Single Junctions Research Articles

Quantum Dots and Molecular Junctions as Energy Filters for Thermal-to-Electric Energy Conversion

The thermoelectric conversion of heat into electricity requires a form of energy filtering, that allows hot electrons to pass while blocking cold electrons. The energy conversion efficiency is determined by the details of the energy filtering, with an infinitely sharp (delta function) transmission spectrum allowing near ideal (Carnot) efficiency. [1]I will introduce this concept and report on a proof-of-performance experiment based on a quantum dot embedded into a single, semiconductor nanowire. This near-ideal quantum-dot heat engine realized power production at maximum power with Curzon-Ahlborn efficiency as well more than 70% of Carnot efficiency at maximum efficiency settings [2].To further enhance efficiency at maximum power one wishes to shape the transmission function to allow a spectrum of warmer electrons to pass while still completely blocking cold electrons. This may be achieved by exploiting quantum interference phenomena to block low-energy electron transmission by destructive interference, and to thus sculpt the transmission function of quantum dots or molecular junctions.[4] In contrast to quantum dots, molecular junctions have the advantage that they can be used at room temperature and can be produced, in principle, cheaply and scalable. To systematically explore the effect of quantum interferences, we designed and synthesized a new class of porphyrins that are expected to feature destructive quantum interference in single molecule junctions with gold electrodes and may thus show high thermopower, as well as a control that does not. We performed detailed experimental single-molecule break-junction studies of conductance and thermopower on porphyrin molecular junctions. We find a somewhat better thermoelectric performance for the porphyrin where we expect destructive interference. However, the predicted large difference in conductance and thermopower is not supported by our experimental findings.[4]Finally, I will also briefly discuss the potential application of the concepts and systems presented here in hot-carrier photovoltaics, as an approach to increasing photovoltaic energy conversion efficiency beyond current limits.[1] T.E. Humphrey et al., Reversible Quantum Brownian Heat Engines for Electrons. Phys. Rev. Lett., 89, 116801 (2002)[2] M. Josefsson et al. A quantum-dot heat engine operated close to thermodynamic efficiency limits. Nature Nanotechn. 13, 920 (2018)[3] O Karlström et al. Increasing thermoelectric performance using coherent transport. Phys. Rev. B 84, 113415 (2011)[4] H. Xu et al. Electrical Conductance and Thermopower of β-Substituted Porphyrin Molecular Junctions Synthesis and Transport. JACS 145 , 23541 (2023) Figure 1

Evidence of an Off-Resonant Electronic Transport Mechanism in Helicenes.

Helical molecules have been proposed as candidates for producing spin-polarized currents, even at room conditions, due to their chiral asymmetry. However, describing their transport mechanism in single molecular junctions is not straightforward. In this work, we show the synthesis of two novel kinds of dithia[11]helicenes to study their electronic transport in break junctions among a series of three helical molecules: dithia[n]helicenes, with n = 7, 9, and 11 molecular units. Our experimental measurements and clustering-based analysis demonstrate low conductance values that remain similar across different applied voltages and molecules. Additionally, we assess the length dependence of the conductance for each helicene, revealing an exponential decay characteristic of off-resonant transport. This behavior is primarily attributed to the misalignment between the energy levels of the molecule-electrodes system. The length dependence trend described above is supported by ab initio calculations, further confirming an off-resonant transport mechanism.

The shot noise in quasi-one-dimensional single spin filter magnetic heterojunctions

Based on the free electronic model and Büttike’s theory on shot noise, we investigated the shot noise of spin electrons in ferromagnetic/non-ferromagnetic insulator/spin filter layer/normal metal (FM/I/SF/NM) quasi-one-dimensional single spin filter tunneling junctions. The calculation results show that the barrier heights and thicknesses of the insulator and spin filter layers strongly affect the values and phases of the Fano factors of spin electrons. Compared with the traditional sandwich structures of ferromagnetic/spin filter layer/normal metal (FM/SF/NM) and ferromagnetic/non-ferromagnetic insulator/normal metal (FM/I/NM), when the thicknesses of the insulator and spin filter layers are very small, in single spin filter magnetic heterojunctions (FM/I/SF/NM), the insulator layer can suppress the Fano factors, while the spin filter layer is easier to separate the Fano factors of electrons whose spin directions are different. Further analysis shows that whether the Rashba coupling in the spin filter layer has an obvious influence on the Fano factors of spin electrons depends on the thickness of the spin filter layer. On the other hand, the Fano factors are strongly dependent on the sizes and directions of the molecular fields of the ferromagnet and spin filter layers. In addition, the electrons are incident with low energy or high energy, and the barrier heights and thicknesses of the spin filter layer and the thicknesses of the insulation layer have a significant effect on the spin-direction-dependent Fano factors of electrons.

HEOM‐QUICK2: A general‐purpose simulator for fermionic many‐body open quantum systems—An update

AbstractMany‐body open quantum systems (OQSs) have a profound impact on various subdisciplines of physics, chemistry, and biology. Thus, the development of a computer program capable of accurately, efficiently, and versatilely simulating many‐body OQSs is highly desirable. In recent years, we have focused on the advancement of numerical algorithms based on the fermionic hierarchical equations of motion (HEOM) theory. Being in‐principle exact, this approach allows for the precise characterization of many‐body correlations, non‐Markovian memory, and non‐equilibrium thermodynamic conditions. These efforts now lead to the establishment of a new computer program, HEOM for QUantum Impurity with a Correlated Kernel, version 2 (HEOM‐QUICK2), which, to the best of our knowledge, is currently the only general‐purpose simulator for fermionic many‐body OQSs. Compared with version 1, the HEOM‐QUICK2 program features more efficient solvers for stationary states, more accurate treatment of non‐Markovian memory, and improved numerical stability for long‐time dissipative dynamics. Integrated with quantum chemistry software, HEOM‐QUICK2 has become a valuable theoretical tool for the precise simulation of realistic many‐body OQSs, particularly the single atomic or molecular junctions. Furthermore, the unprecedented precision achieved by HEOM‐QUICK2 enables accurate simulation of low‐energy spin excitations and coherent spin relaxation. The unique usefulness of HEOM‐QUICK2 is demonstrated through several examples of strongly correlated quantum impurity systems under non‐equilibrium conditions. Thus, the new HEOM‐QUICK2 program offers a powerful and comprehensive tool for studying many‐body OQSs with exotic quantum phenomena and exploring applications in various disciplines.This article is categorized under: Data Science > Computer Algorithms and Programming Software > Simulation Methods Theoretical and Physical Chemistry > Statistical Mechanics

Chiral-induced angular momentum radiation in single molecular junctions

Chiral-induced angular momentum radiation in single molecular junctions

Disordered Ballistic Bismuth Nano-waveguides for Highly Efficient Thermoelectric Energy Conversion.

Junctions based on electronic ballistic waveguides, such as semiconductor nanowires or nanoribbons with transverse structural variations in the order of a large fraction of their Fermi wavelength, are suggested as highly efficient thermoelectric (TE) devices. Full harnessing of their potential requires a capability to either deterministically induce structural variations that tailor their transmission properties at the Fermi level or alternatively to form waveguides that are disordered (chaotic) but can be structurally modified continuously until favorable TE properties are achieved. Well-established methods to realize either of these routes do not exist. Here, disordered bismuth (Bi) waveguides are reported, which are both formed and structurally tuned by electromigration until their efficiency as TE devices is maximized. In accordance with theory, the conductance of the most efficient TE waveguides is in the sub quantum of conductance regime. The stability of these structures is found to be substantially higher than other actively studied devices such as single molecule junctions.

MgB[formula omitted] Josephson Junctions fabricated by Focused Helium Ion Beam with different irradiation doses on SiC and MgO substrates

Recently, high quality MgB2 single junctions and junction arrays fabricated by Focused Helium Ion Beam irradiation (He-FIB) have been reported. However, the effects of irradiation doses and substrates on junction properties have not been analysed systematically. In this work, 30 nm MgB2 thin films were deposited on SiC (0001) and MgO (111) substrates using Hybrid Physical–Chemical Vapour Deposition (HPCVD) technique and then etched into 2–4 μm wide microbridges. 2000–6000 ions/nm doses of He-FIB were irradiated across these microbridges, creating narrow junction barriers. R–T curves exhibit a clear foot-like structure that enlarges as irradiation dose increases. Temperature dependence of junction properties (critical current Ic, junction normal state resistance Rn, characteristic voltage Vc) shows that all junctions in our experiment exhibit superconductor–normal–superconductor (SNS) like behaviour and higher irradiation doses create thicker junction barriers. Furthermore, we analyse junction properties dependence on irradiation doses which yields an exponential change law. Finally, Fraunhofer diffraction-like patterns and Shapiro steps of junctions are also measured. Our results show MgB2 Josephson Junctions with adjustable properties can be fabricated by He-FIB on SiC and MgO substrates, which provides a solid foundation for future application devices research.

Many-body Effects on Electronic Transport in Molecular Junctions: A Quantum Perspective.

This concept delves into quantum particle transport at the nanoscale, with a particular focus on how electrons move through molecular circuits. The thriving field of single molecular electronics benefits from the unique electrical and other properties of nanostructures. It concentrates on single molecular junctions that serve as bridges between electrodes. In this context, the electronic correlation-induced many-body effect gives rise to resonant states. These states, along with conductance, depend on electron spin. Thus, the field acts as a bridge between quantum and macroscopic worlds, unveiling unique behaviors of electrons. Additionally, external factors, such as magnetic fields and voltages, offer means to control the electron correlation in these junctions.

Torque‐tuned I‐V characteristics in a piezoelectric semiconductor composite fiber

AbstractThis paper studies the multi‐physical fields in a torsional composite fiber composed of a non‐piezoelectric semiconductor (PS) core coated with a piezoelectric dielectric shell. Based on the three‐dimensional framework of piezoelectricity and drift‐diffusion theory, we develop a nonlinear one‐dimensional model that incorporates the warping deformation, shear deformation, and axial variations of the electric field and charge transportations. A One‐dimensional model is linearized for small perturbations of charges, and we obtain the analytical solutions for single rods or PN junctions when torques are applied, which explicitly illustrates the electromechanical fields and redistribution of mobile charges. We also examine how the thickness of the composite rods affects the interaction between the piezoelectric and semiconductor components in the model. The optimal thickness ratio for maximizing the overall mobility of carriers has been discovered. This enables us to modify the thickness ratio to achieve the greatest PS interaction performance. Based on the nonlinear equations, we analyze the relationships between electric currents and applied voltages on the end of rods. Finally, we examine how twisting moments influence the characteristics of this I‐V relationship. The presented study provides a potential application for mechanical switches or sensors for PSs.

Power consumption during forward locomotion of C. elegans: an electrical circuit simulation

Biological neuronal networks are of great interest for emerging technological approaches such as neuromorphic engineering due to their capability to efficiently process information. To understand the principles governing this energy efficiency, it is useful to investigate model organisms with small and well-characterized neuronal networks. Caenorhabditis elegans (C. elegans) is such a model organism and perfectly suited for this purpose, because its neuronal network consists of only 302 neurons whose interconnections are known. In this work, we design an ideal electrical circuit modeling this neuronal network in combination with the muscles it controls. We simulate this circuit by a run-time efficient wave digital algorithm. This allows us to investigate the energy consumption of the network occurring during locomotion of C. elegans and hence deduce potential design principles from an energy efficiency point of view. Simulation results verify that a locomotion is indeed generated. We conclude from the corresponding energy consumption rates that a small number of neurons in contrast to a high number of interconnections is favorable for consuming only little energy. This underlines the importance of interneurons. Moreover, we find that gap junctions are a more energy-efficient connection type than synapses, and inhibitory synapses consume more energy than excitatory ones. However, the energetically cheapest connection types are not the most frequent ones in C. elegans’ neuronal network. Therefore, a potential design principle of the network could be a balance between low energy costs and a certain functionality.Graphical abstractEnergy consumption rates during forward locomotion of C. elegans. a Rates for the ion channels of all neurons, and b average rates for ion channels of a single, active neuron. c Comparison of average rates with respect to the number of active sensory, motor, and interneurons. d Rates for all gap junctions and synapses, and e rates for all synapses of a specific neurotransmitter type. f Average rates for a single synaptic or gap junctions connection vs the total number of connections present for the type of connection (i.e. ACh-synapse, GABA-synapse, Glu-synapse, gap junction).

Thermoelectric response of textured Sb2Te3–BiSb and Sb2Te3–Bi2Te3 thin film junctions

Surface mounted thin film thermoelectric (TE) devices for localized cooling, power generation, and sensing are topics of immense current interest. Here, we establish the superior TE performance of thin film junctions made of topological insulators (TIs) Bi85Sb15 (BiSb) and Sb2Te3 by comparing their performance with those of Bi2Te3 and Sb2Te3. Thin films of these TIs were first evaluated for their carrier concentration, Hall mobility, resistivity, and thermopower. The Seebeck coefficient of BiSb, Sb2Te3, and Bi2Te3 measured against copper at ambient temperature is −100, +160, and −70 (±10) μV/K, while their power factors are 0.5, 0.5, and 0.45 (±0.05) 10−3 W m−1 K−2, respectively. Single TE junctions of BiSb–Sb2Te3 and Bi2Te3–Sb2Te3 yield a response of 272 and 240 (±10) μV/K, respectively. This comparative study shows that BiSb is a superior n-type counter electrode for Sb2Te3 compared to the n-type Bi2Te3. Moreover, Bi2Te3 is prone to tellurium antisite disorder, which affects its TE properties significantly.

Emergence of Boltzmann Subspaces in Open Quantum Systems Far from Equilibrium.

Single molecule junctions are important examples of complex out-of-equilibrium many-body quantum systems. We identify a nontrivial clustering of steady state populations into distinctive subspaces with Boltzmann-like statistics, which persist far from equilibrium. Such Boltzmann subspaces significantly reduce the information needed to describe the steady state, enabling modeling of high-dimensional systems that are otherwise beyond the reach of current computations. The emergence of Boltzmann subspaces is demonstrated analytically and numerically for fermionic transport systems of increasing complexity.

Regulation of π-π interactions between single aromatic molecules by bias voltage.

π-stacking interaction, as a fundamental type of intermolecular interaction, plays a crucial role in generating new functional molecules, altering the optoelectronic properties of materials, and maintaining protein structural stability. However, regulating intermolecular π-π interactions at the single-molecule level without altering the molecular conformation as well as the chemical properties remains a significant challenge. To this end, via conductance measurement with thousands of single molecular junctions employing a series of aromatic molecules, we demonstrate that the π-π coupling between neighboring aromatic molecules with rigid structures in a circuit can be greatly enhanced by increasing the bias voltage. We further reveal that this universal regulating effect of bias voltage without molecular conformational variation originates from the increases of the molecular dipole upon an applied electric field. These findings not only supply a non-destructive method to regulate the intermolecular interactions offering an approach to modulate the electron transport through a single molecular junction, but also deepen the understanding of the mechanism of π-π interactions.

Greatly enhanced tunneling electroresistance in ferroelectric tunnel junctions with a double barrier design

We propose that the double barrier effect is expected to enhance the tunneling electroresistance (TER) in the ferroelectric tunnel junctions (FTJs). To demonstrate the feasibility of this mechanism, we design a model structure of Pt/BaTiO3/LaAlO3/Pt/BaTiO3/LaAlO3/Pt double barrier ferroelectric tunnel junction (DB-FTJ), which can be considered as two identical Pt/BaTiO3/LaAlO3/Pt single barrier ferroelectric tunnel junctions (SB-FTJs) connected in series. Based on density functional calculation, we obtain the giant TER ratio of 2.210 × 108% in the DB-FTJ, which is at least three orders of magnitude larger than that of the SB-FTJs of Pt/BaTiO3/LaAlO3/Pt, together with an ultra-low resistance area product (0.093 KΩμm2) in the high conductance state of the DB-FTJ. Moreover, it is possible to control the direction of polarization of the two single ferroelectric barriers separately and thus four resistance states can be achieved, making DB-FTJs promising as multi-state memory devices.

Quantum dynamics of the internal motion of biphenyl-based molecular junctions.

Single molecule junctions based on selected 4,4'-biphenyldithiol and 4,4'-dicyanobiphenyl derivatives bonded to gold electrodes are analyzed from a dynamical point of view. A fully quantum mechanical description of the internal rotation of the biphenyl moiety is carried out in terms of the nuclear wavepacket dynamics obtained by the solution of the time-dependent Schrödinger equation expressed in terms of the torsion angle between the phenyl rings. The required potential energy surfaces are computed using abinitio electronic structure methods. The nature and positions of the substituents on the phenyl rings determine the features of the potential energy surfaces. The effect of the initial conditions on the time propagation of the nuclear wavepackets and, as a consequence, on the evolution of the conformational distribution is also analyzed. In addition, the conductances at zero bias for the nanojunctions were computed for different conformations of the biphenyl fragments. Weighted by the wavepacket amplitudes, non-stationary conductance expectation values, and time-averaged torsion angles and conductances for the entire simulation are obtained. The consequences of using the time-averaged values to perform a linear regression between the conductance and the square of the cosine of the dihedral angle between the phenyl rings are analyzed and compared to the usual static approach based only on the information for equilibrium geometries. The study of the time dependent conformational variations of the biphenyl moieties in the nanojunctions allows for a better understanding of the quantum chemical phenomena that affect their transport properties.

Optimization of the tunneling magnetoresistance and spin-valley polarization in complex magnetic silicene structures

Aperiodic order is ubiquitous in nature and quite relevant in science and technology. There are extensive works in aperiodic structures studying fundamental characteristics in physical properties, such as fractality, self-similarity, and fragmentation. However, there are fewer reports in which aperiodicity signifies an improvement in physical quantities with practical applications. Here, we show that the aperiodicity of fractal or self-similar type optimizes the tunneling magnetoresistance and spin-valley polarization of magnetic silicene structures, raising the prospects of spin-valleytronics. We reach this conclusion by studying the spin-valley-dependent transport properties of complex (Cantor-like) magnetic silicene structures within the lines of the transfer matrix method and the Landauer–Büttiker formalism. We find that the self-similar arrangement of magnetic barriers in conjunction with structural asymmetry reduces the conductance oscillations typical of periodic magnetic silicene superlattices and more importantly makes the K′-spin-down conductance component dominant, resulting in nearly perfect positive and negative spin-valley polarization states accessible by simply reversing the magnetization direction. The tunneling magnetoresistance is not as prominent as in periodic magnetic silicene superlattices; however, it is better than in single magnetic junctions. Furthermore, the optimization of the spin-valley-dependent transport properties caused by the complex structure is superior than the corresponding one reported in typical aperiodic structures, such as Fibonacci and Thue–Morse magnetic silicene superlattices.

Interface engineering for high-performance, triple-halide perovskite-silicon tandem solar cells.

Improved stability and efficiency of two-terminal monolithic perovskite-silicon tandem solar cells will require reductions in recombination losses. By combining a triple-halide perovskite (1.68 electron volt bandgap) with a piperazinium iodide interfacial modification, we improved the band alignment, reduced nonradiative recombination losses, and enhanced charge extraction at the electron-selective contact. Solar cells showed open-circuit voltages of up to 1.28 volts in p-i-n single junctions and 2.00 volts in perovskite-silicon tandem solar cells. The tandem cells achieve certified power conversion efficiencies of up to 32.5%.

The spin-polarized tunnel current and the spin-transfer torque in triple-barrier junctions with external electrodes and quantum wells made of ferromagnetic materials

The electron transport in triple-barrier junctions consisting of external ferromagnetic layers and three non-magnetic barriers separated by two inner ferromagnetic layers is analysed. It is assumed that the magnetic moments in the external electrodes are oriented in the same direction, whereas the magnetic moments of the inner layers can form any angle with this direction. The possibility of the gigantic enhancement of the normal torque component has been found in the junctions with a non-colinear orientation of magnetic moments in the inner layers. This enhancement may be much larger than in the double junctions. The current and the in-plane torque are most amplified when the quantum-well states in both inner layers have similar energies and can form the complex resonant states located slightly below the Fermi level. When the tunnelling by these complex resonant states occurs, the torque is greatest in the magnetic configuration other than that where the current is maximally enhanced. Additionally, the angular dependence of the torque differs significantly from that observed in single tunnel junctions.

Retro and specular Andreev reflections and valley-spin switching effect in graphene superconducting heterojunction

We investigated Andreev reflection of graphene-based normal/superconductor single and double junctions under the modulation of non-resonant circularly polarized light, staggered potential, and exchange field. In the graphene-based normal/superconductor single junction, we discovered that the circularly polarized light can adjust the bandgap of retro Andreev reflection and specular Andreev reflection. The exchange field can change the position of the transition point between retro Andreev reflection and specular Andreev reflection. In the graphene-based normal/superconductor/normal double junction, when the light field is modulated from left circularly polarized light to right circularly polarized light, the valley-spin switching effect between pure elastic co-tunneling and pure crossed Andreev reflection can be realized. By changing the exchange field, we achieved the conversion of non-local transport between pure elastic co-tunneling and pure crossed Andreev reflection. In addition, the energy location and range of crossed Andreev reflection and elastic co-tunneling can be controlled by the staggered potential and the exchange field. Our results suggest that the device can implement light and exchange field control of the Andreev reflection process and the spin-valley switch.

Double‐sided nano‐textured surfaces for industry compatible high‐performance silicon heterojunction and perovskite/silicon tandem solar cells

AbstractNano‐textured surfaces are an intriguing approach for optimizing the optical characteristics for monolithic perovskite/silicon tandem solar cells. Here, the development of different textures of silicon surfaces using various commercial additives is presented and their performance in silicon heterojunction (SHJ) and SHJ–perovskite tandem solar cells is discussed. After optical and electrical characterization, we show that nano‐textured surfaces can easily compete with standard textured surfaces, yielding higher average efficiencies in single junctions. In addition, their compatibility with solution‐processed perovskite top cells is demonstrated, yielding a perovskite/silicon tandem solar cell efficiency of >28% on a bottom cell with nano‐texture on both sides.