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首页> 外文期刊>ACS Macro Letters >Shifting Electronic Structure by Inherent Tension in Molecular Bottlebrushes with Polythiophene Backbones
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Shifting Electronic Structure by Inherent Tension in Molecular Bottlebrushes with Polythiophene Backbones

机译：通过固有张力在具有聚噻吩骨架的分子瓶刷中转移电子结构

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摘要

Bottlebrush macromolecules can be regarded as molecular tensile machines, where tension is self-generated along the backbone due to steric repulsion between densely grafted side chains. This intrinsic tension is amplified upon adsorption of bottlebrush molecules onto a substrate and increases with grafting density, side chain length, and strength of adhesion to the substrate. To investigate the effects of tension on the electronic structure of polythiophene (PT), bottlebrush macromolecules were prepared by grafting poly(n- butyl acrylate) (PBA) side chains from PT macroinitiators by atom transfer radical polymerization (ATRP). The fluores- cence spectra of submonolayers of PT bottlebrushes were measured on a Langmuir-Blodgett (LB) trough with the backbone tension adjusted by controlling the side-chain length, surface pressure, and chemical composition of a substrate. The wavelength of maximum emission has initially red-shifted, followed by a blue-shift as the backbone tension increases from 0 to 2.5 nN, which agrees with DFT calculations. The red-shift is ascribed to an increase in the conjugation length due to the extension of the PT backbone at lower force regime (0-1.0 nN), while the blue- shift is attributed to deformations of bond lengths and angles in the backbone at higher force regime (1.0-2.5 nN).
机译：洗瓶刷大分子可以看作是分子拉伸机，其中由于紧密接枝的侧链之间的空间排斥，沿主链自发产生张力。该固有张力在将洗瓶刷分子吸附到基材上时被放大，并随着接枝密度，侧链长度和与基材的粘合强度而增加。为了研究张力对聚噻吩（PT）电子结构的影响，通过原子转移自由基聚合（ATRP）从PT大分子引发剂接枝聚丙烯酸正丁酯（PBA）侧链，制备了牙刷大分子。在Langmuir-Blodgett（LB）槽上测量PT牙刷亚单层的荧光光谱，并通过控制侧链长度，表面压力和底物的化学成分来调节主链张力。最大发射的波长最初已发生红移，然后随着主干张力从0增大到2.5 nN而发生蓝移，这与DFT计算一致。红移归因于PT骨架在较低受力状态（0-1.0 nN）下的延伸而引起的共轭长度的增加，而蓝移归因于骨架上键长和键长的变形更高的作用力范围（1.0-2.5 nN）。

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