@article{LangKoehnenWarbyetal.2021, author = {Lang, Felix and K{\"o}hnen, Eike and Warby, Jonathan and Xu, Ke and Grischek, Max and Wagner, Philipp and Neher, Dieter and Korte, Lars and Albrecht, Steve and Stolterfoht, Martin}, title = {Revealing fundamental efficiency limits of monolithic perovskite/silicon tandem photovoltaics through subcell characterization}, series = {ACS Energy Letters}, volume = {6}, journal = {ACS Energy Letters}, number = {11}, publisher = {American Chemical Society}, address = {Washington}, issn = {2380-8195}, doi = {10.1021/acsenergylett.1c01783}, pages = {3982 -- 3991}, year = {2021}, abstract = {Perovskite/silicon tandem photovoltaics (PVs) promise to accelerate the decarbonization of our energy systems. Here, we present a thorough subcell diagnosis methodology to reveal deep insights into the practical efficiency limitations of state-of-the-art perovskite/silicon tandem PVs. Our subcell selective intensity-dependent photoluminescence (PL) and injection-dependent electroluminescence (EL) measurements allow independent assessment of pseudo-V-OC and power conversion efficiencies (PCEs) for both subcells. We reveal identical metrics from PL and EL, which implies well-aligned energy levels throughout the entire cell. Relatively large ideality factors and insufficient charge extraction, however, cause each a fill factor penalty of about 6\% (absolute). Using partial device stacks, we then identify significant losses in standard perovskite subcells due to bulk and interfacial recombination. Lastly, we present strategies to minimize these losses using triple halide (CsFAPb(IBrCI)(3)) based perovskites. Our results give helpful feedback for device development and lay the foundation toward advanced perovskite/silicon tandem PVs capable of exceeding 33\% PCE.}, language = {en} } @article{ZuWarbyStolterfohtetal.2021, author = {Zu, Fengshuo and Warby, Jonathan and Stolterfoht, Martin and Li, Jinzhao and Shin, Dongguen and Unger, Eva and Koch, Norbert}, title = {Photoinduced energy-level realignment at interfaces between organic semiconductors and metal-halide perovskites}, series = {Physical review letters}, volume = {127}, journal = {Physical review letters}, number = {24}, publisher = {American Physical Society}, address = {College Park}, issn = {0031-9007}, doi = {10.1103/PhysRevLett.127.246401}, pages = {6}, year = {2021}, abstract = {In contrast to the common conception that the interfacial energy-level alignment is affixed once the interface is formed, we demonstrate that heterojunctions between organic semiconductors and metal-halide perovskites exhibit huge energy-level realignment during photoexcitation. Importantly, the photoinduced level shifts occur in the organic component, including the first molecular layer in direct contact with the perovskite. This is caused by charge-carrier accumulation within the organic semiconductor under illumination and the weak electronic coupling between the junction components.}, language = {en} } @article{YeZhangWarbyetal.2022, author = {Ye, Fangyuan and Zhang, Shuo and Warby, Jonathan and Wu, Jiawei and Gutierrez-Partida, Emilio and Lang, Felix and Shah, Sahil and Saglamkaya, Elifnaz and Sun, Bowen and Zu, Fengshuo and Shoaee, Safa and Wang, Haifeng and Stiller, Burkhard and Neher, Dieter and Zhu, Wei-Hong and Stolterfoht, Martin and Wu, Yongzhen}, title = {Overcoming C-60-induced interfacial recombination in inverted perovskite solar cells by electron-transporting carborane}, series = {Nature Communications}, volume = {13}, journal = {Nature Communications}, number = {1}, publisher = {Nature Publishing Group}, address = {London}, issn = {2041-1723}, doi = {10.1038/s41467-022-34203-x}, pages = {12}, year = {2022}, abstract = {Inverted perovskite solar cells still suffer from significant non-radiative recombination losses at the perovskite surface and across the perovskite/C-60 interface, limiting the future development of perovskite-based single- and multi-junction photovoltaics. Therefore, more effective inter- or transport layers are urgently required. To tackle these recombination losses, we introduce ortho-carborane as an interlayer material that has a spherical molecular structure and a three-dimensional aromaticity. Based on a variety of experimental techniques, we show that ortho-carborane decorated with phenylamino groups effectively passivates the perovskite surface and essentially eliminates the non-radiative recombination loss across the perovskite/C-60 interface with high thermal stability. We further demonstrate the potential of carborane as an electron transport material, facilitating electron extraction while blocking holes from the interface. The resulting inverted perovskite solar cells deliver a power conversion efficiency of over 23\% with a low non-radiative voltage loss of 110mV, and retain >97\% of the initial efficiency after 400h of maximum power point tracking. Overall, the designed carborane based interlayer simultaneously enables passivation, electron-transport and hole-blocking and paves the way toward more efficient and stable perovskite solar cells. Effective transport layers are essential to suppress non-radiative recombination losses. Here, the authors introduce phenylamino-functionalized ortho-carborane as an interfacial layer, and realise inverted perovskite solar cells with efficiency of over 23\% and operational stability of T97=400h.}, language = {en} } @article{PenaCamargoThiesbrummelHempeletal.2022, author = {Pena-Camargo, Francisco and Thiesbrummel, Jarla and Hempel, Hannes and Musiienko, Artem and Le Corre, Vincent M. and Diekmann, Jonas and Warby, Jonathan and Unold, Thomas and Lang, Felix and Neher, Dieter and Stolterfoht, Martin}, title = {Revealing the doping density in perovskite solar cells and its impact on device performance}, series = {Applied physics reviews}, volume = {9}, journal = {Applied physics reviews}, number = {2}, publisher = {AIP Publishing}, address = {Melville}, issn = {1931-9401}, doi = {10.1063/5.0085286}, pages = {11}, year = {2022}, abstract = {Traditional inorganic semiconductors can be electronically doped with high precision. Conversely, there is still conjecture regarding the assessment of the electronic doping density in metal-halide perovskites, not to mention of a control thereof. This paper presents a multifaceted approach to determine the electronic doping density for a range of different lead-halide perovskite systems. Optical and electrical characterization techniques, comprising intensity-dependent and transient photoluminescence, AC Hall effect, transfer-length-methods, and charge extraction measurements were instrumental in quantifying an upper limit for the doping density. The obtained values are subsequently compared to the electrode charge per cell volume under short-circuit conditions ( CUbi/eV), which amounts to roughly 10(16) cm(-3). This figure of merit represents the critical limit below which doping-induced charges do not influence the device performance. The experimental results consistently demonstrate that the doping density is below this critical threshold 10(12) cm(-3), which means << CUbi / e V) for all common lead-based metal-halide perovskites. Nevertheless, although the density of doping-induced charges is too low to redistribute the built-in voltage in the perovskite active layer, mobile ions are present in sufficient quantities to create space-charge-regions in the active layer, reminiscent of doped pn-junctions. These results are well supported by drift-diffusion simulations, which confirm that the device performance is not affected by such low doping densities.}, language = {en} } @article{LeCorreDiekmannPenaCamargoetal.2022, author = {Le Corre, Vincent M. and Diekmann, Jonas and Pe{\~n}a-Camargo, Francisco and Thiesbrummel, Jarla and Tokmoldin, Nurlan and Gutierrez-Partida, Emilio and Peters, Karol Pawel and Perdig{\´o}n-Toro, Lorena and Futscher, Moritz H. and Lang, Felix and Warby, Jonathan and Snaith, Henry J. and Neher, Dieter and Stolterfoht, Martin}, title = {Quantification of efficiency losses due to mobile ions in Perovskite solar cells via fast hysteresis measurements}, series = {Solar RRL}, volume = {6}, journal = {Solar RRL}, number = {4}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {2367-198X}, doi = {10.1002/solr.202100772}, pages = {10}, year = {2022}, abstract = {Perovskite semiconductors differ from most inorganic and organic semiconductors due to the presence of mobile ions in the material. Although the phenomenon is intensively investigated, important questions such as the exact impact of the mobile ions on the steady-state power conversion efficiency (PCE) and stability remain. Herein, a simple method is proposed to estimate the efficiency loss due to mobile ions via "fast-hysteresis" measurements by preventing the perturbation of mobile ions out of their equilibrium position at fast scan speeds (approximate to 1000 V s(-1)). The "ion-free" PCE is between 1\% and 3\% higher than the steady-state PCE, demonstrating the importance of ion-induced losses, even in cells with low levels of hysteresis at typical scan speeds (approximate to 100mv s(-1)). The hysteresis over many orders of magnitude in scan speed provides important information on the effective ion diffusion constant from the peak hysteresis position. The fast-hysteresis measurements are corroborated by transient charge extraction and capacitance measurements and numerical simulations, which confirm the experimental findings and provide important insights into the charge carrier dynamics. The proposed method to quantify PCE losses due to field screening induced by mobile ions clarifies several important experimental observations and opens up a large range of future experiments.}, language = {en} } @article{GrischekCaprioglioZhangetal.2022, author = {Grischek, Max and Caprioglio, Pietro and Zhang, Jiahuan and Pena-Camargo, Francisco and Sveinbjornsson, Kari and Zu, Fengshuo and Menzel, Dorothee and Warby, Jonathan and Li, Jinzhao and Koch, Norbert and Unger, Eva and Korte, Lars and Neher, Dieter and Stolterfoht, Martin and Albrecht, Steve}, title = {Efficiency Potential and Voltage Loss of Inorganic CsPbI2Br Perovskite Solar Cells}, series = {Solar RRL}, volume = {6}, journal = {Solar RRL}, number = {11}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {2367-198X}, doi = {10.1002/solr.202200690}, pages = {12}, year = {2022}, abstract = {Inorganic perovskite solar cells show excellent thermal stability, but the reported power conversion efficiencies are still lower than for organic-inorganic perovskites. This is mainly caused by lower open-circuit voltages (V(OC)s). Herein, the reasons for the low V-OC in inorganic CsPbI2Br perovskite solar cells are investigated. Intensity-dependent photoluminescence measurements for different layer stacks reveal that n-i-p and p-i-n CsPbI2Br solar cells exhibit a strong mismatch between quasi-Fermi level splitting (QFLS) and V-OC. Specifically, the CsPbI2Br p-i-n perovskite solar cell has a QFLS-e center dot V-OC mismatch of 179 meV, compared with 11 meV for a reference cell with an organic-inorganic perovskite of similar bandgap. On the other hand, this study shows that the CsPbI2Br films with a bandgap of 1.9 eV have a very low defect density, resulting in an efficiency potential of 20.3\% with a MeO-2PACz hole-transporting layer and 20.8\% on compact TiO2. Using ultraviolet photoelectron spectroscopy measurements, energy level misalignment is identified as a possible reason for the QFLS-e center dot V-OC mismatch and strategies for overcoming this V-OC limitation are discussed. This work highlights the need to control the interfacial energetics in inorganic perovskite solar cells, but also gives promise for high efficiencies once this issue is resolved.}, language = {en} } @article{WarbyZuZeiskeetal.2022, author = {Warby, Jonathan and Zu, Fengshuo and Zeiske, Stefan and Gutierrez-Partida, Emilio and Frohloff, Lennart and Kahmann, Simon and Frohna, Kyle and Mosconi, Edoardo and Radicchi, Eros and Lang, Felix and Shah, Sahil and Pena-Camargo, Francisco and Hempel, Hannes and Unold, Thomas and Koch, Norbert and Armin, Ardalan and De Angelis, Filippo and Stranks, Samuel D. and Neher, Dieter and Stolterfoht, Martin}, title = {Understanding performance limiting interfacial recombination in pin Perovskite solar cells}, series = {Advanced energy materials}, volume = {12}, journal = {Advanced energy materials}, number = {12}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {1614-6832}, doi = {10.1002/aenm.202103567}, pages = {10}, year = {2022}, abstract = {Perovskite semiconductors are an attractive option to overcome the limitations of established silicon based photovoltaic (PV) technologies due to their exceptional opto-electronic properties and their successful integration into multijunction cells. However, the performance of single- and multijunction cells is largely limited by significant nonradiative recombination at the perovskite/organic electron transport layer junctions. In this work, the cause of interfacial recombination at the perovskite/C-60 interface is revealed via a combination of photoluminescence, photoelectron spectroscopy, and first-principle numerical simulations. It is found that the most significant contribution to the total C-60-induced recombination loss occurs within the first monolayer of C-60, rather than in the bulk of C-60 or at the perovskite surface. The experiments show that the C-60 molecules act as deep trap states when in direct contact with the perovskite. It is further demonstrated that by reducing the surface coverage of C-60, the radiative efficiency of the bare perovskite layer can be retained. The findings of this work pave the way toward overcoming one of the most critical remaining performance losses in perovskite solar cells.}, language = {en} } @article{YeZhangWarbyetal.2022, author = {Ye, Fangyuan and Zhang, Shuo and Warby, Jonathan and Wu, Jiawei and Gutierrez-Partida, Emilio and Lang, Felix and Shah, Sahil and Saglamkaya, Elifnaz and Sun, Bowen and Zu, Fengshuo and Shoai, Safa and Wang, Haifeng and Stiller, Burkhard and Neher, Dieter and Zhu, Wei-Hong and Stolterfoht, Martin and Wu, Yongzhen}, title = {Overcoming C₆₀-induced interfacial recombination in inverted perovskite solar cells by electron-transporting carborane}, series = {Nature Communications}, volume = {13}, journal = {Nature Communications}, number = {1}, publisher = {Springer Nature}, address = {London}, issn = {2041-1723}, doi = {10.1038/s41467-022-34203-x}, pages = {12}, year = {2022}, abstract = {Inverted perovskite solar cells still suffer from significant non-radiative recombination losses at the perovskite surface and across the perovskite/C₆₀ interface, limiting the future development of perovskite-based single- and multi-junction photovoltaics. Therefore, more effective inter- or transport layers are urgently required. To tackle these recombination losses, we introduce ortho-carborane as an interlayer material that has a spherical molecular structure and a three-dimensional aromaticity. Based on a variety of experimental techniques, we show that ortho-carborane decorated with phenylamino groups effectively passivates the perovskite surface and essentially eliminates the non-radiative recombination loss across the perovskite/C₆₀ interface with high thermal stability. We further demonstrate the potential of carborane as an electron transport material, facilitating electron extraction while blocking holes from the interface. The resulting inverted perovskite solar cells deliver a power conversion efficiency of over 23\% with a low non-radiative voltage loss of 110 mV, and retain >97\% of the initial efficiency after 400 h of maximum power point tracking. Overall, the designed carborane based interlayer simultaneously enables passivation, electron-transport and hole-blocking and paves the way toward more efficient and stable perovskite solar cells.}, language = {en} }