A revolution in electronics is in view, with the contemporary evolution of the two novel disciplines of spintronics and molecular electronics. A fundamental link between these two fields can be established using molecular magnetic materials and, in particular, single-molecule magnets. Here, we review the first progress in the resulting field, molecular spintronics, which will enable the manipulation of spin and charges in electronic devices containing one or more molecules. We discuss the advantages over more conventional materials, and the potential applications in information storage and processing. We also outline current challenges in the field, and propose convenient schemes to overcome them.

Molecular spintronics using single-molecule magnets

Shor and Grover demonstrated that a quantum computer can outperform any classical computer in factoring numbers1 and in searching a database2 by exploiting the parallelism of quantum mechanics. Whereas Shor's algorithm requires both superposition and entanglement of a many-particle system3, the superposition of single-particle quantum states is sufficient for Grover's algorithm4. Recently, the latter has been successfully implemented5 using Rydberg atoms. Here we propose an implementation of Grover's algorithm that uses molecular magnets6,7,8,9,10, which are solid-state systems with a large spin; their spin eigenstates make them natural candidates for single-particle systems. We show theoretically that molecular magnets can be used to build dense and efficient memory devices based on the Grover algorithm. In particular, one single crystal can serve as a storage unit of a dynamic random access memory device. Fast electron spin resonance pulses can be used to decode and read out stored numbers of up to 105, with access times as short as 10-10 seconds. We show that our proposal should be feasible using the molecular magnets Fe8 and Mn12.

Quantum computing in molecular magnets

Double-decker phthalocyanine complexes with Tb3+ or Dy3+ showed slow magnetization relaxation as a single-molecular property. The temperature ranges in which the behavior was observed were far higher than that of the transition-metal-cluster single-molecule magnets (SMMs). The significant temperature rise results from a mechanism in the relaxation process different from that in the transition-metal-cluster SMMs. The effective energy barrier for reversal of the magnetic moment is determined by the ligand field around a lanthanide ion, which gives the lowest degenerate substate a large |Jz| value and large energy separations from the rest of the substates in the ground-state multiplets.

Lanthanide Double-Decker Complexes Functioning as Magnets at the Single-Molecular Level

Synthesis of 3d metallic single-molecule magnets

THE precise manner in which quantum-mechanical behaviour at the microscopic level underlies classical behaviour at the macroscopic level remains unclear, despite seventy years of theoretical investigation. Experimentally, the crossover between these regimes can be explored by looking for signatures of quantum-mechanical behaviour—such as tunneling—in macroscopic systems1. Magnetic systems (such as small grains, spin glasses and thin films) are often investigated in this way2–12 because transitions between different magnetic states can be closely monitored. But transitions between states can be induced by thermal fluctuations, as well as by tunnelling, and definitive identification of macroscopic tunnelling events in these complex systems is therefore difficult13. Here we report the results of low-temperature experiments on a single crystal composed of super-paramagnetic manganese clusters (Mn12-ac), which clearly demonstrate the existence of quantum-mechanical tunnelling of the bulk magnetization. In an applied magnetic field, the magnetization shows hysteresis loops with a distinct 'staircase' structure: the steps occur at values of the applied field where the energies of different collective spin states of the manganese clusters coincide. At these special values of the field, relaxation from one spin state to another is enhanced above the thermally activated rate by the action of resonant quantum-mechanical tunnelling. These observations corroborate the results of similar experiments performed recently on a system of oriented crystallites made from a powdered sample4.

Macroscopic quantum tunnelling of magnetization in a single crystal of nanomagnets

Macroscopic quantum tunneling in molecular magnets

Magnetization measurements have been performed on a single monocrystal of the molecule Mn12-acetate (Mn12Ac). Steps were observed in the hysteresis loop for values of the applied field at which level crossings of the collective spin states of each manganese clusters take place. At these fields, the magnetization relaxes at short time scales, being otherwise essentially blocked. This novel behavior is interpreted in terms of resonant quantum tunneling of the magnetization from thermally activated energy levels. Hysteresis loop measurements performed for different field orientations and alternating current (ac) susceptibility experiments confirm this picture.

Thermally assisted macroscopic quantum resonance on a single-crystal of Mn12-acetate

Quantum resonance of the magnetisation in a single-crystal of Mn12-ac

The dynamical properties of the magnetic moment of non-interacting cobalt nanoparticles dispersed in a polymer were investigated by ac-susceptibility (10 Hz < f < 104 Hz). We thus estimated the relaxation time of the magnetisation (τ) associated to the superparamagnetic properties of the particles. τ was found to follow the general Neel-Brown relaxation dynamics, with a pre-exponential relaxation time τ0 of 4(±2)·10−12 s for temperatures between 10 and 20 K. By combining the experimental results from ferromagnetic resonance, ac-susceptibility, and magnetisation, measurements giving the microscopic and macroscopic parameters, we demonstrate for the first time that the Coffey theoretical expressions were able to predict both τ and τ0 values. Finally, the thermal dependence of τ0 is discussed.

F. Lionti

Papers

Macroscopic quantum tunnelling of magnetization in a single crystal of nanomagnets

Macroscopic quantum tunneling in molecular magnets

Thermally assisted macroscopic quantum resonance on a single-crystal of Mn12-acetate

Quantum resonance of the magnetisation in a single-crystal of Mn12-ac

Dynamical properties of non-interacting Co nanoparticles