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Tip-enhanced near-field optical microscopy with a parabolic mirror microscope: Enhancing luminescence emission and Raman scattering by inelastic tunneling

使用抛物面镜显微镜的尖端增强近场光学显微镜：通过非弹性隧道增强发光发射和拉曼散射

基本信息

批准号：
5390614
负责人：
Professor Dr. Alfred J. Meixner
金额：
--
依托单位：
Institut für Physikalische und Theoretische Chemie
依托单位国家：
德国
项目类别：
Research Grants
财政年份：
2002
资助国家：
德国
起止时间：
2001-12-31 至 2015-12-31
项目状态：
已结题

来源：
https://gepris.dfg.de/gepris/projekt/5390614?language=en
关键词：
Tip enhanced near field optical

项目摘要

Based on the successful implementation of the research plans of the previous two funding periods, we aim in the next funding period at combining parabolic mirror assisted near-field optical microscopy with scanning tunneling microscopy. The main goal is to investigate the structure, the optical and the electronic properties of (single) molecule(s) in a tunneling junction as a function of bias voltage by tip-enhanced luminescence- and Raman-spectroscopy. More specifically we will investigate the underlying fundamental physics mechanisms responsible for the novel and important observations from our preliminary work. Such as 1) the modification of Raman spectra of molecules chemisorbed to the gold-substrate as a function of the bias voltage; 2) the enhanced luminescence emission and Raman scattering from tunneling junctions as a function of the bias voltage; 3) the influence of the relative position energy levels with respect to the bias-voltage. For instance: i) the relative energetic arrangement of the highest occupied molecular orbital (HOMO) and the d-band of the Au substrate; and ii) the energetic levels of the virtual state (Raman) or the lowest unoccupied molecular orbital (LUMO) and the Fermi-level of the metal. Furthermore, we will explore under what conditions feedback from the plasmon oscillations between a tip and a substrate can lead to stimulated Raman-scattering and luminescence emissinon. In general, we target at a deeper understanding of the fundamental processes governing the interaction of molecules with a metal surface such as binding, polarization, charge transfer, electronic excitation of the molecule and emission of photons from the gap on one hand and the interaction between nearby molecules on the other hand. The observations and the mechanisms explored in this project will find a variety of applications in the following fields: optical microscopy and spectroscopy with single molecule spatial resolution and chemical contrast; efficient single-molecule optical switches and efficient and stable single-molecule point-like light sources.

基于前两个资助期的研究计划的成功实施，我们的目标是在下一个资助期结合抛物面镜辅助近场光学显微镜和扫描隧道显微镜。主要目的是通过针尖增强发光光谱和拉曼光谱研究隧道结中（单个）分子的结构、光学和电子性质随偏压的变化。更具体地说，我们将调查的基础物理机制负责的新的和重要的意见，从我们的初步工作。例如：1）化学吸附在金衬底上的分子的拉曼光谱随偏置电压的变化而变化; 2）隧道结的增强发光发射和拉曼散射随偏置电压的变化; 3）相对位置能级相对于偏置电压的影响。例如：i）Au衬底的最高占据分子轨道（HOMO）和d带的相对能量排列;以及ii）金属的虚态（拉曼）或最低未占据分子轨道（LUMO）的能级和费米能级。此外，我们将探讨在什么条件下，从一个尖端和基板之间的等离子体激元振荡的反馈可以导致受激拉曼散射和发光emissinon。在一般情况下，我们的目标是在一个更深的理解与金属表面的分子相互作用的基本过程，如结合，极化，电荷转移，电子激发的分子和发射的光子从差距一方面，另一方面附近的分子之间的相互作用。该项目中探索的观察和机制将在以下领域中找到各种应用：具有单分子空间分辨率和化学对比度的光学显微镜和光谱学;高效的单分子光学开关和高效稳定的单分子点状光源。