Enhanced Thermoelectric Performance of CoSb3 Thin Films by Ag and Ti Co-Doping.

The Skutterudites CoSb3 material has been the focus of research for the conversion applications of waste heat to electricity due to its ability to accommodate a large variety of ions in the cages that have been proven effective in improving the thermoelectric performance. Although the co-doped CoSb3 bulk materials have attracted increasing attention and have been widely studied, co-doped CoSb3 thin films have been rarely reported. In this work, Ag and Ti were co-doped into CoSb3 thin films via a facile in situ growth method, and the influence of doping content in the thermoelectric properties was investigated. The results show that all the Ag and Ti co-doped CoSb3 thin films contain a pure well-crystallized CoSb3 phase. Compared to the un-doped thin film, the co-doped samples show simultaneous increase in the Seebeck coefficient and the electrical conductivity, leading to a distinctly enhanced power factor. The high power factor value can reach ~0.31 mWm-1K-2 at 623 K after appropriate co-doping, which is two times the value of the un-doped thin film we have been obtained. All the results show that the co-doping is efficient in optimizing the performance of the CoSb3 thin films; the key point is to control the doping element content so as to obtain high thermoelectric properties.

Crystal Growth Promotion and Defect Passivation by Hydrothermal and Selenized Deposition for Substrate-Structured Antimony Selenosulfide Solar Cells.

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.

Achieving High Thermoelectric Performance of Eco-Friendly SnTe-Based Materials by Selective Alloying and Defect Modulation.

Recently, rock-salt lead-free chalcogenide SnTe-based thermoelectric (TE) materials have been considered an alternative to PbTe because of the nontoxic properties of Sn as compared to Pb. However, high carrier concentration that originated from intrinsic Sn vacancies and relatively high thermal conductivity of pristine SnTe lead to poor TE efficiency, which makes room for improving its TE properties. In this study, we present that the Na incorporation into the SnTe matrix is helpful for modifying the electronic band structure, optimization of carrier concentration, introducing dislocations, and kink planes; benefiting from these synergistic effects obviates the disadvantages of SnTe and makes a significant improvement in TE performance. We reveal that Na favorably impacts the structure of electronic bands by valence, conduction band engineering, leading to a nice enhancement in the Seebeck coefficient, which exhibits the highest power factor value of 37.93 µWcm-1 K-2 at 898 K, representing the best result for the SnTe material system. Moreover, a broader phonon spectrum is introduced by new phonon-scattering centers, scattered by dislocations and kink planes which suppressed lattice thermal conductivity to 0.57 Wm-1 K-1 at 898 K, which is much lower than that of pristine SnTe. Ultimately, a maximum ZT of 1.26 at 898 K is achieved in the Sn1.03Te + 3% Na sample, which is 97% higher than that of the pristine SnTe, suggesting that SnTe-based materials are a robust candidate for TE applications specifically, an ideal alternative of lead chalcogenides for TE power generation at high temperatures.

Heterojunction Annealing Enabling Record Open-Circuit Voltage in Antimony Triselenide Solar Cells.

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.

Organic Chloride Salt Interfacial Modified Crystallization for Efficient Antimony Selenosulfide Solar Cells.

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.

Novel Thermal Diffusion Temperature Engineering Leading to High Thermoelectric Performance in Bi2 Te3 -Based Flexible Thin-Films.

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.

Quasi-Vertically Oriented Sb2Se3 Thin-Film Solar Cells with Open-Circuit Voltage Exceeding 500 mV Prepared via Close-Space Sublimation and Selenization.

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.

Single-Source Vapor-Deposited Cs2AgBiBr6 Thin Films for Lead-Free Perovskite Solar Cells.

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.

Single Source Thermal Evaporation of Two-dimensional Perovskite Thin Films for Photovoltaic Applications.

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.

High-performance p-type inorganic-organic hybrid thermoelectric thin films.

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.

Study on the growth of Al-doped ZnO thin films with (112̄0) and (0002) preferential orientations and their thermoelectric characteristics.

In this work, using a conventional magnetron sputtering system, Al-doped ZnO (AZO) films with (112̄0) 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 (112̄0) preferential oriented ZnO films. The in-plane power factor of the (112̄0) 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.

Love-mode surface acoustic wave devices based on multilayers of TeO2/ZnO(112¯0)/Si(100) with high sensitivity and temperature stability.

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%.

High-performance perovskite CH3NH3PbI3 thin films for solar cells prepared by single-source physical vapour deposition.

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.