Donor-Acceptor Energy Transfer involving Classical and Quantum Light in the Presence of Photonic and Plasmonic Structures

西北大学的George C. Schatz获得了化学系化学理论、模型和计算方法项目的奖励，他开发了描述由金属纳米粒子（通常是银、金或铝）介导的分子间能量转移的理论和模型，这种转移显示出被称为等离子激元激发的强光学吸收特性。该理论建立在过去能量转移研究的历史基础上，但这里适用于科学前沿的问题，其中能量转移可以扩展到10s nm到mm的距离，涉及传统微扰理论方法可能失效的强耦合，并且量子效应提供了对能量转移过程进行根本性改变的机会。涉及金属纳米粒子的能量转移在新兴光学技术中非常重要，包括与光开关、新型光学器件的开发、单光子发射器和安全通信相关的主题。Schatz还将研究与量子光相关的能量转移和其他特性，包括涉及两个纠缠光子的发射、吸收和能量转移。在这个项目中工作的学生和博士后包括相当数量的女性和少数民族，他们将获得独特的技能，可以用来开展自己的职业生涯。此外，还将向K-12团体、本科培训、众多研讨会和讲习班以及与公众的互动进行推广。金属纳米颗粒介导的能量传递是一个相对较新的研究领域，基于量子力学的分析理论是必不可少的。除了分析理论之外，研究还将研究使用该理论的计算算法，以及应用该理论来描述实验合作者所做的实验。该理论包括以下描述：(1)等离子体纳米粒子阵列附近的供体-受体能量转移，其中能量转移可以通过晶格的光学模式介导，并且可以通过控制阵列结构参数和发射器/吸收剂浓度来调节相干性和强光-物质相互作用的问题；(2)由单个或几个纳米粒子介导的能量传递，Schatz将开发一个完整的量子电动力学形式，将等离子体、激子和电磁态平等地结合在一起，并将在基于微扰理论的能量传递理论失效的情况下提供描述量子效应的能力；(3)与纠缠等离子激元耦合的量子光相关的能量转移，包括纠缠光子之间的干扰调制速率的供体-受体能量转移。此外，Schatz将与该领域的几位实验学家合作，他们正在研究与等离子体介导的供体-受体能量转移相关的问题，这些转移涉及供体、受体和纳米颗粒通过DNA结构组织的结构，或者涉及具有独特光学腔特征的阵列。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。

George C. Schatz of Northwestern University is supported by an award from the Chemical Theory, Models and Computational Methods program in the Division of Chemistry to develop theory and models that describe the transfer of energy between molecules that is mediated by metal nanoparticles (typically silver, gold or aluminum) that show strong optical absorption properties known as plasmon excitation. The theory builds from the past history of research on energy transfer, but here is adapted to problems at the leading edge of science, in which energy transfer can extend over distances from 10s of nm to mm, involves strong coupling where traditional perturbation theory approaches can break down, and where quantum effects provide opportunities for making fundamental changes to the energy transfer process. Energy transfer involving metal nanoparticles is important in emerging optical technologies, including topics related to optical switching, in the development of new types of optical devices, in single photon emitters, and in secure communications. Schatz will also study energy transfer and other properties associated with quantum light including the emission, absorption and energy transfer involving two entangled photons. The students and postdocs who work on this project include a significant number of women and minorities, and they will acquire unique skills that they can use to launch their own careers. In addition, there will be outreach to K-12 groups, undergraduate training, numerous seminars and workshops, and interactions with the public.The proposed work on energy transfer mediated by metal nanoparticles is a relatively new field where analytical theory based on quantum mechanics is essential. In addition to analytical theory, the research will pursue computational algorithms for using the theory, and applications of the theory to describe experiments done by experimental collaborators. The theory includes the description of: (1) donor-acceptor energy transfer near arrays of plasmonic nanoparticles where energy transfer can be mediated by optical modes of the lattice, and where issues of coherence and strong light-matter interactions can be tuned by controlling array structural parameters and emitter/absorber concentrations; (2) energy transfer mediated by individual or a few nanoparticles where Schatz will develop a full quantum electrodynamics formalism that incorporates plasmonic, excitonic and electromagnetic states on equal footing and which will provide the capability of describing quantum effects under circumstances where perturbation-theory based energy transfer theory breaks down; (3) energy transfer associated with quantum light that is coupled to entangled plasmons, including donor-acceptor energy transfer in which interference between the entangled photons modulates the rate. In addition, (4) Schatz will collaborate with several experimentalists in the field who are studying problems related to plasmon-mediated donor-acceptor energy transfer involving structures where the donor, acceptor and nanoparticles are organized via DNA structures, or that involve arrays with unique optical cavity features.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.