Bandara Y M N D Y, Nichols Jonathan W, Iroshika Karawdeniya Buddini, Dwyer Jason R
Department of Chemistry, University of Rhode Island, Kingston, RI, USA.
Electrophoresis. 2018 Feb;39(4):626-634. doi: 10.1002/elps.201700299. Epub 2017 Dec 8.
Solid-state nanopores are nanoscale channels through otherwise impermeable membranes. Single molecules or particles can be passed through electrolyte-filled nanopores by, e.g. electrophoresis, and then detected through the resulting physical displacement of ions within the nanopore. Nanopore size, shape, and surface chemistry must be carefully controlled, and on extremely challenging <10 nm-length scales. We previously developed a framework to characterize nanopores from the time-dependent changes in their conductance as they are being formed through solution-phase nanofabrication processes with the appeal of ease and accessibility. We revisited this simulation work, confirmed the suitability of the basic conductance equation using the results of time-dependent experimental conductance measurements during nanopore fabrication by Yanagi et al., and then deliberately relaxed the model constraints to allow for (i) the presence of defects; and (ii) the formation of two small pores instead of one larger one. Our simulations demonstrated that the time-dependent conductance formalism supports the detection and characterization of defects, as well as the determination of pore number, but with implementation performance depending on the measurement context and results. In some cases, the ability to discriminate numerically between the correct and incorrect nanopore profiles was slight, but with accompanying differences in candidate nanopore dimensions that could yield to post-fabrication conductance profiling, or be used as convenient uncertainty bounds. Time-dependent nanopore conductance thus offers insight into nanopore structure and function, even in the presence of fabrication defects.
固态纳米孔是贯穿原本不可渗透膜的纳米级通道。单个分子或颗粒可以通过例如电泳的方式穿过充满电解质的纳米孔,然后通过纳米孔内离子产生的物理位移进行检测。纳米孔的尺寸、形状和表面化学性质必须得到仔细控制,而且是在极具挑战性的小于10纳米的长度尺度上。我们之前开发了一个框架,通过溶液相纳米制造过程中纳米孔形成时其电导率随时间的变化来表征纳米孔,具有简便易行的特点。我们重新审视了这项模拟工作,利用柳木等人在纳米孔制造过程中随时间变化的实验电导率测量结果,证实了基本电导率方程的适用性,然后有意放宽模型约束,以允许(i)存在缺陷;以及(ii)形成两个小孔而不是一个大孔。我们的模拟表明,随时间变化的电导率形式体系支持缺陷的检测和表征以及孔数量的确定,但实施性能取决于测量背景和结果。在某些情况下,从数值上区分正确和不正确的纳米孔轮廓的能力很微弱,但伴随的候选纳米孔尺寸差异可用于制造后电导率分析,或用作方便的不确定度界限。因此,即使存在制造缺陷,随时间变化的纳米孔电导率也能深入了解纳米孔的结构和功能。