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

罗切斯特大学的奥列格·普雷日多获得了化学理论、模型和计算方法项目的一个奖项，该奖项的目的是为非绝热和半经典分子动力学开发新的模拟方法，在时域密度泛函理论中实现这些方法，并调查最近在纳米材料上进行的时间分辨实验中提出的基本问题。这项工作提供了一个详细的，原子的照片激发动态实时和直接与实验。该研究的重点是在纳米尺度下凝聚相环境的量子特性，如退相干，状态特定的动力学，零点能量和非绝热跃迁，提供更严格的超快现象的治疗。这些方法被应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和他的同事们开发了研究纳米系统许多重要特征的方法。这些研究是第一个提供非常理想的细节和许多实验观察到的现象的理解，为新材料和设备的开发产生的理论基础。这些包括太阳能电池，提高光收集和电荷产生由于纳米级的功能，所提出的架构，电池能够高功率存储的结果，大表面积的纳米级材料使用，微型电子和自旋电子器件接近一个原子的厚度，和工具的生物成像，药物输送和DNA测序。PI还开发了新的教学方法，用于入门和高级化学课程。

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.