Molecular Radiative and Relaxation Processes

分子辐射和弛豫过程

基本信息

批准号：
2246379
负责人：
Shaul Mukamel
金额：
$ 70.7万
依托单位：
University of California-Irvine
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：
2023-05-01 至 2027-04-30
项目状态：
未结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=2246379&HistoricalAwards=false
关键词：
Molecular Radiative Relaxation Processes

项目摘要

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.

在加州大学尔湾分校化学系化学理论、模型和计算方法 (CTMC) 项目 Shaul Mukamel 的支持下，欧文市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，穆卡梅尔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，这种量子相关性已在量子计算应用中得到广泛研究。光的量子性质为通过经典光无法实现的窗口监测基本分子事件提供了许多新的机会。将开发模型和实用计算工具来解释和分析所提出的测量结果。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，光学微腔可以通过与局域腔模式的强光-物质耦合来操纵电子和核动力学，从而产生称为极化子的混合光-物质粒子。将研究与相同腔模式相互作用的许多分子的集体响应。将采用相干控制方案来优化所提出的非线性光信号。单个纠缠光子的符合测量和量子干涉技术将用于探测分子手性。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和量子光技术领域的多个全球研究中心的董事会中担任顾问，为更广泛的影响做出贡献。将开发涉及光学腔和量子光的新型光谱技术并应用于研究分子中的基本光物理和光化学过程。将采用结合非绝热分子动力学、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、相位控制和手性偏振配置。受激拉曼技术可以直接探测分子通过微腔中的圆锥形交叉点的通道。量子光学中开发的量子光工程态将以前所未有的时间、光谱和空间分辨率应用于分子光谱应用。光子和物质之间纠缠的来回转移将用于在分子聚集体中创建新类别的相关激发态。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。这些对于人工光采集系统的设计具有广泛的长期科学影响的潜力，这些系统可以高效地将太阳光转化为化学能。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技术进行评估，被认为值得支持。更广泛的影响审查标准。