TY - JOUR A1 - Wang, Qiong A1 - Mosconi, Edoardo A1 - Wolff, Christian Michael A1 - Li, Junming A1 - Neher, Dieter A1 - De Angelis, Filippo A1 - Suranna, Gian Paolo A1 - Grisorio, Roberto A1 - Abate, Antonio T1 - Rationalizing the molecular design of hole-selective contacts to improve charge extraction in Perovskite solar cells JF - dvanced energy materials N2 - Two new hole selective materials (HSMs) based on dangling methylsulfanyl groups connected to the C-9 position of the fluorene core are synthesized and applied in perovskite solar cells. Being structurally similar to a half of Spiro-OMeTAD molecule, these HSMs (referred as FS and DFS) share similar redox potentials but are endowed with slightly higher hole mobility, due to the planarity and large extension of their structure. Competitive power conversion efficiency (up to 18.6%) is achieved by using the new HSMs in suitable perovskite solar cells. Time-resolved photoluminescence decay measurements and electrochemical impedance spectroscopy show more efficient charge extraction at the HSM/perovskite interface with respect to Spiro-OMeTAD, which is reflected in higher photocurrents exhibited by DFS/FS-integrated perovskite solar cells. Density functional theory simulations reveal that the interactions of methylammonium with methylsulfanyl groups in DFS/FS strengthen their electrostatic attraction with the perovskite surface, providing an additional path for hole extraction compared to the sole presence of methoxy groups in Spiro-OMeTAD. Importantly, the low-cost synthesis of FS makes it significantly attractive for the future commercialization of perovskite solar cells. KW - hole extraction KW - hole selective materials KW - perovskite solar cells KW - sulfur KW - triple-cation perovskite Y1 - 2019 U6 - https://doi.org/10.1002/aenm.201900990 SN - 1614-6832 SN - 1614-6840 VL - 9 IS - 28 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Warby, Jonathan A1 - Zu, Fengshuo A1 - Zeiske, Stefan A1 - Gutierrez-Partida, Emilio A1 - Frohloff, Lennart A1 - Kahmann, Simon A1 - Frohna, Kyle A1 - Mosconi, Edoardo A1 - Radicchi, Eros A1 - Lang, Felix A1 - Shah, Sahil A1 - Pena-Camargo, Francisco A1 - Hempel, Hannes A1 - Unold, Thomas A1 - Koch, Norbert A1 - Armin, Ardalan A1 - De Angelis, Filippo A1 - Stranks, Samuel D. A1 - Neher, Dieter A1 - Stolterfoht, Martin T1 - Understanding performance limiting interfacial recombination in pin Perovskite solar cells JF - Advanced energy materials N2 - 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. KW - C60 KW - defects KW - interface recombination KW - loss mechanisms KW - perovskites KW - solar cells Y1 - 2022 U6 - https://doi.org/10.1002/aenm.202103567 SN - 1614-6832 SN - 1614-6840 VL - 12 IS - 12 PB - Wiley-VCH CY - Weinheim ER -