Remote Electronic Control of DNA-Based Reactions and Nanostructure Assembly

Abstract

The use of synthetic DNA to design and build molecular machines and well-defined structures at the nanoscale has greatly impacted the field of nanotechnology. Here we expand the current toolkit in this field by demonstrating an efficient, quantitative, and versatile approach that allows us to remotely control DNA-based reactions and DNA nanostructure self-assembly using electronic inputs. To do so we have deposited onto the surface of disposable chips different DNA input strands that upon the application of a cathodic potential can be desorbed in a remote and controlled way and trigger DNA-based reactions and DNA nanostructure self-assembly. We demonstrate that this effect is specific and versatile and allows the orthogonal control of multiple reactions and multiple structures in the same solution. Moreover, the strategy is highly tunable and can be finely modulated by varying the cathodic potential, the period of applied potential, and the density of the DNA strand on the chip surface. Our approach thus represents a versatile way to remotely control DNA-based circuits and nanostructure assembly and can allow new possible applications of DNA-based nanotools.

Base‐Sequence‐Independent Efficient Redox Switching of Self‐Assembled DNA Nanocages

“…Over the past three decades, dynamic DNA nanotechnology has attracted extensive interest due to its great potential in nanomachinery, smart drug delivery, and biocomputing . Various chemical and physical stimuli have been introduced to trigger a dynamic DNA system, including protons, heat, light, enzymes, metal ions, and redox agents . Among these studies, redox‐responsiveness has been widely pursued, owing to its physiological relevance, which might generate important biotechnical applications .…”

Stimuli‐Responsive DNA Self‐Assembly: From Principles to Applications

“…[125] Ricci and co-workers have utilized ac athodic electrodesorption of thiol-anchored DNA strands on ag old surface to initiate as ubsequent DNA assembly. [126] Different from these electrochemical processes, Simmel and co-workers have createdaDNA-origami-based nanomechanical setup integrated with an electrically manipulated robotic arm under synchronously alternated, quadrupolare lectric fields. [127] Such purely physical driving forces are especially welcome as it represents at ruly non-invasive triggering mechanism.…”

Active Self‐Assembly of Train‐Shaped DNA Nanostructures via Catalytic Hairpin Assembly Reactions

“…[16] Ricci and co-workers used pH and electronics to control the assembly of DNA tiles. [17,18] Seeman and co-workers presented a signal-passing DNA-strandexchange mechanism for the active self-assembly of DNA nanowires. [19] Schulman and co-workers used nano structured caps to terminate DNA tile assembly.…”

“…Mao and co‐workers developed a method for synchronizing two hybridization chain reactions (HCRs) assembly processes or one HCR reaction and one T‐junction cohesion to build responsive DNA nanostructures . Ricci and co‐workers used pH and electronics to control the assembly of DNA tiles . Seeman and co‐workers presented a signal‐passing DNA‐strand‐exchange mechanism for the active self‐assembly of DNA nanowires .…”