Instituto de Óptica-CSIC, Serrano 121, 28006 Madrid, Spain.
Nano Lett. 2011 Jun 8;11(6):2318-23. doi: 10.1021/nl200579f. Epub 2011 May 2.
We present a fully quantum mechanical approach to describe the coupling between plasmons and excitonic systems such as molecules or quantum dots. The formalism relies on Zubarev's Green functions, which allow us to go beyond the perturbative regime within the internal evolution of a plasmonic nanostructure and to fully account for quantum aspects of the optical response and Fano resonances in plasmon-excition (plexcitonic) systems. We illustrate this method with two examples consisting of an exciton-supporting quantum emitter placed either in the vicinity of a single metal nanoparticle or in the gap of a nanoparticle dimer. The optical absorption of the combined emitter-dimer structure is shown to undergo dramatic changes when the emitter excitation level is tuned across the gap-plasmon resonance. Our work opens a new avenue to deal with strongly interacting plasmon-excition hybrid systems.
我们提出了一种完全量子力学的方法来描述等离子体和激子系统(如分子或量子点)之间的耦合。该形式主义依赖于 Zubarev 的格林函数,这使我们能够超越等离子体纳米结构内部演化中的微扰范围,并充分考虑光响应的量子方面和等离子体-激子(plexcitonic)系统中的 Fano 共振。我们通过两个例子来说明这种方法,这两个例子由一个支持激子的量子发射器,要么放置在单个金属纳米粒子的附近,要么放置在纳米粒子二聚体的间隙中。当发射器的激发水平在间隙等离子体共振上调谐时,我们发现组合发射器-二聚体结构的光吸收会发生剧烈变化。我们的工作为处理强相互作用的等离子体-激子混合系统开辟了一条新途径。