Hagness Daniel E, Yang Ying, Ma Yuanqing, Ishtiaq Sumaya, Fan Sanjun, Tilley Richard D, Gooding J Justin
School of Chemistry, The University of New South Wales Sydney New South Wales 2052 Australia
Australia Centre for NanoMedicine, The University of New South Wales Sydney New South Wales 2052 Australia.
Chem Sci. 2025 Apr 15;16(20):8959-8969. doi: 10.1039/d5sc01265a. eCollection 2025 May 21.
Understanding and controlling the fluorescence of dye molecules is essential for many applications especially in biological imaging. Electrochemical-induced modulation of fluorescence provides the capability to non-destructively control the fluorescent emission of fluorophores, allowing new avenues to exploit for fluorescence imaging. This paper reports on the investigation of electrochemical-induced fluorescence modulation, focusing on the effect of the fluorophore chemical structure and the buffer composition. Of the twelve fluorophores investigated, it was observed that any variations in the chemical structure results in differences in how the fluorescence is modulated with potential. Our results showed that different core fluorescent structures exhibited distinctive modulation behaviours, the oxazine fluorophore (ATTO 655) was stable in the non-fluorescent configuration causing a prolonged low signal and the coumarin fluorophore (ATTO 390) possessed low response. Certain trends observed are related to the impact of the chemical structure on the fluorescence modulation with potential. For example, the low fluorescence modulation with potential for ATTO 390 suggests that the presence of the electron withdrawing -NR group facilitates significant modulation, while a lack of the -NR group results in low modulation. The unique response of ATTO 655 suggested the element at the radical site can affect the stability of the radical- and leuco-states and influence the fluorescence modulation that occurs. Additionally, the results show that buffer additives, such as oxygen scavengers and triplet quenchers, affect the fluorescence modulation either by stabilising the non-fluorescent radical or leuco-fluorophore structure, or improving photon emission. The quantitative characterisation of electrochemical fluorescence modulation behaviours for various fluorophores provides a guideline for future application of the fluorophores for sensing or imaging based on their performances.
理解和控制染料分子的荧光对于许多应用至关重要，尤其是在生物成像领域。电化学诱导的荧光调制提供了无损控制荧光团荧光发射的能力，为荧光成像开辟了新途径。本文报道了对电化学诱导荧光调制的研究，重点关注荧光团化学结构和缓冲液组成的影响。在所研究的12种荧光团中，观察到化学结构的任何变化都会导致荧光随电位调制方式的差异。我们的结果表明，不同的核心荧光结构表现出独特的调制行为，恶嗪荧光团（ATTO 655）在非荧光构型中稳定，导致长时间的低信号，而香豆素荧光团（ATTO 390）响应较低。观察到的某些趋势与化学结构对荧光随电位调制的影响有关。例如，ATTO 390的低荧光电位调制表明吸电子-NR基团的存在有利于显著调制，而缺乏-NR基团则导致低调制。ATTO 655的独特响应表明自由基位点的元素可以影响自由基态和无色态的稳定性，并影响发生的荧光调制。此外，结果表明，缓冲添加剂，如氧清除剂和三线态猝灭剂，通过稳定非荧光自由基或无色荧光团结构或改善光子发射来影响荧光调制。对各种荧光团的电化学荧光调制行为进行定量表征，为基于其性能的荧光团在传感或成像中的未来应用提供了指导。
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