Sub-20 nm Core-Shell-Shell Nanoparticles for Bright Upconversion and Enhanced Forster Resonant Energy Transfer

被引:102
作者
Siefe, Chris [1 ]
Mehlenbacher, Randy D. [1 ]
Peng, Chunte Sam [2 ,3 ]
Zhang, Yunxiang [2 ,3 ]
Fischer, Stefan [1 ]
Lay, Alice [4 ]
McLellan, Claire A. [1 ]
Alivisatos, A. Paul [5 ,6 ,7 ,8 ]
Chu, Steven [2 ,3 ]
Dionne, Jennifer A. [1 ]
机构
[1] Stanford Univ, Dept Mat Sci & Engn, Stanford, CA 94305 USA
[2] Stanford Univ, Dept Phys, Stanford, CA 94305 USA
[3] Stanford Univ, Dept Mol & Cellular Physiol, Stanford, CA 94305 USA
[4] Stanford Univ, Dept Appl Phys, Stanford, CA 94305 USA
[5] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA
[6] Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA
[7] Lawrence Berkeley Natl Lab, Mat Sci Div, Berkeley, CA 94720 USA
[8] Kavli Energy NanoSci Inst, Berkeley, CA 94720 USA
基金
芬兰科学院; 美国国家科学基金会; 美国国家卫生研究院;
关键词
SINGLE-MOLECULE; NANOCRYSTALS; SURFACE; DONOR; FRET; LUMINESCENCE; EFFICIENCY; DYNAMICS; CELLS;
D O I
10.1021/jacs.9b09571
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Upconverting nanoparticles provide valuable benefits as optical probes for bioimaging and Forster resonant energy transfer (FRET) due to their high signal-to-noise ratio, photostability, and biocompatibility; yet, making nanoparticles small yields a significant decay in brightness due to increased surface quenching. Approaches to improve the brightness of UCNPs exist but often require increased nanoparticle size. Here we present a unique core-shell-shell nanoparticle architecture for small (sub-20 nm), bright upconversion with several key features: (1) maximal sensitizer concentration in the core for high near-infrared absorption, (2) efficient energy transfer between core and interior shell for strong emission, and (3) emitter localization near the nanoparticle surface for efficient FRET. This architecture consists of beta-NaYbF4 (core) @NaY0.8-xErxGd0.2F4 (interior shell) @NaY0.8Gd0.2F4 (exterior shell), where sensitizer and emitter ions are partitioned into core and interior shell, respectively. Emitter concentration is varied (x = 1, 2, 5, 10, 20, 50, and 80%) to investigate influence on single particle brightness, upconversion quantum yield, decay lifetimes, and FRET coupling. We compare these seven samples with the field-standard core-shell architecture of beta-NaY0.58Gd0.2Yb0.2Er0.02F4 (core) @NaY0.8Gd0.2F4 (shell), with sensitizer and emitter ions codoped in the core. At a single particle level, the core-shell-shell design was up to 2-fold brighter than the standard core-shell design. Further, by coupling a fluorescent dye to the surface of the two different architectures, we demonstrated up to 8-fold improved emission enhancement with the core-shell-shell compared to the core-shell design. We show how, given proper consideration for emitter concentration, we can design a unique nanoparticle architecture to yield comparable or improved brightness and FRET coupling within a small volume.
引用
收藏
页码:16997 / 17005
页数:9
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