Self-Assembled Monolayer Suppresses Interfacial Reaction between NiOx and Perovskite for Efficient and Stable Inverted Inorganic Perovskite Solar Cells.

Inorganic NiOx has attracted tremendous attention in organic-inorganic hybrid perovskite solar cells (PSCs) in recent years but is relatively less used in all-inorganic PSCs. In this study, we have discovered and confirmed the detrimental interfacial reaction between NiOx and DMAI-containing CsPbI3 inorganic perovskites. Thus, a self-assembled monolayer, Br-2PACz, is employed to modify the NiOx surface to obstruct the adverse interfacial reaction and further improve the device performance. The results demonstrate that Br-2PACz modification on NiOx can also improve interface contact, perovskite film morphology, and energy level alignments. Consequently, a champion power conversion efficiency (PCE) of 19.34% with a high open-circuit voltage (VOC) of 1.15 V is obtained for inverted NiOx/Br-2PACz-based CsPbI3 PSCs compared to the reference NiOx-based PSC with a moderate PCE of 15.16% (VOC 1.05 V). Moreover, the stabilities of both CsPbI3 films and devices exhibited significant enhancement after Br-2PACz modification. The unpacked PSCs could maintain 80, 73, and 89% of the initial efficiency after aging in 30-35% RH for 960 h, heating at 60 °C for 48 h, and continuous illumination for 284 h, respectively, highly superior to the reference devices. Our work offers a facile and effective approach for developing high-performance inverted NiOx-based CsPbI3 PSCs.

Reduced trap-density and boosted performance of CH3NH3PbI3solar cells by 1-Pentanethiol enhanced anti-solvent washing route.

Performance and the stability of the perovskite-based photovoltaic devices are directly linked to existing trap-states or defect profiles at the surface and/or in the bulk of perovskite layers. Hence identification of stemming the defects during perovskite formation is crucial for achieving superior and long-lasting performances. Here, we present the effect of 1-Pentanethiol incorporation into the one-step deposition of perovskite layers. A feasible glove box-free route results in high-quality CH3NH3PbI3layers under highly humid conditions (RH > 50%) but at low temperatures (T< 18 °C). 1-Pentanethiol addition into the washing solvent leads to the refinement of I/Pb stoichiometry, elimination of the iodide deficiencies, and reduction of the trap-state densities. Consequently, a precise amount 1-Pentanethiol addition enhances photovoltaic performances, resulting in a 54% PCE improvement for CH3NH3PbI3-based inverted solar cells.

Achieving High Fill Factor in Efficient P-i-N Perovskite Solar Cells.

Lead halide perovskite solar cells (PSCs) have made unprecedented progress, exhibiting great potential for commercialization. Among them, inverted p-i-n PSCs provide outstanding compatibility with flexible substrates, more importantly, with silicon (Si) bottom devices for higher efficiency perovskite-Si tandem solar cells. However, even with recently obtained efficiency over 25%, the investigation of inverted p-i-n PSCs is still behind the n-i-p counterpart so far. Recent progress has demonstrated that the fill factor (FF) in inverted PSCs currently still underperforms relative to open-circuit voltage and short-circuit current density, which requires an in-depth understanding of the mechanism and further research. In this review article, the recent advancements in high FF inverted PSCs by adopting the approaches of interfacial optimization, precursor engineering as well as fabrication techniques to minimize undesirable recombination are summarized. Insufficient carrier extraction and transport efficiency are found to be the main factors that hinder the current FF of inverted PSCs. In addition, insights into the main factors limiting FF and strategies for minimizing series resistance in inverted PSCs are presented. The continuous efforts dedicated to the FF of high-performance inverted devices may pave the way toward commercial applications of PSCs in the near future.

Bridging the Buried Interface with Piperazine Dihydriodide Layer for High Performance Inverted Solar Cells.

Given that it is closely related to perovskite crystallization and interfacial trap densities, buried interfacial engineering is crucial for creating effective and stable perovskite solar cells. Compared with the in-depth studies on the defect at the top perovskite interface, exploring the defect of the buried side of perovskite film is relatively complicated and scanty owing to the non-exposed feature. Herein, the degradation process is probed from the buried side of perovskite films with continuous illumination and its effects on morphology and photoelectronic characteristics with a facile lift-off method. Additionally, a buffer layer of Piperazine Dihydriodide (PDI2 ) is inserted into the imbedded bottom interface. The PDI2 buffer layer is able to lubricate the mismatched thermal expansion between perovskite and substrate, resulting in the release of lattice strain and thus a void-free buried interface. With the PDI2 buffer layer, the degradation originates from the growing voids and increasing non-radiative recombination at the imbedded bottom interfaces are suppressed effectively, leading to prolonged operation lifetime of the perovskite solar cells. As a result, the power conversion efficiency of an optimized p-i-n inverted photovoltaic device reaches 23.47% (with certified 23.42%) and the unencapsulated devices maintain 90.27% of initial efficiency after 800 h continuous light soaking.

Inorganic Perovskite Surface Reconfiguration for Stable Inverted Solar Cells with 20.38% Efficiency and Its Application in Tandem Devices.

Inorganic perovskite solar cells (IPSCs) have garnered attention in tandem solar cells (TSCs) due to their suitable bandgap and impressive thermal stability. However, the efficiency of inverted IPSCs has been limited by the high trap density on the top surface of inorganic perovskite film. Herein, a method for fabricating efficient IPSCs by reconfiguring the surface properties of CsPbI2.85 Br0.15 film with 2-amino-5-bromobenzamide (ABA) is developed. This modification not only exhibits the synergistic coordination of carbonyl (C=O) and amino (NH2 ) groups with uncoordinated Pb2+ , but also the Br fills halide vacancies and suppresses the formation of Pb0 , effectively passivating the defective top surface. As a result, a champion efficiency of 20.38%, the highest efficiency reported for inverted IPSCs to date is achieved. Furthermore, the successful fabrication of a p-i-n type monolithic inorganic perovskite/silicon TSCs with an efficiency of 25.31% for the first time is demonstrated. Crucially, the unencapsulated ABA-treated IPSCs shows enhanced photostability, retaining 80.33% of its initial efficiency after 270 h, and thermal stability (maintain 85.98% of its initial efficiency after 300 h at 65 °C). The unencapsulated ABA-treated TSCs also retains 92.59% of its initial efficiency after 200 h under continuous illumination in ambient air.

Li-Doped ZnO Electron Transport Layer for Improved Performance and Photostability of Organic Solar Cells.

Organic solar cells (OSCs) based on an inverted architecture generally have better stability compared to those based on a standard architecture. However, the photoactive area of the inverted solar cells increases under ultraviolet (UV) or solar illuminatiom because of the too-high conductivity of the UV-illuminated zinc oxide (ZnO) interlayer. This limits the potential of the inverted solar cells for industrial applications. Herein, lithium-doped ZnO (Li-ZnO) films are employed as the cathode interlayer to construct inverted OSCs. The incorporation of Li ions is found to reduce the lateral conductivity of the UV-treated ZnO films because of the presence of Li ions, preventing the high-quality-growth of ZnO nanocrystals. This addresses the problem of having too-high conductivity in the UV-treated ZnO layer, causing the increased photoactive area of inverted solar cells. The overall performance of the solar cell is shown to be higher after the incorporation of Li ions in the ZnO layer, mainly due to the increased fill factor (FF), originating from the reduced trap-assisted recombination losses. Finally, the inverted solar cells based on the Li-ZnO interlayer are demonstrated to have a much better long-term stability, as compared to those based on ZnO. This allows the ZnO-based interlayers to be used for the mass production of organic solar cell modules.

Air-Processed, Stable Organic Solar Cells with High Power Conversion Efficiency of 7.41.

High efficiency, excellent stability, and air processability are all important factors to consider in endeavoring to push forward the real-world application of organic solar cells. Herein, an air-processed inverted photovoltaic device built upon a low-bandgap, air-stable, phenanthridinone-based ter-polymer (C150 H218 N6 O6 S4 )n (PDPPPTD) and [6,6]-phenyl-C61 -butyric acid methyl ester (PC61 BM) without involving any additive engineering processes yields a high efficiency of 6.34%. The PDPPPTD/PC61 BM devices also exhibit superior thermal stability and photo-stability as well as long-term stability in ambient atmosphere without any device encapsulation, which show less performance decay as compared to most of the reported organic solar cells. In view of their great potential, solvent additive engineering via adding p-anisaldehyde (AA) is attempted, leading to a further improved efficiency of 7.41%, one of the highest efficiencies for all air-processed and stable organic photovoltaic devices. Moreover, the device stability under different ambient conditions is also further improved with the AA additive engineering. Various characterizations are conducted to probe the structural, morphology, and chemical information in order to correlate the structure with photovoltaic performance. This work paves a way for developing a new generation of air-processable organic solar cells for possible commercial application.

Understanding the Light Soaking Effects in Inverted Organic Solar Cells Functionalized with Conjugated Macroelectrolyte Electron-Collecting Interlayers.

Three kinds of charged star-shaped conjugated macroelectrolytes, named as PhNBr, TPANBr, and TrNBr, are synthesized as electron-collecting interlayers for inverted polymer solar cells (i-PSCs). Based on these well-defined structured interlayer materials, the light soaking (LS) effect observed in i-PSCs was studied systematically and accurately. The general character of the LS effect is further verified by studying additional i-PSC devices functionalized with other common interlayers. The key-role of UV photons was confirmed by electrochemical impedance spectroscopy and electron-only devices. In addition, the ultraviolet photoelectron spectroscopy measurements indicate that the work function of the indium tin oxide (ITO)/interlayer cathode is significantly reduced after UV treatment. In these i-PSC devices the LS effect originates from the adsorbed oxygen on the ITO substrates when oxygen plasma is used; however, even a small amount of oxygen from the ambient is also enough for triggering the LS effect, albeit with a weaker intensity. Our results suggest that the effect of adsorbed oxygen on ITO needs to be considered with attention while preparing i-PSCs. This is an important finding that can aid the large-scale manufacturing of organic solar cells via printing technologies, which do not always ensure the full protection of the device electrode substrates from oxygen.

Doping ZnO with Water/Alcohol-Soluble Small Molecules as Electron Transport Layers for Inverted Polymer Solar Cells.

By doping ZnO with porphyrin small molecules (FNEZnP-OE and FNEZnP-T) as cathode electron transport layers (ETLs), the inverted polymer solar cells (i-PSC) with PTB7:PC71BM (PTB7: polythieno[3,4-b]-thiophene-co-benzodithiophene, PC71BM:[6, 6]-phenyl-C71-butyric acid methyl ester) as the active materials exhibit enhanced device performance. While the power conversion efficiency (PCE) of the PSCs with pure ZnO ETL is 7.52%, that of the devices with FNEZnP-T-doped ZnO ETL shows a slightly improved PCE of 8.09%, and that of the PSCs with FNEZnP-OE-doped ZnO ETL is further enhanced up to 9.24% with an over 20% improvement compared to that with pure ZnO ETL. The better performance is contributed by the better interfacial contact and reduced work function induced by 9,9-bis(30-(N,N-dimethylamino)propyl)-2,7-fluorenes and 3,4-bis(2-(2-methoxy-ethoxy)-ethoxy)-phenyls in the porphyrin small molecules. More importantly, the PCE is still higher than 8% even when the thickness of FNEZnP-OE-doped ZnO ETL is up to 110 nm, which are important criteria for eventually making organic photovoltaic modules with roll-to-roll coat processing.

Nafion-modified MoOx as effective room-temperature hole injection layer for stable, high-performance inverted organic solar cells.

We present a hole injection layer processed from solution at room temperature for inverted organic solar cells. Bis(2,4-pentanedionato) molybdenum(VI) dioxide (MoO2(acac)2) is used as the precursor for MoOx. Small amounts of Nafion in the precursor solution allow it to form continuous films with good wetting onto the active layers. The hydrolysis of MoO2(acac)2 and the effects of adding Nafion to the precursor solution are studied by Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy. The devices with solution-processed MoOx including Nafion exhibited comparable performance to the reference devices based on the commonly used hole injection layers such as poly(3,4-ethylenedioxythiophene):polystyrenesulfonate (PEDOT:PSS) or evaporated MoO3. Inverted poly(3-hexylthiophene):[6,6]-phenyl C61-butyric acid methyl ester devices with Nafion-modified MoOx maintain 80% of their initial power conversion efficiency upon exposure to ambient air for ∼5000 h, outperforming devices with PEDOT:PSS or with evaporated MoO3.