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Yasuhisa Yamamura1, Aruto Horikoshi, Syuma Yasuzuka

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Summary

Zirconium vanadate (ZrV(2)O(7)) and hafnium vanadate (HfV(2)O(7)) exhibit negative thermal expansion (NTE) due to structural distortions released during phase transitions. These transitions involve specific phonon behaviors characteristic of NTE materials.

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Area of Science:

  • Materials Science
  • Solid State Chemistry
  • Thermodynamics

Background:

  • Negative thermal expansion (NTE) materials are of interest for advanced applications.
  • Zirconium vanadate (ZrV(2)O(7)) and hafnium vanadate (HfV(2)O(7)) are known to exhibit NTE.
  • Understanding the mechanisms behind NTE is crucial for material design.

Purpose of the Study:

  • To investigate the phase transitions and thermal expansion behavior of ZrV(2)O(7) and HfV(2)O(7).
  • To elucidate the relationship between phonon properties and NTE in these compounds.
  • To identify the structural factors contributing to NTE.

Main Methods:

  • X-ray diffraction (XRD) for structural analysis.
  • Heat capacity calorimetry for thermodynamic measurements.
  • Phonon density of states (DOS) and mode-Grüneisen parameter analysis.

Main Results:

  • Two successive phase transitions were observed in both ZrV(2)O(7) and HfV(2)O(7) at specific temperatures.
  • The phase transitions were identified as displacive type based on low transition entropies.
  • Phonon DOS analysis revealed features common to NTE compounds, including low- and high-energy modes and a phonon gap.
  • A negative mode-Grüneisen parameter for low-energy modes was observed, but its small magnitude, due to V(2)O(7) group distortion, led to positive thermal expansion in the low-temperature phase.

Conclusions:

  • The NTE in the high-temperature phase of ZrV(2)O(7) and HfV(2)O(7) arises from the release of structural distortion during successive phase transitions.
  • The observed phonon characteristics support the understanding of NTE mechanisms in these vanadates.
  • Structural distortion plays a critical role in the thermal expansion behavior of these materials.