Abstract:Charge migration along DNA molecules has attracted scientific interest for over half a century.Reports on possible high rates of charge transfer between donor and acceptor through the DNA, obtained in the last decade from solution chemistry experiments on large numbers of molecules, triggered a series of direct electrical transport measurements through DNA single molecules, bundles and networks. These measurements are reviewed and presented here. From these experiments we conclude that electrical transport is … Show more
“…Representative results on the applications of nanogap electrodes in nano-and single molecular devices have been summarized by several authoritative reviews. [164][165][166][167][168][169][170][171][172][173] Limited by the capacity of the present paper, we do not plan to overlap these reviewed topics, and only focus on the possibility of combining conjugated polymers with nanogap electrodes, in order to introduce the properties associated with conjugated polymers into such nanodevices. Based on our recent experience, [156,[174][175][176][177] we will exemplify this combination using a Since the discovery of conductive polymers in the 1970s, thousands of conjugated polymers have been synthesized and investigated, and some have been successfully applied in polymer electronics since the 1990s.…”
Nanogap electrodes (namely, a pair of electrodes with a nanometer gap) are fundamental building blocks for the fabrication of nanometer‐sized devices and circuits. They are also important tools for the examination of material properties at the nanometer scale, even at the molecular scale. In this review, the techniques for the fabrication of nanogap electrodes, the preparation of assembled devices based on the nanogap electrodes, and the potential application of these nanodevices for analysis of material properties are introduced. The history, the research status, and the prospects of nanogap electrodes are also discussed.
“…Representative results on the applications of nanogap electrodes in nano-and single molecular devices have been summarized by several authoritative reviews. [164][165][166][167][168][169][170][171][172][173] Limited by the capacity of the present paper, we do not plan to overlap these reviewed topics, and only focus on the possibility of combining conjugated polymers with nanogap electrodes, in order to introduce the properties associated with conjugated polymers into such nanodevices. Based on our recent experience, [156,[174][175][176][177] we will exemplify this combination using a Since the discovery of conductive polymers in the 1970s, thousands of conjugated polymers have been synthesized and investigated, and some have been successfully applied in polymer electronics since the 1990s.…”
Nanogap electrodes (namely, a pair of electrodes with a nanometer gap) are fundamental building blocks for the fabrication of nanometer‐sized devices and circuits. They are also important tools for the examination of material properties at the nanometer scale, even at the molecular scale. In this review, the techniques for the fabrication of nanogap electrodes, the preparation of assembled devices based on the nanogap electrodes, and the potential application of these nanodevices for analysis of material properties are introduced. The history, the research status, and the prospects of nanogap electrodes are also discussed.
“…Delocalized coherent transport is dismissed in biomolecules due to their lack of periodicity, random fluctuations, and limited conductance values from experiments. Even for a poly-guanine structure (prime candidate for a conduction pathway building block, owing to its relatively low ionization potential), simulations have shown that their stacking in the DNA duplex should not yield any extended states, or that the band gap is very large (For a thorough review of earlier attempts at explaining charge transport, see [3] and the references therein). In contrast to the familiar phonon-assisted hopping of solid-state physics, Schlag et al [39] proposed a "rest and fire" model for charge hopping along a loose peptide backbone, implemented using classical molecular dynamics simulations and chemical kinetics theory of electron transfer.…”
Section: Conductance Theories For Biomoleculesmentioning
confidence: 99%
“…Usually, tight-binding Hamiltonians are employed to describe electronic structures of DNA duplexes -both explicitly (in the form of the "fishbone", "ladder" and similar models -see, for example, [51,53,58,60,[64][65][66][67][68][69][70][71][72] and the pertinent review articles [3,[73][74][75][76][77] ) and implicitly (within the framework of Marcus-type theories of charge transfer, for example, [55,[78][79][80][81] and the references therein). These works were successful in qualitatively (and sometimes even quantitatively) describing numerous experimental data (see, for example, [42,56,57,82,83] and the references therein) on transfer of injected single holes (or injected single electrons) through DNA duplexes.…”
Section: Critical Assessment Of the Biopolymer Charge Transfer/transpmentioning
Nucleic acids and proteins are not only biologically important polymers: They have recently been recognized as novel functional materials surpassing in many aspects the conventional ones. Although Herculean efforts have been undertaken to unravel fine functioning mechanisms of the biopolymers in question, there is still much more to be done. This particular paper presents the topic of biomolecular charge transport, with a particular focus on charge transfer/transport in DNA and protein molecules. Here the experimentally revealed details, as well as the presently available theories, of charge transfer/transport along these biopolymers are critically reviewed and analyzed. A summary of the active research in this field is also given, along with a number of practical recommendations.)Received: ((will be filled in by the editorial staff))Revised: ((will be filled in by the editorial staff))
“…As a consequence, the identification of the relevant charge transport channels in DNA systems becomes a crucial issue. Transport experiments in DNA derivatives are however quite controversial [4,5]. DNA has been characterized as insulating [6], semiconducting [7] or metallic [8,9].…”
Electronic transport through DNA wires in the presence of a strong dissipative environment is investigated. We show that new bath-induced electronic states are formed within the bandgap. These states show up in the linear conductance spectrum as a temperature dependent background and lead to a crossover from tunneling to thermal activated behavior with increasing temperature. Depending on the strength of the electron-bath coupling, the conductance at the Fermi level can show a weak exponential or even an algebraic length dependence. Our results suggest a new environmentalinduced transport mechanism. This might be relevant for the understanding of molecular conduction experiments in liquid solution, like those recently performed on poly(GC) oligomers in a water buffer (B. Xu et al., Nano Lett. 4, 1105 (2004)).In the emerging field of molecular electronics, DNA oligomers have drawn in the last decade the attention of both experimentalists and theoreticians [1]. This has been mainly motivated by DNA exciting potential applications which include its use as a template in molecular devices or by exploiting its self-assembling and selfrecognition properties [2]. Alternatively, DNA strands might act as molecular wires either in periodic conformations as in poly(GC), or by doping with metal cations as is the case of M-DNA [3]. As a consequence, the identification of the relevant charge transport channels in DNA systems becomes a crucial issue. Transport experiments in DNA derivatives are however quite controversial [4,5]. DNA has been characterized as insulating [6], semiconducting [7] or metallic [8,9]. It becomes then apparent that sample preparation and experimental conditions are more critical than in transport experiments on other nanoscale systems. Meanwhile, a variety of factors that appreciably control charge propagation along the double helix have been theoretically identified: static [10] and dynamical [11] disorder related to random base pair sequences and structural fluctuations, respectively, as well as environmental effects associated with correlated fluctuations of counterions [12] or with the formation of localised states within the bandgap [4,13].Recently, Xu et al. [9] have carried out transport experiments on poly(GC) oligomers in aqueous solution. These experiments are remarkable for different reasons: (i) it was shown that transport characteristics of single molecules were probed, (ii) the molecules displayed ohmic-like behavior in the low-bias I-V characteristics and (iii) the linear conductance showed an algebraic dependence g ∼ N −1 on the number N of base pairs. This latter result suggests the dominance of incoherent charge transport processes. Complex band structure calculations [14] for dry poly(GC) oligomers predict, on the contrary, a rather strong exponential dependence of the conductance on the wire length, a typical result for coherent tunneling through band gaps. Hence,
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