Monitoring and Driving Chemical Response with Single Molecule Nanocircuits

分子电子学的概念通常是从小型化、规模化和推广硅技术的困难等方面来阐述的。然而，除了数字逻辑之外，基于分子的结构也可能是化学活性的新型传感器。例如，单分子电子器件可用于将固态电子学与组成生物分子的动态行为相结合。这种新颖的用途改变可能是在分子尺度上制造设备的最具变革性和最具影响力的结果，因为今天没有电子产品以功能方式结合蛋白质、DNA或任何其他生物分子。即使分子设备永远不会像存储器或晶体管设备那样与传统的数字电子设备竞争，这些替代用途也代表着尚未开发的具有巨大潜在重要性的新领域。例如，设想一个可以报告特定酶、药物或催化剂颗粒功能的硅芯片设备。用固态设备直接报告化学活动可以让用户对实时发生的化学事件有新的见解。这些新信息将使新药的有效开发，或催化剂的现场测试，以检查其有效性。这个项目的目的是从实验上证明和测试这一前提，并进一步精确地监测分子的化学活动。这项工作是由最近开发的一种架构实现的，在这种架构中，单分子被集成到功能正常的碳纳米管晶体管设备中。当附着的分子与其直接环境相互作用时，纳米管电导以微秒级的分辨率实时记录化学事件。过去的工作已经成功地记录了与单分子化学相关的复杂的、时变的信号。然而，这些设备的通用性仍然没有得到证实，也不知道化学、电子和机械自由度是如何结合在一起产生感兴趣的信号的。这个项目的一个主要目标是了解这些可能的贡献，以便为如何改进和控制工作中的机制制定设计规则。智力上的优点：这个建议有效地利用了最近的发现来推动分子电子学领域的发展，并朝着直接实用的方向这样做。这些目标旨在提高我们对单分子器件中信号转导的基本理解，这是此类器件可以商业化应用之前的关键一步。该项目是及时和有利的，因为它利用了其他正在进行的研究工作，它在技术上立即是可行的，并且存在有启发性的初步数据。广泛的影响：如果成功，该项目可能有助于开发具有广泛商业意义的电子设备。作为一种高灵敏度和高带宽的传感器，它可以通过新的诊断和研究能力使医疗和制药行业的广泛领域受益，而不依赖于荧光团或其他光学设备。一般而言，通过改进过程监测和控制，对化学加工也有潜在的好处。该项目还将直接支持初级科学家的研究培训，以及对有兴趣成为K-12科学教师的理科专业学生的培训。

AbstractThe idea of molecular electronics is usually stated in terms of miniaturization, scaling, and the difficulties of extending silicon technologies. Aside from digital logic, however, molecule-based architectures could also be novel transducers of chemical activity. For example, single molecule electronic devices might be used to merge solid state electronics with the dynamic behavior of constituent biomolecules. This novel repurposing might be the most transformative and impactful outcome of fabricating devices at molecular scales, since no electronic product today incorporates proteins, DNA, or any other biomolecule in a functional way. Even if molecular devices never compete with traditional digital electronics as memory or transistor devices, these alternate purposes represent untapped new fields with tremendous potential import.For example, imagine a silicon chip device that could report the function of a particular enzyme, or medicine, or catalyst particle. Directly reporting chemical activity with a solid state device could give users new insights into chemistry happening in real time. This new information would enable the efficient development of new drugs, or the in situ testing of catalysts to check their effectiveness. This project aims to experimentally demonstrate and test this premise, and furthermore to monitor chemical activity with molecule-by-molecule precision. The work is made possible by a recently developed architecture in which single molecules are integrated into functioning carbon nanotube transistor devices. The nanotube conductance records chemical events in real time with microsecond resolution, as the attached molecule interacts with its immediate environment. Past work has successfully recorded complex, time varying signals associated single molecule chemistry. However, the generality of the devices remains unproven, and there is no understanding of how chemical, electronic, and mechanical degrees of freedom combine to generate the signals of interest. A primary goal of this project will be to develop an understanding these possible contributions, in order to develop design rules for how to refine and control the mechanisms at work.Intellectual Merit: This proposal makes effective use of recent discoveries to push forward the field of molecular electronics, and it does so in a direction of immediate practicality. The goals are designed to improve our fundamental understanding of signal transduction in single molecule devices, a critical step before such devices can be commercialized for practical applications. The project is timely and well-positioned because it leverages other ongoing research efforts, it is immediately technically feasible, and suggestive preliminary data exist.Broader Impacts: If successful, this project may help develop an electronic device having wide-ranging commercial significance. As a high sensitivity and high bandwidth sensor it could benefit a wide spectrum of the medical and pharmaceutical industries through new diagnostic and research capabilities, independent of fluorophores or other optical equipment. There are also potential benefits to chemical processing generally, through improved process monitoring and control. The project will also directly support the research training of junior scientists, and the training of science majors interested in becoming K-12 science teachers.