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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >A straightforward method of analysis for direct quantum dynamics: Application to the photochemistry of a model cyanine
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A straightforward method of analysis for direct quantum dynamics: Application to the photochemistry of a model cyanine

机译：直接量子动力学的直接分析方法：在模型花菁的光化学中的应用

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摘要

We present a new way of analyzing direct quantum dynamics simulations based on a Mulliken-type population analysis. This provides a straightforward interpretation of the wavepacket in much the same way as semiclassical trajectories are usually analyzed. The result can be seen as a coupled set of quantum trajectories. We apply this to the study of the photochemistry of a 12-atom model cyanine to explore possibilities for intelligent optimal control. The work presented here builds on previous semiclassical dynamics simulations [Hunt, P. A.; Robb, M. A. J. Am. Chem. Soc. 2005, 127, 5720 ]. Those calculations suggested that, by controlling the distribution of momentum components in the initial wavepacket, it should be possible to drive the system to a specific region of the conical intersection seam and ultimately control the product distribution. This was confirmed experimentally by optimal control methods [Dietzek, B.; Brüggemann, B.; Pascher, T.; Yartsev, A. J. Am. Chem. Soc. 2007, 129, 13014]. This paper aims to demonstrate this in a quantum dynamics context and give further insight into the conditions required for control. Our results show that directly addressing the trans-cis torsional modes is not efficient. Instead, one needs to decrease the momentum in the skeletal deformation coordinates to prompt radiationless decay near the minimum conical intersection at large twist angles.
机译：我们提出了一种基于Mulliken型种群分析的直接量子动力学模拟分析的新方法。与通常分析半古典轨迹的方式几乎相同，这提供了对波包的直接解释。结果可以看作是一组量子轨迹。我们将其应用于12原子模型花青的光化学研究，以探索智能最佳控制的可能性。这里介绍的工作建立在以前的半经典动力学模拟的基础上[Hunt，P. A .;罗布（Robb，M.A.J. Am。）化学Soc。 2005，127，5720]。这些计算表明，通过控制初始波包中动量分量的分布，应该有可能将系统驱动到圆锥形相交接缝的特定区域，并最终控制产品分布。通过最佳控制方法实验证实了这一点[Dietzek，B .;布吕格曼，B。帕歇（T. Yartsev，A.J. Am。化学Soc。 2007，129，13014]。本文旨在在量子动力学的背景下证明这一点，并进一步了解控制所需的条件。我们的结果表明，直接解决反式扭转模式是无效的。取而代之的是，需要减小骨骼变形坐标中的动量，以在大扭转角处的最小圆锥形交叉点附近促使无辐射衰减。

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