DNA origami technique, a breakthrough in DNA nanotechnology, has been widely used to prepare complex DNA nanostructures with nanoscale addressability. However, the purity and yield are generally the bottleneck to appl...DNA origami technique, a breakthrough in DNA nanotechnology, has been widely used to prepare complex DNA nanostructures with nanoscale addressability. However, the purity and yield are generally the bottleneck to application of DNA nanostructures, and current methods for purifying DNA origami nanostructures in large quantities are time-consuming and laborious. This study aims to develop a scalable, cost-effective and contamination-free method of purifying DNA origami nanostructures. We employ an effective and convenient purification approach to purify planar rectangle DNA origami structures through rate-zonal centrifugation. By subjecting DNA origami samples to high centrifugal force in a density gradient media of glycerol, well-folded nanostructures and by-products are separated successfully, which are confirmed by agarose gel electrophoresis and atomic force microscopy(AFM). This method will aid the production of pure rectangle DNA origami nanostructures in large quantity.展开更多
DNA origami have been established as versatile templates to fabricate plasmonic nanostructures in predefined shapes and multiple dimensions. Limited to the size of DNA origami, which are approximate to 100 nm, it is h...DNA origami have been established as versatile templates to fabricate plasmonic nanostructures in predefined shapes and multiple dimensions. Limited to the size of DNA origami, which are approximate to 100 nm, it is hard to assemble more intricate plasmonic nanostructures in large scale. Herein, we used rectangular DNA origami as the template to anchor two 30-nm gold nanoparticles(Au NPs) which induced dimers nanostructures. Transmission electron microscopy(TEM) images showed the assembly of Au NPs with high yields. Using the linkers to organize the DNA origami templates into nanoribbons,chains of Au NPs were obtained, which was validated bythe TEM images. Furthermore, we observed a significant Raman signal enhancement from molecules covalently attached to the Au NP-dimers and Au NP-chains. Our method opens up the prospects of high-ordered plasmonic nanostructures with tailored optical properties.展开更多
The spatial arrangement of activating ligands is known to have great influence on T cell activation.However,independently studying each ligand’s spatial organization parameter that affects T cell activation remains a...The spatial arrangement of activating ligands is known to have great influence on T cell activation.However,independently studying each ligand’s spatial organization parameter that affects T cell activation remains a great challenge.Here,with DNA origami,we precisely organized the CD3ɛantibodies simulating T cell receptor(TCR)ligands and CD28 antibodies simulating co-stimulatory ligands to interrogate the independent role of TCR-ligand spacing and local copy numbers as well as the spacing between TCR ligands and co-stimulatory ligands on T cell activation.We found that T cell activation benefited fromlocally concentrated TCR ligands with a shorter spacing and was maximized by an∼38 nm spacing between TCR ligands and co-stimulatory ligands.The T cell expander constructed based on our findings could efficiently expand CD8+T cells for tumor immunotherapy.Thus,the DNA nanostructurebased ligands’precise arrangement can be a unique tool in studying immune cell activations and cellbased immunotherapies.展开更多
DNA origami-assisted nanolithography(DOANL)for fabricating custom-designed nanomaterials through pattern transfer from DNA origami to different substrates materials are presented.However,the pattern's integrity an...DNA origami-assisted nanolithography(DOANL)for fabricating custom-designed nanomaterials through pattern transfer from DNA origami to different substrates materials are presented.However,the pattern's integrity and resolution face considerable challenges due to the uncontrollable growth of the nanomaterials during transformation and the unclear mechanism of DOANL.Herein,we report a DOANL combined with area-selective atomic layer deposition(ALD)strategy for fabricating custom shapes hafnium oxide(HfO2)with the high-fidelity and high-throughput.We find that the HfO_(2)selectively grows on DNA origami substrates in a hydroxyl-rich area instead of a methyl-rich protective layer.Combined with the merit of the area-selective ALD method,theHfO_(2)atom selectively coated on the DNA origami surface,thus,precisely modeling the shapes with high-precision in our study based on the surface groups difference of DNA origami and the naked hexamethyldisilane(HMDS)-treated substrates,which reveal the mechanical of high-fidelity pattern transfer based on DOANL.As a result,DNA origami structures can program the shape ofHfO_(2)nanostructures.The DOANL that is based on the principle of"bottom-up"precision assembly breaks through the shape complexity and high-throughput fabrication limitation of theHfO_(2)nanostructures,including two-and three-dimensional structures,plane and curved structures,monolithic and hollow structures.Based on the"top-down"accurate fabrication principle,the area-selective ALD on methyl-rich protective layer substrates improves the integrity and resolution of the pattern transfer process.Overall,this work provides a general technology for nanofabrication strategy.展开更多
DNA origami is a promising technology for its reproducibility,flexibility,scalability and biocompatibility.Among the several potential applications,DNA origami has been proposed as a tool for drug delivery and as a co...DNA origami is a promising technology for its reproducibility,flexibility,scalability and biocompatibility.Among the several potential applications,DNA origami has been proposed as a tool for drug delivery and as a contrast agent,since a conformational change upon specific target interaction may be used to release a drug or produce a physical signal,respectively.However,its conformation should be robust with respect to the properties of the medium in which either the recognition or the read-out take place,such as pressure,viscosity and any other unspecific interaction other than the desired target recognition.Here we report on the read-out robustness of a tetragonal DNA-origami/gold-nanoparticle hybrid structure able to change its configuration,which is transduced in a change of its plasmonic properties,upon interaction with a specific DNA target.We investigated its response when analyzed in three different media:aqueous solution,solid support and viscous gel.We show that,once a conformational variation is produced,it remains unaffected by the subsequent physical interactions with the environment.展开更多
Controllable strong interactions between a nanocavity and a single emitter is important to manipulating optical emission in a nanophotonic system but challenging to achieve.Herein a three-dimensional DNA origami,named...Controllable strong interactions between a nanocavity and a single emitter is important to manipulating optical emission in a nanophotonic system but challenging to achieve.Herein a three-dimensional DNA origami,named as DNA rack(DR)is proposed and demonstrated to deterministically and precisely assemble single emitters within ultra-small plasmonic nanocavities formed by closely coupled gold nanorods(AuNRs).Uniquely,the DR is in a saddle shape,with two tubular grooves that geometrically allow a snug fit and linearly align two AuNRs with a bending angle <10°.It also includes a spacer at the saddle point to maintain the gap between AuNRs as small as 2-3 nm,forming a nanocavity estimated to be 20 nm^(3) and an experimentally measured O factor of 7.3.A DNA docking strand is designed at the spacer to position a single fluorescent emitter at nanometer accuracy within the cavity.Using Cy5 as a model emitter,a -30-fold fluorescence enhancement and a significantly reduced emission lifetime(from 1.6 ns to 670 ps)were experimentally verified,confirming significant emitter-cavity interactions.This DR-templated assembly method is capable of fitting AuNRs of variable length-to-width aspect ratios to form anisotropic nanocavities and deterministically incorporate different single emitters,thus enabling flexible design of both cavity resonance and emission wavelengths to tailor light-matter interactions at nanometer scale.展开更多
The surface-assisted hierarchical self-assembly of DNA origami lattices represents a versatile and straightforward method for the organization of functional nanoscale objects such as proteins and nanoparticles.Here,we...The surface-assisted hierarchical self-assembly of DNA origami lattices represents a versatile and straightforward method for the organization of functional nanoscale objects such as proteins and nanoparticles.Here,we demonstrate that controlling the binding and exchange of different monovalent and divalent cation species at the DNA-mica interface enables the self-assembly of highly ordered DNA origami lattices on mica surfaces.The development of lattice quality and order is quantified by a detailed topological analysis of high-speed atomic force microscopy(HS-AFM)images.We find that lattice formation and quality strongly depend on the monovalent cation species.Na^(+)is more effective than Li^(+)and K^(+)in facilitating the assembly of high-quality DNA origami lattices,because it is replacing the divalent cations at their binding sites in the DNA backbone more efficiently.With regard to divalent cations,Ca^(2+)can be displaced more easily from the backbone phosphates than Mg^(2+)and is thus superior in guiding lattice assembly.By independently adjusting incubation time,DNA origami concentration,and cation species,we thus obtain a highly ordered DNA origami lattice with an unprecedented normalized correlation length of 8.2.Beyond the correlation length,we use computer vision algorithms to compute the time course of different topological observables that,overall,demonstrate that replacing MgCl_(2) by CaCl_(2) enables the synthesis of DNA origami lattices with drastically increased lattice order.展开更多
During the development of structural DNA nanotechnology,the emerging of scaffolded DNA origami is marvelous.It utilizes DNA double helix inherent specificity of Watson-Crick base pairing and structural features to cre...During the development of structural DNA nanotechnology,the emerging of scaffolded DNA origami is marvelous.It utilizes DNA double helix inherent specificity of Watson-Crick base pairing and structural features to create self-assembling structures at the nanometer scale exhibiting the addressable character.However,the assembly of DNA origami is disorderly and unpredictable.Herein,we present a novel strategy to assemble the DNA origami using rolling circle amplification based DNA nanoribbons as the linkers.Firstly,long single-stranded DNA from Rolling Circle Amplification is annealed with several staples to form kinds of DNA nanoribbons with overhangs.Subsequently,the rectangle origami is formed with overhanged staple strands at any edge that would hybridize with the DNA nanoribbons.By mixing them up,we illustrate the one-dimensional even two-dimensional assembly of DNA origami with good orientation.展开更多
Plasmonic circular dichroism(CD) has been emerged as a promising signal for building biosensors due to its high sensitivity and specificity. In the past years, DNA nanotechnology enabled diverse chiral plasmonic devic...Plasmonic circular dichroism(CD) has been emerged as a promising signal for building biosensors due to its high sensitivity and specificity. In the past years, DNA nanotechnology enabled diverse chiral plasmonic devices, which can response biomolecules and then generate dynamic plasmonic CD signals at the visible range. Although some of them have been successfully employed as biosensors, the detection sensitivity is still relatively low. Herein we report a chiral plasmonic sensor with an improved detection sensitivity by integrating catalytic hairpin assembly circuits into DNA origami structures. We tested two kinds of tumor marker RNA sequences as detection targets and it turns out that the detection limit is below 10 pmol/L, improving one order of magnitude compared to previous work. The chiral plasmonic sensor with internal signal amplification circuits can stimulate a variety of smart nano-sensors for biological detection and offer a promising strategy for pathogenic RNA detection with plasmonic CD output.展开更多
Herein we demonstrate the construction of three types of parallel gold nanorod(AuNR) clusters using a DNA origami rod(DOR) as the template. Based on the precise control over the position of capture strands on DOR, num...Herein we demonstrate the construction of three types of parallel gold nanorod(AuNR) clusters using a DNA origami rod(DOR) as the template. Based on the precise control over the position of capture strands on DOR, number and orientation of the AuNR clusters can be well engineered, as evidenced by biological transmission electron microscope(TEM). Importantly, the AuNR clusters exhibit chiroptical responses which are strongly affected by the number of AuNR on rod-like DNA origami.展开更多
For about three decades, DNA-based nanotechnology has been undergoing development as an assembly method for nanostructured materials. The DNA origami method pioneered by Rothemund paved the way for the formation of 3D...For about three decades, DNA-based nanotechnology has been undergoing development as an assembly method for nanostructured materials. The DNA origami method pioneered by Rothemund paved the way for the formation of 3D structures using DNA self assembly. The origami approach uses a long scaffold strand as the input for the self assembly of a few hundred staple strands into desired shapes. Herein, we present a 3D origami "roller" (75 nm in length) designed using caDNAno software. This has the potential to be used as a template to assemble nanoparticles into different pre-defined shapes. The "roller" was characterized with agarose gel electrophoresis, atomic force microscopy (AFM) and transmission electron microscopy (TEM).展开更多
Anisotropic nanopatterns have potentials in constructing novel plasmonic structures which have various applications in such as super-resolution microscopy, medicine, and sensors. However, it remains challenging to bui...Anisotropic nanopatterns have potentials in constructing novel plasmonic structures which have various applications in such as super-resolution microscopy, medicine, and sensors. However, it remains challenging to build big anisotropic nanopatterns that are suitable for big noble metal nanoparticles. Herein, we report a simple and reliable strategy for constructing DNA origami-based big anisotropic nanopatterns with controlled size and shape, nanoscale resolution, and fully addressability. Two kinds of basic DNA origami nanoblocks-cross-shaped and rectangular DNA origami units were used. We have demonstrated that by encoding nanoblocks' edges, anisotropic higher-order nanopatterns, such as dimer, trimer, tetramer and mini "windmill" like pentamer nanopatterns could be constructed. To show the potential use as template to direct the assembly of anisotropic nanoparticles arrays, a proof of concept work was conducted by anchoring streptavidin nanoparticles on the "windmill" template to form a chiral array. Significantly, these nanopatterns have the sizes of hundreds of nanometers, which are in principle also suitable for big noble metal nanoparticles arrays.展开更多
Hetero-assembling of spherical building blocks with well-defined spatial distribution holds great significance in developing chiral nanostructures. Herein, a strategy for hetero-assembling of gold nanoparticles(Au NPs...Hetero-assembling of spherical building blocks with well-defined spatial distribution holds great significance in developing chiral nanostructures. Herein, a strategy for hetero-assembling of gold nanoparticles(Au NPs) was demonstrated using rigid bifacial DNA origami as templates. By tuning the sizes and the fixed location of Au NPs on DNA origami, right-handed and left-handed Au NPs nanostructures were respectively constructed. Gel electrophoresis indicated the formation of the DNA origami-Au NPs complex and transmission electron microscopy(TEM) visually displayed the arrangement of Au NPs in these two chiral structures. The spatial configuration and 3D geometry of Au NPs were further illustrated by the stereographic TEM with tilting angles from ?30° to 30°. This strategy provides a universal approach to construct the asymmetrical 3D geometries, which may have potential applications in biomimicking and nanophotonics.展开更多
基金Supported by Shanghai Natural Science Foundation(Nos.15ZR1448400 and 15ZR1448700)National Natural Science Foundation of China(No.31300825)
文摘DNA origami technique, a breakthrough in DNA nanotechnology, has been widely used to prepare complex DNA nanostructures with nanoscale addressability. However, the purity and yield are generally the bottleneck to application of DNA nanostructures, and current methods for purifying DNA origami nanostructures in large quantities are time-consuming and laborious. This study aims to develop a scalable, cost-effective and contamination-free method of purifying DNA origami nanostructures. We employ an effective and convenient purification approach to purify planar rectangle DNA origami structures through rate-zonal centrifugation. By subjecting DNA origami samples to high centrifugal force in a density gradient media of glycerol, well-folded nanostructures and by-products are separated successfully, which are confirmed by agarose gel electrophoresis and atomic force microscopy(AFM). This method will aid the production of pure rectangle DNA origami nanostructures in large quantity.
基金supported by the National Natural Science Foundation of China(No.21475064)the Natural Science Foundation of Jiangsu Province(No.BK20151504)+4 种基金Program for Changjiang Scholars and Innovative Research Team in University(No.IRT_15R37)Sci-Tech Support Plan of Jiangsu Province(No.BE2014719)the Priority Academic Program Development of Jiangsu Higher Education Institutions(No.PAPD,YX03001)the Mega-projects of Science and Technology Research(No.AWS13C007)NUPTSF(No.214175)
文摘DNA origami have been established as versatile templates to fabricate plasmonic nanostructures in predefined shapes and multiple dimensions. Limited to the size of DNA origami, which are approximate to 100 nm, it is hard to assemble more intricate plasmonic nanostructures in large scale. Herein, we used rectangular DNA origami as the template to anchor two 30-nm gold nanoparticles(Au NPs) which induced dimers nanostructures. Transmission electron microscopy(TEM) images showed the assembly of Au NPs with high yields. Using the linkers to organize the DNA origami templates into nanoribbons,chains of Au NPs were obtained, which was validated bythe TEM images. Furthermore, we observed a significant Raman signal enhancement from molecules covalently attached to the Au NP-dimers and Au NP-chains. Our method opens up the prospects of high-ordered plasmonic nanostructures with tailored optical properties.
基金supported by the National Research Programs from the Ministry of Science and Technology of China(grant no.2021YFF0701800)the National Natural Science Foundation of China(grant nos.52032008 and 22277071)+1 种基金the Collaborative Innovation Center of Suzhou Nano Science and Technologythe“111”program from the Ministry of Education of China.
文摘The spatial arrangement of activating ligands is known to have great influence on T cell activation.However,independently studying each ligand’s spatial organization parameter that affects T cell activation remains a great challenge.Here,with DNA origami,we precisely organized the CD3ɛantibodies simulating T cell receptor(TCR)ligands and CD28 antibodies simulating co-stimulatory ligands to interrogate the independent role of TCR-ligand spacing and local copy numbers as well as the spacing between TCR ligands and co-stimulatory ligands on T cell activation.We found that T cell activation benefited fromlocally concentrated TCR ligands with a shorter spacing and was maximized by an∼38 nm spacing between TCR ligands and co-stimulatory ligands.The T cell expander constructed based on our findings could efficiently expand CD8+T cells for tumor immunotherapy.Thus,the DNA nanostructurebased ligands’precise arrangement can be a unique tool in studying immune cell activations and cellbased immunotherapies.
基金supported by the National Key R&D Program of China(No.2019YFA0905800)the National Natural Science Foundation of China(No.21705048)+5 种基金Guangdong Basic and Applied Basic Research Foundation(No.2021A1515012333)Natural Science Foundation of Jiangxi Province(No.20192ACBL20046)the Fundamental Research Funds for the Central Universities(No.20720200004)the Key Project of College Youth Natural Fund of Fujian Province(No.JZ160404)the Key Laboratory of Sensing Technology and Biomedical Instruments of Guangdong Province(No.2020B1212060077)support from Qingdao XINO Tech company.Thanks to Yange Wang for his help in AFM scanning。
文摘DNA origami-assisted nanolithography(DOANL)for fabricating custom-designed nanomaterials through pattern transfer from DNA origami to different substrates materials are presented.However,the pattern's integrity and resolution face considerable challenges due to the uncontrollable growth of the nanomaterials during transformation and the unclear mechanism of DOANL.Herein,we report a DOANL combined with area-selective atomic layer deposition(ALD)strategy for fabricating custom shapes hafnium oxide(HfO2)with the high-fidelity and high-throughput.We find that the HfO_(2)selectively grows on DNA origami substrates in a hydroxyl-rich area instead of a methyl-rich protective layer.Combined with the merit of the area-selective ALD method,theHfO_(2)atom selectively coated on the DNA origami surface,thus,precisely modeling the shapes with high-precision in our study based on the surface groups difference of DNA origami and the naked hexamethyldisilane(HMDS)-treated substrates,which reveal the mechanical of high-fidelity pattern transfer based on DOANL.As a result,DNA origami structures can program the shape ofHfO_(2)nanostructures.The DOANL that is based on the principle of"bottom-up"precision assembly breaks through the shape complexity and high-throughput fabrication limitation of theHfO_(2)nanostructures,including two-and three-dimensional structures,plane and curved structures,monolithic and hollow structures.Based on the"top-down"accurate fabrication principle,the area-selective ALD on methyl-rich protective layer substrates improves the integrity and resolution of the pattern transfer process.Overall,this work provides a general technology for nanofabrication strategy.
基金V.M.acknowledges financial support from MIUR(MIUR Giovani-Ambito“Salute dell’uomo”).Work at the Molecular Foundry,under the research project No.3376,was supported by the Office of Science,Office of Basic Energy Sciences,of the U.S.Department of Energy under Contract No.DE-AC02-05CH11231.We acknowledge the Facility of Nanofabrication(FNF)of IOM for the support in sample preparation,Simone Dal Zilio and Silvio Greco for help in data analysis and stimulating discussions.We acknowledge Prof.Giuseppe Firrao for valuable comments and inspiring ideas,the NanoInnovation laboratory(Elettra Sincrotrone)for suggestion provided for AFM analysis and the BioLab(Elettra Sincrotrone)for the use of lab and instrumentation.
文摘DNA origami is a promising technology for its reproducibility,flexibility,scalability and biocompatibility.Among the several potential applications,DNA origami has been proposed as a tool for drug delivery and as a contrast agent,since a conformational change upon specific target interaction may be used to release a drug or produce a physical signal,respectively.However,its conformation should be robust with respect to the properties of the medium in which either the recognition or the read-out take place,such as pressure,viscosity and any other unspecific interaction other than the desired target recognition.Here we report on the read-out robustness of a tetragonal DNA-origami/gold-nanoparticle hybrid structure able to change its configuration,which is transduced in a change of its plasmonic properties,upon interaction with a specific DNA target.We investigated its response when analyzed in three different media:aqueous solution,solid support and viscous gel.We show that,once a conformational variation is produced,it remains unaffected by the subsequent physical interactions with the environment.
基金support from an Army Research Office MURI award no.W91 INF-12-1-0420C.W.thanks the ASU startup funds and National Science Foundation under grant Nos.1711412,1838443,and 1847324 for partially supporting this researchY.Y.thanks the ASU startup funds and National Science Foundation under grant Nos.1809997 for partially supporting this research.
文摘Controllable strong interactions between a nanocavity and a single emitter is important to manipulating optical emission in a nanophotonic system but challenging to achieve.Herein a three-dimensional DNA origami,named as DNA rack(DR)is proposed and demonstrated to deterministically and precisely assemble single emitters within ultra-small plasmonic nanocavities formed by closely coupled gold nanorods(AuNRs).Uniquely,the DR is in a saddle shape,with two tubular grooves that geometrically allow a snug fit and linearly align two AuNRs with a bending angle <10°.It also includes a spacer at the saddle point to maintain the gap between AuNRs as small as 2-3 nm,forming a nanocavity estimated to be 20 nm^(3) and an experimentally measured O factor of 7.3.A DNA docking strand is designed at the spacer to position a single fluorescent emitter at nanometer accuracy within the cavity.Using Cy5 as a model emitter,a -30-fold fluorescence enhancement and a significantly reduced emission lifetime(from 1.6 ns to 670 ps)were experimentally verified,confirming significant emitter-cavity interactions.This DR-templated assembly method is capable of fitting AuNRs of variable length-to-width aspect ratios to form anisotropic nanocavities and deterministically incorporate different single emitters,thus enabling flexible design of both cavity resonance and emission wavelengths to tailor light-matter interactions at nanometer scale.
基金We thank David Contreras for his helpful discussions and comments.This research has been partially funded by the Spanish Ministerio de Ciencia,Innovacion y Universidades-FEDER funds of the European Union support,under projects FIS2016-78883-C2-2-P and PID2019-106339GB-I00(M.C.).
文摘The surface-assisted hierarchical self-assembly of DNA origami lattices represents a versatile and straightforward method for the organization of functional nanoscale objects such as proteins and nanoparticles.Here,we demonstrate that controlling the binding and exchange of different monovalent and divalent cation species at the DNA-mica interface enables the self-assembly of highly ordered DNA origami lattices on mica surfaces.The development of lattice quality and order is quantified by a detailed topological analysis of high-speed atomic force microscopy(HS-AFM)images.We find that lattice formation and quality strongly depend on the monovalent cation species.Na^(+)is more effective than Li^(+)and K^(+)in facilitating the assembly of high-quality DNA origami lattices,because it is replacing the divalent cations at their binding sites in the DNA backbone more efficiently.With regard to divalent cations,Ca^(2+)can be displaced more easily from the backbone phosphates than Mg^(2+)and is thus superior in guiding lattice assembly.By independently adjusting incubation time,DNA origami concentration,and cation species,we thus obtain a highly ordered DNA origami lattice with an unprecedented normalized correlation length of 8.2.Beyond the correlation length,we use computer vision algorithms to compute the time course of different topological observables that,overall,demonstrate that replacing MgCl_(2) by CaCl_(2) enables the synthesis of DNA origami lattices with drastically increased lattice order.
基金This work was supported by grant from the National Natural Science Foundation of China(Nos.21105110&21103219)and the Knowledge Innovation Program of Chinese Academy of Sciences.
文摘During the development of structural DNA nanotechnology,the emerging of scaffolded DNA origami is marvelous.It utilizes DNA double helix inherent specificity of Watson-Crick base pairing and structural features to create self-assembling structures at the nanometer scale exhibiting the addressable character.However,the assembly of DNA origami is disorderly and unpredictable.Herein,we present a novel strategy to assemble the DNA origami using rolling circle amplification based DNA nanoribbons as the linkers.Firstly,long single-stranded DNA from Rolling Circle Amplification is annealed with several staples to form kinds of DNA nanoribbons with overhangs.Subsequently,the rectangle origami is formed with overhanged staple strands at any edge that would hybridize with the DNA nanoribbons.By mixing them up,we illustrate the one-dimensional even two-dimensional assembly of DNA origami with good orientation.
基金This work was supported by the National Natural Science Foundation of China(No.21977112)the Natural Science Foundation of Jiangsu Province,China(No.BK20190227)the Strategic Priority Research Program of Chinese Academy of Sciences(No.XDB36000000).
文摘Plasmonic circular dichroism(CD) has been emerged as a promising signal for building biosensors due to its high sensitivity and specificity. In the past years, DNA nanotechnology enabled diverse chiral plasmonic devices, which can response biomolecules and then generate dynamic plasmonic CD signals at the visible range. Although some of them have been successfully employed as biosensors, the detection sensitivity is still relatively low. Herein we report a chiral plasmonic sensor with an improved detection sensitivity by integrating catalytic hairpin assembly circuits into DNA origami structures. We tested two kinds of tumor marker RNA sequences as detection targets and it turns out that the detection limit is below 10 pmol/L, improving one order of magnitude compared to previous work. The chiral plasmonic sensor with internal signal amplification circuits can stimulate a variety of smart nano-sensors for biological detection and offer a promising strategy for pathogenic RNA detection with plasmonic CD output.
基金supported by the National Natural Science Foundation of China (Nos. 21504053, 21661162001, 21673139, 91527304, 21722502)Shanghai Pujiang Talent Project (No. 16PJ1402700)+1 种基金the Innovation Fund from Joint Research Center for Precision Medicine set up by Shanghai Jiao Tong University & Affiliated Sixth People's Hospital South Campus (No. IFPM 2016B001)the special program for collaborative innovation in Shanghai University of Medicine & Health Sciences (SPCI-17-15-001)
文摘Herein we demonstrate the construction of three types of parallel gold nanorod(AuNR) clusters using a DNA origami rod(DOR) as the template. Based on the precise control over the position of capture strands on DOR, number and orientation of the AuNR clusters can be well engineered, as evidenced by biological transmission electron microscope(TEM). Importantly, the AuNR clusters exhibit chiroptical responses which are strongly affected by the number of AuNR on rod-like DNA origami.
基金supported by the National Basic Research Program of China (2011CB013004)Major Project of State Key Laboratory of Tribology, Tsinghua University (SKLT10A02)
文摘For about three decades, DNA-based nanotechnology has been undergoing development as an assembly method for nanostructured materials. The DNA origami method pioneered by Rothemund paved the way for the formation of 3D structures using DNA self assembly. The origami approach uses a long scaffold strand as the input for the self assembly of a few hundred staple strands into desired shapes. Herein, we present a 3D origami "roller" (75 nm in length) designed using caDNAno software. This has the potential to be used as a template to assemble nanoparticles into different pre-defined shapes. The "roller" was characterized with agarose gel electrophoresis, atomic force microscopy (AFM) and transmission electron microscopy (TEM).
基金supported by the National Basic Research Program of China (2012CB932600)the National Natural Science Foundation of China(20725516, 90913014, 21028005 and 21103219)Shanghai Pujiang Program (11PJ1412000)
文摘Anisotropic nanopatterns have potentials in constructing novel plasmonic structures which have various applications in such as super-resolution microscopy, medicine, and sensors. However, it remains challenging to build big anisotropic nanopatterns that are suitable for big noble metal nanoparticles. Herein, we report a simple and reliable strategy for constructing DNA origami-based big anisotropic nanopatterns with controlled size and shape, nanoscale resolution, and fully addressability. Two kinds of basic DNA origami nanoblocks-cross-shaped and rectangular DNA origami units were used. We have demonstrated that by encoding nanoblocks' edges, anisotropic higher-order nanopatterns, such as dimer, trimer, tetramer and mini "windmill" like pentamer nanopatterns could be constructed. To show the potential use as template to direct the assembly of anisotropic nanoparticles arrays, a proof of concept work was conducted by anchoring streptavidin nanoparticles on the "windmill" template to form a chiral array. Significantly, these nanopatterns have the sizes of hundreds of nanometers, which are in principle also suitable for big noble metal nanoparticles arrays.
基金supported by the National Basic Research Program of China (2012CB933301)the National Natural Science Foundation of China (21305070, 21475064)+2 种基金the Natural Science Foundation of Jiangsu Province (BK20130861)the Sci-tech Support Plan of Jiangsu Province (BE2014719)Science Foundation of Nanjing University of Posts and Telecommunications (213005, 214175).
文摘Hetero-assembling of spherical building blocks with well-defined spatial distribution holds great significance in developing chiral nanostructures. Herein, a strategy for hetero-assembling of gold nanoparticles(Au NPs) was demonstrated using rigid bifacial DNA origami as templates. By tuning the sizes and the fixed location of Au NPs on DNA origami, right-handed and left-handed Au NPs nanostructures were respectively constructed. Gel electrophoresis indicated the formation of the DNA origami-Au NPs complex and transmission electron microscopy(TEM) visually displayed the arrangement of Au NPs in these two chiral structures. The spatial configuration and 3D geometry of Au NPs were further illustrated by the stereographic TEM with tilting angles from ?30° to 30°. This strategy provides a universal approach to construct the asymmetrical 3D geometries, which may have potential applications in biomimicking and nanophotonics.
