Muon Spin Rotation Research Articles

Muon spin force

Current discrepancy between the measurement and the prediction of the muon anomalous magnetic moment can be resolved in the presence of a long-range force created by ordinary atoms acting on the muon spin via axial-vector and/or pseudoscalar coupling, and requiring a tiny O(10−13 eV) spin energy splitting between muon state polarized in the vertical direction. We suggest that an extension of the muon spin resonance (μSR) experiments can provide a definitive test of this class of models. We also derive indirect constraints on the strength of the muon spin force by considering the muon-loop-induced interactions between nuclear spin and external directions. The limits on the muon spin force extracted from the comparison of Hg199/Hg201 and Xe129/Xe131 spin precession are strong for the pseudoscalar coupling but are significantly relaxed for the axial-vector one. These limits suffer from significant model uncertainties, poorly known proton/neutron spin content of these nuclei, and therefore do not exclude the possibility of a muon spin force relevant for the muon g−2. Published by the American Physical Society 2024

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.

Microscopic probing of the superconducting and normal state properties of Ta2V3.1Si0.9 by muon spin rotation

The two-dimensional kagome lattice is an experimental playground for novel physical phenomena, from frustrated magnetism and topological matter to chiral charge order and unconventional superconductivity. A newly identified kagome superconductor, Ta2V3.1Si0.9 has recently gained attention for possessing a record high critical temperature, TC = 7.5 K for kagome metals at ambient pressure. In this study we conducted a series of muon spin rotation measurements to delve deeper into understanding the superconducting and normal state properties of Ta2V3.1Si0.9. We demonstrate that Ta2V3.1Si0.9 is a bulk superconductor with either a s+s-wave or anisotropic s-wave gap symmetry, and has an unusual paramagnetic shift in response to external magnetic fields in the superconducting state. Additionally, we observe an exceptionally low superfluid density − a distinctive characteristic of unconventional superconductivity − which remarkably is comparable to the superfluid density found in hole-doped cuprates. In its normal state, Ta2V3.1Si0.9 exhibits a significant increase in the zero-field muon spin depolarisation rate, starting at approximately 150 K, which has been observed in other kagome-lattice superconductors, and therefore hints at possible hidden magnetism. These findings characterise Ta2V3.1Si0.9 as an unconventional superconductor and a noteworthy new member of the vanadium-based kagome material family.

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.

Evidence for time-reversal symmetry-breaking kagome superconductivity.

Superconductivity and magnetism are often antagonistic in quantum matter, although their intertwining has long been considered in frustrated-lattice systems. Here we utilize scanning tunnelling microscopy and muon spin resonance to demonstrate time-reversal symmetry-breaking superconductivity in kagome metal Cs(V, Ta)3Sb5, where the Cooper pairing exhibits magnetism and is modulated by it. In the magnetic channel, we observe spontaneous internal magnetism in a fully gapped superconducting state. Under the perturbation of inverse magnetic fields, we detect a time-reversal asymmetrical interference of Bogoliubov quasi-particles at a circular vector. At this vector, the pairing gap spontaneously modulates, which is distinct from pair density waves occurring at a point vector and consistent with the theoretical proposal of an unusual interference effect under time-reversal symmetry breaking. The correlation between internal magnetism, Bogoliubov quasi-particles and pairing modulation provides a chain of experimental indications for time-reversal symmetry-breaking kagome superconductivity.

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.

Muonium state exchange dynamics in n -type GaAs

Muonium (Mu), a pseudoisotope of hydrogen with a positively charged muon in place of the proton, takes the form Mu+,0,− (like isolated hydrogen, i.e., H+,0,−) in semiconductors. The specifics of the charge state depend on the local electronic environment of the host. After initial muon implantation, generated Mu centers interact with free charge carriers and electronic spins, transition between sites, and form a dynamic network of state exchange. We identified the model of Mu dynamics in n-type GaAs using the density matrix simulation method and photoexcited muon spin spectroscopy technique. Fitting to the dark and illuminated μSR data provided transition rates between Mu states, revealing the underlying mechanisms at play between the Mu centers (cf. isolated H) and the host. Deduced capture/scattering cross sections of the Mu states reflected the microscopic dynamics of Mu. Illumination studies enabled us to measure interactions between Mu and minority carriers, which would be unavailable in dark measurements without heating. The methodology developed in this study may be applied to other semiconductor systems for a deeper understanding of the Mu state exchange dynamics. Published by the American Physical Society 2024

Emergence of Interfacial Magnetism in Strongly-Correlated Nickelate-Titanate Superlattices.

Strongly-correlated transition-metal oxides are widely known for their various exotic phenomena. This is exemplified by rare-earth nickelates such as LaNiO3, which possess intimate interconnections between their electronic, spin, and lattice degrees of freedom. Their properties can be further enhanced by pairing them in hybrid heterostructures, which can lead to hidden phases and emergent phenomena. An important example is the LaNiO3/LaTiO3 superlattice, where an interlayer electron transfer has been observed from LaTiO3 into LaNiO3 leading to a high-spin state. However, macroscopic emergence of magnetic order associated with this high-spin state has so far not been observed. Here, by using muon spin rotation, x-ray absorption, and resonant inelastic x-ray scattering, direct evidence of an emergent antiferromagnetic order with high magnon energy and exchange interactions at the LaNiO3/LaTiO3 interface is presented. As the magnetism is purely interfacial, a single LaNiO3/LaTiO3 interface can essentially behave as an atomically thin strongly-correlated quasi-2D antiferromagnet, potentially allowing its technological utilization in advanced spintronic devices. Furthermore, its strong quasi-2D magnetic correlations, orbitally-polarized planar ligand holes, and layered superlattice design make its electronic, magnetic, and lattice configurations resemble the precursor states of superconducting cuprates and nickelates, but with an S→1 spin state instead.

Investigation of the solar cell materials Cu(In,Ga)Se2 and Cu2ZnSnS4 with muon spin spectroscopy and density-functional calculations

Investigation of the solar cell materials Cu(In,Ga)Se2 and Cu2ZnSnS4 with muon spin spectroscopy and density-functional calculations

Ubiquitous Order-Disorder Transition in the Mn Antisite Sublattice of the (MnBi2Te4)(Bi2Te3)n Magnetic Topological Insulators.

Magnetic topological insulators (TIs) herald a wealth of applications in spin-based technologies, relying on the novel quantum phenomena provided by their topological properties. Particularly promising is the (MnBi2Te4)(Bi2Te3)n layered family of established intrinsic magnetic TIs that can flexibly realize various magnetic orders and topological states. High tunability of this material platform is enabled by manganese-pnictogen intermixing, whose amounts and distribution patterns are controlled by synthetic conditions. Here, nuclear magnetic resonance and muon spin spectroscopy, sensitive local probe techniques, are employed to scrutinize the impact of the intermixing on the magnetic properties of (MnBi2Te4)(Bi2Te3)nand MnSb2Te4. The measurements not only confirm the opposite alignment between the Mn magnetic moments on native sites and antisites in the ground state of MnSb2Te4, but for the first time directly show the same alignment in (MnBi2Te4)(Bi2Te3)n with n = 0, 1 and 2. Moreover, for all compounds, the static magnetic moment of the Mn antisite sublattice is found to disappear well below the intrinsic magnetic transition temperature, leaving a homogeneous magnetic structure undisturbed by the intermixing. The findings provide a microscopic understanding of the crucial role played by Mn-Bi intermixing in (MnBi2Te4)(Bi2Te3)n and offer pathways to optimizing the magnetic gap in its surfacestates.

Local Environment and Migration Paths of the Proton Defect in Yttria-Stabilized Zirconia Studied by Ab Initio Calculations and Muon-Spin Spectroscopy

The local binding and migration behavior of the proton defect in cubic yttria-stabilized zirconia (YSZ) is studied by first-principles calculations and muon-spin spectroscopy (μSR) measurements. The calculations are based on density-functional theory (DFT) supplemented with a hybrid-functional approach with the proton defect embedded in quasi-random supercells of 10.3 mol% yttria content, where the yttrium–zirconium substitutional defects are charge compensated by oxygen vacancies. Representative migration pathways for the proton comprising both transfer and bond reorientation modes are analysed and linked to the underlying microstructure of the YSZ lattice. The μSR data show the evolution of the diamagnetic fraction corresponding to the muon-isotope analogue with an activation energy of diffusion equal to 0.17 eV. Comparisons between the calculations and the experiment allow an assessment of the character of the short-range migration of the proton particle in cubic YSZ.

Observation of Mermin-Wagner behavior in LaFeO3/SrTiO3 superlattices

Two-dimensional magnetic materials can exhibit new magnetic properties due to the enhanced spin fluctuations that arise in reduced dimension. However, the suppression of the long-range magnetic order in two dimensions due to long-wavelength spin fluctuations, as suggested by the Mermin-Wagner theorem, has been questioned for finite-size laboratory samples. Here we study the magnetic properties of a dimensional crossover in superlattices composed of the antiferromagnetic LaFeO3 and SrTiO3 that, thanks to their large lateral size, allowed examination using a sensitive magnetic probe — muon spin rotation spectroscopy. We show that the iron electronic moments in superlattices with 3 and 2 monolayers of LaFeO3 exhibit a static antiferromagnetic order. In contrast, in the superlattices with single LaFeO3 monolayer, the moments do not order and fluctuate to the lowest measured temperature as expected from the Mermin-Wagner theorem. Our work shows how dimensionality can be used to tune the magnetic properties of ultrathin films.

Analysis of Avoided Level Crossing Muon Spin Resonance Spectra of Muoniated Radicals in Anisotropic Environments: Estimation of Muon Dipolar Hyperfine Parameters for Lorentzian-like Δ1 Resonances

Avoided level crossing muon spin resonance (ALC-μSR) is used to characterize muoniated free radicals. These radicals are used as probes of the local environment and reorientational motion of specific components in complex systems. The parameter that provides information about the anisotropic motion is the motionally-averaged muon dipolar-hyperfine coupling constant (Dμ‖). The ALC-μSR spectra of muoniated radicals in anisotropic environments frequently have Lorentzian-like Δ1 resonances, which makes it challenging to extract Dμ‖. In this paper, we derive a means to estimate|Dμ‖| from ALC-μSR spectra with Lorentzian-like resonances by measuring the amplitude, width, and position of the Δ1 resonance and the amplitude, width, and position of a Δ0 resonance. Numerical simulations were used to test this relationship for radicals with a wide range of muon and proton hyperfine parameters. We use this methodology to determine |Dμ‖| for the Mu adducts of the cosurfactant 2-phenylethanol in C12E4 bilayers. From this we determined the amplitude of the anisotropic reorientational motion of the cosurfactant.

Improving the beam quality of the low-energy muon beamline at Paul Scherrer Institute: Characterization of ultrathin carbon foils

The low-energy muon (LEM) beamline at the Paul Scherrer Institute currently stands as the world’s only facility providing a continuous beam of low-energy muons with keV energies for conducting muon spin rotation experiments on a nanometer depth scale in heterostructures and near a sample’s surface. As such, optimizing the beam quality to reach its full potential is of paramount importance. One of the ongoing efforts is dedicated to improving the already applied technique of single muon tagging through the detection of secondary electrons emerging from an ultrathin carbon foil. In this work, we present the results from installing a thinner foil with a nominal thickness of 0.5 μg cm−2 and compare its performance to that of the previously installed foil with a nominal thickness of 2.0 μg cm−2. Our findings indicate improved beam quality, characterized by smaller beam spots, reduced energy loss and straggling of the muons, and enhanced tagging efficiency. Additionally, we introduce a method utilizing blue laser irradiation for cleaning the carbon foil, further improving and maintaining its characteristics. Published by the American Physical Society 2024

Magnetism in the axion insulator candidate Eu5In2Sb6

Eu5In2Sb6 is a member of a family of orthorhombic nonsymmorphic rare-earth intermetallics that combines large localized magnetic moments and itinerant exchange with a low carrier density and perpendicular glide planes. This may result in special topological crystalline (wallpaper fermion) or axion insulating phases. Recent studies of Eu5In2Sb6 single crystals have revealed colossal negative magnetoresistance and multiple magnetic phase transitions. Here, we clarify this ordering process using neutron scattering, resonant elastic x-ray scattering, muon spin-rotation, and magnetometry. The nonsymmorphic and multisite character of Eu5In2Sb6 results in coplanar noncollinear magnetic structures with an Ising-like net magnetization along the a axis. A reordering transition, attributable to competing ferro- and antiferromagnetic couplings, manifests as the onset of a second commensurate Fourier component. In the absence of spatially resolved probes, the experimental evidence for this low-temperature state can be interpreted either as an unusual double-q structure or in a phase separation scenario. The net magnetization produces variable anisotropic hysteretic effects which also couple to charge transport. The implied potential for functional domain physics and topological transport suggests that this structural family may be a promising platform to implement concepts of topological antiferromagnetic spintronics. Published by the American Physical Society 2024

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

Nonmagnetic Ground State in RuO_{2} Revealed by Muon Spin Rotation.

The magnetic ground state of single crystalline RuO_{2} was investigated by the muon spin rotation and relaxation (μSR) experiment. The spin precession signal due to the spontaneous internal magnetic field B_{loc}, which is expected in the magnetically ordered phase, was not observed in the temperature range 5-400K. Muon sites were evaluated by first-principles calculations using dilute hydrogen simulating muon as pseudohydrogen, and B_{loc} was simulated for the antiferromagnetic structures with a Ru magnetic moment |m_{Ru}|≈0.05μ_{B} suggested from diffraction experiments. As a result, the possibility was ruled out that muons are localized at sites where B_{loc} accidentally cancels. Conversely, assuming that the slow relaxation observed in μSR spectra was part of the precession signal, the upper limit for the magnitude of |m_{Ru}| was estimated to be 4.8(2)×10^{-4}μ_{B}, which is significantly less than 0.05μ_{B}. These results indicate that the antiferromagnetic order, as reported, is unlikely to exist in the bulk crystal.

Producing Conventional and Transient Amino(mercapto)methyl Radicals by Addition of Muonium to a Crystalline Thioformamide (Mes*NHCH=S).

Muonium (Mu=μ+e-) is composed of a muon of light isotope of proton (μ+) and electron (e-) and can be used as a light surrogate for a hydrogen atom. In this paper, we investigated addition of muonium to a newly synthesized Mes*-substituted thioformamide (Mes*NHCH=S, Mes*=2,4,6-tBu3C6H2). Transverse-field muon spin rotation (TF-μSR) of a solution sample of the thioformamide confirmed addition of muonium to the sulfur atom leading to the corresponding C-centered radical [Mes*NHC(H)⋅-SMu]. Density functional theory (DFT) calculations assigned a conventional amino(mercapto)methyl radical, in which both nitrogen and carbon were slightly pyramidalized, and the calculated muon hyperfine coupling constant (hfcc) including the muon isotope effect was compatible with the experimentally determined parameter. However, the muon level-crossing resonance (μLCR) spectrum of an anisotropic crystalline sample indicated two paramagnetic species, and the major product showed the considerably larger muon hfcc compared with the conventional structure of the amino(mercapto)methyl radical. The unusual transient muoniated thioformamide with the larger muon hfcc that showed rapid relaxation could be only explained by a transient structure including planarization of the nitrogen and carbon atoms in Mes*NHC(H)⋅-SMu.

Advanced Magnetocaloric Materials for Energy Conversion: Recent Progress, Opportunities, and Perspective

AbstractSolid‐state caloric effects as intrinsic thermal responses to different physical external stimuli (magnetic‐, uniaxial stress‐, pressure‐, and electric‐fields) can achieve a higher energy efficiency compared with traditional gas compression techniques. Among these effects, magnetocaloric energy conversion is regarded as the best available alternative and has been exploited extensively for promising application scenarios in the last decades. This review systematically introduces the magnetocaloric effect and its applications, and summarizes the corresponding representative magnetocaloric materials, as well as important progress in recent years. Specifically, the review focuses on some key understandings of the magnetocaloric effect by utilizing state‐of‐the‐art technical tools such as synchrotron X‐ray, neutron scattering, muon spin spectroscopy, positron annihilation spectroscopy, high magnetic fields, etc., and highlights their importance toward advanced materials design and development. An overview of the basic principles and applications of these advanced techniques on magnetocaloric materials is provided. Finally, the challenges and perspectives on further developments in this field are discussed. Further in‐depth understanding and manufacturing technology advancement combined with fast‐developed artificial intelligence and machine learning are expected to advance the magnetocaloric energy conversion technology closer to real applications.

µSR studies for radical reactions of unsaturated organophosphorus compounds

In this paper, the µSR studies of some unsaturated organophosphorus compounds containing heavier congeners of cyclobutane-1,3-diyl and anthracene are reviewed by discussing the usefulness of µSR for main group chemistry. The regioselective addition of muonium (Mu = [µ+e–]) to one of the skeletal phosphorus atoms in an electron-donating air-stable crystalline 1,3-diphosphacyclobutane-2,4-diyl leading to the paramagnetic 4-membered P-heterocycle was characterized by the Δ1 (ΔM = ± 1) resonance signal observed by muon (avoided) level-crossing resonance (µLCR). Meanwhile, a crystalline 1,3-diphosphacyclobutane-2,4-diyl bearing an electron-deficient nitrogen heterocyclic unit was analyzed by transverse-field muon spin rotation (TF-µSR) to characterize predominant muoniation at the skeletal radical carbon centre. A 9-phosphaanthracene bearing the trifluoromethyl (CF3) stabilizing groups at the peri positions was also investigated from the views of radical reactivity, and the regioselective addition of muonium to the skeletal sp2-type phosphorus atom was characterized by the muon hyperfine coupling (hfc) constant observed by TF-µSR and the Δ0 (ΔM = 0) signal of µLCR. The light mass of muon (Mass = 0.1134 amu) causes the larger zero-point energy and promotes the high-energy molecular structure in which the fused aromatic rings are almost flat, although the CF3 groups would prefer the non-planar saddle-like 9-phosphaanthracene skeleton.