Abstract
Liquid water, despite its simple molecular structure, remains one of the most fascinating and complex substances. Most notably, many questions continue to exist regarding the phase transitions and anomalous properties of water, which are subtle to observe experimentally. Her; we report a sharp transition in water at 330 K unveiled through experimental measurements of the instantaneous Brownian velocity of NaYF4:Yb/Er upconversion nanoparticles in water. Our experimental investigations, corroborated by molecular dynamics simulations, elucidate a geometrical phase transition where a low-density liquid (LDL) clusters become percolated below 330 K. Around this critical temperature, we find the sizes of the LDL clusters to be similar to those of the nanoparticles, confirming the role of the upconversion nanoparticle as a powerful ruler for measuring the extensiveness of the LDL hydrogen-bond network and nanometer-scale spatial changes (20-100 nm) in liquids. Additionally, a new order parameter that unequivocally classifies water molecules into two local geometric states is introduced, providing a new tool for understanding and modeling water's many anomalous properties and phase transitions.