Coarse-Grained Many-Body Potentials of Ligand-Stabilized Nanoparticles from Machine-Learned Mean Forces

G Giunta and G Campos-Villalobos and M Dijkstra, ACS NANO, 17, 23391-23404 (2023).

DOI: 10.1021/acsnano.3c04162

Colloidal nanoparticles self-assemble into a variety of superstructures with distinctive optical, structural, and electronic properties. These nanoparticles are usually stabilized by a capping layer of organic ligands to prevent aggregation in the solvent. When the ligands are sufficiently long compared to the dimensions of the nanocrystal cores, the effective coarse-grained forces between pairs of nanoparticles are largely affected by the presence of neighboring particles. In order to efficiently investigate the self-assembly behavior of these complex colloidal systems, we propose a machine-learning approach to construct effective coarse-grained many-body interaction potentials. The multiscale methodology presented in this work constitutes a general bottom-up coarse-graining strategy where the coarse-grained forces acting on coarse-grained sites are extracted from measuring the vectorial mean forces on these sites in reference fine-grained simulations. These effective coarse-grained forces, i.e., gradients of the potential of mean force or of the free-energy surface, are represented by a simple linear model in terms of gradients of structural descriptors, which are scalar functions that are rotationally invariant. In this way, we also directly obtain the free-energy surface of the coarse-grained model as a function of all coarse-grained coordinates. We expect that this simple yet accurate coarse-graining framework for the many-body potential of mean force will enable the characterization, understanding, and prediction of the structure and phase behavior of relevant soft-matter systems by direct simulations. The key advantage of this method is its generality, which allows it to be applicable to a broad range of systems. To demonstrate the generality of our method, we also apply it to a colloid-polymer model system, where coarse-grained many-body interactions are pronounced.

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