Exploring hydrodynamic effects in colloidal self-assembly using multiparticle collision dynamics (MPCD) simulations
ORAL
Abstract
Crystal nucleation is an important phenomenon within the broader context of colloidal self-assembly. Yet, most computational studies of colloidal crystallization have largely ignored the role of hydrodynamic interactions (HI) during nucleation, growth, and dissolution. Recent studies, however, have indicated that HI between particles, even in a quiescent liquid medium, may play a significant role during assembly, potentially impacting crystal growth kinetics [1] and gelation [2]. Jenkins et al. [3], and later Lee et al. [4] also showed that hydrodynamic correlations mediate diffusionless transformation pathways in a floppy colloidal crystal comprised of DNA-functionalized particles.
The primary technical challenge associated with including HI into particle simulations is the computational expense associated with the resolution of short-ranged (lubrication) interactions while also capturing Brownian fluctuations. Here, we explore crystallite nucleation, growth and dissolution by multiparticle collision dynamics (MPCD) [5] coupled with molecular dynamics via a discrete particle model (DP) [6]. The use of MPCD+DP is quantitatively validated using four well-defined cases: (1) a particle near a wall, (2) two-particle motion, (3) crowded environment diffusion, and (4) cluster-forming phase separation. The impact of DP resolution is investigated in all four cases. Finally, we demonstrate and analyze significant variations in colloidal crystallite dissolution and growth rates, as well as diffusionless transformation outcomes when HI are included.
[1] G. Fiorucci, G. M. Coli, J. T. Padding, and M. Dijkstra, J. Chem. Phys. 152, 064903 (2020).
[2] Z. Varga, G. Wang, and J. Swan, Soft Matter 11, 9009 (2015).
[3] I. C. Jenkins, M. T. Casey, J. T. McGinley, J. C. Crocker, and T. Sinno, Proc. Natl Acad. Sci. USA 111, 4803–4808 (2014).
[4] Y. K. Lee, X. Li, P. Perdikaris, J. C. Crocker, C. Reina, and T. Sinno, Proc. Natl. Acad. Sci. U. S. A. 117, 12700– 12706 (2020)
[5] A. Malevanets and R. Kapral, J. Chem. Phys. 110, 8605–8613 (1999).
[6] S. Poblete, A. Wysocki, G. Gompper, and R. G. Winkler, Phys. Rev. E 90, 033314 (2014).
The primary technical challenge associated with including HI into particle simulations is the computational expense associated with the resolution of short-ranged (lubrication) interactions while also capturing Brownian fluctuations. Here, we explore crystallite nucleation, growth and dissolution by multiparticle collision dynamics (MPCD) [5] coupled with molecular dynamics via a discrete particle model (DP) [6]. The use of MPCD+DP is quantitatively validated using four well-defined cases: (1) a particle near a wall, (2) two-particle motion, (3) crowded environment diffusion, and (4) cluster-forming phase separation. The impact of DP resolution is investigated in all four cases. Finally, we demonstrate and analyze significant variations in colloidal crystallite dissolution and growth rates, as well as diffusionless transformation outcomes when HI are included.
[1] G. Fiorucci, G. M. Coli, J. T. Padding, and M. Dijkstra, J. Chem. Phys. 152, 064903 (2020).
[2] Z. Varga, G. Wang, and J. Swan, Soft Matter 11, 9009 (2015).
[3] I. C. Jenkins, M. T. Casey, J. T. McGinley, J. C. Crocker, and T. Sinno, Proc. Natl Acad. Sci. USA 111, 4803–4808 (2014).
[4] Y. K. Lee, X. Li, P. Perdikaris, J. C. Crocker, C. Reina, and T. Sinno, Proc. Natl. Acad. Sci. U. S. A. 117, 12700– 12706 (2020)
[5] A. Malevanets and R. Kapral, J. Chem. Phys. 110, 8605–8613 (1999).
[6] S. Poblete, A. Wysocki, G. Gompper, and R. G. Winkler, Phys. Rev. E 90, 033314 (2014).
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Presenters
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Ying-Shuo Peng
University of Pennsylvania
Authors
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Ying-Shuo Peng
University of Pennsylvania
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Talid Sinno
University of Pennsylvania