期刊
ACS NANO
卷 9, 期 2, 页码 1801-1808出版社
AMER CHEMICAL SOC
DOI: 10.1021/nn506715t
关键词
local-field effects; nanocrystals; radiative decay; luminescence quantum yield; lanthanide luminescence
类别
资金
- Nederlandse Organisatie voor Wetenschappelijk Onderzoek (NWO)
Nanocrystals (NCs) doped with luminescent ions form an emerging class of materials. In contrast to excitonic transitions in semiconductor NCs, the optical transitions are localized and not affected by quantum confinement. The radiative decay rates of the dopant emission in NCs are nevertheless different from their bulk analogues due to photonic effects, and also the luminescence quantum yield (QY, important for applications) is affected. In the past, different theoretical models have been proposed to describe the photonic effects for dopant emission in NCs, with little experimental validation. In this work we investigate the photonic effects on the radiative decay rate of luminescent doped NCs using 4 nm LaPO4 NCs doped with Ce3+ or Tb3+ ions in different refractive index solvents and bulk crystals. We demonstrate that the measured influence of the refractive index on the radiative decay rate of the Ce3+ emission, having near unity QY, is in excellent agreement with the theoretical nanocrystal-cavity model. Furthermore, we show how the nanocrystal-cavity model can be used to quantify the nonunity QY of Tb3+-doped LaPO4 NCs and demonstrate that, as a general rule, the QY is higher in media with higher refractive index.
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