Browsing by Author "Das, Chittaranjan"

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    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, Michael
    All-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.
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    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, Michael
    The 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.
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    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, Michael
    Atomic 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.
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    Top‐down approach to study chemical and electronic properties of perovskite solar cells : sputtered depth profiling versus tapered cross‐sectional photoelectron spectroscopies
    (2021) Das, Chittaranjan; Zia, Waqas; Mortan, Claudiu; Hussain, Navid; Saliba, Michael; Ingo Flege, Jan; Kot, Małgorzata
    A study of the chemical and electronic properties of various layers across perovskite solar cell (PSC) stacks is challenging. Depth‐profiling photoemission spectroscopy can be used to study the surface, interface, and bulk properties of different layers in PSCs, which influence the overall performance of these devices. Herein, sputter depth profiling (SDP) and tapered cross‐sectional (TCS) photoelectron spectroscopies (PESs) are used to study highly efficient mixed halide PSCs. It is found that the most used SDP‐PES technique degrades the organic and deforms the inorganic materials during sputtering of the PSCs while the TCS‐PES method is less destructive and can determine the chemical and electronic properties of all layers precisely. The SDP‐PES dissociates the chemical bonding in the spiro‐MeOTAD and perovskite layer and reduces the TiO2, which causes the chemical analysis to be unreliable. The TCS‐PES revealed a band bending only at the spiro‐MeOTAD/perovskite interface of about 0.7 eV. Both the TCS and SDP‐PES show that the perovskite layer is inhomogeneous and has a higher amount of bromine at the perovskite/TiO2 interface.