Molecules in Classical and Quantized Fields: Developing Time-dependent Density Functional and Exact Factorization Methods for Electrons, Ions, and Photons

纽瓦克罗格斯大学的Neepa Maitra教授得到了化学系化学理论、模型和计算方法(CTMC)项目的奖励。Maitra和她的研究小组将通过从第一原理开发电子、离子和光子的关联动力学的新方法，来解决经典和量子化光场中分子的计算模拟中的一些基本挑战。这些项目涉及三个领域，在这三个领域内，她将发展出应该提高今天计算可靠性的近似：通过依赖时间的密度泛函理论的电子动力学，通过精确因式分解方法的关联电子-离子动力学，以及它们对应用于混合轻质态(极化子)的量子化的光-物质相互作用的扩展。这些发展影响了需要了解和了解平衡电子结构以外的知识和知识的应用：从光伏设计到通过阿秒和飞秒激光场或通过调整腔参数对电子和核动力学的量子控制。这个项目将产生广泛的教育影响，通过培训本科生和研究生进行尖端研究，共同组织和参加她研究领域的暑期学校，以及继续举办Zoom博士学生研讨会系列，并建立一个针对服务不足的纽瓦克公立学区的高中外展辅导计划，以缓解我们社会获得教育资源的不均，并促进未被充分代表的少数族裔科学家的发展。完全非微扰过程的依赖时间的密度泛函理论将被重塑，要求仅在线性和二次响应机制中使用交换相关泛函，目前使用的绝热近似最适合于此。将开发从精确表达式推导出的改进的近似。这推动了TDDFT在实时非微扰过程中的应用，就像它在光谱和基态性质中的应用一样。基于精确因式分解的混合量子经典格式将被构造用于光激发后或在激光作用下的关联电子-离子动力学，包括电子退相干和从第一原理开始的波包分支。将这些方法扩展到极化子系统，将使我们对场量子化如何改变化学反应有一个基本的理解，并将产生实用的量子-经典混合方法来研究光学腔中分子的动力学和控制。这项研究正在提供新的计算工具，并影响我们对化学物理、原子和分子物理、材料科学和光-物质相互作用的基本理解。Maitra继续组织暑期学校和教程。该项目将通过她的团队去年夏天发起的Zoom博士学生研讨会，在全球范围内扩大学生研究网络联系。她将在纽瓦克公立学区建立一个高中辅导项目。小组内的指导有助于引导博士后研究员、研究生和本科生走向以科学为导向的未来。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

Professor Neepa Maitra of Rutgers University at Newark is supported by an award from the Chemical Theory, Models and Computational Methods (CTMC) program in the Division of Chemistry. Maitra and her research group will address some of the fundamental challenges in computational simulations of molecules in classical and quantized light fields by developing new methods for the correlated dynamics of electrons, ions, and photons from first-principles. The projects involve three areas, within which she will develop approximations that should increase the reliability of calculations today: electron dynamics via time-dependent density functional theory, correlated electron-ion dynamics via the exact factorization approach, and their extensions to quantized light-matter interactions for applications to hybrid light-matter states (polaritons). The developments impact applications where knowledge and understanding beyond equilibrium electronic structure are necessary: from photovoltaic design to quantum control of electronic and nuclear dynamics by attosecond and femtosecond laser fields, or by tuning cavity parameters. This project will have a broad educational impact through the training of undergraduate and graduate students in cutting-edge research, co-organizing and participating in summer schools in her research field as well as continuing a Zoom PhD Student Seminar series, and establishing a high school outreach tutoring program to the underserved Newark Public School District to mitigate our society's uneven access to educational resources and promote the development of underrepresented minority scientists.Time-dependent density functional theory for fully non-perturbative processes will be re-cast to require the exchange-correlation functionals only in the linear and quadratic response regimes, where the adiabatic approximations in use today are best suited. Improved approximations derived from exact expressions will be developed. This moves TDDFT towards being as confidently used for real-time non-perturbative processes as it is used for spectra and ground-state properties. Practical exact-factorization-based mixed quantum-classical schemes for correlated electron-ion dynamics after photo-excitation or in the presence of laser fields will be constructed, that include electronic decoherence and wavepacket branching from first-principles. Extension of these methods to polaritonic systems will lead to a fundamental understanding of how field quantization can alter chemical reactions, and to practical mixed quantum-classical methods for the dynamics and control of molecules confined in optical cavities. The research is providing new computational tools and impacts our fundamental understanding of chemical physics, atomic and molecular physics, materials science, and light-matter interactions. Maitra continues to organize summer schools and tutorials. This project will expand student research network connections globally through the Zoom PhD Student Seminars her group initiated last summer. She will establish a high school tutoring program in the Newark Public School district. Mentoring within the group helps guide postdoctoral fellows, graduate, and undergraduate students towards scientifically-oriented futures.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.