Light-Mediated Interconversion between a Foldamer and a Self-Replicator.

Area of Science:

• Origin of life studies
• Supramolecular chemistry
• Systems chemistry

Background:

• Self-replicating molecules and folded macromolecules are crucial for life's emergence and evolution.
• The interplay between these structures in abiotic systems is not well understood.

Purpose of the Study:

• To demonstrate an abiotic system where a single building block can form either self-replicating molecules or foldamers.
• To investigate the stimuli that control the formation of these distinct structures.

Main Methods:

• Utilized a disulfide-based dynamic combinatorial library.
• Applied mechanoagitation and controlled pH conditions.
• Introduced a photoacid to manipulate pH with light.

Main Results:

• A single building block selectively formed self-replicating hexamer fibers under agitation and moderate pH.
• A 15-subunit macrocyclic foldamer formed transiently and accumulated at lower pH or without agitation.
• Interconversion between foldamer and self-replicator was achieved via external stimuli, including light-induced pH changes.

Conclusions:

• Demonstrated a controllable abiotic system producing either self-replicators or foldamers from a single precursor.
• Showcased the potential for external stimuli, including light, to drive transitions between these states.
• Provided a model system for understanding the emergence of complexity and dissipative structures in early life.