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Computational Design of a Family of Light-Driven RotaryMolecular Motors with Improved Quantum Efficiency

机译:光驱动回转家族的计算设计具有改善的量子效率的分子电动机

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摘要

Two new light-driven molecular rotary motors based on the N-alkylated indanylidene benzopyrrole frameworks are proposed and studied using quantum chemical calculations and nonadiabatic molecular dynamics simulations. These new motors perform pure axial rotation, and the photochemical steps of the rotary cycle are dominated by the fast bond-length-alternation motion that enables ultrafast access to the S1/S0 intersection. The new motors are predicted to display a quantum efficiency higher than that of the currently available synthetic all-hydrocarbon motors. Remarkably, the quantum efficiency is not governed by the topography (peaked versus sloped) of the minimum-energy conical intersection, whereas the S1 decay time depends on the topography as well as on the energy of the intersection relative to the S1 minimum. It is the axial chirality (helicity), rather than the point chirality, that controls the sense of rotation of the motor.
机译:提出并基于量子化学计算和非绝热分子动力学模拟研究了两种基于N-烷基化的亚茚基苯并吡咯骨架的新型光驱动分子旋转电机。这些新型电机执行纯轴向旋转,旋转周期的光化学步骤主要由快速键长交替运动控制,从而可以超快地进入S1 / S0交叉点。预计新电动机将显示出比目前可用的合成全烃电动机更高的量子效率。值得注意的是,量子效率不受最小能量圆锥形交点的形貌(峰值与倾斜)的控制,而S1衰减时间取决于形貌以及交点相对于S1最小值的能量。控制电机旋转方向的是轴向手性(螺旋度),而不是点手性。

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