Abstract
The structural and electronic properties of high-quality K0.66(6)Fe1.75(10)S2 single crystals have been investigated by angle-resolved X-ray diffraction and 57Fe nuclear forward scattering using synchrotron radiation under pressure at room temperature. The samples exhibit phase separation into antiferromagnetic ordered K2Fe4S5 and nonmagnetic KxFe2S2 phases. It was found that a pressure-induced phase transition occurs at pc = 5.9(4) GPa with simultaneous suppression of the antiferromagnetic and Fe vacancy orders. From the results of 57Fe nuclear forward scattering, the refined magnetic hyperfine field remains unchanged with pressure below pc, suggesting that the Neel temperature does not decrease with pressure up to pc. Above pc, all Fe atoms in K0.66Fe1.75S2 are in the same nonmagnetic state. A discontinuous increase in the center shift was observed at pc, reflecting a change in the Fe electronic state in K0.66Fe1.75S2.
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