State Key Laboratory of Molecular & Process Engineering, Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, 200241, China.
Hongzhiwei Technology (Shanghai) CO.LTD., 1599 Xinjinqiao Road, Pudong, Shanghai, China.
Biosens Bioelectron. 2024 Jun 15;254:116231. doi: 10.1016/j.bios.2024.116231. Epub 2024 Mar 15.
Strong light-matter coupling between molecules and electromagnetic field lead to the formation of hybrid polaritonic states for surface enhanced Raman scattering (SERS) detection. However, owing to the inefficient interaction between zero-point fluctuations of photons/plasmons and molecular electronic transitions, the Raman enhancement is limited in relative low levels. Here, we propose and fabricate a TiO/CuSe/R6G nanocavity based photonic-plasmonic-polaritonic resonator for single molecular SERS detection. Through precisely matching the energy levels of illuminated photon, generated plasmon, and molecular polariton, an extremely high Raman enhancement factor of 2.6 × 10 is implemented. The rationally designed SERS substrate allows sensitive detection of miRNA-21 in single molecular level with a detection limit of 1.58 aM. The hybrid SERS mechanism both from electromagnetic and chemical perspectives in this photonic-plasmonic-polaritonic resonance strategy provides insight into polaritonic semiconductor systems, thus paving the way for new experimental possibilities in light-matter hybrids.
分子与电磁场之间的强光物质耦合导致表面增强拉曼散射 (SERS) 检测中形成混合极化激元态。然而，由于光子/等离子体的零点涨落与分子电子跃迁之间的相互作用效率低下，拉曼增强被限制在相对较低的水平。在这里，我们提出并制造了一种基于 TiO/CuSe/R6G 纳米腔的光子-等离子体-极化激元共振器，用于单分子 SERS 检测。通过精确匹配被照亮光子、产生的等离子体和分子极化激元的能级，实现了极高的拉曼增强因子 2.6×10。这种合理设计的 SERS 基底允许以单分子水平灵敏地检测 miRNA-21，检测限低至 1.58 aM。这种光子-等离子体-极化激元共振策略中的混合 SERS 机制从电磁和化学两个方面提供了对极化激元半导体系统的深入了解，为光物质混合体中的新实验可能性铺平了道路。
