• Accepted Paper

Coupled magnetic and lattice excitations in multiferroic Ba3HoRu2O9: Insights from neutron scattering, Raman spectroscopy, and machine-learned phonon calculations

E. Kushwaha, S. Ghosh, G. Roy, M. Kumar, M. D. Le, J. Shannigrahi, S. D. Kaushik, D. T. Adroja, and T. Basu

Phys. Rev. B - Accepted 5 November, 2026

DOI: https://doi.org/10.1103/1fcf-72wv

Abstract

Inelastic neutron scattering (INS) spectra of} correlated 4d-4f multiferroic oxides are difficult to interpret because magnetic, crystal-field, and lattice excitations frequently overlap in energy. The hexagonal 6H perovskite Ba3HoRu2O9 provides an ideal platform to investigate this interplay owing to the coexistence of Ru2O9 molecular units and localized Ho3+ moments. To identify the contributions from these different excitations, we combine INS with linear spin-wave calculations, crystal-field analysis, Raman spectroscopy, and machine-learned force field (MLFF) phonon calculations. A magnetic excitation below 6.2~meV, observed only in the low-temperature magnetic phase, is reproduced by linear spin-wave theory a collective spin-wave excitation of the coupled Ru-Ho magnetic network. At higher energies, broad excitations centered near 20, 39, 70, and 90~meV are observed that persist far above the magnetic ordering temperatures. The magnetic part of the 39~meV excitation, isolated by subtracting the Bose-corrected high-temperature data, follows the Ho3+ magnetic form factor. Crystal-field calculations based on the Stevens formalism place a group of strong Ho3+ transitions in this energy range, while Raman spectroscopy and MLFF phonon calculations identify optical phonons with comparable energies. Together, these complementary results show that the broad INS feature near 39~meV arises from overlapping Ho3+ crystal-field excitations and lattice vibrations. These findings establish a microscopic framework for understanding the interplay between spin, crystal-field, and lattice degrees of freedom in this multiferroic 4d-4f compound.

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