Charge carriers in the soft and polar perovskite lattice form so-called polaron quasiparticles, charge carriers dressed with a lattice deformation. The spatial extent of a polaron is governed by the material's electron-phonon interaction strength, which determines charge carrier effective mass, mobility, and the so-called Mott polaron density, that is, the maximum stable density of charge carriers that a perovskite can support. Despite its significance, controlling polaron dimensions has been challenging. Here, experimental substantial tuning of polaron dimensions is reported by lattice engineering, through Pb/Sn substitution in CH3NH3SnxPb1-xI3. The polaron dimension is deduced from the Mott polaron density, which can be composition-tuned over an order of magnitude, while charge carrier mobility occurs through band transport, and remains substantial across all compositions, ranging from 10 s to 100 s cm2 V s-1 at room temperature. The effective modulation of polaron size can be understood by considering the bond asymmetry after carrier injection as well as the random spatial distribution of Pb/Sn ions. This study underscores the potential for tailoring polaron dimensions, which is crucial for optimizing applications prioritizing either high charge carrier density or high mobility.
Keywords: Mott polaron density; THz spectroscopy; perovskites; polaron size; polarons.
© 2024 The Author(s). Advanced Materials published by Wiley‐VCH GmbH.