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

俄勒冈大学的杰弗里·A·西纳获得了化学部化学理论、模型和计算方法计划颁发的奖项，以表彰与自然和人工获取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，在由几个光吸收单元组成的现实分子网络中有效地模拟电子能量转移的量子力学方面，并预测和解释在这些重要和广泛研究的系统上进行的有用和具有启发性的超快激光测量结果。CINA将通过为非理科专业的本科生组织关于气候变化科学的研讨会式的本科课程来服务于科学推广。他将继续在他的研究和教学角色中通过实践和模拟欢迎和支持行动来提高科学界的包容性。Jeffrey Cina将与他的研究生同事合作，对一种新的测量策略进行理论研究，该策略将把现有的多维电子光谱学工具(也称为多维波包干涉测量，或WPI)应用于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)的空间定向集合。他将预测和解释超快光谱信号，该信号包含关于位间或激子间电子相干性的时间进程的直接、可隔离的信息--这是激发传输性质和效率的关键决定因素。他将在日益复杂和逼真的模型系统上对这种可测量的信号进行模拟。为了支持这一目标，他将开发、测试和应用一种新的协议，该协议将离散的位置激发或激子状态作为量子力学子系统，同时用紧凑的参数化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，CINA将探索少数发色团复合体中电子激发传输的量子力学“哪条路径”干扰的影响，并确定这一特定相干相关现象的光谱特征。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。

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.