CAREER: Simulating Mesoscale Quantum Dynamics and Non-linear Microscopy

职业：模拟中尺度量子动力学和非线性显微镜

• 批准号: 2341178
• 负责人: Doran Raccah
• 金额: $ 65万
• 依托单位: University of Texas at Austin
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2023
• 资助国家: 美国
• 起止时间: 2023-08-01 至 2027-01-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2341178&HistoricalAwards=false
• 关键词: CAREER; Simulating; Mesoscale; Quantum; Dynamics

This award is funded in whole or in part under the American Rescue Plan Act of 2021 (Public Law 117-2).With support from the Chemical Theory, Models and Computational Methods program in the Division of Chemistry, Doran Bennett of Southern Methodist University is working to uncover the quantum mechanical processes by which molecular materials conduct energy. Next generation technology development stems from advances in our ability to control, manipulate, and redirect energy. Dr Bennett’s group will extend computer simulations of quantum process from the traditional molecular-scale to the nanometer-to-micron scale, (i.e. the ‘mesoscale’) that is relevant to molecular materials. These rigorous computational models are expected to establish how specific materials absorb and deploy energy from light, providing essential information to those looking to engineer novel materials. This research will combine chemistry, computation, and advanced mathematics, STEM fields with severe levels of gender and race disparities. In conjunction with his research, Dr. Bennett will launch an intensive, wrap-around summer research program to reach greater numbers of science majors from underserved groups in an effort to achieve greater excellence through diversity.Doran Bennett’s research under this award will address the pressing need for new computational tools to support an emerging scientific frontier studying mesoscale (10 nm – 1 μm) excited-state dynamics in molecular materials. Rapidly developing synthetic and spectroscopic toolboxes are expected to enable structural control and the establishment of spatially-resolved probes of mesoscale processes. Dr. Bennett and his group will leverage the locality of electronic excited-states to simulate the photophysics of molecular materials within a formally exact (spin-boson) equation-of-motion called the adaptive hierarchy of pure states (adHOPS). Dr. Bennett will extend adHOPS to simulate excited state dynamics in the presence of complex vibrational environments of realistic molecular materials (e.g. involving many frequencies of vibration and timescales of relaxation). He and his team will also endeavor to develop the corresponding computational methods for simulating spatially resolved non-linear spectroscopy. These efforts are expected provide the community with new theoretical tools for interpreting spectroscopic measurements and predicting excited state dynamics in synthetic molecular materials.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.

该奖项全部或部分由2021年美国救援计划法案（公法117-2）资助。在化学系化学理论、模型和计算方法项目的支持下，南卫理公会大学的Doran班尼特正致力于揭示分子材料传导能量的量子力学过程。下一代技术的发展源于我们控制、操纵和重定向能量的能力的进步。班尼特博士的小组将把量子过程的计算机模拟从传统的分子尺度扩展到与分子材料相关的纳米到微米尺度（即“介观尺度”）。这些严格的计算模型预计将确定特定材料如何吸收和部署来自光的能量，为那些希望设计新材料的人提供必要的信息。这项研究将结合联合收割机化学，计算，高等数学，STEM领域与严重的性别和种族差异。为了配合他的研究，班尼特博士将启动一个密集的，一个围绕夏季研究计划，以达到更多的科学专业从服务不足的群体，努力实现更大的卓越通过多样性。多兰班尼特的研究在这个奖项将解决迫切需要新的计算工具，以支持新兴的科学前沿研究中尺度（10 nm - 1 μm）分子材料中的激发态动力学。快速发展的合成和光谱工具箱，预计将使结构控制和建立中尺度过程的空间分辨探针。班尼特博士和他的团队将利用电子激发态的局部性来模拟分子材料在一个形式上精确的（自旋玻色子）运动方程中的物理学，称为纯态的自适应层次（adHOPS）。班尼特博士将扩展adHOPS，以模拟现实分子材料复杂振动环境下的激发态动力学（例如，涉及许多振动频率和弛豫时间尺度）。他和他的团队还将奋进开发相应的计算方法来模拟空间分辨非线性光谱。这些努力预计将为社会提供新的理论工具，解释光谱测量和预测激发态动力学在合成分子material.This奖项反映了NSF的法定使命，并已被认为是值得通过评估使用基金会的智力价值和更广泛的影响审查标准的支持。

项目成果

Simulating optical linear absorption for mesoscale molecular aggregates: An adaptive hierarchy of pure states approach

模拟介观分子聚集体的光学线性吸收：自适应纯态层次方法

• DOI: 10.1063/5.0141882
• 发表时间: 2023
• 期刊: The Journal of Chemical Physics
• 作者: Gera, Tarun;Chen, Lipeng;Eisfeld, Alexander;Reimers, Jeffrey R.;Taffet, Elliot J.;Raccah, Doran I.
• 通讯作者: Raccah, Doran I.

Calculating nonlinear response functions for multidimensional electronic spectroscopy using dyadic non-Markovian quantum state diffusion

• DOI: 10.1063/5.0107925
• 发表时间: 2022-09-21
• 期刊: JOURNAL OF CHEMICAL PHYSICS
• 影响因子: 4.4
• 作者: Chen, Lipeng;Bennett, Doran I. G.;Eisfeld, Alexander
• 通讯作者: Eisfeld, Alexander