Department of Chemical & Nuclear Engineering and Center for Micro-Engineered Materials, University of New Mexico, 87131, USA.
Nat Mater. 2010 Aug;9(8):667-75. doi: 10.1038/nmat2805.
Synthetic solid-state nanopores are being intensively investigated as single-molecule sensors for detection and characterization of DNA, RNA and proteins. This field has been inspired by the exquisite selectivity and flux demonstrated by natural biological channels and the dream of emulating these behaviours in more robust synthetic materials that are more readily integrated into practical devices. So far, the guided etching of polymer films, focused ion-beam sculpting, and electron-beam lithography and tuning of silicon nitride membranes have emerged as three promising approaches to define synthetic solid-state pores with sub-nanometre resolution. These procedures have in common the formation of nominally cylindrical or conical pores aligned normal to the membrane surface. Here we report the formation of 'kinked' silica nanopores, using evaporation-induced self-assembly, and their further tuning and chemical derivatization using atomic-layer deposition. Compared with 'straight through' proteinaceous nanopores of comparable dimensions, kinked nanopores exhibit up to fivefold reduction in translocation velocity, which has been identified as one of the critical issues in DNA sequencing. Additionally, we demonstrate an efficient two-step approach to create a nanopore array exhibiting nearly perfect selectivity for ssDNA over dsDNA. We show that a coarse-grained drift-diffusion theory with a sawtooth-like potential can reasonably describe the velocity and translocation time of DNA through the pore. By control of pore size, length and shape, we capture the main functional behaviours of protein pores in our solid-state nanopore system.
合成固态纳米孔作为单分子传感器,用于检测和表征 DNA、RNA 和蛋白质,目前受到了广泛的研究。这一领域的灵感来自于天然生物通道所展示出的极高选择性和流速,以及在更坚固的合成材料中模拟这些特性的梦想,这些合成材料更易于集成到实际设备中。到目前为止,聚合物薄膜的定向刻蚀、聚焦离子束雕刻、以及氮化硅膜的电子束光刻和调谐,已成为定义具有亚纳米分辨率的合成固态纳米孔的三种有前途的方法。这些方法的共同之处在于形成垂直于膜表面的名义上的圆柱形或圆锥形纳米孔。在这里,我们报告了使用蒸发诱导自组装形成的“弯曲”硅纳米孔,以及使用原子层沉积对其进行进一步的调谐和化学衍生化。与具有类似尺寸的“直通”蛋白质纳米孔相比,弯曲纳米孔的迁移速度降低了五倍,这已被确定为 DNA 测序的关键问题之一。此外,我们还展示了一种高效的两步法,可创建一个纳米孔阵列,该阵列对 ssDNA 具有几乎完美的选择性,而对 dsDNA 则没有选择性。我们表明,具有锯齿状势的粗粒漂移扩散理论可以合理地描述 DNA 通过纳米孔的速度和迁移时间。通过控制孔径、长度和形状,我们在固态纳米孔系统中捕获了蛋白质孔的主要功能行为。