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Light-driven Reciprocating Host–Guest Molecular Machines
JETP Letters ( IF 1.4 ) Pub Date : 2021-05-26 , DOI: 10.1134/s002136402112002x
V. M. Rozenbaum , M. L. Dekhtyar , I. V. Shapochkina , L. I. Trakhtenberg

General operating principles have been established for light-driven molecular machines with different ground- and excited-state potential energies of a Brownian particle in a surrounding force field. The optomechanical coupling between the time dependences of the particle photoexcited-state population and its coordinate is described in terms of a theory developed for the laser-pulse controlled reciprocating Brownian photomotor which consists of the guest dye and host cavitand molecules. The time dependences of spectroscopic and mechanical characteristics have been calculated in the approximation of parabolic potential profiles of the ground and excited states. As shown, the dependence of the average velocity of reciprocating motion on the repetition period of ultrashort laser pulses is a nonmonotonic function, with its maximum specifying the optimal operating mode of the molecular machine. In the case when the inclusion of the dye molecule into the cavitand interior hinders the formation of the fluorescence-quenching twisted state and the deactivation rate constant of the guest molecule decreases with its coordinate, the fluorescence lifetime of the completely cavitand-included dye lengthens significantly, in agreement with the available experimental data. The presented analytical relations between mechanical and optical characteristics of the reciprocating molecular machines under study offer wide opportunities for controlling their motion as well as their observed fluorescence.



中文翻译:

光驱往复式宿主-客体分子机器

已经建立了在周围力场中具有布朗粒子的不同基态和激发态势能的光驱动分子机器的一般操作原理。根据由客体染料和主体空泡分子组成的激光脉冲控制往复式布朗光电机的理论,描述了光激发态粒子的时间依赖性与其坐标之间的光机械耦合。在基态和激发态的抛物线电势曲线的近似值中,已计算出光谱和机械特性的时间依赖性。如图所示,往复运动的平均速度对超短激光脉冲重复周期的依赖性是非单调函数,其最大值指定了分子机器的最佳操作模式。当染料分子包含在空洞内部时,阻碍了荧光猝灭扭曲态的形成,并且客体分子的失活速率常数随着其坐标的降低而降低,完全包含空洞的染料的荧光寿命显着延长。 ,与可用的实验数据一致。所研究的往复式分子机器的机械和光学特性之间的分析关系为控制其运动以及观察到的荧光提供了广泛的机会。当染料分子包含在空洞内部时,阻碍了荧光猝灭扭曲态的形成,并且客体分子的失活速率常数随着其坐标的降低而降低,完全包含空洞的染料的荧光寿命显着延长。 ,与可用的实验数据一致。所研究的往复式分子机器的机械和光学特性之间的分析关系为控制其运动以及观察到的荧光提供了广泛的机会。当染料分子包含在空洞内部时,阻碍了荧光猝灭扭曲态的形成,并且客体分子的失活速率常数随着其坐标的降低而降低,完全包含空洞的染料的荧光寿命显着延长。 ,与可用的实验数据一致。所研究的往复式分子机器的机械和光学特性之间的分析关系为控制其运动以及观察到的荧光提供了广泛的机会。

更新日期:2021-05-26
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