Multi-dimensional Electronic Dynamics beyond the Dipole Approximation

超越偶极近似的多维电子动力学

• 批准号: 1565520
• 负责人: Xiaosong Li
• 金额: $ 53.93万
• 依托单位: University of Washington
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2016
• 资助国家: 美国
• 起止时间: 2016-07-01 至 2019-06-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1565520&HistoricalAwards=false
• 关键词: Multi; dimensional; Electronic; Dynamics; beyond

Xiaosong Li of the University of Washington is supported by an award from the Chemical Theory, Models and Computational Methods program in the Chemistry Division and the Computational and Data-Enabled Science and Engineering program in the Division of Advanced Cyberinfrastructure to develop computational methods and open-source software to study the dynamics of electrons driven by electromagnetic fields. Electronic processes influenced by multiple electromagnetic fields underlie the functionality of many technologically-important materials. The methods developed by Li and his research group yield new and powerful avenues to facilitate scientific discoveries of materials that exhibit desirable optical properties. The project also provides a mechanism for advanced interdisciplinary education and training in the areas of inorganic, theoretical, physical, and materials chemistry. The project prepares participating undergraduate and graduate students for future careers in science, engineering, and education. Through a combination of high-school and community outreach and undergraduate research mentoring, this project promotes and fosters participation of a broad spectrum of youth in science and engineering activities.This project lays the theoretical groundwork for modeling time-resolved, multidimensional electronic spectroscopy, with energies ranging from the UV to X-ray regions of the spectrum and modulated by the delays between pulses, completely within the first-principles framework. On the one hand, the development is able to reveal the physical mechanisms that drive excited state chemical processes/phenomena, which is fundamental to energy research. For example, coherent excitonic and charge transfer dynamics is one potential application. On the other hand, the algorithmic advances greatly broaden the application of excited state electronic structure theory in the non-perturbative, non-linear regime. Here the process of interest requires a description of the system-field interaction that goes beyond the electric-dipole approximation. This research activity is unique in that it seamlessly integrates time-dependent quantum mechanical theories and spectral analysis software tools with modular high-performance numerical libraries that are highly parallelized, extensible, reusable, community-driven, and open-sourced. The research goals are to provide a direct path to the discovery and design of molecules and materials that demonstrate new or enhanced high-order optical, magnetic, electronic, and plasmonic features.

华盛顿大学的李晓松获得了化学系化学理论、模型和计算方法项目以及高级网络基础设施部门计算和数据支持的科学与工程项目的资助，以开发计算方法和开放式计算方法。用于研究电磁场驱动的电子动力学的源软件。受多个电磁场影响的电子过程是许多重要技术材料功能的基础。 李和他的研究小组开发的方法为促进具有理想光学特性的材料的科学发现提供了新的、强大的途径。 该项目还为无机、理论、物理和材料化学领域的高级跨学科教育和培训提供了机制。 该项目帮助参与的本科生和研究生为未来在科学、工程和教育领域的职业生涯做好准备。通过将高中和社区外展以及本科生研究指导相结合，该项目促进和培养广大青年参与科学和工程活动。该项目为时间分辨多维电子光谱建模奠定了理论基础，能量范围从光谱的紫外线到 X 射线区域，并通过脉冲之间的延迟进行调制，完全在第一原理框架内。一方面，这一进展能够揭示驱动激发态化学过程/现象的物理机制，这是能源研究的基础。 例如，相干激子和电荷转移动力学是一种潜在的应用。另一方面，算法的进步极大地拓宽了激发态电子结构理论在非微扰、非线性领域的应用。 这里，感兴趣的过程需要对系统-场相互作用的描述，而不仅仅是电偶极子近似。这项研究活动的独特之处在于，它将瞬态量子力学理论和光谱分析软件工具与高度并行、可扩展、可重用、社区驱动和开源的模块化高性能数值库无缝集成。 研究目标是为分子和材料的发现和设计提供直接途径，以展示新的或增强的高阶光学、磁力、电子和等离子体特征。

项目成果

Generalized Hartree–Fock with Nonperturbative Treatment of Strong Magnetic Fields: Application to Molecular Spin Phase Transitions

强磁场非微扰处理的广义 Hartree-Fock：在分子自旋相变中的应用

• DOI: 10.1021/acs.jctc.8b01140
• 发表时间: 2018-11
• 期刊: Journal of Chemical Theory and Computation
• 影响因子: 5.5
• 作者: Sun, Shichao;Williams;Stetina, Torin F.;Li, Xiaosong
• 通讯作者: Li, Xiaosong

Real-Time TDDFT Investigation of Optical Absorption in Gold Nanowires

金纳米线光吸收的实时 TDDFT 研究

• DOI: 10.1021/acs.jpcc.9b00296
• 发表时间: 2019-05-22
• 期刊: The Journal of Physical Chemistry C
• 作者: Ravithree D. Senanayake;D. Lingerfelt;Gowri U. Kuda;Xiaosong Li;Christine M. Aikens
• 通讯作者: Christine M. Aikens