Molecules in Classical and Quantized Fields: Improving Time-Dependent Density Functional Approximations and Correlated Electron-Ion Methods

纽约城市大学亨特学院的Neepa Maitra教授得到了化学系化学理论、模型和计算方法项目的奖励。梅特拉博士和她的研究小组开发了模拟分子在光下行为的新方法。了解电子和离子在远离其稳定、平衡状态的分子和固体中的运动并进行计算模拟，对于理解光伏过程、光催化、生物分子中的辐射损伤、纳米级电导设备、时间分辨泵浦-探测光谱以及紧凑光源的产生是必要的。梅特拉博士的团队从计算模拟的第一原理发展了理论方法，以可靠而有效地预测这些过程。梅特拉博士组织了电子结构和动力学方面的迷你研讨会，面向更广泛的纽约/新泽西地区。她训练本科生和研究生进行尖端研究，并在本科生课堂上使用创新的同伴教学技术。Maitra和她的研究小组正在开发新的方法来研究电子、离子和光子的相关动力学，目标有三。在一个目标中，推导了非微扰区含时密度泛函理论(TDDFT)的改进泛函近似。这是建立在交换关联势的精确表达式基础上的。这项研究推动了TDDFT在实时动力学中的应用，就像DFT用于基态特性一样。在第二个目标中，我们正在构造基于精确因式分解方法的实用混合量子-经典方法，其中包括电子退相干和从第一性原理出发的波包分支。第三个领域将精确因式分解扩展到光-物质系统，以获得对场量子化如何改变和控制化学反应的基本理解，以及开发实用的量子-经典混合方法来研究腔中分子的动力学和控制。这项研究影响到需要超越基态电子结构的知识和理解的主题应用，包括光伏设计，以及通过阿秒或飞秒激光场对电子和核动力学的量子控制，或通过调节极化化学中的腔参数。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 Hunter College, City University of New York (CUNY) is supported by an award from the Chemical Theory, Models and Computational Methods program in the Division of Chemistry. Dr. Maitra and her research group develop new methods for simulating the behavior of molecules exposed to light. Understanding and computationally modeling the motion of electrons and ions in molecules and solids far from their stable, equilibrium states is necessary for understanding photovoltaic processes, photocatalysis, radiation damage in biomolecules, nanoscale conductance devices, time-resolved pump-probe spectroscopies, and the production of compact light sources. Dr. Maitra's group develops theoretical methods from first-principles for computational simulations to reliably and efficiently predict these processes. Dr. Maitra organizes mini-workshops in electronic structure and dynamics open to the wider New York/New Jersey area. She trains undergraduate and graduate students in cutting-edge research and uses innovative peer instruction teaching techniques in her undergraduate classes.Dr. Maitra and her research group are developing new methods for the correlated dynamics of electrons, ions, and photons, in three aims. In one aim, improved functional approximations for time-dependent density functional theory (TDDFT) in the non-perturbative regime is derived. This is built on an exact expression for the exchange-correlation potential. This research moves TDDFT towards use in real-time dynamics as confidently as DFT is used for ground-state properties. In the second aim, practical mixed quantum-classical methods based on the exact factorization approach for correlated electron-ion dynamics in laser fields are being constructed that include electronic decoherence and wave packet branching from first-principles. The third area extends exact factorization to light-matter systems to gain a fundamental understanding of how field quantization can alter and control chemical reactions, as well as to develop practical mixed quantum-classical methods for the dynamics and control of molecules in cavities. The research impacts topical applications where knowledge and understanding beyond ground-state electronic structure is needed, including photovoltaic design, and quantum control of electronic and nuclear dynamics by attosecond or femtosecond laser fields, or by tuning cavity parameters in polaritonic chemistry.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.