Molecular motor-driven reversible liquid-liquid phase separation of supramolecular assemblies

Area of Science:

• Supramolecular chemistry
• Materials science
• Biomedical engineering

Background:

• Liquid-liquid phase separation (LLPS) is vital for cellular functions and advanced materials.
• Controlling LLPS in supramolecular assemblies, especially reversibly, remains a challenge.
• Molecular motors offer potential for dynamic control over material properties.

Purpose of the Study:

• To develop a molecular motor-driven system for modulating LLPS in supramolecular assemblies.
• To investigate the relationship between molecular structure, hydrophobicity, and phase separation behavior.
• To achieve reversible control over LLPS using light and temperature.

Main Methods:

• Systematic molecular modification of supramolecular building blocks.
• Photothermal isomerization studies to probe molecular dynamics.
• Observation of in situ droplet formation and dissolution under motor rotation.

Main Results:

• Nanoscale rotary motion of molecular motors was shown to modulate LLPS.
• Subtle molecular structure changes influenced hydrophobicity, critical phase separation temperature, and promoted phase separation.
• Assemblies exhibited dynamic formation and dissolution of droplets in non-equilibrium states.

Conclusions:

• Established a molecular motor-driven system for tunable LLPS in supramolecular assemblies.
• Demonstrated an orthogonal strategy for controlling phase separation with light and temperature.
• Paved the way for designing out-of-equilibrium biomedical materials and adaptive soft matter.