DNA-Based Single-Molecule Electronics: From Concept to Function

Wang, Kun

doi:10.3390/jfb9010008

Cited by 54 publications

(28 citation statements)

References 145 publications

(222 reference statements)

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“…Research on charge transfer within DNA over the past two decades has focused primarily on understanding biologically relevant DNA function − and potential use of DNA in molecular electronics. − However, despite the fact that charge transport within DNA is always accompanied by spin transport, there are far fewer studies focused on spin transport within DNA. A notable recent exception has been provided by Naaman and co-workers, who have shown that the helical chirality of DNA allows it to serve as an effective spin filter, , thus expanding the potential applicability of DNA to quantum information science (QIS). − In addition, our group − and that of Majima , demonstrated that radical pairs (RPs) with initially entangled 2-qubit spin states can be prepared within DNA hairpins by selective photoexcitation of different chromophores incorporated into DNA.…”

Section: Introductionmentioning

confidence: 99%

Photogenerated Spin-Entangled Qubit (Radical) Pairs in DNA Hairpins: Observation of Spin Delocalization and Coherence

et al. 2019

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The ability to prepare physical qubits in specific initial quantum states is a critical requirement for their use in quantum information science (QIS). Subnanosecond photoinduced electron transfer in a structurally well-defined donor–acceptor system can be used to produce an entangled spin qubit (radical) pair in a pure initial singlet state fulfilling this criterion. Synthetic DNA is a promising platform on which to build spin qubit arrays with fixed spatial relationships; therefore, we have prepared a series of DNA hairpins in which naphthalenediimide (NDI) is the chromophore/acceptor hairpin linker, variable-length diblock A- and G-tracts are intermediate donors, and a stilbenediether (Sd) is the terminal donor. Photoexcitation of NDI in these DNA hairpins generates high-yield, long-lived, entangled spin qubit pairs at 85 K, and time-resolved and pulse electron paramagnetic resonance (EPR) spectroscopies are used to probe their spin dynamics. Specifically, measurements of the distance-dependent dipolar coupling between the two spins are used to obtain the average spin qubit pair distance in the absence of the terminal Sd donor and reveal that one of the spins is fully delocalized across up to five adjacent guanines in a G-tract on the EPR time scale. We have recently shown that extensive spin hopping between degenerate sites accessible to one spin of the pair may result in spin decoherence. However, we observe a strong out-of-phase electron spin echo envelope modulation (OOP-ESEEM) signal from the NDI•––Sd•+ spin qubit pair in DNA hairpins showing that spin coherence is maintained across a 2 adenine A-tract followed by a 2–4 guanine G-tract as a result of rapid spin transport to Sd. These results demonstrate that pulse-EPR can manipulate coherent spin states in DNA hairpins, which is essential for quantum gate operations relevant to QIS applications.

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Section: Introductionmentioning

confidence: 99%

Photogenerated Spin-Entangled Qubit (Radical) Pairs in DNA Hairpins: Observation of Spin Delocalization and Coherence

et al. 2019

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“…The last two decades have witnessed a surge of studies of DNA as the basis for molecular wires and molecular electronics devices/circuits, based on self-assembly and specific base hybridization [ 11 , 12 , 13 , 14 , 15 ]. The prospect of using DNA in materials science stems from exploiting its properties of molecular recognition, assembly, and processing information [ 11 ] as well as its ability to transfer or transport charge.…”

Section: Introductionmentioning

confidence: 99%

“…Furthermore, currents in the range of 10–100 pA have been measured in G4-DNA over distances in the range of 10–100 nm [ 14 ]. Today, DNA plays an increasingly important role in molecular electronics due to its structural and molecular recognition properties [ 15 ].…”

Section: Introductionmentioning

confidence: 99%

LCAO Electronic Structure of Nucleic Acid Bases and Other Heterocycles and Transfer Integrals in B-DNA, Including Structural Variability

2021

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To describe the molecular electronic structure of nucleic acid bases and other heterocycles, we employ the Linear Combination of Atomic Orbitals (LCAO) method, considering the molecular wave function as a linear combination of all valence orbitals, i.e., 2s, 2px, 2py, 2pz orbitals for C, N, and O atoms and 1s orbital for H atoms. Regarding the diagonal matrix elements (also known as on-site energies), we introduce a novel parameterization. For the non-diagonal matrix elements referring to neighboring atoms, we employ the Slater–Koster two-center interaction transfer integrals. We use Harrison-type expressions with factors slightly modified relative to the original. We compare our LCAO predictions for the ionization and excitation energies of heterocycles with those obtained from Ionization Potential Equation of Motion Coupled Cluster with Singles and Doubles (IP-EOMCCSD)/aug-cc-pVDZ level of theory and Completely Normalized Equation of Motion Coupled Cluster with Singles, Doubles, and non-iterative Triples (CR-EOMCCSD(T))/aug-cc-pVDZ level of theory, respectively, (vertical values), as well as with available experimental data. Similarly, we calculate the transfer integrals between subsequent base pairs, to be used for a Tight-Binding (TB) wire model description of charge transfer and transport along ideal or deformed B-DNA. Taking into account all valence orbitals, we are in the position to treat deflection from the planar geometry, e.g., DNA structural variability, a task impossible for the plane Hückel approach (i.e., using only 2pz orbitals). We show the effects of structural deformations utilizing a 20mer evolved by Molecular Dynamics.

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“…Since then, many publications studying the role of DNA folding into custom shaped nanostructures have been reported with a resolution as small as sub-10 nm . The predefined DNA origami has also been used as a scaffold for construction of higher-order structures. , Correspondingly, the extensive research in DNA origami has opened up new fields like DNA nanolithography and DNA-guided assembly that deliver 2D or 3D nanopatterns with functional electronic materials at high resolutions. − In addition, DNA itself has been observed to have a semiconducting behavior with a large band gap. − When it is used as building blocks for assembling functional nanomaterials, the electronic properties can be further altered through various covalent and noncovalent strategies. − …”

Section: Introductionmentioning

confidence: 99%

DNA-Guided Assemblies toward Nanoelectronic Applications

Vittala

Han

2020

ACS Appl. Bio Mater.

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Programmable DNA-guided self-assembly of nanoscale functional materials is of great interest in the context of nanofabrication or nanoelectronics. Attributed to its unique sequence programmability and precisely defined dimension, DNA has been used as a template for constructing ordered one-, two-, and three-dimensional architectures with organic, inorganic, and polymeric building blocks via various self-assembly strategies. Moreover, the accessible integration capability of DNA with diverse electronics-related materials propels the field of DNA-guided assemblies toward nanoelectronic applications. In this review, we outline the development in the area of DNA-guided assemblies that are constructed from carbon nanotubes, fullerenes, polymers, metals, metal oxides, and minerals using various strategies, with the focus on the bottom-up DNA-guided conducting, semiconducting, and insulating nanomaterials applied on nanoelectronics. We also review some bottom-up and top-down hybrid methods that precisely immobilize functional DNA-guided materials on substrates with high throughput. Finally, we describe the challenges in nanofabrication and potential applications of DNA-guided assemblies in nanoelectronics.

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DNA-Based Single-Molecule Electronics: From Concept to Function

Cited by 54 publications

References 145 publications

Photogenerated Spin-Entangled Qubit (Radical) Pairs in DNA Hairpins: Observation of Spin Delocalization and Coherence

Photogenerated Spin-Entangled Qubit (Radical) Pairs in DNA Hairpins: Observation of Spin Delocalization and Coherence

LCAO Electronic Structure of Nucleic Acid Bases and Other Heterocycles and Transfer Integrals in B-DNA, Including Structural Variability

DNA-Guided Assemblies toward Nanoelectronic Applications

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