High-efficiency Perovskite Solar Cells Research Articles

Homogeneous crystallization of MA-free, wide-bandgap perovskite films via self-assembled monolayer capping for laminated silicon/perovskite tandem solar cells

Methylammonium (MA)-free wide-bandgap perovskite films with improved thermal/light stabilities have gained considerable attention for its application in silicon/perovskite tandem solar cells. However, compared to their MA counterparts, MA-free films often suffer from fast crystallization, resulting in uneven surface morphology, poor crystalline features, and excess PbI2 impurities. To modulate the crystallization dynamics of MA-free wide-bandgap Cs0.22FA0.78Pb(Br0.15I0.85)3 films, this study proposes a self-assembled monolayer (SAM)-capped crystallization strategy, wherein C42H52N6O4RuS2 (Z907) is added to the isopropanol antisolvent in the one-step solution process. The optimized Cs0.22FA0.78Pb(Br0.15I0.85)3 film has a wide bandgap of 1.68 eV with superior morphological/crystalline properties, enhanced thermal/moisture stability, and improved interfacial energy‐level alignment. These favorable characteristics are attributed to the efficient coupling between the positive ion vacancies in the precursor, the −SCN and –COOH functional groups in Z907, and the superhydrophobic nonyl chains in the Z907 SAM. The semitransparent perovskite solar cells (PSCs) built with the optimized Cs0.22FA0.78Pb(Br0.15I0.85)3 films demonstrate substantially high power conversion efficiencies (PCEs) of 21.63 %@0.09 cm2 and 19.12 %@1 cm2. Furthermore, based on the high-efficiency PSCs, the corresponding two-terminal laminated silicon/perovskite tandem solar cells achieved record-high PCEs of 32.07 %@0.09 cm2 and 28.32 %@1 cm2 with negligible hysteresis and improved humidity/thermal stability.

Methylammonium-Free Ink for Blade-Coating of Pure-Phase α-FAPbI3 Perovskite Films in Air.

The α-c (α-FAPbI3) has been extensively employed in the fabrication of high-efficiency perovskite solar cells, yet heavily relied on multiple additives in upscalable fabrication in air. In this work, a simple α-FAPbI3 ink is developed for the blade-coating fabrication of phase-pure α-FAPbI3 in ambient air free from any additives containing extrinsic ions. The introduction of 2-imidazolidinone (IMD) to the FAPbI3 precursor inks leads to the formation of intermediate phases that change the phase transition pathway from δ-FAPbI3 to α-FAPbI3 by tilting the PbI6 octahedrons with strong coordination to Pb2+. Furthermore, the IMD ligands in the intermediate phase gradually escape from the perovskite film during the annealing, leaving a phase-pure α-FAPbI3 film vertically grown with large grains. Consequently, the small-sized PSCs fabricated with blade-coated α-FAPbI3 film achieve an efficiency of up to 23.14%, and the corresponding mini-module yields an efficiency of 19.66%. The device performance is among the highest reported for phase-pure α-FAPbI3 PSCs fabricated in the air without non-native cations or chloride additives, offering a simple and robust fabrication approach of phase-pure α-FAPbI3 films for PV application.

Vertically oriented low-dimensional perovskites for high-efficiency wide band gap perovskite solar cells.

Controlling crystal growth alignment in low-dimensional perovskites (LDPs) for solar cells has been a persistent challenge, especially for low-n LDPs (n < 3, n is the number of octahedral sheets) with wide band gaps (>1.7 eV) impeding charge flow. Here we overcome such transport limits by inducing vertical crystal growth through the addition of chlorine to the precursor solution. In contrast to 3D halide perovskites (APbX3), we find that Cl substitutes I in the equatorial position of the unit cell, inducing a vertical strain in the perovskite octahedra, and is critical for initiating vertical growth. Atomistic modelling demonstrates the thermodynamic stability and miscibility of Cl/I structures indicating the preferential arrangement for Cl-incorporation at I-sites. Vertical alignment persists at the solar cell level, giving rise to a record 9.4% power conversion efficiency with a 1.4 V open circuit voltage, the highest reported for a 2 eV wide band gap device. This study demonstrates an atomic-level understanding of crystal tunability in low-n LDPs and unlocks new device possibilities for smart solar facades and indoor energy generation.

Challenges and opportunities in high efficiency scalable and stable perovskite solar cells

Perovskite solar cells (PSCs) are the fastest-growing photovoltaic (PV) technology and hold great promise for the photovoltaic industry due to their low-cost fabrication and excellent efficiency. To achieve commercial readiness level, the most important factor would be yield beyond 95% at the PSC module levels. The current essential requirements for PSCs are reproducibility of high efficiency devices, scalability, and stability. The reported certified high efficiency (24–26%) results are based on the use of FAPbI3 perovskites with a bandgap of Eg≈ 1.5 eV, and the typical device's active area ranges from ≈ 0.1 cm2 to a maximum of 1 cm2. However, relatively higher bandgap PSCs are essential, especially in tandem solar cell applications. Hence, optimization of higher bandgap PSCs is a necessity. As the bandgap of the perovskites increases, the efficiency goes down due to reduced JSC and increased VOC loss. Therefore, understanding the loss mechanism and corresponding solutions need to be developed. Scaling up the device's active area without compromising the fill factor and, hence, efficiency is non-trivial. So, understanding the loss mechanism in large area devices is crucial. The stability analysis reported in the literature is inconsistent, preventing data comparison and identifying various degradation factors or failure mechanisms. Moreover, how the accelerated tests would be useful in predicting the real lifetime of the solar cells is yet to be developed. So, understanding the knowledge and the technological gaps between laboratory and industry-scale production is crucial for further development. Therefore, in this review article, we discuss the challenges and opportunities for scalable and stable high efficiency PSCs.

Innovative Approaches to Large-Area Perovskite Solar Cell Fabrication Using Slit Coating.

Perovskite solar cells (PSCs) are gaining prominence in the photovoltaic industry due to their exceptional photoelectric performance and low manufacturing costs, achieving a significant power conversion efficiency of 26.4%, which closely rivals that of silicon solar cells. Despite substantial advancements, the effective area of high-efficiency PSCs is typically limited to about 0.1 cm2 in laboratory settings, with efficiency decreasing as the area increases. The limitation poses a major obstacle to commercialization, as large-area, high-quality perovskite films are crucial for commercial applications. This paper reviews current techniques for producing large-area perovskites, focusing on slot-die coating, a method that has attracted attention for its revolutionary potential in PSC manufacturing. Slot-die coating allows for precise control over film thickness and is compatible with roll-to-roll systems, making it suitable for large-scale applications. The paper systematically outlines the characteristics of slot-die coating, along with its advantages and disadvantages in commercial applications, suggests corresponding optimization strategies, and discusses future development directions to enhance the scalability and efficiency of PSCs, paving the way for broader commercial deployment.

Removal of Residual Additive Enabling Perfect Crystallization of Photovoltaic Perovskites.

Achieving high-efficiency perovskite solar cells (PSCs) hinges on the precise control of the perovskite film crystallization process, often improved by the inclusion of additives. While dimethyl sulfoxide (DMSO) is traditionally used to manage this process, its removal from the films is problematic. In this work, methyl phenyl sulfoxide (MPSO) was employed instead of DMSO to slow the crystallization rate, as MPSO is more easily removed from the perovskite structure. The electron delocalization associated with the benzene ring in MPSO decreases the electron density around the oxygen atom in the sulfoxide group, thus reducing its interaction with PbI2. This strategy not only sustains the formation of a crystallization-slowing intermediate phase but also simplifies the elimination of the additive. Consequently, the optimized PSCs achieved a leading power conversion efficiency (PCE) of 25.95% along with exceptional stability. This strategy provides a novel method for fine-tuning perovskite crystallization to enhance the overall performance of photovoltaic devices.

Understanding the Impact of SAM Fermi Levels on High Efficiency p-i-n Perovskite Solar Cells.

Completing the picture of the underlying physics of perovskite solar cell interfaces that incorporate self-assembled molecular layers (SAMs) will accelerate further progress in p-i-n devices. In this work, we modified the Fermi level of a nickel oxide-perovskite interface by utilizing SAM layers with a range of dipole strengths to establish the link between the resulting shift of the built-in potential of the solar cell and the device parameters. To achieve this, we fabricated a series of high-efficiency perovskite solar cells with no hysteresis and characterized them through stabilize and pulse (SaP), JV curve, and time-resolved photoluminescence (TRPL) measurements. Our results unambiguously show that the potential drop across the perovskite layer (in the range of 0.6-1 V) exceeds the work function difference at the device's electrodes. These extracted potential drop values directly correlate to work function differences in the adjacent transport layers, thus demonstrating that their Fermi level difference entirely drives the built-in potential in this device configuration. Additionally, we find that selecting a SAM with a deep HOMO level can result in charge accumulation at the interface, leading to reduced current flow. Our findings provide insights into the device physics of p-i-n perovskite solar cells, highlighting the importance of interfacial energetics on device performance.

Comprehensive study on phase stability of lead-free Sn-based perovskite FAxMA1-xSnI3

Perovskite solar cells have become the most important devices for solar power to electricity conversion. However, currently, high-efficiency perovskite solar cells still rely on the use of Pb, which is harmful to the environment. Seeking environmentally friendly perovskite solar cells is imperative, and Sn is the most effective substitute for Pb. However, Sn-based perovskites face challenges due to their brief lifespan and rapid degradation, underscoring the need to improve their phase stability - a problem with still unclear mechanisms. This study addresses this by adjusting the ratio of formamidinium to methylammonium (FA/MA) in FAxMA1-xSnI3, experimentally finding optimal stability in phase composition and photoluminescence intensity at a ratio where x = 0.75. Using Density Functional Theory (DFT) and a pre-trained, fine-tuned machine-learning model, we explore the favorable molecular structures and configurations within FAxMA1-xSnI3. We discover that the FA0.75MA0.25SnI3 composition exhibits the lowest valence band maximum, indicating minimal oxidation tendency. Further DFT calculations of mixing and formation energies confirm that this composition is the most stable, aligning well with experimental observations and elucidating the underlying mechanisms of phase stability in Sn-based perovskite solar cells.

Cost-Effective Acetonitrile-Based Precursor Solution Mitigates Heterogeneous Nucleation for Efficient and Stable Perovskite Solar Cells.

Solution-processing is the primary method for fabricating high-efficiency perovskite solar cells (PSCs), where solvent choice critically influences film formation and quality. Although additives can optimize film formation dynamics by balancing nucleation and growth of perovskite, they can also induce heterogeneous nucleation due to competitive coordination and varying crystallization kinetics, leading to compositional heterogeneity and structural disorders. Herein, a perovskite precursor solution is developed using acetonitrile (ACN) as a weak coordination host solvent instead of the traditional N,N-dimethylformamide (DMF). The ACN-based perovskite precursor solution reduces heterogeneous nucleation typically caused by the competitive coordination effect of DMF, and cuts costs by half compared to DMF-based precursor solutions. This approach promotes a single crystallization pathway via a dimethyl sulfoxide-solvated intermediate phase to α-FAPbI3, which extends the anti-solvent operation window, and enhances the crystallinity of perovskite films, and reduces defect states. The power conversion efficiencies (PCE) of 23.62% and 20.13% is achieved for the PSC and minimodule, respectively. The PSC retains over 97% of its initial efficiency after 800h of continuous illumination under maximum power point tracking (MPPT). These findings provide valuable insights into solvent interactions in perovskite film formation and offer a cost-effective strategy for improving the device's performance and stability.

Enhancing light trapping for improved efficiency of perovskite solar cells: design and analysis

Abstract A hybrid organic-inorganic perovskite solar cells (PSCs) is explored for its potential to achieve high-efficiency and cost-effective solar energy conversion, especially through improved light management. In this paper, COMSOL Multiphysics is utilized to explore PSCs with light trapping nanostructures which will enhance the optical and electrical properties. A nanometer-scale concave structure is proposed in this paper to direct and capture light. This configuration is compared to a planar structure to see how it affect PSCs optoelectronic performance. Electrical simulations showed that concave nanostructured PSCs increase carrier generation and collect more carriers. The short-circuit current rose from 3.91 mA for the planar structure to 4.95 mA for the concave structure. Power conversion efficiency for concave PSCs increased 11% compared to the planar construction after choosing optimal height of concave structure. Thus, the performance investigation by combined optical and electrical analysis of nanostructures shows that it has the ability to build high-efficiency PSCs with light-trapping approach.

Exploring the efficiency enhancement of perovskite solar cells by chemical bath depositing SnO2 on mesoporous TiO2 electrode

This study presents a groundbreaking approach to enhance the efficiency of perovskite solar cells (PSCs) by employing Chemical Bath Deposited (CBD) SnO2 on mesoporous TiO2 (m-TiO2) as an electron transport layer (ETL) without a traditional compact TiO2 (c-TiO2) layer between FTO (fluorine-doped tin oxide) and m-TiO2 ETL. Our investigation reveals that this method significantly improves carrier dynamics, as evidenced by reduced time constants compared to traditional ETLs. The CBD SnO2 not only augments electron transport but also effectively reduces defect density in m-TiO2 films. These enhancements are reflected in the improved photovoltaic parameters of the cells, including higher open-circuit voltage (VOC), short-circuit current (JSC), fill factor (FF), and an impressive power conversion efficiency (PCE) exceeding 23.62 %. The study further underscores the scalability of this technology, highlighting advancements in screen printing and chemical bath deposition techniques vital for large-area PSC applications. Remarkably, the uniformity of PCE across large-area cells confirms the efficacy and consistency of this approach, which provides a new and general strategy for preparing high-efficiency PSCs.

Multifunctional Guanidine Ionic Liquid with Lactate Anion-Assisted Crystallization and Defect Passivation for High-Efficient and Stable Perovskite Solar Cells

Multifunctional Guanidine Ionic Liquid with Lactate Anion-Assisted Crystallization and Defect Passivation for High-Efficient and Stable Perovskite Solar Cells

Multifunctional Acetaminophen Interlayer for High Efficiency and Durability Lead-Lean Perovskite Solar Cells.

Due to the easy oxidation of Sn2+, which leads to form tin vacancy defects and poor perovskite film quality, caused by the rapid crystallization rate in tin-based perovskite solar cells (PSCs), their efficiency lags far behind that of lead-based PSCs. To improve the photovoltaic (PV) performance and stability of FA0.9PEA0.1SnI3-based PSCs (T-PSCs), a small amount of Pb(SCN)2 is introduced into a perovskite precursor as an antioxidant, and acetaminophen (ACE) with various functional groups is used to modify a poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS)/perovskite interface. The results show that the Pb(SCN)2 additive and ACE interfacial modification can not only optimize energy level alignment in T-PSCs but also inhibit Sn2+ oxidation to reduce the trap-state density, resulting in promoted carrier transport. The synergetic effect of the Pb(SCN)2 antioxidant and ACE interfacial modification significantly reduces nonradiative recombination and improves the PV performance and stability of T-PSCs. Consequently, the unsealed T-PSCs with the Pb(SCN)2 additive and ACE modification achieve a champion efficiency of 12.04% and maintain 99% of their initial PCE after being stored in N2 for more than 2100 h, while reference T-PSCs demonstrate a champion PCE of 6.20% and retain only 72% of its initial PCE. Moreover, the modified T-PSCs without encapsulation demonstrate much better stability in humid air.

Effect of bromine on the formation of δ-CsPbI3 in Cs0.22FA0.78Pb(I1-xBrx)3 perovskite solar cells

Applying CsxFA1-xPbI3 perovskite is a useful strategy for synthesizing high-efficiency organic-inorganic lead halide perovskite solar cells because it improves the stability of the perovskite structure. High concentration of cesium (Cs) in CsFAPbI3 synthesized under ambient conditions typically lead to phase separation due to δ-CsPbI3 formation and moisture, thereby reducing light absorption and increasing non-radiative recombination. To counter this, we fabricated the mixed halide Cs0.22FA0.78Pb(I1-xBrx)3 perovskite films. Introducing bromine (Br) content effectively reduced the δ-CsPbI3 formation and grain boundaries, thus suppressing the non-radiative recombination between perovskite and charge transport layers. Employing this approach, our perovskite solar cells with a 10 % Br concentration achieved a power conversion efficiency of 15.81 %. This demonstrates the potential of Br incorporation in enhancing the stability and efficiency of perovskite solar cells.

High-Efficiency Perovskite Solar Cells with Improved Interfacial Charge Extraction by Bridging Molecules.

The interface between the perovskite layer and electron transporting layer is a critical determinate for the performance and stability of perovskite solar cells (PSCs). The heterogeneity of the interface critically affects the carrier dynamics at the buried interface. To address this, a bridging molecule, (2-aminoethyl)phosphonic acid (AEP), is introduced for the modification of SnO2/perovskite buried interface in n-i-p structure PSCs. The phosphonic acid group strongly bonds to the SnO2 surface, effectively suppressing the surface carrier traps and leakage current, and uniforming the surface potential. Meanwhile, the amino group influences the growth of perovskite film, resulting in higher crystallinity, phase purity, and fewer defects. Furthermore, the bridging molecules facilitate the charge extraction at the interface, as indicated by the femtosecond transient reflection (fs-TR) spectroscopy, leading to champion power conversion efficiency (PCE) of 26.40% (certified 25.98%) for PSCs. Additionally, the strengthened interface enables improved operational durability of ≈1400 h for the unencapsulated PSCs under ISOS-L-1I protocol.

SnSe2 Quantum Dots and Chlorhexidine Acetate Suppress Synergistically Non-radiative Recombination Loss for High Efficiency and Stability Perovskite Solar Cells.

Non-radiative recombination losses limit the property of perovskite solar cells (PSCs). Here, a synergistic strategy of SnSe2QDs doping into SnO2 and chlorhexidine acetate (CA) coating on the surface of perovskite is proposed. The introduction of 2D SnSe2QDs reduces the oxygen vacancy defects and increases the carrier mobility of SnO2. The optimized SnO2 as a buried interface obviously improves the crystallization quality of perovskite. The CA containing abundant active sites of ─NH2/─NH─, ─C═N, CO, ─Cl groups passivate the defects on the surface and grain boundary of perovskite. The alkyl chain of CA also improves the hydrophobicity of perovskite. Moreover, the synergism of SnSe2QDs and CA releases the residual stress and regulates the energy level arrangement at the top and bottom interface of perovskite. Benefiting from these advantages, the bulk and interface non-radiative recombination loss is greatly suppressed and thereby increases the carrier transport and extraction in devices. As a result, the best power conversion efficiency (PCE) of 23.41% for rigid PSCs and the best PCE of 21.84% for flexible PSCs are reached. The rigid PSC maintains 89% of initial efficiency after storing nitrogen for 3100 h. The flexible PSCs retain 87% of the initial PCE after 5000 bending cycles at a bending radius of 5 mm.

Anti-solvent materials enhanced structural and optical properties on ambiently fabricated perovskite thin films

Perovskite solar cells (PSCs) hold potential for low-cost, high-efficiency solar energy, but their sensitivity to moisture limits practical application. Current fabrication requires controlled environments, limiting mass production. Researchers aim to develop stable PSCs with longer lifetimes under ambient conditions. In this research work, we investigated the stability of perovskite films and solar cells fabricated and annealed in natural air using four different anti-solvents: toluene, ethyl acetate, diethyl ether, and chlorobenzene. Films (about 300 nm thick) were deposited via single-step spin-coating and subjected to ambient air-atmosphere for up to 30 days. We monitored changes in crystallinity, electrical properties, and optics over time. Results showed a gradual degradation in the films’ crystallinity, morphology, and electro-optical properties. Notably, films made with ethyl acetate exhibited superior stability compared to other solvents. These findings contribute to advancing stable and high-performance PSCs manufactured under normal ambient conditions. In addition, we also discuss the possible machine learning (ML) approach to our future work direction to optimize the materials structures, and synthesis process parameters for future high-efficient perovskite solar cells fabrication.

Exploring the potential of end-capping acceptor designing on highly soluble and efficient Schiff-based Hole-Transporting materials for High-Efficiency perovskite solar cells

Photovoltaic materials, especially perovskite solar cells (PSCs) are promising candidates for rising global energy demands. Here, five phenothiazine-based hole-transporting materials (AZOM1, AZOM2, AZOM3, AZOM4, and AZOM5) are designed by Schiff base chemistry with A-π-D-π-A framework for PSCs. We executed density functional theory calculations to explore the electronic, photo-physical, photovoltaic, and charge-transporting properties of the studied hole-transporting materials (HTMs). Our results indicate that AZOM1-AZOM5 HTMs possess more negativeHOMO energies (−5.64 to − 5.49 eV), lower bandgaps, and superior solubility as compared to Spiro-OMeTAD (HOMO energy = − 4.47 eV) and reference AZO-II (HOMO energy = − 4.68 eV), which enhanced their hole extraction and open-circuit photo-voltage (VOC). The transition density matrix and hole-electron distribution analyses show that AZOM1- AZOM5 molecules have ultrafast charge transmission, low overlapping between holes and electrons, and a higher dissociation rate than the Spiro-OMeTAD and AZO-II HTMs. The designed HTMs have smaller exciton binding energies than the Spiro-OMeTAD and AZO-II, allowing electron-hole pairs to dissociate into positive and negative charges smoothly. AZOM1-AZOM5 HTMs have higher hole charge transfer integral than the AZO-II, facilitating high hole mobility in PSCs. All designed HTMs have higher VOC (1.49 to 1.64 V) and lower energy losses (0.63 to 1.03 eV) than the Spiro-OMeTAD and AZO-II HTMs. Moreover, the AZOM1-AZOM5 HTMs demonstrated deeper HOMO energies, high solubility, more stability, and high open-circuit photo-voltages than the recently reported HTMs at “MPW1PW91/6-31G (d, p)” level of theory. Overall, the AZOM1-AZOM5 HTMs are very effective in boosting the solubility, charge-transporting ability, and efficiency of PSCs.

Theory of piezotronic and piezo-phototronic effects on high performance perovskite solar cells

Piezotronic and piezo-phototronic effects can effectively modulate the Schottky barrier height (SBH) of the metal-semiconductor contact and the built-in electric field. Most models focus on the built-in electric field of perovskite solar cells, and polarization-modulated SBH is missing. We investigated piezotronic and piezo-phototronic effects on the Schottky barrier and built-in electric field of perovskite solar cells. A model of the surface potential induced by polarization was developed. The analytical and numerical results are calculated for perovskite solar cells. We found that the piezo-phototronic effect can significantly increase the performance of perovskite solar cells by reducing the height of the Schottky barrier. This model not only provides a fundamental physical picture of the piezotronic and piezo-phototronic effect on perovskite solar cells, but also paves a new path to develop high-efficiency perovskite solar cells.

Composites electron transport layer of PVA-regulated SnO2 for high-efficiency stable perovskite solar cells

As a new and efficient solar cell, perovskite solar cell has attracted wide attention due to its excellent performance. The electron transport layer in perovskite solar cells has a significant impact on device performance. SnO2 films that can be prepared by solution method have become the first choice for electron transport layer due to their simple process and excellent performance. However, the defects in SnO2 thin films and non-radiative recombination sites at the SnO2/Perovskite interface will lead to potential losses in the performance of photovoltaic devices. Therefore, in order to improve the interface loss and interface characteristics and prepare more efficient perovskite solar cells. In this work, a functional polymer, polyvinyl alcohol (PVA), is introduced to regulate the arrangement of SnO2 nanocrystals. The SnO2-PVA composite electron transport layer not only improves carrier transport, but also further affects the growth of perovskite films. PVA inhibits the agglomeration of tin dioxide particles by adding it to the aqueous solution of tin dioxide. Meanwhile, the oxygen vacancy defects in the SnO2 layer have also improved. Correspondingly, SnO2-PVA-based PSCs can be obtained a maximum efficiency of 23.73 %. Attributed to the strengthened interface binding and the improved perovskite crystallization process, the devices obtain good long-term stability, retaining 90 % of their initial performance after 1000 h operation at their maximum power point under 1 sun illumination.