Abstract Because of their better chemical stability and fascinating anisotropic characteristics, Dion–Jacobson (DJ)-layered halide perovskites, which owe crystallographic two-dimensional structures, have fascinated growing attention for solar devices. DJ-layered halide perovskites have special structural and photoelectronic features that allow the van der Waals gap to be eliminated or reduced. DJ-layered halide perovskites have improved photophysical characteristics, resulting in improved photovoltaic performance. Nevertheless, owing to the nature of the solution procedure and the fast crystal development of DJ perovskite thin layers, the precursor compositions and processing circumstances can cause a variety of defects to occur. The application of additives can impact DJ perovskite crystallization and film generation, trap passivation in the bulk and/or at the surface, interface structure, and energetic tuning. This study discusses recent developments in additive engineering for DJ multilayer halide perovskite film production. Several additive-assisted bulk and interface optimization methodologies are summarized. Lastly, an overview of research developments in additive engineering in the production of DJ-layered halide perovskite solar cells is offered. 

/pdf/additive-engineering-for-stable-and-efficient-dion-jacobson-2c4w2rn7.pdf

Additive Engineering for Stable and Efficient Dion–Jacobson Phase Perovskite Solar Cells

Green-antisolvent-induced homogeneous phase distribution for efficient and stable MA-free 2D perovskite solar cells

Benefiting from the advantages of a high absorption coefficient, a long charge diffusion length, excellent carrier mobility, and a tunable bandgap, three-dimensional (3D) metal halide perovskites exhibit great potential for application in solar cells. However, 3D perovskite solar cells (PSCs) often suffer from poor long-term stability against moisture, heat, and light. To address this issue, reducing the dimension of perovskite and forming two-dimensional (2D) perovskites can be effective in slowing down the oxidation of the perovskite film and significantly improving device stability. In this study, 2D PSCs were designed with glass/FTO/TiO2/Dion–Jacobson (DJ) perovskite/NiOx/Au structures, based on the solar cell simulation software SCAPS. The absorption layers employed in the study included PeDAMA2Pb3I10, PeDAMA3Pb4I13, PeDAMA4Pb5I16, and PeDAMA5Pb6I19. The influence of the conduction band offset (CBO) variation in the range of −0.5 to 0.5 eV on cell performance was explored through a numerical simulation. The simulation results indicate that the open-circuit voltage and fill factor continue to increase, whereas the short-circuit current density remains almost unchanged when the CBO increases from −0.5 eV to 0 eV. The devices exhibit better performance when the value of the CBO is positive and within a small range. For DJ PSCs, controlling the CBO within 0.1–0.4 eV is conducive to better cell performance. 

Numerical Analysis on the Effect of the Conduction Band Offset in Dion–Jacobson Perovskite Solar Cells

Abstract All‐perovskite tandem solar cells are regarded as the next generation of devices capable of enhancing the solar energy utilization rate. Unlike single‐junction perovskite solar cells (PSCs), the efficacy of tandem cells is contingent upon the performance of both the top and bottom cells. In this study, we employed a simultaneous co‐modification strategy to incorporate phenylethylammonium iodide (PEAI) at both the top and bottom interfaces of the perovskite film, aiming to boost the top cell's performance. Both experimental and theoretical findings indicate that PEAI not only elevates the perovskite film quality through chemical interactions but also mitigates nonradiative recombination within the device. Consequently, the efficiency of the wide‐bandgap (1.77 eV) PSCs based on nickel oxide (NiO x ) attained a level of 16.5%. Simultaneously, the all‐perovskite tandem solar cells achieved an efficiency of 26.81% and demonstrated superior stability. 

Double side passivation of phenylethyl ammonium iodide for all perovskite tandem solar cell with efficiency of 26.8%

With the advance of nanotechnology, the past couple of years have witnessed the fast development of quasi two-dimensional (2D) halide perovskites, which exhibit outstanding long-term stability against moisture and heat, compared with their three-dimensional (3D) counterparts. As one of the most common structures in 2D halide perovskites, quasi-2D Dion-Jacobson (DJ) perovskites show multiple-quantum-well structures with n layers of [BX6]4- octahedral inorganic sheets sandwiched by two layers of diammonium spacers, thus exhibiting superior structural stability due to the elimination of van der Waals gaps. Thanks to the achievement of high power conversion efficiency accompanied by impressive stability, quasi-2D DJ perovskite solar cells (PSCs) have recently drawn extensive attention in the field. This review first introduces the fundamental understanding of quasi-2D DJ halide perovskites, including their superior stability, high exciton binding energy, and compositional flexibility and tunable properties. We then summarize detailed strategies to prepare high-quality quasi-2D DJ perovskites for PSCs, encompassing compositional engineering, solvent engineering, additive addition, and annealing processes. Moreover, the surface/interface modification and 2D-3D hybrid perovskite heterojunction are also discussed, for providing strategies to optimize the fabrication of quasi-2D DJ PSCs. Lastly, current challenges and perspectives toward the future development of quasi-2D DJ perovskites for photovoltaics are outlined.

The rise of quasi-2D Dion-Jacobson perovskites for photovoltaics.

Surface defects-mediated nonradiative recombination plays a critical role in the performance and stability of perovskite solar cells (PSCs) and surface post-treatment is widely used for efficient PSCs. However, the commonly used surface passivation strategies are one-off and the passivation defect ability is limited, which can only solve part of the defects in the topmost surface area. Here, a secondary anti-solvent strategy is proposed to further reduce surface defects based on conventional surface passivation for the first time. Based on this, the crystallization quality of 2D Dion-Jacobson perovskite is enhanced and the surface defects density is further reduced by nearly two orders. In addition, a gradient structure of perovskite with n = 2 phases located at the top of the film and 3D-like phases located at the bottom of the film can also be obtained. The modulated perovskite film boosts the efficiency of 2D perovskites (n = 5) up to 19.55%. This strategy is also very useful in other anti-solvent processed perovskite dipping systems, which paves a promising avenue for minimizing surface defects toward highly efficient perovskite devices.

Secondary Anti-Solvent Treatment for Efficient 2D Dion-Jacobson Perovskite Solar Cells.

Wide-Bandgap Perovskite and Perovskite/Silicon Tandem Solar Cells through Strong Hydrogen Bonding Interaction

Wide‐bandgap (WBG) perovskite solar cells (PSCs) can be combined with other narrow‐bandgap (NBG) cells to form tandem solar cells (TSCs), which have excellent commercialization prospects. However, the component of WBG perovskite is complex, and the crystallization process is difficult to control. Various bulk and surface defects in polycrystalline films lead to severe non‐radiative recombination of photogenerated carriers, resulting in severe open circuit voltage (VOC) loss in WBG PSCs. Here, we introduce a zwitterionic additive to alleviate the VOC deficit. The sulfinyl group (‐S=O) in formamidine sulfinic acid (FSA) has a robust interaction with the Pb2+, which retards the crystallization and improves the crystal quality in perovskite films. Furthermore, FSA has negatively charged centers (‐SO2
‐) and positively charged centers (‐C(NH2)2
+), which can passivate the halogen and cation vacancies, respectively. The improved crystalline quality and passivated defects reduce the capture of carriers by defects and facilitate higher VOC. With this strategy, the 1.68 eV bandgap PSCs achieve a champion efficiency of 22.06% and a high VOC of 1.25 V (VOC loss=0.43 V). Moreover, the 2‐terminal (2‐T) perovskite/silicon TSCs are fabricated with an extraordinary power conversion efficiency (PCE) of 28.81%.This article is protected by copyright. All rights reserved.

Zwitterion Reduces Open‐Circuit Voltage Loss in Wide‐Bandgap Perovskite Solar Cells with 22% Efficiency and Its Application in Tandem Devices

In order to fabricate nickel oxide (NiOX)-based perovskite solar cells with high efficiency and stability, adverse reaction and lattice mismatch are two urgent problems to be overcome. In this respect, interface engineering was carried out by multi-layer passivation NiOX HTLs (NiOX/2PACz/Poly-TPD/PEAI) to provide optimized interface contact between NiOX and perovskite, ameliorate band alignment, and saturate the defect states. Application of 2PACz avoids direct contact of the hydroxyl groups (which causes degeneration of a device), improves conductivity, and reduces interfacial defects. The poly-TPD modification can provide an appropriate band alignment at the interface of NiOX/perovskite. PEAI was used to modify the Poly-TPD surface, and its −NH3 group can passivate unbonded Pb ions of perovskite. Thus, compared with previously reported single-function passivation materials, the multilayer passivation proposed in this paper integrates multiple functions. As a result, the NiOX/2PACz/Poly-TPD/PEAI-based wide bandgap PSCs obtain a champion power conversion efficiency (PCE) of 20.21% and maintain over 95% of their initial PCE values after storage in a nitrogen atmosphere for 1000 h. This finding provides a practical approach for fabricating high-performance regular PSCs with NiOX-based HTLs and supports their commercialization.

https://pubs.aip.org/aip/apl/article-pdf/doi/10.1063/5.0146114/17925551/223903_1_5.0146114.pdf

Triple hole transporting and passivation layers for efficient NiOX-based wide-bandgap perovskite solar cells

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Papers

Secondary Anti-Solvent Treatment for Efficient 2D Dion-Jacobson Perovskite Solar Cells.

Wide-Bandgap Perovskite and Perovskite/Silicon Tandem Solar Cells through Strong Hydrogen Bonding Interaction

Zwitterion Reduces Open‐Circuit Voltage Loss in Wide‐Bandgap Perovskite Solar Cells with 22% Efficiency and Its Application in Tandem Devices

Triple hole transporting and passivation layers for efficient NiOX-based wide-bandgap perovskite solar cells