Realization of large-area ultraflat chiral blue phosphorene

Abstract Blue phosphorene (BlueP), a theoretically proposed phosphorous allotrope with buckled honeycomb lattice, has attracted considerable interest due to its intriguing properties. Introducing chirality into BlueP can further enrich its physical and chemical properties, expanding its potential for applications. However, the synthesis of chiral BlueP remains elusive. Here, we demonstrate the growth of large-area BlueP films on Cu(111), with lateral size limited by the wafer dimensions. Importantly, we discovered that the BlueP is characterized by an ultraflat honeycomb lattice, rather than the prevailing buckled structure, and develops highly ordered spatial chirality plausibly resulting from the rotational stacking with the substrate and interface strain release, as further confirmed by the geometric phase analysis. Moreover, spectroscopic measurements reveal its intrinsic metallic nature and different characteristic quantum oscillations in the image-potential states, which can be exploited for a range of potential applications including polarization optics, spintronics, and chiral catalysis.