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Area of Science:

  • Coordination chemistry
  • Quantum physics
  • Materials science

Background:

  • Single-molecule magnets (SMMs) are crucial for developing advanced magnetic materials.
  • Understanding the influence of nuclear spin on SMM properties is essential for quantum applications.

Purpose of the Study:

  • To synthesize and characterize two dysprosium isotopic isomers with different nuclear spins.
  • To investigate the impact of nuclear spin on the magnetic properties and quantum tunneling of magnetization (QTM) in SMMs.
  • To explore the potential of these systems for quantum information processing (QIP).

Main Methods:

  • Synthesis of tetraethylammonium salts of 163Dy and 164Dy phthalocyaninato complexes.
  • Ac-susceptibility measurements to probe magnetic properties.
  • Muon spin spectroscopy (μ-SQUID) to study quantum tunneling of the magnetization (QTM).

Main Results:

  • Both isotopologues function as SMMs, but exhibit different relaxation times and magnetic hysteresis.
  • Nuclear-spin-driven QTM events were observed in the 163Dy isomer (I=5/2), enabling determination of hyperfine coupling and nuclear quadrupole splitting.
  • The 164Dy isomer (I=0) displayed significantly reduced QTM at zero magnetic field.
  • The 163Dy isomer demonstrated potential as a multilevel nuclear spin qubit (qudit, d=6) for QIP.

Conclusions:

  • Nuclear spin plays a critical role in the magnetic behavior of lanthanide-based SMMs.
  • The 163Dy isomer represents a novel system for exploring nuclear spin effects in molecular magnetism and QIP.
  • Design principles for molecular qubits and SMMs must incorporate lanthanide nuclear spin characteristics.