Subgap States Research Articles

A Facile Method Based on Oxide Semiconductor Reduction for Controlling the Photoresponse Characteristic of Flexible and Transparent Optoelectronic Devices

AbstractA facile method is presented involving a reducing agent, sodium dithionite (Na2S2O4), to control the photoresponse characteristics of oxide semiconductors that detect visible‐light. The method exhibits extraordinary potential for fabricating a diverse range of optoelectronic devices. Due to its weak S–S bond, Na2S2O4 generates excessive subgap states and oxygen vacancies in hafnium–indium–gallium–zinc oxide (HIGZO) thin‐film during the reduction treatment (RDT). It is achievable to finely tune the photoresponse characteristic by adjusting the molarity of Na2S2O4, implying superior applicability of RDT into various applications. First, HIGZO phototransistors with photoresponsivity of 626.32 A W−1, photosensitivity of 3.32 × 107, and detectivity of 7.18 × 1011 Jones under 10 mW mm−2 of red light illumination are fabricated using 0.1 m Na2S2O4. Second, 0.5 m Na2S2O4 is chosen for photomemory‐based neuromorphic devices with a paired‐pulse facilitation index of 142.6% when the input pulse of red light with an intensity of 1 mW mm−2 is introduced. In addition, major synaptic functions such as short‐term memory and long‐term memory behaviors, originated from persistent photoconductivity and depending on sequential pulse condition, are successfully emulated. These results indicate that RDT can control the photoresponse of oxide semiconductors to expand the applicability of oxide semiconductors without using a light absorption layer.

Electron-boson-interaction induced particle-hole symmetry breaking of conductance into subgap states in superconductors

Particle-hole symmetry (PHS) of conductance into subgap states in superconductors is a fundamental consequence of a noninteracting mean-field theory of superconductivity. The breaking of this PHS has been attributed to a noninteracting mechanism, i.e., quasiparticle poisoning (QP), a process detrimental to the coherence of superconductor-based qubits.Here, we show that the ubiquitous electron-boson interactions in superconductors can also break the PHS of subgap conductances. We study the effect of such couplings on the PHS of subgap conductances in superconductors using both the rate equation and Keldysh formalism, which have different regimes of validity. In both regimes, we found that such couplings give rise to a particle-hole $asymmetry$ in subgap conductances which increases with increasing coupling strength, increasing subgap-state particle-hole content imbalance and decreasing temperature. Our proposed mechanism is general and applies even for experiments where the subgap-conductance PHS breaking cannot be attributed to QP.

Charge-neutral nonlocal response in superconductor-InAs nanowire hybrid devices

Nonlocal quasiparticle transport in normal-superconductor-normal (NSN) hybrid structures probes sub-gap states in the proximity region and is especially attractive in the context of Majorana research. Conductance measurement provides only partial information about nonlocal response composed from both electron-like and hole-like quasiparticle excitations. In this work, we show how a nonlocal shot noise measurement delivers a missing puzzle piece in NSN InAs nanowire-based devices. We demonstrate that in a trivial superconducting phase quasiparticle response is practically charge-neutral, dominated by the heat transport component with a thermal conductance being on the order of conductance quantum. This is qualitatively explained by numerous Andreev reflections of a diffusing quasiparticle, that makes its charge completely uncertain. Consistently, strong fluctuations and sign reversal are observed in the sub-gap nonlocal conductance, including occasional Andreev rectification signals. Our results prove conductance and noise as complementary measurements to characterize quasiparticle transport in superconducting proximity devices.

Theory of Coulomb blockaded transport in realistic Majorana nanowires

Coulomb blockaded transport of topological superconducting nanowires provides an opportunity to probe the localization of states at both ends of the system in a two-terminal geometry. In addition, it provides a way for checking for subgap states away from the leads. At the same time, Coulomb blockade transport is difficult to analyze because of the interacting nature of the problem arising from the nonperturbative Coulomb interaction inherent in the phenomenon. Here we show that the Coulomb blockade transport can be modeled at the same level of complexity as quantum point contact tunneling that has routinely been used in mesoscopic physics to understand nanowire experiments provided we consider the regime where the tunneling rate is below the equilibration rate of the nanowire. This assumption leads us to a generalized Meir-Wingreen formula for the tunnel conductance which we use to study various features of the nanowire such as Andreev bound states, self-energy, and soft gap. We anticipate that our theory will provide a route to interpret Coulomb blockade transport in hybrid Majorana systems as resulting from features of the nanowire, such as Andreev bound states and soft gaps.

Novel Method for Fabricating Visible-Light Phototransistors Based on a Homojunction-Porous IGZO Thin Film Using Mechano-Chemical Treatment.

A homojunction-structured oxide phototransistor based on a mechano-chemically treated indium-gallium-zinc oxide (IGZO) absorption layer is reported. Through this novel and facile mechano-chemical treatment, mechanical removal of the cellophane adhesive tape induces reactive radicals and organic compounds on the sputtered IGZO film surface. Surface modification, following the mechano-chemical treatment, caused porous sites in the solution-processed IGZO film, which can give rise to a homojunction-porous IGZO (HPI) layer and generate sub-gap states from oxygen-related defects. These intentionally generated sub-gap states played a key role in photoelectron generation under illumination with relatively long-wavelength visible light despite the wide band gap of IGZO (>3.0 eV). Compared with conventional IGZO phototransistors, our HPI phototransistor displayed outstanding optoelectronic characteristics and sensitivity; we measured a threshold voltage (Vth) shift from 3.64 to -6.27 V and an on/off current ratio shift from 4.21 × 1010 to 4.92 × 102 under illumination with a 532 nm green light of 10 mW/mm2 intensity and calculated a photosensitivity of 1.16 × 108. The remarkable optoelectronic characteristics and high optical transparency suggest optical sensor applications.

Direct observation of trap-assisted recombination in organic photovoltaic devices

Trap-assisted recombination caused by localised sub-gap states is one of the most important first-order loss mechanism limiting the power-conversion efficiency of all solar cells. The presence and relevance of trap-assisted recombination in organic photovoltaic devices is still a matter of some considerable ambiguity and debate, hindering the field as it seeks to deliver ever higher efficiencies and ultimately a viable new solar photovoltaic technology. In this work, we show that trap-assisted recombination loss of photocurrent is universally present under operational conditions in a wide variety of organic solar cell materials including the new non-fullerene electron acceptor systems currently breaking all efficiency records. The trap-assisted recombination is found to be induced by states lying 0.35-0.6 eV below the transport edge, acting as deep trap states at light intensities equivalent to 1 sun. Apart from limiting the photocurrent, we show that the associated trap-assisted recombination via these comparatively deep traps is also responsible for ideality factors between 1 and 2, shedding further light on another open and important question as to the fundamental working principles of organic solar cells. Our results also provide insights for avoiding trap-induced losses in related indoor photovoltaic and photodetector applications.

Highly sensitive active pixel image sensor array driven by large-area bilayer MoS2 transistor circuitry

Various large-area growth methods for two-dimensional transition metal dichalcogenides have been developed recently for future electronic and photonic applications. However, they have not yet been employed for synthesizing active pixel image sensors. Here, we report on an active pixel image sensor array with a bilayer MoS2 film prepared via a two-step large-area growth method. The active pixel of image sensor is composed of 2D MoS2 switching transistors and 2D MoS2 phototransistors. The maximum photoresponsivity (Rph) of the bilayer MoS2 phototransistors in an 8 × 8 active pixel image sensor array is statistically measured as high as 119.16 A W−1. With the aid of computational modeling, we find that the main mechanism for the high Rph of the bilayer MoS2 phototransistor is a photo-gating effect by the holes trapped at subgap states. The image-sensing characteristics of the bilayer MoS2 active pixel image sensor array are successfully investigated using light stencil projection.

Yu-Shiba-Rusinov states and ordering of magnetic impurities near the boundary of a superconducting nanowire

We theoretically study the spectrum induced by one and two magnetic impurities near the boundary of a one-dimensional nanowire in proximity to a conventional $s$-wave superconductor and extract the ground state magnetic configuration. We show that the energies of the subgap states, supported by the magnetic impurities, are strongly affected by the boundary for distances less than the superconducting coherence length. In particular, when the impurity is moved towards the boundary, multiple quantum phase transitions periodically occur in which the parity of the superconducting condensate oscillates between even and odd. We find that the magnetic ground state configuration of two magnetic impurities depends not only on the distance between them but also explicitly on their distance away from the boundary of the nanowire. As a consequence, the magnetic ground state can switch from ferromagnetic to antiferromagnetic while keeping the inter-impurity distance unaltered by simultaneously moving both impurities away from the boundary. The ground state magnetic configuration of two impurities is found analytically in the weak coupling regime and exactly for an arbitrary impurity coupling strength using numerical tight-binding simulations.

Quasiparticle Poisoning of Majorana Qubits.

Qubits based on Majorana zero modes are a promising path towards topological quantum computing. Such qubits, though, are susceptible to quasiparticle poisoning which does not have to be small by topological argument. We study the main sources of the quasiparticle poisoning relevant for realistic devices-nonequilibrium above-gap quasiparticles and equilibrium localized subgap states. Depending on the parameters of the system and the architecture of the qubit either of these sources can dominate the qubit decoherence. However, we find in contrast to naive estimates that in moderately disordered, floating Majorana islands the quasiparticle poisoning can have timescales exceeding seconds.

Resolving the mechanism of oxygen vacancy mediated nonradiative charge recombination in monoclinic bismuth vanadate

We report ab initio time-domain simulations of nonradiative electron-hole recombination in bismuth vanadate (BiVO4). Nonadiabatic molecular dynamics (NA-MD) simulation results demonstrate that the charge recombination in BiVO4 is greatly enhanced by a factor of ~50 after an oxygen vacancy introduced. Oxygen vacancy introduces a sub-gap state close to conduction band (CB) and capable of trapping holes, which in turn rapidly recombine with CB electrons for large transition rate. This is the first report on the excited states dynamics of BiVO4 and provide design principle for achieving high-efficiency light-harvesting devices based on BiVO4 and other transition metal oxides materials.

Depairing Current Density in a Nutshell

Microscopic theory of the depairing current density (jd) is briefly reviewed for the applied-superconductivity communities. The goal of this article is to introduce the Kupriyanov-Lukichev-Maki theory of jd for s-wave superconductors in the diffusive limit, which is the most reliable calculation of jd based on the BCS theory and is relevant to various superconducting devices. The effect of subgap states on jd is also discussed.

Two-level systems in superconducting quantum devices due to trapped quasiparticles.

A major issue for the implementation of large-scale superconducting quantum circuits is the interaction with interfacial two-level system (TLS) defects that lead to qubit parameter fluctuations and relaxation. Another major challenge comes from nonequilibrium quasiparticles (QPs) that result in qubit relaxation and dephasing. Here, we reveal a previously unexplored decoherence mechanism in the form of a new type of TLS originating from trapped QPs, which can induce qubit relaxation. Using spectral, temporal, thermal, and magnetic field mapping of TLS-induced fluctuations in frequency tunable resonators, we identify a highly coherent subset of the general TLS population with a low reconfiguration temperature ∼300 mK and a nonuniform density of states. These properties can be understood if the TLS are formed by QPs trapped in shallow subgap states formed by spatial fluctutations of the superconducting order parameter. This implies that even very rare QP bursts will affect coherence over exponentially long time scales.

Influence of superconductivity on the magnetic moment of quantum impurity embedded in BCS superconductor

We study the influence of superconductivity on the formation of the localized magnetic moment for a single-level quantum impurity embedded in an s-wave Bardeen–Cooper–Schrieffer (BCS) superconducting medium, modeled by single-impurity Anderson Hamiltonian. We have combined Bogoliubov transformation with Green’s function method within self-consistent Hartree–Fock mean field approximation to analyze the conditions necessary in metal (in the superconducting) for the formation of the magnetic moment at the impurity site for the low-frequency limit |ω| ≪ Δsc as well as for the finite superconducting gap Δsc. We have compared these results with other theoretical results and with the single-level quantum impurity embedded in the normal metallic host. Further, we analyze the spectral density of the quantum impurity embedded in a superconducting host to study the sub-gap states as a function of impurity parameters.

Elucidating the Influence of Sulfur Vacancies on Nonradiative Recombination Dynamics in Cu2ZnSnS4 Solar Absorbers.

We report a time-domain ab initio simulation of charge carrier trapping and relaxation dynamics in pristine and defect-containing kesterite Cu2ZnSnS4 (CZTS) structures. Our simulations show that introduction of a neutral sulfur vacancy in the CZTS system leads to a decrease of the charge recombination rate by a factor of ∼4, and the doubly positively charged sulfur vacancy results in a minor decrease of carrier lifetime, as compared to the pristine CZTS system. The neutral sulfur vacancy weakens the nonadiabatic (NA) electron-phonon coupling by moderately localizing charge density and accelerates the pure dephasing process, extending charge carrier lifetime. Therefore, the neutral sulfur vacancy is electrically benign. The doubly positively charged sulfur vacancy introduces a subgap state which is hardly populated, and recombination of the electron and hole bypassing the trap state dominates. As a result, the recombination rate decreases in the doubly charged sulfur vacancy structure. The reported results identified the key role of the sulfur-related vacancy on charge carrier trapping and relaxation of CZTS materials, carrying important implications for further optimization of CZTS and other thin-film solar cell materials.

Anomalous Hall effect in single-band chiral superconductors from impurity superlattices

Unlike anomalous quantum Hall insulators, clean single-band chiral superconductors do not exhibit intrinsic Hall effect at the one-loop approximation. Finite ac Hall conductance was found to emerge beyond one-loop, such as with vertex corrections associated with extrinsic random impurity scatterings. In this paper, we investigate the effect of impurities embedded in single-band chiral superconductors in a superlattice pattern, instead of in random distributions. The impurity-induced Bogoliubov quasiparticle bound states hybridize to form subgap bands, constituting an emergent low-energy effective theory whose Hall effect can be studied with ease. We demonstrate that the occurrence of the Hall effect depends on the superlattice geometry and on the parity of the chiral pairing. In particular, due to the mixed particle-hole character of the subgap states, the Hall conductance may arise at the one-loop level of the current-current correlator in our effective model. Our theory provides a new insight into the impurity-induced anomalous Hall effect in chiral superconductors.

Hard-Gap Spectroscopy in a Self-Defined MesoscopicInAs/AlNanowire Josephson Junction

Superconductor/semiconductor-nanowire hybrid structures can serve as versatile building blocks to realize Majorana circuits or superconducting qubits based on quantized levels such as Andreev qubits. For all these applications it is essential that the superconductor-semiconductor interface is as clean as possible. Furthermore, the shape and dimensions of the superconducting electrodes needs to be precisely controlled. We fabricated self-defined InAs/Al core/shell nanowire junctions by a fully in-situ approach, which meet all these criteria. Transmission electron microscopy measurements confirm the sharp and clean interface between the nanowire and the in-situ deposited Al electrodes which were formed by means of shadow evaporation. Furthermore, we report on tunnel spectroscopy, gate and magnetic field-dependent transport measurements. The achievable short junction lengths,the observed hard-gap and the magnetic field robustness make this new hybrid structure very attractive for applications which rely on a precise control of the number of sub-gap states, like Andreev qubits or topological systems.

Charge-generating mid-gap trap states define the thermodynamic limit of organic photovoltaic devices

Detailed balance is a cornerstone of our understanding of artificial light-harvesting systems. For next generation organic solar cells, this involves intermolecular charge-transfer (CT) states whose energies set the maximum open circuit voltage VOC. We have directly observed sub-gap states significantly lower in energy than the CT states in the external quantum efficiency spectra of a significant number of organic semiconductor blends. Taking these states into account and using the principle of reciprocity between emission and absorption results in non-physical radiative limits for the VOC. We propose and provide compelling evidence for these states being non-equilibrium mid-gap traps which contribute to photocurrent by a non-linear process of optical release, upconverting them to the CT state. This motivates the implementation of a two-diode model which is often used in emissive inorganic semiconductors. The model accurately describes the dark current, VOC and the long-debated ideality factor in organic solar cells. Additionally, the charge-generating mid-gap traps have important consequences for our current understanding of both solar cells and photodiodes – in the latter case defining a detectivity limit several orders of magnitude lower than previously thought.

Superconductivity in La2Ni2In

We report here the properties of single crystals of La$_2$Ni$_2$In. Electrical resistivity and specific heat measurements concur with the results of Density Functional Theory (DFT) calculations, finding that La$_{2}$Ni$_{2}$In is a weakly correlated metal, where the Ni magnetism is almost completely quenched, leaving only a weak Stoner enhancement of the density of states. Superconductivity is observed at temperatures below 0.9$\,$K. A detailed analysis of the field and temperature dependencies of the resistivity, magnetic susceptibility, and specific heat at the lowest temperatures reveals that La$_2$Ni$_2$In is a dirty type-II superconductor with likely s-wave gap symmetry. Nanoclusters of ferromagnetic inclusions significantly affect the subgap states resulting in a non-exponential temperature dependence of the specific heat $C(T)$ at $T\ll T_\text{c}$.

Defect/Interface Recombination Limited Quasi-Fermi Level Splitting and Open-Circuit Voltage in Mono- and Triple-Cation Perovskite Solar Cells.

Multication metal-halide perovskites exhibit desirable performance and stability, compared to their monocation counterparts. However, the study of the photophysical properties and the nature of defect states in these materials is still a challenging and ongoing task. Here, we study bulk and interfacial energy loss mechanisms in solution-processed MAPbI3 (MAPI) and (CsPbI3)0.05[(FAPbI3)0.83(MAPbBr3)0.17]0.95 (triple cation) perovskite solar cells using absolute photoluminescence (PL) measurements. In neat MAPI films, we find a significantly smaller quasi-Fermi level splitting than for the triple cation perovskite absorbers, which defines the open-circuit voltage of the MAPI cells. PL measurements at low temperatures (∼20 K) on MAPI films demonstrate that emissive subgap states can be effectively reduced using different passivating agents, which lowers the nonradiative recombination loss at room temperature. We conclude that while triple cation perovskite cells are limited by interfacial recombination, the passivation of surface trap states within the MAPI films is the primary consideration for device optimization.

Photon-assisted resonant Andreev reflections: Yu-Shiba-Rusinov and Majorana states

Photon-assisted tunneling frequently provides detailed information on the underlying charge-transfer process. In particular, the Tien-Gordon approach and its extensions predict that the sideband spacing in bias voltage is a direct fingerprint of the number of electrons transferred in a single tunneling event. Here, we analyze photon-assisted tunneling into subgap states in superconductors in the limit of small temperatures and bias voltages where tunneling is dominated by resonant Andreev processes and does not conform to the predictions of simple Tien-Gordon theory. Our analysis is based on a systematic Keldysh calculation of the subgap conductance and provides a detailed analytical understanding of photon-assisted tunneling into subgap states, in excellent agreement with a recent experiment. We focus on tunneling from superconducting electrodes and into Yu-Shiba-Rusinov states associated with magnetic impurities or adatoms, but we also explicitly extend our results to include normal-metal electrodes or other types of subgap states in superconductors. In particular, we argue that photon-assisted Andreev reflections provide a high-accuracy method to measure small, but nonzero energies of subgap states which can be important for distinguishing conventional subgap states from Majorana bound states.