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Stabilization of ultra-small [Ag2](2+) and [Agm](n+) nano-clusters through negatively charged tetrahedrons in oxyfluoride glass networks: To largely enhance the luminescence quantum yields

Abstract : Herein, three different silver species were stably formed in SiO-AlO-BO-NaO-ZnF-CaF glasses and were identified by their characteristic luminescence bands: violet blue luminescence (Ag: 4d5s → 4d), green white molecular fluorescence (molecule-like [Ag], named ML-Ag) and orange molecular fluorescence ([Ag] pairs). Due to the relatively low aggregation degrees of [Ag] and [Ag], non-radiative transitions were highly suppressed, and the PL quantum yields (QYs) of ML-Ag and [Ag] pairs reached 73.7% and 89.7%, respectively. The substitution of 0.5BO-0.5NaO with SiO promoted the partial reduction of Ag to Ag and the subsequent aggregation of Ag and Ag to form [Ag] (ML-Ag). The absence of NaO also resulted in an increasing amount of Ag-Ag pairs with closing interionic distance to form [Ag] in glass. According to the X-ray photoelectron spectra (XPS) and magic angle spinning (MAS) nuclear magnetic resonance (NMR) spectra, a solubility strategy and a charge compensation model were proposed to describe the transformations between different silver species. The formation of ML-Ag was further controlled via the solubility of Ag in glass, whereas [Ag] centers could be effectively produced by lowering the total amount of other competitive charge compensators, such as Na, or by introducing negatively charged [BO], [AlO], and [ZnO] tetrahedrons into the glass matrix.
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https://hal-univ-rennes1.archives-ouvertes.fr/hal-01579655
Contributor : Laurent Jonchère <>
Submitted on : Thursday, August 31, 2017 - 2:41:22 PM
Last modification on : Friday, July 10, 2020 - 4:24:51 PM

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Ronghua Ma, Junjie Zhao, Xiaotong Chen, Xvsheng Qiao, Xianping Fan, et al.. Stabilization of ultra-small [Ag2](2+) and [Agm](n+) nano-clusters through negatively charged tetrahedrons in oxyfluoride glass networks: To largely enhance the luminescence quantum yields. Physical Chemistry Chemical Physics, Royal Society of Chemistry, 2017, 19 (34), pp.22638-22645. ⟨10.1039/c7cp02531a⟩. ⟨hal-01579655⟩

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