Multifunctional nanopore electrode array method for characterizing and manipulating single entities in attoliter-volume enclosures
Multifunctional nanopore electrode array method for characterizing and manipulating single entities in attoliter-volume enclosures
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DOI：
10.1063/5.0101693
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发表时间：
2022-11
影响因子：
3.2
通讯作者：
Seol Baek;Allison R. Cutri;Donghoon Han;Seung-Ryong Kwon;Julius Reitemeier;Vignesh Sundaresan;P. Bohn-P.-B
中科院分区：
文献类型：
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作者：
Seol Baek;Allison R. Cutri;Donghoon Han;Seung-Ryong Kwon;Julius Reitemeier;Vignesh Sundaresan;P. Bohn-P.-B
结构规则的纳米孔阵列制造包含独立可控的环形电极代表了一种新的架构，能够电化学解决小集合的物质，下降到单个实体（分子，粒子和生物细胞）的水平。此外，这些纳米孔电极阵列（NEAs）也可以被光学询问，以实现单一实体光谱电化学。较大的实体，如纳米粒子和单个细菌细胞的暗场散射和电位控制的单细胞发光实验，分别进行了研究，而NEA限制的分子探测单分子发光。通过在相同构造的纳米孔阵列中进行这些实验，可以同时研究单个实体的大规模并行集合。NEAs的多层金属-绝缘体设计使高效的氧化还原循环实验成为可能，大大提高了化学传感应用的分析灵敏度。NEA还可以用另外的正交设计的纳米孔层（例如结构化嵌段共聚物）来增强，以实现具有多个刺激响应性传输控制机制的分级组织的多层结构。最后，用透明底层构建的NEA允许光学进入纳米孔的内部，这可以导致远场模式传播的截止，有效地将辐射捕获在纳米孔内的超小体积中。底部金属层可以用作工作电极和光学包覆层，因此，产生能够进行光谱电化学研究到单分子水平的双功能电化学零模式波导架构。
Structurally regular nanopore arrays fabricated to contain independently controllable annular electrodes represent a new kind of architecture capable of electrochemically addressing small collections of matter—down to the single entity (molecule, particle, and biological cell) level. Furthermore, these nanopore electrode arrays (NEAs) can also be interrogated optically to achieve single entity spectroelectrochemistry. Larger entities such as nanoparticles and single bacterial cells are investigated by dark-field scattering and potential-controlled single-cell luminescence experiments, respectively, while NEA-confined molecules are probed by single molecule luminescence. By carrying out these experiments in arrays of identically constructed nanopores, massively parallel collections of single entities can be investigated simultaneously. The multilayer metal–insulator design of the NEAs enables highly efficient redox cycling experiments with large increases in analytical sensitivity for chemical sensing applications. NEAs may also be augmented with an additional orthogonally designed nanopore layer, such as a structured block copolymer, to achieve hierarchically organized multilayer structures with multiple stimulus-responsive transport control mechanisms. Finally, NEAs constructed with a transparent bottom layer permit optical access to the interior of the nanopore, which can result in the cutoff of far-field mode propagation, effectively trapping radiation in an ultrasmall volume inside the nanopore. The bottom metal layer may be used as both a working electrode and an optical cladding layer, thus, producing bifunctional electrochemical zero-mode waveguide architectures capable of carrying out spectroelectrochemical investigations down to the single molecule level.