Journal Article

PUBDB-2025-02456

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png On the Accessibility of Higher‐ n Phases in Formamidinium‐Based Ruddlesden‐Popper and Dion–Jacobson Layered Hybrid Perovskites

AlSabeh, G. ; Slama, V. ; Almalki, M. ; Merten, L.Extern* ; Zimmermann, P.Extern* ; Hinderhofer, A.Extern* ; Schouwink, P.Extern* ; Carnevali, V. ; Lempesis, N. ; Agosta, L. ; Schreiber, F.Extern* ; Rothlisberger, U. (Corresponding author) ; Grätzel, M. (Corresponding author) ; Milić, J. V. (Corresponding author)

2025
Wiley-VCH Verlag GmbH & Co. KG Weinheim

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Please use a persistent id in citations: doi:10.1002/aelm.202500164  doi:10.3204/PUBDB-2025-02456

Abstract: Layered (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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Contributing Institute(s):

1. DOOR-User (DOOR ; HAS-User)

Research Program(s):

1. 6G3 - PETRA III (DESY) (POF4-6G3) (POF4-6G3)
2. FS-Proposal: I-20220258 (I-20220258) (I-20220258)
3. 05K19VTA - Entwicklung einer kompakten Probenumgebung mit Spin-Coater für in-situ Röntgenstreuung an PETRA III. (BMBF-05K19VTA) (BMBF-05K19VTA)
4. PANACEA - A Pan-European Solid-State NMR Infrastructure for Chemistry-Enabling Access (101008500) (101008500)

Experiment(s):

1. PETRA Beamline P23 (PETRA III)

Appears in the scientific report 2025

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