TY  - JOUR
A1  - Pranav, Manasi
A1  - Hultzsch, Thomas
A1  - Musiienko, Artem
A1  - Sun, Bowen
A1  - Shukla, Atul
A1  - Jaiser, Frank
A1  - Shoaee, Safa
A1  - Neher, Dieter
T1  - Anticorrelated photoluminescence and free charge generation proves field-assisted exciton dissociation in low-offset PM6:Y5 organic solar cells
JF  - APL materials : high impact open access journal in functional materials science
N2  - Understanding the origin of inefficient photocurrent generation in organic solar cells with low energy offset remains key to realizing high-performance donor-acceptor systems. Here, we probe the origin of field-dependent free-charge generation and photoluminescence in wnon-fullereneacceptor (NFA)-based organic solar cells using the polymer PM6 and the NFA Y5-a non-halogenated sibling to Y6, with a smaller energetic offset to PM6. By performing time-delayed collection field (TDCF) measurements on a variety of samples with different electron transport layers and active layer thickness, we show that the fill factor and photocurrent are limited by field-dependent free charge generation in the bulk of the blend. We also introduce a new method of TDCF called m-TDCF to prove the absence of artifacts from non-geminate recombination of photogenerated and dark charge carriers near the electrodes. We then correlate free charge generation with steady-state photoluminescence intensity and find perfect anticorrelation between these two properties. Through this, we conclude that photocurrent generation in this low-offset system is entirely controlled by the field-dependent dissociation of local excitons into charge-transfer states. (c) 2023 Author(s).
Y1  - 2023
U6  - https://doi.org/10.1063/5.0151580
SN  - 2166-532X
VL  - 11
IS  - 6
PB  - AIP Publishing
CY  - Melville
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  - Ye, Fangyuan
A1  - Zhang, Shuo
A1  - Warby, Jonathan
A1  - Wu, Jiawei
A1  - Gutierrez-Partida, Emilio
A1  - Lang, Felix
A1  - Shah, Sahil
A1  - Saglamkaya, Elifnaz
A1  - Sun, Bowen
A1  - Zu, Fengshuo
A1  - Shoaee, Safa
A1  - Wang, Haifeng
A1  - Stiller, Burkhard
A1  - Neher, Dieter
A1  - Zhu, Wei-Hong
A1  - Stolterfoht, Martin
A1  - Wu, Yongzhen
T1  - Overcoming C-60-induced interfacial recombination in inverted perovskite solar cells by electron-transporting carborane
JF  - Nature Communications
N2  - 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.
Y1  - 2022
U6  - https://doi.org/10.1038/s41467-022-34203-x
SN  - 2041-1723
VL  - 13
IS  - 1
PB  - Nature Publishing Group
CY  - London
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  - Poelking, Carl
A1  - Benduhn, Johannes
A1  - Spoltore, Donato
A1  - Schwarze, Martin
A1  - Roland, Steffen
A1  - Piersimoni, Fortunato
A1  - Neher, Dieter
A1  - Leo, Karl
A1  - Vandewal, Koen
A1  - Andrienko, Denis
T1  - Open-circuit voltage of organic solar cells
BT  - interfacial roughness makes the difference
JF  - Communications physics
N2  - Organic photovoltaics (PV) is an energy-harvesting technology that offers many advantages, such as flexibility, low weight and cost, as well as environmentally benign materials and manufacturing techniques. Despite growth of power conversion efficiencies to around 19 % in the last years, organic PVs still lag behind inorganic PV technologies, mainly due to high losses in open-circuit voltage. Understanding and improving open circuit voltage in organic solar cells is challenging, as it is controlled by the properties of a donor-acceptor interface where the optical excitations are separated into charge carriers. Here, we provide an electrostatic model of a rough donor-acceptor interface and test it experimentally on small molecule PV materials systems. The model provides concise relationships between the open-circuit voltage, photovoltaic gap, charge-transfer state energy, and interfacial morphology. In particular, we show that the electrostatic bias generated across the interface reduces the photovoltaic gap. This negative influence on open-circuit voltage can, however, be circumvented by adjusting the morphology of the donor-acceptor interface. 
Organic solar cells, despite their high power conversion efficiencies, suffer from open circuit voltage losses making them less appealing in terms of applications. Here, the authors, supported with experimental data on small molecule photovoltaic cells, relate open circuit voltage to photovoltaic gap, charge-transfer state energy, and donor-acceptor interfacial morphology.
Y1  - 2022
U6  - https://doi.org/10.1038/s42005-022-01084-x
SN  - 2399-3650
VL  - 5
IS  - 1
PB  - Nature portfolio
CY  - Berlin
ER  - 
TY  - JOUR
A1  - Vollbrecht, Joachim
A1  - Tokmoldin, Nurlan
A1  - Sun, Bowen
A1  - Brus, Viktor V.
A1  - Shoaee, Safa
A1  - Neher, Dieter
T1  - Determination of the charge carrier density in organic solar cells
BT  - a tutorial
JF  - Journal of applied physics
N2  - The increase in the performance of organic solar cells observed over the past few years has reinvigorated the search for a deeper understanding of the loss and extraction processes in this class of device. A detailed knowledge of the density of free charge carriers under different operating conditions and illumination intensities is a prerequisite to quantify the recombination and extraction dynamics. Differential charging techniques are a promising approach to experimentally obtain the charge carrier density under the aforementioned conditions. In particular, the combination of transient photovoltage and photocurrent as well as impedance and capacitance spectroscopy have been successfully used in past studies to determine the charge carrier density of organic solar cells. In this Tutorial, these experimental techniques will be discussed in detail, highlighting fundamental principles, practical considerations, necessary corrections, advantages, drawbacks, and ultimately their limitations. Relevant references introducing more advanced concepts will be provided as well. Therefore, the present Tutorial might act as an introduction and guideline aimed at new prospective users of these techniques as well as a point of reference for more experienced researchers. Published under an exclusive license by AIP Publishing.
KW  - Electrical properties and parameters
KW  - Organic semiconductors
KW  - Solar cells
KW  - Photoconductivity
KW  - Capacitance spectroscopy
Y1  - 2022
U6  - https://doi.org/10.1063/5.0094955
SN  - 0021-8979
SN  - 1089-7550
SN  - 1520-8850
VL  - 131
IS  - 22
PB  - American Institute of Physics
CY  - Melville, NY
ER  - 
TY  - JOUR
A1  - Sun, Bowen
A1  - Sandberg, Oskar
A1  - Neher, Dieter
A1  - Armin, Ardalan
A1  - Shoaee, Safa
T1  - Wave optics of differential absorption spectroscopy in thick-junction organic solar cells
BT  - optical artifacts and correction strategies
JF  - Physical review applied / The American Physical Society
N2  - Differential absorption spectroscopy techniques serve as powerful techniques to study the excited species in organic solar cells. However, it has always been challenging to employ these techniques for characterizing thick-junction organic solar cells, especially when a reflective top contact is involved. In this work, we present a detailed and systematic study on how a combination of the presence of the interference effect and a nonuniform charge-distribution profile, severely manipulates experimental spectra and the decay dynamics. Furthermore, we provide a practical methodology to correct these optical artifacts in differential absorption spectroscopies. The results and the proposed correction method generally apply to all kinds of differential absorption spectroscopy techniques and various thin-film systems, such as organics, perovskites, kesterites, and two-dimensional materials. Notably, it is found that the shape of differential absorption spectra can be strongly distorted, starting from 150-nm active-layer thickness; this matches the thickness range of thick-junction organic solar cells and most perovskite solar cells and needs to be carefully considered in experiments. In addition, the decay dynamics of differential absorption spectra is found to be disturbed by optical artifacts under certain conditions. With the help of the proposed correction formalism, differential spectra and the decay dynamics can be characterized on the full device of thin-film solar cells in transmission mode and yield accurate and reliable results to provide design rules for further progress.
Y1  - 2022
U6  - https://doi.org/10.1103/PhysRevApplied.17.054016
SN  - 2331-7019
VL  - 17
IS  - 5
PB  - American Physical Society
CY  - College Park
ER  - 
TY  - JOUR
A1  - Fritsch, Tobias
A1  - Kurpiers, Jona
A1  - Roland, Steffen
A1  - Tokmoldin, Nurlan
A1  - Shoaee, Safa
A1  - Ferron, Thomas
A1  - Collins, Brian A.
A1  - Janietz, Silvia
A1  - Vandewal, Koen
A1  - Neher, Dieter
T1  - On the interplay between CT and singlet exciton emission in organic solar cells with small driving force and its impact on voltage loss
JF  - Advanced energy materials
N2  - The interplay between free charge carriers, charge transfer (CT) states and singlet excitons (S-1) determines the recombination pathway and the resulting open circuit voltage (V-OC) of organic solar cells. 
By combining a well-aggregated low bandgap polymer with different blend ratios of the fullerenes PCBM and ICBA, the energy of the CT state (E-CT) is varied by 130 meV while leaving the S-1 energy of the polymer (ES1\[{E_{{{\rm{S}}_1}}}\]) unaffected. 
It is found that the polymer exciton dominates the radiative properties of the blend when ECT\[{E_{{\rm{CT}}}}\] approaches ES1\[{E_{{{\rm{S}}_1}}}\], while the V-OC remains limited by the non-radiative decay of the CT state. 
It is concluded that an increasing strength of the exciton in the optical spectra of organic solar cells will generally decrease the non-radiative voltage loss because it lowers the radiative V-OC limit (V-OC,V-rad), but not because it is more emissive. 
The analysis further suggests that electronic coupling between the CT state and the S-1 will not improve the V-OC, but rather reduce the V-OC,V-rad. 
It is anticipated that only at very low CT state absorption combined with a fairly high CT radiative efficiency the solar cell benefit from the radiative properties of the singlet excitons.
KW  - external quantum efficiency
KW  - organic photovoltaics
KW  - ternary blends
KW  - voltage losses
Y1  - 2022
U6  - https://doi.org/10.1002/aenm.202200641
SN  - 1614-6832
SN  - 1614-6840
VL  - 12
IS  - 31
PB  - Wiley-VCH
CY  - Weinheim
ER  - 
TY  - JOUR
A1  - Ye, Fangyuan
A1  - Zhang, Shuo
A1  - Warby, Jonathan
A1  - Wu, Jiawei
A1  - Gutierrez-Partida, Emilio
A1  - Lang, Felix
A1  - Shah, Sahil
A1  - Saglamkaya, Elifnaz
A1  - Sun, Bowen
A1  - Zu, Fengshuo
A1  - Shoai, Safa
A1  - Wang, Haifeng
A1  - Stiller, Burkhard
A1  - Neher, Dieter
A1  - Zhu, Wei-Hong
A1  - Stolterfoht, Martin
A1  - Wu, Yongzhen
T1  - Overcoming C₆₀-induced interfacial recombination in inverted perovskite solar cells by electron-transporting carborane
JF  - Nature Communications
N2  - 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.
Y1  - 2022
U6  - https://doi.org/10.1038/s41467-022-34203-x
SN  - 2041-1723
VL  - 13
PB  - Springer Nature
CY  - London
ER  - 
TY  - JOUR
A1  - Perdigon-Toro, Lorena
A1  - Le Quang Phuong, 
A1  - Eller, Fabian
A1  - Freychet, Guillaume
A1  - Saglamkaya, Elifnaz
A1  - Khan, Jafar
A1  - Wei, Qingya
A1  - Zeiske, Stefan
A1  - Kroh, Daniel
A1  - Wedler, Stefan
A1  - Koehler, Anna
A1  - Armin, Ardalan
A1  - Laquai, Frederic
A1  - Herzig, Eva M.
A1  - Zou, Yingping
A1  - Shoaee, Safa
A1  - Neher, Dieter
T1  - Understanding the role of order in Y-series non-fullerene solar cells to realize high open-circuit voltages
JF  - Advanced energy materials
N2  - Non-fullerene acceptors (NFAs) as used in state-of-the-art organic solar cells feature highly crystalline layers that go along with low energetic disorder. 
Here, the crucial role of energetic disorder in blends of the donor polymer PM6 with two Y-series NFAs, Y6, and N4 is studied. 
By performing temperature-dependent charge transport and recombination studies, a consistent picture of the shape of the density of state distributions for free charges in the two blends is developed, allowing an analytical description of the dependence of the open-circuit voltage V-OC on temperature and illumination intensity. 

Disorder is found to influence the value of the V-OC at room temperature, but also its progression with temperature. Here, the PM6:Y6 blend benefits substantially from its narrower state distributions. 
The analysis also shows that the energy of the equilibrated free charge population is well below the energy of the NFA singlet excitons for both blends and possibly below the energy of the populated charge transfer manifold, indicating a down-hill driving force for free charge formation. 
It is concluded that energetic disorder of charge-separated states has to be considered in the analysis of the photovoltaic properties, even for the more ordered PM6:Y6 blend.
KW  - energetic disorder
KW  - non-fullerene acceptors
KW  - open-circuit voltage
KW  - organic solar cells
Y1  - 2022
U6  - https://doi.org/10.1002/aenm.202103422
SN  - 1614-6832
SN  - 1614-6840
VL  - 12
IS  - 12
PB  - Wiley-VCH
CY  - Weinheim
ER  -