title: Dielectric relaxation dynamics of water in model membranes probed by terahertz spectroscopy.
abstract: We study hydrated model membranes, consisting of stacked bilayers of 1,2-dioleoyl-sn-glycero-3-phosphocholine lipids, using terahertz time-domain spectroscopy and infrared spectroscopy. Terahertz spectroscopy enables the investigation of water dynamics, owing to its sensitivity to dielectric relaxation processes associated with water reorientation. By controlling the number of water molecules per lipid molecule in the system, we elucidate how the interplay between the model membrane and water molecules results in different water dynamics. For decreasing hydration levels, we observe the appearance of new types of water dynamics: the collective bulklike dynamics become less pronounced, whereas an increased amount of both very slowly reorienting (i.e., irrotational) and very rapidly reorienting (i.e., fast) water molecules appear. Temperature-dependent measurements reveal the interconversion between the three distinct types of water present in the system.
authors.affiliation: FOM Institute for Atomic and Molecular Physics (AMOLF), Amsterdam, The Netherlands. tielrooij@amolf.nl
authors.forename: K J
authors.initials: KJ
authors.lastname: Tielrooij
authors.forename: D
authors.initials: D
authors.lastname: Paparo
authors.forename: L
authors.initials: L
authors.lastname: Piatkowski
authors.forename: H J
authors.initials: HJ
authors.lastname: Bakker
authors.forename: M
authors.initials: M
authors.lastname: Bonn
mesh_terms: D016880:Anisotropy; D001703:Biophysics / Q000379:methods*; D006860:Hydrogen Bonding; D008051:Lipid Bilayers / Q000737:chemistry*; D008055:Lipids / Q000737:chemistry; D015233:Models, Statistical; D009502:Neutrons; D010713:Phosphatidylcholines / Q000737:chemistry; D013055:Spectrophotometry, Infrared / Q000379:methods; D013696:Temperature; D055068:Terahertz Spectroscopy / Q000379:methods*; D013997:Time Factors; D014867:Water / Q000737:chemistry*
chemical_list: D008051:Lipid Bilayers; D008055:Lipids; D010713:Phosphatidylcholines; D014867:Water; C017251:1,2-oleoylphosphatidylcholine