Excited State Vibrations of Isotopically Labeled FMN Free and Bound to a Light-Oxygen-Voltage (LOV) Protein.
Excited State Vibrations of Isotopically Labeled FMN Free and Bound to a Light-Oxygen-Voltage (LOV) Protein.
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DOI：
10.1021/acs.jpcb.0c04943
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发表时间：
2020-08-20
期刊：
影响因子：
--
通讯作者：
Meech SR
中科院分区：
文献类型：
--
作者：
Iuliano JN;Hall CR;Green D;Jones GA;Lukacs A;Illarionov B;Bacher A;Fischer M;French JB;Tonge PJ;Meech SR
黄素蛋白是光生物学中重要的蓝光传感器，在光遗传学中起着关键作用。因此，表征其激发态结构和动力学是一个重要的目标。在这里，我们提出了一个详细的研究激发态的振动光谱的黄素monopolytide（FMN），在解决方案和绑定到LOV-2（光氧电压）域的燕麦phototropin。通过共振超快飞秒受激拉曼光谱（FSRS），确定了光激发单重态和活性三重态的振动频率。为了分配所观察到的光谱，振动频率的激发态的计算使用密度泛函理论，测量和理论都适用于四个不同的同位素FMN。激发态模式的分配细化在这两个国家和它们的灵敏度氘和蛋白质环境进行了研究。我们表明，共振FSRS提供了一个有用的工具，用于表征光敏黄素蛋白，并能够突出发色团本地化模式，并记录氢/氘交换。
Flavoproteins are important blue light sensors in photobiology and play a key role in optogenetics. The characterization of their excited state structure and dynamics is thus an important objective. Here we present a detailed study of excited state vibrational spectra of flavin mononucleotide (FMN), in solution and bound to the LOV-2 (Light-Oxygen-Voltage) domain of Avena sativa phototropin. Vibrational frequencies are determined for the optically excited singlet state and the reactive triplet state, through resonant ultrafast femtosecond stimulated Raman spectroscopy (FSRS). To assign the observed spectra, vibrational frequencies of the excited states are calculated using density functional theory, and both measurement and theory are applied to four different isotopologues of FMN. Excited state mode assignments are refined in both states and their sensitivity to deuteration and protein environment are investigated. We show that resonant FSRS provides a useful tool for characterizing photoactive flavoproteins, and is able to highlight chromophore localized modes, and to record hydrogen/deuterium exchange.
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影响因子：
15
作者：
Brust R;Lukacs A;Haigney A;Addison K;Gil A;Towrie M;Clark IP;Greetham GM;Tonge PJ;Meech SR
通讯作者：
Meech SR
影响因子：
2.9
作者：
Iuliano JN;Gil AA;Laptenok SP;Hall CR;Tolentino Collado J;Lukacs A;Hag Ahmed SA;Abyad J;Daryaee T;Greetham GM;Sazanovich IV;Illarionov B;Bacher A;Fischer M;Towrie M;French JB;Meech SR;Tonge PJ
通讯作者：
Tonge PJ
影响因子：
2.9
作者：
Harper, SM;Christie, JM;Gardner, KH
通讯作者：
Gardner, KH
影响因子：
2.9
作者：
Haigney, Allison;Lukacs, Andras;Tonge, Peter J.
通讯作者：
Tonge, Peter J.
DOI：
10.1126/science.aah3404
发表时间：
2016-12-16
期刊：
Science (New York, N.Y.)
影响因子：
--
作者：
Dagliyan O;Tarnawski M;Chu PH;Shirvanyants D;Schlichting I;Dokholyan NV;Hahn KM
通讯作者：
Hahn KM