Electrostatic Forces in Field-Perturbed Equilibria: Nanopore Analysis of Cage Complexes

Stefan Borsley, Marius M. Haugland, Samuel Oldknow, James A. Cooper, Michael J. Burke, Aaron Scott, William Grantham, Julia Vallejo, Euan K. Brechin, Paul J. Lusby, Scott L. Cockroft

Research output: Contribution to journalArticlepeer-review

Abstract / Description of output

Molecular recognition has been widely investigated under equilibrium conditions, but little is known about such processes when perturbed by external forces. Here, we investigate the influence of electric fields on complexes formed between metallosupramolecular cages and a protein nanopore at the single-molecule level. Association rates were dominated by the applied voltage, whereas local electrostatic interactions between the cage and the nanopore more greatly influenced the dissociation kinetics. By exploiting these principles, we showed that the externally applied voltage could be used to selectively bind a specific cage from a mixture containing a large excess of other cages. Moreover, the applied voltage could also be used to drive supramolecular enantioinversion of the chiral cages or, occasionally, the non-equilibrium capture and disassembly of cages deep within the nanopore. Similar principles might be exploited in the design of other molecular devices that operate within externally applied electric fields or biogenic transmembrane potentials.

Original languageEnglish
Pages (from-to)1275-1292
Number of pages18
JournalChem
Volume5
Issue number5
Early online date8 Apr 2019
DOIs
Publication statusPublished - 9 May 2019

Keywords / Materials (for Non-textual outputs)

  • ALPHA-HEMOLYSIN
  • NUCLEOBASE RECOGNITION
  • MOLECULAR MOTORS
  • PROTEIN
  • BINDING
  • SYSTEMS
  • PORE
  • IDENTIFICATION
  • TRANSLOCATION
  • CHIRALITY

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