Time-domain ab initio studies of excitation dynamics in nanoscale materials

华盛顿大学的奥列格·普雷日多得到了理论、模型和计算方法项目的支持，该奖项旨在开发非绝热和半经典分子动力学的新模拟方法，它们在时间域密度泛函理论中的实现，以及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的研究。这项工作提供了一幅详细的、原子化的实时光激发动力学图像，并直接与实验联系在一起。这些研究集中在纳米尺度下凝聚相环境的量子性质，如退相干、特定态动力学、零点能量和非绝热跃迁，为超快现象提供了更严格的处理方法。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粒子。Pi和他的同事们发展了一些方法来研究纳米系统的许多重要特征。这些研究首次为许多实验观察到的现象提供了非常理想的细节和理解，为开发用于太阳能转换、电子学和成像的新型器件提供了理论基础。PI还开发了用于入门和高级化学课程的新型教学工具。

Oleg Prezhdo of the University of Washington is supported by an award from the 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 devices for solar energy conversion, electronics, and imaging. The PI also develops novel teaching tools for use both in introductory and advanced chemistry courses.