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Interfacial dynamics in inverted-headgroup lipid membranes.

Euihyun Lee1, Xiao You1, Carlos R Baiz1

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Synthetic lipids with inverted headgroups do not alter interfacial water H-bond dynamics. However, they slightly disrupt water H-bonds near the lipid tail linker region, impacting hydration shells.

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Area of Science:

  • Biophysics
  • Computational Chemistry
  • Lipid Bilayer Research

Background:

  • Interfacial water orientation is crucial for lipid bilayer function.
  • Headgroup electrostatics, including charges and dipoles, influence interfacial water.
  • Synthetic lipids offer models to study headgroup effects.

Purpose of the Study:

  • To investigate the impact of inverted headgroup dipoles on interfacial water H-bond dynamics.
  • To compare H-bond dynamics in natural vs. synthetic lipid bilayers.
  • To characterize water structure around lipid headgroups.

Main Methods:

  • Two-dimensional infrared spectroscopy of the ester carbonyl band.
  • Molecular dynamics simulations of lipid bilayers.
  • Analysis of interfacial water H-bond populations and structure.

Main Results:

  • Inverted headgroup dipoles in DOCPe did not affect carbonyl H-bond populations or overall water dynamics.
  • Phosphate-associated water structure was similar between lipid types.
  • Carbonyl-associated water showed a disrupted H-bond structure in DOCPe, particularly in the second hydration shell.

Conclusions:

  • Reverse dipoles in inverted-headgroup lipids have a limited effect on interfacial water H-bond dynamics.
  • Water H-bonds at the headgroup-tail linker region are weakly perturbed by changes in water orientation.
  • Synthetic lipids provide insights into the subtle interplay between lipid structure and water behavior.