Electron Transport Calculations Research Articles

Two-Dimensional Gallium Oxide Monolayer for Gas-Sensing Application.

A two-dimensional (2D) Ga2O3 monolayer with an asymmetric quintuple-layer configuration was reported as a novel 2D material with excellent stability and strain tunability. This unusual asymmetrical structure opens up new possibilities for improving the selectivity and sensitivity of gas sensors by using selected surface orientations. In this study, the surface adsorptions of nine molecular gases, namely, O2, CO2, CO, SO2, NO2, H2S, NO, NH3, and H2O, on the 2D Ga2O3 monolayer are systematically investigated through first-principles calculations. The intrinsic dipole of the system leads to different adsorption energies and changes in the electronic structures between the top- and bottom-surface adsorptions. Analyses of electronic structures and charge transport calculations indicate a potential application of the 2D Ga2O3 monolayer as a room-temperature NO gas-sensing device with high sensitivity and tunable adsorption energy using plenary strain-induced lattice distortion.

Studying the lifetime of charge and heat carriers due to intrinsic scattering mechanisms in FeVSb half-Heusler thermoelectric

This work, presents a study of lifetime of carriers due to intrinsic scattering mechanisms viz. electron–electron interaction (EEI), electron–phonon interaction (EPI) and phonon–phonon interaction (PPI) in a promising half-Heusler thermoelectric FeVSb. Using the full-GW method, the effect of EEI and temperature on the valence and conduction band extrema and band gap are studied. The lifetime of carriers with temperature are estimated at these band extrema. At 300 K, estimated value of lifetime at VBM (CBM) is ∼1.91 × 10−14 s (∼2.05 × 10−14 s). The estimated ground state band gap considering EEI is ∼378 meV. Next, the effect of EPI on the lifetime of electrons and phonons with temperature are discussed. The comparison of two electron lifetimes suggests that EEI should be considered in transport calculations along with EPI. The average acoustic, optical and overall phonon lifetimes due to EPI are studied with temperature. Further, the effect of PPI is studied by computing average phonon lifetime for acoustic and optical phonon branches. The lifetime of the acoustic phonons are higher compared to optical phonons which indicates acoustic phonons contribute more to lattice thermal conductivity (κ ph). The comparison of phonon lifetime due to EPI and PPI suggests that, above 500 K EPI is the dominant phonon scattering mechanism and cannot be ignored in κ ph calculations. Lastly, a prediction of the power factor and figure of merit of n-type and p-type FeVSb is made by considering the temperature dependent carrier lifetime for the electronic transport terms. This study shows the importance of considering EEI in electronic transport calculations and EPI in phonon transport calculations in FeVSb. Our study is expected to provide results to further explore the thermoelectric transport in this material.

Ferromagnetism in a Semiconductor with Mobile Carriers via Low-Level Nonmagnetic Doping

We show that doped cubic iron pyrite, which is a diamagnetic semiconductor, becomes ferromagnetic when $p$-type doped. We furthermore find that this material can exhibit high spin polarization both for tunneling and transport devices. These results are based on first principles electronic structure and transport calculations. This illustrates the use of $p$-type doping without magnetic impurities as a strategy for obtaining ferromagnetic semiconducting behavior, with implications for spintronic applications that require both magnetic ordering and good mobility. This is a combination that has been difficult to achieve by doping semiconductors with magnetic impurities. We show that phosphorus and arsenic may be effective dopants for achieving this behavior.

An Inorganic–Organic Hybrid Polymer Cocatalyst for Photoelectrochemical Water Oxidation with Dual Functions of Accelerating Kinetics and Improving Charge Transfer

Oxygen evolution cocatalysts (OECs) play important roles in improving the efficiency of photocatalysts in solar water splitting. Inorganic–organic hybrid polymers (IOHPs), which have good electroly...

An improved set of electron-THFA cross sections refined through a neural network-based analysis of swarm data.

We review experimental and theoretical cross sections for electron transport in α-tetrahydrofurfuryl alcohol (THFA) and, in doing so, propose a plausible complete set. To assess the accuracy and self-consistency of our proposed set, we use the pulsed-Townsend technique to measure drift velocities, longitudinal diffusion coefficients, and effective Townsend first ionization coefficients for electron swarms in admixtures of THFA in argon, across a range of density-reduced electric fields from 1 to 450 Td. These measurements are then compared to simulated values derived from our proposed set using a multi-term solution of Boltzmann's equation. We observe discrepancies between the simulation and experiment, which we attempt to address by employing a neural network model that is trained to solve the inverse swarm problem of unfolding the cross sections underpinning our experimental swarm measurements. What results from our neural network-based analysis is a refined set of electron-THFA cross sections, which we confirm is of higher consistency with our swarm measurements than that which we initially proposed. We also use our database to calculate electron transport coefficients in pure THFA across a range of reduced electric fields from 0.001 to 10 000 Td.

Individual Identification of Amino Acids on an Atomically Thin Hydrogen Boride System Using Electronic Transport Calculations

Recently synthesized two-dimensional hydrogen boride (HB) with a hexagonal boron network offers excellent opportunities for nanoscale electronic device applications. Herein, we have proposed a type...

The scaling laws of edge vs. bulk interlayer conduction in mesoscale twisted graphitic interfaces

The unusual electronic properties of edges in graphene-based systems originate from the pseudospinorial character of their electronic wavefunctions associated with their non-trivial topological structure. This is manifested by the appearance of pronounced zero-energy electronic states localized at the material zigzag edges that are expected to have a significant contribution to the interlayer transport in such systems. In this work, we utilize a unique experimental setup and electronic transport calculations to quantitatively distinguish between edge and bulk transport, showing that their relative contribution strongly depends on the angular stacking configuration and interlayer potential. Furthermore, we find that, despite of the strong localization of edge state around the circumference of the contact, edge transport in incommensurate interfaces can dominate up to contact diameters of the order of 2 μm, even in the presence of edge disorder. The intricate interplay between edge and bulk transport contributions revealed in the present study may have profound consequences on practical applications of nanoscale twisted graphene-based electronics.

Organ Dose Calculations Using ICRP Adult Voxel Phantoms and TRIPOLI-4 Monte Carlo Code

Abstract The ICRP 110 adult male and female voxel phantoms are the official computational models representing the ICRP (International Commission on Radiological Protection) Reference Male and Reference Female. In 2018, the Working Group 6 (WG6) of European Radiation Dosimetry Group (EURADOS) organized a study on the usage of the ICRP voxel reference phantoms. Organ dose calculation tasks with radiation transport codes were proposed in occupational, environmental, and medical dosimetry. The TRIPOLI-4 Monte Carlo radiation transport code has been widely used in radiation shielding, criticality safety, and reactor physics fields for supporting French nuclear energy research and industrial applications. To enhance the application fields of TRIPOLI-4, the 2018 EURADOS-WG6 tasks are being taken into account by using different features of the TRIPOLI-4 code. In this work, the ICRP reference voxel phantoms were first adapted into TRIPOLI-4. More than 14 × 106 voxels were represented in a mixed lattice geometry including 140 organs-tissues and 52 tissue media. Diverse exposure scenarios were then investigated by using 60Co and 241Am gamma-ray sources, 16N beta source, and 10 keV neutron source. The TRIPOLI-4 standard nuclear data library was utilized on these neutron, photon, electron, and positron-coupled transport calculations. Energy deposition estimators for electron, positron, neutron, and photon coupled with mesh tally options were used to calculate the organ absorbed dose DT and the effective dose E. TRIPOLI-4 calculation methods and primary results for the EURADOS-WG6 voxel phantom exercise on organ dose study tasks are reported here.

Generation of empirical pseudopotentials for transport applications and their application to group IV materials

Empirical pseudopotentials (EPs) allow for accurate and efficient modeling of atomistic electron transport. Unfortunately, EPs are available only for a few materials and atomic configurations. Furthermore, EPs for nanostructures have historically been described using a variety of different parameterized forms. To compete with more general first-principles methods, we propose an automated workflow to generate EPs of a general form for any material and atomistic configuration. In particular, we focus on the generation of EPs for electron transport calculations, i.e., we provide an EP that accurately reproduces a reference band structure. To demonstrate the applicability of the proposed method, we generate the EPs to reproduce the band structure for bulk Si, Ge, 3C–SiC (zinc-blende polytype), 4H–SiC (hexagonal polytype), diamond, and hydrogen terminated ⟨100⟩ oriented Si and Ge thin films, calculated using first principles. In addition, using the generated EPs, along with the virtual crystal approximation, we demonstrate that our method reproduces accurately the band structure related properties of Si1−xGex alloy as a function of Ge mole fraction, x. As an application of our generated EPs, we perform ballistic quantum transport simulations of extremely scaled (≈0.6 nm wide), hydrogen terminated, ⟨100⟩ oriented Ge and Si gate-all-around nanowire field-effect transistors and compare their transfer characteristics.

Multi-Space Excitation as an Alternative to the Landauer Picture for Nonequilibrium Quantum Transport.

While the Landauer viewpoint constitutes a modern basis to understand nanoscale electronic transport and to realize first‐principles implementations of the nonequilibrium Green's function (NEGF) formalism, seeking an alternative picture can be beneficial for the fundamental understanding and practical calculations of quantum transport processes. Herein, introducing a micro‐canonical picture that maps the finite‐bias quantum transport process to a drain‐to‐source or multi‐electrode optical excitation, the multi‐space constrained‐search density functional theory (MS‐DFT) formalism for first‐principles electronic structure and quantum transport calculations is developed. Performing MS‐DFT calculations for the benzenedithiolate single‐molecule junction, it is shown that MS‐DFT and standard DFT‐NEGF calculations produce practically equivalent electronic and transmission data. Importantly, the variational convergence of “nonequilibrium total energy” within MS‐DFT is demonstrated, which should have significant implications for in operando studies of nanoscale devices. Establishing a viable alternative to the Landauer viewpoint, the developed formalism should provide valuable atomistic information in the development of next‐generation nanodevices.

Complexion dictated thermal resistance with interface density in reactive metal multilayers

Multilayers composed of aluminum (Al) and platinum (Pt) exhibit a nonmonotonic trend in thermal resistance with bilayer thickness as measured by time domain thermoreflectance. The thermal resistance initially increases with reduced bilayer thickness only to reach a maximum and then decrease with further shrinking of the multilayer period. These observations are attributed to the evolving impact of an intermixed amorphous complexion approximately 10 nm in thickness, which forms at each boundary between Al- and Pt-rich layers. Scanning transmission electron microscopy combined with energy dispersive x-ray spectroscopy find that the elemental composition of the complexion varies based on bilayer periodicity as does the fraction of the multilayer composed of this interlayer. These variations in complexion mitigate boundary scattering within the multilayers as shown by electronic transport calculations employing density-functional theory and nonequilibrium Green's functions on amorphous structures obtained via finite temperature molecular dynamics. The lessening of boundary scattering reduces the total resistance to thermal transport leading to the observed nonmonotonic trend thereby highlighting the central role of complexion on thermal transport within reactive metal multilayers.

Material Descriptors for the Discovery of Efficient Thermoelectrics

The predictive performance screening of novel compounds can significantly promote the discovery of efficient, cheap, and non-toxic thermoelectric materials. Large efforts to implement machine-learning techniques coupled to materials databases are currently being undertaken, but the adopted computational methods can dramatically affect the outcome. With regards to electronic transport and power factor calculations, the most widely adopted and computationally efficient method, is the constant relaxation time approximation (CRT). This work goes beyond the CRT and adopts the proper, full energy and momentum dependencies of electron-phonon and ionized impurity scattering, to compute the electronic transport and perform power factor optimization for a group of half-Heusler alloys. Then the material parameters that determine the optimal power factor based on this more advanced treatment are identified. This enables the development of a set of significantly improved descriptors that can be used in materials screening studies, and which offer deeper insights into the underlying nature of high performance thermoelectric materials. We have identified $n_v$$\epsilon_r$ / $D_o^2m_{cond}$ as the most useful and generic descriptor, a combination of the number of valleys, the dielectric constant, the conductivity effective mass, and the deformation potential for the dominant electron-phonon process. The proposed descriptors can accelerate the discovery of new efficient and environment friendly thermoelectric materials in a much more accurate and reliable manner, and some predictions for very high performance materials are presented.

SAKE: first-principles electron transport calculation code

We developed and implemented a numerical code called SAKE, which stands for (simulation code for atomistic Kohn–Sham equation). We developed it for first-principle electron transport calculations based on density-functional theory and non-equilibrium Green’s function formalism. First, we present the central calculation parts of the formalism of the electronic states and transport properties for open and non-equilibrium systems. We show specific computational techniques, such as the use of a complex contour integration for charge density from the density matrix, which is compared with the calculation method of summing the residues of the Fermi-Dirac distribution, as well as the efficient achievement of the self-consistent procedures. Thereafter, for applications of the present computation code, SAKE, we present first-principle calculation results of three different systems. We first analyze electronic structures of polythiophene molecular wires, compare summation techniques for the density matrix. We show thermoelectric properties of an n-type antiferromagnetic semiconductor CuFeS2 as a second application. The electrical conductance, electrical thermal conductance, and the Seebeck coefficients with carrier doping are examined, and the analytical form of the Seebeck coefficient is briefly described. For the third application, we analyze the electron transport properties of polyaniline molecular wires under structural deformations, i.e. rotations around the transport direction. The thermally averaged current-voltage characteristics are also analyzed. The results show that the current decreases as the temperature increases which are determined based on the competition between the thermal energy and the electronic energy, which increases with the rotation angle.

(Invited) First Principles Electron Transport Calculations: From Molecular Contacts to Large 2D Devices

The combination of Density Functional Theory (DFT) with non-equilibrium Greens functions (NEGF) allows for first principles calculations of electronic devices under working conditions, i.e. under the non-equilibrium conditions in the presence of finite electronic current[1]. I will show examples of how the DFT-NEGF method is used to gain insights into the non-equilibrium conduction and current-induced atomic forces in molecular contacts[2]. I will describe how we apply DFT-NEGF including electrostatic gating to study devices based on 2D materials[3,4]. Finally, I will present a recently developed multi-scale approach, combining spatial regions described by DFT with larger regions described by DFT-derived tight-binding. We have employed the multi-scale approach to study transport in molecular-based 2D graphene nanomesh structures going towards the (100 nm)-by-(100 nm) scale[5].

Directional bonding explains the high conductance of atomic contacts in bcc metals

Atomic-sized junctions of iron, created by controlled rupture, present unusually high values of conductance compared to other metals. This result is counter-intuitive since, at the nanoscale, body-centered cubic metals are expected to exhibit lower coordination than face-centered cubic metals. In this work, classical molecular dynamics simulations of contact rupture, using an interatomic potential that accounts for directional bonding, yield highly-coordinated stable structures before rupture, unlike an isotropic bonding potential, which results in the expected stable single-atom contacts. Density functional theory electronic transport calculations show that conductance values of these highly coordinated and highly stable structures, can explain the experimentally measured values for conductance of body-centered cubic atomic contacts, thus revealing the important role of directional bonding in these metals.

Gate-Tunable Reversible Rashba-Edelstein Effect in a Few-Layer Graphene/2H-TaS2 Heterostructure at Room Temperature.

We report the observation of current-induced spin polarization, the Rashba-Edelstein effect (REE), and its Onsager reciprocal phenomenon, the spin galvanic effect (SGE), in a few-layer graphene/2H-TaS2 heterostructure at room temperature. Spin-sensitive electrical measurements unveil full spin-polarization reversal by an applied gate voltage. The observed gate-tunable charge-to-spin conversion is explained by the ideal work function mismatch between 2H-TaS2 and graphene, which allows for a strong interface-induced Bychkov-Rashba interaction with a spin-gap reaching 70 meV, while keeping the Dirac nature of the spectrum intact across electron and hole sectors. The reversible electrical generation and control of the nonequilibrium spin polarization vector, not previously observed in a nonmagnetic material, are elegant manifestations of emergent two-dimensional Dirac Fermions with robust spin-helical structure. Our experimental findings, supported by first-principles relativistic electronic structure and transport calculations, demonstrate a route to design low-power spin-logic circuits from layered materials.

First-principles electronic structure, phonon properties, lattice thermal conductivity and prediction of figure of merit of FeVSb half-Heusler

In this work, we have studied the electronic structure of a promising thermoelectric half-Heusler FeVSb using FP-LAPW method and SCAN meta-GGA including spin–orbit coupling. Using the obtained electronic structure and transport calculations we try to address the experimental Seebeck coefficient S of FeVSb samples. The good agreement between the experimental and calculated S suggests the band gap could be ∼0.7 eV. This is supported by the obtained mBJ band gap of ∼0.7 eV. Further, we study and report the phonon dispersion, density of states and thermodynamic properties. The effect of long range Coulomb interactions on phonon frequencies are also included by nonanalytical term correction. Under quasi-harmonic approximation, the thermal expansion behaviour up to 1200 K is calculated. Using the first-principles anharmonic phonon calculations, the lattice thermal conductivity κ ph of FeVSb is obtained under single-mode relaxation time approximation considering the phonon-phonon interaction. At 300 K, the calculated κ ph is ∼18.6 W m−1 K−1 which is higher compared to experimental value. But, above 500 K the calculated κ ph is in good agreement with experiment. A prediction of figure of merit ZT and efficiency for p-type and n-type FeVSb is made by finding out optimal carrier concentration. At 1200 K, a maximum ZT of ∼0.66 and ∼0.44 is expected for p-type and n-type FeVSb, respectively. For p-type and n-type materials, maximum efficiency of ∼12.2% and ∼6.0% are estimated for hot and cold temperature of 1200 K and 300 K, respectively. A possibility of achieving n-type and p-type FeVSb by elemental doping/vacancy is also discussed. Our study is expected to help in further exploring the thermoelectric material FeVSb.

Generalized quadrature for finite temperature Green’s function methods

In electronic structure and quantum transport calculations, many physical quantities are integrations over the electron energy, weighted by the Fermi–Dirac distribution function. Green’s function based approaches commonly circumvent the numerically difficult real energy integration by extending the integrand analytically into the complex energy plane, and using a Gaussian quadrature integration over a complex energy contour for zero temperature. For finite temperatures, a much slower convergent sum over the Matsubara frequencies is necessary. We present a generalized quadrature method that uses orthogonal polynomials on the manifold of Matsubara frequencies to enable rapid convergence. Both Gaussian quadrature integration and Matsubara frequency summation methods are shown to be limiting cases of the generalized method. Tests on an all-electron ab initio code and total energy calculation of interacting Anderson impurity model show convergence with a small number of energy mesh points.

Giant Conductance Enhancement of Intramolecular Circuits through Interchannel Gating

Summary For neutral intramolecular circuits with two constitutionally identical branches, a maximum 4-fold increase in total conductance can be obtained according to constructive quantum interference (CQI). For charged intramolecular circuits, however, the strong electrostatic interactions entangle the quantum states of these two parallel pathways, thus introducing complicated transport behavior that warrants experimental investigation of the intramolecular circuit rules. Here, we report that a tetracationic cyclophane with parallel channels exhibits a 50-fold conductance enhancement compared with that of a single-channel control, an observation that supplements intramolecular circuit law in systems with strong Coulombic interactions. Flicker noise measurements and theoretical calculations show that strong electrostatic interactions between charged parallel channels—serving as the chemical gate to promote the effective conductance of each channel—and CQI boosts the total conductance of the two-channel circuit. The molecular design presented herein constitutes a proof-of-principle approach to charged intramolecular circuits that are desirable for quantum circuits and devices.

An empirical law on the finite-size effects in electronic transport calculations of tungsten

When the size of a supercell employed in theoretical calculations is smaller obviously than the mean free path of electrons in metals, the computed values of the electrical conductivity and the electronic thermal conductivity show a striking finite-size effect, and such a size-dependent value cannot be used for direct comparison with that from experiments. We hereby propose an empirical law to unified describe the relation between the conductivity (including the electrical conductivity and the electronic thermal conductivity) of infinite-size crystal and that of finite-size supercell in calculations for tungsten (W). Our calculations demonstrate that it is very convenient to achieve the electrical conductivity and the electronic thermal conductivity of W metal by using this empirical law. In addition, we provide a simple power law (∼T−1.35) to describe the finite-size effects at different temperatures. Furthermore, the mean free path of electrons, which tightly correlates to the finite-size effects exhibited in the electronic transport calculations of W at different temperatures, are revealed. The proposed empirical law in this work is robust and may be valid for other metals.