This thesis presents a highly innovative study of the ultrafast
structural and vibrational dynamics of hydrated phospholipids, the
basic constituents of cell membranes. As a novel approach to the
water-phospholipid interface, the author studies phosphate
vibrations using the most advanced methods of nonlinear vibrational
spectroscopy, including femtosecond two-dimensional infrared
spectroscopy. He shows for the first time that the structure of
interfacial water undergoes very limited fluctuations on a 300 fs
time scale and that the lifetimes of hydrogen bonds with the
phospholipid are typically longer than 10 ps. Such properties
originate from the steric hindrance of water fluctuations at the
interface and the orienting action of strong electric fields from
the phospholipid head group dipoles. In an extensive series of
additional experiments, the vibrational lifetimes of the different
vibrations and the processes of energy dissipation are elucidated
in detail.
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