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通过晶格匹配实现具有增强发光和稳定性的上转换钙钛矿纳米晶体异质结构

Upconversion Perovskite Nanocrystal Heterostructures with Enhanced Luminescence and Stability by Lattice Matching.

作者信息

Ruan Longfei, Zhang Yong

机构信息

Department of Biomedical Engineering, Faculty of Engineering, National University of Singapore, Singapore 117583.

NUS Graduate School for Integrative Sciences and Engineering, National University of Singapore, Singapore 117456.

出版信息

ACS Appl Mater Interfaces. 2021 Nov 3;13(43):51362-51372. doi: 10.1021/acsami.1c14711. Epub 2021 Oct 19.

Abstract

Lead halide perovskite quantum dots (PQDs) exhibit excellent photoelectric and optical properties, but their poor stability and low multiphoton absorption efficiency greatly limit their biological applications. Efforts have been made to combine upconversion nanoparticles (UCNPs) with PQDs to produce a composite material that is NIR-excitable, upconverting, and emission-tunable due to the unique optical properties of UCNPs, which converts tissue-penetrating near-infrared light into visible light based on an upconversion multiphoton excitation process. However, it is challenging to make such a nanocrystal heterostructure and maintain good optical properties and stability of both UCNPs and PQDs because they have different crystal structures. Here, we report the synthesis of heterostructured UCNP-PQD nanocrystals to bring hexagonal-phase NaYF UCNPs and cubic-phase CsPbBrX PQDs in close proximity in a single nanocrystal, leading to efficient Förster resonance energy transfer (FRET) from the UCNP to the PQD under NIR excitation, as compared to their counterparts in solution. Moreover, by further improving the lattice matching between the UCNP and PQD using Gd to replace Y, heterostructured CsPbBr-NaGdF:Yb,Tm nanocrystals are successfully synthesized, with much enhanced luminescence and stability at high temperatures or in polar solvents or under continuous ultraviolet light excitation as compared to those of the CsPbBr-NaYF:Yb,Tm nanocrystals and pure PQDs.

摘要

卤化铅钙钛矿量子点(PQDs)具有优异的光电和光学性质,但其稳定性差和多光子吸收效率低极大地限制了它们的生物应用。人们已努力将上转换纳米颗粒(UCNPs)与PQDs结合,以制备一种复合材料,由于UCNPs具有独特的光学性质,该复合材料可被近红外光激发、具有上转换特性且发射可调谐,它基于上转换多光子激发过程将穿透组织的近红外光转换为可见光。然而,制备这样的纳米晶体异质结构并保持UCNPs和PQDs良好的光学性质和稳定性具有挑战性,因为它们具有不同的晶体结构。在此,我们报道了异质结构UCNP-PQD纳米晶体的合成,使六方相NaYF UCNPs和立方相CsPbBrX PQDs在单个纳米晶体中紧密相邻,与它们在溶液中的对应物相比,在近红外激发下导致从UCNP到PQD的高效Förster共振能量转移(FRET)。此外,通过用Gd取代Y进一步改善UCNP和PQD之间的晶格匹配,成功合成了异质结构的CsPbBr-NaGdF:Yb,Tm纳米晶体,与CsPbBr-NaYF:Yb,Tm纳米晶体和纯PQDs相比,在高温、极性溶剂中或连续紫外光激发下具有大大增强的发光和稳定性。

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