Heterostructured materials (e.g.,
metals with multimodal microstructures)
offer the promise of unprecedented functionality and performance by
avoiding trade-offs between competing properties such as strength
and ductility. However, methods to reproducibly synthesize heterostructured
materials with explicit microstructural control are still elusive,
and therefore optimizing their mechanical and functional properties
via microstructural engineering is presently infeasible. Here, we
describe a broadly applicable method to synthesize metallic films
with precisely defined multimodal microstructures. This method enables
explicit control of the size, volume fraction, and spatial connectivity
of fine and coarse grains by exploiting two distinct forms of film
growth (epitaxial and Volmer–Weber) simultaneously. We fabricated
Cu and Fe films with bimodal and multimodal microstructures using
this method and investigated their mechanical properties, which reveals
a hitherto unknown breakdown in the strength–ductility synergy
produced by such microstructures at small sample dimensions. Our approach
enables systematic design of multimodal microstructures to tailor
the mechanical properties of metallic materials and provides a platform
to create functional thin films and 2D materials with prescribed phase
morphologies and microstructures.