Over 99% Photoluminescence Quantum Yield by Kernel Regulation in 8-Hydroxyquinoline-Based Icosahedral Sn<sub>12</sub>-Oxo Cluster.
basic_science · Level V
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- Record sourced from PubMed, PMID 41031603.
- Also identified by DOI 10.1021/acsnano.5c13021.
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Abstract
Luminescent metal nanoclusters are of great importance as an alternative to rare-earth phosphors for white light-emitting diodes (WLEDs), but they usually show low photoluminescence quantum yield (PLQY) due to a lack of effective control over relaxation and radiation induced by kernel-ligand interaction. Here, a hydrolysis-delayed coordination synthetic strategy is developed in 8-hydroxyquinoline-based tin-oxo clusters covering from doubly vertex-missed icosahedral <b>Sn</b><sub><b>10</b></sub> to icosahedral <b>Sn</b><sub><b>12</b></sub> and <b>Sn</b><sub><b>12</b></sub><b>-Me</b>. 99.29% ultrabright green PLQY is achieved in <b>Sn</b><sub><b>12</b></sub>, exhibiting a 6.4-fold enhancement compared to 15.43% in <b>Sn</b><sub><b>10</b></sub>. Femtosecond transient absorption spectroscopy and time-dependent density functional theory reveal a kernel-regulated ligand-centered emission mechanism: the rigid kernel suppresses nonradiative decay through core-to-shell confinement effects, while structural deformation in an unstable kernel disrupts electronic coupling, thereby reducing radiative transitions. <b>Sn</b><sub><b>12</b></sub>-based WLEDs demonstrate a high color rendering index of up to 87.7, as well as adjustable correlated color temperature. This work provides key insight into high PLQY and suitable solid-state lighting luminescent nanoclusters via kernel regulation.