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Area of Science:

  • Supramolecular Chemistry
  • Chemical Biology
  • Systems Chemistry

Background:

  • Cellular transformations rely on intercommunication between dynamic chemical networks.
  • Constitutional dynamic networks (CDNs) offer a programmable framework for complex chemical systems.

Purpose of the Study:

  • To engineer and investigate the intercommunication between two distinct constitutional dynamic networks (CDNs).
  • To demonstrate how external triggers can modulate the behavior of these interconnected CDNs.
  • To achieve programmed temporal control over molecular concentrations within the CDNs.

Main Methods:

  • Construction of two CDNs, 'S' and 'T', each with four specific supramolecular constituents.
  • Conjugation of each constituent to a Mg2+-ion-dependent DNAzyme reporter for concentration monitoring.
  • Incorporation of Mg2+-ion-dependent DNAzymes as activators for inter-network signaling.
  • Application of specific hairpin triggers (Hdd' and Haa') to initiate intercommunication.

Main Results:

  • Triggering one CDN with specific input strands affects the re-equilibration of constituents in the other CDN.
  • The dynamic equilibrium of the triggering CDN remains unaffected.
  • Autonomous positive/positive or positive/negative feedback loops were stimulated.
  • Programmed time-dependent up-regulation or down-regulation of constituents was achieved.

Conclusions:

  • Demonstrated successful intercommunication between two CDNs via DNAzyme-mediated signaling.
  • Showcased the ability to control CDN behavior and achieve programmed temporal regulation of molecular constituents.
  • Established a foundation for designing complex, responsive chemical systems inspired by biological networks.