Large polarons in lead halide perovskites

By K. Miyata, D. Meggiolaro, M. T. Trinh, P. Joshi, E. Mosconi, S. C. Jones, F. De Angelis, Xiaoyang Zhu. Science Advances, 2017

671 citations recorded by the source corpus.

Charge carriers in both hybrid and all-inorganic lead halide perovskites form large polarons. Lead halide perovskites show marked defect tolerance responsible for their excellent optoelectronic properties. These properties might be explained by the formation of large polarons, but how they are formed and whether organic cations are essential remain open questions. We provide a direct time domain view of large polaron formation in single-crystal lead bromide perovskites CH3NH3PbBr3 and CsPbBr3. We found that large polaron forms predominantly from the deformation of the PbBr3− frameworks, irrespective of the cation type. The difference lies in the polaron formation time, which, in CH3NH3PbBr3 (0.3 ps), is less than half of that in CsPbBr3 (0.7 ps). First-principles calculations confirm large polaron formation, identify the Pb-Br-Pb deformation modes as responsible, and explain quantitatively the rate difference between CH3NH3PbBr3 and CsPbBr3. The findings reveal the general advantage of the soft [PbX3]− sublattice in charge carrier protection and suggest that there is likely no mechanistic limitations in using all-inorganic or mixed-cation lead halide perovskites to overcome instability problems and to tune the balance between charge carrier protection and mobility.

Subfields: Electrical and Electronic Engineering, Materials Chemistry

View Paper: https://www.semanticscholar.org/paper/0f96c1a711fa7e67fde7c1da5eb29b3d3d1e2bf6

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Citations in the corpus

• Wigner Formulation of Thermal Transport in Solids (2021, methodology): “Lattice parameters of orthorhombic CsPbBr3, obtained by first-principles simulations or experiments [22, 207].”