Self-Assembled Single-Stranded DNA Nano-Networks in Solution and at Surfaces

We studied the directed self-assembly of two types of complementary single-stranded DNA (ssDNA) strands [i.e., poly(dA) and poly(dT)] into more complex, organized, and percolating networks in dilute solutions and at surfaces. Understanding ssDNA self-assembly into 2D networks on surfaces is important for the use of such networks in the fabrication of well-defined nanotechnological devices, as, for instance, required in nanoelectronics or for biosensing. To control the formation of 2D networks on surfaces, it is important to know whether DNA assemblies are formed already in dilute solutions or only during the drying/immobilization process at the surface, where the concentration automatically increases. Fluorescence cross-correlation spectroscopy dearly shows the presence of larger DNA complexes in mixed poly(dA) and poly(dT) solutions already at very low DNA concentrations (<1 nM), that is, well below the overlap concentration. Here, we describe for the first time such supramolecular complexes in solution and how their structure depends on the ssDNA length and concentration and ionic strength. Hence, future attempts to control such networks should also focus on network precursors in solution and not only on their immobilization on surfaces.

Automated summary

This study investigates the directed self-assembly of complementary single-stranded DNA strands (poly(dA) and poly(dT)) into complex, organized, and percolating networks in dilute solutions and at surfaces. The knowledge of DNA assemblies in solution and their impact on network formation is crucial for controlling the fabrication of nanotechnological devices. Fluorescence cross-correlation spectroscopy confirms the presence of larger DNA complexes in mixed solutions at low concentrations, emphasizing the importance of considering network precursors in solution.