Real-time observation of ultrafast Rabi oscillations between excitons and plasmons in metal nanostructures with J-aggregates
Real-time observation of ultrafast Rabi oscillations between excitons and plasmons in metal nanostructures with J-aggregates
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DOI：
10.1038/nphoton.2012.340
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发表时间：
2013-02-01
期刊：
影响因子：
35
通讯作者：
Lienau, Christoph
中科院分区：
文献类型：
--
作者：
Vasa, Parinda;Wang, Wei;Lienau, Christoph
表面等离子体激元（SPP），金属和电介质之间界面处的光学激发，具有在纳米尺度上引导和操纵光的巨大潜力（1-3）。然而，它们弱的光学非线性阻碍了有源器件的制造，例如，用于全光开关（4-7）或信息处理（8，9）。最近，已经证明了SPP和非线性量子发射器之间的强光学偶极耦合，其简正模分裂高达700 meV（参考文献10-15）。量子发射体和SPP场之间预测的超快能量转移可能是在纳米尺度上通过光切换光的关键微观机制。在这里，我们提出了第一个实时观察超快拉比振荡的J-聚集体/金属纳米结构，表明激子量子发射体和SPP字段之间的相干能量转移。我们展示了通过控制激子密度在10 fs时间尺度上的耦合能量的相干操纵，这代表了向相干的全光超快等离子体电路和设备迈出的一步。
Surface plasmon polaritons (SPPs), optical excitations at the interface between a metal and a dielectric, carry significant potential for guiding and manipulating light on the nanoscale(1-3). However, their weak optical nonlinearities hinder active device fabrication, for example, for all-optical switching(4-7) or information processing(8,9). Recently, strong optical dipole coupling has been demonstrated between SPPs and nonlinear quantum emitters with normal mode splittings of up to 700 meV (refs 10-15). The predicted ultrafast energy transfer between quantum emitters and SPP fields could be a crucial microscopic mechanism for switching light by light on the nanoscale. Here, we present the first real-time observation of ultrafast Rabi oscillations in a J-aggregate/metal nanostructure, indicating coherent energy transfer between excitonic quantum emitters and SPP fields. We demonstrate coherent manipulation of the coupling energy by controlling the exciton density on a 10 fs timescale, which represents a step towards coherent, all-optical ultrafast plasmonic circuits and devices.