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Digital histogram generation for time-resolved measurements with single-photon avalanche diode (SPAD) sensors requires the storage of many timestamp signals. This work presents a mixed-signal time-to-digital converter (TDC) that uses analog storage to achieve an area-efficient design that can be integrated in large SPAD arrays. Fabricated using a 150 nm CMOS process, the prototype occupies an area of only 18.3 µm × 36.5 µm, a notable size reduction compared to conventional designs. The experimental results demonstrated high performance, with an integral nonlinearity (INL) of 0.35/0.14 least significant bit (LSB) and a differential nonlinearity (DNL) of 0.14/-0.12 LSB. In addition, the proposed TDC can support the construction of histograms comprising up to 512 bins, making it an effective solution to accommodate a wide range of resolution requirements. Validated in a point-of-care (PoC) device for fluorescence lifetime measurements, it distinguished between lifetimes of approximately 4.1 ns, 3.6 ns and 80 ns with the Alexa Fluor (AF) 546 and 568 dyes and Quantum Dot (QD) 705, respectively. The analog storage design and area-efficient architecture offer a novel approach to integrating TDCs in SPAD-based systems, with potential applications in medical diagnostics and beyond.

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Nowadays, the extensively used lead sulfide (PbS) quantum dot (QD) hole transport layer (HTL) relies on layer-by-layer method to replace long chain oleic acid (OA) ligands with short 1,2-ethanedithiol (EDT) ligands for preparation. However, the inevitable significant volume shrinkage caused by this traditional method will result in undesired cracks and disordered QD arrangement in the film, along with adverse increased defect density and inhomogeneous energy landscape. To solve the problem, a novel method for EDT passivated PbS QD (PbS-EDT) HTL preparation using small-sized benzoic acid (BA) as intermediate ligands is proposed in this work. BA is substituted for OA ligands in solution followed by ligand exchange with EDT layer by layer. With the new method, smoother PbS-EDT films with more ordered and closer QD packing are gained. It is demonstrated stronger coupling between QDs and reduced defects in the QD HTL owing to the intermediate BA ligand exchange. As a result, the suppressed nonradiative recombination and enhanced carrier mobility are achieved, contributing to ≈20% growth in short circuit current density (Jsc) and a 23.4% higher power conversion efficiency (PCE) of 13.2%. This work provides a general framework for layer-by-layer QD film manufacturing optimization.

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Inkjet printing is a powerful direct material writing process. It can be used to deposit microfluidic droplets in designated patterns at submicrometer resolution, which reduces materials usage. Nonetheless, predicting jetting characterizations is not easy because of the intrinsic complexity of the ink-nozzle-air interactions. Thus, inkjet processes are monitored by skilled engineers to ensure process reliability. This is a bottleneck in industry, resulting in high labor costs for multiple nozzles. To address this, we present a deep learning-based method for jetting characterizations. Inkjet printing is recorded by an in situ CCD camera and each droplet is detected by YOLOv5, a 1-stage detector using a convolutional neural network (CNN). The precision, recall, and mean average precision (mAP) at a 0.5 intersection over the union (IoU) threshold of the trained model were 0.86, 0.89, and 0.90, respectively. Each regression result for a detected droplet is accumulated in chronological order for each class of droplet and nozzle. The quantified information includes velocity, diameter, length, and translation, which can be used to synchronize multinozzle jetting and, eventually, the printed patterns. This demonstrates the feasibility of autonomous real-time process testing for large-scale electronics manufacturing, such as the high-resolution patterning of biosensor electrodes and QD display pixels while exploiting big data obtained from jetting characterizations.

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A defect-passivated photosensor based on cesium lead bromide (CsPbBr3) perovskite quantum dots (QD) was fabricated using parylene films, and the photosensor was applied for the microbial detection. The CsPbBr3 perovskite QDs were synthesized to be homogeneous in size under thermodynamic control, and the perovskite QD-based photosensor was fabricated using MoS2 flakes as the electron transfer layer. In this work, a parylene film with functional groups was deposited on a photosensor for physical protection (waterproof) and defect (halide vacancy) passivation of the perovskite QD. As the first effect of the parylene film, the physical protection of the perovskite QD from water was estimated by comparing the photosensor performance after incubation in water. As the second effect of the parylene, the interaction between the functional groups of the parylene film and the halide vacancies of the perovskite QDs was investigated through the bandgap, crystal structure, and trap-state density analysis. Additionally, density functional theory analysis on Mulliken charges, lattice parameters, and Gibbs free energy demonstrated the effect of the defect passivation by parylene films. Finally, the parylene-passivated QD-based photosensor was applied to the detection of two kinds of food-poisoning and gastroduodenal disease bacteria (Listeria monocytogenes and Helicobacter pylori).

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CONTEXT: In this paper, we simulate a single-molecule diode to calculate the effective coupling and investigate the conductivity, as well as the effect of the electric field on these two parameters. First, we obtain the molecule states and energies at 0 V. The next step is to calculate the electrode/molecule coupling using the obtained electrode and molecule Hamiltonian. The electrode/molecule coupling depends on distance. By increasing the distance from 5 to 5.5 angstroms, the coupling decreases from 0.004 to 0.0002 eV. After calculating the electrode/molecule coupling, which is the most significant parameter in electron transfer, the results can be used to obtain the current-voltage and conductivity curves of the device. Simulation results demonstrate that externally applied electric field to the benzene molecule (isolated molecule) can cause a reduction in the effective coupling between the Au electrode and benzene, leading to decreased current and conductivity. Additionally, the applied electric field narrows the gap between the HOMO and LUMO energy levels. METHODS: We conducted this computational work using Gaussian 09 software and a MATLAB code, both of which are based on the density functional theory (DFT) approach and the self-consistent field (SCF) method. For DFT calculations, we employed the three-parameter Beck hybrid exchange functional (B3), hybridized with the nonlocal correlation functional developed by Lee, Yang, and Parr (LYP). All optimizations were performed with triple-zeta polarized (TZP) split-valence 6-311G basis sets. The final step involved calculating the electrode/molecule coupling using the Huckel method and integrating the site-to-state transformation with Huckel parameters and the Fermi golden rule. After this calculation, we obtained the current-voltage and conductivity curves using MATLAB software.

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Charge imbalance in quantum-dot light-emitting diodes (QLEDs) causes emission degradation. Therefore, many studies focused on improving hole injection into the QLEDs-emitting layer owing to lower hole conductivity compared to electron conductivity. Herein, CuCo2O4 has a relatively higher hole conductivity than other binary oxides and can induce an improved charge balance. As the annealing temperature decreases, the valence band maximum (VBM) of CuCo2O4 shifts away from the Fermi energy level (EF), resulting in an enhanced hole injection through better energy level alignment with hole transport layer. The maximum luminance and current efficiency of the CuCo2O4 hole injection layer (HIL) of the QLED were measured as 93,607 cd/m2 and 11.14 cd/A, respectively, resulting in a 656% improvement in luminous performance of QLEDs compared to conventional metal oxide HIL-based QLEDs. These results demonstrate that the electrical properties of CuCo2O4 can be improved by adjusting the annealing temperature, suggesting that solution-processed spinel can be applied in various optoelectronic devices.

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Perovskite CsPbI3 quantum dots (QDs) were synthesized as a hole-transporting layer (HTL) of a planar perovskite solar cell (PSC). By using the Octam solution during the ligand engineering, CsPbI3 QDs exhibits a denser grain and a larger grain size due to the short-chain ligands of Octam. In addition, CsPbI3 QDs with the Octam solution showed a smooth and uniform surface on MAPbI3 film, indicating the QDs improved the microstructure of the MAPbI3 perovskite film. As a result, the PSC with CsPbI3 QDs as an HTL has the optimal open-circuit voltage as 1.09 V, the short-circuit current as 20.5 mA/cm2, and the fill factor (FF) as 75.7%, and the power conversion efficiency (PCE) as 17.0%. Hence, it is inferred that introducing QDs as a HTL via the ligand engineering can effectively improve the device performance of the PSC.

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In this study, blue perovskite quantum dots (PQDs) were prepared using didodecyldimethylammonium bromide (DDAB), which can passivate surface defects caused by the loss of surface ligands and reduce particle size distribution. After the passivation of DDAB, blue CsPbClxBr3-x PQDs dispersed in n-octane produced a more compact and uniform PQD thin film than the non-passivated ones. The resulting device showed a stabile lifetime, and an EL peak of 470 nm and a maximum EQE of 1.63% were obtained at an operating voltage of 2.6 V and a current density of 0.34 mA/cm2. This work aims to provide a simple method to prepare blue-emitting PQDs and high-performance PQD-based light-emitting devices.

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By virtue of its high sensitivity, bioluminescence imaging (BLI) is an important tool for biosensing and bioimaging in life sciences. Compared to fluorescence imaging (FLI), BLI has a superior advantage that the background signals resulting from autofluorescence are almost zero due to the unnecessity of external excitation. In addition, BLI can permit a long-term observation of living cells because BL results in very low photocytotoxicity toward the host cells. Although BLI has such superior properties over FLI, the available wavelengths in BLI are mostly limited to the visible region. Here we present bioluminescence resonance energy transfer (BRET)-based visible and near-infrared dual-color molecular imaging using a quantum dot (QD) and luciferase-protein conjugate.

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Zinc oxide (ZnO) nanowire (NW) based lead sulfide (PbS) quantum dot solar cells (QDSCs), i.e., bulk heterojunction QDSCs, have been widely investigated because of the excellent photoelectronic properties of PbS QDs and ZnO NWs. To further improve the efficiency of this type of QDSCs, various passivation methods are applied to ZnO NWs to suppress interface recombination caused by trap defects. However, the comparison among passivation using organic, inorganic, and inorganic-organic hybrid materials with different properties has been less studied. In this work, the effect of passivation with inorganic Mg-doped ZnO (ZMO), organic 1,2-ethanedithiol (EDT) and both of them on ZnO NWs and PbS QDSCs are investigated. As a result, ZnO NWs purely passivated by organic material EDT show the best performance with fewer surface defects and better matched energy level with the PbS QD layer. A nearly 1.7 times larger power conversion efficiency (PCE) of 6.9% is achieved for the solar device using ZnO NW @EDT, compared with that (4.1%) of the untreated one. The work provides a promising way to impede interlayer charge recombination and facilitate carrier transport, thus enhancing the photovoltaic performance of the device.

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Quantum dots (QDs) are semiconductor nanoparticles with outstanding optoelectronic properties. More specifically, QDs are highly bright and exhibit wide absorption spectra, narrow light bands, and excellent photovoltaic stability, which make them useful in bioscience and medicine, particularly for sensing, optical imaging, cell separation, and diagnosis. In general, QDs are stabilized using a hydrophobic ligand during synthesis, and thus their hydrophobic surfaces must undergo hydrophilic modification if the QDs are to be used in bioapplications. Silica-coating is one of the most effective methods for overcoming the disadvantages of QDs, owing to silica's physicochemical stability, nontoxicity, and excellent bioavailability. This review highlights recent progress in the design, preparation, and application of silica-coated QDs and presents an overview of the major challenges and prospects of their application.

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We have studied the parallel and perpendicular electric field effects on the system of SiGe prolate and oblate quantum dots numerically, taking into account the wetting layer and quantum dot size effects. Using the effective-mass approximation in the two bands model, we computationally calculated the extensive variation of dipole matrix (DM) elements, bandgap and non-linear optical properties, including absorption coefficients, refractive index changes, second harmonic generation and third harmonic generation as a function of the electric field, wetting layer size and the size of the quantum dot. The redshift is observed for the non-linear optical properties with the increasing electric field and an increase in wetting layer thickness. The sensitivity to the electric field toward the shape of the quantum dot is also observed. This study is resourceful for all the researchers as it provides a pragmatic model by considering oblate and prolate shaped quantum dots by explaining the optical and electronic properties precisely, as a consequence of the confined stark shift and wetting layer.

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From molecular probes, also known as fluorophores (typically emitting a longer wavelength than the absorbing wavelength), to inorganic nanoparticles, various light-emitting materials have been actively studied and developed for various applications in life science owing to their superior imaging and sensing ability. Especially after the breakthrough development of quantum dots (QDs), studies have pursued the development of the optical properties and biological applications of luminescent inorganic nanoparticles such as upconversion nanoparticles (UCNPs), metal nanoclusters, carbon dots, and so on. In this review, we first provide a brief explanation about the theoretical background and traditional concepts of molecular fluorophores. Then, currently developed luminescent nanoparticles are described as sensing and imaging platforms from general aspects to technical views.

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In this review, we focus on sensing techniques and biological applications of various luminescent nanoparticles including quantum dot (QD), up-conversion nanoparticles (UCNPs) following the previous chapter. Fluorescent phenomena can be regulated or shifted by interaction between biological targets and luminescence probes depending on their distance, which is so-called FÓ§rster resonance energy transfer (FRET). QD-based FRET technique, which has been widely applied as a bioanalytical tool, is described. We discuss time-resolved fluorescence (TRF) imaging and flow cytometry technique, using photoluminescent nanoparticles with unique properties for effectively improving selectivity and sensitivity. Based on these techniques, bioanalytical and biomedical application, bioimaging with QD, UCNPs, and Euripium-activated luminescent nanoprobes are covered. Combination of optical property of these luminescent nanoparticles with special functions such as drug delivery, photothermal therapy (PTT), and photodynamic therapy (PDT) is also described.

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We investigated the effect of intense-pulsed light (IPL) post-treatment on the time-dependent characteristics of ZnO nanoparticles (NPs) used as an electron transport layer (ETL) of quantum-dot light-emitting diodes (QLEDs). The time-dependent characteristics of the charge injection balance in QLEDs was observed by fabrication and analysis of single carrier devices (SCDs), and it was confirmed that the time-dependent characteristics of the ZnO NPs affect the device characteristics of QLEDs. Stabilization of the ZnO NPs film properties for improvement of the charge injection balance in QLEDs was achieved by controlling the current density characteristics via filling of the oxygen vacancies by IPL post-treatment.

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Optimization of ink-jet printing conditions of quantum-dot (QD) ink by cosolvent process and improvement of quantum-dot light-emitting diodes (QLEDs) characteristics assisted by vacuum annealing were analyzed in this research. A cosolvent process of hexane and ortho-dichlorobenzene (oDCB) was optimized at the ratio of 1:2, and ink-jetting properties were analyzed using the Ohnesorge number based on the parameters of viscosity and surface tension. However, we found that these cosolvents systems cause an increase in the boiling point and a decrease in the vapor pressure, which influence the annealing characteristics of the QD emission layer (EML). Therefore, we investigated QLEDs' performance depending on the annealing condition for ink-jet printed QD EML prepared using cosolvents systems of hexane and oDCB. We enhanced the quality of QD EML and device performance of QLEDs by a vacuum annealing process, which was used to prevent exposure to moisture and oxygen and to promote effective evaporation of solvent in QD EML. As a result, the characteristics of QLEDs formed using ink-jet printed QD EML annealed under vacuum environment increased luminescence (L), current efficiency (CE), external quantum efficiency (EQE), and lifetime (LT50) by 30.51%, 33.7%, 21.70%, and 181.97%, respectively, compared to QLEDs annealed under air environment.

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Graphene quantum dots (QDs) are intensively studied as platforms for the next generation of quantum electronic devices. Fine tuning of the transport properties in monolayer graphene QDs, in particular with respect to the independent modulation of the tunnel barrier transparencies, remains challenging and is typically addressed using electrostatic gating. We investigate charge transport in back-gated graphene mechanical break junctions and reveal Coulomb blockade physics characteristic of a single, high-quality QD when a nanogap is opened in a graphene constriction. By mechanically controlling the distance across the newly formed graphene nanogap, we achieve reversible tunability of the tunnel coupling to the drain electrode by 5 orders of magnitude, while keeping the source-QD tunnel coupling constant. The break junction device can therefore become a powerful platform to study the physical parameters that are crucial to the development of future graphene-based devices, including energy converters and quantum calorimeters.

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Antibody microarrays have become a powerful tool in multiplexed immunoassay technologies. The advantage of microarray technology is the possibility of rapid analysis of multiple targets in a single sample with a high sensitivity, which makes them ideal for high throughput screening. Usually these microarrays contain biological recognition molecules, such as full-size antibodies, antigen-binding fragments, and single-domain antibodies, and a label for detection. Organic fluorophores are the most popular labels, but they suffer from low sensitivity and instability due to their photodegradation. Here, we describe a protocol for fabricating an antibody microarray with highly fluorescent semiconductor nanocrystals or quantum dots (QDs) as the source of fluorescent signals, which may significantly improve the properties of microarrays, including their sensitivity and specificity. Our approach to analyte detection is based on the use of sandwich approach with streptavidin-biotin to assess and monitor the fluorescence signal instead of direct labeling of samples, which helps improve the reproducibility of results and sensitivity of the microarrays. The antibody microarray developed has been tested for its capacity of detecting DNA-PKcs in glial cell lines and measuring cell protein phosphorylation changes caused by camptothecin-induced DNA damage with different protein kinase inhibitors in HeLa cells.

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The performance of colloidal quantum dot light-emitting diodes (QD-LEDs) have been rapidly improved since metal oxide semiconductors were adopted for an electron transport layer (ETL). Among metal oxide semiconductors, zinc oxide (ZnO) has been the most generally employed for the ETL because of its excellent electron transport and injection properties. However, the ZnO ETL often yields charge imbalance in QD-LEDs, which results in undesirable device performance. Here, to address this issue, we introduce double metal oxide ETLs comprising ZnO and tin dioxide (SnO2) bilayer stacks. The employment of SnO2 for the second ETL significantly improves charge balance in the QD-LEDs by preventing spontaneous electron injection from the ZnO ETL and, as a result, we demonstrate 1.6 times higher luminescence efficiency in the QD-LEDs. This result suggests that the proposed double metal oxide ETLs can be a versatile platform for QD-based optoelectronic devices.

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Bacteria naturally alter the redox state of many compounds and perform atom-by-atom nanomaterial synthesis to create many inorganic materials. Recent advancements in synthetic biology have spurred interest in using biological systems to manufacture nanomaterials, implementing biological strategies to specify the nanomaterial characteristics such as size, shape, and optical properties. Here, we combine the natural synthetic capabilities of microbes with engineered genetic control circuits toward biogenically synthesized semiconductor nanomaterials. Using an engineered strain of Shewanella oneindensis with inducible expression of the cytochrome complex MtrCAB, we control the reduction of manganese (IV) oxide. Cytochrome expression levels were regulated using an inducer molecule, which enabled precise modulation of dopant incorporation into manganese doped zinc sulfide nanoparticles (Mn:ZnS). Thereby, a synthetic gene circuit controlled the optical properties of biogenic quantum dots. These biogenically assembled nanomaterials have similar physical and optoelectronic properties to chemically synthesized particles. Our results demonstrate the promise of implementing synthetic gene circuits for tunable control of nanomaterials made by biological systems.