Strong Relativistic Effects in Lanthanide-Based Single-Molecule Magnets

Area of Science:

• Quantum computing
• Materials science
• Computational chemistry

Background:

• Lanthanide-based single-molecule magnets (SMMs) are key for quantum memory and spintronics.
• Accurate spin-orbit coupling (SOC) calculations are vital for designing SMMs with long spin relaxation times.
• Traditional perturbation theory for SOC is unreliable for heavy lanthanide elements.

Purpose of the Study:

• To assess the accuracy of perturbation-based SOC estimates for lanthanide SMMs.
• To investigate the role of SOC and electron correlation in spin relaxation mechanisms.
• To provide a more reliable computational approach for designing advanced SMMs.

Main Methods:

• Variational solution of the Dirac equation for the [DyO]+ molecule.
• Calculation of electronic structure and energy splittings.
• Analysis of the interplay between SOC and dynamic electron correlation.

Main Results:

• The Dirac equation provides a more accurate description of SOC in lanthanide systems.
• Energy splittings crucial for spin relaxation are influenced by strong SOC and electron correlation.
• The interplay affects spin-vibrational transition resonances, impacting spin relaxation time.

Conclusions:

• Advanced relativistic calculations are necessary for accurate SOC in lanthanide SMMs.
• Understanding the interplay of SOC and electron correlation is critical for optimizing SMM performance.
• This work offers a validated computational framework for developing next-generation quantum materials.