Title: Nanoscale Control of Molecules via Strong Light-Matter Interactions

Abstract:

I propose to remotely manipulate molecules at the nanoscale using strong light-matter

interactions. When light and matter exchange energy faster than their dephasing, hybrid light–

matter states known as polaritons are formed. These polariton states provide an exciting avenue to

manipulate matter with light. Recent research has shown that polaritons can form with molecules via an optical resonator that sufficiently enhances the light-matter interaction. Molecular polariton formation results in modifications to chemical properties such as chemical reactivity or conductivity; however, the effects are small and poorly understood. I seek to create nanoscale molecular polaritons, comprising only hundreds or just tens of molecules, to not only enhance polariton-mediated effects, but to also gain mechanistic insights afforded by the controlled nanoscale setting. My objectives are to: (1) develop optical resonators that confine polaritons to the nanoscale and (2) use these polaritons to control chemical properties such as the rate of charge transfer. Toward the first objective, I will pursue novel optical resonator schemes, making use of surface plasmon/phonon-polariton excitations in nanomaterials, to produce nanoscale molecular polaritons. Since polariton dynamics occurs on the sub-picosecond timescale, the molecular polaritons will be probed using ultrafast spectroscopy. My research is informed by my background studying the photoconductivity of single-molecule junctions using the scanning tunneling microscope-based break junction technique. The proposed work, under the co-mentorship of Drs. Andrew Musser, Greg Fuchs, and Jeff Moses, will allow controlled excitation and manipulation of molecular polaritons at the nanoscale, enabling applications in energy conversion, molecular sensing, and quantum information science.