A Microscopic and Spectroscopic View of Quantum Tunneling of Magnetization

TL;DR

This paper provides a microscopic and spectroscopic analysis of quantum tunneling of magnetization in single-molecule magnets, emphasizing the role of exchange interactions, symmetry, and higher order effects on tunneling behavior.

Contribution

It introduces a detailed group theoretic framework and experimental insights to understand how exchange strength and symmetry influence quantum tunneling of magnetization.

Findings

Strong exchange leads to $D_{2h}$ symmetry in the spin Hamiltonian.

Weaker exchange allows additional symmetries via excited state mixing.

Magnetization hysteresis and EPR measurements support the theoretical models.

Abstract

This chapter takes a microscopic view of quantum tunneling of magnetization (QTM) in single-molecule magnets (SMMs), focusing on the interplay between exchange and anisotropy. Careful consideration is given to the relationship between molecular symmetry and the symmetry of the spin Hamiltonian that dictates QTM selection rules. Higher order interactions that can modify the usual selection rules are shown to be very sensitive to the exchange strength. In the strong coupling limit, the spin Hamiltonian possess rigorous $D_{2h}$ symmetry (or $C_{\infty}$ in high-symmetry cases). In the case of weaker exchange, additional symmetries may emerge through mixing of excited spin states into the ground state. Group theoretic arguments are introduced to support these ideas, as are extensive results of magnetization hysteresis and electron paramagnetic resonance measurements.