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We combined high field magnetization and magneto-optical spectroscopy to investigate spincharge coupling in Mn-substituted rare-earth indium oxides of chemical formula RIn1−xMnxO3 (R = Tb, Dy). The edge states, on-site Mn 3+ d to d excitations, and rare-earth f -manifold excitations all track the magnetization energy due to dominant Zeeman interactions. The field-induced modifications to the rare-earth excitations are quite large because spin-orbit coupling naturally mixes spin and charge, suggesting that the next logical step in the design strategy should be to bring spin-orbit coupling onto the trigonal bipyramidal chromophore site with a 4 or 5d center.

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