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Bismuth-based chalcogenides have emerged as promising candidates for next-generation, solution-processable semiconductors, mainly benefiting from their facile fabrication, low cost, excellent stability, and tunable optoelectronic properties. Particularly, the recently developed AgBiS2 solar cells have shown striking power conversion efficiencies. High performance bismuth-based photodetectors have also been extensively studied in the past few years. However, the fundamental properties of these Bi-based semiconductors have not been sufficiently investigated, which is crucial for further improving the device performance. Here, we introduce multiple time-resolved and steady-state techniques to fully characterize the charge carrier dynamics and charge transport of solution-processed Bi-based nanocrystals. It was found that the Ag-Bi ratio plays a critical role in charge transport. For Ag-deficient samples, silver bismuth sulfide thin films behave as localized state induced hopping charge transport, and the Ag-excess samples present band-like charge transport. This finding is crucial for developing more efficient Bi-based semiconductors and optoelectronic devices.
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Antimony selenide (Sb2 Se3 ) is a highly promising photovoltaic material thanks to its outstanding optoelectronic properties, as well as its cost-effective and eco-friendly merits. However, toxic CdS is widely used as an electron transport layer (ETL) in efficient Sb2 Se3 solar cells, which largely limit their development toward market commercialization. Herein, an effective green Cd-free ETL of SnOx is introduced and deposited by atomic layer deposition method. Additionally, an important post-annealing treatment is designed to further optimize the functional layers and the heterojunction interface properties. Such engineering strategy can optimize SnOx ETL with higher nano-crystallinity, higher carrier density, and less defect groups, modify Sb2 Se3 /SnOx heterojunction with better interface performance and much desirable "spike-like" band alignment, and also improve the Sb2 Se3 light absorber layer quality with passivated bulk defects and prolonged carrier lifetime, and therefore to enhance carrier separation and transport while suppressing non-radiative recombination. Finally, the as-fabricated Cd-free Mo/Sb2 Se3 /SnOx /ITO/Ag thin-film solar cell exhibits a stimulating efficiency of 7.39%, contributing a record value for Cd-free substrate structured Sb2 Se3 solar cells reported to date. This work provides a viable strategy for developing and broadening practical applications of environmental-friendly Sb2 Se3 photovoltaic devices.
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Renewable energy is crucial for sustainable future, and Cu2ZnSnS4 (CZTS) based solar cells shine as a beacon of hope. CZTS, composed of abundant, low-cost, and non-toxic elements, shares similarities with Cu(In,Ga)Se2 (CIGS). However, despite its promise and appealing properties for solar cells, CZTS-based solar cells faces performance challenges owing to inherent issues with CZTS material, and conventional substrate structure complexities. This review critically examines these roadblocks, explores ongoing efforts and breakthroughs, providing insight into the evolving landscape of CZTS-based solar cells research. Furthermore, as an optimistic turn in the field, the review first highlights the crucial need to transition to a superstrate structure for CZTS-based single junction devices, and summarizes the substantial progress made in this direction. Subsequently, dive into the discussion about the fascinating realm of CZTS-based tandem devices, providing an overview of the existing literature as well as outlining the possible potential strategies for enhancing the efficiency of such devices. Finally, the review provides a useful outlook that outlines the priorities for future research and suggesting where efforts should concentrate to shape the future of CZTS-based solar cells.
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Exploring new near-room-temperature thermoelectric materials is significant for replacing current high-cost Bi2Te3. This study highlights the potential of Ag2Se for wearable thermoelectric electronics, addressing the trade-off between performance and flexibility. A record-high ZT of 1.27 at 363 K is achieved in Ag2Se-based thin films with 3.2 at.% Te doping on Se sites, realized by a new concept of doping-induced orientation engineering. We reveal that Te-doping enhances film uniformity and (00l)-orientation and in turn carrier mobility by reducing the (00l) formation energy, confirmed by solid computational and experimental evidence. The doping simultaneously widens the bandgap, resulting in improved Seebeck coefficients and high power factors, and introduces TeSe point defects to effectively reduce the lattice thermal conductivity. A protective organic-polymer-based composite layer enhances film flexibility, and a rationally designed flexible thermoelectric device achieves an output power density of 1.5 mW cm-2 for wearable power generation under a 20 K temperature difference.
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Despite the fact that antimony triselenide (Sb2 Se3 ) thin-film solar cells have undergone rapid development in recent years, the large open-circuit voltage (VOC ) deficit still remains as the biggest bottleneck, as even the world-record device suffers from a large VOC deficit of 0.59 V. Here, an effective interface engineering approach is reported where the Sb2 Se3 /CdS heterojunction (HTJ) is subjected to a post-annealing treatment using a rapid thermal process. It is found that nonradiative recombination near the Sb2 Se3 /CdS HTJ, including interface recombination and space charge region recombination, is greatly suppressed after the HTJ annealing treatment. Ultimately, a substrate Sb2 Se3 /CdS thin-film solar cell with a competitive power conversion efficiency of 8.64% and a record VOC of 0.52 V is successfully fabricated. The device exhibits a much mitigated VOC deficit of 0.49 V, which is lower than that of any other reported efficient antimony chalcogenide solar cell.
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Antimony selenosulfide, Sb2(SSe)3, is recognized as an excellent photoactive material owing to its light harvesting capability. There is still room for improvement of the film quality for device performance improvement. Herein, an organic chloride salt [diethylamine hydrochloride, DEA(Cl)] has been introduced for fabricating Sb2(SSe)3 solar cells for the first time. A champion device with a power conversion efficiency (PCE) of 9.17% has been achieved with a relatively improved fill factor and open-circuit voltage (VOC). It has been revealed that DEA(Cl) successfully interacts with Sb2(SSe)3, which can facilitate the crystallization process to give rise to the closely packed bigger grain sizes with reduced surface cracks; it successfully suppressed the oxidized Sb species (Sb2O3) in the Sb2(SSe)3 film to give rise to phase purity, thus leading to superior surface morphology and electrical characteristics of DEA(Cl)-modified Sb2(SSe)3 absorber films. Chloride modification is thus efficiently helpful in suppressing interfacial defects, improving junction quality, and optimizing energy-level alignment. This facile interfacial modification demonstrates the remarkable potential for efficient Sb2(SSe)3 solar cells.
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Flexible Bi2 Te3 -based thermoelectric devices can function as power generators for powering wearable electronics or chip-sensors for internet-of-things. However, the unsatisfied performance of n-type Bi2 Te3 flexible thin films significantly limits their wide application. In this study, a novel thermal diffusion method is employed to fabricate n-type Te-embedded Bi2 Te3 flexible thin films on flexible polyimide substrates, where Te embeddings can be achieved by tuning the thermal diffusion temperature and correspondingly result in an energy filtering effect at the Bi2 Te3 /Te interfaces. The energy filtering effect can lead to a high Seebeck coefficient ≈160 µV K-1 as well as high carrier mobility of ≈200 cm2 V-1 s-1 at room-temperature. Consequently, an ultrahigh room-temperature power factor of 14.65 µW cm-1 K-2 can be observed in the Te-embedded Bi2 Te3 flexible thin films prepared at the diffusion temperature of 623 K. A thermoelectric sensor is also assembled through integrating the n-type Bi2 Te3 flexible thin films with p-type Sb2 Te3 counterparts, which can fast reflect finger-touch status and demonstrate the applicability of as-prepared Te-embedded Bi2 Te3 flexible thin films. This study indicates that the thermal diffusion method is an effective way to fabricate high-performance and applicable flexible Te-embedded Bi2 Te3 -based thin films.
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Antimony sulfide-selenide (Sb2(S,Se)3) is a promising light-harvesting material for stable and high-efficiency thin-film photovoltaics (PV) because of its excellent light-harvesting capability, abundant elemental storage, and excellent stability. This study aimed to expand the application of Sb2(S,Se)3 solar cells with a substrate structure as a flexible or tandem device. The use of a hydrothermal method accompanied by a postselenization process for the deposition of Sb2(S,Se)3 film based on the solar cell substrate structure was first demonstrated. The mechanism of postselenization treatment on crystal growth promotion of the Sb2(S,Se)3 film and the defect passivation of the Sb2(S,Se)3 solar cell were revealed through different characterization methods. The crystallinity and the carrier transport property of the Sb2(S,Se)3 film improved, and both the interface defect density of the Sb2(S,Se)3/CdS interface and the bulk defect density of the Sb2(S,Se)3 absorber decreased. Through these above-mentioned processes, the transport and collection of electronics can be improved, and the defect recombination loss can be reduced. By using postselenization treatment to optimize the absorber layer, Sb2(S,Se)3 solar cells with the configuration SLG/Mo/Sb2(S,Se)3/CdS/ITO/Ag achieved an efficiency of 4.05%. This work can provide valuable information for the further development and improvement of Sb2(S,Se)3 solar cells.
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Sb2Se3, one of the most desirable absorption materials for next-generation thin-film solar cells, has an excellent photovoltaic characteristic. The [hk1]-oriented (quasi-vertically oriented) Sb2Se3 thin film is more beneficial for promoting efficient carrier transport than the [hk0]-oriented Sb2Se3 thin film. Controlling thin-film orientation remains the main obstacle to the further improvement in the efficiency of Sb2Se3-based solar cells. In this work, the controlled [hk0] or [hk1] orientation of the Sb2Se3 precursor is readily adjusted by tuning the substrate temperature and the distance between the source and the sample in close-space sublimation (CSS). Well-crystallized stoichiometric Sb2Se3 thin films with the desired orientation and large crystal grains are successfully prepared after selenization. Sb2Se3 thin-film solar cells in a substrate configuration of glass/Mo/Sb2Se3/CdS/ITO/Ag are fabricated with a power conversion efficiency of 4.86% with a record open-circuit voltage (VOC) of 509 mV. The significant improvement in VOC is closely related to the quasi-vertically oriented Sb2Se3 absorber layer with reduced deep-level defect density in the bulk and defect passivation at the Sb2Se3/CdS heterojunction. This work indicates that CSS and selenization show a remarkable potential for the fabrication of high-efficiency Sb2Se3 solar cells.
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Photocatalysts are widely used for the elimination of organic contaminants from waste-water and H2 evaluation by water-splitting. Herein, the nanohybrids of lanthanum (La) and selenium (Se) co-doped bismuth ferrites with graphene oxide were synthesized. A structural analysis from X-ray diffraction confirmed the transition of phases from rhombohedral to the distorted orthorhombic. Scanning electron microscopy (SEM) revealed that the graphene nano-sheets homogenously covered La-Se co-doped bismuth ferrites nanoparticles, particularly the (Bi0.92La0.08Fe0.50Se0.50O3-graphene oxide) LBFSe50-G sample. Moreover, the band-gap nanohybrids of La-Se co-doped bismuth ferrites were estimated from diffuse reflectance spectra (DRS), which showed a variation from 1.84 to 2.09 eV, because the lowering of the band-gap can enhance photocatalytic degradation efficiency. Additionally, the photo-degradation efficiencies increased after the incorporation of graphene nano-sheets onto the La-Se co-doped bismuth ferrite. The maximum degradation efficiency of the LBFSe50-G sample was up to 80%, which may have been due to reduced band-gap and availability of enhanced surface area for incoming photons at the surface of the photocatalyst. Furthermore, photoluminescence spectra confirmed that the graphene oxide provided more electron-capturing sites, which decreased the recombination time of the photo-generated charge carriers. Thus, we can propose that the use of nanohybrids of La-Se co-doped bismuth ferrite with graphene oxide nano-sheets is a promising approach for both water-treatment and water-splitting, with better efficiencies of BiFeO3.
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Hybrid two-dimensional (2D) halide perovskites has been widely studied due to its potential application for high performance perovskite solar cells. Understanding the relationship between microstructural and opto-electronic properties is very important for fabricating high-performance 2D perovskite solar cell. In this work, the effect of solvent annealing on grain growth was investigated to enhance the efficiency of photovoltaic devices with 2D perovskite films based on (BA)2(MA)3Pb4I13 prepared by single-source thermal evaporation. Results show that solvent annealing with the introduction of solvent vapor can effectively enhance the crystallization of the (BA)2(MA)3Pb4I13 thin films and produce denser, larger-crystal grains. The thin films also display a favorable band gap of 1.896 eV, which benefits for increasing the charge-diffusion lengths. The solvent-annealed (BA)2(MA)3Pb4I13 thin-film solar cell prepared by single-source thermal evaporation shows an efficiency range of 2.54-4.67%. Thus, the proposed method can be used to prepare efficient large-area 2D perovskite solar cells.
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Lead-free double perovskites have been considered as a potential environmentally friendly photovoltaic material for substituting the hybrid lead halide perovskites due to their high stability and nontoxicity. Here, lead-free double perovskite Cs2AgBiBr6 films are initially fabricated by single-source evaporation deposition under high vacuum condition. X-ray diffraction and scanning electron microscopy characterization show that the high crystallinity, flat, and pinhole-free double perovskite Cs2AgBiBr6 films were obtained after post-annealing at 300 °C for 15 min. By changing the annealing temperature, annealing time, and film thickness, perovskite Cs2AgBiBr6 solar cells with planar heterojunction structure of FTO/TiO2/Cs2AgBiBr6/Spiro-OMeTAD/Ag achieve an encouraging power conversion efficiency of 0.70%. Our preliminary work opens a feasible approach for preparing high-quality double perovskite Cs2AgBiBr6 films wielding considerable potential for photovoltaic application.
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The performance of organic-inorganic hybrid thermoelectric thin films can be dramatically enhanced by optimizing energy filtering and carrier transport states at the organic-inorganic interfaces. In this work, p-type "Sb2Te3/CH3NH3I/Sb2Te3" multilayer thin films were firstly fabricated with varied contents of CH3NH3I, and then an annealing process was used in order to form homogeneous organic-inorganic hybrid thin films. The results revealed that the introduced organic component can promote thin film growth and develop a dense nanostructure with improved crystallinity, thus resulting in a significantly increased Seebeck coefficient and a reduced thermal conductivity as a result of the optimized electronic transport characteristics and enhanced effects of phonon scattering. As is expected, the thermoelectric performance of the hybrid-nanocomposite films is enhanced, achieving the maximum ZT value of 1.55 at a temperature of 413 K, which is several times higher than that of the as-fabricated film, thereby suggesting that the proposed strategy can be applied as an efficient method for the preparation of high-performance thermoelectric thin films.
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In this work, using a conventional magnetron sputtering system, Al-doped ZnO (AZO) films with (112Ì0) and (0002) preferential orientations were grown on r-sapphire and a-sapphire substrates, respectively. The effect of substrate and deposition temperature on the growth of AZO films and their preferential orientations were investigated. The crystallographic characteristics of AZO films were characterized by X-ray diffraction (XRD). The surface morphology of AZO films was studied by scanning electron microscopy (SEM) and atomic force microscopy (AFM). It is found that the lattice mismatch between AZO and substrate determines the growth of AZO films and their preferential orientations. The thermoelectric properties are strongly dependent on the crystal grain shape and the grain boundaries induced by the preferred orientation. The highly connected and elongated grains lead to high thermoelectric properties. The in-plane anisotropy performances of thermoelectric characteristics were found in the (112Ì0) preferential oriented ZnO films. The in-plane power factor of the (112Ì0) preferential oriented ZnO films in the [0001] direction was more than 1.5 × 10-3 W m-1 K-2 at 573 K, which is larger than that of the (0002) preferential oriented ZnO films.
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A multilayer structure of TeO2/interdigital transducers (IDTs)/ZnO(112¯0)/Si(100) was proposed and investigated to achieve both high sensitivity and temperature-stability for bio-sensing applications. Dispersions of phase velocities, electromechanical coupling coefficients K2, temperature coefficient of delay (TCD) and sensitivity in the multilayer structures were simulated as functions of normalized thicknesses of ZnO (hZnO/λ) and TeO2 (hTeO2/λ) films. The fundamental mode of Love mode (LM) - surface acoustic wave (SAW) shows a larger value of K2 and higher sensitivity compared with those of the first mode. TeO2 film with a positive TCD not only compensates the temperature effect induced due to the negative TCD of ZnO(112¯0)/Si(100), but also enhances the sensitivity of the love mode device. The optimal normalized thickness ratios were identified to be hTeO2/λ=0.021 and hZnO/λ=0.304, and the devices with such structures can which generate a normalized sensitivity of -1.04×10-3m3/kg, a TCD of 0.009ppm/°C, and a K2 value of 2.76%.
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In this work, an alternative route to fabricating high-quality CH3NH3PbI3 thin films is proposed. Single-source physical vapour deposition (SSPVD) without a post-heat-treating process was used to prepare CH3NH3PbI3 thin films at room temperature. This new process enabled complete surface coverage and moisture stability in a non-vacuum solution. Moreover, the challenges of simultaneously controlling evaporation processes of the organic and inorganic sources via dual-source vapour evaporation and the heating process required to obtain high crystallization were avoided. Excellent composition with stoichiometry transferred from the powder material, a high level of tetragonal phase-purity, full surface coverage, well-defined grain structure, high crystallization and reproducibility were obtained. A PCE of approximately 10.90% was obtained with a device based on SSPVD CH3NH3PbI3. These initial results suggest that SSPVD is a promising method to significantly optimize perovskite CH3NH3PbI3 solar cell efficiency.