Gaseous Synergistic Self‐Assembly and Arraying to Develop Bio‐Organic Photocapacitors for Neural Photostimulation

Abstract Bioinspired supramolecular architectonics is attracting increasing interest due to their flexible organization and multifunctionality. However, state‐of‐the‐art bioinspired architectonics generally take place in solvent‐based circumstance, thus leading to achieving precise control over the self‐assembly remains challenging. Moreover, the intrinsic difficulty of ordering the bio‐organic self‐assemblies into stable large‐scale arrays in the liquid environment for engineering devices severely restricts their extensive applications. Herein, a gaseous organization strategy is proposed with the physical vapor deposition (PVD) technology, allowing the bio‐organic monomers not only self‐assemble into architectures well‐established from the solvent‐based approaches but morphologies distinct from those delivered from the liquid cases. Specifically, 9‐fluorenylmethyloxycarbonyl‐phenylalanine‐phenylalanine (Fmoc‐FF) self‐assembles into spheres with tailored dimensions in the gaseous environment rather than conventional nanofibers, due to the distinct organization mechanisms. Arraying of the spherical architectures can integrate their behaviors, thus endorsing the bio‐organic film the ability of programmable optoelectronic properties, which can be employed to design P‐N heterojunction‐based bio‐photocapacitors for non‐invasive and nongenetic neurostimulations. The findings demonstrate that the gaseous strategy may offer an alternative approach to achieve unprecedented bio‐organic superstructures, and allow ordering into large‐scale arrays for behavior integration, potentially paving the avenue of developing supramolecular devices and promoting the practical applications of bio‐organic architectonics.