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Molecular dynamics simulations struggle to accurately capture the local dynamics of supercooled water in "no man's land." Results show simulated water dynamics deviate significantly from experimental data at lower temperatures.

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Area of Science:

  • Physical Chemistry
  • Computational Physics
  • Materials Science

Background:

  • Supercooled water exhibits complex dynamics within the experimentally challenging "no man's land" (NML) region.
  • Molecular dynamics (MD) simulations offer insights into water's structural and dynamical properties at low temperatures.
  • Previous MD studies have explored water behavior in NML, but discrepancies with experimental data persist.

Purpose of the Study:

  • To compare the accuracy of different molecular dynamics (MD) water models in reproducing experimental quasielastic neutron scattering (QENS) data.
  • To assess the temperature dependence of MD simulation accuracy for supercooled water dynamics in the NML.
  • To identify discrepancies between simulated and experimental water dynamics at the molecular level.

Main Methods:

  • Utilized molecular dynamics (MD) simulations with one-, three-, and four-body water models.
  • Compared simulation results with experimentally measured quasielastic neutron scattering (QENS) spectra.
  • Analyzed the agreement between simulated and experimental data across a range of temperatures, focusing on the NML.

Main Results:

  • Agreement between MD simulations and experimental QENS data significantly degrades as temperature decreases toward the deeply supercooled regime.
  • The local dynamics of water molecules are poorly reproduced by the MD models, more so than macroscopic properties like the diffusion coefficient.
  • Discrepancies highlight limitations in the molecular mechanisms captured by current MD water models.

Conclusions:

  • Current MD models exhibit significant limitations in accurately describing the local dynamics of supercooled water in the NML.
  • Simulated structural and dynamical properties of water in NML should be interpreted with caution due to poor agreement with experimental data.
  • Further development of MD water models is needed to improve the representation of molecular mechanisms governing water dynamics.