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Seeding method for ice nucleation under shear.

Amrita Goswami1, Indranil Saha Dalal1, Jayant K Singh1

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Hydrodynamic flow significantly impacts homogeneous nucleation rates. This study introduces a new theory and simulations to precisely calculate nucleation rates in sheared systems, revealing optimal shear rates for ice formation.

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Area of Science:

  • Thermodynamics and Fluid Dynamics
  • Materials Science and Crystallization
  • Computational Physics

Background:

  • Homogeneous nucleation rates are sensitive to hydrodynamic flow, but theoretical frameworks are limited.
  • Classical Nucleation Theory (CNT) does not fully account for shear effects.
  • Understanding shear effects is crucial for various applications, including materials processing and atmospheric science.

Purpose of the Study:

  • To develop a general theoretical formalism for calculating nucleation rates in simply sheared systems.
  • To extend Classical Nucleation Theory by explicitly incorporating shear rate.
  • To investigate the influence of shear on ice nucleation behavior using a specific water model.

Main Methods:

  • Extension of Classical Nucleation Theory to include shear rate.
  • Seeded molecular dynamics simulations.
  • Analysis of competing energetic and kinetic effects of shear.

Main Results:

  • Identified shear regimes for ice nucleation in the mW water model.
  • Defined crossover shear rates (1000-10000 s⁻¹) where nucleation rate increases with shear.
  • Determined optimal shear rates (≈10⁶-10⁷ s⁻¹) for maximum nucleation at specific temperatures (235-260 K).
  • Observed strong nucleation inhibition at very high shear rates (>10⁸ s⁻¹).
  • Found a non-monotonic temperature dependence for optimal shear rates.

Conclusions:

  • The developed formalism accurately captures shear-induced changes in nucleation rates.
  • Shear can be used to control and optimize ice nucleation.
  • The findings unify disparate experimental trends and provide a predictive framework for shear-influenced nucleation.