Local Electronic Structure and Dynamics of Muon-Polaron Complexes in Fe_{2}O_{3}.

We perform detailed muon spin rotation (µSR) measurements in the classic antiferromagnet Fe_{2}O_{3} and explain the spectra by considering dynamic population and dissociation of charge-neutral muon-polaron complexes. We show that charge-neutral muon states in Fe_{2}O_{3}, despite lacking the signatures typical of charge-neutral muonium centers in nonmagnetic materials, have a significant impact on the measured µSR frequencies and relaxation rates. Our identification of such polaronic muon centers in Fe_{2}O_{3} suggests that isolated hydrogen (H) impurities form analogous complexes, and that H interstitials may be a source of charge carrier density in Fe_{2}O_{3}.

Direct observation of muonium reacting with uncapped gold nanoparticles in porous silica and nature of the final state.

We report the reaction of muonium (Mu = [µ+e-]), a light isotopic analog of hydrogen, with uncapped gold nanoparticles embedded in mesoporous silica. Using the radio-frequency muon spin rotation (RF-µSR) technique, we directly observe and characterize the resulting final state on the nanoparticle surface, showing conclusively its diamagnetic nature. The magnetic environment experienced by the reacted muons is only weakly perturbed compared to that of muons in a silica reference, consistent with the surface of the gold nanoparticles being metallic and non-magnetic. We demonstrate the potential of RF-µSR for the investigation of the surface properties of nanoparticles and show the feasibility of Knight shift measurements of muons on metal surfaces.

Bi-Arrhenius Diffusion and Surface Trapping of

We report measurements of the diffusion rate of isolated ion-implanted ^{8}Li^{+} within ∼120 nm of the surface of oriented single-crystal rutile TiO_{2} using a radiotracer technique. The α particles from the ^{8}Li decay provide a sensitive monitor of the distance from the surface and how the depth profile of ^{8}Li evolves with time. The main findings are that the implanted Li^{+} diffuses and traps at the (001) surface. The T dependence of the diffusivity is described by a bi-Arrhenius expression with activation energies of 0.3341(21) eV above 200 K, whereas at lower temperatures it has a much smaller barrier of 0.0313(15) eV. We consider possible origins for the surface trapping, as well the nature of the low-T barrier.

Communication: Chemisorption of muonium on gold nanoparticles: A sensitive new probe of surface magnetism and reactivity.

Chemisorption of muonium onto the surface of gold nanoparticles has been observed. Muonium (µ+e-), a light hydrogen-like atom, reacts chemically with uncapped 7 nm gold nanoparticles embedded in mesoporous silica (SBA-15) with a strong temperature-dependent rate. The addition rate is fast enough to allow coherent spin transfer into a diamagnetic muon state on the nanoparticle surface. The muon is well established as a sensitive probe of static or slowly fluctuating magnetic fields in bulk matter. These results represent the first muon spin rotation signal on a nanoparticle surface or any metallic surface. Only weak magnetic effects are seen on the surface of these Au nanoparticles consistent with Pauli paramagnetism.

ß-NMR Investigation of the Depth-Dependent Magnetic Properties of an Antiferromagnetic Surface.

By measuring the prototypical antiferromagnet α-Fe_{2}O_{3}, we show that it is possible to determine the static spin orientation and dynamic spin correlations within nanometers from an antiferromagnetic surface using the nuclear spin polarization of implanted ^{8}Li^{+} ions detected with ß-NMR. Remarkably, the first-order Morin spin reorientation in single crystal α-Fe_{2}O_{3} occurs at the same temperature at all depths between 1 and 100 nm from the (110) surface; however, the implanted nuclear spin experiences an increased 1/T_{1} relaxation rate at shallow depths revealing soft-surface magnons. The surface-localized dynamics decay towards the bulk with a characteristic length of ε=11±1 nm, closely matching the finite-size thresholds of hematite nanostructures.

The phase diagram of electron-doped La(2-x)Ce(x)CuO(4-δ).

Superconductivity is a striking example of a quantum phenomenon in which electrons move coherently over macroscopic distances without scattering. The high-temperature superconducting oxides (cuprates) are the most studied class of superconductors, composed of two-dimensional CuO2 planes separated by other layers that control the electron concentration in the planes. A key unresolved issue in cuprates is the relationship between superconductivity and magnetism. Here we report a sharp phase boundary of static three-dimensional magnetic order in the electron-doped superconductor La(2-x)Ce(x)CuO(4-δ), where small changes in doping or depth from the surface switch the material from superconducting to magnetic. Using low-energy spin-polarized muons, we find that static magnetism disappears close to where superconductivity begins and well below the doping level at which dramatic changes in the transport properties are reported. These results indicate a higher degree of symmetry between the electron and hole-doped cuprates than previously thought.

Controlling the near-surface superfluid density in underdoped YBa2Cu3O(6+x) by photo-illumination.

The interaction with light weakens the superconducting ground state in classical superconductors. The situation in cuprate superconductors is more complicated: illumination increases the charge carrier density, a photo-induced effect that persists below room temperature. Furthermore, systematic investigations in underdoped YBa2Cu3O(6+x) (YBCO) have shown an enhanced critical temperature Tc. Until now, studies of photo-persistent conductivity (PPC) have been limited to investigations of structural and transport properties, as well as the onset of superconductivity. Here we show how changes in the magnetic screening profile of YBCO in the Meissner state due to PPC can be determined on a nanometer scale utilizing low-energy muons. The data obtained reveal a strongly increased superfluid density within the first few tens of nanometers from the sample surface. Our findings suggest a non-trivial modification of the near-surface band structure and give direct evidence that the superfluid density of YBCO can be controlled by light illumination.

Nature of weak magnetism in SrTiO3/LaAlO3 multilayers.

We report the observation of weak magnetism in superlattices of LaAlO(3)/SrTiO(3) using ß-detected nuclear magnetic resonance. The spin lattice relaxation rate of ^{8}Li in superlattices with a spacer layers of 8 and 6 unit cells of LaAlO(3) exhibits a strong peak near ~35 K, whereas no such peak is observed in a superlattice with spacer layer thickness of 3 unit cells. We attribute the observed temperature dependence to slowing down of weakly coupled electronic moments at the LaAlO(3)/SrTiO(3) interface. These results show that the magnetism at the interface depends strongly on the thickness of the spacer layer, and that a minimal thickness of ~4-6 unit cells is required for the appearance of magnetism. A simple model is used to determine that the observed relaxation is due to small fluctuating moments (~0.002µ(B)) in the two samples with a larger LaAlO(3) spacer thickness.

Proximal magnetometry in thin films using betaNMR.

Low energy ion implantation of hyperpolarized radioactive magnetic resonance probes allows the NMR study of thin film heterostructures by enabling depth-resolved measurements on a nanometer lengthscale. By stopping the probe ions in a layer adjacent to a layer of interest, it is possible to study magnetic fields proximally. Here we show that, in the simplest case of a uniformly magnetized layer, this yields an unperturbed in situ frequency reference. We also discuss demagnetization contributions to measured shifts for this case. With a simple illustrative calculation, we show how a nonuniformly magnetized layer causes a strongly depth-dependent line broadening in an adjacent layer. We then give some experimental examples of resonance line broadening in heterostructures.

Local magnetic properties of a monolayer of Mn12 single molecule magnets.

The magnetic properties of a monolayer of Mn12 single molecule magnets grafted onto a silicon (Si) substrate have been investigated using depth-controlled beta-detected nuclear magnetic resonance. A low-energy beam of spin-polarized radioactive 8Li was used to probe the local static magnetic field distribution near the Mn12 monolayer in the Si substrate. The resonance line width varies strongly as a function of implantation depth as a result of the magnetic dipolar fields generated by the Mn12 electronic magnetic moments. The temperature dependence of the line width indicates that the magnetic properties of the Mn12 moments in this low-dimensional configuration differ from bulk Mn12.

Magnetic-field effects on the size of vortices below the surface of NbSe2 detected using low energy beta-NMR.

A low energy radioactive beam of polarized 8Li has been used to observe the vortex lattice near the surface of superconducting NbSe2. The inhomogeneous magnetic-field distribution associated with the vortex lattice was measured using depth-resolved beta-detected NMR. Below Tc, one observes the characteristic line shape for a triangular vortex lattice which depends on the magnetic penetration depth and vortex core radius. The size of the vortex core varies strongly with the magnetic field. In particular, in a low field of 10.8 mT, the core radius is much larger than the coherence length. The possible origin of these giant vortices is discussed.

beta-NMR of isolated lithium in nearly ferromagnetic palladium.

The temperature dependence of the frequency shift and spin-lattice relaxation rate of isolated, nonmagnetic (8)Li impurities implanted in a nearly ferromagnetic host (Pd) are measured by means of beta-detected nuclear magnetic resonance (beta-NMR). The shift is negative, very large, and increases monotonically with decreasing T in proportion to the bulk susceptibility of Pd for T > T* approximately 100 K. Below T*, an additional shift occurs which we attribute to the response of Pd to the defect. The relaxation rate is much slower than expected for the large shift and is linear with T below T*, showing no sign of additional relaxation mechanisms associated with the defect.

Near-surface structural phase transition of SrTiO3 studied with zero-field beta-detected nuclear spin relaxation and resonance.

We demonstrate that zero-field beta-detected nuclear quadrupole resonance and spin relaxation of low energy (8)Li can be used as a sensitive local probe of structural phase transitions near a surface. We find that the transition near the surface of a SrTiO(3) single crystal occurs at T(c) approximately 150K, i.e., approximately 45K higher than T(c)bulk, and that the tetragonal domains formed below T(c) are randomly oriented.

Local structure of isolated positively charged muonium as an analog for the hydrogen ion in p-type GaAs.

We determine the local structure of isolated positively charged muonium (Mu+) in heavily doped p-type GaAs based on muon level crossing resonance and zero applied field muon spin depolarization data. These measurements provide the first direct experimental confirmation that Mu+, and by analogy H+, is located within a stretched Ga-As bond. The distances between Mu+ and the nearest neighbor Ga and As atoms are estimated to be 1.83 +/- 0.10 A; and 1.76 +/- 0.10 A, respectively. These results are compared to existing theoretical calculations on the structure of hydrogen in GaAs and additionally provide data on the induced electric field gradients.

Depth-controlled beta-NMR of 8Li in a thin silver film.

Depth-controlled beta-NMR can be used to probe the magnetic properties of thin films and interfaces on a nanometer length scale. A 30 keV beam of highly spin-polarized 8Li+ ions was slowed down and implanted into a 50 nm film of Ag deposited on a SrTiO3 substrate. A novel high field beta-NMR spectrometer was used to observe two well resolved resonances which are attributed to Li occupying substitutional and octahedral interstitial sites in the Ag lattice. The temperature dependence of the Knight shifts and spin relaxation rates are consistent with the Korringa law for a simple metal, implying that the NMR of implanted 8Li reflects the spin suspectibility of bulk metallic silver.

Local magnetic susceptibility of the positive muon in the quasi-one-dimensional S=1/2 antiferromagnet dichlorobis (pyridine) copper (II).

We report muon spin rotation measurements of the local magnetic susceptibility around a positive muon in the paramagnetic state of the quasi-one-dimensional spin 1/2 antiferromagnet dichlorobis (pyridine) copper (II). Signals from three distinct sites are resolved and have a temperature dependent frequency shift which is significantly different than the magnetic susceptibility. This difference is attributed to a muon induced perturbation of the spin 1/2 chain. The obtained frequency shifts are compared with transfer matrix density-matrix renormalization-group numerical simulations.

Temperature dependence of the magnetic penetration depth in the vortex state of the pyrochlore superconductor, Cd2Re2O7.

We report transverse-field and zero-field muon spin rotation and relaxation studies of the superconducting rhenium oxide pyrochlore, Cd2Re2O7. Transverse-field measurements (H=0.007 T) show line broadening below T(c), which is characteristic of a vortex state, demonstrating conclusively the type-II nature of this superconductor. The penetration depth is seen to level off below about 400 mK (T/T(c) approximately 0.4), with a rather large value of lambda(T=0) approximately 7500 A. The temperature independent behavior below approximately 400 mK is consistent with a nodeless superconducting energy gap. Zero-field measurements indicate no static magnetic fields developing below the transition temperature.

Evidence for static magnetism in the vortex cores of ortho-II YBa2Cu3O6.50.

Evidence for static alternating magnetic fields in the vortex cores of underdoped YBa2Cu3O6+x is reported. Muon spin rotation measurements of the internal magnetic field distribution of the vortex state of YBa2Cu3O6.50 in applied fields of H = 1 T and H = 4 T reveal a feature in the high-field tail of the field distribution which is not present in optimally doped YBa2Cu3O6.95 and which fits well to a model with static magnetic fields in the vortex cores. The magnitude of the fields is estimated to be 18(2) G and decreases above T = 10 K. We discuss possible origins of the additional vortex core magnetism within the context of existing theories.

Muonium analog of hydrogen passivation: observation of the Mu+-Zn- reaction in GaAs.

We report direct detection of the formation and subsequent breakup of a complex containing positively charged muonium ( Mu+) and a substitutional Zn(Ga) acceptor in heavily doped p-type GaAs:Zn. Mu+ diffuses above 200 K with a hop rate nu = nu(0)e(-E(nu)/k(B)T) where nu(0) = (7.7+/-2.0)x10(8) s(-1) and E(nu) = 0.15(4) eV. Above 350 K, it forms the complex with a trapping radius of 500+/-200 A. The Mu-Zn complex breaks up above 550 K with a dissociation energy of 0.88(7) eV and prefactor of (5+/-4)x10(12) s(-1). Above 750 K, the cyclic reaction Mu+<--> Mu0 takes place.

Anomalous weak magnetism in superconducting YBa2Cu3O6+x.

For some time now, there has been considerable experimental and theoretical effort to understand the role of the normal-state "pseudogap" phase in underdoped high-temperature cuprate superconductors. Recent debate has centered on the question of whether the pseudogap is independent of superconductivity. We provide evidence from zero-field muon spin relaxation measurements in YBa2Cu3O6+x for the presence of small spontaneous static magnetic fields of electronic origin intimately related to the pseudogap transition. Our most significant finding is that, for optimal doping, these weak static magnetic fields appear well below the superconducting transition temperature. The two compositions measured suggest the existence of a quantum critical point somewhat above optimal doping.