Efficient Inverted Perovskite Photovoltaics Through Surface State Manipulation.

Inverted perovskite solar cells (PSCs) are considered as the most promising avenue for the commercialization of PSCs due to their potential inherent stability. However, suboptimal interface contacts between electron transport layer (ETL) (such as C60 ) and the perovskite absorbing layer within inverted PSCs always result in reduced efficiency and poor stability. Herein, a surface state manipulation strategy has been developed by employing a highly electronegative 4-fluorophenethylamine hydrochloride (p-F-PEACl) to effectively address the issue of poor interface contacts in the inverted PSCs. The p-F-PEACl demonstrates a robust interaction with perovskite film through bonding of amino group and Cl- with I- and Pb2+ ions in the perovskite, respectively. As such, the surface defects of perovskite film can be significantly reduced, leading to suppressed non-radiative recombination. Moreover, p-F-PEACl also plays a dual role in enhancing the surface potential and improving energy-level alignment at the interfaces between the perovskite and C60 carrier transport layer, which directly contributes to efficient charge extraction. Finally, the open-circuit voltage (Voc ) of devices increases from 1.104 V to 1.157 V, leading to an overall efficiency improvement from 22.34% to 24.78%. Furthermore, the p-F-PEACl-treated PSCs also display excellent stability.

Suppressing Halide Segregation via Pyridine-Derivative Isomers Enables Efficient 1.68 eV Bandgap Perovskite Solar Cells.

Light-induced phase segregation is one of the main issues restricting the efficiency and stability of wide-bandgap perovskite solar cells (WBG PSCs). Small organic molecules with abundant functional groups can passivate various defects, and therefore suppress the ionic migration channels for phase segregation. Herein, a series of pyridine-derivative isomers containing amino and carboxyl are applied to modify the perovskite surface. The amino, carboxyl, and N-terminal of pyridine in all of these molecules can interact with undercoordinated Pb2+ through coordination bonds and suppress halide ions migration via hydrogen bonding. Among them, the 5-amino-3-pyridine carboxyl acid (APA-3) treated devices win the champion performance, enabling an efficiency of 22.35% (certified 22.17%) using the 1.68 eV perovskite, which represents one of the highest values for WBG-PSCs. This is believed to be due to the more symmetric spatial distribution of the three functional groups of APA-3, which provides a better passivation effect independent of the molecular arrangement orientation. Therefore, the APA-3 passivated perovskite shows the slightest halide segregation, the lowest defect density, and the least nonradiative recombination. Moreover, the APA-3 passivated device retains 90% of the initial efficiency after 985 h of operation at the maximum power point, representing the robust durability of WBG-PSCs under working conditions.

Modulation of Charge Transport from Two-Dimensional Perovskites to Industrial Charge Transport Layers by the Organic Spacer-Dependent Exciton-Phonon Interactions.

In the past decade, two-dimensional (2D) perovskite surface treatment has emerged as a promising strategy to improve the performance of three-dimensional (3D) perovskite solar cells (PSCs). However, systematic studies on the impact of organic spacers of 2D perovskites on charge transport in 2D/3D PSCs are still lacking. Here, using 2D perovskite film/C60 heterostructures with different organic spacers [butylamine (BA), phenylethylamine (PEA), and 3-fluorophenethylamine (m-F-PEA)], we systematically investigated the carrier diffusion and interfacial transfer process. Using a 2D perovskite film with a thickness of ∼7 nm, we observed subtle differences in electron transfer time between 2D perovskites and C60 layers, which can be attributed to limited thickness and similar electron coupling strength. However, with the thickness of 2D perovskite increasing, electron transfer efficiency in the (BA)2PbI4/C60 heterostructure exhibits the most rapid decrease due to poor carrier diffusion of (BA)2PbI4 caused by stronger exciton-phonon interactions compared to (PEA)2PbI4 and (m-F-PEA)2PbI4 in thickness-dependent charge transfer research. Meanwhile, the fill factor of 2D/3D PSC treated with BAI exhibits the most rapid decrease compared to PEAI- and m-F-PEAI-treated 2D/3D PSCs with the concentration increase of passivators. This study indicates that it is easier to enhance open-circuit voltages and minimize the decrease of fill factor by increasing the concentration of passivators in 2D/3D PSCs when using passivators with a rigid molecular structure.

Inhibited Crack Development by Compressive Strain in Perovskite Solar Cells with Improved Mechanical Stability.

Metal halide perovskites are promising as next-generation photovoltaic materials, but stability issues are still a huge obstacle to their commercialization. Here, the formation and evolution of cracks in perovskite films during thermal cycling, which affect their mechanical stability, are investigated. Compressive strain is employed to suppress cracks and delamination by in situ formed polymers with low elastic modulus during crystal growth. The resultant devices pass the thermal-cycling qualification (IEC61215:2016), retaining 95% of the initial power conversion efficiency (PCE) and compressive strain after 230 cycles. Meanwhile, the p-i-n devices deliver PCEs of 23.91% (0.0805 cm2 ) and 23.27% (1 cm2 ). The findings shed light on strain engineering with respect to their evolution, which enables mechanically stable perovskite solar cells.

Strain Modulation for Light-Stable n-i-p Perovskite/Silicon Tandem Solar Cells.

Perovskite/silicon tandem solar cells are promising to penetrate photovoltaic market. However, the wide-bandgap perovskite absorbers used in top-cell often suffer severe phase segregation under illumination, which restricts the operation lifetime of tandem solar cells. Here, a strain modulation strategy to fabricate light-stable perovskite/silicon tandem solar cells is reported. By employing adenosine triphosphate, the residual tensile strain in the wide-bandgap perovskite absorber is successfully converted to compressive strain, which mitigates light-induced ion migration and phase segregation. Based on the wide-bandgap perovskite with compressive strain, single-junction solar cells with the n-i-p layout yield a power conversion efficiency (PCE) of 20.53% with the smallest voltage deficits of 440 mV. These cells also maintain 83.60% of initial PCE after 2500 h operation at the maximum power point. Finally, these top cells are integrated with silicon bottom cells in a monolithic tandem device, which achieves a PCE of 26.95% and improved light stability at open-circuit.

Synergistic Effects of Eu-MOF on Perovskite Solar Cells with Improved Stability.

Enhancing device lifetime is one of the essential challenges in perovskite solar cells. The ultrathin Eu-MOF layer is introduced at the interface between the electron-transport layer and the perovskite absorber to improve the device stability. Both Eu ions and organic ligands in the MOF can reduce the defect concentration and improve carrier transport. Moreover, due to the Förster resonance energy transfer effect, Eu-MOF in perovskite films can improve light utilization and reduce the decomposition under ultraviolet light. Meanwhile, Eu-MOF also turns tensile strain to compressive strain in the perovskite films. As a result, the corresponding devices achieve a champion power conversion efficiency (PCE) of 22.16%. In addition, the devices retain 96% of their original PCE after 2000 h under the relative humidity of 30% and 91% of their original PCE after 1200 h after continuous 85 °C aging condition in N2 .

Interfacial Residual Stress Relaxation in Perovskite Solar Cells with Improved Stability.

To improve the photovoltaic performance (both efficiency and stability) in hybrid organic-inorganic halide perovskite solar cells, perovskite lattice distortion is investigated with regards to residual stress (and strain) in the polycrystalline thin films. It is revealed that residual stress is concentrated at the surface of the as-prepared film, and an efficient method is further developed to release this interfacial stress by A site cation alloying. This results in lattice reconstruction at the surface of polycrystalline thin films, which in turn results in low elastic modulus. Thus, a "bone-joint" configuration is constructed within the interface between the absorber and the carrier transport layer, which improves device performance substantially. The resultant photovoltaic devices exhibit an efficiency of 21.48% with good humidity stability and improved resistance against thermal cycling.

Grain-Boundary "Patches" by In Situ Conversion to Enhance Perovskite Solar Cells Stability.

The power conversion efficiency of organic-inorganic hybrid perovskite solar cells has increased rapidly, but the device stability remains a big challenge. Previous studies show the grain boundary (GB) can facilitate ion migration and initiate device degradation. Herein, methimazole (MMI) is employed for the first time to construct a surface "patch" by in situ converting residual PbI2 at GBs. The resultant MMI-PbI2 complex can effectively suppress ion migration and inhibit diffusion of the metal electrodes. The origin of the surface "patch" effect and their working mechanisms are investigated experimentally and theoretically at the microscopic level. It hence demonstrates a simple and effective method to prolong the device stability in the context of GB engineering, which could be extensively applied to perovskite-based optoelectronics.