Interface Reactive Sputtering of Transparent Electrode for High-Performance Monolithic and Stacked Perovskite Tandem Solar Cells.

Sputtered indium tin oxide (ITO) fulfills the requirements of top transparent electrodes (TTEs) in semitransparent perovskite solar cells (PSCs) and stacked tandem solar cells (TSCs), as well as of the recombination layers in monolithic TSCs. However, the high-energy ITO particles will cause damage to the devices. Herein, the interface reactive sputtering strategy is proposed to construct cost-effective TTEs with high transmittance and excellent carrier transporting ability. Polyethylenimine (PEI) is chosen as the interface reactant that can react with sputtered ITO nanoparticles, so that, coordination compounds can be formed during the deposition process, facilitating the carrier transport at the interface of C60/PEI/ITO. Besides, the impact force of energetic ITO particles is greatly alleviated, and the intactness of the underlying C60 layer and perovskite layer is guaranteed. Thus, the prepared semitransparent subcells achieve a significantly enhanced power conversion efficiency (PCE) of 19.17%, surpassing those based on C60/ITO (11.64%). Moreover, the PEI-based devices demonstrate excellent storage stability, which maintains 98% of their original PCEs after 2000 h. On the strength of the interface reactive sputtering ITO electrode, a stacked all-perovskite TSC with a PCE of 26.89% and a monolithic perovskite-organic TSC with a PCE of 24.33% are successfully fabricated.

Amphoteric Ion Bridged Buried Interface for Efficient and Stable Inverted Perovskite Solar Cells.

Synergistic morphology and defects management at the buried perovskite interface are challenging but crucial for the further improvement of inverted perovskite solar cells (PerSCs). Herein, an amphoteric organic salt, 2-(4-fluorophenyl)ethylammonium-4-methyl benzenesulfonate (4FPEAPSA), is designed to optimize the film morphology and energy level alignment at the perovskite buried interface. 4FPEAPSA treatment promotes the growth of a void-free, coarse-grained, and hydrophobic film by inducing the crystal orientation. Besides, the dual-functional 4FPEAPSA can chemically interact with the perovskite film, and passivate the defects of iodine and formamidine vacancies, tending to revert the fermi level of perovskite to its defect-free state. Meanwhile, the formation of a p-type doping buried interface can facilitate the interfacial charge extraction and transport of PerSCs for reduced carrier recombination loss. Consequently, 4FPEAPSA treatment improves the efficiency of the perovskite devices to 25.03% with better storage, heat, and humidity stability. This work contributes to strengthening the systematic understanding of the perovskite buried interface, providing a synergetic approach to realize precise morphology control, effective defect suppression, and energy level alignment for efficient PerSCs.

Transparent Recombination Electrode with Dual-Functional Transport and Protective Layer for Efficient and Stable Monolithic Perovskite/Organic Tandem Solar Cells.

Rational selection and design of recombination electrodes (RCEs) are crucial to enhancing the power conversion efficiency (PCE) and stability of monolithic tandem solar cells (TSCs). Sputtered indium tin oxide (ITO) with high conductivity and excellent transmittance is introduced as RCE in perovskite/organic TSCs. To prevent high-energy ITO particles destroy the underlying material during sputtering, dual-functional transport and protective layer (C1) is employed. The styryl group in C1 can be thermally crosslinked to serve as a sputtering protective layer. Meanwhile, the conjugated phenanthroline skeleton in C1 shows high electron mobility and hole blocking capability to promote the electron transport process at the interfaces and effectively reduce charge accumulation. Monolithic perovskite/organic TSC with high PCE of 24.07% and excellent stability is demonstrated by stacking a 1.77 eV bandgap perovskite layer and a 1.35 eV bandgap organic active layer. This strategy provides new insights for overcoming the fundamental efficiency limits of single-junction devices and promotes the further development of TSC devices.

Managing Interfacial Charged Defects with Multiple Active Sited Macrocyclic Valinomycin for Efficient and Stable Inverted Perovskite Solar Cells.

The unavoidably positively and negatively charged defects at the interface between perovskite and electron transport layer (ETL) often lead to severe surface recombination and unfavorable energy level alignment in inverted perovskite solar cells (PerSCs). Inserting interlayers at this interface is an effective approach to eliminate charged defects. Herein, the macrocyclic molecule valinomycin (VM) with multiple active sites of ─C═O, ─NH, and ─O─ is employed as an interlayer at the perovskite/ETL contact to simultaneously eliminate positively and negatively charged defects. Combined with a series of theoretical calculations and experimental analyzes, it is demonstrated that the ─C═O and ─O─ groups in VM can immobilize the uncoordinated Pb2+ to manage the positively charged defect and the formation of N─H···I hydrogen bonding can recompense the formamidine vacancies to eliminate the negatively charged defect. In addition, the VM interlayer induces a favorable downshift band bending at the perovskite/ETL interface, facilitating charge separation and boosting charge transfer. Thanks to the reduced charged defects and favorable energy level alignment, the fabricated inverted PerSC delivers an outstanding power conversion efficiency of 24.06% with excellent long-term ambient and thermal stability. This work demonstrates that managing charged defects via multiple functional groups and simultaneously regulating energy level alignment is a reliable strategy to boost the performance of PerSCs.

Hexachlorotriphosphazene-assisted buried interface passivation for stable and efficient wide-bandgap perovskite solar cells.

Large open-circuit voltage (Voc) loss is the main issue limiting the efficiency improvement in wide bandgap perovskite solar cells (PerSCs). Herein, a facile buried interface treatment by hexachlorotriphosphazene is developed to suppress the Voc loss. The PerSCs include a [Cs0.22FA0.78Pb(I0.85Br0.15)3]0.97(MAPbCl3)0.03 (1.67 eV) absorber and deliver an efficiency of 21.47% and a Voc of 1.21 V (Voc loss of 0.46 V). More importantly, the unencapsulated PerSCs maintain 90% of the initial efficiency after aging 500 h in N2.

Self-Aggregated Light-Trapping Nanodots for Highly Efficient Organic Solar Cells.

The typical thickness of the photoactive layer in organic solar cells (OSCs) is around 100 nm, which limits the absorption efficiency of the incident light and the power conversion efficiency (PCE) of OSCs. Therefore, light-trapping schemes to reduce the optical losses in the thin photoactive layers are critically important for efficient OSCs. Herein, light-trapping and electron-collection dual-functional small organic molecules, N,N,N',N'-tetraphenyloxalamide (TPEA) and N,N,N',N'-tetraphenylmalonamide (TPMA), are designed and synthesized by a one-step acylation reaction. Driven by strong intermolecular force, TPEA and TPMA tend to self-aggregate into hemispherical light-trapping nanodots on the photoactive layer, resulting in enhanced light harvesting. Meanwhile, TPEA and TPMA demonstrate high electron mobility and excellent electron-collection ability.  Compared with the device without cathode buffer layer (CBL, PCE = 14.09%), PM6:BTP-eC9 based OSCs with TPEA and TPMA light-trapping CBLs demonstrate greatly enhanced PCE of 16.21% and 17.85%, respectively. Furthermore, a record PCE of 19.02% can be achieved for PM6:BTP-eC9:PC71 BM based ternary OSC with TPMA light-trapping CBL. Moreover, TPMA exhibits a low synthesis cost of only 0.61 $ g-1 with high yield. These findings could open a window for the rational design of multifunctional CBLs for efficient and stable OSCs.

Revival of Insulating Polyethylenimine by Creatively Carbonizing with Perylene into Highly Crystallized Carbon Dots as the Cathode Interlayer for High-Performance Organic Solar Cells.

The development of new electron transporting layer (ETL) materials to improve the charge carrier extraction and collection ability between cathode and the active layer has been demonstrated to be an effective approach to enhance the photovoltaic performance of organic solar cells (OSCs). Herein, water-soluble carbon dots (CDs) as ETL material have been creatively synthesized by a vigorous chemical reaction between polyethylenimine (PEI) and 3,4,9,10-perylenetetracarboxylic dianhydride (PTCDA) via a simple one-step hydrothermal method. Taking full advantage of the high electron transfer property of PTCDA and the work function (WF) reduction ability of PEI, CD gained high electron mobility due to its large π-conjugated area and reduced the WF of indium tin oxide (ITO) by 0.75 eV. As for the photovoltaic performance of devices, inverted OSCs based on CDs have achieved a high power conversion efficiency (PCE) of 17.35%, exhibiting no burn-in effect with no reduction in PCE after more than 4000 h of storage. The successful application of CDs in OPV has developed a new avenue for designing efficient ETL materials that benefits the photovoltaic performance of OSCs.

Morphological Stabilization in Organic Solar Cells via a Fluorene-Based Crosslinker for Enhanced Efficiency and Thermal Stability.

Power conversion efficiencies (PCEs) and device stability are two key technical factors restricting the commercialization of organic solar cells (OSCs). In the past decades, though the PCEs of OSCs have been significantly enhanced, device instability, especially in the state-of-the-art nonfullerene system, still needs to be solved. In this work, an effective crosslinker (namely, DTODF-4F), with conjugated fluorene-based backbone and crosslinkable epoxy side-chains, has been designed and synthesized, which is introduced to enhance the morphological stabilization of the PM6:Y6-based film. This crosslinker with two epoxy groups can be in situ crosslinked into a stable network structure under ultraviolet radiation. We demonstrate that DTODF-4F, which acted as a third component, can promote the exciton dissociation rate and reduce traps/defects, finally resulting in the enhancement of efficiency. In particular, the OSC devices exhibit better stability under continuous heating owing to the morphology fixation of the bulk heterojunction. This work drives the development direction of morphological stabilization to further improve the performance and stability of OSCs.