Long-lived polarization memory in the electronic states of lead-halide perovskites from local structural dynamics.
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Authors
Rivett, Jasmine PH
Price, Michael B
Bourelle, Sean A
Davis, Nathaniel JLK
Xiao, James
Zou, Yatao
Sun, Baoquan
Publication Date
2018-08-30Journal Title
Nat Commun
ISSN
2041-1723
Publisher
Springer Science and Business Media LLC
Volume
9
Issue
1
Pages
3531
Language
eng
Type
Article
Physical Medium
Electronic
Metadata
Show full item recordCitation
Rivett, J. P., Tan, L. Z., Price, M. B., Bourelle, S. A., Davis, N. J., Xiao, J., Zou, Y., et al. (2018). Long-lived polarization memory in the electronic states of lead-halide perovskites from local structural dynamics.. Nat Commun, 9 (1), 3531. https://doi.org/10.1038/s41467-018-06009-3
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.
Sponsorship
EPSRC (1360817)
EPSRC (1494744)
Engineering and Physical Sciences Research Council (EP/G037221/1)
Engineering and Physical Sciences Research Council (EP/L015978/1)
EPSRC (1804146)
Identifiers
External DOI: https://doi.org/10.1038/s41467-018-06009-3
This record's URL: https://www.repository.cam.ac.uk/handle/1810/284695
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