High‐performance tin‐lead perovskite solar cells (PSCs) are needed for all‐perovskite‐tandem solar cells. However, iodide related fast photodegradation severely limits the operational stability of Sn‐Pb perovskites despite the demonstrated high efficiency and thermal stability. Herein, this work employs an alkylammonium pseudo‐halogen additive to enhance the power conversion efficiency (PCE) and photostability of methylammonium (MA)‐free, Sn‐Pb PSCs. Density functional theory (DFT) calculations reveal that the pseudo‐halogen tetrafluoroborate (BF4−) has strong binding capacity with metal ions (Sn2+/Pb2+) in the Sn‐Pb perovskite lattice, which lowers iodine vacancy formation. Upon combining BF4−with an octylammonium (OA+) cation, the PCE of the device with a built‐in light‐scattering layer is boosted to 23.7%, which represents a new record for Sn‐Pb PSCs. The improved efficiency benefits from the suppressed defect density. Under continuous 1 sun illumination, the OABF4embodied PSCs show slower generation of interstitial iodides and iodine, which greatly improves the device photostability under open‐circuit condition. Moreover, the device based on OABF4retains 88% of the initial PCE for 1000 h under the maximum‐power‐point tracking (MPPT) without cooling.
- Award ID(s):
- 1900510
- NSF-PAR ID:
- 10337644
- Date Published:
- Journal Name:
- Journal of Materials Chemistry A
- Volume:
- 10
- Issue:
- 1
- ISSN:
- 2050-7488
- Page Range / eLocation ID:
- 234 to 244
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Enhancing Photostability of Sn‐Pb Perovskite Solar Cells by an Alkylammonium Pseudo‐Halogen Additivemore » « less
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Development of high‐performance wide‐bandgap perovskites is a key component to enable tandem solar cells with either a silicon or low‐bandgap perovskites. However, the presence of defects in the Br‐rich wide‐bandgap perovskites, especially in the grain boundaries (GBs) has been particularly challenging and limits its performance. Herein, to accomplish the passivation of these defects, a combination of cation management with rubidium (Rb) introduction into the triple cation combination of cesium/formamidinium/methylammonium (CsFAMA) is exercised. Passivation is further enhanced by secondary growth (SG) using guanidinium iodide. In‐depth assessments of GB defect passivation are performed using Kelvin probe force microscopy (KPFM) and nanoscale charge‐carrier dynamics mappings provide insightful details on the presence of GBs defects and their suppression by the cation management and SG techniques. Reduction of unreacted PbX2to realize a highly crystalline perovskite surface is achieved after incorporating Rb and SG treatment. As a result, a champion cell for 1.78 eV (FA0.79MA0.16Cs0.05)0.95Rb0.05Pb(I0.6Br0.4)3wide‐bandgap perovskite with an efficiency of 17.71% along with enhancement in all photovoltaic parameters is achieved. This study introduces a new way to analyze GB defects and reveals the consequence of defect passivation on charge‐carrier dynamics for realizing efficient perovskites.
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null (Ed.)The past decade has witnessed tremendous advances in synthesis of metal halide perovskites and their use for a rich variety of optoelectronics applications. Metal halide perovskite has the general formula ABX 3 , where A is a monovalent cation (which can be either organic ( e.g. , CH 3 NH 3 + (MA), CH(NH 2 ) 2 + (FA)) or inorganic ( e.g. , Cs + )), B is a divalent metal cation (usually Pb 2+ ), and X is a halogen anion (Cl − , Br − , I − ). Particularly, the photoluminescence (PL) properties of metal halide perovskites have garnered much attention due to the recent rapid development of perovskite nanocrystals. The introduction of capping ligands enables the synthesis of colloidal perovskite nanocrystals which offer new insight into dimension-dependent physical properties compared to their bulk counterparts. It is notable that doping and ion substitution represent effective strategies for tailoring the optoelectronic properties ( e.g. , absorption band gap, PL emission, and quantum yield (QY)) and stabilities of perovskite nanocrystals. The doping and ion substitution processes can be performed during or after the synthesis of colloidal nanocrystals by incorporating new A′, B′, or X′ site ions into the A, B, or X sites of ABX 3 perovskites. Interestingly, both isovalent and heterovalent doping and ion substitution can be conducted on colloidal perovskite nanocrystals. In this review, the general background of perovskite nanocrystals synthesis is first introduced. The effects of A-site, B-site, and X-site ionic doping and substitution on the optoelectronic properties and stabilities of colloidal metal halide perovskite nanocrystals are then detailed. Finally, possible applications and future research directions of doped and ion-substituted colloidal perovskite nanocrystals are also discussed.more » « less
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Grain boundaries (GBs) in perovskite solar cells and optoelectronic devices are widely regarded as detrimental defects that accelerate charge and energy losses through nonradiative carrier trapping and recombination, but the mechanism is still under debate owing to the diversity of GB configurations and behaviors. We combine ab initio electronic structure and machine learning force field to investigate evolution of the geometric and electronic structure of a CsPbBr 3 GB on a nanosecond timescale, which is comparable with the carrier recombination time. We demonstrate that the GB slides spontaneously within a few picoseconds increasing the band gap. Subsequent structural oscillations dynamically produce midgap trap states through Pb–Pb interactions across the GB. After several hundred picoseconds, structural distortions start to occur, increasing the occurrence of deep midgap states. We identify a distinct correlation of the average Pb–Pb distance and fluctuations in the ion coordination numbers with the appearance of the midgap states. Suppressing GB distortions through annealing and breaking up Pb–Pb dimers by passivation can efficiently alleviate the detrimental effects of GBs in perovskites. The study provides new insights into passivation of the detrimental GB defects, and demonstrates that structural and charge carrier dynamics in perovskites are intimately coupled.more » « less
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Abstract In recent years, hybrid perovskite solar cells (HPSCs) have received considerable research attention due to their impressive photovoltaic performance and low‐temperature solution processing capability. However, there remain challenges related to defect passivation and enhancing the charge carrier dynamics of the perovskites, to further increase the power conversion efficiency of HPSCs. In this work, the use of a novel material, phenylhydrazinium iodide (PHAI), as an additive in MAPbI3perovskite for defect minimization and enhancement of the charge carrier dynamics of inverted HPSCs is reported. Incorporation of the PHAI in perovskite precursor solution facilitates controlled crystallization, higher carrier lifetime, as well as less recombination. In addition, PHAI additive treated HPSCs exhibit lower density of filled trap states (1010cm−2) in perovskite grain boundaries, higher charge carrier mobility (≈11 × 10−4cm2V−1s), and enhanced power conversion efficiency (≈18%) that corresponds to a ≈20% improvement in comparison to the pristine devices.
- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1039/d1ta09027e
