Many-electron multiconfigurational ab initio calculations are combined with x-ray spectroscopy to scrutinize a popular model for electron transfer in lanthanide-doped crystals which hypothesizes that the electrons are conveyed by the conduction band of the host. Contrary to this accepted picture, our combined theoretical-experimental effort shows that the reversible electron phototransfer from ${\mathrm{Eu}}^{2+}$ to ${\mathrm{Sm}}^{3+}$ in ${\mathrm{CaF}}_2$ is direct, from metal to metal. It is theoretically predicted and experimentally verified that visible light induces the reverse electron transfer.

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• Atomic & molecular clusters
• Electronic transitions
• Rare-earth doped crystals
• Configuration interaction
• Luminescence
• Optical absorption spectroscopy
• Photoluminescence
• Pump-probe spectroscopy
• Resonant inelastic x-ray scattering
• X-ray absorption near-edge spectroscopy