We report muon spin relaxation and magnetometry studies of bulk Mn$_{1.4}$Pt$_{0.9}$Pd$_{0.1}$Sn and MnNiGa, two materials which have recently been proposed to host topological magnetic states in thin lamella (antiskyrmions for Mn$_{1.4}$Pt$_{0.9}$Pd$_{0.1}$Sn and biskyrmions for MnNiGa), and show spin reorientation transitions in bulk. These measurements shed light on the magnetic dynamics surounding the two magnetic phase transitions in each material. In particular, we demonstrate that the behaviour approaching the higher temperature transition in both samples is best understood by considering a slow decrease in the frequency of dynamics with temperature, rather than the sharp critical slowing down typical of second order transitions. Furthermore, at low temperatures the two samples both show spin dynamics over a broad range of frequencies that persist below the spin reorienation transition. The dynamic behavior we identify gives new insight into the bulk magnetism of these materials that may help underpin the stabilization of the topologically non-trivial phases that are seen in thin lamellae.
We review examples of muon-spin relaxation measurements on molecule-based magnetic coordination polymers, classified by their magnetic dimensionality. These include the one-dimensional s=1/2 spin chain Cu(pyz)(NO3)2 and the two-dimensional s=1/2 layered material [Cu(HF2)(pyz)2]BF4. We also describe some of the more exotic ground states that may become accessible in the future given the ability to tune the interaction strengths of our materials through crystal engineering.
We present the results of muon-spin relaxation (muSR) measurements on the hexagonal manganite HoMnO3. Features in the temperature-dependent relaxation rate, lambda, correlate with the magnetic transitions at 76 K, 38 K and 34 K. The highest temperature transition, associated with the ordering of Mn3+ moments has the largest effect on lambda. The application of a static electric field of E=10^4 Vm^-1 below T=50 K causes a small reduction in lambda which is suggestive of coupling between ferroelectric and magnetic domain walls in the ordered state of the material.
We demonstrate that quantum-critical spin dynamics can be probed in high magnetic fields using muon-spin relaxation ($μ^{+}$SR). Our model system is the strong-leg spin ladder bis(2,3-dimethylpyridinium) tetrabromocuprate (DIMPY). In the gapless Tomonaga-Luttinger liquid phase we observe finite-temperature scaling of the $μ^{+}$SR $1/T_1$ relaxation rate which allows us to determine the Luttinger parameter $K$. We discuss the benefits and limitations of local probes compared with inelastic neutron scattering.
We present a detailed study of the magnetic properties of weakly ferromagnetic/quantum critical Nb$_{1-y}$Fe$_{2+y}$ using muon spin rotation and relaxation ($μ$SR). By means of an angular dependent study of the muon spin rotation signal in applied magnetic fields on a single crystal in the paramagnetic state we establish the muon stopping site in the crystallographic lattice of NbFe$_2$. With this knowledge we develop models to describe the muon spin rotation and relaxation signals in the weakly ferromagnetic, spin density wave and quantum critical phases of Nb$_{1-y}$Fe$_{2+y}$ and fit the c…
The effect of randomness on the quantum spin system Tl$_{1-x}$K$_x$CuCl$_3$ with ${\boldmath $x$}$ = 0.44 studied by the Zero-field Muon-Spin-Relaxation (ZF-$μ$SR) method
Muon spin relaxation measurements are reported on samples of dimethylammonium metal formates containing magnetic divalent nickel, cobalt, manganese, and copper ions. These hybrid organic-inorganic perovskites exhibit weak ferromagnetism and are, apart from the copper system, multiferroics with well separated magnetic and antiferroelectric transitions. We use muons to follow the sublattice magnetization, observing the effect of the spin reorientation transitions below TN and the criticality approaching TN. The multiferroic samples have three-dimensional antiferromagnetic interactions, but the c…
We report the results of muon-spin relaxation measurements on the low-dimensional antiferromagnet Rb4Cu(MoO4)3. No long-range magnetic order is observed down to 50 mK implying a ratio T_N/J<0.005 (where J is the principal exchange strength along the spin chains) and an effective ratio of interchain to intrachain exchange of |J_perp/J|<2 x 10^-3, making the material an excellent realization of a one-dimensional quantum Heisenberg antiferromagnet. We probe the persistent spin excitations at low temperatures and find that ballistic spin transport dominates the excitations detected below 0.3 K.
Muon-spin relaxation results on the pyrochlore iridate Nd$_2$Ir$_2$O$_7$ are reported. Spontaneous coherent muon-spin precession below the metal-insulator transition (MIT) temperature of about 33 K is observed, indicating the appearance of a long-ranged magnetic ordering of Ir$^{4+}$ moments. With further decrease in temperature, the internal field at the muon site increases again below about 9 K. The second increase of internal field suggests the ordering of Nd$^{3+}$ moments, which is consistent with a previous neutron experiment. Our results suggest that the MIT and magnetic ordering of Ir$…
We present a detailed local probe study of the magnetic order in the oxychalcogenide La2O2Fe2OSe2 utilizing 57Fe Moessbauer, 139La NMR, and muon spin relaxation spectroscopy. This system can be regarded as an insulating reference system of the Fe arsenide and chalcogenide superconductors. From the combination of the local probe techniques we identify a non-collinear magnetic structure similar to Sr2F2Fe2OS2. The analysis of the magnetic order parameter yields an ordering temperature TN = 90.1 K and a critical exponent of beta = 0.133, which is close to the 2D Ising universality class as report…
The results of muon-spin relaxation and heat capacity measurements on two pyroxene compounds LiFeSi2O6 and NaFeSi2O6 demonstrate that despite their underlying structural similarity the magnetic ordering is considerably different. In LiFeSi2O6 a single muon precession frequency is observed below TN, consistent with a single peak at TN in the heat capacity and a commensurate magnetic structure. In applied magnetic fields the heat capacity peak splits in two. In contrast, for natural NaFeSi2O6, where multiferroicity has been observed in zero-magnetic-field, a rapid Gaussian depolarization is obse…
A crystal structure that cannot be superposed on its mirror image by any combination of rotations and translations is classified as chiral. Such crystal structures have gained importance in recent years since they are prone to host unconventional magnetic orders and to exhibit topological magnetic textures. These properties result from the Dzyaloshinskii-Moriya antisymmetric exchange interaction which is authorized when space inversion is broken. While recent reports have shown the muon spin rotation and relaxation technique to provide unique information about structural and dynamical properti…
We present the results of zero-field muon-spin relaxation measurements made on the double perovskite insulators Sr$_{2}B$OsO$_6$ ($B={\rm Fe, Y, In}$). Spontaneous muon-spin precession indicative of quasistatic long range magnetic ordering is observed in Sr$_{2}$FeOsO$_6$ within the AF1 antiferromagnetic phase for temperatures below $T_{\rm N}=135 \pm 2~{\rm K}$. Upon cooling below $T_2 \approx 67~{\rm K}$ the oscillations cease to be resolvable owing to the coexistence of the AF1 and AF2 phases, which leads to a broader range of internal magnetic fields. Using density functional calculations …
The stretched diamond lattice material LiYbO2 has recently been reported to exhibit two magnetic transitions ($T_{N1} = 1.1 K$, $T_{N2} = 0.45 K$) via specific heat, magnetization, and neutron scattering measurements [Bordelon et al., Phys. Rev. B 103, 014420 (2021)]. Here we report complementary magnetic measurements down to T = 0.28 K via the local probe technique of muon spin relaxation. While we observe a rapid increase in the zero-field muon depolarization rate at $T_{N1}$, we do not observe any spontaneous muon precession for $T < T_{N1}$, which is typically associated with long-range ma…
We present the results of a muon-spin relaxation (muSR) investigation into magnetic ordering in several families of layered quasi-two-dimensional molecular antiferromagnets based on transition metal ions such as S=1/2 Cu2+ bridged with organic ligands such as pyrazine. In many of these materials magnetic ordering is difficult to detect with conventional magnetic probes. In contrast, muSR allows us to identify ordering temperatures and study the critical behavior close to T_N . Combining this with measurements of in-plane magnetic exchange J and predictions from quantum Monte Carlo simulations …
We present muon spin relaxation ($μ$SR) and specific-heat versus temperature $C(T)$ measurements on polycrystalline and single-crystal samples of the pyrochlore magnet Yb$_2$Ti$_2$O$_7$. $C(T)$ exhibits a sharp peak at a $T_\mathrm{C}$ of 0.21 and 0.26~K for the single-crystal and polycrystalline samples respectively. For both samples, the magnetic entropy released between 50~mK and 30~K amounts to $R\ln2$ per Yb. At temperatures below $T_\mathrm{C}$ we observe a steep drop in the asymmetry of the zero-field $μ$SR time spectra at short time scales, as well as a decoupling of the muon spins fro…
We report the results of a muon-spin relaxation ($μ$SR) investigation of La$_{2-x}$Sr$_{x}$CoO$_{4}$, an antiferromagnetic insulating series which has been shown to support charge ordered and magnetic stripe phases and an hourglass magnetic excitation spectrum. We present a revised magnetic phase diagram, which shows that the suppression of the magnetic ordering temperature is highly sensitive to small concentrations of holes. Distinct behavior within an intermediate $x$ range ($0.2 \leq x \lesssim 0.6$) suggests that the putative stripe ordered phase extends to lower $x$ than previously thoug…
We report a muon spin rotation/relaxation ($μ$SR) study of single-crystalline samples of the $α$-RuCl$_3$ honeycomb magnet, which is presumed to be a model compound for the Kitaev-Heisenberg interaction. It is inferred from magnetic susceptibility and specific-heat measurements that the present samples exhibit successive magnetic transitions at different critical temperatures $T_{\rm N}$ with decreasing temperature, eventually falling into the $T_{\rm N}=7$ K antiferromagnetic (7 K) phase that has been observed in only single-crystalline specimens with the least stacking fault. Via $μ$SR measu…
We have observed an electronic energy level crossing in a molecular nanomagnet (MNM) using muon-spin relaxation. This effect, not observed previously despite several muon studies of MNM systems, provides further evidence that the spin relaxation of the implanted muon is sensistive to the dynamics of the electronic spin. Our measurements on a broken ring MNM [H_{2}N^{t}Bu^{is}Pr][Cr_{8}CdF_{9}(O_{2}CC(CH_{3})_{3})_{18}] (hereafter Cr_{8}Cd), which contains eight Cr ions, show clear evidence for the S=0 to S=1 transition that takes place at B_{c}=2.3 T. The crossing is observed as a resonance-li…
We present longitudinal-field muon-spin relaxation (LF $μ$SR) measurements on two systems that stabilize a skyrmion lattice (SkL): Cu$_2$OSeO$_3$, and Co$_x$Zn$_y$Mn$_{20-x-y}$ for $(x,y)~=~(10,10)$, $(8,9)$ and $(8,8)$. We find that the SkL phase of Cu$_2$OSeO$_3$ exhibits emergent dynamic behavior at megahertz frequencies, likely due to collective excitations, allowing the SkL to be identified from the $μ$SR response. From measurements following different cooling protocols and calculations of the muon stopping site, we suggest that the metastable SkL is not the majority phase throughout the …
Positive-muon ($μ^+$) Knight shifts have been measured in the paramagnetic states of Pr$_{1-x}$Nd$_x$Os$_4$Sb$_{12}$ alloys, where $x =$ 0, 0.25, 0.45, 0.50, 0.55, 0.75, and 1.00. In Pr-substituted NdOs$_4$Sb$_{12}$ ($x \le$ 0.75), but not in NdOs$_4$Sb$_{12}$, Clogston-Jaccarino plots of $μ^+$ Knight shift~$K$ versus magnetic susceptibility~$χ$ exhibit an anomalous saturation of $K(χ)$ at $\sim-$0.5% for large susceptibilities (low temperatures), indicating a reduction of the coupling strength between $μ^+$ spins and $4f$ paramagnetism for temperatures $\lesssim$ 15~K. We speculate that itine…
We have carried out neutron diffraction, muon spin relaxation (muSR) and inelastic neutron scattering investigations on a polycrystalline sample of CeOs2Al10 to investigate the nature of the phase transition observed near 29 K in the resistivity and heat capacity. Our muSR data clearly reveal coherent frequency oscillations below 28 K, indicating the presence of an internal field at the muon site, which confirms the long-range magnetic ordering of the Ce-moment below 28 K. Upon cooling the sample below 15 K, unusual behaviour of the temperature dependent muSR frequencies may indicate either a …
To clarify the magnetic properties of cluster-glass states in Sr1-xLaxRuO3 (0.3 <= x <= 0.5), we report herein the results of muon spin relaxation (muSR) and neutron powder diffraction measurements. The muSR experiments showed that magnetic clusters start developing well above the peak temperature T^* in the ac susceptibility. The volume fraction of the magnetically ordered region increases continuously with decreasing temperature, showing no anomaly at T^*, and reaches nearly 100% at the lowest temperature. The temperature variation of the volume fraction is essentially independent of the La …
The muon spin relaxation method (μSR) is a powerful microscopic tool to probe electronic states of materials observing local magnetic field distributions on the muon. It often happens that a distribution of local magnetic fields shows intermediate state between Gaussian and Lorentzian shapes. In order to generally describe intermediate field distributions, we dealt the convolution of two isotropic distributions in the three dimension and derived exact muon-spin relaxation functions which can be applied to all crossover regimes between the Gaussian and Lorentzian.
Muon spin relaxation on Nd$_2$Ti$_2$O$_7$ (NTO) and NdLaTi$_2$O$_7$ (NLTO) compounds are presented. The time spectra for both compounds are as expected for the paramagnetic state at high temperatures, but deviate from the exponential function below about 100 K. The muon spin relaxation rate increases with decreasing temperature firstly, and then levels off below about 10 K, which is reminiscent of the frustrated systems. An enhancement of the relaxation rate by a longitudinal field in the paramagnetic state is observed for NTO, and eliminated by a magnetic dilution for the NLTO sample. This su…
We report muon spin relaxation rate measurements on films composed of aluminum grains having a size of a few nm, with a large energy level splitting of the order of 100 K. The films range from weakly metallic to insulating. In the insulating case the low temperature relaxation rate is consistent with the presence of single electron spins in grains having an odd number of electrons. The relaxation rate temperature dependence follows an activation law having an energy scale in agreement with the average level splitting. In weakly metallic films the relaxation rate is smaller and decreases faster…
We report results of a muon spin relaxation study of slow magnetic fluctuations in the pseudogap phase of underdoped single-crystalline YBa$_{2}$Cu$_{3}$O$_{y}$, $y = 6.77$ and 6.83. The dependence of the dynamic muon spin relaxation rate on applied magnetic field yields the rms magnitude~$B\mathrm{_{loc}^{rms}}$ and correlation time~$τ_c$ of fluctuating local fields at muon sites. The observed relaxation rates do not decrease with decreasing temperature~$T$ below the pseudogap onset at $T^\ast$, as would be expected for a conventional magnetic transition; both $B\mathrm{_{loc}^{rms}}$ and $τ_…
The magnetic and quadrupolar ordered states of polycrystalline YbRu2Ge2 have been investigated using zero-field muon spin relaxation (μSR) and neutron diffraction measurements. Specific heat measurements show three successive phase transitions, with decreasing temperature from a paramagnetic to a quadrupolar state at T0 ~ 10 K, from the quadrupolar to a magnetic state at T1 ~ 6.5 K and a possible change in the magnetic ground state at T2 ~ 5.5 K. Clear evidence for the magnetic transition below 7 K (spectrum at 8 K reveals paramagnetic state) and a likely change in the magnetic structure near …
The effects of electron (Ir) and hole (Re) doping on the hybridization gap and antiferromagnetic order have been studied by magnetization, muon spin relaxation ($μ^+$SR), and inelastic neutron scattering on the polycrystalline samples of Ce(Os$_{1-x}$Ir$_x$)$_2$Al$_{10}$ ($x$ = 0.08 and 0.15) and CeOs$_{1.94}$Re$_{0.06}$Al$_{10}$. $μ^+$SR spectra clearly reveals magnetic ordering below 20 and 10 K for $x$ = 0.08 and 0.15 samples respectively with a very weak signature of oscillations of the muon initial asymmetry at very short time scale. Our important findings are that small amount of electro…
At low temperatures, spin dynamics in ideal spin ice is due mainly to dilute, thermally excited magnetic monopole excitations. I consider how these will affect the dynamics of a nuclear spin (the same theory applies to muon spin resonance if implanted muons do not diffuse). Up to the time scale for nearby monopoles to be rearranged, a stretched-exponential form of the relaxation functions is expected. I work out the expected exponent in that exponential and the formulas for the $T_1$ (longitudinal) and $T_2$ (dephasing) relaxations, as a function of the monopole density. Experimental NMR is in…
We interpret recent measurements of the zero field muon relaxation rate in the frustrated magnetic pyrochlore Dy$_2$Ti$_2$O$_7$ as resulting from the quantum diffusion of muons in the substance. In this scenario, the plateau observed at low temperature ($<7$ K) in the relaxation rate is due to coherent tunneling of the muons through a spatially disordered spin state and not to any magnetic fluctuations persisting at low temperature. Two further regimes either side of a maximum relaxation rate at $T^* = 50$ K correspond to a crossover between tunnelling and incoherent activated hopping motion o…
We present measurements of magnetic field and frequency dependences of the low temperature (T = 1.8 K) AC-susceptibility, and temperature and field dependences of the longitudinal field positive muon spin relaxation (μSR) for LiY$_{1-x}$Ho$_x$F$_4$ with x = 0.0017, 0.0085, 0.0408, and 0.0855. The fits of numerical simulations to the susceptibility data for the x = 0.0017, 0.0085 and 0.0408 show that Ho-Ho cross-relaxation processes become more important at higher concentrations, signaling the crossover from single-ion to correlated behavior. We simulate the muon spin depolarization using the p…
Longitudinal-field muon-spin-relaxation measurements have revealed inhomogeneous distribution of the internal magnetic field at temperatures above the bulk superconducting (SC) transition temperature, $T_{\rm c}$, in slightly overdoped Bi$_2$Sr$_2$Ca$_{1-x}$Y$_x$Cu$_2$O$_{8+δ}$. The distribution width of the internal magnetic field, $Δ$, evolves continuously with decreasing temperature toward $T_{\rm c}$. The origin of the increase in $Δ$ is discussed in terms of the creation of SC domains in a sample.
Muon spin relaxation measurements on some quantum spin ice candidate materials, the insulating pyrochlores Pr2B2O7 (B = Sn, Zr, Hf), have been performed for temperatures in the range 0.05-280 K. The results are indicative of a static distribution of magnetic moments which appears to grow on cooling and whose size at low temperatures is significantly larger than that expected for Pr nuclear moments. Using density functional theory we show how this effect can be explained via a hyperfine enhancement arising from a splitting of the non-Kramers doublet ground states on Pr ions close to the muon wh…
We present the results of muon-spin relaxation measurements of spin excitations in the one-dimensional quantum Heisenberg antiferromagnet Cu(pyz)(NO$_{3}$)$_{2}$. Using density-functional theory we propose muon sites and assess the degree of perturbation the muon probe causes on the system. We identify a site involving the muon forming a hydroxyl-type bond with an oxygen on the nitrate group that is sensitive to the characteristic spin dynamics of the system. Our measurements of the spin dynamics show that in the temperature range $T_{\mathrm{N}}<T<J$ (between the ordering temperature $T_{\mat…
