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  - García-Benito, Inés
A1  - Quarti, Claudio
A1  - Queloz, Valentin I. E.
A1  - Hofstetter, Yvonne J.
A1  - Becker-Koch, David
A1  - Caprioglio, Pietro
A1  - Neher, Dieter
A1  - Orlandi, Simonetta
A1  - Cavazzini, Marco
A1  - Pozzi, Gianluca
A1  - Even, Jacky
A1  - Nazeeruddin, Mohammad Khaja
A1  - Vaynzof, Yana
A1  - Grancini, Giulia
T1  - Fluorination of organic spacer impacts on the structural and optical response of 2D perovskites
JF  - Frontiers in Chemistry
N2  - Low-dimensional hybrid perovskites have triggered significant research interest due to their intrinsically tunable optoelectronic properties and technologically relevant material stability. In particular, the role of the organic spacer on the inherent structural and optical features in two-dimensional (2D) perovskites is paramount for material optimization. To obtain a deeper understanding of the relationship between spacers and the corresponding 2D perovskite film properties, we explore the influence of the partial substitution of hydrogen atoms by fluorine in an alkylammonium organic cation, resulting in (Lc)(2)PbI4 and (Lf)(2)PbI4 2D perovskites, respectively. Consequently, optical analysis reveals a clear 0.2 eV blue-shift in the excitonic position at room temperature. This result can be mainly attributed to a band gap opening, with negligible effects on the exciton binding energy. According to Density Functional Theory (DFT) calculations, the band gap increases due to a larger distortion of the structure that decreases the atomic overlap of the wavefunctions and correspondingly bandwidth of the valence and conduction bands. In addition, fluorination impacts the structural rigidity of the 2D perovskite, resulting in a stable structure at room temperature and the absence of phase transitions at a low temperature, in contrast to the widely reported polymorphism in some non-fluorinated materials that exhibit such a phase transition. This indicates that a small perturbation in the material structure can strongly influence the overall structural stability and related phase transition of 2D perovskites, making them more robust to any phase change. This work provides key information on how the fluorine content in organic spacer influence the structural distortion of 2D perovskites and their optical properties which possess remarkable importance for future optoelectronic applications, for instance in the field of light-emitting devices or sensors.
KW  - fluorinated organic spacer
KW  - 2D perovskites
KW  - phase transition
KW  - temperature dependence
KW  - excitonic materials
Y1  - 2020
U6  - https://doi.org/10.3389/fchem.2019.00946
SN  - 2296-2646
VL  - 7
SP  - 1
EP  - 11
PB  - Frontiers Media
CY  - Lausanne
ER  -