The magnet-like behavior can beobserved by slow relaxation of the magnetization below theblocking temperature. Since the discovery of SMMs in theearly 1990s, this assumption has formed the basis for theunderstanding of the origin of the anisotropic barrier.However, in recent years the development of novel lantha-nide-only SMMs that challenge and defy this theory pose anumber of questions:

A Polynuclear Lanthanide Single-Molecule Magnet with a Record

Engineering intramolecular exchange interactions between magnetic metal atoms is a ubiquitous strategy for designing molecular magnets. For lanthanides, the localized nature of 4f electrons usually results in weak exchange coupling. Mediating magnetic interactions between lanthanide ions via radical bridges is a fruitful strategy towards stronger coupling. In this work we explore the limiting case when the role of a radical bridge is played by a single unpaired electron. We synthesize an array of air-stable Ln2@C80(CH2Ph) dimetallofullerenes (Ln2 = Y2, Gd2, Tb2, Dy2, Ho2, Er2, TbY, TbGd) featuring a covalent lanthanide-lanthanide bond. The lanthanide spins are glued together by very strong exchange interactions between 4f moments and a single electron residing on the metal–metal bonding orbital. Tb2@C80(CH2Ph) shows a gigantic coercivity of 8.2 Tesla at 5 K and a high 100-s blocking temperature of magnetization of 25.2 K. The Ln-Ln bonding orbital in Ln2@C80(CH2Ph) is redox active, enabling electrochemical tuning of the magnetism. Dilanthanide complexes that possess radical bridges exhibit enhanced magnetic exchange coupling, affording molecular magnets with high blocking temperatures. Here, the authors explore a series of dilanthanide-encapsulated fullerenes where the radical bridge is taken to its limit and the role is played by a single unpaired electron.

/pdf/air-stable-redox-active-nanomagnets-with-lanthanide-spins-1ayambrtva.pdf

Air-stable redox-active nanomagnets with lanthanide spins radical-bridged by a metal-metal bond.

Recently, the field of molecular magnets has experienced a remarkable result: magnetic remanence above liquid nitrogen temperatures (> 77 K); this represents the first example of a Single-Molecule Magnet (SMM) that holds technological relevance. Here, we review the seminal lanthanide-based SMMs which led to the findings of remanence at 80 K. The scalability of the design principles employed in molecular systems is examined and applied with the goal of achieving functional hybrid materials and single-atom magnets on surfaces. With the future objective of molecule-based memory, it is imperative that the inherent magnetic anisotropy of lanthanides be preserved in advanced materials.

Magnetic Axiality: Design Principles from Molecules to Materials

Emerging Trends on Designing High-Performance Dysprosium(III) Single-Molecule Magnets

Combining Ising-type magnetic anisotropy with collinear magnetic interactions in single-molecule magnets (SMMs) is a significant synthetic challenge. Herein we report a Dy[15-MCCu -5] (1-Dy) SMM, where a DyIII ion is held in a central pseudo-D5h pocket of a rigid and planar Cu5 metallacrown (MC). Linking two Dy[15-MCCu -5] units with a single hydroxide bridge yields the double-decker {Dy[15-MCCu -5]}2 (2-Dy) SMM where the anisotropy axes of the two DyIII ions are nearly collinear, resulting in magnetic relaxation times for 2-Dy that are approximately 200 000 times slower at 2 K than for 1-Dy in zero external field. Whereas 1-Dy and the YIII -diluted Dy@2-Y analogue do not show remanence in magnetic hysteresis experiments, the hysteresis data for 2-Dy remain open up to 6 K without a sudden drop at zero field. In conjunction with theoretical calculations, these results demonstrate that the axial ferromagnetic Dy-Dy coupling suppresses fast quantum tunneling of magnetization (QTM). The relaxation profiles of both complexes curiously exhibit three distinct exponential regimes, and hold the largest effective energy barriers for any reported d-f SMMs up to 625 cm-1 .

Opening Magnetic Hysteresis by Axial Ferromagnetic Coupling: From Mono-Decker to Double-Decker Metallacrown

https://pubs.rsc.org/en/content/articlepdf/2018/CC/C8CC04736G

Carbide clusterfullerene DyYTiC@C80 featuring three different metals in the endohedral cluster and its single-ion magnetism

https://pubs.rsc.org/en/content/articlepdf/2018/cc/c8cc05029e

Strong carbon cage influence on the single molecule magnetism in Dy–Sc nitride clusterfullerenes

Relaxation of magnetization in endohedral metallofullerenes DySc2N@C80 is studied at different temperatures, in different magnetic fields, and in different molecular arrangements. Magnetization behavior and relaxation are analyzed for powder sample, and for DySc2N@C80 diluted in non-magnetic fullerene Lu3N@C80, adsorbed in voids of a metal–organic framework, and dispersed in a polymer. The magnetic field dependence and zero-field relaxation are also studied for single-crystals of DySc2N@C80 co-crystallized with Ni(II) octaethylporphyrin, as well as for the single crystal diluted with Lu3N@C80. Landau–Zener theory is applied to analyze quantum tunneling of magnetization in the crystals. The field dependence of relaxation rates revealed a dramatic dependence of the zero-field tunneling resonance width on the dilution and is explained with the help of an analysis of dipolar field distributions. AC magnetometry is used then to get access to the relaxation of magnetization in a broader temperature range, from 2 to 87 K. Finally, a theoretical framework describing the spin dynamics with dissipation is proposed to study magnetization relaxation phenomena in single molecule magnets.

/pdf/magnetization-relaxation-in-the-single-ion-magnet-dysc2n-c80-50v5sf33q7.pdf

Magnetization relaxation in the single-ion magnet DySc2N@C80: quantum tunneling, magnetic dilution, and unconventional temperature dependence

Tremendous progress in the development of single molecule magnets (SMMs) raises the question of their device integration. On this route, understanding the properties of low-dimensional assemblies of SMMs, in particular in contact with electrodes, is a necessary but difficult step. Here, it is shown that fullerene SMM self-assembled on metal substrate from solution retains magnetic hysteresis up to 10 K. Fullerene-SMM DySc2N@C80 and Dy2ScN@C80 are derivatized to introduce a thioacetate group, which is used to graft SMMs on gold. Magnetic properties of grafted SMMs are studied by X-ray magnetic circular dichroism and compared to the films of nonderivatized fullerenes prepared by sublimation. In self-assembled films, the magnetic moments of the Dy ions are preferentially aligned parallel to the surface, which is different from the disordered orientation of endohedral clusters in nonfunctionalized fullerenes. Whereas chemical derivatization reduces the blocking temperature of magnetization and narrows the hysteresis of Dy2ScN@C80, for DySc2N@C80 equally broad hysteresis is observed as in the fullerene multilayer. Magnetic bistability in the DySc2N@C80 grafted on gold is sustained up to 10 K. This study demonstrates that self-assembly of fullerene-SMM derivatives offers a facile solution-based procedure for the preparation of functional magnetic sub-monolayers with excellent SMM performance.

https://onlinelibrary.wiley.com/doi/pdf/10.1002/advs.202000777

Magnetic Hysteresis at 10 K in Single Molecule Magnet Self-Assembled on Gold

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Papers

Carbide clusterfullerene DyYTiC@C80 featuring three different metals in the endohedral cluster and its single-ion magnetism

Strong carbon cage influence on the single molecule magnetism in Dy–Sc nitride clusterfullerenes

Magnetization relaxation in the single-ion magnet DySc2N@C80: quantum tunneling, magnetic dilution, and unconventional temperature dependence

Magnetic Hysteresis at 10 K in Single Molecule Magnet Self-Assembled on Gold