Chemical Gating of a Tube-in-a-Tube Semiconductor

描述（由申请人提供）：2013年全球有超过800万例癌症相关死亡。根据世界卫生组织的数据，到2030年，这一死亡人数将达到1310万，除非开发出快速和具有成本效益的诊断技术，以早期发现这种疾病。目前的诊断技术，如酶联免疫吸附法，在护理点的设置是耗时的，往往是成本高昂的发展中国家的资源稀缺。在这里，我们提出了一种潜在的变革性全碳电子生物传感器，它基于我们的研究团队创建的管中管半导体（Tube ^2）。电子管^[2]是由一个原子厚度的半导体嵌套在一个带电的共价功能壳层中构成的。我们假设，通过半导体的电导可以完全由壳上的表面官能团控制，从而可以通过电学检测到少量靶向癌症标志物的结合。我们的初步研究已经证明了利用薄膜管传感器进行DNA的化学门控场效应检测的可行性。拟议中的研究将集中在三个具体目标上：1）建立Tube^2的无电极化学门控基础; 2）光同轴化学光刻; 3）Tube^2传感器对癌症生物标志物的无标记和多路检测。在目标1中，一系列芳基官能团将以受控的密度共价连接在管^[2]上，以定量测定表面官能团的门控效应。在目标2中，我们将研究光驱动的电子管去功能化和再功能化，以此作为一种直接的、全新的电子传感器阵列制造方法的基础。在目标3中，将在薄膜管传感器阵列中研究模型癌症标志物（包括前列腺特异性抗原和甲胎蛋白）的化学门控场效应检测。这项工作可能为开发快速和具有成本效益的医疗诊断技术提供新的基础。

DESCRIPTION (provided by applicant): There were over 8 million cancer-related deaths worldwide in 2013. According to the World Health Organization, this death toll will reach 13.1 million by 2030 unless rapid and cost- effective diagnostic technologies are developed for the early detection of the disease. Current diagnostic techniques such as ELISA are time-consuming for point-of-care settings and often cost-prohibitive for developing countries where resources are scarce. Here, we propose a potentially transformative all-carbon electronic biosensor based on a tube-in-a-tube semiconductor (Tube^2) created by our research team. A Tube^2 is composed of an atom-thick semiconductor nested within a charged, covalent functional shell. We hypothesize that conductance through the semiconductor can be completely controlled solely by surface functional groups on the shell such that binding of a small number of targeted cancer markers can be detected electrically. Our preliminary studies have shown evidence of chemically gated field effect detection of DNA using thin-film Tube^2 sensors. The proposed research will focus on three specific aims: 1) establishing the fundamentals of electrode-free chemical gating of Tube^2; 2) coaxial chemical lithography with light; and 3) label-free and multiplexed detection of cancer biomarkers by Tube^2 sensors. In Aim 1, a series of aryl functional groups will be attached covalently at controlled densities on Tube^2 to quantitatively determine the gating effects of surface functional groups. In Aim 2, we will investigate light-driven defunctionalization and re-functionalization of Tube^2 as the basis for a straightforward, fundamentally new fabrication approach to electronic sensor arrays. In Aim 3, chemically gated field effect detection of model cancer markers, including prostate-specific antigen and α-fetoprotein, will be investigated in thin-film Tube^2 sensor arrays. This work may provide a new foundation for the development of rapid and cost-effective medical diagnostic technologies.