Optical spectra, crystal-field parameters, and magnetic susceptibility of the new multiferroic NdFe3(BO3)4

TL;DR

This study investigates the optical spectra, crystal-field parameters, and magnetic susceptibility of NdFe3(BO3)4, revealing its magnetic properties and exchange interactions, and providing a detailed theoretical model of its electronic structure.

Contribution

The paper presents a comprehensive analysis combining experimental optical spectra with crystal-field calculations and magnetic susceptibility modeling for NdFe3(BO3)4, a multiferroic material.

Findings

Determined energies, symmetries, and exchange splittings of Nd3+ doublets.

Calculated crystal-field parameters and magnetic g-factors.

Modeled magnetic susceptibility consistent with experimental data.

Abstract

We report high-resolution optical absorption spectra for NdFe3(BO3)4 trigonal single crystal which is known to exhibit a giant magnetoelectric effect below the temperature of magnetic ordering TN = 33 K. The analysis of the temperature-dependent polarized spectra reveals the energies and, in some cases, symmetries and exchange splittings of Nd3+ 84 Kramers doublets. We perform crystal-field calculations starting from the exchange-charge model, obtain a set of six real crystal-field parameters, and calculate wave functions and magnetic g-factors. In particular, the values g(perpendicular) = 2.385, g(parallel) = 1.376 were found for the Nd3+ ground-state doublet. We obtain Bloc=7.88 T and |JFN|= 0.48 K for the values of the local effective magnetic field at liquid helium temperatures at the Nd3+ site and the Nd - Fe exchange integral, respectively, using the experimentally measured Nd3+ ground-state splitting of 8.8 cm-1. To check reliability of our set of crystal field parameters we model the magnetic susceptibility data from literature. A dimer containing two nearest-neighbor iron ions in the spiral chain is considered to partly account for quasi-one-dimensional properties of iron borates, and then the mean-field approximation is used. The results of calculations with the exchange parameters for Fe3+ ions Jnn = -6.25 K (intra-chain interactions) and Jnnn = -1.92 K (inter-chain interactions) obtained from fitting agree well with the experimental data.