Abstract

We combined high field magnetization and magneto-optical spectroscopy to investigate spin-charge coupling in Mn-substituted rare-earth indium oxides of chemical formula $R{\mathrm{In}}_{1\ensuremath{-}x}{\mathrm{Mn}}_{x}{\mathrm{O}}_{3}$ ($R=\text{Tb}$, Dy). The edge states, on-site ${\mathrm{Mn}}^{3+}\phantom{\rule{0.16em}{0ex}}d$ 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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