Quenched Spin Tunneling and Diabolical Points in Magnetic Molecules: I. Symmetric Configurations

Abstract

The perfect quenching of spin tunneling that has previously been discussed in terms of interfering instantons, and has recently been observed in the magnetic molecule \Fe8, is treated using a discrete phase integral (or Wentzel-Kramers-Brillouin) method. The simplest model Hamiltonian for the phenomenon leads to a Schrödinger equation that is a five-term recursion relation. This recursion relation is reflection-symmetric when the magnetic field applied to the molecule is along the hard magnetic axis. A completely general Herring formula for the tunnel splittings for all reflection-symmetric five-term recursion relations is obtained. Using connection formulas for a new type of turning point that may be described as lying "under the barrier", and which underlies the oscillations in the splitting as a function of magnetic field, this Herring formula is transformed into two other formulas that express the splittings in terms of a small number of action and action-like integrals. These latter formulas appear to be generally valid, even for problems where the recursion contains more than five terms. The results for the model Hamiltonian are compared with experiment, numerics, previous instanton based approaches, and the limiting case of no magnetic field.