Fast and accurate detection of light in the near-infrared (NIR) spectral range plays a crucial role in modern society, from alleviating speed and capacity bottlenecks in optical communications to enhancing the control and safety of autonomous vehicles through NIR imaging systems. Several technological platforms are currently under investigation to improve NIR photodetection, aiming to surpass the performance of established III-V semiconductor p-i-n (PIN) junction technology. These platforms include-grown inorganic nanocrystals (NCs) and nanowire arrays, as well as hybrid organic-inorganic materials such as graphene-perovskite heterostructures.
View Article and Find Full Text PDFQuantum effects in nanoscale electronic devices promise to lead to new types of functionality not achievable using classical electronic components. However, quantum behaviour also presents an unresolved challenge facing electronics at the few-nanometre scale: resistive channels start leaking owing to quantum tunnelling. This affects the performance of nanoscale transistors, with direct source-drain tunnelling degrading switching ratios and subthreshold swings, and ultimately limiting operating frequency due to increased static power dissipation.
View Article and Find Full Text PDFGraphene nanoribbons (GNRs), nanometre-wide strips of graphene, are promising materials for fabricating electronic devices. Many GNRs have been reported, yet no scalable strategies are known for synthesizing GNRs with metal atoms and heteroaromatic units at precisely defined positions in the conjugated backbone, which would be valuable for tuning their optical, electronic and magnetic properties. Here we report the solution-phase synthesis of a porphyrin-fused graphene nanoribbon (PGNR).
View Article and Find Full Text PDFWhen designing a molecular electronic device for a specific function, it is necessary to control whether the charge-transport mechanism is phase-coherent transmission or particle-like hopping. Here we report a systematic study of charge transport through single zinc-porphyrin molecules embedded in graphene nanogaps to form transistors, and show that the transport mechanism depends on the chemistry of the molecule-electrode interfaces. We show that van der Waals interactions between molecular anchoring groups and graphene yield transport characteristic of Coulomb blockade with incoherent sequential hopping, whereas covalent molecule-electrode amide bonds give intermediately or strongly coupled single-molecule devices that display coherent transmission.
View Article and Find Full Text PDFSince the early days of quantum mechanics, it has been known that electrons behave simultaneously as particles and waves, and now quantum electronic devices can harness this duality. When devices are shrunk to the molecular scale, it is unclear under what conditions does electron transmission remain phase-coherent, as molecules are usually treated as either scattering or redox centers, without considering the wave-particle duality of the charge carrier. Here, we demonstrate that electron transmission remains phase-coherent in molecular porphyrin nanoribbons connected to graphene electrodes.
View Article and Find Full Text PDFThe outcome of an electron-transfer process is determined by the quantum-mechanical interplay between electronic and vibrational degrees of freedom. Nonequilibrium vibrational dynamics are known to direct electron-transfer mechanisms in molecular systems; however, the structural features of a molecule that lead to certain modes being pushed out of equilibrium are not well understood. Herein, we report on electron transport through a porphyrin dimer molecule, weakly coupled to graphene electrodes, that displays sequential tunneling within the Coulomb-blockade regime.
View Article and Find Full Text PDFMany spintronic devices rely on the presence of spin-polarized currents at zero magnetic field. This is often obtained by spin exchange-bias, where an element with long-range magnetic order creates magnetized states and displaces the hysteresis loop. Here we demonstrate that exchange-split spin states are observable and usable in the smallest conceivable unit: a single magnetic molecule.
View Article and Find Full Text PDFThe 1T polytype of TaS has been studied extensively as a strongly correlated system. As 1T-TaS is thinned toward the 2D limit, its phase diagram shows significant deviations from that of the bulk material. Optoelectronic maps of ultrathin 1T-TaS have indicated the presence of nonequilibrium charge density wave phases within the hysteresis region of the nearly commensurate (NC) to commensurate (C) transition.
View Article and Find Full Text PDFElectron-electron interactions are at the heart of chemistry and understanding how to control them is crucial for the development of molecular-scale electronic devices. Here, we investigate single-electron tunneling through a redox-active edge-fused porphyrin trimer and demonstrate that its transport behavior is well described by the Hubbard dimer model, providing insights into the role of electron-electron interactions in charge transport. In particular, we empirically determine the molecule's on-site and inter-site electron-electron repulsion energies, which are in good agreement with density functional calculations, and establish the molecular electronic structure within various oxidation states.
View Article and Find Full Text PDFConductance signatures that signal the presence of Majorana zero modes in a three terminal nanowire-topological superconductor hybrid system are analyzed in detail, in both the clean nanowire limit and in the presence of non-coherent dephasing interactions. In the coherent transport regime for a clean wire, we point out contributions of the local Andreev reflection and the non-local transmissions toward the total conductance lineshapes while clarifying the role of contact broadening on the Majorana conductance lineshapes at the magnetic field parity crossings. Interestingly, at larger-field parity crossings, the contribution of the Andreev reflection process decreases which is compensated by the non-local processes in order to maintain the conductance quantum regardless of contact coupling strength.
View Article and Find Full Text PDFSignificant advances in the synthesis of low-dimensional materials with unique and tuneable electrical, optical and magnetic properties has led to an explosion of possibilities for realising hybrid nanomaterial devices with unconventional and desirable characteristics. However, the lack of ability to precisely integrate individual nanoparticles into devices at scale limits their technological application. Here, we report on a graphene nanogap based platform which employs the large electric fields generated around the point-like, atomically sharp nanogap electrodes to capture single nanoparticles from solution at predefined locations.
View Article and Find Full Text PDFQuantum phenomena are typically observable at length and time scales smaller than those of our everyday experience, often involving individual particles or excitations. The past few decades have seen a revolution in the ability to structure matter at the nanoscale, and experiments at the single particle level have become commonplace. This has opened wide new avenues for exploring and harnessing quantum mechanical effects in condensed matter.
View Article and Find Full Text PDFOff-resonant charge transport through molecular junctions has been extensively studied since the advent of single-molecule electronics and is now well understood within the framework of the non-interacting Landauer approach. Conversely, gaining a qualitative and quantitative understanding of the resonant transport regime has proven more elusive. Here, we study resonant charge transport through graphene-based zinc-porphyrin junctions.
View Article and Find Full Text PDFThe electronic and magnetic properties of single-molecule transistors depend critically on the molecular charge state. Charge transport in single-molecule transistors is characterized by Coulomb-blocked regions in which the charge state of the molecule is fixed and current is suppressed, separated by high-conductance, sequential-tunneling regions. It is often difficult to assign the charge state of the molecular species in each Coulomb-blocked region due to variability in the work-function of the electrodes.
View Article and Find Full Text PDFThe superconducting proximity effect is probed experimentally in Josephson junctions fabricated with InAs nanowires contacted by Nb leads. Contact transparencies [Formula: see text] are observed. The electronic phase coherence length at low temperatures exceeds the channel length.
View Article and Find Full Text PDFTo exploit a given physical system for quantum information processing, it is critical to understand the different types of noise affecting quantum control. Distinguishing coherent and incoherent errors is extremely useful as they can be reduced in different ways. Coherent errors are generally easier to reduce at the hardware level, e.
View Article and Find Full Text PDFEntanglement, one of the central mysteries of quantum mechanics, plays an essential role in numerous tasks of quantum information science. A natural question of both theoretical and experimental importance is whether universal entanglement detection can be accomplished without full state tomography. In this Letter, we prove a no-go theorem that rules out this possibility for nonadaptive schemes that employ single-copy measurements only.
View Article and Find Full Text PDFSpin systems controlled and probed by magnetic resonance have been valuable for testing the ideas of quantum control and quantum error correction. This paper introduces an X-band pulsed electron spin resonance spectrometer designed for high-fidelity coherent control of electron spins, including a loop-gap resonator for sub-millimeter sized samples with a control bandwidth ∼40MHz. Universal control is achieved by a single-sideband upconversion technique with an I-Q modulator and a 1.
View Article and Find Full Text PDFOne of the major experimental achievements in the past decades is the ability to control quantum systems to high levels of precision. To quantify the level of control we need to characterize the dynamical evolution. Full characterization via quantum process tomography is impractical and often unnecessary.
View Article and Find Full Text PDFEffective electron mobilities are obtained by transport measurements on InAs nanowire field-effect transistors at temperatures ranging from 10 to 200 K. The mobility increases with temperatures below ∼30-50 K, and then decreases with temperatures above 50 K, consistent with other reports. The magnitude and temperature dependence of the observed mobility can be explained by Coulomb scattering from ionized surface states at typical densities.
View Article and Find Full Text PDFMany problems of interest in physics, chemistry and computer science are equivalent to problems defined on systems of interacting spins. However, most such problems require computational resources that are out of reach with classical computers. A promising solution to overcome this challenge is quantum simulation.
View Article and Find Full Text PDFWe demonstrate coherent control of two nuclear spins mediated by the magnetic resonance of a hyperfine-coupled electron spin. This control is used to create a double-nuclear coherence in one of the two electron spin manifolds, starting from an initial thermal state, in direct analogy to the creation of an entangled (Bell) state from an initially pure unentangled state. We identify challenges and potential solutions to obtaining experimental gate fidelities useful for quantum information processing in this type of system.
View Article and Find Full Text PDFWe report the implementation of a 3-qubit quantum error-correction code on a quantum information processor realized by the magnetic resonance of carbon nuclei in a single crystal of malonic acid. The code corrects for phase errors induced on the qubits due to imperfect decoupling of the magnetic environment represented by nearby spins, as well as unwanted evolution under the internal Hamiltonian. We also experimentally demonstrate sufficiently high-fidelity control to implement two rounds of quantum error correction.
View Article and Find Full Text PDFWe report the electrical induction and detection of dynamic nuclear polarization in the spin-blockade regime of double GaAs vertical quantum dots. The nuclear Overhauser field measurement relies on bias voltage control of the interdot spin exchange coupling and measurement of dc current at variable external magnetic fields. The largest Overhauser field observed was about 4 T, corresponding to a nuclear polarization approximately 40% for the electronic g factor typical of these devices, |g*| approximately 0.
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