Bioinspired hybrid DNA/dendrimer-based films with supramolecular chirality

Abstract

Bioinspired hybrid DNA/dendrimer films were obtained by heating long double-stranded DNA (dsDNA) above its melting temperature and, while in the denatured state, mixing it with poly(amidoamine) (PAMAM) dendrimers, followed by controlled cooling. The formation of these new types of films was found to be dependent on several parameters, including the initial heating temperature, pH, buffer composition, dendrimer generation, amine/phosphate (N/P) ratio, and cooling speed. In addition to the PAMAM dendrimers (generations 3, 4, and 5), films could also be produced with branched poly(ethylenimine) with a molecular weight of 25 kDa. The results indicated that these films were formed not only through electrostatic interactions established between the negatively charged DNA molecules and the positive dendrimers, as expected, but also through random rehybridization of the single-stranded DNA (ssDNA) during the cooling process. The resulting films are water-insoluble, transparent when thin, highly elastic when air-dried, exceptionally stable over extended periods, cytocompatible, and easily scalable. Notably, the slow cooling process allowed for the establishment of at least a partially ordered structure in the films, as revealed by circular dichroism, providing evidence of supramolecular chirality. It is envisioned that these films may have significant potential in biomedical applications, such as drug/gene delivery systems, platforms for cell-free DNA transcription and components in biosensors.