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The pursuit of high power conversion efficiency (PCE) and cost‐effective perovskite solar cells (PSCs) has spawned many innovative device structure designs. Compared with the traditional NIP type PSCs, electron transport layer (ETL) free PSCs have attracted growing attention due to their enormous potential in large area, low‐cost flexible application. However, there is still a lack of in‐depth understanding of the energy level arrangement indium tin oxide (ITO)/perovskite interface, resulting in poor device performance. Here, a metal/insulator/n‐type perovskite/p‐type spiro‐MeOTAD (MINP) structure is proposed to elaborate on the influence of the apparent work function and contact barrier change of the metal–semiconductor (MS) and metal–insulator–semiconductor (MIS) junction on the carrier transfer and collection. Common and easily available 5‐amino‐valeric acid is inserted into the ITO/perovskite interface to form an insulating dipole layer and to ensure quasi‐ohmic contact at the front interface. Consequently, the device changes from Schottky/PN cascade heterojunction type to a single PN heterojunction device with its ideal factor decreasing from 3.35 to 2.05. Accordingly, the champion device achieves 19.37% PCE with significantly increased Voc and FF compared to the pristine device. This work provides a facile and effective method to improve the application potential of novel ETL‐free PSCs. [ABSTRACT FROM AUTHOR]

Efficient electron transport layer-free perovskite solar cells (ETL-free PSCs) are promising designs because they offer low-cost, simpler device configuration and greatly promote the large area flexible application of PSCs. Meanwhile, compared to traditional PSCs with ETL, the development of ETL-free PSCs is hindered by their low performance due to serious interfacial energy loss. Herein, we reveal that ETL-free devices with relatively low carrier lifetimes of perovskite films exhibit more substantial photogenerated carrier loss, resulting in a lower electron-injection rate at the FTO (fluorine-containing tin oxide)/perovskite interface, which is mainly responsible for the performance loss. Moreover, we demonstrate that improving the carrier lifetimes of perovskite films can remedy the poor carrier extraction efficiency at the FTO/perovskite interface through three typical perovskite films. Similarly, for all-inorganic perovskite with lower carrier lifetime and hole transport layer-free devices, prolonging carrier lifetime may be an important measure to improve the device performance. Benefiting from this discovery, increasing the carrier lifetime of the perovskite films can counterbalance the inferior device interfaces, endowing the ETL-free PSCs with high performance close to that of the ETL devices. Our research provides insights into ETL-free PSCs and offers opportunities for high-performance ETL-free PSC device design. [ABSTRACT FROM AUTHOR]

CsPbI2Br all-inorganic perovskite solar cells (PSCs) have attracted much attention due to their suitable bandgap and outstanding thermostability. However, the large energy loss of CsPbI2Br PSCs generally endows low open circuit voltage (VOC) and unsatisfactory power conversion efficiency (PCE), which severely hamper its further development. Herein, we proposed a facile route to modify the ZnO electron transporting layer (ETL) by in situ chemical doping strategy with metal ions. The doped ZnO ETL with Pb(Ac)2 or CsAc cannot only effectively tune its energy levels, conductivity, and charge extraction but also ameliorate the crystallization and morphology of upper perovskite films. Particularly, Pb(Ac)2-doped ZnO (ZnO:Pb) induces an energy level offset of 0.15 eV relative to the conduction band of CsPbI2Br with largely reduced Ohmic loss. Thus, the highest VOC is significantly boosted to above 1.3 V for the CsPbI2Br PSCs with a champion PCE of 16.36%, while the reference PSC just yields a moderate PCE of 14.43% with a low VOC of 1.168 V. Moreover, considerable improvements in device stability are achieved for the PSCs with doped ZnO ETLs than those of the ZnO-based device. Our work provides a promising strategy to alleviate the VOC deficit toward the attainment of highly efficient and stable PSCs. [ABSTRACT FROM AUTHOR]

[Display omitted] • HEMA additive was added to the CsPbI 2 Br precursor solution to improve crystallization. • HEMA molecules could passivate defects and suppress charge recombination. • A champion efficiency of 16.13% was obtained with greatly enhanced device stability. CsPbI 2 Br all-inorganic perovskite has attracted considerable attention due to its high thermal stability and suitable bandgap, while the unsatisfactory crystallization quality and moisture instability significantly hinder its further application. Herein, a novel multifunctional liquid additive, 2-hydroxyethyl methacrylate (HEMA), is introduced into the CsPbI 2 Br precursor to ameliorate the above issues. Our results demonstrate that the functional groups of HEMA can interact with perovskite precursor, thus improving crystallization and passivating defects at the same time, and leading to a champion power conversion efficiency of up to 16.13%. Importantly, HEMA molecule in perovskite films will polymerize to a hydrophobic polymer at grain boundaries through breaking C = C bonds during the high temperature annealing process (160 °C). Moreover, this multifunctional liquid additive strategy endows perovskite films with promoted moisture tolerance by crosslinking perovskite grains and blocking moisture penetration, thus the unencapsulated device maintains 78% of its initial efficiency after aging at 30% relative humidity for 1000 h. These results demonstrate that the additive engineering with multifunctional molecule is applicable strategy for developing CsPbI 2 Br all-inorganic perovskite solar cells with both high efficiency and stability. [ABSTRACT FROM AUTHOR]