Long-lived polarization memory in the electronic states of lead-halide perovskites from local structural dynamics

Jasmine P. H. Rivett, Liang Z. Tan, Michael B. Price, Sean A. Bourelle, Nathaniel J. L. K. Davis, James Xiao, Yatao Zou, Rox Middleton, Baoquan Sun, Andrew M. Rappe, Dan Credgington () and Felix Deschler ()
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Jasmine P. H. Rivett: University of Cambridge
Liang Z. Tan: University of Pennsylvania
Michael B. Price: University of Cambridge
Sean A. Bourelle: University of Cambridge
Nathaniel J. L. K. Davis: Victoria University of Wellington
James Xiao: University of Cambridge
Yatao Zou: Soochow University
Rox Middleton: University of Cambridge
Baoquan Sun: Soochow University
Andrew M. Rappe: University of Pennsylvania
Dan Credgington: University of Cambridge
Felix Deschler: University of Cambridge

Nature Communications, 2018, vol. 9, issue 1, 1-8

Abstract: Abstract Anharmonic crystal lattice dynamics have been observed in lead halide perovskites on picosecond timescales. Here, we report that the soft nature of the perovskite crystal lattice gives rise to dynamic fluctuations in the electronic properties of excited states. We use linear polarization selective transient absorption spectroscopy to study the charge carrier relaxation dynamics in lead-halide perovskite films and nanocrystals. We find that photo-excited charge carriers maintain an initial polarization anisotropy for several picoseconds, independent of crystallite size and composition, and well beyond the reported timescales of carrier scattering. First-principles calculations find intrinsic anisotropies in the transition dipole moment, which depend on the orientation of light polarization and the polar distortion of the local crystal lattice. Lattice dynamics are imprinted in the optical transitions and anisotropies arise on the time-scales of structural motion. The strong coupling between electronic states and structural dynamics requires a unique interpretation of recombination and transport mechanisms.

Date: 2018
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DOI: 10.1038/s41467-018-06009-3

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