Stress accumulation versus shape flattening in frustrated, warped-jigsaw particle assemblies

TL;DR

This paper introduces a novel 2D particle shape called 'warped jigsaw' that causes frustration in assembly, leading to self-limiting ribbon sizes through elastic stress mechanisms, with implications for designing finite-sized nanostructures.

Contribution

It proposes and analyzes a new particle design that induces shape frustration and elastic stress accumulation, controlling assembly size limits.

Findings

WJ particles favor anisotropic ribbon assemblies.

Self-limiting size depends on interaction range and shape misfit.

Elastic mode crossover determines maximum assembly size.

Abstract

Geometrically frustrated assembly has emerged as an attractive paradigm for understanding and engineering assemblies with self-limiting, finite equilibrium dimensions. We propose and study a novel 2D particle based on a so-called "warped jigsaw" (WJ) shape design: directional bonds in a tapered particle favor curvature along multi-particle rows that frustrate 2D lattice order. We investigate how large-scale intra-assembly stress gradients emerge from the microscopic properties of the particles using a combination of numerical simulation and continuum elasticity. WJ particles can favor anisotropic ribbon assemblies, whose lateral width may be self-limiting depending on the relative strength of cohesive to elastic forces in the assembly, which we show to be controlled by the range of interactions and degree of shape misfit. The upper limits of self-limited size are controlled by the crossover between two elastic modes in assembly: the accumulation of shear with increasing width at small widths giving way to unbending of preferred row curvature, permitting assembly to grow to unlimited sizes. We show that the stiffness controlling distinct elastic modes is governed by combination and placement of repulsive and attractive binding regions, providing a means to extend the range of accumulating stress to sizes that are far in excess of the single particle size, which we corroborate via numerical studies of discrete particles of variable interactions. Lastly, we relate the ground-state energetics of the model to lower and upper limits on equilibrium assembly size control set by the fluctuations of width along the ribbon boundary.