Photo-induced charge and energy transport: from single molecules to disordered materials

光诱导电荷和能量传输：从单分子到无序材料

• 批准号: RGPIN-2017-05119
• 负责人: Kelly, Aaron
• 金额: $ 1.53万
• 依托单位: Dalhousie University
• 依托单位国家: 加拿大
• 项目类别: Discovery Grants Program - Individual
• 财政年份: 2022
• 资助国家: 加拿大
• 起止时间: 2022-01-01 至 2023-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=747939
• 关键词: Photo; induced; charge; energy; transport

My research interests center on the flow of energy and electric charge in, and between, molecules. Chemical energy and electric charge flow during fundamental chemical reaction events, such as when a molecule changes shape, or transfers an electron to one of its neighbors. These processes are especially important when a molecular system interacts with light; after the light energy is absorbed the system must then find some way to “relax”. Describing these sorts of processes from a theoretical perspective requires the development and application of simulation methods that lie at the interface of statistical mechanics and quantum dynamics. Combining these areas is essential to accurately capture these fundamental chemical steps in many forefront problems ranging from solar energy conversion and chemical catalysis to biological sensing and signaling. Molecular simulations of this type can help uncover the underlying mechanisms that lie at the heart of many energy conversion problems, and the ultimate goal of my research program is to extend and apply these approaches to study light-initiated charge and energy transport. In general, studying charge and energy transfer problems in molecular systems is an essential step to engineering new systems that can be manipulated in order to achieve desired outcomes. For example, our current understanding of how naturally occurring systems, such as plants and bacteria, harvest and harness energy from the sun lacks the detail necessary to provide a sufficient set of “design principles” for the development of improved synthetic light-harvesting systems that can perform similar functions. The challenge inherent in these problems is that the behavior of the quantum system is determined by interactions with its environment. These interactions can span many natural time and length scales, and the environment can be disordered. Bridging length and time-scales in molecular simulation is a long-standing holy grail' problem in the research community. Indeed, emerging computational infrastructures continue to push the boundaries in terms of the systems and processes that can be treated. However, these computational speed-ups are far out-paced by the inherent exponential scaling of the equations of quantum mechanics. For this reason, new dynamics algorithms are currently needed in order to access the relevant length and time-scales in, for example, the fundamental processes at play in a solar cell or a light-harvesting bacterium. These insights into how molecular systems and their environments can be tuned to alter their functionality will lead to a deeper understanding of how to leverage molecular-level design principles to aid in the development of improved solar energy conversion materials, molecular electronics, and catalytic systems. Hence, the impact of this work will have importance in many other areas of chemistry, in physics, and in materials science.

我的研究兴趣集中在基本化学反应事件期间分子内部和分子之间的能量和电荷流动，例如当分子改变形状或将电子转移到其邻居之一时。当分子系统与光相互作用时，这些过程尤其重要；吸收光能后，系统必须找到某种方法来“放松”，这需要开发和应用模拟方法。统计力学和量子动力学的接口。这些领域对于准确捕获从太阳能转换和化学催化到生物传感和信号传导等许多前沿问题中的基本化学步骤至关重要，此类分子模拟可以帮助揭示许多能源转换问题核心的潜在机制。 ，我的研究计划的最终目标是扩展和应用这些方法来研究光引发的电荷和能量传输。一般来说，研究分子系统中的电荷和能量转移问题是设计可操纵的新系统的重要一步。以达到预期的结果。我们目前对植物和细菌等自然系统如何收集和利用太阳能量的理解缺乏必要的细节，无法为开发改进的合成光收集系统提供足够的“设计原则”，这些系统可以执行类似的任务这些问题固有的挑战是量子系统的行为是由与其环境的相互作用决定的，这些相互作用可以跨越许多自然时间和长度尺度，并且分子中的桥接长度和时间尺度可能是无序的。模拟是由来已久的神圣事实上，新兴的计算基础设施不断突破可处理的系统和过程的界限，然而，这些计算速度远远超过了方程固有的指数缩放。因此，目前需要新的动力学算法来获取相关的长度和时间尺度，例如太阳能电池或光捕获细菌中发挥作用的基本过程。分子系统及其环境可以调整其功能将导致更深入地了解如何利用分子级设计原理来帮助开发改进的太阳能转换材料、分子电子学和催化系统。因此，这项工作的影响将具有重要意义。化学、物理学和材料科学的许多其他领域。