Kavli Affiliate: David T. Limmer
| First 5 Authors: Yoonjae Park, Yoonjae Park, , ,
| Summary:
Lead halide perovskites have been extensively studied as a class of materials
with unique optoelectronic properties. A fundamental aspect that governs
optical and electronic behaviors within these materials is the intricate
coupling between charges and their surrounding lattice. Unravelling the role of
charge-lattice interactions on the optoelectronic properties in lead halide
perovskites is necessary to understand their photophysics. Unlike traditional
semiconductors where a harmonic approximation often suffices to capture lattice
fluctuations, lead halide perovskites have a significant anharmonicity
attributed from the rocking and tilting motions of inorganic framework. Thus,
while there is broad consensus on the importance of the structural deformations
and polar fluctuations on the behavior of charge carriers and quasiparticles,
the strongly anharmonic nature of these fluctuations and their strong
interactions render theoretical descriptions of lead halides perovskites
challenging. In this Account, we review our recent efforts to understand how
the soft, polar lattice of this class of materials alter their quasiparticle
binding energies and fine structure, charge mobilities, and lifetimes of
phonons and excess charges. Throughout, these are aimed at characterizing the
interplay between lattice fluctuations and optoelectronic properties of lead
halide perovskites and are reviewed in the context of the effective models we
have built, and the novel theoretical methods we have developed to understand
bulk crystalline materials, as well as nanostructures, and lower dimensionality
lattices. By integrating theoretical advances with experimental observations,
the perspective we detail in this account provides a comprehensive picture that
serves as both design principles for optoelectronic materials and a set of
theoretical tools to study them when charge-lattice interactions are important.
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