Electron Transport Calculations Research Articles

Ab initiononequilibrium quantum transport and forces with the real-space projector augmented wave method

We present an efficient implemention of a non-equilibrium Green function (NEGF) method for self-consistent calculations of electron transport and forces in nanostructured materials. The electronic structure is described at the level of density functional theory (DFT) using the projector augmented wave method (PAW) to describe the ionic cores and an atomic orbital basis set for the valence electrons. External bias and gate voltages are treated in a self-consistent manner and the Poisson equation with appropriate boundary conditions is solved in real space. Contour integration of the Green function and parallelization over k-points and real space makes the code highly efficient and applicable to systems containing several hundreds of atoms. The method is applied to a number of different systems demonstrating the effects of bias and gate voltages, multiterminal setups, non-equilibrium forces, and spin transport.

Atomic-scale model for the contact resistance of the nickel-graphene interface

We perform first-principles calculations of electron transport across a nickel-graphene interface. Four different geometries are considered, where the contact area, graphene and nickel surface orientations, and the passivation of the terminating graphene edge are varied. We find covalent bond formation between the graphene layer and the nickel surface, in agreement with other theoretical studies. We calculate the energy-dependent electron transmission for the four systems and find that the systems have very similar edge contact resistance, independent of the contact area between nickel and graphene, and in excellent agreement with recent experimental data. A simple model where graphene is bonded with a metal surface shows that the results are generic for covalently bonded graphene, and the minimum attainable edge contact resistance is twice the ideal edge quantum contact resistance of graphene.

Conductance quantization in graphene nanoconstrictions with mesoscopically smooth but atomically stepped boundaries

We present the results of million atom electronic quantum transport calculations for graphene nanoconstrictions with edges that are smooth apart from atomic scale steps. We find conductances quantized in integer multiples of 2e2/h and a plateau at ~0.5*2e2/h as in recent experiments [Tombros et al., Nature Physics 7, 697 (2011)]. We demonstrate that, surprisingly, conductances quantized in integer multiples of 2e2/h occur even for strongly non-adiabatic electron backscattering at the stepped edges that lowers the conductance by one or more conductance quanta below the adiabatic value. We also show that conductance plateaus near 0.5*2e2/h can occur as a result of electron backscattering at stepped edges even in the absence of electron-electron interactions.

Accuracy of the electron transport inmcnp5and its suitability for ionization chamber response simulations: A comparison with theegsnrcandpenelopecodes

In this work, accuracy of the mcnp5 code in the electron transport calculations and its suitability for ionization chamber (IC) response simulations in photon beams are studied in comparison to egsnrc and penelope codes. The electron transport is studied by comparing the depth dose distributions in a water phantom subdivided into thin layers using incident energies (0.05, 0.1, 1, and 10 MeV) for the broad parallel electron beams. The IC response simulations are studied in water phantom in three dosimetric gas materials (air, argon, and methane based tissue equivalent gas) for photon beams ((60)Co source, 6 MV linear medical accelerator, and mono-energetic 2 MeV photon source). Two optional electron transport models of mcnp5 are evaluated: the ITS-based electron energy indexing (mcnp5(ITS)) and the new detailed electron energy-loss straggling logic (mcnp5(new)). The electron substep length (ESTEP parameter) dependency in mcnp5 is investigated as well. For the electron beam studies, large discrepancies (>3%) are observed between the MCNP5 dose distributions and the reference codes at 1 MeV and lower energies. The discrepancy is especially notable for 0.1 and 0.05 MeV electron beams. The boundary crossing artifacts, which are well known for the mcnp5(ITS), are observed for the mcnp5(new) only at 0.1 and 0.05 MeV beam energies. If the excessive boundary crossing is eliminated by using single scoring cells, the mcnp5(ITS) provides dose distributions that agree better with the reference codes than mcnp5(new). The mcnp5 dose estimates for the gas cavity agree within 1% with the reference codes, if the mcnp5(ITS) is applied or electron substep length is set adequately for the gas in the cavity using the mcnp5(new). The mcnp5(new) results are found highly dependent on the chosen electron substep length and might lead up to 15% underestimation of the absorbed dose. Since the mcnp5 electron transport calculations are not accurate at all energies and in every medium by general clinical standards, caution is needed, if mcnp5 is used with the current electron transport models for dosimetric applications.

A Computationally Efficient Treatment of Polarizable Electrochemical Cells Held at a Constant Potential

A computationally efficient method is presented for the treatment of electrostatic interactions between polarizable metallic electrodes held at a constant potential and separated by an electrolyte. The method combines a fluctuating uniform electrode charge with explicit image charges to account for the polarization of the electrode by the electrolyte, and a constant uniform charge added to the fluctuating uniform electrode charge to account for the constant potential condition. The method is then used to calculate electron transport rates using Marcus theory and these rates are incorporated in a Kinetic Monte Carlo - Molecular Dynamics simulation scheme to efficiently model oxidation/reduction reactions in an electrochemical cell.

First-principles study of (InAs)1/(GaSb)1 superlattice atomic chains

The atomic structure, the mechanical properties, the electronic band structure, and the phonon structure of (InAs)1/(GaSb)1 superlattice atomic chain are investigated by first-principles pseudopotential plane wave method, and the quantum transport properties are also calculated by the density functional theory numerical atomic orbit pseudopotential method in combination with nonequilibrium Green's function formalism. Compared with two-dimensional layer structural (InAs)1/(GaSb)1 superlattice, the (InAs)1/(GaSb)1 superlattice atomic chains have obviously different band structures, and represent metal energy band characteristics in certain conditions. The calculated mechanical strength of (InAs)1/(GaSb)1 superlattice atomic chains indicates that such structures can sustain the strain as high as =0.19. The structural stability of (InAs)1/(GaSb)1 superlattice atomic chains is investigated by full Brillouin zone analysis for phonon structure. The electron transport calculations for (InAs)1/(GaSb)1 superlattice atomic chain segments in between Al electrodes show that the conductance exhibits nontrivial features as the chain length or strain is varied. The calculated optical absorption spectra represent precipitous cutoff absorptions in infrared regime, and the cutoff wavelength varies with chain structure. InAs/GaSb superlattice atomic chains are predicted to be applied to infrared optoelectronic nanodevices, modifying optoelectronic response wavelength range by changing the structures of superlattice atomic chains.

Conduction modulation of π-stacked ethylbenzene wires on Si(100) with substituent groups

For the realization of molecular electronics, one essential goal is the ability to systematically fabricate molecular functional components in a well-controlled manner. Experimental techniques have been developed such that π-stacked ethylbenzene molecules can now be routinely induced to self-assemble on an H-terminated Si(100) surface at precise locations and along precise directions. Electron transport calculations predict that such molecular wires could indeed carry an electrical current, but the Si substrate may play a considerable role as a competing pathway for conducting electrons. In this work, we investigate the effect of placing substituent groups of varying electron donating or withdrawing strengths on the ethylbenzene molecules to determine how they would affect the transport properties of such molecular wires. The systems consist of a line of π-stacked ethylbenzene molecules covalently bonded to a Si substrate. The ethylbenzene line is bridging two Al electrodes to model current through the molecular stack. For our transport calculations, we employ a first-principles technique where density functional theory (DFT) is used within the non-equilibrium Green’s function formalism (NEGF). The calculated density of states suggest that substituent groups are an effective way to shift molecular states relative to the electronic states associated with the Si substrate. The electron transmission spectra obtained from the NEGF–DFT calculations reveal that the transport properties could also be extensively modulated by changing substituent groups. For certain molecules, it is possible to have a transmission peak at the Fermi level of the electrodes, corresponding to high conduction through the molecular wire with essentially no leakage into the Si substrate.

Bipolar magnetic semiconductors: a new class of spintronics materials

Electrical control of spin polarization is very desirable in spintronics, since electric fields can be easily applied locally, in contrast to magnetic fields. Here, we propose a new concept of bipolar magnetic semiconductors (BMS) in which completely spin-polarized currents with reversible spin polarization can be created and controlled simply by applying a gate voltage. This is a result of the unique electronic structure of BMS, where the valence and conduction bands possess opposite spin polarization when approaching the Fermi level. BMS is thus expected to have potential for various applications. Our band structure and spin-polarized electronic transport calculations on semi-hydrogenated single-walled carbon nanotubes confirm the existence of BMS materials and demonstrate the electrical control of spin-polarization in them.

Redox-switchable devices based on functionalized graphene nanoribbons

The possibility of tuning the electronic properties of graphene by tailoring the morphology at the nanoscale or by chemical functionalization opens interesting perspectives towards the realization of devices for nanoelectronics. Indeed, the integration of the intrinsic high carrier mobilities of graphene with functionalities that are able to react to external stimuli allows in principle the realization of highly efficient nanostructured switches. In this paper, we report a novel approach to the design of reversible switches based on functionalized graphene nanoribbons, operating upon application of an external redox potential, which exhibit unprecedented ON/OFF ratios. The properties of the proposed systems are investigated by electronic structure and transport calculations based on density functional theory and rationalized in terms of valence-bond theory and Clar's sextet theory.

Electron transport simulation in resonant-tunneling GaN/AlGaN heterostructures

A numerical method for electron transport calculations in resonant-tunneling GaN/AlGaN heterostructures has been developed on the basis of a self-consistent solution of the Schrodinger and Poisson equations. Dependences of the system’s transmission coefficient on the external field and of the peak current on the ratio between the well and barrier widths have been studied for a double-barrier resonant-tunneling diode. For technical applications, the optimal values of the structure’s parameters have been found.

Molecular dynamics study of the thermopower of Ag, Au, and Pt nanocontacts

Using molecular dynamics simulations of many junction stretching processes combined with tight-binding-based electronic structure and transport calculations, we analyze the thermopower of silver (Ag), gold (Au), and platinum (Pt) atomic contacts. In all cases we observe that the thermopower vanishes on average within the standard deviation and that its fluctuations increase for a decreasing minimum cross section of the junctions. However, we find a suppression of the fluctuations of the thermopower for the $s$-valent metals Ag and Au, when the conductance originates from a single, perfectly transmitting channel. Essential features of the experimental results for Au, Ag, and copper (Cu) of Ludoph and van Ruitenbeek [Phys. Rev. B 59, 12290 (1999)], as yet unaddressed by atomistic studies, can hence be explained by considering the atomic and electronic structure at the disordered narrowest constriction of the contacts. For the multivalent metal Pt our calculations predict the fluctuations of the thermopower to be larger by one order of magnitude as compared to Ag and Au, and suppressions of the fluctuations as a function of the conductance are absent. Main features of our results are explained in terms of an extended single-level model.

Stability analysis of multiple nonequilibrium fixed points in self-consistent electron transport calculations

We present a method to perform stability analysis of nonequilibrium fixed points appearing in self-consistent electron transport calculations. The nonequilibrium fixed points are given by the self-consistent solution of stationary, nonlinear kinetic equation for single-particle density matrix. We obtain the stability matrix by linearizing the kinetic equation around the fixed points and analyze the real part of its spectrum to assess the asymptotic time behavior of the fixed points. We derive expressions for the stability matrices within Hartree-Fock and linear response adiabatic time-dependent density functional theory. The stability analysis of multiple fixed points is performed within the nonequilibrium Hartree-Fock approximation for the electron transport through a molecule with a spin-degenerate single level with local Coulomb interaction.

Graphene nanogap for gate-tunable quantum-coherent single-molecule electronics

We present atomistic calculations of quantum coherent electron transport through fulleropyrrolidine terminated molecules bridging a graphene nanogap. We predict that three difficult problems in molecular electronics with single molecules can be solved by utilizing graphene contacts: (1) a back gate modulating the Fermi level in the graphene leads facilitates control of the device conductance in a transistor effect with high on-off current ratio; (2) the size mismatch between leads and molecule is avoided, in contrast to the traditional metal contacts; (3) as a consequence, distinct features in charge flow patterns throughout the device are directly detectable by scanning techniques. We show that moderate graphene edge disorder is unimportant for the transistor function.

Electronic Enhancement Effect of Copper Modification of Base Pairs on the Conductivity of DNA

The effect of the new designed multicopper modification of base pairs on the conductivity of DNA was investigated by the nonequilibrium Green’s function method combined with density functional theory. Electronic transport calculations revealed that the equi-number H-by-Cu replacement can significantly enhance the conductivity of DNA from two aspects: transverse base-to-base communication along the hydrogen-bond direction and longitudinal transport along the DNA duplex. Furthermore, the enhancement effect on the longitudinal direction is more notable than that on the transverse. A tunneling mechanism is suggested for the short DNA segments. The decay factor of conductance in Cu-DNA decreases by half compared with the native DNA, thus making it more promising for constructing nanowires. In addition, Cu-DNA may prefer electron migration to hole transport with the lengthening of DNA segments. This work will shed some light on the design of promising DNA-based molecular wires.

Controlling the transmission line shape of molecular t-stubs and potential thermoelectric applications

Asymmetric line shapes can occur in the transmission function describing electron transport in the vicinity of a minimum caused by quantum interference effects. Such asymmetry can be used to increase the thermoelectric efficiency of molecular junctions. So far, however, asymmetric line shapes have been only empirically found for just a few rather complex organic molecules where the origins of the line shapes relation to molecular structure were not resolved. In the present, work we introduce a method to analyze the structure dependence of the asymmetry of interference dips from simple two site tight-binding models, where one site corresponds to a molecular π orbital of the wire and the other to an atomic p(z) orbital of a side group, which allows us to characterize analytically the peak shape in terms of just two parameters. We assess our scheme with first-principles electron transport calculations for a variety of t-stub molecules and also address their suitability for thermoelectric applications.

Ni(111)|graphene|h-BN junctions as ideal spin injectors

Deposition of graphene on top of hexagonal boron nitride (h-BN) was very recently demonstrated while graphene is now routinely grown on Ni. Because the in-plane lattice constants of graphite, h-BN, graphite-like BC2N and of the close-packed surfaces of Co, Ni and Cu match almost perfectly, it should be possible to prepare ideal interfaces between these materials which are respectively, a semimetal, insulator, semiconductor, ferromagnetic and nonmagnetic metals. Using parameter-free energy minimization and electronic transport calculations, we show how h-BN can be combined with the perfect spin filtering property of Ni|graphite and Co|graphite interfaces to make perfect tunnel junctions or ideal spin injectors (SI) with any desired resistance-area product.

Electronic promotion effect of double proton transfer on conduction of DNA through improvement of transverse electronic communication of base pairs

The effect of double proton transfer (DPT) on charge migration of DNA was investigated by the nonequilibrium Green's function method combined with density functional theory. The results revealed that DPT not only lowers ionization potentials, but also improves the delocalization of the localized π-orbitals at each base moiety through adjusting energy levels and spatial distributions of their molecular orbitals. Furthermore, DPT leads to both the strengthening of the second-order interactions of the Watson-Crick H-bond zones, and the promotion of the charge transfer transitions between two pairing bases in the UV absorption spectra. Electronic transport calculations indicated that DPT can improve the charge migration along the DNA duplex for specific sequences through enhancing transverse base-to-base electronic communication. This work will provide a new insight into the understanding of DNA charge conduction which can be electronically promoted or regulated by DPT.

Algorithm for efficient elastic transport calculations for arbitrary device geometries

With the growth in interest in graphene, controlled nanoscale device geometries with complex form factors are now being studied and characterized. There is a growing need to understand new techniques to handle efficient electronic transport calculations for these systems. We present an algorithm that dramatically reduces the computational time required to find the local density of states and transmission matrix for open systems regardless of their topology or boundary conditions. We argue that the algorithm, which generalizes the recursive Green's function method by incorporating the reverse Cuthill-McKee algorithm for connected graphs, is ideal for calculating transmission through devices with multiple leads of unknown orientation and becomes a computational necessity when the input and output leads overlap in real space. This last scenario takes the Landauer-Buttiker formalism to general scattering theory in a computational framework that makes it tractable to perform full-spectrum calculations of the quantum scattering matrix in mesoscopic systems. We demonstrate the efficacy of these approaches on graphene stadiums, a system of recent scientific interest, and contribute to a physical understanding of Fano resonances which appear in these systems.

Stabilized scattering wave-function calculations using the Lippmann-Schwinger equation for long conductor systems

We present an improvement of the Lippmann-Schwinger equation method, which calculates electron-scattering wave functions of a nanoscale conductor suspended between a pair of electrodes. The improvement eliminates the numerical collapse which frequently occurs while solving the Lippmann-Schwinger equation for long conductor systems and originates from evanescent wave components of the retarded Green's function of the Lippmann-Schwinger equation. We introduce regularization and ratio expression into the Green's function matrix and discover that the resultant Green's function does not suffer from the numerical collapse without increasing computational cost. As a performance test, we carry out electron transport calculations of Al monoatomic linear chains with a length of up to 75.6 bohrs. The numerical test demonstrates that the improved Lippmann-Schwinger equation method is applicable to long conductor systems with no numerical collapse and adequate computational accuracy.

First-principles calculation of electronic transport in low-dimensional disordered superconductors

We present a novel formulation to calculate transport through disordered superconductors connected between two metallic leads. An exact analytical expression for the current is derived and applied to a superconducting sample described by the negative-$U$ Hubbard model. A Monte Carlo algorithm that includes thermal phase and amplitude fluctuations of the superconducting order parameter is employed, and a new efficient algorithm is described. This improved routine allows access to relatively large systems, which we demonstrate by applying it to several cases, including superconductor-normal interfaces and Josephson junctions. Moreover, we can link the phenomenological parameters describing these effects to the underlying microscopic variables. The effects of decoherence and dephasing are shown to be included in the formulation, which allows the unambiguous characterization of the Kosterlitz-Thouless transition in two-dimensional systems and the calculation of the finite resistance due to vortex excitations in quasi-one-dimensional systems. Effects of magnetic fields can be easily included in the formalism, and are demonstrated for the Little-Parks effect in superconducting cylinders. Furthermore, the formalism enables us to map the local super and normal currents, and the accompanying electrical potentials, which we use to pinpoint and visualize the emergence of resistance across the superconductor-insulator transition.