TY  - JOUR
A1  - Stolterfoht, Martin
A1  - Wolff, Christian Michael
A1  - Amir, Yohai
A1  - Paulke, Andreas
A1  - Perdigón-Toro, Lorena
A1  - Caprioglio, Pietro
A1  - Neher, Dieter
T1  - Approaching the fill factor Shockley-Queisser limit in stable, dopant-free triple cation perovskite solar cells
JF  - Energy & Environmental Science
N2  - Perovskite solar cells now compete with their inorganic counterparts in terms of power conversion efficiency, not least because of their small open-circuit voltage (V-OC) losses. A key to surpass traditional thin-film solar cells is the fill factor (FF). Therefore, more insights into the physical mechanisms that define the bias dependence of the photocurrent are urgently required. In this work, we studied charge extraction and recombination in efficient triple cation perovskite solar cells with undoped organic electron/hole transport layers (ETL/HTL). Using integral time of flight we identify the transit time through the HTL as the key figure of merit for maximizing the fill factor (FF) and efficiency. Complementarily, intensity dependent photocurrent and V-OC measurements elucidate the role of the HTL on the bias dependence of non-radiative and transport-related loss channels. We show that charge transport losses can be completely avoided under certain conditions, yielding devices with FFs of up to 84%. Optimized cells exhibit power conversion efficiencies of above 20% for 6 mm(2) sized pixels and 18.9% for a device area of 1 cm(2). These are record efficiencies for hybrid perovskite devices with dopant-free transport layers, highlighting the potential of this device technology to avoid charge-transport limitations and to approach the Shockley-Queisser limit.
Y1  - 2017
U6  - https://doi.org/10.1039/c7ee00899f
SN  - 1754-5692
SN  - 1754-5706
VL  - 10
SP  - 1530
EP  - 1539
PB  - Royal Society of Chemistry
CY  - Cambridge
ER  - 
TY  - JOUR
A1  - Wang, Qiong
A1  - Smith, Joel A.
A1  - Skroblin, Dieter
A1  - Steele, Julian A.
A1  - Wolff, Christian Michael
A1  - Caprioglio, Pietro
A1  - Stolterfoht, Martin
A1  - Köbler, Hans
A1  - Turren-Cruz, Silver-Hamill
A1  - Li, Meng
A1  - Gollwitzer, Christian
A1  - Neher, Dieter
A1  - Abate, Antonio
T1  - Managing phase purities and crystal orientation for high-performance and photostable cesium lead halide perovskite solar cells
JF  - Solar RRL
N2  - Inorganic perovskites with cesium (Cs+) as the cation have great potential as photovoltaic materials if their phase purity and stability can be addressed. Herein, a series of inorganic perovskites is studied, and it is found that the power conversion efficiency of solar cells with compositions CsPbI1.8Br1.2, CsPbI2.0Br1.0, and CsPbI2.2Br0.8 exhibits a high dependence on the initial annealing step that is found to significantly affect the crystallization and texture behavior of the final perovskite film. At its optimized annealing temperature, CsPbI1.8Br1.2 exhibits a pure orthorhombic phase and only one crystal orientation of the (110) plane. Consequently, this allows for the best efficiency of up to 14.6% and the longest operational lifetime, T-S80, of approximate to 300 h, averaged of over six solar cells, during the maximum power point tracking measurement under continuous light illumination and nitrogen atmosphere. This work provides essential progress on the enhancement of photovoltaic performance and stability of CsPbI3 - xBrx perovskite solar cells.
KW  - cesium lead halides
KW  - crystal orientation
KW  - inorganic perovskites
KW  - ISOS-L-1I protocol
KW  - phase purity
KW  - photostability
Y1  - 2020
VL  - 4
IS  - 9
PB  - WILEY-VCH
CY  - Weinheim
ER  - 
TY  - JOUR
A1  - Stolterfoht, Martin
A1  - Lang, Felix
T1  - All-perovskite tandems get flexible
JF  - Nature energy
N2  - Flexible all-perovskite tandem photovoltaics open up new opportunities for application compared to rigid devices, yet their performance lags behind. Now, researchers show that molecule-bridged interfaces mitigate charge recombination and crack formation, improving the efficiency and mechanical reliability of flexible devices.
Y1  - 2022
U6  - https://doi.org/10.1038/s41560-022-01087-6
SN  - 2058-7546
VL  - 7
IS  - 8
SP  - 688
EP  - 689
PB  - Nature Publishing Group
CY  - London
ER  - 
TY  - GEN
A1  - Saliba, Michael
A1  - Stolterfoht, Martin
A1  - Wolff, Christian Michael
A1  - Neher, Dieter
A1  - Abate, Antonio
T1  - Measuring aging stability of perovskite solar cells
T2  - Joule
Y1  - 2018
U6  - https://doi.org/10.1016/j.joule.2018.05.005
SN  - 2542-4351
VL  - 2
IS  - 6
SP  - 1019
EP  - 1024
PB  - Cell Press
CY  - Cambridge
ER  - 
TY  - JOUR
A1  - Stolterfoht, Martin
A1  - Grischek, Max
A1  - Caprioglio, Pietro
A1  - Wolff, Christian Michael
A1  - Gutierrez-Partida, Emilio
A1  - Peña-Camargo, Francisco
A1  - Rothhardt, Daniel
A1  - Zhang, Shanshan
A1  - Raoufi, Meysam
A1  - Wolansky, Jakob
A1  - Abdi-Jalebi, Mojtaba
A1  - Stranks, Samuel D.
A1  - Albrecht, Steve
A1  - Kirchartz, Thomas
A1  - Neher, Dieter
T1  - How to quantify the efficiency potential of neat perovskite films
BT  - Perovskite semiconductors with an implied efficiency exceeding 28%
JF  - Advanced Materials
N2  - Perovskite photovoltaic (PV) cells have demonstrated power conversion efficiencies (PCE) that are close to those of monocrystalline silicon cells; however, in contrast to silicon PV, perovskites are not limited by Auger recombination under 1-sun illumination. Nevertheless, compared to GaAs and monocrystalline silicon PV, perovskite cells have significantly lower fill factors due to a combination of resistive and non-radiative recombination losses. This necessitates a deeper understanding of the underlying loss mechanisms and in particular the ideality factor of the cell. By measuring the intensity dependence of the external open-circuit voltage and the internal quasi-Fermi level splitting (QFLS), the transport resistance-free efficiency of the complete cell as well as the efficiency potential of any neat perovskite film with or without attached transport layers are quantified. Moreover, intensity-dependent QFLS measurements on different perovskite compositions allows for disentangling of the impact of the interfaces and the perovskite surface on the non-radiative fill factor and open-circuit voltage loss. It is found that potassium-passivated triple cation perovskite films stand out by their exceptionally high implied PCEs > 28%, which could be achieved with ideal transport layers. Finally, strategies are presented to reduce both the ideality factor and transport losses to push the efficiency to the thermodynamic limit.
KW  - non-radiative interface recombination
KW  - perovskite solar cells
KW  - photoluminescence
Y1  - 2020
U6  - https://doi.org/10.1002/adma.202000080
SN  - 0935-9648
SN  - 1521-4095
VL  - 32
IS  - 17
SP  - 1
EP  - 10
PB  - Wiley-VCH
CY  - Weinheim
ER  - 
TY  - JOUR
A1  - Zeiske, Stefan
A1  - Sandberg, Oskar J.
A1  - Zarrabi, Nasim
A1  - Wolff, Christian Michael
A1  - Raoufi, Meysam
A1  - Peña-Camargo, Francisco
A1  - Gutierrez-Partida, Emilio
A1  - Meredith, Paul
A1  - Stolterfoht, Martin
A1  - Armin, Ardalan
T1  - Static disorder in lead halide perovskites
JF  - The journal of physical chemistry letters
N2  - In crystalline and amorphous semiconductors, the temperature-dependent Urbach energy can be determined from the inverse slope of the logarithm of the absorption spectrum and reflects the static and dynamic energetic disorder. Using recent advances in the sensitivity of photocurrent spectroscopy methods, we elucidate the temperature-dependent Urbach energy in lead halide perovskites containing different numbers of cation components. We find Urbach energies at room temperature to be 13.0 +/- 1.0, 13.2 +/- 1.0, and 13.5 +/- 1.0 meV for single, double, and triple cation perovskite. Static, temperature-independent contributions to the Urbach energy are found to be as low as 5.1 ?+/- 0.5, 4.7 +/- 0.3, and 3.3 +/- 0.9 meV for the same systems. Our results suggest that, at a low temperature, the dominant static disorder in perovskites is derived from zero-point phonon energy rather than structural disorder. This is unusual for solution-processed semiconductors but broadens the potential application of perovskites further to quantum electronics and devices.
KW  - Cations
KW  - External quantum efficiency
KW  - Perovskites
KW  - Solar cells
KW  - Solar energy
Y1  - 2022
U6  - https://doi.org/10.1021/acs.jpclett.2c01652
SN  - 1948-7185
VL  - 13
IS  - 31
SP  - 7280
EP  - 7285
PB  - American Chemical Society
CY  - Washington
ER  - 
TY  - JOUR
A1  - Le Corre, Vincent M.
A1  - Diekmann, Jonas
A1  - Peña-Camargo, Francisco
A1  - Thiesbrummel, Jarla
A1  - Tokmoldin, Nurlan
A1  - Gutierrez-Partida, Emilio
A1  - Peters, Karol Pawel
A1  - Perdigón-Toro, Lorena
A1  - Futscher, Moritz H.
A1  - Lang, Felix
A1  - Warby, Jonathan
A1  - Snaith, Henry J.
A1  - Neher, Dieter
A1  - Stolterfoht, Martin
T1  - Quantification of efficiency losses due to mobile ions in Perovskite solar cells via fast hysteresis measurements
JF  - Solar RRL
N2  - 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.
KW  - hysteresis
KW  - mobile ions
KW  - perovskite solar cells
Y1  - 2021
U6  - https://doi.org/10.1002/solr.202100772
SN  - 2367-198X
VL  - 6
IS  - 4
PB  - Wiley-VCH
CY  - Weinheim
ER  - 
TY  - JOUR
A1  - Zu, Fengshuo
A1  - Warby, Jonathan
A1  - Stolterfoht, Martin
A1  - Li, Jinzhao
A1  - Shin, Dongguen
A1  - Unger, Eva
A1  - Koch, Norbert
T1  - Photoinduced energy-level realignment at interfaces between organic semiconductors and metal-halide perovskites
JF  - Physical review letters
N2  - 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.
Y1  - 2021
U6  - https://doi.org/10.1103/PhysRevLett.127.246401
SN  - 0031-9007
SN  - 1079-7114
VL  - 127
IS  - 24
PB  - American Physical Society
CY  - College Park
ER  - 
TY  - JOUR
A1  - Grischek, Max
A1  - Caprioglio, Pietro
A1  - Zhang, Jiahuan
A1  - Pena-Camargo, Francisco
A1  - Sveinbjornsson, Kari
A1  - Zu, Fengshuo
A1  - Menzel, Dorothee
A1  - Warby, Jonathan H.
A1  - Li, Jinzhao
A1  - Koch, Norbert
A1  - Unger, Eva
A1  - Korte, Lars
A1  - Neher, Dieter
A1  - Stolterfoht, Martin
A1  - Albrecht, Steve
T1  - Efficiency Potential and Voltage Loss of Inorganic CsPbI2Br Perovskite Solar Cells
JF  - Solar RRL
N2  - 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.
KW  - CsPbI2Br
KW  - efficiency potentials
KW  - inorganic perovskites
KW  - photoluminescence
KW  - solar cells
KW  - voltage losses
Y1  - 2022
U6  - https://doi.org/10.1002/solr.202200690
SN  - 2367-198X
VL  - 6
IS  - 11
PB  - Wiley-VCH
CY  - Weinheim
ER  - 
TY  - JOUR
A1  - Lang, Felix
A1  - Köhnen, Eike
A1  - Warby, Jonathan
A1  - Xu, Ke
A1  - Grischek, Max
A1  - Wagner, Philipp
A1  - Neher, Dieter
A1  - Korte, Lars
A1  - Albrecht, Steve
A1  - Stolterfoht, Martin
T1  - Revealing fundamental efficiency limits of monolithic perovskite/silicon tandem photovoltaics through subcell characterization
JF  - ACS Energy Letters
N2  - 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.
Y1  - 2021
U6  - https://doi.org/10.1021/acsenergylett.1c01783
SN  - 2380-8195
VL  - 6
IS  - 11
SP  - 3982
EP  - 3991
PB  - American Chemical Society
CY  - Washington
ER  -