arXiv subjects

C. J. Lambert

Publications and source records attributed to C. J. Lambert.

At least 19 recordsLinked to original sources

arXiv2020

Electrical molecular switch addressed by chemical stimuli

We demonstrate that the conductance switching of benzo-bis(imidazole) molecules upon protonation depends on the lateral functional groups. The protonated H-substituted molecule shows a higher conductance than the neutral one (Gpro>Gneu), while the opposite (Gneu>Gpro) is observed for a molecule laterally functionalized by amino-phenyl groups. These results are demonstrated at various scale lengths : self-assembled monolayer, tiny nanodot-molecule junction and single molecules. From ab-initio theoretical calculations, we conclude that for the H-substituted molecule, the result Gpro>Gneu is correctly explained by a reduction of the LUMO-HOMO gap, while for the amino-phenyl functionnalized molecule, the result Gneu>Gpro is consistent with a shift of HOMO, which reduces the density of states at the Fermi energy.

physics.app-ph↗

arXiv2016

A Three State NDI Switch: Integration of Pendant Redox Unit for Conductance Tuning

We studied charge transport phenomena through a core substituted naphthalenediimide (NDI) single-molecule junctions using the electrochemical STM-based break junction technique in combination with DFT calculations. The conductance switch among three well-defined states is acquired by electrochemically controlling the redox state of the pendent diimide unit of the molecule in ionic liquid, and the conductance difference is more than one order of magnitude between di-anion states and neutral state. The potential dependent charge transport characteristics of the NDI molecules are confirmed by DFT calculations accounting for electrochemical double-layer effects on the conductance of the NDI junctions. This work suggests that the integration of redox unit in the pendent position with strong coupling to molecular backbone can significantly tune the charge transport of the single-molecule device by controlling different redox states.

cond-mat.mes-hall↗

arXiv2016

Asymmetry-induced resistive switching in Ag-Ag$_{2}$S-Ag memristors enabling a simplified atomic-scale memory design

Prevailing models of resistive switching arising from electrochemical formation of conducting filaments across solid state ionic conductors commonly attribute the observed polarity of the voltage-biased switching to the sequence of the active and inert electrodes confining the resistive switching memory cell. Here we demonstrate equivalent, stable switching behavior in metallic Ag-Ag$_{2}$S-Ag nanojunctions at room temperature. Our experimental results and numerical simulations reveal that the polarity of the switchings is solely determined by the geometrical asymmetry of the electrode surfaces. By the lithographical design of a proof of principle device we demonstrate the merits of simplified fabrication of atomic-scale, robust planar Ag$_{2}$S memory cells.

cond-mat.mes-hall↗

arXiv2016

Quasiparticle and excitonic gaps of one-dimensional carbon chains

We report diffusion quantum Monte Carlo (DMC) calculations of the quasiparticle and excitonic gaps of hydrogen-terminated oligoynes and polyyne. The electronic gaps are found to be very sensitive to the atomic structure in these systems. We have therefore optimised the geometry of polyyne by directly minimising the DMC energy with respect to the lattice constant and the Peierls-induced carbon-carbon bond-length alternation. We find the bond-length alternation of polyyne to be 0.136(2) Å and the excitonic and quasiparticle gaps to be 3.30(7) and 3.4(1) eV, respectively. The DMC zone-centre longitudinal optical phonon frequency of polyyne is 2084(5) cm$^{-1}$, which is consistent with Raman spectroscopic measurements for large oligoynes.

cond-mat.mes-hall↗

arXiv2015

Creating molecular structures from bilayer graphene and other materials

We demonstrate a new technique for creating unique forms of pure sp2-bonded carbon and unprecedented hetero-molecules. These new structures, which we refer to as sculpturenes, are formed by sculpting selected shapes from bilayer graphene, hetero-bilayers or multi-layered materials and allowing the shapes to spontaneously reconstruct. The simplest sculpturene is topologically equivalent to a torus, with dimensions comparable to those of fullerenes. The topology of these new molecular structures is stable against atomic scale defects.

cond-mat.mtrl-sci↗

arXiv2015

Thermopower of crown-ether-bridged anthraquinones

We investigate strategies for increasing the thermopower of crown-ether-bridged anthraquinones. The novel design feature of these molecules is the presence of either (1) crown-ether or (2) diaza-crown-ether bridges attached to the side of the current-carrying anthraquinone wire. The crown-ether side groups selectively bind alkali- metal cations and when combined with TCNE or TTF dopants, provide a large phase-space for optimising thermoelectric properties. We find that the optimum combination of cations and dopants depends on the temperature range of interest. The thermopowers of both 1 and 2 are negative and at room temperature are optimised by binding with TTF alone, achieving thermpowers of -600 microvolts/K and -285 microvolts/K respectively. At much lower temperatures, which are relevant to cascade coolers, we find that for 1, a combination of TTF and Na+ yields a maximum thermopower of -710 microvolts/K at 70K, whereas a combination of TTF and Li+ yields a maximum thermopower of -600 microvolts/K at 90K. For 2, we find that TTF doping yields a maximum thermopower of -800 microvolts/K at 90K, whereas at 50K, the largest thermopower (of -600 microvolts/K) is obtain by a combination TTF and K+ doping. At room temperature, we obtain power factors of 73 microwatts/m.K2 for 1 (in combination with TTF and Na+ ) and 90 microwatts/m.K2 for 2 (with TTF). These are higher or comparable with reported power factors of other organic materials.

cond-mat.mes-hall↗

arXiv2015

Thermoelectric properties of graphene/boron nitride heterostructures

Using density functional theory combined with a Green's function scattering approach, we examine the thermoelectric properties of hetero-nanoribbons formed from alternating lengths of graphene and boron nitride. In such structures, the boron nitride acts as a tunnel barrier, which weakly couples states in the graphene, to form mini-bands . In un-doped nanoribbons, the mini bands are symmetrically positioned relative to the Fermi energy and do not enhance thermoelectric performance significantly. In contrast, when the ribbons are doped by electron donating or electron accepting adsorbates, the thermopower S and electronic figure of merit are enhanced and either positive or negative thermopowers can be obtained. In the most favourable case, doping with the electron donor tetrathiafulvalene (TTF) increases the room-temperature thermopower to -284 μv/K and doping by the electron acceptor tetracyanoethylene (TCNE) increases S to 210 μv/K. After including both electron and phonon contributions to the thermal conductance, figures of merit ZT up to of order 0.9 are obtained.

cond-mat.mes-hall↗

arXiv2015

Effects of asymmetric contacts on single molecule conductances of HS(CH2)nCOOH in nano-electrical junctions

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 as being highly sensitive to the type of the anchoring group is also strongly influenced by contact-asymmetry of the single molecular junction which in this case decreases the transmission. This highlights that contact asymmetry is a significant factor to be considered when evaluating nano-electrical junctions incorporating single molecules.

cond-mat.mes-hall↗

arXiv2015

Electrical Properties of Sculpturenes

We investigate the electronic properties of sculpturenes, formed by sculpting selected shapes from bilayer graphene, boron-nitride or graphene-boron-nitride hetero-bilayers and allowing the shapes to spontaneously reconstruct. The simplest sculpturenes are periodic nanotubes, containing lines of non-hexagonal rings. More complex sculpturenes formed from shapes with non-trivial topologies, connectivities and materials combinations may also be constructed. Results are presented for the reconstructed geometries, electronic densities of states and current-voltage relations of these new structures.

cond-mat.mes-hall↗

arXiv2015

GOLLUM: a next-generation simulation tool for electron, thermal and spin transport

We have developed an efficient simulation tool 'GOLLUM' for the computation of electrical, spin and thermal transport characteristics of complex nanostructures. The new multi-scale, multi-terminal tool addresses a number of new challenges and functionalities that have emerged in nanoscale-scale transport over the past few years. To illustrate the flexibility and functionality of GOLLUM, we present a range of demonstrator calculations encompassing charge, spin and thermal transport, corrections to density functional theory such as LDA+U and spectral adjustments, transport in the presence of non-collinear magnetism, the quantum-Hall effect, Kondo and Coulomb blockade effects, finite-voltage transport, multi-terminal transport, quantum pumps, superconducting nanostructures, environmental effects and pulling curves and conductance histograms for mechanically-controlled-break-junction experiments.

cond-mat.mes-hall↗

arXiv2011

Room temperature ballistic transport in InSb quantum well nanodevices

We report the room temperature observation of significant ballistic electron transport in shallow etched four-terminal mesoscopic devices fabricated on an InSb/AlInSb quantum well (QW) heterostructure with a crucial partitioned growth-buffer scheme. Ballistic electron transport is evidenced by a negative bend resistance signature which is quite clearly observed at 295 K and at current densities in excess of 10$^{6}$ A/cm$^{2}$. This demonstrates unequivocally that by using effective growth and processing strategies, room temperature ballistic effects can be exploited in InSb/AlInSb QWs at practical device dimensions.

cond-mat.mes-hall↗

arXiv2011

Quantum Interference in Single Molecule Electronic Systems

We present a general analytical formula and an ab initio study of quantum interference in multi-branch molecules. Ab initio calculations are used to investigate quantum interference in a benzene-1,2-dithiolate (BDT) molecule sandwiched between gold electrodes and through oligoynes of various lengths. We show that when a point charge is located in the plane of a BDT molecule and its position varied, the electrical conductance exhibits a clear interference effect, whereas when the charge approaches a BDT molecule along a line normal to the plane of the molecule and passing through the centre of the phenyl ring, interference effects are negligible. In the case of olygoynes, quantum interference leads to the appearance of a critical energy $E_c$, at which the electron transmission coefficient $T(E)$ of chains with even or odd numbers of atoms is independent of length. To illustrate the underlying physics, we derive a general analytical formula for electron transport through multi-branch structures and demonstrate the versatility of the formula by comparing it with the above ab-initio simulations. We also employ the analytical formula to investigate the current inside the molecule and demonstrate that large counter currents can occur within a ring-like molecule such as BDT, when the point charge is located in the plane of the molecule. The formula can be used to describe quantum interference and Fano resonances in structures with branches containing arbitrary elastic scattering regions connected to nodal sites.

cond-mat.mes-hall↗

arXiv2010

Ballistic transport and boundary scattering in InSb/InxAl1-xSb mesoscopic devices

We describe the influence of hard wall confinement and lateral dimension on the low temperature transport properties of long diffusive channels and ballistic crosses fabricated in an InSb/InxAl1-xSb heterostructure. Partially diffuse boundary scattering is found to play a crucial role in the electron dynamics of ballistic crosses and substantially enhance the negative bend resistance. Experimental observations are supported by simulations using a classical billiard ball model for which good agreement is found when diffuse boundary scattering is included.

cond-mat.mes-hall↗

arXiv2010

Chiral currents in gold nanotubes

Results are presented for the electron current in gold chiral nanotubes (AuNTs). Starting from the band structure of (4,3) and (5,3) AuNTs, we find that the magnitude of the chiral currents are greater than those found in carbon nanotubes. We also calculate the associated magnetic flux inside the tubes and find this to be higher than the case of carbon nanotubes. Although (4,3) and (5,3) AuNTs carry transverse momenta of similar magnitudes, the low-bias magnetic flux carried by the former is far greater than that carried by the latter. This arises because the low-bias longitudinal current carried by a (4,3) AuNT is significantly smaller than that of a (5,3) AuNT.

cond-mat.mes-hall↗

arXiv2009

Carbon nanotube quantum pumps

Recently nanomechanical devices composed of a long stationary inner carbon nanotube and a shorter, slowly-rotating outer tube have been fabricated. In this Letter, we study the possibility of using such devices as adiabatic quantum pumps. Using the Brouwer formula, we employ a Green's function technique to determine the pumped charge from one end of the inner tube to the other, driven by the rotation of a chiral outer nanotube. We show that there is virtually no pumping if the chiral angle of the two nanotubes is the same, but for optimal chiralities the pumped charge can be a significant fraction of a theoretical upper bound.

cond-mat.mes-hall↗

arXiv2008

Giant thermopower and figure of merit in single-molecule devices

We present a study of the thermopower $S$ and the dimensionless figure of merit $ZT$ in molecules sandwiched between gold electrodes. We show that for molecules with side groups, the shape of the transmission coefficient can be dramatically modified by Fano resonances near the Fermi energy, which can be tuned to produce huge increases in $S$ and $ZT$. This shows that molecules exhibiting Fano resonances have a high efficiency of thermoelectric cooling which is not present for conventional un-gated molecules with only delocalized states along their backbone.

cond-mat.mtrl-sci↗

arXiv2008

Tailoring the Fermi level of the leads in molecular-electronic devices

The dependence of the transport properties on the specific location of the Fermi level in molecular electronics devices is studied by using electrodes of different materials. The zero-bias transport properties are shown to depend dramatically on the elemental composition of the electrodes, even though the shape of the transmission coefficients is very similar. By using alkaline materials it is possible to move the Fermi level from the HOMO-LUMO gap to the LUMO resonance and change dramatically the length dependence of the conductance of molecular wires, which opens the possibility of using molecules with different lengths and very similar conductances in nanoscale circuits. This method shows how to dramatically increase the conductance of molecular devices and alter qualitatively and quantitatively their electronic and transport properties.

cond-mat.mes-hall↗

arXiv2008

Andreev reflection through Fano resonances in molecular wires

We study Andreev reflection in a normal conductor-molecule-superconductor junction using a first principles approach. In particular, we focus on a family of molecules consisting of a molecular backbone and a weakly coupled side group. We show that the presence of the side group can lead to a Fano resonance in the Andreev reflection. We use a simple theoretical model to explain the results of the numerical calculations and to make predictions about the possible sub-gap resonance structures in the Andreev reflection coefficient.

cond-mat.mes-hall↗