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Structure induced Yb valence changes in the solid solution Yb(x)Ca(1-x)C2.

Pascal Link1, Pieter Glatzel, Kristina Kvashnina

  • 1Department of Chemistry, University of Cologne, Greinstrasse 6, D-50939 Cologne, Germany.

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This study reveals that the Ytterbium (Yb) valence state in Yb(x)Ca(1-x)C2 solid solutions is strongly dependent on crystal structure and temperature. These findings offer insights into rare earth element behavior in materials science.

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Area of Science:

  • Materials Science
  • Solid-State Chemistry
  • Rare Earth Chemistry

Background:

  • The Yb(x)Ca(1-x)C2 solid solution system presents complex structural and electronic properties.
  • Understanding the interplay between crystal structure and Yb valence is crucial for materials design.

Purpose of the Study:

  • To investigate the crystal structure, Yb valence state, and their relationship in Yb(x)Ca(1-x)C2 solid solutions.
  • To explore the influence of temperature on structural phase transitions and Yb valence changes.

Main Methods:

  • Synthesis of Yb(x)Ca(1-x)C2 solid solutions at 1323 K.
  • Synchrotron and neutron powder diffraction for crystal structure determination.
  • High-energy-resolution fluorescence-detection X-ray absorption near-edge structure (HERFD-XANES) spectroscopy for Yb valence analysis.
  • Differential scanning calorimetry (DSC) for lattice strain analysis.

Main Results:

  • Yb(x)Ca(1-x)C2 exhibits structure-dependent Yb valence states: tetragonal phases (x ≥ 0.75) show mixed-valent Yb (~75% Yb3+), while monoclinic phases (x ≤ 0.75) contain exclusively Yb2+.
  • Significant deviations from Vegard's law in monoclinic phases are attributed to these distinct Yb valence states.
  • Temperature-induced phase transitions lead to drastic Yb valence changes, e.g., from ~2.70 to 2.0 in compounds with x = 0.75 and x = 0.91.

Conclusions:

  • Yb(x)Ca(1-x)C2 is a rare system demonstrating a strong structure-dependent Yb valence state.
  • Temperature plays a critical role in inducing phase transitions that alter the Yb valence and associated structural properties.
  • The findings highlight the intricate relationship between crystal structure, Yb valence, and material properties in this solid solution series.