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上转换纳米粒子与氧化石墨烯的共振能量转移对发光猝灭的贡献。

Contribution of resonance energy transfer to the luminescence quenching of upconversion nanoparticles with graphene oxide.

机构信息

Department of Chemistry in Pharmaceutical Sciences, Universidad Complutense de Madrid, 28040 Madrid, Spain.

Departament of Optics, Universidad Complutense de Madrid, 28037 Madrid, Spain.

出版信息

J Colloid Interface Sci. 2020 Sep 1;575:119-129. doi: 10.1016/j.jcis.2020.04.076. Epub 2020 Apr 20.

Abstract

Upconversion nanoparticles (UCNP) are increasingly used due to their advantages over conventional fluorophores, and their use as resonance energy transfer (RET) donors has permitted their application as biosensors when they are combined with appropriate RET acceptors such as graphene oxide (GO). However, there is a lack of knowledge about the design and influence that GO composition produces over the quenching of these nanoparticles that in turn will define their performance as sensors. In this work, we have analysed the total quenching efficiency, as well as the actual values corresponding to the RET process between UCNPs and GO sheets with three different chemical compositions. Our findings indicate that excitation and emission absorption by GO sheets are the major contributor to the observed luminescence quenching in these systems. This challenges the general assumption that UCNPs luminescence deactivation by GO is caused by RET. Furthermore, RET efficiency has been theoretically calculated by means of a semiclassical model considering the different nonradiative energy transfer rates from each Er ion to the GO thin film. These theoretical results highlight the relevance of the relative positions of the Er ions inside the UCNP with respect to the GO sheet in order to explain the RET-induced efficiency measurements.

摘要

上转换纳米粒子(UCNP)由于其优于传统荧光团的优势而被越来越多地使用,并且当它们与适当的共振能量转移(RET)受体(如氧化石墨烯(GO))结合使用时,它们作为 RET 供体的应用已使其可用作生物传感器。然而,对于 GO 组成对上转换纳米粒子猝灭的设计和影响知之甚少,而这反过来又将定义它们作为传感器的性能。在这项工作中,我们分析了总猝灭效率,以及与具有三种不同化学组成的 GO 片之间的 RET 过程相对应的实际值。我们的研究结果表明,GO 片的激发和发射吸收是这些体系中观察到的发光猝灭的主要贡献者。这对 GO 通过 RET 导致 UCNP 发光失活的一般假设提出了挑战。此外,通过考虑从每个 Er 离子到 GO 薄膜的不同非辐射能量转移率的半经典模型,理论上计算了 RET 效率。这些理论结果强调了 UCNP 内部 Er 离子相对于 GO 片的相对位置对于解释 RET 诱导的效率测量的相关性。

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