Muon Spin Relaxation Research Articles

Discovery of superconductivity and electron-phonon drag in the non-centrosymmetric Weyl semimetal LaRhGe3

We present an exploration of the effect of electron-phonon coupling and broken inversion symmetry on the electronic and thermal properties of the semimetal LaRhGe3. Our transport measurements reveal evidence for electron-hole compensation at low temperatures, resulting in a large magnetoresistance of 3000% at 1.8 K and 14 T. The carrier concentration is on the order of 1021/cm3 with high carrier mobilities of 2000 cm2/Vs. When coupled to our theoretical demonstration of symmetry-protected almost movable Weyl nodal lines, we conclude that LaRhGe3 supports a Weyl semimetallic state. We discover superconductivity in this compound with a Tc of 0.39(1) K and Bc(0) of 2.2(1) mT, with evidence from specific heat and transverse-field muon spin relaxation. We find an exponential dependence in the normal state electrical resistivity below ~50 K, while Seebeck coefficient and thermal conductivity measurements each reveal a prominent peak at low temperatures, indicative of strong electron-phonon interactions. To this end, we examine the temperature-dependent Raman spectra of LaRhGe3 and find that the lifetime of the lowest energy A1 phonon is dominated by phonon-electron scattering instead of anharmonic decay. We conclude that LaRhGe3 has strong electron-phonon coupling in the normal state, while the superconductivity emerges from weak electron-phonon coupling. These results open up the investigation of electron-phonon interactions in the normal state of superconducting non-centrosymmetric Weyl semimetals.

Unusual spin dynamics in the van der Waals antiferromagnet FeGa2S4

Spin dynamics in the van der Waals antiferromagnet FeGa2S4with triangular lattices are investigated using magnetometry, neutron scattering, and muon spin relaxation measurements. The characteristic spin relaxation time is thoroughly clarified over thirteen orders of magnitude. Although the temperature dependence of DC and AC susceptibilities recalls a conventional spin-glass transition, nonlinear susceptibilities showing no divergences at the anomalous temperature,T∗=16.87(7) K, deny that and instead hint at other mechanisms. Elastic neutron scattering together with previously measured muon results depict a slowly fluctuated (∼10-5 s) spin state aboveT∗. In juxtaposing the underlying simplest structure among frustrated magnets with an intricate hierarchy of time scales, FeGa2S4can be a playground for studying temporal spin correlations in the two-dimensional limit.

Tuning the spin dynamics and magnetic phase transitions of the Cantor alloy via composition and sample processing protocols: A muon spin relaxation study

Tuning the spin dynamics and magnetic phase transitions of the Cantor alloy via composition and sample processing protocols: A muon spin relaxation study

Depth-dependent study of time-reversal symmetry-breaking in the kagome superconductor AV3Sb5

The breaking of time-reversal symmetry (TRS) in the normal state of kagome superconductors AV3Sb5 stands out as a significant feature, but its tunability is unexplored. Using low-energy muon spin rotation and local field numerical analysis, we study TRS breaking as a function of depth in single crystals of RbV3Sb5 (with charge order) and Cs(V0.86Ta0.14)3Sb5 (without charge order). In the bulk of RbV3Sb5 (>33 nm from the surface), we observed an increase in the internal magnetic field width in the charge-ordered state. Near the surface (<33 nm), the muon spin relaxation rate is significantly enhanced and this effect commences at temperatures significantly higher than the onset of charge order. In contrast, no similar field width enhancement was detected in Cs(V0.86Ta0.14)3Sb5, either in the bulk or near the surface. These observations indicate a strong connection between charge order and TRS breaking and suggest that TRS breaking can occur prior to long-range charge order.

Muon spin relaxation study of spin dynamics on a Kitaev honeycomb material H3LiIr2O6

The vacancy effect in quantum spin liquid (QSL) has been extensively studied. A finite density of random vacancies in the Kitaev model can lead to a pileup of low-energy density of states (DOS), which is generally experimentally determined by a scaling behavior of thermodynamic or magnetization quantities. Here, we report detailed muon spin relaxation (μSR) results of H3LiIr2O6, a Kitaev QSL candidate with vacancies. The absence of magnetic order is confirmed down to 80 mK, and the spin fluctuations are found to be persistent at low temperatures. Intriguingly, the time-field scaling law of longitudinal-field (LF)-μSR polarization is observed down to 0.1 K. This indicates a dynamical scaling, whose critical exponent of 0.46 is excellently consistent with the scaling behavior of specific heat and magnetization data. All the observations point to the finite DOS with the form N(E)∼E−ν\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$N(E)\\sim {E}^{-\ u }$$\\end{document}, which is expected for the Kitaev QSL in the presence of vacancies. Our μSR study provides a dynamical fingerprint of the power-law low-energy DOS and introduces a crucial new insight into the vacancy effect in QSL.

Planar XY magnetic glass state in the Gd2ScNbO7 pyrochlore

Here a spin glass system with emergent planar ordered spin clusters is investigated. The mixed B-site pyrochlore Gd2ScNbO7has been synthesized and characterized through a variety of techniques, including x-ray diffraction, magnetic susceptibility, muon spin relaxation, heat capacity and neutron scattering. Despite a Curie-Weiss temperature of -3.93(3) K, indicating net antiferromagnetic interactions, no signs of long ranged magnetic ordering are found down toT= 0.3 K. Instead, a disordered magnetic state emerges with a small correlation length of 2.1(1) Å of single tetrahedra. A Reverse Monte Carlo analysis of the polarized neutron scattering data reveals short-range antiferromagnetic order with emergent XY spin ordering similar to the parent pyrochlore compounds. Muon spin relaxation, and AC susceptibility measurements confirm that the magnetization condenses into a glass, with 10 % of the potential entropy missing in the specific heat. This magnetic ground state is similar to what is observed in Gd2Sn2O7just above the ordering temperature, without the eventual long-range ordering at low temperature.

Magnetic ordering in the frustrated pyrochlore Yb2Ru2O7

Yb2Ru2O7 was studied using neutron diffraction and muon spin relaxation measurements to investigate the effect of the Yb anisotropy and Yb-Ru exchange interaction on the magnetic ordering transitions in this material. The Ru moments order into a long range ordered state below 85 K, while the Yb moments start to freeze/order below 20 K, which is at a higher temperature as suggested by previous reported bulk measurements. No structural distortions are observed at the magnetic transitions. Representational analysis shows that the ordering of the Ru and Yb moments can be described by the same irreducible representation. The two magnetic sublattices are, however, antiferromagnetically coupled. Unlike what has been suggested by bulk measurements and has been observed in other members of this family of Ru pyrochlores, the Yb single ion planar anisotropy, surprisingly, does not influence the Ru moment ordering. The ordering of the Ru moments, on the other hand, does influence freezing/ordering of the Yb moments.

Weyl fermion excitations in the ideal Weyl semimetal CuTlSe2

An ideal Weyl semimetal is characterized by a dispersion in which only Weyl cones intersect the Fermi level, with low-energy behavior being governed by Weyl fermions. Although ideal Weyl semimetals have long been anticipated, only a few are realized in nonmagnetic materials. In this study, we confirm the presence of Weyl-fermion excitations in the ideal Weyl semimetal CuTlSe2 via a combination of magnetoresistance, Hall-effect, magnetic-susceptibility, nuclear magnetic resonance (NMR), and muon-spin relaxation (µSR) experiments. Magnetoresistance measurements reveal a negative longitudinal magnetoresistance (LMR), which scales as B2, while Hall-effect results indicate a predominant contribution from Weyl fermions with a hole-type charge. Magnetic susceptibility and µSR measurements indicate the lack of any intrinsic spontaneous magnetic moments down to base temperature. Finally, the NMR results can be modeled by a two-component effective Hamiltonian, which reproduces well the temperature-dependent Cu63 NMR (T1T)−1 factor, shown to scale as T2 below 100 K and as T1 above 100 K. Overall, we find that the extremely low concentration (1017cm−3) of carriers in CuTlSe2 originates from an ideal nonmagnetic Weyl semimetallic state, persisting up to a thermal excitation energy of 9 meV (100 K), above which trivial electronic bands close to EF take over. Our findings highlight CuTlSe2 as a new member of the intriguing class of Weyl semimetals. Published by the American Physical Society 2024

Spin order and dynamics in the topological rare-earth germanide semimetals

The REAl(Si,Ge) (RE = rare earth) family, known to break both the inversion- and time-reversal symmetries, represents one of the most suitable platforms for investigating the interplay between correlated-electron phenomena and topologically nontrivial bands. Here, we report on systematic magnetic, transport, and muon-spin rotation and relaxation (uSR) measurements on (Nd,Sm)AlGe single crystals, which exhibit antiferromagnetic (AFM) transitions at TN = 6.1 and 5.9 K, respectively. In addition, NdAlGe undergoes also an incommensurate-to-commensurate ferrimagnetic transition at 4.5 K. Weak transverse-field µSR measurements confirm the AFM transitions, featuring a ∼90% magnetic volume fraction. Zero-field (ZF) µSR measurements reveal a more disordered internal field distribution in NdAlGe than in SmAlGe, reflected in a larger transverse muon-spin relaxation rate λT at T ≪ TN. This may be due to the complex magnetic structure of NdAlGe, which undergoes a series of metamagnetic transitions in an external magnetic field, while SmAlGe shows only a robust AFM order. In NdAlGe, the topological Hall effect (THE) appears between the first and the second metamagnetic transitions for H ∥ c, while it is absent in SmAlGe. Such THE in NdAlGe is most likely attributed to the field-induced topological spin textures. The longitudinal muon-spin relaxation rate λL, diverges near the AFM order, followed by a clear drop at T < TN. In the magnetically ordered state, spin fluctuations are significantly stronger in NdAlGe than in SmAlGe. In general, our longitudinal-field μSR data indicate vigorous spin fluctuations in NdAlGe, thus providing valuable insights into the origin of THE and of the possible topological spin textures in REAl(Si,Ge) Weyl semimetals.

Tc and the elastocaloric effect of Sr2RuO4 under 〈110〉 uniaxial stress: No indications of transition splitting

There is considerable evidence that the superconductivity of Sr2RuO4 has two components. Among this evidence is a jump in the shear elastic modulus c66 at the critical temperature Tc, observed in ultrasound measurements. Such a jump is forbidden for homogeneous single-component order parameters, and it implies that Tc should develop as a cusp under the application of shear strain with 〈110〉 principal axes. This shear strain should split the onset temperatures of the two components, if they coexist, or select one component if they do not. Here, we report measurements of Tc and the elastocaloric effect of Sr2RuO4 under uniaxial stress applied along the [110] lattice direction. Within experimental resolution, we resolve neither a cusp in the stress dependence of Tc, nor any second transition in the elastocaloric effect data. We show that reconciling these null results with the observed jumps in c66 requires extraordinarily fine tuning to a triple point of the Ginzburg-Landau parameter space. In addition, our results are inconsistent with homogeneous time-reversal symmetry breaking at a temperature T2≤Tc as identified in muon spin relaxation experiments. Published by the American Physical Society 2024

Static magnetic order with strong quantum fluctuations in spin-1/2 honeycomb magnet Na2Co2TeO6

Kitaev interactions, arising from the interplay of frustration and bond anisotropy, can lead to strong quantum fluctuations and, in an ideal case, to a quantum-spin-liquid state. However, in many nonideal materials, spurious non-Kitaev interactions typically promote a zigzag antiferromagnetic order in the d-orbital transition-metal compounds. Here, by combining neutron scattering with muon-spin rotation and relaxation techniques, we provide mechanism insights into the exotic properties of Na2Co2TeO6, a candidate material of the Kitaev model. Below TN, the zero-field muon-spin relaxation rate becomes almost constant (~0.45 μs−1). We attribute this temperature-independent relaxation rate to the strong quantum fluctuations, as well as to the frustrated Kitaev interactions. As the magnetic field increases, neutron scattering data indicate a broader spin-wave excitation at the K-point. Therefore, quantum fluctuations seem not only robust but are even enhanced by the applied magnetic field. Our findings provide valuable hints for understanding the onset of the quantum-spin-liquid state in Kitaev materials.

Magnetic skin effect in Pb(Fe _{1/2}$ Nb _{1/2}$ )O3

Relaxor-ferroelectrics display exceptional dielectric properties resulting from the underlying random dipolar fields induced by strong chemical inhomogeneity. An unusual structural aspect of relaxors is a skin-effect where the near-surface region in single crystals exhibit structures and critical phenomena that differ from the bulk. Relaxors are unique in that this skin effect extends over a macroscopic lengthscale of ∼100 μm whereas usual surface layers only extend over a few unit cells (or ∼nm). We present a muon spectroscopy study of Pb(Fe _{1/2} Nb _{1/2} )O3 (PFN) which displays ferroelectric order, including many relaxor-like dielectric properties such as a frequency broadened dielectric response, and antiferromagnetism with spatially short-range polar correlations and hence can be termed a multiferroic. In terms of the magnetic behavior determined by the Fe3+ ( S=5/2 , L ≈ 0) ions, PFN has been characterized as a unique example of a ‘cluster spin-glass’. We use variable momentum muon spectroscopy to study the depth dependence of the slow magnetic relaxations in a large 1 cm3 crystal of PFN. Zero-field positive muon spin relaxation is parameterized using a stretched exponential, indicative of a distribution of relaxation rates of the Fe3+ spins. This bandwidth of frequencies changes as a function of muon momentum, indicative of a change in the Fe3+ relaxation rates as a function of muon implantation depth in our single crystal. Using negative muon elemental analysis, we find small-to-no measurable change in the Fe3+/Nb5+ concentration with depth implying that chemical concentration alone cannot account for the change in the relaxational dynamics. PFN displays an analogous magnetic skin effect reported to exist in the structural properties of relaxor-ferroelectrics.

Slow polymer dynamics in poly(3-hexylthiophene) probed by muon spin relaxation

Slow polymer dynamics in poly(3-hexylthiophene) probed by muon spin relaxation

Disordered magnetic ground state in a quasi-1-D d4columnar iridate Sr3LiIrO6.

Spin-orbit coupling (SOC) offers a large variety of novel and extraordinary magnetic and electronic properties in otherwise 'ordinary pool' of heavy ion oxides. Here we present a detailed study on an apparently isolated hexagonal 2Hspin-chain d4iridate Sr3LiIrO6(SLIO) with geometric frustration. Our structural studies reveal Li-Ir chemical order with desired stoichiometry in this compound, while x-ray absorption together with x-ray photoemission spectroscopic characterizations establish pure 5+ valence of Ir. We have established a magnetic ground state with finite Ir5+magnetic moments in this compound, contrary to the anticipated nonmagnetic Jeff= 0 state, through combined dc susceptibility,7Li nuclear magnetic resonance (NMR), muon spin relaxation (μSR) and ab-initio electronic structure studies. These investigations together with ac magnetic susceptibility and specific heat measurements reveal that despite having noticeable antiferromagnetic correlation among the Ir5+local moments, this system does not magnetically order down to at least 0.05 K, possibly due to geometrical exchange frustration, arising from the comparable nearest- and next-nearest-neighbor interchain Ir-O-O-Ir superexchange interaction strengths with opposite signs. However, the zero-field (ZF) μSR analysis shows emergence of a considerable proportion of spin-freezing on top of a spin-fluctuating dynamic magnetic background down to the lowest measured&#xD;temperature of 1.7 K, possibly due to some inhomogeneity and/or the much stronger intra-column Ir-Ir magnetic exchange interaction&#xD;strength relative to the inter-column Ir-Ir ones. The linear temperature dependence of the magnetic specific heat (Cm) in both zero and applied magnetic fields, plus the power-law behavior of the NMR spin-lattice relaxation rate suggest a gapless spinon density of states in this charge gapped disordered magnetic ground state of Sr3LiIrO6.

Gapless dynamic magnetic ground state in the charge-gapped trimer iridate Ba4NbIr3O12

We present an experimental investigation of the magnetic ground state in Ba4NbIr3O12, a fractional valent trimer iridate. X-ray absorption and photoemission spectroscopy show that the Ir valence lies between 3+ and 4+ while Nb is pentavalent. Combined dc/ac magnetization, specific heat, and muon spin rotation/relaxation (µSR) measurements reveal no magnetic phase transition down to 0.05 K. Despite a significant Weiss temperature (ΘW∼−15 to −25 K) indicating antiferromagnetic correlations, a quantum spin-liquid (QSL) phase emerges and persists down to 0.1 K. This state likely arises from geometric frustration in the edge-sharing equilateral triangle Ir network. Our µSR analysis reveals a two-component depolarization, arising from the coexistence of rapidly (90%) and slowly (10%) fluctuating Ir moments. Powder x-ray diffraction and Ir-L3edge x-ray absorption fine structure spectroscopy identify 8–10% Nb/Ir site-exchange, reducing frustration within part of the Ir network, and likely leading to the faster muon spin relaxation, while the structurally ordered Ir ions remain highly geometrically frustrated, giving rise to the rapidly spin-fluctuating QSL ground state. At low temperatures, the magnetic specific heat varies as γT+αT2, indicating gapless spinon excitations, and possible Dirac QSL features with linear spinon dispersion, respectively. Published by the American Physical Society 2024

Evidence of Spin Density Waves in La_{3}Ni_{2}O_{7-δ}.

The recently discovered superconductivity with critical temperature T_{c} up to 80K in the double-layer Nickelate La_{3}Ni_{2}O_{7-δ} under pressure has drawn great attention. Here, we report the positive muon spin relaxation (μ^{+}SR) study of polycrystalline La_{3}Ni_{2}O_{6.92} under ambient pressure. Zero-field μ^{+}SR experiments reveal the existence of magnetic order in La_{3}Ni_{2}O_{6.92} with T_{N}=154 K. The weak transverse field μ^{+}SR measurements reveal the bulk nature of magnetism. In addition, a small quantity of oxygen deficiencies can greatly broaden the internal magnetic field distribution sensed by muons.

Random singlet-like state in the dimer-based triangular antiferromagnet Ba6Y2Rh2Ti2O17−δ

We present the magnetic, thermodynamic, and muon spin relaxation (μSR) results of the dimer-based triangular antiferromagnet Ba6Y2Rh2Ti2O17−δ. The magnetic susceptibility data show the sub-Curie-Weiss behavior χ(T)∝T−αχ below 100 K, suggesting random magnetism. The isothermal magnetization results reveal the presence of weakly interacting structural orphan spins about 6.1% at 2 K, arising from the oxygen deficiency. The comprehensive μSR experiments exhibit the coexisting relaxing and nonrelaxing components along with the thermally activated behavior in the muon spin relaxation rate, reflecting the fluctuating orphan spins in the dimer singlet background. In addition, we observe the scaling behavior of M(H,T) in H/T and Pz(t) in t/HLF with the scaling exponents αχ=αM=0.75 and αμ=0.72, respectively, but not for the magnetic specific heat data. The failure of the scaling relation in Cm(H,T)/T implies low-energy excitations dressed by the conventional orphan spins. Based on these observations, we find that the magnetic ground state resembles random singlets and discuss the possible configurations of the spin dimer unit Rh2O9. Our results shed light on the role of quenched disorder in the dimer-based frustrated magnets. Published by the American Physical Society 2024

Muon spin relaxation and emergence of disorder-induced unconventional dynamic magnetic fluctuations in Dy2Zr2O7

The disordered pyrochlore oxide Dy2Zr2O7 shows the signatures of field-induced spin freezing with remnant zero-point spin-ice entropy at 5 kOe magnetic field. We have performed zero-field and longitudinal field Muon spin relaxation (µSR) studies on Dy2Zr2O7. Our zero field studies reveal the absence of both long-range ordering and spin freezing down to 62 mK. The µSR relaxation rate exhibits a temperature-independent plateau below 4 K, indicating a dynamic ground state of fluctuating spins similar to the well-known spin ice system Dy2Ti2O7. The low-temperature spin fluctuations persist in the longitudinal field of 20 kOe as well and show unusual field dependence of the relaxation rate, which is uncommon for a spin-liquid system. Our results, combined with the previous studies do not show any evidence of spin ice or spin glass ground state, rather point to a disorder-induced dynamic magnetic ground state in the Dy2Zr2O7 material.

Development and application of a three-dimensional pseudo-Voigt function for muon spin relaxation analysis of weakly magnetic materials.

We present a three-dimensional pseudo-Voigt function to analyze muon spin relaxation (μSR) in weakly magnetic materials. Our approach approximates the Voigt function by superimposing Gaussian and Lorentzian functions using a one-dimensional method proposed by Di Rocco and Cruzado [Acta Phys. Pol., A 122, 666 (2012)]. We derive the peak of the Voigt function analytically and express the Half Width at Half Maximum (HWHM) of the Voigt function as a function of the HWHMs of the Gaussian and Lorentzian functions. We compare the pseudo-Voigt function to the exact Voigt function and find a maximum normalized discrepancy of ∼20% at the tail of the distribution function, depending on the ratio of Lorentzian to Gaussian HWHMs and internal magnetic field. We apply the derived three-dimensional pseudo-Voigt function to calculate μSR functions for zero- and longitudinal-field experiments and use them to fit μSR time spectra of La2-xSrxCuO4 with 2.4% Sr, employing a strong collision model with the static-based pseudo-Voigt muon spin relaxation function as the initial condition. Our results show that the Gaussian- and Lorentzian-fitted parameters and fluctuation rate are in good agreement with results from the exact Voigt function for a temperature range of 30-200K, with the deviation of Gaussian and Lorentzian width parameters reaching ∼0.15G below 30K.

Frustration-induced quantum criticality in Ni-doped CePdAl as revealed by the µSR technique

In CePdAl, the 4f moments of cerium arrange to form a geometrically frustrated kagome lattice. Due to frustration, in addition to Kondo and Ruderman-Kittel-Kasuya-Yosida interactions, this metallic system shows a long-range magnetic order (LRO) with a TN of only 2.7 K. Upon Ni doping at the Pd sites, TN is further suppressed, to reach zero at a critical concentration xc≈0.15. Here, by using muon-spin relaxation and rotation (µSR), we investigate CePd1−xNixAl at a local level for five different Ni concentrations, both above and below xc. Like the parent CePdAl compound, for x=0.05, we observe an incommensurate LRO, which turns into a quasistatic magnetic order for x=0.1 and 0.14. More interestingly, away from xc, for x=0.16 and 0.18, we still observe a non-Fermi-liquid (NFL) regime, evidenced by a power-law divergence of the longitudinal relaxation at low temperatures. In this case, longitudinal field measurements exhibit a time-field scaling, indicative of cooperative spin dynamics that persists for x&gt;xc. Furthermore, like the externally applied pressure, the chemical pressure induced by Ni doping suppresses the region below T*, characterized by a spin-liquid-like dynamical behavior. Our results suggest that the magnetic properties of CePdAl are similarly affected by the hydrostatic and the chemical pressure. We also confirm that the unusual NFL regime (compared with conventional quantum critical systems) is due to the presence of frustration that persists up to the highest Ni concentrations. Published by the American Physical Society 2024