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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.

Cooperative effects determine the spin-state bistability of spin-crossover molecules (SCMs). Herein, the ultimate scale limit at which cooperative spin switching becomes effective is investigated in a complex [Fe(H 2 B(pz) 2 ) 2 (bipy)] deposited on a highly oriented pyrolytic graphite surface, using x-ray absorption spectroscopy. This system exhibits a complete thermal- and light-induced spin transition at thicknesses ranging from submonolayers to multilayers. On increasing the coverage from 0.35(4) to 10(1) monolayers, the width of the temperature-induced spin transition curve narrows significantly, evidencing the buildup of cooperative effects. While the molecules at the submonolayers exhibit an apparent anticooperative behavior, the multilayers starting from a double-layer exhibit a distinctly cooperative spin switching, with a free-molecule-like behavior indicated at around a monolayer. These observations will serve as useful guidelines in designing SCM-based devices. Spin-crossover molecules offer a potential route towards molecular spintronics, but retaining the bistability of the spin state upon surface deposition is challenging. Here, the authors study the spin-crossover behaviours of an Fe(II) complex deposited on graphite, determining the scale limit at which cooperative spin switching becomes effective.

The random fluctuations of spins give rise to many interesting physical phenomena, such as the ‘order-from-disorder’ arising in frustrated magnets and unconventional Cooper pairing in magnetic superconductors. Here we show that the exchange of spin waves between extended topological defects, such as domain walls, can result in novel magnetic states. We report the discovery of an unusual incommensurate phase in the orthoferrite TbFeO 3 using neutron diffraction under an applied magnetic field. The magnetic modulation has a very long period of 340 Å at 3 K and exhibits an anomalously large number of higher-order harmonics. These domain walls are formed by Ising-like Tb spins. They interact by exchanging magnons propagating through the Fe magnetic sublattice. The resulting force between the domain walls has a rather long range that determines the period of the incommensurate state and is analogous to the pion-mediated Yukawa interaction between protons and neutrons in nuclei. The interaction between spins in magnetic materials gives rise to a number of interesting effects. An example is the discovery of an unusual magnetic state based on a long-range ordering force between magnetic domain walls that is analogous to the interaction between protons and neutrons in atomic nuclei.

Ferrimagnetic alloys are extensively studied for their unique magnetic properties leading to possible applications in perpendicular magnetic recording, due to their deterministic ultrafast switching and heat assisted magnetic recording capabilities. On a prototype ferrimagnetic alloy we demonstrate fascinating properties that occur close to a critical temperature where the magnetization is vanishing, just as in an antiferromagnet. From the X-ray magnetic circular dichroism measurements, an anomalous ‘wing shape’ hysteresis loop is observed slightly above the compensation temperature. This bears the characteristics of an intrinsic exchange bias effect, referred to as atomic exchange bias . We further exploit the X-ray magnetic linear dichroism (XMLD) contrast for probing non-collinear states which allows us to discriminate between two main reversal mechanisms, namely perpendicular domain wall formation versus spin-flop transition. Ultimately, we analyze the elemental magnetic moments for the surface and the bulk parts, separately, which allows to identify in the phase diagram the temperature window where this effect takes place. Moreover, we suggests that this effect is a general phenomenon in ferrimagnetic thin films which may also contribute to the understanding of the mechanism behind the all optical switching effect.

The random fluctuations of spins give rise to many interesting physical phenomena, such as the 'order-from-disorder' arising in frustrated magnets and unconventional Cooper pairing in magnetic superconductors. Here we show that the exchange of spin waves between extended topological defects, such as domain walls, can result in novel magnetic states. We report the discovery of an unusual incommensurate phase in the orthoferrite TbFeO sub(3) using neutron diffraction under an applied magnetic field. The magnetic modulation has a very long period of 340Aa at 3K and exhibits an anomalously large number of higher-order harmonics. These domain walls are formed by Ising-like Tb spins. They interact by exchanging magnons propagating through the Fe magnetic sublattice. The resulting force between the domain walls has a rather long range that determines the period of the incommensurate state and is analogous to the pion-mediated Yukawa interaction between protons and neutrons in nuclei.

Ferrimagnetic alloys are extensively studied for their unique magnetic properties leading to possible applications in perpendicular magnetic recording, due to their deterministic ultrafast switching and heat assisted magnetic recording capabilities. On a prototype ferrimagnetic alloy we demonstrate fascinating properties that occur close to a critical temperature where the magnetization is vanishing, just as in an antiferromagnet. From the X-ray magnetic circular dichroism measurements, an anomalous 'wing shape' hysteresis loop is observed slightly above the compensation temperature. This bears the characteristics of an intrinsic exchange bias effect, referred to as atomic exchange bias. We further exploit the X-ray magnetic linear dichroism (XMLD) contrast for probing non-collinear states which allows us to discriminate between two main reversal mechanisms, namely perpendicular domain wall formation versus spin-flop transition. Ultimately, we analyze the elemental magnetic moments for the surface and the bulk parts, separately, which allows to identify in the phase diagram the temperature window where this effect takes place. Moreover, we suggests that this effect is a general phenomenon in ferrimagnetic thin films which may also contribue to the understanding of the mechanism behind the all optical switching effect.

Cubic chiral magnets, such as Cu\\(_{2}\\)OSeO\\(_{3}\\), exhibit a variety of non-collinear spin textures, including a trigonal lattice of spin whirls, so-called skyrmions. Using magnetic resonant elastic x-ray scattering (REXS) on a crystalline Bragg peak and its magnetic satellites while exciting the sample with magnetic fields at GHz frequencies, we probe the ferromagnetic resonance modes of these spin textures by means of the scattered intensity. Most notably, the three eigenmodes of the skyrmion lattice are detected with large sensitivity. As this novel technique, which we label REXS-FMR, is carried out at distinct positions in reciprocal space, it allows to distinguish contributions originating from different magnetic states, providing information on the precise character, weight and mode mixing as a prerequisite of tailored excitations for applications.

A spin liquid is a new state of matter with topological order where the spin moments continue to fluctuate coherently down to the lowest temperatures rather than develop static long-range magnetic order as found in conventional magnets. For spin liquid behavior to arise in a material the magnetic Hamiltonian must be \"frustrated\" where the combination of lattice geometry, interactions and anisotropies gives rise to competing spin arrangements in the ground state. Theoretical Hamiltonians which produce spin liquids are spin ice, the Kitaev honeycomb model and the Heisenberg kagome antiferromagnet. Spin liquid behavior however in real materials is rare because they can only approximate these Hamiltonians and often have weak higher order terms that destroy the spin liquid state. Ca10Cr7O28 is a new quantum spin liquid with magnetic Cr5+ ions that possess quantum spin number S=1/2. The spins are entirely dynamic in the ground state and the excitation spectrum is broad and diffuse as is typical of spinons which are the excitations of a spin liquid. In this paper we determine the Hamiltonian of Ca10Cr7O28 using inelastic neutron scattering under high magnetic field to induce a ferromagnetic ground state and spin-wave excitations that can be fitted to extract the interactions. We further explore the phase diagram by using inelastic neutron scattering and heat capacity measurements and establish the boundaries of the spin liquid phase as a function of magnetic field and temperature. Our results show that Ca10Cr7O28 consists of distorted kagome bilayers with several isotropic ferromagnetic and antiferromagnetic interactions where unexpectedly the ferromagnetic interactions are stronger than the antiferromagnetic ones. This complex Hamiltonian does not correspond to any known spin liquid model and points to new directions in the search for quantum spin liquid behavior.

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. Such phenomena is usually sought in simple lattices where antiferromagnetic interactions and/or anisotropies that favor specific alignments of the magnetic moments are \"frustrated\" by lattice geometries incompatible with such order e.g. triangular structures. Despite an extensive search among such compounds, experimental realizations remain very few. Here we describe the investigation of a novel, unexplored magnetic system consisting of strong ferromagnetic and weaker antiferromagnetic isotropic interactions as realized by the compound Ca\\(_{10}\\)Cr\\(_7\\)O\\(_{28}\\). Despite its exotic structure we show both experimentally and theoretically that it displays all the features expected of a quantum spin liquid including coherent spin dynamics in the ground state and the complete absence of static magnetism.

We present new experimental low-temperature heat capacity and detailed dynamical spin-structure factor data for the quantum spin liquid candidate material Ca\\(_{10}\\)Cr\\(_7\\)O\\(_{28}\\). The measured heat capacity shows an almost perfect linear temperature dependence in the range \\(0.1\\) K \\(\\lesssim T\\lesssim0.5\\) K, reminiscent of fermionic spinon degrees of freedom. The spin structure factor exhibits two energy regimes of strong signal which display rather different but solely diffuse scattering features. We theoretically describe these findings by an effective spinon hopping model which crucially relies on the existence of strong ferromagnetically coupled triangles in the system. Our spinon theory is shown to naturally reproduce the overall weight distribution of the measured spin structure factor. Particularly, we argue that various different observed characteristic properties of the spin structure factor and the heat capacity consistently indicate the existence of a spinon Fermi surface. A closer analysis of the heat capacity at the lowest accessible temperatures hints towards the presence of weak \\(f\\)-wave spinon pairing terms inducing a small partial gap along the Fermi surface (except for discrete nodal Dirac points) and suggesting an overall \\(\\mathbb{Z}_2\\) quantum spin liquid scenario for Ca\\(_{10}\\)Cr\\(_7\\)O\\(_{28}\\).