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Magnetic Ordering in Gold Nanoclusters.

Mikhail Agrachev1, Sabrina Antonello1, Tiziano Dainese1

  • 1Department of Chemistry, University of Padova, via Marzolo 1, 35131 Padova, Italy.

ACS Omega
|August 29, 2019
PubMed
Summary

Magnetism in gold nanoclusters is complex, influenced by factors like crystal order and spin-orbit coupling. Precise control over sample composition, charge state, and crystallinity is crucial for reproducible magnetic behavior.

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Area of Science:

  • Nanomaterials Science
  • Quantum Chemistry
  • Solid-State Physics

Background:

  • Conflicting reports exist regarding magnetism in monolayer-protected gold clusters.
  • Previous studies on Au25(SCH2CH2Ph)18^0 primarily detected paramagnetism.
  • A precise understanding of the magnetic phenomena in these gold clusters is lacking.

Purpose of the Study:

  • To investigate the magnetic behaviors of Au25(SCH2CH2Ph)18^0 across varying crystallographic orders.
  • To elucidate the underlying factors contributing to magnetism in gold nanoclusters.
  • To establish conditions for reproducible magnetic measurements in these systems.

Main Methods:

  • Electron paramagnetic resonance (EPR) spectroscopy was employed to study magnetic properties.
  • Hysteresis experiments were conducted on single crystals.
  • Density functional theory (DFT) calculations were performed on single cluster and periodic models.

Main Results:

  • Au25(SCH2CH2Ph)18^0 films exhibit paramagnetism, with detectable ferromagnetic interactions at low temperatures.
  • Single crystals show ferromagnetism upon physical reorientation in an applied field.
  • Microcrystalline samples display paramagnetic, superparamagnetic, and ferromagnetic behaviors at room temperature.
  • EPR spectral simulations indicate the importance of spin-orbit coupling and crystal distortion.
  • DFT calculations support EPR findings regarding spin-orbit coupling and crystal-splitting effects.

Conclusions:

  • Magnetism in gold nanoclusters arises from a delicate interplay of factors, including spin-orbit coupling and crystal distortion.
  • Achieving reproducible results necessitates precise control over sample monodispersity, charge state, crystallinity, and experimental conditions.
  • This study demonstrates ferromagnetism in gold nanoclusters, challenging previous observations.