Theoretical studies of coherent energy transfer in photosynthetic systems

光合系统相干能量转移的理论研究

• 批准号: 1112825
• 负责人: Jianshu Cao
• 金额: $ 42万
• 依托单位: Massachusetts Institute of Technology
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2011
• 资助国家: 美国
• 起止时间: 2011-07-01 至 2016-06-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1112825&HistoricalAwards=false
• 关键词: Theoretical; studies; coherent; energy; transfer

Jianshu Cao of the Massachusetts Institute of Technology is supported by an award from the Chemical Theory, Models and Computational Methods program in the Chemistry Division to computationally investigate how efficient and robust coherent energy transfer arises in photosynthesis and how structure-function relations observed in light-harvesting systems can help the design of artificial energy devices. The steps involved in the current project will involve (1) characterizing quantum coherence in light-harvesting systems, (2) using the stochastic wave-function method to realistically explore spatial-temporal correlations in the presence of disorder and noise, and (3) applying optimal design theory to maximizing energy transfer and thus exploring the importance of connectivity and symmetry in donor-acceptor arrays. Understanding the microscopic mechanisms of energy transfer in photosynthetic systems is of larger significance since it is reasonable to expect that coherent transfer within collaborative protein environments may become a pervasive theme in the future. This work will, in addition to providing cutting-edge training for students and postdocs, be incorporated in the MIT curriculum, public-access MIT OpenCourseWare and public lectures on photosynthesis and basic energy sciences.Photosynthesis in plants starts with the absorption of light by proteins in chlorophyll-containing photosynthetic reaction centers. The absorbed energy is rapidly transferred elsewhere in the complex protein environment by transfer of electrons to be stored as chemical energy. A mystery of much interest is how the electron transfer events occur in such a way as to avoid randomizing the energy before storage occurs. These ultrafast events are increasingly able to be studied by new laser-based experiments, but modeling the proteins by classical ball-and-spring models cannot reproduce the coordinated, or coherent, energy transfer. Coherence is usually regarded as requiring a description by quantum mechanics, and the PI is therefore developing quantum mechanical approaches to understanding the microscopic mechanisms underlying extremely efficient energy transfer in photosynthesis. The fact that nature has found a way to establish this collaboration in complicated protein environments raises the hope, to be explored in this project, that we can learn to control and optimize energy transfer efficiency for application in future man-made light-harvesting devices.

麻省理工学院的曹建树得到了化学系化学理论、模型和计算方法项目的一项奖励的支持，该奖项旨在通过计算研究光合作用中如何产生高效而稳健的相干能量转移，以及在光收集系统中观察到的结构-功能关系如何有助于人工能源设备的设计。本项目涉及的步骤包括：(1)表征光捕获系统中的量子相干性，(2)使用随机波函数方法在无序和噪声存在的情况下现实地探索时空相关性，以及(3)应用优化设计理论来最大化能量转移，从而探索连通性和对称性在施主-受主阵列中的重要性。理解光合作用系统中能量转移的微观机制具有更大的意义，因为可以合理地预期协同蛋白质环境中的相干转移可能成为未来普遍存在的主题。除了为学生和博士后提供尖端培训外，这项工作还将被纳入麻省理工学院的课程、公共访问的麻省理工学院开放式课程以及关于光合作用和基础能源科学的公共讲座。植物中的光合成始于含有叶绿素的光合作用反应中心的蛋白质对光的吸收。被吸收的能量通过电子的转移迅速转移到复杂的蛋白质环境中的其他地方，并储存为化学能。一个非常令人感兴趣的谜团是，电子转移事件是如何发生的，以避免在存储发生之前将能量随机化。越来越多的人能够通过新的基于激光的实验来研究这些超快事件，但用经典的球弹模型对蛋白质进行建模，不能再现协调的或连贯的能量转移。相干性通常被认为需要量子力学的描述，因此PI正在开发量子力学方法来理解光合作用中极其有效的能量转移背后的微观机制。大自然已经找到了在复杂的蛋白质环境中建立这种合作的方法，这一事实增加了我们在这个项目中探索的希望，即我们可以学习控制和优化能量转移效率，以便应用于未来的人造光收集设备。

项目成果

Efficiency at maximum power of a laser quantum heat engine enhanced by noise-induced coherence

通过噪声引起的相干性增强激光量子热机最大功率的效率

• DOI: 10.1103/physreve.97.042120
• 发表时间: 2018-04-13
• 期刊: PHYSICAL REVIEW E
• 影响因子: 2.4
• 作者: Dorfman, Konstantin E.;Xu, Dazhi;Cao, Jianshu
• 通讯作者: Cao, Jianshu

A unified stochastic formulation of dissipative quantum dynamics. I. Generalized hierarchical equations

• DOI: 10.1063/1.5018725
• 发表时间: 2018-01-07
• 期刊: JOURNAL OF CHEMICAL PHYSICS
• 影响因子: 4.4
• 作者: Hsieh, Chang-Yu;Cao, Jianshu
• 通讯作者: Cao, Jianshu