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High pressure transforms palladium trifluoride (PdF3) into a genuine palladium(III) fluoride (PdIII F3) phase. This study reveals novel high-pressure structures and potential magnetic properties of PdF3 under extreme compression.

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Area of Science:

  • Solid State Chemistry
  • Materials Science under Extreme Conditions
  • Inorganic Chemistry

Background:

  • Palladium trifluoride (PdF3) is typically a mixed-valent compound (PdII PdIV F6), not a true Pd(III) fluoride.
  • Investigating high-pressure effects on transition metal fluorides can reveal novel phases and properties.

Purpose of the Study:

  • To determine if high pressure can induce the formation of a genuine palladium(III) fluoride (PdIII F3).
  • To characterize the structural and potential magnetic properties of PdF3 under extreme compression (> 1 GPa).

Main Methods:

  • Joint theoretical (hybrid density functional calculations) and experimental study of palladium trifluoride under high pressure.
  • X-ray diffraction and high-pressure techniques to observe phase transitions and determine crystal structures.

Main Results:

  • Theoretical calculations predicted a preference for single-valent polymorphs above 30 GPa.
  • Experimental observation of phase transitions: R3̅ to P1̅ above 42 GPa, and P1̅ to C2/c above ~50 GPa.
  • The C2/c phase, appearing above ~50 GPa, contains genuine Pd(III) centers, confirming the formation of PdIII F3.

Conclusions:

  • High pressure (above ~50 GPa) successfully induces a phase transition in palladium trifluoride, leading to the formation of a genuine palladium(III) fluoride (PdIII F3).
  • Novel high-pressure crystal structures (triclinic P1̅ and monoclinic C2/c) were identified.
  • The C2/c phase exhibits potential for strong one-dimensional antiferromagnetic exchange interactions.