PNNL

Abstract

Tailoring complex hierarchical structures are key objectives of mod-ern nanomaterial design, especially for bio-inspired nanomaterials such as protein/inorganic nanoparticle hybrids owing to flexible functionalities and resultant unique material structures and properties. However, it is still imposing consequential challenges due to a lack of understanding of temporal and spatial interplay over a wide range of scales via fundamental physicochemical interactions. Motivated by dynamic light scattering experiments for a solid-binding Car9 peptides/silica nanoparticles hybrid system that show pH-dependent reversibility in self-assembly at particle scales, we have developed a theoretical framework where interactions at molecular and macroscopic scales are rigorously coupled based on colloidal theory and atomistic molecular dynamics simulations and then integrated into a predictive coarse-grained model. The model has successfully described the pH-dependent reversibility that is also confirmed by small-angle x-ray scattering experiments at collective scales. Our framework provides a fundamental basis to connect microscopic details to macroscopic phenomena of many complex bio-inspired material systems to understand both equilibrium and non-equilibrium characteristics, which is necessary for dynamic control of such complex systems.