Fractional quantum conductance in gold nanowires

The conductance of a nanoscopic wire decreases in steps when it is stretched until it breaks. This is due to narrowing of the wire whereby quantized conductance channels sequentially close. However the conductance plateaus seldom occur at integral multiples of the quantum of conductance G₀ and most steps are much smaller than G₀. High speed precision measurements of the conductance steps reveal that the nanowires are composed of not one but several quantized conductors in series and that a step is caused by a quantized conductance change in one of the elements in the sequence. Resolved series conductance quanta up to 20 G₀ have been observed at room temperature. The effect is explained in terms of elastic electronic scattering and has important consequences for nano-electronic circuitry.     

Fractional conductance in hydrogen-embedded gold nanowires

Interaction of the physically adsorbed molecular hydrogen with a breaking gold nanowire results in additional stable atomic configurations in few atom contacts and appearance of fractional peaks in the conductance histogram. This effect is explained by peculiar dynamic evolution of the hydrogen-embedded nanoconstriction due to competition between tensile and capillary forces. Dimerization within the atomic wire and hydrogen-assisted stabilization of gold dimers results in preferable atomic arrangements with conductivity close to 0.5 and 1.5 of quantum conductance unit G(0)=2e(2)/h.     

Novel structures and properties of gold nanowires

The structures of free-standing gold nanowires are studied by using molecular-dynamics-based genetic algorithm simulations. Helical and multiwalled cylindrical structures are found for the thinner nanowires, while bulk-like fcc structures eventually form in the thicker nanowires up to 3 nm in diameter. This noncrystalline-crystalline transition starts from the core region of nanowires. The vibrational, electronic, and transport properties of nanowires are investigated based on the optimal structures. Bulklike behaviors are found for the vibrational and electronic properties of the nanowires with fcc crystalline structure. The conductance of nanowires generally increases with wire diameter and depends on the wire structure.     

Structural and electronic properties of gold nanowires

We have used high resolution transmission electron microscopy to determine the structure of gold nanowires generated by mechanical stretching. Just before rupture, the contacts adopt only three possible atomic configurations, whose occurrence probabilities and quantized conductance were subsequently estimated. These predictions have shown a remarkable agreement with conductance measurements from a break junction operating in ultra-high-vacuum, corroborating the derived correlation between nanowire atomic structure and conductance behavior. Received 28 November 2000     

Welding of gold nanowires with different joining procedures

Welding of single-crystal metallic nanowires is likely to have an important role in the bottom-up fabrication of nanodevices. The welding effects of free ends of two single-crystal gold nanowires (Au–Au) were demonstrated by Monte Carlo simulations in this paper. The quantum corrected Sutton–Chen type many-body potential was used to model the metal–metal interactions. Metallic nanowires were first placed closely with head-to-head, head-to-side and side-to-side joining procedures. Two ends were successfully welded together to form a continuous nanowire by annealing at different temperatures. The welding effects of the different joining procedure with different temperatures were compared. Structures of the welded specimens were characterized by the common neighbor analysis technique. Variable atomic mobility, freedom and contacting angles may result in different bonding strengths in the three different configurations. The results showed that the joint structure welded at low temperature were similar to the cold welding without fusion meanwhile the molten phase was presented in the joint when processing at the high temperatures.     

Synthesis of gold nanowires with controlled crystallographic characteristics

The controlled fabrication of poly- and single-crystalline Au nanowires is reported. In polycarbonate templates, prepared by heavy-ion irradiation and subsequent etching, Au nanowires with diameters down to 25 nm are electrochemically synthesized. Four-circle X-ray diffraction and transmission electron microscopy measurements demonstrate that wires deposited potentiostatically at a voltage of -1.2 V at 65 °C are single-crystalline and oriented along the [110] direction. By reverse-pulse electrodeposition, wires oriented along the [100] direction are grown. The wires are cylindrical over their whole length. The morphology of the caps growing on top of poly- and single-crystalline wires is a strong indication of the particular crystalline structure of the nanowires. PACS 61.46.-w; 81.07.-b     

Two-stage formation model and helicity of gold nanowires

A model for the formation of helical multishell gold nanowires is proposed and is confirmed with quantum mechanical molecular dynamics simulations. The model can explain the magic number of the helical gold nanowires in the multishell structure. The reconstruction from ideal nonhelical to realistic helical nanowires consists of two stages: dissociations of atoms on the outermost shell from atoms on the inner shell and slip deformations of atom rows generating (111)-like structure on the outermost shell. The elementary processes are governed by competition between energy loss and gain by s and d electrons together with the width of the d band. The possibility for the helical nanowires of platinum, silver, and copper is discussed.     

Role of ions in the colloidal synthesis of gold nanowires

Gold nanocrystals of different shapes have been made by a wet chemical approach based on a two-step, seed-mediated synthesis. In this paper, we demonstrate a one-step synthetic method for achieving simple and systematic control over the shape of gold nanoparticles. Gold nanowires, which have been prepared by multi-step approaches, are produced in very high yield in this single-step technique. The width of the rods can be varied over a broader range compared to previously reported methods. Rectangle-, cube- or tetrapod-like gold nanocrystals can also be prepared in aqueous solution at room temperature. The formation of various shapes, in the presence of silver nitrate, requires bromide ion and alkylammonium surfactant ion of appropriate hydrocarbon tail length. The shape, dimension and yield of the nanocrystals depend on the nature and concentrations of the stabilizing cationic surfactants and other additives, such as salts, in addition to the reactants.     

Magnetic properties of one-dimensional embedded nickel nanostructures in gold nanowires

Magnetic nanostructures of nickel embedded in gold were successfully fabricated by electrochemical deposition in porous alumina templates. Structural characterization of the samples confirmed the formation of pure phase, crystalline multi-segmented Au-Ni-Au nanowires. Magnetic characterization of the wires reveals that ferromagnetism arises as a result of Ni embedded in Au segments. An interesting behavior of coercivity was observed that showed a rapid decrease of coercivity for smaller Ni segments while a monotonic decrease was found for the larger segments. Finally, the saturation magnetization of the wires exhibited a slower increase for smaller Ni segments while a sharp increase was observed for larger Ni segments.     

Effect of impurities in the large Au-Au distances in gold nanowires

Experimentally obtained atomically thin gold nanowires have presented exceedingly large Au-Au interatomic distances before they break. Since no theoretical calculations of pure gold nanowires have been able to produce such large distances, we have investigated, through ab initio calculations, how impurities could affect them. We have studied the effect of H, B, C, N, O, and S impurities on the nanowire electronic and structural properties, in particular how they affect the maximum Au-Au bond length. We find that the most likely candidates to explain the distances in the range of 3.6 A and 4.8 A are H and S impurity atoms, respectively.     

First-principles study of electron-conduction properties of helical gold nanowires

Multishell helical gold nanowires (HGNs) suspended between semi-infinite electrodes are found to exhibit peculiar electron-conduction properties by first-principles calculations based on the density functional theory. Our results that the numbers of conduction channels in the HGNs and their conductances are smaller than those expected from a single-atom row nanowire verify the recent experiment. In addition, we obtained a more striking result that, in the cases of thin HGNs, distinct magnetic fields are induced by the electronic current helically flowing around the shells. This finding indicates that the HGNs can be good candidates for nanometer-scale solenoids.     

Signature of atomic structure in the quantum conductance of gold nanowires

We have used high resolution transmission electron microscopy to determine the structure of gold nanowires generated by mechanical stretching. Just before rupture, the contacts adopt only three possible atomic configurations, whose occurrence probabilities and quantized conductance were subsequently estimated. These predictions have shown a remarkable agreement with conductance measurements from a break junction operating in ultrahigh vacuum, corroborating the derived correlation between nanowire atomic structure and conductance behavior.     

Novel voltage signal at proximity-induced superconducting transition temperature in gold nanowires

We observed a novel voltage peak in the proximity-induced superconducting gold (Au) nanowire while cooling the sample through the superconducting transition temperature. The voltage peak turned dip during warming. The voltage peak or dip was found to originate respectively from the emergence or vanishing of the proximity-induced superconductivity in the Au nanowire. The amplitude of the voltage signal depends on the temperature scanning rate, and it cannot be detected when the temperature is changed slower than 0.03 K/min. This transient feature suggests the non-equilibrium property of the effect. Ginzburg-Landau model clarified the voltage peak by considering the emergence of Cooper pairs of relatively lower free energy in superconducting W contact and the non-equilibrium diffusion of Cooper pairs and quasiparticles.     

Molecular dynamics simulation of the solidification of liquid gold nanowires

The solidification behavior of liquid gold nanowires with about 1.84 nm in diameter has been studied by using molecular dynamics simulation with an embedded atom potential. It is found the cooling rate has great effect on the final structure of the gold nanowires during solidification from liquid. With the decrease of cooling rates, the final structure of the gold nanowires varies from amorphous to crystalline via helical multi-shelled structure. The face-centered cubic structure of the gold nanowires is proven energetically the most stable form.     

Formation of gold nanowires through self-assembly during scanning force microscopy

Gold films with a nominal thickness of 5–40 monolayers were grown on dielectric substrates and imaged by scanning force microscopy (SFM). The films originally consisted of well-separated or densely packed clusters. During imaging in contact mode, the morphology of the films changed drastically. At low coverage, i.e. Θ<10 monolayers, the well-known stripes originating from mobile clusters, eventually accumulated into larger aggregates, were observed. In contrast, at larger coverage, highly ordered structures consisting of one-dimensional wires evolved during scanning. They often were parallel with equal separation, i.e. well-defined periodicity, over distances of several μm. Typically, the wires were 5–10 nm high and 50–100 nm wide. Investigations of Au films prepared at varying temperature on different dielectric substrates allow us to suggest a self-assembling mechanism for wire formation in which gold is periodically collected by the SFM tip and redeposited as soon as a critical amount is reached. Received: 22 February 1999 / Accepted: 2 March 1999 / Published online: 7 April 1999     

Circular dichroism in the optical second-harmonic emission of curved gold metal nanowires

Here we report the experimental observation of circular dichroism in the second-harmonic field (800-400 nm conversion) generated by self-organized gold nanowire arrays with subwavelength periodicity (160 nm). Such circular dichroism, raised by a nonlinear optical extrinsic chirality, is the evident signature of the sample morphology. It arises from the curvature of the self-assembled wires, producing a lack of symmetry at oblique incidence. The results were compared, both in the optical linear and nonlinear regime, with a reference sample composed of straight wires. Despite the weak extrinsic optical chirality of our samples (not observable by our optical linear measurements), high visibility (more than 50%) was obtained in the second-harmonic generated field.     

Electrochemical albumin sensing based on silicon nanowires modified by gold nanoparticles

Si nanowires (SiNWs) were modified by Au nanoparticles (AuNPs) using a self-assembled monolayer of aminopropyltriethoxysilane (APTES) and used for direct sensing of the bovine serum albumin (BSA). It was shown that repeated thermal treatment of the sensor greatly enhanced the reliability of the SiNW sensor by increasing the electrical conductivity largely from carbonization of the APTES molecules and from bringing the AuNPs in intimate contact with the SiNW surface. The AuNP-modified SiNW array sensor was able to detect 1-7 μM of BSA. The sensor exhibited a good sensitivity over the tested concentration range and linear behavior. It is expected that the proposed label-free biosensor can be further developed to selectively detect and quantify biomolecules other than BSA.     

Synthesis and thermal stability of gold nanowires within monolithic mesoporous silica

This paper describes the preparation, by a novel and simple method, and the thermal stability of gold nanowires within monolithic mesoporous silica, involving soaking monolithic mesoporous silica in HAuCl₄ aqueous solution, followed by drying and subsequent step-annealing. It has been shown that reduction of Au³⁺ within silica pores can occur during the drying process at 80 °C without any special reduction treatment. After initial annealing at 300 °C, Au nanowires are formed within the pores and are stable at temperatures up to 500 °C. Increasing the annealing temperature leads to a wire-to-rod-to-sphere morphological transformation of the Au nanowires. The surface-mediated reducing groups (-OH) on the silica pore are responsible for the low-temperature reduction of Au³⁺ ions, and the formation of Au nanowires is attributed to the uni-directional diffusion of Au atoms and the confinement of the pore channels. Spheroidization and breaking at some defects in the Au nanowires during annealing at elevated temperature result in the wire-to-rod-to-sphere transformation, accompanied by a blue-shift of the surface plasmon resonance over a very wide region in the optical spectrum. PACS 81.07.-b; 81.40.-z; 81.05.Rm     

Morphology of Si nanowires fabricated by laser ablation using gold catalysts

Si nanowires (NWs) were fabricated successfully by laser ablation using Au as catalyst. Si wafers were used as the collector. The diameters of Si NWs ranged from 20 to 150 nm. Different forms of Si NWs were observed at different local sites inside a furnace: Si NWs with a high aspect ratio of length to diameter, Si NWs with defects and Si NWs with Au-containing nanoparticles being embedded. Especially, a nano-particle embedded Si NW is a new nanostructure that is observed for the first time. PACS 81.07.-b; 81.07.Bc; 81.16.-c; 81.20.-n     

Helical [110] gold nanowires make longer linear atomic chains

Quantum mechanical molecular dynamics shows that gold nanowires formed along the [110] direction reconstruct upon stress to form helical nanowires. The mechanism for this formation is discussed. These helical nanowires evolve on stretching to form linear atomic chains. Because helical nanowires do not form symmetrical tips, a requirement to stop the growth of atomic chains, these nanowires produce longer atomic chains than other nanowires. These results are obtained resorting to the use of tight-binding molecular dynamics and ab initio electronic structure calculations.