Speeding up the self-assembly of a DNA nanodevice using a variety of polar solvents.

The specific recognition and programmable assembly properties make DNA a potential material for nanodevices. However, the more intelligent the nanodevice is, the more complicated the structure of the nanodevice is, which limits the speed of DNA assembly. Herein, to address this problem, we investigate the performance of DNA Strand Displacement Reaction (DSDR) in a mixture of polar organic solvents and aqueous buffer and demonstrate that the organic polar solvent can speed up DNA self-assembly efficiently. Taking DSDR in 20% ethanol as an example, first we have demonstrated that the DSDR is highly accelerated in the beginning of the reaction and it can complete 60% of replacement reactions (160% enhancement compared with aqueous buffer) in the first 300 seconds. Secondly, we calculated that the ΔΔG of the DSDR in 20% ethanol (-18.2 kcal mol(-1)) is lower than that in pure aqueous buffer (-32.6 kcal mol(-1)), while the activation energy is lowered by introducing ethanol. Finally, we proved that the DSDR on the electrode surface can also be accelerated using this simple strategy. More importantly, to test the efficacy of this approach in nanodevices with a complicated and slow DNA self-assembly process, we apply this strategy in the hybridization chain reaction (HCR) and prove the acceleration is fairly obvious in 20% ethanol, which demonstrates the feasibility of the proposed strategy in DNA nanotechnology and DNA-based biosensors.

[1]  Kristin B Cederquist,et al.  An ultrasensitive universal detector based on neutralizer displacement. , 2012, Nature chemistry.

[2]  Robert M. Dirks,et al.  Triggered amplification by hybridization chain reaction. , 2004, Proceedings of the National Academy of Sciences of the United States of America.

[3]  N. Seeman,et al.  Synthesis from DNA of a molecule with the connectivity of a cube , 1991, Nature.

[4]  Hao Yan,et al.  DNA Origami with Complex Curvatures in Three-Dimensional Space , 2011, Science.

[5]  Hao Yan,et al.  DNA-tile-directed self-assembly of quantum dots into two-dimensional nanopatterns. , 2008, Angewandte Chemie.

[6]  Jonathan Bath,et al.  Remote toehold: a mechanism for flexible control of DNA hybridization kinetics. , 2011, Journal of the American Chemical Society.

[7]  Erik Winfree,et al.  Catalyzed relaxation of a metastable DNA fuel. , 2006, Journal of the American Chemical Society.

[8]  Pamela E. Constantinou,et al.  From Molecular to Macroscopic via the Rational Design of a Self-Assembled 3D DNA Crystal , 2009, Nature.

[9]  Chunhai Fan,et al.  Target-responsive structural switching for nucleic acid-based sensors. , 2010, Accounts of chemical research.

[10]  Itamar Willner,et al.  Amplified analysis of DNA by the autonomous assembly of polymers consisting of DNAzyme wires. , 2011, Journal of the American Chemical Society.

[11]  Dongsheng Liu,et al.  A responsive hidden toehold to enable controllable DNA strand displacement reactions. , 2011, Angewandte Chemie.

[12]  Hao Yan,et al.  Charge transport within a three-dimensional DNA nanostructure framework. , 2012, Journal of the American Chemical Society.

[13]  A. Turberfield,et al.  A DNA-fuelled molecular machine made of DNA , 2022 .

[14]  Jehoshua Bruck,et al.  Neural network computation with DNA strand displacement cascades , 2011, Nature.

[15]  C. Mao,et al.  Hierarchical self-assembly of DNA into symmetric supramolecular polyhedra , 2008, Nature.

[16]  M. Egholm,et al.  Sequence-selective recognition of DNA by strand displacement with a thymine-substituted polyamide. , 1991, Science.

[17]  Ruojie Sha,et al.  A Bipedal DNA Brownian Motor with Coordinated Legs , 2009, Science.

[18]  P. Yin,et al.  Complex shapes self-assembled from single-stranded DNA tiles , 2012, Nature.

[19]  Lulu Qian,et al.  Supporting Online Material Materials and Methods Figs. S1 to S6 Tables S1 to S4 References and Notes Scaling up Digital Circuit Computation with Dna Strand Displacement Cascades , 2022 .

[20]  Harry M. T. Choi,et al.  Programming biomolecular self-assembly pathways , 2008, Nature.

[21]  Jonathan Bath,et al.  Reversible logic circuits made of DNA. , 2011, Journal of the American Chemical Society.

[22]  D. Boger,et al.  A fluorescent intercalator displacement assay for establishing DNA binding selectivity and affinity. , 2004, Accounts of chemical research.

[23]  Xi Chen,et al.  Probing spatial organization of DNA strands using enzyme-free hairpin assembly circuits. , 2012, Journal of the American Chemical Society.

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

[25]  Michael R. Diehl,et al.  Configuring robust DNA strand displacement reactions for in situ molecular analyses , 2011, Nucleic acids research.

[26]  L. Shlyakhtenko,et al.  Melting of DNA in ethanol–water solutions , 1974, Biopolymers.

[27]  N. Seeman DNA in a material world , 2003, Nature.

[28]  I. Willner,et al.  Functionalized DNA nanostructures. , 2012, Chemical reviews.

[29]  DNA and DNAzyme-mediated 2D colloidal assembly. , 2008, Journal of the American Chemical Society.

[30]  Luca Cardelli,et al.  Design and analysis of DNA strand displacement devices using probabilistic model checking , 2012, Journal of The Royal Society Interface.

[31]  N. Seeman,et al.  Operation of a DNA Robot Arm Inserted into a 2D DNA Crystalline Substrate , 2006, Science.

[32]  G. Seelig,et al.  DNA as a universal substrate for chemical kinetics , 2010, Proceedings of the National Academy of Sciences.

[33]  E. Shapiro,et al.  An autonomous molecular computer for logical control of gene expression , 2004, Nature.

[34]  N. Seeman Nucleic Acid Nanostructures and Topology. , 1998, Angewandte Chemie.

[35]  B. V. van Wees,et al.  Direct observation of the spin-dependent Peltier effect. , 2012, Nature nanotechnology.

[36]  G. Seelig,et al.  Dynamic DNA nanotechnology using strand-displacement reactions. , 2011, Nature chemistry.

[37]  Jonathan Bath,et al.  A DNA-based molecular motor that can navigate a network of tracks. , 2012, Nature nanotechnology.

[38]  A. Turberfield,et al.  DNA fuel for free-running nanomachines. , 2003, Physical review letters.

[39]  D. Y. Zhang,et al.  Engineering Entropy-Driven Reactions and Networks Catalyzed by DNA , 2007, Science.

[40]  Hao Yan,et al.  A DNA Nanostructure‐based Biomolecular Probe Carrier Platform for Electrochemical Biosensing , 2010, Advanced materials.

[41]  Hao Yan,et al.  PNA-peptide assembly in a 3D DNA nanocage at room temperature. , 2013, Journal of the American Chemical Society.

[42]  H. Pei,et al.  Self-assembled multivalent DNA nanostructures for noninvasive intracellular delivery of immunostimulatory CpG oligonucleotides. , 2011, ACS nano.

[43]  Andrew J. Turberfield,et al.  Kinetically controlled self-assembly of DNA oligomers. , 2009, Journal of the American Chemical Society.

[44]  Kevin W Plaxco,et al.  Preparation of electrode-immobilized, redox-modified oligonucleotides for electrochemical DNA and aptamer-based sensing , 2007, Nature Protocols.

[45]  D. Y. Zhang,et al.  Control of DNA strand displacement kinetics using toehold exchange. , 2009, Journal of the American Chemical Society.