等离子体纳米天线附近分子中高阶多极跃迁的增强与干涉

Enhancement of and interference among higher order multipole transitions in molecules near a plasmonic nanoantenna.

作者信息

Rusak Evgenia, Straubel Jakob, Gładysz Piotr, Göddel Mirko, Kędziorski Andrzej, Kühn Michael, Weigend Florian, Rockstuhl Carsten, Słowik Karolina

机构信息

Institute of Theoretical Solid State Physics, Karlsruhe Institute of Technology, 76131, Karlsruhe, Germany.

Institute of Physics, Faculty of Physics, Astronomy and Informatics, Nicolaus Copernicus University, Grudziadzka 5, 87-100, Torun, Poland.

出版信息

Nat Commun. 2019 Dec 18;10(1):5775. doi: 10.1038/s41467-019-13748-4.

DOI:10.1038/s41467-019-13748-4

PMID:31852897

原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC6920377/

Abstract

Spontaneous emission of quantum emitters can be modified by their optical environment, such as a resonant nanoantenna. This impact is usually evaluated under assumption that each molecular transition is dominated only by one multipolar channel, commonly the electric dipole. In this article, we go beyond the electric dipole approximation and take light-matter coupling through higher-order multipoles into account. We investigate a strong enhancement of the magnetic dipole and electric quadrupole emission channels of a molecule adjacent to a plasmonic nanoantenna. Additionally, we introduce a framework to study interference effects between various transition channels in molecules by rigorous quantum-chemical calculations of their multipolar moments and a consecutive investigation of the transition rate upon coupling to a nanoantenna. We predict interference effects between these transition channels, which allow in principle for a full suppression of radiation by exploiting destructive interference, waiving limitations imposed on the emitter's coherence time by spontaneous emission.

摘要

量子发射体的自发发射可被其光学环境（如共振纳米天线）所改变。这种影响通常是在每个分子跃迁仅由一个多极通道（通常是电偶极）主导的假设下进行评估的。在本文中，我们超越了电偶极近似，考虑了通过高阶多极的光与物质的耦合。我们研究了与等离子体纳米天线相邻的分子的磁偶极和电四极发射通道的强烈增强。此外，我们引入了一个框架，通过对分子多极矩进行严格的量子化学计算以及随后对与纳米天线耦合时的跃迁速率进行研究，来研究分子中各种跃迁通道之间的干涉效应。我们预测了这些跃迁通道之间的干涉效应，这原则上允许通过利用相消干涉来完全抑制辐射，从而摆脱自发发射对发射体相干时间所施加的限制。