Hidden in Plain Sight: The Overlooked Influence of the Cs+ Substructure on Transformations in Cesium Lead Halide Nanocrystals

Stefano Toso,Liberato Manna,Dmitry Baranov

doi:10.1021/acsenergylett.0c02029

Stefano Toso, Liberato Manna + Show 1 more

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https://doi.org/10.1021/acsenergylett.0c02029

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Abstract

Hidden in Plain Sight: The Overlooked Influence of the Cs<sup>+</sup> Substructure on Transformations in Cesium Lead Halide Nanocrystals

Highlights

Cesium lead halide perovskite nanocrystals, with formula CsPbX3 (X = Cl, Br, I), have received enormous attention in the last five years because of their efficient, narrow, and tunable light emission.[1]
Perovskites are only some of the many compositions and structures found in the Cs−Pb−X ternary system: together with the two binary compounds CsX and PbX2, the best-known structures in the system are Cs4PbX6, the perovskites α,β,γ-CsPbX3, the nonperovskite δ-CsPbX3, and CsPb2X5
The reports describing compositional and structural interconversions are often focused on pairs of compounds, e.g., the CsPbX3 ⇄ Cs4PbX6 or the CsPbX3 ⇄ Cs4Pb2X5

Summary

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As more experimental data have become available over time, it is possible to connect different reactions and construct a unifying picture of the reactivity of the Cs−Pb−X compounds Such a view has been missing to date, mainly because these materials are often approached with a focus on how their structures are related to their properties and less to their reactivity. Such octahedra are disconnected in Cs4PbX6, but share corners in the perovskite CsPbX3 and faces in the δ-CsPbX3 nonperovskite structure This rationalization is useful when discussing electronic properties, as they mostly depend on the Pb−X−Pb connectivity.[3] reasoning in terms of [PbX6]4− octahedra excludes many of the materials in the Cs− Pb−X system that can either generate or be generated from one of the three above through a chemical reaction and hides deeper structural connections across the whole series. Depending on the amount of PbX2 added, the anionic network adapts its connectivity to ensure the charge balance, and we obtain the whole series of structures

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