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Gd(5)Si(4-x)P(x): targeted structural changes through increase in valence electron count.

Volodymyr Svitlyk1, Gordon J Miller, Yurij Mozharivskyj

  • 1Department of Chemistry, McMaster University, Hamilton, Ontario, L8S 4M1, Canada.

Journal of the American Chemical Society
|February 10, 2009
PubMed
Summary
This summary is machine-generated.

Phase transformations in gadolinium silicon phosphide (Gd(5)Si(4-x)P(x)) systems were studied. Increased phosphorus substitution breaks interslab dimers, altering crystal structure and extending Sm(5)Ge(4)-type structures.

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Area of Science:

  • Materials Science
  • Solid State Chemistry
  • Crystallography

Background:

  • Gadolinium silicides and their alloys exhibit interesting structural and electronic properties.
  • Understanding phase transformations is crucial for tailoring material characteristics.

Purpose of the Study:

  • To investigate phase transformations in the Gd(5)Si(4-x)P(x) system.
  • To correlate crystal structure changes with valence electron count.
  • To explore the stability of Sm(5)Ge(4)-type structures.

Main Methods:

  • X-ray diffraction (XRD) for structural analysis.
  • Systematic substitution of Si with P in Gd(5)Si(4-x)P(x).
  • Tight-binding linear-muffin-tin-orbital (TB-LMTO) calculations.

Main Results:

  • Phase transformations observed in Gd(5)Si(4-x)P(x) systems (0 ≤ x ≤ 2).
  • Increased valence electron count via P substitution leads to the breaking of interslab T-T dimers.
  • The Gd(5)Si(2.75)P(1.25) phase exhibits shear movement of [Gd(5)T(4)] slabs.
  • Orthorhombic Sm(5)Ge(4)-type structures are stabilized at valence electron counts > 31 e(-)/formula unit.

Conclusions:

  • A strong coupling exists between crystal structure and valence electron count in the studied system.
  • P substitution influences interslab bonding and slab arrangements.
  • TB-LMTO calculations confirm the electronic origin of dimer cleavage due to antibonding state population.