Morrin Gregory T, Kienle Daniel F, Schwartz Daniel K
Department of Chemical and Biological Engineering, University of Colorado Boulder, Boulder, CO 80309, USA.
Analyst. 2019 Apr 8;144(8):2628-2634. doi: 10.1039/c8an02300j.
Strongly confined environments (confined dimensions between 1-100 nm) represent unique challenges and opportunities for understanding and manipulating molecular behavior due to the significant effects of electric double layers, high surface-area to volume ratios, and other phenomena at the nanoscale. Convex Lens-induced Confinement (CLiC) can be used to analyze the dynamics of individual molecules or particles confined in a planar slit geometry with continuously varying gap thickness. We describe an interferometry-based method for precise measurement of the slit pore geometry. Specifically, this approach permitted accurate characterization of separation distances as small as 5 nm, with 1 nm precision, without a priori knowledge or assumptions about the contact geometry, as well as a greatly simplified experimental setup that required only a lens, coverslip, and inverted microscope. The interferometry-based measurement of gap height offered a distinct advantage over conventional fluorescent dye-based methods; e.g., accurate interferometric height measurements were made at low gap heights regardless of solution conditions, while the concentration of fluorescent dye was significantly impacted by solution conditions such as ionic strength or pH. The accuracy of the interferometric measurements was demonstrated by comparing the experimentally measured concentration of a charged fluorescent dye as a function of gap thickness with dye concentration profiles calculated using Debye-Hückel theory. Accurate characterization of nanoscale gap thickness will enable researchers to study a variety of practical and biologically relevant systems within the CLiC geometry.
强受限环境(受限尺寸在1 - 100纳米之间)由于双电层的显著影响、高表面积与体积比以及纳米尺度的其他现象,为理解和操纵分子行为带来了独特的挑战与机遇。凸透镜诱导受限(CLiC)可用于分析单个分子或粒子在具有连续变化间隙厚度的平面狭缝几何结构中的动力学。我们描述了一种基于干涉测量法的精确测量狭缝孔隙几何结构的方法。具体而言,这种方法能够精确表征小至5纳米的分离距离,精度达到1纳米,无需关于接触几何结构的先验知识或假设,并且实验装置大大简化,仅需一个透镜、盖玻片和倒置显微镜。基于干涉测量法的间隙高度测量相对于传统的基于荧光染料的方法具有明显优势;例如,无论溶液条件如何,在低间隙高度下都能进行精确的干涉高度测量,而荧光染料的浓度会受到离子强度或pH值等溶液条件的显著影响。通过将实验测量的带电荧光染料浓度作为间隙厚度的函数与使用德拜 - 休克尔理论计算的染料浓度分布进行比较,证明了干涉测量的准确性。纳米尺度间隙厚度的精确表征将使研究人员能够在CLiC几何结构中研究各种实际的和与生物学相关的系统。