Steady-like topology of the dynamical hydrogen bond network in supercooled water
We investigate the link between topology of the hydrogen bond network (HBN) and large-scale density fluctuations in water from ambient conditions to the glassy state. We observe a transition from a temperature-dependent topology at high temperatures, to a steady-like topology below the Widom temperature TW ∼ 220 K signaling the fragile-to-strong crossover and the maximum in structural fluctuations. As a consequence of the steady topology, the network suppresses large-scale density fluctuations much more efficiently than at higher temperatures. Below TW, the contribution of coordination defects of the kind A2D1 (two acceptors and one donor) to the kinetics of the HBN becomes progressively more pronounced, suggesting that A2D1 configurations may represent the main source of dynamical heterogeneities. Below the vitrification temperature, the freezing of rotational and translational degrees of freedom allow for an enhanced suppression of large-scale density fluctuations and the sample reaches the edges of nearly hyperuniformity. The formed network still hosts coordination defects, hence implying that nearly hyperuniformity goes beyond the classical continuous random network paradigm of tetrahedral networks and can emerge in scenarios much more complex than previously assumed. Our results unveil a hitherto undisclosed link between network topology and properties of water essential for better understanding water’s rich and complex nature. Beyond implications for water, our findings pave the way to a better understanding of the physics of supercooled liquids and disordered hyperuniform networks at large.