Self-Directed Reconstitution of Proteorhodopsin with Amphiphilic Block Copolymers Induces the Formation of Hierarchically Ordered Proteopolymer Membrane Arrays

Manipulating recognition and transport at the nanoscale holds great promise for technological breakthroughs in energy conversion, catalysis, and information processing. Living systems evolve specialized membrane proteins (MPs) embedded in lipid bilayers to exquisitely control communications across the insulating membrane boundaries. Harnessing MP functions directly in synthetic systems opens up enormous opportunities for nanotechnology, but there exist fundamental challenges of how to address the labile nature of lipid bilayers that renders them of inadequate value under a broad range of harsh non-biological conditions, and how to reconstitute MPs coherently in two or three dimensions into non-lipid-based artificial membranes. Here we show that amphiphilic block copolymers can be designed to direct proteorhodopsin reconstitution and formation of hierarchically ordered proteopolymer membrane arrays spontaneously, even when the membrane-forming polymer blocks are in entangled states. These findings unfold a viable approach for the development of robust and chemically versatile nanomembranes with MP-regulated recognition and transport performance.