Zeta Potential Transition Correlates with Optimal DNA Origami Silicification Temperature

Abstract

DNA origami templates enable precise construction of inorganic nanostructures via silicification, yet optimal reaction conditions are often determined empirically. Here, we demonstrate that the temperature-dependent evolution of DNA origami zeta potential provides a simple, design-independent predictor of favourable silicification. Four distinct architectures, square, triangle, 14-helix bundle, and ring, were examined, revealing that the highest silicification thickness is achieved near the temperature at which the zeta potential distribution begins transitioning from unimodal to bimodal, while maintaining a relatively low thickness coefficient of variation (Thickness CV), which is used as a measure of interparticle uniformity in silicification. Above this range, conformational heterogeneity increases, reducing silica deposition efficiency. Molecular dynamics simulations indicate that moderate thermal fluctuations expose additional binding sites while preserving structural integrity, whereas excessive heating destabilizes helices. This approach offers a rapid, predictive strategy to guide reproducible inorganic coating across diverse DNA nanostructures.