Order-disorder phase transition driven by interlayer sliding in lead iodides

Seyeong Cha, Giyeok Lee, Sol Lee, Sae Hee Ryu, Yeongsup Sohn, Gijeong An, Changmo Kang, Minsu Kim, Kwanpyo Kim, Aloysius Soon () and Keun Su Kim ()
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Seyeong Cha: Yonsei University
Giyeok Lee: Yonsei University
Sol Lee: Yonsei University
Sae Hee Ryu: E. O. Lawrence Berkeley National Laboratory
Yeongsup Sohn: Yonsei University
Gijeong An: Yonsei University
Changmo Kang: Yonsei University
Minsu Kim: Yonsei University
Kwanpyo Kim: Yonsei University
Aloysius Soon: Yonsei University
Keun Su Kim: Yonsei University

Nature Communications, 2023, vol. 14, issue 1, 1-7

Abstract: Abstract A variety of phase transitions have been found in two-dimensional layered materials, but some of their atomic-scale mechanisms are hard to clearly understand. Here, we report the discovery of a phase transition whose mechanism is identified as interlayer sliding in lead iodides, a layered material widely used to synthesize lead halide perovskites. The low-temperature crystal structure of lead iodides is found not 2H polytype as known before, but non-centrosymmetric 4H polytype. This undergoes the order-disorder phase transition characterized by the abrupt spectral broadening of valence bands, taken by angle-resolved photoemission, at the critical temperature of 120 K. It is accompanied by drastic changes in simultaneously taken photocurrent and photoluminescence. The transmission electron microscopy is used to reveal that lead iodide layers stacked in the form of 4H polytype at low temperatures irregularly slide over each other above 120 K, which can be explained by the low energy barrier of only 10.6 meV/atom estimated by first principles calculations. Our findings suggest that interlayer sliding is a key mechanism of the phase transitions in layered materials, which can significantly affect optoelectronic and optical characteristics.

Date: 2023
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DOI: 10.1038/s41467-023-37740-1

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