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Area of Science:

  • Physical Chemistry
  • Materials Science
  • Atmospheric Science

Background:

  • Heterogeneous ice nucleation is crucial in nature but its kinetics are poorly understood.
  • Current theories emphasize minimal lattice mismatch between nucleator and ice.
  • This view is challenged by observations on various substrates.

Purpose of the Study:

  • To investigate the microscopic factors governing heterogeneous ice nucleation kinetics.
  • To re-evaluate the role of lattice mismatch versus other factors.
  • To identify a fundamental descriptor for ice nucleation efficiency.

Main Methods:

  • Utilized forward flux sampling (FFS) simulations.
  • Analyzed interfacial water properties on graphene substrates.
  • Correlated nucleation rates with surface characteristics like hydrophilicity and lattice mismatch.

Main Results:

  • The criterion of minimal lattice mismatch breaks down for graphene.
  • Highest ice nucleation rates occur at specific lattice constants, not matching ice or critical nucleus.
  • Interfacial water-ice density difference in the first contact layer is identified as the key factor.
  • Enhanced hydrophilicity leads to negative lattice mismatch, minimizing density difference and maximizing nucleation rate.

Conclusions:

  • The interfacial water-ice density difference is a fundamental descriptor of ice nucleation efficiency.
  • This density difference exhibits a global correlation with nucleation rates across varying surface properties.
  • Density difference, rather than lattice match, provides a more accurate and transferable understanding of heterogeneous ice nucleation.