Hydration Dynamics of a Peripheral Membrane Protein

Olivier Fisette, Christopher Päslack, Ryan Barnes, J. Mario Isas, Ralf Langen, Matthias Heyden, Songi Han, Lars V. Schäfer

Research output: Contribution to journalArticlepeer-review

37 Scopus citations

Abstract

Water dynamics in the hydration shell of the peripheral membrane protein annexin B12 were studied using MD simulations and Overhauser DNP-enhanced NMR. We show that retardation of water motions near phospholipid bilayers is extended by the presence of a membrane-bound protein, up to around 10 Å above that protein. Near the membrane surface, electrostatic interactions with the lipid head groups strongly slow down water dynamics, whereas protein-induced water retardation is weaker and dominates only at distances beyond 10 Å from the membrane surface. The results can be understood from a simple model based on additive contributions from the membrane and the protein to the activation free energy barriers of water diffusion next to the biomolecular surfaces. Furthermore, analysis of the intermolecular vibrations of the water network reveals that retarded water motions near the membrane shift the vibrational modes to higher frequencies, which we used to identify an entropy gradient from the membrane surface toward the bulk water. Our results have implications for processes that take place at lipid membrane surfaces, including molecular recognition, binding, and protein-protein interactions.

Original languageEnglish (US)
Pages (from-to)11526-11535
Number of pages10
JournalJournal of the American Chemical Society
Volume138
Issue number36
DOIs
StatePublished - Sep 14 2016
Externally publishedYes

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

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