High-throughput ensemble characterization of individual core-shell nanoparticles with quantitative 3D density from XFEL single-particle imaging

TL;DR

This paper demonstrates a high-throughput method using XFEL single-particle imaging and advanced algorithms to analyze thousands of core-shell nanoparticles, revealing their 3D structures, heterogeneities, and elastic strains with atomic-level insight.

Contribution

It introduces a novel high-throughput approach combining XFEL imaging and multiple-model 3D algorithms for detailed ensemble analysis of nanoparticles.

Findings

Identified intrinsic heterogeneities in nanoparticle ensembles.

Quantified 3D morphology, facet indices, and elastic strains.

Corroborated elastic energy distribution with molecular dynamics simulations.

Abstract

The structures, as building-blocks for designing functional nanomaterials, have fueled the development of versatile nanoprobes to understand local structures of noncrystalline specimens. Progresses in analyzing structures of individual specimens with atomic scale accuracy have been notable recently. In most cases, however, only a limited number of specimens are inspected lacking statistics to represent the systems with structural inhomogeneity. Here, by employing single-particle imaging with X-ray free electron lasers and new algorithm for multiple-model 3D imaging, we succeeded in investigating several thousand specimens in a couple of hours, and identified intrinsic heterogeneities with 3D structures. Quantitative analysis has unveiled 3D morphology, facet indices and elastic strains. The 3D elastic energy distribution is further corroborated by molecular dynamics simulations to gain mechanical insight at atomic level. This work establishes a new route to high-throughput characterization of individual specimens in large ensembles, hence overcoming statistical deficiency while providing quantitative information at the nanoscale.