Molecular Radiative and Relaxation Processes

在加州大学Shaul Mukamel化学系化学理论、模型和计算方法（CTMC）项目的支持下，Irvine正在开发利用光脉冲量子性质研究分子过程的新方法。特别是，Mukamel将探索如何利用光子的量子相关性（称为纠缠）来控制分子与光之间的相互作用，这种量子相关性在量子计算应用中得到了广泛的研究。光的量子性质提供了许多新的机会，通过经典光无法实现的窗口来监测基本分子事件。将为解释和分析拟议的测量结果开发模型和实用的计算工具。将通过电子结构和量子动力学模拟与最先进的量子光学技术相结合来解释所提出的量子信号。此外，光学微腔可以通过强的光-物质耦合到局域腔模来操纵电子和核动力学，这产生了被称为极化激元的混合光-物质粒子。研究了多个分子与同一腔模相互作用的集体响应。相干控制方案将被用来优化所提出的非线性光信号。纠缠光子的符合测量和量子干涉技术将被用来探测分子的手性。从事该项目的学生将沉浸在与量子信息科学相关的前沿研究中。 Mukamel博士还将继续在非线性超快光谱学和量子光技术领域的几个全球研究中心的董事会中担任顾问角色，并将开发和应用涉及光学腔和量子光的新型光谱技术来研究分子中的基本物理和光化学过程。将采用结合联合收割机非绝热分子动力学、量子核自由度的波包模拟和量子光子统计的计算技术。将利用脉冲整形、相位控制和手征偏振配置。受激拉曼技术，可以直接探测通过微腔中的锥形交叉点的分子的通道将被预测。在量子光学中开发的量子光的工程状态将被采用到具有前所未有的时间、光谱和空间分辨率的分子光谱学应用中。光子和物质之间纠缠的来回转移将用于在分子聚集体中产生新的相关激发态。将使用新技术研究分子聚集体和光合作用中的基本电荷和能量迁移过程。这些研究成果对设计将太阳光高效转化为化学能的人工集光系统具有广泛的长期科学影响。该奖项反映了NSF的法定使命，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。

With support from the Chemical Theory, Models and Computational Methods (CTMC) program in the Division of Chemistry, Shaul Mukamel of the University of California, Irvine is developing new methods for studying molecular processes which make use of the quantum nature of light pulses. In particular, Mukamel will explore how the quantum correlation of photons, known as entanglement, which has been extensively studied in quantum computing applications, can be used to control the interaction between molecules and light. The quantum nature of light offers numerous new opportunities for monitoring elementary molecular events through windows that are unavailable by classical light. Models and practical computational tools will be developed for the interpretation and analysis of the proposed measurements. Interpreting the proposed quantum signals will be made by the combination of electronic structure and quantum dynamics simulations with state-of-the-art quantum optics technology. In addition, optical microcavities can manipulate electron and nuclear dynamics by strong light-matter coupling to localized cavity modes, which create hybrid light-matter particles known as polaritons. The collective response of many molecules interacting with the same cavity mode will be investigated. Coherent control schemes will be employed to optimize the proposed nonlinear optical signals. Coincidence measurements of individual entangled photons and quantum interferometry techniques will be employed to probe molecular chirality. Students working on this project will be immersed in frontier research relevant to quantum information science. Also contributing to the broader impacts, Dr. Mukamel will continue to serve an advisory role on the boards of several worldwide research centers in the field of nonlinear ultrafast spectroscopy and quantum light technology.Novel spectroscopic techniques that involve optical cavities and quantum light will be developed and applied to study elementary photophysical and photochemical processes in molecules. Computational techniques that combine nonadiabatic molecular dynamics, wavepacket simulations of quantum nuclear degrees of freedom, and quantum photon statistics will be employed. Pulse shaping, phase control, and chiral polarization configurations will be utilized. Stimulated Raman techniques that can directly probe the passage of molecules through conical intersections in microcavities will be predicted. Engineered states of quantum light developed in quantum optics will be adopted to molecular spectroscopy applications with unprecedented temporal, spectral, and spatial resolutions. The back and forth transfer of entanglement between photons and matter will be used to create new classes of correlated excited states in molecular aggregates. The elementary charge and energy migration processes in molecular aggregates and in photosynthesis will be investigated using the new techniques. These have the potential for broad long-term scientific impact for the design of artificial light harvesting systems that convert sunlight to chemical energy with high efficiency.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.