Fluorescence-Detected Circular Dichroism of a Chiral Molecular Monolayer with Dielectric Metasurfaces,Journal of the American Chemical Society

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Fluorescence-Detected Circular Dichroism of a Chiral Molecular Monolayer with Dielectric Metasurfaces
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2020-10-13 , DOI: 10.1021/jacs.0c07140
Michelle L. Solomon ₁ , John M. Abendroth ₁ , Lisa V. Poulikakos _{1,

2} , Jack Hu ₁ , Jennifer A. Dionne ₁

Affiliation

Strong enhancement of molecular circular dichroism (CD) has the potential to enable efficient asymmetric photolysis, a method of chiral separation that has conventionally been impeded by insufficient yield and low enantiomeric excess. Here, we study experimentally how predicted enhancements in optical chirality density near resonant silicon nanodisks boost CD. We use fluorescence-detected circular dichroism (FDCD) spectroscopy to measure indirectly the differential absorption of circularly polarized light by a monolayer of optically active molecules functionalized to silicon nanodisk arrays. Importantly, the molecules and nanodisk antennas have spectrally coincident resonances, and our fluorescence technique allows us to deconvolute absorption in the nanodisks from the molecules. We find that enhanced FDCD signals depend on nanophotonic resonances, in good agreement with simulated differential absorption and optical chirality density, while no signal is detected from molecules adsorbed on featureless silicon surfaces. These results verify the potential of nanophotonic platforms to be used for asymmetric photolysis with lower energy requirements.

中文翻译：

具有介电超表面的手性分子单层的荧光检测圆二色性

分子圆二色性 (CD) 的强增强有可能实现有效的不对称光解，这是一种手性分离方法，通常受到收率不足和对映体过量低的阻碍。在这里，我们通过实验研究了共振硅纳米盘附近光学手性密度的预测增强如何促进 CD。我们使用荧光检测圆二色性 (FDCD) 光谱来间接测量圆偏振光由功能化到硅纳米盘阵列的单层光学活性分子的差异吸收。重要的是，分子和纳米盘天线具有光谱重合的共振，我们的荧光技术使我们能够解卷积纳米盘中分子的吸收。我们发现增强的 FDCD 信号依赖于纳米光子共振，与模拟的微分吸收和光学手性密度非常一致，而从吸附在无特征硅表面上的分子中没有检测到信号。这些结果验证了纳米光子平台用于具有较低能量需求的不对称光解的潜力。

更新日期：2020-10-13

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