Scientific Highlights

Here we present a study of magnetism in Co_0.05Ti_0.95O_2−δ anatase films grown by pulsed laser deposition under a variety of oxygen partial pressures and deposition rates. Energy-dispersive spectrometry and transmission electron microscopy analyses indicate that a high deposition rate leads to a homogeneous microstructure, while a very low rate or postannealing results in cobalt clustering. Depth resolved low-energy muon spin rotation experiments show that films grown at a low oxygen partial pressure (≈10⁻⁶ torr) with a uniform structure are fully magnetic, indicating intrinsic ferromagnetism. First principles calculations identify the beneficial role of low oxygen partial pressure in the realization of uniform carrier-mediated ferromagnetism. This work demonstrates that Co:TiO₂ is an intrinsic diluted magnetic semiconductor.

By means of magnetization, specific heat, and muon-spin relaxation measurements, we investigate newly synthesized high-pressure oxidized Cu_0.75Mo_0.25Sr₂YCu₂O_7.54, in which overdoping is achieved up to p ˜ 0.46 hole/Cu, well beyond the T_c-p superconducting dome of cuprates, where Fermi-liquid behavior is expected. Surprisingly, we find bulk superconductivity with T_c = 84 K and superfluid density similar to those of optimally doped YBa₂Cu₃O_7-δ. On the other hand, specific heat data display a large electronic contribution at low temperature, comparable to that of nonsuperconducting overdoped La_2−xSr_xCuO₄. These results point at an unusual high-T_c phase with a large fraction of unpaired holes. Further experiments may assess the Fermi-liquid properties of the present phase, which would put into question the paradigm that the high T_c of cuprates originates from a non-Fermi-liquid ground state.

Pressure-induced ordering close to a z = 1 quantum-critical point is studied in the presence of bond disorder in the quantum spin system (C₄H₁₂N₂)Cu₂(Cl_1−xBr_x)₆ (PHCX) by means of muon-spin rotation and relaxation. As for the pure system (C₄H₁₂N₂)Cu₂Cl₆, pressure allows PHCX with small levels of disorder (x ≤ 7.5%) to be driven through a quantum-critical point separating a low-pressure quantum paramagnetic phase from magnetic order at high pressures. However, the pressure-induced ordered state is highly inhomogeneous for disorder concentrations x > 1%. This behavior might be related to the formation of a quantum Griffiths phase above a critical disorder concentration 7.5% < x_c < 15%. Br substitution increases the critical pressure and suppresses critical temperatures and ordered moment sizes.

RENiO₃ (RE=rare-earth element) and V₂O₃ are archetypal Mott insulator systems. When tuned by chemical substitution (RENiO₃) or pressure (V₂O₃), they exhibit a quantum phase transition (QPT) between an antiferromagnetic Mott insulating state and a paramagnetic metallic state. Because novel physics often appears near a Mott QPT, the details of this transition, such as whether it is first or second order, are important. Here, we demonstrate through muon spin relaxation/rotation (μSR) experiments that the QPT in RENiO₃ and V₂O₃ is first order: the magnetically ordered volume fraction decreases to zero at the QPT, resulting in a broad region of intrinsic phase separation, while the ordered magnetic moment retains its full value until it is suddenly destroyed at the QPT. These findings bring to light a surprising universality of the pressure-driven Mott transition, revealing the importance of phase separation and calling for further investigation into the nature of quantum fluctuations underlying the transition.

Unlike conventional magnets where the magnetic moments are partially or completely static in the ground state, in a quantum spin liquid they remain in collective motion down to the lowest temperatures. The importance of this state is that it is coherent and highly entangled without breaking local symmetries. In the case of magnets with isotropic interactions, spin-liquid behaviour is sought in simple lattices with antiferromagnetic interactions that favour antiparallel alignments of the magnetic moments and are incompatible with the lattice geometries. Despite an extensive search, experimental realizations remain very few. Here we investigate the novel, unexplored magnet Ca₁₀Cr₇O₂₈, which has a complex Hamiltonian consisting of several different isotropic interactions and where the ferromagnetic couplings are stronger than the antiferromagnetic ones. We show both experimentally and theoretically that it displays all the features expected of a quantum spin liquid. Thus spin-liquid behaviour in isotropic magnets is not restricted to the simple idealized models currently investigated, but can be compatible with complex structures and ferromagnetic interactions.

New exotic phenomena have recently been discovered in oxides of paramagnetic Ir⁴⁺ ions, widely known as ‘iridates’. Their remarkable properties originate from concerted effects of the crystal field, magnetic interactions and strong spin-orbit coupling, characteristic of 5d metal ions. Despite numerous experimental reports, the electronic structure of these materials is still challenging to elucidate, and not attainable in the isolated, but chemically inaccessible, [IrO₆]^8– species (the simplest molecular analogue of the elementary {IrO₆}^8– fragment present in all iridates). Here, we introduce an alternative approach to circumvent this problem by substituting the oxide ions in [IrO₆]^8– by isoelectronic fluorides to form the fluorido-iridate: [IrF₆]^2–. This molecular species has the same electronic ground state as the {IrO₆}^8– fragment, and thus emerges as an ideal model for iridates. These results may open perspectives for using fluorido-iridates as building-blocks for electronic and magnetic quantum materials synthesized by soft chemistry routes.

The temperature-pressure phase diagram of the ferromagnet LaCrGe₃ is determined for the first time from a combination of magnetization, muon-spin-rotation, and electrical resistivity measurements. The ferromagnetic phase is suppressed near 2.1 GPa, but quantum criticality is avoided by the appearance of a magnetic phase, likely modulated, AFM_Q. Our density functional theory total energy calculations suggest a near degeneracy of antiferromagnetic states with small magnetic wave vectors Q allowing for the potential of an ordering wave vector evolving from Q=0 to finite Q, as expected from the most recent theories on ferromagnetic quantum criticality. Our findings show that LaCrGe₃ is a very simple example to study this scenario of avoided ferromagnetic quantum criticality and will inspire further study on this material and other itinerant ferromagnets.

The organization of single-molecule magnets (SMMs) on surfaces via thermal sublimation is a prerequisite for the development of future devices for spintronics exploiting the richness of properties offered by these magnetic molecules. However, a change in the SMM properties due to the interaction with specific surfaces is usually observed. Here we present a rare example of a SMM system which can be thermally sublimated on gold surfaces while maintaining its intact chemical structure and magnetic properties. Muon spin relaxation and ac susceptibility measurements are used to demonstrate that, unlike other SMMs, the magnetic properties of this system in thin films are very similar to those in the bulk, throughout the full volume of the film, including regions near the metal and vacuum interfaces. These results exhibit the robustness of chemical and magnetic properties of this complex and provide important clues for the development of nanostructures based on SMMs.

We show using detailed magnetic and thermodynamic studies and theoretical calculations that the ground state of Ba₃ZnIr₂O₉ is a realization of a novel spin-orbital liquid state. Our results reveal that Ba₃ZnIr₂O₉ with Ir⁵⁺ (5d⁴) ions and strong spin-orbit coupling (SOC) arrives very close to the elusive J 1⁄4 0 state but each Ir ion still possesses a weak moment. Ab initio density functional calculations indicate that this moment is developed due to superexchange, mediated by a strong intradimer hopping mechanism. While the Ir spins within the structural Ir₂O₉ dimer are expected to form a spin-orbit singlet state (SOS) with no resultant moment, substantial frustration arising from interdimer exchange interactions induce quantum fluctuations in these possible SOS states favoring a spin-orbital liquid phase down to at least 100 mK.

The family of iron-based superconductors has recently acquired a new member material, FeS. Theoretically, this compound has been shown to have electronic structure similar to that of the superconducting FeSe. However, contradictory ground states have been predicted for FeS. In this work, a collaboration of authors from Switzerland and Germany use muon spin rotation and relaxation to show that weak-moment magnetism microscopically coexists with bulk superconductivity. Additionally, in contrast with some earlier studies, the results suggest a fully gapped superconducting state of FeS.

The transfer rate of a probe molecule across the interfacial layer of a water-in-oil (w/o) microemulsion was investigated using a combination of transverse field muon spin rotation (TF-μSR), avoided level crossing muon spin resonance (ALC-μSR), and Monte Carlo simulations. Reverse micro-emulsions consist of nanometer-sized water droplets dispersed in an apolar solvent separated by a surfactant monolayer. Although the thermodynamic, static model of these systems has been well described, our understanding of their dynamics is currently incomplete. For example, what is the rate of solute transfer between the aqueous and apolar solvents, and how this is influenced by the structure of the interface? With an appropriate choice of system and probe molecule, μSR offers a unique opportunity to directly probe these interfacial transfer dynamics.