Lash Miller Chemical Laboratories, Institute for Optical Sciences and Centre for Quantum Information and Quantum Control, University of Toronto, 80 St. George St., Toronto, Canada.
Faraday Discuss. 2013;163:341-51; discussion 393-432. doi: 10.1039/c3fd00009e.
The mounting evidence of recent years regarding long-lived coherent dynamics of electronic excitations in several light-harvesting antenna proteins suggests the possibility of realizing and exploiting light-initiated quantum dynamics in synthetic molecular devices based on electronic energy transfer. Inspired by the field of molecular logic, we focus this discussion on the prospect of using quantum coherence to control the direction of energy flow in a molecular circuit. As a prototype system we consider a circuit consisting of three chromophores that deliver energy to two trap chromophores. Our aim is to control to which trap the energy is more likely to be delivered. This is achieved by switching one of the circuit chromophores ON and OFF from the system, such that the direction of energy flow substantially changes from the ON and OFF states of the circuit. We find that quantum coherence can allow a significant ability to direct energy transfer in the circuit. However, when realistic levels of noise are added, quantum coherence only slightly improves the ability to direct electronic energy in comparison to a classical hopping mechanism.
近年来,越来越多的证据表明,在几种光捕获天线蛋白质中,电子激发的长寿命相干动力学是存在的,这表明在基于电子能量转移的合成分子器件中实现和利用光引发的量子动力学是有可能的。受分子逻辑领域的启发,我们将讨论的重点放在利用量子相干来控制分子电路中能量流动方向的前景上。作为一个原型系统,我们考虑了一个由三个发色团组成的电路,这些发色团将能量传递给两个捕获发色团。我们的目的是控制能量更有可能被传递到哪个捕获发色团。这是通过从系统中打开和关闭一个电路发色团来实现的,从而使能量流动的方向从电路的打开和关闭状态发生实质性的改变。我们发现,量子相干可以显著提高电路中能量转移的方向性。然而,当加入现实水平的噪声时,与经典的跳跃机制相比,量子相干只是略微提高了引导电子能量的能力。