05 Fakultät Informatik, Elektrotechnik und Informationstechnik
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Item Open Access 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, MałgorzataA 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.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 Photoelectrochemical water‐splitting using CuO‐based electrodes for hydrogen production : a review(2021) Siavash Moakhar, Roozbeh; Hosseini‐Hosseinabad, Seyed Morteza; Masudy‐Panah, Saeid; Seza, Ashkan; Jalali, Mahsa; Fallah‐Arani, Hesam; Dabir, Fatemeh; Gholipour, Somayeh; Abdi, Yaser; Bagheri‐Hariri, Mohiedin; Riahi‐Noori, Nastaran; Lim, Yee‐Fun; Hagfeldt, Anders; Saliba, MichaelThe cost‐effective, robust, and efficient electrocatalysts for photoelectrochemical (PEC) water‐splitting has been extensively studied over the past decade to address a solution for the energy crisis. The interesting physicochemical properties of CuO have introduced this promising photocathodic material among the few photocatalysts with a narrow bandgap. This photocatalyst has a high activity for the PEC hydrogen evolution reaction (HER) under simulated sunlight irradiation. Here, the recent advancements of CuO‐based photoelectrodes, including undoped CuO, doped CuO, and CuO composites, in the PEC water‐splitting field, are comprehensively studied. Moreover, the synthesis methods, characterization, and fundamental factors of each classification are discussed in detail. Apart from the exclusive characteristics of CuO‐based photoelectrodes, the PEC properties of CuO/2D materials, as groups of the growing nanocomposites in photocurrent‐generating devices, are discussed in separate sections. Regarding the particular attention paid to the CuO heterostructure photocathodes, the PEC water splitting application is reviewed and the properties of each group such as electronic structures, defects, bandgap, and hierarchical structures are critically assessed.Item Open Access Characterizing the influence of charge extraction layers on the performance of triple‐cation perovskite solar cells(2023) Siekmann, Johanna; Kulkarni, Ashish; Akel, Samah; Klingebiel, Benjamin; Saliba, Michael; Rau, Uwe; Kirchartz, ThomasSelecting suitable charge transport layers and suppressing non-radiative recombination at interfaces with the absorber layer is vital for maximizing the efficiency of halide perovskite solar cells. In this study, high-quality perovskite thin films and devices are fabricated with different fullerene-based electron transport layers and different self-assembled monolayers as hole transport layers. Then, a comparative study of a significant variety of different electrical, optical, and photoemission-based characterization techniques is performed to quantify the properties of the solar cells, individual layers, and, importantly, the interfaces between them. In addition, the limitations and problems of the different measurements, the insights gained by combining different methods, and the different strategies for extracting information from the experimental raw data, are highlighted.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.