We have performed broad-band spectroscopic investigations of vibrational and relaxational excitations of water molecules confined to nanocages within artificial beryl and mineral cordierite crystals. Signatures of quantum critical phenomena within the H2O molecular network are registered in beryl. In cordierite, a density functional analysis is applied to reconstruct the potential energy landscape experienced by H2O molecules, revealing a pronounced anisotropy with a potential well of about 10 meV for the molecular dipole moment aligned along the b-axis. This anisotropy leads to a strongly temperature dependent and anisotropic relaxational response of the dipoles at radiofrequencies with the activation energies corresponding to the barriers of the rotational potential. At T ≈ 3 K, we identify signatures of a transition into a glassy state composed by clusters of H2O dipoles. Rich set of anisotropic and temperature-dependent excitations are observed in the terahertz frequency range which we associate with rotational/translational vibrations.