Jacob M Majikes, Seulki Cho, Thomas Cleveland, James Alexander Liddle, Arvind Balijepalli
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引用次数: 0
Abstract
Electronic measurements of engineered nanostructures comprised solely of DNA (DNA origami) enable new signal conditioning modalities for use in biosensing. DNA origami, designed to have arbitrary shapes with programmable motion triggered by conjugated biomolecules, have sufficient mass and charge to generate a large electrochemical signal. Here, we demonstrate the ability to electrostatically control the DNA origami conformation, and thereby the resulting signal amplification, when the structure binds a nucleic acid analyte. Critically, unlike previous studies that employ DNA origami to amplify an electrical signal, we show that the conformation changes under an applied field are reversible. This applied field simultaneously accelerates structural transitions above the rate determined by thermal motion. We tuned this property of the structures to achieve a response that was ≈ 2×104 times greater than the value from DNA hybridization under similar conditions. Because this signal amplification is independent of DNA origami-analyte interactions, our approach is agnostic of the end application. Furthermore, since large signal changes are only triggered in response to desirable interactions, we minimize the deleterious effects of non-specific binding. The above benefits of self-assembled DNA origami make them ideally suited for multiplexed biosensing when paired with highly parallel electronic readout.
对仅由 DNA 组成的工程纳米结构(DNA 折纸)进行电子测量,可实现用于生物传感的新信号调节模式。DNA 折纸设计成任意形状,可在共轭生物分子的触发下进行可编程运动,其质量和电荷足以产生大量电化学信号。在这里,我们展示了静电控制 DNA 折纸构象的能力,从而在该结构与核酸分析物结合时实现信号放大。重要的是,与以往利用 DNA 折纸放大电信号的研究不同,我们证明了在外加电场作用下的构象变化是可逆的。外加电场同时加速了结构转换,使其速率超过热运动决定的速率。我们对结构的这一特性进行了调整,使其响应值比类似条件下的 DNA 杂交值高出 ≈ 2×104 倍。由于这种信号放大与 DNA 原型-分析物之间的相互作用无关,因此我们的方法与最终应用无关。此外,由于只有在理想的相互作用下才会触发较大的信号变化,因此我们最大程度地降低了非特异性结合的有害影响。自组装 DNA 折纸的上述优点使其非常适合与高度并行的电子读出技术相结合,用于多重生物传感。
期刊介绍:
Nanoscale is a high-impact international journal, publishing high-quality research across nanoscience and nanotechnology. Nanoscale publishes a full mix of research articles on experimental and theoretical work, including reviews, communications, and full papers.Highly interdisciplinary, this journal appeals to scientists, researchers and professionals interested in nanoscience and nanotechnology, quantum materials and quantum technology, including the areas of physics, chemistry, biology, medicine, materials, energy/environment, information technology, detection science, healthcare and drug discovery, and electronics.