Time-Domain Atomistic Theory and Simulation of Excitation Dynamics on the Nanoscale

时域原子理论与纳米尺度激发动力学模拟

• 批准号: 1300118
• 负责人: Oleg Prezhdo
• 金额: $ 48万
• 依托单位: University of Rochester
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2013
• 资助国家: 美国
• 起止时间: 2013-03-15 至 2015-04-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1300118&HistoricalAwards=false
• 关键词: Time; Domain; Atomistic; Theory; Simulation

Oleg Prezhdo of the University of Rochester is supported by an award from the Chemical Theory, Models and Computational Methods program for the development of novel simulations approaches for nonadiabatic and semiclassical molecular dynamics, their implementation within time-domain density functional theory and the investigation of the fundamental questions posed in the recent time-resolved experiments performed on nanoscale materials. This work provides a detailed, atomistic picture of photo excitation dynamics in real-time and in direct connection with experiment. The research focuses on the quantum properties of condensed phase environments at the nanoscale, such as decoherence, state-specific dynamics, zero-point energy, and non-adiabatic transitions, providing more rigorous treatments of ultrafast phenomena. These methods are applied to the excitation dynamics in novel nanomaterials, including wet-electrons, carbon nanotubes and nanoribbons, and metallic particles.The PI and his coworkers develop methods to study many important features of nanoscale systems. These studies are the first to provide the highly desirable details and understanding of many experimentally observed phenomena, generating the theoretical basis for the development of novel materials and devices. These include solar cells that enhance light harvesting and charge generation due to nanoscale features of the proposed architectures, batteries capable of high power storage as a result of large surface area of the nanoscale materials used, miniature electronic and spintronics devices approaching one atom thickness, and tools for biological imaging, drug delivery and DNA sequencing. The PI also develops novel teaching approaches for use both in introductory and advanced chemistry courses.

罗切斯特大学的奥列格·普雷日多 (Oleg Prezhdo) 获得了化学理论、模型和计算方法项目的奖项，以表彰其开发非绝热和半经典分子动力学的新颖模拟方法、它们在时域密度泛函理论中的实现以及对最近在纳米级材料上进行的时间分辨实验提出了基本问题。这项工作提供了实时且与实验直接相关的光激发动力学的详细原子图。该研究重点关注纳米尺度凝聚相环境的量子特性，例如退相干、特定态动力学、零点能量和非绝热跃迁，为超快现象提供更严格的处理。这些方法适用于新型纳米材料的激发动力学，包括湿电子、碳纳米管和纳米带以及金属颗粒。PI 和他的同事开发了研究纳米级系统的许多重要特征的方法。这些研究首次提供了许多实验观察到的现象的非常理想的细节和理解，为新型材料和设备的开发提供了理论基础。其中包括由于所提出的架构的纳米级特征而增强光收集和电荷产生的太阳能电池、由于所使用的纳米级材料的大表面积而能够高功率存储的电池、接近一个原子厚度的微型电子和自旋电子器件，以及用于生物成像、药物输送和 DNA 测序的工具。 PI 还开发了用于入门和高级化学课程的新颖教学方法。