Modular assembly of a library of hybrid superlattices and artificial quantum solids

Hybrid superlattices, composed of two-dimensional atomic crystals (2DACs) and self-assembled molecular layers, provide a platform for synergizing the rich physical properties of solid-state 2DACs with customizable molecular functionalities. This study introduces a modular electrostatic co-assembly approach for synthesizing 53 distinct hybrid superlattices, using various 2DACs and molecular building blocks. Mechanistic studies reveal that the electrostatic assembly is governed by charge balance and the equilibrium between electrostatic and van der Waals interactions. Leveraging the charge balance principle, we demonstrate a precise control over the number of molecular layers and interlayer spacing by modulating the molecular charge density. Our study establishes a universal approach to a library of layered hybrid superlattices, incorporating versatile molecular functionalities into solid-state 2DACs. It promises a novel class of artificial quantum solids with designable electronic band offsets, tailored charge ordering, superconducting phase transitions, and magnetic ordering.