TY - JOUR
T1 - The effect of hydrodynamics on the crystal nucleation of nearly hard spheres
AU - Fiorucci, Giulia
AU - Coli, Gabriele M.
AU - Padding, Johan T.
AU - Dijkstra, Marjolein
PY - 2020/2/14
Y1 - 2020/2/14
N2 - We investigate the effect of hydrodynamic interactions (HIs) on the crystal nucleation of hard-sphere colloids for varying supersaturations. We use molecular dynamics and stochastic rotation dynamics techniques to account for the HIs. For high supersaturation values, we perform brute force simulations and compute the nucleation rate, obtaining good agreement with previous studies where HIs were neglected. In order to access low supersaturation values, we use a seeding approach method and perform simulations with and without HIs. We compute the nucleation rates for the two cases and surprisingly find good agreement between them. The nucleation rate in both cases follows the trend of the previous numerical results, thereby corroborating the discrepancy between experiments and simulations. Furthermore, we investigate the amount of fivefold symmetric clusters (FSCs) in a supersaturated fluid under different physical conditions, following the idea that FSCs compete against nucleation. To this end, we explore the role of the softness of the pair interactions, different solvent viscosities, and different sedimentation rates in simulations that include HIs. We do not find significant variations in the amount of FSCs, which might reflect the irrelevance of these three features on the nucleation process.
AB - We investigate the effect of hydrodynamic interactions (HIs) on the crystal nucleation of hard-sphere colloids for varying supersaturations. We use molecular dynamics and stochastic rotation dynamics techniques to account for the HIs. For high supersaturation values, we perform brute force simulations and compute the nucleation rate, obtaining good agreement with previous studies where HIs were neglected. In order to access low supersaturation values, we use a seeding approach method and perform simulations with and without HIs. We compute the nucleation rates for the two cases and surprisingly find good agreement between them. The nucleation rate in both cases follows the trend of the previous numerical results, thereby corroborating the discrepancy between experiments and simulations. Furthermore, we investigate the amount of fivefold symmetric clusters (FSCs) in a supersaturated fluid under different physical conditions, following the idea that FSCs compete against nucleation. To this end, we explore the role of the softness of the pair interactions, different solvent viscosities, and different sedimentation rates in simulations that include HIs. We do not find significant variations in the amount of FSCs, which might reflect the irrelevance of these three features on the nucleation process.
UR - http://www.scopus.com/inward/record.url?scp=85079425876&partnerID=8YFLogxK
U2 - 10.1063/1.5137815
DO - 10.1063/1.5137815
M3 - Article
C2 - 32061217
AN - SCOPUS:85079425876
SN - 0021-9606
VL - 152
JO - Journal of Chemical Physics
JF - Journal of Chemical Physics
IS - 6
M1 - 064903
ER -