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

University Of Washington, Seattle WA

Investigators

Abstract

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.