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Adv."],"published-print":{"date-parts":[[2026,10,2]]},"abstract":"<jats:p>\n                    DNA nanotechnology leverages the molecular design resolution of the DNA double helix to fold and tile matter into designer architectures. Recent advances in bioinorganic chemistry have exploited DNA\/Ag\n                    <jats:sup>+<\/jats:sup>\n                    affinity to carry out the templated reduction of silver nanoclusters. Here, we develop a unified method that leverages the topology of DNA triangles with embedded silver base pairs to nucleate controlled cluster growth in a mesoporous 3D lattice. Use of confocal fluorescence microscopy allows for the direct observation of reaction kinetics and reconstruction of the optical bandgap. These crystals yield molecular structures of Ag\n                    <jats:sub>4<\/jats:sub>\n                    and Ag\n                    <jats:sub>6<\/jats:sub>\n                    by x-ray diffraction in varying pyrimidine:pyrimidine pairs. Intercluster distances of less than 2\u00a0nanometers show observable electronic coupling, with red shifting observed relative to literature standards. A thorough computational investigation establishes a theoretical basis for our observed behavior and establishes the interplay between cluster size, charge, geometry, and resonance. 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