Electrically controlled emission from singlet and triplet exciton species in atomically thin light emitting diodes
Andrew Y. Joe, Luis A. Jauregui, Kateryna Pistunova, Andrés M. Mier Valdivia, Zhengguang Lu, Dominik S. Wild, Giovanni Scuri, Kristiaan De Greve, Ryan J. Gelly,… 展开作者
Andrew Y. Joe, Luis A. Jauregui, Kateryna Pistunova, Andrés M. Mier Valdivia, Zhengguang Lu, Dominik S. Wild, Giovanni Scuri, Kristiaan De Greve, Ryan J. Gelly, You Zhou, Jiho Sung, Andrey Sushko, Takashi Taniguchi, Kenji Watanabe, Dmitry Smirnov, Mikhail D. Lukin, Hongkun Park, Philip Kim
Excitons are composite bosons that can feature spin singlet and triplet states. In usual semiconductors, without an additional spin-flip mechanism, triplet excitons are extremely inefficient optical emitters. Transition metal dichalcogenides (TMDs), with their large spin-orbit coupling, have been of special interest for valleytronic applications for their coupling of circularly polarized light to excitons with selective valley and spin$^{1-4}$. In atomically thin MoSe$_2$/WSe$_2$ TMD van der Waals (vdW) heterostructures, the unique atomic registry of vdW layers provides a quasi-angular momentum to interlayer excitons$^{5,6}$, enabling emission from otherwise dark spin triplet excitons. Here, we report electrically tunable spin singlet and triplet exciton emission from atomically aligned TMD heterostructures. We confirm the spin configurations of the light-emitting excitons employing magnetic fields to measure effective exciton g-factors. The interlayer tunneling current across the TMD vdW heterostructure enables the electrical generation of singlet and triplet exciton emission in this atomically thin PN junction. We demonstrate electrically tunability between the singlet and triplet excitons that are generated by charge injection. Atomically thin TMD heterostructure light emitting diodes thus enables a route for optoelectronic devices that can configure spin and valley quantum states independently by controlling the atomic stacking registry.
The p-n diodes represent the most fundamental device building block for diverse optoelectronic functions, but are difficult to achieve in atomically thin transition metal dichalcogenides (TMDs) due to the inability to selectively dope them into p- or n-type semiconductors. Here we report the first demonstration of an atomically thin and atomically sharp heterojunction p-n diode by vertically stacking p-type monolayer tungsten diselenide (WSe2) and n-type few-layer molybdenum disulfide (MoS2). Electrical measurement demonstrates excellent diode characteristics with well-defined current rectific…
We have studied the current through a carbon nanotube quantum dot with one ferromagnetic and one normal-metal lead. For the values of gate voltage at which the normal lead is resonant with the single available non-degenerate energy level on the dot, we observe a pronounced decrease in the current for one bias direction. We show that this rectification is spin-dependent, and that it stems from the interplay between the spin accumulation and the Coulomb blockade on the quantum dot. Our results imply that the current is spin-polarized for one direction of the bias, and that the degree of spin pol…
Transition metal dichalcogenides (TMDs) are optically active layered materials providing potential for fast optoelectronics and on-chip photonics. We demonstrate electrically driven single-photon emission from localised sites in tungsten diselenide (WSe2) and tungsten disulphide (WS2). To achieve this, we fabricate a light emitting diode structure comprising single layer graphene, thin hexagonal boron nitride and TMD mono- and bi-layers. Photon correlation measurements are used to confirm the single-photon nature of the spectrally sharp emission. These results present the TMD family as a platf…
Excitons are composite bosons that can feature spin singlet and triplet states. In usual semiconductors, without an additional spin-flip mechanism, triplet excitons are extremely inefficient optical emitters. Large spin-orbit coupling in transition metal dichalcogenides (TMDs) couples circularly polarized light to excitons with selective valley and spin. Here, we demonstrate electrically controlled brightening of spin-triplet interlayer excitons in a MoSe$_2$/WSe$_2$ TMD van der Waals (vdW) heterostructure. The atomic registry of vdW layers in TMD heterostructures provides a quasi-angular mome…
Semiconductor heterostructures form the cornerstone of many electronic and optoelectronic devices and are traditionally fabricated using epitaxial growth techniques. More recently, heterostructures have also been obtained by vertical stacking of two-dimensional crystals, such as graphene and related two- dimensional materials. These layered designer materials are held together by van der Waals forces and contain atomically sharp interfaces. Here, we report on a type- II van der Waals heterojunction made of molybdenum disulfide and tungsten diselenide monolayers. The junction is electrically tu…
One of the most fundamental devices for electronics and optoelectronics is the PN junction, which provides the functional element of diodes, bipolar transistors, photodetectors, LEDs, and solar cells, among many other devices. In conventional PN junctions, the adjacent p- and n-type regions of a semiconductor are formed by chemical doping. Materials with ambipolar conductance, however, allow for PN junctions to be configured and modified by electrostatic gating. This electrical control enables a single device to have multiple functionalities. Here we report ambipolar monolayer WSe2 devices in …
We report single-photon emission from electrically driven site-controlled InGaN/GaN quantum dots, fabricated from a planar light-emitting diode structure containing a single InGaN quantum well using a top-down approach. The location, dimension, and height of each single-photon-emitting diode are controlled lithographically, providing great flexibility for chip-scale integration.
We show how to increase the capacitance of super-capacitors by modifying the otherwise passive separator layer and turn it into an active diode-like structure. We demonstrate 15% capacitance increase for a diode-like separators without a bias. Additional 15% capacitance increase has been observed for biased separators.
Compact and electrically controllable on-chip sources of indistinguishable photons are desirable for the development of integrated quantum technologies. We demonstrate that two quantum dot light emitting diodes (LEDs) in close proximity on a single chip can function as a tunable, all-electric quantum light source. Light emitted by an electrically excited driving LED is used to excite quantum dots the neighbouring diode. The wavelength of the quantum dot emission from the neighbouring driven diode is tuned via the quantum confined Stark effect. We also show that we can electrically tune the fin…
Electrically-driven light emission from carbon nanotubes could be exploited in nano-scale lasers and single-photon sources, and has therefore been the focus of much research. However, to date, high electric fields and currents have been either required for electroluminescence, or have been an undesired side effect, leading to high power requirements and low efficiencies. In addition, electroluminescent linewidths have been broad enough to obscure the contributions of individual optical transitions. Here, we report electrically-induced light emission from individual carbon nanotube p-n diodes. …
Nanoscale electrothermal-switch superconducting diode for electrically programmable superconducting circuits
Nanjing University（南京大学）；Purple Mountain Laboratories（紫金山实验室）；Zhejiang University（浙江大学）；Nanjing University of Science and Technology（南京理工大学）；State Key Laboratory of Spintronics Devices and Technologies, Nanjing University（南京大学自旋电子学器件与技术国家重点实验室）
Light-emitting diodes are of importance for lighting, displays, optical interconnects, logic and sensors. Hence the development of new systems that allow improvements in their efficiency, spectral properties, compactness and integrability could have significant ramifications. Monolayer transition metal dichalcogenides have recently emerged as interesting candidates for optoelectronic applications due to their unique optical properties. Electroluminescence has already been observed from monolayer MoS2 devices. However, the electroluminescence efficiency was low and the linewidth broad due both …
Two-dimensional semiconductors have emerged as a new class of materials for nanophotonics for their strong exciton-photon interaction and flexibility for engineering and integration. Taking advantage of these properties, we engineer an efficient lasing medium based on dipolar interlayer excitons, in rotationally aligned atomically thin heterostructures. Lasing is measured from a transition metal dichalcogenide hetero-bilayer integrated in a silicon nitride grating resonator. A sharp increase in the spatial coherence of the emission was observed across the lasing threshold. The work establishes…
Atomically-thin 2D semiconducting materials integrated into van der Waals heterostructures have enabled architectures that hold great promise for next generation nanoelectronics. However, challenges still remain to enable their full acceptance as compliant materials for integration in logic devices. Two key-components to master are the barriers at metal/semiconductor interfaces and the mobility of the semiconducting channel, which endow the building-blocks of ${pn}$ diode and field effect transistor. Here, we have devised a reverted stacking technique to intercalate a wrinkle-free h-BN tunnel …
Two-dimensional (2D) atomic crystals, such as graphene and atomically thin transition metal dichalcogenides (TMDCs), are currently receiving a lot of attention. They are crystalline, and thus of high material quality, even so, they can be produced in large areas and are bendable, thus providing opportunities for novel applications. Here, we report a truly 2D p-n junction diode, based on an electrostatically doped tungsten diselenide (WSe2) monolayer. As p-n diodes are the basic building block in a wide variety of optoelectronic devices, our demonstration constitutes an important advance toward…
Recent developments in fabrication of van der Waals heterostructures enable new type of devices assembled by stacking atomically thin layers of two-dimensional materials. Using this approach, we fabricate light-emitting devices based on a monolayer WSe$_2$, and also comprising boron nitride tunnelling barriers and graphene electrodes, and observe sharp luminescence spectra from individual defects in WSe$_2$ under both optical and electrical excitation. This paves the way towards the realization of electrically-pumped quantum emitters in atomically thin semiconductors. In addition we demonstrat…
We demonstrate the first wavelength-tunable electrically-pumped source of non-classical light that can emit photons with wavelength in resonance with the D2 transitions of 87Rb atoms. The device is fabricated by integrating a novel GaAs single-quantum-dot light-emitting-diode (LED) onto a piezoelectric actuator. By feeding the emitted photons into a 75-mm-long cell containing warm 87Rb atom vapor, we observe slow-light with a temporal delay of up to 3.4 ns. In view of the possibility of using 87Rb atomic vapors as quantum memories, this work makes an important step towards the realization of h…
We report on the fabrication and transport characterization of atomically-precise single molecule devices consisting of a magnetic porphyrin covalently wired by graphene nanoribbon electrodes. The tip of a scanning tunneling microscope was utilized to contact the end of a GNR-porphyrin-GNR hybrid system and create a molecular bridge between tip and sample for transport measurements. Electrons tunneling through the suspended molecular heterostructure excited the spin multiplet of the magnetic porphyrin. The detachment of certain spin-centers from the surface shifted their spin-carrying orbitals…
We propose a semiconductor device that can electrically generate entangled electron spin-photon states, providing a building block for entanglement of distant spins. The device consists of a p-i-n diode structure that incorporates a coupled double quantum dot. We show that electronic control of the diode bias and local gating allow for the generation of single photons that are entangled with a robust quantum memory based on the electron spins. Practical performance of this approach to controlled spin-photon entanglement is analyzed.
The role of polariton-electron scattering on the performance characteristics of an electrically injected GaAs-based quantum well microcavity diode in the strong coupling regime has been investigated. An electron gas is introduced in the quantum wells by modulation doping with silicon dopants. It is observed that polariton-electron scattering suppresses the relaxation bottleneck in the lower polariton branch. However, it is not adequate to produce a degenerate coherent condensate at k|| ~ 0 and coherent emission.
High energy resolution spectroscopic studies of quantum magnets have proven to be extremely valuable in directly accessing magnetodynamics quantities, such as energy barriers, magnetic interactions, lifetime of excited states and fluctuations at the most fundamental level. Here, we explore the existence of a new flavor of low-energy spin-excitations for quantum spins coupled to an electron bath. In sharp contrast to the usual tunneling signature of two steps symmetrically centered around the Fermi level, we find a single step in the conductance. Combining time-dependent and many-body perturbat…
We describe a new means for electrically creating spin polarization in semiconductors. In contrast to spin injection of electrons by tunneling through a reverse-biased Schottky barrier, we observe spin accumulation at the metal/semiconductor interface of forward-biased ferromagnetic Schottky diodes, which is consistent with a theory of spin-dependent reflection off the interface. Spatiotemporal Kerr microscopy is used to image the electron spin and the resulting dynamic nuclear polarization that arises from the non equilibrium carrier polarization.
Semiconductor p-n junctions are essential building blocks for modern electronics and optoelectronics. In conventional semiconductors, a p-n junction produces depletion regions of free charge carriers at equilibrium and built-in potentials associated with uncompensated dopant atoms. Carrier transport across the junction occurs by diffusion and drift processes defined by the spatial extent of this region. With the advent of atomically thin van der Waals (vdW) materials and their heterostructures, we are now able to realize a p-n junction at the ultimate quantum limit. In particular, vdW junction…
The advent of graphene and related 2D materials has recently led to a new technology: heterostructures based on these atomically thin crystals. The paradigm proved itself extremely versatile and led to rapid demonstration of tunnelling diodes with negative differential resistance, tunnelling transistors5, photovoltaic devices, etc. Here we take the complexity and functionality of such van der Waals heterostructures to the next level by introducing quantum wells (QWs) engineered with one atomic plane precision. We describe light emitting diodes (LEDs) made by stacking up metallic graphene, insu…
The heteroepitaxy of III-V semiconductors on silicon is a promising approach for making silicon a photonic platform for on-chip optical interconnects and quantum optical applications. Monolithic integration of both material systems is a long-time challenge, since different material properties lead to high defect densities in the epitaxial layers. In recent years, nanostructures however have shown to be suitable for successfully realising light emitters on silicon, taking advantage of their geometry. Facet edges and sidewalls can minimise or eliminate the formation of dislocations, and due to t…
Optical quantum emitters are a key component of quantum devices for metrology and information processing. In particular, atomic defects in 2D materials can operate as optical quantum emitters that overcome current limitations of conventional bulk emitters, such as yielding a high single-photon generation rate and offering surface accessibility for excitation and photon extraction. Here we demonstrate electrically stimulated photon emission from individual point defects in a 2D material. Specifically, by bringing a metallic tip into close proximity to a discrete defect state in the band gap of …
We show that thin film diode structures, such as photovoltaics and light emitting arrays, can undergo zero threshold localized thermal runaway leading to thermal and electrical nonuniformities spontaneously emerging in originally uniform systems. The linear stability analysis is developed for a system of thermally and electrically coupled two discrete diodes, and for a distributed system. These results are verified with numerical modeling that is not limited to small fluctuations. The discovered instability negatively affects the device performance and reliability. It follows that these proble…
Atomically thin boron nitride (BN) nanosheets have many properties desirable for surface enhanced Raman spectroscopy (SERS). BN nanosheets have a strong surface adsorption capability towards airborne hydrocarbon and aromatic molecules. For maximized adsorption area and hence SERS sensitivity, atomically thin BN nanosheet covered gold nanoparticles have been prepared for the first time. When placed on top of metal nanoparticles, atomically thin BN nanosheets closely follow their contours so that the plasmonic hot spots are retained. Electrically insulating BN nanosheets also act as a barrier la…
Two-dimensional dilute magnetic semiconductors can provide fundamental insights in the very nature of magnetic orders and their manipulation through electron and hole doping. Despite the fundamental physics, due to the large charge density control capability in these materials, they can be extremely important in spintronics applications such as spin valve and spin-based transistors. In this article, we studied a two-dimensional dilute magnetic semiconductors consisting of phosphorene monolayer doped with cobalt atoms in substitutional and interstitial defects. We show that these defects can be…
Quantifying the spin-spin interactions which influence electronic transitions in organic semiconductors is crucial for understanding their magneto-optoelectronic properties. By combining a theoretical model for three spin interactions in the coherent regime with pulsed electrically detected magnetic resonance experiments on MEH-PPV diodes, we quantify the spin-coupling within complexes comprising three spin-half particles. We determine that these particles form triplet-exciton:polaron pairs, where the polaron:exciton exchange is over 5 orders of magnitude weaker (less than 170 MHz) than that w…
Understanding of the electroluminescence (EL) mechanism in optoelectronic devices is important for further optimization of their efficiency and effectiveness. Here, a quantum mechanical approach is formulated for modeling EL processes in nanoscale light emitting diodes (LED). Based on nonequilibrium Green's function quantum transport equations, interactions with electromagnetic vacuum environment is included to describe electrically driven light emission in the devices. Numerical studies of a silicon nanowire LED device are presented. EL spectra of the nanowire device under different bias volt…
Compared to monolayer graphene, electrons in Bernal-stacked bilayer graphene (BLG) have an additional layer degree of freedom, offering a platform for developing {\it layered spintronics} with the help of proximity-induced magnetism. Based on an effective phenomenological model, we systematically study the effect of this magnetism on the spin-dependent band structure near the Fermi energy and identify the magnetic phases induced in BLG by proximity with magnets. We show that spin polarization can develop in BLG due to this proximity effect. This spin polarization depends strongly on the layer …
Graphene and related two-dimensional materials are promising candidates for atomically thin, flexible, and transparent optoelectronics. In particular, the strong light-matter interaction in graphene has allowed for the development of state-of-the-art photodetectors, optical modulators, and plasmonic devices. In addition, electrically biased graphene on SiO2 substrates can be used as a low-efficiency emitter in the mid-infrared range. However, emission in the visible range has remained elusive. Here we report the observation of bright visible-light emission from electrically biased suspended gr…
Advent of new materials such as van der Waals heterostructures, propels new research directions in condensed matter physics and enables development of novel devices with unique functionalities. Here, we show experimentally that a monolayer of MoSe2 embedded in a charge controlled heterostructure can be used to realize an electrically tunable atomically-thin mirror, that effects 90% extinction of an incident field that is resonant with its exciton transition. The corresponding maximum reflection coefficient of 45% is only limited by the ratio of the radiative decay rate to the linewidth of exci…
In the present study, we developed a fabrication process of an electrically driven single-photon LED based on InP QDs emitting in the red spectral range, the wavelength of interest coinciding with the high efficiency window of Si APDs. A deterministic lithography technique allowed for the pre-selection of a suitable QD, here exclusively operated under electrical carrier injection. The final device was characterized under micro-electroluminescence in direct current, as well as in pulsed excitation mode. In particular, under pulsed excitation of one device, single-photon emission of a spectral l…
Quantum confinement in atomically-thin TMDCs enables the realization of deterministic single-photon emitters. The position and polarization control of single photons have been achieved via local strain engineering using nanostructures. However, most existing TMDC-based emitters are operated by optical pumping, while the emission sites in electrically pumped emitters are uncontrolled. Here, we demonstrate electrically driven single-photon emitters located at the positions where strains are induced by atomic-force-microscope indentation on a van der Waals heterostructure consisting of graphene, …
Boosting the sensitivity of solid-state gas sensors by incorporating nanostructured materials as the active sensing element can be complicated by interfacial effects. Interfaces at nanoparticles, grains, or contacts may result in non-linear current-voltage response, high electrical resistance, and ultimately, electric noise that limits the sensor read-out. Here we report the possibility to prepare nominally one atom thin, electrically continuous metals, by straightforward physical vapor deposition on the carbon zero-layer grown epitaxially on silicon carbide. With platinum as the metal, its el…
We report the room-temperature electroluminescence (EL) with nearly pure circular polarization (CP) from GaAs-based spin-polarized light-emitting diodes (spin-LEDs). External magnetic fields are not used during device operation. There are two small schemes in the tested spin-LEDs: firstly, the stripe-laser-like structure that helps intensifying the EL light at the cleaved side walls below the spin injector Fe slab, and secondly, the crystalline AlOx spin tunnel barrier that ensures electrically stable device operation. The purity of CP is depressively low in the low current density (J) region,…
Entangled light emitting diodes based on semiconductor quantum dots are promising devices for security sensitive quantum network applications, thanks to their natural lack of multi photon-pair generation. Apart from telecom wavelength emission, network integrability of these sources ideally requires electrical operation for deployment in compact systems in the field. For multiplexing of entangled photons with classical data traffic, emission in the telecom O-band and tuneability to the nearest wavelength channel in compliance with coarse wavelength division multiplexing standards (20 nm channe…
Atomically thin two dimensional (2D) layered materials have emerged as a new class of material for nanoelectromechanical systems (NEMS) due to their extraordinary mechanical properties and ultralow mass density. Among them, graphene has been the material of choice for nanomechanical resonator. However, recent interest in 2D chalcogenide compounds has also spurred research in using materials such as MoS2 for NEMS applications. As the dimensions of devices fabricated using these materials shrink down to atomically thin membrane, strain and nonlinear effects have become important. A clear underst…
Two-dimensional (2D) semiconductors provide a unique opportunity for optoelectronics due to their layered atomic structure, electronic and optical properties. To date, a majority of the application-oriented research in this field has been focused on field-effect electronics as well as photodetectors and light emitting diodes. Here we present a perspective on the use of 2D semiconductors for photovoltaic applications. We discuss photonic device designs that enable light trapping in nanometer-thickness absorber layers, and we also outline schemes for efficient carrier transport and collection. W…
Transition metal dichalcogenide monolayers are promising candidates for exploring new electronic and optical phenomena and for realizing atomically thin optoelectronic devices. They host tightly bound electron-hole pairs (excitons) that can be efficiently excited by resonant light fields. Here, we demonstrate that a single monolayer of molybdenum diselenide (MoSe2) can dramatically modify light transmission near the excitonic resonance, acting as an electrically switchable mirror that reflects up to 85% of incident light at cryogenic temperatures. This high reflectance is a direct consequence …
Nonlocal and nonlinear plasmonics in atomically thin heterostructures
University of Southern Denmark（南丹麦大学）；POLIMA—Center for Polariton-driven Light–Matter Interactions, University of Southern Denmark（极化激元驱动光-物质相互作用中心，南丹麦大学）；Danish Institute for Advanced Study, University of Southern Denmark（丹麦高级研究院，南丹麦大学）
We investigate a semiconductor $p$-$n$ junction in contact with superconducting leads that is operated under forward bias as a light-emitting diode. The presence of superconductivity results in a significant increase of the electroluminescence in a certain frequency window. We demonstrate that the tunneling of Cooper pairs induces an additional luminescence peak on resonance. There is a transfer of superconducting to photonic coherence which results in the emission of entangled photon pairs and squeezing of the fluctuations in the quadrature amplitudes of the emitted light. The squeezing angle…
Electromagnetically induced transparency (EIT) is a promising technology for the enhancement of light-matter interactions, and recent demonstrations of the quantum EIT realized in artificial micro-structured medium have remarkably reduced the extreme requirement for experimental observation of EIT spectrum. In this paper, we propose to electrically control the EIT spectrum in a metamaterial for an electromagnetic modulator. A diode acting as a tunable resistor is loaded in the gap of two paired wires to inductively tune the magnetic resonance, which induces remarkable modulation on the EIT spe…
Scalability and foundry compatibility (as for example in conventional silicon based integrated computer processors) in developing quantum technologies are exceptional challenges facing current research. Here we introduce a quantum photonic technology potentially enabling large scale fabrication of semiconductor-based, site-controlled, scalable arrays of electrically driven sources of polarization-entangled photons, with the potential to encode quantum information. The design of the sources is based on quantum dots grown in micron-sized pyramidal recesses along the crystallographic direction (1…
Electrically addressing spin systems is predicted to be a key component in developing scalable semiconductor-based quantum processing architectures, to enable fast spin qubit manipulation and long-distance entanglement via microwave photons. However, single spins have no electric dipole, and therefore a spin-orbit mechanism must be integrated in the qubit design. Here, we propose to couple microwave photons to atomically precise donor spin qubit devices in silicon using the hyperfine interaction intrinsic to donor systems and an electrically-induced spin-orbit coupling. We characterise a one-e…
Van der Waals (vdW) tunnel junctions are attractive due to their atomically sharp interface, gate tunablity, and robustness against lattice mismatch between the successive layers. However, the negative differential resistance (NDR) demonstrated in this class of tunnel diodes often exhibits noisy behaviour with low peak current density, and lacks robustness and repeatability, limiting their practical circuit applications. Here we propose a strategy of using a 1L-WS$_2$ as an optimum tunnel barrier sandwiched in a broken gap tunnel junction of highly doped black phosphorus (BP) and SnSe$_2$. We …
