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 Ca10Cr7O28. 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.A quantum spin liquid is a macroscopic lattice of interacting magnetic ions with quantum spin number S=½, whose ground state has no static long-range magnetic order, instead the magnetic moments fluctuate coherently down to the lowest temperatures [1, 2]. It contrasts with the static long-range magnetically ordered ground states usually observed, and also with spin glass states where the spins are frozen into static short-range ordered configurations [3]. The excitations are believed to be spinons which have fractional quantum spin number S=½, and are very different from spin-waves or magnons that possess quantum spin number S=1 and are the characteristic excitations of conventional magnets. Spin liquids exist in one-dimensional magnets and the chain of spin-½ magnetic ions coupled by nearestneighbor, Heisenberg (isotropic), antiferromagnetic interactions is a well-established example [4]. This system has no static long-range magnetic order and the excitations are spinons. There is no energetic reason for the spinons to bind together, indeed if a spin-1 excitation is created e.g. by reversing a spin in the chain, it fractionalizes into two spin-½ spinons [5][6][7][8][9][10][11][12].The existence of spin liquids in dimensions greater than one is much less established. While static order does not occur in one-dimensional magnets, conventional two-and three-dimensional magnets order at temperatures at or above zero Kelvin [13]. This order can be suppressed by introducing competition (known as frustration) between the interactions that couple the magnetic ions. Geometrical frustration is achieved when the magnetic ions are located on lattices constructed from triangular motifs and are coupled by antiferromagnetic interactions. The antiferromagnetic coupling favors antiparallel spin alignment between nearest neighbor spins which can never be fully satisfied since the number of spins around the triangle is odd. This typically leads to h...

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 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 candidate with magnetic Cr 5+ 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 field polarized paramagnetic 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. INTRODUCTIONConventional magnets in condensed matter typically develop long-range magnetic order when cooled to low temperatures [1]. Below their ordering temperature the magnetic moments develop a static component which acts as the order parameter for the phase transition and the spin ordering is observable as magnetic Bragg peaks which characterize the type of order. The excitations are usually spin-waves which are collective oscillations of the spins about their ordering directions. The transition can be described by Landau theory where symmetry is broken and the new phase is characterized by a local order parameter [2].It was recently realized that some states of matter are characterized by topological order, rather than by symmetry breaking and a local order parameter [3]. This important discovery promises new, exotic and potentially useful properties that could be of relevance e.g. to information technologies. For example topological order gives rise to coherent states which can be highly robust to the usual perturbations that destroy coherence in ordinary states due to the non-local nature of their correlations.One potential applicati...

A detailed diffraction study of Ca10Cr7O28 is presented which adds significant new insights into the structural and magnetic properties of this compound. A new crystal structure type was used where the a and b axes are doubled compared to previous models providing a more plausible structure where all crystallographic sites are fully occupied. The presence of two different valences of chromium was verified and the locations of the magnetic Cr 5+ and non-magnetic Cr 6+ ions were identified. The Cr 5+ ions have spin-1 /2 and form distorted kagome bilayers which are stacked in an ABC arrangement along the c axis. These results lay the foundation for understanding of the quantum spin liquid behavior in Ca10Cr7O28 which has recently been reported in [C. Balz et al., Nature Physics, 12, 942 (2016)].

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This corrects the article DOI: 10.1103/PhysRevLett.116.147201.