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Crystallization is a phase transformation process in which crystals are precipitated from a supersaturated solution or formed from other sources. During crystallization, atoms or molecules arrange themselves into a well-defined, rigid crystal lattice to minimize energy.
Initiating crystallization involves manipulating the concentration of the solute and the temperature of the solution. Since crystal growth occurs when the ratio of concentration and solubility of the solute in the solvent...
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Single-Crystal Growth and Characterization of High-Entropy Phosphides ASiP2.

Yasuyuki Iwabuchi1, Mingyu Xu2, Weiwei Xie2

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High-entropy engineering created novel phosphide single crystals with potential for nonlinear optics. These materials exhibit unique microstructures and optical properties, opening new avenues in materials science.

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Area of Science:

  • Materials Science
  • Solid-State Chemistry
  • Crystallography

Background:

  • High-entropy materials offer tunable properties.
  • Ternary phosphides are less explored for high-entropy applications.
  • MgSiP2 serves as a base for novel high-entropy phosphides.

Purpose of the Study:

  • To synthesize and characterize new high-entropy phosphide single crystals.
  • To investigate the structural and optical properties of these novel materials.
  • To explore the potential of high-entropy engineering in phosphide systems.

Main Methods:

  • High-entropy engineering applied to MgSiP2.
  • Synthesis of (Mg, Zn, Cd, Mn)SiP2 (A4SiP2) and (Mg, Ca, Sr, Ba, Zn)SiP2 (A5SiP2) single crystals.
  • Sb-flux method for crystal growth.
  • Scanning electron microscopy with energy dispersive X-ray spectroscopy (SEM-EDX) for composition analysis.

Main Results:

  • Successful synthesis of A4SiP2 and A5SiP2 single crystals.
  • A5SiP2 crystallized in a new space group (I4̅2m) with multiple high-entropy sites.
  • Unique microstructure in A5SiP2 with a (Mg, Zn)SiP2 core and high-entropy shell.
  • Both A4SiP2 and A5SiP2 exhibited optical second harmonic generation (non-linear optical response).
  • Observed band-gap narrowing compared to parent phases.

Conclusions:

  • High-entropy engineering is feasible in ternary phosphides.
  • A novel crystal structure (I4̅2m) was discovered in A5SiP2.
  • The synthesized phosphides show promise as nonlinear optical materials.
  • This work expands the scope of high-entropy materials into the phosphide domain.