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

某些光合生物的一个令人鼓舞的特点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，这种非凡的光收集过程深深植根于生理温度下的量子力学过程。模仿这些过程，在生物组装纳米结构组成的系统中沿特定路径产生高效和超长距离的能量流，是一个具有许多技术影响的变革性研究前沿。这需要未知的能力，以非常低的损失来控制真实空间中的能量传递路线。该项目是亨茨维尔阿拉巴马大学纳米光子学研究小组和俄克拉荷马大学病毒纳米技术研究小组之间跨学科合作的成果。该团队将开发变革性的概念和物理/生物过程，使病毒能量电路中的激发能在与纳米器件及其集成相关的超长距离上转移。这种受生物启发的能量电路将由一条由基因修饰的蛋白质景观（噬菌体）和半导体纳米晶体组成的纳米线，以及两种指定的纳米晶体，分别充当光收集和接收天线。该团队将开发一种新的材料平台，可以极大地改变这种纳米晶体的正常特性，使病毒纳米线能够通过模仿光合作用过程远距离传输能量。这包括通过与金属纳米结构相互作用而相互关联的纳米晶体域之间的能量转移。该项目为应用生物学构建纳米级器件提供了一条新的途径。它还将为设计用于发光器件、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指导组成部分来整合体育和生物教育，并将向高中生介绍纳米技术和纳米科学的本质。该项目的总体目标是为能量传输材料开发变革性概念和物理/生物过程，这些材料将涉及生物无机复合结构和生物启发的集体特性。这些过程允许病毒能量电路中的激发能在与纳米器件及其集成（100纳米或更远）相关的超长距离上转移。通过转基因无毒病毒形成的量子点纳米线将被用作能量通道。这些量子点包覆的病毒纳米线一端与光收集天线（上转换纳米粒子）结合，另一端与量子点接收器结合，形成生物模板化的能量电路。该团队将开发一种称为金属氧化物等离子体元基板（MOPM）的新型材料结构景观，以产生所需的转换过程，使光收集纳米天线吸收的光能沿着量子点纳米线以低能量损失传输到量子点接收器。mopm将通过金属纳米天线阵列、介电材料和金属氧化物的创造性组合而形成。将生物模板化的能量电路固定在MOPM上导致(i)在病毒纳米线上的量子点之间形成相相关的偶极子-偶极子耦合域，（ii）其辐射衰减的超高增强（Purcell效应），以及（iii）抑制其缺陷环境。病毒量子点纳米线之间的能量传输是通过在相相关域之间而不是在单个量子点之间传递激发能，以及利用表面晶格共振或等离子体耦合形成域间耦合来实现的。MOPM显著增强了量子点诱导的激子-等离子体耦合，使量子点在每个域中的偶极子对齐，同时抑制了量子点的能量向金属纳米天线的转移。在辐射或非辐射损失开始之前，这些导致了超长范围的域间能量转移。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。

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.