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![Possible routes to develop future integrated DNA circuits by combining DNA origami technologies (upper row) and appropriate modifications of the electronic structure of individual DNA molecule (lower row). The middle frame of the upper row is reprinted with permission from ref. [34]. Copyright (2017) Nature Publishing Group. The right frame of the upper row is reprinted with permission from ref. [143]. Copyright (2017) Nature Publishing Group. The middle and right frames of the lower row are reprinted with permission from ref. [116]. Copyright (2010) ELSEVIER.](profile/Kun-Wang-29/publication/322552391/figure/fig4/AS:583824043945985@1516205907407/Possible-routes-to-develop-future-integrated-DNA-circuits-by-combining-DNA-origami.png)
Possible routes to develop future integrated DNA circuits by combining DNA origami technologies (upper row) and appropriate modifications of the electronic structure of individual DNA molecule (lower row). The middle frame of the upper row is reprinted with permission from ref. [34]. Copyright (2017) Nature Publishing Group. The right frame of the upper row is reprinted with permission from ref. [143]. Copyright (2017) Nature Publishing Group. The middle and right frames of the lower row are reprinted with permission from ref. [116]. Copyright (2010) ELSEVIER.
Source publication
Beyond being the repository of genetic information, DNA is playing an increasingly important role as a building block for molecular electronics. Its inherent structural and molecular recognition properties render it a leading candidate for molecular electronics applications. The structural stability, diversity and programmability of DNA provide ove...
Citations
... Low-and intermediate-bias current measurements are increasingly used in biosensing applications involving aptamers [30] or DNA strands [31]. ...
Food and drinks can be contaminated with pollutants such as lead and strontium, which poses a serious danger to human health. For this reason, a number of effective sensors have been developed for the rapid and highly selective detection of such contaminants. TBA, a well-known aptamer developed to selectively target and thereby inhibit the protein of clinical interest α-thrombin, is receiving increasing attention for sensing applications, particularly for the sensing of different cations. Indeed, TBA, in the presence of these cations, folds into the stable G-quadruplex structure. Furthermore, different cations produce small but significant changes in this structure that result in changes in the electrical responses that TBA can produce. In this article, we give an overview of the expected data regarding the use of TBA in the detection of lead and strontium, calculating the expected electrical response using different measurement techniques. Finally, we conclude that TBA should be able to detect strontium with a sensitivity approximately double that achievable for lead.
... It is thus obvious that such devices are extremely sensitive to any variation in their environment, such as any decrease or increase in inter-nanoparticle distance, changes in the dielectric constant of the surrounding medium, and the introduction of functionalization materials between distinct NPs or between NP aggregates. On the other hand, dsDNA exhibits interesting electrical properties and is known to facilitate charge transport via tunneling over shorter oligonucleotides or via multi-step hopping over longer DNA paths [54]; this is also the case for ssDNA, albeit with conductivity that is order of magnitudes lower than that of dsDNA [55]. The electrical In the current study, sensors that incorporate thiol-modified DNAzymes for lead and cadmium, as well as sensors that incorporate amino-modified DNAzymes for all heavy metal ions, feature a similar dynamic response. ...
... It is thus obvious that such devices are extremely sensitive to any variation in their environment, such as any decrease or increase in inter-nanoparticle distance, changes in the dielectric constant of the surrounding medium, and the introduction of functionalization materials between distinct NPs or between NP aggregates. On the other hand, dsDNA exhibits interesting electrical properties and is known to facilitate charge transport via tunneling over shorter oligonucleotides or via multi-step hopping over longer DNA paths [54]; this is also the case for ssDNA, albeit with conductivity that is order of magnitudes lower than that of dsDNA [55]. The electrical properties of dsDNA and its respective charge transport, using the HOMO/LUMO and the π-electronic system of stacked base pairs, have been studied extensively, yet many phenomena still need to be understood; more specifically, distinctive DNA base pairs have been found to promote charge transport, while others act as electric barriers [54]. ...
A hybrid noble nanoparticle/DNAzyme electrochemical biosensor is proposed for the detection of Pb2+, Cd2+, and Cr3+. The sensor takes advantage of a well-studied material that is known for its selective interaction with heavy metal ions (i.e., DNAzymes), which is combined with metallic nanoparticles. The double-helix structure of DNAzymes is known to dissociate into smaller fragments in the presence of specific heavy metal ions; this results in a measurable change in device resistance due to the collapse of conductive inter-nanoparticle DNAzyme bridging. The paper discusses the effect of DNAzyme anchoring groups (i.e., thiol and amino functionalization groups) on device performance and reports on the successful detection of all three target ions in concentrations that are well below their maximum permitted levels in tap water. While the use of DNAzymes for the detection of lead in particular and, to some extent, cadmium has been studied extensively, this is one of the few reports on the successful detection of chromium (III) via a sensor incorporating DNAzymes. The sensor showed great potential for its future integration in autonomous and remote sensing systems due to its low power characteristics, simple and cost-effective fabrication, and easy automation and measurement.
... Low and intermediate bias current measurements are increasingly used in biosensing applications involving aptamers [26] or DNA strands [27]. ...
Food and drinks can be contaminated with pollutants such as lead and strontium and this poses a serious danger to human health. For this reason, a number of effective sensors have been developed for the rapid and highly selective detection of such contaminants. TBA, a well-known aptamer developed to selectively target and thereby inhibit the protein of clinical interest -thrombin, is receiving increasing attention for sensing applications, particularly for the sensing of different cations. Indeed, TBA, in the presence of these cations, folds into the stable G-quadruplex structure. Furthermore, different cations produce small but significant changes in this structure that result in changes in the electrical responses that TBA can produce. In this article we produce an overview of the expected data regarding the use of TBA in the detection of lead and strontium, calculating the expected electrical response using different measurement techniques. Finally, we conclude that the TBA should perform better as a detector of strontium rather than lead.
... In order to make DNA nanostructures into electronic devices, one approach is to determine how to make DNA conductive. While there is some evidence that DNA itself can be a conductive material [19,20], its conductivity is relatively low [21]. ...
The seminal recognition by Ned Seeman that DNA could be programmed via base-pairing to form higher order structures is well known. What may have been partially forgotten is one of Dr. Seeman’s strong motivations for forming precise and programmable nanostructures was to create nanoelectronic devices. This motivation is particularly apt given that modern electronic devices require precision positioning of conductive elements to modulate and control electronic properties, and that such positioning is inherently limited by the scaling of photoresist technologies: DNA may literally be one of the few ways to make devices smaller (Liddle and Gallatin in Nanoscale 3:2679–2688 [1]). As with many other insights regarding DNA at the nanoscale, Ned Seeman recognized the possibilities of DNA-templated electronic devices as early as 1987 (Robinson and Seeman in Protein Eng. 1:295–300 [2]). As of 2002, Braun’s group attempted to develop methods for lithography that involved metalating DNA (Keren et al. in Science 297:72–75 [3]). However, this instance involved linear, double-stranded DNA, in which portions were separated using RecA, and thus, the overall complexity of the lithography was limited. Since then, the extraordinary control afforded by DNA nanotechnology has provided equally interesting opportunities for creating complex electronic circuitry, either via turning DNA into an electronic device itself (Gates et al. in Crit. Rev. Anal. Chem. 44:354–370 [4]), or by having DNA organize other materials (Hu and Niemeyer in Adv. Mat. 31(26), [5]) that can be electronic devices (Dai et al. in Nano Lett. 20:5604–5615 [6]).
... DNA has attracted considerable interest in the nanoscience and nanotechnology communities in recent years. DNA's unique structural, mechanical, and self-assembly properties yield new opportunities for nanometer-scale material placement and control, and its electronic properties have yielded interesting options for electronic devices and biosensing applications [1][2][3]. Recently, the single-molecule break-junction (SMBJ) technique has arisen as a promising tool for probing the single-molecule conductance value for various DNA and RNA sequences [4], their conformations [5], environmental effects [6], and base mismatches [7]. The detection of biologically relevant RNA duplex structures at extremely low concentrations is one of the great advantages that SMBJ offers [8]. ...
... In this case, because of the repeating G-triplets within each of the oligonucleotide sequences, we hypothesized that high conductance peaks would originate from the formation of G-quadraplexes in the solution, which could readily form in these guanine-rich sequences [21,22] and that the other would come from double-stranded (ds)DNA. With this hypothesis, we will refer to double-stranded versions of each of the two sequences as ds(CG 3 ) 3 and ds(C 3 G 3 ) 2 , G-quadruplex versions as (CG 3 ) 3 -G-quad, and (C 3 G 3 ) 2 -G-quad, and solutions containing both configurations as simply (CG 3 ) 3 and (C 3 G 3 ) 2 . ...
... The conductance histograms obtained for (CG 3 ) 3 and (C 3 G 3 ) 2 in a 100 mM KCl solution now show only a single conductance peak ( Figure 5C,D). The conductance values are 3.13 ± 0.8 × 10 −4 G 0 and 3.36 ± 0.3 × 10 −4 G 0 and relate to the expected values for ds(CG 3 ) 3 and ds(C 3 G 3 ) 2 , respectively. These values are similar to but slightly different from those obtained in 100 mM PBS, which is probably due to small differences in the B-form conformation in the presence of different ions [44,45]. ...
DNA is an attractive material for a range of applications in nanoscience and nanotechnology, and it has recently been demonstrated that the electronic properties of DNA are uniquely sensitive to its sequence and structure, opening new opportunities for the development of electronic DNA biosensors. In this report, we examine the origin of multiple conductance peaks that can occur during single-molecule break-junction (SMBJ)-based conductance measurements on DNA. We demonstrate that these peaks originate from the presence of multiple DNA conformations within the solutions, in particular, double-stranded B-form DNA (dsDNA) and G-quadruplex structures. Using a combination of circular dichroism (CD) spectroscopy, computational approaches, sequence and environmental controls, and single-molecule conductance measurements, we disentangle the conductance information and demonstrate that specific conductance values come from specific conformations of the DNA and that the occurrence of these peaks can be controlled by controlling the local environment. In addition, we demonstrate that conductance measurements are uniquely sensitive to identifying these conformations in solutions and that multiple configurations can be detected in solutions over an extremely large concentration range, opening new possibilities for examining low-probability DNA conformations in solutions.
... [23,24,25] These variables can have a profound effect on the charge transport properties of dsDNA, changing the conductance over many orders of magnitude. [26,27] These results all indicate that DNA is a versatile material with many parameters that could be engineered to exhibit desirable electronic properties in designed structures such as DNA origami. ...
Exploring the structural and electrical properties of DNA origami nanowires is an important endeavor for the advancement of DNA nanotechnology and DNA nanoelectronics. Highly conductive DNA origami nanowires are a desirable target for creating low‐cost self‐assembled nanoelectronic devices and circuits. In this work, the structure‐dependent electrical conductance of DNA origami nanowires is investigated. A silicon nitride (Si3N4) on silicon semiconductor chip with gold electrodes was used for collecting electrical conductance measurements of DNA origami nanowires, which are found to be an order of magnitude less electrically resistive on Si3N4 substrates treated with a monolayer of hexamethyldisilazane (HMDS) (∼10¹³ ohms) than on native Si3N4 substrates without HMDS (∼10¹⁴ ohms). Atomic force microscopy (AFM) measurements of the height of DNA origami nanowires on mica and Si3N4 substrates reveal that DNA origami nanowires are ∼1.6 nm taller on HMDS‐treated substrates than on the untreated ones indicating that the DNA origami nanowires undergo increased structural deformation when deposited onto untreated substrates, causing a decrease in electrical conductivity. This study highlights the importance of understanding and controlling the interface conditions that affect the structure of DNA and thereby affect the electrical conductance of DNA origami nanowires.
... Such as fast response time, simple structure, high reliability, and low cost [7,14]. In the era of the constant demand for electronic components, molecular electronics have attracted more and more attention, and increasingly research objects have entered view, including atomic chains, organic molecules, Fullerene, DNA molecules [15], carbon nanotubes [6], etc. In the past few decades, many techniques and concepts related to molecular electronics have been originally explored, and significant progress has been made in the field of single-molecule electronics. ...
... We study the CT for four typical number of units (n = 5, 10,15,20). The excited states correspond to the strongest absorption peaks in the NIR and MIR regions for molecules of different lengths. ...
Atomic chains and organic conjugated molecules are of great important research value in molecular optoelectronics, due to their special optoelectronic properties. The fully conjugated nature of ladder phenylenes (LPs) provide some unique properties that have potential applications in the fabrication of molecular electronics devices. Our results reveal optoelectronic properties apply density function theory and non-equilibrium green's function theory, including unit-dependent light absorption, Raman scattering, phonon energy band structure, the chemical potential dependent density of states, electrical conductivity, I-V curve, transmission spectrum, etc. Our research provides theoretical guidance for the regulation of light-harvesting regions based on LPs structures, and theoretical support for the design of nano-scale optoelectronic devices.
... In the quest of the miniaturization of electronic devices, dsDNA has emerged as a promising candidate to replace the conventional materials [15][16][17] . Charge migration in dsDNA is a vast research area leading to the development of several practical applications, from the construction of nanoscale biosensors to an enzymatic tool to detect damage in the genome 15,[17][18][19][20][21][22][23][24][25][26][27][28] . dsDNA molecules inevitably suffer oxidative damages by the reactive oxidative species (ROS) 29,30 causing several DNA lesions and diseases such as cancer and holds a huge biological significance [30][31][32][33][34] . ...
In this work, we report a novel strategy to construct molecular diodes with a record tunable rectification ratio of as high as 10^6 using oxidatively damaged DNA molecules. Being exposed to several endogenous and exogenous events, DNA suffers constant oxidative damages leading to oxidation of guanine to 8-Oxoguanine (8oxoG). Here, we study the charge migration properties of native and oxidatively damaged DNA using a multiscale multiconfigurational methodology comprising of molecular dynamics, density functional theory and kinetic Monte Carlo simulations. We perform a comprehensive study to understand the effect of different concentrations and locations of 8oxoG in a dsDNA sequence on its CT properties and find tunable rectifier properties having potential applications in molecular electronics such as molecular switches and molecular rectifiers. We also discover the negative differential resistance properties of fully oxidized Drew-Dickerson sequence. The presence of 8oxoG guanine leads to the trapping of charge, thus operates as a charge sink, which reveals how oxidized guanine saves the rest of the genome from further oxidative damage.
... Since then, many fundamental aspects of molecular electronics have been extensively developed, helped by the development of platforms to reliably electrically contact molecules and methods to theoretically model their transport properties. [2][3][4][5] Molecular electronics has even been extended beyond fundamental studies, for example larger area molecular junctions (MJs) have been recently commercially deployed as an active component in audio distortion circuits for guitar pedals 6 . Efficient charge transport across individual molecules and electrode interfaces is essential for many chemical, physical and biological processes. ...
... The alteration of a single base in the stack can either increase or decrease the conductivity of the dsDNA helix. For example, while switching a T-A bp to a T-G bp can increase the DNA conductance by 50%, changing a well-matched C-G bp to C-A can decrease its conductance by more than an order of magnitude [21]. All of the above properties make DNA a superior choice as a switchable material. ...
Over the past few decades, optoelectronic devices have played a crucial role in human life and modern technology. To meet the development trends of the industry, photonics with tunable functions have emerged as building blocks with immense potential in controlling light–matter interactions, sensors, and integrated photonics. Compared with artificially designed materials and physical approaches, stimuli-responsive biointerfaces enable a higher level of functionalities and versatile means to tailor optical responses at the nanoscale. Recent advances in biological tunable photonics have attracted tremendous attention owing to the incorporation of living biomaterials into organic photonic and photoelectric devices. In this review, we highlight the advances made in biological tunable photonics during the past five years. We begin with an overview of the competency of natural biological materials, followed by the introduction of key stimuli that have a dominant influence on the development of active biointerfaces. Lastly, we present a comprehensive summary of optoelectronic applications that utilize living biomaterials as active controls. Such applications include bioactivated light-emitting diodes, biological lasers, active plasmonics, robotics, biological logic gates, light-harvesting antennas, molecular photonic wires, and biophotovoltaics. The opportunities and challenges for future research directions are also discussed.
