Imaging Heterogeneous 3D Dynamics of Individual Solutes in a Polyelectrolyte Brush
Imaging Heterogeneous 3D Dynamics of Individual Solutes in a Polyelectrolyte Brush
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聚电解质刷中单个溶质的异质 3D 动力学成像
DOI：
10.1021/acs.langmuir.3c00868
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发表时间：
2023
期刊：
影响因子：
3.9
通讯作者：
Landes, Christy F.
中科院分区：
文献类型：
--
作者：
Fan, Dongyu;Bajgiran, Shahryar Ramezani;Samghabadi, Farshad Safi;Dutta, Chayan;Gillett, Emil;Rossky, Peter J.;Conrad, Jacinta C.;Marciel, Amanda B.;Landes, Christy F.
了解聚电解质刷（PEBs）中的分子运输对于分离、药物输送、防污和生物传感器等应用至关重要，其中聚合物的结构特征控制着分子间的相互作用。peb的复杂结构和局部非均质性虽然是理论预测的，但很难用常规的实验方法得到。在这项工作中，我们使用3D单分子跟踪来了解阳离子聚(2-（N，N-二甲氨基）丙烯酸乙酯（PDMAEA）刷内的传输行为，使用阴离子染料Alexa Fluor 546作为探针。分析是通过并行，无偏的三维跟踪算法完成的。我们的结果明确地表明，刷内的空间异质性表现为单分子位移的异质性。我们发现了两种不同的探针运动，具有反相关的轴向和横向传输限制，我们认为这对应于链内和链间的探针运动。
Understanding molecular transport in polyelectrolyte brushes (PEBs) is crucial for applications such as separations, drug delivery, anti-fouling, and biosensors, where structural features of the polymer control intermolecular interactions. The complex structure and local heterogeneity of PEBs, while theoretically predicted, are not easily accessed with conventional experimental methods. In this work, we use 3D single-molecule tracking to understand transport behavior within a cationic poly(2-(N,N-dimethylamino)ethyl acrylate) (PDMAEA) brush using an anionic dye, Alexa Fluor 546, as the probe. The analysis is done by a parallelized, unbiased 3D tracking algorithm. Our results explicitly demonstrate that spatial heterogeneity within the brush manifests as heterogeneity of single-molecule displacements. Two distinct populations of probe motion are identified, with anticorrelated axial and lateral transport confinement, which we believe to correspond to intra- vs inter-chain probe motion.