Nanoparticle Hybrid Materials Using Plasmonic-Enhanced Upconversion FRET for Multiplexed Sensing and Optical Barcoding

使用等离子体增强上转换 FRET 进行多重传感和光学条形码的纳米粒子混合材料

• 批准号: 280181689
• 负责人: Professorin Dr. Christina Graf
• 金额: --
• 依托单位: Single Molecule BioNanophotonics group
• 依托单位国家: 德国
• 项目类别: Research Grants
• 财政年份: 2015
• 资助国家: 德国
• 起止时间: 2014-12-31 至 2019-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/280181689?language=en
• 关键词: Nanoparticle; Hybrid; Materials; Using; Plasmonic

The development of photoluminescent nanomaterials (PNMs) with tailored photophysical properties is a dynamic area of materials science. Much effort has been devoted to high-order multiplexing in sensing as well as optical barcoding for security applications and quality control using PNMs by tuning of the photoluminescence (PL) color, intensity, and lifetime. NIR-excitable upconverting nanoparticles (UCNPs) are newly emerging PNMs, which provide higher penetration depths in water and biological tissues, strongly anti-Stokes shifted emission, high photostability and strongly reduced autofluorescence background. Although UCNPs are considered ideal candidates for the applications mentioned above, they face challenges regarding low PL quantum yields (QY), limited color and lifetime tunability, and low stability in aqueous solution.5 renowned research teams from 3 European countries form the nanohype concept-driven project consortium, which combines computational modeling, synthesis, and experimental validation to design novel metal-shelled UCNPs to obtain: - 50-fold PL QY enhancement- tunable PL lifetimes between 100 ns - 600 µs- tunable PL colors by multiplexed Förster Resonance Energy Transfer (FRET) to quantum dots (QDs) or dyesThe novel PNMs will consist of silica-embedded UCNPs with metal surface coatings for plasmonic PL enhancement, and lifetime tunability and different QD or dye FRET acceptors for PL color and lifetime tuning by UCNP to QD/dye distance arrangement. For this purpose, techniques of synthesizing fluorescent nanomaterials, metal nanoshells, and UCNPs will be further optimized based on predictive modeling and simulation. By precisely tuning the distance and material parameters by combined computational modeling, materials engineering and synthesis, targeted PL properties for optimal multiplexing capabilities with improved QY will be obtained.The predictive power of computational modeling of the variable PNM structures will provide a recipe for PNM synthesis with targeted PL properties. The modeled structural properties will be produced as follows. Defect-free UCNPs will be synthesized and coated with undoped lanthanides and silica shells with precisely controlled thickness, which will enable precise positioning of FRET acceptors in or on the shells. These PNMs will then be coated with complete or partly open metal shells to utilize plasmonic interactions for an enhancement in excitation and emission and to enable access of analytes to the FRET acceptors. The proposed modeling/synthesis approach will result in the development of design criteria for such UCNP-based PNMs. We will provide the experimental validation of the predicted target properties of the novel PNMs for sensing and optical barcoding and demonstrate their superiority resulting from tailored synthesis. The multidisciplinary consortium will significantly contribute to strengthen the European Integrated Computational Materials Engineering community.

具有可定制的光致发光纳米材料（PNM）的开发是材料科学的一个动态领域。许多努力已经致力于高阶多路复用在传感以及光学条形码的安全应用和质量控制使用PNM通过调谐的光致发光（PL）的颜色，强度和寿命。近红外可激发的上转换纳米粒子（UCNPs）是近年来出现的一种新型的PNM，具有在水和生物组织中的穿透深度高、强反斯托克斯位移发射、高光稳定性和强自发荧光背景降低等优点。虽然UCNPs被认为是上述应用的理想候选者，但它们面临着低PL量子产率（QY），有限的颜色和寿命可调性以及水溶液中低稳定性的挑战。来自3个欧洲国家的知名研究团队组成了nanohype概念驱动的项目联盟，该联盟结合了计算建模，合成和实验验证来设计新型金属壳UCNPs，以获得： 50-倍PL QY增强- 可调PL寿命在100 ns - 600 µs- 新型PNM将由二氧化硅嵌入的UCNP组成，其具有用于等离子体激元PL增强的金属表面涂层和寿命可调谐性，以及不同的QD或染料FRET受体，用于通过UCNP到QD/染料距离排列的PL颜色和寿命调谐。为此，将基于预测建模和模拟进一步优化合成荧光纳米材料、金属纳米壳和UCNP的技术。通过结合计算建模、材料工程和合成来精确地调整距离和材料参数，将获得具有改进的QY的最佳复用能力的目标PL性质。可变PNM结构的计算建模的预测能力将为具有目标PL性质的PNM合成提供配方。建模的结构特性将如下产生。将合成无缺陷的UCNP，并涂覆有具有精确控制厚度的未掺杂镧系元素和二氧化硅壳，这将使得FRET受体能够精确定位在壳中或壳上。然后，这些PNM将涂覆有完全或部分开放的金属壳，以利用等离子体相互作用来增强激发和发射，并使分析物能够接近FRET受体。所提出的建模/综合方法将导致这种基于UCNP的PNM的设计标准的发展。我们将提供用于传感和光学条形码的新型PNM的预测目标特性的实验验证，并证明其从定制合成产生的优越性。该多学科联盟将大大有助于加强欧洲综合计算材料工程界。

项目成果

Sensitization of upconverting nanoparticles with a NIR-emissive cyanine dye using a micellar encapsulation approach

• DOI: 10.1088/2050-6120/aafe1f
• 发表时间: 2019-01
• 期刊: Methods and Applications in Fluorescence
• 影响因子: 3.2
• 作者: Maysoon I Saleh;Ihor D Panas;Florian Frenzel;C. Würth;Bastian Rühle;Y. Slominskii;A. Demchenko;U. Resch‐Genger

Multiband emission from single β-NaYF4(Yb,Er) nanoparticles at high excitation power densities and comparison to ensemble studies

• DOI: 10.1007/s12274-021-3350-y
• 发表时间: 2021-02-24
• 期刊: NANO RESEARCH
• 影响因子: 9.9
• 作者: Frenzel, Florian;Wuerth, Christian;Resch-Genger, Ute
• 通讯作者: Resch-Genger, Ute