Adaptable Self‐Assembly of a PEG Dendrimer‐Coiled Coil Conjugate

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Abstract
Self‐assembly of designed molecules has enabled the construction of a variety of functional nanostructures. Specifically, adaptable self‐assembly has demonstrated several advantageous features for smart materials. Here, we demonstrate that an α‐helical coiled coil conjugated with a dendrimer can adapt to spatial restriction due to the strong steric repulsion between dendrimer chains. The adaptable transformation of a tetrameric coiled coil to a trimeric coiled coil can be confirmed using analytical ultracentrifugation upon conjugation of the dendrimer to the coiled coil‐forming building block. Interestingly, circular dichroism spectroscopy analysis of the dendrimer conjugate revealed an unconventional trend: the multimerization of the coiled coil is inversely dependent on concentration. This result implies that the spatial crowding between the bulky dendritic chains is significantly stronger than that between linear chains, thereby affecting the overall assembly process. We further illustrated the application potential by decorating the surface of gold nanorods (AuNRs) with the adaptable coiled coil. The dendrimer‐coiled coil peptide conjugate can be utilized to fabricate organic‐inorganic nanohybrids with enhanced colloidal and thermal stabilities. This study demonstrates that the coiled coil can engage in the adaptable mode of self‐assembly with the potential to form dynamic peptide‐based materials.

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