,$7 meV at the same wave vector, which persists above T$_{\rm c}$ and is characterized by the ratio $\hslashω_0/k_\text{B}T_\text{c}\approx\,$6.2, which is significantly higher than typical values for the magnetic resonant modes in iron pnictides (~4.3). The temperature dependence of magnetic intensity at 7 meV revealed an anomaly around T* = 45 K related to the disappearance of this new mode. A suppression of the spin-lattice relaxation rate, $1/T_1T$, observed by NMR immediately below T* without any notable subsequent anomaly at T$_{\rm c}$, indicates that T* could mark the onset of a pseudogap in (CaFe$_{1-x}$Pt$_x$As)$_{10}$Pt$_3$As$_8$, which is likely associated with the emergence of preformed Cooper pairs.

cond-mat.supr-con↗