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Dye sensitization is becoming a new dimension to highly improve the upconversion luminescence (UCL) of lanthanide-doped upconversion nanoparticles (UCNPs). However, there is still a lack of general understanding of the dye-UCNPs interactions, especially the confused large mismatch between the inputs and outputs. By taking dye-sensitized NaYF 4 :Yb/Er@NaYF 4 :Nd UCNPs as a model system, we not only revealed the in-depth energy-dissipative process for dye-sensitized UCL but also confirmed the first ever experimental observation of the energy back transfer (EBT) in the dye-sensitized UCL. Furthermore, this energy-dissipative EBT restricted the optimal ratio of dyes to UCNP. By unearthing all of the energy loss behind the EBT, energy transfer, and energy migration processes, this paper sheds light on the further design of effective dye-sensitized nanosystems for UCL or even downconversion luminescence.

Ultrastrong Absorption Meets Ultraweak Absorption: Unraveling the Energy-Dissipative Routes for Dye-Sensitized Upconversion Luminescence