基于分子转子的Bioprobe-PicoGreen的超快速动力学：对原纤维传感机理的理解。,The Journal of Physical Chemistry B

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基于分子转子的Bioprobe-PicoGreen的超快速动力学：对原纤维传感机理的理解。
The Journal of Physical Chemistry B ( IF 2.8 ) Pub Date : 2019-10-04 , DOI: 10.1021/acs.jpcb.9b05922
Aruna K Mora _{1,

2} , Sukhendu Nath _{1,

2}

Affiliation

最近的一份报告显示，基于花青的分子转子PicoGreen对淀粉样蛋白原纤维具有非常强的亲和力，并且在与胰岛素淀粉样蛋白原纤维结合后，其发射产率大大提高。为了获得有关引起其淀粉样蛋白传感行为的激发态分子过程的更深入的知识，已经研究了PicoGreen在具有不同极性和粘度的分子溶剂中的详细超快动力学。我们对飞秒时间分辨PicoGreen发射的详细研究表明，介质的极性和粘度在其光激发态的失活中都起着至关重要的作用。对时间分辨数据的详细分析表明，分子内电荷转移（ICT）状态的形成与溶剂粘度无关，发生在超快时间范围内（<2 ps），然后在较长的时间尺度内在极性溶剂中形成扭曲的ICT（TICT）状态。由于粘度状态下的激发态动力学，在激发态下由于振幅大的扭转运动而从ICT态形成了TICT。最后，在原纤维介质中的动力学研究表明，在激发态扭转运动中存在阻滞作用，这主要是由于其在胰岛素淀粉样蛋白原纤维中观察到了较大的荧光增强。

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Ultrafast Dynamics of a Molecular Rotor-Based Bioprobe-PicoGreen: Understanding toward Fibril Sensing Mechanism.

A recent report shows that the cyanine-based molecular rotor, PicoGreen, has very strong affinity toward amyloid fibrils and shows large increase in its emission yield upon binding with insulin amyloid fibrils. To gain deeper knowledge about the excited-state molecular processes that are responsible for its amyloid sensing behavior, detailed ultrafast dynamics of PicoGreen in molecular solvents with varying polarity and viscosity have been investigated. Our detailed studies on femtosecond time-resolved emission of PicoGreen show that both polarity and viscosity of the medium a play vital role in the deactivation of its photoexcited state. Detailed analysis of the time-resolved data suggests the formation of the intramolecular charge transfer (ICT) state, which is independent of solvent viscosity, takes place in ultrafast time scales (<2 ps), followed by the formation of a twisted ICT (TICT) state at a longer time scale in polar solvents. The formation of TICT from the ICT state due to the large amplitude torsional motion in its excited state has been supported by viscosity-dependent excited-state dynamics. Finally, the dynamical studies in fibrillar medium demonstrate the retardation in the excited-state torsional motion, which is primarily responsible for its observed large fluorescence enhancement in insulin amyloid fibrils.

更新日期：2019-10-05

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