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Detecting a single-molecule fluorescent spectrum with a low quantum yield needs to enhance the signal greatly overcome the noise disturbance. Based on plasmon-enhanced fluorescence method with single gold nanorods antenna, we measured the emission spectra of a single methylene blue or crystal violet molecules with an effective integration time of ~2.14 milliseconds at room temperature. These transient spectra have revealed the single-molecule spectral shape and intensity fluctuations. We found that the transient spectral shape is dominated by the molecule, while the plasmon resonance determines the averaged spectral shape. These fluctuations can be understood as transitions between metastable minima in the molecular potential-energy surface, as supported by complementary ab initio simulations.
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Te Wen, Xiaowei Zhang, Yuqing Cheng, Guowei Lu, Qihuang Gong, "Transient spectral fluctuations of single-molecule fluorescence enhanced by a single optical antenna," Proc. SPIE 11556, Nanophotonics and Micro/Nano Optics VI, 115560O (10 October 2020); https://doi.org/10.1117/12.2573537