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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 $\alpha$-RuCl$_3$ system. This proves that it is possible to tune the Kitaev interactions by replacing Cl with heavier halogen elements such as Br., Comment: 5 pages, 5 figures

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., Comment: 11 pages, 5 figures. This work builds on our earlier findings on LBCO, arXiv:2008.01159, and substantially expands it

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 ($\mu$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 $\mu$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., Comment: 9 pages, 8 figures

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., Comment: 14 pages, 13 figures

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., Comment: To appear in Physical Review Letters (2020)

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 $\mu$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$_2$., Comment: submission to Scipost Physics

We report a combined $^{115}$In NQR, $^{51}$V NMR and $\mu$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 N\'eel 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$_3$., Comment: 16 pages, 19 figures

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 $\mu$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) $\mu$SR studies confirm the absence of any long range magnetic order state down to 0.05K ($\sim J$/80). Current $\mu$SR results together with the so far available bulk characterization data suggest that NaYbS$_2$ is an ideal candidate to identify QSL ground state., Comment: Submitted to PRB as Rapid communication on 18th Oct19

We report muon spin rotation ($\mu$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}

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.

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 \Theta$_{CW}$ and effective magnetic moment \mu$_{eff}$ 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 $\mu$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.

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., Comment: 19 pages, 17 figures

Kitaev's honeycomb spin-liquid model and its proposed realization in materials such as $\alpha$-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., Comment: To appear in PRB as Rapid Communication

We report muon spin rotation ($\mu$SR) and magnetization measurements under pressure on Fe$_{1+\delta}$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 $\geq0.2$., Comment: 10 pages, 6 figures, including supplemental material

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$_{\rm x}$., Comment: 8 pages, 5 figures

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., Comment: 9 pages, 6 figures

In general, magnetism and superconductivity are antagonistic to each other. However, there are several families of superconductors, in which superconductivity may coexist with magnetism, and only a few examples are known, when superconductivity itself induces spontaneous magnetism. The most known compounds are Sr$_2$RuO$_4$ and some noncentrosymmetric superconductors. Here, we report the finding of a narrow dome of a novel $s+is'$ superconducting (SC) phase with broken time-reversal symmetry (BTRS) inside the broad $s$-wave SC region of the centrosymmetric multiband superconductor Ba$_{\rm 1-x}$K$_{\rm x}$Fe$_2$As$_2$ ($0.7 \lesssim x \lesssim 0.85$). We observe spontaneous magnetic fields inside this dome using the muon spin relaxation ($\mu$SR) technique. Furthermore, our detailed specific heat study reveals that the BTRS dome appears very close to a change in the topology of the Fermi surface (Lifshitz transition). With this, we experimentally demonstrate the emergence of a novel quantum state due to topological changes of the electronic system., Comment: 28 pages, 11 figures

Platelike high-quality NaYbS$_{2}$ rhombohedral single crystals with lateral dimensions of a few mm have been grown and investigated in great detail by bulk methods like magnetization and specific heat, but also by local probes like nuclear magnetic resonance (NMR), electron-spin resonance (ESR), muon-spin relaxation ($\mu$SR), and inelastic neutron scattering (INS) over a wide field and temperature range. Our single-crystal studies clearly evidence a strongly anisotropic quasi-2D magnetism and an emerging spin-orbit entangled $S=1/2$ state of Yb towards low temperatures together with an absence of long-range magnetic order down to 260~mK. In particular, the clear and narrow Yb ESR lines together with narrow $^{23}$Na NMR lines evidence an absence of inherent structural distortions in the system, which is in strong contrast to the related spin-liquid candidate YbMgGaO$_{4}$ falling within the same space group $R\overline{3}m$. This identifies NaYbS$_{2}$ as a rather pure spin-1/2 triangular lattice magnet and a new putative quantum spin liquid.

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., Comment: 6 pages, 6 figures

Static and dynamic magnetic properties of P\={3}1$m$-phase MnSb$_2$O$_6$ have been studied by means of muon spin relaxation ($\mu$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 $\mu$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 $\Delta \approx 18$\,GHz which implies small but finite magnetic anisotropy.

Magnetic frustration and disorder are key ingredients to prevent the onset of magnetic order. In the disordered hexagonal double perovskite BaTi$_{1/2}$Mn$_{1/2}$O$_{3}$, Mn$^{4+}$ cations, with $S=3/2$ spins, can either form highly correlated states of magnetic trimers or dimers or remain as weakly interacting orphan spins. At low temperature ($T$), the dimer response is negligible, and magnetism is dominated by the trimers and orphans. To explore the role of magnetic frustration, disorder and possibly of quantum fluctuations, the low-$T$ magnetic properties of the remaining magnetic degrees of freedom of BaTi$_{1/2}$Mn$_{1/2}$O$_{3}$ are investigated. Heat-capacity data and magnetic susceptibility display no evidence for a phase transition to a magnetically ordered phase but indicate the formation of a correlated spin state. The low-temperature spin dynamics of this state is then explored by $\mu$SR experiments. The zero field $\mu^{+}$ relaxation rate data show no static magnetism down to $T=19$ mK and longitudinal field experiments support as well that dynamic magnetism persists at low $T$. Our results are interpreted in terms of a spin glass state which stems from a disordered lattice of orphans spins and trimers. A spin liquid state in BaTi$_{1/2}$Mn$_{1/2}$O$_{3}$, however, is not excluded and is also discussed., Comment: Main Text: 6 pages, 4 figures; Supplemental: 11 pages, 7 figures

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 ($\mu$SR) measurements. The $\mu$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 $\Lambda \propto T^{-0.4}$. 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., Comment: 15 pages, 16 figures

We report on isothermal magnetization, M\"ossbauer 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 $\mu_0H = 11.6\,$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 $\Delta E \approx 1100\,$K. The relaxation times follow Arrhenius behavior for $T > 25\,$K. For $T < 10\,$K, however, the relaxation times of $\tau \approx 10^{10}\,$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., Comment: 12 pages, 10 figures

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., Comment: 9 pages, 5 figures

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.

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 ($\mu$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., Comment: 9 pages (includes 4 figures) + supplementary information file

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 M\"ossbauer 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.

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 ($\mu$SR) and $^{57}$Fe M\"ossbauer spectroscopy. Zero-field (ZF)-$\mu$SR and $^{57}$Fe M\"ossbauer studies confirm static long range magnetic ordering below $T_{\mathrm{N}}$ $\approx$ 164\,K. Both transverse-field (TF) and ZF-$\mu$SR results evidence 100\% magnetic volume fraction in the ordered state. The ZF-$\mu$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 M\"ossbauer 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 $\mu$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$_3$.

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$^{5+}$., Comment: 8 pages, 7 figures

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., Comment: 5 pages, 3 figures, and supplementary materials

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 ($\mu$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 $\mu$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$\mu_B$. With increasing As substitution the ordered moment is reduced by half at $x = 0.04$ and to less than 0.005 $\mu_B$ at $x=0.08$. The dynamic behavior in the $\mu$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., Comment: 6 pages, 4 figures

$^{75}$As Nuclear Magnetic (NMR) and Quadrupolar (NQR) Resonance were used, together with M\"{o}ssbauer 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 $Q_1=(\pi,0)$ and $Q_2=(0,\pi)$ ordering vectors. These results give compelling evidence that F-doped LaFeAsO is a strongly correlated electron system at the verge of an electronic instability., Comment: 5 pages, 5 figures and 4 pages of supplemental material

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 {\mu}SR 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., Comment: 15 Pages, 18 figures, To appear in PRB

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., Comment: 24 pages including supplementary information

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$_7$., Comment: 11 pages, 11 figures, Substantial changes have been made

We report local probe ($\mu$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 ($10^{-2}-10^{-3}\mu_\mathrm{B})$ 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 $\mu$SR we obtain an in-plane penetration depth $\lambda_\mathrm{ab}(0)=223(2)$ nm for FeS. The temperature dependence of the corresponding superfluid density $\lambda_\mathrm{ab}^{-2}(T)$ 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., Comment: 10 pages, 7 figures, including supplemental material

A combination of phenomenological analysis and M\"ossbauer spectroscopy experiments on the tetragonal Fe$_{1+y}$Te system indicates that the magnetic ordering transition in compounds with higher Fe-excess, $y\ge$ 0.11, is unconventional. Experimentally, a liquid-like magnetic precursor with quasi-static spin-order is found from significantly broadened M\"ossbauer spectra at temperatures above the antiferromagnetic transition. The incommensurate spin-density wave (SDW) order in Fe$_{1+y}$Te is described by a magnetic free energy that violates the weak Lifshitz condition in the Landau theory of second-order transitions. The presence of multiple Lifshitz invariants provides the mechanism to create multidimensional, twisted, and modulated solitonic phases., Comment: 5 pages, 2 figures

Using a combination of muon-spin relaxation ($\mu$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 $\mu$SR relaxation-rate measurements indicates the presence of two superconducting gaps, $\Delta_\text{1}\gg\Delta_\text{2}$. According to our INS measurements, commensurate spin fluctuations are centered at the ($\pi$, 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 $\hslash\omega_0=\,$7 meV at the same wave vector, which persists above T$_{\rm c}$ and is characterized by the ratio $\hslash\omega_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.

We report bulk superconductivity (SC) in Ca$_3$Ir$_4$Sn$_{13}$ by means of $^{119}$Sn nuclear magnetic resonance (NMR) experiments. Two classical signatures of BCS superconductivity in spin-lattice relaxation rate ($1/T_1$), namely the Hebel-Slichter coherence peak just below the $T_c$ and the exponential decay in the superconducting phase, are evident. The noticeable decrease of $^{119}$Sn Knight shift below $T_c$ indicates spin-singlet superconductivity. The temperature dependence of the spin-lattice relaxation rate ($1/T_1$) is convincingly described by the multigap isotropic superconducting gap. Present NMR experiments do not witness any sign of enhanced spin fluctuations in the normal state.

We present a detailed local probe study of the magnetic order in the oxychalcogenide La2O2Fe2OSe2 utilizing 57Fe Moessbauer, 139La NMR, and muon spin relaxation spectroscopy. This system can be regarded as an insulating reference system of the Fe arsenide and chalcogenide superconductors. From the combination of the local probe techniques we identify a non-collinear magnetic structure similar to Sr2F2Fe2OS2. The analysis of the magnetic order parameter yields an ordering temperature TN = 90.1 K and a critical exponent of beta = 0.133, which is close to the 2D Ising universality class as reported in the related oxychalcogenide family.

We report detailed $^{75}$As-NQR investigations of the locally non-centrosymmetric superconductor SrPtAs. The spin-lattice relaxation studies prove weakly coupled multi-gap superconductivity. The Hebel-Slichter peak, a hallmark of conventional superconductivity, is strongly suppressed, which points to an unconventional superconducting state. The observed behavior excludes a superconducting order parameter with line nodes and is consistent with proposed $f$-wave and chiral $d$-wave order parameters.

We provide direct experimental evidence for the identical effect of the in-plane Fe$_{1-x}$Co$_{x}$ and of the out-of-plane O$_{1-x}$F$_{x}$ chemical dilutions on the itinerant spin-density-wave (SDW) magnetic phase in CeFeAsO. Remarkably, the suppression of SDW is not sensitive at all to the different kinds of disorder introduced in the two cases. Still, it is clearly shown that the sizeable in-plane disorder induced by the Fe$_{1-x}$Co$_{x}$ substitution is highly effective in suppressing $T_{\textrm{c}}$. Differently from what is observed in CeFeAsO$_{1-x}$F$_{x}$, the ordered magnetic phase of the Ce sublattice is preserved throughout the whole phase diagram in CeFe$_{1-x}$Co$_{x}$AsO ($x \leq 0.2$). An intriguing effect is encountered, whereby the magnetic coupling among Ce$^{3+}$ ions is enhanced by the superconducting phase., Comment: 8 pages (Main text: 4 pages. Paper merged with supplemental information)

We report the structural and magnetic phase transitions of triclinic Ca10(FeAs)10(Pt3As8). High-resolution X-ray powder diffraction reveals splitting of the in-plane (a,b) lattice parameters at Ts ~ 120 K. Platinum-doping weakens the distortion and shifts the transition temperature to 80 K in Ca10(Fe1-xPt_xAs)10(Pt3As8) with x = 0.03. muSR experiments show the onset of magnetic order near Ts and a broad magnetic phase transition. No symmetry breaking is associated to the structural transition in Ca10(FeAs)10(Pt3As8) in contrast to the other parent compounds of iron arsenide superconductors., Comment: 3 pages, 5 figures

We report the magnetic and superconducting properties of locally noncentrosymmetric SrPtAs obtained by muon-spin-rotation/relaxation (muSR) measurements. Zero-field muSR reveals the occurrence of small spontaneous static magnetic fields with the onset of superconductivity. This finding suggests that the superconducting state of SrPtAs breaks time-reversal symmetry. The superfluid density as determined by transverse field muSR is nearly flat approaching T = 0 K proving the absence of extended nodes in the gap function. By symmetry, several superconducting states supporting time-reversal symmetry breaking in SrPtAs are allowed. Out of these, a dominantly d + id (chiral d-wave) order parameter is most consistent with our experimental data., Comment: Additional experimental results supporting TRS breaking have been added