Probing multivalent interactions in a synthetic host-guest complex by dynamic force spectroscopy

A. Gomez Casado, H.H. Dam, M.D. Yilmaz, D. Florea, Daniel Florea, Pascal Jonkheijm, Jurriaan Huskens

Research output: Contribution to journalArticleAcademicpeer-review

55 Citations (Scopus)

Abstract

Multivalency is present in many biological and synthetic systems. Successful application of multivalency depends on a correct understanding of the thermodynamics and kinetics of this phenomenon. In this Article, we address the stability and strength of multivalent bonds with force spectroscopy techniques employing a synthetic adamantane/β-cyclodextrin model system. Comparing the experimental findings to theoretical predictions for the rupture force and the kinetic off-rate, we find that when the valency of the complex is increased from mono- to di- to trivalent, there is a transition from quasi-equilibrium, with a constant rupture force of 99 pN, to a kinetically dependent state, with loading-rate-dependent rupture forces from 140 to 184 pN (divalent) and 175 to 210 pN (trivalent). Additional binding geometries, parallel monovalent ruptures, single-bound divalent ruptures, and single- and double-bound trivalent ruptures are identified. The experimental kinetic off-rates of the multivalent complexes show that the stability of the complexes is significantly enhanced with the number of bonds, in agreement with the predictions of a noncooperative multivalent model.
Original languageEnglish
Pages (from-to)10849-10857
Number of pages9
JournalJournal of the American Chemical Society
Volume133
Issue number28
DOIs
Publication statusPublished - 2011

Keywords

  • METIS-282171
  • IR-104543

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