Emerging correlated charge orders in a layered super-atomic crystal

Synthesis of emergent crystals is the foundation of discovering novel phenomena and exploring intriguing properties. Comparing to the diverse exotic quantum states of covalent crystals, the unique super-atomic crystals are far from being extensively investigated in the case of their versatile superatoms (building blocks) and inter-superatom coupling (noncovalent interactions). Here, we investigate the correlated electronic structures in the layered super-atomic crystal of AuTe2Se4/3 (ATS), which can be assumed as three-dimensional triclinic stacking of the cube super-atoms (Au6Te12Se8, 0D) with the anisotropic covalent-like intercube Te...Te bonds. The sequential-emerged anisotropic triple CDW charge modulation, antipolar charge orders and quasi-2D Fermi surface were discovered in ATS using scanning tunneling microscopy/spectroscopy (STM/STS) in combination with angle-resolved photoemission spectroscopy (ARPES), transport measurement and Raman spectra. DFT calculations disclose the emerging and correlation mechanism of CDW and antipolar charge orders via the unique layered super-atomic crystal geometry and electronic structures. This work not only provides an unprecedented microscopic picture of novel electronic phase in the ATS, but also suggests a new category of super-atom layered materials with manipulatable properties through their high and precise tunability of super-atomic units and inter-unit interactions. + These authors contributed equally: Shuya Xing, Linglu Wu, Zilu Wang, Xu Chen. * Email: zhihaicheng@ruc.edu.cn jgguo@iphy.ac.cn scw@ruc.edu.cn wji@ruc.edu.cn