Plasmon Coupling Correlation Spectroscopy

在化学系化学测量和成像计划和材料研究部生物材料计划的支持下，波士顿大学的莱因哈德教授和他的团队正在开发光学光谱技术，在单分子水平上研究生物分子的结构和运动。单分子测量提供了关于每个分子的快速移动或罕见事件的信息，否则这些信息将被整体测量所掩盖。为了在如此小的范围内监测生物分子的运动和结构变化，莱因哈德教授制作了一种基于金纳米颗粒(NPs)光学相互作用的分子标尺。生物分子结构和运动的快速和细微变化导致这些金纳米粒子的光谱特征发生变化，这些特征可以快速捕获并用于了解生物分子的行为。这项发展的技术可以阐明蛋白质和其他生物分子的结构波动在复杂生物系统中的作用，这可能会导致生物、生物医学和环境研究的新进展。莱因哈德教授与他的研究生和本科生在这个项目上合作，为他们提供了一个在生物物理化学、生物等离子体和生物材料之间进行研究的机会。莱因哈德教授还组织研讨会，提供研究实习机会，并开发网络模块，与公众分享他的研究成果。他的推广活动的一个特别重点是吸引科学和工程领域代表性不足的群体的成员参与这个项目的研究。莱因哈德教授正在开发一种基于局域表面等离子体共振(LSPR)的相关光谱学。他利用等离子体NPs之间的距离依赖近场耦合，导致远场光谱波动来监控粒子间的分离，这将使他能够完全获得单个生物聚合物分子的长期信号相关性研究，而不需要闪烁的人工制品。在这个项目中，莱因哈德教授使用等离子体耦合相关光谱(PCCS)来测量纳米约束对DNA力学性质的影响，并在实验上测试了传统聚合物模型在纳米约束下的有效性。他还致力于了解内在无序蛋白质(IDP)的结构动力学，通过提供广泛频率范围内结构波动的准确表征，以便开发基于结构动力学的预测函数模型。能够阐明结构波动对无序蛋白质和其他生物聚合物功能的作用对于从根本上理解它们的工作机制是重要和必要的，这仍然是一个谜。该项目涉及测试在生物系统中普遍存在的空间纳米限制如何影响并可能改变生物聚合物的结构动力学。除了研究目标，莱因哈德教授还致力于一系列教育和外展活动，以积极指导学生进行跨学科研究，并鼓励未被充分代表的群体参与科学和工程。该奖项反映了NSF的法定使命，并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。

With support from the Chemical Measurement and Imaging Program in the Division of Chemistry and the Biomaterials Program in the Division of Materials Research, Professor Reinhard and his team at Boston University are developing optical spectroscopic techniques to investigate the structure and movement of biomolecules at the single molecule level. Single molecule measurements provide information about each molecules that move at a fast rate or rare events that would otherwise be buried by bulk measurements. To monitor the movement and structural changes of biomolecules at such a small scale, Professor Reinhard makes a molecular ruler based on optical interaction of gold nanoparticles (NPs). Fast and subtle changes in biomolecular structure and movements lead to changes in the spectral signature of these gold NPs, which can be captured at fast speed and be used to understand the behavior of biomolecules. The developed technique could elucidate the role of structural fluctuations of proteins and other biomolecules in complex biological systems, which could lead to new advances in biological, biomedical, and environmental research. Professor Reinhard works with his graduate and undergraduate students on the project, providing them an opportunity to work at the interface between biophysical chemistry, bioplasmonics, and biomaterials. Professor Reinhard also organizes workshops, offers research internships, and develops web-modules to share with the general public of his research outcomes. A particular emphasis of his outreach activities is to attract members of groups that are underrepresented in science and engineering to the research of this project.Professor Reinhard is developing a localized surface plasmon resonance (LSPR) based correlation spectroscopy. He utilizes distance-dependent near-field coupling between plasmonic NPs that cause spectral fluctuations in the far-field to monitor interparticle separations which would allow him to obtain long-time signal correlation studies of individual biopolymer molecules entirely without blinking artefacts. In this project, Professor Reinhard uses plasmon coupling correlation spectroscopy (PCCS) to measure the effect of nanoconfinement on the mechanical properties of DNA and experimentally test the validity of conventional polymer models under nano-confinement. He also works on understanding the structural dynamics of intrinsically disordered proteins (IDPs) by providing an accurate characterization of the structural fluctuations over a broad frequency range in order to develop predictive function models based on structural dynamics. The ability to elucidate the role of structural fluctuations for the function of disordered proteins and other biopolymers is important and necessary to develop a fundamental understanding of their working mechanism, which remains enigmatic. The project involves testing how spatial nanoconfinement, which is ubiquitous in biological systems, effects and potentially changes the structural dynamics of biopolymers. Besides the research goals, Professor Reinhard is working on a series of educational and outreach activities to actively mentoring students in interdisciplinary research and encourage the participation of underrepresented groups in science and engineering.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.