Quantum Dot Layers Research Articles

Plasmonic Modulation of Gold Nanoplates on Multiwavelength Emission.

Plasmonic regulation introduced by metallic nanoparticles is a useful method to improve the detection performance of plasmon-based systems. Herein, we observed a unique enhancement of surface plasmon-coupled emission (SPCE) using plate-shaped plasmonic nanostructures. By assembling Au nanoplates (Au NPLs) via electrostatic adsorption between the Au nanofilm and the quantum dot (QD) layer (630 nm), the fluorescence signal of SPCE was enhanced 90 times more than that of normal SPCE after the conditions were optimized. This enhancement was mainly induced by the intense localized electromagnetic field at the tip of Au NPLs and a novel plasmonic distribution around the "hot-spot" structure between the nanoparticle and Au nanofilm. These effectively mitigated the inherent signal quenching of SPCE and enhanced the emission signal of ultrathin samples on the surface of the NPL-modified Au nanofilm structure. This strategy can be used to improve the detection sensitivity and information integrity of SPCE-based biosensing and bioimaging systems containing ultrathin luminous layers. The different enhancement efficiencies for multiwavelengths were successfully obtained through various emission angles in light of the wavelength resolution of SPCE, thus verifying the existence and importance of energy-matching coupling, and the emission for the fluorophore with low excitation efficiency could also be detected. Benefiting from this, the Au NPL-modulated SPCE system could be a candidate for simultaneous multiwavelength enhancement and high-throughput detection in multicomponent analysis.

Diagnosing the Charge Dynamic Behaviors in Quantum-Dot Light-Emitting Diodes by Temperature-Dependent Measurements.

Distinguishing and understanding the nonradiative recombination of charges are crucial for optimizing quantum-dot light-emitting diodes (QLEDs). Auger recombination (AR), a well-known nonradiative process, is widely recognized to occur in QLEDs. However, it has not yet been directly observed in a real working QLED. Here, the AR effect is verified in the QLED at temperatures of <150 K. At low temperatures, the QLED exhibits a unique S-shaped external quantum efficiency (EQE) evolution as the driving current density increases. Experimental and modeling results indicate that this S-shaped EQE results from the asynchronous changes in the behavior of injection of electrons and holes into the quantum-dot emission layer. At low driving voltages, both electron and hole currents are limited by the Fowler-Nordheim (F-N) tunneling behavior. The relatively low barrier for electrons leads to overwhelming electron injection and seriously imbalanced charges in the quantum dots, triggering the AR process. As the voltage increases, the electron current within the emission layer is no longer governed by F-N tunneling but limited by space charges. Then, charge injection becomes balanced, and the EQE increases. These results offer valuable insights into the charge injection and recombination processes within QLEDs, as well as implications for device design.

CdSe quantum dots photoelectric memristors for simulating biological visual system behavior

The visual system is the most important in the biological neurosensory system, so simulation of the biological visual system is the key for developing artificial nervous system. This work incorporates a CdSe quantum dot layer into silk fibroin based memristor device, endowing the devices with light-responsive capability. Furthermore, interesting phenomena were observed when the device operated as artificial synapses: excessive voltage stimulation led to a reduction in synaptic weight compared to the responses observed under normal electrical stimulation. This behavior mirrors sensations associated with pain, neuroprotection, and potential injuries to the neural system. At the end, we designed a visual perception system, simulating processes of the biological light intensity perception and the visual degradation response under intense light stimulation. Our research demonstrates the feasibility of constructing an artificial visual nervous system using a hardware system based on memristors.

Quantitative photothermal investigation of nonradiative recombination parameters in GaAs/InAs(QD)/GaAs quantum dot structures using a three-layer laser beam deflection model

In this paper, we developed a theoretical model for the photothermal deflection technique in order to investigate the electronic parameters of three-layer semiconductor structures. This model is based on the resolution of thermal and photogenerated carrier diffusion-wave equations in different media. Theoretical results show that the amplitude and phase of the photothermal deflection signal is very sensitive to the nonradiative recombination parameters. The theoretical model is applied to one layer of InAs quantum dots (QDs) inserted in GaAs matrix InAs/GaAs QDs in order to investigate the QD density effects on nonradiative recombination parameters in InAs through fitting the theoretical photothermal beam deflection signal to the experimental data. It was found that the minority carrier lifetime and the electronic diffusivity decrease as functions of increasing InAs QD density. This result is also related to the decrease in the mobility from 21.58 to 4.17 (±12.9%) cm2/V s and the minority carrier diffusion length from 0.62 (±5.8%) to 0.14 (±10%) μm, respectively. Furthermore, both interface recombination velocities S2/3 of GaAs/InAs (QDs) and S1/2 of InAs (QDs)/GaAs increase from 477.7 (±6.2%) to 806.5 (±4%) cm/s and from 75 (±7.8%) to 148.1 (±5.5%) cm/s, respectively.

Gradient Hole Injection Inducing Efficient Exciton Recombination in Blue (475 nm) Perovskite QLEDs.

Perovskite quantum dots (QDs) are emerging as excellent light sources for light-emitting diodes (LEDs). However, the performance of blue perovskite QD-based LEDs (QLEDs) still lags behind that of red and green counterparts, which is hindered by blue perovskite QDs with broad bandgaps that tend to increase nonradiative recombination. Here, we designed a gradient energy for hole injection utilizing multiple hole injection layers (HTLs) combined with carbazole-based small-molecule modification to reduce the hole injection barrier between HTLs and QD layers and improve the hole injection efficiency, realizing efficient exciton recombination in blue perovskite QLEDs. Moreover, the QD film on the designed HTLs demonstrates a lower surface roughness and improved photoluminescence properties. The optimized blue CsPbCl3-xBrx QLEDs exhibit an impressive external quantum efficiency of 20.7% with an electroluminescence peak at 475 nm and a turn-on voltage of 2.6 V, representing the state-of-the-art for blue perovskite LEDs emitting in the range of 460-480 nm.

Fullerene‐Free p–i–n Perovskite Solar Cells: Direct Deposition of Tin Oxide on Perovskite Layer Using Ligand Bridges

AbstractIn p–i–n perovskite solar cells (PSCs), fullerene derivatives are predominantly used as an electron transport material (ETM) despite their disadvantages, such as parasitic absorption in the short wavelength range and high cost. State‐of‐the‐art n‐i‐p PSCs are fabricated using SnO2 as the ETM due to their high charge transfer ability, transparency, and low cost. However, in p–i–n PSCs, dispersing SnO2 nanoparticles in a solvent that does not damage the perovskite and forming a uniform layer is challenging. Herein, a strategy of directly depositing SnO2 quantum dots (QDs) on perovskite using ethylenediamine (EDA) for high‐performance applications is reported, which involves a SnO2 QD solution designed with a damage‐free cosolvent. Treating the SnO2 QD layer with the EDA strategy creates a conformal SnO2 QD layer and improves charge transport. This strategy achieves a high power conversion efficiency (PCE) of 18.9% in PSCs with a 1.77 eV bandgap, which is the highest PCE reported for wide bandgap p–i–n PSCs using an inorganic ETM. The top SnO2 layer enables ITO deposition without sputtering damage and achieves a bifacial factor of 99% due to the high transmittance of SnO2 QD. The resulting four‐terminal all‐perovskite tandem exhibited a PCE of 27.0%.

Direct Photopatterning of Colloidal Quantum Dots with Electronically Optimized Diazirine Cross-Linkers.

Colloidal quantum dots (QDs) with a wide color gamut and high luminescent efficiency are promising for next-generation electronic and photonic devices. However, precise and scalable patterning of QDs without degrading their properties and their integration into commercially relevant devices, such as digitally addressable QD light-emitting diode (QLED) displays, remain challenging. Here, we develop electronically optimized diazirine-based cross-linkers for nondestructive, direct photopatterning of QDs and, ultimately, building the active-matrix QLED displays. The key to the cross-linker design is the introduction of electron-donating substituents that permit the formation of ground-state singlet carbenes for air-stable and benign QD photopatterning. Under ambient conditions, these cross-linkers enable the patterning of heavy metal-free QDs at a resolution of over 13,000 pixels per inch using commercial i-line photolithography. The patterned QD layers fully preserved their optical and optoelectronic properties. Pixelated electroluminescent devices with patterned InP/ZnSe/ZnS QD layers show a peak external quantum efficiency of 15.3% and a maximum luminance of about 40,000 cd m-2, outperforming those made by existing QD patterning approaches. We further show the seamless integration of patterned QLEDs with thin-film transistor circuits and the fabrication of dual-color active-matrix displays. These results underscore the importance of designing photochemistry for QD patterning, and promise the implementation of direct photopatterning methods in manufacturing commercial QLED displays and other integrated QD device platforms.

Direct Photo‐Crosslinking Patterning for High‐Performance 0D–2D Hybrid Photodetectors

AbstractHigh‐performance 0D–2D hybrid photodetectors integrated with a crosslinker for direct pattering of quantum dots on the large‐scale synthesized MoS2 layer are reported. In the patterned hybrid structure, QD layers are patterned with a resolution of up to 2 µm, ensuring high precision. Enhanced charge transfer from QDs to 2D materials is confirmed using PL quenching, TR‐PL, and UPS analysis. As a result, the QD/2D hybrid photodetectors with crosslinker‐assisted direct patterning demonstrated a remarkable photoresponsivity of ≈105 A W−1 and a specific detectivity of over 1011 Jones, attributed to the difference in built‐in potential. The crosslinker patterning of QDs opens up potential applications for the photodetectors in highly integrated image sensors and can be further extended to high‐resolution display industries, eliminating unnecessary fabrication processes.

Enhanced detection of cardiac troponin-I using CdSe/CdS/ZnS core-shell quantum dot/TiO2 heterostructure photoelectrochemical sensor

This paper introduces a photoelectrochemical sensor employing red-emitting CdSe/CdS/ZnS core-shell quantum dot/TiO2 heterostructure for detecting cardiac troponin-I (cTnI) biomarkers. The sensor utilizes a photoactive layer-by-layer self-assembly of CdSe/CdS/ZnS nanocrystals within a TiO2 nanoparticle photon-sensitive layer to enhance charge separation, thereby boosting sensor photocurrent. Additionally, the CdSe/CdS/ZnS quantum dot layer enhances photocurrent stability by facilitating the separation of photo-excited electrons and holes. Functionalization of the CdSe/CdS/ZnS core-shell quantum dot/TiO2 heterostructure-based photoelectrochemical sensor with anti-troponin involves first activating -COOH functionalized CdSe/CdS/ZnS with carbodiimide cross-linkers, followed by cTnI protein capture. Photocurrent changes are measured using amperometry. The sensor format exhibits an enhanced photocurrent signal proportional to concentration, with a detection range of 10 pg/mL to 0.2 ng/mL of cTnI protein. The use of a red-emitting CdSe/CdS/ZnS quantum dot layer ensures chemical stability during and after chemical coupling on the sensor. This study showcases the successful application of CdSe/CdS/ZnS core-shell quantum dot/TiO2 heterostructure-based photoelectrochemical sensors for early detection of troponin-I protein in cardiac disease diagnostics.

ETL and HTL Engineering in MAPbI3 based stable and efficient perovskite solar cell with a PbS QD layer using SETFOS 5.3

ETL and HTL Engineering in MAPbI3 based stable and efficient perovskite solar cell with a PbS QD layer using SETFOS 5.3

Colloidal 2D Layered SiC Quantum Dots from a Liquid Precursor: Surface Passivation, Bright Photoluminescence, and Planar Self-Assembly.

We report the bottom-up synthesis of colloidal two-dimensional (2D) layered silicon carbide (SiC) quantum dots with a cubic structure, lateral size of 5-10 nm, ⟨110⟩ exfoliation to few atomic layers, and surface passivation with 1-dodecene. Samples shielded from oxygen and plasma-annealed for purity exhibit narrow blue photoluminescence (PL) with quantum yields (QYs) over 60% in exceptional cases, while unshielded nanocrystals (NCs) exhibit broad blue/green/white PL with 10-15% QY. The latter scenario is attributed to excess surface carbon and oxygen accrued during synthesis and processing, with size separation through ultracentrifugation revealing size-dependent impurity emission. In contrast, the shape of the bright narrow blue PL shows little variation with NC size, while in both scenarios, the maximum QY occurs near four atomic layers. When dried under heat, the disk-like NC suspensions are observed to aggregate into microscale domains, with further self-assembly into planar superlattice domains with common crystalline orientation. The results are compared with photophysical simulations and bring clarity to the broad emission commonly reported for top-down approaches, while inspiring bottom-up schemes directed at improved material quality.

Influence of carrier localization on photoluminescence emission from sub-monolayer quantum dot layers

We have investigated the origins of photoluminescence from quantum dot (QD) layers prepared by alternating depositions of sub-monolayers and a few monolayers of size-mismatched species, termed as sub-monolayer (SML) epitaxy, in comparison with their Stranski–Krastanov (SK) QD counterparts. Using measured nanostructure sizes and local In-compositions from local-electrode atom probe tomography as input into self-consistent Schrödinger–Poisson simulations, we compute the 3D confinement energies, probability densities, and photoluminescence (PL) spectra for both InAs/GaAs SML- and SK-QD layers. A comparison of the computed and measured PL spectra suggests one-dimensional electron confinement, with significant 3D hole localization in the SML-QD layers that contribute to their enhanced PL efficiency in comparison to their SK-QD counterparts.

Effects of Dislocation Filtering Layers on Optical Properties of Third Telecom Window Emitting InAs/InGaAlAs Quantum Dots Grown on Silicon Substrates.

Integrating light emitters based on III-V materials with silicon-based electronics is crucial for further increase in data transfer rates in communication systems since the indirect bandgap of silicon prevents its direct use as a light source. We investigate here InAs/InGaAlAs quantum dot (QD) structures grown directly on 5° off-cut Si substrate and emitting light at 1.5 μm, compatible with established telecom platform. Using different dislocation defect filtering layers, exploiting strained superlattices, and supplementary QD layers, we mitigate the effects of lattice constant and thermal expansion mismatches between III-V materials and Si during growth. Complementary optical spectroscopy techniques, i.e. photoreflectance and temperature-, time- and polarization-resolved photoluminescence, allow us to determine the optical quality and application potential of the obtained structures by comparing them to a reference sample-state-of-the-art QDs grown on InP. Experimental findings are supported by calculations of excitonic states and optical transitions by combining multiband k•p and configuration-interaction methods. We show that our design of structures prevents the generation of a considerable density of defects, as intended. The emission of Si-based structures appears to be much broader than for the reference dots, due to the creation of different QD populations which might be a disadvantage in particular laser applications, however, could be favorable for others, e.g., in broadly tunable devices, sensors, or optical amplifiers. Eventually, we identify the overall most promising combination of defect filtering layers and discuss its advantages and limitations and prospects for further improvements.

Quantum Dot/TiO2 Nanocomposite-Based Photoelectrochemical Sensor for Enhanced H2O2 Detection Applied for Cell Monitoring and Visualization.

This workexploits the possibility of using CdSe/ZnS quantum dot (QD)-electrodes to monitor the metabolism of living cells based on photoelectrochemical (PEC) measurements. To realize that, the PEC setup is improved with respect to an enhanced photocurrent signal, better stability, and an increased signal-to-noise ratio, but also for a better biocompatibility of the sensor surface on which cells have been grown. To achieve this, a QD-TiO2 heterojunction is introduced with the help of atomic layer deposition (ALD). The heterojunction reduces the charge carrier recombination inside the semiconductor nanoparticles and improves the drift behavior. The PEC performance is carefully analyzed by adjusting the TiO2 thickness and combining this strategy with multilayer immobilizations of QDs. The optimal thickness of this coating is ≈5nm; here, photocurrent generation can be enhanced significantly (e.g., for a single QD layer electrode by more than one order of magnitude at 0V vs Ag/AgCl). The resulting optimized electrode is used for hydrogen peroxide (H2O2) sensing with a good sensitivity down to µmolar concentrations, reusability, stability, response rate, and repeatability. Finally, the sensing system is applied to monitor the activity of cells directly grown on top of the electrode surface.

Origin of the Efficiency Roll-off in Quantum Dot Light-Emitting Diodes: An Electrically Excited Transient Absorption Spectroscopy Study.

In situ characterizations of charge injection dynamics, equilibrated concentration, and electric field distributions shed light on the critical mechanisms of quantum dot light-emitting diodes (QD-LEDs). In this work, we developed electrically excited transient absorption spectroscopy, which can provide the above key information, to investigate the efficiency roll-off of QD-LEDs. We found that the average electron populations per QD are low when QD-LEDs exhibit efficiency roll-off, excluding Auger recombination as the main cause. We also revealed that the weak electrical field inside the QD layer under forward biases has a negligible impact on the efficiency. Interestingly, we found that as the voltage increases the electron concentration in the QD layer saturates at very low levels. When combined with the concomitant efficiency roll-off, we propose electron leakage is the main loss at elevated driving voltages. We further demonstrate that increasing the electron confinement potential with the ZnS shell enables us to efficiently mitigate the efficiency roll-off.

Suppressing Charge Extraction Loss in Quantum Dot Infrared Photovoltaics by Optimizing the Charge Transport Layer.

Infrared solar cells (IRSCs), capable of converting low-energy infrared photons to electron-hole pairs, are promising infrared optoelectronic devices because of their extended utilization region of the solar to short-wavelength infrared region. For PbS QDs IRSCs, charge extraction loss, easily generated at the interfaces, has been one of the dominate obstacles impeding the improvement of device efficiencies due to too many trap states and mismatched energy levels between the photoactive layer and electron transport layer (ETL). Herein, an advanced ZnO ETL was developed to improve the extraction of photogenerated charges from the PbS QD photoactive layer to ETLs. The advanced ETL film exhibited effectively suppressed trap states and better-matched energy levels compared with the QD layer. As a consequence, high-performance PbS QD IRSCs with the highest infrared power conversion efficiencies of 1.26% under 1100 nm filtered solar illumination are achieved, suggesting an effective and facile route for enhancing the charge extraction in infrared photovoltaics.

Probing the Operation of Quantum-Dot Light-Emitting Diodes Using Electrically Pumped Transient Absorption Spectroscopy.

The quantum-dot light-emitting diode (QLED) is a new generation light emission source that holds great promise for display and lighting applications. Understanding the dynamics of electrons and holes in QLEDs during their operation is crucial for future QLED optimization, but a time-resolved technology capable of characterizing electrons is still lacking. To tackle this challenge, we develop a unique electrically pumped transient absorption (E-TA) spectroscopy to probe the density of electrons in the QD layer with a nanosecond time resolution. The E-TA result provides a comprehensive understanding of the electron dynamics in QLEDs by quantifying the electron injection time after external voltage on, electron release time after external voltage off, and equilibrated electron density (Ne) in the QD layer during device operation. By combining E-TA technology with time-resolved electroluminescence and transient current measurements, we present a comprehensive overview of the dynamics of both electrons and holes in a QLED during operation.

Chiral 3D structures through multi-dimensional transfer printing of multilayer quantum dot patterns

Three-dimensional optical nanostructures have garnered significant interest in photonics due to their extraordinary capabilities to manipulate the amplitude, phase, and polarization states of light. However, achieving complex three-dimensional optical nanostructures with bottom-up fabrication has remained challenging, despite its nanoscale precision and cost-effectiveness, mainly due to inherent limitations in structural controllability. Here, we report the optical characteristics of intricate two- and three-dimensional nanoarchitectures made of colloidal quantum dots fabricated with multi-dimensional transfer printing. Our customizable fabrication platform, directed by tailored interface polarity, enables flexible geometric control over a variety of one-, two-, and three-dimensional quantum dot architectures, achieving tunable and advanced optical features. For example, we demonstrate a two-dimensional quantum dot nanomesh with tuned subwavelength square perforations designed by finite-difference time-domain calculations, achieving an 8-fold enhanced photoluminescence due to the maximized optical resonance. Furthermore, a three-dimensional quantum dot chiral structure is also created via asymmetric stacking of one-dimensional quantum dot layers, realizing a pronounced circular dichroism intensity exceeding 20°.

Microfluid biosensor for detection of hpv in patient scraping samples: Determining E6 and E7 oncogenes

E6 and E7 oncogenes are pivotal in the carcinogenic transformation in HPV infections and efficient diagnostic methods can ensure the detection and differentiation of HPV genotype. This study describes the development and validation of an electrochemical, label-free genosensor coupled with a microfluidic system for detecting the E6 and E7 oncogenes in cervical scraping samples. The nanostructuring employed was based on a cysteine and graphene quantum dots layer that provides functional groups, surface area, and interesting electrochemical properties. Biorecognition tests with cervical scraping samples showed differentiation in the voltammetric response. Low-risk HPV exhibited a lower biorecognition response, reflected in ΔI% values of 82.33 % ± 0.29 for HPV06 and 80.65 % ± 0.68 for HPV11 at a dilution of 1:100. Meanwhile, high-risk, HPV16 and HPV18, demonstrated ΔI% values of 96.65 % ± 1.27 and 93 % ± 0.026, respectively, at the same dilution. Therefore, the biorecognition intensity followed the order: HPV16 >HPV18 >HPV06 >HPV11. The limit of detection and the limit of quantification of E6E7 microfluidic LOC−Genosensor was 26 fM, and 79.6 fM. Consequently, the E6E7 biosensor is a valuable alternative for clinical HPV diagnosis, capable of detecting the potential for oncogenic progression even in the early stages of infection.

Chiral Perovskite Heterostructure Films of CsPbBr3 Quantum Dots and 2D Chiral Perovskite with Circularly Polarized Luminescence Performance and Energy Transfer.

This work reports the synthesis of chiral perovskite heterostructure films by combining a two-dimensional (2D) chiral (R-/S-MBA)2PbI4 perovskite with CsPbBr3 quantum dots (QDs). The as-synthesized chiral heterostructure films exhibit obvious circularly polarized luminescence (CPL) properties, even though pure 2D chiral perovskite cannot present photoluminescence. It indicates that the chirality of the excited state of the QDs originates from the 2D chiral perovskite. The circular polarization-resolved transient absorption (TA) spectra further demonstrate that the CPL response of heterostructure films originates from the energy transfer between the chiral perovskite layer and QDs layer and the suppression of spin relaxation, which induces the imbalance of the spin population of excited states in QDs layer. In addition, the photoluminescence (PL), circular dichroism (CD), and CPL spectra of these heterostructure films can be controlled by varying the thickness and component of the chiral perovskite layer, which demonstrates that the anion exchange between chiral perovskite and CsPbBr3 QDs can tune the chemical composition and optoelectronic properties due to the low bonding energy difference between them and decrease the strain within the QDs layer to reduce the radiative recombination lifetime. This work provides guidance for the synthesis of chiral perovskites with a strong CPL response and further provides insight into the origination of CPL.