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• W3204393947 abstract "The far-from-equilibrium alkaline dissolution of initially flat and defect-free calcite surfaces is modeled with kinetic Monte Carlo simulations of site detachment from a Kossel crystal and with scaling approaches. The surface retreat velocity is strongly dependent on the detachment rate of the highest coordination sites, which represent molecules in the middle of (101̅4) terraces. The comparison with a recent velocity estimate from digital holographic microscopy predicts the removal rate of those molecules between 2 × 10–7 and 4 × 10–6 s–1 at room temperature, which improves a previous estimate from a grain dissolution model. The activation energy for this molecular-scale process is estimated as 92 ± 6 kJ/mol (assuming the same prefactor ∼3 × 1010 s–1 of kink and step sites). The areal density of nonterrace sites (mostly steps and kinks) is also related to that removal rate, so we propose that the measurement of this density may provide independent estimates of the above quantities. Arrhenius plots of the retreat velocities obtained in high-temperature simulations predict the (macroscopic) activation energy of 69 ± 4 kJ/mol for dissolution of smooth surfaces. We also show that the scaling of the surface roughness in time and size is the same as in the Kardar–Parisi–Zhang (KPZ) equation of kinetic roughening. However, room-temperature roughening of initially smooth calcite surfaces is so slow that it is unlikely to be observed in typical experimental times and the alkaline conditions modeled here. Since the rates in acidic media are larger and arguing that the microscopic symmetries of the molecule detachment processes should be preserved, we suggest the investigation of KPZ scaling under those conditions." @default.
• W3204393947 created "2021-10-11" @default.
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• W3204393947 date "2021-09-23" @default.
• W3204393947 modified "2023-10-15" @default.
• W3204393947 title "Simulations of Dissolution of Initially Flat Calcite Surfaces: Retreat Velocity Control and Surface Roughness Scaling" @default.
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• W3204393947 doi "https://doi.org/10.1021/acsearthspacechem.1c00153" @default.
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