Master Equations for pulsed magnetic fields: Application to magnetic molecules

We extend spin-lattice relaxation theory to incorporate the use of pulsed magnetic fields for probing the hysteresis effects and magnetization steps and plateaus exhibited, at low temperatures, by the dynamical magnetization of magnetic molecules. The main assumption made is that the lattice degrees of freedom equilibrate in times much shorter than both the experimental time scale (determined by the sweep rate) and the typical spin-lattice relaxation time. We first consider the isotropic case (a magnetic molecule with a ground state of spin $S$ well separated from the excited levels and also the general isotropic Heisenberg Hamiltonian where all energy levels are relevant) and then we include small off-diagonal terms in the spin Hamiltonian to take into account the Landau-Zener-St\"{u}ckelberg (LZS) effect. In the first case, and for an $S=1/2$ magnetic molecule we arrive at the generalized Bloch equation recently used for the magnetic molecule \{V$_6$\} in Phys. Rev. Lett. 94, 147204 (2005). An analogous equation is derived for the magnetization, at low temperatures, of antiferromagnetic ring systems. The LZS effect is discussed for magnetic molecules with a low spin ground state, for which we arrive at a very convenient set of equations that take into account the combined effects of LZS and thermal transitions. In particular, these equations explain the deviation from exact magnetization reversal at $B\approx 0$ observed in \{V$_6$\}. They also account for the small magnetization plateaus (``magnetic Foehn effect''), following the LZS steps, that have been observed in several magnetic molecules. Finally, we discuss the role of the Phonon Bottleneck effect at low temperatures and specifically we indicate how this can give rise to a pronounced Foehn effect.Comment: 10 pages, 4 figure

Zero-field Time Correlation Functions of Four Classical Heisenberg Spins on a Ring

A model relevant for the study of certain molecular magnets is the ring of N=4 classical spins with equal near-neighbor isotropic Heisenberg exchange interactions. Assuming classical Heisenberg spin dynamics, we solve explicitly for the time evolution of each of the spins. Exact triple integral representations are derived for the auto, near-neighbor, and next-nearest-neighbor time correlation functions for any temperature. At infinite temperature, the correlation functions are reduced to quadrature. We then evaluate the Fourier transforms of these functions in closed form, which are double integrals. At low temperatures, the Fourier transform functions explicitly demonstrate the presence of magnons. Our exact results for the infinite temperature correlation functions in the long-time asymptotic limit differ qualitatively from those obtained assuming diffusive spin dynamics. Whether such explicitly non-hydrodynamic behavior would be maintained for large-N rings is discussed.Comment: 18 pages, 21 figure

Theory of severe slowdown in the relaxation of rings and clusters with antiferromagnetic interactions

We show that in the severe slowing down temperature regime the relaxation of antiferromagnetic rings and similar magnetic nanoclusters is governed by the quasi-continuum portion of their quadrupolar fluctuation spectrum and not by the lowest excitation lines. This is at the heart of the intriguing near-universal power-law temperature dependence of the electronic correlation frequency $\omega_c$ with an exponent close to 4. The onset of this behavior is defined by an energy scale which is fixed by the lowest spin gap $\Delta_0$. This explains why experimental curves of $\omega_c$ for different cluster sizes and spins nearly coincide when $T$ is rescaled by $\Delta_0$.Comment: new slightly extended version (6 pages, 1 fig. added

Metamagnetic phase transition of the antiferromagnetic Heisenberg icosahedron

The observation of hysteresis effects in single molecule magnets like Mn$_{12}$-acetate has initiated ideas of future applications in storage technology. The appearance of a hysteresis loop in such compounds is an outcome of their magnetic anisotropy. In this Letter we report that magnetic hysteresis occurs in a spin system without any anisotropy, specifically, where spins mounted on the vertices of an icosahedron are coupled by antiferromagnetic isotropic nearest-neighbor Heisenberg interaction giving rise to geometric frustration. At T=0 this system undergoes a first order metamagnetic phase transition at a critical field \Bcrit between two distinct families of ground state configurations. The metastable phase of the system is characterized by a temperature and field dependent survival probability distribution.Comment: 4 pages, 4 figures, submitted to Physical Review Letter

Determination of exchange energies in the sawtooth spin ring {Mo75V20} by ESR

The magnetism of the polyoxometalate cluster {Mo75V20}, containing a sawtooth ring of 10 corner-sharing triangles located on the equator of the barrel-shaped molecule, has remained debatable since it is masked by contributions from impurities as well as temperature-independent paramagnetism. In this article we demonstrate the usefulness of ESR measurements since the temperature dependence of the ESR intensity can discriminate between impurity and molecular contributions. We determine the exchange parameters and therefore also the low-lying spectrum of {Mo75V20}, especially the low-lying singlet states which so far have been probed solely by specific heat measurements.Comment: 5 pages, 5 figures, submitted to PR