Lattice Modulation on Singlet-Triplet Splitting of Silver Cluster Boosting Near-Unity Photoluminescence Quantum Yield.

Autor: Tian WD; Shandong University, School of Chemistry and Chemical Engineering, State Key Laboratory of Crystal Materials, CHINA., Zhang C; Shandong University, School of Chemistry and Chemical Engineering, State Key Laboratory of Crystal Materials, CHINA., Paul S; Indian Institute of Technology Kharagpur, Department of Chemistry, INDIA., Si WD; Shandong University, School of Chemistry and Chemical Engineering, State Key Laboratory of Crystal Materials, CHINA., Wang Z; Shandong University, School of Chemistry and Chemical Engineering, State Key Laboratory of Crystal Materials, CHINA., Sun PP; Shandong University, School of Chemistry and Chemical Engineering, State Key Laboratory of Crystal Materials, CHINA., Anoop A; Indian Institute of Technology Kharagpur, Department of Chemistry, INDIA., Tung CH; Shandong University, School of Chemistry and Chemical Engineering, State Key Laboratory of Crystal Materials, CHINA., Sun D; Shandong University, Department of Chemistry and Chemical Engineering, Shanda South Road 27, 250100, Jinan, CHINA.
Jazyk: angličtina
Zdroj: Angewandte Chemie (International ed. in English) [Angew Chem Int Ed Engl] 2024 Dec 15, pp. e202421656. Date of Electronic Publication: 2024 Dec 15.
DOI: 10.1002/anie.202421656
Abstrakt: Developing thermally activated delayed fluorescence (TADF)-active silver clusters with near-unity quantum efficiency is of practical importance in cutting-edge optoelectronic devices, but remains a tremendous challenge due to the difficulty of de novo synthesis and uncertainty of properties. Herein, we demonstrate a lattice modulation on parent TADF-activate silver cluster, acheving TADF-driven photoluminescence quantum yield (PLQY) from 12% to near-unity. Systematic experimental and calculated results reveal that the lattice modulation effectively lower the singlet-triplet splitting (ΔEST) from 718 to 549 cm-1, thereby facilitating thermally activated reverse intersystem crossing: T5→S5, leading to extremely efficient TADF by surpassing both phosphorescence and non-radiative decay, thus boosting the near-unity PLQY. Such high PLQY are extremely rare in the TADF-active silver clusters and even in the whole noble-metal clusters. This research showcases an unparalleled example of lattice modulation to realize near unity PLQY of TADF-active silver clusters.
(© 2024 Wiley‐VCH GmbH.)
Databáze: MEDLINE
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