Spatiotemporal control of DNA-based chemical reaction network via electrochemical activation in microfluidics

In recent years, DNA computing frameworks have been developed to create dynamical systems which can be used for information processing. These emerging synthetic biochemistry tools can be leveraged to gain a better understanding of fundamental biology but can also be implemented in biosensors and unconventional computing. Most of the efforts so far have focused on changing the topologies of DNA molecular networks or scaling them up. Several issues have thus received little attention and remain to be solved to turn them into real life technologies. In particular, the ability to easily interact in real-time with them is a key requirement. The previous attempts to achieve this aim have used microfluidic approaches, such as valves, which are cumbersome. We show that electrochemical triggering using DNA-grafted micro-fabricated gold electrodes can be used to give instructions to these molecular systems. We demonstrate how this approach can be used to release at specific times and locations DNA- based instructions. In particular, we trigger reaction-diffusion autocatalytic fronts in microfluidic channels. While limited by the stability of the Au-S bond, this easy to implement, versatile and scalable technique can be used in any biology laboratory to provide new ways to interact with any DNA-based computing framework.

[1]  T. Fujii,et al.  Dynamic DNA-toolbox reaction circuits: a walkthrough. , 2014, Methods.

[2]  G Gines,et al.  Microscopic agents programmed by DNA circuits. , 2017, Nature nanotechnology.

[3]  E. Shapiro,et al.  Programmable and autonomous computing machine made of biomolecules , 2001, Nature.

[4]  Marc Tornow,et al.  Controlling the surface density of DNA on gold by electrically induced desorption. , 2007, Biosensors & bioelectronics.

[5]  Teruo Fujii,et al.  Bottom-up construction of in vitro switchable memories , 2012, Proceedings of the National Academy of Sciences.

[6]  Erik Winfree,et al.  Enzyme-free nucleic acid dynamical systems , 2017, Science.

[7]  Sabine Szunerits,et al.  Characterization of peptide attachment on silicon nanowires by X-ray photoelectron spectroscopy and mass spectrometry. , 2017, The Analyst.

[8]  Kevin W Plaxco,et al.  Linear, redox modified DNA probes as electrochemical DNA sensors. , 2007, Chemical communications.

[9]  C. Mirkin,et al.  A fluorescence-based method for determining the surface coverage and hybridization efficiency of thiol-capped oligonucleotides bound to gold thin films and nanoparticles. , 2000, Analytical chemistry.

[10]  Yannick Rondelez,et al.  Synthesis and materialization of a reaction–diffusion French flag pattern , 2017, Nature Chemistry.

[11]  G. Seelig,et al.  Enzyme-Free Nucleic Acid Logic Circuits , 2022 .

[12]  L M Adleman,et al.  Molecular computation of solutions to combinatorial problems. , 1994, Science.

[13]  Teruo Fujii,et al.  Nucleic acids for the rational design of reaction circuits. , 2013, Current opinion in biotechnology.

[14]  Teruo Fujii,et al.  Spatial waves in synthetic biochemical networks. , 2013, Journal of the American Chemical Society.

[15]  Yiping Cui,et al.  Remote-Controlled DNA Release from Fe3O4@Au Nanoparticles Using an Alternating Electromagnetic Field. , 2015, Journal of biomedical nanotechnology.

[16]  Wilhelm T S Huck,et al.  Grip on complexity in chemical reaction networks , 2017, Beilstein journal of organic chemistry.

[17]  Teruo Fujii,et al.  Programming an in vitro DNA oscillator using a molecular networking strategy , 2011, Molecular Systems Biology.

[18]  Feng Li,et al.  Thermal Stability of DNA Functionalized Gold Nanoparticles , 2013, Bioconjugate chemistry.

[19]  Y. Sakai,et al.  Programming an in vitro DNA oscillator using a molecular networking strategy , 2011, Molecular systems biology.

[20]  Y. Rondelez,et al.  Pursuit-and-Evasion Reaction-Diffusion Waves in Microreactors with Tailored Geometry. , 2015, The journal of physical chemistry. B.

[21]  G. Church,et al.  Next-Generation Digital Information Storage in DNA , 2012, Science.

[22]  Yannick Rondelez,et al.  A Viewpoint on : Synthesis of Programmable Reaction-Diffusion Fronts Using DNA Catalyzers , 2015 .

[23]  Kevin W Eliceiri,et al.  NIH Image to ImageJ: 25 years of image analysis , 2012, Nature Methods.

[24]  A. Barabasi,et al.  Network biology: understanding the cell's functional organization , 2004, Nature Reviews Genetics.