Certified Power Conversion Efficiency Research Articles

Asymmetric Modification of Carbazole Based Self-Assembled Monolayers by Hybrid Strategy for Inverted Perovskite Solar Cells.

Carbazole-based self-assembled molecules (SAMs) are widely applied in inverted perovskite solar cells (iPSCs) due to their unique molecular properties. However, the symmetrical structure of the carbazole-based SAMs makes it difficult to finely regulate their performance, which impedes the further enhancement of the efficiency and stability of iPSCs. This work shows that by building an asymmetric carbazole core, the crucial properties of SAM molecules can be effectively regulated. It has been confirmed that the hybrid thieno[2,3-b]thiophene unit of this asymmetric core governs the energy level, the surface wettability, and the defect passivation capability of the SAMs, while the substituent of core has a greater impact on the molecular dipole and device stability. The synergistic effects from thieno[2,3-b]thiophene and fluorine lead to the KF-derived iPSC demonstrating a certified power conversion efficiency (PCE) of 25.17% and excellent operational stability. This hybrid design concept offers a promising approach for the further structural modification of SAMs in iPSCs.

High-efficiency and thermally stable FACsPbI3 perovskite photovoltaics.

α-FA1-xCsxPbI3 is a promising absorber material for efficient and stable perovskite solar cells (PSCs)1,2. However, the most efficient α-FA1-xCsxPbI3 PSCs require the inclusion of methylammonium chloride (MACl) additive3,4, which generates volatile organic residues (i.e., MA) that limit device stability at elevated temperatures5. To date, the highest certified power-conversion efficiency (PCE) of α-FA1-xCsxPbI3 PSCs without MACl was only ~24% (ref.6,7), and has yet to exhibit any stability advantages. Here, we identify interfacial contact loss caused by the Cs+ accumulation for the conventional α-FA1-xCsxPbI3 PSCs, which deteriorates the device performance and stability. Through in-situ GIWAXS analysis and DFT calculations, we demonstrate an intermediate phase-assisted crystallization pathway enabled by acetate surface coordination to fabricate high-quality α-FA1-xCsxPbI3 film, without using MA-additive. We herein report a certified stabilized power output (SPO) efficiency of 25.94% and a reverse-scanning PCE of 26.64% for α-FA1-xCsxPbI3 PSCs, exhibiting negligible contact losses and enhanced operational stability. The devices retain >95% of their initial PCEs after over 2,000 hours operating at maximum power point under 1 sun, 85 °C, and 60% relative humidity (ISOS-L-3).

Enhanced Design of Kesterite Solar Cells through High-Throughput Screening and Machine Learning Approaches.

Kesterite Cu2ZnSnS4 (CZTS) is regarded as one of the most promising materials for thin-film solar cells due to its high light absorption capability, composition of earth-abundant and nontoxic elements, and ease of low-cost mass production. Although the certified power conversion efficiency (PCE) of kesterite solar cells has exceeded 14%, this efficiency remains significantly below the Shockley-Queisser limit. In this study, we generated a Perdew-Burke-Ernzerhof (PBE) band gap data set encompassing 263 64-atom species for high-throughput screening by substituting elements at different sites in A2BCX4 quaternary kesterite materials. Additionally, we utilized a symbolic regression method based on genetic programming to explore the functional relationship among the oxidation state, ionic radius, and electronegativity of kesterites with PBE band gaps. Simultaneously, we employed decision tree models (XGBoost, LightGBM, CatBoost, and random forest) and convolutional neural network (CNN) models (CustomCNN, VGG16, DenseNet121, Xception, and EfficientNetV2B0) to predict band gaps, achieving a coefficient of determination (R2) of up to 0.93. Furthermore, we selected 54 kesterite materials with PBE band gaps ranging from 0.4 to 1.5 eV for detailed electronic structure calculations with Heyd-Scuseria-Ernzerhof (HSE06) functional and investigated the effects of B-site atomic substitutions on the performance of solar cell materials. Compared to Ag2CaSnSe4, Ag2SrSnSe4 exhibits fewer deep defects and richer shallow defects, which contribute to an increased carrier concentration and reduced charge and energy losses, making it a superior candidate for solar cell applications.

Effects of Alkali Elements on Copper Indium Gallium Aluminum Selenide Flexible Solar Cells Fabricated on Polyimide Substrates.

Polycrystalline Cu(InGaAl)Se2 (CIGAS) thin films were prepared on polyimide (PI) foils by depositing aluminum (Al) and CIGS precursor layers. Three ceramic CIGS quaternary targets with different sodium (Na) contents were used for investigating the influences of alkali doping at an annealing temperature of 500 °C. The Al concentration was enriched at the front interfaces of absorber films with different Na doping amounts after annealing. Na in the precursor layer diffused to both interfaces during the annealing process, most Na diffused into the Mo layer, and Na existed in the annealed film as compounds Na2Sex and Na2SeO3. An appropriate amount Na element could be beneficial for grain growth in the region beneath the surface. Low Na doping had no significant effect on the crystallization property. High Na doping effected the diffusion of the Cu2-xSe liquid phase and reduced the grain size. On the basis of good crystallization, the passivation effect of Na can effectively improve the performance of cells. A certified power conversion efficiency of 16.19% of a CIGAS flexible solar cell with a 0.54 cm2 active area has been achieved.

Surface chemical polishing and passivation minimize non-radiative recombination for all-perovskite tandem solar cells

All-perovskite tandem solar cells have shown great promise in breaking the Shockley–Queisser limit of single-junction solar cells. However, the efficiency improvement of all-perovskite tandem solar cells is largely hindered by the surface defects induced non-radiative recombination loss in Sn–Pb mixed narrow bandgap perovskite films. Here, we report a surface reconstruction strategy utilizing a surface polishing agent, 1,4-butanediamine, together with a surface passivator, ethylenediammonium diiodide, to eliminate Sn-related defects and passivate organic cation and halide vacancy defects on the surface of Sn–Pb mixed perovskite films. Our strategy not only delivers high-quality Sn–Pb mixed perovskite films with a close-to-ideal stoichiometric ratio surface but also minimizes the non-radiative energy loss at the perovskite/electron transport layer interface. As a result, our Sn–Pb mixed perovskite solar cells with bandgaps of 1.32 and 1.25 eV realize power conversion efficiencies of 22.65% and 23.32%, respectively. Additionally, we further obtain a certified power conversion efficiency of 28.49% of two-junction all-perovskite tandem solar cells.

Critical review on the controllable growth and post-annealing on the heterojunction of the kesterite solar cells

Abstract Kesterite-structured solar cells have drawn significant attention due to their low-cost and environmental friendly composition. Recently, a remarkable certified power conversion efficiency (PCE) of 14.9% has been achieved, indicating a broader prospect for kesterite solar cells. However, this PCE is still far below the theoretical efficiency and the PCE of predecessor Cu(In,Ga)Se2 solar cells, which have been commercialized successfully. The relatively low device efficiency primarily originates from the unfavourable bulk and heterojunction of kesterite solar cell. Therefore, the achievement of high PCE in kesterite solar cells heavily relies on high-quality absorber layers and appropriate heterojunction contact. In this review, we first summarize the recent studies on the controllable growth of kesterite thin film. Based on different fabrication methods, various endeavors in revealing the reaction mechanism and manipulating the growth pathway of kesterite thin films have been introduced. Subsequently, studies related to the optimization of heterojunction by post-annealing process are also summarized. This simple and convenient approach can effectively enhance the heterojunction contact and promote the carrier transportation. Finally, this article discusses the future development strategy and perspectives towards achieving enhanced PCE in kesterite thin film solar cells

Enhanced Photodetection and Air Stability of Lead‐Free Tin Perovskite Photodiodes via Germanium Incorporation and Organic Cation‐Mediated Dimensionality Control

AbstractThis work presents the advancement of lead‐free tin perovskite photodiodes in terms of their photodetection and air stability by incorporating germanium (Ge) and ethylenediamine (EDA) to formamidinium tin iodide (FASnI3). EDA0.01FA0.98SnI3:Ge‐based photodiodes demonstrate a significantly improved specific detectivity (1.6 × 1012 Jones at −0.1 V), cut‐off frequency (6.6 × 105 Hz), response speed (0.53 µs), and signal‐to‐noise ratio (45 dB) compared with control devices. The superior performance is attributed to the stronger Ge─I bond, the passivation of Sn2+ and I– vacancies by smaller Ge2+ ions, the promotion of a fully 3D perovskite structure, the elevation of the conduction band energy level, and the formation of a protective GeO layer. Various film analyses, including X‐ray photoelectron spectroscopy, UV photoelectron spectroscopy, density functional theory, as well as device testing using time‐of‐flight secondary ion mass spectrometry and voltage‐dependent admittance, support and explain the mechanisms behind the enhancements. Ge‐ and EDA‐incorporated photodiodes exhibit excellent air stability, as evidenced by the time‐dependent ultraviolet visible spectra and the considerably high certified power conversion efficiency without encapsulation in air, demonstrating their potential for practical applications. The obtained photodetection performance is highest among the published lead‐free tin‐based perovskite photodetectors, presenting a monumental progress from the previous report of the same group.

Synchronized crystallization in tin-lead perovskite solar cells

Tin-lead halide perovskites with a bandgap near 1.2 electron-volt hold great promise for thin-film photovoltaics. However, the film quality of solution-processed Sn-Pb perovskites is compromised by the asynchronous crystallization behavior between Sn and Pb components, where the crystallization of Sn-based perovskites tends to occur faster than that of Pb. Here we show that the rapid crystallization of Sn is rooted in its stereochemically active lone pair, which impedes coordination between the metal ion and Lewis base ligands in the perovskite precursor. From this perspective, we introduce a noncovalent binding agent targeting the open metal site of coordinatively unsaturated Sn(II) solvates, thereby synchronizing crystallization kinetics and homogenizing Sn-Pb alloying. The resultant single-junction Sn-Pb perovskite solar cells achieve a certified power conversion efficiency of 24.13 per cent. The encapsulated device retains 90 per cent of the initial efficiency after 795 h of maximum power point operation under simulated one-sun illumination.

Advancements and Challenges in Wide‐Bandgap Perovskite Solar Cells: From Single Junction to Tandem Solar Cells

The exceptional optoelectronic performance and cost‐effectiveness of manufacturing have propelled organic–inorganic hybrid perovskite solar cells (PSCs) into the spotlight within the photovoltaic community. Currently, the single‐junction PSCs have achieved a certified power conversion efficiency surpassing 26%, edging closer to the illustrious Shockley–Queisser theoretical limit. To further enhance device performance, researchers are currently directing their attention toward the integration of wide‐bandgap (WBG) perovskites (Eg > 1.60 eV) as top subcells in conjunction with narrow‐bandgap materials, such as perovskite, crystalline silicon, and copper indium gallium selenium, to construct multijunction tandem devices that maximize solar spectral utilization and minimize thermal losses. However, WBG perovskites encounter challenges associated with suboptimal crystal quality, high defect density, and severe phase separation, leading to significant voltage losses and inferior performance. In this regard, extensive research has been conducted, yielding significant findings. This review article summarizes the advancements in composition engineering, additive engineering, and interface engineering of WBG PSCs. Furthermore, the applications of WBG PSCs in various tandem solar cells and their development are discussed. Finally, future prospects for the development of WBG PSCs are outlined.

Shallow-level defect passivation by 6H perovskite polytype for highly efficient and stable perovskite solar cells

The power conversion efficiency of perovskite solar cells continues to increase. However, defects in perovskite materials are detrimental to their carrier dynamics and structural stability, ultimately limiting the photovoltaic characteristics and stability of perovskite solar cells. Herein, we report that 6H polytype perovskite effectively engineers defects at the interface with cubic polytype FAPbI3, which facilitates radiative recombination and improves the stability of the polycrystalline film. We particularly show the detrimental effects of shallow-level defect that originates from the formation of the most dominant iodide vacancy (VI+) in FAPbI3. Furthermore, additional surface passivation on top of the hetero-polytypic perovskite film results in an ultra-long carrier lifetime exceeding 18 μs, affords power conversion efficiencies of 24.13% for perovskite solar cells, 21.92% (certified power conversion efficiency: 21.44%) for a module, and long-term stability. The hetero-polytypic perovskite configuration may be considered as close to the ideal polycrystalline structure in terms of charge carrier dynamics and stability.

Solvent‐Assisted Surface Modification Using Metallocene‐Based Molecules for High‐Efficiency Perovskite/Silicon Tandem Solar Cells

AbstractThe presence of a high density of defects at the perovskite/electron transport layer (ETL) interface results in significant nonradiative recombination losses, thus impeding the efficiency enhancement of perovskite/silicon tandem solar cells (TSCs). In this investigation, a metallocene‐based molecule, cobalt (III) dichlorophene hexafluorophosphate (CcPF6), is employed for perovskite surface passivation. To maximize its efficacy, the molecule is dissolved in a mixed solvent of acetonitrile and chlorobenzene, leading to the reconstruction of the perovskite surface and effective passivation of surface defects. This modification strategy substantially enhances the overall efficiency of perovskite/silicon tandem solar cells by mitigating the issue of low fill factor resulting from non‐uniform coating of the top perovskite layer on the textured silicon bottom cell. Leveraging a double‐sided textured silicon heterojunction (HJT) bottom cell, a certified power conversion efficiency (PCE) of 30.43% for a monolithic perovskite/silicon TSC (1.00 cm2) is achieved, featuring an open‐circuit voltage (Voc) of 1.93 V and a fill factor (FF) of 78.43%. After storage in the drying cabinet (5% humidity at 20 °C) for 1000 h, the device retains 94.27% of its initial performance.

Soft Lattice and Phase Stability of α‐FAPbI3

AbstractSince the certified power conversion efficiency (PCE) of perovskite solar cells (PSCs) has reached 26.1%, exactly equal to that of crystalline silicon solar cells, a strong demand for ensuring the long‐term stability of PSCs has arisen for commercialization. The intrinsic stability of the perovskite layer must be guaranteed as a top priority to ensure the whole device's stability. Recently, the state‐of‐the‐art PSCs, performing a high PCE, employ α‐FAPbI3 (FA = formamidinium) for the perovskite layer in spite of its metastable tendency to spontaneously transform into its photoinactive polymorph at PSC operating temperature. In this review paper, the intrinsic structural stability of α‐FAPbI3 soft lattice is understood from the thermodynamic point of view, with key parameters to restrain the undesirable phase transition. Besides, reported experimental results are closely examined to find fundamental origins, derive the enhanced phase stability in each experiment, and understand their role in maintaining the lattice structure from the collective perspective.

Stress-induced phase stability and optoelectronic property changes in cesium lead halide perovskites

Over the past decade, the certified power conversion efficiency of perovskite solar cells (PSCs) has increased to 26.1%. However, phase instability originating from lattice strains, has limited their commercialization. Strains will inevitably be generated during the PSC fabrication and service process due to the “soft lattice” nature of halide perovskites. In particular, flexible PSCs are subjected to not only mechanical tensile and compressive loads, but also suffer from thermal stresses. In this study, strain-induced changes in the phase stability and the corresponding optoelectronic properties of CsPbI3−xBrx (CsPbI3, CsPbBr3, and CsPbI2Br) systems under tensile and compressive stresses were investigated using first-principles calculations. The results showed that compressive stresses reduce the bandgap value and increase the light absorption coefficient; thus, the optoelectronic performance is improved, whereas the light absorption coefficient decreases regardless of how the bandgap changes under tensile stresses. Moreover, under the same stress, the tensile strain value was twice that of the compressive strain, and the critical value of the transition from the cubic to tetragonal phase was lower, indicating that phase stability was worse under tensile stresses. Therefore, during the fabrication of PSCs, the tensile stress state should be adjusted to the compressive stress state, which is favorable for enhancing PSCs photovoltaic performance and phase stability. The results not only provide direct evidence of tensile and compressive strains influencing the phase stability and optoelectronic property changes in halide perovskites, but also highlight lattice-strain tailoring for the composition design, process optimization, and interface engineering of efficient and stable PSCs.

Smart Materials to Empowering Perovskite Solar Cells with Self‐Healing Capability

Inspired by nature, intelligent self‐healing materials have recently been exploited also in the field of photovoltaics to mimic natural systems achieving self‐repairing. The past decade has witnessed perovskite solar cells (PSCs) skyrocketing to a certified power conversion efficiency of 26.1%. However, their intrinsic instability, when exposing to moisture, high temperature, and continuous illumination, hampers their commercial development for a long‐term use in ambient operating conditions. Therefore, the use of smart self‐healing materials, based on self‐assembling properties and dynamic interactions, empowers PSCs with self‐recovery abilities to reinforce their pivotal role as efficient photovoltaic devices and encourage their exploitation in the market. Herein, the current progress in self‐healing perovskite materials with a special focus on self‐recovery after moisture exposure or mechanical damage with the aim to provide a valuable insight for research on this topic to accelerate the PSC commercialization process is highlighted.

Unraveling the Molecular Size Effect on Surface Engineering of Perovskite Solar Cells.

Surface engineering in perovskite solar cells, especially for the upper surface of perovskite, is widely studied. However, most of these studies have primarily focused on the interaction between additive functional groups and perovskite point defects, neglecting the influence of other parts of additive molecules. Herein, additives with -NH3 + functional group are introduced at the perovskite surface to suppress surface defects. The chain lengths of these additives vary to conduct a detailed investigation into the impact of molecular size. The results indicate that the propane-1,3-diamine dihydroiodide (PDAI2 ), which possesses the most suitable size, exhibited obvious optimization effects. Whereas the molecules, methylenediamine dihydroiodide (MDAI2 ) and pentane-1,5-diamine dihydroiodide (PentDAI2 ) with unsuitable size, lead to a deterioration in device performance. The PDAI2 -treated devices achieved a certified power conversion efficiency (PCE) of 25.81% and the unencapsulated devices retained over 80% of their initial PCE after 600h AM1.5 illumination.

Homogeneous crystallization and buried interface passivation for perovskite tandem solar modules.

Scalable fabrication of all-perovskite tandem solar cells is challenging because the narrow-bandgap subcells made of mixed lead-tin (Pb-Sn) perovskite films suffer from nonuniform crystallization and inferior buried perovskite interfaces. We used a dopant from Good's list of biochemical buffers, aminoacetamide hydrochloride, to homogenize perovskite crystallization and used it to extend the processing window for blade-coating Pb-Sn perovskite films and to selectively passivate defects at the buried perovskite interface. The resulting all-perovskite tandem solar module exhibited a certified power conversion efficiency of 24.5% with an aperture area of 20.25 square centimeters.

A Universal Perovskite/C60 Interface Modification via Atomic Layer Deposited Aluminum Oxide for Perovskite Solar Cells and Perovskite-Silicon Tandems.

The primary performance limitation in inverted perovskite-based solar cells is the interface between the fullerene-based electron transport layers and the perovskite. Atomic layer deposited thin aluminum oxide (AlOX) interlayers that reduce nonradiative recombination at the perovskite/C60 interface are developed, resulting in >60 millivolts improvement in open-circuit voltage and 1% absolute improvement in power conversion efficiency. Surface-sensitive characterizations indicate the presence of a thin, conformally deposited AlOx layer, functioning as a passivating contact. These interlayers work universally using different lead-halide-based absorbers with different compositions where the 1.55 electron volts bandgap single junction devices reach >23% power conversion efficiency. A reduction of metallic Pb0 is found and the compact layer prevents in- and egress of volatile species, synergistically improving the stability. AlOX-modified wide-bandgap perovskite absorbers as a top cell in a monolithic perovskite-silicon tandem enable a certified power conversion efficiency of 29.9% and open-circuit voltages above 1.92 volts for 1.17 square centimeters device area.

Oriented Molecular Bridge Constructs Homogeneous Buried Interface for Perovskite Solar Cells with Efficiency Over 25.3.

Buried interface optimization matters the efficiency improvement of planar perovskite solar cells (PSCs), and the molecular bridge is reported to be an effective approach. Herein, a molecular bridge is constructed at buried interface using 4-chloro-3-sulfamoylbenzoic acid (CSBA), and its preferred arrangement is systematically investigated. It is elucidated that the CSBA molecular is prone to be orientationally absorbed on TiO2 surface through COOH-Ti, and then connect with perovskite through S═O-Pb, resulting in a feasible oriented molecular bridge. Contributing to the passivated interfacial defects, optimized interfacial energy level, and released perovskite tensile stress, resulting from the oriented CSBA molecular bridge, the PSCs with an active area of 0.08 cm2 achieve a certified power conversion efficiency (PCE) of 25.32%, the highest among the TiO2-based planar PSCs. Encouragingly, the PSCs with an active area of 1 cm2 achieve a champion PCE of 24.20%, significantly promoting the efficiency progress of large-area PSCs. In addition, the PSCs with oriented CSBA molecular bridge possess enhanced stability, the unencapsulated PSCs can maintain ≈91% and ≈85% of their initial PCE after 3000 h aging under ambient condition and 1200 h aging under exposure to UV irradiation.

Sublimed C60 for efficient and repeatable perovskite-based solar cells

Thermally evaporated C60 is a near-ubiquitous electron transport layer in state-of-the-art p–i–n perovskite-based solar cells. As perovskite photovoltaic technologies are moving toward industrialization, batch-to-batch reproducibility of device performances becomes crucial. Here, we show that commercial as-received (99.75% pure) C60 source materials may coalesce during repeated thermal evaporation processes, jeopardizing such reproducibility. We find that the coalescence is due to oxygen present in the initial source powder and leads to the formation of deep states within the perovskite bandgap, resulting in a systematic decrease in solar cell performance. However, further purification (through sublimation) of the C60 to 99.95% before evaporation is found to hinder coalescence, with the associated solar cell performances being fully reproducible after repeated processing. We verify the universality of this behavior on perovskite/silicon tandem solar cells by demonstrating their open-circuit voltages and fill factors to remain at 1950 mV and 81% respectively, over eight repeated processes using the same sublimed C60 source material. Notably, one of these cells achieved a certified power conversion efficiency of 30.9%. These findings provide insights crucial for the advancement of perovskite photovoltaic technologies towards scaled production with high process yield.

Performance of Hydride Vapor Phase Epitaxy‐Grown GaInP Photovoltaics with Double‐Sided Al‐Containing Passivation Layers Under Air Mass 1.5 Global Solar Irradiation and Low‐Intensity Indoor Light Irradiation

High‐performance III–V photovoltaic devices have the potential for various applications; however, their high production cost represents a challenge for market expansion. Hydride vapor phase epitaxy (HVPE) is a fabrication technology that can reduce the epitaxial growth cost of III–V compound semiconductors. This study demonstrates the performances of HVPE‐grown GaInP photovoltaic devices for solar and indoor photovoltaic applications. Herein, HVPE‐grown GaInP photovoltaic devices with AlInP frontside and AlGaInP backside passivation layers are fabricated for the first time. The developed GaInP photovoltaic device measured under air mass 1.5 global solar spectrum illumination achieves an independently certified power conversion efficiency of 17.3%, which is a new record efficiency among HVPE‐grown GaInP single‐junction solar cells. Furthermore, the GaInP photovoltaic device grown using HVPE exhibits a high power conversion efficiency (34.7–37.1%) under an illumination of 500–2000 lux, respectively, emitted by a white light‐emitting diode. These results demonstrate that HVPE‐grown GaInP photovoltaic devices can be used in low‐intensity indoor light energy harvesting systems.