Scientific Highlights

Transition metal dichalcogenides (TMDs) are interesting for understanding the fundamental physics of two-dimensional (2D) materials as well as for applications to many emerging technologies, including spin electronics. Here, we report the discovery of long-range magnetic order below T_M = 40 and 100 K in bulk semiconducting TMDs 2H-MoTe₂ and 2H-MoSe₂, respectively, by means of muon spin rotation (μSR), scanning tunneling microscopy (STM), and density functional theory (DFT) calculations. The μSR measurements show the presence of large and homogeneous internal magnetic fields at low temperatures in both compounds indicative of long-range magnetic order. DFT calculations show that this magnetism is promoted by the presence of defects in the crystal. The STM measurements show that the vast majority of defects in these materials are metal vacancies and chalcogen-metal antisites, which are randomly distributed in the lattice at the subpercent level. DFT indicates that the antisite defects are magnetic with a magnetic moment in the range of 0.9 to 2.8 μ_B. Further, we find that the magnetic order stabilized in 2H-MoTe₂ and 2H-MoSe₂ is highly sensitive to hydrostatic pressure. These observations establish 2H-MoTe₂ and 2H-MoSe₂ as a new class of magnetic semiconductors and open a path to studying the interplay of 2D physics and magnetism in these interesting semiconductors.

To trace the origin of time-reversal symmetry breaking (TRSB) in Re-based superconductors, we performed comparative muon-spin rotation and relaxation (μSR) studies of superconducting noncentro-symmetric Re_0.82Nb_0.18 (T_c=8.8 K) and centrosymmetric Re (T_c=2.7 K). In Re_0.82Nb_0.18, the low–temperature superfluid density and the electronic specific heat evidence a fully gapped superconducting state, whose enhanced gap magnitude and specific-heat discontinuity suggest a moderately strong electron- phonon coupling. In both Re_0.82Nb_0.18 and pure Re, the spontaneous magnetic fields revealed by zero-field μSR below T_c indicate time-reversal symmetry breaking and thus unconventional superconductivity. The concomitant occurrence of TRSB in centrosymmetric Re and noncentrosymmetric ReT (T=transition metal), yet its preservation in the isostructural noncentrosymmetric superconductors Mg₁₀Ir₁₉B₁₆ and Nb_0.5Os_0.5, strongly suggests that the local electronic structure of Re is crucial for understanding the TRSB superconducting state in Re and ReT. We discuss the superconducting order parameter symmetries that are compatible with the experimental observations.

GdPtBi and NdPtBi belong to the Heusler family of compounds and are conventional antiferromagnets below 9 and 2.1 K, respectively. We present evidence for magnetic-field–induced Weyl physics in these compounds, namely, a chiral anomaly (negative magnetoresistance) and an anomalous Hall effect (AHE) with a large anomalous Hall angle over a wide range of temperature. The AHE and chiral anomaly have a similar temperature dependence, indicating their common origin. These studies plus band structure calculations reveal that GdPtBi and NdPtBi develop Weyl points in the presence of an external magnetic field that arises from an exchange field. Our observations open the path to the realization of the quantum AHE in antiferromagnetic Heusler thin films.

Two-dimensional magnetic systems with continuous spin degrees of freedom exhibit a rich spectrum of thermal behaviour due to the strong competition between fluctuations and correlations. When such systems incorporate coupling via the anisotropic dipolar interaction, a discrete symmetry emerges, which can be spontaneously broken leading to a low-temperature ordered phase. However, the experimental realisation of such two-dimensional spin systems in crystalline materials is difficult since the dipolar coupling is usually much weaker than the exchange interaction. Here we realise two-dimensional magnetostatically coupled XY spin systems with nanoscale thermally active magnetic discs placed on square lattices. Using low-energy muon-spin relaxation and soft X-ray scattering, we observe correlated dynamics at the critical temperature and the emergence of static long-range order at low temperatures, which is compatible with theoretical predictions for dipolar-coupled XY spin systems. Furthermore, by modifying the sample design, we demonstrate the possibility to tune the collective magnetic behaviour in thermally active artificial spin systems with continuous degrees of freedom.

Muon spin relaxation (μSR) experiments on a single molecule magnet enriched in different Dy isotopes detect unambiguously a slowing down of the zero field spin dynamics for the non-magnetic isotope. This occurs in the low temperature regime dominated by quantum tunnelling, in agreement with previous ac susceptibility investigations. In contrast to the latter, however, μSR is sensitive to all fluctuation modes affecting the lifetime of the spin levels.

We have observed the spatial distribution of magnetic flux in Nb, Cu/Nb, and Cu/Nb/Co thin films using muon-spin rotation. In an isolated 50-nm-thick Nb film, we find a weak flux expulsion (Meissner effect) which becomes significantly enhanced when adding an adjacent 40 nm layer of Cu. The added Cu layer exhibits a Meissner effect (due to induced superconducting pairs) and is at least as effective as the Nb to expel flux. These results are confirmed by theoretical calculations using the quasiclassical Green’s function formalism. An unexpected further significant enhancement of the flux expulsion is observed when adding a thin (2.4 nm) ferromagnetic Co layer to the bottom side of the Nb. This observed cooperation between superconductivity and ferromagnetism, by an unknown mechanism, forms a key ingredient for developing superconducting spintronics.

Temperature-pressure phase diagram of the Kitaev hyperhoneycomb iridate β-Li₂IrO₃ is explored using magnetization, thermal expansion, magnetostriction, and muon spin rotation measurements, as well as single-crystal x-ray diffraction under pressure and ab initio calculations. The Néel temperature of β-Li₂IrO₃ increases with the slope of 0.9 K/GPa upon initial compression, but the reduction in the polarization field H_c reflects a growing instability of the incommensurate order. At 1.4 GPa, the ordered state breaks down upon a first-order transition, giving way to a new ground state marked by the coexistence of dynamically correlated and frozen spins. This partial freezing in the absence of any conspicuous structural defects may indicate the classical nature of the resulting pressure-induced spin liquid, an observation paralleled to the increase in the nearest-neighbor off-diagonal exchange Γ under pressure.

A quantum spin liquid state has long been predicted to arise in spin-1/2 Heisenberg square-lattice antiferromagnets at the boundary region between Néel (nearest-neighbor interaction dominates) and columnar (next-nearest-neighbor interaction dominates) antiferromagnetic order. However, there are no known compounds in this region. Here we use d¹⁰ – d⁰ cation mixing to tune the magnetic interactions on the square lattice while simultaneously introducing disorder. We find spin-liquid-like behavior in the double perovskite Sr₂Cu(Te_0.5W_0.5)O₆, where the isostructural end phases Sr₂CuTeO₆ and Sr₂CuWO₆ are Néel and columnar type antiferromagnets, respectively. We show that magnetism in Sr₂Cu(Te_0.5W_0.5)O₆ is entirely dynamic down to 19 mK. Additionally, we observe at low temperatures for Sr₂Cu(Te_0.5W_0.5)O₆ - similar to several spin liquid candidates—a plateau in muon spin relaxation rate and a strong T-linear dependence in specific heat. Our observations for Sr₂Cu(Te_0.5W_0.5)O₆ highlight the role of disorder in addition to magnetic frustration in spin liquid physics.

High carrier density quantum wells embedded within a Mott insulating matrix present a rich arena for exploring unconventional electronic phase behavior ranging from non-Fermi-liquid transport and signatures of quantum criticality to pseudogap formation. Probing the proposed connection between unconventional magnetotransport and incipient electronic order within these quantum wells has however remained an enduring challenge due to the ultra-thin layer thicknesses required. Here we address this challenge by exploring the magnetic properties of high-density SrTiO₃ quantum wells embedded within the antiferromagnetic Mott insulator SmTiO₃ via muon spin relaxation and polarized neutron reflectometry measurements. The one electron per planar unit cell acquired by the nominal d⁰ band insulator SrTiO₃ when embedded within a d¹ Mott SmTiO₃ matrix exhibits slow magnetic fluctuations that begin to freeze into a quasistatic spin state below a critical temperature T^*. The appearance of this quasistatic well magnetism coincides with the previously reported opening of a pseudogap in the tunneling spectra of high carrier density wells inside this film architecture. Our data suggest a common origin of the pseudogap phase behavior in this quantum critical oxide heterostructure with those observed in bulk Mott materials close to an antiferromagnetic instability.