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CrI 3 has raised as an important system to the emergent field of two-dimensional van der Waals magnetic materials. However, it is still unclear why CrI 3 which has a ferromagnetic rhombohedral structure in bulk, changed to anti-ferromagnetic monoclinic at thin layers. Here we show that this behaviour is due to the coexistence of both monoclinic and rhombohedral crystal phases followed by three magnetic transitions at T C1  = 61 K, T C2  = 50 K and T C3  = 25 K. Each transition corresponds to a certain fraction of the magnetically ordered volume as well as monoclinic and rhombohedral proportion. The different phases are continuously accessed as a function of the temperature over a broad range of magnitudes. Our findings suggest that the challenge of understanding the magnetic properties of thin layers CrI 3 is in general a coexisting structural-phase problem mediated by the volume-wise competition between magnetic phases already present in bulk. CrI 3 is a popular van der Waals magnet that exhibits anomalous magnetic properties between bulk and thin layers due to different crystal symmetry. Here, the authors report the coexistence of different magnetostructural phases over the entire range of temperatures, solving a long-standing puzzle.

The van-der-Waals material CrSBr stands out as a promising two-dimensional magnet. Here, we report on its detailed magnetic and structural characteristics. We evidence that it undergoes a transition to an A-type antiferromagnetic state below T N  ≈ 140 K with a pronounced two-dimensional character, preceded by ferromagnetic correlations within the monolayers. Furthermore, we unravel the low-temperature hidden-order within the long-range magnetically-ordered state. We find that it is associated to a slowing down of the magnetic fluctuations, accompanied by a continuous reorientation of the internal field. These take place upon cooling below T s  ≈ 100 K, until a spin freezing process occurs at T * ≈ 40 K. We argue this complex behavior to reflect a crossover driven by the in-plane uniaxial anisotropy, which is ultimately caused by its mixed-anion character. Our findings reinforce CrSBr as an important candidate for devices in the emergent field of two-dimensional magnetic materials. A 2D magnet CrSBr has attracted interest for applications in spintronics due to its high critical temperature and interesting magneto-electrical properties. Here the authors report a detailed study of its magnetic and structural phases and uncover a hidden magnetic order inside the magnetically-ordered phase.

The recently discovered kagome superconductor CsV3Sb5 (Tc ≃ 2.5 K) has been found to host charge order as well as a non-trivial band topology, encompassing multiple Dirac points and probable surface states. Such a complex and phenomenologically rich system is, therefore, an ideal playground for observing unusual electronic phases. Here, we report anisotropic superconducting properties of CsV3Sb5 by means of transverse-field muon spin rotation (μSR) experiments. The fits of temperature dependences of in-plane and out-of-plane components of the magnetic penetration depth suggest that the superconducting order parameter may have a two-gap (s + s)-wave symmetry. The multiband nature of superconductivity could be further supported by the different temperature dependences of the anisotropic magnetic penetration depth γλ(T) and upper critical field γBc2(T). The relaxation rates obtained from zero field μSR experiments do not show noticeable change across the superconducting transition, indicating that superconductivity does not break time reversal symmetry.

Strontium ruthenate (Sr2RuO4) continues to present an important test of our understanding of unconventional superconductivity, because while its normal-state electronic structure is known with precision, its superconductivity remains unexplained. There is evidence that its order parameter is chiral, but reconciling this with recent observations of the spin part of the pairing requires an order parameter that is either finely tuned or implies a new form of pairing. Therefore, a definitive resolution of whether the superconductivity of Sr2RuO4 is chiral is important for the study of superconductivity. Here we report the measurement of zero-field muon spin relaxation—a probe sensitive to weak magnetism—on samples under uniaxial stresses. We observe stress-induced splitting between the onset temperatures of superconductivity and time-reversal symmetry breaking—consistent with the qualitative expectations for a chiral order parameter—and argue that this observation cannot be explained by conventional magnetism. In addition, we report the appearance of bulk magnetic order under higher uniaxial stress, above the critical pressure at which a Lifshitz transition occurs in Sr2RuO4.When strain is applied to strontium ruthenate, superconductivity emerges at a different temperature to the breaking of time-reversal symmetry. This indicates that the superconductivity could have a chiral d-wave order parameter.

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 Ca 10 Cr 7 O 28 , 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. A detailed and systematic study of Ca 10 Cr 7 O 28 reveals all the hallmarks of spin-liquid behaviour, in spite of the compound’s unusually complex structure.

By harnessing the charge transfer that takes place at the interface between a metal and a layer of molecules, the usually non-magnetic materials copper and manganese are made magnetic at room temperature. Designer magnetism in copper and manganese This paper shows that thin films of non-magnetic metals such as copper and manganese can be made magnetic at room temperature by harnessing the charge transfer that takes place at the interface between the metal and a layer of molecules. Such a strategy potentially broadens the range of materials that could be used for magnetic and spintronic devices. Only three elements are ferromagnetic at room temperature: the transition metals iron, cobalt and nickel. The Stoner criterion explains why iron is ferromagnetic but manganese, for example, is not, even though both elements have an unfilled 3 d shell and are adjacent in the periodic table: according to this criterion, the product of the density of states and the exchange integral must be greater than unity for spontaneous spin ordering to emerge 1 , 2 . Here we demonstrate that it is possible to alter the electronic states of non-ferromagnetic materials, such as diamagnetic copper and paramagnetic manganese, to overcome the Stoner criterion and make them ferromagnetic at room temperature. This effect is achieved via interfaces between metallic thin films and C 60 molecular layers. The emergent ferromagnetic state exists over several layers of the metal before being quenched at large sample thicknesses by the material’s bulk properties. Although the induced magnetization is easily measurable by magnetometry, low-energy muon spin spectroscopy 3 provides insight into its distribution by studying the depolarization process of low-energy muons implanted in the sample. This technique indicates localized spin-ordered states at, and close to, the metal–molecule interface. Density functional theory simulations suggest a mechanism based on magnetic hardening of the metal atoms, owing to electron transfer 4 , 5 . This mechanism might allow for the exploitation of molecular coupling to design magnetic metamaterials using abundant, non-toxic components such as organic semiconductors. Charge transfer at molecular interfaces may thus be used to control spin polarization or magnetization, with consequences for the design of devices for electronic, power or computing applications (see, for example, refs 6 and 7 ).

Manipulating the spin state of thin layers of superconducting material is a promising route to generate dissipationless spin currents in spintronic devices. Approaches typically focus on using thin ferromagnetic elements to perturb the spin state of the superconducting condensate to create spin-triplet correlations. We have investigated simple structures that generate spin-triplet correlations without using ferromagnetic elements. Scanning tunneling spectroscopy and muon-spin rotation are used to probe the local electronic and magnetic properties of our hybrid structures, demonstrating a paramagnetic contribution to the magnetization that partially cancels the Meissner screening. This spin-orbit generated magnetization is shown to derive from the spin of the equal-spin pairs rather than from their orbital motion and is an important development in the field of superconducting spintronics. The authors study a Pt/Nb hybrid structure by scanning microscopy and muon spin rotation. They find an anomalous absence of Meissner screening near the Pt/Nb interface due to spin-triplet pair correlations driven by spin-orbit coupling alone with no ferromagnetic layer necessary.

The charge ordered structure of ions and vacancies characterizing rare-earth pyrochlore oxides serves as a model for the study of geometrically frustrated magnetism. The organization of magnetic ions into networks of corner-sharing tetrahedra gives rise to highly correlated magnetic phases with strong fluctuations, including spin liquids and spin ices. It is an open question how these ground states governed by local rules are affected by disorder. Here we demonstrate in the pyrochlore Tb 2 Hf 2 O 7 , that the vicinity of the disordering transition towards a defective fluorite structure translates into a tunable density of anion Frenkel disorder while cations remain ordered. Quenched random crystal fields and disordered exchange interactions can therefore be introduced into otherwise perfect pyrochlore lattices of magnetic ions. We show that disorder can play a crucial role in preventing long-range magnetic order at low temperatures, and instead induces a strongly fluctuating Coulomb spin liquid with defect-induced frozen magnetic degrees of freedom. Experimental studies of frustrated spin systems such as pyrochlore magnetic oxides test our understanding of quantum many-body physics. Here the authors show experimentally that Tb 2 Hf 2 O 7 may be a model material for investigating how structural disorder can stabilize a quantum spin liquid phase.

Two-dimensional (2D) kagome lattice metals are interesting because their corner sharing triangle structure enables a wide array of electronic and magnetic phenomena. Recently, post-growth annealing is shown to both suppress charge density wave (CDW) order and establish long-range CDW with the ability to cycle between states repeatedly in the kagome antiferromagnet FeGe. Here we perform transport, neutron scattering, scanning transmission electron microscopy (STEM), and muon spin rotation ( μ SR) experiments to unveil the microscopic mechanism of the annealing process and its impact on magneto-transport, CDW, and magnetism in FeGe. Annealing at 560 °C creates uniformly distributed Ge vacancies, preventing the formation of Ge-Ge dimers and thus CDW, while 320 °C annealing concentrates vacancies into stoichiometric FeGe regions with long-range CDW. The presence of CDW order greatly affects the anomalous Hall effect, incommensurate magnetic order, and spin-lattice coupling in FeGe, placing FeGe as the only kagome lattice material with tunable CDW and magnetic order. FeGe is an antiferromagnetic kagome metal with a rich magnetic and electronic phase diagram. Recently it was found that post-growth annealing of FeGe can suppress or induce charge density wave order depending on the annealing temperature. Here, Klemm, Siddique et al show the critical role that annealing induced Ge-vacancies and stacking faults play in the formation of charge density wave order in FeGe.

The interplay between superconductivity and charge or spin order is a key focus in condensed matter physics, with kagome lattice systems providing unique insights. The kagome superconductor LaRu 3 Si 2 ( T c  ≃ 6.5 K) features a characteristic kagome band structure and a hierarchy of charge order transitions at T co,I  ≃ 400 K and T co,II  ≃ 80 K, along with an additional transition at T * ≃ 35 K associated with electronic and magnetic responses. Using magnetotransport under pressure up to 40 GPa, we find T c peaks at 9 K (2 GPa)—the highest among kagome superconductors—remains nearly constant up to 12 GPa, and then decreases to 2 K at 40 GPa, forming a dome-shaped phase diagram. Similarly, both the resistivity anomaly at T * and the magnetoresistance exhibit a dome-shaped pressure dependence. Moreover, above 12 GPa, X-ray diffraction reveals that the charge order evolves from long-range to short-range, coinciding with the suppression of T c . These observations indicate that superconductivity in LaRu 3 Si 2 is closely linked to the charge-ordered state and the electronic responses at T co,II and T *. The authors study kagome superconductor LaRu3Si2 under pressure up to 40 GPa. They find a superconducting dome as a function of pressure, with Tc reaching its maximum when the coexisting charge order remains long-range.