Van der Waals Heterostructures and Superlattices—Boundless Opportunities at Bondless Boundaries

The rise of two-dimensional atomic crystals (2DACs) and van der Waals heterostructures (vdWHs) has catalyzed a bonding-free strategy for constructing heterostructures beyond the limits of traditional epitaxial approaches. In this talk, I will start with a brief overview of the early exploration of van der Waals (vdW) interactions for the heterogeneous integration of highly disparate materials with pristine electronic interfaces. I will then focus on our recent efforts in synthesizing and investigating a rich family of vdW superlattices (vdWSLs) consisting of alternating crystalline atomic layers and self-assembled molecular interlayers of customizable chemical compositions and structural motifs. I discuss how we may use the molecular interlayers to tailor the electronic and optical properties of various 2DACs, and particularly highlight a unique class of chiral molecular intercalation superlattices exhibiting robust chiral-induced spin selectivity and elusive chiral superconductivity. With versatile molecular design and modular assembly strategies, 2D-molecular vdWSLs offer unprecedented flexibility for weaving distinct building constituents into artificial solids with customizable chemical modulation, structural topology, and artificial potential landscapes in 3D space. This opens boundless opportunities to tailor the electronic, optical, and quantum properties, thus defining a rich material platform for diverse emerging technologies.