Magnetic excitations in molecular magnets with complex bridges: The tetrahedral molecule Ni$_4$Mo$_{12}$

TL;DR

This paper develops a modified spin Hamiltonian to analyze magnetic excitations in complex molecular magnets, successfully explaining experimental data for Ni$_4$Mo$_{12}$ by linking spectral features to molecular geometry and chemical structure.

Contribution

Introduces a novel spin Hamiltonian with discrete coupling parameters to model magnetic excitations in complex molecular magnets, applied specifically to Ni$_4$Mo$_{12}$.

Findings

The model accurately reproduces experimental magnetic excitation spectra.

Spectral features are linked to the geometry and chemical structure of exchange bridges.

The approach explains peak splitting and broadening in the excitation spectrum.

Abstract

We investigate the spectroscopic magnetic excitations in molecular magnets with complex intermediate structure among the magnetic ions. Our approach consists in introducing a modified spin Hamiltonian that allows for discrete coupling parameters accounting for all energetically favorable spatial distributions of the valence electrons along the exchange bridges connecting the constituent magnetic ions. We discuss the physical relevance of the constructed Hamiltonian and derive its eigenvalues. The model is applied to explore the magnetic excitations of the tetrameric molecular magnet Ni$_4$Mo$_{12}$. Our results are in a very good agreement with the available experimental data. We show that the experimental magnetic excitations in the named tetramer can be traced back to the specific geometry and complex chemical structure of the exchange bridges leading to the splitting and broadness of the peaks centered about 0.5 meV and 1.7 meV.