Nonequilibrium Green Function Research Articles

Giant tunneling resistance and robust switching behavior in ferroelectric tunnel junctions of WS2/Ga2O3 heterostructures: The influence of metal–semiconductor contacts

The ferroelectric tunneling junctions (FTJs) are widely recognized as one of the non-volatile memories with significant potential. Ferroelectricity usually fades away as materials are thinned down below a critical value, and this problem is particularly acute in the case of shrinking device sizes, thus attracting attention to two-dimensional ferroelectric materials (2DFEMs). In this work, we designed 2D ferroelectric Ga2O3-based FTJs with out-of-plane polarization, and the influence of metal–semiconductor contact in the electrode region on the system is considered. Here, using density functional theory combined with the non-equilibrium Green's function approach to quantum transport calculations, we demonstrate robust ferroelectric polarization-controlled switching behavior between metallic and semiconducting states in Ga2O3/WS2 ferroelectric heterostructures. The potential barrier of the metal–semiconductor contact in the electrode region is lower than that of the intrinsic material, thereby resulting in an increased probability of electron tunneling. Our results reveal the crucial role of 2DFEMs in the construction of FTJs and highlight the significant impact of electrode contact types on performance. This provides a promising approach for developing high-density ferroelectric memories based on 2D ferroelectric semiconductor heterostructures.

Edge state regulation and interfacial design on spin transport properties of VC2-based nanoscale devices

Edge state and interfacial design are efficient strategies to regulate the spin-transport properties of nanoscale devices. Spin-polarized transport properties of VC2 nanoribbon device and poly-(terphenylene-butadiynylene) PTB molecular junctions are studied by using density functional theory (DFT) and non-equilibrium Green function. Results show good self-selected filtering properties for spin-up current are highly suppressed, where there is only spin-down current that can propagate through the scattering region of such a nanoribbon device. What needs to be pointed out is that spin-down current exhibits an obvious negative differential resistance effect. Current and transmission spectrum peaks are significantly weakened, and the negative differential resistance effect disappears after a PTB molecule is embedded between two semi-infinite VC2 nanoribbon electrodes. This work provides a basis for improving the design and method of spintronic devices.

A systematic study of switching, optoelectronics, and gas‐sensitive properties of PCF‐graphene‐based nanodevices: Insights from DFT study

AbstractTwo‐dimensional materials exhibit significant potential and wide‐ranging application prospects owing to their remarkable tunability, pronounced quantum confinement effects, and notable surface sensitivity. The switching, optoelectronics, and gas‐sensitive properties of the new carbon material poly‐cyclooctatetraene framework (PCF)‐graphene were systematically studied using density functional theory combined with the nonequilibrium Green's function method. First, the diode device based on PCF‐graphene monolayer exhibited an impressive switching ratio of 106, demonstrating excellent diode characteristics. Moreover, in the investigation of the pin junction utilizing monolayer PCF‐graphene, it is noteworthy that significant photocurrent responses were observed in both the zigzag and armchair directions, specifically within the visible and ultraviolet regions. Finally, gas sensors employing monolayer and bilayer PCF‐graphene demonstrate significant chemical adsorption capabilities for NO and NO2. Notably, the maximum gas sensitivity for NO is achieved in monolayer PCF‐graphene, reaching 322% at a bias voltage of 1.0 V. Meanwhile, for bilayer PCF‐graphene‐based gas sensor, the maximum gas sensitivity reaches 52% at a bias voltage of 0.4 V. In addition, the study also examined the influence of various environmental conditions, specifically H2O, O, and OH, on the system under investigation. The obtained results emphasize the multifunctional properties of PCF‐graphene, exhibiting significant potential for various applications, including switching devices, optoelectronic devices, and gas sensors.

GPU-Enabled Exascale Quantum Transport Modeling of Carbon Nanotube Devices

The work will describe our efforts to develop an exascale electrostatic-quantum transport framework, Quantum-eXstatic (https://github.com/AMReX-Microelectronics/eXstatic), currently supporting the modeling of carbon nanotube field-effect transistors (CNTFETs). The framework is capable of modeling realistic three-dimensional structures, efficiently, using CPU/GPU heterogeneous architectures of state-of-the-art supercomputers. It is built on top of the AMReX library, which is a GPU-enabled software library containing functionality for writing particle-mesh applications on structured grids. The Quantum-eXstatic framework comprises three major components: the electrostatic module, the quantum transport module, and the part that self-consistently couples the two modules. The electrostatic module using a finite-volume multigrid solver to compute the electrostatic potential induced by charges on the surface of carbon nanotubes, as well as by source, drain, and gate terminals, which can be modeled using an embedded boundary approach to allow for intricate shapes. The quantum transport module uses the Nonequilibrium Green's Function (NEGF) method to model induced charge. Currently, it supports coherent (ballistic) transport, mode-space approximation for subbands of nanotube, contacts modeled as semi-infinite leads, and Hamiltonian representation using the tight-binding approximation. Special features are being included for accurate modeling of long nanotubes, such as adaptive refinement of integration contours to resolve van Hove singularities in long channels. Particular attention is paid to overlap computations with communication to optimize GPU performance. The self-consistency between the two modules is achieved using Broyden's modified second algorithm, which is parallelized using CPUs and GPUs. Preliminary scaling studies show that the code exhibits ~77% weak-scaling efficiency on 512 NVIDIA A100 GPUs of Perlmutter supercomputer for modeling gate-all-around CNTFETs with a channel length of 13.5 microns at equilibrium conditions. This case involved computations of electrostatic potential in 14.5 billion computational cells and Green’s function computation for a Hamiltonian of size 131,072 x 131,072. For problems of this large size, the code takes about 5 min to reach self-consistency. Figure 1

A Mechanism of Resistance Switching in CNT Based Memory Devices

Carbon nanotubes (CNTs) show promise for high energy efficiency electronic devices due to their high electrical conductivity. One possible application is in the fabrication of resistance-change computer memory, where the application of an external electrical bias can use a CNT layer as the switching element in a RAM cell. Memory cells of this type have been extensively demonstrated, where the electrical resistance of a switching layer of CNTs can be reversibly controlled by the application of external bias [1].To better understand these devices, we have developed a nanoscale model of their electrical switching. Towards this end, first-principles calculations of the electrical conductivity of CNT-CNT junctions were performed using the Density Functional Tight Binding (DFTB) in combination with the Non-Equilibrium Greens functions (NEGF) approach, enabling an improved understanding of the tunnelling of electrons across a range of CNT junctions [2]. These results demonstrate that the conductivity of CNT contacts depends on the overlap area between nanotubes and exponentially on the distances between the carbon atoms of the interacting CNTs. Secondly, we employed coarse-grained molecular dynamics [3,4] to produce nanoscale dense CNT film models like those used in the devices. We devise a set of metrics for characterising the structural properties of CNT films, and apply them to a set of model films designed to mimic those used in microelectronics devices. In order to understand how the geometrical properties of CNTs affect the film structure, we analyse films with different CNT chirality and length distributions. Unlike previous studies that focused on relatively low-density systems below ∼0.4 g/cm3, we also consider films with density of ∼0.6 g/cm3, as employed in experimentally fabricated CNT-based NRAM devices. By adding amorphous carbon to the film models, in varying amounts, we are then able to assess its effects. Finally, these two elements were combined to produce electrical simulations of the conductivity of the CNT films connected to TiN electrodes. These electrodes are shown to be partially oxidized during the device fabrication. The electrical conductivity in a device is characterized by formation of conduction paths formed by CNTs between the electrodes and connected via the CNT junctions. The conductivity is modulated by charging of CNTs and amorphous carbon present in the film.Using these simulations, we propose a resistance switching mechanism in TiN/CNT/TiN devices based on the physical movement of CNTs. During the initial operation of the device, oxygen is released from the oxidized bottom electrode and this readily reacts with individual CNTs to form charge trapping sites. Once these sites have become charged, they enable controllable movement of CNTs at the bottom electrode under the application of electric field. By reversibly connecting and disconnecting such CNTs from the bottom electrode, the electrical conductivity through the CNT film as a whole can be controlled.

Enhanced thermoelectric properties in hybrid graphane/graphene nanoribbons

The thermoelectric properties of hybrid graphane and graphene nanoribbons (GGNRs) are studied by the Landauer formula within the atomistic non-equilibrium Green's function. It is shown that hybrid GGNRs present the tunable band gap depending upon the width ratio of their components. Modulation of hybrid GGNRs can give rise to the lower thermal conductance of phonons and the better thermoelectric properties compared to pure graphene nanoribbons and graphane nanoribbons. Introducing the hydrogen defects can enhance the maximum of ZT (ZTmax) in both armchair GGNRs (AGGNRs) and zigzag GGNRs (ZGGNRs). Such the enhancement of ZTmax sensitively depends upon the defect concentrations. Among different defect concentrations, ZTmax for the 20 % defect concentration has the highest value, which can be enhanced to 0.42 and 0.24 at T = 300 K in AGGNRs and ZGGNRs, respectively. A laconic analysis of these results is given.

Kadanoff-Baym Equations for Interacting Systems with Dissipative Lindbladian Dynamics.

The extraordinary quantum properties of nonequilibrium systems governed by dissipative dynamics have become a focal point in contemporary scientific inquiry. The nonequilibrium Green's functions (NEGF) theory provides a versatile method for addressing driven nondissipative systems, utilizing the powerful diagrammatic technique to incorporate correlation effects. We here present a second-quantization approach to the dissipative NEGF theory, reformulating Keldysh ideas to accommodate Lindbladian dynamics and extending the Kadanoff-Baym equations accordingly. Generalizing diagrammatic perturbation theory for many-body Lindblad operators, the formalism enables correlated and dissipative real-time simulations for the exploration of transient and steady-state changes in the electronic, transport, and optical properties of materials.

Electron Transport through Linear-, Broken-, and Cross-Conjugated Polycyclic Compounds.

Quantum interference (QI) effects offer unique opportunities to modulate charge transport through single molecules. In recent years, several transmission selection rules have been developed to determine constructive and destructive QIs in an intuitive and simple manner, although some of these rules fail for cross-conjugated systems. In this work, we evaluate the performance of distinct transmission rules on a broad series of anthracene and fluorene derivatives with distinctive structural features including linear-, broken-, and cross-conjugation, heteroatoms, and five-membered rings as such species affords a predictive challenge for the qualitative selection rules for QI effects. The electron transport properties and local transmission plots are first evaluated by combining DFT and the nonequilibrium Green function method allowing for an equal-footing comparison of the conductance of the different polycyclic compounds. Our findings are in line with experimental observations on the influence of the type of conjugation and the connectivity to the metallic electrodes on the transport properties. Thus, cross-conjugated systems exhibit reduced conductance values as compared to the linear-conjugated ones, although the transmission is enhanced in the meta-connected junctions. Remarkably, our study reveals that aromatic cores exhibit generally larger zero-bias conductance for a given connectivity, in contrast to the negative aromaticity-conductance relationship found in literature.

First-Principles Insights into Highly Sensitive and Reusable MoS2 Monolayers for Heavy Metal Detection.

This study explores the potential of MoS2 monolayers as heavy metal sensors for As, Cd, Hg, and Pb using density functional theory (DFT) and Non-Equilibrium Green's Function (NEGF) simulations. Our findings reveal that As and Pb adsorption significantly alters the surface structure and electronic properties of MoS2, introducing impurity levels and reducing the band gap. Conversely, Cd and Hg exhibit weaker interactions with the MoS2 surface. The MoS2 monolayer sensors demonstrate exceptional sensitivity for all four target heavy metals, with values reaching 126,452.28% for As, 1862.67% for Cd, 427.71% for Hg, and 83,438.90% for Pb. Additionally, the sensors demonstrate selectivity for As and Pb through distinct response peaks at specific bias voltages. As and Pb adsorption also induces magnetism in the MoS2 system, potentially enabling magnetic sensing applications. The MoS2 monolayer's moderate adsorption energy facilitates rapid sensor recovery at room temperature for As, Hg, and Cd. Notably, Pb recovery time can be significantly reduced at elevated temperatures, highlighting the reusability of the sensor. These results underscore the potential of MoS2 monolayers as highly sensitive, selective, and regenerable sensors for real-time heavy metal detection.

Spin-filtering properties of topological structures based on stanene and bismuthene nanoribbons with one edge magnetism

The transport properties of spin filters based on two-dimensional magnetic topological insulators (TI) with magnetism at one edge are theoretically studied. The non-equilibrium-Green’s-function (NEGF) formalism based on density functional theory (DFT) derived Hamiltonian is used to study the one-way helical edge states in these structures. We investigated the electronic and magnetic properties of stanene and bismuthene nanoribbons with various metal edge modifications. Our DFT simulations predict the formation of one-way helical edge states in stanene nanoribbons with asymmetric edge passivation. Our results suggest that the spin filtering properties of such structures outperform a comparable spin filter based on spin-polarized quantum-anomalous-Hall effect, as it bypasses a need for a strict interplay of magnetism, topology, and a large electric field (around 2 V gate voltage difference).

Exploring the effects of molecular beam epitaxy growth characteristics on the temperature performance of state-of-the-art terahertz quantum cascade lasers

This study conducts a comparative analysis, using non-equilibrium Green’s functions (NEGF), of two state-of-the-art two-well (TW) Terahertz Quantum Cascade Lasers (THz QCLs) supporting clean 3-level systems. The devices have nearly identical parameters and the NEGF calculations with an abrupt-interface roughness height of 0.12 nm predict a maximum operating temperature (Tmax) of ~ 250 K for both devices. However, experimentally, one device reaches a Tmax of ~ 250 K and the other a Tmax of only ~ 134 K. Both devices were fabricated and measured under identical conditions in the same laboratory, with high quality processes as verified by reference devices. The main difference between the two devices is that they were grown in different MBE reactors. Our NEGF-based analysis considered all parameters related to MBE growth, including the maximum estimated variation in aluminum content, growth rate, doping density, background doping, and abrupt-interface roughness height. From our NEGF calculations it is evident that the sole parameter to which a drastic drop in Tmax could be attributed is the abrupt-interface roughness height. We can also learn from the simulations that both devices exhibit high-quality interfaces, with one having an abrupt-interface roughness height of approximately an atomic layer and the other approximately a monolayer. However, these small differences in interface sharpness are the cause of the large performance discrepancy. This underscores the sensitivity of device performance to interface roughness and emphasizes its strategic role in achieving higher operating temperatures for THz QCLs. We suggest Atom Probe Tomography (APT) as a path to analyze and measure the (graded)-interfaces roughness (IFR) parameters for THz QCLs, and subsequently as a design tool for higher performance THz QCLs, as was done for mid-IR QCLs. Our study not only addresses challenges faced by other groups in reproducing the record Tmax of ~ 250 K and ~ 261 K but also proposes a systematic pathway for further improving the temperature performance of THz QCLs beyond the state-of-the-art.

Density Functional Theory Provides Insights into β-SnSe Monolayers as a Highly Sensitive and Recoverable Ozone Sensing Material.

This study explores the potential of β-SnSe monolayers as a promising material for ozone (O3) sensing using density functional theory (DFT) combined with the non-equilibrium Green's function (NEGF) method. The adsorption characteristics of O3 molecules on the β-SnSe monolayer surface were thoroughly investigated, including adsorption energy, band structure, density of states (DOSs), differential charge density, and Bader charge analysis. Post-adsorption, hybridization energy levels were introduced into the system, leading to a reduced band gap and increased electrical conductivity. A robust charge exchange between O3 and the β-SnSe monolayer was observed, indicative of chemisorption. Recovery time calculations also revealed that the β-SnSe monolayer could be reused after O3 adsorption. The sensitivity of the β-SnSe monolayer to O3 was quantitatively evaluated through current-voltage characteristic simulations, revealing an extraordinary sensitivity of 1817.57% at a bias voltage of 1.2 V. This sensitivity surpasses that of other two-dimensional materials such as graphene oxide. This comprehensive investigation demonstrates the exceptional potential of β-SnSe monolayers as a highly sensitive, recoverable, and environmentally friendly O3 sensing material.

Design and characterization of colloidal quantum dot photoconductors for multi-color mid-infrared detection

This report paves the way for low cost, multi-color, room-temperature, and easily-feasible mid-IR photodetector with distinct output currents. The proposed device is designed and simulated to be fabricated by the solution-process technology thanks to its simplicity and fabrication ease, room-temperature operation capability, low production cost, and excellent photoelectric properties. In this approach, the proposed structure is composed of an array of n × n pixels, where each pixel is designed to enable multi-wavelength detection. The absorber layer consists of different sized quantum dots that absorb distinct wavelengths simultaneously through interband transitions in the mid-infrared region. Selective energy contacts based on quantum well structures are designed to be deposited on interdigitated contacts as a means of extracting the stimulated carriers from the absorber layers to the metal contacts. Through resonant tunneling, the excited carriers are transferred, which generates the output photocurrent and significantly reduces the dark current. In order to model the designed multi-color photoconductor, coupled rate equations and three-dimensional Schrodinger-Poisson equations have been developed and solved self-consistently. As a way of demonstrating the validity of the introduced model, a experimentally fabricated photoconductor and a theoretically modeled photodetector using the nonequilibrium Green’s function (NEGF) model have been simulated; the comparison between the simulation results is quite satisfactory. In order to simplify the theoretical model, two different sizes of InSb/ZnSe core/shell quantum dots have been considered in the theoretical model to detect two MIR wavelengths (3 µm and 4 µm) of the incident light. Simulation results indicate that the peak responsivities are about 3.3(A/W) and 6(A/W), and the high specific detectivities D* are about 9 × 1010(cm.Hz1/2W−1) and 15 × 1010(cm.Hz1/2W−1) for the wavelengths of 4 µm and 3 µm, respectively.

High tunneling magneto-resistance ratio in Co2FeAl Heusler alloy and WSe2 2D material tunnel barrier-based magnetic tunnel junctions

This paper presents a Magnetic Tunnel Junction (MTJ) based on Co2FeAl Heusler alloy and 2D material WSe2 with an enhanced tunnelling magneto-resistance (TMR). Our study is inspired by recent investigations of 2D materials and Heusler alloys. By employing static Density Functional Theory (DFT) simulations coupled with Non-Equilibrium Green’s Function (NEGF) transport models, we evaluate conductance properties in Co2FeAl/WSe2/Co2FeAl MTJ. The half metallicity of Co2FeAl and quantum confinement properties of WSe2 are compatible, which enhances the TMR of MTJ.

Nonequilibrium Green's function approach to low-energy fission dynamics: Fluctuations in fission reactions

Nonequilibrium Green's function approach to low-energy fission dynamics: Fluctuations in fission reactions

Half-Metallic Transport and Spin-Polarized Tunneling through the van der Waals Ferromagnet Fe4GeTe2.

We examine the coherent spin-dependent transport properties of the van der Waals (vdW) ferromagnet Fe4GeTe2 using density functional theory combined with the nonequilibrium Green's function method. Our findings reveal that the conductance perpendicular to the layers is half-metallic, meaning that it is almost entirely spin-polarized. This property persists from the bulk to a single layer, even under significant bias voltages and with spin-orbit coupling. Additionally, using dynamical mean field theory for quantum transport, we demonstrate that electron correlations are important for magnetic properties but minimally impact the conductance, preserving almost perfect spin-polarization. Motivated by these results, we then study the tunnel magnetoresistance (TMR) in a magnetic tunnel junction consisting of two Fe4GeTe2 layers with the vdW gap acting as an insulating barrier. We predict a TMR ratio of ∼500%, which can be further enhanced by increasing the number of Fe4GeTe2 layers in the junction.

Enabling Ab Initio Molecular Dynamics under Bias: The CP2K+SMEAGOL Interface for Integrating Density Functional Theory and Non-Equilibrium Green Functions.

Density functional theory (DFT) combined with non-equilibrium Green's functions (NEGF) is a powerful approach to model quantum transport under external bias potentials at reasonable computational cost. In this work, we present a new interface between the popular mixed Gaussian/plane waves electronic structure package, CP2K, and the NEGF, code SMEAGOL, the most feature-rich implementation of DFT-NEGF available for CP2K to date. The CP2K+SMEAGOL interface includes the implementation of current induced forces. We verify this implementation for a variety of systems: an infinite 1D Au wire, a parallel-plate capacitor, and a Au-H2-Au junction. We find good agreement with SMEAGOL calculations performed with SIESTA for the same systems and with the example of a solvated Au wire demonstrating for the first time that DFT-NEGF can be used to perform molecular dynamics simulations under bias of large-scale condensed phase systems under realistic operating conditions.

Observing the Role of Electron Delocalization in Electronic Transport by Incorporating Actinides into Ligated Metal-Chalcogenide Superatoms.

Since delocalization of electronic states is a prerequisite for exerting unique electron transport properties, early actinides (An) with highly delocalized 5f/6d orbitals are natural candidates. However, given the experimental difficulties of such radioactive compounds and the complex relativistic effects in theoretical studies, understanding the electronic structure and bonding of actinides is underdeveloped on the periodic table. A further challenge is the very complicated electronic structures encountered in the confinement of actinides, as vividly illustrated by the weakly radioactive Th(Thorium)-encapsulated metal chalcogenide clusters, Th@Co6Te8L6 (L = PH3, PMe3, PEt3). Here we report the electronic structure and the electron transport properties of the Th@Co6Te8L6 clusters and compare them with those of the hollow Co6Te8L6 clusters using the nonequilibrium Green's function combined with relativistic density functional theory (NEGF-DFT). We found that the equilibrium conductance in Th@Co6Te8(PH3)6 (0.76 G0) has been greatly improved over that in Co6Te8(PH3)6 (0.03 G0), which has also been verified under an applied different bias voltage. The covalent bonding character between 6d (Th) and 3d (Co) atomic orbitals resulting from steric confinement is the source of the performance enhancement and a most important factor governing the accessibility of such 5f/6d orbitals. The results are of significance to the rapidly developing field of molecular nanoelectronics.

Thermoelectric Phenomena in a Magnetic Heterostructure with AAH Modulation: Charge and Spin Figure of Merits

ABSTRACT We put forward a prescription of getting a higher value of the spin-dependent figure of merit in comparison with its charge counterpart in the case of a 1D magnetic heterostructure (a ferromagnetic (FM) chain sandwiched between two non-magnetic 1D lattices) where all the site energies of the heterostructure follow cosine form of modulation defined in Aubry-Andre-Harper (AAH) model. It is shown that due to having a greater number of non-uniform peaks in its transmission spectra, the thermoelectric efficiency of this heterostructure becomes superior compared to that is obtained in a fully ferromagnetic 1D chain. It is also reported that the maximum value of the thermoelectric figure of merit (for both spin and charge-dependent cases) of the heterostructure in a specified energy range gets enhanced in a continuous manner as the disorder strength of the AAH modulation is increased. The Hamiltonian of the proposed quantum system is described within a tight-binding (TB) framework and after the evaluation of transmission probability by utilizing the non-equilibrium Green’s function (NEGF) technique, all the important thermoelectric quantities are determined on the basis of Landauer formalism. We believe that our study on this particular topic of spin caloritronics, a subject associated with temperature-dependent spin transmission through a quantum channel, may help to explore several fascinating ideas about spin-related thermoelectric efficiency in many other ferromagnetic quasicrystals.

Thermoelectric Properties Regulated by Quantum Size Effects in Quasi-One-Dimensional γ-Graphdiyne Nanoribbons.

Using density functional theory combined with the first principles calculation method of non-equilibrium Green's function (NEGF-DFT), we studied the thermoelectric (TE) characteristics of one-dimensional γ-graphdiyne nanoribbons (γ-GDYNRs). The study found that the thermal conductivity of γ-GDYNRs has obvious anisotropy. At the same temperature and geometrical size, the lattice thermal conductivity of zigzag-edged γ-graphdiyne nanoribbons (γ-ZGDYNRs) is much lower than that of armchair-edged γ-graphdiyne nanoribbons (γ-AGDYNRs). We disclose the underlying mechanism for this intrinsic orientation. That is, γ-AGDYNRs have more phonon dispersion over the entire frequency range. Furthermore, the orientation dependence increases when the width of the γ-GDYNRs decreases. These excellent TE properties allow armchair-edged γ-graphdiyne nanoribbons with a planar width of 1.639 nm (γ-Z(2)GDYNRs) to have a higher power factor and lower thermal conductivity, ultimately resulting in a significantly higher TE conversion rate than other γ-GDYNR structures.