Probing the strongly correlated magnetic state of Co2C nanoparticles at low temperatures usingµSR.

Co2C nanoparticles (NPs) are amongst transition metal carbides whose magnetic properties have not been well explored. An earlier study (Royet al2021J. Phys.: Condens. Matter33375804) showed that a pellet made from Co2C NPs exhibits exchange bias (EB) effect below a temperature,TEB= 50 K and a spin glass (SG) feature emerges belowTSG= 5 K. In the current study we use magnetic, electrical transport, specific heat, and muon spin rotation (µSR) measurements to explore further the magnetic properties of a pellet made with 40 nm diameter pure Co2C NPs. We uncover the onset of Kondo localization at Kondo temperatureTK(= 40.1 K), which is close to the onset temperature (TEB) of the EB effect. A crossover from the Kondo-screened scenario to the Ruderman-Kittel-Kasuya-Yosida interaction-dominated regime is also observed forT

Muons at ISIS.

For the last 30 years, muon experiments at ISIS pulsed neutron and muon facility at the Rutherford Appleton Laboratory, Oxfordshire have been making a significant contribution to a number of scientific fields. The muon facilities at ISIS consist of eight experimental areas. The European Commission Muon facility consists of three experimental areas with a fixed momentum (28 MeV c-1). The RIKEN-RAL facility has a variable momentum (17-90 MeV c-1) and a choice of negative or positive muons delivering muons to four experimental areas. There is also an area recently used for a muon ionization cooling experiment. In this paper, the ISIS pulsed muon facilities are reviewed, including the beam characteristics that could be useful for muography experiments.This article is part of the Theo Murphy meeting issue 'Cosmic-ray muography'.

Photoexcited Muon Spin Spectroscopy: A New Method for Measuring Excess Carrier Lifetime in Bulk Silicon.

We have measured excess carrier lifetime in silicon using photoexcited muon spin spectroscopy. Positive muons implanted deep in a wafer can interact with the optically injected excess carriers and directly probe the bulk carrier lifetime while minimizing the effect from surface recombination. The method is based on the relaxation rate of muon spin asymmetry, which depends on the excess carrier density. The underlying microscopic mechanism has been understood by simulating the four-state muonium model in Si under illumination. We apply the technique to different injection levels and temperatures, and demonstrate its ability for injection- and temperature-dependent lifetime spectroscopy.

Temporal mapping of photochemical reactions and molecular excited states with carbon specificity.

Photochemical reactions are essential to a large number of important industrial and biological processes. A method for monitoring photochemical reaction kinetics and the dynamics of molecular excitations with spatial resolution within the active molecule would allow a rigorous exploration of the pathway and mechanism of photophysical and photochemical processes. Here we demonstrate that laser-excited muon pump-probe spin spectroscopy (photo-µSR) can temporally and spatially map these processes with a spatial resolution at the single-carbon level in a molecule with a pentacene backbone. The observed time-dependent light-induced changes of an avoided level crossing resonance demonstrate that the photochemical reactivity of a specific carbon atom is modified as a result of the presence of the excited state wavefunction. This demonstrates the sensitivity and potential of this technique in probing molecular excitations and photochemistry.

The new high field photoexcitation muon spectrometer at the ISIS pulsed neutron and muon source.

A high power pulsed laser system has been installed on the high magnetic field muon spectrometer (HiFi) at the International Science Information Service pulsed neutron and muon source, situated at the STFC Rutherford Appleton Laboratory in the UK. The upgrade enables one to perform light-pump muon-probe experiments under a high magnetic field, which opens new applications of muon spin spectroscopy. In this report we give an overview of the principle of the HiFi laser system and describe the newly developed techniques and devices that enable precisely controlled photoexcitation of samples in the muon instrument. A demonstration experiment illustrates the potential of this unique combination of the photoexcited system and avoided level crossing technique.

Spin dynamics in Na(4-x)Ir3O8 (x = 0.3 and 0.7) investigated by ²³Na NMR and µSR.

We report (23)Na nuclear magnetic resonance (NMR) and zero-field (ZF) and longitudinal-field (LF) muon spin relaxation (µSR) measurements of the depleted hyperkagome compounds Na(4-x)Ir3O8 (x = 0.3 and 0.7), which undergo an insulator-semimetal transition as a function of x. The (23)Na spin-lattice relaxation rates, T1(-1), follow a T(2.5) power law behavior at accessible temperatures of T = 120-350 K. A substantial temperature dependence of T1(-1) indicates the presence of gapped excitations at elevated temperatures through the transition to a semimetallic phase. ZF-µSR results reveal that hole-doping leads to a melting of quasi-static order to a dynamically fluctuating state. The very slow muon depolarization rate which varies hardly with temperature indicates that spins are close to an itinerant limit in the largest doping x = 0.7. The dynamic relaxation rates extracted from the LF-µSR spectra show a three-dimensional diffusive transport. Our combined NMR and µSR results suggest the occurrence of intriguing spin and charge excitations across the insulator-semimetal transition.

Importance of spin-orbit interaction for the electron spin relaxation in organic semiconductors.

Despite the great interest organic spintronics has recently attracted, there is only a partial understanding of the fundamental physics behind electron spin relaxation in organic semiconductors. Mechanisms based on hyperfine interaction have been demonstrated, but the role of the spin-orbit interaction remains elusive. Here, we report muon spin spectroscopy and time-resolved photoluminescence measurements on two series of molecular semiconductors in which the strength of the spin-orbit interaction has been systematically modified with a targeted chemical substitution of different atoms at a particular molecular site. We find that the spin-orbit interaction is a significant source of electron spin relaxation in these materials.

Gapless spin liquid ground state in the S = 1/2 vanadium oxyfluoride kagome antiferromagnet [NH4]2[C7H14N][V7O6F18].

The vanadium oxyfluoride [NH(4)](2)[C(7)H(14)N][V(7)O(6)F(18)] (DQVOF) is a geometrically frustrated magnetic bilayer material. The structure consists of S = 1/2 kagome planes of V(4+) d(1) ions with S = 1 V(3+) d(2) ions located between the kagome layers. Muon spin relaxation measurements demonstrate the absence of spin freezing down to 40 mK despite an energy scale of 60 K for antiferromagnetic exchange interactions. From magnetization and heat capacity measurements we conclude that the S = 1 spins of the interplane V(3+) ions are weakly coupled to the kagome layers, such that DQVOF can be viewed as an experimental model for S = 1/2 kagome physics, and that it displays a gapless spin liquid ground state.

Design and commissioning of a high magnetic field muon spin relaxation spectrometer at the ISIS pulsed neutron and muon source.

The high magnetic field (HiFi) muon instrument at the ISIS pulsed neutron and muon source is a state-of-the-art spectrometer designed to provide applied magnetic fields up to 5 T for muon studies of condensed matter and molecular systems. The spectrometer is optimised for time-differential muon spin relaxation studies at a pulsed muon source. We describe the challenges involved in its design and construction, detailing, in particular, the magnet and detector performance. Commissioning experiments have been conducted and the results are presented to demonstrate the scientific capabilities of the new instrument.

Muonium chemistry and spin dynamics in sulphur, modelling interstitial hydrogen.

The nature of the elusive muonium centre in sulphur is re-examined in the light of new data on its level-crossing resonance and spin-lattice relaxation. The aim is to provide a model for the solid-state chemistry of interstitial hydrogen in this element, which is as yet unknown, as well as to solve one of the longest standing puzzles in µSR spectroscopy, namely the surprisingly strong depolarization of muons mimicking ion-implanted protons in this innocuous non-magnetic material. The paramagnetic muonium (and by inference hydrogen) centre is confirmed to have the character of a molecular radical, but with huge anisotropy at cryogenic temperatures and a striking shift of the resonance at ordinary temperatures, the hyperfine parameters appearing to collapse and vanish towards the melting point. New density-functional supercell calculations identify a number of possible structures for the defect centre, including a novel form of bond-centred muonium in a closed-ring S(8)Mu complex. Simulations of the spin dynamics and fits to the spectra suggest a dynamical equilibrium or chemical exchange between several configurations, with occupancy of the bond-centre site falling from unity at low cryogenic temperatures to zero near the melting point.

Dynamic fields in the partial magnetization plateau of Ca3Co2O6.

Fluctuation dynamics in magnetization plateaus is a relatively poorly explored area in frustrated magnetism. Here we use muon spin relaxation to determine the fluctuation timescale and associated field distribution width in the partial magnetization plateau of Ca(3)Co(2)O(6). The muon spin relaxation rate has a simple and characteristic field dependence which we model and, by fitting to the data at 15 K, we extract a fluctuation timescale τ = 880(30) ps and a field distribution width Δ = 40.6(3) mT. Comparison with previous results on Ca(3)Co(2)O(6) suggests that this fluctuation timescale can be associated with short-range, slowly fluctuating magnetic order.

Quantum magnetism in the paratacamite family: towards an ideal kagomé lattice.

We report muon spin rotation measurements on the S=1/2 (Cu2+) paratacamite ZnxCu4-x(OH)6Cl2 family. Despite a Weiss temperature of approximately -300 K, the x=1 compound is found to have no transition to a magnetic frozen state down to 50 mK as theoretically expected for the kagomé Heisenberg antiferromagnet. We find that the limit between a dynamical and a partly frozen ground state occurs around x=0.5. For x=1, we discuss the relevance to a singlet picture.

Muon spin rotation studies of spin dynamics at avoided level crossings in LiY0.998Ho0.002F4.

We have studied the Ho3+ spin dynamics for LiY0.998Ho0.002F4 via the positive muon (mu+) transverse field depolarization rate lambdaTF as a function of temperature and magnetic field. We find sharp minima in lambdaTF(H) at fields for which the Ho3+ ion system has field-induced (avoided) level crossings. The reduction scales with calculated level repulsions, suggesting that mu+ depolarization by slow fluctuations of nonresonant Ho3+ spin states is partly suppressed when resonant tunneling opens new fluctuation channels at frequencies much greater than the muon precession frequency.

Magnetic and electronic properties of Bi(0.75)Ca(0.25)MnO(3).

The magnetic, structural and electronic properties of Bi(0.75)Ca(0.25)MnO(3) have been investigated in comparison with those of Bi(0.75)Sr(0.25)MnO(3). Magnetometry, diffraction and muon spin relaxation (µSR) data confirm different structural, magnetic and electronic transitions in the two compounds. The anisotropic changes of cell parameters across the structural transition in Bi(0.75)Ca(0.25)MnO(3) (275 K) differ markedly from the lattice anomalies in Bi(0.75)Sr(0.25)MnO(3) (600 K) and also from those in Bi(0.50)Ca(0.50)MnO(3) (325 K). The ground state of Bi(0.75)Ca(0.25)MnO(3) is characterized by a high degree of spin disorder and frustrated interactions. There is no evidence of a ferromagnetic component in the ground state of Bi(0.75)Ca(0.25)MnO(3). However, the application of a magnetic field (even of a few gauss) produces a continuous progressive polarization of the Mn moments (≈2 µ(B)/Mn at 5 T, ZFC, 5 K). Differences between Ca and Sr perovskites with x = 1/4 are greater than for the x = 1/2 counterparts, and point to distinct ground states and charge/orbital configurations.

Experimental confirmation of the predicted shallow donor hydrogen state in zinc oxide.

We confirm the recent prediction that interstitial protium may act as a shallow donor in zinc oxide, by direct spectroscopic observation of its muonium counterpart. On implantation into ZnO, positive muons--chemically analogous to protons in this context--form paramagnetic centers below about 40 K. The muon-electron contact hyperfine interaction, as well as the temperature and activation energy for ionization, imply a shallow level. Similar results for the cadmium chalcogenides suggest that such shallow donor states are generic to the II-VI compounds. The donor level depths should serve as a guide for the electrical activity of interstitial hydrogen.