Temperature-Controlled Reconfigurable Nanoparticle Binary Superlattices

Abstract

The presence of diffusionless transformations during the assembly of DNA-functionalized particles (DFPs) is highly significant in designing reconfigurable materials whose structure and functional properties are tunable with controllable variables. In this paper, we first use a variety of computational models and techniques (including free energy methods) to address the nature of such transformations between face-centered cubic (FCC) and body-centered cubic (BCC) structures in a three-dimensional binary system of multiflavored DFPs. We find that the structural rearrangements between BCC and FCC structures are thermodynamically reversible and dependent on crystallite size. Smaller nuclei favor nonclosepacked BCC structures, whereas close-packed FCC structures are observed during the growth stage once the crystallite size exceeds a threshold value. Importantly, we show that a similar reversible transformation between BCC/FCC structures can be driven by changing temperature without introducing additional solution components, highlighting the feasibility of creating reconfigurable crystalline materials. Lastly, we validate this thermally responsive switching behavior in a DFP system with explicit DNA (un)hybridization, demonstrating our findings' applicability to experimentally realizable systems.

From Nanoscopic to Macroscopic Materials by Stimuli‐Responsive Nanoparticle Aggregation

“…Ordered NP assembly (Figure 5a) by external stimuli has become a crucial strategy in designing and fabricating ordered functional materials such as superlattices, [22,94,95] crystals, [96,97] Adv. Mater [54] Copyright 2016, Wiley-VCH.…”

“…Ordered NP assembly ( Figure a) by external stimuli has become a crucial strategy in designing and fabricating ordered functional materials such as superlattices, [ 22,94,95 ] crystals, [ 96,97 ] helical superstructures, [ 98 ] and honeycomb‐like superstructures. [ 99 ] Compared with disordered NP aggregation, ordered NP aggregation generally need a precise and rigorous assembly process, such as solvent evaporation‐induced assembly at air/liquid–liquid interfaces, destabilization‐based assembly by slow diffusion of the nonsolvent into solvent, and DNA‐guided NP assembly by programmable sequence.…”

Controlling the two components modified on nanoparticles to construct nanomaterials

“…2D). Mao et al 57 used molecular dynamics (MD) methods to study the transition of two-component DNA-modified nanoparticles between FCC and BCC crystals. They found that the structural rearrangements between the BCC and FCC structures are thermodynamically reversible and related to the crystallite size.…”

Employing Artificial Neural Networks to Identify Reaction Coordinates and Pathways for Self-Assembly

“…For example, DNA nanostructures are highly promising drug delivery vehicles because of their high biocompatibility, in vivo stability, and ability to deliver large quantities of cargo to specified targets; DNA wireframe cages can carry proteins and selectively enter cells via suitably designed receptors on the cage surface. , DNA molecules can also be employed to control the diameter and open-state lifetime of peptide pores for single-molecule analytics . The specificity offered by designing BP sequences has also been exploited for the self-assembly of “patchy” colloidal particles coated with complementary DNA strands. − …”