CAREER: Molecular polaritonics: new opportunities for spectroscopy and control of charge and energy transport

职业：分子极化子学：光谱学以及电荷和能量传输控制的新机遇

基本信息

批准号：
1654732
负责人：
Joel Yuen-Zhou
金额：
$ 65.7万
依托单位：
University of California-San Diego
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：
2017-02-01 至 2025-01-31
项目状态：
未结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1654732&HistoricalAwards=false
关键词：
CAREER Molecular polaritonics new opportunities

项目摘要

Joel Yuen-Zhou, of the University of California San Diego (UCSD), is supported by an award from the Chemical Theory, Models and Computational Methods program in the Division of Chemistry and the Condensed Matter and Materials Theory program in the Division of Materials Research to develop theoretical and computational methods to study hybrid quantum mechanical states of light (photons) interacting excited molecular states (excitons). These light-matter hybrid states, known as polaritons, have emergent properties that do not exist in the separate components alone. This research harnesses the duality of polaritons to design ways in which light-matter interactions may be exploited to obtain novel ways to manipulate transport of charge and light-harvested energy. Typically, energy captured from sunlight moves across a molecular antenna in the form of excitons, neutral nanoscale excitations transported across molecules. Understanding and controlling exciton transport in molecular materials is a significant challenge for the theory of condensed phases physics and chemistry, as well as a primary concern for studies of photosynthesis and new light-harvesting technologies, such as organic solar cells. This project trains graduate students and postdoctoral fellows to be conversant on research at the intersection of theoretical chemistry, nano-photonics, and condensed matter theory. It also develops a broad outreach plan to school students via a series of performance choreographies mimicking collective phenomena in topological materials. Dr. Yuen-Zhou is also involved in developing a new orientation strategy to accommodate the increasing international graduate student population in his department at UCSD.Polaritons inherit wavelike properties from light such as extended spatial coherence, but also matter properties which allow energy to localize energy and give rise to a chemical reaction or to strong interactions between charged particles. This research harnesses the duality of polaritons to design ways in which light-matter interaction interact to produce phenomena that do not occur via each of the components alone. An example of this is enhanced charge transport or topologically-protected energy transport in the nano- and mesoscales. Here, topological refers to properties that do not require fine-tuning of parameters to survive, but rather, rely on global characteristics which are robust to material imperfections and impurities. This investigation focuses on the unusually delocalized exciton states of molecular polaritons. By noting that dipolar light-matter interaction is anisotropic and isomorphic to spin-orbit coupling, the research harnesses the latter to induce exotic polaritonic effects akin to those found in topological insulators, giving rise to spatial and directional control of nano- and mesoscale energy flow which is robust to disorder. These ideas are first tested on purely excitonic systems of porphyrin arrays and then on similar systems of chromophores in confined electromagnetic environments. Analogies to Dirac systems in two-dimensional materials such as graphene prove fruitful and give rise to unexplored frontiers of molecular aggregates. The Yuen-Zhou group also addresses recent observations suggesting that confined electromagnetic fields can enhance the conductivity of organic polymers owing to the formation of delocalized polaritons, opening new avenues for control of electron transport in molecular materials. Even though the project is theoretical in nature, it has a strong spectroscopic component aimed at simulating measurements that experimentalists might produce. Collaborations with experimentalists are a strong component of the work. Yuen-Zhou and coworkers are providing the first theoretical and computational framework to describe the interplay between topological band structures and vibronic degrees of freedom, including the deleterious or beneficial effects of vibrational decoherence. They are also studying a comprehensive theory for polaritons-assisted charge transport. These studies provide insights on the limits of controllability of energy and charge flow in the nano- and mesoscales, as well as new paradigms for the design light-harvesting technologies and optical logic devices. The development of the scientific component is accompanied by the training of graduate students and postdoctoral fellows in an interdisciplinary environment. Upon completion of their work, trainees are prepared to face a wide variety of contemporary scientific challenges, both in academic and industrial settings. The project also includes a multifaceted educational project with the goal of popularizing abstract concepts of topological phases of matter to a broad audience. This consists of a series of experiential and interpretative dance events termed Top-Dances, where high-school students participate in collective choreographies that aim to recreate energy and charge transport in quasi-two-dimensional materials such as those addressed in the project. These events are recorded, analyzed, digested in the events, and distributed in social media to provide alternative and intuitive ways to visualize the aforementioned concepts. Finally, as a response to the recent rise of international graduate students in the Department of Chemistry and Biochemistry of UCSD, Professor Yuen-Zhou also redesigns an orientation program with the goal of fostering a more effective integration of these students into a challenging academic and research environment. This goal is carried out through a series of workshops addressing issues of academic leadership and diversity, as well as the installation of a mentoring support network within the department.

加利福尼亚大学圣地亚哥分校（UCSD）的Joel Yuen-Zhou得到了化学理论，模型和计算方法计划的奖项，以及在材料研究中的凝结物和材料理论计划开发理论和计算方法中的凝结物质和材料理论计划，以研究杂交（光子）相互作用的杂交机械状态（ixcit Molectormult）（ICK ICKIT）。这些轻质杂种状态（称为北极子）具有仅在单独的组件中存在的新兴特性。这项研究利用了极化子的二元性来设计可利用光线相互作用的方式，以获取操纵电荷运输和轻度收获能量的新方法。通常，从阳光捕获的能量以激子的形式移动到分子天线，中性纳米级激发跨分子。在分子材料中理解和控制激子转运是凝结相物理和化学理论的重大挑战，也是光合作用和新的轻度收获技术（例如有机太阳能电池）研究的主要关注点。该项目训练研究生和博士后研究员在理论化学，纳米词汇和凝结物质理论的交集上进行研究。它还通过模仿拓扑材料中的集体现象的一系列表演编排为学校学生制定了广泛的外展计划。 Yuen-Zhou博士还参与制定一种新的取向策略，以适应UCSD的部门的国际研究生人数不断增长。Polaritons从诸如扩展的空间连贯性等光中继承了波动型的特性，但也可以使能量能够局部能量，并引起能量并引起化学反应或强烈的相互作用，从而引起了强烈的相互作用，或者是在带电的颗粒之间引起的强大相互作用。这项研究利用了极化子的二元性设计方式，使光结合相互作用相互作用以产生不单独通过每个组件发生的现象。一个例子是在纳米和介质中增强电荷运输或受拓扑保护的能量传输。在这里，拓扑是指不需要对参数进行微调的属性才能生存，而是依靠全球特征，这些特征可用于物质缺陷和杂质。这项研究集中于分子极化子的异常离域激子状态。通过注意到偶极光 - 摩托的相互作用是各向异性和同构与自旋轨道耦合的同构，该研究利用后者诱导类似于拓扑绝缘子发现的异国情调的极化效应，从而产生了对纳米和中心能量流动的空间和方向控制，这是强大的，这是强大的，这是稳固的。这些想法首先在卟啉阵列的纯激发量系统上进行测试，然后在密闭电磁环境中的发色团系统上进行测试。类似于二维材料（例如石墨烯）的狄拉克系统（Dirac Systems）证明了富有成效，并引起了未开发的分子聚集体的前沿。 Yuen-Zhou组还解决了最近的观察结果，该观察结果表明，由于形成了分离式极化子的形成，受封闭的电磁场可以提高有机聚合物的电导率，这为控制分子材料中电子传输的新途径开辟了新的途径。尽管该项目本质上是理论上的，但它具有强大的光谱成分，旨在模拟实验者可能会产生的测量。与实验者的合作是工作的重要组成部分。 Yuen-Zhou及其同事提供了第一个理论和计算框架，以描述拓扑带结构与振动自由度之间的相互作用，包括振动反应的有害或有益效应。他们还在研究北极星辅助电荷运输的综合理论。这些研究提供了有关纳米和介质中能量和电荷流的可控性限制的见解，以及设计光收获技术和光学逻辑设备的新范式。科学组成部分的发展伴随着跨学科环境中研究生和博士后研究员的培训。完成工作后，学员准备在学术和工业环境中面临各种当代科学挑战。该项目还包括一个多方面的教育项目，其目的是将物质拓扑阶段的抽象概念推广给广泛的受众。这包括一系列被称为上舞的体验和解释性舞蹈活动，高中生参加了集体编舞，旨在重新创建能源和电荷运输，以诸如项目中的诸如项目中的材料。在事件中记录，分析，消化这些事件，并在社交媒体中分发，以提供可视化上述概念的替代和直观的方式。最后，作为对UCSD化学和生物化学系的国际研究生最近兴起的回应，Yuen-Zhou教授还重新设计了一个方向计划，目的是将这些学生更有效地整合到一个充满挑战的学术和研究环境中。该目标是通过一系列研讨会来实现的，该研讨会解决了学术领导力和多样性的问题，以及在部门内部安装指导支持网络。

项目成果

期刊论文数量（14）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

Two-dimensional infrared spectroscopy of vibrational polaritons

DOI：
10.1073/pnas.1722063115
发表时间：
2018-05-08
期刊：
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
影响因子：
11.1
作者：
Xiang, Bo;Ribeiro, Raphael F.;Xiong, Wei
通讯作者：
Xiong, Wei

Manipulating optical nonlinearities of molecular polaritons by delocalization