Quantum Dynamical Studies of Time-resolved Nonlinear Optical Signals from Spatially Oriented Electronic Energy Transfer Complexes

俄勒冈大学的Jeffrey A. Cina获得了化学系化学理论、模型和计算方法项目的奖项，以表彰他对与自然和人工收集太阳能相关的分子能量转移过程的理论研究。他的研究小组将开发和实施方法，以有效地模拟由几个光吸收单元组成的现实分子网络中电子能量传递的量子力学方面，并预测和解释在这些重要和广泛研究的系统上有用和揭示超快激光测量的结果。中国将为非理科生举办气候变化科学研讨班式的本科课程，开展科学推广。他将继续通过在他的研究和教学角色中锻炼和塑造欢迎、支持的行为来促进科学界的包容性。在与他的研究生同事合作中，Jeffrey china将对一种新的测量策略进行理论研究，该策略将应用现有的多维电子能谱（也称为多维波包干涉测量，或WPI）工具来测量电子激发能量转移二聚体、三聚体或四聚体（或单个小多聚体）的空间定向集成。他将预测和解释超快光谱信号，这些信号包含直接的、可分离的关于场间或激子间电子相干的时间过程的信息——这是激发输运性质和效率的关键决定因素。他将在越来越复杂和现实的模型系统上对这类可测量信号进行模拟。为了支持这一目标，他将开发、测试和应用一种新的协议，该协议将离散的点激发态或激子态作为量子力学子系统，同时用紧参数化的半经典试验波包模拟分子内、发色团介质和介质核自由度的动力学。此外，中国将探索电子激发输运在少数发色团配合物中的量子力学“哪路”干扰的影响，并确定这种特定相干依赖现象的光谱特征。该奖项反映了美国国家科学基金会的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

Jeffrey A. Cina of the University of Oregon is supported by an award from the Chemical Theory, Models and Computational Methods program in the Division of Chemistry for the theoretical study of molecular energy-transfer processes of relevance to the natural and artificial harvesting of solar energy. His research group will develop and implement methods to efficiently simulate quantum mechanical aspects of electronic energy transfer in realistic molecular networks comprising several light-absorbing units and to predict and interpret the results of useful and revealing ultrafast-laser measurements on these important and widely studied systems. Cina will serve scientific outreach by organizing a seminar-style undergraduate course for non-science majors on the science of climate change. He will continue to foster improved inclusivity in the scientific community by exercising and modeling welcoming, supportive actions in his research and teaching roles.In collaboration with his graduate-student co-workers, Jeffrey Cina will carry out theoretical investigations of a new measurement strategies that will apply existing tools of multi-dimensional electronic spectroscopy (also known as multi-dimensional wave-packet interferometry, or WPI) to spatially oriented ensembles of electronic excitation energy transfer dimers, trimers, or tetramers (or to individual small multimers). He will predict and interpret ultrafast spectroscopy signals containing direct, isolable information on the time-course of intersite or interexciton electronic coherence—key determinants of the nature and efficiency of excitation transport. He will carry out simulations of measurable signals of this kind on model systems of increasing degrees of complexity and realism. In support of this objective, he will develop, test, and apply a new protocol that treats discrete site-excited or excitonic states as a quantum mechanical subsystem while modeling the dynamics of intramolecular, chromophore-medium, and medium nuclear degrees of freedom with compactly parametrized, semiclassical trial wave packets. In addition, Cina will explore the effects of quantum mechanical "which-path" interference of electronic excitation transport in few-chromophore complexes, and identify spectroscopic signatures of this specific coherence-dependent phenomenon.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.