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ACS Applied Nano Materials · 2023 · IF 5.9

Topological Control of Lanthanide-Doped Upconversion Nanocrystals for Improved FRET Coupling Efficiency in Second Near-Infrared-Triggered Photodynamic Therapy

Wang Wang,Qiqing Li,Haoran Chen,Xiaoyu Xie,Bin Li,Xianggui Kong,Yulei Chang

The precise control of the topological morphology and hierarchical composition is essential for the specific design of multifunctional lanthanide-doped nanocrystals (NCs). This control also enhances our understanding of the epitaxial growth mechanism in core–shell nanostructures, particularly in the case of NaErF4-based NCs, which exhibit minimal detectable upconversion emission without an epitaxial shell. Herein, we established a precise regulation strategy for the fabrication of disk- and rod-shaped core–shell NCs, catering to the growing interest in anisotropic core–shell NCs and aiming to improve Förster resonance energy transfer (FRET) efficiency for photodynamic therapy (PDT) applications. We synthesized NaErF4@NaREF4 NCs (RE = Y, Lu) with distinct topological morphologies by deliberately controlling the Ostwald ripening process. Furthermore, we observed that sacrifice NCs obtained through varying treatment times had diverse ion and oleate ligand release rates. These differences in the ripening reaction pathways were responsible for the ultimate variation in topological morphologies. Steady-state and dynamic luminescence studies revealed that the ligand-free rod-shaped NCs exhibited more robust upconversion emissions, and higher FRET coupling efficiency (54.0%) with photosensitizers, resulting in more generation efficiency of singlet oxygen. These findings suggest promising applications in second near-infrared-triggered PDT.

研究领域: 材料科学 · 生物医学工程 · 光学
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Small · 2023 · IF 13.3

Heteroepitaxial Growth to Construct Hexagonal/Hexagonal β-NaYF4:Yb,Tm/Cs4PbBr6 Multi-Code Emitting Core/Shell Nanocrystals

Rui Gao,Wanqing Xu,Zhiqing Wang,Fen Li,Yueli Liu,Guogang Li,Keqiang Chen

Synthesis of upconversion nanoparticles (UCNPs)-metal halide perovskites (MHPs) heterostructure is garnered immense attentions due to their unparalleled photophysical properties. However, the obvious difference in their structural forms makes it a huge challenge. Herein, hexagonal β-NaYF 4 and hexagonal Cs 4 PbBr 6 are filtrated to construct the UCNP/MHP heterostructural luminescent material. The similarity in their crystal structures facilitate the heteroepitaxial growth of Cs 4 PbBr 6 on the surface of β-NaYF 4 NPs, leading to the formation of high-quality β-NaYF 4 :Yb,Tm/Cs 4 PbBr 6 core/shell nanocrystals (NCs). Interestingly, this heterostructure endows the core/shell NCs with typically narrow-band green emission centered at 524 nm under 980 nm excitation, which should be attributed to the Förster resonance energy transfer (FRET) from Tm 3+ to Cs 4 PbBr 6 . It is noteworthy that the FRET efficiency of β-NaYF 4 :Yb,Tm/Cs 4 PbBr 6 core/shell NCs (58.33%) is much higher than that of the physically mixed sample (1.84%). In addition, the reduced defect density, lattice anchoring effect, as well as diluted ionic bonding proportion induced by the core/shell structure further increase the excellent water-resistance and thermal cycling stability of Cs 4 PbBr 6 . These findings open up a new way to construct UCNP/MHP heterostructure with better multi-code luminescence performance and stability and promote its wide optoelectronic applications.

研究领域: 材料科学 · 光学
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Nanoscale · 2018 ·Vol. 10 ·期 14 ·6611-6619 · IF 7.233

Combining gold nanoparticle antennas with single-molecule fluorescence resonance energy transfer (smFRET) to study DNA hairpin dynamics

Jinyong Hu,Meiyan Wu,Li Jiang,Zhensheng Zhong,Zhangkai Zhou,Thitima Rujiralai,Jie Ma

The association of a plasmonic nano-antenna with single-molecule FRET technique presents new prospects to investigate the dynamics of biological molecules. However, the presence of a plasmonic nano-antenna significantly modifies the FRET rate and efficiency; this makes its applicability to the prevalent single-molecule FRET experiments unclear. Herein, using gold nanoparticle antennas of different sizes and DNA hairpins labelled with FRET pairs (Cy3 and Cy5) as the model system, we performed experiments to study the folding dynamics of single DNA hairpins at various salt concentrations. Our results indicate that gold nanoparticle antennas can enhance single-molecule fluorescence of Cy3 and Cy5 up to 3–5 folds, substantially reduce the FRET efficiency, and alter the obtained FRET efficiency histograms. However, the folding dynamics of DNA hairpins remains unaffected, and the correct kinetic and dynamic information can still be extracted from the seriously modified FRET efficiencies. Therefore, our experiments demonstrate the feasibility and compatibility for applying plasmonic nano-antennas to the mostly used single-molecule FRET assays, which provide a broad range of possibilities for the future applications of these nano-antennas in studying various essential biological processes.

研究领域: 生物物理 · 分子生物学 · 纳米技术
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JOURNAL OF FLUORESCENCE · 2015 ·Vol. 25 ·期 5 ·1267-1277 · IF 1.927

Fluorescence Detection of Single DNA Molecules

Huang Weidong,Wang Yue,Wang Zhimin

Single-molecule detection (SMD) and single-molecule fluorescence resonance energy transfer (smFRET) were conducted using Cy3- and Cy5-labeled single-strand DNAs (ssDNAs) either immobilized on substrates or encapsulated in microdroplets. High-quality fluorescent images were obtained using a total internal reflection fluorescence microscope (TIRFM). In the substrate system, deposition of a low concentration of fluorescence molecules on substrates through electrostatic adsorption showed that most of the fluorescence spots were single molecules, and the mean value of signal to noise ratio (S/N) reached 6.9 ± 0.34. smFRET analysis was conducted through immobilization of donor- and acceptor-labeled oligonucleotides on substrates. In the droplet system, fluorophor-labeled oligonucleotides were injected into T-type microfluidics. Single and double fluorophor-labeled DNA molecules encapsulated in droplets were detected, the FRET efficiency and inter-dye distance of a single donor-acceptor pair were measured accurately. smFRET was conducted detailedly in the tortuous channel for the first time.

CAS / MDL: 919-30-2
研究领域: 生物化学 · 分子生物学 · 生物物理学
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