Title: Towards Designable Quantum Solids with Layered Hybrid Superlattices: Boundless Opportunities at Bondless Boundaries

Solid-state materials are typically grown at high temperature and exhibit thermodynamics dictated crystalline ordering, a prerequisite for their remarkable electronic and macroscopic quantum properties, but usually with limited customization space. Conversely, synthetic molecular systems feature highly tunable structural topologies and versatile functionalities, albeit lacking long-range ordering necessary for scalable electronic technologies. An integration of these two systems could allow to exploit the versatile molecular design strategies to tailor crystalline solids and create artificial materials with tunable electronic structures and exotic quantum properties. However, this has been difficult to realize due to highly disparate bonding structures and processing conditions of these two notably different systems. The two-dimensional atomic crystals (2DACs) feature covalently bonded crystalline atomic layers separated by non-bonding van der Waals gaps, into which molecules of designable size, symmetry, chirality, topology and functional substituents may insert and self-assemble into highly ordered molecular layers. Herein, I will introduce our recent efforts in combining 2DACs of distinct physical properties with diverse molecular systems to create a new family of layered hybrid superlattices (LHSLs) consisting of alternating crystalline atomic layers and self-assembled molecular layers with designable chemical compositions and structural motifs. In particular, I will discuss how we may use a molecular intercalation strategy to tailor the electronic and optical properties of various 2DACs, and highlight a unique class of chiral molecular intercalation superlattices hosting robust chiral-induced spin selectivity and elusive chiral superconductivity. With the versatile molecular design and modular assembly strategies, the LHSLs allow vast flexibility for weaving distinct building constituents into artificial solids with designable chemical modulation, structural topology and 3D potential landscape. It opens unprecedented ways to tailor the electronic, optical and quantum properties, thus defining a rich material platform for diverse emerging technologies.