TOWARD SINGLE MOLECULE NANOCAVITY POLARITONS
Abstract
The goal of this research proposal is to develop a microscopy and spectroscopy system that allows temperature dependent investigation of molecular polaritons in optical nanocavities, pushing the limit of strong coupling to a single and a few molecules level. Single molecule polaritons have the necessary attributes for creating repeatable qubits for quantum information technology, sensing and fundamental studies of photochemistry. There is currently only one report that claims observation of single molecule polaritons at room temperature based on dark-field scattering spectral splitting that has been attributed to the hybridization molecular and plasmonic cavity resonances. However, close observation of the experimental results in this singular report reveals misinterpretation of data that arises from ignoring the photochemical conversion of the molecules at ambient condition. In addition, recent studies indicate that the conclusion of strong coupling based on spectral splitting in dark-field scattering signal can be misleading due to other contributing factors. The proposed instrumentation aims to provide unambiguous evidence for the creation of molecular polaritons by relying on temperature-dependent photoluminescence measurements for confirming signatures of strong coupling in carefully integrated moleculenanocavity systems. The specific experiments that will be performed using the new capability includes investigation of molecular polaritons in RoM (rod-on-mirror) nanocavities that support plasmon resonances with superior optical quality than other nanocavities. The resonance energy of the RoM plasmonic nanocavities will be tuned by changing the gap length with sub-nanometer accuracy, and the fundamental optical properties will be established by analyzing inelastic light scattering, photothermal effects, electron-plasmon-vibration coupling and chemical reactivity. Molecular polaritons will be investigated systematically to achieve strong coupling at single molecule level by placing and orienting molecules at optimal distances from the metal surfaces. Sample fabrication will be carried out by taking advantage of the advanced materials fabrication facilities available within the University of New Mexico (UNM) as well as in the national labs particularly the Center for Integrated Nanotechnologies, Sandia National Labs. The development of the instrumentation will have transformational impact on enhancing the quality and depth of the research activities in the PI’s lab (currently supported by the AFOSR Grant No. FA9550-18-1-0512), while enhancing collaborations with researchers within UNM and the federal labs in New Mexico including the Air Force, Sandia and Los Alamos National Labs. The capability will improve the educational outcomes for the undergraduate and graduate students, who will be involved in the research activities that are of interest to the Department of Defense.
Document Details
- Document Type
- DoD Grant Award
- Publication Date
- Apr 20, 2023
- Source ID
- FA95502210477
Entities
People
- Terefe G Habteyes
Organizations
- Air Force Office of Scientific Research
- United States Air Force
- University of New Mexico