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arXiv 2104.00852cond-mat.mes-hallphysics.chem-phphysics.opticsquant-ph
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作为非线性光学超材料的强耦合单分子等离子体微腔无序系综

Disordered ensembles of strongly coupled single-molecule plasmonic picocavities as nonlinear optical metamaterials

Felipe Herrera, Marina Litinskaya

摘要:

我们建议使用分子picocavity合奏宏观相干非线性光学器件,使纳米级强耦合。对于一个通用的picocavity模型,包括分子和光子的无序,我们推导出理论上的性能界限相干交叉相位调制信号使用弱经典场的不同频率。我们表明,强耦合的picocavity { \it vacua}与特定的振动边带中的分子发射光谱的结果在一个显着的变化的超材料的有效折射率相对于一个无分子的情况下,由于真空诱导的Autler-Townes效应。对于一个现实的分子无序模型,我们证明了交叉相位调制的光场弱至10千瓦/厘米$^2$是可行的,在室温下使用分子picocavities的稀系综,提供了有限的真空是不共振驱动的外部探测场}。我们的工作为利用强耦合进行光态制备和量子控制的等离子体超材料的发展铺平了道路。

英文摘要:

We propose to use molecular picocavity ensembles as macroscopic coherent nonlinear optical devices enabled by nanoscale strong coupling. For a generic picocavity model that includes molecular and photonic disorder, we derive theoretical performance bounds for coherent cross-phase modulation signals using weak classical fields of different frequencies. We show that strong coupling of the picocavity {\it vacua} with a specific vibronic sideband in the molecular emission spectrum results in a significant variation of the effective refractive index of the metamaterial relative to a molecule-free scenario, due to a vacuum-induced Autler-Townes effect. For a realistic molecular disorder model, we demonstrate that cross-phase modulation of optical fields as weak as 10 kW/cm$^2$ is feasible using dilute ensembles of molecular picocavities at room temperature, provided that the confined vacuum is not resonantly driven by the external probe field}. Our work paves the way for the development of plasmonic metamaterials that exploit strong coupling for optical state preparation and quantum control.

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