Scott Zoe, Muhammad Shafi, Shahbazyan Tigran V
Department of Physics, Jackson State University, Jackson, Mississippi 39217, USA.
J Chem Phys. 2022 May 21;156(19):194702. doi: 10.1063/5.0083197.
We present an analytical model describing the transition to a strong coupling regime for an ensemble of emitters resonantly coupled to a localized surface plasmon in a metal-dielectric structure. The response of a hybrid system to an external field is determined by two distinct mechanisms involving collective states of emitters interacting with the plasmon mode. The first mechanism is the near-field coupling between the bright collective state and the plasmon mode, which underpins the energy exchange between the system components and gives rise to exciton-induced transparency minimum in scattering spectra in the weak coupling regime and to emergence of polaritonic bands as the system transitions to the strong coupling regime. The second mechanism is the Fano interference between the plasmon dipole moment and the plasmon-induced dipole moment of the bright collective state as the hybrid system interacts with the radiation field. The latter mechanism is greatly facilitated by plasmon-induced coherence in a system with the characteristic size below the diffraction limit as the individual emitters comprising the collective state are driven by the same alternating plasmon near field and, therefore, all oscillate in phase. This cooperative effect leads to scaling of the Fano asymmetry parameter and of the Fano function amplitude with the ensemble size, and therefore, it strongly affects the shape of scattering spectra for large ensembles. Specifically, with increasing emitter numbers, the Fano interference leads to a spectral weight shift toward the lower energy polaritonic band.
我们提出了一个分析模型,用于描述在金属 - 介质结构中,与局域表面等离子体共振耦合的一组发射器向强耦合 regime 的转变。混合系统对外场的响应由两种不同机制决定,这两种机制涉及发射器的集体态与等离子体模式的相互作用。第一种机制是亮集体态与等离子体模式之间的近场耦合,它支撑着系统组件之间的能量交换,并在弱耦合 regime 下导致散射光谱中激子诱导的透明度最小值,以及在系统转变为强耦合 regime 时产生极化子带。第二种机制是当混合系统与辐射场相互作用时,等离子体偶极矩与亮集体态的等离子体诱导偶极矩之间的 Fano 干涉。在特征尺寸低于衍射极限的系统中,由于构成集体态的各个发射器由相同的交变等离子体近场驱动,因此都同相振荡,等离子体诱导的相干极大地促进了后一种机制。这种协同效应导致 Fano 不对称参数和 Fano 函数幅度随系综大小缩放,因此,它对大系综的散射光谱形状有强烈影响。具体而言,随着发射器数量的增加,Fano 干涉导致光谱权重向较低能量的极化子带转移。