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We report neutron scattering measurements, which reveal spin-liquid polymorphism in a 11 iron chalcogenide superconductor, a poorly-metallic magnetic FeTe tuned towards superconductivity by substitution of a small amount of Tellurium with iso-electro nic Sulphur. We observe liquid-like magnetic dynamics, which is described by a competition of two phases with different local structure, whose relative abundance depends on temperature. One is the ferromagnetic (FM) plaquette phase observed in the non-superconducting FeTe, which preserves the C$_4$ symmetry of the underlying square lattice and is favored at high temperatures. The other is the antiferromagnetic plaquette phase with broken C$_4$ symmetry, which emerges with doping and is predominant at low temperatures. These findings suggest a first-order liquid-liquid phase transition in the electronic spin system of FeTe$_{1-x}$(S,Se)$_x$. We thus discover remarkable new physics of competing spin liquid polymorphs in a correlated electron system approaching superconductivity. Our results facilitate an understanding of large swaths of recent experimental data in unconventional superconductors.
The anisotropic triangular lattice of the crednerite system Cu(Mn1-xCux)O2 is used as a basic model for studying the influence of spin disorder on the ground state properties of a two-dimensional frustrated antiferromagnet. Neutron diffraction measur ements show that the undoped phase (x=0) undergoes a transition to antiferromagnetic long-range order that is stabilized by a frustration-relieving structural distortion. Small deviation from the stoichiometric composition alters the magnetoelastic characteristics and reduces the effective dimensionality of the magnetic lattice. Upon increasing the doping level, the interlayer coupling changes from antiferromagnetic to ferromagnetic. As the structural distortion is suppressed, the long-range magnetic order is gradually transformed into a two-dimensional order.
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