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      DNA-Driven Dynamic Assembly/Disassembly of Inorganic Nanocrystals for Biomedical Imaging


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          DNA-mediated programming is emerging as an effective technology that enables controlled dynamic assembly/disassembly of inorganic nanocrystals (NC) with precise numbers and spatial locations for biomedical imaging applications. In this review, we will begin with a brief overview of the rules of NC dynamic assembly driven by DNA ligands, and the research progress on the relationship between NC assembly modes and their biomedical imaging performance. Then, we will give examples on how the driven program is designed by different interactions through the configuration switching of DNA-NC conjugates for biomedical applications. Finally, we will conclude with the current challenges and future perspectives of this emerging field. Hopefully, this review will deepen our knowledge on the DNA-guided precise assembly of NCs, which may further inspire the future development of smart chemical imaging devices and high-performance biomedical imaging probes.

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          A DNA-based method for rationally assembling nanoparticles into macroscopic materials.

          Colloidal particles of metals and semiconductors have potentially useful optical, optoelectronic and material properties that derive from their small (nanoscopic) size. These properties might lead to applications including chemical sensors, spectroscopic enhancers, quantum dot and nanostructure fabrication, and microimaging methods. A great deal of control can now be exercised over the chemical composition, size and polydispersity of colloidal particles, and many methods have been developed for assembling them into useful aggregates and materials. Here we describe a method for assembling colloidal gold nanoparticles rationally and reversibly into macroscopic aggregates. The method involves attaching to the surfaces of two batches of 13-nm gold particles non-complementary DNA oligonucleotides capped with thiol groups, which bind to gold. When we add to the solution an oligonucleotide duplex with 'sticky ends' that are complementary to the two grafted sequences, the nanoparticles self-assemble into aggregates. This assembly process can be reversed by thermal denaturation. This strategy should now make it possible to tailor the optical, electronic and structural properties of the colloidal aggregates by using the specificity of DNA interactions to direct the interactions between particles of different size and composition.
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            Folding DNA to create nanoscale shapes and patterns.

            'Bottom-up fabrication', which exploits the intrinsic properties of atoms and molecules to direct their self-organization, is widely used to make relatively simple nanostructures. A key goal for this approach is to create nanostructures of high complexity, matching that routinely achieved by 'top-down' methods. The self-assembly of DNA molecules provides an attractive route towards this goal. Here I describe a simple method for folding long, single-stranded DNA molecules into arbitrary two-dimensional shapes. The design for a desired shape is made by raster-filling the shape with a 7-kilobase single-stranded scaffold and by choosing over 200 short oligonucleotide 'staple strands' to hold the scaffold in place. Once synthesized and mixed, the staple and scaffold strands self-assemble in a single step. The resulting DNA structures are roughly 100 nm in diameter and approximate desired shapes such as squares, disks and five-pointed stars with a spatial resolution of 6 nm. Because each oligonucleotide can serve as a 6-nm pixel, the structures can be programmed to bear complex patterns such as words and images on their surfaces. Finally, individual DNA structures can be programmed to form larger assemblies, including extended periodic lattices and a hexamer of triangles (which constitutes a 30-megadalton molecular complex).
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              Organization of 'nanocrystal molecules' using DNA.

              Patterning matter on the nanometre scale is an important objective of current materials chemistry and physics. It is driven by both the need to further miniaturize electronic components and the fact that at the nanometre scale, materials properties are strongly size-dependent and thus can be tuned sensitively. In nanoscale crystals, quantum size effects and the large number of surface atoms influence the, chemical, electronic, magnetic and optical behaviour. 'Top-down' (for example, lithographic) methods for nanoscale manipulation reach only to the upper end of the nanometre regime; but whereas 'bottom-up' wet chemical techniques allow for the preparation of mono-disperse, defect-free crystallites just 1-10 nm in size, ways to control the structure of nanocrystal assemblies are scarce. Here we describe a strategy for the synthesis of 'nanocrystal molecules', in which discrete numbers of gold nanocrystals are organized into spatially defined structures based on Watson-Crick base-pairing interactions. We attach single-stranded DNA oligonucleotides of defined length and sequence to individual nanocrystals, and these assemble into dimers and trimers on addition of a complementary single-stranded DNA template. We anticipate that this approach should allow the construction of more complex two- and three-dimensional assemblies.

                Author and article information

                Chem Biomed Eng
                Chem Biomed Eng
                Chemical & Biomedical Imaging
                Nanjing University and American Chemical Society
                08 May 2023
                24 July 2023
                : 1
                : 4
                : 340-355
                []Institute of Pharmaceutics, College of Pharmaceutical Sciences, Zhejiang University , Hangzhou 310058, P. R. China
                []Frontiers Science Center for Transformative Molecules, School of Chemistry and Chemical Engineering, National Center for Translational Medicine, State Key Laboratory of Oncogenes and Related Genes, Shanghai Jiao Tong University , Shanghai 200240, P. R. China
                [§ ]World Laureates Association (WLA) Laboratories , Shanghai 201203, P. R. China
                []Hangzhou Institute of Innovative Medicine, Zhejiang University , Hangzhou 310058, P. R. China
                Author notes
                Author information
                © 2023 The Authors. Co-published by Nanjing University and American Chemical Society

                Permits non-commercial access and re-use, provided that author attribution and integrity are maintained; but does not permit creation of adaptations or other derivative works ( https://creativecommons.org/licenses/by-nc-nd/4.0/).

                : 15 February 2023
                : 07 April 2023
                : 20 March 2023
                Funded by: Shanghai Science and Technology Development Foundation, doi 10.13039/100012543;
                Award ID: 22TS1400700
                Funded by: Innovative Research Team of High-Level Local Universities in Shanghai, doi NA;
                Award ID: SHSMU-ZDCX20210900
                Funded by: Natural Science Foundation of Zhejiang Province, doi 10.13039/501100004731;
                Award ID: LR22C100001
                Funded by: Science and Technology Commission of Shanghai Municipality, doi 10.13039/501100003399;
                Award ID: 21XD1422100
                Funded by: Ministry of Science and Technology of the People''s Republic of China, doi 10.13039/501100002855;
                Award ID: 2022YFB3203804
                Funded by: Ministry of Science and Technology of the People''s Republic of China, doi 10.13039/501100002855;
                Award ID: 2022YFB3203801
                Funded by: Ministry of Science and Technology of the People''s Republic of China, doi 10.13039/501100002855;
                Award ID: 2022YFB3203800
                Funded by: Chinese Academy of Sciences, doi 10.13039/501100002367;
                Award ID: JCTD-2020-08
                Funded by: Ministry of Education of the People''s Republic of China, doi 10.13039/501100002338;
                Award ID: NA
                Funded by: National Natural Science Foundation of China, doi 10.13039/501100001809;
                Award ID: 32071374
                Custom metadata

                dna nanotechnology,programmable materials,self-assembly,dynamic assembly,responsive materials,dna probe,bioimaging,biomedical diagnosis


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