Interplay between disorder and collective coherent response: Superradiance and spectral motional narrowing in the time domain
Interplay between disorder and collective coherent response: Superradiance and spectral motional narrowing in the time domain
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DOI：
10.1103/physreva.106.053703
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发表时间：
2022-04
影响因子：
2.9
通讯作者：
Hsing-Ta Chen;Zeyu Zhou;M. Sukharev;Joseph E. Subotnik;A. Nitzan
中科院分区：
文献类型：
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作者：
Hsing-Ta Chen;Zeyu Zhou;M. Sukharev;Joseph E. Subotnik;A. Nitzan
分子系综中的静态无序和动态无序以及集体光学响应之间的相互作用是纳米等离子体和纳米光子分子系统的一个重要特征。在这里，我们研究了环境无序影响下量子发射体分子系综的合作超辐射响应，包括非均匀展宽(由分子跃迁频率的静态随机分布引起)和运动窄化(由这些激发能的随机调制引起)。非均匀展宽的作用是破坏集体分子激发的相干性，抑制超辐射发射。然而，分子激发能的快速随机调制可以有效地恢复量子发射体的相干性，导致超辐射发射的恢复，这是运动窄化的一种意想不到的表现。对于非共振入射脉冲诱导的光散射过程，随机调制导致长时间处于平均激发能量的非弹性荧光发射，这表明动态无序效应实际上可以导致分子系综的集体激发。
The interplay between static and dynamic disorder and collective optical response in molecular ensembles is an important characteristic of nanoplasmonic and nanophotonic molecular systems. Here we investigate the cooperative superradiant response of a molecular ensemble of quantum emitters under the influence of environmental disorder, including inhomogeneous broadening (as induced by static random distribution of the molecular transition frequencies) and motional narrowing (as induced by stochastic modulation of these excitation energies). The effect of inhomogeneous broadening is to destroy the coherence of the collective molecular excitation and suppress superradiant emission. However, fast stochastic modulation of the molecular excitation energy can effectively restore the coherence of the quantum emitters and lead to a recovery of superradiant emission, which is an unexpected manifestation of motional narrowing. For a light scattering process as induced by an off-resonant incident pulse, stochastic modulation leads to inelastic fluorescence emission at the average excitation energy at long times and suggests that dynamic disorder effects can actually lead to collective excitation of the molecular ensemble.