Quantum-dynamical methods for modelling photo-induced processes in molecules

我们将开发新的量子动力学方法来模拟分子中的光化学和光物理过程。这些过程在许多生物过程中起着至关重要的作用，例如人类的视觉和植物的光合作用，并涉及捕获和利用太阳能。这些过程的第一原理建模对于获得原子级理解和设计控制方案至关重要。这种建模在计算上具有挑战性。它需要分子动力学的量子描述，这需要发展有效的数值技术。我们的量子动力学方法基于三个组成部分：1)第一性原理电子结构计算，提供电子态及其耦合；2)描述多电子态核动力学的波包技术；3)量子非平衡统计力学方法引入不太显著的核自由度或模拟自然阳光的非相干光。这些组件使我们能够处理各种时间尺度和分子系统中原子间相互作用的复杂性。新的发展将帮助我们：了解各种光条件下分子系统中的光-物质相互作用；为研究光化学反应机理提供有效的数值方法；为光谱实验研究提供计算模型支持。我们项目的实际成果将包括计算机软件建模，新的数值方法，化学结构理论的修订，以及新型有机发光二极管视觉过程和操作的机理见解。在项目实施过程中，我们将培养研究生和本科生在量子分子动力学、电子结构、计算机编程、演讲和科学写作方面的知识。许多技能是可转让的，有助于其他经济领域和学员的成功。

We will develop novel quantum dynamical approaches to model photochemical and photophysical processes in molecules. Such processes play a paramount role in many biological processes, such as human vision and photosynthesis in plants, and are involved in capturing and utilizating solar energy. First principles modelling of these processes is crucial for obtaining an atomistic level understanding and for designing control schemes. This modelling is computationally challenging. It needs a quantum description of molecular dynamics, which requires the development of efficient numerical techniques. Our approach to quantum dynamics is based on three components: 1) first principles electronic structure calculations to provide electronic states and their couplings; 2) wave-packet techniques to describe nuclear dynamics on multiple electronic states, and; 3) methods of quantum non-equilibrium statistical mechanics to introduce either less significant nuclear degrees of freedom or incoherent light modelling natural sunlight. The components allow us to address a variety of timescales and the complexity of interatomic interactions in molecular systems. New developments will help us to: understand light-matter interaction in molecular systems for a variety of light conditions; provide efficient numerical approaches for investigating mechanisms of photochemical reactions, and; give computational modelling support to experimental spectroscopic studies. Tangible outcomes of our program will include modelling computer software, novel numerical methods, revisions of chemical structure theory, and mechanistic insights in the vision process and operation of new organic light-emitting diodes. In the course of program implementation, we will train graduate and undergraduate students in quantum molecular dynamics, electronic structure, computer programming, presentation giving, and scientific writing. Many of the skills are transferable, contributing to other areas of economy and to the success of the trainees.