Interweaving Polar Charge Orders in a Layered Metallic Super-atomic Crystal

Abstract

Electronic properties of super-atomic crystals have not been sufficiently explored due to the versatility of their building units; moreover, their inter-unit couplings are even poorly understood. Here, we present a joint experiment-theory investigation of a rational-designed layered super-atomic crystal of Au6Te12Se8 cubes, stacked by non-covalent inter-cube quasi-bonds. We found a sequential-emerged anisotropic triple-cube charge-density-wave (tc-CDW) and polarized metallic states below 120 K, as revealed via scanning tunneling microscopy/spectroscopy, angle-resolved photoemission spectroscopy, transport measurement, Raman spectra, and density functional theory. The polarized states are locked in an anti-parallel configuration, which is required for maintaining the inversion symmetry of the center-cube in the tc-CDW. The anti-polar metallic states are thus interweaved by the charge-density-wave and the polarized metallic states, and primarily ascribed to electronic effects via theoretical calculations. This work not only demonstrates a microscopic picture of the interweaved CDW and polarized charge orders in the super-atomic crystal of ATS, but also sheds light on expanding the existing category of quantum materials to non-covalent solids.