All-inorganic Perovskite Solar Cells Research Articles

Preparation of Highly Efficient and Stable All-Inorganic CsPbBr3 Perovskite Solar Cells Using Pre-Crystallization Multi-Step Spin-Coating Method

All-inorganic CsPbBr3 perovskite solar cells have garnered extensive attention in the photovoltaic domain due to their remarkable environmental stability. Nevertheless, CsPbBr3 prepared using the conventional sequential deposition method suffers from issues such as inferior crystallinity, low phase purity, and poor film morphology. Herein, we propose a pre-crystallization methodology by introducing a minute quantity of CsBr into the PbBr2 precursor solution to generate a small amount of CsPb2Br5 crystals within the PbBr2 film, leading to a porous PbBr2 film with enhanced crystallinity. Under the influence of more pores and CsPb2Br5 crystals as nucleation sites for inducing growth, a CsPbBr3 film with a larger crystal size, lower grain boundary density, stronger crystallinity, and higher phase purity is formed. Compared with untreated devices, photovoltaic devices prepared using the pre-crystallization method achieved a champion photovoltaic conversion efficiency (PCE) of 8.62%. Furthermore, pre-crystallized devices demonstrate higher stability than untreated ones and can still retain 94% of the original PCE after being exposed to air for 1000 h without encapsulating.

Tri-Step Water-Assisted Strategy for Suppressing Cs4PbBr6 Phase in Printable Carbon-Based CsPbBr3 Solar Cells to Achieve High Stability.

Often deemed the "natural nemesis" of perovskites, water molecules have been largely circumvented by the majority of researchers in the field of perovskite solar cells. This has resulted in significant hurdles in investigating the beneficial impacts of water molecules on perovskite crystallization. Herein, it is found that by utilizing ethanol with minimal water content and subjecting all-inorganic perovskite to three distinct annealing temperatures within the same solvent, the residual CsBr can be effectively removed, and the formation of the Cs4PbBr6 phase can be curtailed. By selecting an optimal water content, substantial improvements are observed in the crystalline quality of CsPbBr3, the perovskite/carbon interface, and the mesoporous filling effect. The Urbach energy (Eu) is reduced from 38.96 to 35.59meV, and the defect density decreased from 4.16×1014 to 3.39×1014cm-3. As a result, the power conversion efficiency (PCE) improved from 7.55% in the control group to 9.37%. Under severe environmental conditions with a temperature (T) of 85°C and a relative humidity (RH) of 40%, tracking tests over 1200h retained 89.3% of the initial PCE. This research signifies a breakthrough in the fabrication of highly stable and efficient all-inorganic printable mesoscopic perovskite solar cells.

Effective surface treatment for efficient and stable inverted inorganic CsPbI2Br perovskite solar cells

The interest in all-inorganic perovskite solar cells (PSCs) featuring a p-i-n structure is on the rise, attributed to their superior heat resistance and adaptability with tandem cell methods. However, their progress has been far from the regular structure owing to the comparatively low open circuit voltage (Voc). This research employs phenylethylammonium iodide, incorporating various side groups, as passivators to tackle the previously mentioned problems and investigate their effects on passivation. It is found that a reduction of trap-state density in perovskite film was accomplished due to the PEAI effective passivation effect by establishing coordination with the under-coordinated Pb2+ ions. Furthermore, there was an enhancement in the alignment of energy levels at the CsPbI2Br perovskite/PCBM junction, resulting in better charge extraction from the CsPbI2Br layer to the charge transport layer. As a result, an improved champion efficiency of 14.26 % with a Voc of 1.11 V, Jsc of 16.21 mA/cm2, and FF of 79.28 % was yielded for the PEAI treatment inverted CsPbI2Br device, compared with the 12.15 % efficiency of the control device. Superior device stability was exhibited for the optimal PEAI-treated devices without encapsulation. This research validates the significance of a side group on a surface passivation molecule to effectively passivate defects and optimize energy levels, especially for boosting Voc.

Pseudohalide-Based Ionic Liquids: Advancing Crystallization Kinetics and Optoelectronic Properties in All-Inorganic Perovskite Solar Cells.

This study delves into the innovative approach of enhancing the efficiency and stability of all-inorganic perovskite solar cells (I-PSCs) through the strategic incorporation of thiocyanate (SCN-) ions via pseudohalide-based ionic liquid (IL) configurations. This straightforward methodology has exhibited captivating advancements in the kinetics of crystallization as well as the optoelectronic characteristics of the resulting perovskite films. These developments hold the promise of enhancing not only the quality and uniformity of the films but also aspects such as band alignment and the efficacy of charge transfer mechanisms. Calculation results corroborate that the incorporation of 1-butyl-3-methylimidazolium thiocyanate (BmimSCN)led to a significant redistribution of electron state density and enhanced electron-donating properties, indicating a substantial electron transfer between the perovskite material and the IL. Notably, the engineered devices demonstrate a remarkable efficiency surpassing 15%, a substantial enhancement attributed to the synergistic effects of the SCN- ion. Additionally, this approach offers inherent stability benefits, thereby addressing a significant challenge in I-PSC technology. This IL maintains >90% of the initial efficiency after 600h, while the control device decreased to <20% of its initial value after only 100h. 1-butyl-3-methylimidazolium iodide (BmimI) is also employed to further investigate the effects of SCN- ions on device performance.

Design and optimization of all-inorganic lead-free perovskite solar cells with RbGeI3/KSnI3 heterojunction structure

Currently, the performance of inorganic and non-toxic perovskite solar cells (PSCs) lags far behind that of organic and Pb-containing PSCs. To enhance the photovoltaic capabilities of inorganic and non-toxic perovskites, a fully inorganic RbGeI3/KSnI3 heterojunction without hole transport layer is proposed, and simulation and optimization are performed using SCAPS-1D software. Research findings indicate that the RbGeI3/KSnI3 perovskite heterojunction significantly improves the quantum efficiency compared to single-layer perovskite, and due to the more matched energy levels, it improves the electric field of the cell and is more conducive to the migration of photogenerated carriers, resulting in excellent device performance. Moreover, PSCs undergo optimization across multiple parameters, including materials for the charge transport layer, perovskite layer thickness, defect density, bandgap, operating temperature, and so on. This comprehensive approach involves analyzing changes in electric field, band structure, and recombination rate. Finally, the power conversion efficiency of the optimized device achieves 40.44 %, marking a significant 440 % increase compared to the 7.49 % efficiency of single-layer PSCs. This work proposes a heterojunction structure to create efficient inorganic and non-toxic perovskite solar cells, providing a novel strategy for further development in this field.

Non-destructive buffer enabling near-infrared-transparent inverted inorganic perovskite solar cells toward 1400 h light-soaking stable perovskite/Cu(In,Ga)Se2 tandem solar cells

Near-infrared (NIR) transparent inverted all-inorganic perovskite solar cells (PSCs) are excellent top cell candidates in tandem applications. An essential challenge is the replacement of metal contacts with transparent conductive oxide (TCO) electrodes, which requires the introduction of a buffer layer to prevent sputtering damage. In this study, we show that the conventional buffers (i.e., small organic molecules and atomic layer deposited metal oxides) used for organic-inorganic hybrid perovskites are not applicable to all-inorganic perovskites, due to non-uniform coverage of the vulnerable layers underneath, deterioration upon ion bombardment and moisture induced perovskite phase transition. A thin film of metal oxide nanoparticles by the spin-coating method serves as a non-destructive buffer layer for inorganic PSCs. All-inorganic inverted near-infrared-transparent PSCs deliver a PCE of 17.46% and an average transmittance of 73.7% between 780 and 1200 nm. In combination with an 18.56% Cu(In,Ga)Se2 bottom cell, we further demonstrate the first all-inorganic perovskite/CIGS 4-T tandem solar cell with a PCE of 24.75%, which exhibits excellent illumination stability by maintaining 86.7% of its initial efficiency after 1400 h. The non-destructive buffer lays the foundation for efficient and stable NIR-transparent inverted inorganic perovskite solar cells and perovskite-based tandems.

Additive engineering by dicyandiamide for high-performance carbon-based inorganic perovskite solar cells

Hole transport layer (HTL)-free, all-inorganic CsPbIxBr3-x carbon-based perovskite solar cells (C-PSCs) have attracted much attention due to their low cost and excellent stability. The poor device efficiency is a barrier to constrain its commercialization, mainly due to the large amount of interfacial and bulk defects existed in inorganic perovskite films. In this study, an organic small molecule dicyandiamide (DCD) is added to the perovskite precursor as an additive to adjust the crystallization kinetics and passivate defects of inorganic perovskite films, simultaneously. It is demonstrated that the introduction of DCD can not only accelerate the transition process from intermediate-phase DMAPbI3 to inorganic perovskite, but also passivate defects through the Lewis acid-base interaction between cyano (CN), imine (CN) groups, and uncoordinated Pb2+. Meanwhile, the energy level alignment was optimized, which effectively improves the charge transport efficiency of CsPbIxBr3-x C-PSCs. As a result, optimized device shows an enhanced efficiency from 14.07% to 15.84%, accompanied by improved long-term stability.

Passivation of interfacial defects of ZnO and CsPbBr3 by inserting NaSCN in all-inorganic perovskite solar cells

Passivation of interfacial defects of ZnO and CsPbBr3 by inserting NaSCN in all-inorganic perovskite solar cells

Screening of Functional Small Molecules via Modified Machine Learning Strategy toward Efficient All-Inorganic Perovskite Solar Cells.

Organic small molecules are proven to be capable of passivating the bulk/interfacial defects in inorganic perovskite solar cells. Considering the burdensome situation to screen the functional small molecules, we employ a modified machine learning (ML) strategy to guide screening suitable small molecules toward efficient solar cells through three modified ML algorithms to construct the prediction model: (i) random forest algorithm (RF), (ii) support vector machine algorithm (SVR), and (iii) XGBoost. Among them, the XGBoost algorithm displays a better overall predictive performance, whereby the R2 index reaches 0.939. Accordingly, eight small molecules are selected to modify the interface of perovskite films, and both the theoretical and experimental results certify that the difluorobenzylamine with additional fluorine atoms has a better interface modification effect among the small molecules containing functional groups, e.g., the benzene ring and amino group. The high accuracy of the modified machine learning model enables us to simplify the small-molecule screening process and form an important step for ongoing developments in perovskite solar cells and other optoelectronic devices.

Interface engineering for highly efficient carbon-based all-inorganic perovskite solar cells using functionalized amino acid salts

Interface engineering for highly efficient carbon-based all-inorganic perovskite solar cells using functionalized amino acid salts

Theoretical Study and Analysis of CsSnX3 (X = Cl, Br, I) All-Inorganic Perovskite Solar Cells with Different X-Site Elements.

In this research, SCAPS-1D simulation software (Version: 3.3.10) was employed to enhance the efficiency of CsSnX3 (X = Cl, Br, I) all-inorganic perovskite solar cells. By fine-tuning essential parameters like the work function of the conductive glass, the back contact point, defect density, and the thickness of the light absorption layer, we effectively simulated the optimal performance of CsSnX3 (X = Cl, Br, I) all-inorganic perovskite solar cells under identical conditions. The effects of different X-site elements on the overall performance of the device were also explored. The theoretical photoelectric conversion efficiency of the device gradually increases with the successive substitution of halogen elements (Cl, Br, I), reaching 6.09%, 17.02%, and 26.74%, respectively. This trend is primarily attributed to the increasing size of the halogen atoms, which leads to better light absorption and charge transport properties, with iodine (I) yielding the highest theoretical conversion efficiency. These findings suggest that optimizing the halogen element in CsSnX3 can significantly enhance device performance, providing valuable theoretical guidance for the development of high-efficiency all-inorganic perovskite solar cells.

Challenges and modification strategies of air-processed all-inorganic CsPbX3 perovskite films for efficient photovoltaics

All-inorganic perovskites CsPbX3 (X: halogen ions) have gained significant attention for application in next generation photovoltaic technologies due to their superior thermal stability and excellent optoelectronic properties. Compared with fabrication in N2 glove boxes, ambient air processing could simplify the operation and reduce the fabrication cost, which is favorable for boosting the commercialization of perovskite solar cells (PSCs). However, the moisture in ambient air tends to cause the phase transformation of inorganic perovskite from the photoactive black phase to the photo-inactive yellow one, thus deteriorating the photovoltaic performance. Considering the obstacles from both the intrinsic structure instability and the external atmosphere, tremendous efforts have been made for pursuing high-efficiency and stable all-inorganic PSCs that can be processed in ambient air. In this review, we first analyze the challenges for fabricating CsPbX3 in ambient air from both the intrinsic characters and external atmosphere and then overview the progress of the air-fabricated CsPbX3 films for photovoltaic applications. The recently reported various modification strategies, including the compositional/precursor, solvent, additive, and interface engineering, for achieving high-quality and stable CsPbX3 films are comprehensively summarized. Finally, a brief conclusion and outlook is given to inspire more research interest on air-fabricated CsPbX3 photovoltaics. This review provides significant guidance for further optimizing the air-processible CsPbX3 films to boost the large-scale commercialization of cost-effective PSCs in the future.

Effects of 3-Bromo-N-methylbenzylamine modification on CsPbI2Br perovskite films and perovskite solar cells

In this work, 3-Bromo-N-methylbenzylamine (3-B-N-MB) was designed to modify CsPbI2Br/hole transport layer interface to reduce the interfacial non-radiative recombination loss of all-inorganic CsPbI2Br perovskite solar cells (PSCs). The effects of 3-B-N-MB modification on the morphology, structure, optical absorption, defect concentration, carrier lifetime, energy level, hydrophobicity of CsPbI2Br perovskite film and device performance, and carrier dynamics, as well as their mechanisms were systematically studied. The results show that the lone pair electrons in the N atom of N-H group in strongly alkaline 3-B-N-MB is more conducive to coordinate with uncoordinated Pb2+/Cs+ in CsPbI2Br, meanwhile the H atom of N-H group in 3-B-N-MB can react with I−/Br− in CsPbI2Br through hydrogen bonding, passivating interface defects to increase grain size and enhance the crystallinity and density of CsPbI2Br films, optimizing interface energy level matching to promote carrier transport, thus suppressing interfacial non-radiative recombination to improve device performance. As a result, the PCE of the 3-B-N-MB modified PSCs significantly enhanced ∼32.5 % as compared to that of the pristine one and the air stability of the device has also improved. The 3-B-N-MB modification provides a new strategy to enhance the efficiency and stability of all-inorganic perovskite solar cells.

CsPbI3 all-inorganic perovskite solar cells: Development status and theoretical prediction

In this paper, the crystal structure, physical properties, photoelectric conversion efficiency and large-area development of CsPbI3 all-inorganic perovskite solar cells are comprehensively analyzed. The research results of the material in photoelectric conversion efficiency, large-area development and preparation technology are summarized. In addition, through theoretical prediction and simulation, this study simulated a CsPbI3 all-inorganic perovskite solar cell with a photoelectric conversion efficiency of 28.29 %, which provided a theoretical basis for the preparation of high-performance devices.

Bridging the buried interface with conjugated molecule for highly efficient carbon-based inorganic CsPbI2Br perovskite solar cells fabricated in air

Manipulating the buried interface of all-inorganic perovskite solar cells (PSCs) is essential to improve the performance of devices. However, the conventional modifiers of interface typically present insulating feature that can impede the transportation of carrier, leading to an inferior charge transport efficiency. Herein, we propose a conjugated molecule, 2,4-hexadienoic acid potassium salt, which can act as a bridge at the buried interface of device and improve the crystallization of perovskite film. Besides, this interfacial modifier also promotes larger and denser grains, passivating defects and suppress non-radiative recombination of buried interface. Simultaneously, the electrical performance of tin oxide film is enhanced and facilitate a better energy level alignment. Consequently, carbon electrodes-based PSCs (C-PSCs) are fabricated via a hot air-assisted method in air, and C-PSCs based on all-inorganic perovskite demonstrate significant enhancement of open circuit voltage (1.25 V) via conjugated molecule modification, and the power conversion efficiency (PCE) increase significantly from 10.86 % to 13.11 %. Moreover, unencapsulated target devices exhibit better stability than the control devices. This work offers a new idea to construct an interfacial bridge via conjugated molecule for efficient and stable C-PSCs fabricated in air.

Design tungsten oxides hole transport layers (HTLs) to modify the back interface in all-inorganic carbon-based CsPbBr3 solar cells

To enhance the inferior photovoltaic performance of all-inorganic carbon-based perovskite solar cells (C-PSCs) caused by inefficient charge extraction and transport processes of the CsPbBr3/carbon back interface, three types of tungsten oxides (WO3, WO2.72, WO2) are synthesized as low cost and stable hole transport layers (HTLs) to modify the back interface by tunning the energy level alignment. Among the three kinds of tungsten oxides, WO3 shows the best hole extraction and transport capability and the C-PSCs using WO3 HTL generates a power conversion efficiency (PCE) of 7.90% with a high open circuit voltage (Voc) of 1.307 V, indicating a great PCE enhancement of 43.9%, as compared with the device without HTL (5.49%). Meanwhile, WO2.72 and WO2 also are also proved to be qualified HTLs and the devices show PCE values of 7.57% and 6.24%, respectively. Importantly, WO3 and WO2.72 based device show excellent stabilities with PCE retention over 90% of the initial PCE values under ambient conditions for 60 days.

Maximizing photovoltaic performance of all-inorganic perovskite CsSnI3-xBrx solar cells through bandgap grading and material design

In the modern era of technology, worldwide paradigms have been shifted toward the utilization of green energy. Sun energy is the most astonishing eco-friendly resource of energy and can be harnessed with the help of photovoltaic cells. Hybrid (Organic-Inorganic) perovskite solar cells (PSCs) are emerged with incredible photovoltaic (PV) performance. Nevertheless, a significant challenge lies in their lower stability under diverse environmental conditions. To deal with this challenge, all inorganic cesium-based PSC has been studied and analyzed, results improved stability in comparison to hybrid PSC. However, the noxious nature of lead is deleterious to the environment. So, this work primarily aimed, to study lead-free all inorganic tin-based perovskite compound CsSnI3-xBrx, as the main light absorber layer. Further, to elevate the PV performance of PSC, bandgap grading is performed on CsSnI3-xBrx by varying bromide concentration x from 0 to 3. Bandgap grading encourages the absorption of a wide range of the light spectrum, by modulating bandgap (Eg) / affinity(χ) through the distance of the CsSnI3-xBrx layer. Additionally, it enhances light-generated charge carrier separation and collection by end electrodes. In this work, two different strategies have been adopted, linear and parabolic. During linear grading, the impact of variation in x (0 to 3) has been analyzed over the thickness 50–––500 nm in 10 linear steps for CsSnI3-xBrx. The highest PCE fetched from linearly graded layered FTO / CeO2 / CsSnI3-xBrx / CFTS / Gold PSC is 21.68 %. Similarly, in the parabolic graded absorber layer, the influence of change in the bowing factor (0 to 1), has been analyzed relative to different values of x (0 to 3). With improvement in PV performance, the maximum PCE delivered by parabolic-graded PSC is 23.61 %. Additionally, this work extends to check the compatibility of distinct electron transport layers (ETLs) and hole transport layers (HTLs). Upon analysis, it has been found that the best PV performance was obtained while selecting SnO2 / PEDOT as ETL / HTL respectively.

Over 12% efficient CsSnI3 perovskite solar cells enabled by surface post-treatment with bi-functional polar molecules

Eco-friendly all-inorganic tin halide perovskite compounds have drawn significant attention for photovoltaic applications. Nevertheless, the non-radiative recombination derived from the uncoordinated Sn2+ cations at surface and the electron extraction barrier between different functional layers significantly impair the performance of perovskite device. Here we for the first time show that thiophene derivative, 3-thiophenemethylammonium iodide, as an interface modifier between the CsSnI3 perovskite surface and electron transport layer, can passivate defects and reduce the electron extraction potential barrier. The molecules of 3-thiophenemethylammonium iodide can autonomously inter-connect with uncoordinated Sn2+via lone electron pairs of the donated π electrons in electronic-rich thiophene molecule. Moreover, such interface modifier lowers the electron extraction potential barrier at the perovskite/electron transport layer junction in which an interface dipole electric field form. Consequently, the optimized planar solar cell with a structure of ITO/PEDOT:PSS/CsSnI3/ICBA/BCP/Ag, exhibited a power conversion efficiency of 12.05 % under AM 1.5G illumination condition. To the best of our knowledge, this is the highest efficiency for fully inorganic CsSnI3-based devices reported so far. This study represents an innovative approach to realize high-efficiency all-inorganic CsSnI3 perovskite solar cells.

Enhancing carrier collection in CsPbBr3 solar cells through crystal orientation and defect passivation

All-inorganic carbon-based CsPbBr3 perovskite solar cells (PSCs) have gained growing interest for their remarkable stability. However, compared to their organic–inorganic hybrid counterparts, there is still substantial room for improving their performance primarily due to the inferior photogenerated carrier collection efficiency. Here, we employ area-dependent transient photocurrent to assess the carrier transit time in CsPbBr3 PSCs, revealing that an extended carrier transit time relative to the lifetime significantly contributes to their low carrier collection efficiency. To address this challenge, we narrow the gap between carrier transit time and lifetime by introducing a dual-functional additive, serving to facilitate both crystallization orientation and defect passivation. Consequently, we achieve enhanced short-circuit current and efficiency in CsPbBr3 PSCs.

Multifunctional Interface Modification Enables Efficient and Stable HTL-Free Carbon-Electroded CsPbI2Br Perovskite Solar Cells.

In recent years, hole transport layer-free all-inorganic CsPbI2Br carbon-electroded perovskite solar cells (C-PSCs) have garnered significant attention due to a trade-off between stability and photovoltaic performance. However, there are inevitably many defects generated at the surfaces or grain boundaries of CsPbI2Br perovskite films, which will serve as carrier non-radiative recombination centers, and CsPbI2Br perovskite films are sensitive to water molecules to degrade, together with energy level mismatch between CsPbI2Br perovskite and carbon electrodes. Herein, 1-benzyl-3-methylimidazolium hexafluorophosphate (1-B-3-MIMPF6), an imidazolium-based ionic liquid simultaneously containing benzene ring and fluorine atoms, was introduced for the modification of the perovskite/carbon interface. The results showed that it could effectively reduce defects, enhance carrier transfer, mitigate carrier non-radiative recombination, facilitate energy alignment, and block moisture intrusion. Therefore, the photovoltaic performance of the modified PSCs with ITO/SnO2/CsPbI2Br/1-B-3-MIMPF6/carbon architecture has been boosted with a champion power conversion efficiency (PCE) of 13.47 %, open circuit voltage of 1.20 V, short circuit current density of 14.69 mA/cm2, and fill factor of 76 %. Moreover, the unencapsulated modified devices exhibited an improved stability and the PCE maintained 78 % of their initial PCE after 24 h storage at room temperature in a 30 %-35 % humidity environment, whereas that of the pristine devices dropped to almost zero.