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Compression transforms arsenic sulfide (α-As₂S₃) from covalent to metavalent bonding, altering its electronic and vibrational properties without a first-order phase transition. This high-pressure behavior may apply to other group-15 sesquichalcogenides.

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Area of Science:

  • Materials Science
  • Solid-State Physics
  • Crystallography

Background:

  • Layered monoclinic arsenic sulfide (α-As₂S₃), also known as orpiment, is a mineral with unique structural and electronic properties.
  • Understanding material behavior under extreme conditions like high pressure is crucial for discovering new phenomena and applications.

Purpose of the Study:

  • To investigate the structural, vibrational, and electronic properties of α-As₂S₃ under compression.
  • To determine the equation of state and identify phase transitions in orpiment up to 25 GPa.
  • To explore the nature of bonding changes and their impact on material properties at high pressures.

Main Methods:

  • Joint experimental and theoretical study combining X-ray diffraction and Raman scattering measurements.
  • High-pressure experiments on orpiment samples.
  • Ab initio calculations to support experimental findings and assign vibrational modes.

Main Results:

  • No first-order phase transition was observed up to 25 GPa at room temperature.
  • An isostructural phase transition occurs above 20 GPa, marked by an increase in As coordination from threefold to over fivefold.
  • Compression leads to a transition from covalent to metavalent bonding, decreasing the bandgap and softening optical modes.

Conclusions:

  • High pressure induces a metavalent bonding state in α-As₂S₃, altering its electronic and optical properties.
  • This metavalent bonding transition is proposed as a general mechanism for group-15 sesquichalcogenides under pressure.
  • The findings suggest a pathway from covalent to metavalent and ultimately metallic bonding in these materials.