Collaborative Research: Plasmonically-Induced Phase-Correlated Ultralong Transport of Excitation Energy in Viral Quantum Dot Circuits

某些光合作用有机体的一个令人振奋的特征是它们能够以显著的效率和范围将能量从一种蛋白质转移到另一种蛋白质。研究表明，在生理温度下，这种非凡的光捕获过程深深植根于量子力学过程。在由生物组装的纳米结构组成的系统中，模拟这种过程以产生沿特定路径的高效和超长范围的能量流动，是具有许多技术影响的变革性研究前沿。这需要未知的能力来控制真实空间中的能量传输路线，而损失非常小。该项目是阿拉巴马大学亨茨维尔分校纳米光子学专业研究小组和俄克拉荷马大学病毒纳米技术研究小组之间的跨学科合作。该团队将开发与纳米设备及其集成相关的变革性概念和物理/生物过程，允许在与纳米设备及其集成相关的超长距离病毒能量电路中转移激发能量。受生物启发的能量电路将由一根纳米线和两个指定的纳米晶组成，纳米线由可遗传修饰的蛋白质景观(噬菌体)和半导体纳米晶体形成，两个指定的纳米晶体充当光收集和接收器天线。该团队将开发一种新的材料平台，可以极大地改变此类纳米晶体的正常性质，允许病毒纳米线通过紧密模仿光合作用过程来远距离传输能量。这包括通过它们与金属纳米结构的相互作用而相互关联的纳米晶域之间的能量转移。该项目为构建纳米尺度的设备提供了一条生物学应用的新途径。它还将为设计用于发光设备、探测器和传感器的高效生物-无机混合系统创造新的机会。这个跨学科的项目将通过实施强有力的教学和辅导部分来整合物理和生物教育，并将向高中生介绍纳米技术和纳米科学的精髓。技术上，该项目的总体目标是为能量传输材料发展具有变革性的概念和物理/生物过程，其中将涉及生物-无机复合结构和生物启发的集体性质。这些过程允许在与纳米设备及其集成(100纳米或更长)相关的超长距离上在病毒能量电路中转移激发能量。通过基因工程无毒病毒形成的量子点纳米线将被用作能量通道。这些包裹着量子点的病毒纳米线将在生物上连接到一端的捕光天线(上转换纳米粒子)和另一端的量子点接收器，形成生物模板化的能量电路。该团队将开发一种名为金属氧化物等离子体元基质(MOPM)的材料结构的新景观，以产生所需的转化过程，使光收集纳米天线吸收的光能以低能量损失沿着量子点纳米线传输到量子点接收器。MOPM将通过创造性地组合金属纳米天线阵列、介质材料和金属氧化物来形成。将生物模板能量电路固定到MOPM上导致(I)在病毒纳米线上的量子点之间形成相位相关的偶极-偶极耦合区域，(Ii)它们的辐射衰减(Purcell效应)的超高增强，以及(Iii)它们的缺陷环境的抑制。能量在病毒量子点纳米线上的传输是通过激发能量在相关域之间而不是单个量子点之间的转移来实现的，并且通过表面晶格共振或等离子体耦合形成域间耦合。MOPM显著增强了量子点诱导的激子-等离子体耦合，使量子点的偶极子排列在每个区域，同时抑制了它们的能量向金属纳米天线的转移。这一奖项反映了NSF的法定使命，通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

An inspiring feature of certain photosynthetic organisms is their ability to transfer energy from one protein to another with significant efficiency and range. It has been shown that such a remarkable light harvesting process is deeply rooted in quantum mechanical processes at physiological temperatures. Imitating such processes to generate efficient and ultra-long range of flow of energy along specific paths in systems consisting of biologically assembled nanostructures is a transformative frontier of research with many technological impacts. This requires uncharted capabilities to control the energy transfer routes in real space with very low amount of loss. This project is a collaborative interdisciplinary effort between research groups with expertise in nanophotonics at the University of Alabama in Huntsville and virus nanotechnology at the University of Oklahoma. The team will develop transformative concepts and physical/biological processes that allow transfer of excitation energy in viral energy circuits over ultra-long distances that are relevant to nanodevices and their integration. The biologically-inspired energy circuits will consist of a nanowire, formed via a genetically modifiable protein landscape (phage) and semiconductor nanocrystals, and two designated nanocrystals that act as light harvesting and receiver antennas. The team will develop a novel material platform that can dramatically change the normal properties of such nanocrystals, allowing the viral nanowires to transport energy over long distances by closely imitating photosynthesis process. This includes energy transfer between domains of nanocrystals correlated with each other via their interaction with metallic nanostructures. This project offers a new path towards application of biology for building devices with nanoscale dimension. It will also create new opportunities for the design of efficient bio-inorganic hybrid systems for light emitting devices, detectors, and sensors. This interdisciplinary project will integrate physical and biological education by implementing a strong teaching and mentoring component, and will introduce the essence of nanotechnology and nanoscience to high school students. Technical The overall goal of this project is to develop transformative concepts and physical/biological processes for energy-transporting materials that will involve bio-inorganic composite structures and biologically-inspired collective properties. These processes allow transfer of excitation energy in viral energy circuits over ultra-long distances that are relevant to nanodevices and their integration (100 nm or more). Quantum dot nanowires formed via genetically engineered non-toxic virus will be used as energy channels. These quantum dot-coated viral nanowires will be biologically conjugated to a light harvesting antenna (Up-Conversion Nanoparticles) in one end and quantum dot receivers at the other end, forming biologically-templated energy circuits. The team will develop a novel landscape of material structure called metal oxide plasmonic metasubstrate (MOPM) to generate the transformative processes needed to allow the light energy absorbed by the light harvesting nanoantennas to be transported to the QD receivers along QD nanowires with low energy loss. MOPMs will be formed via the creative composition of metallic nanoantenna arrays, dielectric materials, and metal oxides. Immobilizing the biologically-templated energy circuits to MOPM leads to (i) formation of domains of phase-correlated dipole-dipole coupling between QDs across the viral nanowires, (ii) ultrahigh enhancement of their radiative decay (Purcell effect), and (iii) suppression of their defect environments. The transport of the energy across viral QD nanowires occurs via the transfer of excitation energy between the phase-correlated domains, rather than between individual QDs, and formation of inter-domain coupling using surface lattice resonances or plasmonic coupling. MOPM enhances QD-induced exciton-plasmon coupling significantly, aligning the dipoles of QDs in each domain while suppressing transfer of their energies to the metallic nanoantennas. These lead to ultralong range inter-domain energy transfer before radiative or non-radiative losses kick in.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.