Efficient and stable pure α-phase FAPbI3 perovskite solar cells with a dual engineering strategy: Additive and dimensional engineering approaches

Solution‐processed 2D perovskite films generally contain mixed quantum wells (QWs) with multiple well width distribution, which seriously weakens the charge transfer. To achieve regulation of the QW width, strategies to optimize the crystallization dynamics of 2D perovskite films are urgently needed. In this review, systematic summary on QW distribution and guidelines for 2D perovskite phase regulation is provided, aiming to establish a general manual for preparing efficient 2D perovskite solar cells (PSCs). The factors affecting the distribution of multiple‐QWs in 2D perovskite films, including component engineering, additive engineering, process optimization, are first generalized. Then an extensive review of these factors that are widely used to reconstruct 2D perovskite crystallization process is conducted. Leveraging these insights, the effect of QWs distributions on 2D PSCs properties is also summarized. Similarly, considering the crystallization kinetics and device performance, the QWs width control of 2D perovskite films from the aspects of ligand engineering, precursor design, and fabrication optimization, is rationalized. Finally, an outlook on how to realize ordered QWs distribution in perovskite films for efficient 2D PSCs is proposed.

Regulation of Quantum Wells Width Distribution in 2D Perovskite Films for Photovoltaic Application

Despite their multifaceted advantages, inverted perovskite solar cells (PSCs) still suffer from lower power conversion efficiencies (PCEs) than their regular counterparts, which is largely due to recombination energy losses (Eloss) that arise from the chemical, physical, and energy level mismatches, especially at the interfaces between perovskites and fullerene electron transport layers (ETLs). To address this problem, we herein introduce an aminium iodide derivative of a buckybowl (aminocorannulene) that is molecularly layered at the perovskite-ETL interface. Strikingly, besides passivating the PbI2-rich perovskite surface, the aminocorannulene enforces a vertical dipole and enhances the surface n-type character that is more compatible with the ETL, thus boosting the electron extraction and transport dynamics and suppressing interfacial Eloss. As a result, the champion PSC achieves an excellent PCE of over 22%, which is superior compared to that of the control device (∼20%). Furthermore, the device stability is significantly enhanced, owing to a lock-and-key-like grip on the mobile iodides by the buckybowls and the resultant increase of the interfacial ion-migration barrier. This work highlights the potential of buckybowls for the multifunctional surface engineering of perovskite toward high-performance and stable PSCs.

Surface Re-Engineering of Perovskites with Buckybowls to Boost the Inverted-Type Photovoltaics.

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Manipulate energy transport via fluorinated spacers towards record-efficiency 2D Dion-Jacobson CsPbI3 solar cells.

Heterostructures involving two-dimensional/three-dimensional (2D/3D) perovskites have recently attracted increased attention due to their ability to combine the high photovoltaic performance of 3D perovskites with the increased stability of 2D perovskites. Here we report ammonium thiocyanate (NH4SCN) passivated 3D methylammonium lead triiodide (MAPbI3) perovskite active layer and deposition of 2D perovskite capping layer using xylylene diammonium iodide (XDAI) organic cation. The 2D/3D perovskite heterojunction formation is probed by using FESEM and UPS spectroscopy. The NH4SCN passivated MAPbI3 perovskite has shown 19.6% PCE compared to the 17.18% PCE of pristine MAPbI3 perovskite solar cells (PSCs). Finally, the champion 2D/3D perovskite heterojunction based solar cells have achieved the remarkable PCE of 20.74%. The increased PCE in 2D/3D PSCs is mainly attributed to the reduced defect density and suppressed nonradiative recombination losses. Moreover, the hydrophobic 2D capping layer endows the 2D/3D heterojunction perovskites with exceptional moisture, thermal and UV stability, highlighting the promise of highly stable and efficient 2D/3D PSCs.

Highly Efficient and Stable 2D Dion Jacobson/3D Perovskite Heterojunction Solar Cells.

In recent years, 2D Ruddlesden-Popper (2DRP) perovskite materials have been explored as emerging semiconductor materials in solar cells owing to their excellent stability and structural diversity. Although 2DRP perovskites have achieved photovoltaic efficiencies exceeding 19%, their widespread use is hindered by their inferior charge-carrier transport properties in the presence of diverse organic spacer cations, compared to that of traditional 3D perovskites. Hence, a systematic understanding of the carrier transport mechanism in 2D perovskites is critical for the development of high-performance 2D perovskite solar cells (PSCs). Here, the recent advances in the carrier behavior of 2DRP PSCs are summarized, and guidelines for successfully enhancing carrier transport are provided. First, the composition and crystal structure of 2DRP perovskite materials that affect carrier transport are discussed. Then, the features of 2DRP perovskite films (phase separation, grain orientation, crystallinity kinetics, etc.), which are closely related to carrier transport, are evaluated. Next, the principal direction of carrier transport guiding the selection of the transport layer is revealed. Finally, an outlook is proposed and strategies for enhancing carrier transport in high-performance PSCs are rationalized. 

Charge‐Carrier Transport in Quasi‐2D Ruddlesden–Popper Perovskite Solar Cells

Formamidinium (FA) based perovskites are considered as one of the most promising light-absorbing perovskite materials owing to their narrower band gap and better thermal stability compared to conventional methylammonium-based perovskites. Constant improvement by using various additives stimulates the potential application of these perovskites. Amine molecules with different structures have been widely used as typical additives in FA-based perovskite solar cells, and decent performances have been achieved. Thus, a systematic review focusing on structural regulation and functional construction of amines in FA-based perovskites is of significance. Herein, we analyze the construction mechanism of different structural amines on the functional perovskite crystals. The influence of amine molecules on specific perovskite properties including defect conditions, charge transfer, and moisture resistance are evaluated. Finally, we summarize the design rules of amine molecules for the application in high-performance FA-based perovskites and propose directions for the future development of additive molecules. 

Gerd Kaupp

Papers

Charge‐Carrier Transport in Quasi‐2D Ruddlesden–Popper Perovskite Solar Cells

From Structural Design to Functional Construction: Amine Molecules in High‐Performance Formamidinium‐Based Perovskite Solar Cells