Spin-enhanced magnetocaloric effect in molecular nanomagnets

An unusually large magnetocaloric effect for the temperature region below 10 K is found for the Fe-14 molecular nanomagnet. This is to large extent caused by its extremely large spin S ground state combined with an excess of entropy arising from the presence of low-lying excited S states. We also show that the highly symmetric Fe-14 cluster core, resulting in small cluster magnetic anisotropy, enables the occurrence of long-range antiferromagnetic order below T-N=1.87 K

Enhanced magnetocaloric effect in frustrated magnetic molecules with icosahedral symmetry

We investigate the magnetocaloric properties of certain antiferromagnetic spin systems that have already been or very likely can be synthesized as magnetic molecules. It turns out that the special geometric frustration which is present in antiferromagnets that consist of corner-sharing triangles leads to an enhanced magnetocaloric effect with high cooling rates in the vicinity of the saturation field. These findings are compared with the behavior of a simple unfrustrated spin ring as well as with the properties of the icosahedron. To our surprise, also for the icosahedron large cooling rates can be achieved but due to a different kind of geometric frustration.Comment: 5 pages, 8 figures, more information at http://obelix.physik.uni-osnabrueck.de/~schnack

Influence of antisymmetric exchange interaction on quantum tunneling of magnetization in a dimeric molecular magnet Mn6

We present magnetization measurements on the single molecule magnet Mn6, revealing various tunnel transitions inconsistent with a giant-spin description. We propose a dimeric model of the molecule with two coupled spins S=6, which involves crystal-field anisotropy, symmetric Heisenberg exchange interaction, and antisymmetric Dzyaloshinskii-Moriya exchange interaction. We show that this simplified model of the molecule explains the experimentally observed tunnel transitions and that the antisymmetric exchange interaction between the spins gives rise to tunneling processes between spin states belonging to different spin multiplets.Comment: 5 pages, 4 figure

Direct Observation of Quantum Coherence in Single-Molecule Magnets

Direct evidence of quantum coherence in a single-molecule magnet in frozen solution is reported with coherence times as long as T2 = 630 ns. We can strongly increase the coherence time by modifying the matrix in which the single-molecule magnets are embedded. The electron spins are coupled to the proton nuclear spins of both the molecule itself and interestingly, also to those of the solvent. The clear observation of Rabi oscillations indicates that we can manipulate the spin coherently, an essential prerequisite for performing quantum computations.Comment: 5 Pages, 4 Figures, final version published in PR

Tunable dipolar magnetism in high-spin molecular clusters

We report on the Fe17 high-spin molecular cluster and show that this system is an exemplification of nanostructured dipolar magnetism. Each Fe17 molecule, with spin S=35/2 and axial anisotropy as small as D=-0.02K, is the magnetic unit that can be chemically arranged in different packing crystals whilst preserving both spin ground-state and anisotropy. For every configuration, molecular spins are correlated only by dipolar interactions. The ensuing interplay between dipolar energy and anisotropy gives rise to macroscopic behaviors ranging from superparamagnetism to long-range magnetic order at temperatures below 1K.Comment: Replaced with version accepted for publication in Physical Review Letter

Relaxation dynamics in a Fe7 nanomagnet

We investigate the phonon-induced relaxation dynamics in the Fe 7 magnetic molecule, which is made of two Fe 3 + triangles bridged together by a central Fe 3 + ion. The competition between different antiferromagnetic exchange interactions leads to a low-spin ground state multiplet with a complex pattern of low-lying excited levels. We theoretically investigate the decay of the time correlation function of molecular observables, such as the cluster magnetization, due to the spin-phonon interaction. We find that more than one time contributes to the decay of the molecular magnetization. The relaxation dynamics is probed by measurements of the nuclear spin-lattice relaxation rate 1 /T 1 . The interpretation of these measurements allows the determination of the magnetoelastic coupling strength and to set the scale factor of the relaxation dynamics time scales. In our theoretical interpretation of 1 /T 1 data we also take into account the wipeout effect at low temperature

Tracking nuclear motion in single-molecule magnets using femtosecond X-ray absorption spectroscopy

The development of new data storage solutions is crucial for emerging digital technologies. Recently, all-optical magnetic switching has been achieved in dielectrics, proving to be faster than traditional methods. Despite this, single-molecule magnets (SMMs), which are an important class of magnetic materials due to their nanometre size, remain underexplored for ultrafast photomagnetic switching. Herein, we report femtosecond time-resolved K-edge X-ray absorption spectroscopy (TR-XAS) on a Mn(III)-based trinuclear SMM. Exploiting the elemental specificity of XAS, we directly track nuclear dynamics around the metal ions and show that the ultrafast dynamics upon excitation of a crystal-field transition are dominated by a magnetically active Jahn-Teller mode. Our results, supported by simulations, reveal minute bond length changes from 0.01 to 0.05 \uc5 demonstrating the sensitivity of the method. These geometrical changes are discussed in terms of magneto-structural relationships and consequently our results illustrate the importance of TR-XAS for the emerging area of ultrafast molecular magnetism