Rectangular-Phase Tellurene on Ni(111) from Monolayer Films to Periodic Striped Patterns

As an emerging member of monoelemental two-dimensional (2D) materials, 2D tellurium (tellurene) has recently attracted intensive attention due to its polymorphism arising from the multivalent nature and fascinating properties such as wide-range band gaps, high carrier mobilities, etc. Herein, we predict the formation of a rectangular-phase tellurene on Ni(111) by first-principles density functional theory (DFT) calculations and realize its direct syntheses and characterizations by molecular beam epitaxy (MBE) and scanning tunneling microscopy (STM). We reveal that the monolayer rectangular tellurene and underlying Ni(111) substrate are strongly coupled, along with good lattice registry along two mutually perpendicular directions, which serves as the key driving force for the tellurene formation. We also uncover the unique morphological transitions of Te/Ni(111) from rectangular tellurene monolayer, to uniform periodic striped patterns at the second layer, and then to thick striped patterns. This work should offer valuable insights for the substrate-mediated syntheses of monoelemental 2D materials, thus propelling their phase engineering and intriguing property explorations.