Reconfigurable pH-Responsive DNA Origami Lattices

Loading...
Thumbnail Image

Access rights

openAccess
publishedVersion

URL

Journal Title

Journal ISSN

Volume Title

A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä

Date

2023-06-13

Major/Subject

Mcode

Degree programme

Language

en

Pages

Series

ACS Nano, Volume 17, issue 11, pp. 11014–11022

Abstract

DNA nanotechnology enables straightforward fabrication of user-defined and nanometer-precise templates for a cornucopia of different uses. To date, most of these DNA assemblies have been static, but dynamic structures are increasingly coming into view. The programmability of DNA not only allows for encoding of the DNA object shape but also it may be equally used in defining the mechanism of action and the type of stimuli-responsiveness of the dynamic structures. However, these “robotic” features of DNA nanostructures are usually demonstrated for only small, discrete, and device-like objects rather than for collectively behaving higher-order systems. Here, we show how a large-scale, two-dimensional (2D) and pH-responsive DNA origami-based lattice can be assembled into two different configurations (“open” and “closed” states) on a mica substrate and further switched from one to the other distinct state upon a pH change of the surrounding solution. The control over these two configurations is achieved by equipping the arms of the lattice-forming DNA origami units with “pH-latches” that form Hoogsteen-type triplexes at low pH. In short, we demonstrate how the electrostatic control over the adhesion and mobility of the DNA origami units on the surface can be used both in the large lattice formation (with the help of directed polymerization) and in the conformational switching of the whole lattice. To further emphasize the feasibility of the method, we also demonstrate the formation of pH-responsive 2D gold nanoparticle lattices. We believe this work can bridge the nanometer-precise DNA origami templates and higher-order large-scale systems with the stimuli-induced dynamicity.

Description

| openaire: EC/H2020/101002258/EU//ProCrystal Funding Information: This work was supported by the Academy of Finland (project numbers 308578 and 314671), European Research Council (ERC) and ERA Chair MATTER under the European Union’s Horizon 2020 research and innovation programme (grant agreement numbers 101002258 and 856705, respectively), Aalto University School of Chemical Engineering, Victoriastiftelsen, Finnish Cultural Foundation (Maili Autio Fund), Jane and Aatos Erkko Foundation, Sigrid Jusélius Foundation, Emil Aaltonen Foundation, and Vilho, Yrjö, and Kalle Väisälä Foundation of the Finnish Academy of Science and Letters. The work was carried out under the Academy of Finland Centers of Excellence Programme (2022-2029) in Life-Inspired Hybrid Materials (LIBER), project number 346110. The authors thank E. Kaipia for assisting in preparing the DNA-functionalized AuNPs, J. V. I. Timonen for technical assistance, as well as A. Keller and H. Ijäs for fruitful discussions. The authors also acknowledge the provision of facilities and technical support by Aalto University Bioeconomy Facilities, OtaNano - Nanomicroscopy Center (Aalto-NMC) and Micronova Nanofabrication Center.

Keywords

DNA nanotechnology, DNA origami, DNA triplex, hierarchical self-assembly, metal nanoparticles, pH control

Other note

Citation

Julin, S, Linko, V & Kostiainen, M A 2023, ' Reconfigurable pH-Responsive DNA Origami Lattices ', ACS Nano, vol. 17, no. 11, pp. 11014–11022 . https://doi.org/10.1021/acsnano.3c03438