Ion-Assisted Nanoscale Material Engineering in Atomic Layers

Achieving deterministic control over the properties of low-dimensional materials with nanoscale precision is a long-sought goal. Mastering this capability has a transformative effect on the design of multifunctional electrical and optical devices. Here, we present an ion-assisted synthetic technique that enables precise control over the material composition and energy landscape of two-dimensional (2D) atomic crystals. Our method transforms binary transition-metal dichalcogenides, like MoSe2, into ternary MoS2αSe2(1−α) alloys with systematically adjustable compositions, α. By piecewise assembly of the lateral, compositionally modulated MoS2αSe2(1−α) segments within 2D atomic layers, we present a synthetic pathway toward the realization of multicompositional designer materials. Our technique enables the fabrication of advanced 2D structures with arbitrary boundaries, dimensions as small as 30 nm, and fully customizable energy landscapes. Our optical characterizations further showcase the potential for implementing tailored optoelectronics in these engineered 2D crystals.