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.

在化学理论，化学理论的支持下，化学划分中的模型和计算方法（CTMC）计划，加利福尼亚大学的Shaul Mukamel，Irvine的Shaul Mukamel正在开发用于研究分子过程的新方法，以利用光脉冲的量子性质。特别是，Mukamel将探索如何使用在量子计算应用中进行广泛研究的光子的量子相关性，可用于控制分子与光之间的相互作用。光的量子性质提供了许多新的机会，可以通过窗户监视基本分子事件，而这些窗户无法获得经典的光。将开发模型和实用计算工具，以解释和分析所提出的测量。解释所提出的量子信号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的结合来制作。此外，光学微腔可以通过与局部腔模式结合强的光耦合来操纵电子和核动力学，从而产生杂交光粒子颗粒，称为polaritons。许多分子与相同的空腔模式相互作用的集体响应将进行研究。连贯的控制方案将采用优化所提出的非线性光学信号。将采用单个纠缠光子和量子干涉仪技术的重合测量来探测分子性手性。从事该项目的学生将沉浸在与量子信息科学相关的Frontier研究中。同样为更广泛的影响做出了贡献，Mukamel博士将继续在非线性超快光谱和量子光技术领域的几个全球研究中心的董事会中发挥咨询作用。novel Spectroscopic技术涉及光学腔和量子光，将开发并应用于基本的摄影和摄影过程。将采用结合非绝热分子动力学的计算技术，量子核自由度的波袋模拟以及量子光子统计。将利用脉冲塑形，相控制和手性极化构型。可以预测的刺激拉曼技术可以直接探测分子在微腔中通过圆锥形交集的通过。量子光学中开发的量子光的工程状态将用于具有前所未有的时间，光谱和空间分辨率的分子光谱应用。光子和物质之间纠缠的后退来回传递将用于在分子聚集体中创建新的相关激发态。分子聚集体和光合作用中的基本电荷和能量迁移过程将使用新技术研究。这些具有广泛的长期科学影响对人造光收集系统的设计，这些系统以高效的效率将阳光转化为化学能源。该奖项反映了NSF的法定任务，并被认为是值得通过基金会的智力优点和更广泛影响的评估标准来通过评估来获得支持的。