Sharif Digital Repository

Perovskite solar cells suffer from various instabilities on all time scales. Some of them are driven by light, in particular when employing compounds with mixed halides. Such light soaking effects have been observed to result in performance changes of solar-cell devices. They have also been spectroscopically investigated in detail on films, where the formation of a low-gap iodine-rich phase, seen as a red shift of the PL, has been found to be responsible for a reduced open-circuit voltage. However, studies synchronously examining device performance and its relation to spectroscopy data are scarce. Here, we perform an in operando study, where we investigate the changes of open-circuit voltage... 

A key direction toward enhancing the long term and outdoor stability of the perovskite solar cells is encapsulation. As a result, a suitable encapsulation package is required to prevent moisture and oxygen penetration toward the perovskite solar cells. In this work, a low-cost commercially available bilayer structure of poly (methyl methacrylate)/ room-temperature vulcanizing silicone rubber (RTV) encapsulation package for enhancing the long term stability of the perovskite solar cells has been investigated. Encapsulated cells retained more than 80% of the initial efficiency at the environmental condition of 50% moisture, and room temperature after 1000 h, however reference cell efficiency... 

Alkaline doping (Cs, Rb) in CH3NH3PbI3 (MAPbI3) is known to enhance the stability of perovskite solar cells. The films are usually deposited using anti-solvent method, which is tricky and not applicable for large scale deposition. Besides, in case of CsxMA1−xPbI3 the amount of Cs must be carefully controlled to prevent CsI phase formation. Herein, we report an atmospheric pressure vapor assisted solution process (AP-VASP) for the growth of Cs doped MAPbI3 perovskite films that features highly uniform morphology, pin-hole free films, large grain size, as well as being scalable. The CsxMA1−xPbI3 films are formed by the reaction of Cs doped PbI2 films with MAI vapor in a simple oven. We... 

We performed density functional calculations aimed at identifying the atomistic and electronic structure origin of the valence and conduction band, and band gap tunability of halide perovskites ABX3 upon variations of the monovalent and bivalent cations A and B and the halide anion X. We found that the two key ingredients are the overlap between atomic orbitals of the bivalent cation and the halide anion, and the electronic charge on the metal center. In particular, lower gaps are associated with higher negative antibonding overlap of the states at the valence band maximum (VBM), and higher charge on the bivalent cation in the states at the conduction band minimum (CBM). Both VBM orbital... 

Organic-inorganic lead halide perovskites have emerged as very promising semiconductors with efficiencies exceeding 22% making them a serious candidate for next generation solar cells. All current high performance perovskite solar cells (PSCs), including the most recent world records, were achieved using the so-called anti-solvent method. Here, an anti-solvent, typically chlorobenzene (CB), is used to induce rapid crystallisation of a liquid perovskite precursor resulting in highly homogenous, pinhole-free planar perovskite films. While this has yielded very impressive high-performance results, few efforts have been dedicated to the fundamental understanding of the anti-solvent method. In... 

Herein, we report a modified two-step method to construct a uniform and pinhole-free polycrystalline perovskite film with large grains up to the microscale using lead mixed-halide (PbI2-PbCl2) precursor solutions to guarantee the device functioning. Commonly used sequential deposition methods based on dip- and spin-coatings are combined with a vapor-assisted solution process to improve the perovskite morphology and tune the residual lead mixed-halides. These can enhance the optical absorption and efficiency of perovskite solar cell (PSC) devices. The impact of the Cl content in the lead mixed-halide precursors and the employed preparation methods on the photovoltaic performance of PSCs are... 

The effect of substitutional Li doping into NiOx hole transporting layer (HTL) for use in inverted perovskite solar cells was systematically studied. Li doped NiOx thin films with preferential crystal growth along the (111) plane were deposited using a simple solution-based process. Mott-Schottky analysis showed that hole carrier concentration (NA) is doubled by Li doping. Utilizing 4 % Li in NiOx improved the power conversion efficiency (PCE) of solar devices from 9.0 % to 12.6 %. Photoluminescence quenching investigations demonstrate better hole capturing properties of Li:NiOx compared to that of NiOx, leading to higher current densities by Li doping. The electrical conductivity of NiOx is... 

Perovskite solar cells have been constructed under ambient conditions by using 2,2',7,7'-Tetrakis-(N,N-di-4-methoxyphenylamino)-9,9'-spirobifluorene (spiro-OMeTAD) mixed with a small quantity of soluble tetra-n-butyl substituted copper phthalocyanine as hole transporting material. The introduction of the phthalocyanine derivative resulted in an impressive increase of cell efficiency, which changed from 10.4% in the absence to 15.4% in the presence of phthalocyanine. This effect is related to the creation of deep traps in the hole transporting phase which block back-travelling electrons as well as to the improvement of the structural quality of the spiro-OMeTAD film in the presence of... 

Perovskite solar cells have been constructed under ambient conditions by using 2,2',7,7'-Tetrakis-(N,N-di-4-methoxyphenylamino)-9,9'-spirobifluorene (spiro-OMeTAD) mixed with a small quantity of soluble tetra-n-butyl substituted copper phthalocyanine as hole transporting material. The introduction of the phthalocyanine derivative resulted in an impressive increase of cell efficiency, which changed from 10.4% in the absence to 15.4% in the presence of phthalocyanine. This effect is related to the creation of deep traps in the hole transporting phase which block back-travelling electrons as well as to the improvement of the structural quality of the spiro-OMeTAD film in the presence of... 

Interfacial engineering between the perovskite and hole transport layers has emerged as an effective way to improve perovskite solar cell (PSC) performance. A variety of organic halide salts are developed to passivate the traps and enhance the charge carrier transport. Here, the use of guanidinium iodide (GuaI) for interfacial modification of mixed-cation (Cs)x(FA)1−xPbI3 perovskite films, which results in the formation of a low-dimensional δ-FAPbI3-like phase on the 3D perovskite surface, is reported. The presence of this thin layer facilitates charge transfer at interfaces and reduces charge carrier recombination pathways as evidenced by enhanced carrier lifetimes and favorable interfacial... 

The improvement of the quality of the hole transporting layer (HTL) plays a key role in the fabrication of highly efficient and stable perovskite solar cells (PSCs). Here, we used rubrene as a surface treatment agent on top of a spiro HTL. We found that rubrene can cover the pinholes of the spiro layer and provide an excellent contact layer for planar PSCs. Based on this modification, mobile gold ions from the metal electrode are prevented from diffusing through the HTL hindering the degradation of PSCs. The optimized device shows a maximum power conversion efficiency (PCE) of 19.87% and a 79% fill factor (FF), which are higher than the 17.98% PCE and 72% FF of the reference device. In... 

Interfacial studies and band alignment engineering on the electron transport layer (ETL) play a key role for fabrication of high-performance perovskite solar cells (PSCs). Here, an amorphous layer of SnO2 (a-SnO2) between the TiO2 ETL and the perovskite absorber is inserted and the charge transport properties of the device are studied. The double-layer structure of TiO2 compact layer (c-TiO2) and a-SnO2 ETL leads to modification of interface energetics, resulting in improved charge collection and decreased carrier recombination in PSCs. The optimized device based on a-SnO2/c-TiO2 ETL shows a maximum power conversion efficiency (PCE) of 21.4% as compared to 19.33% for c-TiO2 based device.... 

Hybrid perovskite solar cells (PSCs) have gained significant attention owing to their excellent physicochemical and photovoltaic properties. PSCs typically consist of a perovskite light absorber sandwiched between two carrier selective layers optimized with respect to optimal band alignment and low interfacial recombination. The quality of the perovskite layer and interfaces play major roles in the fabrication of high-performance PSCs. In the present work, we systematically investigate the planar structure PSCs based on TiO2 and TiO2/ZnO electron transport layers (ETLs), which provide deeper insight into the charge recombination and accumulation mechanisms. We show that the double-layer... 

Efficient electron transport layers (ETLs) play a pivotal role in the performance of solar cells. In recent years, Indium sulfide (In2S3) has been studied as a promising ETL in CuInGaS(e)2, Cu2ZnSnS(e)4, and perovskite solar cells. Despite several studies on spray-deposited In2S3, there is no complete experimental investigation on In2S3 thin films. The effect of the molar ratio of S/In and the type of indium precursor on the structural, morphological, optical, and electrical properties of sprayed-In2S3 layers has been studied. Films were characterized using x-ray diffraction, scanning electron microscopy (SEM), optical transmission (UV-Vis), Mott-Schottky analysis, four-point probe, and... 

Hole-transporter-free perovskite solar cells carrying a carbon back contact electrode provide the possibility of making full printable low cost and stable devices, even though their efficiency is substantially lower than those made in the standard configuration. The present work searched for simple and easy routes for constructing such devices, demonstrating that organic components do enhance device efficiency but only to a level that is not worth the trouble nor the cost. Devices based on a triple mesoporous layer of titania/zirconia/carbon with perovskite infiltration gave an efficiency of 10.7%. After 180 days of storing under ambient conditions, a small loss of efficiency has been... 

In the last decade, the power conversion efficiency (PCE) of solution-processed perovskite solar cells (PSCs) in the lab-scale has reached an incredible level of 25.5%. Generally, PSCs are composed of a stack consisting of a perovskite thin-film sandwiched between an electron transporting layer (ETL) and a hole transporting layer (HTL). Although the quality of the ETL and HTL interfaces with the perovskite thin-film is important, the quality of the perovskite thin-film is also critical to achieving high-performance PSCs. Low-temperature deposition of organic-inorganic perovskite thin-films by simple solution processes is one of the significant advantages of PSCs compared to other... 

Perovskite solar cells have been constructed under the standard procedure by employing soluble tetratriphenylamine-substituted Zn phthalocyanine as hole transporting material. Solution processed device construction was carried out under ambient conditions of 50–60% ambient humidity. Triphenylamine substitution played the double role of imparting solubility to the core metal phthalocyanine as well as to introduce electron-rich ligands, which could enhance the role of Zn phthalocyanine as hole transporter. Indeed, the obtained material was functional. The present data highlight tetratriphenylamine-substituted Zn phthalocyanine as hole transporting material but also highlight the importance of... 

Copper phthalocyanine can effectively act as alternative small molecule hole transporting material in perovskite solar cells. In order to produce solution processed devices, a soluble copper phtalocyanine has been synthesized by n-butyl substitution and it was compared to commercially available tert-butyl substituted copper phthalocyanine. It was found that the configuration of the butyl chain plays a very important role in film conductivity and in the subsequent efficiency of solar cells, n-bytyl derivative being the most effective hole transporter. Such a result is due to the fact that n-butyl derivative allows better packing of the molecules in the film and stronger π-π interaction  

Surface modification of SnO2 electron transporting layer (ETL) plays a critical role in the performance of SnO2-based planar perovskite solar cells (PSC). Here, we show how long-time NH4F-based water bath treatment of SnO2 layer makes smoothing and morphological improvements and enhances the device performance. Recently it was shown that short-time NH4F treatment (2 sec) with spin coating method reduces interface traps by improving surface chemistry. Here we observe the smoothing of SnO2 films as a result of long-time NH4F treatment, which could be a result of a slight etching-deposition process. Absorption and resistivity measurements indicate that SnO2 etching process is involved in...