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Title: Hydration-mediated stiffening of collective membrane dynamics by cholesterol

Abstract

The collective behaviour of individual lipid molecules determines the properties of phospholipid membranes. Yet, the collective molecular motions often remain challenging to characterise at the desired spatial and temporal resolution. In this work, we study collective vibrational motion on picosecond time scales in dioleoylphosphatidylcholine lipid bilayers with varying cholesterol content using all-atom molecular dynamics simulations. Cholesterol is found to not only laterally compact the lipid bilayer, but also to change the velocity of longitudinal density fluctuations propagating in the plane of the membrane. Cholesterol-induced reduction of the area per lipid alters the collective dynamics of the lipid headgroups, but not of the lipid tails. The introduction of cholesterol reduces the number of water molecules interacting with the lipid headgroups, leading to a decrease in the velocity of the laterally-propagating sound mode. Thus, the stiffening effect of cholesterol is found to be indirect: decreasing the area per lipid weakens the interactions between the lipid headgroups and water. The collective modes characterised in this work can enable the membrane to dissipate excess energy and thus maintain its structural integrity, e.g., under mechanical stress.

Authors:
 [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [1]
  1. Ruhr Univ., Bochum (Germany)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
  3. Arizona State Univ., Tempe, AZ (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23); German Research Foundation (DFG)
OSTI Identifier:
1564188
Alternate Identifier(s):
OSTI ID: 1511502
Grant/Contract Number:  
AC05-00OR22725; FWP ERKP752
Resource Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP (Print)
Additional Journal Information:
Journal Name: Physical Chemistry Chemical Physics. PCCP (Print); Journal Volume: 21; Journal Issue: 20; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 59 BASIC BIOLOGICAL SCIENCES

Citation Formats

Päslack, Christopher, Smith, Jeremy C., Heyden, Matthias, and Schäfer, Lars V. Hydration-mediated stiffening of collective membrane dynamics by cholesterol. United States: N. p., 2019. Web. doi:10.1039/c9cp01431d.
Päslack, Christopher, Smith, Jeremy C., Heyden, Matthias, & Schäfer, Lars V. Hydration-mediated stiffening of collective membrane dynamics by cholesterol. United States. doi:10.1039/c9cp01431d.
Päslack, Christopher, Smith, Jeremy C., Heyden, Matthias, and Schäfer, Lars V. Tue . "Hydration-mediated stiffening of collective membrane dynamics by cholesterol". United States. doi:10.1039/c9cp01431d.
@article{osti_1564188,
title = {Hydration-mediated stiffening of collective membrane dynamics by cholesterol},
author = {Päslack, Christopher and Smith, Jeremy C. and Heyden, Matthias and Schäfer, Lars V.},
abstractNote = {The collective behaviour of individual lipid molecules determines the properties of phospholipid membranes. Yet, the collective molecular motions often remain challenging to characterise at the desired spatial and temporal resolution. In this work, we study collective vibrational motion on picosecond time scales in dioleoylphosphatidylcholine lipid bilayers with varying cholesterol content using all-atom molecular dynamics simulations. Cholesterol is found to not only laterally compact the lipid bilayer, but also to change the velocity of longitudinal density fluctuations propagating in the plane of the membrane. Cholesterol-induced reduction of the area per lipid alters the collective dynamics of the lipid headgroups, but not of the lipid tails. The introduction of cholesterol reduces the number of water molecules interacting with the lipid headgroups, leading to a decrease in the velocity of the laterally-propagating sound mode. Thus, the stiffening effect of cholesterol is found to be indirect: decreasing the area per lipid weakens the interactions between the lipid headgroups and water. The collective modes characterised in this work can enable the membrane to dissipate excess energy and thus maintain its structural integrity, e.g., under mechanical stress.},
doi = {10.1039/c9cp01431d},
journal = {Physical Chemistry Chemical Physics. PCCP (Print)},
number = 20,
volume = 21,
place = {United States},
year = {2019},
month = {4}
}

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