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首页> 外文期刊>Chemistry: A European journal >Bioluminophore and Flavin Mononucleotide Fluorescence Quenching of Bacterial Bioluminescence-A Theoretical Study
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Bioluminophore and Flavin Mononucleotide Fluorescence Quenching of Bacterial Bioluminescence-A Theoretical Study

机译：细菌生物发光的生物发光和黄素单核苷酸荧光猝灭-理论研究

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摘要

Bacterial bioluminescence with continuous glow has been applied to the fields of environmental toxin monitoring, drug screening, and in vivo imaging. Nonetheless, the chemical form of the bacterial bioluminophore is still a bone of contention. Flavin mononucleotide (FMN), one of the light-emitting products, and 4a-hydroxy-5-hydro flavin mononucleotide (HFOH), an intermediate of the chemical reactions, have both been assumed candidates for the light emitter because they have similar molecular structures and fluorescence wavelengths. The latter is preferred in experiments and was assigned in our previous density functional study. HFOH displays weak fluorescence in solutions, but exhibits strong bioluminescence in the bacterial luciferase. FMN shows the opposite behavior; its fluorescence is quenched when it is bound to the luciferase. This is the first example of flavin fluorescence quenching observed in bioluminescent systems and is merely an observation, both the quenching mechanism and quencher are still unclear. Based on theoretical analysis of high-level quantum mechanics (QM), combined QM and molecular mechanics (QM/MM), and molecular dynamics (MD), this paper confirms that HFOH in its first singlet excited state is the bioluminophore of bacterial bioluminescence. More importantly, the computational results indicate that Tyr110 in the luciferase quenches the FMN fluorescence via an electron-transfer mechanism.
机译：具有连续发光的细菌生物发光已被应用于环境毒素监测，药物筛选和体内成像领域。尽管如此，细菌生物发光体的化学形式仍然是争论的焦点。黄素单核苷酸（FMN）（一种发光产物）和4a-羟基-5-氢黄素单核苷酸（HFOH）（一种化学反应的中间体）都被认为是发光体的候选物，因为它们具有相似的分子结构和荧光波长。后者在实验中是首选，并在我们之前的密度泛函研究中分配。 HFOH在溶液中显示弱荧光，但在细菌荧光素酶中显示强生物发光。 FMN显示相反的行为;当它与荧光素酶结合时，其荧光被淬灭。这是在生物发光系统中观察到的黄素荧光猝灭的第一个例子，仅是一个观察，猝灭机理和猝灭剂仍然不清楚。基于对高级量子力学（QM），QM和分子力学（QM / MM）以及分子动力学（MD）的理论分析，本文证实HFOH在其第一个单重激发态是细菌生物发光的生物发光体。更重要的是，计算结果表明，荧光素酶中的Tyr110通过电子转移机制淬灭了FMN荧光。

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