Showing papers on "Quantum dot published in 2020"

Metal Halide Perovskite Nanocrystals: Synthesis, Post-Synthesis Modifications and Their Optical Properties

Abstract: Metal halide perovskites represent a flourishing area of research, driven by both their potential application in photo-voltaics and optoelectronics, and for the fundamental science underpinning their unique optoelectronic properties. The advent of colloidal methods for the synthesis of halide perovskite nanocrystals has brought to the attention inter-esting aspects of this new type of materials, above all their defect-tolerance. This review aims to provide an updated survey of this fast-moving field, with a main focus on their colloidal synthesis. We examine the chemistry and the ca-pability of different colloidal synthetic routes to control the shape, size and optical properties of the resulting nano-crystals. We also provide an up to date overview of their post-synthesis transformations, and summarize the various so-lution processes aimed at fabricating halide perovskite-based nanocomposites. We then review the fundamental optical properties of halide perovskite nanocrystals, by focusing on their linear optical properties, on the effects of quantum confinement and, then, on the current knowledge of their exciton binding energies. We also discuss the emergence of non-linear phenomena such as multiphoton absorption, biexcitons and carrier multiplication. At last, we provide an outlook in the field, with the most cogent open questions and possible future directions.

Bipolar-shell resurfacing for blue LEDs based on strongly confined perovskite quantum dots

Abstract: Colloidal quantum dot (QD) solids are emerging semiconductors that have been actively explored in fundamental studies of charge transport1 and for applications in optoelectronics2. Forming high-quality QD solids—necessary for device fabrication—requires substitution of the long organic ligands used for synthesis with short ligands that provide increased QD coupling and improved charge transport3. However, in perovskite QDs, the polar solvents used to carry out the ligand exchange decompose the highly ionic perovskites4. Here we report perovskite QD resurfacing to achieve a bipolar shell consisting of an inner anion shell, and an outer shell comprised of cations and polar solvent molecules. The outer shell is electrostatically adsorbed to the negatively charged inner shell. This approach produces strongly confined perovskite QD solids that feature improved carrier mobility (≥0.01 cm2 V−1 s−1) and reduced trap density relative to previously reported low-dimensional perovskites. Blue-emitting QD films exhibit photoluminescence quantum yields exceeding 90%. By exploiting the improved mobility, we have been able to fabricate CsPbBr3 QD-based efficient blue and green light-emitting diodes. Blue devices with reduced trap density have an external quantum efficiency of 12.3%; the green devices achieve an external quantum efficiency of 22%. A solution-based ligand-exchange strategy enables the realization of close-packed quantum dot solid films with near-unity photoluminescence quantum yield and high charge carrier mobility.

Ligand-assisted cation-exchange engineering for high-efficiency colloidal Cs1−xFAxPbI3 quantum dot solar cells with reduced phase segregation

Abstract: The mixed caesium and formamidinium lead triiodide perovskite system (Cs1−xFAxPbI3) in the form of quantum dots (QDs) offers a pathway towards stable perovskite-based photovoltaics and optoelectronics. However, it remains challenging to synthesize such multinary QDs with desirable properties for high-performance QD solar cells (QDSCs). Here we report an effective oleic acid (OA) ligand-assisted cation-exchange strategy that allows controllable synthesis of Cs1−xFAxPbI3 QDs across the whole composition range (x = 0–1), which is inaccessible in large-grain polycrystalline thin films. In an OA-rich environment, the cross-exchange of cations is facilitated, enabling rapid formation of Cs1−xFAxPbI3 QDs with reduced defect density. The hero Cs0.5FA0.5PbI3 QDSC achieves a certified record power conversion efficiency (PCE) of 16.6% with negligible hysteresis. We further demonstrate that the QD devices exhibit substantially enhanced photostability compared with their thin-film counterparts because of suppressed phase segregation, and they retain 94% of the original PCE under continuous 1-sun illumination for 600 h.

Micro-light-emitting diodes with quantum dots in display technology

Abstract: Micro-light-emitting diodes (μ-LEDs) are regarded as the cornerstone of next-generation display technology to meet the personalised demands of advanced applications, such as mobile phones, wearable watches, virtual/augmented reality, micro-projectors and ultrahigh-definition TVs. However, as the LED chip size shrinks to below 20 μm, conventional phosphor colour conversion cannot present sufficient luminance and yield to support high-resolution displays due to the low absorption cross-section. The emergence of quantum dot (QD) materials is expected to fill this gap due to their remarkable photoluminescence, narrow bandwidth emission, colour tuneability, high quantum yield and nanoscale size, providing a powerful full-colour solution for μ-LED displays. Here, we comprehensively review the latest progress concerning the implementation of μ-LEDs and QDs in display technology, including μ-LED design and fabrication, large-scale μ-LED transfer and QD full-colour strategy. Outlooks on QD stability, patterning and deposition and challenges of μ-LED displays are also provided. Finally, we discuss the advanced applications of QD-based μ-LED displays, showing the bright future of this technology. Micrometre-sized light-emitting diodes (LEDs) based on quantum dots (QDs) will propel the next generation of display technologies, a review by leading researchers shows. Conventional LED designs, with phosphor coatings that convert light to different colours, are difficult to make smaller than 20 micrometres. Jr-Hau He at City University of Hong Kong and co-workers explain how this problem can be tackled using QDs, tiny particles whose optical properties can be tuned by varying their size, providing brighter and more precise colours. Ultra-high-resolution displays based on phospholuminescent QD-LEDs are now being released to the market thanks to finely-controlled methods for synthesising QDs and depositing them onto films. Further research should focus on the best ways to stabilise and protect QD films within LEDs, and to continue developing electroluminescent QD-LEDs, which could potentially outperform their phospholuminescent cousins.

1D porous tubular g-C3N4 capture black phosphorus quantum dots as 1D/0D metal-free photocatalysts for oxytetracycline hydrochloride degradation and hexavalent chromium reduction

Abstract: As an "up-and-coming" two-dimensional (2D) material, black phosphorus (BP) has attracted much attention due to its abundant metal-free properties and broad application prospects in photocatalysis. This study introduces a promising sunlight-driven metal-free photocatalyst for oxytetracycline hydrochloride degradation and hexavalent chromium reduction in water and wastewater. The roles of BP quantum dots (BPQDs) in the distribution of electrons and photocatalytic performances were well identified by experimental and density functional theory (DFT) calculations. As expected, the specially designed 0D/1D structure shows unusual photocatalytic efficiency toward the degradation of oxytetracycline hydrochloride (0.0276 min−1) and reduction of hexavalent chromium (0.0404 min−1). Reactive species, namely, O2− and h+ comprised the primary photocatalytic mechanisms for oxytetracycline hydrochloride degradation. This work highlights that the combination of tubular g-C3N4 (TCN) with BPQDs facilitates the charge spatial separation in the photocatalytic process, and provides alternative strategy for design of highly active and metal-free nanomaterials toward environmental remediation and sustainable solar-to-chemical energy conversion.

Full-color fluorescent carbon quantum dots

Abstract: Quantum dots have innate advantages as the key component of optoelectronic devices. For white light-emitting diodes (WLEDs), the modulation of the spectrum and color of the device often involves various quantum dots of different emission wavelengths. Here, we fabricate a series of carbon quantum dots (CQDs) through a scalable acid reagent engineering strategy. The growing electron-withdrawing groups on the surface of CQDs that originated from acid reagents boost their photoluminescence wavelength red shift and raise their particle sizes, elucidating the quantum size effect. These CQDs emit bright and remarkably stable full-color fluorescence ranging from blue to red light and even white light. Full-color emissive polymer films and all types of high-color rendering index WLEDs are synthesized by mixing multiple kinds of CQDs in appropriate ratios. The universal electron-donating/withdrawing group engineering approach for synthesizing tunable emissive CQDs will facilitate the progress of carbon-based luminescent materials for manufacturing forward-looking films and devices.

Efficient and stable blue quantum dot light-emitting diode.

Abstract: The visualization of accurate colour information using quantum dots has been explored for decades, and commercial products employing environmentally friendly materials are currently available as backlights1. However, next-generation electroluminescent displays based on quantum dots require the development of an efficient and stable cadmium-free blue-light-emitting device, which has remained a challenge because of the inferior photophysical properties of blue-light-emitting materials2,3. Here we present the synthesis of ZnSe-based blue-light-emitting quantum dots with a quantum yield of unity. We found that hydrofluoric acid and zinc chloride additives are effective at enhancing luminescence efficiency by eliminating stacking faults in the ZnSe crystalline structure. In addition, chloride passivation through liquid or solid ligand exchange leads to slow radiative recombination, high thermal stability and efficient charge-transport properties. We constructed double quantum dot emitting layers with gradient chloride content in a light-emitting diode to facilitate hole transport, and the resulting device showed an efficiency at the theoretical limit, high brightness and long operational lifetime. We anticipate that our efficient and stable blue quantum dot light-emitting devices can facilitate the development of electroluminescent full-colour displays using quantum dots. Cadmium-free blue quantum dot light-emitting diodes are constructed with a quantum yield of unity, an efficiency at the theoretical limit, high brightness and long operational lifetime.

Reversible 3D laser printing of perovskite quantum dots inside a transparent medium

Abstract: The three-dimensional (3D) patterning of semiconductors is potentially important for exploring new functionalities and applications in optoelectronics1,2. Here, we show that it is possible to write on demand 3D patterns of perovskite quantum dots (QDs) inside a transparent glass material using a femtosecond laser. By utilizing the inherent ionic nature and low formation energy of perovskite, highly luminescent CsPbBr3 QDs can be reversibly fabricated in situ and decomposed through femtosecond laser irradiation and thermal annealing. This pattern of writing and erasing can be repeated for many cycles, and the luminescent QDs are well protected by the inorganic glass matrix, resulting in stable perovskite QDs with potential applications such as high-capacity optical data storage, information encryption and 3D artwork. Luminescent CsPbBr3 quantum dots can be written into glass using femtosecond laser pulses and thermal annealing, and erased by further femtosecond laser irradiation. The resulting quantum dot patterns could prove useful for data storage, decoration or security purposes.

Bright high-colour-purity deep-blue carbon dot light-emitting diodes via efficient edge amination

Abstract: Deep-blue light-emitting diodes (LEDs) (emitting at wavelengths of less than 450 nm) are important for solid-state lighting, vivid displays and high-density information storage. Colloidal quantum dots, typically based on heavy metals such as cadmium and lead, are promising candidates for deep-blue LEDs, but these have so far had external quantum efficiencies lower than 1.7%. Here we present deep-blue light-emitting materials and devices based on carbon dots. The carbon dots produce emission with a narrow full-width at half-maximum (about 35 nm) with high photoluminescence quantum yield (70% ± 10%) and a colour coordinate (0.15, 0.05) closely approaching the standard colour Rec. 2020 (0.131, 0.046) specification. Structural and optical characterization, together with computational studies, reveal that amine-based passivation accounts for the efficient and high-colour-purity emission. Deep-blue LEDs based on these carbon dots display high performance with a maximum luminance of 5,240 cd m−2 and an external quantum efficiency of 4%, notably exceeding that of previously reported quantum-tuned solution-processed deep-blue LEDs. Deep-blue high-colour-purity light-emitting materials are developed by using amine-based edge passivation. The light-emitting diodes based on the carbon dots exhibit a maximum luminance of 5,240 cd m–2 and an external quantum efficiency of 4%.

Highly Selective CO 2 Electroreduction to CH 4 by In Situ Generated Cu 2 O Single-Type Sites on a Conductive MOF: Stabilizing Key Intermediates with Hydrogen Bonding

Abstract: It is still a great challenge to achieve high selectivity of CH4 in CO2 electroreduction reactions (CO2 RR) because of the similar reduction potentials of possible products and the sluggish kinetics for CO2 activation. Stabilizing key reaction intermediates by single type of active sites supported on porous conductive material is crucial to achieve high selectivity for single product such as CH4 . Here, Cu2 O(111) quantum dots with an average size of 3.5 nm are in situ synthesized on a porous conductive copper-based metal-organic framework (CuHHTP), exhibiting high selectivity of 73 % towards CH4 with partial current density of 10.8 mA cm-2 at -1.4 V vs. RHE (reversible hydrogen electrode) in CO2 RR. Operando infrared spectroscopy and DFT calculations reveal that the key intermediates (such as *CH2 O and *OCH3 ) involved in the pathway of CH4 formation are stabilized by the single active Cu2 O(111) and hydrogen bonding, thus generating CH4 instead of CO.

Operation of a silicon quantum processor unit cell above one kelvin

Abstract: Quantum computers are expected to outperform conventional computers in several important applications, from molecular simulation to search algorithms, once they can be scaled up to large numbers—typically millions—of quantum bits (qubits)1–3. For most solid-state qubit technologies—for example, those using superconducting circuits or semiconductor spins—scaling poses a considerable challenge because every additional qubit increases the heat generated, whereas the cooling power of dilution refrigerators is severely limited at their operating temperature (less than 100 millikelvin)4–6. Here we demonstrate the operation of a scalable silicon quantum processor unit cell comprising two qubits confined to quantum dots at about 1.5 kelvin. We achieve this by isolating the quantum dots from the electron reservoir, and then initializing and reading the qubits solely via tunnelling of electrons between the two quantum dots7–9. We coherently control the qubits using electrically driven spin resonance10,11 in isotopically enriched silicon12 28Si, attaining single-qubit gate fidelities of 98.6 per cent and a coherence time of 2 microseconds during ‘hot’ operation, comparable to those of spin qubits in natural silicon at millikelvin temperatures13–16. Furthermore, we show that the unit cell can be operated at magnetic fields as low as 0.1 tesla, corresponding to a qubit control frequency of 3.5 gigahertz, where the qubit energy is well below the thermal energy. The unit cell constitutes the core building block of a full-scale silicon quantum computer and satisfies layout constraints required by error-correction architectures8,17. Our work indicates that a spin-based quantum computer could be operated at increased temperatures in a simple pumped 4He system (which provides cooling power orders of magnitude higher than that of dilution refrigerators), thus potentially enabling the integration of classical control electronics with the qubit array18,19. A scalable silicon quantum processor unit cell made of two qubits confined to quantum dots operates at about 1.5 K, achieving 98.6% single-qubit gate fidelities and a 2 μs coherence time.

Rational design of two-dimensional nanomaterials for lithium–sulfur batteries

Abstract: The inherent technical challenges of lithium–sulfur (Li–S) batteries have arisen from the intrinsic redox electrochemistry occurring on the Li and S electrodes, which can significantly deteriorate the S utilization and life cycle. Two-dimensional (2D) nanomaterials composed of atomic or near-atomic thickness with infinite lateral dimensions have been proven to be meritorious as emerging materials for energy storage applications due to their unique structures, remarkable physical properties, and tunable surface chemistry. Herein, we argue that surface functionalization or heteroatom doping of 2D materials, hybridization with other nanostructured materials (0D quantum dots, 1D nanotubes/nanowires, and other 2D nanosheets), and finally architecting into 3D structures along with the advantages of 2D building blocks can open up new opportunities for Li–S batteries. We also focus on the future directions of Li–S batteries in the design of S cathodes and separators utilizing the intrinsic and extrinsic properties of 2D nanomaterials.

Synthesis, optoelectronic properties and applications of halide perovskites

Abstract: Halide perovskites have emerged as a class of most promising and cost-effective semiconductor materials for next generation photoluminescent, electroluminescent and photovoltaic devices. These perovskites have high optical absorption coefficients and exhibit narrow-band bright photoluminescence, in addition to their halide-dependent tuneable bandgaps, low exciton binding energies, and long-range carrier diffusion. These properties make these perovskites superior to classical semiconductors such as silicon. Most importantly, the simple synthesis of perovskites in the form of high quality films, single crystals, nanocrystals and quantum dots has attracted newcomers to develop novel perovskites with unique optoelectronic properties for optical and photovoltaic applications. Here, we comprehensively review recent advances in the synthesis and optoelectronic properties of films, microcrystals, nanocrystals and quantum dots of lead halide and lead-free halide perovskites. Followed by the classification of synthesis, we address the ensemble and single particle properties of perovskites from the viewpoints of the confinement and transport of charge carriers or excitons. Further, we correlate the charge carrier properties of perovskite films, microcrystals, nanocrystals and quantum dots with the crystal structure and size, halide composition, temperature, and pressure. Finally, we illustrate the emerging applications of perovskites to solar cells, LEDs, and lasers, and discuss the ongoing challenges in the field.

Universal quantum logic in hot silicon qubits.

Abstract: Quantum computation requires many qubits that can be coherently controlled and coupled to each other1. Qubits that are defined using lithographic techniques have been suggested to enable the development of scalable quantum systems because they can be implemented using semiconductor fabrication technology2-5. However, leading solid-state approaches function only at temperatures below 100 millikelvin, where cooling power is extremely limited, and this severely affects the prospects of practical quantum computation. Recent studies of electron spins in silicon have made progress towards a platform that can be operated at higher temperatures by demonstrating long spin lifetimes6, gate-based spin readout7 and coherent single-spin control8. However, a high-temperature two-qubit logic gate has not yet been demonstrated. Here we show that silicon quantum dots can have sufficient thermal robustness to enable the execution of a universal gate set at temperatures greater than one kelvin. We obtain single-qubit control via electron spin resonance and readout using Pauli spin blockade. In addition, we show individual coherent control of two qubits and measure single-qubit fidelities of up to 99.3 per cent. We demonstrate the tunability of the exchange interaction between the two spins from 0.5 to 18 megahertz and use it to execute coherent two-qubit controlled rotations. The demonstration of 'hot' and universal quantum logic in a semiconductor platform paves the way for quantum integrated circuits that host both the quantum hardware and its control circuitry on the same chip, providing a scalable approach towards practical quantum information processing.

Red-Carbon-Quantum-Dot-Doped SnO2 Composite with Enhanced Electron Mobility for Efficient and Stable Perovskite Solar Cells.

Abstract: An efficient electron transport layer (ETL) plays a key role in promoting carrier separation and electron extraction in planar perovskite solar cells (PSCs). An effective composite ETL is fabricated using carboxylic-acid- and hydroxyl-rich red-carbon quantum dots (RCQs) to dope low-temperature solution-processed SnO2 , which dramatically increases its electron mobility by ≈20 times from 9.32 × 10-4 to 1.73 × 10-2 cm2 V-1 s-1 . The mobility achieved is one of the highest reported electron mobilities for modified SnO2 . Fabricated planar PSCs based on this novel SnO2 ETL demonstrate an outstanding improvement in efficiency from 19.15% for PSCs without RCQs up to 22.77% and have enhanced long-term stability against humidity, preserving over 95% of the initial efficiency after 1000 h under 40-60% humidity at 25 °C. These significant achievements are solely attributed to the excellent electron mobility of the novel ETL, which is also proven to help the passivation of traps/defects at the ETL/perovskite interface and to promote the formation of highly crystallized perovskite, with an enhanced phase purity and uniformity over a large area. These results demonstrate that inexpensive RCQs are simple but excellent additives for producing efficient ETLs in stable high-performance PSCs as well as other perovskite-based optoelectronics.

Identification of Halogen-Associated Active Sites on Bismuth-Based Perovskite Quantum Dots for Efficient and Selective CO2-to-CO Photoreduction.

Abstract: All-inorganic Pb-free bismuth (Bi) halogen perovskite quantum dots (PQDs) with distinct structural and photoelectric properties provide plenty of room for selective photoreduction of CO2. However, ...

Advances in carbon dots: from the perspective of traditional quantum dots

Abstract: Quantum dots (QDs) have been the core concept of nanoscience and nanotechnology since their inception, and play a dominant role in the development of the nano-field. Carbon dots (CDots), defined by a feature size of <10 nm, have become a rising star in the crossover field of carbon materials and traditional QDs (TQDs). CDots possess many unique structural, physicochemical and photochemical properties that render them a promising platform for biology, devices, catalysis and other applications. However, due to the complex nature of CDots, to gain a profound understanding of the physical and chemical properties of CDots is still a great challenge. Many key issues including structure, synthesis, and optical properties are unclear, leaving open arguments and nonuniform description of their basics. The achievements and experience of TQDs in the past four decades are expected to provide crucial values for further development of CDots. Here, we will compare the research outputs of TQDs and CDots and try to give a comprehensive picture of their differences and correlations in structure, synthesis, properties and applications. Along this line, further perspectives are given on future directions and key issues toward a better understanding of the basic properties of TQDs and CDots in a unified manner. We expect the researchers in the community to foresee the great potential of CDots, and focus on the critical results obtained during the development of TQDs, paying special attention to the profound principles behind the synthetic chemistry, luminescence mechanisms and applications.

A bilateral interfacial passivation strategy promoting efficiency and stability of perovskite quantum dot light-emitting diodes

Abstract: Perovskite quantum-dot-based light-emitting diodes (QLEDs) possess the features of wide gamut and real color expression, which have been considered as candidates for high-quality lightings and displays. However, massive defects are prone to be reproduced during the quantum dot (QD) film assembly, which would sorely affect carrier injection, transportation and recombination, and finally degrade QLED performances. Here, we propose a bilateral passivation strategy through passivating both top and bottom interfaces of QD film with organic molecules, which has drastically enhanced the efficiency and stability of perovskite QLEDs. Various molecules were applied, and comparison experiments were conducted to verify the necessity of passivation on both interfaces. Eventually, the passivated device achieves a maximum external quantum efficiency (EQE) of 18.7% and current efficiency of 75 cd A−1. Moreover, the operational lifetime of QLEDs is enhanced by 20-fold, reaching 15.8 h. These findings highlight the importance of interface passivation for efficient and stable QD-based optoelectronic devices. Perovskite quantum-dots are promising candidates for light-emitting diodes but the defects limit the device performance. Here Xu et al. show a passivation strategy to reduce the defect density at both interfaces, which increases the external quantum efficiency (EQE) and lifetime by more than 2-fold and 20-fold, respectively.

Progress in quantum-dot single photon sources for quantum information technologies: A broad spectrum overview

Abstract: Semiconductor quantum dots (QDs) of various material systems are being heavily researched for the development of solid state single photon emitters, which are required for optical quantum computing and related technologies such as quantum key distribution and quantum metrology. In this review article, we give a broad spectrum overview of the QD-based single photon emitters developed to date, from the telecommunication bands in the IR to the deep UV.

A bright and fast source of coherent single photons

Abstract: A single photon source is a key enabling technology in device-independent quantum communication, quantum simulation for instance boson sampling, linear optics-based and measurement-based quantum computing. These applications involve many photons and therefore place stringent requirements on the efficiency of single photon creation. The scaling on efficiency is an exponential function of the number of photons. Schemes taking full advantage of quantum superpositions also depend sensitively on the coherence of the photons, i.e. their indistinguishability. It is therefore crucial to maintain the coherence over long strings of photons. Here, we report a single photon source with an especially high system efficiency: a photon is created on-demand at the output of the final optical fibre with a probability of 57%. The coherence of the photons is very high and is maintained over a stream consisting of thousands of photons; the repetition rate is in the GHz regime. We break with the established semiconductor paradigms, such as micropillars, photonic crystal cavities and waveguides. Instead, we employ gated quantum dots in an open, tunable microcavity. The gating ensures low-noise operation; the tunability compensates for the lack of control in quantum dot position and emission frequency; the output is very well-matched to a single-mode fibre. An increase in efficiency over the state-of-the-art by more than a factor of two, as reported here, will result in an enormous decrease in run-times, by a factor of $10^{7}$ for 20 photons.

Cascade surface modification of colloidal quantum dot inks enables efficient bulk homojunction photovoltaics.

Abstract: Control over carrier type and doping levels in semiconductor materials is key for optoelectronic applications. In colloidal quantum dots (CQDs), these properties can be tuned by surface chemistry modification, but this has so far been accomplished at the expense of reduced surface passivation and compromised colloidal solubility; this has precluded the realization of advanced architectures such as CQD bulk homojunction solids. Here we introduce a cascade surface modification scheme that overcomes these limitations. This strategy provides control over doping and solubility and enables n-type and p-type CQD inks that are fully miscible in the same solvent with complete surface passivation. This enables the realization of homogeneous CQD bulk homojunction films that exhibit a 1.5 times increase in carrier diffusion length compared with the previous best CQD films. As a result, we demonstrate the highest power conversion efficiency (13.3%) reported among CQD solar cells. It is challenging to realize doping and surface passivation simultaneously in colloidal quantum dot inks. Here Choi et al. employ a cascade surface modification approach to solve the problem and obtain record high efficiency of 13.3% for bulk homojunction solar cells based on these inks.

Graphene Quantum Dots/Multiwalled Carbon Nanotubes Composite-Based Electrochemical Sensor for Detecting Dopamine Release from Living Cells

Abstract: Dopamine (DA) is an important neurotransmitter associated with nerve signaling and some diseases. Therefore, it is very significant to detect DA in patients to regulate body function. Compared with...

Photocatalytic solar fuel production and environmental remediation through experimental and DFT based research on CdSe-QDs-coupled P-doped-g-C3N4 composites

Abstract: Solar energy harvesting and conversion into useful chemical energy with the aid of semiconductor photocatalysts is a promising technique to solve both energy and environmental issues. This work reports a successful synthesis of CdSe quantum dots (QDs) modified phosphorus doped g-C3N4 (P-CN) for advanced photocatalytic applications. Phosphorus doping and structural coupling with CdSe QDs are shown to significantly extend visible-light response of g-C3N4 up to 700 nm. The optimized sample 4CdSe/P-CN demonstrates enhanced visible-light driven overall water splitting activities for H2 and O2 evolution i.e. 113 and 55.5 μmol.h−1. g−1, respectively, as well as very high photocatalytic CO2 to CH4 conversion efficiency (47 μmol.h−1. g−1). It also exhibit higher activity (78 %) for 2,4-dichlorophenol degradation as compared to pristine CN-sample. Combined photoluminescence, transient/single wavelength photocurrent, photoelectrochemical, and coumarin fluorescence spectroscopy demonstrate that 4CdSe/P-CN nanocomposite exhibit enhanced charge separation efficiency which is responsible for improved visible light catalytic activities. Our work thus provide a new strategy to design low-cost and sustainable photocatalysis with wide visible-light activity for practical overall water splitting and CO2 reduction applications.

Electrochemically-stable ligands bridge the photoluminescence-electroluminescence gap of quantum dots.

Abstract: Colloidal quantum dots are promising emitters for quantum-dot-based light-emitting-diodes. Though quantum dots have been synthesized with efficient, stable, and high colour-purity photoluminescence, inheriting their superior luminescent properties in light-emitting-diodes remains challenging. This is commonly attributed to unbalanced charge injection and/or interfacial exciton quenching in the devices. Here, a general but previously overlooked degradation channel in light-emitting-diodes, i.e., operando electrochemical reactions of surface ligands with injected charge carriers, is identified. We develop a strategy of applying electrochemically-inert ligands to quantum dots with excellent luminescent properties to bridge their photoluminescence-electroluminescence gap. This material-design principle is general for boosting electroluminescence efficiency and lifetime of the light-emitting-diodes, resulting in record-long operational lifetimes for both red-emitting light-emitting-diodes (T95 > 3800 h at 1000 cd m−2) and blue-emitting light-emitting-diodes (T50 > 10,000 h at 100 cd m−2). Our study provides a critical guideline for the quantum dots to be used in optoelectronic and electronic devices. New design principles for bridging the photoluminescence and electroluminescence of colloidal quantum dots are needed. In this work, the authors report electrochemically-inert ligands as a general material-design strategy for realizing high-performance LEDs based on quantum dots.

The germanium quantum information route

Abstract: In the effort to develop disruptive quantum technologies, germanium is emerging as a versatile material to realize devices capable of encoding, processing and transmitting quantum information. These devices leverage the special properties of holes in germanium, such as their inherently strong spin–orbit coupling and their ability to host superconducting pairing correlations. In this Review, we start by introducing the physics of holes in low-dimensional germanium structures, providing key insights from a theoretical perspective. We then examine the materials-science progress underpinning germanium-based planar heterostructures and nanowires. We go on to review the most significant experimental results demonstrating key building blocks for quantum technology, such as an electrically driven universal quantum gate set with spin qubits in quantum dots and superconductor–semiconductor devices for hybrid quantum systems. We conclude by identifying the most promising avenues towards scalable quantum information processing in germanium-based systems. Germanium is a promising material to build quantum components for scalable quantum information processing. This Review examines progress in materials science and devices that has enabled key building blocks for germanium quantum technology, such as hole-spin qubits and superconductor–semiconductor hybrids.

Ultrasensitive and ultrathin phototransistors and photonic synapses using perovskite quantum dots grown from graphene lattice.

Abstract: Organic-inorganic halide perovskite quantum dots (PQDs) constitute an attractive class of materials for many optoelectronic applications. However, their charge transport properties are inferior to materials like graphene. On the other hand, the charge generation efficiency of graphene is too low to be used in many optoelectronic applications. Here, we demonstrate the development of ultrathin phototransistors and photonic synapses using a graphene-PQD (G-PQD) superstructure prepared by growing PQDs directly from a graphene lattice. We show that the G-PQDs superstructure synchronizes efficient charge generation and transport on a single platform. G-PQD phototransistors exhibit excellent responsivity of 1.4 × 108 AW–1 and specific detectivity of 4.72 × 1015 Jones at 430 nm. Moreover, the light-assisted memory effect of these superstructures enables photonic synaptic behavior, where neuromorphic computing is demonstrated by facial recognition with the assistance of machine learning. We anticipate that the G-PQD superstructures will bolster new directions in the development of highly efficient optoelectronic devices.

Control and single-shot readout of an ion embedded in a nanophotonic cavity.

Abstract: Distributing entanglement over long distances using optical networks is an intriguing macroscopic quantum phenomenon with applications in quantum systems for advanced computing and secure communication1,2. Building quantum networks requires scalable quantum light–matter interfaces1 based on atoms3, ions4 or other optically addressable qubits. Solid-state emitters5, such as quantum dots and defects in diamond or silicon carbide6–10, have emerged as promising candidates for such interfaces. So far, it has not been possible to scale up these systems, motivating the development of alternative platforms. A central challenge is identifying emitters that exhibit coherent optical and spin transitions while coupled to photonic cavities that enhance the light–matter interaction and channel emission into optical fibres. Rare-earth ions in crystals are known to have highly coherent 4f–4f optical and spin transitions suited to quantum storage and transduction11–15, but only recently have single rare-earth ions been isolated16,17 and coupled to nanocavities18,19. The crucial next steps towards using single rare-earth ions for quantum networks are realizing long spin coherence and single-shot readout in photonic resonators. Here we demonstrate spin initialization, coherent optical and spin manipulation, and high-fidelity single-shot optical readout of the hyperfine spin state of single 171Yb3+ ions coupled to a nanophotonic cavity fabricated in an yttrium orthovanadate host crystal. These ions have optical and spin transitions that are first-order insensitive to magnetic field fluctuations, enabling optical linewidths of less than one megahertz and spin coherence times exceeding thirty milliseconds for cavity-coupled ions, even at temperatures greater than one kelvin. The cavity-enhanced optical emission rate facilitates efficient spin initialization and single-shot readout with conditional fidelity greater than 95 per cent. These results showcase a solid-state platform based on single coherent rare-earth ions for the future quantum internet. Single ytterbium ion qubits in nanophotonic cavities have long coherence times and can be optically read out in a single shot, establishing them as excellent candidates for optical quantum networks.