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Register a new userMolecular motions in lipid bilayers studied by the neutron backscattering technique
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Maikel Rheinstaedter
Publication date
2005
fields
Physics
and research's language is
English
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We report a high energy-resolution neutron backscattering study to investigate slow motions on nanosecond time scales in highly oriented solid supported phospholipid bilayers of the model system DMPC -d54 (deuterated 1,2-dimyristoyl-sn-glycero-3-phoshatidylcholine), hydrated with heavy water. This technique allows to discriminate the onset of mobility at different length scales for the different molecular components, as e.g.@ the lipid acyl-chains and the hydration water in between the membrane stacks, respectively, and provides a benchmark test regarding the feasibility of neutron backscattering investigations on these sample systems. We discuss freezing of the lipid acyl-chains, as observed by this technique, and observe a second freezing transition which we attribute to the hydration water.
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Lipid membranes in a physiological context cannot be understood without taking into account their mobile environment. Here, we report on a high energy-resolution neutron backscattering study to investigate slow motions on nanosecond time scales in highly oriented solid supported phospholipid bilayers of the model system DMPC -d54 (deuterated 1,2-dimyristoyl-sn-glycero-3-phoshatidylcholine). This technique allows discriminating the Q-dependent onset of mobility and provides a benchmark test regarding the feasibility of dynamical neutron scattering investigations on these sample systems. Apart from freezing of the lipid acyl-chains, we could observe a second freezing temperature that we attribute to the hydration water in between the membrane stacks. The freezing is lowered several degrees as compared to (heavy) bulk water.
We report a high energy-resolution neutron backscattering study to investigate slow motions on nanosecond time scales in highly oriented solid supported phospholipid bilayers of the model system DMPC -d54 (deuterated 1,2-dimyristoyl-sn-glycero-3-phoshatidylcholine), hydrated with heavy water. Wave vector resolved quasi-elastic neutron scattering (QENS) is used to determine relaxation times $tau$, which can be associated with different molecular components, i.e., the lipid acyl chains and the interstitial water molecules in the different phases of the model membrane system. The inelastic data are complemented both by energy resolved and energy integrated in-situ diffraction. From a combined analysis of the inelastic data in the energy and time domain, the respective character of the relaxation, i.e., the exponent of the exponential decay is also determined. From this analysis we quantify two relaxation processes. We associate the fast relaxation with translational diffusion of lipid and water molecules while the slow process likely stems from collective dynamics.
We have studied the collective short wavelength dynamics in deuterated DMPC bilayers by inelastic neutron scattering. The corresponding dispersion relation $hbaromega$(Q) is presented for the gel and fluid phase of this model system. The temperature dependence of the inelastic excitations indicates a phase coexistence between the two phases over a broad range and leads to a different assignment of excitations than that reported in a preceding inelastic x-ray scattering study [Phys. Rev. Lett. {bf 86}, 740 (2001)]. As a consequence, we find that the minimum in the dispersion relation is actually deeper in the gel than in the fluid phase. Finally, we can clearly identify an additional non-dispersive (optical) mode predicted by Molecular Dynamics (MD) simulations [Phys. Rev. Lett. {bf 87}, 238101 (2001)].
This paper has been withdrawn.
We report on atomistic simulations of DPPC lipid monolayers using the CHARMM36 lipid force field and four-point OPC water model. The entire two-phase region where domains of the `liquid-condensed (LC) phase coexist with domains of the `liquid-expanded (LE) phase has been explored. The simulations are long enough that the complete phase-transition stage, with two domains coexisting in the monolayer, is reached in all cases. Also, system sizes used are larger than in previous works. As expected, domains of the minority phase are elongated, emphasizing the importance of anisotropic van der Waals and/or electrostatic dipolar interactions in the monolayer plane. The molecular structure is quantified in terms of distribution functions for the hydrocarbon chains and the PN dipoles. In contrast to previous work, where average distributions are calculated, distributions are here extracted for each of the coexisting phases by first identifying lipid molecules that belong to either LC or LE regions. The three-dimensional distributions show that the average tilt angle of the chains with respect to the normal outward direction is $(39.0pm 0.1)^{circ}$ in the LC phase. % and $(48.1pm 0.5)^{circ}$ in the LC phase. In the case of the PN dipoles the distributions indicate a tilt angle of $(110.8pm 0.5)^{circ}$ in the LC phase and $(112.5pm 0.5)^{circ}$ in the LE phase. These results are quantitatively different from previous works, which indicated a smaller normal component of the PN dipole. Also, the distributions of the monolayer-projected chains and PN dipoles have been calculated. Chain distributions peak along a particular direction in the LC domains, while they are uniform in the LE phase. Long-range ordering associated with the projected PN dipoles is absent in both phases.
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