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Chemical and Structural Segregation in Quaternary Ni-Cu-Fe-Co Nanoparticles: Atomistic Simulation and Experiment.

Andrey Yu Kolosov1, Nikita Nepsha1, Denis Sokolov1

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Summary

This study reveals that quaternary nickel-copper-iron-cobalt (Ni-Cu-Fe-Co) nanoparticles exhibit a unique hierarchical structure. Copper-rich shells and Ni/Fe-dominated cores form, influenced by particle size and synthesis conditions.

Keywords:
Monte Carlo methodmolecular dynamics methodnanoparticlesquaternary nanoparticlessegregationtight-binding potential

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Area of Science:

  • Materials Science
  • Nanotechnology
  • Computational Materials Science

Background:

  • Quaternary nanoparticles are crucial in various applications.
  • Understanding nanoparticle structure-property relationships is essential.
  • Previous studies have not fully explored Ni-Cu-Fe-Co systems.

Purpose of the Study:

  • To comprehensively investigate the structural and energetic properties of Ni-Cu-Fe-Co nanoparticles.
  • To elucidate the influence of particle size on nanoparticle characteristics.
  • To combine experimental synthesis and characterization with atomistic simulations.

Main Methods:

  • Solution combustion synthesis for nanoparticle fabrication.
  • X-ray diffraction (XRD) for phase and structure analysis.
  • Transmission Electron Microscopy with Energy Dispersive X-ray Spectroscopy (TEM-EDS) for elemental mapping.
  • Atomistic modeling including molecular dynamics (MD) and Monte Carlo (MC) simulations.

Main Results:

  • Predominance of face-centered cubic (fcc) structure with coexisting hexagonal close-packed (hcp) phases observed via XRD.
  • TEM-EDS confirmed significant surface segregation of Copper (Cu) and partial Cobalt (Co) enrichment, with Nickel (Ni) and Iron (Fe) concentrating in particle cores.
  • MD simulations indicated an increase in melting temperature (Tm) with particle size and a decrease in crystallization temperature (Tc) with faster cooling rates.
  • Potential energy stabilized and surface energy decreased with increasing particle size, correlating with Cu segregation.

Conclusions:

  • Ni-Cu-Fe-Co nanoparticles intrinsically form hierarchical, labyrinth-like structures.
  • Cu-rich shells and Ni/Fe-dominated cores are characteristic of these nanoparticles.
  • The study provides critical insights into the interplay between synthesis, size, structure, and elemental distribution in complex nanoparticles.