III-V Quantum Dots Research Articles

Fluorescent Sensing for the Detection and Quantification of Sulfur-Containing Gases.

Sulfur-containing gases, such as H2S and SO2, play significant roles in a multitude of biological processes affecting human life and health. Precise and efficient detection of these gases is therefore crucial for advancing one's understanding of their biological roles and developing effective diagnostic strategies. Fluorescent sensing offers a highly sensitive and versatile approach for detecting these gases. This Review examines the recent advances in the fluorescent detection of H2S and SO2, highlighting the key mechanisms involved in fluorescence signal transduction, including changes in intensity and wavelength shifts. The diverse array of probe molecules employed for this purpose, including those utilizing mechanisms such as nucleophilic reactions, Förster resonance energy transfer (FRET), and sulfur affinity interactions are explored. In additional to organic sensors, the focus of the Review is particularly directed toward quantum dot (QD) systems, emphasizing their tunable optical properties that hold immense potential for fluorescence sensing. Beyond the traditional III-V QDs, we delve into the emerging fluorescence sensors based on halide perovskite QDs, upconversion nanocrystals, and other novel materials. These advanced QD systems hold promise for the development of highly sensitive and cost-effective gas detectors, paving the way for significant advances in biomedical and environmental monitoring. This Review provides a comprehensive overview of the current state-of-the-art in QD-based fluorescence sensing of sulfur-containing gases and provides a multifaceted discussion comparing organic fluorescent sensors with QD sensors, highlighting the key challenges and opportunities for the integration of fluorescence sensing as it evolves. The Review aims to facilitate further research and development of innovative sensing platforms to enable more accurate and sensitive detection of these important gases.

(Invited) Epitaxial III-V Nanomaterials on the Si Platform for Quantum and Data Communications

As Si-based integrated photonic components begin to replace older technologies for optical data communications, the need for better integration of semiconductor lasers on the Si platform is greater than ever. In addition, emerging interest in integrated-photonic-based quantum computing and quantum sensing presents a further need for quantum light emitters—entangled and single-photon—on Si. III-V quantum dots represent a promising solution, both for the active region of telecommunications-wavelength lasers and for quantum emitters. However, epitaxial quantum dots grown on conventional (100) substrates typically lack the high symmetry required for entangled-photon emission.This presentation will discuss our recent work to develop a novel approach for III-V direct growth on Si via an ultrathin (<10 nm) single crystal strain relieving buffer layer, realized by the selective oxidation and condensation of an amorphous SiGe surface layer. The fabrication and properties of this novel Ge-rich buffer layer, as well as its use for subsequent III-V organometallic vapor-phase epitaxy will be presented.The second part of the talk will present our recent work on the epitaxial growth and characterization of (In,Ga)As quantum dots for the above-mentioned applications. Specifically, I will show that surface-energy-modifying surfactants (Sb, Bi) present the possibility to externally direct quantum dot formation “on-demand” in strained InAs layers on GaAs(111) substrates, where quantum dot formation by the Stranski–Krastanov process does not naturally occur. These nanostructures are prospective for high-symmetry entangled-photon emitters. The three-dimensional (3D) composition profile of InAs quantum dot layers is characterized by atom-probe microscopy (APT), elucidating the real-world quantum dot matrix. This 3D composition data is input into a finite element solver to determine the quantum dot energies and wavefunctions for electrons and holes. The modeling reveals that in high-density quantum dot layers, the electron and hole states are hybridized between multiple quantum dots in the matrix. This has important consequences for design of quantum dot light emitters. The predicted transition energies are in agreement with low-temperature photoluminescence. This work constitutes a promising approach for integrating telecommunications-wavelength quantum dot lasers and entangled photon emitters on the Si integrated photonics platform.

Reduction of GaAs Buffer Thickness and Its Impact on Epitaxially Integrated III-V Quantum Dot Lasers on a Si Substrate.

Monolithic integration of III-V quantum dot (QD) lasers onto a Si substrate is a scalable and reliable approach for obtaining highly efficient light sources for Si photonics. Recently, a combination of optimized GaAs buffers and QD gain materials resulted in monolithically integrated butt-coupled lasers on Si. However, the use of thick GaAs buffers up to 3 μm not only hinders accurate vertical alignment to the Si optical waveguide but also imposes considerable growth costs and time constraints. Here, for the first time, we demonstrate InAs QD lasers epitaxially grown on a 700 nm thick GaAs/Si template, which is approximately four times thinner than the conventional III-V buffers on Si. The optimized 700 nm GaAs buffer yields a remarkably smooth surface and low threading dislocation density of 4 × 108 cm-2, which is sufficient for QD laser growth. The InAs QD lasers fabricated on these ultrathin templates still lase at room temperature with a threshold current density of 661 A/cm2 and a characteristic temperature of 50 K. We believe that these results are important for the monolithically integrated III-V QD lasers for Si photonics applications.

E-Band InAs Quantum Dot Micro-Disk Laser with Metamorphic InGaAs Layers Grown on GaAs/Si (001) Substrate.

The direct growth of III-V quantum dot (QD) lasers on silicon substrate has been rapidly developing over the past decade and has been recognized as a promising method for achieving on-chip light sources in photonic integrated circuits (PICs). Up to date, O- and C/L-bands InAs QD lasers on Si have been extensively investigated, but as an extended telecommunication wavelength, the E-band QD lasers directly grown on Si substrates are not available yet. Here, we demonstrate the first E-band (1365 nm) InAs QD micro-disk lasers epitaxially grown on Si (001) substrates by using a III-V/IV hybrid dual-chamber molecular beam epitaxy (MBE) system. The micro-disk laser device on Si was characterized with an optical threshold power of 0.424 mW and quality factor (Q) of 1727.2 at 200 K. The results presented here indicate a path to on-chip silicon photonic telecom-transmitters.

One-pot heat-up synthesis of short-wavelength infrared, colloidal InAs quantum dots.

III-V colloidal quantum dots (QDs) promise Pb and Hg-free QD compositions with which to build short-wavelength infrared (SWIR) optoelectronic devices. However, their synthesis is limited by the availability of group-V precursors with controllable reactivities to prepare monodisperse, SWIR-absorbing III-V QDs. Here, we report a one-pot heat-up method to synthesize ∼8nm edge length (∼6.5nm in height) tetrahedral, SWIR-absorbing InAs QDs by increasing the [In3+]:[As3+] ratio introduced using commercially available InCl3 and AsCl3 precursors and by decreasing the concentration and optimizing the volume of the reducing reagent superhydride to control the concentration of In(0) and As(0) intermediates through QD nucleation and growth. InAs QDs are treated with NOBF4, and their deposited films are exchanged with Na2S to yield n-type InAs QD films. We realize the only colloidal InAs QD photoconductors with responsivity at the technologically important wavelength of 1.55μm.

Colloidal InSb Quantum Dots for 1500nm SWIR Photodetector with Antioxidation of Surface.

III-V quantum dots (QDs) have emerged as significant alternatives to Cd- and Pb-based QDs, garnering notable attention over the past two decades. However, the understanding of III-V QDs, particularly in the short wave-infrared (SWIR) region, remains limited. InAs QDs are widely recognized as the most prominent SWIR QDs, but their absorption beyond 1400nm presents various challenges. Consequently, InSb QDs with relatively narrower bandgaps have been investigated; however, research on their device applications is lacking. In this study, InSb QDs are synthesized with absorption ranging from 1000 to 1700nm by introducing Cl- ions to enhance QD surface stability during synthesis. Additionally, it coated InAs and ZnSe shells onto the InSb QDs to validate photoluminescence in the SWIR region and improve photostability. Subsequently, these QDs are employed in the fabrication of photodetector devices, resulting in photodetection above 1500nm using Pb-free QDs. The photodetection device exhibited an external quantum efficiency (EQE) of 11.4% at 1370nm and 6.3% at 1520nm for InSb core QDs, and 4.6% at 1520nm for InSb/InAs core/shell QDs, marking the successful implementation of such a device. In detail, the 1520nm for InSb core device showed a dark current density(JD ) value of: 1.46 × 10-9 A/cm2 , responsivity(R): 0.078 A/W, and specific detectivity based on the shot noise(Dsh *): 3.6×1012 Jones at 0V.

Tailoring Eco-Friendly Colloidal Quantum Dots for Photoelectrochemical Hydrogen Generation.

A photoelectrochemical (PEC) cell is able to realize effective solar-to-hydrogen energy conversion from water by using the semiconductor photoelectrode. Semiconducting colloidal quantum dots (QDs) with captivating features of size-tunable optoelectronic properties and broad light absorption are regarded as promising photosensitizers in solar-driven PEC systems. Up to now, different types of QDs have been developed to achieve high-efficiency PEC H2 generation, while the majority of state-of-the-art QDs-PEC systems are still fabricated from QDs consisting of heavy metals (e.g., Cd and Pb), which are extremely harmful to the human health and natural environment. In this context, substantial efforts have been made to mitigate the usage of highly toxic heavy metals and concurrently promote the development of alternative environment-friendly QDs with comparable features. This review presents recent advances of solar-driven PEC devices based on several typical environment-friendly QDs (e.g., carbon QDs, I-III-VI QDs and III-V QDs). A variety of techniques (e.g., shell thickness tuning, alloying/doping, and ligands exchange, etc.) to engineer these QD's optoelectronic properties and achieve high-efficiency PEC H2 production are thoroughly discussed. Furthermore, the critical challenges and future perspectives of advanced eco-friendly QDs-PEC systems in terms of QDs' synthesis, photo-induced charge kinetics, and operation stability/efficiency are briefly proposed.

Low-loss grating coupler based on inter-layer mode interference in a hybrid silicon nitride platform.

Surface grating couplers are an important component for interfacing photonic integrated circuits with optical fibers. However, conventional coupler designs typically provide limited performance due to low directionality and poor fiber-to-grating field overlap. The efficiency can be improved by using non-uniform grating structures at the expense of small critical dimensions complicating the fabrication process. While uniform gratings can alleviate this constraint, they produce an exponentially decaying near-field with the Gaussian fiber mode overlap limited to a theoretical maximum of 80%. In this work, we propose a uniform grating coupler that circumvents this field overlap limitation. This is achieved by leveraging inter-layer mode interference through a virtual directional coupler effect in a hybrid amorphous-silicon (α-Si) on silicon nitride (Si3N4) platform. By optimizing the inter-layer gap and grating geometry, a near-Gaussian profile of the out-radiated beam is achieved, resulting in an unprecedented grating-to-fiber overlap of 96%. The full three-dimensional (3D) finite-difference time-domain (FDTD) simulations show a high directionality of 84% and a record coupling loss of -1.27 dB with a 1-dB bandwidth of 20 nm for the uniform grating coupler design. Our device is designed for a wavelength of 950 nm aimed for use in hybrid quantum photonic integrated circuits using III-V quantum dot single photon sources.

Continuous-wave operation of Si-based 1.31 μm InAs/GaAs quantum-dot laser grown by molecular beam epitaxy

Excellent performance III-V quantum-dot (QD) lasers grown on Si substrates by molecular beam epitaxy (MBE) are the most promising candidates for commercially viable Si-based lasers. This makes coveted chip-to-chip and system-to-system optical interconnections feasible. This paper reports the realization of high performance 1.31 μm InAs/GaAs QD lasers on a Si substrate with all-MBE The transition from Si to GaAs was realized using Ge as the intermediary layer, and the InAs/GaAs QD laser structure was grown on the GaAs/Ge buffer. Under continuous wave (CW) operation mode, a low threshold current density of 375 A cm−2, high output power of 63 mW, and high operating temperature of 80 °C, have been achieved using Si-based InAs QD lasers with a narrow ridge structure. It has great potential for application in the development of Si-based photonic integration circuits.

High-Performance Monolithic Integration of III-V QD Lasers on Si Substrates

With the development of digital processes, the speed and efficiency of information exchange has increased to a great extent. Silicon-based photonics allows for large-scale photonic integration through CMOS manufacturing processes, the advantages of which lie in the low cost, low energy consumption and high quality of such processes. Currently, silicon-based monolithic integrated quantum dot lasers have achieved lifetimes comparable to those of heterogeneous integrated lasers and are even available for commercial applications. The silicon photonic platform also offers low-loss passive devices, as well as high-speed optical modulators and photodetectors. However, device performance suffers due to differences in physical properties between group III-V lasers and substrate materials, an important factor limiting the development of silicon-based monolithic integrated quantum dot lasers. This paper reviews the respective characteristics of silicon-based monolithic and heterogeneous integration. The advantages of monolithically integrated III-V quantum dot lasers over heterogeneous integration are highlighted, as well as the challenges, solutions and recent developments.

Design Rules for Obtaining Narrow Luminescence from Semiconductors Made in Solution.

Solution-processed semiconductors are in demand for present and next-generation optoelectronic technologies ranging from displays to quantum light sources because of their scalability and ease of integration into devices with diverse form factors. One of the central requirements for semiconductors used in these applications is a narrow photoluminescence (PL) line width. Narrow emission line widths are needed to ensure both color and single-photon purity, raising the question of what design rules are needed to obtain narrow emission from semiconductors made in solution. In this review, we first examine the requirements for colloidal emitters for a variety of applications including light-emitting diodes, photodetectors, lasers, and quantum information science. Next, we will delve into the sources of spectral broadening, including "homogeneous" broadening from dynamical broadening mechanisms in single-particle spectra, heterogeneous broadening from static structural differences in ensemble spectra, and spectral diffusion. Then, we compare the current state of the art in terms of emission line width for a variety of colloidal materials including II-VI quantum dots (QDs) and nanoplatelets, III-V QDs, alloyed QDs, metal-halide perovskites including nanocrystals and 2D structures, doped nanocrystals, and, finally, as a point of comparison, organic molecules. We end with some conclusions and connections, including an outline of promising paths forward.

Cation Exchange Synthesis of Aliovalent Doped InP QDs and Their ZnSexS1-x Shell Coating for Enhanced Fluorescence Properties.

III-V quantum dots (QDs), in particular InP QDs, have emerged as high-performance and environmentally friendly candidates to replace cadmium based QDs. InP QDs exhibit properties of direct band gap structure, low toxicity, and high mobility, which make them suitable for high-performance optoelectronic applications. However, it is still challenging to precisely regulate the components and crystal structure of InP QDs, especially in the engineered stable aliovalent doping. In this work, we developed our original reverse cation exchange strategy to achieve Cu+ doped InP (InP:Cu) QDs at lower temperature. A ZnSexS1-x shell was then homogeneously grown on the InP:Cu QDs as the passivation shell. The as-prepared InP:Cu@ZnSexS1-x core-shell QDs exhibited better fluorescence properties with a photoluminescence quantum yield (PLQY) of 56.47%. Due to the existence of multiple luminous centers in the QDs, variable temperature-dependent fluorescence characteristics have been studied. The high photoluminescence characteristics in the near-infrared region indicate their potential applications in optoelectronic devices and biological fields.

Optimization of heterogeneously integrated InP-Si on-chip photonic components.

We demonstrate comprehensive numerical studies on a hybrid III-V/Si-based waveguide system, serving as a platform for efficient light coupling between an integrated III-V quantum dot emitter to an on-chip quantum photonic integrated circuit defined on a silicon substrate. We propose a platform consisting of a hybrid InP/Si waveguide and an InP-embedded InAs quantum dot, emitting at the telecom C-band near 1550 nm. The platform can be fabricated using existing semiconductor processing technologies. Our numerical studies reveal nearly 87% of the optical field transfer efficiency between geometrically-optimized InP/Si and Si waveguides, considering propagating field along a tapered geometry. The coupling efficiency of a directional dipole emission to the hybrid InP/Si waveguide is evaluated to ∼38%, which results in more than 33% of the total on-chip optical field transfer efficiency from the dipole to the Si waveguide. We also consider the off-chip outcoupling efficiency of the propagating photon field along the Si waveguide by examining the normal to the chip plane and in-plane outcoupling configurations. In the former case, the outcoupling amounts to ∼26% when using the circular Bragg grating outcoupler design. In the latter case, the efficiency reaches up to 8%. Finally, we conclude that the conceptual device's performance is weakly susceptible to the transferred photon wavelength, offering a broadband operation within the 1.5-1.6 µm spectral range.

Novel InGaSb/AlP Quantum Dots for Non-Volatile Memories.

Non-volatile memories based on the flash architecture with self-assembled III-V quantum dots (SAQDs) used as a floating gate are one of the prospective directions for universal memories. The central goal of this field is the search for a novel SAQD with hole localization energy (Eloc) sufficient for a long charge storage (10 years). In the present work, the hole states' energy spectrum in novel InGaSb/AlP SAQDs was analyzed theoretically with a focus on its possible application in non-volatile memories. Material intermixing and formation of strained SAQDs from a GaxAl1-xSbyP1-y, InxAl1-xSbyP1-y or an InxGa1-xSbyP1-y alloy were taken into account. Critical sizes of SAQDs, with respect to the introduction of misfit dislocation as a function of alloy composition, were estimated using the force-balancing model. A variation in SAQDs' composition together with dot sizes allowed us to find that the optimal configuration for the non-volatile memory application is GaSbP/AlP SAQDs with the 0.55-0.65 Sb fraction and a height of 4-4.5 nm, providing the Eloc value of 1.35-1.50 eV. Additionally, the hole energy spectra in unstrained InSb/AlP and GaSb/AlP SAQDs were calculated. Eloc values up to 1.65-1.70 eV were predicted, and that makes unstrained InGaSb/AlP SAQDs a prospective object for the non-volatile memory application.

Controlled-phase gate by dynamic coupling of photons to a two-level emitter

We propose an architecture for achieving high-fidelity deterministic quantum logic gates on dual-rail encoded photonic qubits by letting photons interact with a two-level emitter (TLE) inside an optical cavity. The photon wave packets that define the qubit are preserved after the interaction due to a quantum control process that actively loads and unloads the photons from the cavity and dynamically alters their effective coupling to the TLE. The controls rely on nonlinear wave mixing between cavity modes enhanced by strong externally modulated electromagnetic fields or on AC Stark shifts of the TLE transition energy. We numerically investigate the effect of imperfections in terms of loss and dephasing of the TLE as well as control field miscalibration. Our results suggest that III-V quantum dots in GaAs membranes is a promising platform for photonic quantum information processing.

Monolithic Integration of O-Band InAs Quantum Dot Lasers with Engineered GaAs Virtual Substrate Based on Silicon.

The realization of high-performance Si-based III-V quantum-dot (QD) lasers has long attracted extensive interest in optoelectronic circuits. This manuscript presents InAs/GaAs QD lasers integrated on an advanced GaAs virtual substrate. The GaAs layer was originally grown on Ge as another virtual substrate on Si wafer. No patterned substrate or sophisticated superlattice defect-filtering layer was involved. Thanks to the improved quality of the comprehensively modified GaAs crystal with low defect density, the room temperature emission wavelength of this laser was allocated at 1320 nm, with a threshold current density of 24.4 A/cm−2 per layer and a maximum single-facet output power reaching 153 mW at 10 °C. The maximum operation temperature reaches 80 °C. This work provides a feasible and promising proposal for the integration of an efficient O-band laser with a standard Si platform in the near future.

ZnF2-Assisted Synthesis of Highly Luminescent InP/ZnSe/ZnS Quantum Dots for Efficient and Stable Electroluminescence

High-quality InP-based quantum dots (QDs) have become very promising, environmentally benign light emitters for display applications, but their synthesis generally entails hazardous hydrofluoric acid. Here, we present a highly facile route to InP/ZnSe/ZnS core/shell/shell QDs with a near-unity photoluminescence quantum yield. As the key additive, the inorganic salt ZnF2 mildly reacts with carboxylic acid at a high temperature and in situ generates HF, which eliminates surface oxide impurities, thus facilitating epitaxial shell growth. The resulting InP/ZnSe/ZnS QDs exhibit a narrower emission line width and better thermal stability in comparison with QDs synthesized with hydrofluoric acid. Light-emitting diodes using large-sized InP/ZnSe/ZnS QDs without replacing original ligands achieve the highest peak external quantum efficiency of 22.2%, to the best of our knowledge, along with a maximum brightness of >110 000 cd/m2 and a T95 lifetime of >32 000 h at 100 cd/m2. This safe approach is anticipated to be applied for a wide range of III-V QDs.

Recent Progress of Quantum Dot Lasers Monolithically Integrated on Si Platform

With continuously growing global data traffic, silicon (Si)-based photonic integrated circuits have emerged as a promising solution for high-performance Intra-/Inter-chip optical communication. However, a lack of a Si-based light source remains to be solved due to the inefficient light-emitting property of Si. To tackle the absence of a native light source, integrating III-V lasers, which provide superior optical and electrical properties, has been extensively investigated. Remarkably, the use of quantum dots as an active medium in III-V lasers has attracted considerable interest because of various advantages, such as tolerance to crystalline defects, temperature insensitivity, low threshold current density and reduced reflection sensitivity. This paper reviews the recent progress of III-V quantum dot lasers monolithically integrated on the Si platform in terms of the different cavity types and sizes and discusses the future scope and application.

Features of the MBE growth of nanowires with quantum dots on the silicon surface

The development of a new semiconductor element base is necessary to create a new generation of applications. At present time, the synthesis of high-quality hybrid nanostructures based on III-V quantum dots in the body of nanowires of a wide range of material systems is an urgent and important task. In work hybrid III-V nanostructures based on QDs in the body of NWs in GaP/GaAs and AlGaP/InGaP material systems were synthesized in on silicon substrates and their physical properties were investigated.

Bandgap Engineering of the II-IV, III-V and IV-VI Semiconductor Quantum Dots for Technological Applications

Bandgap Engineering of the II-IV, III-V and IV-VI Semiconductor Quantum Dots for Technological Applications