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The organizational complexity of biominerals has long fascinated scientistsseeking to understand biological programming and implement new developments inbiomimetic materials chemistry. Nonclassical crystallization pathways have beenobserved and analyzed in typical crystalline biominerals, involving thecontrolled attachment and reconfiguration of nanoparticles and clusters onorganic templates. However, the understanding of templated amorphous silicamineralization remains limited, hindering the rational design of complexsilica-based materials. Here, we present a systematic study on thestabilization of self-capping cationic silica cluster (CSC) and their assemblydynamics using DNA nanostructures as programmable attachment templates. Bytuning the composition and structure of CSC, we demonstrate high-fidelitysilicification at single-cluster resolution, revealing a process of adaptivetemplating involving cooperative adjustments of both the DNA framework andcluster morphology. Our results provide a unified model of silicification bycluster attachment and pave the way towards the molecular tuning of pre- andpost-nucleation stages of sol-gel reactions. Overall, our findings provide newinsights for the design of silica-based materials with controlled organizationand functionality, bridging the gap between biomineralization principles andthe rational design of biomimetic material.

Molecular tuning of DNA framework-programmed silicification by cationic silica cluster attachment