Formation of Moiré Superlattices via Surfactant/Nanosheet-Co-mediated Crystallization

Moiré superlattices (MSLs) of two-dimensional (2D) van der Waals materials have attracted considerable attention in recent years; however, studies of bottom-up growth of twisted MSL structures via solution-processed crystallization are rarely reported. Through facile one-pot solvothermal synthesis, here we demonstrate a nonclassical surfactant/nanosheet-co-mediated crystallization pathway for formation of MSL structures with two models of SnS₂ and SnSe₂. Our experimental results reveal that attractive interactions between 2D inorganic building blocks and surfactant organic molecules during the initial stage of crystallization are crucial to drive surfactant-covered nanosheets to crystallize into molecule-intercalated nanosheet aggregates. Under the high-pressure condition, further crystallograpic fusion can occur if the reaction time is prolonged, which alters the interactions of adjacent layers during the coalescence of small-grain-size 2D domains due to insertion of foreign molecules, leading to interlayer rotations. This work uncovers an interesting organic-inorganic cocrystallization growth mode and provides a novel pathway for large-scale fabrication of MSLs.