Balancing Molecular Sensitization and Surface Passivation in Lanthanide-Doped Nanoparticle-Based Organic-Inorganic Nanohybrids.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 41150653.
- Also identified by DOI 10.1021/acs.nanolett.5c04324 and PMC identifier 12616780.
- Licence recorded as CC BY.
- The licence permits redistribution, so the abstract is shown in full and the full text is available from the publisher.
Abstract
Lanthanide-doped nanoparticles (LnNPs) are promising for advanced photonic applications due to their unique optical properties. However, their practical implementation is hindered by surface quenching and weak absorption. Surface passivation through core-shell architectures is effective in mitigating quenching. However, it creates a fundamental trade-off by impeding molecular sensitization via energy transfer (ET) in the organic-inorganic hybrid systems. Here, we investigate this trade-off by fabricating core-shell LnNPs with precisely controlled shell thicknesses ranging from 0.8 to 3.0 nm. Surface passivation yields enhancements in 290-fold upconversion intensity and 25-fold downshifting intensity. Using 9-anthracenecarboxylic acid, we demonstrate that ET efficiency exhibits a nonmonotonic dependence on the shell thickness, with optimal performance achieved at a shell thickness of ∼0.8 nm. Through steady-state and time-resolved spectroscopic studies, we elucidate the complex ET dynamics. Our findings reveal the optimal shell thickness and answer whether no shell is the best in this nanohybrid system.