厦门大学Jian-Feng Li研究组的最新研究实现了在单一纳米腔中调节荧光磷光发射。该研究于2023年9月5日发表于国际一流学术期刊《美国化学会杂志》上。

在这项工作中，该研究组通过将单线态-三重态分子发射器与合理设计的等离子体腔耦合来实现暗磷光过程的发光捕获。该方法所实现的珀塞尔增强效应超过1000倍，可以克服三重态跃迁禁阻，使辐射增强具有可选择的发射波长。光谱结果和理论模拟表明，荧光-磷光峰位置可以在可见光到近红外的宽波长范围内智能定制。

他们的研究为等离子体调节分子发射行为提供了新的思路，这对于推进光电和生物医学领域等离子体调节荧光磷光光谱的研究至关重要。

据了解，在单一系统中实现荧光-磷光的双发射是生物成像、传感、信息加密等领域的一个极其重要的课题。然而，室温下的磷光过程一般处于一种内在的“暗态”中，这是由于自旋禁阻跃迁和三线态的快速非辐射衰变导致的。

附：英文原文

Title: Tailoring Fluorescence–Phosphorescence Emission with a Single Nanocavity

Author: Wei Peng, Yao-Hui Wang, Jiaxing He, Jing-Liang Yang, Jingyu Wang, Petar M. Radjenovic, Jia-Sheng Lin, Zhilin Yang, Ming-De Li, Fan-Li Zhang, Yue-Jiao Zhang, Jun Yi, Jian-Feng Li

Issue&Volume: September 5, 2023

Abstract: Realizing the dual emission of fluorescence–phosphorescence in a single system is an extremely important topic in the fields of biological imaging, sensing, and information encryption. However, the phosphorescence process is usually in an inherently “dark state” at room temperature due to the involvement of spin-forbidden transition and the rapid non-radiative decay rate of the triplet state. In this work, we achieved luminescent harvesting of the dark phosphorescence processes by coupling singlet-triplet molecular emitters with a rationally designed plasmonic cavity. The achieved Purcell enhancement effect of over 1000-fold allows for overcoming the triplet forbidden transitions, enabling radiation enhancement with selectable emission wavelengths. Spectral results and theoretical simulations indicate that the fluorescence–phosphorescence peak position can be intelligently tailored in a broad range of wavelengths, from visible to near-infrared. Our study sheds new light on plasmonic tailoring of molecular emission behavior, which is crucial for advancing research on plasmon-tailored fluorescence–phosphorescence spectroscopy in optoelectronics and biomedicine.

DOI: 10.1021/jacs.3c05496

Source: https://pubs.acs.org/doi/10.1021/jacs.3c05496