Nonlinear Born-Kuhn Analog for Chiral Plasmonics,ACS Photonics

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Nonlinear Born-Kuhn Analog for Chiral Plasmonics
ACS Photonics ( IF 6.5 ) Pub Date : 2019-12-05 , DOI: 10.1021/acsphotonics.9b01400
Lili Gui _{1,

2} , Mario Hentschel ₁ , Josselin Defrance ₁ , Joachim Krauth ₁ , Thomas Weiss ₁ , Harald Giessen ₁

Affiliation

Chiral plasmonic metasurfaces are intriguing platforms to achieve large nonlinear chiroptical effects, which could be desirable for sensitive chiral molecular analysis. The combination of a superlinear response with high plasmonic near-field enhancement leads to large nonlinear optical activity, which can be much stronger than its linear counterpart. A complex mixture of multiresonances, structural symmetry, and anisotropy in 3D chiral plasmonic nanostructures as well as experimental configurations has up to now hampered understanding of the underlying physics and quantitative modeling of the relevant nonlinear chiroptical effects. Here we study third-harmonic circular dichroism of archetypical Born-Kuhn type bilayer chiral metasurfaces made of corner-stacked orthogonal gold nanorods arranged in C₄ symmetry, which avoids most of the aforementioned issues. With a coupled anharmonic oscillator model built upon chirally coupled electric dipole moments, we are able to retrieve the nonlinear chiroptical response of such chiral nanostructures. The comparison of nonlinear spectroscopic measurements with our model as well as nonlinear simulations enables interpretation of the large nonlinear circular dichroism. Our research might pave the way toward flexible control over nonlinear susceptibility tensors of artificial chiral meta-molecules at will and could allow for highly sensitive nonlinear chiral sensing.

中文翻译：

用于手性等离子体的非线性Born-Kuhn模拟

手性等离子体超表面是实现大型非线性手性效应的有趣平台，这对于灵敏的手性分子分析可能是理想的。超线性响应与高等离激元近场增强的组合会导致较大的非线性光学活动，这可能比其线性对应物强得多。到目前为止，3D手性等离子体纳米结构中的多共振，结构对称和各向异性的复杂混合物以及实验配置阻碍了对基础物理学的理解以及对相关非线性手性效应的定量建模。在这里，我们研究由角堆积的正交金纳米棒排列在C _4中的原型Born-Kuhn型双层手性超表面的三次谐波圆二色性对称性，避免了大多数上述问题。利用建立在手性偶极矩上的耦合非谐振荡器模型，我们能够检索这种手性纳米结构的非线性手性响应。将非线性光谱测量值与我们的模型以及非线性模拟进行比较，可以解释大型非线性圆二色性。我们的研究可能为随意控制人工手性元大分子的非线性磁化张量铺平了道路，并可能允许高度灵敏的非线性手性传感。

更新日期：2019-12-05

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