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High pressure induced spin changes and magneto-structural correlations in hexametallic SMMs
Alessandro Prescimone1, Constantinos J Milios, Javier Sanchez-Benitez
1Centre for Science at Extreme Conditions, The University of Edinburgh, UK.
High pressure distorts polymetallic clusters, weakening magnetic exchange and altering ground states. This structural change impacts single-molecule magnet behavior, reducing energy barriers for magnetization reversal.
Area of Science:
- Materials Science
- Solid State Physics
- Magnetism
Background:
- Polymetallic clusters are investigated for their unique magnetic properties.
- Single-molecule magnets (SMMs) exhibit slow magnetic relaxation, making them promising for data storage and quantum computing.
- Understanding structure-property relationships is crucial for designing advanced magnetic materials.
Purpose of the Study:
- To investigate the combined effects of high pressure on the structure and magnetic properties of two polymetallic clusters.
- To correlate structural distortions with changes in magnetic exchange interactions and ground states.
- To determine how pressure influences the magnetic anisotropy and energy barriers in single-molecule magnets.
Main Methods:
- High-pressure single-crystal X-ray diffraction was employed to analyze structural changes.
- High-pressure magnetic susceptibility (dc and ac) measurements were performed.
- Analysis of magnetic data was used to determine changes in magnetic exchange coupling (|J|) and anisotropy (|D|).
Main Results:
- Significant structural distortions of the metallic skeletons were observed at 1.5 GPa.
- Hydrostatic pressure weakened the magnetic exchange interactions between metal centers by flattening Mn-N-O-Mn torsion angles.
- One magnetic interaction switched from ferromagnetic to antiferromagnetic, and Jahn-Teller axes reoriented.
- Ground states changed from S=12 to S=11 for compound 1 and S=10 for compound 2.
- A decrease in |D| was observed, and the effective energy barrier for magnetization reversal significantly decreased.
Conclusions:
- High pressure directly influences the structure and magnetic properties of polymetallic clusters.
- Structural changes, particularly the reorientation of Jahn-Teller axes, are key to modifying magnetic exchange and ground states.
- The observed pressure-induced changes highlight the tunability of SMM properties and offer insights for designing pressure-resistant magnetic materials.
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