Van der Waals epitaxy of tunable moirés enabled by alloying

The unique physics in moiré superlattices of twisted or lattice-mismatched atomic layers holds great promise for future quantum technologies. However, twisted configurations are thermodynamically unfavourable, making accurate twist angle control during growth implausible. While rotationally aligned, lattice-mismatched moirés such as WSe₂/WS₂ can be synthesized, they lack the critical moiré period tunability, and their formation mechanisms are not well understood. Here, we report the thermodynamically driven van der Waals epitaxy of moirés with a tunable period from 10 to 45 nanometres, using lattice mismatch engineering in two WSSe layers with adjustable chalcogen ratios. Contrary to conventional epitaxy, where lattice-mismatch-induced stress hinders high-quality growth, we reveal the key role of bulk stress in moiré formation and its unique interplay with edge stress in shaping the moiré growth modes. Moreover, the superlattices display tunable interlayer excitons and moiré intralayer excitons. Our studies unveil the epitaxial science of moiré synthesis and lay the foundations for moiré-based technologies.