Since the original observation of an ordered set of water molecules, 1, 2 termed the “spine of hydration,” within the primary hydration sphere of the minor groove of duplex B-form DNA, numerous studies have concentrated upon the function and role-(s) of minor groove hydration. In the described spine of hydration, individual water molecules bridge the N3- nitrogens of adenines and the O2-carbonyls of thymines at adjacent base pairs. A second ...