PbS Colloidal Quantum Dots Research Articles

Optical engineering of PbS colloidal quantum dot solar cells via Fabry–Perot resonance and distributed Bragg reflectors

A tradeoff between light absorption and charge transport is a well-known issue in PbS colloidal quantum dot (CQD) solar cells because the carrier diffusion length in PbS CQD films is comparable to the thickness of CQD film. We reduce the tradeoff between light absorption and charge transport by combining a Fabry–Perot (FP) resonator and a distributed Bragg reflector (DBR). A FP resonance is formed between the DBR and a dielectric-metal-dielectric film as a top transparent electrode. A SiO2-TiO2 multilayer is used to form a DBR. The FP resonance enhances light absorption near the resonant wavelength of the DBR without changing the CQD film thickness. The light absorption near the FP resonance wavelength is further boosted by coupling the FP resonance with the high reflectivity of the Ag-coated DBR. When the FP resonance and DBR are combined, the power conversion efficiency (PCE) of PbS CQD solar cells increases by 54%. Moreover, the DBR assisted FP resonance enables a very thin PbS layer to absorb near infrared light four times more. The overall PCE of the thin PbS CQD solar cell increases by 24% without sacrificing the average visible transmittance (AVT). Our results show how to overcome the inherence problem of the CQD and develop a semi-transparent solar cell where the wavelength-selective absorption and the transparency for visible light are important.

A Broadband Photodetector Based on PbS Quantum Dots and Graphene with High Responsivity and Detectivity.

A high-efficiency photodetector consisting of colloidal PbS quantum dots (QDs) and single-layer graphene was prepared in this research. In the early stage, PbS QDs were synthesized and characterized, and the results showed that the product conformed with the characteristics of high-quality PbS QDs. Afterwards, the photodetector was derived through steps, including the photolithography and etching of indium tin oxide (ITO) electrodes and the graphene active region, as well as the spin coating and ligand substitution of the PbS QDs. After application testing, the photodetector, which was prepared in this research, exhibited outstanding properties. Under visible and near-infrared light, the highest responsivities were up to 202 A/W and 183 mA/W, respectively, and the highest detectivities were up to 2.24 × 1011 Jones and 2.47 × 108 Jones, respectively, with light densities of 0.56 mW/cm2 and 1.22 W/cm2, respectively. In addition to these results, the response of the device and the rise and fall times for the on/off illumination cycles showed its superior performance, and the fastest response times were approximately 0.03 s and 1.0 s for the rise and fall times, respectively. All the results illustrated that the photodetector based on PbS and graphene, which was prepared in this research, possesses the potential to be applied in reality.

Minority carrier diffusion length in interface-confined PbS colloidal quantum dot (CQD): Effect of CQD surface modification on diffusion length in ultrathin PbS CQD films

Photocurrent microscopy (PCM) is a versatile tool for probing charge carrier transport associated with energy band bending at an interface. For the first time, we report the ligand-dependent electronic properties of interface-confined colloidal quantum dots (CQDs) near a metal electrode and gate dielectric layers using ultrathin lead sulfide (PbS) CQD films embedded in field effect transistors (FETs). We have compared the minority carrier (electron) diffusion length (MCDL) of ultrathin PbS CQD films treated with 1,2-ethanedithiol (EDT) and ammonium sulfide ((NH4)2S) using a bottom-contact FET structure in combination with PCM. We found that the MCDL was greater in the EDT-treated PbS CQDs than in the (NH4)2S-treated PbS CQDs. The MCDL at the 2D carrier accumulation layer was observed to depend on the concentration of the majority carrier (hole). During effective electrical channel formation by electrical gating, the MCDL decreased with hole accumulation (decreasing gate voltage) in the p-channel (NH4)2S-treated PbS CQD FET, whereas it remained similar in the EDT-treated PbS CQD FET. The effect of the majority carrier concentration on the MCDL was more pronounced in the (NH4)2S-treated sample than in the EDT-treated sample. The difference in the MCDL is attributed to a difference in the surface trap density caused by different ligand treatments.

PHOTOSENSITIVITY OF PbS COLLOIDAL QUANTUM DOTS BASED NANOSTRUCTURES WITH AN ENERGY BARRIER

A new architecture of photosensitive elements for the near (0.7–1.4 μm) and short-wavelength (1.4–3.0 μm) infrared regions of the spectrum based on hybrid nanostructures consisting of PbS colloidal quantum dots and functional layers of ZnO and AgNW silver nanowires is proposed. Small-sized (12 × 12 μm) photosensitive elements with an energy barrier at the contact between layers of n- and p-type CQDs have been studied. The current-voltage characteristics, spectral dependences of optical absorption and relative spectral photosensitivity of Si(λ)/Si(λmax) barrier structures at room temperature have been studied. It is shown that the proposed architecture of barrier structures provides photosensitivity in a wide spectral range from 0.4 µm to 2.0 µm. An excess of the average value of the relative spectral sensitivity Si(λ)/Si(λmax) about 1.5 times compared to those previously observed in the wavelength range of 0.9–1.85 μm for barrier nanostructures from PbS CQDs was found.

Optical engineering of infrared PbS CQD photovoltaic cells for wireless optical power transfer systems

Infrared photovoltaic cells (IRPCs) have attracted considerable attention for potential applications in wireless optical power transfer (WOPT) systems. As an efficient fiber-integrated WOPT system typically uses a 1550 nm laser beam, it is essential to tune the peak conversion efficiency of IRPCs to this wavelength. However, IRPCs based on lead sulfide (PbS) colloidal quantum dots (CQDs) with an excitonic peak of 1550 nm exhibit low short circuit current (Jsc) due to insufficient absorption under monochromatic light illumination. Here, we propose comprehensive optical engineering to optimize the device structure of IRPCs based on PbS CQDs, for 1550 nm WOPT systems. The absorption by the device is enhanced by improving the transmittance of tin-doped indium oxide (ITO) in the infrared region and by utilizing the optical resonance effect in the device. Therefore, the optimized device exhibited a high short circuit current density of 37.65 mA/cm2 under 1 sun (AM 1.5G) solar illumination and 11.91 mA/cm2 under 1550 nm illumination 17.3 mW/cm2. Furthermore, the champion device achieved a record high power conversion efficiency (PCE) of 7.17% under 1 sun illumination and 10.29% under 1550 nm illumination. The PbS CQDs IRPCs under 1550 nm illumination can even light up a liquid crystal display (LCD), demonstrating application prospects in the future.Graphical

Fluorescence enhancement of PbS colloidal quantum dots from silicon metasurfaces sustaining bound states in the continuum

Abstract PbS colloidal quantum dots (CQDs) can be considered a promising lighting material, but their emission performance is mired by defect sites, strong photo-induced activity, and interaction with the environment. Here, we utilize periodic silicon metasurface sustaining a symmetry-protected bound state in the continuum to enhance the near-infrared emission of PbS CQDs at room temperature. In the experimental investigation, it is observed that the fluorescence of the coated PbS CQDs is enhanced by 10 times by the fabricated metasurface, and the emission peak has a quality factor up to 251 at wavelength 1408 nm. Meanwhile, the potential of this work in sensing is demonstrated by showing that the enhanced emission is disturbed by the introduction of sparse gold nanoparticles. In all, this work confirms that dielectric metasurfaces sustaining bound states in the continuum can be adopted to efficiently improve the emission performance of PbS CQDs which may find various practical applications including on-chip silicon-based optical sources and integrated sensors.

Quantum Dot-Siloxane Anchoring on Colloidal Quantum Dot Film for Flexible Photovoltaic Cell.

Lead sulfide (PbS) colloidal quantum dots (CQDs) are promising materials for next-generation flexible solar cells because of near-infrared absorption, facile bandgap tunability, and superior air stability. However, CQD devices still lack enough flexibility to be applied to wearable devices owing to the poor mechanical properties of CQD films. In this study, a facile approach is proposed to improve the mechanical stability of CQDs solar cells without compromising the high power conversion efficiency (PCE) of the devices. (3-aminopropyl)triethoxysilane (APTS) is introduced on CQD films to strengthen the dot-to-dot bonding via QD-siloxane anchoring, and as a result, crack pattern analysis reveals that the treated devices become robust to mechanical stress. The device maintains 88% of the initial PCE under 12000 cycles at a bending radius of 8.3mm. In addition, APTS forms a dipole layer on CQD films, which improves the open circuit voltage (VOC ) of the device, achieving a PCE of 11.04%, one of the highest PCEs in flexible PbS CQD solar cells.

Carbon Nanotube Transistor with Colloidal Quantum Dot Photosensitive Gate for Ultrahigh External Quantum Efficiency Photodetector

PbS colloidal quantum dots (CQDs) are promising building block for developing the next-generation high-performance near-infrared (NIR) photodetector. However, due to the surface ligand isolation and surface defects, PbS CQDs usually suffer from low carrier mobility, which limits further optimization of PbS CQDs-based optoelectronic devices. Here, the combination of PbS CQD photodiode and carbon nanotube (CNT) film field-effect transistor (FET) achieves a transistorized NIR photodetector with a photosensitive gate. The photogenerated electrons are drifted to the dielectric surface by a negative gate electric field and built-in electric field, serving as an equivalent gate voltage to turn on the CNT FET, thus realizing the conversion of optical signals to electrical signals. The photodetector exhibits high performance, with a responsivity and detectivity of 41.9 A/W and 3.04 × 1011 Jones under 950 nm illumination, respectively. More importantly, the photodetector achieves an ultrahigh external quantum efficiency (EQE) of 5470% due to the CNT FET amplification function. Besides, the photodetector demonstrates a versatile photoresponse that allows for regulation of responsivity, detectivity, and EQE over a wide range through gate voltage control. The photodetector shows immense potential in NIR photodetection applications, and the distinctive structure of the optical module and electrical module separation also provides fresh thinking for the research and development of the next generation of optoelectronic devices.

Photosensitising reactive oxygen species with titanium dioxide nanoparticles decorated with PbS quantum dots

The development of new efficient photocatalysts based on nanostructured materials with a wide range of photosensitivity in visible and near-infra-red regions and high efficiency of reactive oxygen species generation is an important task. The purpose of this project was to establish the possibility of photosensitising the process of generating reactive oxygen species (ROSs) with TiO2 nanoparticles (NPs) decorated with colloidal PbS quantum dots (QDs) passivated with 3-mercaptopropionic acid (3MPA) as well as the possibility of increasing the spectral sensitivity of synthesised nanoheterosystems into the redregion. The paper analyses the photocatalytic properties of TiO2 NPs with an anatase structure and average size of 12 nm decorated with colloidal PbS QDs with an average size of 2.7 nm passivated with 3MPA. It also provides structural and spectral substantiation of the formation of TiO2 NPs – PbS/3MPA QDs nanoheterostructures. Absorption and luminescence techniques were used to establish the efficiency of generating various ROSs by TiO2 NPs – PbS/3MPA nanoheterostructures and their individual components under excitation in the UV and visible radiation. It was shown that TiO2 NPs decoration with PbS QDs extends the spectral range of sensitivity to the generation of reactive oxygen species in the UV to 1,100 nm. The study revealed an increased efficiency of hydrogen peroxide generation by nanoheterostructures as compared to individual PbS QDs and TiO2 nanoparticles.

Trap state and exciton luminescence of colloidal PbS quantum dots coated with thioglycolic acid molecules

This work presents the results of studying the IR luminescence of colloid PbS quantum dots coated with molecules of thioglycolic acid. Luminescence of the sample was recorded using the InGaAs image sensor PDF 10C/M (ThorlabsInc., USA) and a diffraction monochromator with 600 mm-1 grating. To study the temperature dependence of luminescence, the sample was cooled in a nitrogen cryostat down to 80 К. A redistribution of the luminescence intensity between two peaks (1100 and 1280 nm) was identified upon a decrease in temperature. It was shown that an exciton absorption peak was present in the excitationspectrum for the short-wave luminescence peak, and the Stokes shift was ΔEstokes ~ 0.1 eV. On the contrary, the exciton peak was absent in the luminescence excitation spectrum of the long-wave band, and its red boundary was shifted towards the short-wave region, that provided the Stokes shift of more than 0.3 eV. It was concluded that the short-wave luminescence band appeared as a result of the radiative annihilation of an exciton, while the long-wave band appeared due to the recombination of charge carriers at trap states. Trap state luminescence was effectively excited upon direct absorption of the radiation by the luminescence centre. A three-level diagram was suggested that determined the IR luminescence of colloid PbS quantum dots coated with thioglycolic acid molecules.

Photo-sensitive Structures with Cascade Radiation Concentrators Based on Colloidal Quantum Dots of Metal Chalcogenides

Introduction . The problem of increasing the efficiency of existing photodetectors and creating their new types attracts much research attention. Among new photodetector types are photosensitive structures based on cascade concentrators, whose operational principle involves the absorption of optical radiation followed by its reemission at a longer wavelength and radiation concentration onto a highly efficient small-area photodetector. The absorption and re-emission spectra of each cascade layer depend on the characteristics of the material used. Сolloidal quantum dots are among the most promising materials for cascade layers due to their manufacturing technology, which provides for accurate control over the photoluminescence maximum position. It seems highly relevant to develop and to study photosensitive structures with cascade concentrators of various shapes based on CdS, CdSe/ZnS, and PbS colloidal quantum dots. Aim . To develop photosensitive structures with a wide-range sensitivity spectrum based on concentrators containing arrays of metal chalcogenide CQDs and to study their characteristics. Materials and methods . Cascade photosensitive structures were manufactured based on layers made of polymethyl methacrylate and layers of colloidal quantum dots embedded in a polystyrene matrix. Results . Three-layer concentrators were manufactured with different colloidal quantum dots in each concentrator layers. A 22 % increase in the output power was observed for a three-layer cascade structure based on different cascade layer materials compared to a similar structure using a single layer concentrator. Conclusion . The conducted studies showed an increase in the efficiency of photosensitive structures with a cascade concentrator based on colloidal quantum dots of various types (CdS, CdSe/ZnS, and PbS) in the cascade layers.

High-Radiance Shortwave Infrared Light-Emitting Diodes Based on Highly Stable PbS Colloidal Quantum Dots

PbS quantum dot light-emitting diodes (QLEDs) emitting around 1550 nm promise important applications in optical communications. However, due to insufficient suppression of surface traps for large-size PbS quantum dots (QDs), their performance under large driving current density was not satisfactory. In this work, octanethiol surfactant was added into a PbS QD solution and adsorbed onto the dot surface. As a result, the surface traps and the continuous oxidation of the unprotected (100) facets in PbS QDs were greatly suppressed. Therefore, the PbS QDs with octanethiol doubled their photoluminescence efficiency and showed outstanding stability. The PbS-based QLEDs with benchmark device structure showed a breakthrough high radiance of 18.3 W sr-1 m-2 with >2000 mA/cm2 driving current density. The efficient passivation of surface traps with octanethiol surfactant and the suppressed coupling between excitons and surface states under large working current were the main reasons for achieving the breakthrough high radiance.

Stabilization of PbS colloidal-quantum-dot gas sensors using atomic-ligand engineering

Colloidal quantum dots (CQDs) are promising materials candidates for next-generation semiconductor gas sensors, due to their high surface activity and solution-processability. Despite the improved sensitivity demonstrated by PbS CQDs, their long-term stability remains a challenge for practical applications. In this paper, we propose a stabilization strategy for PbS CQD gas sensors by using atomic-ligand engineering. The oleic acid ligands surrounding PbS CQDs are replaced by halide ligands (Cl–, Br– and I–, respectively) via a phase-transfer ligand exchange method. The sensitivity and long-term stability of the PbS CQD gas sensor towards nitrogen dioxide (NO2) at room temperature are impressively improved. The excellent humidity stability of the iodine ligand exchanged PbS CQD gas sensor is also demonstrated. The mechanism is investigated by real-time electrical measurement, combined with operando diffuse reflection Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy analysis. The results indicate that the large atomic radius and high binding energy of iodide ligands enhance surface passivation and provide favorable conditions for NO2 adsorption and charge transfer. This study highlights the importance of surface ligand engineering in the development of practical CQD gas sensors.

Extended wavelength and enhanced sensitivity of PbS colloidal quantum dots/Bi2Te3 photodetector by band alignment engineering

The tunable band gap of PbS colloidal quantum dots (CQDs) from ultraviolet (UV) to short-wave infrared (SWIR) bands provides many potential applications in optoelectronics. However, synthesis of large-sized CQDs that exhibit good stability and sensitivity for extended wavelength still remains a technological challenge. In this paper, a novel broadband photodetector based on small size PbS CQDs (with exciton absorption peak at 927 nm) and Bi2Te3 (with wide spectral sensitivity and high absorption) was developed and studied. The device, which comprised of ITO/AZO/PbS CQDs/Bi2Te3/Al, provided an excellent band alignment that facilitated charge dissociation and transmission hence improving the device sensitivity. Furthermore, wavelength extension was also realized through the synergistic effect of these materials, thus demonstrating broadband photodetection with high sensitivity. The heterostructure photodetector demonstrated good performance in the visible and near infrared ranges, especially at a wavelength of 1050 nm exhibiting a high responsivity (R) and detectivity (D*) of 161 A/W and 3.2 × 1013 Jones, respectively. In addition, the device exhibited excellent stability and reversibility after one month of storage without any encapsulation. This work lays a good foundation for the construction of the next generation of highly sensitive broadband CQDs photodetectors.

Monolithically Integrated PbS Colloidal Quantum Dot Photodetector Crossbar Array for Short‐Wavelength Infrared Imaging

AbstractMonolithically integrated pixels, with stacked PbS colloidal quantum dot (CQD) photodiodes and organic blocking diodes, are developed as the building block for constructing a short‐wavelength infrared (SWIR) crossbar imaging array. Arising from the back‐to‐back stacked configuration and a favorable energy level alignment, holes are blocked from the photodiode at zero and forward biases, which results in the normally‐OFF behavior of the pixels. Based on such device characteristics, the monolithically integrated pixels can effectively suppress electrical crosstalk under illumination in the crossbar array and consume nearly zero standby power. Furthermore, an 8×8 crossbar imaging array with both high imaging quality and low power consumption is achieved, which features as a high‐performance visible–SWIR imaging sensor.

Size effect features and mechanism of luminescence of colloidal PbS quantum dots, passivated with thioglicolic acid

Size effect features and mechanism of luminescence of colloidal PbS quantum dots, passivated with thioglicolic acid

High-Performance Colloidal Quantum Dot Photodiodes via Suppressing Interface Defects.

PbS colloidal quantum dot (CQD) infrared photodiodes have attracted wide attention due to the prospect of developing cost-effective infrared imaging technology. Presently, ZnO films are widely used as the electron transport layer (ETL) of PbS CQDs infrared photodiodes. However, ZnO-based devices still suffer from the problems of large dark current and low repeatability, which are caused by the low crystallinity and sensitive surface of ZnO films. Here, we effectively optimized the device performance of PbS CQDs infrared photodiode via diminishing the influence of adsorbed H2O at the ZnO/PbS CQDs interface. The polar (002) ZnO crystal plane showed much higher adsorption energy of H2O molecules compared with other nonpolar planes, which could reduce the interface defects induced by detrimentally adsorbed H2O. Based on the sputtering method, we obtained the [002]-oriented and high-crystallinity ZnO ETL and effectively suppressed the adsorption of detrimental H2O molecules. The prepared PbS CQDs infrared photodiode with the sputtered ZnO ETL demonstrated lower dark current density, higher external quantum efficiency, and faster photoresponse compared with the sol-gel ZnO device. Simulation results further unveiled the relationship between interface defects and device dark current. Finally, a high-performance sputtered ZnO/PbS CQDs device was obtained with a specific detectivity of 2.15 × 1012 Jones at -3 dB bandwidth (94.6 kHz).

High-Performance Near-Infrared Photodetector Based on PbS Colloidal Quantum Dots/ZnO-Nanowires Hybrid Nanostructures.

Quantum dots have found significant applications in photoelectric detectors due to their unique electronic and optical properties, such as tunable bandgap. Recently, colloidal quantum dots (CQDs) have attracted much interest because of the ease of controlling the dot size and low production cost. In this paper, a high-performance ZnO/PbS heterojunction photodetector was fabricated by spin-coating PbS CQDs onto the surface of a hydrothermally grown vertical array of ZnO nanowires (NWs) on an indium tin oxide (ITO) substrate. Under 940 nm near-infrared light illumination, the device demonstrated a responsivity and detectivity of ~3.9 × 104 A/W and ~9.4 × 1013 Jones, respectively. The excellent performances and low cost of this nanocomposite-based photodetector show that it has the potential for widespread applications ranging from medical diagnosis to environmental monitoring.

Tutorial: Lead sulfide colloidal quantum dot infrared photodetector

Lead sulfide (PbS) colloidal quantum dots (CQDs) is emerging as a promising material for infrared photodetectors because of its strong absorbance in the near infrared region, the tunable energy gap, facile fabrication, and excellent electrical properties. This Tutorial gives a comprehensive introduction of materials and devices of PbS CQD based infrared photodetectors. First, we introduce the concept of CQDs and the typical characters of CQDs. The synthesis of PbS CQDs and a solid film fabrication method are then summarized. Subsequently, the study for defect passivation and carrier transport in a PbS CQD thin film is presented. In the end, the device structure, the electrical diagram, and strategies for enhancing device performance of three kinds of infrared photodetector are concluded.

Mid-infrared response of PbS colloidal quantum dot solids

Owing to their large surface-to-volume ratio, it easily introduces dopants to CQDs surface. Hence, by incorporating oxidation into the energy band using KNO2, PbS CQD photoconductors exhibit an extrinsic response under 3000 nm illumination.