Molecular Radiative and Relaxation Processes

分子辐射和弛豫过程

• 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

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.

在化学系化学理论、模型和计算方法（CTMC）项目的支持下，加州大学欧文分校的Shaul Mukamel正在开发利用光脉冲的量子特性研究分子过程的新方法。特别是，Mukamel将探索光子的量子相关，即在量子计算应用中被广泛研究的纠缠，如何用于控制分子和光之间的相互作用。光的量子特性为通过窗口监测基本分子事件提供了许多新的机会，这是经典光无法实现的。将开发模型和实用的计算工具，以解释和分析拟议的测量结果。将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光-物质耦合到局域腔模式来操纵电子和核动力学，从而产生被称为极化子的混合光-物质粒子。许多分子与相同的腔模式相互作用的集体响应将被研究。将采用相干控制方案来优化所提出的非线性光信号。单个纠缠光子的重合测量和量子干涉测量技术将被用于探测分子手性。参与该项目的学生将沉浸在量子信息科学的前沿研究中。此外，Mukamel博士还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担任顾问。涉及光腔和量子光的新型光谱学技术将被开发并应用于研究分子中的基本光物理和光化学过程。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被采用。脉冲整形，相位控制和手性极化配置将被利用。受激拉曼技术可以直接探测分子通过微腔中的锥形交叉点的通道。量子光学中发展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。光子和物质之间的纠缠来回转移将用于在分子聚集体中创建新的相关激发态类别。利用新技术将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。这对于设计将太阳光高效转化为化学能的人工光收集系统具有广泛而长期的科学影响。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。

项目成果

Intraband Exciton Transitions in Photosynthetic Complexes Revealed by Novel Five-Wave-Mixing Spectroscopy

新型五波混合光谱揭示光合复合物中的带内激子跃迁

• DOI: 10.1021/acs.jctc.3c00919
• 发表时间: 2024
• 期刊: Journal of Chemical Theory and Computation
• 影响因子: 5.5
• 作者: Kizmann, Matthias;Yadalam, Hari Kumar;Chernyak, Vladimir Y.;Mukamel, Shaul
• 通讯作者: Mukamel, Shaul

Direct Monitoring of Conical Intersection Passage via Electronic Coherences in Twisted X-Ray Diffraction

通过扭曲 X 射线衍射中的电子相干性直接监测圆锥形交叉口通道

• DOI: 10.1103/physrevlett.129.103001
• 发表时间: 2022
• 期刊: Physical Review Letters
• 影响因子: 8.6
• 作者: Yong, Haiwang;Rouxel, Jérémy R.;Keefer, Daniel;Mukamel, Shaul
• 通讯作者: Mukamel, Shaul

Novel Ultrafast Molecular Imaging Based on the Combination of X-ray and Electron Diffraction

基于 X 射线和电子衍射相结合的新型超快分子成像

• DOI: 10.1021/acs.jpca.2c08024
• 发表时间: 2023
• 期刊: The Journal of Physical Chemistry A
• 作者: Yong, Haiwang;Keefer, Daniel;Mukamel, Shaul
• 通讯作者: Mukamel, Shaul

Optical Cavity Manipulation and Nonlinear UV Molecular Spectroscopy of Conical Intersections in Pyrazine

吡嗪圆锥形相交的光腔操纵和非线性紫外分子光谱

• DOI: 10.1021/jacs.2c00921
• 发表时间: 2022
• 期刊: Journal of the American Chemical Society
• 影响因子: 15
• 作者: Cho, Daeheum;Gu, Bing;Mukamel, Shaul
• 通讯作者: Mukamel, Shaul

Photon Correlation Signals in Coupled-Cavity Polaritons Created by Entangled Light

• DOI: 10.1021/acsphotonics.1c01755
• 发表时间: 2022-02
• 期刊: ACS Photonics
• 影响因子: 7
• 作者: B. Gu;S. Mukamel