Flexible and broadband colloidal quantum dots photodiode array for pixel-level X-ray to near-infrared image fusion.

Combining information from multispectral images into a fused image is informative and beneficial for human or machine perception. Currently, multiple photodetectors with different response bands are used, which require complicated algorithms and systems to solve the pixel and position mismatch problem. An ideal solution would be pixel-level multispectral image fusion, which involves multispectral image using the same photodetector and circumventing the mismatch problem. Here we presented the potential of pixel-level multispectral image fusion utilizing colloidal quantum dots photodiode array, with a broadband response range from X-ray to near infrared and excellent tolerance for bending and X-ray irradiation. The colloidal quantum dots photodiode array showed a specific detectivity exceeding 1012 Jones in visible and near infrared range and a favorable volume sensitivity of approximately 2 × 105 µC Gy-1 cm-3 for X-ray irradiation. To showcase the advantages of pixel-level multispectral image fusion, we imaged a capsule enfolding an iron wire and soft plastic, successfully revealing internal information through an X-ray to near infrared fused image.

High-Performance and Stable Colloidal Quantum Dots Imager via Energy Band Engineering.

Solution-processed colloidal quantum dot (CQD) photodiodes are compatible for monolithic integration with silicon-based readout circuitry, enabling ultrahigh resolution and ultralow cost infrared imagers. However, top-illuminated CQD photodiodes for longer infrared imaging suffer from mismatched energy band alignment between narrow-bandgap CQDs and the electron transport layer. In this work, we designed a new top-illuminated structure by replacing the sputtered ZnO layer with a SnO2 layer by atomic layer deposition. Benefiting from matched energy band alignment and improved heterogeneous interface, our top-illuminated CQD photodiodes achieve a broad-band response up to 1650 nm. At 220 K, these SnO2-based devices exhibit an ultralow dark current density of 3.5 nA cm-2 at -10 mV, reaching the noise limit for passive night vision. The detectivity is 4.1 × 1012 Jones at 1530 nm. These SnO2-based devices also demonstrate exceptional operation stability. By integrating with silicon-based readout circuitry, our CQD imager realizes water/oil discrimination and see-through smoke imaging.

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.

Large-area flexible colloidal-quantum-dot infrared photodiodes for photoplethysmogram signal measurements.

Epitaxially grown photodiodes are the foundation of infrared photodetection technology; however, their rigid structure and limited area scaling limit their use in advanced applications. Colloidal-quantum-dot (CQD) infrared photodiodes have increased active areas through solution processing, and are thus potential candidates for large-area flexible photodetection, but these large-area photodiodes have disadvantages such as large dark current density, poor homogeneity, and poor stability. Therefore, this study established a fabrication strategy for large-area flexible CQD photodiodes that involves introducing polyimide to CQD ink to improve CQD passivation, monodisperse ink persistence, and film morphology. The resulting CQD photodiodes exhibited reduced dark current density and improved homogeneity and work stability. Furthermore, the as-prepared photodiodes exhibited a detectivity (D*) of greater than 1013 Jones, which was higher than other reported CQD photodetectors. The CQD photodiodes developed in this study can be used for wearable photoplethysmogram (PPG) signal measurement under ambient light at reduced cost and power consumption.

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).

HTL-Free Sb2(S, Se)3 Solar Cells with an Optimal Detailed Balance Band Gap.

Antimony chalcogenides are widely studied as a light-absorbing material due to their merits of low toxicity, efficient cost, and excellent photovoltaic properties. However, the band gaps of antimony selenide (approximately 1.1 eV) and antimony sulfide (approximately 1.7 eV) both deviate from the optimal detailed balance band gap (∼1.3 eV) for terrestrial single-junction solar cells. Notably, the band gap of Sb2(S, Se)3 can be tunable in the range from 1.1 to 1.7 eV, which can cover the detailed balance band gap. In this work, the vapor transport deposition method with two independent evaporation sources is used to deposit Sb2(S, Se)3 thin films. By carefully optimizing the evaporation temperature and the start evaporation time of the Sb2Se3 and Sb2S3 sources, a suitable band gap of 1.33 eV is obtained. Finally, on the basis of the optimal Sb2(S, Se)3 films, Sb2(S, Se)3 solar cells without a hole transport layer achieved an efficiency of 7.03%.

Sb2Se3 film with grain size over 10 µm toward X-ray detection.

Direct X-ray detectors are considered as competitive next-generation X-ray detectors because of their high spatial resolution, high sensitivity, and simple device configuration. However, their potential is largely limited by the imperfections of traditional materials, such as the low crystallization temperature of α-Se and the low atomic numbers of α-Si and α-Se. Here, we report the Sb2Se3 X-ray thin-film detector with a p-n junction structure, which exhibited a sensitivity of 106.3 µC/(Gyair·cm2) and response time of < 2.5 ms. This decent performance and the various advantages of Sb2Se3, such as the average atomic number of 40.8 and µτ product (µ is the mobility, and τ is the carrier lifetime) of 1.29 × 10-5 cm2/V, indicate its potential for application in X-ray detection.

Possible top cells for next-generation Si-based tandem solar cells.

Si-based solar cells, which have the advantages of high efficiency, low manufacturing costs, and outstanding stability, are dominant in the photovoltaic market. Currently, state-of-the-art Si-based solar cells are approaching the practical limit of efficiency. Constructing Si-based tandem solar cells is one available pathway to break the theoretical efficiency limit of single-junction silicon solar cells. Various top cells have been explored recently in the construction of Si-based tandem devices. Nevertheless, many challenges still stand in the way of extensive commercial application of Si-based tandem solar cells. Herein, we summarize the recent progress of representative Si-based tandem solar cells with different top cells, such as III-V solar cells, wide-bandgap perovskite solar cells, cadmium telluride (CdTe)-related solar cells, Cu(In,Ga)(Se,S)2 (CIGS)-related solar cells, and amorphous silicon (a-Si) solar cells, and we analyze the main bottlenecks for their next steps of development. Subsequently, we suggest several potential candidate top cells for Si-based tandem devices, such as Sb2S3, Se, CdSe, and Cu2O. These materials have great potential for the development of high-performance and low-cost Si-based tandem solar cells in the future.

Orientation Engineering in Low-Dimensional Crystal-Structural Materials via Seed Screening.

The orientation of low-dimensional crystal-structural (LDCS) films significantly affects the performance of photoelectric devices, particularly in vertical conducting devices such as solar cells and light-emitting diodes. According to film growth theory, the initial seeds determine the final orientation of the film. Ruled by the minimum energy principle, lying (chains or layers parallel to the substrate) seeds bonding with the substrate through van der Waals forces are easier to form than standing (chains or layers perpendicular to the substrate) seeds bonding with the substrate by a covalent bond. Utilizing high substrate temperature to re-evaporate the lying seeds and preserve the standing seeds, the orientation of 1D crystal-structural Sb2 Se3 is successfully controlled. Guided by this seed screening model, highly [211]- and [221]-oriented Sb2 Se3 films on an inert TiO2 substrate are obtained; consequently, a record efficiency of 7.62% in TiO2 /Sb2 Se3 solar cells is achieved. This universal model of seed screening provides an effective method for orientation control of other LDCS films.

Vapor transport deposition of antimony selenide thin film solar cells with 7.6% efficiency.

Antimony selenide is an emerging promising thin film photovoltaic material thanks to its binary composition, suitable bandgap, high absorption coefficient, inert grain boundaries and earth-abundant constituents. However, current devices produced from rapid thermal evaporation strategy suffer from low-quality film and unsatisfactory performance. Herein, we develop a vapor transport deposition technique to fabricate antimony selenide films, a technique that enables continuous and low-cost manufacturing of cadmium telluride solar cells. We improve the crystallinity of antimony selenide films and then successfully produce superstrate cadmium sulfide/antimony selenide solar cells with a certified power conversion efficiency of 7.6%, a net 2% improvement over previous 5.6% record of the same device configuration. We analyze the deep defects in antimony selenide solar cells, and find that the density of the dominant deep defects is reduced by one order of magnitude using vapor transport deposition process.