用于生物传感器应用的金刚石
Diamond for biosensor applications
摘要：
综述了化学气相沉积（CVD）单晶金刚石薄膜的光电表面改性。胺-和苯基-连接分子层的共价键合形成的特征在于使用X-射线光电子能谱学（XPS），原子力显微镜（AFM），循环伏安法和场效应晶体管表征实验。胺层和苯基层在形成、生长、厚度和分子排列方面非常不同。我们在金刚石上检测到一个密度约为1014 cm-2（10%的碳键）的胺连接分子的单分子层。胺分子仅在最初的H-封端的表面区域上与碳键合。在苯基层的电化学沉积的情况下，由于三维（3D）生长而检测到多层形成。这导致形成典型的25 μ m厚的层。硼掺杂金刚石的电化学接枝作用于氢终止和氧化表面。在这种膜与异双功能交联剂分子反应后，巯基修饰的ss-DNA标记物键合到有机系统上。应用荧光和原子力显微镜杂交DNA膜显示密度高达1013 cm-2的密集安排。DNA相对于金刚石表面倾斜约35 °。将巯基修饰的ss-DNA的键合时间缩短至10分钟导致DNA密度降低至约1012 cm-2。AFM划痕实验的应用表明，结合在苯基接头分子上的DNA的阈值去除力约为75 nN，结合在胺接头分子上的DNA的阈值去除力约为45 nN。介绍了Fe（CN 6）3-/4-介体氧化还原分子、阻抗谱和DNA场效应晶体管器件性能在DNA传感器中的应用。
英文摘要：
A summary of photo- and electrochemical surface modifications applied on single-crystalline chemical vapor deposition (CVD) diamond films is given. The covalently bonded formation of amine- and phenyl-linker molecule layers are characterized using X-ray photoelectron spectroscopy (XPS), atomic force microscopy (AFM), cyclic voltammetry and field-effect transistor characterization experiments. Amine- and phenyl-layers are very different with respect to formation, growth, thickness and molecule arrangement. We detect a single molecular layer of amine linker-molecules on diamond with a density of about 1014 cm-2 (10 % of carbon bonds). Amine molecules are bonded only on initially H-terminated surface areas to carbon. In case of electrochemical deposition of phenyl-layers, multi-layer formation is detected due to three dimensional (3D) growths. This gives rise to the formation of typically 25 Å thick layers. The electrochemical grafting of boron doped diamond works on H-terminated and oxidized surfaces. After reacting of such films with heterobifunctional crosslinker-molecules, thiol-modified ss-DNA markers are bonded to the organic system. Application of fluorescence and atomic force microscopy on hybridized DNA films show dense arrangements with densities up to 1013 cm-2. The DNA is tilted by an angle of about 35o with respect to the diamond surface. Shortening the bonding time of thiol-modified ss-DNA to 10 minutes cause a decrease of DNA density to about 1012 cm-2. Application of AFM scratching experiments show threshold removal forces around 75 nN for DNA bonded on phenyl linker-molecules and of about 45 nN for DNA bonded to amine linker-molecules. DNA sensor applications using Fe(CN6)3-/4- mediator redox-molecules, impedance spectroscopy and DNA-field effect transistor devices performances are introduced and discussed.
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