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Tuesday, October 8th, 3:30-4:30 PM

Physics Building, Room 104

M. Sheldon

University of California, Irvine

Abstract

We are developing experimental platforms to probe vibrational strong coupling (VSC) between molecules and resonant infrared (IR) nanophotonic architectures, in order to understand how this coupling can fundamentally control chemical reactivity, as well as enable new classes of light-matter interaction. This method of altering the potential energy surface of a chemical process via coherent, electromagnetic perturbation of vibrating bonds has also been termed “polaritonic chemistry”. We employ a combined experimental strategy leveraging expertise in (1) the design of IR “metasurfaces” composed of plasmonic metal substrates that provide tailorable VSC to molecules within their optical near-field; and (2) multiple continuous wave (CW) spectroscopic techniques that enable analysis of several non-equilibrium, dynamic electronic effects in the metal substrate. Taken together, these tools allow studies into new regimes of spectral bandwidth (e.g. simultaneous multi-mode coupling), coupling strength, and time domains (e.g. studies of long lived and steady-state phenomena) that have been inaccessible using conventional optical cavities and time-resolved spectroscopies performed to date.

Vibrational strong coupling is fundamentally interesting because it is a coherent interaction between radiation and molecular motion. The direct manipulation of a molecular process using externally controlled forcefields to obtain a desired outcome, i.e. “coherent control” or “quantum control”, has been a long-standing goal connected to the central aims of chemical science. Thus, this presentation will discuss the limits of physiochemical control at interfaces leveraging a framework based on coherent interactions between controllable features of the engineered surface geometry and the molecular systems under study.

 Bio

Matthew T. Sheldon received his BA from Carleton College (Chemistry), PhD from UC Berkeley (Chemistry), and performed his postdoc at Caltech (Mat.Sci./App.Phys.). He is the recipient of the 2015 Air Force Office of Scientific Research Young Investigator Program (AFOSR YIP) Award, the Kaneka Junior Faculty Award (2017), and was selected as a 2017 Inventor Fellow by the Gordon and Betty Moore Foundation.  In 2019 he was elected to the executive committee of the American Physical Society (APS) Topical Group on Energy Research and Applications (GERA), and in 2021 he was awarded the Early Career award from the journal Nanophotonics. He started his independent career at Texas A&M University (Chemistry) and moved to the University of California, Irvine (Chemistry) in January 2024.

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