Judicious tailoring of the interface between the SnO2 electron‐transport layer and the perovskite buried surface plays a pivotal role in obtaining highly efficient and stable perovskite solar cells (PSCs). Herein, a DL‐carnitine hydrochloride (DL) is incorporated into the perovskite/SnO2 interface to suppress the defect‐states density. A DL‐dimer is obtained at the interface by an intermolecular esterification reaction. For the SnO2 film, the Cl− in the DL‐dimer can passivate oxygen vacancies (VO) through electrostatic coupling, while the N in the DL‐dimer can coordinate with the Sn4+ to passivate Sn‐related defects. For the perovskite film, the DL‐dimer can passivate FA+ defects via hydrogen bonding and Pb‐related defects more efficiently than the DL monomer. Upon DL‐dimer modification, the interfacial defects are effectively passivated and the quality of the resultant perovskite film is improved. As a result, the DL‐treated device achieves a gratifying open‐circuit voltage (VOC) of 1.20 V and a champion power conversion efficiency (PCE) of 25.24%, which is a record value among all the reported FACsPbI3 PSCs to date. In addition, the unencapsulated devices exhibit a charming stability, sustaining 99.20% and 90.00% of their initial PCEs after aging in air for 1200 h and continuously operating at the maximum power point tracking for 500 h, respectively.

25.24%‐Efficiency FACsPbI3 Perovskite Solar Cells Enabled by Intermolecular Esterification Reaction of DL‐Carnitine Hydrochloride

Formamidinium (FA)-rich lead iodide perovskite solar cells (PSCs) are gaining popularity because of their excellent photovoltaic performance. Nevertheless, the FA-rich perovskites processed by a two-step sequential deposition method usually possess...

Modulation of Nucleation and Crystallization in PbI2 Films Promoting Preferential Perovskite Orientation Growth for Efficient Solar Cells

Perovskite solar cells (PSCs) are now one of the most promising solar cells due to advantages such as high‐power conversion efficiency (PCE), low cost, and ease of fabrication. Among PSCs, flexible perovskite solar cells (FPSCs) are lightweight and bendable, making them easier to transport and install than rigid PSCs, and hence can be used in wearable and portable electronics, space energy systems, multifunctional integrated buildings, unmanned systems, and other applications. Compared with regular n–i–p FPSCs, inverted p–i–n FPSCs possess advantages of reliable operational stability, reduced hysteresis effect, low‐temperature fabrication process, and strong potential for tandem devices. At present, the PCEs of single‐junction and tandem‐inverted FPSCs have reached 21.76% and 24.7%, respectively, indicating promising commercial applications. In this review, first, the developments of device functional layers including flexible substrates, flexible conductive electrodes, charge transport layers, and perovskite active layers in inverted FPSCs are elucidated and discussed thoroughly. Then, the technologies for accelerating commercialization of inverted FPSCs are summarized in detail. Finally, perspectives on the development and commercialization of inverted FPSCs are provided.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/sstr.202200338

Functional Layers of Inverted Flexible Perovskite Solar Cells and Effective Technologies for Device Commercialization

Mechanical endurance and long-term operational stability are critical factors for the commercialization of flexible perovskite solar cells (f-PSCs), attributable to defects in the perovskite layer. In this study, we synthesized...

Molecular dipole engineering assisted strain release for mechanically robust flexible perovskite solar cells

Interface engineering is of paramount importance for optimizing carrier dynamics and stability of perovskite solar cells (PSCs), but little attention has been paid to understanding and managing the buried interfaces. Here, a molecular bridge strategy is developed to modify the properties of buried interfaces in n–i–p PSCs by introducing a multi-functional additive 2-Hydroxyethyl trimethylammonium chloride (ChCl) in the bottom SnO2 electron transport layer. The ChCl treatment enables bifacial defects passivation and improved perovskite quality, leading to notably enhanced electron extraction and suppressed non-radiative recombination at the buried interfaces. As a result, a significantly improved power conversion efficiency (PCE) from 20.0% to 23.07% with a remarkable open-circuit voltage (Voc) of up to 1.193 V is achieved, along with superior stability (up to 4000 h) for the unsealed devices under different conditions (moisture, heat and maximum power point). Furthermore, this molecular bridge strategy demonstrates the ability to release the stress in perovskite thin film and simultaneously strengthen the interfacial toughness in flexible PSCs, yielding remarkable mechanical stability and a champion PCE of 21.50%. This study offers deep insights into understanding and engineering the buried interfaces and provides effective strategies to further enhance the performance and stability of PSCs. 

Molecular Bridge Assisted Bifacial Defect Healing Enables Low Energy Loss for Efficient and Stable Perovskite Solar Cells

Flexible perovskite solar cells (FPSCs) represent a promising technology in the development of next‐generation photovoltaic and optoelectronic devices. SnO2 electron transport layers (ETL) typically undergo significant cracking during the bending process of FPSCs, which can significantly compromise their charge transport properties. Herein, the semi‐planar non‐fullerene acceptor molecule Y6 (BT‐core‐based fused‐unit dithienothiophen [3,2‐b]‐pyrrolobenzothiadiazole derivative) is introduced as the buffer layer for SnO2‐based FPSCs. It is found that the Y6 buffer layer can enhance the ability of charge extraction and bending stability for SnO2 ETL. Moreover, the internal stress of perovskite films is also reduced. As a result, SnO2/Y6‐based FPSCs achieved a power conversion efficiency (PCE) of 20.09% and retained over 80% of their initial efficiency after 1000 bending cycles at a curvature radius of 8 mm, while SnO2‐based devices only retain 60% of their initial PCE (18.60%) upon the same bending cycles. In addition, the interfacial charge extraction is also effectively improved in conjunction with reduced defect density upon incorporation of Y6 on the SnO2 ETL, as revealed by femtosecond transient absorption (Fs‐TA) measurements.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/advs.202105739

Semi‐Planar Non‐Fullerene Molecules Enhance the Durability of Flexible Perovskite Solar Cells

SnO2 as an electron transport layer (ETL) has recently been used for perovskite solar cells (PSCs) due to high transmittance and electron mobility. However, the mismatched band energy alignment of ETL and perovskite layer result in serious nonradiative recombination limiting the improvement of PSCs performance. Here, 2-(Diphenylphosphino)ethanaminium tetrafluoroborate (DPEBF4) as buried interface was introduced between ETL and perovskite. The [BF4]− anion in DPEBF4 can interact with SnO2 to reduce the surface defect of SnO2. While [DPE]+ cation is more inclined to interact with Pb2+ and I−, the terminal strong interaction will promote crystallization of perovskite film quality and passivate buried surface defects. As a result, device performance was significantly improved by introducing DPEBF4 layer, the power conversion efficiency (PCE) increase from 20.50 % for control devices to 23.84 %. The work provides an interfacial double-tonic strategy for ETL and perovskite crystals to achieve high-performance perovskite photovoltaic devices. 

Interfacial bidirectional binding for improving photovoltaic performance of perovskite solar cells

Reducing the interfacial defects of perovskite films is key to improving the performance of perovskite solar cells (PSCs). In this study, two kinds of perylene monoimide (PMI) derivative phosphonium bromide salts were designed and used as a multifunctional interface-modified layer in PSCs. These two molecules are inserted between SnO2 and perovskite to produce a bidirectional passivation effect. The interaction with SnO2 reduces the oxygen vacancy on the surface of SnO2 and tunes the energy level of the electron transport layer, making more matches with the perovskite layer. The modified layer can promote the growth of perovskite crystals and reduce the interfacial defects of the perovskite film. Furthermore, the power conversion efficiency (PCE) of PSCs increased from 19.49 to 22.85%, and the open-circuit voltage (VOC) increased from 1.06 to 1.14 V. At the same time, the PCE of the SnO2/PMI-TPP-based device remained 88% of the initial PCE after 240 h of continuous illumination. In addition, these two PMI derivatives with a quasi-planar structure can improve the flexibility of flexible PSCs. This study provided a new strategy for the interfacial modification of PSCs and a new insight into the application of flexible PSCs.

Perylene Monoimide Phosphorus Salt Interfacial Modified Crystallization for Highly Efficient and Stable Perovskite Solar Cells.

First-principles study of size effects on electrical properties of AlN/GaN heterostructured nanofilms

Perovskite film-quality is a crucial factor to improve the photovoltaic properties of perovskite solar cells, which is closely related to the morphology of crystallization grain size of the perovskite layer. However, defects and trap sites are inevitably generated on the surface and at the grain boundaries of the perovskite layer. Here, we report a convenient method for preparing dense and uniform perovskite films, employing g-C3N4 quantum dots doped into the perovskite layer by regulating proper proportions. This process produces perovskite films with dense microstructures and flat surfaces. As a result, the higher fill factor (0.78) and a power conversion efficiency of 20.02% are obtained by the defect passivation of g-C3N4QDs.

/pdf/reduced-electron-relaxation-time-of-perovskite-films-via-g-13rbuetf.pdf

Reduced electron relaxation time of perovskite films via g-C3N4 quantum dot doping for high-performance perovskite solar cells

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