TY  - JOUR
A1  - Zhang, Shanshan
A1  - Hosseini, Seyed Mehrdad
A1  - Gunder, Rene
A1  - Petsiuk, Andrei
A1  - Caprioglio, Pietro
A1  - Wolff, Christian Michael
A1  - Shoaee, Safa
A1  - Meredith, Paul
A1  - Schorr, Susan
A1  - Unold, Thomas
A1  - Burn, Paul L.
A1  - Neher, Dieter
A1  - Stolterfoht, Martin
T1  - The Role of Bulk and Interface Recombination in High-Efficiency Low-Dimensional Perovskite Solar Cells
JF  - Advanced materials
N2  - 2D Ruddlesden-Popper perovskite (RPP) solar cells have excellent environmental stability. However, the power conversion efficiency (PCE) of RPP cells remains inferior to 3D perovskite-based cells. Herein, 2D (CH3(CH2)(3)NH3)(2)(CH3NH3)(n-1)PbnI3n+1 perovskite cells with different numbers of [PbI6](4-) sheets (n = 2-4) are analyzed. Photoluminescence quantum yield (PLQY) measurements show that nonradiative open-circuit voltage (V-OC) losses outweigh radiative losses in materials with n > 2. The n = 3 and n = 4 films exhibit a higher PLQY than the standard 3D methylammonium lead iodide perovskite although this is accompanied by increased interfacial recombination at the top perovskite/C-60 interface. This tradeoff results in a similar PLQY in all devices, including the n = 2 system where the perovskite bulk dominates the recombination properties of the cell. In most cases the quasi-Fermi level splitting matches the device V-OC within 20 meV, which indicates minimal recombination losses at the metal contacts. The results show that poor charge transport rather than exciton dissociation is the primary reason for the reduction in fill factor of the RPP devices. Optimized n = 4 RPP solar cells had PCEs of 13% with significant potential for further improvements.
KW  - 2D perovskites
KW  - interface recombination
KW  - perovskite solar cells
KW  - photoluminescence
KW  - V-OC loss
Y1  - 2019
U6  - https://doi.org/10.1002/adma.201901090
SN  - 0935-9648
SN  - 1521-4095
VL  - 31
IS  - 30
PB  - Wiley-VCH
CY  - Weinheim
ER  - 
TY  - JOUR
A1  - Stolterfoht, Martin
A1  - Caprioglio, Pietro
A1  - Wolff, Christian Michael
A1  - Marquez, Jose A.
A1  - Nordmann, Joleik
A1  - Zhang, Shanshan
A1  - Rothhardt, Daniel
A1  - Hörmann, Ulrich
A1  - Amir, Yohai
A1  - Redinger, Alex
A1  - Kegelmann, Lukas
A1  - Zu, Fengshuo
A1  - Albrecht, Steve
A1  - Koch, Norbert
A1  - Kirchartz, Thomas
A1  - Saliba, Michael
A1  - Unold, Thomas
A1  - Neher, Dieter
T1  - The impact of energy alignment and interfacial recombination on the internal and external open-circuit voltage of perovskite solar cells
JF  - Energy & environmental science
N2  - Charge transport layers (CTLs) are key components of diffusion controlled perovskite solar cells, however, they can induce additional non-radiative recombination pathways which limit the open circuit voltage (V-OC) of the cell. In order to realize the full thermodynamic potential of the perovskite absorber, both the electron and hole transport layer (ETL/HTL) need to be as selective as possible. By measuring the photoluminescence yield of perovskite/CTL heterojunctions, we quantify the non-radiative interfacial recombination currents in pin- and nip-type cells including high efficiency devices (21.4%). Our study comprises a wide range of commonly used CTLs, including various hole-transporting polymers, spiro-OMeTAD, metal oxides and fullerenes. We find that all studied CTLs limit the V-OC by inducing an additional non-radiative recombination current that is in most cases substantially larger than the loss in the neat perovskite and that the least-selective interface sets the upper limit for the V-OC of the device. Importantly, the V-OC equals the internal quasi-Fermi level splitting (QFLS) in the absorber layer only in high efficiency cells, while in poor performing devices, the V-OC is substantially lower than the QFLS. Using ultraviolet photoelectron spectroscopy and differential charging capacitance experiments we show that this is due to an energy level mis-alignment at the p-interface. The findings are corroborated by rigorous device simulations which outline important considerations to maximize the V-OC. This work highlights that the challenge to suppress non-radiative recombination losses in perovskite cells on their way to the radiative limit lies in proper energy level alignment and in suppression of defect recombination at the interfaces.
Y1  - 2019
U6  - https://doi.org/10.1039/c9ee02020a
SN  - 1754-5692
SN  - 1754-5706
VL  - 12
IS  - 9
SP  - 2778
EP  - 2788
PB  - Royal Society of Chemistry
CY  - Cambridge
ER  -