Stimulus-Induced Relief of Intentionally Incorporated Frustration Drives Refolding of a Water-Soluble Biomimetic Foldamer

Hanne C. Henriksen, Adam J. Sowers, Christopher R. Travis, Troy D. Vulpis, Thomas A. Cope, Sarah K. Ouslander, Alexander F. Russell, Michel R. Gagné, Vojislava Pophristic, Zhiwei Liu, Marcey L. Waters

Research output: Contribution to journalArticlepeer-review

Abstract

Frustrated, or nonoptimal, interactions have been proposed to be essential to a protein’s ability to display responsive behavior such as allostery, conformational signaling, and signal transduction. However, the intentional incorporation of frustrated noncovalent interactions has not been explored as a design element in the field of dynamic foldamers. Here, we report the design, synthesis, characterization, and molecular dynamics simulations of the first dynamic water-soluble foldamer that, in response to a stimulus, exploits relief of frustration in its noncovalent network to structurally rearrange from a pleated to an intercalated columnar structure. Thus, relief of frustration provides the energetic driving force for structural rearrangement. This work represents a previously unexplored design element for the development of stimulus-responsive systems that has potential application to materials chemistry, synthetic biology, and molecular machines.

Original languageEnglish (US)
Pages (from-to)27672-27679
Number of pages8
JournalJournal of the American Chemical Society
Volume145
Issue number50
DOIs
StatePublished - Dec 20 2023

All Science Journal Classification (ASJC) codes

  • Catalysis
  • General Chemistry
  • Biochemistry
  • Colloid and Surface Chemistry

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