Interweaving Polar Charge Orders in a Layered Metallic Superatomic Crystal

Abstract

Electronic properties of superatomic crystals have not been sufficiently explored due to the versatility of their building units; moreover, their interunit couplings are even poorly understood. Here, we present a joint experiment-theory investigation of a rationally designed layered superatomic crystal of Au_{6}Te_{12}Se_{8} (ATS) cubes stacked by noncovalent intercube quasibonds. We find a sequential-emerged anisotropic triple-cube charge density wave (TCCDW) and polarized metallic states below 120 K, as revealed via scanning tunneling microscopy and spectroscopy, angle-resolved photoemission spectroscopy, transport measurement, Raman spectra, and density-functional theory. The polarized states are locked in an antiparallel configuration, which is required for maintaining the inversion symmetry of the center cube in the TCCDW. The antipolar metallic states are thus interweaved by the CDW 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 superatomic crystal of ATS, but also sheds light on expanding the existing category of quantum materials to noncovalent solids.