Photonic Molecular Processors by means of Quantum Phase Control of Electron and Exciton Transport

在高度组织的分子系统中，激发转移和电子转移等相干光化学反应可以以量子力学波包的相干运动的形式非常快地（小于1ps）发生。本工作是从观察蒽、苝和卟啉树状大分子二聚体中激子运动的量子相干性开始的。量子拍出现在荧光各向异性衰变中，是指激子在能量转移到最终态过程中的振荡运动。锁相双脉冲激发方法的发展为我们提供了另一种检测反应量子相干性的方法。此外，该方法允许我们通过控制两个激光脉冲的相位来检查相干光反应的光开关行为。

In highly organized molecular systems, the coherent photochemical reactions such as excitation transfer and electron transfer can occur very fast (less than 1 ps) as a coherent motion of quantum mechanical wavepacket. The present work has been started with observation of the quantum coherence of exciton motion in molecular dimers of anthracene, perylene and in porphyrin dendrimers. Quantum beats appeared on fluorescence anisotropy decay which means the oscillatory motion of exciton in the course of energy transfer processes into the final state. The phase-locked double-pulse excitation method has been developed and provided us with another method to examine the quantum coherence of the reaction. Furthermore, this method allowed us to examine the photoswitching behavior of the coherent photoreaction by controlling the phase of two laser pulses.