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

华盛顿大学的大卫J. Masiello得到了化学系化学理论、模型和计算方法项目的CAREER奖的支持，以开发第一个能够关联快速（即，Masiello教授及其研究小组将特别：1）建立第一性原理、多尺度的理论框架，能够严格描述当分子与等离子体激元环境强烈耦合时，分子电子结构的严重变形，用连续电动力学来描述; 2）数值实现快速电子的电动力学及其与复杂纳米级环境的相互作用，以表征电子和光子驱动的等离子体激元激发及其相关纳米光子性质之间的关系; 3）关联电子激发源和光子激发源以了解在量子发射器/吸收器的存在下等离子体活性金属纳米结构中近场和远场之间的能量再分配以及纳米限制热，重点是实现高空间和光谱分辨率。这项研究将广泛影响下一代切割-在纳米光子学和纳米等离子体的边缘实验，通过建立严格的和计算易处理的理论方法，能够阐明和预测观察的第一原理的方式。 重大的影响将在理解各种等离子体增强的分子光学过程，从线性和非线性光学光谱传感和催化，下降到单分子水平。 从这项研究中获得的知识将为未来医疗和国防部门使用的高效太阳能集光设备和化学传感器奠定基础。 Masiello教授和他的小组还将通过华盛顿大学的数学学院和路易斯·斯托克斯少数民族参与桥梁计划联盟，在高中和大学阶段指导代表性不足的少数民族学生。 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增强的新型太阳能电池架构的效率，从而激发少数民族对科学，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.