Orthogonally Photocontrolled Non-Autonomous DNA Walker.

There is considerable interest in developing progressively moving devices on the nanoscale, with the aim of using them as parts of programmable therapeutics, smart materials, and nanofactories. Present here is an entirely light-induced DNA walker based on orthogonal photocontrol. Implementing two azobenzene derivatives, S-DM-Azo and DM-Azo, enabled precise coordination of strand displacement reactions that powered a biped walker and guided it along a defined track in a non-autonomous way. This unprecedented type of molecular walker design offers high precision control over the movement in back-and-forth directions as desired, and is regulated solely by the sequence of the irradiation wavelengths. This concept may open new avenues for advancing non-autonomous progressive molecular motors, ultimately facilitating their application at the nanoscale.

[1]  Weihong Tan,et al.  An autonomous and controllable light-driven DNA walking device. , 2012, Angewandte Chemie.

[2]  P. Yin,et al.  A DNAzyme that walks processively and autonomously along a one-dimensional track. , 2005, Angewandte Chemie.

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

[4]  A. Romieu,et al.  Bioconjugatable azo-based dark-quencher dyes: synthesis and application to protease-activatable far-red fluorescent probes. , 2013, Chemistry.

[5]  H. Asanuma,et al.  A photon-fueled DNA nanodevice that contains two different photoswitches. , 2012, Angewandte Chemie.

[6]  Jun Liu,et al.  Orthogonal navigation of multiple visible-light-driven artificial microswimmers , 2017, Nature Communications.

[7]  Julián Valero,et al.  A bio-hybrid DNA rotor/stator nanoengine that moves along predefined tracks , 2018, Nature Nanotechnology.

[8]  Juan Cheng,et al.  From bistate molecular switches to self-directed track-walking nanomotors. , 2014, ACS nano.

[9]  Hiroyuki Asanuma,et al.  Photoregulation der Bildung und Dissoziation eines DNA‐Duplexes durch cis‐trans‐Isomerisierung einer Azobenzoleinheit , 1999 .

[10]  Hui Zhao,et al.  Orthogonal light-induced self-assembly of nanoparticles using differently substituted azobenzenes. , 2015, Angewandte Chemie.

[11]  Jeffrey S. Hannam,et al.  Expanding the Toolbox of Photoswitches for DNA Nanotechnology Using Arylazopyrazoles. , 2018, Chemistry.

[12]  Arne Gennerich,et al.  Walking the walk: how kinesin and dynein coordinate their steps. , 2009, Current opinion in cell biology.

[13]  H. Asanuma,et al.  Photoregulation of the Formation and Dissociation of a DNA Duplex by Using the cis-trans Isomerization of Azobenzene. , 1999, Angewandte Chemie.

[14]  Weihong Tan,et al.  Building a nanostructure with reversible motions using photonic energy. , 2012, ACS nano.

[15]  M. Schliwa,et al.  Molecular motors , 2003, Nature.

[16]  Michael Famulok,et al.  Reversible Light Switch for Macrocycle Mobility in a DNA Rotaxane , 2012, Journal of the American Chemical Society.

[17]  M. Famulok,et al.  Temporal and Reversible Control of a DNAzyme by Orthogonal Photoswitching. , 2018, Journal of the American Chemical Society.

[18]  Xingguo Liang,et al.  Photo-regulation of DNA function by azobenzene-tethered oligonucleotides. , 2003, Nucleic acids research. Supplement.

[19]  Ruchuan Liu,et al.  Bipedal nanowalker by pure physical mechanisms. , 2012, Physical review letters.

[20]  Pete Crisalli,et al.  Multi-path quenchers: efficient quenching of common fluorophores. , 2011, Bioconjugate chemistry.

[21]  D. Leigh,et al.  Synthetic molecular walkers. , 2014, Topics in current chemistry.

[22]  Xingguo Liang,et al.  Effect of the ortho modification of azobenzene on the photoregulatory efficiency of DNA hybridization and the thermal stability of its cis form. , 2010, Chemistry.

[23]  H. Asanuma,et al.  2',6'-Dimethylazobenzene as an efficient and thermo-stable photo-regulator for the photoregulation of DNA hybridization. , 2007, Chemical communications.

[24]  Erik Winfree,et al.  Molecular robots guided by prescriptive landscapes , 2010, Nature.

[25]  Julián Valero,et al.  Allosteric Control of Oxidative Catalysis by a DNA Rotaxane Nanostructure. , 2017, Journal of the American Chemical Society.

[26]  David A Leigh,et al.  Walking molecules. , 2011, Chemical Society reviews.

[27]  Michael P. Sheetz,et al.  Identification of a novel force-generating protein, kinesin, involved in microtubule-based motility , 1985, Cell.

[28]  B. Feringa,et al.  Orthogonal photoswitching in a multifunctional molecular system , 2016, Nature Communications.

[29]  Jie Chao,et al.  DNA-based nanoscale walking devices and their applications , 2017 .

[30]  C. Bochet,et al.  Wavelength-controlled orthogonal photolysis of protecting groups. , 2002, The Journal of organic chemistry.

[31]  Itamar Willner,et al.  DNA machines: bipedal walker and stepper. , 2011, Nano letters.

[32]  N. Pierce,et al.  A synthetic DNA walker for molecular transport. , 2004, Journal of the American Chemical Society.