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A computational study of high pressure polymorphic transformations in monazite-type LaPO4.

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Density functional theory (DFT) calculations reveal pressure-induced phase transformations in Lanthanum Phosphate (LaPO4). A predicted monazite-type to barite-type transformation at 16.2 GPa is not experimentally observed, suggesting kinetic barriers.

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Area of Science:

  • Solid-state chemistry
  • Materials science
  • Computational materials science

Background:

  • Lanthanum Phosphate (LaPO4) exhibits complex polymorphic transformations under pressure.
  • Understanding these transformations is crucial for predicting material behavior in high-pressure environments.

Purpose of the Study:

  • To investigate pressure-induced polymorphic transformations in LaPO4 using first-principles calculations.
  • To determine the stability and properties of different LaPO4 polymorphs as a function of pressure.

Main Methods:

  • Density Functional Theory (DFT) calculations employing the generalized gradient approximation.
  • Analysis of pressure-volume relations, unit-cell dimensions, equation of state, elastic constants, and phonon dispersion curves.
  • Identification of structural transformation pathways and their associated pressures.

Main Results:

  • A theoretical monazite-type (P21/n) to barite-type (Pbnm) transformation was identified at 16.2 GPa, but not observed experimentally near this pressure.
  • A significant discontinuity in the pressure-volume relation (4.16% volume change) was observed around 28 GPa, aligning with experimental data.
  • The barite-type (Pbnm) and post-barite-type (P212121) structures are mechanically and dynamically stable at 27 GPa, suggesting kinetic hindrance for the monazite-to-barite transition.

Conclusions:

  • The monazite-type to barite-type phase transformation in LaPO4 may be kinetically hindered.
  • The transformation is driven by the softening of the C25 elastic constant and involves changes in La coordination polyhedra.
  • DFT calculations provide valuable insights into the complex high-pressure behavior of LaPO4 polymorphs.