Mastering energy landscapes via liquid liquid phase separation to program active supramolecular coassembly from the nano to macro scale

TL;DR

This paper demonstrates how liquid liquid phase separation (LLPS) can be used to control and engineer the energy landscapes of supramolecular assemblies, enabling hierarchical, life-like structures from nano to macro scales.

Contribution

It introduces LLPS as a novel method to map and manipulate energy landscapes in coassembly systems, facilitating predictive control over hierarchical structure formation.

Findings

Quantitative mapping of energy barriers and transition states.

Controlled hierarchical assembly from nano to macro scales.

Achieved spatially organized, non-equilibrium architectures.

Abstract

The energy landscape dictates pathways and outcomes in supramolecular selfassembly, yet harnessing it from the nano to the macro scales remains a major challenge. Here, we demonstrate liquid liquid phase separation (LLPS) as a powerful tool to navigate and engineer the energy landscapes of coassembly systems comprising disordered proteins and peptides. We quantitatively map the energy barriers and transition states governing structural transitions, enabling predictive on off control of assembly and hierarchical order from nano to macro scales. By integrating supramolecular biofabrication, we achieve spatially organized architectures with life like non equilibrium behaviour. Crucially, assembly stability and scalable selfsorting are shown to depend on accessing minimum energy states, regardless of whether the co assembled structures are disordered or ordered. This work establishes energy landscape mediation via LLPS as a general framework for designing lifelike, hierarchically structured materials.