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首页> 美国卫生研究院文献>Proceedings of the National Academy of Sciences of the United States of America >Optimally designed nanolayered metal-dielectric particles as probes for massively multiplexed and ultrasensitive molecular assays
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Optimally designed nanolayered metal-dielectric particles as probes for massively multiplexed and ultrasensitive molecular assays

机译：优化设计的纳米层金属介电粒子作为大规模多重和超灵敏分子测定的探针

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An outstanding challenge in biomedical sciences is to devise a palette of molecular probes that can enable simultaneous and quantitative imaging of tens to hundreds of species down to ultralow concentrations. Addressing this need using surface-enhanced Raman scattering-based probes is potentially possible. Here, we theorize a rational design and optimization strategy to obtain reproducible probes using nanospheres with alternating metal and reporter-filled dielectric layers. The isolation of reporter molecules from metal surfaces suppresses chemical enhancement, and consequently signal enhancements are determined by electromagnetic effects alone. This strategy synergistically couples interstitial surface plasmons and permits the use of almost any molecule as a reporter by eliminating the need for surface attachment. Genetic algorithms are employed to optimize the layer dimensions to provide controllable enhancements exceeding 11 orders of magnitude and of single molecule sensitivity for nonresonant and resonant reporters, respectively. The strategy also provides several other opportunities, including a facile route to tuning the response of these structures to be spectrally flat and localization of the enhancement within a specific volume inside or outside the probe. The spectrally uniform enhancement for multiple excitation wavelengths and for different shifts enables generalized probes, wheras enhancement tuning permits a large dynamic range by suppression of enhancements from outside the probe. Combined, these theoretical calculations open the door for a set of reproducible and robust probes with controlled sensitivity for molecular sensing over a concentration range of over 20 orders of magnitude.
机译：生物医学科学面临的一项严峻挑战是设计一种分子探针板，以实现对数十种至数百种低至超低浓度物种的同时定量成像。使用基于表面增强的拉曼散射的探针来满足这一需求是可能的。在这里，我们对合理的设计和优化策略进行理论化，以使用具有交替的金属层和填充有报告层的介电层的纳米球来获得可重现的探针。报告分子与金属表面的隔离抑制了化学增强，因此信号增强仅由电磁效应决定。该策略协同地耦合间隙表面等离子体激元，并且通过消除表面附着的需要而允许几乎任何分子用作报告分子。遗传算法用于优化层尺寸，以分别为非共振和共振报道分子提供超过11个数量级的可控增强和单分子敏感性。该策略还提供了其他一些机会，包括将这些结构的响应调整为光谱平坦的便捷途径，以及在探针内部或外部的特定体积内增强的定位。针对多个激发波长和不同位移的光谱均一增强，使通用的探头成为可能，而通过增强抑制来自探头外部的增强，惠拉增强调谐允许较大的动态范围。综合起来，这些理论计算为一系列可重现且坚固耐用的探针打开了大门，这些探针具有可控制的灵敏度，可在浓度范围超过20个数量级时进行分子传感。

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