We report the observation of steps at regular intervals of magnetic field in the hysteresis loop of a macroscopic sample of oriented Mn 12 O 12 (CH 3 COO) 16 (H 2 O) 4 crystals. The magnetic relaxation rate increases substantially when the field is tuned to a step. We propose that these effects are manifestations of thermally assisted, field-tuned resonant tunneling between quantum spin states, and attribute the observation of quantum-mechanical phenomena on a macroscopic scale to tunneling in a large (Avogadro's) number of magnetically identical molecules. [S0031-9007(96)00131-7]

This is the first book presenting a coherent theoretical and experimental treatment of the rapidly developing field of macroscopic quantum tunneling of the magnetic moment. The theory is based on the concept of the magnetic instanton and its renormalization by the dissipative environment. The book includes discussions of the tunneling of magnetic moment in small ferromagnetic grains, tunneling of the Ne'el vector in antiferromagnetic grains, quantum nucleation of magnetic domains, and quantum depinning of domain walls. The experimental part collects the majority of recent data that are, or may be, relevant to spin tunneling. Among the topics described are low temperature magnetic relaxation and its interpretation in various systems, experiments on single particles and mesoscopic wires, and resonant spin tunneling in molecular magnets. This study of an important new field in condensed matter physics by two leading contributors to the subject will be of interest to theorists and experimentalists alike.

Interest in metal-organic open-framework structures has increased enormously in the past few years because of the potential benefits of using crystal engineering techniques to yield nanoporous materials with predictable structures and interesting properties. Here we report a new efficient methodology for the preparation of metal-organic open-framework magnetic structures based on the use of a persistent organic free radical (PTMTC), functionalized with three carboxylic groups. Using this approach, we create an open-framework structure Cu3(PTMTC)2(py)6(CH3CH2OH)2(H2O), which we call MOROF-1, combining very large pores (2.8-3.1 nm) with bulk magnetic ordering. MOROF-1 shows a reversible and highly selective solvent-induced 'shrinking-breathing' process involving large volume changes (25-35%) that strongly influence the magnetic properties of the material. This magnetic sponge-like behaviour could be the first stage of a new route towards magnetic solvent sensors.

Zero-field-cooled magnetization, magnetic relaxation, and a.c. susceptibility measurements have been performed on a Mn12-Ac oriented powdered sample as a function of temperature, field, and orientation. Magnetization jumps and susceptibility peaks have been observed about magnetic-field values Bn = nB1, where B1 ≈ 5 kG. These anomalies are due to the existence of relaxation rate maxima near Bn. From these experimental results we infer the existence of resonant spin tunnelling between degenerate excited levels of opposite spin orientation.

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