量子态动力学演化的多维谱学研究

The proposed project aims at developing and applying quantum chemistry methods, to simulate the use of the multi-dimensional spectroscopy technique for detecting quantum state dynamics evolutions in carbon nano-materials. The detecting mechanisms to be investigated include I) multi-dimensional ultraviolet and visible spectra probing single photon state couplings, II) multi-dimensional electronic spectra probing single electronic state couplings, and III) multi-dimensional infrared and Raman spectra probing single phonon state and its couplings to electronic states. Using the polycrystalline graphene structures with designed defects, dopings and oxide groups, and the fullerenes and arene-transition metal sandwich complexes with adjusted external electric or force fields, we will study the evolution of quantum states induced by structural and environmental variations, and reveal the mechanisms of those key processes of photo-excitations, exciton migrations, population transportations, and energy relaxations from the multi-dimensional spectroscopic features. Also, a multi-scale theoretical framework for single quantum systems will be built during the simulations of multi-dimensional spectroscopy. With the developed theoretical framework, this project will lead to powerful tools for viewing the key physics, chemistry, information processes in quantum devices at the single quantum state level.

本项目致力于发展和应用量子化学理论方法，模拟多维光谱探测纳米碳材料中的量子态动力学演化过程。具体探测机理包括多维紫外和可见光谱探测单光子态耦合，多维电子光谱探测单电子态耦合，多维红外光谱与拉曼光谱探测单声子态及其与电子态的耦合。我们将以多晶石墨烯复合结构和碳球-芳烃过渡元素拓扑结构为研究对象，分别通过调节材料结构（缺陷、掺杂、及氧化基团），和外加电场或力场，来研究材料结构与环境变化对量子态的影响，并模拟多维光谱反映的光学跃迁、激子转移、载流子输运、能量弛豫过程来理解量子态的运动规律。本项目将以纳米碳材料的多维光谱模拟工作为契机，整合相关理论，发展一套适用于单量子体系量子态研究的多尺度理论框架。应用该框架探索的多维光谱精密探测量子态的机理，将为在单量子态层面理解物理与化学过程提供技术手段。

我们设计并构筑了几种新型的复合结构，集成了具有光电转换功能的半导体纳米结构、具有催化活性和近场光子操纵能力的金属纳米结构、和具有柔性导电功能的低维碳纳米结构。基于表征实验中获得的电子运动信息，我们的通过第一性原理的计算模拟研究，理解和发掘出了这些复合材料体系中（半导体-金属、金属-石墨烯、半导体-低维碳材料）的量子态耦合（态密度、电荷分布、势能面、耦合常数等）对尺寸、结构及化学组成等纳米结构参数的依赖性原理及其控制方式。通过揭示复合材料中的电子态动力学演化规律并掌握其微观过程的协同和调控原理，我们较好的完成了研究计划。