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Increasing electric current from a single-electron source is a main challenge in an effort to establish the standard of the ampere defined by the fixed value of the elementary charge $e$ and operation frequency $f$. While the current scales with $f$, due to an operation frequency limit for maintaining accurate single-electron transfer, parallelisation of singleelectron sources is expected to be a more practical solution to increase the generated electric current $I = Nef$, where $N$ is a number of parallelised devices. One way to parallelise single-electron sources without increasing the complexity in device operation is to use a common gate. Such a scheme will require each device to have the same operation parameters for single-electron transfer. In order to investigate this possibility, we study the statistics for operation gate voltages using single-electron sources embedded in a multiplexer circuit. The multiplexer circuit allows us to measure 64 single-electron sources individually in a single cooldown. We also demonstrate the parallelisation of three single-electron sources and observe the generated current enhanced by a factor of three., Comment: 5 pages, 3 figures

We present an efficient machine learning based automated framework for the fast tuning of single-electron pump devices into current quantization regimes. It uses a sparse measurement approach based on an iterative active learning algorithm to take targeted measurements in the gate voltage parameter space. When compared to conventional parameter scans, our automated framework allows us to decrease the number of measurement points by about an order of magnitude. This corresponds to an eight-fold decrease in the time required to determine quantization errors, which are estimated via an exponential extrapolation of the first current plateau embedded into the algorithm. We show the robustness of the framework by characterizing 28 individual devices arranged in a GaAs/AlGaAs multiplexer array, which we use to identify a subset of devices suitable for parallel operation at communal gate voltages. The method opens up the possibility to efficiently scale the characterization of such multiplexed devices to a large number of pumps., Comment: 6 pages, 3 figures

The development of nanoscale solid-state devices exploiting the promising topological surface states of topological insulator materials requires careful device engineering and improved materials quality. For instance, the introduction of a substrate, device contact or the formation of oxide layers can cause unintentional doping of the material, spoiling the sought-after properties. In support of this, nanoscale imaging tools can provide useful materials information without the need for complex device fabrication. Here we study Bi$_2$Se$_3$ nanoribbons suspended across multiple material stacks of SiO$_2$ and Au using infrared scattering scanning near-field optical microscopy. We validate our observations against a multilayer finite dipole model to obtain quantitative imaging of the local Bi$_2$Se$_3$ properties that vary depending on the local environment. Moreover, we identify experimental signatures that we associate with quantum well states at the Bi$_2$Se$_3$ surfaces. Our approach opens a new direction for future engineering of nanoelectronic devices based on topological insulator materials.

The developments of quantum computing algorithms and experiments for atomic scale simulations have largely focused on quantum chemistry for molecules, while their application in condensed matter systems is scarcely explored. Here we present a quantum algorithm to perform dynamical mean field theory (DMFT) calculations for condensed matter systems on currently available quantum computers, and demonstrate it on two quantum hardware platforms. DMFT is required to properly describe the large class of materials with strongly correlated electrons. The computationally challenging part arises from solving the effective problem of an interacting impurity coupled to a bath, which scales exponentially with system size on conventional computers. An exponential speedup is expected on quantum computers, but the algorithms proposed so far are based on real time evolution of the wavefunction, which requires high-depth circuits and hence very low noise levels in the quantum hardware. Here we propose an alternative approach, which uses the variational quantum eigensolver (VQE) method for ground and excited states to obtain the needed quantities as part of an exact diagonalization impurity solver. We present the algorithm for a two site DMFT system, which we benchmark using simulations on conventional computers as well as experiments on superconducting and trapped ion qubits, demonstrating that this method is suitable for running DMFT calculations on currently available quantum hardware.

Stable organic radicals integrated into molecular junctions represent a practical realization of the single-orbital Anderson impurity model. Motivated by recent experiments for perchlorotriphenylmethyl (PTM) molecules contacted to gold electrodes, we develop a method that combines density functional theory (DFT), quantum transport theory, numerical renormalization group (NRG) calculations and renormalized super-perturbation theory (rSPT) to compute both equilibrium and non-equilibrium properties of strongly correlated nanoscale systems at low temperatures effectively from first principles. We determine the possible atomic structures of the interfaces between the molecule and the electrodes, which allow us to estimate the Kondo temperature and the characteristic transport properties, which compare well with experiments. By using the non-equilibrium rSPT results we assess the range of validity of equilibrium DFT+NRG-based transmission calculations for the evaluation of the finite voltage conductance. The results demonstrate that our method can provide qualitative insights into the properties of molecular junctions when the molecule-metal contacts are amorphous or generally ill-defined, and that it can further give a fully quantitative description when the experimental contact structures are well characterized., Comment: Nanoscale, 2018

Reversible resistive switching between high-resistance and low-resistance states in metal-oxide-metal heterostructures makes them very interesting for applications in random access memories. While recent experimental work has shown that inserting a metallic "oxygen scavenger layer" between the positive electrode and oxide improves device performance, the fundamental understanding of how the scavenger layer modifies heterostructure properties is lacking. We use density functional theory to calculate thermodynamic properties and conductance of TiN/HfO$_2$/TiN heterostructures with and without Ta scavenger layer. First, we show that Ta insertion lowers the formation energy of low-resistance states. Second, while the Ta scavenger layer reduces the Schottky barrier height in the high-resistance state by modifying the interface charge at the oxide-electrode interface, the heterostructure maintains a high resistance ratio between high- and low-resistance states. Finally, we show that the low-bias conductance of device on-states becomes much less sensitive to the spatial distribution of oxygen removed from the HfO$_2$ in the presence of the Ta layer. By providing fundamental understanding of the observed improvements with scavenger layers, we open a path to engineer interfaces with oxygen scavenger layers to control and enhance device performance. In turn, this may enable the realization of a non-volatile low-power memory technology with concomitant reduction in energy consumption by consumer electronics and significant benefits to society., Comment: 9 pages, 10 figures

The effects of local electronic interactions and finite temperatures upon the transmission across the Cu$_4$CoCu$_4$ metallic heterostructure are studied in a combined density functional and dynamical mean field theory. It is shown that, as the electronic correlations are taken into account via a local but dynamic self-energy, the total transmission at the Fermi level gets reduced (predominantly in the minority spin channel), whereby the spin polarization of the transmission increases. The latter is due to a more significant $d$-electrons contribution, as compared to the non-correlated case in which the transport is dominated by $s$ and $p$ electrons., Comment: 29 pages, 7 figures, submited to PRB

We present a computational scheme for extracting the energy level alignment of a metal/molecule interface, based on constrained density functional theory and local exchange and correlation functionals. The method, applied here to benzene on Li(100), allows us to evaluate charge transfer energies, as well as the spatial distribution of the image charge induced on the metal surface. We systematically study the energies for charge transfer from the molecule to the substrate as function of the molecule-substrate distance, and investigate the effects arising from image charge confinement and local charge neutrality violation. For benzene on Li(100) we find that the image charge plane is located at about 1.8 \AA above the Li surface, and that our calculated charge transfer energies compare perfectly with those obtained with a classical electrostatic model having the image plane located at the same position. The methodology outlined here can be applied to study any metal/organic interface in the weak coupling limit at the computational cost of a total energy calculation. Most importantly, as the scheme is based on total energies and not on correcting the Kohn-Sham quasiparticle spectrum, accurate results can be obtained with local/semi-local exchange and correlation functionals. This enables a systematic approach to convergence.

Rapid and cost-effective DNA sequencing at the single nucleotide level might be achieved by measuring a transverse electronic current as single-stranded DNA is pulled through a nano-sized pore. In order to enhance the electronic coupling between the nucleotides and the electrodes and hence the current signals, we employ a pair of single-walled close-ended (6,6) carbon nanotubes (CNTs) as electrodes. We then investigate the electron transport properties of nucleotides sandwiched between such electrodes by using first-principles quantum transport theory. In particular we consider the extreme case where the separation between the electrodes is the smallest possible that still allows the DNA translocation. The benzene-like ring at the end cap of the CNT can strongly couple with the nucleobases and therefore both reduce conformational fluctuations and significantly improve the conductance. The optimal molecular configurations, at which the nucleotides strongly couple to the CNTs, and which yield the largest transmission, are first identified. Then the electronic structures and the electron transport of these optimal configurations are analyzed. The typical tunneling currents are of the order of 50 nA for voltages up to 1 V. At higher bias, where resonant transport through the molecular states is possible, the current is of the order of several $\mu$A. Below 1 V the currents associated to the different nucleotides are consistently distinguishable, with adenine having the largest current, guanine the second-largest, cytosine the third and finally thymine the smallest. We further calculate the transmission coefficient profiles as the nucleotides are dragged along the DNA translocation path and investigate the effects of configurational variations. Based on these results we propose a DNA sequencing protocol combining three possible data analysis strategies., Comment: 12 pages, 17 figures, 3 tables

We investigate the spin transport properties of molecules belonging to the acenes series by using density functional theory combined with the non-equilibrium Green's function approach to electronic transport. While short acenes are found to be non-magnetic, molecules comprising more than nine acene rings have a spin-polarized ground state. In their gas phase these have a singlet total spin configuration, since the two unpaired electrons occupying the doubly degenerate highest molecular orbital are antiferromagnetically coupled to each other. Such an orbital degeneracy is however lifted once the molecule is attached asymmetrically to Au electrodes via thiol linkers, leading to a fractional magnetic moment. In this situation the system Au/n-acene/Au can act as an efficient spin-filter with interesting applications in the emerging field of organic spintronics., Comment: 13 pages,9 figures

The bias-dependent transport properties of short poly(G)-poly(C) A-DNA strands attached to Au electrodes are investigated with first principles electronic transport methods. By using the non- equilibrium Green's function approach combined with self-interaction corrected density functional theory, we calculate the fully self-consistent coherent I-V curve of various double-strand polymeric DNA fragments. We show that electronic wave-function localization, induced either by the native electrical dipole and/or by the electrostatic disorder originating from the first few water solvation layers, drastically suppresses the magnitude of the elastic conductance of A-DNA oligonucleotides. We then argue that electron transport through DNA is the result of sequence-specific short-range tunneling across a few bases combined with general diffusive/inelastic processes., Comment: 15 pages, 13 figures, 1 table

The effects of water wetting conditions on the transport properties of molecular nano-junctions are investigated theoretically by using a combination of classical molecular dynamics and first principles electronic transport calculations. These are at the level of the non-equilibrium Green's function method implemented for self-interaction corrected density functional theory. We find that water effectively produces electrostatic gating to the molecular junction, with a gating potential determined by the time-averaged water dipole field. Such a field is large for the polar benzene-dithiol molecule, resulting in a transmission spectrum shifted by about 0.6 eV with respect to that of the dry junction. The situation is drastically different for carbon nanotubes (CNTs). In fact, because of their hydro-phobic nature the gating is almost negligible, so that the average transmission spectrum of wet Au/CNT/Au junctions is essentially the same as that in dry conditions. This suggests that CNTs can be used as molecular interconnects also in water-wet situations, for instance as tips for scanning tunnel microscopy in solution or in biological sensors.

We demonstrate that the different magnetic states of a Mn12 molecule can be distinguished in a two-probe transport experiment from a complete knowledge of the current-voltage curve. Our results, obtained with state-of-the-art non-equilibrium transport methods combined with density functional theory, demonstrate that spin configuration-specific negative differential resistances (NDRs) appear in the I-V curves. These originate from the interplay between electron localization and the re-hybridization of the molecular levels in an external electric field and allow the detection of the molecule's spin-state., Comment: 8 pages, 8 figures, 2 page supplementary material

The interface structure of Fe/MgO(100) magnetic tunnel junctions predicted by density functional theory (DFT) depends significantly on the choice of exchange and correlation functional. Bader analysis reveals that structures obtained by relaxing the cell with the local spin-density approximation (LSDA) display a different charge transfer than those relaxed with the generalized gradient approximation (GGA). As a consequence, the electronic transport is found to be extremely sensitive to the interface structure. In particular, the conductance for the LSDA-relaxed geometry is about one order of magnitude smaller than that of the GGA-relaxed one. The high sensitivity of the electronic current to the details of the interface might explain the discrepancy between the experimental and calculated values of magnetoresistance., Comment: Submitted to PRL, 5 figures

In this work, we calculate with ab initio methods the current-voltage characteristics for ideal single- and double-barrier Fe/MgO (001) magnetic tunnel junctions. The current is calculated in the phase-coherent limit by using the recently developed SMEAGOL code, combining the nonequilibrium Green function formalism with density-functional theory. In general we find that double-barrier junctions display a larger magnetoresistance, which decays with bias at a slower pace than their single-barrier counterparts. This is explained in terms of enhanced spin filtering from the middle Fe layer sandwiched in between the two MgO barriers. In addition, for double-barrier tunnel junctions, we find a well defined peak in the magnetoresistance at a voltage of V=0.1 V. This is the signature of resonant tunneling across a majority quantum well state. Our findings are discussed in relation to recent experiments.