TY - CHAP A1 - Kot, Małgorzata A1 - Kegelmann, Lukas A1 - Kus, Peter A1 - Tsud, Nataliya A1 - Matolínová, Iva A1 - Albrecht, Steve A1 - Matolin, Vladimir A1 - Schmeißer, Dieter T1 - Room temperature atomic layer deposition for perovskite solar cells T2 - Verhandlungen der Deutschen Physikalischen Gesellschaft, Reihe 6, Band 53,3 N2 - After few years of efficiency driven research on perovskite solar cells, the focus now is shifting to understand the underlying processes governing the high efficiency and also to obtain long-term stable devices. Among various deposition methods, atomic layer deposition (ALD) may represent one of the best options, being possible to coat substrates in a very efficient way and at very low temperatures. In our previous work [1] we reported that the efficiency of the solar cell containing aged perovskite film can be enhanced twice while covering the perovskite with a thin ALD alumina film at room temperature. In this work, the chemical, electronic and morphological properties of the fresh perovskite film treated by ALD pulses of the trimethylaluminium and water at room temperature investigated using X-ray Photoelectron Spectroscopy and Field Emission Scanning Electron Microscopy will be discused and correlated with the solar cells performance and stability. [1] M. Kot et al., ChemSusChem 2016, 9, 3401. KW - Perovskite solar cells KW - atomic layer deposition KW - X-Ray photoelectron spectroscopy (XPS) KW - atomic force microscopy KW - field emission scanning electron microscopy KW - photo-conversion efficiency Y1 - 2018 SN - 0420-0195 SP - S. 174 PB - Deutsche Physikalische Gesellschaft CY - Bad Honnef ER - TY - GEN A1 - Kot, Małgorzata A1 - Kegelmann, Lukas A1 - Das, Chittaranjan A1 - Kus, Peter A1 - Tsud, Nataliya A1 - Matolínová, Iva A1 - Albrecht, Steve A1 - Matolin, Vladimir A1 - Schmeißer, Dieter T1 - Room temperature atomic layer deposited Al₂O₃ improves perovskite solar cells efficiency over time T2 - ChemSusChem N2 - Electrical characterisation of perovskite solar cells consisting of room-temperature atomic-layer-deposited aluminium oxide (RT-ALD-Al₂O₃) film on top of a methyl ammonium lead triiodide (CH₃NH₃PbI₃) absorber showed excellent stability of the power conversion efficiency (PCE) over along time. Under the same environmental conditions (for 355 d), the average PCE of solar cells without the ALD layer decreased from 13.6 to 9.6 %, whereas that of solar cells containing 9 ALD cycles of depositing RT-ALD-Al₂O₃on top of CH₃NH₃PbI₃ increased from 9.4 to 10.8 %. Spectromicroscopic investigations of the ALD/perovskite interface revealed that the maximum PCE with the ALD layer is obtained when the so-called perovskite cleaning process induced by ALD precursors is complete. The PCE enhancement over time is probably related to a self-healing process induced by the RT-ALD-Al₂O₃ film. This work may provide a new direction for further improving the long-term stability and performance of perovskite solar cells. KW - Perovskite Solar Cells (PSCs) KW - Atomic layer deposition (ALD) KW - long time stabilty KW - X-Ray photoelectron spectroscopy (XPS) KW - Field-emission scanning electron microscopy (FESEM) Y1 - 2018 U6 - https://doi.org/10.1002/cssc.201801434 SN - 1864-5631 SN - 1864-564X VL - 11 IS - 20 SP - 3640 EP - 3648 ER - TY - GEN A1 - Schmeißer, Dieter A1 - Henkel, Karsten A1 - Pożarowska, Emilia A1 - Kegelmann, Lukas A1 - Tsud, Nataliya A1 - Kot, Małgorzata T1 - Point Defect-Mediated Interface Formation and Appearance of a Cooper Minimum for AlOₓ Atomic-Layer-Deposited Films on CH₃NH₃PbI₃ T2 - The Journal of Physical Chemistry. C N2 - We report on the interaction of CH₃NH₃PbI₃ substrates with AlOx films prepared by atomic layer deposition at room temperature. We use synchrotron radiation-based photoemission spectroscopy and study the Pb 4f, I 3d, and Al 2p core levels as well as the corresponding valence band states (Pb 5d and O 2p). A Cooper minimum is observed for both the Pb 5d and O 2p states, and it indicates that the bonding at the interface must be covalent. We focus on the electronic properties of the substrate and its interface and identify a delicate charge balance between polaronic and excitonic states in MAPI and AlOₓ. The perovskite vacancy sites, identified by changes in the core-level intensities, mediate the charge balance and covalent interaction. KW - Resonant photoelectron spectroscopy KW - Al₂O₃-CH₃NH₃PbI₃ interaction KW - Cooper minimum KW - point defects in CH₃NH₃PbI₃ KW - electronic structure of CH₃NH₃PbI₃ Y1 - 2019 U6 - https://doi.org/10.1021/acs.jpcc.9b05282 SN - 1932-7447 SN - 1932-7455 VL - 123 IS - 38 SP - 23352 EP - 23360 ER - TY - GEN A1 - Kot, Małgorzata A1 - Henkel, Karsten A1 - Müller, Klaus A1 - Kegelmann, Lukas A1 - Albrecht, Steve A1 - Tsud, Nataliya A1 - Kús, Peter A1 - Matolinová, Iva A1 - Schmeißer, Dieter T1 - Al2O3-Atomic Layer Deposited Films on CH3NH3PbI3 : Intrinsic Defects and Passivation Mechanisms T2 - Energy Technology , The Journal of Physical Chemistry C N2 - The initial interaction of atomic layer deposited films of Al2O3 at room temperature on CH3NH3PbI3 (MAPI) films is studied. Synchrotron radiation–based photoelectron spectroscopy is applied to analyze the initial changes in the Al-derived features by comparing samples with different Al2O3 film thicknesses. It is found that polarons and excitons, both intrinsic defects of Al2O3, play a key role in the interface formation. The polaronic states uptake a charge from the MAPI substrate. This charge is transferred to and stabilized in the excitonic state of Al2O3 which is assigned to predominately tetrahedral coordinated Al sites. This charge transfer is initiated by vacancies present in the MAPI substrate and stabilizes a covalent bonding at the Al2O3–MAPI interface but also causes a roughening of the interface which may lead to the formation of grain boundaries. On top of the rough interface, 2D Al2O3 clusters with an increasing number of octahedrally coordinated Al—O bonds grow, and with increasing Al2O3 coverage, they introduce self-healing of the structural defects. KW - charge donation and transfer cycles KW - covalent interfaces KW - defect monitoring KW - model of Al2O3–CH3NH3PbI3 interactions KW - resonant photoelectron spectroscopy Y1 - 2019 U6 - https://doi.org/10.1002/ente.201900975 SN - 2194-4288 SN - 2194-4296 VL - 7 IS - 11 ER -