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首页> 外文学位 >Single molecule chiroptical spectroscopy: Fluorescence excitation circular dichroism and circular polarized luminescence of bridged triarylamine helicenes.
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Single molecule chiroptical spectroscopy: Fluorescence excitation circular dichroism and circular polarized luminescence of bridged triarylamine helicenes.

机译：单分子光谱法：桥联的三芳基胺螺旋体的荧光激发圆二色性和圆偏振发光。

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摘要

In this thesis, I describe the first exploratory experimental efforts probing light-matter interactions of chiral systems at the single molecule level. The dissymmetric single molecule chiroptical response in both excitation and emission polarization has been studied for different diastereomeric forms of bridged triarylamine helicenes. Fluorescence excitation circular dichroism (FECD), measuring the dissymmetric absorption with respect to excitation polarization, reports on the response to excitation polarization. The magnitude and distribution of chiroptical single molecule responses suggest both surface and orientation effects play a significant role. Computational modeling done to calculate the dissymmetry for specific orientations supports orientational dependence. Using a defocused imaging technique, which can be used to obtain orientation information for linear dipoles, emission patterns were obtained that lacked bilateral symmetry. These emission patterns were simulated using a semi-classical model that closely approximated the lack of bilateral symmetry. Refinement of the model and additional experiments using oriented molecules will allow for direct correlation of orientation and dissymmetry which is important for understanding the heterogeneities in the single molecule responses. In addition, dissymmetry in emission polarization has been studied using a novel imaging technique resolving polarization components on a frame-by-frame basis. The research into the intersection of single molecule spectroscopy and chiroptics has given new insight into the role of solvation and local environment in chiroptical interactions and may be useful for understand chiral-based photonics and advancing new technologies.
机译：在这篇论文中，我描述了在单分子水平上探索手性系统的光-质相互作用的第一个探索性实验工作。对于桥联的三芳基胺螺旋烯的不同非对映异构形式，已经研究了激发和发射极化中的不对称单分子手性响应。荧光激发圆二色性（FECD），测量关于激发偏振的不对称吸收，报告对激发偏振的响应。手性的单分子反应的大小和分布表明表面和定向作用都起着重要作用。为计算特定方向的不对称性而进行的计算建模支持方向依赖性。使用可用于获得线性偶极子的取向信息的散焦成像技术，可以获得缺乏双边对称性的发射模式。使用半经典模型模拟了这些发射模式，该模型非常接近缺乏双边对称性。改进模型和使用定向分子的其他实验将允许定向和不对称性的直接相关，这对于理解单分子响应中的异质性很重要。另外，已经使用一种新颖的成像技术研究了在发射极化中的不对称性，该技术在逐帧的基础上解决了极化分量。对单分子光谱学和手性学的交叉的研究为溶剂化和局部环境在手性相互作用中的作用提供了新的见解，对于理解基于手性的光子学和发展新技术可能有用。

著录项

  • 作者

    Paradise, Ruthanne Hassey.;

  • 作者单位

    University of Massachusetts Amherst.;

  • 授予单位 University of Massachusetts Amherst.;
  • 学科 Chemistry Physical.
  • 学位 Ph.D.
  • 年度 2009
  • 页码 95 p.
  • 总页数 95
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

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