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Area of Science:

  • Solid State Chemistry
  • High-Pressure Physics
  • Materials Science

Background:

  • Understanding the structural behavior of lead sulfate (PbSO4) under extreme pressure is crucial for materials science.
  • Barite-type structures are common in ABO4 compounds, but their high-pressure phases are less understood.
  • Phase transitions in minerals provide insights into geological processes and material properties under extreme conditions.

Purpose of the Study:

  • To investigate the pressure-induced phase transitions of lead sulfate using synchrotron X-ray diffraction.
  • To determine the high-pressure crystal structure and thermodynamic stability of lead sulfate polymorphs.
  • To elucidate the mechanism, kinetics, and physical properties (compressibility, anisotropy) of the observed phase transition.

Main Methods:

  • Synchrotron X-ray diffraction (XRD) measurements were conducted on lead sulfate up to 67 GigaPascals (GPa).
  • Helium (He) was utilized as the pressure-transmitting medium to ensure hydrostatic conditions.
  • Density Functional Theory (DFT) calculations were employed to complement experimental findings and predict stable structures.

Main Results:

  • A reversible pressure-induced phase transition from the Pnma barite-type to the P212121 post-barite-type structure was observed above 27 GPa.
  • The transition involves a significant volume collapse of 2.4% and exhibits a notable pressure overshoot, indicating a large kinetic barrier.
  • DFT calculations confirmed the experimental results and identified the post-barite-type phase as the thermodynamically stable high-pressure structure for ABO4 oxides.

Conclusions:

  • Lead sulfate transitions to a novel post-barite-type structure at high pressures, which is the stable form for specific ABO4 compounds.
  • The phase transition is kinetically hindered, requiring substantial pressure to overcome the energy barrier.
  • The study provides a detailed understanding of lead sulfate's high-pressure behavior, including its compressibility and structural anisotropy.