Understanding the function of moisture on perovskite is challenging since the random environmental moisture strongly disturbs the perovskite structure. Here, we develop various N2-protected characterization techniques to comprehensively study the effect of moisture on the efficient cesium, methylammonium, and formamidinium triple-cation perovskite (Cs0.05FA0.75MA0.20)Pb(I0.96Br0.04)3. In contrast to the secondary measurements, the established air-exposure-free techniques allow us directly monitor the influence of moisture during perovskite crystallization. We find a controllable moisture treatment for the intermediate perovskite can promote the mass transportation of organic salts, and help them enter the buried bottom of the films. This process accelerates the quasi-solid-solid reaction between organic salts and PbI2, enables a spatially homogeneous intermediate phase, and translates to high-quality perovskites with much-suppressed defects. Consequently, we obtain a champion device efficiency of approaching 24% with negligible hysteresis. The devices exhibit an average T80-lifetime of 852 h (maximum 1210 h) working at the maximum power point.

Constructing 2D/3D perovskite heterojunctions is effective for the surface passivation of perovskite solar cells (PSCs). However, previous reports that studying perovskite post-treatment only physically deposits 2D perovskite on the 3D perovskite, and the bulk 3D perovskite remains defective. Herein, we propose Cl2-dissolved chloroform as a multifunctional solvent for concurrently constructing 2D/3D perovskite heterojunction and inducing the secondary growth of the bulk grains. The mechanism of how Cl2 affects the performance of PSCs is clarified. Specifically, the dissolved Cl2 reacts with the 3D perovskite, leading to Cl/I ionic exchange and Ostwald ripening of the bulk grains. The generated Cl− further diffuses to passivate the bulk crystal and buried interface of PSCs. Hexylammonium bromide dissolved in the solvent reacts with the residual PbI2 to form 2D/3D heterojunctions on the surface. As a result, we achieved high-performance PSCs with a champion efficiency of 24.21% and substantially improved thermal, ambient, and operational stability.

Wide-bandgap (WBG) perovskite solar cells suffer from severe non-radiative recombination and exhibit relatively large open-circuit voltage (VOC) deficits, limiting their photovoltaic performance. Here, we address these issues by in-situ forming a well-defined 2D perovskite (PMA)2PbCl4 (phenmethylammonium is referred to as PMA) passivation layer on top of the WBG active layer. The 2D layer with highly pure dimensionality and halide components is realized by intentionally tailoring the side-chain substituent at the aryl ring of the post-treatment reagent. First-principle calculation and single-crystal X-ray diffraction results reveal that weak intermolecular interactions between bulky PMA cations and relatively low cation-halide hydrogen bonding strength are crucial in forming the well-defined 2D phase. The (PMA)2PbCl4 forms improved type-I energy level alignment with the WBG perovskite, reducing the electron recombination at the perovskite/hole-transport-layer interface. Applying this strategy in fabricating semi-transparent WBG perovskite solar cells (indium tin oxide as the back electrode), the VOC deficits can be reduced to 0.49 V, comparable with the reported state-of-the-art WBG perovskite solar cells using metal electrodes. Consequently, we obtain hysteresis-free 18.60%-efficient WBG perovskite solar cells with a high VOC of 1.23 V. Graphical Abstract

SnO2 is widely used as the electron transport layer (ETL) in perovskite solar cells (PSCs) due to its excellent electron mobility, low processing temperature, and low cost. And the most common way of preparing the SnO2 ETL is spin-coating using the corresponding colloid solution. However, the spin-coated SnO2 layer is sometimes not so compact and contains pinholes, weakening the hole blocking capability. Here, a SnO2 thin film prepared through magnetron-sputtering was inserted between ITO and the spin-coated SnO2 to act as an interlayer. This strategy can combine the advantages of efficient electron extraction and hole blocking due to the high compactness of the sputtered film and the excellent electronic property of the spin-coated SnO2. Therefore, the recombination of photo-generated carriers at the interface is significantly reduced. As a result, the semitransparent perovskite solar cells (with a bandgap of 1.73 eV) based on this double-layered SnO2 demonstrate a maximum efficiency of 17.70% (stabilized at 17.04%) with negligible hysteresis. Moreover, the shelf stability of the device is also significantly improved, maintaining 95% of the initial efficiency after 800-hours of aging.

Although the commercial application of solar cells pursues scalable and large-area devices, small-area solar cells in the scale of several centimeters possess many advantages such as low fabrication cost and facile high-throughput screening in the research laboratory. Most emerging photovoltaic technology start from studying small-area devices. Recently, perovskite/silicon tandem solar cells have attracted extensive research interest because they can break the radiative efficiency limit of single-junction solar cells. However, when cutting commercial large-area silicon cells into small-area (square centimeters) for laboratory use, there occurs a significant efficiency loss, limiting the performance of tandem cells. Herein, to eliminate the thermal damage caused by the traditional laser cutting method and reduce the non-radiative recombination of heterojunction silicon cells after cutting, a cold-manufacturing method of grinding wheel dicing is used to cut heterojunction silicon cells. This method is realized by high-speed mechanical grinding accompanied by liquid washing, which avoids edge damage of solar cells caused by heat. Compared with the devices cut by laser, the heterojunction silicon cells cut by the cold-manufacturing method exhibit less cross-sectional damage. Scanning electron microscopy (SEM) and three-dimensional optical profilometer measurements reveal that the morphology of the device edge is smoother than that cut by laser. Device physics measurements including electrochemical impedance spectroscopy (EIS), dark current-voltage curves, transient photovoltage (TPV), transient photocurrent (TPC), and the dependence of short-circuit current density and open-circuit voltage on light intensity reveal that the cold-manufacturing method enables a significant inhibition of non-radiative recombination of the heterojunction silicon cells after cutting. These results indicate that the edge-recombination of the silicon solar cells cut by grinding wheels is reduced compared with that cut by laser. As a result, statistical analysis of the device performance reveals that both the open-circuit voltage and fill factor of the device are improved, and the average photoelectric conversion efficiency increases by an absolute efficiency of~1%. Stacking the obtained silicon cells with the normal transparent perovskite solar cells, the obtained four-terminal perovskite/silicon tandem solar cells deliver an efficiency of over 28%. This work emphasizes the importance of reducing efficiency loss during manufacturing the heterojunction silicon solar cell in fabricating high-performance silicon-based tandem solar cells.