Resonant Transport Research Articles

Resonant transport in a double-barrier heterostructure AlxGa1−xAs/GaAs and mass discontinuity: a semiclassical path integral approach

In this paper, we investigate the dependence of the resonant carrier transport in an AlGaAs/GaAs double-barrier heterostructure on the electron’s effective mass discontinuity between the well and the barrier layer. We use a one-dimensional model for the effective potential and consider the activation of the resonant tunneling mechanism when a bias is applied between the emitter and the collector. We calculate the system’s Green’s function through semiclassical path integration to obtain the complex spectrum. Electron’s effective mass discontinuity affects our calculations through the contributions of the various propagations inside the heterostructure and the multiple reflections from the turning points. Our findings show that the lowest resonance energy decreases linearly with increasing bias, while the real energy shift of the resonance decreases in a non-linear manner with the mass discontinuity. We also observe that the resonant transport time increases nearly linearly with the mass discontinuity. These results demonstrate the impact of the carrier’s inertia enhancement on the resonance characteristics and are consistent with established concepts in quantum mechanics and previously published works. Furthermore, we identify a critical bias value that distinguishes the behavior of the symmetric and asymmetric heterostructure. Additionally, the derivative of the transport time with respect to mass discontinuity is found to be independent of the applied bias. Our results provide concise analytical relationships involving parameters such as barrier and well thickness and shape, enabling the prediction and optimization of various nanoscale devices’ performance.

Boosting thermoelectric performance of molecular junction by utilizing edge branches and weak coupling

In this study, we investigated the thermoelectric properties of molecular junctions, created by trapping naphthacene (C18H12) and rubrene (C42H28) molecules between two graphene electrodes. It is found that the charge transport of naphthacene-based and rubrene-based graphene junctions is not sensitive to the introduction of edge side branches or the increase in molecular length and still maintains resonance transport at the Fermi level. Notably, the presence of pendant branches on the molecular trunk in rubrene-based graphene junctions leads to a suppression of phonon transport, attributed to multiple scattering at the branch attachment points or Fano resonance scattering. The phonon thermal conductance of the rubrene junctions can be reduced by nearly half compared to that of naphthalene junctions. Furthermore, the room-temperature figure of merit (ZT) is significantly enhanced from 0.2 to 1.1 upon constructing weak coupling junctions, representing an almost tenfold increase over covalent junctions. These findings mean that it is highly desirable to find a mechanism that can suppress the phonon thermal conductance of self-assembled molecular films, while preserving their power factor at optimal levels to obtain high-efficiency thermoelectric performance.

Anisotropic Spin Fluctuations Induced by Spin-Orbit Coupling in a Misfit Layer Compound (LaSe)1.14(NbSe2).

Spin-orbit coupling (SOC) has significant effects on the superconductivity and magnetism of transition metal dichalcogenides (TMDs) at the 2D limit. Although 2D TMD samples possess many exotic properties different from those of bulk samples, experimental characterization in this field is still limited, especially for magnetism. Recent studies have revealed that bulk misfit layer compounds (MLCs) with (LaSe)1.14(NbSe2)n = 1,2 exhibit an Ising superconductivity similar to that of heavily electron-doped NbSe2 monolayers. This offers an opportunity to study the effect of SOC on the magnetism of 2D TMDs. Here, the possible SOC effect in (LaSe)1.14(NbSe2) is investigated by measuring nuclear magnetic resonance (NMR) and electrical transport. It is found that the LaSe layer not only functions as a charge reservoir for transferring electrons into the NbSe2 layer but also remarkably influences the local electronic environment around the 93Nb nuclei. More importantly, the significant SOC induces both a weak antilocalization (WAL) effect and anisotropic spin fluctuations in noncentrosymmetric NbSe2 layers. The present work contributes to a deep understanding of the role of the SOC effect in 2D TMDs and supports MCLs as an intriguing platform for exploring exotic physical properties within the 2D limit.

Effects of internal and external decoherence on the resonant transport and Anderson localization of fermionic particles in disordered tight-binding chains

Effects of internal and external decoherence on the resonant transport and Anderson localization of fermionic particles in disordered tight-binding chains

Negative Differential Resistance in Single‐Molecule Junctions Based on Heteroepitaxial Spherical Au/Pt Nanogap Electrodes

AbstractSingle‐molecule junctions exploit the internal structure of molecular orbitals to construct a new class of functional quantum devices. The demonstration of negative differential resistance (NDR) in single‐molecule junctions is direct evidence of quantum mechanical tunneling through a molecular orbital. Here, a pronounced NDR effect is reported with a peak‐to‐valley ratio of 30.1 on a single‐molecule junction of π‐conjugated quinoidal‐fused oligosilole derivatives, Si2 × 2, embedded between the unique electroless gold‐plated heteroepitaxial spherical Au/Pt nanogap electrodes. This NDR feature persists in a consecutive endurance test of 180 current traces. the thermally stable NDR effects in the Si2 × 2 single‐molecule junctions between 9 and 300 K are demonstrated. The density functional theory calculations under electric fields indicate that the NDR effect can be ascribed to the bias‐dependent resonant tunneling transport via the polarized HOMO, which has asymmetrically changed electrode coupling with increased bias voltages. The results confirm a promising electrical platform for constructing functional quantum devices at the single‐molecule level.

Active control of Alfvén eigenmodes by external magnetic perturbations with different spatial spectra

Alfvén eigenmodes have been suppressed and excited in tokamak plasmas by (just) modifying the poloidal spectra of externally applied static magnetic perturbations. This effect is observed experimentally when toroidal spectra of n = 2, n = 4 as well as a mixed spectrum of n = 2 and n = 4 is applied. Under the n = 2 magnetic perturbations, the modes are excited or suppressed by modifying the coil phasing between the upper and the lower set of coils. Regardless of the absolute rotation, an even parity for the n = 4 perturbation is observed to reduce the amplitude of the Alfvénic instabilities, while an odd parity amplifies it. To combine the stabilizing (and destabilizing) effect of n = 2 and n = 4, a mixed spectrum is applied, finding similar reduction (and amplification) trends. However, the impact on the mode amplitude is more subtle, due to the reduced coil current required for a mixed spectrum. The signal level on the fast-ion loss detector is sensitive to the applied poloidal spectrum, which is consistent with Hamiltonian full-orbit modelling of an edge resonant transport layer activated by the 3D perturbative fields. An internal redistribution of the fast-ion population is induced, modifying the phase-space gradients driving the Alfvénic instabilities, and ultimately determining their existence. The calculated edge resonant layers for both n = 2 and n = 4 toroidal spectra are consistent with the observed suppressed and excited phases. Moreover, hybrid kinetic-magnetohydrodynamic (MHD) simulations reveal that this edge resonant transport layer overlaps in phase-space with the population responsible for the fast-ion drive. The results presented here may help to control fast-ion driven Alfvénic instabilities in future burning plasmas with a significant fusion born alpha particle population.

Precision Basecalling of Single DNA Nucleotide from Overlapped Transmission Readouts with Machine Learning Aided Solid-State Nanogap.

DNA sequencing with the quantum tunneling technique heralds a paradigm shift in genetic analysis, promising rapid and accurate identification for diverging applications ranging from personalized medicine to security issues. However, the widespread distribution of molecular conductance, conduction orbital alignment for resonant transport, and decoding crisscrossing conductance signals of isomorphic nucleotides have been persistent experimental hurdles for swift and precise identification. Herein, we have reported a machine learning (ML)-driven quantum tunneling study with solid-state model nanogap to determine nucleotides at single-base resolution. The optimized ML basecaller has demonstrated a high predictive basecalling accuracy of all four nucleotides from seven distinct data pools, each containing complex transmission readouts of their different dynamic conformations. ML classification of quaternary, ternary, and binary nucleotide combinations is also performed with high precision, sensitivity, and F1 score. ML explainability unravels the evidence of how extracted normalized features within overlapped nucleotide signals contribute to classification improvement. Moreover, electronic fingerprints, conductance sensitivity, and current readout analysis of nucleotides have promised practical applicability with significant sensitivity and distinguishability. Through this ML approach, our study pushes the boundaries of quantum sequencing by highlighting the effectiveness of single nucleotide basecalling with promising implications for advancing genomics and molecular diagnostics.

From Liouville to Landauer: Electron transport and the bath assumptions made along the way

A generalized quantum master equation approach is introduced to describe electron transfer in molecular junctions that spans both the off-resonant (tunneling) and resonant (hopping) transport regimes. The model builds on prior insights from scattering theory but is not limited to a certain parameter range with regard to the strength of the molecule–electrode coupling. The framework is used to study the simplest case of energy and charge transfer between the molecule and the electrodes for a single site noninteracting Anderson model in the limit of symmetric and asymmetric coupling between the molecule and the electrodes. In the limit of elastic transport, the Landauer result is recovered for the current by invoking a single active electron Ansatz and a binary collision approximation for the memory kernel. Inelastic transport is considered by allowing the excitation of electron–hole pairs in the electrodes in tandem with charge transport. In the case of low bias voltages where the Fermi levels of the electrodes remain below the molecular state, it is shown that the current arises from tunneling and the molecule remains neutral. However, once the threshold is reached for aligning the fermi level of one electrode with the molecular orbital, a small amount of charge transfer occurs with a negligible amount of hopping current. While inelasticity in the current has a minimal impact on the shape of the current–voltage curve in the case of symmetric electrode coupling, the results for a slight asymmetry in coupling demonstrate complete charge transfer and a significant drop in current. These results provide encouraging confirmation that the framework can describe charge transport across a wide range of electrode–molecule coupling and provide a unique perspective for developing new master equation treatments for energy and charge transport in molecular junctions. An extension of this work to account for inelastic scattering from electron–vibrational coupling at the molecule is straightforward and will be the subject of subsequent work.

Superfluid response of two-dimensional filamentary superconductors

Different classes of low-dimensional superconducting systems exhibit an inhomogeneous filamentary superconducting condensate whose macroscopic coherence still needs to be fully investigated and understood. Here, we present a thorough analysis of the superfluid response of a prototypical filamentary superconductor embedded in a two-dimensional metallic matrix. By mapping the system into an exactly solvable random impedance network, we show how the dissipative (reactive) response of the system non-trivially depends on both the macroscopic and microscopic characteristics of the metallic (superconducting) fraction. We compare our calculations with resonant microwave transport measurements performed on LaAlO_33/SrTiO_33 heterostructures over an extended range of temperatures and carrier densities finding that the filamentary character of superconductivity accounts for unusual peculiar features of the experimental data.

Resonant Charge Transport Assisted by the Molecular Vibration in Single-Molecule Junction from Time-Domain ab initio Nonadiabatic Molecular Dynamics Simulations

Using ab initio nonadiabatic molecular dynamics simulation, we study the time-dependent charge transport dynamics in a single-molecule junction formed by gold (Au) electrodes and a single benzene-1,4-dithiol (BDT) molecule. Two different types of charge transport channels are found in the simulation. One is the routine non-resonant charge transfer path, which occurs in several picoseconds. The other is activated when the electronic state of the electrodes and that of the molecule get close in energy, which is referred to as the resonant charge transport. More strikingly, the resonant charge transfer occurs in an ultrafast manner within 100 fs, which notably increases the conductance of the device. Further analysis shows that the resonant charge transport is directly assisted by the B 2 and A 1 molecular vibration modes. Our study provides atomic insights into the time-dependent charge transport dynamics in single-molecule junctions, which is important for designing highly efficient single-molecule devices.

Non-Markovian master equation for quantum transport of fermionic carriers.

We propose a simple, yet feasible, model for quantum transport of fermionic carriers across tight-binding chain connecting two reservoirs maintained at arbitrary temperatures and chemical potentials. The model allows for elementary derivation of the master equation for the reduced single particle density matrix in a closed form in both Markov and Born approximations. In the Markov approximation the master equation is solved analytically, whereas in the Born approximation the problem is reduced to an algebraic equation for the single particle density matrix in the Redfield form. The non-Markovian equation is shown to lead to resonant transport similar to Landauer's conductance. It is shown that in the deep non-Markovian regime the transport current can be matched with that obtained by the non-equilibrium Green's function method.

Phase slip from weak links formed in artificially-stacked NbSe2

The rich nature of van der Waals interactions between artificially-stacked atomic layers has been demonstrated by various quantum states and resonant tunneling transport in low-dimensional materials. However, the role of topological fluctuations in quantum transport through artificially-stacked junctions of 2D superconducting materials, and the resulting energy dissipation, remain elusive. In this research, unique phase-slip centers are designed in artificially-stacked junction areas, where nonequilibrium quasiparticles are formed and relaxed with energy dissipation. The phase slips are observed as voltage steps (peaks or valleys) in transport measurements across a junction between two exfoliated NbSe2 flakes, and at a distance of 4 μm from the junction using local and nonlocal chemical potential probes. Accordingly, two types of energy dissipation modes are newly identified in the artificially-stacked NbSe2 when subjected to an in-plane magnetic field, which implies distinct vortex formation and current flow in the superconducting junction under magnetic fields.

Charge-state lifetimes of single molecules on few monolayers of NaCl

In molecular tunnel junctions, where the molecule is decoupled from the electrodes by few-monolayers-thin insulating layers, resonant charge transport takes place by sequential charge transfer to and from the molecule which implies transient charging of the molecule. The corresponding charge state transitions, which involve tunneling through the insulating decoupling layers, are crucial for understanding electrically driven processes such as electroluminescence or photocurrent generation in such a geometry. Here, we use scanning tunneling microscopy to investigate the decharging of single ZnPc and H2Pc molecules through NaCl films of 3 to 5 monolayers thickness on Cu(111) and Au(111). To this end, we approach the tip to the molecule at resonant tunnel conditions up to a regime where charge transport is limited by tunneling through the NaCl film. The resulting saturation of the tunnel current is a direct measure of the lifetimes of the anionic and cationic states, i.e., the molecule’s charge-state lifetime, and thus provides a means to study charge dynamics and, thereby, exciton dynamics. Comparison of anion and cation lifetimes on different substrates reveals the critical role of the level alignment with the insulator’s conduction and valence band, and the metal-insulator interface state.

Stationary transport above the critical velocity in a one-dimensional superflow past an obstacle

We consider in this work the different possible stationary flows of a one-dimensional quantum fluid in the mean-field regime. We focus on the supersonic regime where a transition from a time-dependent flow to a stationary diffractive flow occurs at a given critical velocity. We give nonperturbative results for this critical velocity in the presence of a localised obstacle of arbitrary size and strength. In addition, we discuss the existence of superfluid-like solution in the supersonic regime due to resonant transport and provide a complete map of the different regimes of stationary transport of a quantum fluid.

Single-molecule photoelectron tunnelling spectroscopy.

Experimental mapping of transmission is essential for understanding and controlling charge transport through molecular devices and materials. Here we developed a single-molecule photoelectron tunnelling spectroscopy approach for mapping transmission beyond the HOMO-LUMO gap of the single diketopyrrolopyrrole molecule junction using an ultrafast-laser combined scanning tunnelling microscope-based break junction set-up at room temperature. Two resonant transport channels of ultrafast photocurrent are found by our photoelectron tunnelling spectroscopy, ranging from 1.31 eV to 1.77 eV, consistent with the LUMO + 1 and LUMO + 2 in the transmission spectrum obtained by density functional theory calculations. Moreover, we observed the modulation of resonant peaks by varying bias voltages, which demonstrates the ability to quantitatively characterize the effect of the electric field on frontier molecular orbitals. Our single-molecule photoelectron tunnelling spectroscopy offers an avenue that allows us to explore the nature of energy-dependent charge transport through single-molecule junctions.

Optimum Contact Configurations for Quasi-One-Dimensional Phosphorene Nanodevices.

We employ atomistic quantum transport simulations based on non-equilibrium Green's function (NEGF) formalism of quasi-one-dimensional (quasi-1D) phosphorene, or phosphorene nanoribbons (PNRs), to explore routes towards minimizing contact resistance (RC) in devices based on such nanostructures. The impact of PNR width scaling from ~5.5 nm down to ~0.5 nm, different hybrid edge-and-top metal contact configurations, and various metal-channel interaction strengths on the transfer length and RC is studied in detail. We demonstrate that optimum metals and top-contact lengths exist and depend on PNR width, which is a consequence of resonant transport and broadening effects. We find that moderately interacting metals and nearly edge contacts are optimum only for wider PNRs and phosphorene, providing a minimum RC of ~280 Ωμm. Surprisingly, ultra-narrow PNRs benefit from weakly interacting metals combined with long top contacts that lead to an added RC of only ~2 Ωμm in the 0.49 nm wide quasi-1D phosphorene nanodevice.

Defeating broken symmetry with doping: Symmetric resonant tunneling in noncentrosymetric heterostructures

Resonant tunneling transport in polar heterostructures is intimately connected to the polarization fields emerging from the geometric Berry-phase. In these structures, quantum confinement results not only in a discrete electronic spectrum, but also in built-in polarization charges exhibiting a broken inversion symmetry along the transport direction. Thus, electrons undergo highly asymmetric quantum interference effects with respect to the direction of current flow. By employing doping to counter the broken symmetry, we deterministically control the resonant transmission through GaN/AlN resonant tunneling diodes and experimentally demonstrate the recovery of symmetric resonant tunneling injection across the noncentrosymmetric double-barrier potential.

Active Control of Alfvén Eigenmodes by Externally Applied 3D Magnetic Perturbations.

The suppression and excitation of Alfvén eigenmodes have been experimentally obtained, for the first time, by means of externally applied 3D perturbative fields with different spatial spectra in a tokamak plasma. The applied perturbation causes an internal fast-ion redistribution that modifies the phase-space gradients responsible for driving the modes, determining, ultimately their existence. Hybrid kinetic-magnetohydrodynamic simulations reveal an edge resonant transport layer activated by the 3D perturbative field as the responsible mechanism for the fast-ion redistribution. The results presented here may help to control fast-ion driven Alfvénic instabilities in future burning plasmas with a significant fusion born alpha particle population.

Resonant transport in a highly conducting single molecular junction via metal-metal covalent bond.

Achieving highly transmitting molecular junctions through resonant transport at low bias is key to the next-generation low-power molecular devices. Although resonant transport in molecular junctions was observed by connecting a molecule between the metal electrodes via chemical anchors by applying a high source-drain bias (>1 V), the conductance was limited to <0.1G0, G0 being the quantum of conductance. Herein, we report electronic transport measurements by directly connecting a ferrocene molecule between Au electrodes under ambient conditions in a mechanically controllable break junction setup (MCBJ), revealing a conductance peak at ∼0.2G0 in the conductance histogram. A similar experiment was repeated for ferrocene terminated with amine (-NH2) and cyano (-CN) anchors, where conductance histograms exhibit an extended low conductance feature, including the sharp high conductance peak, similar to pristine ferrocene. The statistical analysis of the data and density functional theory-based transport calculation suggest a possible molecular conformation with a strong hybridization between the Au electrodes, and that the Fe atom of ferrocene is responsible for a near-perfect transmission in the vicinity of the Fermi energy, leading to the resonant transport at a small applied bias (<0.5 V). Moreover, calculations including van der Waals/dispersion corrections reveal a covalent-like organometallic bonding between Au and the central Fe atom of ferrocene, having bond energies of ∼660 meV. Overall, our study not only demonstrates the realization of an air-stable highly transmitting molecular junction, but also provides important insights about the nature of chemical bonding at the metal/organo-metallic interface.

Account of non-standard orbits in computations of neoclassical toroidal viscous torque in the resonant plateau regime of a tokamak

This article extends theoretical details based on a short paper originally submitted to the 2022 EPS conference in plasma physics [1]. The quasilinear theory of resonant transport regimes in a tokamak is developed for the general case of orbits forming various classes separated in phase space by homoclinic orbits with infinite bounce time. Beyond standard orbits (banana and passing orbits) also all types of non-standard orbits (e.g. “potato” orbits) are taken into account. In case of a weak radial electric field, such orbits are usually present only near the magnetic axis. If the radial electric field cannot be treated as weak, there can be arbitrary many classes, located elsewhere. The present approach covers all such cases and is demonstrated on a specific example of a radial electric field profile. The resulting quasilinear kinetic equation is applicable to compute neoclassical toroidal viscous (NTV) torque in a tokamak with non-axisymmetric magnetic field perturbations. A fully non-local approach to NTV computation has been realized in the upgraded version of the code NEO-RT. Based on a generalization of magnetic flux surfaces to drift surfaces, the notion of a local thermodynamic equilibrium is extended for our purpose. We obtain an expression for the integral toroidal torque within a chosen flux surface and dicuss means to compute such integrals taking singularities in bounce and precession frequencies into account.