High-performance Perovskite Solar Cells Research Articles

Components and defect density optimization of FAxMA1-xPbI3 based on simulation for high performance perovskite solar cells

Choosing FA+/MA+ mixed-ion perovskite material as the active layer of the perovskite solar cells hold out the prospect of high efficiency and high stability. In this paper, the FA+/MA + ratio is modified to optimize the performance of FAxMA1-xPbI3-based perovskite solar cells utilizing SCAPS-1D. The results indicate that the PCE of the devices reached a minimum of 21 % when x is greater than or equal to 0.6 in FAxMA1-xPbI3(FTO/NiOx/FAxMA1-xPbI3/C60/BCP/Al). When x = 0.6, the impact of the bottom interface defects on the solar cell performance is dominant and the thickness of the active layer should be controlled within a range of 0.4 μm–0.8 μm, while the defect density of the layer is expected to be between 1013 1/cm3 and 1014 1/cm3. By optimizing the perovskite layer thickness, defect density and changing the type of back electrode material, the efficiency is reaching 25.74 % based on the device(FTO/NiOx/FA6MA4PbI3/C60/BCP/Au). This study provides theoretical guidance for experimental research on interface modification, defect passivation and manufacturing of high-efficiency FAxMA1-xPbI3-based perovskite solar cells.

Overcoming stability challenges in perovskite solar cells: Addressing Li ions movement in Spiro-OMeTAD layer through nano-graphdiyne incorporation

The most used hole transport material in high-performance perovskite solar cells (PSCs) is the lithium compounds-doped 2,2′,7,7′-tetrakis(N,N-di-p-methoxyphenylamine)-9,9′-spirobifluorene (Spiro-OMeTAD). However, PSCs based on the Spiro-OMeTAD suffer from serious instability induced by Li+ migration and aggregation. Herein, nano-graphdiyne (nano-GDY) was incorporated into the Spiro-OMeTAD to retard such free Li+ movement and reduce its impact on device operation stability. We verify that the nano-GDY-modified HTL efficiently enhances carrier transport and promotes favorable energy level alignment compared to that of the control HTL, contributing to improved device performance. Furthermore, the coordination interaction between the nano-GDY and Li+ significantly retrains the Li+ migration into the perovskite and SnO2 layers, and meanwhile, eliminates their aggregation with HTLs under elevated temperature and prolonged light soaking. Consequently, the nano-GDY incorporated PSCs exhibit a champion power-conversion efficiency (PCE) of 24.16 % with negligible hysteresis. Encouragingly, the devices also exhibit robust stability, retaining 97 % and 80 % of peak PCE at maxima power point tracking for 6000 s and continuous illumination for 1080 h, respectively.

Side chain modulated ferrocene derivative as the interstitial conductive medium for high-performance and stable perovskite solar cells

The interfacial nonradiative recombination loss caused by the deep traps and mismatched band alignment restrained the commercial viability of perovskite solar cells (PSCs). Herein, we have constructed ferrocene carboxylic acid (FcA) and octafluoropentyl-ferrocenyl-carboxylate (OFFcA) interstitial conductive mediums to modulate the integral heterointerface properties and the photovoltaic performances of PSCs. By comparing the passivation strengths of the two molecules, we found that the synergistic effects among Fc/Fc+ redox shuttle, C=O group, and F substituents realize the optimal elimination of interfacial trap sources. Electron-withdrawing F groups reinforce the capacity of the Fc/Fc+ redox shuttle for the healing of metallic Pb defects and provide extensive anchoring sites to stabilize the organic components. Additionally, the homogeneity of the OFFcA layer as well as the humidity stability of perovskite film are facilitated through the introduction of F substituents, which reduce the contact resistance and improve the interfacial charge transfer. The champion OFFcA-modified device delivers an exceptional PCE of 23.62%, exceeding those of the control (PCE=22.32%) and FcA-modified (PCE=23.06%) devices. Moreover, the unencapsulated OFFcA-modified device retains 82.7% of the primary efficiency at 60% RH for more than 50 d and only loses less than 10% of the primary efficiency when stored in a glove box for more than 2000 h.

Novel dual absorber configuration for eco-friendly perovskite solar cells: design, numerical investigations and performance of ITO-C60-MASnI3-RbGeI3-Cu2O-Au

Perovskite solar cells (PSCs) are increasingly being used as the foundation of the worldwide photovoltaic (PV) industry because of their cost-effective production and durable stability. Perovskite materials, both organic and inorganic, possess distinct optical, mechanical, and electrical properties, such as a high absorption coefficient, a customizable band gap, and a synthesis method based on solutions. This study employed numerical investigations to devise and propose innovative solar cell configurations utilizing the SCAPS-1D simulator. This research presents a Perovskite solar cell design comprising an ITO-C60-MASnI3-RbGeI3-Cu2O-Au solar cell configuration. The unique arrangement of this setup incorporates the use of Indium Tin-oxide (ITO) as the upper contact layer, which is directly exposed to light. The electron transport layer (ETL) is composed of a 0.030 μm thick layer of C60, while the light-harvesting/absorber layers are made up of MASnI3 and RbGeI3, each with a thickness of 0.4 µm. A layer of Cu2O with a thickness of 0.12 μm is employed as the hole transport layer (HTL), whereas the back-contact layer consists of Au. A comparison research was conducted to examine the optimal device configuration. Comprehensive studies are performed to assess the effects of different variables on optimized device performance and power conversion efficiency (PCE). These factors include interface defect densities, thicknesses of different structural layers, band gaps, series and shunt resistance, and operational temperature. The current density (Jsc) is calculated as 32.7 mA/cm2 at an open circuit voltage (Voc) of 0.914 V. Additionally, we observed a power conservation efficiency (PCE) of 20.19 % and an improved fill factor (FF) value of 65.49 %. The ongoing investigations are likely to be valuable for the development and production of cost-effective and high-performance PSCs.

In situ Blending For Co-Deposition of Electron Transport and Perovskite Layers Enables Over 24% Efficiency Stable Conventional Solar Cells.

Simplifying the manufacturing processes of multilayered high-performance perovskite solar cells (PSCs) is yet of vital importance for their cost-effective production. Herein, an in situ blending strategy is presented for co-deposition of electron transport layer (ETL) and perovskite absorber by incorporating (3-(7-butyl-1,3,6,8-tetraoxo-3,6,7,8-tetrahydrobenzo- [lmn][3,8]phenanthrolin-2(1H)-yl)propyl)phosphonic acid (NDP) into the perovskite precursor solutions. The phosphonic acid-like anchoring group coupled with its large molecular size drives the migration of NDP toward indium tin oxide (ITO) surface to form a distinct ETL during perovskite film forming. This strategy circumvents the critical wetting issue and simultaneously improves the interfacial charge collection efficiencies. Consequently, n-i-p PSCs based on in situ blended NDP achieve a champion power conversion efficiency (PCE) of 24.01%, which is one of the highest values for PSCs using organic ETLs. This performance is notably higher than that of ETL-free (21.19%) and independently spin-coated (21.42%) counterparts. More encouragingly, the in situ blending strategy dramatically enhances the device stability under harsh conditions by retaining over 90% of initial efficiencies after 250h in 100°C or 65% humidity storage. Moreover, this strategy is universally adaptable to various perovskite compositions, device architectures, and electron transport materials (ETMs), showing great potential for applications in diverse optoelectronic devices.

Highly flexible and transparent colorless polyimide substrate sandwiched between plasma polymerized fluorocarbon and InGaTiO for high performance flexible perovskite solar cells

ABSTRACT We integrated transparent antireflective coatings and transparent electrodes onto flexible colorless polyimide (CPI) substrates to fabricate high-performance flexible perovskite solar cells. Multifunctional PPFC/CPI/IGTO substrates were fabricated by sputtering the optimal plasma-polymerized fluorocarbon (PPFC) antireflective coating and InGaTiO (IGTO) electrode films on both sides of the CPI substrate. By applying PPFC with a low refractive index (1.38) as an antireflective coating, the transparency of the PPFC/CPI/IGTO substrate increased by an additional 1.2%. In addition, owing to the amorphous characteristics of the PPFC and IGTO layers, the PPFC/CPI/IGTO substrate showed constant sheet resistance and transmittance change even after 10,000 cycles during the bending tests. The flexible perovskite solar cells, fabricated on the PPFC/CPI/IGTO substrate, exhibited an increase in current density of 1.48 mA/cm2 after the deposition of the PPFC antireflective coating. These results confirmed that the PPFC/CPI/IGTO substrate was durable against high-temperature treatment, flexible, and exhibited excellent electrical characteristics. This enhanced the efficiency and durability of the flexible perovskite solar cells. Moreover, the hydrophobic PPFC layer allowed the self-cleaning of inflexible perovskite solar cells. Given these attributes, the PPFC/CPI/IGTO structure has been recognized as a good choice for multifunctional substrates of flexible perovskite solar cells, presenting the potential for enhancing performance.

Blade-Coating (100)-Oriented α-FAPbI3 Perovskite Films via Crystal Surface Energy Regulation for Efficient and Stable Inverted Perovskite Photovoltaics.

Photoactive black-phase formamidinium lead triiodide (α-FAPbI3) perovskite has dominated the prevailing high-performance perovskite solar cells (PSCs), normally for those spin-coated, conventional n-i-p structured devices. Unfortunately, α-FAPbI3 has not been made full use of its advantages in inverted p-i-n structured PSCs fabricated via blade-coating techniques owing to uncontrollable crystallization kinetics and complicated phase evolution of FAPbI3 perovskites during film formation. Herein, a customized crystal surface energy regulation strategy has been innovatively developed by incorporating 0.5 mol % of N-aminoethylpiperazine hydroiodide (NAPI) additive into α-FAPbI3 crystal-derived perovskite ink, which enabled the formation of highly-oriented α-FAPbI3 films. We deciphered the phase transformation mechanisms and crystallization kinetics of blade-coated α-FAPbI3 perovskite films via combining a series of in-situ characterizations and theoretical calculations. Interestingly, the strong chemical interactions between the NAPI and inorganic Pb-I framework help to reduce the surface energy of (100) crystal plane by 42 %, retard the crystallization rate and lower the formation energy of α-FAPbI3. Benefited from multifaceted advantages of promoted charge extraction and suppressed non-radiative recombination, the resultant blade-coated inverted PSCs based on (100)-oriented α-FAPbI3 perovskite films realized promising efficiencies up to 24.16 % (~26.5 % higher than that of the randomly-oriented counterparts), accompanied by improved operational stability. This result represented one of the best performances reported to date for FAPbI3-based inverted PSCs fabricated via scalable deposition methods.

Gas Molecule Assisted All-Inorganic Dual-Interface Passivation Strategy for High-Performance Perovskite Solar Cells.

The trap states at both the upper and bottom interfaces of perovskite layers significantly impact non-radiative carrier recombination. The widely used solvent-based passivation methods result in the disordered distribution of surface components, posing challenges for the commercial application of large-area perovskite solar cells (PSCs). To address this issue, a novel NH3 gas-assisted all-inorganic dual-interfaces passivation strategy is proposed. Through the gas treatment of the perovskite surface, NH3 molecules significantly enhanced the iodine vacancy formation energy (1.54eV) and bonded with uncoordinated Pb2+ to achieve non-destructive passivation. Meanwhile, the reduction of the film defect states is accompanied by a decrease in the work function, which promotes carrier transport between the interface. Further, a stable passivation layer is constructed to manage the bottom interfacial defects using inorganic potassium tripolyphosphate (PT), whose ─P═O group effectively mitigated the charged defects and lowered the carrier transport barriers and nucleation barriers of PVK, while the gradient distribution of K+ improved the crystalline quality of PVK film. Based on the dual-interface synergistic effect, the optimal MA-contained PSCs with an effective area of 0.1 cm2 achieved an efficiency of 24.51% and can maintain 90% of the initial value after aging (10-20% RH and 20°C) for 2000h.

Defect Passivation and Crystallization Regulation for Efficient and Stable Formamidinium Lead Iodide Solar Cells with Multifunctional Amidino Additive.

Amidino-based additives show great potential in high-performance perovskite solar cells (PSCs). However, the role of different functional groups in amidino-based additives have not been well elucidated. Herein, two multifunctional amidino additives 4-amidinobenzoic acid hydrochloride (ABAc) and 4-amidinobenzamide hydrochloride (ABAm) are employed to improve the film quality of formamidinium lead iodide (FAPbI3) perovskites. Compared with ABAc, the amide group imparts ABAm with larger dipole moment and thus stronger interactions with the perovskite components, i.e., the hydrogen bonds between N…H and I- anion and coordination bonds between C = O and Pb2+ cation. It strengthens the passivation effect of iodine vacancy defect and slows down the crystallization process of α-FAPbI3, resulting in the significantly reduced non-radiative recombination, long carrier lifetime of 1.7 µs, uniformly large crystalline grains, and enhances hydrophobicity. Profiting from the improved film quality, the ABAm-treated PSC achieves a high efficiency of 24.60%, and maintains 93% of the initial efficiency after storage in ambient environment for 1200 hours. This work provides new insights for rational design of multifunctional additives regarding of defect passivation and crystallization control toward highly efficient and stable PSCs.

Non-Fullerene Organic Electron Transport Materials toward Stable and Efficient Inverted Perovskite Photovoltaics.

Inverted perovskite solar cells (PSCs) attract continuing interest due to their low processing temperature, suppressed hysteresis, and compatibility with tandem cells. Considerable progress has been made with reported power conversion efficiency (PCE) surpassing 26%. Electron transport Materials (ETMs) play a critical role in achieving high-performance PSCs because they not only govern electron extraction and transport from the perovskite layer to the cathode, but also protect the perovskite from contact with ambient environment. On the other hand, the non-radiative recombination losses at the perovskite/ETM interface also limits the future development of PSCs. Compared with fullerene derivatives, non-fullerene n-type organic semiconductors feature advantages like molecular structure diversity, adjustable energy level, and easy modification. Herein, the non-fullerene ETM is systematically summarized based on the molecular functionalization strategy. Various types of molecular design approaches for producing non-fullerene ETM are presented, and the insight on relationship of chemical structure and device performance is discussed. Meantime, the future trend of non-fullerene ETM is analyzed. It is hoped that this review provides insightful perspective for the innovation of new non-fullerene ETMs toward more efficient and stable PSCs.

Ionic liquid gel microspheres as multifunctional bi-component additives for the crystallinity manipulation and defect passivation in all-air-processed perovskite solar cells

Additives have played a critical role in enhancing the efficiency and stability of perovskite solar cells (PSCs). At present, most of the effective additives are composed of one component, with little attention being given to the potential of bi-component. Herein, we report a novel synergistic strategy to construct ionic liquid gel microspheres (ILG-microspheres) as multifunctional bi-component additives by emulsion polymerization. The synergistic effect of polymeric methyl methacrylate and 1-butyl-3-methylimidazole hexafluorophosphate (BMIMPF6) can effectively improve perovskite crystallization quality and passivated GBs. As a result, an all-air-processed champion device with ILG-microsphere exhibits a power conversion efficiency of 22.31 % with a Voc of 1.206 V. Moreover, the long-term stability of optimized PSC remains 86.5 % of initial efficiency after being stored in the air atmosphere for 1500 h, and its thermal stability is also enhanced. This exploitation of ILG-microsphere as multifunctional bi-component additives provides a promising strategy for the development of all-air-processed high-performance PSCs.

Designed Additive to Regulated Crystallization for High Performance Perovskite Solar Cell

AbstractIt is a crucial role for enhancing the power conversion efficiency (PCE) of perovskite solar cells (PSCs) to prepare high‐quality perovskite films, which can be achieved by delaying the crystallization of perovskite film. Hence, we designed difluoroacetic anhydride (DFA) as an additive to regulating crystallization process thus reducing defect formation during perovskite film formation. It was found DFA reacts with DMSO by forming two molecules, difluoroacetate thioether ester (DTE) and difluoroacetic acid (DA). The strong bonding DTE⋅PbI2 and DA⋅PbI2 retard perovskite crystallization process for high‐quality film formation, which was monitored through in situ UV/Vis and PL tests. By using DFA additives, we prepared perovskite films with high‐quality and low defects. Finally, a champion PCE of 25.28 % was achieved with excellent environmental stability, which retained 95.75 % of the initial PCE after 1152 h at 25 °C under 25 % RH.

Designed Additive to Regulated Crystallization for High Performance Perovskite Solar Cell.

It is a crucial role for enhancing the power conversion efficiency (PCE) of perovskite solar cells (PSCs) to prepare high-quality perovskite films, which can be achieved by delaying the crystallization of perovskite film. Hence, we designed difluoroacetic anhydride (DFA) as an additive to regulating crystallization process thus reducing defect formation during perovskite film formation. It was found DFA reacts with DMSO by forming two molecules, difluoroacetate thioether ester (DTE) and difluoroacetic acid (DA). The strong bonding DTE⋅PbI2 and DA⋅PbI2 retard perovskite crystallization process for high-quality film formation, which was monitored through in situ UV/Vis and PL tests. By using DFA additives, we prepared perovskite films with high-quality and low defects. Finally, a champion PCE of 25.28 % was achieved with excellent environmental stability, which retained 95.75 % of the initial PCE after 1152 h at 25 °C under 25 % RH.

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.

Advancing optoelectronic characteristics of Diketopyrrolopyrrole-Based molecules as donors for organic and as hole transporting materials for perovskite solar cells

A stable and efficient hole-transport material (HTM) is crucial for high-performance perovskite solar cells (PSCs). A 2,2′,7,7′-tetrakis[N,N-di(4-methoxyphenyl)amino]-9,9′-spirobifluorene (Spiro-MeOTAD) being used widely to prepare highly efficient PSCs. However, Spiro-MeOTAD has some limitations due to its complex synthesis, which increases its cost, and it also requires dopants to improve its performance. Therefore, we designed thirteen unique small-molecule-based HTMs (MK1-MK13), which are easy to synthesize, highly cost-effective, and don’t require dopants to prepare efficient PSCs. Their electrical and optical properties are then investigated theoretically using advanced quantum chemical approaches. The designed molecules showed lower energy gaps and improved optical and optoelectronic characteristics because of the improved phase inversion geometry. The detailed photo-physical and optoelectronic characteristics have been studied using density functional theory (DFT) and time-dependent (TD-DFT) calculations. Moreover, we investigated the impact of holes and electrons and the density of states, open-circuit voltage, frontier molecular orbital, transition density matrix, and other structural and photovoltaic characteristics of these materials. Among these, the MK3 molecule possesses the much narrower optical band gap of 1.04 eV and absorbance (λ max) of 684 nm, respectively. In addition, a profound investigation of the MK3/PC61BM blend shows excellent charge transfer at the acceptor–donor interface. Therefore, our proposed technique is necessary for generating appropriate photovoltaic materials for efficient optoelectronic devices and is helpful in further advancing the field.

Air-Processed All-Inorganic Halide Perovskites Integrated Photorechargeable Supercapacitors.

Due to their easy integration for self-powered operation, integrated energy harvesting and storage could be the game changer in smart, flexible, and portable electronic devices. Three-electrode integration is the most promising approach among all possible configurations because it is less complex and compatible with most techniques. Although the photoconversion efficiency has increased above 20% due to the integration of high-performance perovskite solar cells, the electrochemical storage efficiency (efficacy of the integration) is much below 80% due to a significant potential drop and impedance mismatch. In this context, we introduced perovskite-based solid-state thin film supercapacitors integrated with stable, air-processed perovskite solar cells for an uninterrupted power supply. Our measurement shows that the best performance can be achieved by optimizing several parameters, including series-connected solar cells, light intensity, and photovoltaic active area. The critical challenge with these integrated systems is to maintain a uniform charging current of the supercapacitors throughout the charging cycle while minimizing self-discharging. We achieved an electrochemical storage efficiency of ∼87% at an overpotential of 0.8 V. The overpotential can be as low as 2 mV. We fabricated fully solution-processed series-connected solar cells to integrate with stacked supercapacitors to improve the operating voltage beyond 2.1 V. The photocharging and dark discharging of these integrated devices have been tested over 200 cycles, and a negligible drop in efficiency has been observed. Our detailed energy conversion and storage analysis in these systems unveils the mechanism and losses due to three-terminal integration.

Trade-off effect of hydrogen-bonded dopant-free hole transport materials on performance of inverted perovskite solar cells

Benefiting from their ordered orientation and superior stability compared to traditional conjugated materials, hydrogen bonding (HB)-induced H-aggregates in organic small molecule hole-transport materials (HTMs) hold a big potential for high-performance inverted perovskite solar cells (IPSCs). However, H-aggregates can also lead to excessive face-aggregation by forming the gaps between aggregates, which is in turn unfavorable for charge mobility and thus for the overall device performance. Herein, we design and synthesize a new set of HB-containing triphenylamine-based small molecules to tailor the degree of H-aggregation, namely O1 (without HB), O2 (unilateral HB unit), and O3 (bilateral HB units). These HTMs make a clear trade-off effect on the charge mobility within the HTM and the interfacial properties of perovskite and HTM. Although the interfacial hole extraction process is promoted upon the HB-functionalized interface, the best performance of IPSCs is still achieved by O1 HTM, which is mainly influenced by the higher hole mobility without HB-induced H-aggregates. Nevertheless, the photo stability of as-fabricated devices is effectively improved upon the HB passivation effect on the interface of HTM (O2 or O3) and perovskite, as well as the better quality of atop perovskite layers with less grain boundary compared to the reference case (O1).

Synergistic Modulation of Sn-Based Perovskite Solar Cells with Crystallization and Interface Engineering.

A high-quality Sn-based perovskite absorption layer and effective carrier transport are the basis for high-performance Sn-based perovskite solar cells. The suppression of Sn2+ oxidation and rapid crystallization is the key to obtaining high-quality Sn-based perovskite film. And interface engineering is an effective strategy to enhance carrier extraction and transport. In this work, tin fluoride (SnF2) was introduced to the perovskite precursor solution, which can effectively modulate the crystallization and morphology of Sn-based perovskite layer. Furthermore, the hole-transporting layer of PEDOT:PSS was modified with CsI to enhance the hole extraction and transport. As a result, the fabricated inverted Sn-based perovskite solar cells demonstrated a power conversion efficiency of 7.53% with enhanced stability.

In Situ Growth of Nickel Oxide Hole-Transport Layer through the Nickel Oleate Route for High-Performance Perovskite Solar Cells

In Situ Growth of Nickel Oxide Hole-Transport Layer through the Nickel Oleate Route for High-Performance Perovskite Solar Cells

Modulating vacancy-related defects and hole extraction via a multifunctional additive for high-performance perovskite solar cells

Modulating vacancy-related defects and hole extraction via a multifunctional additive for high-performance perovskite solar cells