Muons and magnets

Abstract:

Muons are particles with a spin of ½ that can be implanted into a wide range of condensed matter materials to act as a local probe of the surrounding atomic environment. Measurement of the muon’s precession and relaxation provides an insight into how it interacts with its local environment. From this, unique information is obtained about the static and dynamic properties of the material of interest. This has enabled muon spin spectroscopy, more commonly known as muon spin rotation/relaxation/resonance (μSR), to develop into a powerful tool to investigate material properties such as fundamental magnetism, superconductivity and functional materials. Alongside this, μSR may be used to study, for example, energy storage materials, ionic diffusion in potential batteries, the dynamics of soft matter, free radical chemistry, reaction kinetics, semiconductors, advanced manufacturing and cultural artefacts. This Primer is intended as an introductory article and introduces the μSR technique, the typical results obtained and some recent advances across various fields. Data reproducibility and limitations are also discussed, before highlighting promising future developments.

Abstract:

We present here a study of the magnetic properties of the antiferromagnetic dimer material CuVOF4(H2O)6·H2O, in which the dimer unit is composed of two different S=1/2 species, Cu(II) and V(IV). An applied magnetic field of μ0Hc1=13.1(1) T is found to close the singlet-triplet energy gap, the magnitude of which is governed by the antiferromagnetic intradimer J0≈21 K, and interdimer J′≈1 K, exchange energies, determined from magnetometry and electron-spin resonance measurements. The results of density functional theory (DFT) calculations are consistent with the experimental results. The DFT calculations predict antiferromagnetic coupling along all nearest-neighbor bonds, with the magnetic ground state comprising spins of different species aligning antiparallel to one another, while spins of the same species are aligned parallel. The magnetism in this system cannot be accurately described by the overlap between localized V orbitals and magnetic Cu orbitals lying in the Jahn-Teller (JT) plane, with a tight-binding model based on such a set of orbitals incorrectly predicting that interdimer exchange should be dominant. DFT calculations indicate significant spin density on the bridging oxide, suggesting instead an unusual mechanism in which intradimer exchange is mediated through the O atom on the Cu(II) JT axis.

Abstract:

Muons implanted into ionic fluorides often lead to a so-called F–μ–F state, in which the time evolution of the muon spin contains information about the geometry and nature of the muon site. Nuclei more distant from the muon than the two nearest-neighbor fluorine ions result in decoherence of the F–μ–F system, and this can yield additional quantitative information about the state of the muon. We demonstrate how this idea can be applied to the determination of muon sites within the ionic fluorides α-PbF2 and YF3, which contain fluoride ions in different crystallographic environments. Our results can be used to distinguish between different crystal phases and provide strong evidence for the existence of anion Frenkel defects in α-PbF2.

Abstract:

We present a systematic investigation of muon-stopping states in superconductors that reportedly exhibit spontaneous magnetic fields below their transition temperatures due to time-reversal symmetry breaking. These materials include elemental rhenium, several intermetallic systems, and Sr₂RuO₄. We demonstrate that the presence of the muon leads to only a limited and relatively localized perturbation to the local crystal structure, while any small changes to the electronic structure occur several electron volts below the Fermi energy, leading to only minimal changes in the charge density on ions close to the muon. Our results imply that the muon-induced perturbation alone is unlikely to lead to the observed spontaneous fields in these materials, whose origin is more likely intrinsic to the time-reversal symmetry-broken superconducting state.