Seeding method for ice nucleation under shear
A Goswami and IS Dalal and JK Singh, JOURNAL OF CHEMICAL PHYSICS, 153, 094502 (2020).
Hydrodynamic flow can have complex and far-reaching consequences on the rate of homogeneous nucleation. We present a general formalism for calculating the nucleation rates of simply sheared systems. We have derived an extension to the conventional Classical Nucleation Theory, explicitly embodying the shear rate. Seeded molecular dynamics simulations form the backbone of our approach. The framework can be used for moderate supercooling, at which temperatures brute-force methods are practically infeasible. The competing energetic and kinetic effects of shear arise naturally from the equations. We show how the theory can be used to identify shear regimes of ice nucleation behavior for the mW water model, unifying disparate trends reported in the literature. At each temperature, we define a crossover shear rate in the limit of 1000 s(-1)-10 000 s(-1), beyond which the nucleation rate increases steadily up to a maximum, at the optimal shear rate. For 235 K, 240 K, 255 K, and 260 K, the optimal shear rates are in the range of approximate to 10(6) s(-1)-10(7) s(-1). For very high shear rates beyond 10(8) s(-1), nucleation is strongly inhibited. Our results indicate that the optimal shear rates have a non-monotonic dependence on temperature.
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