Fabrication and Comparative Quantitative Analysis of Plasmonic-Polymer Nanocomposites as Optical Platforms
Fabrication and Comparative Quantitative Analysis of Plasmonic-Polymer Nanocomposites as Optical Platforms
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作为光学平台的等离子体聚合物纳米复合材料的制备和比较定量分析
DOI：
10.1021/acs.langmuir.1c01826
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发表时间：
2021
期刊：
影响因子：
3.9
通讯作者：
De Silva Indrasekara, Agampodi Swarnapali
中科院分区：
文献类型：
--
作者：
Folks, Casey;Phuyal, Uttam Sharma;Rajesh, Mahima;Arja, Nagathushara;Gladden, Michael;Hamm, Logan;De Silva Indrasekara, Agampodi Swarnapali
等离子体-聚合物纳米复合材料可以作为一种多功能的平台，用于生物化学传感和光热治疗等广泛的应用领域，它们可以协同受益于等离子体纳米颗粒(NPs)的非凡光学性质和生物聚合物的生物相容性特性。等离子体-聚合物纳米复合材料的场平移需要可扩展和可重复制造的设计规则，具有可调和可预测的光学性质，并实现最佳性能。纳米粒子的光学性质和纳米复合材料的最佳分析性能可能会受到许多制备参数的影响，但对这些参数的基本了解仍然很少。在这里，我们系统地研究了金纳米星(GNS)-聚合物纳米复合材料中NP的分布及其光学性质随GNS浓度、聚合物特性以及GNS掺杂到聚合物基质中的方法的变化。我们利用暗场光谱分析了琼脂糖凝胶和壳聚糖水凝胶包埋和表面沉积形成的GNS的单粒子散射光谱。虽然GNS的相对浓度影响GNS在两种聚合物基质中的散射性质分布，但聚合物基质与GNS之间的化学作用是决定GNS在纳米复合材料中稳定性和均匀分布的关键因素。当GNS被嵌入到聚合物基质中时，GNS与聚合物之间有较强的化学相互作用，在所有浓度下，GNS的聚集明显减少，分布更均匀，导致GNS的光学性质保持率更高。在一项概念验证表面增强拉曼光谱(SERS)研究中，我们观察到SERS检测效率由GNS的分析物可访问性决定，而GNS的分析物可访问性由聚合物基质孔隙率、聚合物-GNS相互作用和其他聚合物物理特性决定。这项工作展示了关键制造参数和基础设计参数之间的相互作用，以便更可预测和可靠地制备作为光学平台的等离子体-聚合物纳米复合材料。
Plasmonic-polymer nanocomposites can serve as a multifunctional platform for a wide range of applications such as biochemical sensing and photothermal treatments, where they synergistically benefit from the extraordinary optical properties of plasmonic nanoparticles (NPs) and biocompatible characteristics of biopolymers. The field translation of plasmonic-polymer nanocomposites requires design rules for scalable and reproducible fabrication with tunable and predictable optical properties and achieving the best performance. The optical properties of NPs and the optimal analytical performance of nanocomposites could be affected by many fabrication parameters, but a fundamental understanding of such parameters is still minimal. Herein, we systematically investigated the NP distribution and their optical properties in gold nanostar (GNS)-polymer nanocomposites as a function of GNS concentration, polymer identity, and the method of GNS incorporation into a polymer matrix. We performed a comprehensive analysis of the single-particle scattering spectra of GNS incorporated into agarose gel and chitosan hydrogels via embedding and surface deposition, using dark-field spectroscopy. While relative GNS concentration affects the GNS scattering property distribution in both polymer matrices, chemical interactions between a polymer matrix and GNS is the key determinant of the GNS stability and homogenous distribution in nanocomposites. When GNS are embedded in a polymer matrix and there are stronger chemical interactions between GNS and a polymer, significantly less aggregation and a more homogenous distribution of GNS, which leads to a larger percentage of GNS optical property preservation, were observed at all the concentrations. In a proof-of-concept surface-enhanced Raman spectroscopy (SERS) study, we observed that the SERS detection efficiency is dictated by the analyte accessibility of GNS, which is governed by the polymer matrix porosity, polymer-GNS interactions, and other polymer physical characteristics. This work presents the interplay between key fabrication parameters and foundational design parameters for more predictable and reliable fabrication of plasmonic-polymer nanocomposites as an optical platform.