Quasielastic neutron scattering measurements of fast local translational diffusion of lipid molecules in phospholipid bilayers

Tabony, J.; Perly, Bruno

doi:10.1016/0005-2736(91)90354-b

Cited by 78 publications

(64 citation statements)

References 23 publications

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“…The smallest timescales considered in the table (2–10 ps) are similar to the timescales accessed by neutron scattering experiments (1–10 ps). Interestingly, the simulated diffusion coefficients on the 2–10-ps timescale are more similar to experimental values obtained at elevated temperatures ([50] reports a translational diffusion coefficient of

14 \times 10^{- 8}

^{2} \cdot

^{- 1}

for a system at 30

^{\circ}

C and 400 ×

10^{- 8}

^{2} \cdot

^{- 1}

for a system at 63

^{\circ}

C; [51] reports in-plane diffusion coefficients on the order of 15 ×

10^{- 8}

–600 ×

10^{- 8}

^{2} \cdot

^{- 1}

for a system at 60

^{\circ}

C). As diffusion constants inferred from experiments and simulations typically depend on the timescale considered, also the effect of salt on the diffusion constants may depend on the timescales.…”

Section: Resultssupporting

confidence: 77%

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Effect of Sodium and Chloride Binding on a Lecithin Bilayer. A Molecular Dynamics Study

2017

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The effect of ion binding on the structural, mechanical, dynamic and electrostatic properties of a 1-palmitoyl-2-oleoyl-sn-glycero-3-phosphocholine (POPC) bilayer in a 0.5 M aqueous NaCl solution is investigated using classical atomistic molecular dynamics simulation with different force-field descriptions for ion-ion and ion-lipid interactions. Most importantly, the repulsive Lennard–Jones parameters for the latter were modified, such that approximately similar binding of cations and anions to the lipid membrane is achieved. This was done to qualitatively improve the apparent ion-lipid binding constants obtained from simulations with the original force field (Berger lipids and GROMOS87 ions in combination with the SPC water model) in comparison to experimental data. Furthermore, various parameters characterizing membrane structure, elasticity, order and dynamics are analyzed. It is found that ion binding as observed in simulations involving the modified in comparison to the original force-field description leads to: (i) a smaller salt-induced change in the area per lipid, which is in closer agreement with the experiment; (ii) a decrease in the area compressibility and bilayer thickness to values comparable to a bilayer in pure water; (iii) lipid deuterium order parameters and lipid diffusion coefficients on nanosecond timescales that are very similar to the values for a membrane in pure water. In general, salt effects on the structural properties of a POPC bilayer in an aqueous sodium-chloride solution appear to be reproduced reasonably well by the new force-field description. An analysis of membrane-membrane disjoining pressure suggests that the smaller salt-induced change in area per lipid induced by the new force-field description is not due to the alteration of membrane-associated net charge, but must rather be understood as a consequence of ion-specific effects on the arrangement of lipid molecules.

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14 \times 10^{- 8}

^{2} \cdot

^{- 1}

for a system at 30

^{\circ}

C and 400 ×

10^{- 8}

^{2} \cdot

^{- 1}

for a system at 63

^{\circ}

C; [51] reports in-plane diffusion coefficients on the order of 15 ×

10^{- 8}

–600 ×

10^{- 8}

^{2} \cdot

^{- 1}

for a system at 60

^{\circ}

Section: Resultssupporting

confidence: 77%

“…Neutron scattering experiments deliver diffusion coefficients on a short timescale of 1–10 ps [50,51]; however, the influence of salts is unknown to date.…”

Section: Resultsmentioning

confidence: 99%

Effect of Sodium and Chloride Binding on a Lecithin Bilayer. A Molecular Dynamics Study

2017

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“…The short-time diffusion coefficient extracted from the present simulations is about 4.5 to 6.0×10 −7 cm 2 /s, a value that is roughly consistent with the estimate of 2–5×10 −7 cm 2 /s from quasi-elastic neutron scattering. 102 The long-time lateral diffusion coefficient extracted from the present simulations is about 1.0 to 2.5×10 −8 cm 2 /s. The calculated value overlaps with the broad range of 2 to 30×10 −8 cm 2 /s estimated from fluorescence recovery.…”

Section: Resultsmentioning

confidence: 54%

“…A number of experimental techniques have been employed for measuring the coefficient of lateral diffusion in lipids in bilayers, with values ranging from 0.1 to 22.4×10 −7 cm 2 /s depending on the experimental technique employed. 101–106 The short-time diffusion coefficient estimated from quasi-elastic neutron scattering experimental is on the order of 2 to 5×10 −7 cm 2 /s, 102 while the long-time diffusion coefficient display more variability. One value estimated from fluorescence recovery photobleaching (FRAP) experimental is on the order of 2 to 30×10 −8 cm 2 /s.…”

Section: Resultsmentioning

confidence: 99%

Drude Polarizable Force Field for Molecular Dynamics Simulations of Saturated and Unsaturated Zwitterionic Lipids

Chowdhary

Huang

et al. 2017

J. Chem. Theory Comput.

105

129

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Additive force fields are designed to account for induced electronic polarization in a mean-field average way using effective empirical fixed charges. The limitation of this approximation is cause for serious concerns, particularly in the case of lipid membranes, where the molecular environment undergoes dramatic variations over microscopic length scales. A polarizable force field based on the classical Drude oscillator offers a practical and computationally efficient framework for an improved representation of electrostatic interactions in molecular simulations. Building on the first-generation Drude polarizable force field for the dipalmitoylphosphatidylcholine 1,2-dipalmitoyl-sn-glycero-3-phosphocholine (DPPC) molecule, the present effort was undertaken to improve this initial model and expand the force field to a wider range of phospholipid molecules. New lipids parameterized include dimyristoylphosphatidylcholine (DMPC), dilauroylphosphatidylcholine (DLPC), 1-palmitoyl-2-oleoyl-sn-glycero-3-phosphocholine (POPC), 1,2-Dioleoyl-sn-glycero-3-phosphocholine (DOPC), dipalmitoylphosphatidylethanolamine (DPPE), 1-Palmitoyl-2-oleoyl-sn-glycero-3-phosphoethanolamine (POPE), and 1,2-Dioleoyl-sn-glycero-3-phosphoethanolamine (DOPE). The iterative optimization protocol employed in this effort led to lipid models that achieve a good balance between reproducing quantum mechanical data on model compound representative of phospholipids and reproducing a range of experimental condensed phase properties of bilayers. A parameterization strategy based on a restrained ensemble - maximum entropy methodology was used to help accurately match the experimental NMR order parameters in the polar headgroup region. All the parameters were developed to be compatible with the remainder of the Drude polarizable force field that includes water, ions, proteins, DNA and selected carbohydrates.

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“…Experimental studies using pulsed field gradient nuclear magnetic resonance, 46 single particle tracking, 47 fluorescence recovery after photobleaching, 48 or from fluorescence correlation spectroscopy 49 report values within 0.5 × 10 −7 cm 2 /s and 1 × 10 −7 cm 2 /s. Neutron scattering experiments, operating in the picosecond range, produce diffusion coefficients significantly higher, 7,8,50 in the range of 1 to 10 × 10 −7 cm 2 /s. Furthermore, there exists a controversy concerning the existence of two regimes working on the dynamics of lipids, namely (1) the fast confined motion limited by the neighboring lipids, i.e., rattling in a cage effect, 14 probably due to the wagging of lipid tails, as it has been observed for some fatty acids 51 at short timescales and (2) the slower long-range diffusion exhibited at longer timescales.…”

Section: Mechanisms Of Lipid Diffusionmentioning

confidence: 99%

Diffusion and spectroscopy of water and lipids in fully hydrated dimyristoylphosphatidylcholine bilayer membranes

Yang

Calero

Martı́

2014

The Journal of Chemical Physics

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Microscopic structure and dynamics of water and lipids in a fully hydrated dimyristoylphosphatidylcholine phospholipid lipid bilayer membrane in the liquid-crystalline phase have been analyzed with all-atom molecular dynamics simulations based on the recently parameterized CHARMM36 force field. The diffusive dynamics of the membrane lipids and of its hydration water, their reorientational motions as well as their corresponding spectral densities, related to the absorption of radiation, have been considered for the first time using the present force field. In addition, structural properties such as density and pressure profiles, a deuterium-order parameter, surface tension, and the extent of water penetration in the membrane have been analyzed. Molecular self-diffusion, reorientational motions, and spectral densities of atomic species reveal a variety of time scales playing a role in membrane dynamics. The mechanisms of lipid motion strongly depend on the time scale considered, from fast ballistic translation at the scale of picoseconds (effective diffusion coefficients of the order of 10 −5 cm 2 /s) to diffusive flow of a few lipids forming nanodomains at the scale of hundreds of nanoseconds (diffusion coefficients of the order of 10 −8 cm 2 /s). In the intermediate regime of subdiffusion, collisions with nearest neighbors prevent the lipids to achieve full diffusion. Lipid reorientations along selected directions agree well with reported nuclear magnetic resonance data and indicate two different time scales, one about 1 ns and a second one in the range of 2-8 ns. We associated the two time scales of reorientational motions with angular distributions of selected vectors. Calculated spectral densities corresponding to lipid and water reveal an overall good qualitative agreement with Fourier transform infrared spectroscopy experiments. Our simulations indicate a blue-shift of the low frequency spectral bands of hydration water as a result of its interaction with lipids. We have thoroughly analyzed the physical meaning of all spectral features from lipid atomic sites and correlated them with experimental data. Our findings include a "wagging of the tails" frequency around 30 cm −1 , which essentially corresponds to motions of the tail-group along the instantaneous plane formed by the two lipid tails, i.e., in-plane oscillations are clearly of bigger importance than those along the normal-to-the plane direction. © 2014 AIP Publishing LLC.

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Quasielastic neutron scattering measurements of fast local translational diffusion of lipid molecules in phospholipid bilayers

Cited by 78 publications

References 23 publications

Effect of Sodium and Chloride Binding on a Lecithin Bilayer. A Molecular Dynamics Study

Effect of Sodium and Chloride Binding on a Lecithin Bilayer. A Molecular Dynamics Study

Drude Polarizable Force Field for Molecular Dynamics Simulations of Saturated and Unsaturated Zwitterionic Lipids

Diffusion and spectroscopy of water and lipids in fully hydrated dimyristoylphosphatidylcholine bilayer membranes

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