Unique determination of localized basis in molecular spin

TL;DR

This paper introduces a new method for uniquely determining localized basis functions in molecular spin systems, enhancing understanding of magnetic dynamics and aiding theoretical modeling.

Contribution

It proposes a novel approach leveraging time-reversal symmetry and magnetic axis orientation for localized basis determination in molecular spins.

Findings

Provides a rigorous method for basis determination

Enables clear association of spin wave functions with magnetic orientations

Simplifies modeling of magnetic dynamics in molecular systems

Abstract

Localized basis plays an important role in comprehending the magnetic dynamics in molecular spins from a physics perspective. Nonetheless, the uniqueness and rigor of its determination have received limited attention. In this study, we propose a new determination of the localized basis applicable to both non-Kramers and Kramers molecular spin systems, leveraging the time-reversal symmetry of the spin Hamiltonian and the molecular spin's main magnetic axis. By introducing this, we establish a distinct and practical means of determining the localized basis, enabling the association of a molecular spin wave function with either an "up" or "down" magnetic moment orientation in molecular spins. This finding facilitates a comprehensive interpretation of magnetic dynamics and simplifies the construction of theoretical models for materials analysis.