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Charge transfer-mediated sensitization of lanthanide dopants by perovskite quantum dots

The electronically isolated f-orbitals of Ln3+ ions endow these species ultranarrow (atom-like) emission with a long lifetime, which are suitable for the optical generation and propagation of spin qubits, even after the coordination inside the semiconductor matrices. To overcome the low extinction coefficient of the Ln3+ ions, indirect sensitization of Ln3+ ions via energy transfer from the perovskite quantum dots (QDs) is performed through partial substitution of the perovskite matrix with Ln3+ ions. Here, we suggest a charge transfer type intermediate is involved in the energy transfer process, rather than utilizing conventional Forster or Dexter energy transfer. By comparing the static and dynamic process of the perovskite QDs doped with seven different Ln3+ species, we find that only Ln3+ species with low Ln2+ formation energy further advances the non-radiative recombination of the QDs’ delocalized charge carriers, which can potentially sensitize the Ln3+ excited states. The formation of the Ln2+ state naturally implies that energy transfer proceeds through sequential electron and hole transfer. The general mechanistic understanding of Ln3+ dopant sensitization opens the door for targeting multiple emission wavelengths by choosing the right combination of host matrices and Ln3+ species.