Abstract
Electrostatically tunable quantum confinement in nanoscale systems offers unprecedented opportunities for manipulating artificial quantum matter, positioning these platforms at the frontier of quantum science. The strategic integration of distinct confinement mechanisms could revolutionize quantum functionality by enabling novel states with enhanced coherence properties. Here, we demonstrate inherently interfacial potential engineering by combining lateral semiconductor 2D moiré potentials with vertical quantum confinement effects in semimetal bismuth nanofilms, creating localized periodic sites for quantum-confined charges. Using scanning tunneling microscopy, we observe moiré-mediated Wigner crystals with self-organized electron lattices arising from strong Coulomb interactions, exhibiting unexplored multiple energy quantization behaviors that can be manipulated by quantum well states in ultrathin bismuth films. These precisely localizable charge states provide a promising platform for van der Waals (vdW) charge qubits electrostatically confined within 2D materials. Our work demonstrates extended tunability of artificial atom states in phase, space, and energy regimes. With optimized designs, these 2D vdW architectures bridge fundamental Wigner crystallization phenomena with practical applications in advanced electronic systems and quantum state manipulation.