Observation of liquid-solid transition of nanoconfined water at ambient temperature

Abstract: Nanoconfined water plays an indispensable role in various phenomena in biology, chemistry, and engineering. It exhibits many abnormal properties compared to bulk water, especially under strong confinement. However, the origin of those anomalies is still elusive due to the lack of structural information on hydrogen-bonding networks. Considering the inhomogeneity of the nanocavity and the tiny amount of water molecules, conventional optical spectroscopies and nuclear magnetic resonance (NMR) fail to realize the structure analysis of nanoconfined water. Here, we addressed this issue by combining scanning probe microscopy (SPM) with advanced quantum sensing(QS) based on an atomic-size quantum sensor like nitrogen-vacancy (NV) center in diamond, which can apply the nanoscale-NMR for characterizing both the dynamics and structure of confined water at ambient conditions. We built a two-dimensional (2D) nanoconfined water system with a hexagonal-boron nitride (hBN) flake and a hydrophilic diamond surface. By using the SPM tip to measure the confinement size precisely, we observed a critical confinement size of ~2 nm, below which the water diffusion was significantly suppressed and the hydrogen-bonding network of water showed an ordered structure. Meanwhile, molecular dynamics (MD) simulation revealed a solid-like water contact layer on the diamond surface under strong confinement, which also reproduced the measured nanoscale-NMR spectra and confirmed the liquid-solid phase transition observed in the experiments. Notably, with this new SPM-QS platform, our results showed a promising way to elucidate the abnormal properties of nanoconfined water in future applications.