Tuning Structure and Excitonic Properties of 2D Ruddlesden–Popper Germanium, Tin, and Lead Iodide Perovskites via Interplay between Cations

化学 锗化合物 碘化物 铅(地质) 结晶学 凝聚态物理 无机化学 物理 地质学 地貌学 有机化学
作者
Willa Mihalyi‐Koch,Giulia Folpini,Chris R. Roy,Waldemar Kaiser,Chun‐Sheng Wu,Kyana M. Sanders,Ilia A. Guzei,John C. Wright,Filippo De Angelis,Daniele Cortecchia,Annamaria Petrozza,Song Jin
出处
期刊:Journal of the American Chemical Society [American Chemical Society]
卷期号:145 (51): 28111-28123 被引量:33
标识
DOI:10.1021/jacs.3c09793
摘要

The compositional tunability of 2D metal halide perovskites enables exploration of diverse semiconducting materials with different structural features. However, rationally tuning the 2D perovskite structures to target physical properties for specific applications remains challenging, especially for lead-free perovskites. Here, we study the effect of the interplay of the B-site (Ge, Sn, and Pb), A-site (cesium, methylammonium, and formamidinium), and spacer cations on the structure and optical properties of a new series of 2D Ruddlesden-Popper perovskites using the previously unreported spacer cation 4-bromo-2-fluorobenzylammonium (4Br2FBZ). We report eight new crystal structures and study the consequence of varying the B-site (Pb, Sn, Ge) and dimension (n = 1, 2, vs 3D). Dimension strongly influences local distortion and structural symmetry, and the increased octahedral tilting and lone pair effects in Ge perovskites lead to a polar n = 2 perovskite that exhibits second harmonic generation, (4Br2FBZ)2(Cs)Ge2I7. In contrast, the analogous Sn and Pb perovskites remain centrosymmetric, but the B-site metal influences the photoluminescence properties. The Pb perovskites exhibit broad, defect-mediated emission at low temperature, whereas the Sn perovskites show purely excitonic emission over the entire temperature range, but the carrier recombination dynamics depend on dimensionality and dark excitonic states. Wholistic understanding of these differences that arise based on cations and dimensionality can guide the rational materials design of 2D perovskites for targeting physical properties for optoelectronic applications based on the interplay of cations and the connectivity of the inorganic framework.
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