SrTiO3/Al2O3‐Graphene Electron Transport Layer for Highly Stable and Efficient Composites‐Based Perovskite Solar Cells with 20.6% Efficiency

For practical use of perovskite solar cells (PSCs) the instability issues of devices, attributed to degradation of perovskite molecules by moisture, ions migration, and thermal‐ and light‐instability, have to be solved. Herein, highly efficient and stable PSCs based on perovskite/Ag‐reduced graphene oxide (Ag‐rGO) and mesoporous Al₂O₃/graphene (mp‐AG) composites are reported. The mp‐AG composite is conductive with one‐order of magnitude higher mobility than mp‐TiO₂ and used for electron transport layer (ETL). Compared to the mp‐TiO₂ ETL based cells, the champion device based on perovskite/Ag‐rGO and SrTiO₃/mp‐AG composites shows overall a best performance (i.e., V_OC = 1.057 V, J_SC = 25.75 mA cm^?2, fill factor (FF) = 75.63%, and power conversion efficiency (PCE) = 20.58%). More importantly, the champion device without encapsulation exhibits not only remarkable thermal‐ and photostability but also long‐term stability, retaining 97–99% of the initial values of photovoltaic parameters and sustaining ≈93% of initial PCE over 300 d under ambient conditions.     

Record Open‐Circuit Voltage Wide‐Bandgap Perovskite Solar Cells Utilizing 2D/3D Perovskite Heterostructure

In this work, the authors realize stable and highly efficient wide‐bandgap perovskite solar cells that promise high power conversion efficiencies (PCE) and are likely to play a key role in next generation multi‐junction photovoltaics (PV). This work reports on wide‐bandgap (≈1.72 eV) perovskite solar cells exhibiting stable PCEs of up to 19.4% and a remarkably high open‐circuit voltage (V_OC) of 1.31 V. The V_OC‐to‐bandgap ratio is the highest reported for wide‐bandgap organic?inorganic hybrid perovskite solar cells and the V_OC also exceeds 90% of the theoretical maximum, defined by the Shockley–Queisser limit. This advance is based on creating a hybrid 2D/3D perovskite heterostructure. By spin coating n‐butylammonium bromide on the double‐cation perovskite absorber layer, a thin 2D Ruddlesden–Popper perovskite layer of intermediate phases is formed, which mitigates nonradiative recombination in the perovskite absorber layer. As a result, V_OC is enhanced by 80 mV.     

Wide‐Bandgap Perovskite/Gallium Arsenide Tandem Solar Cells

Gallium arsenide (GaAs) photovoltaic (PV) cells have been widely investigated due to their merits such as thin‐film feasibility, flexibility, and high efficiency. To further increase their performance, a wider bandgap PV structure such as indium gallium phosphide (InGaP) has been integrated in two‐terminal (2T) tandem configuration. However, it increases the overall fabrication cost, complicated tunnel‐junction diode connecting subcells are inevitable, and materials are limited by lattice matching. Here, high‐efficiency and stable wide‐bandgap perovskite PVs having comparable bandgap to InGaP (1.8–1.9 eV) are developed, which can be stable low‐cost add‐on layers to further enhance the performance of GaAs PVs as tandem configurations by showing an efficiency improvement from 21.68% to 24.27% (2T configuration) and 25.19% (4T configuration). This approach is also feasible for thin‐film GaAs PV, essential to reduce its fabrication cost for commercialization, with performance increasing from 21.85% to 24.32% and superior flexibility (1000 times bending) in a tandem configuration. Additionally, potential routes to over 30% stable perovskite/GaAs tandems, comparable to InGaP/GaAs with lower cost, are considered. This work can be an initial step to reach the objective of improving the usability of GaAs PV technology with enhanced performance for applications for which lightness and flexibility are crucial, without a significant additional cost increase.     

Ultrathin Nanosheets of Oxo‐functionalized Graphene Inhibit the Ion Migration in Perovskite Solar Cells

Mixed cation/halide perovskites have led to a significant increase in the efficiency and stability of perovskite solar cells. However, mobile ionic defects inevitably exacerbate the photoinduced phase segregation and self‐decomposition of the crystal structure. Herein, ultrathin 2D nanosheets of oxo‐functionalized graphene/dodecylamine (oxo‐G/DA) are used to solve ion migration in cesium (Cs)‐formamidinium (FA)‐methylammonium (MA) triple‐cation‐based perovskites. Based on the superconducting carbon skeleton and functional groups that provide lone pairs of electrons on it, the ultrathin 2D network structure can fit tightly on the crystals and wrap them, isolating them, and thus reducing the migration of ions within the built‐in electric field of the perovskite film. As evidence of the formation of sharp crystals with different orientation within the perovskite film, moiré fringes are observed in transmission electron microscopy. Thus, a champion device with a power conversion efficiency (PCE) of 21.1% (the efficiency distribution is 18.8 ± 1.7%) and a remarkable fill factor of 81%, with reduced hysteresis and improved long‐term stability, is reported. This work provides a simple method for the improvement of the structural stability of perovskite in solar cells.     

Graphene‐Based Electron Transport Layers in Perovskite Solar Cells: A Step‐Up for an Efficient Carrier Collection

The electron transport layer (ETL) plays a fundamental role in perovskite solar cells. Recently, graphene‐based ETLs have been proved to be good candidate for scalable fabrication processes and to achieve higher carrier injection with respect to most commonly used ETLs. Here, the effects of different graphene‐based ETLs in sensitized methylammonium lead iodide (MAPI) solar cells are experimentally studied. By means of time‐integrated and picosecond time‐resolved photoluminescence techniques, the carrier recombination dynamics in MAPI films embedded in different ETLs is investigated. Using graphene doped mesoporous TiO₂ (G+mTiO₂) with the addition of a lithium‐neutralized graphene oxide (GO‐Li) interlayer as ETL, it is found find that the carrier collection efficiency is increased by about a factor two with respect to standard mTiO₂. Taking advantage of the absorption coefficient dispersion, the MAPI layer morphology is probed, along the thickness, finding that the MAPI embedded in the ETL composed by G+mTiO₂ plus GO‐Li brings to a very good crystalline quality of the MAPI layer with a trap density about one order of magnitude lower than that found with the other ETLs. In addition, this ETL freezes MAPI at the tetragonal phase, regardless of the temperature. Graphene‐based ETLs can open the way to significant improvement of perovskite solar cells.     

Carbon Nanoparticles in High‐Performance Perovskite Solar Cells

In the past few years, organic–inorganic metal halide ABX₃ perovskites (A = Rb, Cs, methylammonium, formamidinium (FA); B = Pb, Sn; X = Cl, Br, I) have rapidly emerged as promising materials for photovoltaic applications. Tuning the film morphology by various deposition techniques and additives is crucial to achieve solar cells with high performance and long‐term stability. In this work, carbon nanoparticles (CNPs) containing functional groups are added to the perovskite precursor solution for fabrication of fluorine‐doped tin oxide/TiO₂/perovskite/spiro‐OMeTAD/gold devices. With the addition of CNPs, the perovskite films are thermally more stable, contain larger grains, and become more hydrophobic. NMR experiments provide strong evidence that the functional groups of the CNPs interact with FA cations already in the precursor solution. The fabricated solar cells show a power‐conversion efficiency of 18% and negligible hysteresis.