CAREER: Elucidating Light-Matter Interactions on the Nanoscale Using Quantum Many-Body Theory and the Electrodynamics of Swift Electrons

华盛顿大学的David J. Masiello获得了化学部门化学理论、模型和计算方法项目的CAREER奖，他开发了纳米级光-物质相互作用的第一个多尺度理论，能够将快速（即相对运动）电子与光子相关联，以阐明嵌入在极端等离子体支持环境中的量子发射器/吸收器的结构和动力学。特别是，Masiello教授和他的研究小组将：1)建立一个第一性原理，多尺度的理论框架，能够严格描述当与等离子体环境强耦合时分子电子结构的严重变形，由连续统电动力学描述；2)数值模拟快速电子的电动力学及其与复杂纳米环境的相互作用，以表征电子和光子驱动的等离子体激发之间的关系及其相关的纳米光子性质；3)将电子和光子激发源关联起来，了解等离子体活性金属纳米结构中存在量子发射体/吸收体时，近场和远场以及纳米限制热之间的能量再分配，重点是实现高空间和光谱分辨率。这项研究将通过建立严格的、计算上易于处理的理论方法，以第一性原理的方式阐明和预测观测，广泛地影响下一代纳米光子学和纳米等离子体学的前沿实验。将对理解各种等离子体增强的分子光学过程产生重大影响，从线性和非线性光谱学到传感和催化，直至单分子水平。从这项研究中获得的知识将为未来在医疗和国防部门使用的高效太阳能收集设备和化学传感器奠定所需的基础科学基础。Masiello教授和他的团队还将通过华盛顿大学数学学院和路易斯·斯托克斯少数民族参与联盟桥梁项目，指导高中和大学阶段被忽视的少数民族学生。这些努力的目标是通过使用先进的计算技术来模拟通过添加等离子体纳米粒子组件而提高的新型太阳能电池结构的效率，从而激发未被充分代表的少数群体对科学、技术、工程和数学的兴趣。

David J. Masiello of the University of Washington is supported by a CAREER award from the Chemical Theory, Models and Computational Methods program in the Chemistry division to develop the first multiscale theory of nanoscale light-matter interaction capable of correlating swift (i.e., relativistically moving) electrons with photons to elucidate the structure and dynamics of quantum emitters/absorbers embedded within extreme plasmon-supporting environments.In particular, Professor Masiello and his research group will:1) Establish a first-principles, multiscale theoretical framework capable of rigorously describing the severe deformations of a molecule's electronic structure when coupled strongly to a plasmonic environment, described by continuum electrodynamics;2) Numerically implement the electrodynamics of a swift electron and its interactions with a complex nanoscopic environment to characterize the relationship between electron and photon-driven plasmonic excitations and their associated nanophotonic properties;3) Correlate electron- and photon-excitation sources to learn about the redistribution of energy between near- and far-field and nanoconfined heat in plasmonically active metal nanostructures in the presence of quantum emitters/absorbers, with an emphasis on the achieving high spatial and spectral resolution.This research will broadly impact the next generation of cutting-edge experiments in nanophotonics and nanoplasmonics by establishing rigorous and computationally tractable theoretical methods capable of elucidating and predicting observation in a first-principles manner. Significant impact will be made in understanding a variety of plasmon-enhanced molecular-optical processes from linear and nonlinear optical spectroscopy to sensing and catalysis, down to the single-molecule level. The knowledge gained from this research will establish the basic scientific underpinnings needed for future high-efficiency solar light-harvesting devices and chemical sensors of use in the medical and defense sectors. Professor Masiello and his group will also mentor under-represented minority students at the high-school and college-level through the University of Washington's Math Academy and Louis Stokes Alliance for Minority Participation Bridge Program. The goal of these efforts is to stimulate interest in science, technology, engineering, and mathematics among under-represented minorities by using advanced computational techniques to simulate the increased efficiency of novel solar-cell architectures enhanced by the addition of plasmonic nanoparticle assemblies.