DNA Base Pair Stacking Crystallization of Gold Colloids.

We describe a DNA base pair (bp) stacking driven 3D crystallization of 70-80 nm gold nanospheres (Au NSs) into a large-area, face-centered-cubic (FCC) lattice. Although great advances have been achieved over the past decade, DNA nanoparticle (NP) crystallization has relied solely on the base complementary binding. This limits the accessible crystal size particularly for the larger and heavier Au NPs (>50 nm). In this work, we argue that the use of DNA bp-stacking (so-called blunt-end stacking) instead of complementary binding can widen the scope of controlled interparticle interactions used to assemble larger Au colloids into a larger-area crystal. Through the optimization of the melting transition, relatively large Au NSs (e.g., 75 nm) with nearly ideal roundness can be crystallized into FCC crystals with the area of up to approximately 1400 μm. A strong metallodielectric stopband is experimentally observed in the visible range, confirming the high quality of our self-assembled Au colloidal crystals.