Magnetic properties of nickel and platinum quaternary borocarbides

The zero‐field μ⁺SR technique is employed to study the magnetic properties of the non‐superconducting borocarbides Sm_1-xLu_xNi₂B₂C (x=0.0,\ 0.2) and NdPt_1.5Au_0.6B₂C. Coherent ordering of the Sm electronic moments appears below T_N=9.86(3) and 4.15(3) K for the x=0.0 and 0.2 compositions, respectively. No long range order of the Nd₃₊ moments is found in NdPt_1.5Au_0.6B₂C down to 80 mK. Freezing of the electronic moments into a spin‐glass state occurs at T_f\approx 1.2 K. A stretched exponential decay of the μ⁺ spin polarisation is observed above T_f with the exponent \beta smoothly decreasing on approaching T_f from above, reminiscent of the behaviour in other spin glasses. This revised version was published online in July 2006 with corrections to the Cover Date.     

Muon behaviour in diamond grown by chemical vapour deposition

Transverse‐field μSR spectroscopy was used to study the behaviour of positive muons implanted in polycrystalline chemical‐vapour‐deposited (CVD) diamond. Measurements were made at sample temperatures of 10 K, 100 K, and 300 K at a magnetic field of 7.5 mT to study the behaviour of the “normal” (isotropic) muonium state (Mu_T) and the diamagnetic states (μ^d), and at 10 K and 300 K at the so‐called “magic field” of 407.25 mT to study the anomalous (bond‐centred) muonium state (Mu_BC) and μ^d. The absolute fractions of the muonium states in the CVD diamond are observed to be close to those in high‐quality natural type‐IIa single crystal diamond. This revised version was published online in August 2006 with corrections to the Cover Date.     

Electric field gradients probed by μ+SR in Sc and \alpha\mbox-ScH_x solid solutions

In Sc and \alpha\mbox-ScH_x below 40 K two μ⁺ states are formed: a tunnelling state extending over two adjacent tetrahedral (T) interstices sharing one face in the ab‐plane of the hcp host lattice and a static μ⁺–Sc–H configuration analog to the T‐pair state formed by two H atoms across a Sc site along the crystalline c‐axis. This explains perfectly the high transverse‐field (TF) μSR measurements at low temperature and allows a qualitative understanding of the temperature dependence. The modelling of the low TF measurements requires in addition the consideration of the electric field gradient (EFG) components acting on the Sc nuclei near the μ⁺, i.e., of the radial EFG due to the μ⁺ and of the axially symmetric crystal field. The magnetic field dependence of the anisotropic μ⁺SR relaxation rate is strongly influenced by the H‐concentration in the solid solution system. This revised version was published online in August 2006 with corrections to the Cover Date.     

μSR on the novel heavy‐fermion system Nd2-yCeyCuO4

The magnetic correlations in Nd_2-yCe_yCuO₄ have been studied by zero and longitudinal field μSR. Nd_1.8Ce_0.2CuO₄ reveals a saturation of the muon relaxation rate below 0.5 K. Even down to 70 mK LF spectra evidence spin fluctuations in the dynamic regime with a rate of \sim 10⁹ s^-1 excluding long range magnetic order or spin glass freezing. The average Nd moment is estimated to be \approx 0.2\mu_B, i.e., strongly reduced from the value determined for the ground state Kramers doublet of Nd₂CuO₄. Extending former μSR measurements on Nd₂CuO₄, a gradual enhancement of the internal field has been detected below 10 K which is accompanied by an increase of the relaxation rate. These results are attributed to the development of ordered Nd moments. This revised version was published online in July 2006 with corrections to the Cover Date.     

High‐pressure μSR studies of ferro‐ and antiferromagnetic metals

High‐pressure μSR experiments on ferromagnetic nickel and \alpha‐iron and antiferromagnetic chromium are reported. In Ni above 260 K B_Fermi was found to be proportional to the saturation magnetization, whereas at lower temperatures it is temperature independent apart from a small anomaly below 30 K which is presumably caused by a magnetoelastic interaction. There was no evidence for an occupation of metastable sites by the μ⁺ below the Curie temperature. By contrast, in \alpha‐Fe the temperature dependence of \curpartialB_μ/\curpartialp shows a structure which might be attributed to the occupation of excited muon states at elevated temperatures. High‐pressure zero‐field experiments on Cr performed in the temperature regime between 4.5 K and 8 K revealed a pressure dependence of B_μ as large as \curpartialB_μ/\curpartialp=-(89.15\pm 0.06)\times 10^-12 T/Pa. In terms of volume dependence a very large negative Grüneisen parameter \gamma =-27 was obtained. This revised version was published online in July 2006 with corrections to the Cover Date.     

Theory of muon spin depolarization in condensed phases of hydrogen isotopes

A theory of muon spin depolarization in the molecular ion ( H₂μ)⁺(( D_2μ)) formed in a crystalline phase of hydrogen isotopes is presented. It is shown that the molecular ion ( H_2μ)⁺ has no time to thermalize during the muon lifetime, but after \tau\ll \tau_μ has time to transit to the lowest energy levels of the vibration‐rotation spectrum. The depolarization of the muon spin is determined by the interaction of the ion’s electric dipole moment with the lattice and by spin‐rotation interactions V_LS in the ion. This mechanism is analogous to that of “muonium”, replacing the hyperfine interaction by V_LS. The results can explain the experimental data and in particular the absence of a strong isotopic effect. This revised version was published online in August 2006 with corrections to the Cover Date.     

μSR on an induced‐moment spin glass system: Hg1-xFexSe

Zero and longitudinal field μSR have been used to examine the singlet ground state magnetism of the diluted magnetic semiconductor Hg_1-xFe_xSe. For x\geq 0.05\ μSR experiments indicate spin glass behaviour which is limited to sample regions with locally enhanced Fe²⁺ content. Longitudinal field spectra in the glassy state reveal a static local field \sim 50 mT due to induced moments of Fe²⁺. These are proposed to originate from a distribution of bound magnetic polaron energies. This revised version was published online in July 2006 with corrections to the Cover Date.     

μSR studies of fullerenes and their derivatives

The dynamic properties of pristine C₆₀ and C₇₀ are reviewed, emphasizing the results of the ZF‐ and ALC‐μ⁺SR techniques. In C₆₀, the \mboxfcc\rightarrow\mboxsc transition is accompanied by a change in the dynamics from isotropic reorientational to quasi‐random jump motion between nearly‐degenerate orientations. C₇₀ is frozen on a timescale of 30 ns up to 170 K. At higher temperatures, the motion is found to be complex, consisting of a uniaxial rotation part together with a nutational or jumping motion of the unique axis. Anisotropy on the 30 ns timescale persists to 370 K, well into the fcc phase. The ZF‐μ⁺SR technique has been also employed to study the magnetic properties of fullerides. In the organic salt (TDAE)C₆₀, spontaneous magnetic order is directly observed below a Curie temperature of 16.1 K, higher than any other organic material. In the quasi‐one‐dimensional conductor CsC₆₀, static magnetic order of a random nature is observed to develop in the vicinity of the metal–insulator transition at 30 K with no direct evidence of long range order present. This revised version was published online in August 2006 with corrections to the Cover Date.     

Diffusion, trapping, and relaxation of Mu+ and Mu- in heavily‐doped GaAs

The diamagnetic muonium states in heavily doped GaAs are investigated with a combination of transverse‐field and longitudinal‐field μSR techniques. In metallic n‐type GaAs, formation of Mu^- occurs because of the high Fermi energy. This analog of the hydride ion (H^-) is located in a T_Ga interstice where it is essentially immobile up to about 500 K. At higher temperatures, Mu_T acts as an electron–hole recombination center. In p‐type GaAs, Mu⁺ traps at two different sites, one at low temperatures and a second at higher temperatures after detrapping from the first. This revised version was published online in August 2006 with corrections to the Cover Date.     

Muon spin relaxation investigation of frustrated antiferromagnetic pyrochlores A2B2O7

In a system where magnetic ions occupy the vertices of edge or corner sharing triangular units, the natural antiferromagnetic coupling between ions is geometrically frustrated. A wide variety of interesting magnetic behaviour has been observed in pyrochlores, where magnetic ions form a network of corner sharing tetrahedra. The low temperature spin dynamics of a number of pyrochlores A₂B₂O₇ have been investigated using the technique of μ SR. For example, Y₂Mo₂O₇ shows a transition to a disordered magnetic state similar to a spin glass at T_F=22 K. However, unlike conventional metallic spin glasses, a non‐zero muon spin depolarization rate is observed to persist well below 0.1\ T_F. These results suggest that there is a finite density of states for magnetic excitations in this system near zero energy. This revised version was published online in July 2006 with corrections to the Cover Date.     

Muonium addition to vinylaromatics and to diacetylenes: formation and stability of arylethyl/vinylcyclohexadienyl and alkynylvinyl radicals

According to TF‐μSR measurements and PM3 M.O.calculations, free radicals formed by muonium addition to styrene, 1‐vinylnaphthalene and 2‐vinylnaphthalene are of the arylethyl type ( ArCHCH₂Mu\mbox$\bullet$) since it is energetically considerably more favourable for Mu\mbox$\bullet$ to add to the vinyl group than to the aromatic rings. In contrast, Mu\mbox$\bullet$ adds to 9‐vinylanthracene at the 10‐position yielding the 4‐vinyldibenzocyclohexadienyl radical, which is more stable by ca 7 kcal/mol than the 9‐anthrylethyl radical. For diacetylenes (i.e. MeC₄Me) the propensity for muonium addition is to the terminal carbon atoms, but the choice is less clear for Me₃SiC₄SiMe₃. For PhC₄Ph, 3 radicals are detected and are assigned to the C1, C2 and ortho ring adducts, with the couplings (and yields): 334 (5.7%), 389 (4.2%), 439 (3.6%). This revised version was published online in August 2006 with corrections to the Cover Date.     

Muons in type-II superconductors: μ+ diffusion in ultra-pure niobiumdiffusion in ultra-pure niobium

The diffusivityD _μ of positive muons (μ⁺) in the mixed state of superconducting high-purity, high-perfection niobium single crystals is investigated by measurements of the relaxation of the transverse muon spin polarization (μ⁺SR). The method makes use of the strong magnetic field gradients existing in the mixed state of Type-II superconductors and monitorsD _μ through the variation of the magnetic field felt by the μ⁺ during their diffusion through the crystals. For μ⁺ near the centres of the flux lines inNb it givesD _μ(4.6 K)=(8±2)·10⁻¹¹m²S⁻¹. The positive temperature coefficient ofD _μ indicates that at liquid-helium temperatures the diffusivity of μ⁺ inNb is mainly due to phonon-assisted tunnelling processes.     

Spin fluctuations and magnetic order in the heavy fermion compound CePt2Sn2

We present zero and longitudinal field μ SR measurements of single crystal and polycrystalline specimens of the heavy fermion compound CePt₂Sn₂. Above 1 K the behaviour of the two samples is indistinguishable; the muon 1/T_1 increases with decreasing temperature until 25 K when it plateaus. The 1/T_1 relaxation rate differs strongly for the two cases below \sim\,0.8\ K. At 0.1 K a rate of about 20 μ s^-1 is seen in the polycrystal while in the single crystal it is only about 5 μ s^-1. Even more revealing is the fact that longitudinal field decoupling spectra at very low temperatures demonstrate an essentially static spin system to be present in the polycrystalline material while the single crystal shows definite dynamic spin properties. We conclude that, in the presence of the distortion, long range magnetic order occurs below 0.9 K while in tetragonal symmetry long range order is suppressed (probably due to frustration) and spin fluctuations remain for T\rightarrow0. This revised version was published online in July 2006 with corrections to the Cover Date.     

Evidence for muonium emission from an SiO2 layer on n-type Si and the positive muon state in Si

Evidence for the emission of slow muonium atoms from a 3.0-nm-thick SiO₂ layer covered on an n-type Si is reported. Also, upon applying an rf-resonance technique at the muon frequency, a time-differential observation of a delayed state-change from muonium to diamagnetic muon at room temperature was observed. Combining results obtained by use of longitudinal field decoupling and transverse spin rotation methods, the conversion rate was estimated to be 5 to 10 μs⁻¹. Both of the above results, namely the observation of the emission and state-change of muonium, suggest a process in which μ⁺ initially captures an electron from Si, then quickly converts to μ⁺ again during thermal diffusion in the Si towards the SiO₂ layer. Within the oxide layer, muonium is again formed and subsequently is emitted from the SiO₂ surface.     

Muon spin relaxation measurements of CsC60, RbC60, KC60

Muon spin relaxation (μ⁺SR) measurements of CsC₆₀ and RbC₆₀ have revealed magnetic ordering at 20 K and 15 K respectively, with static internal fields at the muon site of \sim7 G for both samples. No magnetic ordering is seen in KC₆₀ down to 2.5 K. An apparent small increase in muon spin relaxation which had been seen at 70 K in RbC₆₀ is ascribed to an extrinsic effect, originating in muons which stopped in the aluminum sample holder. This revised version was published online in July 2006 with corrections to the Cover Date.     

Time‐differential radio‐frequency muon spin resonance (TD‐RFμSR) technique at a pulsed muon beam

Longitudinal‐field μSR methods, e.g., radio‐frequency μ⁺ spin resonance (RFμSR), are well suited to investigate dynamic processes that destroy the phase coherence of the muon spin ensemble. Additional information on relaxation processes of the muon species under investigation is obtained from time‐differential (TD) data acquisition. In this paper we describe the set‐up of a TD‐RFμSR spectrometer installed at the ISIS pulsed muon facility at the Rutherford Appleton Laboratory (RAL, Chilton, UK). As an example, results of TD‐RFμSR measurements on muons in diamagnetic environment μ^d in a boron‐doped silicon sample under illumination at 55 K are presented. This revised version was published online in August 2006 with corrections to the Cover Date.     

Zero‐field μ+SR study of the colossal magnetoresistance material La0.67Ca0.33MnO3

Zero‐field μ⁺SR and resistivity experiments on La_0.67Ca_0.33MnO₃ powder show that the ferromagnetic transition temperature (T_C=274\ K) and resistivity peak temperature coincide to within 1 K, about 10 K higher than T_C determined from the bulk magnetization. The sublattice magnetization \nu_μ(T) is well described for T ≤ T_C by (1-T/T_C)^β , where β =0.345 ± 0.015. Unusual relaxation dynamics suggest a wide distribution of Mn‐ion correlation times. These results are discussed in terms of the effects of polarons on the spin and charge dynamics. This revised version was published online in July 2006 with corrections to the Cover Date.     

μ+SR study of heavy-fermion magnetism in Ce(Cu1-xNix)2Ge2

We report muon spin relaxation (μ⁺SR) studies on the magnetic phase diagram of Ce(Cu_1-xNi_x)₂Ge₂ polycrystals for 0.5≤ x ≤ 0.8. A sharp magnetic transition, evidenced by the appearance of a fast Gaussian relaxation component σ, has been observed in the x = 0.5 alloy at 4.0 K in zero applied field. The average local field < B_μ> at the stopping sites of the muons, extracted from σ, exhibits a linear temperature dependence. We associate these features with an incommensurate spin density wave (SDW) ordering. Magnetic ordering, either long range or short range, and signatures of non-Fermi liquid behaviour have not been observed down to 2.0 K at x = 0.8. This revised version was published online in August 2006 with corrections to the Cover Date.     

Search for magnetic order in undoped and doped spin‐gap systems by μSR

We introduce our μSR investigations of spin‐gap systems, such as, (1) a 2‐leg spin‐ladder material SrCu₂O₃, (2) a Haldane material (S=1 spin‐chain) Y₂BaNiO₅, (3) a spin‐Peierls material CuGeO₃, (4) a spin‐chain# material Sr₆Ca₈Cu₂₄O₄₁. All of these antiferromagnetic spin systems are characterized by a spin‐gap between the singlet ground‐state and the triplet first excited states. In the above‐mentioned materials, we confirmed the absence of magnetic order down to milli‐Kelvin regime, supporting the non‐magnetic feature of the ground‐state. If a spin‐gap system is doped with charges and/or vacancies at the spin site, unpaired spins are induced out of the singlet ground‐state. In some materials, doping completely destroys the singlet ground‐state and induces a bulk magnetic order. We report μSR investigations of doped materials as well, which clarifies the existence/absence of a magnetic order upon doping. This revised version was published online in July 2006 with corrections to the Cover Date.     

Longitudinal field repolarization studies of reorientational dynamics in the fullerenes C60 and C70

LFμSR studies on the pure fullerenes C₆₀ and C₇₀ show temperature dependent features associated with the reorientational behaviour of the fullerenyl radicals MuC₆₀ and MuC₇₀ in the crystalline host substrate. If not excluded from the experimental setup, molecular oxygen undergoes spin exchange reactions with the radicals. The data for C₆₀ correspond to a situation effectively static at 150 K and fully averaged to isotropy at 300 K, while for C₇₀ the data conspicuously do not conform to the predictions of the pseudostatic model employed in ALC‐μSR studies. This revised version was published online in August 2006 with corrections to the Cover Date.