Master Equations for pulsed magnetic fields: Application to magnetic molecules

TL;DR

This paper develops a generalized spin-lattice relaxation theory for pulsed magnetic fields, explaining magnetization phenomena in magnetic molecules, including hysteresis, Landau-Zener-Stückelberg effects, and phonon bottleneck influences.

Contribution

It introduces a new set of equations incorporating LZS effects and phonon bottleneck phenomena, extending existing models for magnetic molecule magnetization dynamics under pulsed fields.

Findings

Derived generalized Bloch equations for $S=1/2$ molecules.

Explained deviations in magnetization reversal near zero field.

Accounted for small magnetization plateaus observed experimentally.

Abstract

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.