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Area of Science:

  • Physical Chemistry
  • Soft Matter Physics
  • Thermodynamics

Background:

  • Water exhibits anomalous kinetic and thermodynamic properties, particularly in its supercooled state.
  • These anomalies are often linked to structural changes and suggest a singularity around 225 K.
  • Previous simulations aligned with mode-coupling theory for structural relaxation, but experimental validation was lacking.

Purpose of the Study:

  • To experimentally characterize the structural relaxation in supercooled water.
  • To provide unambiguous evidence for or against predictions from simple mode-coupling theory.
  • To elucidate the origin of the anomalous properties of water.

Main Methods:

  • Time-resolved optical Kerr effect measurements were employed.
  • The study focused on liquid and weakly supercooled water.
  • Experimental data was compared with predictions from simple mode-coupling theory.

Main Results:

  • Experimental results unambiguously confirmed the predictions of simple mode-coupling theory for structural relaxation.
  • The behavior of liquid and weakly supercooled water aligns with this dynamical model.
  • No evidence for a thermodynamic origin of the singularity was found.

Conclusions:

  • The singularity in water's properties is likely a purely dynamical transition.
  • Anomalous behavior in weakly supercooled water can be explained by a dynamic model alone.
  • Water behaves similarly to other fragile glass-forming molecular liquids.