Dipartimento di Fisica, Università di Pavia, via Bassi 6, 27100 Pavia, Italy.
Center for Biomolecular Nanotechnologies @ UNILE - Istituto Italiano di Tecnologia, 73010 Arnesano, Italy.
Sci Rep. 2016 Oct 18;6:34772. doi: 10.1038/srep34772.
We report theoretical evidence that bulk nonlinear materials weakly interacting with highly localized plasmonic modes in ultra-sub-wavelength metallic nanostructures can lead to nonlinear effects at the single plasmon level in the visible range. In particular, the two-plasmon interaction energy in such systems is numerically estimated to be comparable with the typical plasmon linewidths. Localized surface plasmons are thus predicted to exhibit a purely nonclassical behavior, which can be clearly identified by a sub-Poissonian second-order correlation in the signal scattered from the quantized plasmonic field under coherent electromagnetic excitation. We explicitly show that systems sensitive to single-plasmon scattering can be experimentally realized by combining electromagnetic confinement in the interstitial region of gold nanodimers with local infiltration or deposition of ordinary nonlinear materials. We also propose configurations that could allow to realistically detect such an effect with state-of-the-art technology, overcoming the limitations imposed by the short plasmonic lifetime.
我们的理论研究表明,在亚波长金属纳米结构中,与高度局域化的等离子体模式弱相互作用的大块非线性材料,可在可见光波段于单个等离子体水平上产生非线性效应。具体而言,此类系统中的双等离子体相互作用能量被数值估计与典型等离子体线宽相当。因此,局域表面等离子体有望表现出纯粹的非经典行为,通过相干电磁激发下从量化等离子体场散射的信号中的亚泊松二阶相关,可清晰识别这种行为。我们明确表明,通过将金纳米二聚体的间隙区域中的电磁限制与普通非线性材料的局部渗透或沉积相结合,可在实验上实现对单等离子体散射敏感的系统。我们还提出了一些配置,这些配置可利用现有技术,克服由等离子体短寿命带来的限制,来实际探测到这种效应。