In vacuo synthesis of single-layer Ni3(HITP)2 on HOPG surface using metallo-organic precursor

Abstract

Single-layer conjugated metal-organic frameworks (SL c-MOFs) are predicated theoretically to host rich quantum phases. To date, however, the experimental synthesis has largely resulted in SL c-MOFs on metal substrates, whose intrinsic properties are strongly screened due to substrate hybridization. To overcome this obstacle, here we develop a method to grow clean SL c-MOF Ni3(HITP)2 on a chemically inert substrate of highly oriented pyrolytic graphite (HOPG). By means of an ultra-high vacuum based multi-step protocol using nickel acetylacetonate [Ni(acac)2] precursor, we obtain continuous single-layer Ni3(HITP)2. Scanning tunneling microscopy reveals a well-defined hexagonal framework with a uniform azimuthal orientation rotated by approximately 30 degrees with respect to the underlying graphite lattice. Furthermore, we control the growth of bilayer Ni3(HITP)2 which features an unusual AA stacking configuration. This work establishes metallo-organic chemistry as an efficient route for integrating 2D c-MOFs onto inert substrates, which opens a new avenue for exploring the exotic quantum properties of SL c-MOFs.