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DNAzyme- and light-induced dissipative and gated DNA networks.

ABSTRACT: Nucleic acid-based dissipative, out-of-equilibrium systems are introduced as functional assemblies emulating transient dissipative biological transformations. One system involves a Pb²⁺-ion-dependent DNAzyme fuel strand-driven network leading to the transient cleavage of the fuel strand to "waste" products. Applying the Pb²⁺-ion-dependent DNAzyme to two competitive fuel strand-driven systems yields two parallel operating networks. Blocking the competitively operating networks with selective inhibitors leads, however, to gated transient operation of dictated networks, yielding gated catalytic operations. A second system introduces a "non-waste" generating out-of-equilibrium, dissipative network driven by light. The system consists of a trans-azobenzene-functionalized photoactive module that is reconfigured by light to an intermediary state consisting of cis-azobenzene units that are thermally recovered to the original trans-azobenzene-modified module. The cyclic transient photoinduced operation of the device is demonstrated. The kinetic simulation of the systems allows the prediction of the transient behavior of the networks under different auxiliary conditions.

SUBMITTER: Wang J

PROVIDER: S-EPMC8386649 | biostudies-literature | 2021 Aug

REPOSITORIES: biostudies-literature

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DNAzyme- and light-induced dissipative and gated DNA networks.

Wang Jianbang J Li Zhenzhen Z Zhou Zhixin Z Ouyang Yu Y Zhang Junji J Ma Xiang X Tian He H Willner Itamar I

Chemical science 20210720 33

Nucleic acid-based dissipative, out-of-equilibrium systems are introduced as functional assemblies emulating transient dissipative biological transformations. One system involves a Pb<sup>2+</sup>-ion-dependent DNAzyme fuel strand-driven network leading to the transient cleavage of the fuel strand to "waste" products. Applying the Pb<sup>2+</sup>-ion-dependent DNAzyme to two competitive fuel strand-driven systems yields two parallel operating networks. Blocking the competitively operating networ ...[more]

PMID: 34522318

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Project description:Dissipative self-assembly, one of fundamentally important out-of-equilibrium self-assembly systems, can serve as a controllable platform to exhibit temporal processes for various non-stimulus responsive properties. However, construction of light-fueled dissipative self-assembly structures with transformable morphology to modulate non-photoresponsive properties remains a great challenge. Here, we report a light-activated photodeformable dissipative self-assembly system in aqueous solution as metastable fluorescent palette. Zwitterionic sulfonato-merocyanine is employed as a light-induced amphiphile to co-assemble with polyethyleneimine after light irradiation. The formed spherical nanoparticles spontaneously transform into cuboid ones in the dark with simultaneous variation of the particle sizes. Then the two kinds of nanoparticles can reversibly interconvert to each other by periodical light irradiation and thermal relaxation. Furthermore, after loading different fluorophores exhibiting red, green, blue emissions and their mixtures, all these fluorescent dissipative deformable nanoparticles display time-dependent fluorescence variation with wide range of colors. Owing to the excellent performance of photodeformable dissipative assembly platform, the light-controlled fluorescence has achieved a 358-fold enhancement. Therefore, exposing the nanoparticles loaded with fluorophores to light in a spatially controlled manner allows us to draw multicolored fluorescent images that spontaneously disappeared after a specific period of time. Dissipative self-assembly can serve as a controllable platform to exhibit temporal processes for various non-stimulus responsive properties but construction of light-fueled dissipative self-assembly structures with transformable morphology to modulate non-photoresponsive properties remains a challenge. Here, the authors report a light-activated photodeformable dissipative self-assembly system in aqueous solution as metastable fluorescent platform.

Dataset Information

DNAzyme- and light-induced dissipative and gated DNA networks.

Publications

DNAzyme- and light-induced dissipative and gated DNA networks.

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