Quantum Dots Research Articles

Facile Synthesis of Fluorescent Carbon Quantum Dots with High Product Yield Using a Solid-Phase Strategy

The liquid-phase method is the most commonly utilized strategy for synthesizing fluorescent carbon quantum dots (CQDs). However, the liquid-phase synthesis of CQDs faces challenges such as low yield, complex purification, and the use of toxic solvents, which limit large-scale production and practical applications. In this study, fluorescent CQDs with a high product yield of 78% were synthesized using glucose as a carbon source through a green and facile one-step solid-phase approach, without solvents or post-treatment. A systematic study of the structure and fluorescence properties of the synthesized CQDs was conducted using various characterization techniques. The results indicated that the mean size of obtained CQDs was 4.1 nm, and that their surface had abundant oxygen-containing functional groups, resulting in favorable water solubility. The synthesized CQDs exhibited excitation-dependent fluorescence, with optimal excitation and emission wavelengths at 358 and 455 nm, respectively. Additionally, the CQDs solution showed bright blue fluorescence under 365 nm UV light, with a quantum yield of 6.21% and a fluorescence lifetime of 3.02 ns. This study offers valuable insights into the green and efficient synthesis of fluorescent CQDs powder.

Sensitive detection of gallic acid in food by electrochemical sensor fabricated by integrating nanochannel film with nanocarbon nanocomposite

Sensitive detection of gallic acid (GA) in foods is of great significance for assessing the antioxidant properties of products and ensuring consumer health. In this work, a simple electrochemical sensor was conveniently fabricated by integrating vertically-ordered mesoporous silica film (VMSF) with electrochemically reduced graphene oxide (ErGO) and nitrogen graphene quantum dots (NGQDs) nanocomposite, enabling sensitive detection of GA in food sample. A water-soluble mixture of graphene oxide (GO) and NGQDs was drop-cast onto the common carbon electrode, glassy carbon electrode (GCE), followed by rapid growth of VMSF using an electrochemically assisted self-assembly method (EASA). The negative voltage applied during VMSF growth facilitated the in situ reduction of GO to ErGO. The synergistic effects of ErGO, NGQDs, and the nanochannels of VMSF led to nearly a tenfold enhancement of the GA signal compared to that obtained on electrodes modified with either ErGO or NGQDs alone. Sensitive detection of GA was realized with a linear concentration range from 0.1 to 10 μM, and from 10 to 100 μM. The limit of detection (LOD), determined based on a signal-to-noise ratio of three (S/N = 3), was found to be 81 nM. Combined with the size-exclusion property of VMSF, the fabricated sensor demonstrated high selectivity, making it suitable for the sensitive electrochemical detection of gallic acid in food samples.

Photothermally Active Quantum Dots in Cancer Imaging and Therapeutics: Nanotheranostics Perspective.

Cancer is becoming a global threat, as the cancerous cells manipulate themselves frequently, resulting in mutants and more abnormalities. Early-stage and real-time detection of cancer biomarkers can provide insight into designing cost-effective diagnostic and therapeutic modalities. Nanoparticle and quantum dot (QD)-based approaches have been recognized as clinically relevant methods to detect disease biomarkers at the molecular level. Over decades, as an emergent noninvasive approach, photothermal therapy has evolved to eradicate cancer. Moreover, various structures, viz., nanoparticles, clusters, quantum dots, etc., have been tested as bioimaging and photothermal agents to identify tumor cells selectively. Among them, QDs have been recognized as versatile probes. They have attracted enormous attention for imaging and therapeutic applications due to their unique colloidal stability, optical and physicochemical properties, biocompatibility, easy surface conjugation, scalable production, etc. However, a few critical concerns of QDs, viz., precise engineering for molecular imaging and sensing, selective interaction with the biological system, and their associated toxicity, restrict their potential intervention in curing cancer and are yet to be explored. According to the U.S. Food and Drug Administration (FDA), there is no specific regulation for the approval of nanomedicines. Therefore, these nanomedicines undergo the traditional drug, biological, and device approval process. However, the market survey of QDs is increasing, and their prospects in translational nanomedicine are very promising. From this perspective, we discuss the importance of QDs for imaging, sensing, and therapeutic usage pertinent to cancer, especially in its early stages. Moreover, we also discuss the rapidly growing translational view of QDs. The long-term safety studies and cellular interaction of these QDs could enhance their visibility and bring photothermally active QDs to the clinical stage and concurrently to FDA approval.

Pursuing high-fidelity control of spin qubits in natural Si/SiGe quantum dot

Electron spins in silicon quantum dots are a promising platform for fault-tolerant quantum computing. Low-frequency noise, including nuclear spin fluctuations and charge noise, is a primary factor limiting gate fidelities. Suppressing this noise is crucial for high-fidelity qubit operations. Here, we report on a two-qubit quantum device in natural silicon with universal qubit control, designed to investigate the upper limits of gate fidelities in a non-purified Si/SiGe quantum dot device. By employing advanced device structures, qubit manipulation techniques, and optimization methods, we have achieved single-qubit gate fidelities exceeding 99% and a two-qubit controlled-Z (CZ) gate fidelity of 91%. Decoupled CZ gates are used to prepare Bell states with an average fidelity of 91%, typically exceeding previously reported values in natural silicon devices. These results underscore that even natural silicon has the potential to achieve high-fidelity gate operations, particularly with further optimization methods to suppress low-frequency noise.

CsPbBr3 perovskite quantum dots/p-GaN heterojunction for ultraviolet-visible spectrum photodetectors

All-inorganic perovskites have attracted increasing attention because of their strong environmental stability and excellent photoelectric properties. However, the limited spectral response range of perovskite photodetectors restricts them in practical applications. In this work, an ultraviolet–visible photodetector with a wide spectral response and a high responsivity was prepared by constructing a CsPbBr3 quantum dots (QDs)/p-GaN heterojunction. The type-II energy band alignment formed by the heterojunction is conducive to the transport of photogenerated carriers, resulting in a high responsivity. Under certain conditions, the device can obtain responsivity values of 5 A/W and 850 mA/W under 350 and 725 nm illumination, respectively, which are comparable to those of other perovskite-based photodetectors. In addition, the photoresponse mechanism of the device is revealed through first-principles calculations of the heterojunction and the device. The enhanced light absorption of the heterojunction and the special band bending under different bias voltages improve the photoelectric performance of the device. This work can provide valuable insights into high-performance photodetectors based on all-inorganic perovskite QDs heterojunctions in terms of band regulation and device performance improvement.

Incorporation of Graphene Quantum Dots into Magnesium Copper Phosphate (GQDs-MgCuPO4) for Supercapattery and Electrocatalysis Applications

Abstract We efficiently synthesize magnesium copper phosphate nanoparticles (MgCuPO4) doped with graphene quantum dots (GQDs) using a hydrothermal method for supercapattery and oxygen evolution reactions in KOH electrolyte. The GQDs-MgCuPO4 electrode has a high specific capacity (1188 Cg-1 at 1.0 Ag-1) and a high-rate capability (67%). The symmetric supercapattery (GQDs-MgCuPO4/GQDs-MgCuPO4) provides a staggering energy density of 46 Wh-kg-1, as well as a high-power density of 1300 W-kg-1 and a high cyclic stability of 93% after 10,000 cycles. Furthermore, it demonstrates high efficiency in the oxygen evolution reaction (OER) and the hydrogen evolution reaction (HER), with corresponding low overpotentials of 181 mV and 119 mV. The GQDs-MgCuPO4 stands out as a capable solution for various energy storage and conversion difficulties.

Inkjet printing of mixed layers comprising multinary semiconductor quantum dots and charge transport materials for light‐emitting diode displays

AbstractQuantum dots (QDs) are important luminescent structures with applications in wide‐color‐gamut displays requiring exceptional color reproducibility. Multinary semiconductor QDs are expected to serve as eco‐friendly materials to replace conventional QDs owing to the narrow spectral widths and tunable bandgaps of these QDs. However, the application of multinary QDs, which tend to exhibit defect‐related emissions, to QD light‐emitting diode (QLED) displays will require electroluminescence to be obtained from QLEDs incorporating inkjet‐printed emitting layers. The present work examines QLEDs exhibiting vibrant color emissions based on blue‐emitting Zn–Se–Te QDs, green‐emitting Ag–In–Ga–S QDs, and red‐emitting Ag–Cu–In–Ga–S QDs. Each such QLED contains QD emitting layers comprising a mixture of charge transport materials. The spectra obtained from these RGB QLEDs fabricated by spin‐coating show very high color purity. Passive matrix QLED displays incorporating these QDs are also fabricated by inkjet printing to demonstrate the high color purity that can be obtained from multinary QDs in displays. In conjunction with passive matrix driving, these displays produce clear moving images with vibrant electroluminescence originating from the multinary QDs. The present results indicate that these QDs have significant potential for utilization in wide‐color‐gamut displays.

Harnessing the Potential of Graphene Quantum Dots for Multifunctional Biomedical Applications.

The existing and emerging demand for materials for life and health has contributed to the cultivation and development of respective markets. Nevertheless, the current generation of biomedical materials has yet to fully satisfy the clinical requirements of the market, which is still in its relative infancy. Research and development in this area must be prioritized in light of the pivotal role of new life and health materials in the biological field. Among many life and health materials, GQDs, an emerging nanomaterial, exhibit considerable promise in the biomedical field, primarily due to their exceptional properties. Furthermore, the direct preparation and functionalization of GQDs have facilitated the development of specific functional composites based on GQDs. The biological applications of GQDs are undergoing rapid growth, which makes it necessary to publish a review article presenting the latest advances in this field. This review provides an overview of the significant advances in synthesizing GQDs, the techniques employed for structural characterizations, and the properties that have been elucidated. Furthermore, it presents recent findings on applying GQDs in antimicrobial, anticancer, biosensing, drug delivery, and bioimaging applications. Finally, it explores the potential of GQDs in biomedicine and biotechnology, highlighting the current challenges that remain to be addressed.

Spin-photon entanglement with direct photon emission in the telecom C-band.

Quantum networks, relying on the distribution of quantum entanglement between remote locations, have the potential to transform quantum computation and secure long-distance quantum communication. However, a fundamental ingredient for fibre-based implementations of such networks, namely entanglement between a single spin and a photon directly emitted at telecom wavelengths, has been unattainable so far. Here, we use a negatively charged exciton in an InAs/InP quantum dot to implement an optically active spin qubit taking advantage of the lowest-loss transmission window, the telecom C-band. We investigate the coherent interactions of the spin-qubit system under resonant excitation, demonstrating high fidelity spin initialisation and coherent control using picosecond pulses. We further use these tools to measure the coherence of a single, undisturbed electron spin in our system. Finally, we demonstrate spin-photon entanglement in a solid-state system with entanglement fidelity F = 80.07 ± 2.9%, more than 10 standard deviations above the classical limit.

Highly Active MXene Quantum Dots/CuSe n-p Plasmonic Heterostructures for Ultrafast Photocatalytic Removal of Cr(VI) under Full Solar Spectrum.

Identifying effective plasmonic photocatalysts exhibiting robust activities across the entire solar spectrum poses a significant challenge. CuSe, with its local surface plasmon resonance (LSPR) effect, has garnered attention as a prospective plasmonic photocatalyst. However, severe charge recombination and insufficient light absorption limit its photocatalytic performance. To enhance the performance, constructing CuSe-based n-p plasmonic semiconductor heterostructures is a potential strategy. MXene quantum dots (MQDs), a kind of n-type plasmonic semiconductor with metallic conductivity and a high LSPR effect, are a promising candidate to couple with p-type CuSe. According to the complementary principle, we designed a 0D/2D MQDs/CuSe n-p plasmonic semiconductor, achieved by wrapping CuSe nanosheets with MQDs. This n-p plasmonic heterostructure exhibits a synergistic effect on an enhanced electronic field, facilitating charge transfer and separation, thereby enhancing charge excitation, carrier migration, and photothermal effect. Furthermore, optimizing the MQD loading content leads to an ultrafast photocatalytic reaction rate, achieving 100% Cr(VI) reduction efficiency within just 60 min with a reaction kinetics of 0.069 min-1, surpassing the performance of bare CuSe. Our work presents a promising approach for developing advanced n-p plasmonic heterostructures based on MQDs for wastewater treatment and other photocatalytic applications.

Reinforcing Photogenerated Carrier Extraction of Environment-Friendly InP/ZnSeS Quantum Dots for High-Performing Photoelectrochemical Photodetection and Solar Energy Conversion.

Colloidal InP/ZnSeS-based quantum dots (QDs) are considered promising building blocks for light-emitting devices due to their environmental friendliness, high quantum yield (QY), and narrow emission. However, the intrinsic type-I band structure severely hinders potential photoelectrochemical (PEC) applications requiring efficient photoexcited carrier separation and transfer. In this study, the optoelectronic properties of InP/ZnSeS QDs are tailored by introducing Al dopants in the ZnSeS layer, which concurrently passivate the surface defects and act as shallow donor states for suppressed non-radiative recombination and improved charge extraction efficiency. Consequently, as-fabricated InP/ZnSeS:Al QDs-based PEC-type photodetector exhibited a high detectivity up to 1011 Jones and a remarkable responsivity of 0.66 AW-1 at 600nm even under self-powered condition (0V bias). In addition, as-prepared InP/ZnSeS:Al QDs-based photoanode can be alternatively used for PEC hydrogen generation, showing an H2 production rate of 73.7µmol cm-2h-1 under 1 sun illumination (AM 1.5G, 100mW cm-2). The results offer a prospective strategy for optimizing eco-friendly QDs for high-performance multifunctional light detection/conversion devices.

Monolithically Integrated Quantum Dots in a 22‐nm Fully Depleted Silicon‐on‐Insulator Process Operating at 3 K

ABSTRACTQuantum computers comprising large‐scale arrays of qubits will enable complex algorithms to be executed to provide a quantum advantage for practical applications. A prerequisite for this milestone is a power‐efficient qubit control and detection system operating at cryogenic temperatures. Implementing such systems in complementary metal‐oxide‐semiconductor (CMOS) technology offers clear advantages in terms of scalability. Here, we present a fully integrated quantum dot array in which silicon quantum wells are co‐located with control and detection circuitry on the same die in a commercial 22‐nm fully depleted silicon‐on‐insulator (FDSOI) process. Our system comprises a two‐dimensional quantum dot array, integrated with 8 detectors and 32 injectors, operating at 3 K inside a cryo‐cooler. The power consumption of the control and detection circuitry is 2.5 mW per qubit without body biasing. The design utilizes 0.8‐V nominal devices. The setup allows us to verify discrete charge injection control and detection at the quantum dot array and demonstrate the feasibility of this architecture for scaling up the existing quantum core to hundreds and thousands of physical qubits.

FeOOH Quantum Dots Assembled MXene-Decorated 3D Photothermal Evaporator for Synergy Application in Solar Evaporation and Fenton Degradation.

Solar-driven water evaporation is considered as the sustainable approach to alleviate freshwater resource crisis through direct use of solar energy. However, it is still challenging to achieve the multifunctional solar evaporators equipped with both high evaporation and purification performance to handle practical complex wastewater. Here, a simple and cost-effective multifunctional 3D solar evaporator is prepared by alternately decorating the commercial sponge with FeOOH quantum dots (FQDs) supported MXene sheets composites and chitosan hydrogel coatings for enabling the solar water evaporation and organic wastewater photodegradation simultaneously. MXene composites allow the solar evaporator with excellent photothermal conversion performance, the hydrophilic chitosan hydrogel coated interconnecting skeleton structures of sponge serve as the mass transfer and water transport channels. The Fenton-catalytic FQDs anchored on the MXene sheets surface accept the photo-generated electrons of MXene sheets to induce the organic pollutant photo-Fenton degradation reaction under sunlight irradiation. The resulting evaporator possesses both excellent water evaporation rate of 2.54kg m-2h-1 and high degradation efficiency (99.24% for methylene blue), coupled with durable salt-resisting performance during long-term seawater desalination (20 wt.% NaCl). This work provides a simple and feasible strategy for designing multifunctional solar evaporators to meet the potential application scenarios in practice.

Spin-valley locked excited states spectroscoy in a one-particle bilayer graphene quantum dot

Current semiconductor qubits rely either on the spin or on the charge degree of freedom to encode quantum information. By contrast, in bilayer graphene the valley degree of freedom, stemming from the crystal lattice symmetry, is a robust quantum number that can therefore be harnessed for this purpose. The simplest implementation of a valley qubit would rely on two states with opposite valleys as in the case of a single-carrier bilayer graphene quantum dot immersed in a small perpendicular magnetic field (B⊥ ≲ 100 mT). However, the single-carrier quantum dot excited states spectrum has not been resolved to date in the relevant magnetic field range. Here, we fill this gap, by measuring the parallel and perpendicular magnetic field dependence of this spectrum with an unprecedented resolution of 4 μeV. We use a time-resolved charge detection technique that gives us access to individual tunnel events. Our results come as a direct verification of the predicted spectrum and establish a new upper-bound on inter-valley mixing, equal to our energy resolution. Our charge detection technique opens the door to measuring the relaxation time of a valley qubit in a single-carrier bilayer graphene quantum dot.

Predicting Fatigue Damage in Hydrogels Through Force-Induced Luminescence Enhancement.

Fatigue damage of polymers occurs under long-term load cycling, resulting in irreversible fracture failure, which is difficult to predict. The real-time monitoring of material fatigue damage is of great significance. Here, tough hydrogels are prepared with force-induced confined luminescence enhancement of carbonated polymer quantum dot(CPD) clusters to realize the visualization of fracture process and the monitoring of fatigue damage. The enhanced interactions induced by force between the clusters and the polymer in the confined space inhibit the non-radiative leaps and promote the radiative leaps to quantify the fatigue damage into optical signals. Rigid CPDs with abundant active sites on the surface can form dynamic reversible bonds with polymer and dissipate stress concentration, which significantly enhances the crack propagation strain (8000%) and fracture energy (26.4kJ m-2) of hydrogels. CPDhydrogelshave a wide range of applications in novel information encryption and luminescent robotics.

Germylene Mediated Reductive C−C and C−N Coupling of an Isocyanide and its Device Application

AbstractWe have demonstrated a unique reductive coupling of 4‐iodophenyl isocyanide, facilitated by a perimidine‐based N‐heterocyclic germylene (NHGe), which yields a bis‐spirogerma compound featuring simultaneous C−C and C−N bond formation. This reaction, which leads to the oxidation of germanium from +2 to +4, represents a significant departure from previously documented isocyanide‐germylene interactions. The product exhibits extensive conjugation across its bicyclic C4Ge2N2 framework, conferring distinct photophysical properties, including prominent orange luminescence in both solution and solid states. The photophysical properties are supported by the TD‐DFT calculations confirming an n→π* transition. The potential application of this compound in optoelectronic devices, particularly as a hole transport layer in PbS quantum dot solar cells, is also explored, with promising preliminary results.

Germylene Mediated Reductive C-C and C-N Coupling of an Isocyanide and its Device Application.

We have demonstrated a unique reductive coupling of 4-iodophenyl isocyanide, facilitated by a perimidine-based N-heterocyclic germylene (NHGe), which yields a bis-spirogerma compound featuring simultaneous C-C and C-N bond formation. This reaction, which leads to the oxidation of germanium from +2 to +4, represents a significant departure from previously documented isocyanide-germylene interactions. The product exhibits extensive conjugation across its bicyclic C4Ge2N2 framework, conferring distinct photophysical properties, including prominent orange luminescence in both solution and solid states. The photophysical properties are supported by the TD-DFT calculations confirming an n→π* transition. The potential application of this compound in optoelectronic devices, particularly as a hole transport layer in PbS quantum dot solar cells, is also explored, with promising preliminary results.

Compact Carbon-Based Ultra-High-Power Electrodes: A Sodium Alginate-Induced Self-Shrinkage and Densification Approach.

The trade-off between compact energy storage and high-power performance presents a significant challenge in device development. While densifying carbon materials enhances volumetric energy density by optimizing the balance between porosity and packing density, it often disrupts electronic conductivity due to random physical contact between nanomodules, limiting the power performance. This work presents a sodium alginate (SA)-induced self-shrinkage densification strategy that overcomes this limitation by incorporating nanometer-sized "spacers," namely carbon quantum dots (CQDs), into graphene nanosheets and crosslinking them by carbonizing SA accompanying with the shrinkage. These CQDs and SA-derived carbon enhance specific surface area, electronic conductivity, and ion transport rate due to the CQDs' spacer function and the formation of welded junction between the reduced graphene oxide (rGO)/CQDs nanosheets. Subsequently, the rGO/CQDs/SA-derived carbon film exhibits an extraordinary volumetric power density of 12307.7W cm-3 in an aqueous electrolyte under a mass loading of 0.12mg cm-2. Notably, the assembled aqueous supercapacitors achieve a high volumetric power density of 349.5W cm-3 under a higher mass loading of 0.49mg cm-2. This paves the way for developing compact, highly conductive carbon-based electrodes without compromising high porosity, offering a significant advancement in ultra-high-power energy storage devices.

P-Type AgAuSe Quantum Dots.

Control over the carrier type of semiconductor quantum dots (QDs) is pivotal for their optoelectronic device applications, and it remains a nontrivial and challenging task. Herein, a facile doping strategy via K impurity exchange is proposed to convert the NIR n-type toxic heavy-metal-free AgAuSe (AAS) QDs to p-type. When the dopant reaches saturation at approximately 22.2%, the Femi level shifts down to near the valence band, with the p-type carrier characteristics confirmed through photoluminescence, X-ray photoelectron spectroscopy, and ultraviolet photoelectron spectroscopy analysis. First-principles calculations reveal that K impurities preferentially occupy interstitial positions and form complex defects when combined with the abundant cationic vacancy in AAS caused by the high mobility of Ag, thereby functioning as a shallow acceptor to enhance p-type conductivity. A p-n homojunction based on AAS QDs has been fabricated and served as the active layer in a photodiode device, which demonstrates an excellent room-temperature detectivity of up to 2.29 × 1013 Jones and an outstanding linear dynamic range of over 103 dB. This study provides guidance for future design of the p-n homojunction using the toxic-metal-free Ag-based QDs and further unleashes their potential in advanced optoelectronic device applications.

Design and Performance of an InAs Quantum Dot Scintillator with Integrated Photodetector

A new scintillation material composed of InAs quantum dots (QDs) hosted within a GaAs matrix was developed, and its performance with different types of radiation is evaluated. A methodology for designing an integrated photodetector (PD) with a low defect density and that is optically matched to the QD’s emission spectrum is introduced, utilizing an engineered epitaxial InAlGaAs metamorphic buffer layer. The photoluminescence (PL) collection efficiency of the integrated PD is examined using two-dimensional scanning laser excitation. The detector response to 5.5 MeV α-particles and 122 keV photons is presented. Yields of 13 electrons/keV for α-particles and 30–60 electrons/keV for photons were observed. The energy resolution of 12% observed with α-particles was mainly limited by noise- and geometry-related optical losses. The radiation hardness of an InAs QDs hosted within GaAs and a wider band gap AlGaAs ternary alloy was studied under a 1 MeV proton implantation up to a 1014 cm−2 dose. The integrated PL responses were compared to evaluate PL quenching due to non-radiative defects. The QDs embedded in the AlGaAs demonstrated improved radiation hardness compared to QDs in the GaAs matrix and in the InGaAs quantum wells.