Unlocking the potential of colloidal metamaterials—artificial materials mirroring molecular structures—holds promise for diverse applications, from optical engineering to catalytic chemistry. Yet, orchestrating precise self-assembly of colloidal metamaterials remains challenging due to the lack of regioselective surface chemistry. Addressing this, we introduce a novel strategy employing DNA-patched nanoparticles to drive the self-assembly of colloidal metamolecules. By utilizing magnetic bead-assisted DNA cluster transfer, we overcome geometrical constraints, enabling regioselective DNA patches. This approach is highly scalable and versatile, affording diverse configurations. We showcase the creation of gold and silver nanoparticle-based colloidal metamolecules, demonstrating the strategy's broad applicability. Notably, we employ this method to position fluorescent nanodiamonds within silver nanocube dimers, enabling precise control over photophysical properties. Our approach revolutionizes colloidal metamaterial synthesis, paving the way for tailored nanoscale functionalities in fields such as biological sensing and optical physics.
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