OP-Molecular Radiative and Relaxation Processes

OP-分子辐射和弛豫过程

基本信息

批准号：
1663822
负责人：
Shaul Mukamel
金额：
$ 48万
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：
2017
资助国家：
美国
起止时间：
2017-08-01 至 2021-07-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1663822&HistoricalAwards=false
关键词：
OP Molecular Radiative Relaxation Processes

项目摘要

Shaul Mukamel, of the University of California, Irvine is supported by an award from the Chemical Theory, Models and Computational Methods program in the Division of Chemistry. Mukamel and his coworkers design cutting-edge spectroscopy experiments and develop models and methods for interpreting the results. Understanding and controlling the motions of electrons and nuclei in molecules can determine the rates and outcomes of chemical reactions and energy transfer processes. These include the conversion of solar energy into electric energy in natural photosynthesis and in artificial light harvesting devices. This program develops methods for studying these elementary events by measuring the response of complex molecules to sequences of ultrafast optical laser pulses. Such experiments are made possible by newly-developed laser sources. Models and practical computational tools are developed for the interpretation and analysis of these experiments and extracting the underlying molecular information. Professor Mukamel and his research group collaborate closely with leading experimental research groups all over the world.Novel experimental techniques involving carefully-timed pulse sequences are designed and broadly applied to molecules and molecular aggregates as well as in the condensed phase. Spectroscopic techniques that aim at the direct detection of electronic and vibrational coherence, as well as nonadiabatic dynamics where the Born Oppenheimer approximation breaks down, are developed. Broadband resonant and off-resonant Raman techniques that can directly probe the passage of molecules through conical intersections are designed, and adequate protocols for their simulation are developed. A highly-intuitive, diagrammatic superoperator formalism is developed for computing the response of molecules to quantum and stochastic light and applied towards creating novel optical pulse sequences by utilizing pulse shaping, phase control, and chiral polarization configurations. New nonlinear signals aimed at providing unambiguous spectroscopic signatures of conical intersections through electronic and nuclear coherences are investigated. The quantum properties of light, such as photon entanglement are used as additional tools for probing molecules and chromophore aggregates by providing information that is not accessible by classical light. For example, entangled and squeezed photons offer temporal and spectral resolutions not achievable by other means. Detection schemes that combine coincidence measurements of individual entangled photons and interferometry are explored and used to investigate the elementary charge and energy migration processes in light harvesting in photosynthetic antennae and reaction centers. Signals involving multiple photon coincidence with temporal and spectral gating are predicted. Photon statistics measurements and higher-order radiation field correlation functions are calculated and shown to provide novel spectroscopic tools for molecular dynamical processes. Incoherent detection schemes of coherent optical signals by fluorescence or electric currents, which are very sensitive and can allow the study of single molecules are developed and investigated.

加州大学尔湾分校的Shaul Mukamel得到了化学理论，模型和计算方法计划的奖项的支持。 Mukamel和他的同事设计了尖端的光谱实验，并开发了解释结果的模型和方法。理解和控制分子中电子和核的运动可以确定化学反应和能量转移过程的速率和结果。这些包括在自然光合作用和人造光收集设备中将太阳能转化为电能。该程序通过测量复杂分子对超快光学激光脉冲序列的响应来开发研究这些基本事件的方法。新开发的激光源使这种实验成为可能。开发了模型和实用计算工具，用于解释和分析这些实验并提取基本的分子信息。 Mukamel教授及其研究小组与全世界的领先实验研究小组紧密合作。涉及精心定时脉冲序列的实验技术的设计并广泛应用于分子和分子聚集体以及凝结阶段。开发了旨在直接检测电子和振动连贯性的光谱技术，以及出生的Oppenheimer近似分解的非绝热动力学。设计了可以直接探测分子通过圆锥形交叉路口的通过，并开发了足够的模拟协议的宽带共振和谐振拉曼技术。开发了一种高度直觉的图形超级操作器形式主义，用于计算分子对量子和随机光的响应，并通过利用脉冲形状，相位控制和手性极化构型来应用于创建新型光学脉冲序列。研究了新的非线性信号，旨在通过电子和核一致性提供锥形交叉点的明确光谱特征。光（例如光子纠缠）的量子特性通过提供经典光无法访问的信息来探测分子和发色团骨料的其他工具。例如，纠缠和挤压的光子提供时间和光谱分辨率，无法通过其他方式实现。探索并用于研究光合作用天线和反应中心中的光收集中的基本电荷和能量迁移过程，并用于研究基本电荷和能量迁移过程的检测方案。预测涉及与时间和光谱门控的多个光子重合的信号。计算光子统计测量和高阶辐射场相关函数，并证明为分子动力学过程提供了新型的光谱工具。通过荧光或电流对相干光学信号的不一致检测方案，它们非常敏感并且可以允许研究单分子的研究。

项目成果

期刊论文数量（40）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

Flux-Conserving Diagrammatic Formulation of Optical Spectroscopy of Open Quantum Systems

DOI：
10.1021/acs.jpcc.9b08635
发表时间：
2019-09
期刊：
The Journal of Physical Chemistry C
影响因子：
0
作者：
S. Mukamel;Michael Galperin
通讯作者：
S. Mukamel;Michael Galperin

Two-Dimensional Impulsively Stimulated Resonant Raman Spectroscopy of Molecular Excited States

DOI：
10.1103/physrevx.10.011051
发表时间：
2020-02-28
期刊：
PHYSICAL REVIEW X
影响因子：
12.5
作者：
Fumero, Giuseppe;Schnedermann, Christoph;Scopigno, Tullio
通讯作者：
Scopigno, Tullio

X-Ray Sum Frequency Diffraction for Direct Imaging of Ultrafast Electron Dynamics

DOI：
10.1103/physrevlett.120.243902
发表时间：
2018-06-12
期刊：
PHYSICAL REVIEW LETTERS
影响因子：
8.6
作者：
Rouxel, Jeremy R.;Kowalewski, Markus;Mukamel, Shaul
通讯作者：
Mukamel, Shaul

Imaging of transition charge densities involving carbon core excitations by all X-ray sum-frequency generation

通过所有 X 射线和频生成对涉及碳核激发的跃迁电荷密度进行成像

DOI：
10.1098/rsta.2017.0470
发表时间：
2019
期刊：
Physical and Engineering Sciences
影响因子：
0
作者：
Cho, Daeheum;Rouxel, Jérémy R.;Kowalewski, Markus;Lee, JinYong;Mukamel, Shaul
通讯作者：
Mukamel, Shaul

Attosecond X-ray Diffraction Triggered by Core or Valence Ionization of a Dipeptide