The goal of the proposed research is to utilize fundamental light-matter interactions of strong coupling and confinement, facilitated by hybrid plasmonic and dielectric metamaterials, to alter molecular potential energy surfaces (PESs). Optical control of molecular potential energy surfaces by these strong light-matter interactions can be used to control chemical reaction dynamics. Strong coupling has recently been explored in a variety of plasmonic and dielectric materials to enable the following: Rabi splitting, enhanced chemical reactivity, and delocalized vibrational coherence. Our central objective is to demonstrate how strong light-matter interactions can be used for innovation in chemistry, materials science, and photonics. This research proposal explores three interrelated topics aimed at deeper understanding and utilization of strong coupling and confinement with hybrid plasmonic-dielectric metamaterials. Topic 1: Strong coupling of plasmonic-dielectric metamaterials for Rabi splitting in optical devices. We will control Rabi splitting in optical devices through the use of hybrid plasmonic waveguides (HPWGs). Using HPWGs we will (1) create static two-level splitting in J-aggregated doped HPWGs; (2) design the first excited state transient Rabi splitting optical device with HPWGs; (3) investigate the timescales of Rabi splitting using different excited state lifetimes of dopant molecules in the HPWG. Topic 2: Confinement effects on PESs investigated and utilized with stimulated Raman scattering (SRS). SRS has been proposed as an explanation for the observation of new chemical phenomena in strongly confined optical cavities. We propose a detailed investigation of SRS in the strong confinement regime for: (1) understanding the influence of the optomechanical cavity theory (OCT) to tip-enhanced Raman scattering (TERS); (2) observe coherent Raman scattering (CRS) effects in spontaneous Raman scattering by light-matter interactions with the tip-sample junction in TERS; (3) use the effects of confinement with SRS in TERS to study elementary reactions of small nonresonant molecules. Topic 3: Polaritonic molecular states by strong confinement and coupling. To understand polaritonic molecular states that arise from strong coupling and confinement by cavity modes, we will: (1) use the sensitivity of CRS to probe small molecule strong coupling in molecular-optical cavity polaritonic states and (2) perform spectroelectrochemistry in coupled molecular-electrochemical cavities to examine vibrational polaritonic effects.
|Effective start/end date||9/30/17 → 3/31/24|
- Office of Naval Research (N00014-17-1-3024 P00005)
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