DNA Glass: Encasing Diffraction-Quality, Mesoporous DNA Crystals in Silica

Self-assembling DNA crystals have emerged over the last two decades as an efficient and effective means of organizing matter at the nanoscale, but functionalization of these lattices has proved challenging as physiological buffer conditions are required to maintain structural integrity. In this manuscript, we demonstrate the silicification of porous DNA crystals using sol-gel chemistry. We identify reaction conditions that produce the minimum coating thickness to confer environmental protection, and subsequently measure the protective ability of the silica coating to various stressors, including heat, low ionic strength solution, organic solvents, and unprotected flash freezing. By soaking ions and dyes into the lattice after silica coating, we demonstrate that the crystals maintain their pores, and that the major groove of the DNA can still be used as a site-specific template for chemical modifications. We image a library of different crystal motifs by electron microscopy and confirm the presence of silica using energy dispersive spectroscopy. Finally, we perform X-ray diffraction on these crystals, both with and without cryoprotection and determine the structure of the DNA frame, underscoring the conserved molecular order after coating. We anticipate these mesoporous silica composites for use in applications involving extreme, non-physiological conditions and for experiments which utilize the DNA glass described here as a template for surface science.