Issue 18, 2023

Thermally reversible pattern formation in arrays of molecular rotors

Abstract

Control over the mesoscale to microscale patterning of materials is of great interest to the soft matter community. Inspired by DNA origami rotors, we introduce a 2D nearest-neighbor lattice of spinning rotors that exhibit discrete orientational states and interactions with their neighbors. Monte Carlo simulations of rotor lattices reveal that they exhibit a variety of interesting ordering behaviors and morphologies that can be modulated through rotor design parameters. The rotor arrays exhibit diverse patterns including closed loops, radiating loops, and bricklayer structures in their ordered states. They exhibit specific heat peaks at very low temperatures for small system sizes, and some systems exhibit multiple order–disorder transitions depending on inter-rotor interaction design. We devise an energy-based order parameter and show via umbrella sampling and histogram reweighting that this order parameter captures well the order–disorder transitions occurring in these systems. We fabricate real DNA origami rotors which themselves can order via programmable DNA base-pairing interactions and demonstrate both ordered and disordered phases, illustrating how rotor lattices may be realized experimentally and used for responsive organization. This work establishes the feasibility of realizing structural nanomaterials that exhibit locally mediated microscale patterns which could have applications in sensing and precision surface patterning.

Graphical abstract: Thermally reversible pattern formation in arrays of molecular rotors

Supplementary files

Article information

Article type
Paper
Submitted
19 Oct 2022
Accepted
13 Apr 2023
First published
14 Apr 2023

Nanoscale, 2023,15, 8356-8365

Author version available

Thermally reversible pattern formation in arrays of molecular rotors

M. DeLuca, W. G. Pfeifer, B. Randoing, C. Huang, M. G. Poirier, C. E. Castro and G. Arya, Nanoscale, 2023, 15, 8356 DOI: 10.1039/D2NR05813H

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