Electrical conduction through DNA molecules

The question of whether DNA is able to transport electrons has attracted much interest, particularly as this ability may play a role as a repair mechanism after radiation damage to the DNA helix. Experiments addressing DNA conductivity have involved a large number of DNA strands doped with intercalated donor and acceptor molecules, and the conductivity has been assessed from electron transfer rates as a function of the distance between the donor and acceptor sites. But the experimental results remain contradictory, as do theoretical predictions. Here we report direct measurements of electrical current as a function of the potential applied across a few DNA molecules associated into single ropes at least 600 nm long, which indicate efficient conduction through the ropes. We find that the resistivity values derived from these measurements are comparable to those of conducting polymers, and indicate that DNA transports electrical current as efficiently as a good semiconductor. This property, and the fact that DNA molecules of specific composition ranging in length from just a few nucleotides to chains several tens of micrometres long can be routinely prepared, makes DNA ideally suited for the construction of mesoscopic electronic devices.     

DNA trapping electrophoresis

Attempts to improve the size separation of single-stranded DNA in polyacrylamide gels by field-inversion gel electrophoresis (FIGE) have met with limited success. Here we show that attaching a neutral globular protein, streptavidin, to one end of a single-stranded DNA molecule profoundly alters the DNA mobility pattern and increases the band separation manyfold within a size range controlled by voltage and pulse cycle. In constant field, short modified fragments are only slightly retarded but long molecules are retarded dramatically above a 'threshold size' of 0.6 kilobases at 60 V per cm. At this voltage, molecules above a 1.2-kilobase 'cut-off' do not enter the gel. Both the threshold and the cut-off sizes decrease as the voltage increases. In FIGE, the longer the reverse pulse, the larger the modified fragments that enter the gel. We interpret these results as the trapping by the gel matrix of the protein attached to the DNA. The probability of release then depends on the balance between the electric field and thermal motion: the larger the DNA and the higher the voltage, the harder it is to release.     

A nanometre-scale electronic switch consisting of a metal cluster and redox-addressable groups

So-called bottom-up fabrication methods aim to assemble and integrate molecular components exhibiting specific functions into electronic devices that are orders of magnitude smaller than can be fabricated by lithographic techniques. Fundamental to the success of the bottom-up approach is the ability to control electron transport across molecular components. Organic molecules containing redox centres-chemical species whose oxidation number, and hence electronic structure, can be changed reversibly-support resonant tunnelling and display promising functional behaviour when sandwiched as molecular layers between electrical contacts, but their integration into more complex assemblies remains challenging. For this reason, functionalized metal nanoparticles have attracted much interest: they exhibit single-electron characteristics (such as quantized capacitance charging) and can be organized through simple self-assembly methods into well ordered structures, with the nanoparticles at controlled locations. Here we report scanning tunnelling microscopy measurements showing that organic molecules containing redox centres can be used to attach metal nanoparticles to electrode surfaces and so control the electron transport between them. Our system consists of gold nanoclusters a few nanometres across and functionalized with polymethylene chains that carry a central, reversibly reducible bipyridinium moiety. We expect that the ability to electronically contact metal nanoparticles via redox-active molecules, and to alter profoundly their tunnelling properties by charge injection into these molecules, can form the basis for a range of nanoscale electronic switches.     

Dependence of single-molecule junction conductance on molecular conformation

Since it was first suggested that a single molecule might function as an active electronic component, a number of techniques have been developed to measure the charge transport properties of single molecules. Although scanning tunnelling microscopy observations under high vacuum conditions can allow stable measurements of electron transport, most measurements of a single molecule bonded in a metal-molecule-metal junction exhibit relatively large variations in conductance. As a result, even simple predictions about how molecules behave in such junctions have still not been rigorously tested. For instance, it is well known that the tunnelling current passing through a molecule depends on its conformation; but although some experiments have verified this effect, a comprehensive mapping of how junction conductance changes with molecular conformation is not yet available. In the simple case of a biphenyl--a molecule with two phenyl rings linked by a single C-C bond--conductance is expected to change with the relative twist angle between the two rings, with the planar conformation having the highest conductance. Here we use amine link groups to form single-molecule junctions with more reproducible current-voltage characteristics. This allows us to extract average conductance values from thousands of individual measurements on a series of seven biphenyl molecules with different ring substitutions that alter the twist angle of the molecules. We find that the conductance for the series decreases with increasing twist angle, consistent with a cosine-squared relation predicted for transport through pi-conjugated biphenyl systems.     

基于可控Cd掺杂In2O3纳米线的电学特性研究

文章利用化学气相沉积法合成了不同摩尔比的Cd掺杂的In2O3纳米线,制备了基于单根In2O3纳米线的底栅场效应晶体管,并研究了其电输运特性。结果表明,相对未掺杂的In2O3纳米线,In2O3∶Cd纳米线的电导率有1～2个数量级变化,载流子迁移率高达58.1cm2/(V.s),载流子浓度高达3.7×1018 cm-3。可控Cd掺杂In2O3纳米线将在纳米光电子器件方面有着广泛的应用前景。     

应变SrTiO_3/GaAs异质结的整流特性研究

采用脉冲激光沉积法在P型GaAs基片上制备了缺氧的钛SrTiO3薄膜.X射线衍射测量证明SrTiO3薄膜外延生长.I-V曲线测量显示很好的整流性,说明该SrTiO3薄膜与GaAs形成p-n结.该结的电输运机制为应变导致的隧穿电流,且其电输运性质不受光照影响.     

分子链长对分子结电输运性质的影响

利用杂化密度泛函理论,研究了烷烃硫醇分子与金电极形成分子结的电子结构,利用弹性散射格林函数方法研究了烷烃硫醇分子的电输运性质,并同实验结果进行了比较。研究结果表明,在低的外加偏压下,烷烃硫醇分子电流值随着分子链长度的增加而指数减小。     

Functional analysis of an archaebacterial voltage-dependent K+ channel

All living organisms use ion channels to regulate the transport of ions across cellular membranes. Certain ion channels are classed as voltage-dependent because they have a voltage-sensing structure that induces their pores to open in response to changes in the cell membrane voltage. Until recently, the voltage-dependent K+, Ca2+ and Na+ channels were regarded as a unique development of eukaryotic cells, adapted to accomplish specialized electrical signalling, as exemplified in neurons. Here we present the functional characterization of a voltage-dependent K+ (K(V)) channel from a hyperthermophilic archaebacterium from an oceanic thermal vent. This channel possesses all the functional attributes of classical neuronal K(V) channels. The conservation of function reflects structural conservation in the voltage sensor as revealed by specific, high-affinity interactions with tarantula venom toxins, which evolved to inhibit eukaryotic K(V) channels.     

Atomic scale movement of the voltage-sensing region in a potassium channel measured via spectroscopy

Voltage-gated ion channels are transmembrane proteins that are essential for nerve impulses and regulate ion flow across cell membranes in response to changes in membrane potential. They are made up of four homologous domains or subunits, each of which contains six transmembrane segments. Studies of potassium channels have shown that the second (S2) and fourth (S4) segments contain several charged residues, which sense changes in voltage and form part of the voltage sensor. Although these regions clearly undergo conformational changes in response to voltage, little is known about the nature of these changes because voltage-dependent distance changes have not been measured. Here we use lanthanide-based resonance energy transfer to measure distances between Shaker potassium channel subunits at specific residues. Voltage-dependent distance changes of up to 3.2 A were measured at several sites near the S4 segment. These movements directly correlated with electrical measurements of the voltage sensor, establishing the link between physical changes and electrical charge movement. Measured distance changes suggest that the region associated with the S4 segment undergoes a rotation and possible tilt, rather than a large transmembrane movement, in response to voltage. These results demonstrate the first in situ measurement of atomic scale movement in a trans-membrane protein.     

Exciton condensation and perfect Coulomb drag

Coulomb drag is a process whereby the repulsive interactions between electrons in spatially separated conductors enable a current flowing in one of the conductors to induce a voltage drop in the other. If the second conductor is part of a closed circuit, a net current will flow in that circuit. The drag current is typically much smaller than the drive current owing to the heavy screening of the Coulomb interaction. There are, however, rare situations in which strong electronic correlations exist between the two conductors. For example, double quantum well systems can support exciton condensates, which consist of electrons in one well tightly bound to holes in the other. 'Perfect' drag is therefore expected; a steady transport current of electrons driven through one quantum well should be accompanied by an equal current of holes in the other. Here we demonstrate this effect, taking care to ensure that the electron-hole pairs dominate the transport and that tunnelling of charge between the quantum wells, which can readily compromise drag measurements, is negligible. We note that, from an electrical engineering perspective, perfect Coulomb drag is analogous to an electrical transformer that functions at zero frequency.     

电势降落对DNA分子器件电荷输运的影响

基于晶格格林函数和Landauer-Büttiker公式,研究了脱氧核糖核酸分子器件在不同电势降落下的电荷输运性质。界面处的电势降落可以导致负微分电导现象的出现,而且随着电势降落在脱氧核糖核酸分子上的比例的提高,这个效应更加明显。电势降落导致的分子轨道的局域化是产生负微分电导现象的关键因素。     

Pr替代La5/8Ca3/8MnO3体系的磁性与电输运特性

系统地研究了多晶La5/8-xPrxCa3/8MnO3(x=0,0.10,0.13,0.15)体系的磁性和电输运特性,并报道了这一体系的电阻率极小值行为.X射线粉末衍射测量表明,所有的样品都具有较好的单相结构;电输运和磁性测量结果表明,随掺杂量的增大,居里温度Tc和绝缘体-金属转变温度TMI都向低温区移动.在较低温度下电阻率表现出了极小值现象,而这一现象随外加磁场的增大逐渐受到抑制,对此现象从强电子-电子相互作用角度进行了分析讨论.在Tc和TMI转变温.度区域,样品表现出较大的磁电阻效应.样品在高温下的电输运行为可根据可变程跃迁机制得到很好的解释.     

Electrical effects of spin density wave quantization and magnetic domain walls in chromium

The role of magnetic domains (and the walls between domains) in determining the electrical properties of ferromagnetic materials has been investigated in great detail for many years, not least because control over domains offers a means of manipulating electron spin to control charge transport in 'spintronic' devices. In contrast, much less attention has been paid to the effects of domains and domain walls on the electrical properties of antiferromagnets: antiferromagnetic domains show no net external magnetic moment, and so are difficult to manipulate or probe. Here we describe electrical measurements on chromium--a simple metal and quintessential spin density wave antiferromagnet--that show behaviour directly related to spin density wave formation and the presence of antiferromagnetic domains. Two types of thermal hysteresis are seen in both longitudinal and Hall resistivity: the first can be explained by the quantization of spin density waves due to the finite film thickness (confirmed by X-ray diffraction measurements) and the second by domain-wall scattering of electrons. We also observe the striking influence of the electrical lead configuration (a mesoscopic effect) on the resistivity of macroscopic samples in the spin density wave state. Our results are potentially of practical importance, in that they reveal tunable electrical effects of film thickness and domain walls that are as large as the highest seen for ferromagnets.     

有机手性分子器件的光电特性

目前多种有机手性分子器件虽已研制成功,但其内在的物理机理仍有许多未解之谜,其中手性分子的圆二色性精细结构、手性诱导的自旋选择效应等是有机手性分子研究的核心。为设计基于手性的新型有机功能器件提供理论指导,考虑有机手性分子螺旋势场诱导的自旋-轨道耦合,围绕分子的光电特性及其调控展开了系列研究。根据光致跃迁理论,得到手性分子的光吸收谱和圆二色谱,发现光吸收峰发生劈裂,圆二色谱由轨道磁矩和自旋磁矩共同贡献。此外,从极化子输运的图像解释了手性诱导自旋选择效应的来源,并利用其电输运特性,设计了手性异质结器件,发现其手性电阻可达7%,整流比达48。     

Nanomechanical oscillations in a single-C60 transistor

The motion of electrons through quantum dots is strongly modified by single-electron charging and the quantization of energy levels. Much effort has been directed towards extending studies of electron transport to chemical nanostructures, including molecules, nanocrystals and nanotubes. Here we report the fabrication of single-molecule transistors based on individual C60 molecules connected to gold electrodes. We perform transport measurements that provide evidence for a coupling between the centre-of-mass motion of the C60 molecules and single-electron hopping--a conduction mechanism that has not been observed previously in quantum dot studies. The coupling is manifest as quantized nano-mechanical oscillations of the C60 molecule against the gold surface, with a frequency of about 1.2 THz. This value is in good agreement with a simple theoretical estimate based on van der Waals and electrostatic interactions between C60 molecules and gold electrodes.     

DNA 分子中热变现象的简化动力学模型探索

在用非平衡态输运理论对ＤＮＡ分子的热变现象进行描述与研究的基础上,力图寻求一个能较全面考虑ＤＮＡ分子结构及其动力学行为的较为合理的简化动力学模型,并期望此模型不但能描述ＤＮＡ分子的整体热变性质,而且还能描述ＤＮＡ局部热变,以便能进一步探索热变的动力学机制,是用理论物理方法探讨生物学现象的初步尝试。     

Eu-Ru共掺NiO-SnO2复合纳米粒子薄膜的阻变特性

通过低温水浴法制备了Eu-Ru共掺杂NiO-SnO2复合纳米粒子，透射电镜图像显示纳米粒子粒径均匀，选区电子衍射表明结晶性差，所测晶面间距与SnO2和NiO相应卡片数据一致，水热机理分析表明纳米粒子由NiO-SnO2微观p-n结组成.原子力显微镜测试薄膜表面平均粗糙度约025nm，由于薄膜太薄及样品结晶性差，XRD分析未见明显衍射峰.电学测试表明纳米粒子薄膜具有可重复双极阻变特性，阈值电压约1V，开关比约500.薄膜高阻态电学输运符合缺陷俘获载流子所致空间电荷限制导电机制，低阻态呈欧姆特性，故阻变机理应为电荷俘获及再释.     

Single-electron transistor of a single organic molecule with access to several redox states

A combination of classical Coulomb charging, electronic level spacings, spin, and vibrational modes determines the single-electron transfer reactions through nanoscale systems connected to external electrodes by tunnelling barriers. Coulomb charging effects have been shown to dominate such transport in semiconductor quantum dots, metallic and semiconducting nanoparticles, carbon nanotubes, and single molecules. Recently, transport has been shown to be also influenced by spin--through the Kondo effect--for both nanotubes and single molecules, as well as by vibrational fine structure. Here we describe a single-electron transistor where the electronic levels of a single pi-conjugated molecule in several distinct charged states control the transport properties. The molecular electronic levels extracted from the single-electron-transistor measurements are strongly perturbed compared to those of the molecule in solution, leading to a very significant reduction of the gap between the highest occupied molecular orbital and the lowest unoccupied molecular orbital. We suggest, and verify by simple model calculations, that this surprising effect could be caused by image charges generated in the source and drain electrodes resulting in a strong localization of the charges on the molecule.     

AlGaN/GaN heterostructure field transistor for label-free detection of DNA hybridization

This paper demonstrates electrical detection of single strand deoxyribonucleic acid (ssDNA) conjugation by AlGaN/GaN hetero-structure field effect transistor (HFET) biological sensors. The probe ssDNA molecules are modified by thiol groups. The immobilization of probe molecules is achieved by S-Au bonding on a thin layer of gold film in the sensing area. The immobilization and hybridization process are firstly implemented on Si surfaces and checked by fluorescent and atomic force microscopy (AFM) imaging. The hybridization process is monitored on AlGaN/GaN HFETs. Time-dependent current change is observed when a matched ssDNA solution is applied, while no response is observed for a mismatched ssDNA sequence. The DNA hybridization process is dominated by the conjugation between matched ssDNA sequences in the first few tens of seconds. After that, the hybridization process is dominated by mass transfer processes and saturation of the immobilized probe ssDNA molecules.