We have fabricated graphene devices with a top gate separated from the graphene layer by an air gap--a design which does not decrease the mobility of charge carriers under the gate. This gate is used to realise p-n-p structures where the conducting properties of chiral carriers are studied. The band profile of the structures is calculated taking into account the specifics of the graphene density of states and is used to find the resistance of the p-n junctions expected for chiral carriers. We show that ballistic p-n junctions have larger resistance than diffusive ones. This is caused by suppressed transmission of chiral carriers at angles away from the normal to the junction.
CO adsorption on an Au monatomic chain is studied within density functional theory in nanocontact geometries as a function of the contact stretching. We compare the bridge and atop adsorption sites of CO, finding that the bridge site is energetically favored at all strains studied here. Atop adsorption gives rise to an almost complete suppression of the ballistic conductance of the nanocontact, while adsorption at the bridge site results in a conductance value close to 0.6 G0, in agreement with previous experimental data. We show that only the bridge site can qualitatively account for the evol…
We carry out a first-principles density functional study of the interaction between a monatomic Pt wire and a CO molecule, comparing the energy of different adsorption configurations (bridge, on top, substitutional, and tilted bridge) and discussing the effects of spin-orbit (SO) coupling on the electronic structure and on the ballistic conductance of two of these systems (bridge and substitutional). We find that, when the wire is unstrained, the bridge configuration is energetically favored, while the substitutional geometry becomes possible only after the breaking of the Pt-Pt bond next to C…
We study the role of anharmonicity at interfaces with an added intermediate layer designed to facilitate interfacial phonon transport. Our results demonstrate that while in the harmonic limit the bridge may lower the conductance due to fewer available channels, anharmonicity can strongly enhance the thermal conductance of the bridged structure due to added inelastic channels. Moreover, we show that the effect of anharmonicity on the conductance can be tuned by varying temperature or the bridge layer thickness, as both parameters change the total rate of occurrence of phonon-phonon scattering p…
The conductance of a molecular junction is commonly determined by either charge-transfer-doping, where alignment of the Fermi energy to the molecular levels is achieved, or tunnelling through the tails of molecular resonances within the highest-occupied and lowest-unoccupied molecular-orbital gap. Here, we present an alternative mechanism where electron transport is dominated by electrode surface states. They give rise to metallization of the molecular bridge and additional, pronounced conductance resonances allowing for substantial tailoring of its electronic properties via, e.g. a gate volta…
Recent years have shown steady progress in research towards molecular electronics [1,2], where molecules have been investigated as switches [3-5], diodes [6], and electronic mixers [7]. In much of the previous work a Scanning Tunnelling Microscope was employed to address an individual molecule. As this arrangement does not provide long-term stability, more recently metal-molecule-metal links have been made using break junction devices [8-10]. However, it has been difficult to establish unambiguously that a single molecule forms the contact [11]. Here, we show that a single H2 molecule can form…
A scanning tunnelling microscope has been used to determine the conductance of single molecular wires with the configuration X-bridge-X, X-bridge-Y and Y-bridge-Y (X = thiol terminus and Y = COOH). We find that for molecular wires with mixed functional groups (X-bridge-Y) the single molecule conductance decreases with respect to the comparable symmetric molecules. These differences are confirmed by theoretical computations based on a combination of density functional theory and the non-equilibrium Green functions formalism. This study demonstrates that the apparent contact resistance, as well …
We study the thermal conductance across solid-solid interfaces as the composition of an intermediate matching layer is varied. In absence of phonon-phonon interactions, an added layer can make the interfacial conductance increase or decrease depending on the interplay between (1) an increase in phonon transmission due to better bridging between the contacts, and (2) a decrease in the number of available conduction channels that must conserve their momenta transverse to the interface. When phonon-phonon interactions are included, the added layer is seen to aid conductance when the decrease in r…
We study the energetics, the electronic structure, and the ballistic transport of an infinite Au monatomic chain with an adsorbed CO molecule. We find that the bridge adsorption site is energetically favored with respect to the atop site, both at the equilibrium Au-Au spacing of the chain and at larger spacings. Instead, a substitutional configuration requires a very elongated Au-Au bond, well above the rupture distance of the pristine Au chain. The electronic structure properties can be described by the Blyholder model, which involves the formation of bonding/antibonding pairs of 5σ and 2π* s…
Stable, single-molecule conducting-bridge configurations are typically identified from peak structures in a conductance histogram. In previous work on Pt with H$_2$ at cryogenic temperatures it has been shown that a peak near 1 $G{_0}$ identifies a single molecule Pt-H$_{2}$-Pt bridge. The histogram shows an additional structure with lower conductance that has not been identified. Here, we show that it is likely due to a hydrogen decorated Pt chain in contact with the H$_2$ molecular bridge.
The low conductance of nickel atomic junctions in the hydrogen environment is studied using the nonequilibrium Green's function theory combined with first-principles calculations. The Ni junction bridged by a $H_2$ molecule has a conductance of approximately 0.7 $G_0$. This conductance is contributed by the anti-bonding state of the $H_2$ molecule, which forms a bonding state with the $3d$ orbitals of the nearby Ni atoms. In contrast, the Ni junction bridged by the two single H atoms has a conductance of approximately 1 $G_0$, which is weakly spin-polarized. The spin-up channels were found to …
We present a single-exposure fabrication technique for a very large array of microscopic air-bridges using a tri-layer resist process with electron-beam lithography. The technique is capable of forming air-bridges with strong metal-metal or metal-substrate connections. This was demonstrated by its application in an electron tunnelling device consisting of 400 identical surface gates for defining quantum wires, where the air-bridges are used as suspended connections for the surface gates. This technique enables us to create a large array of uniform one-dimensional channels that are open at both…
A conducting bridge of a single hydrogen molecule between Pt electrodes is formed in a break junction experiment. It has a conductance near the quantum unit, G_0 = 2e^2/h, carried by a single channel. Using point contact spectroscopy three vibration modes are observed and their variation upon stretching and isotope substitution is obtained. The interpretation of the experiment in terms of a Pt-H_2-Pt bridge is verified by Density Functional Theory calculations for the stability, vibrational modes, and conductance of the structure.
We study the temperature and gate voltage dependence of the conductance of the single electron transistor focusing on highly conducting devices. Electron tunneling is treated nonperturbatively by means of path integral Monte Carlo techniques and the conductance is determined from the Kubo formula. A regularized singular value decomposition scheme is employed to calculate the conductance from imaginary time simulation data. Our findings are shown to bridge between available analytical results in the semiclassical and perturbative limits and are found to explain recent experimental results in a …
Vibrational nonequilibrium effects in charge transport through single-molecule junctions are investigated. Focusing on molecular bridges with multiple electronic states, it is shown that electronic-vibrational coupling triggers a variety of vibronic emission and absorption processes, which influence the conductance properties and mechanical stability of single-molecule junctions profoundly. Employing a master equation and a nonequilibrium Green's function approach, these processes are analyzed in detail for a generic model of a molecular junction and for benzenedibutanethiolate bound to gold e…
Taking into account an inner structure of the arms of the Aharonov-Bohm ring (AB ring) we have analyzed the transport features related to the topological phase transition which is induced in a superconducting wire (SC wire) with strong spin-orbit interaction (SOI). The SC wire acts as a bridge connecting the arms. The in-plane magnetic-field dependence of linear-response conductance obtained using the nonequilibrium Green's functions in the tight-binding approximation revealed the Breit-Wigner and Fano resonances (FRs) if the wire is in the nontrivial phase. The effect is explained by the pres…
We discuss the conductance of a molecular bridge between mesoscopic electrodes supporting low-dimensional transport and bearing an internal structure. As an example for such nanoelectrodes we assume semi-infinite (carbon) nanotubes. In the Landauer scattering matrix approach, we show that the conductance of this hybrid is very sensitive to the geometry of the contact unlike the usual behaviour in the presence of bulk electrodes.
Interface phonon modes that are generated by several atomic layers at the heterointerface play a major role in the interface thermal conductance for nanoscale high-power devices such as nitride-based high-electron-mobility transistors and light emitting diodes. Here we measure the local phonon spectra across AlN/Si and AlN/Al interfaces using atomically resolved vibrational electron energy-loss spectroscopy in a scanning transmission electron microscope. At the AlN/Si interface, we observe various localized phonon modes, of which the extended and interfacial modes act as bridges to connect the…
Feedback-controlled electric breakdown of graphene in air or vacuum is a well-established way of fabricating tunnel junctions, nanogaps, and quantum dots. We show that the method is equally applicable to encapsulated graphene constrictions fabricated using hydrogen silsesquioxane. The silica-like layer left by hydrogen silsesquioxane resist after electron-beam exposure remains intact after electric breakdown of the graphene. We explore the conductance switching behavior that is common in graphene nanostructures fabricated via feedback-controlled breakdown, and show that it can be attributed to…
Graphene is the first example of truly two-dimensional crystals - it's just one layer of carbon atoms. It turns out to be a gapless semiconductor with unique electronic properties resulting from the fact that charge carriers in graphene demonstrate charge-conjugation symmetry between electrons and holes and possess an internal degree of freedom similar to ``chirality'' for ultrarelativistic elementary particles. It provides unexpected bridge between condensed matter physics and quantum electrodynamics (QED). In particular, the relativistic Zitterbewegung leads to the minimum conductivity of or…
We study electron transport through single-molecule junctions formed by an octanethiol molecule bonded with the thiol anchoring group to a gold electrode and the opposing methyl endgroup to a carbon tip. Using the scanning tunneling microscope based break junction technique, we measure the electrical conductance of such molecular junctions. We observe the presence of well-defined conductance plateaus during the stretching of the molecular bridge, which is the signature of the formation of a molecular junction.
We study the properties of an electron on a catenoid surface. The catenoid is understood as a realization of a bridge connecting two graphene layer by a smooth surface. The curvature induces a symmetrical reflectionless potential well around the bridge with one bound-state for $m=0$. For $m\neq 0$, a centrifugal potential barrier arises controlling the tunnelling between the layers. An external electric field breaks the parity symmetry and provides a barrier that controls the conductance from one layer to another. By applying a constant magnetic field the effective potential exhibits a confini…
If the factors controlling the decay in single-molecule electrical conductance G with molecular length L could be understood and controlled, then this would be a significant step forward in the design of high-conductance molecular wires. For a wide variety of molecules conducting by phase coherent tunneling, conductance G decays with length following the relationship G = Aexp-\bηL. It is widely accepted that the attenuation coefficient \bη is determined by the position of the Fermi energy of the electrodes relative to the energy of frontier orbitals of the molecular bridge, whereas the termina…
We demonstrate the reversible in situ photoreduction of molecular junctions of phosphomolybdate [PMo12O40]3- monolayer self-assembled on flat gold electrodes, connected by the tip of a conductive atomic force microscope. The conductance of the one electron reduced [PMo12O40]4- molecular junction is increased by ca. 10, this open-shell state is stable in the junction in air at room temperature. The analysis of a large current-voltage dataset by unsupervised machine learning and clustering algorithms reveals that the electron transport in the pristine phosphomolybdate junctions leads to symmetri…
The interplay between groups of water molecules and single-atom contacts, as reflected in the electrical conductances and mechanical forces of copper atomic junctions, is explored by means of first-principles theory and semi-empirical calculations. We study the influence of the atomic geometries of copper electrodes with pyramidal and non-crystalline structures in the presence and absence of water on the conductance profiles as the electrodes approach each other. It is shown that the atomic arrangements of nano-contacts have crucial effects on the formation of plateaus and the conductance valu…
We investigate the formation and evolution of Au-CO single-molecule break junctions. The conductance histogram exhibits two distinct molecular configurations, which are further investigated by a combined statistical analysis. According to conditional histogram and correlation analysis these molecular configurations show strong anticorrelations with each other and with pure Au monoatomic junctions and atomic chains. We identify molecular precursor configurations with somewhat higher conductance which are formed prior to single-molecule junctions. According to detailed length analysis two distin…
A simple and fast analysis method to sort large data sets into groups with shared distinguishing characteristics is described, and applied to single molecular break junction conductance versus electrode displacement data. The method, based on principal component analysis, successfully sorted data sets based on the projection of the data onto the first or second principal component of the correlation matrix without the need to assert any specific hypothesis about the expected features within the data. This was an improvement on the current correlation matrix analysis approach because it sorted …
Motivated by recent experiments of successfully carving out stable carbon atomic chains from graphene, we investigate a device structure of a carbon chain connecting two zigzag graphene nanoribbons with highly tunable spin-dependent transport properties. Our calculation based on the non-equilibrium Green's function approach combined with the density functional theory shows that the transport behavior is sensitive to the spin configuration of the leads and the bridge position in the gap. A bridge in the middle gives an overall good coupling except for around the Fermi energy where the leads wit…
We have performed first-principles calculations for the mechanic and electric properties of pure Pt nano-contacts and a Pt contact with a single CO molecule adsorbed. For the pure Pt contacts we see a clear difference between point contacts and short chains in good agreement with experiments. We identify a tilted bridge configuration for the Pt-CO-Pt contact, which is stable and has a conductance close to $0.5G_0$ ($G_0=2e^2/h$), and we propose that this structure is responsible for an observed peak at $0.5G_0$ in the conductance histogram for Pt exposed to a CO gas. We explain the main featur…
We validate that off-resonant electron transport across {\it ultra-short} oligomer molecular junctions is characterised by a conductance which decays exponentially with length, and we discuss a method to determine the damping factor via the energy spectrum of a periodic structure as a function of complex wavevector. An exact mapping to the complex wavevector is demonstrated by first-principle-based calculations of: a) the conductance of molecular junctions of phenyl-ethynylene wires covalently bonded to graphitic ribbons as a function of the bridge length, and b) the complex-band structure of …
We consider a model inspired by a metal break-junction hypothetically caught at its breaking point, where the non-adiabatic center-of-mass motion of the bridging atom can be treated as a two-level system. By means of Numerical Renormalization Group (NRG) we calculate the influence of the two level system on the ballistic conductance across the bridge atom. The results are shown to be fully consistent with a conformal field theory treatment. We find that the conductance, calculated by coupling Fermi liquid theory to our NRG is always finite and fractional at zero temperature, but drops quite fa…
Confinement of electrons in graphene to make devices has proven to be a challenging task. Electrostatic methods fail because of Klein tunneling, while etching into nanoribbons requires extreme control of edge terminations, and bottom-up approaches are limited in size to a few nanometers. Fortunately, its mechanical flexibility raises the possibility of using strain to alter graphene's properties and create novel straintronic devices. Here, we report transport studies of nanowires created by linearly-shaped strained regions resulting from individual folds formed by layer transfer onto hexagonal…
The interaction between doped graphene nanoislands connected by narrow junctions constitutes an ideal testbed to probe quantum effects in plasmonic systems. Here, the interaction between graphene plasmons in neighboring nanoislands is predicted to be extremely sensitive to the size and shape of the junctions. The reported {\it ab initio} calculations reveal three different regimes of interaction: (1) for narrow bridges ($<4$ carbon-atom rows), the conductance of the junction is too low to allow electron transport and the optical response is dominated by a characteristic bonding dipolar dimer m…
A high-sensitivity resistance bridge for nanoscale thermal microscopy
Laboratoire national de métrologie et d’essais（法国国家计量和测试实验室）；Institut Langevin, ESPCI Paris, Université PSL, CNRS（朗之万研究所，巴黎高等物理化工学院，巴黎文理研究大学，法国国家科学研究中心）
