Tuning Molecular Superlattice by Charge-Density-Wave Patterns in Two-Dimensional Monolayer Crystals.

Charge density wave (CDW) in two-dimensional (2D) crystals plays a vital role in tuning the interface structures and properties. However, how the CDW tunes the self-assembled molecular superlattice still remains unclear. In this study, we investigated the self-assembled manganese phthalocyanine (MnPc) molecular superlattice on single-layered 1T- and 2H-NbSe2 crystals under regulation by distinct CDW patterns. We observe that, in low coverage, MnPc molecules preferentially adsorb on 2H-NbSe2 compared to 1T-NbSe2. With increasing coverage, MnPc can form a highly ordered superlattice on 2H-NbSe2; however, it is randomly distributed on 1T-NbSe2. We reveal a perfect geometric commensurability between the molecular superlattice and intrinsic CDW pattern in 2H-NbSe2 and a poor commensurability for that of 1T-NbSe2. We believe that the subtly different geometric commensurability dominates the different adsorption and arrangement of the molecular superlattices on 2D CDW patterns. Our study provides a pioneering approach for tuning the molecular superlattices using the CDW patterns.