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Issue 34, 2017
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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

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Abstract

Herein, three different silver species were stably formed in SiO2–Al2O3–B2O3–Na2O–ZnF2–CaF2 glasses and were identified by their characteristic luminescence bands: violet blue luminescence (Ag+: 4d95s1 → 4d10), green white molecular fluorescence (molecule-like [Agm]n+, named ML-Ag) and orange molecular fluorescence ([Ag2]2+ pairs). Due to the relatively low aggregation degrees of [Agm]n+ and [Ag2]2+, non-radiative transitions were highly suppressed, and the PL quantum yields (QYs) of ML-Ag and [Ag2]2+ pairs reached 73.7% and 89.7%, respectively. The substitution of 0.5B2O3−0.5Na2O with SiO2 promoted the partial reduction of Ag+ to Ag0 and the subsequent aggregation of Ag+ and Ag0 to form [Agm]n+ (ML-Ag). The absence of Na2O also resulted in an increasing amount of Ag+–Ag+ pairs with closing interionic distance to form [Ag2]2+ 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 [Ag2]2+ centers could be effectively produced by lowering the total amount of other competitive charge compensators, such as Na+, or by introducing negatively charged [BO4], [AlO4], and [ZnO4]2− tetrahedrons into the glass matrix.

Graphical abstract: 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

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Publication details

The article was received on 18 Apr 2017, accepted on 30 May 2017 and first published on 30 May 2017


Article type: Paper
DOI: 10.1039/C7CP02531A
Citation: Phys. Chem. Chem. Phys., 2017,19, 22638-22645
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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

    R. Ma, J. Zhao, X. Chen, X. Qiao, X. Fan, J. Du and X. Zhang, Phys. Chem. Chem. Phys., 2017, 19, 22638
    DOI: 10.1039/C7CP02531A

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