The dynamics of water between highly oriented multilayers of 1,2-dipalmitoyl-sn-glycero-3-phosphocholine (DPPC) has been studied in two time domains at different hydration levels. Incoherent quasielastic neutron scattering (QENS) and deuterium-nuclear magnetic resonance (NMR) longitudinal (T-1) relaxation were employed to investigate both the high-frequency motions of water (10(-9)-10(-11) s time scale) and their anisotropy, while 2H-NMR transverse (T-2) relaxation was used for obtaining information on low frequency dynamical processes (microsecond time scale). Our results show that high frequency dynamics (picosecond-time scale) at low hydration (three to four water molecules per lipid) can be understood solely as a uniaxial rotation of the water molecules tightly bound to DPPC head groups with a correlation time tau(rot) approximate to 62 ps at 55 degrees C and a rotational radius of 1 +/- 0.1 Angstrom, but with no detectable translational degrees of freedom. The 2H-NMR T-1 data (nanosecond-time scale) can be explained satisfactorily on the basis of fast rotations with the correlation time above and a slower reorientation of the rotational axis (correlation time tau 1 approximate to 6 ns). Both QENS and 2H-NMR T-1 measurements provide an apparent activation energy of E(a) = 32 +/- 1.0 kJ/mol for this process. Increasing the hydration level of the multilayers leaves the rotational motion essentially unchanged, but enables additional translational motion which can be considered as a jump diffusion process (diffusion coefficient D = 16 +/- 1X10(-10) m(2)/s at 44 degrees C and a mean residence time of tau(o) = 2.0 +/- 0.5 ps) of nonbound water. It is interesting to note that this diffusion is completely isotropic on the characteristic length scale of this QENS experiment (equal to or less than 10 Angstrom). Temperature variation shows that the phase state of the lipids has no significant effect on the high frequency dynamics of the water molecules. Measurements of the 2H-NMR quadrupolar splitting of water (D2O) at temperatures around the phase transition temperature T-m of the oriented DPPC multilayers clearly show a coexistence of the crystalline L(beta’) phase and of the fluid L(alpha) phase over a range of up to 4 degrees C at both sides of T-m. The intermediate P-beta’ ("ripple") phase is suppressed as we worked at hydration levels below saturation. In the coexistence range, exchange of water takes place between crystalline and fluid lipid domains due to water diffusion. This exchange causes a pronounced minimum of the 2H-NMR transverse relaxation time T-2 at T-m since this low frequency process satisfies approximately a critical damping condition for a two-site chemical exchange process.