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We investigate the magnetoelectric coupling in CaMn7O12 (CMO) through a comprehensive spectroscopic analysis combining inelastic neutron scattering (INS), x-ray absorption spectroscopy (XAS), and synchrotron-based powder x-ray diffraction (PXRD). CMO's intricate interplay between magnetism and ferroelectricity is dissected to uncover its underlying mechanisms. XAS reveals a mixed valency of Mn ions in CMO, reflecting the presence of Mn3+ and Mn4+ ions, which contributes to its magnetoelectric properties. The double structure in Mn-K near-edge absorption spectra reinforces multiple Mn sites as well as the mixed valency of the compound. Synchrotron-based PXRD experiments conducted over a range of temperatures unveil structural distortions near the magnetic transition temperatures of CMO. These distortions coincide with anomalies in lattice parameters and bond lengths, shedding light on the link between structural modulations and magnetoelectric behavior. Furthermore, INS measurements identify specific energy bands (E1, E2, and E3) associated with distinct exchange interactions between Mn ions. This work advances our understanding of magnetoelectric coupling mechanisms and showcases the potential of multifunctional materials for applications in spintronics and related fields. Published by the American Physical Society 2024
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