Andrews David L, Crisp Richard G, Li Shaopeng
Nanostructures and Photomolecular Systems, School of Chemical Sciences, University of East Anglia, Norwich NR4 7TJ, United Kingdom.
J Chem Phys. 2007 Nov 7;127(17):174702. doi: 10.1063/1.2781392.
Through photonic mechanisms based on near-field coupling, laser radiation can engage with resonant energy transfer in a variety of suitably designed materials and molecular structures. Energy that has been acquired, through the initial absorption of resonant laser light, undergoes transfer between chromophores only on the throughput of off-resonant light, the process known as laser-assisted resonance energy transfer. The comprehensive results that are presented here extend and generalize the theory for both single and dual beam configurations, producing results that are applicable to media of various types including doped crystals, heterogeneous multichromophore solids, and solutions. The detailed principles, here explained in terms of both energetics and optical selection rule criteria, are specifically illustrated for a variety of materials. It is shown how general application of the theory can facilitate the elucidation of experiments, by clearly interpreting the effects of laser polarization manipulation. On further analysis of the photophysical mechanisms it is also demonstrated that such effects represent an entirely practicable basis for optical switching and logic gate operation. The additional polarization selectivity afforded by a two-beam setup proves to allow the most complete system control. With such a configuration, there is considerable promise for the realization of new optically driven logic and molecular devices.
通过基于近场耦合的光子机制，激光辐射能够与各种经过适当设计的材料和分子结构中的共振能量转移相互作用。通过对共振激光的初始吸收而获得的能量，仅在非共振光的通过过程中，在发色团之间进行转移，这个过程被称为激光辅助共振能量转移。这里展示的综合结果扩展并概括了单光束和双光束配置的理论，得出的结果适用于包括掺杂晶体、多发色团异质固体和溶液等各种类型的介质。这里从能量学和光学选择规则标准两方面解释的详细原理，针对各种材料进行了具体说明。通过清晰地解释激光偏振操纵的效果，展示了该理论的普遍应用如何有助于阐明实验。在对光物理机制的进一步分析中还表明，这些效果代表了光开关和逻辑门操作完全可行的基础。双光束设置所提供的额外偏振选择性被证明能够实现最完整的系统控制。有了这样的配置，实现新型光驱动逻辑和分子器件有很大的前景。
