Significant efficiency enhancement of carbon-based CsPbI2Br perovskite solar cells enabled by optimizing tin oxide electron transport layer

Carbon-based perovskite solar cells (C-PSCs) have been popular for achieving low-cost and stable photovoltaics. To overcome an obstacle of high-temperature annealing process for producing titanium dioxide (TiO₂), CsPbI₂Br C-PSCs based on a device structure of FTO/tin oxide (SnO₂)/CsPbI₂Br/carbon electrode can be fabricated at the low-temperature annealing process of 280 °C for 180 s, where SnO₂ is used as the electron transporting layer (ETL). Experimental results showed that the suitable concentration of SnO₂ ETL could yield smooth surface CsPbI₂Br films with free-pinhole and larger grain-sized crystallization. In combination with prolonging annealing time, a champion power conversion efficiency of 9.68% with a larger open-circuit voltage (V_oc) of 1.14 V was obtained for CsPbI₂Br C-PSC based on SnO₂ ETL. Here, a simple low-temperature fabricating process of SnO₂ ETL can be adapted to flexible substrates for C-PSCs and furtherly reduce the manufacturing cost.

     

BaPbO3 conductive coating layers on platinized Si substrate for the growth of PbZr1−xTixO3 thin films

Barium metaplumbate (BaPbO₃, BPO) thin films were prepared on Pt/Ti/SiO₂/Si substrates by a sol–gel method and a rapid thermal annealing (RTA) process. X-ray diffraction (XRD) was used to characterize the crystalline structure of the resultant films. It was shown that the formation of perovskite BPO greatly depends on the lead concentration and the final annealing temperature. In terms of the semi-quantitative energy dispersion spectrum (EDS) analysis, the ratio of Pb/Ba in the BPO ceramic films increases as the final heating temperature increases. Using BPO as buffer layers, PZT thin films with a pure perovskite structure were grown at a very low temperature of 500 °C by the sol–gel technique and the RTA process. The remanent polarization of Pt/PZT/BPO/Pt ferroelectric capacitors is about 17 μC/cm² at an applied voltage of 3 V.     

Highly Efficient and Stable Flexible Perovskite Solar Cells with Metal Oxides Nanoparticle Charge Extraction Layers

In this study, the fabrication of highly efficient and durable flexible inverted perovskite solar cells (PSCs) is reported. Presynthesized, solution‐derived NiO_x and ZnO nanoparticles films are employed at room temperature as a hole transport layer (HTL) and electron transport layer (ETL), respectively. The triple cation perovskite films are produced in a single step and for the sake of comparison, ultrasmooth and pinhole‐free absorbing layers are also fabricated using MAPbI₃ perovskite. The triple cation perovskite cells exhibit champion power conversion efficiencies (PCEs) of 18.6% with high stabilized power conversion efficiency of 17.7% on rigid glass/indium tin oxide (ITO) substrates (comparing with 16.6% PCE with 16.1% stabilized output efficiency for the flexible polyethylene naphthalate (PEN)/thin film barrier/ITO substrates). More interestingly, the durability of flexible PSC under simulation of operative condition is proved. Over 85% of the maximum stabilized output efficiency is retained after 1000 h aging employing a thin MAPbI₃ perovskite (over 90% after 500 h with a thick triple cation perovskite). This result is comparable to a similar state of the art rigid PSC and represents a breakthrough in the stability of flexible PSC using ETLs and HTLs compatible with roll to roll production speed, thanks to their room temperature processing.     

Strategically Constructed Bilayer Tin (IV) Oxide as Electron Transport Layer Boosts Performance and Reduces Hysteresis in Perovskite Solar Cells

Nanostructured tin (IV) oxide (SnO₂) is emerging as an ideal inorganic electron transport layer in n–i–p perovskite devices, due to superior electronic and low‐temperature processing properties. However, significant differences in current–voltage performance and hysteresis phenomena arise as a result of the chosen fabrication technique. This indicates enormous scope to optimize the electron transport layer (ETL), however, to date the understanding of the origin of these phenomena is lacking. Reported here is a first comparison of two common SnO₂ ETLs with contrasting performance and hysteresis phenomena, with an experimental strategy to combine the beneficial properties in a bilayer ETL architecture. In doing so, this is demonstrated to eliminate room‐temperature hysteresis while simultaneously attaining impressive power conversion efficiency (PCE) greater than 20%. This approach highlights a new way to design custom ETLs using functional thin‐film coatings of nanomaterials with optimized characteristics for stable, efficient, perovskite solar cells.     

Cu2ZnSnS4 films by paste coating and their optoelectronic properties

Cu₂ZnSnS₄ (CZTS) thin films were prepared by a paste coating method as the absorb layer of solar cells. This method is more eco-friendly using ethanol as solvent and more convenient than traditional sol–gel method. The effects of sulfurization temperature on properties of thin film were studied. The results of X-ray diffraction and Raman spectroscopy showed the formation of kesterite structure of CZTS films. The scanning electron microscopy images revealed that CZTS thin film obtained at 550 °C were compact and uniform. The optical band gap of the CZTS film was about 1.5 eV, and the CZTS film had an obvious optoelectronic response. Moreover, CZTS solar cell was prepared with a conversion efficiency of 0.47 %.     

Damping properties of epoxy-based composite embedded with sol–gel-derived Pb(Zr<Subscript>0.53</Subscript>Ti<Subscript>0.47</Subscript>)O<Subscript>3</Subscript> thin film annealed at different temperatures

Pb(Zr_0.53Ti_0.47)O₃ (PZT) thin films were prepared on Pt/Ti/SiO₂/Si substrate by sol–gel method. The effect of annealing temperature on microstructure, ferroelectric and dielectric properties of PZT films was investigated. When the films were annealed at 550–850 °C, the single-phase PZT films were obtained. PZT films annealed at 650–750 °C had better dielectric and ferroelectric properties. The sandwich composites with epoxy resin/PZT film with substrate/epoxy resin were prepared. The annealing temperature of PZT films influenced their damping properties, and the epoxy-based composites embedded with PZT film annealed at 700 °C had the largest damping loss factor of 0.923.     

Improvement of physical properties of IGZO thin films prepared by excimer laser annealing of sol–gel derived precursor films

Indium gallium zinc oxide (IGZO) transparent semiconductor thin films were prepared by KrF excimer laser annealing of sol–gel derived precursor films. Each as-coated film was dried at 150 °C in air and then annealed using excimer laser irradiation. The influence of laser irradiation energy density on surface conditions, optical transmittances, and electrical properties of laser annealed IGZO thin films were investigated, and the physical properties of the excimer laser annealed (ELA) and the thermally annealed (TA) thin films were compared. Experimental results showed that two kinds of surface morphology resulted from excimer laser annealing. Irradiation with a lower energy density (≤250 mJ cm⁻²) produced wavy and irregular surfaces, while irradiation with a higher energy density (≥350 mJ cm⁻²) produced flat and dense surfaces consisting of uniform nano-sized amorphous particles. The explanation for the differences in surface features and film quality is that using laser irradiation energy to form IGZO thin films improves the film density and removes organic constituents. The dried IGZO sol–gel films irradiated with a laser energy density of 350 mJ/cm² had the best physical properties of all the ELA IGZO thin films. The mean resistivity of the ELA 350 thin films (4.48 × 10³ Ω cm) was lower than that of TA thin films (1.39 × 10⁴ Ω cm), and the average optical transmittance in the visible range (90.2%) of the ELA 350 thin films was slightly higher than that of TA thin films (89.7%).     

Enhanced photocatalytic activity of Mg0.05Zn0.95O thin films prepared by sol–gel method through a cycle

Mg_0.05Zn_0.95O thin films were prepared on silicon substrates by a sol–gel dip-coating technique. Microstructure, surface topography and optical properties of the thin films were characterized by X-ray diffraction, atom force microscopy, Fourier transform infrared spectrophotometer and fluorescence spectrometer. The results show that the thin film annealed at 700 °C has the largest average grain size and exhibits the best c-axis preferred orientation. As annealing temperature increases to 800 °C, the grain along c-axis has been suppressed. Roughness factor and average particle size increase with the increase of annealing temperature. The IR absorption peak appearing at about 416 cm^?1 is assigned to hexagonal wurtzite ZnO. The thin film annealed at 700 °C has the maximum oxygen vacancy, which can be inferred from the green emission intensity. Photocatalytic results show that the thin film annealed at 700 °C exhibits remarkable photocatalytic activity, which may be attributed to the larger grain size, roughness factor and concentration of oxygen vacancy. Enhanced photocatalytic activity of Mg_0.05Zn_0.95O thin films after a cycle may be attributed to the increase of surface oxygen vacancy and photocorrosion of amorphous MgO on the surface of thin film under UV irradiation.     

Effect of heat-treatment on LaNiO3 film electrode of PZT thin films derived by a sol–gel method

Lanthanum nickel oxide (LaNiO₃ or LNO) conducting thin films that could be used as electrodes for improving fatigue and aging properties of ferroelectric thin films were investigated. In this paper, LNO films were directly spin-coated onto SiO₂/Si(1 0 0) substrates followed by thermal treatment in air and in oxygen. It was found that crack-free dense and uniform films with good crystallinity and medium grains were obtained, preferentially (1 0 0)-oriented LNO thin films could be formed at a lower annealing temperature of 550 °C and that with the increase in thermal annealing temperature the LNO thin film possessed better electrical properties especially at 750 °C. However, the LNO film displayed a structure transformation above 850 °C. A phenomenon was found that the first heat-treatment temperature and time played a key role to determine the crystallite size of LNO films. A subsequent deposition of a sol–gel derived Pb(Zr_0.53Ti_0.47)O₃ (PZT53/47) thin film on the LNO-coated SiO₂/Si(1 0 0) substrates was also found to have a (1 0 0)-oriented texture. Moreover, the Au/PZT/LNO capacitor was found to significantly improve the fatigue and the effects of the LNO electrodes to the fatigue were discussed.     

Low-Temperature Chemical Bath Deposition of Conformal and Compact NiOX for Scalable and Efficient Perovskite Solar Modules

A scalable and low-cost deposition of high-quality charge transport layers and photoactive perovskite layers are the grand challenges for large-area and efficient perovskite solar modules and tandem cells. An inverted structure with an inorganic hole transport layer is expected for long-term stability. Among various hole transport materials, nickel oxide has been investigated for highly efficient and stable perovskite solar cells. However, the reported deposition methods are either difficult for large-scale conformal deposition or require a high vacuum process. Chemical bath deposition is supposed to realize a uniform, conformal, and scalable coating by a solution process. However, the conventional chemical bath deposition requires a high annealing temperature of over 400 °C. In this work, an amino-alcohol ligand-based controllable release and deposition of NiO_X using chemical bath deposition with a low calcining temperature of 270 °C is developed. The uniform and conformal in-situ growth precursive films can be adjusted by tuning the ligand structure. The inverted structured perovskite solar cells and large-area solar modules reached a champion PCE of 22.03% and 19.03%, respectively. This study paves an efficient, low-temperature, and scalable chemical bath deposition route for large-area NiO_X thin films for the scalable fabrication of highly efficient perovskite solar modules.     

SnO2退火温度对钙钛矿太阳能电池性能的影响

电子传输层是钙钛矿太阳能电池的关键部分, 起到阻挡空穴、传输电子和减少电子空穴复合的作用。本研究采用低温溶液法制备SnO₂薄膜作为钙钛矿电池的电子传输层, 研究SnO₂的退火温度对电子传输层微观形貌、物理性能以及钙钛矿太阳能电池性能的影响。结果表明: 当退火温度为60、90、120和240 ℃时, SnO₂薄膜表面存在较多的孔隙; 而退火温度为150、180和210 ℃时, 薄膜表面孔隙较少。在实验温度下, 制备的SnO₂薄膜为四方相, FTO玻璃上涂覆SnO₂薄膜后其透过率要优于空白FTO玻璃的透过率。当SnO₂退火温度为180 ℃时, 薄膜的电子迁移率最高, 钙钛矿电池具有最佳的传输电阻和复合电阻, 所得电池的性能最优, 其光电转换效率为17.28%, 开路电压为1.09 V, 短路电流为20.91 mA/cm², 填充因子为75.91%。     

Post annealing effect on structural and optical properties of ZnO thin films derived by sol–gel route

Zinc oxide thin films have been spun coated on p-Si (100) substrates by sol–gel route. These films were annealed at different annealing temperatures from 300 to 1,000 °C in the oxygen ambient. In this way a suitable annealing temperature window for the sol–gel derived ZnO films exhibiting minimum defects (points and dislocations) and better quality (crystal and optical) was investigated. The structural and optical features of ZnO thin films have been examined by X-ray diffraction, atomic force microscopy, UV–Vis spectroscopy, and photoluminescence spectra. The results revealed that the crystallization in the films initiated at 300 °C, improved further with annealing. All the deposited films exhibited wurtzite phase with c-axis orientations. The variations in the position of characteristic (002) peak, stress, strain and lattice parameters are investigated as a function of annealing temperature. The optical band gap is not significantly affected with annealing as observed by UV–Vis transmission spectroscopy. The Photoluminescence spectra exhibited three luminescence centers. The near band edge esmission was observed in UV region which enhanced with the heat treatment, is an indication of improvement in the optical quality of films. The other two visible emissions are related to native defects in ZnO lattice were appeared only for higher annealing (≥700 °C).     

Synthesis of SiOF nanoporous ultra low-k thin film

In this work, we have investigated the effect of annealing temperature on physical, chemical and electrical properties of Fluorine (F) incorporated porous SiO₂ xerogel low-k films. The SiO₂ xerogel thin films were prepared by sol–gel spin-on method using tetraethylorthosilicate as a source of Si. The hydrofluoric acid was used as a catalyst for the incorporation of F ion in the film matrix. The thickness and refractive index (RI) of the films were observed to be decreasing with increase in annealing temperature with minimum value 156 nm and 1.31 respectively for film annealed at 400 °C. Based on measured RI value, the 34 % porosity and 1.53 gm/cm³ density of the film annealed at 400 °C have been determined. The roughness of the films as a function of annealing temperature measured through AFM was found to be increased from 0.9 to 1.95 nm. The Electrical properties such as dielectric constant and leakage current density were evaluated with capacitance–voltage (C–V) and leakage current density–voltage (J–V) measurements of fabricated Al/SiO₂ xerogel/P–Si metal–insulator-semiconductor (MIS) structure. Film annealed at 400 °C, was observed to be with the lowest dielectric constant value (k = 2) and with the lowest leakage current (3.4 × 10^?8 A/cm²) with high dielectric breakdown.     

Seed‐Assisted Growth for Low‐Temperature‐Processed All‐Inorganic CsPbIBr2 Solar Cells with Efficiency over 10%

All‐inorganic CsPbIBr₂ perovskite has recently received growing attention due to its balanced band gap and excellent environmental stability. However, the requirement of high‐temperature processing limits its application in flexible devices. Herein, a low‐temperature seed‐assisted growth (SAG) method for high‐quality CsPbIBr₂ perovskite films through reducing the crystallization temperature by introducing methylammonium halides (MAX, X = I, Br, Cl) is demonstrated. The mechanism is attributed to MA cation based perovskite seeds, which act as nuclei lowering the formation energy of CsPbIBr₂ during the annealing treatment. It is found that methylammonium bromide treated perovskite (Pvsk‐Br) film fabricated at low temperature (150 °C) shows micrometer‐sized grains and superior charge dynamic properties, delivering a device with an efficiency of 10.47%. Furthermore, an efficiency of 11.1% is achieved for a device based on high‐temperature (250 °C) processed Pvsk‐Br film via the SAG method, which presents the highest reported efficiency for inorganic CsPbIBr₂ solar cells thus far.     

Influence of sintering temperatures of ceramic targets on microstructures and photoelectric properties of titanium-doped ZnO nano-films

Thin films of Ti-doped ZnO (TZO) were prepared by RF magnetron sputtering using targets prepared with sintering temperatures in the range 1100–1500 °C; the microstructures and optoelectronic properties of the TZO targets and films were characterized by SEM, XRD, Hall Effect analysis, UV–VIS spectrophotometry and physical property measurement system. Results indicated that the target sintering temperature affected both the TZO targets and films. The Ti/Zn atomic ratios in the targets decreased progressively with increasing sintering temperature, but by a smaller amount in films prepared from them. XRD patterns showed that all films were preferentially oriented along the c axis at 2θ ~ 34° in their XRD patterns. The films sputtered with targets sintered at above 1300 °C were relatively smooth, and had larger average grain size. The target sintered at 1450 °C had the highest density. The best optoelectronic properties were found with the film sputtered from the target sintered at 1300 °C; this sample had superior crystal properties, high average optical transmittance (88.9%), and the lowest resistivity (8.47 × 10^?4 Ω cm). Furthermore, the resistivity of all the films changed with temperature between 10 and 350 K, they experienced an initial decrease followed by an increase as the temperature was raised.     

Efficient Flexible Solar Cell based on Composition‐Tailored Hybrid Perovskite

Organic–inorganic hybrid perovskites (OIHPs) are new photoactive layer candidates for lightweight and flexible solar cells due to their low‐temperature process capability; however, the reported efficiency of flexible OIHP devices is far behind those achieved on rigid glass substrates. Here, it is revealed that the limiting factor is the different perovskite film deposition conditions required to form the same film morphology on flexible substrates. An optimized perovskite film composition needs a different precursor ratio, which is found to be essential for the formation of high‐quality perovskite films with longer radiative carrier recombination lifetime, smaller density of trap states, reduced precursor residue, and uniform and pin‐hole free films. A record efficiency of 18.1% is achieved for the flexible perovskite solar‐cell devices made on an indium tin oxide/poly(ethylene terephthalate) substrate via a low temperature (≤100 °C) solution process.     

Nanocrystalline CuO thin films: synthesis, microstructural and optoelectronic properties

Nanocrystalline copper oxide (CuO) thin films have been synthesized by a sol–gel method using cupric acetate Cu (CH₃COO) as a precursor. The as prepared powder was sintered at various temperatures in the range of (300–700?°C) and has been deposited onto a glass substrates using spin coating technique. The structural, compositional, morphological, electrical optical and gas sensing properties of CuO thin films have been studied by X-ray diffraction, Scanning Electron Microscopy (SEM), Four Probe Resistivity measurement and UV–visible spectrophotometer. The variation in annealing temperature affected the film morphology and optoelectronic properties. X-ray diffraction patterns of CuO films show that all the films are nanocrystallized in the monoclinic structure and present a random orientation. The crystallite size increases with increasing annealing temperature (40–45?nm).The room temperature dc electrical conductivity was increased from 10^?6 to 10^?5 (Ω?cm)^?1, after annealing due to the removal of H₂O vapor which may resist conduction between CuO grain. The thermopower measurement shows that CuO films were found of n-type, apparently suggesting the existence of oxygen vacancies in the structure. The electron carrier concentration (n) and mobility (μ) of CuO films annealed at 400–700?°C were estimated to be of the order of 4.6–7.2?×?10¹⁹?cm^?3 and 3.7–5.4?×?10^?5?cm²?V^?1?s^?1?respectively. It is observed that CuO thin film annealing at 700?°C after deposition provide a smooth and flat texture suited for optoelectronic applications. The optical band gap energy decreases (1.64–1.46?eV) with increasing annealing temperature. It was observed that the crystallite size increases with increasing annealing temperature. These modifications influence the morphology, electrical and optical properties.     

On the preparation of PLZT thin films grown by pulsed laser deposition

Polycrystalline PLZT thin films have been grown onto glass slides substrate, from a sintered stoichiometric 9/65/35 commercial target, by using a Nd:YAG laser (1064 nm, 7 ns, 10 Hz). The substrate temperature and oxygen pressure were varied during the deposition, as was the post-deposition annealing temperature in order to achieve stoichiometric films with a perovskite structure and with a composition near the ratio 9/65/35. Perovskite PLZT is formed around the substrate temperature of 500°C and oxygen pressure of ∼0.5 mbar after annealing at 580°C during 90 min. The pyrochlore structure, on the other hand, is always formed in the films during the deposition. However, this structure disappear for annealing temperatures above 550°C, for the films grown at oxygen pressure in the range 0.5–1 mbar and temperature deposition above 450°C. The degree of crystallinity and the structure present in the films is correlated with the deposition conditions. The influence of post-deposition annealing conditions on the formation of perovskite PLZT structure and optical transparency of the films is also discussed.     

Growth and optical properties of Sn–Si nanocomposite thin films

The growth and optical properties of nanocomposite thin films comprising of nanocrystalline Sn and Si are reported. The nanocomposite films are produced by thermal annealing of bilayers of Sn and Si deposited on borosilicate glass substrates at various temperatures from 300 to 500 °C for 1 h in air. X-ray diffraction reveals that the as-deposited bilayers consist of nanocrystalline Sn films with a crystallite size of 30 nm, while the Si thin films are amorphous. There is onset of crystallinity in Si on annealing to 300 °C with the appearance of the (111) peak of the diamond cubic structure. The crystallite size of Si increases from 5 to 18 nm, whereas the Sn crystallite size decreases with increase in annealing temperature. Significantly, there is no evidence for any Sn–Si compound, and therefore it is concluded that the films are nanocomposites of Sn and Si. Measured spectral transmittance curves show that the films have high optical absorption in the as-deposited form which decreases on annealing to 300 °C. The films show almost 80 % transmission in the visible-near infrared region when the annealing temperature is increased to 500 °C. There is concomitant decrease in refractive index from 4.0, at 1750 nm, for the as-deposited film, to 1.88 for the film annealed at 500 °C. The optical band gap of the films increases on annealing (from 1.8 to ~2.9 eV at 500 °C). The Sn-Si nanocomposites have high refractive index, large band gap, and low optical absorption, and can therefore be used in many optical applications.     

Red-Carbon-Quantum-Dot-Doped SnO2 Composite with Enhanced Electron Mobility for Efficient and Stable Perovskite Solar Cells

An efficient electron transport layer (ETL) plays a key role in promoting carrier separation and electron extraction in planar perovskite solar cells (PSCs). An effective composite ETL is fabricated using carboxylic-acid- and hydroxyl-rich red-carbon quantum dots (RCQs) to dope low-temperature solution-processed SnO₂, which dramatically increases its electron mobility by ≈20 times from 9.32 × 10⁻⁴ to 1.73 × 10⁻² cm² V⁻¹ s⁻¹. The mobility achieved is one of the highest reported electron mobilities for modified SnO₂. Fabricated planar PSCs based on this novel SnO₂ ETL demonstrate an outstanding improvement in efficiency from 19.15% for PSCs without RCQs up to 22.77% and have enhanced long-term stability against humidity, preserving over 95% of the initial efficiency after 1000 h under 40–60% humidity at 25 °C. These significant achievements are solely attributed to the excellent electron mobility of the novel ETL, which is also proven to help the passivation of traps/defects at the ETL/perovskite interface and to promote the formation of highly crystallized perovskite, with an enhanced phase purity and uniformity over a large area. These results demonstrate that inexpensive RCQs are simple but excellent additives for producing efficient ETLs in stable high-performance PSCs as well as other perovskite-based optoelectronics.