05 Fakultät Informatik, Elektrotechnik und Informationstechnik
Permanent URI for this collectionhttps://elib.uni-stuttgart.de/handle/11682/6
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Item Open Access Coordination chemistry as a universal strategy for a controlled perovskite crystallization(2023) Zuo, Weiwei; Byranvand, Mahdi Malekshahi; Kodalle, Tim; Zohdi, Mohammadreza; Lim, Jaekeun; Carlsen, Brian; Magorian Friedlmeier, Theresa; Kot, Małgorzata; Das, Chittaranjan; Flege, Jan Ingo; Zong, Wansheng; Abate, Antonio; Sutter‐Fella, Carolin M.; Li, Meng; Saliba, MichaelThe most efficient and stable perovskite solar cells (PSCs) are made from a complex mixture of precursors. Typically, to then form a thin film, an extreme oversaturation of the perovskite precursor is initiated to trigger nucleation sites, e.g., by vacuum, an airstream, or a so-called antisolvent. Unfortunately, most oversaturation triggers do not expel the lingering (and highly coordinating) dimethyl sulfoxide (DMSO), which is used as a precursor solvent, from the thin films; this detrimentally affects long-term stability. In this work, (the green) dimethyl sulfide (DMS) is introduced as a novel nucleation trigger for perovskite films combining, uniquely, high coordination and high vapor pressure. This gives DMS a universal scope: DMS replaces other solvents by coordinating more strongly and removes itself once the film formation is finished. To demonstrate this novel coordination chemistry approach, MAPbI3 PSCs are processed, typically dissolved in hard-to-remove (and green) DMSO achieving 21.6% efficiency, among the highest reported efficiencies for this system. To confirm the universality of the strategy, DMS is tested for FAPbI3 as another composition, which shows higher efficiency of 23.5% compared to 20.9% for a device fabricated with chlorobenzene. This work provides a universal strategy to control perovskite crystallization using coordination chemistry, heralding the revival of perovskite compositions with pure DMSO.Item Open Access Ionic liquid Stabilizing high‐efficiency tin halide perovskite solar cells(2021) Li, Guixiang; Su, Zhenhuang; Li, Meng; Yang, Feng; Aldamasy, Mahmoud H.; Pascual, Jorge; Yang, Fengjiu; Liu, Hairui; Zuo, Weiwei; Di Girolamo, Diego; Iqbal, Zafar; Nasti, Giuseppe; Dallmann, André; Gao, Xingyu; Wang, Zhaokui; Saliba, Michael; Abate, AntonioTin halide perovskites attract incremental attention to deliver lead‐free perovskite solar cells. Nevertheless, disordered crystal growth and low defect formation energy, related to Sn(II) oxidation to Sn(IV), limit the efficiency and stability of solar cells. Engineering the processing from perovskite precursor solution preparation to film crystallization is crucial to tackle these issues and enable the full photovoltaic potential of tin halide perovskites. Herein, the ionic liquid n‐butylammonium acetate (BAAc) is used to tune the tin coordination with specific O…Sn chelating bonds and NH…X hydrogen bonds. The coordination between BAAc and tin enables modulation of the crystallization of the perovskite in a thin film. The resulting BAAc‐containing perovskite films are more compact and have a preferential crystal orientation. Moreover, a lower amount of Sn(IV) and related chemical defects are found for the BAAc‐containing perovskites. Tin halide perovskite solar cells processed with BAAc show a power conversion efficiency of over 10%. This value is retained after storing the devices for over 1000 h in nitrogen. This work paves the way toward a more controlled tin‐based perovskite crystallization for stable and efficient lead‐free perovskite photovoltaics.Item Open Access Pure tin halide perovskite solar cells : focusing on preparation and strategies(2022) Liu, Hairui; Zhang, Zuhong; Zuo, Weiwei; Roy, Rajarshi; Li, Meng; Byranvand, Mahdi Malekshahi; Saliba, MichaelMetal halide perovskite solar cells (PSCs) have emerged as an important direction for photovoltaic research. Although the power conversion efficiency (PCE) of lead‐based PSCs has reached 25.7%, still the toxicity of Pb remains one main obstacle for commercial adoption. Thus, to address this issue, Pb‐free perovskites have been proposed. Among them, tin‐based perovskites have emerged as promising candidates. Unfortunately, the fast oxidation of Sn2+ to Sn4+ leads to low stability and efficiency. Many strategies have been implemented to address these challenges in Sn‐based PSCs. This work introduces stability and efficiency improvement strategies for pure Sn‐based PSCs by optimization of the crystal structure, processing and interfaces as well as, implementation of low‐dimension structures. Finally, new perspectives for further developing Sn‐based PSCs are provided.Item Open Access High‐stable lead‐free solar cells achieved by surface reconstruction of quasi‐2D tin‐based perovskites(2023) Yang, Feng; Zhu, Rui; Zhang, Zuhong; Su, Zhenhuang; Zuo, Weiwei; He, Bingchen; Aldamasy, Mahmoud Hussein; Jia, Yu; Li, Guixiang; Gao, Xingyu; Li, Zhe; Saliba, Michael; Abate, Antonio; Li, MengTin halide perovskites are an appealing alternative to lead perovskites. However, owing to the lower redox potential of Sn(II)/Sn(IV), particularly under the presence of oxygen and water, the accumulation of Sn(IV) at the surface layer will negatively impact the device's performance and stability. To this end, this work has introduced a novel multifunctional molecule, 1,4‐phenyldimethylammonium dibromide diamine (phDMADBr), to form a protective layer on the surface of Sn‐based perovskite films. Strong interactions between phDMADBr and the perovskite surface improve electron transfer, passivating uncoordinated Sn(II), and fortify against water and oxygen. In situ grazing incidence wide‐angle X‐ray scattering (GIWAXS) analysis confirms the enhanced thermal stability of the quasi‐2D phase, and hence the overall enhanced stability of the perovskite. Long‐term stability in devices is achieved, retaining over 90% of the original efficiency for more than 200 hours in a 10% RH moisture N2 environment. These findings propose a new approach to enhance the operational stability of Sn‐based perovskite devices, offering a strategy in advancing lead‐free optoelectronic applications.Item Open Access Understanding the crystallization mechanism of organic-inorganic perovskite films(2025) Zuo, Weiwei; Saliba, Michael (Prof. Dr.)Item Open Access All-inorganic CsPbI2Br perovskite solar cells with thermal stability at 250 °C and moisture-resilience via polymeric protection layers(2025) Roy, Rajarshi; Byranvand, Mahdi Malekshahi; Zohdi, Mohamed Reza; Magorian Friedlmeier, Theresa; Das, Chittaranjan; Hempel, Wolfram; Zuo, Weiwei; Kedia, Mayank; Rendon, Jose Jeronimo; Boehringer, Stephan; Hailegnanw, Bekele; Vorochta, Michael; Mehl, Sascha; Rai, Monika; Kulkarni, Ashish; Mathur, Sanjay; Saliba, MichaelAll-inorganic perovskites, such as CsPbI2Br, have emerged as promising compositions due to their enhanced thermal stability. However, they face significant challenges due to their susceptibility to humidity. In this work, CsPbI2Br perovskite is treated with poly(3-hexylthiophen-2,5-diyl) (P3HT) during the crystallization resulting in significant stability improvements against thermal, moisture and steady-state operation stressors. The perovskite solar cell retains ∼90% of the initial efficiency under relative humidity (RH) at ∼60% for 30 min, which is among the most stable all-inorganic perovskite devices to date under such harsh conditions. Furthermore, the P3HT treatment ensures high thermal stress tolerance at 250 °C for over 5 h. In addition to the stability enhancements, the champion P3HT-treated device shows a higher power conversion efficiency (PCE) of 13.5% compared to 12.7% (reference) with the stabilized power output (SPO) for 300 s. In addition, the P3HT-protected perovskite layer in ambient conditions shows ∼75% of the initial efficiency compared to the unprotected devices with ∼28% of their initial efficiency after 7 days of shelf life.Item Open Access Mitigating the amorphization of perovskite layers by using atomic layer deposition of alumina(2025) Kedia, Mayank; Das, Chittaranjan; Kot, Malgorzata; Yalcinkaya, Yenal; Zuo, Weiwei; Tabah Tanko, Kenedy; Matvija, Peter; Ezquer, Mikel; Cornago, Iñaki; Hempel, Wolfram; Kauffmann, Florian; Plate, Paul; Lira-Cantu, Monica; Weber, Stefan A. L.; Saliba, MichaelAtomic layer deposition of aluminum oxide (ALD-Al2O3) layers has recently been studied for stabilizing perovskite solar cells (PSCs) against environmental stressors, such as humidity and oxygen. In addition, the ALD-Al2O3 layer acts as a protective barrier, mitigating pernicious halide ion migration from the perovskite towards the hole transport interface. However, its effectiveness in preventing the infiltration of ions and additives from the hole-transport layer into perovskites remains insufficiently understood. Herein, we demonstrate the deposition of a compact ultrathin (∼0.75 nm) ALD-Al2O3 layer that conformally coats the morphology of a triple-cation perovskite layer. This promotes an effective contact of the hole transporter layer on top of the perovskite, thereby improving the charge carrier collection between these two layers. Upon systematically investigating the layer-by-layer structure of the PSC, we discovered that ALD-Al2O3 also acts as a diffusion barrier for the degraded species from the adjacent transport layer into the perovskite. In addition to these protective considerations, ALD-Al2O3 impedes the transition of crystalline perovskites to an undesired amorphous phase. Consequently, the dual functionality (i.e., enhanced contact and diffusion barrier) of the ALD-Al2O3 protection enhanced the device performance from 19.1% to 20.5%, while retaining 98% of its initial performance compared to <10% for pristine devices after 1500 h of outdoor testing under ambient conditions. Finally, this study deepens our understanding of the mechanism of ALD-Al2O3 as a two-way diffusion barrier, highlighting the multifaceted role of buffer layers in interfacial engineering for the long-term stability of PSCs.