Abstract
Lipid multibilayers are excellent model systems for studying water structures and dynamics near biological membrane surfaces. In particular, the orientational distribution and rotational dynamics of water molecules near hydrophilic lipid groups are found to be sensitive to the chemical nature and charge distributions of the amphiphilic lipids. To elucidate how different parts of these lipids affect the water hydrogen-bonding structure and dynamics and to directly compare with recent experimental results, we carried out molecular dynamics (MD) simulations of lipid multibilayer systems. We found that the water molecules close to positively charged choline groups have a broad distribution of orientations due to the clathratelike shell formation around the choline groups but that those associated with phosphate groups, even in the second hydration shell, are orientationally restricted due to their strong hydrogen bonding with the phosphate group. These MD simulation results are in excellent agreement with our time-resolved infrared pump-probe anisotropy measurements, and we believe that they provide valuable insights into the role of water molecules in maintaining lipid bilayer integrity.
| Original language | English |
|---|---|
| Article number | 114705 |
| Journal | Journal of Chemical Physics |
| Volume | 151 |
| Issue number | 11 |
| DOIs | |
| Publication status | Published - 2019 Sep 21 |
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ASJC Scopus subject areas
- Physics and Astronomy(all)
- Physical and Theoretical Chemistry
Cite this
Water hydrogen-bonding structure and dynamics near lipid multibilayer surface : Molecular dynamics simulation study with direct experimental comparison. / Lee, Euihyun; Kundu, Achintya; Jeon, Jonggu; Cho, Minhaeng.
In: Journal of Chemical Physics, Vol. 151, No. 11, 114705, 21.09.2019.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Water hydrogen-bonding structure and dynamics near lipid multibilayer surface
T2 - Molecular dynamics simulation study with direct experimental comparison
AU - Lee, Euihyun
AU - Kundu, Achintya
AU - Jeon, Jonggu
AU - Cho, Minhaeng
PY - 2019/9/21
Y1 - 2019/9/21
N2 - Lipid multibilayers are excellent model systems for studying water structures and dynamics near biological membrane surfaces. In particular, the orientational distribution and rotational dynamics of water molecules near hydrophilic lipid groups are found to be sensitive to the chemical nature and charge distributions of the amphiphilic lipids. To elucidate how different parts of these lipids affect the water hydrogen-bonding structure and dynamics and to directly compare with recent experimental results, we carried out molecular dynamics (MD) simulations of lipid multibilayer systems. We found that the water molecules close to positively charged choline groups have a broad distribution of orientations due to the clathratelike shell formation around the choline groups but that those associated with phosphate groups, even in the second hydration shell, are orientationally restricted due to their strong hydrogen bonding with the phosphate group. These MD simulation results are in excellent agreement with our time-resolved infrared pump-probe anisotropy measurements, and we believe that they provide valuable insights into the role of water molecules in maintaining lipid bilayer integrity.
AB - Lipid multibilayers are excellent model systems for studying water structures and dynamics near biological membrane surfaces. In particular, the orientational distribution and rotational dynamics of water molecules near hydrophilic lipid groups are found to be sensitive to the chemical nature and charge distributions of the amphiphilic lipids. To elucidate how different parts of these lipids affect the water hydrogen-bonding structure and dynamics and to directly compare with recent experimental results, we carried out molecular dynamics (MD) simulations of lipid multibilayer systems. We found that the water molecules close to positively charged choline groups have a broad distribution of orientations due to the clathratelike shell formation around the choline groups but that those associated with phosphate groups, even in the second hydration shell, are orientationally restricted due to their strong hydrogen bonding with the phosphate group. These MD simulation results are in excellent agreement with our time-resolved infrared pump-probe anisotropy measurements, and we believe that they provide valuable insights into the role of water molecules in maintaining lipid bilayer integrity.
UR - http://www.scopus.com/inward/record.url?scp=85072527066&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85072527066&partnerID=8YFLogxK
U2 - 10.1063/1.5120456
DO - 10.1063/1.5120456
M3 - Article
C2 - 31542031
AN - SCOPUS:85072527066
VL - 151
JO - Journal of Chemical Physics
JF - Journal of Chemical Physics
SN - 0021-9606
IS - 11
M1 - 114705
ER -