Computational Reverse-Engineering Analysis for Scattering Experiments of Assembled Binary Mixture of Nanoparticles

In this paper, we describe a computational method for analyzing results from scattering experiments on dilute solutions of supraparticles, where each supraparticle is created by the assembly of nanoparticle mixtures. Taking scattering intensity profiles and nanoparticle mixture composition and size distributions in each supraparticle as input, this computational approach called computational reverse engineering analysis for scattering experiments (CREASE) uses a genetic algorithm to output information about the structure of the assembled nanoparticles (e.g., real space pair correlation function, extent of nanoparticle mixing/segregation, sizes of domains) within a supraparticle. We validate this method by taking as input in silico scattering intensity profiles from coarse-grained molecular simulations of a binary mixture of nanoparticles, forming a close-packed structure and testing if our computational method can correctly reproduce the nanoparticle structure observed in those simulations. We test the strengths and limitations of our method using a variety of in silico scattering intensity profiles obtained from simulations of a spherical or a cubic supraparticle comprising binary nanoparticle mixtures with varying chemistries, with and without dispersity in sizes, that exhibit well-mixed to strongly segregated structures. The strengths of the presented method include its capability to analyze scattering intensity profiles even when the wavevector q range is limited, to handily provide all of the pairwise radial distribution functions, and to correctly determine the extent of segregation/mixing of the nanoparticles assembled in complex geometries.