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000633991 1001_ $$0P:(DE-HGF)0$$aAlSabeh, Ghewa$$b0
000633991 245__ $$aOn the Accessibility of Higher‐ n Phases in Formamidinium‐Based Ruddlesden‐Popper and Dion–Jacobson Layered Hybrid Perovskites
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000633991 520__ $$aLayered (2D) hybrid perovskites offer a promising alternative for stabilizing halide perovskite materials, with a growing interest in formamidinium (FA+) lead iodide derivatives for photovoltaics due to their exceptional optoelectronic properties. While their potential increases with the number of inorganic layers (n), the experimental evidence suggests that obtaining n > 2 phases is challenging for FA-based layered perovskites. To address this challenge and identify the conditions governing the formation of higher-n phases, representative FA-based layered hybrid perovskite materials containing aromatic spacer cations, namely benzylammonium (BNA) and 1,4-phenylenedimethanammonium (PDMA)—are investigated as model systems for the corresponding Ruddlesden-Popper and Dion-Jacobson phases based on (BNA)2FAn–1PbnI3n+1 and (PDMA)FAn–1PbnI3n+1 formulations (n = 1–3), respectively. Moreover, the effect of Cs+ cations on the formation of n > 1 phases is explored through a combination of X-ray scattering measurements, solid-state NMR spectroscopy, optoelectronic characterization, and density functional theory calculations. Despite improved photovoltaic performances, the formation of higher (n > 2) phases is excluded, even in the presence of Cs+, due to the favorable formation of other low-dimensional phases revealed by the theoretical investigation. The results contribute to a comprehensive understanding of these materials of broad interest to their application in optoelectronics.
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000633991 7001_ $$0P:(DE-HGF)0$$aSlama, Vladislav$$b1
000633991 7001_ $$0P:(DE-HGF)0$$aAlmalki, Masaud$$b2
000633991 7001_ $$0P:(DE-H253)PIP1088631$$aMerten, Lena$$b3
000633991 7001_ $$0P:(DE-H253)PIP1101502$$aZimmermann, Paul$$b4
000633991 7001_ $$0P:(DE-H253)PIP1081858$$aHinderhofer, Alexander$$b5
000633991 7001_ $$0P:(DE-H253)PIP1011835$$aSchouwink, Pascal$$b6
000633991 7001_ $$0P:(DE-HGF)0$$aCarnevali, Virginia$$b7
000633991 7001_ $$0P:(DE-HGF)0$$aLempesis, Nikolaos$$b8
000633991 7001_ $$0P:(DE-HGF)0$$aAgosta, Lorenzo$$b9
000633991 7001_ $$0P:(DE-H253)PIP1008437$$aSchreiber, Frank$$b10
000633991 7001_ $$0P:(DE-HGF)0$$aRothlisberger, Ursula$$b11$$eCorresponding author
000633991 7001_ $$0P:(DE-HGF)0$$aGrätzel, Michael$$b12$$eCorresponding author
000633991 7001_ $$0P:(DE-HGF)0$$aMilić, Jovana V.$$b13$$eCorresponding author
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