0000000000513243
AUTHOR
Boxuan Shen
Biotemplated Lithography of Inorganic Nanostructures (BLIN) for Versatile Patterning of Functional Materials
Here, we present a highly parallel fabrication method dubbed biotemplated lithography of inorganic nanostructures (BLIN) that enables large-scale versatile substrate patterning of metallic and semi...
Applications of DNA self-assembled structures in nanoelectronics and plasmonics
In this thesis, the potential applications of DNA self-assembled structures were explored in both nanoelectronics and plasmonics. The works can be divided into two parts: electrical characterization of unmodified multilayered DNA origami and DNA-gold-nanoparticle conjugates after they were trapped between gold nanoelectrodes by dielectrophoresis, and the development of a novel fabrication method using DNA origami as a template for smooth, high resolution metallic nanostructures as well as optical characterization of them. One of the biggest challenges in self-assembled nanoelectronic devices is to connect them to macroscopic circuits. Dielectrophoretic (DEP) trapping has been used extensivel…
Reconfigurable DNA Origami Nanocapsule for pH-Controlled Encapsulation and Display of Cargo
DNA nanotechnology provides a toolbox for creating custom and precise nanostructures with nanometer-level accuracy. These nano-objects are often static by nature and serve as versatile templates for assembling various molecular components in a user-defined way. In addition to the static structures, the intrinsic programmability of DNA nanostructures allows the design of dynamic devices that can perform predefined tasks when triggered with external stimuli, such as drug delivery vehicles whose cargo display or release can be triggered with a specified physical or chemical cue in the biological environment. Here, we present a DNA origami nanocapsule that can be loaded with cargo and reversibl…
Unraveling the interaction between doxorubicin and DNA origami nanostructures for customizable chemotherapeutic drug release
We thank Dr H. Häkkänen for technical assistance and S. Julin for the 24HB DNA origami design. We acknowledge the provision of facilities and technical support by Aalto University Bioeconomy Facilities and OtaNano – Nanomicroscopy Center (Aalto-NMC). The research was carried out under the Academy of Finland Centres of Excellence Programme (2014–2019). Academy of Finland [308578 to M.A.K.]; Deutsche Forschungsgemeinschaft [Emmy Noether Programme to A.H.-J., SFB1032 (Project A06) to T.L.]; Emil Aaltonen Foundation [to H.I. and V.L.]; Jane and Aatos Erkko Foundation [to J.A.I. and V.L.]; Sigrid Jusélius Foundation [to V.L.]; Vilho, Yrjö and Kalle Väisälä Foundation of the Finnish Academy of Sc…
Dynamic DNA Origami Devices
DNA nanotechnology provides an excellent foundation for diverse nanoscale structures that can be used in various bioapplications and materials research. Among all existing DNA assembly techniques, DNA origami proves to be the most robust one for creating custom nanoshapes. Since its invention in 2006, building from the bottom up using DNA advanced drastically, and therefore, more and more complex DNA-based systems became accessible. So far, the vast majority of the demonstrated DNA origami frameworks are static by nature; however, there also exist dynamic DNA origami devices that are increasingly coming into view. In this review, we discuss DNA origami nanostructures that exhibit controlled…
Unraveling the interaction between doxorubicin and DNA origami nanostructures for customizable chemotherapeutic drug release
Doxorubicin (DOX) is a commonly employed drug in cancer chemotherapy, and its high DNA-binding affinity can be harnessed in preparing programmable DOX-loaded DNA nanostructures that can be further tailored for targeted delivery and therapeutics. Although DOX has been widely studied, the existing literature of promising DOX-loaded DNA nanocarriers remains limited and incoherent. A number of reports have over-looked the fundamentals of the DOX-DNA interaction, let alone the peculiarities arising from the complexity of the system as a whole. Here, based on an in-depth spectroscopic analysis, we characterize and optimize the DOX loading into different 2D and 3D scaffolded DNA origami nanostruct…
Metallic Nanostructures Based on DNA Nanoshapes
Metallic nanostructures have inspired extensive research over several decades, particularly within the field of nanoelectronics and increasingly in plasmonics. Due to the limitations of conventional lithography methods, the development of bottom-up fabricated metallic nanostructures has become more and more in demand. The remarkable development of DNA-based nanostructures has provided many successful methods and realizations for these needs, such as chemical DNA metallization via seeding or ionization, as well as DNA-guided lithography and casting of metallic nanoparticles by DNA molds. These methods offer high resolution, versatility and throughput and could enable the fabrication of arbit…
Probing the Conformational States of a pH-Sensitive DNA Origami Zipper via Label-Free Electrochemical Methods
Funding Information: Financial support from EPSRC DTP (grant EP/R513349/1), the Emil Aaltonen Foundation, the Sigrid Jusélius Foundation, the Jane and Aatos Erkko Foundation, and the Vilho, Yrjö and Kalle Väisälä Foundation of the Finnish Academy of Science and Letters is gratefully acknowledged. This work was carried out under the Academy of Finland Centers of Excellence Programme (2014–2019). We acknowledge the provision of facilities and technical support by Aalto University Bioeconomy Facilities and OtaNano—Nanomicroscopy Center (Aalto-NMC) and Micronova Nanofabrication Center. Publisher Copyright: © 2021 The Authors. Published by American Chemical Society DNA origami structures represe…
Toward Single Electron Nanoelectronics Using Self-Assembled DNA Structure
DNA based structures offer an adaptable and robust way to develop customized nanostructures for various purposes in bionanotechnology. One main aim in this field is to develop a DNA nanobreadboard for a controllable attachment of nanoparticles or biomolecules to form specific nanoelectronic devices. Here we conjugate three gold nanoparticles on a defined size TX-tile assembly into a linear pattern to form nanometer scale isolated islands that could be utilized in a room temperature single electron transistor. To demonstrate this, conjugated structures were trapped using dielectrophoresis for current-voltage characterization. After trapping only high resistance behavior was observed. However…
Dielectrophoretic trapping of multilayer DNA origami nanostructures and DNA origami-induced local destruction of silicon dioxide
DNA origami is a widely used method for fabrication of custom-shaped nanostructures. However, to utilize such structures, one needs to controllably position them on nanoscale. Here we demonstrate how different types of 3D scaffolded multilayer origamis can be accurately anchored to lithographically fabricated nanoelectrodes on a silicon dioxide substrate by DEP. Straight brick-like origami structures, constructed both in square (SQL) and honeycomb lattices, as well as curved "C"-shaped and angular "L"-shaped origamis were trapped with nanoscale precision and single-structure accuracy. We show that the positioning and immobilization of all these structures can be realized with or without thi…
Dynamic DNA Origami Devices: from Strand-Displacement Reactions to External-Stimuli Responsive Systems
DNA nanotechnology provides an excellent foundation for diverse nanoscale structures that can be used in various bioapplications and materials research. Among all existing DNA assembly techniques, DNA origami proves to be the most robust one for creating custom nanoshapes. Since its invention in 2006, building from the bottom up using DNA advanced drastically, and therefore, more and more complex DNA-based systems became accessible. So far, the vast majority of the demonstrated DNA origami frameworks are static by nature; however, there also exist dynamic DNA origami devices that are increasingly coming into view. In this review, we discuss DNA origami nanostructures that exhibit controlled…
One-step large-scale deposition of salt-free DNA origami nanostructures
AbstractDNA origami nanostructures have tremendous potential to serve as versatile platforms in self-assembly -based nanofabrication and in highly parallel nanoscale patterning. However, uniform deposition and reliable anchoring of DNA nanostructures often requires specific conditions, such as pre-treatment of the chosen substrate or a fine-tuned salt concentration for the deposition buffer. In addition, currently available deposition techniques are suitable merely for small scales. In this article, we exploit a spray-coating technique in order to resolve the aforementioned issues in the deposition of different 2D and 3D DNA origami nanostructures. We show that purified DNA origamis can be …
Custom-shaped metal nanostructures based on DNA origami silhouettes.
The DNA origami technique provides an intriguing possibility to develop customized nanostructures for various bionanotechnological purposes. One target is to create tailored bottom-up-based plasmonic devices and metamaterials based on DNA metallization or controlled attachment of nanoparticles to the DNA designs. In this article, we demonstrate an alternative approach: DNA origami nanoshapes can be utilized in creating accurate, uniform and entirely metallic (e.g. gold, silver and copper) nanostructures on silicon substrates. The technique is based on developing silhouettes of the origamis in the grown silicon dioxide layer, and subsequently using this layer as a mask for further patterning…
DNA-Assisted Molecular Lithography
During the past decade, DNA origami has become a popular method to build custom two- (2D) and three-dimensional (3D) DNA nanostructures. These programmable structures could further serve as templates for accurate nanoscale patterning, and therefore they could find uses in various biotechnological applications. However, to transfer the spatial information of DNA origami to metal nanostructures has been limited to either direct nanoparticle-based patterning or chemical growth of metallic seed particles that are attached to the DNA objects. Here, we present an alternative way by combining DNA origami with conventional lithography techniques. With this DNA-assisted lithography (DALI) method, we…
Plasmonic nanostructures through DNA-assisted lithography
DALI combines DNA origami with conventional top-down fabrication for creating designer high-resolution plasmonic nanostructures.
Aptamer-embedded DNA origami cage for detecting (glycated) hemoglobin with a surface plasmon resonance sensor
DNA origami-based cages functionalized with aptamer motifs, were used to detect hemoglobin and glycated hemoglobin. The binding between the cages and hemoglobin was monitored using a surface plasmon resonance (SPR) sensor. One DNA strand in the nano-cage was replaced with an aptamer that demonstrated a high affinity to hemoglobin (Hb) or glycated hemoglobin (gHb). Three types of the DNA nano-cages designed to fit the size and shape of hemoglobin were evaluated: one without an aptamer, one with the Hb-affinity aptamer (HA) and one with the gHb-affinity aptamer (GHA). Both DNA nano-cages embedded with HA and GHA showed significantly more stable binding with Hb and gHb by 5 and 9 times, respec…
Growth of immobilized DNA by polymerase: bridging nanoelectrodes with individual dsDNA molecules.
We present a method for controlled connection of gold electrodes with dsDNA molecules (locally on a chip) by utilizing polymerase to elongate single-stranded DNA primers attached to the electrodes. Thiol-modified oligonucleotides are directed and immobilized to nanoscale electrodes by means of dielectrophoretic trapping, and extended in a procedure mimicking PCR, finally forming a complete dsDNA molecule bridging the gap between the electrodes. The technique opens up opportunities for building from the bottom-up, for detection and sensing applications, and also for molecular electronics.
DNA Origami-Mediated Substrate Nanopatterning of Inorganic Structures for Sensing Applications
Structural DNA nanotechnology provides a viable route for building from the bottom-up using DNA as construction material. The most common DNA nanofabrication technique is called DNA origami, and it allows high-throughput synthesis of accurate and highly versatile structures with nanometer-level precision. Here, it is shown how the spatial information of DNA origami can be transferred to metallic nanostructures by combining the bottom-up DNA origami with the conventionally used top-down lithography approaches. This allows fabrication of billions of tiny nanostructures in one step onto selected substrates. The method is demonstrated using bowtie DNA origami to create metallic bowtie-shaped an…