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Ferroelectric large polarons

Nature Materials volume 17, pages 379–381 (2018)Cite this article

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Kiyoshi Miyata and X.-Y. Zhu analyse the ferroelectric-like dielectric response of lead halide perovskites in the terahertz region and discuss the potential role of polar nanodomains in accounting for the defect tolerance and low recombination rates of these materials.

To understand how such phonon behaviour affects the formation and properties of large polarons, we examine the dielectric function of LHPs, ε(ν) = ε1(ν) + iε2(ν), where ε1 describes polarization and ε2 absorption, ν is frequency. Polarization is related to the dielectric function by Re(P) = ε0(ε1 − 1)Ef, where ε0 is the vacuum permittivity. At frequencies above about 10 THz, ε(ν) is mainly determined by valence-electron densities, whereas at frequencies below 10 THz it reflects how phonons respond to an external electric field. We show ε(ν) of methylammonium lead iodide (MAPbI3) in Fig. 1c. In the frequency range of 107 Hz to 1014 Hz, ε1changes in two steps: the first at about 6 GHz (νrot) when ε1 doubles because of reorientational relaxation of dipolar MA+ cations3,5, and the second at about 1 THz when ε1 increases by an order of magnitude following the excitation of transverse optical (TO) phonon modes of the PbI3− inorganic sublattice (νTO).

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Fig. 1: Ferroelectric-like behaviour of lead halide perovskites and implications for the large polaron model.

adapted from ref. 3, Royal Society of Chemistry and ref. 5, Wiley (c); ref. 14, Univ. of Missouri-Kansas City (d); ref. 15, AIP (e); ref. 16, Academic (f).

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Acknowledgements

X.Y.Z. acknowledges support by the Vannevar Bush Faculty Fellowship through Office of Naval Research grant no. N00014-18-1-2080 during the writing of this paper. K.M. acknowledges the Japan Society for the Promotion of Science for financial support.

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  1. Department of Chemistry, Columbia University, New York, NY, USA

    Kiyoshi Miyata & X.-Y. Zhu

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  1. Kiyoshi Miyata
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Correspondence to X.-Y. Zhu.

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Miyata, K., Zhu, XY. Ferroelectric large polarons. Nature Mater 17, 379–381 (2018). https://doi.org/10.1038/s41563-018-0068-7

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