Molecular dynamics simulations were used to investigate the reorientation dynamics of water confined within graphite nanoslits of size less than 2 nm, where molecules formed inner and interfacial layers parallel to the confining walls. Significantly related to molecular reorientations, the hydrogen-bond (HB) network of nanoconfined water therein was scrutinized by HB configuration fractions compared to those of bulk water and the influences on interfacial-molecule orientations relative to a nearby C atom plate. The second-rank orientation time correlation functions (OTCFs) of nanoconfined water were calculated and found to follow stretched-exponential, power-law, and power-law decays in a time series. To understand this nai ̈ve behavior of reorientation relaxation, the approach of statistical mechanics was adopted in our studies. In terms of the orientation Van Hove function (OVHF), an alternative meaning was given to the second-rank OTCF, which is a measure of the deviation of the OVHF between a molecular system and free molecules in random orientations. Indicated by the OVHFs at related time scales, the stretched-exponential decay of the second-rank OTCF resulted from molecules evacuating out of HB cages formed by their neighbors. After the evacuations, the inner molecules relaxed at relatively fast rates toward random orientations, but the interfacial molecules reoriented at slow rates due to restrictions by hydrophobic interactions with graphite walls. The first power-law decay of the second-rank OTCF was attributed to the distinct relaxation rates of inner and interfacial molecules within a graphite nanoslit. When the inner molecules were completely random in orientation, the second-rank OTCFs changed to another power law decay with a power smaller than the first one.
