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.
Colloidal Semiconductor Nanocrystals offer a potential path forward to lowering the bar for access to Quantum Emitters. While demonstrations of single photons from nanocrystals have existed for two decades, intermittent periods of low light emission ("blinking") and transient emission from multiple emissive states ("spectral diffusion") have limited the usefulness of these sources. One underlying clue to the mechanism causing these two phenomena is whether or not these two effects are related. While evidence for blinking at fast timescales (~10s of us) is observable with modern electronics, the emission spectra cannot easily be captured at those timescales due to the inherent limitations of building up spectra in spectrometers. We utilize the indistinguishability of subsequent photons to determine the timescale spectral diffusion occurs and find that blinking can happen independently of spectral diffusion on the ~10us timescale, only becoming correlated at the ~1s timescale.
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