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首页> 外文期刊>ACS Macro Letters >Polymer Surface Transport Is a Combination of in-Plane Diffusion and Desorption-Mediated Flights
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Polymer Surface Transport Is a Combination of in-Plane Diffusion and Desorption-Mediated Flights

机译：聚合物表面传输是平面扩散和解吸介导的飞行的结合

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摘要

Previous studies of polymer motion at solid/liquid interfaces described the transport in the context of a continuous time random walk (CTRW) process, in which diffusion switches between desorption-mediated "flights" (i.e., hopping) and surface-adsorbed waiting-time intervals. However, it has been unclear whether the waiting times represented periods of complete immobility or times during which molecules engaged in a different (e.g., slower or confined) mode of interfacial transport. Here we designed high-throughput, single-molecule tracking measurements to address this question. Specifically, we studied polymer dynamics on either chemically homogeneous or nanopatterned surfaces (hexagonal diblock copolymer films) with chemically distinct domains, where polymers were essentially excluded from the low-affinity domains, eliminating the possibility of significant continuous diffusion in the absence of desorption-mediated flights. Indeed, the step-size distributions on homogeneous surfaces exhibited an additional diffusive mode that was missing on the chemically heterogeneous nanopatterned surfaces, confirming of a slow continuous mode due to 2D in-plane diffusion. Kinetic Monte Carlo simulations were performed to test this model and, with the theoretical in-plane diffusion coefficient of D-2D = 0.20 mu m(2)/s, we found a good agreement between simulations and experimental data on both chemically homogeneous and nanopatterned surfaces.
机译：先前在固/液界面处聚合物运动的研究描述了在连续时间随机游走（CTRW）过程中的传输，其中扩散在解吸介导的“飞行”（即跳跃）和表面吸附的等待时间之间切换间隔。然而，尚不清楚等待时间是否代表完全不动的时期或分子以不同（例如，较慢或受限）界面运输模式参与的时间。在这里，我们设计了高通量，单分子跟踪测量来解决这个问题。具体而言，我们研究了具有化学上不同域的化学均质或纳米图案表面（六嵌段共聚物嵌段共聚物）上的聚合物动力学，其中聚合物基本上被排除在低亲和力域之外，从而消除了在不存在解吸介导的情况下显着连续扩散的可能性航班。实际上，在均质表面上的步长分布表现出在化学异质纳米图案化表面上缺失的附加扩散模式，这证实了由于二维平面内扩散而产生的缓慢连续模式。进行了动力学蒙特卡洛模拟以测试该模型，并且在D-2D的理论面内扩散系数= 0.20μm（2）/ s的情况下，我们在化学均质和纳米图案化的模拟和实验数据之间发现了很好的一致性表面。

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