The phospholipid membrane is a self-assembled, dynamic molecular system that may exist alone in association with only water, or in complex systems comprised of multiple lipid types and proteins. In this dissertation the intra- and inter-molecular forces responsible for the atomistic, molecular and collective equilibrium structure and dynamics are studied by nuclear magnetic resonance spectroscopy (NMR). The multinuclear NMR measurements and various experimental techniques are able to provide data that enable the characterization of the hierarchical spatio-temporal organization of the phospholipid membrane. The experimental and theoretical studies conducted target membrane interactions ranging from model systems composed of only water and lipids, to multiple component domain forming membranes that are in association with peripheral and trans-membrane proteins. These measurements consisit of frequency spectrum lineshapes and nuclear-spin relaxation rates obtained using 2H NMR, 13C NMR, 31P NMR and 1H NMR. The changes of these experimental observables are interpreted within a statistical thermodynamic framework that allows the membrane structure, activation energies, and correlation times of motion to be determined. The cases presented demonstrate how fundamental principles of NMR spectroscopy may be applied to a host of membranes, leading to the biophysical characterization of membrane structure and dynamics.
|Advisor:||Brown, Michael F.|
|Commitee:||Cordes, Matthew J., Sanov, Andrei, Visscher, Koen|
|School:||The University of Arizona|
|School Location:||United States -- Arizona|
|Source:||DAI-B 71/05, Dissertation Abstracts International|
|Subjects:||Physical chemistry, Physics, Biophysics|
|Keywords:||Biophysics, Nuclear spin relaxation, Osmotic stress, Peripheral protein, Phospholipid membrane, Solid-state nuclear magnetic resonance|
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