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

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Interlayer sliding drives phase transitions in lead iodides, altering their optical properties. This mechanism, observed in a novel 4H polytype, offers insights into layered material behavior.

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Area of Science:

  • Materials Science
  • Condensed Matter Physics
  • Solid State Chemistry

Background:

  • Two-dimensional layered materials exhibit diverse phase transitions.
  • Understanding the atomic-scale mechanisms of these transitions is challenging.
  • Lead iodide is a key material in lead halide perovskite synthesis.

Purpose of the Study:

  • To investigate the phase transition mechanism in lead iodides.
  • To identify the low-temperature crystal structure of lead iodides.
  • To elucidate the impact of the phase transition on material properties.

Main Methods:

  • Angle-resolved photoemission spectroscopy (ARPES) to study electronic band structure changes.
  • Transmission electron microscopy (TEM) to visualize structural rearrangements.
  • First-principles calculations to determine energy barriers for interlayer sliding.

Main Results:

  • The low-temperature structure of lead iodide is identified as a non-centrosymmetric 4H polytype, not the previously assumed 2H.
  • An order-disorder phase transition occurs at 120 K, marked by spectral broadening of valence bands.
  • Interlayer sliding of the 4H polytype structure above 120 K was observed via TEM.
  • First-principles calculations revealed a low energy barrier (10.6 meV/atom) for this sliding.

Conclusions:

  • Interlayer sliding is identified as the primary mechanism for the observed phase transition in lead iodides.
  • This phase transition significantly impacts the optoelectronic and optical characteristics of lead iodide.
  • The findings highlight interlayer sliding as a crucial mechanism in phase transitions of layered materials.