Employing Radicals and Bismuth in Lanthanide Single-Molecule Magnet Design
Molecules that possess an energy barrier to spin inversion have intriguing potential
applications in areas such as magnetic refrigeration, molecular spintronics and high-density
information storage. For these applications, however, key performance characteristics such
as large spin-relaxation barriers (Ueff) and high magnetic blocking temperatures (TB) are
required. Lanthanides have been proven to be particularly well-suited for the design of singlemolecule
magnets owing to their large magnetic moments and magnetic anisotropy that stem
from strong spin-orbit coupling of the 4f orbitals. By using lanthanide ions such as Tb3+, Dy3+,
and Er3+ which possess intrinsically large orbital angular momentum, significantly higher Ueff
and TB can be achieved. A general methodology to improve TB in multinuclear single-molecule
magnets is to generate strong magnetic exchange between lanthanide centers through the
employment of radical bridging ligands with diffuse spin orbitals that can penetrate the core
electron density of the lanthanide ions where the 4f spin orbitals lie buried. Another successful
approach to strong coupling targets the use of heavy p-block elements since their diffuse
valence orbitals facilitate better penetration of the core electron density of the lanthanide ions
relative to diamagnetic ligands comprising lighter p-block elements. Here, we will present the
synthesis of multiple lanthanide single-molecule magnets that contain radical ligands and
bismuth clusters, respectively [1-3]. The latter class of compounds were synthesized through a
solution organometallic approach and represent the first single-molecule magnets containing
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