Tuning the energetics and tailoring the optical properties of silver clusters confined in zeolites.
The integration of metal atoms and clusters in well-defined dielectric cavities is a powerful strategy to impart new properties to them that depend on the size and geometry of the confined space as well as on metal-host electrostatic interactions. Here, we unravel the dependence of the electronic properties of metal clusters on space confinement by studying the ionization potential of silver clusters embedded in four different zeolite environments over a range of silver concentrations. Extensive characterization reveals a strong influence of silver loading and host environment on the cluster ionization potential, which is also correlated to the cluster's optical and structural properties. Through fine-tuning of the zeolite host environment, we demonstrate photoluminescence quantum yields approaching unity. This work extends our understanding of structure-property relationships of small metal clusters and applies this understanding to develop highly photoluminescent materials with potential applications in optoelectronics and bioimaging.
ISIS &icFRC, Université de Strasbourg &CNRS, 8, allée Gaspard Monge, 67000 Strasbourg, France.
Oliver
O
Fenwick
Department of Chemistry, KU Leuven, Celestijnenlaan 200F, B-3001 Leuven, Belgium.
Eduardo
E
Coutiño-Gonzalez
Laboratory of Solid State Physics and Magnetism, KU Leuven, Celestijnenlaan 200D, B-3001 Leuven, Belgium.
Didier
D
Grandjean
Department of Chemistry, KU Leuven, Celestijnenlaan 200F, B-3001 Leuven, Belgium.
Wouter
W
Baekelant
ISIS &icFRC, Université de Strasbourg &CNRS, 8, allée Gaspard Monge, 67000 Strasbourg, France.
Fanny
F
Richard
ISIS &icFRC, Université de Strasbourg &CNRS, 8, allée Gaspard Monge, 67000 Strasbourg, France.
Sara
S
Bonacchi
Department of Microbial and Molecular Systems, KU Leuven, Celestijnenlaan 200F, B-3001 Leuven, Belgium.
Dirk
D
De Vos
Laboratory of Solid State Physics and Magnetism, KU Leuven, Celestijnenlaan 200D, B-3001 Leuven, Belgium.
Peter
P
Lievens
Department of Microbial and Molecular Systems, KU Leuven, Celestijnenlaan 200F, B-3001 Leuven, Belgium.
Maarten
M
Roeffaers
Department of Chemistry, KU Leuven, Celestijnenlaan 200F, B-3001 Leuven, Belgium.
Johan
J
Hofkens
ISIS &icFRC, Université de Strasbourg &CNRS, 8, allée Gaspard Monge, 67000 Strasbourg, France.
Paolo
P
Samorì